£EPA
820-R-10-015
Fluoride: Exposure and
Relative Source
Contribution Analysis
Health and Ecological Criteria Division
Office of Water
December 2010
U.S. Environmental Protection Agency
Washington, D.C.
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PREFACE
In March, 2006, the National Academy of Sciences National Research Council (NRC) released
the Report entitled "Fluoride in Drinking Water: A Scientific Review of EPA's Standards". The
NRC stated that "in light of the collected evidence on various health endpoints and total
exposure to fluoride, the committee concludes the EPA's MCLG of 4 mg/L should be lowered".
They further suggested that, in order to develop an MCLG (Maximum Contaminant Level Goal)
that is protective against severe enamel fluorosis, clinical stage II skeletal fluorosis and bone
fractures, EPA should:
Develop better estimates of total exposure for individuals,
Use current approaches for quantifying risk,
Consider susceptible populations, and
Characterize uncertainties and variability.
In response to the NRC (2006) recommendations, the Office of Water (OW) collected available
data on the various media that contribute to fluoride exposure in the United States for the
purpose of estimating total exposures for children during the period of sensitivity to severe dental
fluorosis (six months to 14 years). Data were also collected to develop an exposure estimate for
the adult population. This document presents the exposure analysis.
The objective of the OW's exposure and relative source contribution analysis was to quantify the
fluoride exposures for children and adults in the United States to accomplish the following:
Determine sources of fluoride exposure for the U.S. population.
Quantify exposures where possible for the age groups of concern.
Compare oral intake estimates to the reference dose established in the companion dose-
response assessment.
Estimate the relative source contribution for each exposure source.
Provide information for use in characterizing opportunities for reducing population risk
from fluoride in public drinking water systems and facilitating any necessary
adjustment in the regulatory non-enforceable Maximum Contaminant Level Goal
(MCLG).
This document addresses the relative source contribution for drinking water from public systems
and contains information from peer-reviewed publications on multiple topics; these topics
include concentrations of fluoride in foods and beverages, estimated dietary exposure estimates
for fluoride, concentrations of fluoride in tap water delivered by public drinking water systems,
estimated fluoride intakes from toothpaste, and estimated fluoride exposures from sulfuryl
fluoride (a pesticide).
In addition, this report presents background on the analytical methods used to measure fluoride
in various media, as well as approaches applied in developing dietary exposure assessments. The
background information is included to provide perspective on how methods of analysis used in
individual studies have impacted the exposure estimates.
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There are a number of factors that the reader should consider when reviewing this document
characterizing the relative source contribution from tap water to total fluoride intake:
Only peer-reviewed and published data from the United States and Canada were used in
the assessment (excepting the Information Collection Request data collected by Office of
Water for the second six-year review of its regulations).
Water intakes are those for public water systems and consumers only (EPA, 2004).
EPA conducted no independent study measuring dietary exposure; data employed are
from the published papers.
Exposure estimates for sulfuryl fluoride were prepared for the OW by the Office of
Pesticide Programs.
Office of Water policies applied in the relative source contribution analysis are those
presented in EPA (2000b).
The age groupings selected were those used by Ershow and Cantor (1987). The Ershow
and Cantor (1987) publication provided the best available water intake data for the time
period of the critical study (1930-1940).
The document is structured (see map below) to present the published information available on
fluoride in foods (Chapter 2), fluoride in drinking water from public and nonpublic sources
(Chapter 3), fluoride in toothpaste (Chapter 4), and fluoride from more minor exposure sources
(Chapter 5). Each chapter also presents published exposure estimates applicable to each
exposure medium when available. Chapters 2 and 3 include background data on the analytical
methods used for the analyses in the cited studies and the experimental approaches used to assess
dietary exposures.
Chapter 6 identifies the studies selected for the quantitative exposure analysis and the reasons
supporting their selection. The RSC calculations and sensitivity analysis are found in Chapter 7
while Chapter 8 compares current exposure values to the reference dose from the dose-response
document (EPA, 2010a) and nutritional guidelines from the Institute of Medicine (IOM, 1997).
Appendices A and B located at the end of this document (beginning at page 127), were provided
by the Office of Pesticide Programs and retain their original pagination.
The OW has also prepared and peer reviewed a second document that provides an estimate of the
RfD for fluoride. This second document, Fluoride: Dose-Response Analysis for Non-cancer
Effects (EPA Report No. 820-R-10-019), can be accessed through the following url:
..http : //water . epa . gov/ action/ advisories /drinking/ fluoride index, cfm
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Introduction
Foods
and
Dietary Exposure
Drinking Water
Dental Products
Other Exposure
Media
Selection of Critical Studies
RSC Catenation
Exposure Analysis
Exposure and Relative Source Contribution Analysis Document Map
111
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TABLE OF CONTENTS
PREFACE i
LIST OF TABLES vi
LIST OF FIGURES viii
ACKNOWLEDGMENTS ix
LIST OF ACRONYMS x
AUTHORS, CONTRIBUTORS AND REVIEWERS xi
EXECUTIVE SUMMARY xiii
1. INTRODUCTION 1
1.1. Background 1
1.2. U.S. EPA RSC Policies 1
2. EXPOSURE FROM FOODS AND BEVERAGES 4
2.1. Analytical Methods 4
2.1.1. Sample Preparation 4
2.1.2. Fluoride Recovery 5
2.1.3. Measurement and Quantitation of Fluoride Ion 6
2.1.4. Confidence in Analytical Results 8
2.2. Natural Fluoride Levels in Solid Foods 9
2.2.1. Fluoride in Infant Foods 10
2.2.2. Fluoride in Foods of Children and Adults 15
2.2.3. Summary of the Data on Fluoride in Solid Foods 21
2.3. Fluoride in Beverages 23
2.3.1. Non-Alcoholic Beverages 23
2.3.2. Alcoholic Beverages 26
2.3.3. Summary for Fluoride in Beverages 26
2.4. Indirect Exposure from Pesticide Residues on Food 26
2.5. Estimates of Dietary Fluoride Intake 29
2.5.1. Exposure Assessment Methodologies 29
2.5.2. Infants 33
2.5.3. Children to 14 Years of Age 39
2.5.4. Older Children and Adults 46
2.5.5. Combined Exposure Estimates for Age Groups of Concern 52
3. EXPOSURE FROM DRINKING WATER 57
3.1. Analytical Methods 57
3.2. Natural Sources 58
3.4. Fluoridation Contributions 66
3.5. Bottled Water 67
3.6. Exposure from Drinking Water 68
4. FLUORIDE IN DENTAL PRODUCTS 71
4.1. Toothpaste 71
4.2. Topical Applications and Mouth Rinses 78
4.3. Summary of Fluoride Exposure from Dental Products 80
5. OTHER SOURCES OF EXPOSURE 83
5.1. Exposure from Air 83
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5.1.1. Monitoring Data 83
5.1.2. Exposure to Airborne Fluoride 84
5.2. Oral Supplements 84
5.3. Soil Ingestion by Children 86
5.4. Pharmaceuticals 87
5.5. Occupational Exposures 87
5.6. Smoking 87
6. EXPOSURE ASSESSMENT SUMMARY 88
6.1. Dietary Intake 89
6.2. Drinking Water 93
6.3. Toothpaste 94
6.4. Soils 95
6.5. Uncertainty 95
7. RELATIVE SOURCE CONTRIBUTION (RSC) 97
8. RELATIONSHIP OF EXPOSURE ESTIMATES TO DIETARY GUIDELINES 102
8.1. Estimates of Daily Dietary Needs 102
8.2. Estimates of Tolerable Upper Limit Level 103
8.3. Exposure Profiles 104
8.4. Summary of findings 108
9. REFERENCES CITED Ill
APPENDICES 128
Appendix A. Fluoride Chronic Dietary Exposure Analysis
Appendix B. Sulfuryl Fluoride: Estimates of Fluoride Exposure from Pesticidal Sources - Customized
Age Groups
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LIST OF TABLES
Table 2-1. Fluoride Concentrations in Infant Formula (Dabeka and Mckenzie, 1987) 10
.Table 2-2. Mean Fluoride Concentrations (mg/L) in Infant Formulas (McKnight-Hanes et al.,
1988) 11
Table 2-3. Fluoride Concentrations in Infant Formulas (Van Winkle et al., 1995) 12
Table 2-4. Fluoride Levels in Infant Formulas Reconstituted with Deionized Water (Siew et al.,
2009) 12
Table 2-5. Fluoride Concentrations in Infant Foods as Reported by Singer & Ophaug, 1979 13
Table 2-6. Fluoride Concentrations in Infant Foods as Reported by Heilman et al., 1997 14
Table 2-7. Fluoride Concentrations in Infant Foods as Summarized by USDA (2005) 15
Table 2-8. Fluoride Content of Food Commodity Groups 15
Table 2-9. Fluoride Content of Composite Food Groups for Four Geographic Regions of the U.S 16
Table 2-10. Fluoride Content of Four Representative Diets for 2-Year-Olds 17
Table 2-11. Fluoride Concentrations in Food Products 17
Table 2-12. Fluoride Concentrations in Foods Obtained in Winnipeg, Canada 18
Table 2-13. Fluoride Concentrations of Noncooked and Nonreconstituted Foods and Beverages
Consumed by Adolescents 12-14 Years Old" 19
Table 2-14. Fluoride Concentrations (mg/kg) of Drinking Water and Foods and Beverages
Reconstituted in or Cooked in Tapwater 19
Table 2-15. Fluoride Concentrations in Foods as Summarized by the USDA, 2005 20
Table 2-16. Comparison of Food Group Measures over a 30-Year Period 22
Table 2-17. Fluoride Content of Canned Vegetables 23
Table 2-18. Fluoride Concentrations in Beverages in Two Canadian Towns 24
Table 2-19. Fluoride Levels in Beverages as Summarized by the USDA, 2005 25
Table 2-20. Fluoride Concentration in Tea as Served 25
Table 2-21. Estimated Food Group Exposures of the General U.S. Population to Fluoride from
Sulfuryl Fluoride Tolerances 29
Table 2-22. Fluoride Intake of Infants 6 Months Old (Singer and Ophaug, 1979) 34
Table 2-23. Fluoride Intake (mg F/day) by Infants 6 Months Old in Four Regions of the U.S 35
Table 2-24. Estimated Fluoride Intake of 6-Month Old Infants in Different Regions of the U.S 36
Table 2-25. Mean Dietary Fluoride Intake of 6-Month-Old Infants (Ophaug et al., 1985) 36
Table 2-26. Estimated Fluoride Intake of 4-10 Month Old Infants with Varying Intakes of Milk or
Formula 37
Table 2-27. Dietary Fluoride Intake of Infants from the 1960s to the 1990s 37
Table 2-28. Updated Estimated Fluoride Intake of 4-10 Month Old Infants with Varying Intakes of
Milk and Formula (Fomon et al., 2000) 38
Table 2-29. Volume of Formula Consumed and Body Weights from Birth to 12 Months
(Siew et al., 2009) 38
Table 2-30. Fluoride Intake (mg F/day) by Children 2 Years Old in Four Regions of the U.S 39
Table 2-31. Dietary Fluoride Intake of an Average 2-Year-Old Child 40
Table 2-32. Mean Dietary Fluoride Intake of 2-Year-Olds 41
Table 2-33. Estimated Fluoride Intake of 3- to 5-Year-Old Children Living in a Nonfluoridated and
Fluoridated Community 42
Table 2-34. Estimated Fluoride Intake of 6 to 11 and 12 to 19 Year Olds Living in a Nonfluoridated
Community 43
Table 2-35. Estimated Fluoride Intake of 6 to 11 and 12 to 19 Year Old Children Living in a
Fluoridated Community 44
Table 2-36. Dietary Fluoride Intake of 16-40 Month Old Children 45
Table 2-37. Fluoride Content of Four Two-week Representative Diets for Teens 16-19 Years Old 47
Table 2-38. Average Daily Fluoride Intake of 16-19 Year Olds Residing in Four Cities 47
Table 2-39. Daily Fluoride Intake Based on Composite Diets 48
Table 2-40. Average Daily Fluoride Intake (mg/day) of 16-19 Year Olds 49
Table 2-41. Daily Fluoride Intake based on 6-day Hospital Diets 49
Table 2-42. Fluoride Intake of Individuals on a Metabolic Diet over a Six-Year Period 50
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Table 2-43. Fluoride Intake from a General Hospital Diet Prepared with and without Fluoridated
Water 51
Table 2-44. Dietary Fluoride Intake in Sixteen U.S. Cities 52
Table 2-45. Summary of Daily Dietary Fluoride Intakes for Age Groups of Concern 53
Table 2-46. Estimates of Daily Dietary Fluoride from Beverages for Age Groups of Concern 54
Table 2-47. Summary of Pesticidal Fluoride Contributions to Dietary Fluoride Exposure 56
Table 3-1. Public Water System Monitoring Data 1998-2005 64
Table 3-2. A Summary of Public Water System Fluoride Monitoring Data from Systems for
Systems with at Least One Detection of 2 mg/L or Higher during the Year of Monitoring 65
Table 3-3. CDC Recommendations for Optimal Fluoride Concentrations in Public Water Supply
Systems 66
Table 3-4. Estimated Daily Fluid and Plain Water Regional Intake in Children 1-10 Years Old 67
Table 3-5. Fluoride Intake from Consumption of Municipal Water (Direct and Indirect") at the
Average Concentration (0.87 mg/L) Determined from Monitoring Records for 2002
through 2005 68
Table 3-6. Consumers Only Fluoride Intake from Consumption of Municipal Water (Direct and
Indirect") at the Average Concentration (0.87 mg/L) Determined from Monitoring
Records for 2002 through 2005 69
Table 3-7. Fluoride Intake From Average Drinking Water Consumption and 90th Percentile
Fluoride Concentration (1.43 mg/L) Determined from Monitoring Records for 2002
through 2005 70
Table 4-1. Toothpaste Use and Estimated Fluoride Ingestion by Children 2-5 Years Old 73
Table 4-2. Toothpaste Use by Children 6 to 12 Months Old 74
Table 4-3. Age-Related Estimates of Fluoride Ingestion from Toothpaste Use 75
Table 4-4. Toothpaste Use and Fluoride Ingestion in Children Two to Seven Years Old 76
Table 4-5. Estimated Fluoride Intake from Toothpaste" in Children 1.5 to 36 Months Old 77
Table 4-6. Toothpaste Use and Ingestion by Children Ages 16 to 36 Months 77
Table 4-7. Fluoride Ingestion from Toothpaste Use and Fluorosis 78
Table 4-8. Percentage of Children Receiving Fluoride Treatments by Age Groups 79
Table 4-9. Age-Related Exposure Estimates for Fluoride From Toothpaste 80
Table 4-10. Number of Toothbrushings Per Day Reported for Children (Six Months to Five Years
Old) 81
Table 5-1. Daily Fluoride Supplementation Recommended by the ADA and the American Academy of
Pediatric Dentistry 84
Table 5-2. Fluoride Intake from Supplements in Children 1.5 to 36 Months Old 85
Table 6-1. Estimated Daily Dietary Fluoride Intakes from Solid Foods for Age Groups of Concern 90
Table 6-2. Estimated Daily Fluoride Intake from Beverages Only for Age Groups of Concern 92
Table 6-3. Fluoride Intake from Consumption of Municipal Water (Direct and Indirect") at the
Average Concentration (0.87 mg/L) Determined from Monitoring Records for 2002
through 2005 94
Table 6-4. Age-Related Exposure Estimates for Fluoride From Toothpaste 94
Table 6-5. Sulfuryl Fluoride Contributions to Dietary Fluoride Exposure 96
Table 7-1. Representative Values for Fluoride Intakes Used in Calculation of the Relative Source
Contribution for Drinking Water 98
Table 7-2. Representative Values for Fluoride Intakes (Including Sulfuryl Fluoride) Used in
Calculation of the Relative Source Contribution from Drinking Water 98
Table 8-1. Comparison of Total Fluoride Intake Estimates to the Dietary Adequate Intake (AI) 103
Table 8-2. Comparison of Total Fluoride Intake Estimates to the IOM (1997) Tolerable Upper
Intake Level and the OW Age-Specific Benchmarks 104
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LIST OF FIGURES
Figure 3-1. Fluoride Levels in Groundwater in the U.S. (Fleischer et al., 1974) 59
Figure 3-2. Arid Regions in the U.S. (McGinnies et al., 1968) 59
.Figure 7-1. Percentage Media Contribution to Total Daily Fluoride Intake: 90th Percentile Drinking
Water Intakes for Consumers Only and a Fluoride Concentration of 0.87 mg/L 99
Figure 8-1. Total Daily Fluoride Intake Estimates Relative to the Proposed RfD Using 90th
Percentile Drinking Water Intake Data for Consumers Only and the Mean Drinking
Water Fluoride Concentration (0.87 mg/L) 105
Figure 8-2. Total Daily Fluoride Intake Estimates Relative to the Proposed RfD Using the Mean
Drinking Water Intake Data for Consumers Only and the Mean Drinking Water
Fluoride Concentration (0.87 mg/L) 106
Figure 8-3. Total Daily Fluoride Intake Estimates Relative to the Proposed RfD using Mean
Drinking Water Intakes for Consumers Only and the 90th percentile Fluoride
Concentration for all Systems Reporting Detections of Fluoride 107
Figure 8-4. Total Daily Fluoride Intake Estimates Relative to the Proposed RfD using 90th Percentile
Drinking Water Intakes for Consumers Only and Average Concentration (1.76 mg/L)
for those Systems that Reached or Exceeded the SMCL of 2 mg/L at Least Once During
the ICR Monitoring Period for the Second Six-year Review 107
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ACKNOWLEDGMENTS
This document was prepared by staff of Oak Ridge National Laboratory, Oak Ridge, Tennessee,
under work assignment 2006-014, under the U.S. EPA IAGNumber DW-89-9220971. The
Lead EPA Scientists are Joyce M. Donohue, Ph.D., and Tina Duke, M.P.H, Health and
Ecological Criteria Division, Office of Science and Technology, Office of Water, U.S.
Environmental Protection Agency, Washington, DC.
The Oak Ridge National Laboratory is managed and operated by UT-Battelle, LLC., for the U.S.
Department of Energy under Contract No. DE-AC05-OOOR22725.
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LIST OF ACRONYMS
ADA American Dental Association
ANOVA Analysis of Variance
ATSDR Agency for Toxic Substances and Disease Registry
AWQC Ambient Water Quality Criteria
BW Body weight
CAMP Continuous Air Monitoring Project
CDC Centers for Disease Control
CI Confidence Interval
CSFII Continuing Survey of Food Intake by Individuals
CTE Central Tendency Exposure
DI Drinking water intake
F Fluoride
FDA Food and Drug Administration
GI Gastrointestinal
HMDS Hexamethyldisiloxane
IOM Institute of Medicine (of The National Academies)
ISE Ion-selective electrode
MCL Maximum contaminant level
MCLG Maximum contaminant level goal
NDL Nutrient Data Laboratory (U.S. Department of Agriculture)
NF Non-fluoridated
NFCS Nationwide Food Consumption Survey
NHANES National Health and Nutrition Examination Survey
NIDR National Institute of Dental Research
NIPDWR National Interim Primary Drinking Water Regulations
nmole Nanomole
NRC National Research Council (of The National Academies)
OR Odds ratio
OPF Optimal fluoride level
OSHA Occupational Safety and Health Administration
RDA Recommended Daily Allowance
RfD Reference dose (in mg/kg/day)
RMCL Recommended Maximum Contaminant Level
RME Reasonable Maximum Exposure
RSC Relative Source Contribution
SD Standard Deviation
SE Standard Error
SEM Standard Error of the Mean
SDWA Safe Drinking Water Act
SMCL Secondary Maximum Contaminant Level
USDA U.S. Department of Agriculture
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AUTHORS, CONTRIBUTORS AND REVIEWERS
Joyce Morrissey Donohue, Ph.D., R.D.
Health and Ecological Criteria Division
Office of Water
U.S. Environmental Protection Agency
Tina Duke, M.P.H.
Health and Ecological Criteria Division
Office of Water
U.S. Environmental Protection Agency
Dennis Opresko, Ph.D.
Toxicology and Hazard Assessment
Oak Ridge National Laboratory
Oak Ridge, TN
Annetta Watson, Ph.D.
Toxicology and Hazard Assessment
Oak Ridge National Laboratory
Oak Ridge, TN
Bruce Tomkins, Ph.D.
Chemical Sciences Division
Oak Ridge National Laboratory
Oak Ridge, TN
INTERNAL EPA REVIEWERS
Brenda Foos, MS
Office of Children's Health Protection
U.S. Environmental Protection Agency
Denis Borum, MS
Office of Congressional and Intergovernmental Relations
U.S. Environmental Protection Agency
Lisa Melnyk, Ph.D.
National Exposure Research Laboratory
Office of Research and Development
U.S. Environmental Protection Agency
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EXTERNAL PEER REVIEWERS
Linda C. Abbott, Ph.D.
Regulatory Risk Analyst
Office of Risk Assessment and Cost-Benefit Analysis
U.S. Department of Agriculture
Mary A. Fox, Ph.D.
Assistant Professor
Department of Health Policy and Management
Johns Hopkins Bloomberg School of Public Health
E. Angeles Martinez Mier, DOS, MSD, Ph.D.
Associate Professor
Department of Preventive and Community Dentistry
Indiana University School of Dentistry
David L. Ozsvath, Ph.D.
Professor of Geology and Water Science
Department of Geography/Geology
University of Wisconsin-Stevens Point
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EXECUTIVE SUMMARY
In response to the 2006 National Research Council (NRC) report: Fluoride in Drinking Water: A
Scientific Review of EPA 's Standards, the U.S. EPA Office of Water (OW) initiated an
examination of dose-response data for critical noncancer effects of fluoride on teeth and bone in
light of the NRC (2006) conclusion that "the EPA's MCLG of 4 mg/L should be lowered," so as
to reduce the risk of severe enamel fluorosis and to minimize the risk for bone fractures and
skeletal fluorosis in adults. Dose-response assessment for fluoride was updated using current
approaches for quantifying risk with consideration given to susceptible populations as well as
uncertainties and variability in the data (U.S. EPA, 2010a).
One goal of the exposure and relative source contribution (RSC) analyses was to obtain and
evaluate available U.S. domestic exposure data that could be used by the Office of Water during
its reconsideration of the current USEPA Maximum Contaminant Level Goal (MCLG;
nonenforceable) for fluoride. This assessment examined data on the concentrations of fluoride in
foods and beverages, available dietary exposure estimates for fluoride, concentrations of fluoride
in the tap water delivered by public drinking water systems, incidental ingestion of fluoride from
toothpaste use and potential exposures to fluoride from sulfuryl fluoride (pesticide) applications.
The information utilized was largely drawn from peer-reviewed published literature that
examined the exposure of US domestic or in some cases Canadian populations and communities.
Once information on the various media contributing to fluoride exposure were assembled and
analyzed, total exposures for the period of sensitivity to severe dental fluorosis (six months to 14
years) were estimated. An exposure estimate was also developed for the adult population. The
RSC determination followed the methodology established by the OW for chemicals found in
drinking water which use average exposures for all media except residential drinking water from
public drinking water systems. The drinking water component of the relative source analysis is
based on the average fluoride concentration (-0.9 mg/L) from public drinking water systems that
reported detectable levels of fluoride during the second six-year review of U.S. EPA drinking
water regulations and the intake data (direct and indirect) for the 90th percentile consumer from
the U.S. Department of Agriculture (USD A) Continuing Survey of Food Intake by Individual
(CSFII). The analysis considers susceptible populations, and the impact of the uncertainties and
variability in the data as part of the RSC analysis.
Among the age groups evaluated, the RSC values for drinking water range from 40 to 70 percent,
with the higher values associated with infants fed with powdered formula or concentrate
reconstituted with residential tap water (70%) and adults (60%). Comparison of the age-specific
total estimated exposure for the 90th percentile drinking water consumer to the daily reference
dose suggests that some children at ages less than seven years old may be at risk for severe
dental fluorosis. The major contributors to total daily fluoride intakes for these age groups are
their drinking water, commercial beverages, solid foods and swallowed toothpaste.
In addition to the exposure information, this report presents background information on the
strengths and weaknesses of the analytical methods that were used to measure fluoride in various
media for the key critical studies and the approaches applied in developing dietary exposure
assessments.
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1. Introduction
1.1. Background
In 2006, the National Research Council (NRC) released: Fluoride in Drinking Water: A
Scientific Review of EPA 's Standards, a three year effort to examine the health effects of
ingested fluoride in drinking water. The development of the NRC (2006) report was funded by
the U. S. EPA Office of Water (OW). The project was initiated as a result of the 2002/2003
review of the Maximum Contaminant Level Goal (MCLG) and the Maximum Contaminant
Level (MCL) for fluoride.
NRC (2006) concluded that EPA's current MCLG of 4 mg/L for fluoride should be lowered to
reduce the risk of severe enamel fluorosis and minimize the risk for bone fractures and skeletal
fluorosis in adults. In response, the U.S. EPA OW initiated an examination of the dose-response
data for the critical noncancer effects of fluoride on teeth and bone. The dose-response
assessment for fluoride was updated using current approaches for quantifying risk with
consideration given to susceptible populations and the uncertainties and variability in the data
(U.S. EPA, 2010a).
The U.S. EPA (2010a) report identifies the fluoride concentration in drinking water that was not
associated with an increased risk of severe dental fluorosis in 99.5% of children in selected
towns distributed across the United States (Dean (1942) prior to the introduction of fluoridation
and fluoridated dental products. The U.S. EPA (2010a) report includes an estimated Reference
Dose (RfD) for severe dental fluorosis derived from the Dean (1942) data. It also determined
that the RfD associated with severe dental fluorosis is similar to or lower than that associated
with an increased risk of bone fracture or Stage III skeletal fluorosis.
At the time the dose-response data were collected the fluoride in drinking water was largely
determined by local geological composition of the soils and bedrock; there was no intentional
fluoridation of public drinking water supplies and no commercial fluoride-containing dental
products. Currently, exposures to fluoride come from drinking water, foods, beverages, dental
products (toothpaste, mouth rinses), supplements, industrial emissions, pharmaceuticals, and
pesticides. In the case of young children, ingestion of fluoride-containing soil is another source
of exposure. These exposure pathways are discussed in this report and quantified where possible.
The data presented include some of the studies that were considered by the NRC (2006) report in
their analysis of relative source exposures as well as additional published papers identified by the
OW.
The ratio between exposure from drinking water and total exposure is called the relative source
contribution (RSC). The OW traditionally uses the RSC in the derivation of noncancer MCLGs
for a drinking water regulation. Section 1.2 below describes OW RSC policies.
1.2. U.S. EPA RSC Policies
The OW RSC policies have evolved gradually over the more than twenty years since fluoride
was regulated. The derivation of the fluoride MCLG did not include an RSC, in part because the
data supporting the critical effect of crippling skeletal fluorosis in adults were derived primarily
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from the ingestion of fluoride from drinking water. The diet was assumed to have a minimal
contribution to total intake and was not reported in the critical studies. The MCLG was derived
from an estimated 20 mg/day chronic fluoride intake divided by a drinking water intake of 2
L/day and a 2.5 safety factor yielding an MCLG of 4 mg/L. This same approach was used in
determining the MCLG values for a few other contaminants (i.e. nitrate, copper, barium) because
the exposure and toxicology data applied to drinking water and did not include background
intakes from other sources.
Currently calculation of the MCLG for noncancer endpoints, in almost all cases, utilizes the
Reference Dose (RfD) as the point of departure. The reference dose is defined as: "an estimate
(with uncertainty spanning perhaps an order of magnitude) of a daily oral exposure to the human
population (including sensitive subgroups) that is likely to be without an appreciable risk of
deleterious effects during a lifetime" (U.S. EPA,
..http://www.epa.gov/ncea/iris/helpques.htmtfrfd).
The MCLG is usually derived from the RfD using the following equation.
MCLG = RfD x BW x RSC
DI
where:
BW = Average body weight (70 kg for an adult)
DI = 90th percentile drinking water
RSC = Relative Source Contribution
DI = 90th percentile drinking water intake (2 L/day for an adult)
Prior to the 1998 Stage I Disinfectants and Disinfection Byproducts rule [Fed. Reg.
63(241):69389-69476], a 20% default RSC was applied for the majority of MCLGs for
noncancer effects. The few exceptions to this practice were those cases where published data
were used to support an alternate RSC. A shift away from automatically defaulting to 20% was
an outgrowth of the 2000 publication of the Ambient Water Quality Criteria (AWQC) for Human
Health which included a peer reviewed decision tree approach for determining the RSC (EPA,
2000b). The human health AWQC applies to the intake of a contaminant from both drinking
water and fish/shellfish from ambient surface waters of interest. It is easily adapted for use with
drinking water alone scenarios. It was used for determining the RSC values for chloroform,
monochloroacetic acid, and trichloroacetic acid in the 2003 Stage II Disinfection By-product
Rule [Fed. Reg. 71(2):387-493]. The MCLGs for all three compounds are based on the RfD
rather than a cancer endpoint. The MCLG for all carcinogens is currently zero and does not
require an RSC.
Key features of the Human Health AWQC Decision Tree as applied to drinking water can be
summarized as follows:
The RSC value used is determined by the type and amount of data available. The data
should be representative of the population of concern (adults, child, pregnant
woman, etc).
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The RSC is based on national exposure estimates that, at a minimum, provide average
values and associated confidence bounds. Knowledge of the properties of the chemical
and more limited exposure data can be used when nationally representative data are not
fully available.
All known exposure routes and media are considered.
The lowest RSC is 20% based on the assumption that regulatory or guideline values for
chemicals with exposures that are less than 20% of the total will not provide a
meaningful opportunity to reduce risk for the population. In these cases the greatest
health benefit can be achieved by establishing guidance or regulations for the medium
that contributes the major portion of the total exposure.
The highest allowable RSC is 80% based on the assumption that there may be many
minor sources of exposure that will not be captured by the available data.
Subtraction and percentage options are available but are bounded by the 20% floor and
80% ceiling. There are policy limitations on the use of the subtraction approach. It can be
applied only under circumstances where the MCLG is the sole health-based U.S. EPA
criterion for the contaminant. For example, the subtraction approach is not possible for
fluoride because pesticides containing fluoride have established tolerances for food crops.
Average exposure values are used to represent the contribution from the diet, ambient air,
soil ingestion, and other exposure media.
The drinking water intake contribution to total exposure is represented by the 90th
percentile value and the average analyte drinking water concentration because drinking
water is the exposure route of concern for the OW.
The body weight is an average for the population of interest (e.g. adults, infants, and
children).
Exposures to drinking water contaminants that occur during showering, bathing, laundry,
etc. are not included as part of drinking water ingestion intake. They are included in the
other sources of exposure.
In determining the RSC as a percentage, the estimated daily analyte intake from a 90th
percentile tap water consumption estimate at the average analyte concentration from
public water systems is divided by the total uptake into the body from all quantified
exposure routes.
The OW is in the process of considering refinements to the 2000 decision tree methodology for
ambient water and drinking water. However, those modifications were not available for the
fluoride exposure assessment. Accordingly, the RSC for fluoride has been developed using
human health AWQC methodology framework.
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2. Exposure from Foods and Beverages
In the 30-year period covered by the data in this report, there have been changes in analytical
methods and instrumentation that have led to improvements in the accuracy and precision of
measurements of fluoride in food and beverages. The early studies usually relied on colorimetric
techniques for the measurement of fluoride; such techniques were subject to interference from
other elements in the food matrix. Most later studies employed a fluoride ion-specific electrode
in the measurement of fluoride. Some changes in the measured levels of fluoride in foods and
beverages over the years covered in this report and in EPA (2010a) appear to be a consequence
of differences in the analytical methodologies used to measure fluoride as well as changes in
food consumption patterns. Section 2.1 below provides background historic information on
analytical methods used to measure fluoride in food. The methodological impacts on
measurements of fluoride concentrations in foods are discussed in Sections 2.1, 2.2.3 and 2.3.3.
2.1. Analytical Methods
Procedures for the determination of fluoride in foods typically exhibit three distinct phases:
digestion, isolation and quantification. In the digestion phase, samples are ashed in the presence
of a caustic agent such as concentrated calcium or sodium hydroxide. The caustic agent not only
serves to help digest the organic sample, but also acts as a trapping agent for fluoride ion.
Several methods can be used in the isolation phase. In one method, the ashed residue is
dissolved in concentrated acid. Fluoride ion is converted to volatile hydrofluoric or
hydrofluosilicic acid, distilled from the residues, and collected in a clean aqueous distillate.
Successful isolation of fluoride ion from the ashed residues has also been accomplished by
merely allowing the analyte to diffuse through a membrane into a strongly basic trapping
medium. Hexamethyldisiloxane accelerates this process significantly. Once the fluoride is
isolated, several approaches can be employed in the quantification phase, including (a) titration
with colorimetric reagents; (b) reaction with a colored reagent followed by spectrophotometric
measurement; (c) measurement using a fluoride ion-selective electrode, and (d) gas
chromatography. Further details about each of these basic steps are provided below.
2.1.1. Sample Preparation
Food samples are primarily composed of bulk organic matter which is largely insoluble in water,
with small concentrations of inorganic species of interest. The bulk organic matrix must be
removed while inorganic analytes such as fluoride are retained. In many cases, some form of
"trapping" medium is required to ensure that fluoride is not lost during the digestion process.
Mineralization by ashing of the food sample is used to remove the organic matrix. The process
was initially described in AOAC (1945), and has been virtually unchanged in more than fifty
years (AOACI, 2000). Modest quantities of dry material, liquid samples, and undried food
products or plant material are selected for analysis, depending upon the expected fluoride content
and interferences. The sample is mixed with a calcium hydroxide (lime) suspension or sodium
hydroxide, dried and ashed in a muffle furnace at 600° C. Variations of the official methods can
employ smaller samples, different trapping agents, or both (Malde et. al., 2001; Venkateswarlu,
1975; Singer and Ophaug, 1979).
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Venkateswarlu (1975) compared "closed ashing", employing a standard oxygen bomb technique,
with the "open ashing" employing a muffle furnace, described above. Both procedures are
applicable to solid samples, soft tissue, and liquid samples that are low in organic matter. In all
cases, the "closed ashing" approach required that samples be pressed into pellets containing up to
1 g of solid. Blank values were typically < 0.05 jig fluoride. The recoveries of fluoride from
bovine albumin and serum at concentrations of 0.28 and 0.05 jig fluoride per gram sample
exceeded 95%. A comparison between results obtained from "closed" vs. "open" ashing for
bovine and human sera samples suggested that the values obtained by the open ashing process
are frequently lower than those obtained with closed ashing in an oxygen-enriched chamber.
Several authors have described procedures for quantifying fluoride in food matter that do not
involve ashing; these changes are a reflection of improvements in analytical instrumentation.
Pesselman et al. (1989) described an alternative preparation for soluble samples such as cocoa
powder that did not involve ashing. Small samples were mixed with doubly-deionized water and
blended using a simple Waring blender. The product was then centrifuged and vacuum filtered.
Nedeljkovic et al. (1991) homogenized food samples and transferred the resulting slurry to a
"microdiffusion" cell, described below, containing sodium hydroxide solution as the trapping
medium. Both methods employed a fluoride ion selective electrode, described below, for final
measurement of fluoride concentration in solution.
2.1.2. Fluoride Recovery
Distillation. In the classical approach for isolating fluoride from interfering elements in the
mineralized ash, fluoride is converted to hydrofluosilicic acid by adding perchloric or sulfuric
acid to water (the former is preferable, since nearly all of the perchlorates are very soluble). This
method was described by Willard and Winter (1933) almost seventy-five years ago. Several
pieces of glass are added to the sample in a distillation flask, and distilled. When only a small
quantity of fluorine (10 mg or less) is present in the sample and the temperature is not allowed to
rise above approximately 125 °C, the pieces of glass appear to supply the silica necessary to
combine with the fluorine to form hydrofluosilicic acid, and there is no noticeable etching of the
flask. The authors presented data showing that 7-10 mg of fluoride (as sodium fluoride) could be
recovered with >95% efficiency from a variety of matrices, such as plant ash, gelatinous silica,
boric acid, and aluminum chloride. A similar approach is presented in APHA/AWWA/WEF
(2005) as "Method 4500 F. B. Preliminary Distillation Step."
Microdiffusion and Trapping of Fluoride. Many investigators have reported concerns with the
standard method, including losses of a volatile fluoride species through the ground glass joints,
the possibility of a perchlorate explosion, the obvious skill needed to make the distillation work
properly, and the time and effort required for a proper isolation. For these reasons, investigators
have tried to develop simpler and faster isolation methods with analyte recovery comparable to
that of the standard method. Most of these involve the diffusion of hydrogen fluoride through
modified polypropylene "Conway cells" (Obrink, 1955; Conway, 1950), a specific
microdiffusion cell design.
The "Conway cell" operates in the following manner: According to Singer and Armstrong
(1965), a strongly-basic "trapping solution" for HF, e.g., 2.5 N sodium hydroxide is placed into
the center well ("inner chamber") of the diffusion cell. The sample containing fluoride is
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acidified strongly with perchloric acid and placed into the sample compartment ("outer
chamber"). The cell is then sealed using a small Petri dish, heated to 55-60 °C, and left
undisturbed for 22 hours. Hydrogen fluoride diffuses from the sample compartment into the
headspace of the sealed cell, and is collected in the trapping solution contained in the inner
chamber. The authors demonstrated that the recovery of 0.1 -2 jig fluoride from samples of rat
liver, beef liver, and beef muscle, by use of this diffusion procedure was virtually identical to
that obtained using the Willard and Winter (1933) distillation procedure. This new method was
considered a reasonable substitute for the traditional distillation procedure because both
approaches produced the same results at or below the microgram level for fluoride. Additional
experiments with 0.5 or 1 jig of F18, a radioactive tracer, confirmed that the recoveries of fluoride
typically exceeded 95% from human plasma, saliva, and urine when using the microdiffusion
cell to isolate the analyte.
Taves (1968a) found that the diffusion of fluoride increased if silicone grease was used to seal
the Conway cells. In follow-up work, the author used 6 M hydrochloric acid saturated with 0.5
mL hexamethyldisiloxane (HMDS) in the "outer chamber" of the Conway cell, and examined the
rate of fluoride diffusion into a variety of trapping agents with and without HMDS present
(Taves, 1968b). All recovery measurements were performed using the radioactive tracer F18.
Without the HMDS present, there was practically no diffusion of fluoride. When the HMDS-
saturated hydrochloric acid was present, but not in contact with sample, one-third of the fluoride
diffused to the trapping solution in 10 minutes, owing to the volatilization of the HMDS. Mixing
the solutions increased the rate of diffusion appreciably and continuous rotary motion resulted in
over 80% recovery of the radioactive tracer in only 10 minutes, a very rapid process. In one hour
at room temperature, >97% tracer recovery was attained by this method (Taves, 1968b). HMDS
is presumed to accelerate the diffusion of fluoride by formation of trimethylfluorosilane.
2.1.3. Measurement and Quantitation of Fluoride Ion
Ion-selective electrode (ISE). The fluoride ion-selective electrode (ISE) was introduced in the
mid-1960s (Buck and Lindner, 2001), and quickly became the industry-wide standard for the
accurate determination of fluoride concentrations. When this electrode is compared to later
spectrophotometric methods, such as that employing the SPADNS [sodium 2-
(parasulfophenylazo)-l, 8-dihydroxy-3, 6-naphthalene disulfonate] reagent, the former exhibits
superior selectivity when challenged with chloride, chlorine, color and turbidity, iron, phosphate,
sulfate, and aluminum (APHA/AWWA/WEF, 2005).
The key element in the fluoride electrode is the laser-type doped lanthanuim fluoride crystal
across which a potential is established by fluoride solutions of different concentrations. The
crystal contacts the same solution at one face and an internal reference solution at the other.
Strictly speaking, the fluoride electrode measures the ion activity of fluoride in solution rather
than concentration. Fluoride ion activity depends on the solution total ionic strength and pH, and
on fluoride complexing species. For that reason, adding an appropriate buffer provides a nearly
uniform ionic strength background, adjusts pH, and breaks up complexes so that, in effect, the
electrode measures concentration (APHA/AWWA/WEF, 2005; Omega, 1993). The literature
documents successful use of the fluoride ISE in quantifying this analyte in many different foods
and materials.
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Singer and Ophaug (1979) presented a side-by-side comparison of fluoride concentration results
obtained using both a colorimetric and fluoride ISE approach. The results were entirely
comparable for strained meats (chicken and beef with respective broths), milk-based infant
formula, and vegetables (green beans, peas, and spinach) at concentrations ranging between 0.1-
6 mg F/kg sample. When fruits (pears, applesauce, peaches, etc.) were analyzed, substantially
(-20 times) higher levels were observed with the colorimetric method. It thus appears that
reagents employing eriochromecyanin R (see "Spectrophotometric determination", below) to
determine fluoride in the diffusates of unashed foods may result in erroneously high values.
Spectrophotometric Determination. The introduction of the Beckman Model DU
spectrophotometer, an instrument which could measure absorbance in both the ultra-violet and
visible ranges, in 1941 (Simoni et. al., 2003) rendered the classic titration-methods for
quantifying fluoride ion obsolete. Spectrophotometric procedures frequently employed a
zirconium-alizarin or eriochromecyanin R (syn. Eriochrome Cyanine R) lake dye, whose
absorbance fades with increasing fluoride ion concentration (Singer and Armstrong, 1959;
Megregarian and Maier, 1952) over the range of 0-4 ppm. This method was highly dependent
upon the presence of phosphate and iron, but relatively insensitive to bicarbonate, chloride, and
sulfate. Grutsch et al. (1953) demonstrated that the interferences from iron, manganese, and
chlorine could be eliminated by adding thioglycolic acid to the aqueous samples.
The above approach is still one of those accepted for the determination of fluoride ion, albeit in a
modified form (APHA/AWWA/WEF, 2005). The SPADNS colorimetric method (Bellack and
Schouboe, 1968) is based on the reaction between fluoride and a zirconium-dye lake. Fluoride
reacts with the dye lake, dissociating a portion of it into a colorless complex anion, (ZrF6)2". As
the amount of fluoride increases and reacts with the dye, the color produced becomes
progressively lighter; absorbance is measured at 570 nm.
Taves (1968c) described a related approach, in which the concentration of fluoride ion was
related to the fluorescence quenching of a Morin (pentahydroxyflavone aluminum complex)-
thorium complex, rather than the change in absorbance described above. The standard
quenching curve was linear between 0-10 nmoles of fluoride ion, after which significant
deviations from linearity were observed. The Morin-thorium reagent was also more sensitive to
the fluoride than to the sulfate and phosphate ions by factors of twenty and forty, respectively.
Nitrate has no immediate effect, but has a marked effect within 18 hours. When the same
amount of acid is used, the effect of chloride, perchlorate, and nitrate is only 1/80,000 that of
fluoride.
The method described in Elvove (1933) uses "Nessler" color comparison tubes and the human
eye as the detector. Known quantities of fluoride, typically ranging between 0 and 55 |ig/mL,
were mixed with a fixed quantity of zierconium-alizarin reagent, permitted to stand undisturbed,
and then compared with the color of unknowns prepared in the same fashion.
Titration. The classical titration of fluoride ion is based upon a two-step process. Initially,
fluoride ion (colorless) reacts with a zirconium-alizarin lake dye (red) to form a zirconium-
fluoride complex (colorless) and free alizarin (yellow) (Grutsch et. al., 1953). The resulting
solution is then back-titrated with a standardized solution of thorium nitrate, which decomposes
the zirconium-fluoride complex and permits the zirconium-lake complex (red) to reform. The
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endpoint of the titration is the faint permanent reappearance of the lake color. (Willard and
Winter, 1933). Willard and Winter (1933) employed this procedure for quantifying fluoride
accurately at the milligram level. This procedure was modified to employ "Nessler tubes" for
color comparison in the Official Methods of Analysis (AOAC, 1945; AOACI, 2000), and has not
been changed in more than fifty years.
The procedures discussed above all employed distillation of volatile hydrogen fluoride prior to
titration. Singer and Armstrong (1965) described a titration of fluoride collected in the "trapping
solution" of a "Conway cell", described above, using hydrochloric acid as the titrant to a simple
phenolphthalein endpoint. The authors do mention a Beckman model B spectrophotometer in
the method, but it is not clear how this instrument was used.
Gas Chromatography. In this procedure, as described by Fresen et al. (1968), an alkyl or
arylchlorsilane (e.g., trimethylchlorsilane) is converted by water into the corresponding silanol
which then reacts selectively with fluoride to form fluorsilane. The fluorsilane is extracted from
an acidified (1 M HC1) sample with an organic solvent such as benzene. The amount of fluoride
still present in the aqueous layer after extraction is negligible. The fluorsilane is injected into a
gas chromatograph using an internal standard such as isopentane. The relative peak height
(corrected with a blank value) is linearly proportional to the fluoride content in the sample. A
solution of 0.6 mg trimethylchlorsilane per mL benzene is sufficient to determine amounts of
fluoride from 0.01 to 10 jig.
2.1.4. Confidence in Analytical Results
Analytical procedures for the determination of fluoride in foods and drinking water samples have
been studied, evaluated, and improved since the 1930's. During all of that time, questions and
concerns raised by analytical chemists have remained the same, viz., (a) accuracy, (b) precision,
(c) detection limit, (d) calibration range, (e) low blank, and (f) interferences. It is certainly true
that current methods employing the fluoride ion-selective electrode, for example, are easier to
use, exhibit a lower blank, and are more selective than predecessor methods. However, from the
onset, it is evident that investigators were keenly aware of technology limitations, and made
strenuous attempts to correct or account for potential interferences. Investigators tried to
simplify or eliminate the traditional "open ashing" procedure, which reduces the mass and
volume of the sample matrix and the ensuing distillation procedure for further isolating fluoride.
The method used to detect fluoride can often be predicted based upon the date of the research.
Prior to approximately 1950, the only method available was based upon titrations employing a
zirconium-alizarin reagent first, followed by back-titration with thorium nitrate. Between
approximately 1950 and 1965, the preferred method was spectrophotometry using the zirconium-
alizarin reagent alone. Work reported after 1965 almost always employs the fluoride ion-
selective electrode.
The results obtained using the earlier titration, spectrophotometric or colorimetric procedures
exhibited sufficient precision and accuracy to support a reasonable estimate for the concentration
of fluoride in environmental media. For example, McClure (1939) employed a titration-based
method to evaluate the fluoride content in a very wide variety of foods. With the exception of
items grown in a fluoride-containing area or sprayed with a fluoride-containing pesticide,
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McClure (1939) reported typical concentrations below 10 ppm, and frequently below 1 ppm,
however levels of detection appear to have been better with some food matrices than others.
Forty years later, Singer and Ophaug (1979) employed an ion-selective electrode-based method
and reported very similar results for a smaller variety of foodstuffs. Taken together, the newer
methods may be easier to perform, are faster, more selective, and more sensitive than their earlier
counterparts. In some cases the results from the older methods are comparable to those from the
newer ones but that is not always the situation. A number of interferences and methodological
variables can result in reported concentrations in foods being lower or higher than the actual
concentration.
The most current methods of analysis for fluoride adopted by the Association of Official
Analytical Chemists International (AOACI) include ion chromatography for inorganic fluoride in
water; the ion selective electrode for fluoride in wine and other beverages, and the distillation
method for fluorine in food (see: ..http://www.eoma.aoac.org/methods.).
2.2. Natural Fluoride Levels in Solid Foods
Several studies suggest that natural fluoride in foods may not be as bioavailable as that from
inorganic fluoride compounds. IOM (1997) notes that when a soluble inorganic fluoride
compound such as sodium fluoride is ingested with milk, baby formula, or foods with high
concentrations of calcium, or certain other divalent or trivalent ions that form insoluble
compounds, absorption may be reduced by 10 to 25%. Trautner and Siebert (1986) investigated
the bioavailability in food products rich in natural fluoride (bone meal, fish bone meal, seaweed
flour, canned sardines, chicken bone meal, tea, krill). Fluoride concentrations in plasma and
saliva over 8 hr, as well as 24 hr urinary fluoride excretions, were determined in healthy adult
volunteers receiving single oral doses containing between 2 and 10 mg F. Comparisons were
made with sodium fluoride (administered as 2, 5, 7.5 and 10 mg doses in NaF solution, or 2, 5
and 8 mg doses as NaF tablets) which was assumed to be 100% bioavailable as reported by
Ekstrand et al. (1978). Plasma, saliva, and urinary fluoride levels were determined with a
fluoride ion-specific electrode. Fluoride in food items was determined by gas chromatography
after extraction with HC1. Bioavailability (B) of fluoride from different substances (sub) was
calculated from the plasma data as:
B% = AAUCSUb x DNaF x 100
AAUCNaF x Dsub
where: D = the quantity of the substance administered or present in the NaF reference sample,
and AAUC is the net area under the fluoride plasma concentration curve minus the background
fluoride levels in the control samples. The same procedure was used to calculate bioavailability
from values of urinary fluoride:
Bo/o = AUsub x DNaF x IQO
X Dsub
where: AU is the net amount of fluoride excreted in the urine during 24 hr.
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The tested foods and beverages varied widely in their bioavailabilities. Relative to sodium
fluoride, bones of mammals, chicken, and fish, whole fish, were poor sources of fluoride
(bioavailability less than one-fourth that of sodium fluoride). In contrast, tea had a
bioavailability close to that of sodium fluoride.
Spak et al. (1982) evaluated the bioavailability of fluoride added to baby formula and milk.
Three different 500 mL solutions (water, milk or formula) containing 10 ppm F (from sodium
fluoride) were administered to volunteers aged 23-25 yr. Fluoride levels in plasma and urine
were determined with a modified microdiffusion technique (Taves, 1968b). The results indicated
that 72% of the fluoride in milk and 65% in the baby formula were absorbed.
2.2.1. Fluoride in Infant Foods
Breast Milk. Concentrations of fluoride in human breast milk are very low. Dabeka et al.
(1986) analyzed 210 samples of breast milk from Canadian women and found detectable
concentrations in 92 (44%). Fluoride concentrations ranged from <0.002 to 0.097 mg/L. The
mean concentration in milk from mothers in fluoridated communities (1 mg F/L water) was
0.0098 mg/L; in nonfluoridated communities the mean was 0.0044 mg/L. Fluoride
concentrations in breast milk were directly related to the fluoride concentration in the mother's
drinking water (p = 0.007). The IOM (1997) reported that concentrations in human milk ranged
from 0.007 to 0.011 mg/L based on data from Ekstrand et al. (1984), Esala et al. (1982) and Spak
etal. (1982).
Infant Formula. Infant formula varies in fluoride content, depending on the type of formula
and the water with which it is prepared.
Dabeka and McKenzie (1987) analyzed fluoride levels in about 115 samples of infant formulas.
Fluoride content was determined by micro-diffusion and a fluoride ion-specific electrode.
Results are shown in Table 2-1.
Table 2-1. Fluoride Concentrations in Infant Formula (Dabeka and Mckenzie, 1987)
Category
Ready to use formula, all:
Ready to use formula, Canadian
Ready to use formula, US
Ready to use formula, glass; all:
Canadian
US
Ready to use formula, canned; all:
Canadian
US
Cone, liquid formula
Powdered infant formula
Milk, evaporated
Number of
No. Samples
41
34
7
23
20
3
18
14
4
33
18
9
Fluoride Concentration (mg/kg food)
Mean
0.79
0.90
0.23
0.75
0.82
0.28
0.84
1.02
0.19
0.60
1.13
0.23
Range
0.15-2.31
0.35-2.31
0.15-0.28
0.28-1.13
0.46-1.13
0.28-0.28
0.15-2.31
0.35-2.31
0.15-0.26
0.15-1.47
0.14-5.53
0.06-0.55
Mean fluoride levels ranged from 0.23 mg/kg for evaporated milk to 1.13 mg/kg for powdered
formula concentrate. Dabeka and McKenzie (1987) note that a major source of fluoride in infant
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formula appeared to be the processing water used by the manufacturer. The concentrations of
fluoride in the U.S. products appear to be lower than those in the Canadian products.
Johnson and Bawden (1987) analyzed fluoride levels in infant formulas obtained from local
supermarkets in 7 cities across the U.S. (Minneapolis, Los Angeles, New York, Dallas, Seattle,
Largo, Florida, and Chapel Hill, North Carolina). Between 7 and 24 products were collected in
each location. Concentrated and powdered formulas were reconstituted with de-ionized water
according to manufacturers' directions. Those from Chapel Hill were also reconstituted with
fluoridated tapwater (1.1 mg F/L). Fluoride was analyzed using the Taves microdiffusion
method and a fluoride ion-specific electrode. The mean fluoride concentration in ready-to-feed
formulas ranged from 0.06 to 0.38 mg/L. Mean fluoride levels in liquid concentrates
reconstituted with de-ionized water ranged from 0.04 to 0.32 mg/L, whereas the Chapel Hill
formulas reconstituted with tapwater containing 1.1 mg F/L ranged from 0.60 to 0.72 mg F/L.
For the powder concentrates reconstituted with de-ionized water, mean fluoride levels were 0.03
to 0.24 mg/L, whereas those from Chapel Hill reconstituted with tapwater containing 1.1 mg F/L
ranged from 1.00 to 1.25 mg/L. The overall mean fluoride concentration was 0.21 mg/L for
ready-to-feed formulas, 0.10 mg/L for liquid concentrates and 0.12 mg/L for powder
concentrates.
McKnight-Hanes et al. (1988) analyzed fluoride levels in infant formulas purchased in the
Rochester, NY, area. The formulas were prepared with de-ionized water or with water
containing 0.15 mg F/L or 1.0 mg F/L. Fluoride was separated from 3 mL of the prepared
formula as hydrofluoric acid, appropriately buffered, and analyzed directly using a fluoride ion-
specific electrode. The Taves method was used to separate the acid-diffusible fluoride from the
sample. Results are shown in Table 2-2. Results indicate that there is a significantly greater
amount of fluoride in the ready-to-eat soy-based formula and the liquid concentrate soy-based
formula than the corresponding milk-based formulas.
Table 2-2. Mean Fluoride Concentrations (mg/L) in Infant Formulas (McKnight-Hanes et al., 1988)
Type
Milk-based formulas:
Ready-to-use3
Liquid concentrates3
Powdered concentrates3
Soy-based formulas:
Ready-to-use3
Liquid concentrates3
Powdered concentrates3
Dilutent
Deionized
Water
0.127
0.121
0.055
0.305
0.242
0.084
0.15 mg F/L
0.196
0.170
0.317
0.200
1.0 mg F/L
0.621
0.825
0.742
0.854
Student's
t-Test
t=3.3
t = 2.9
t=1.4
p<0.01b
p < 0.02b
N.S.
SOURCE: McKnight-Hanes et al., 1988.
aUndiluted.
bSignificantly greater than milk-based, ready-to-use formula.
°Significantly greater than milk-based liquid concentrate formula.
Van Winkle et al. (1995) analyzed fluoride levels in water and formula fed to 1,308 children
younger than 2 years of age who were participants in the Iowa Fluoride Study. Mothers of
newborns completed questionnaires and 3-day food and beverage and dental care diaries which
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were used to document fluoride intake from diet, supplements and dentifrice. Information was
obtained at 6 weeks, when the children were 3 months old, and every 3-4 months thereafter.
Water sources other than unfiltered public water supplies were assayed for fluoride using a
fluoride ion-specific electrode. All formulas that appeared in the diaries were purchased and
analyzed for fluoride using direct readout (DR) from a fluoride ion-specific electrode (milk-
based formulas) or the modified Taves microdiffusion method (soy-based formulas) followed by
fluoride ion-specific electrode analysis. All powder and liquid concentrates were reconstituted
with distilled water (0 mg F/L). Fluoride levels in the various types of formula are given in
Table 2-3. Fluoride levels in soy-based formulas were higher than those in milk-based formulas.
Table 2-3. Fluoride Concentrations in Infant Formulas (Van Winkle et al., 1995)
Category
Milk-based formulas:
Ready-to-use
Liquid concentrates3
Powdered concentrates3
Soy-based formulas:
Ready-to-use
Liquid concentrates3
Powdered concentrates3
Number of
No. Samples
16
14
17
5
6
6
Fluoride Concentration (mg/L)
Mean
(mg/L)
0.17
0.12
0.14
0.30
0.24
0.24
Range
(mg/L)
0.04-0.55
0.04-0.19
0.05-0.28
0.17-0.38
0.04-0.47
0.19-0.28
SOURCE: Van Winkle etal., 1995.
Reconstituted with distilled water.
Siew et al. (2009) analyzed fluoride concentrations of 27 powdered and 13 liquid infant formula
concentrates and nine ready-to-feed formulas purchased in the Chicago area. The formulas
included both milk-based and soy-based varieties. The powdered and liquid concentrate
formulas were reconstituted with deionized water according to the manufacturers' instructions.
Powdered formulas were reconstituted by adding 2 ounces of deionized water to one scoop of
formula, and liquid concentrates were reconstituted 1:1 with deionized water. The total fluoride
content of the formulas was analyzed using a modified Taves diffusion method and a fluoride
ion-specific electrode. Results are shown in Table 2-4.
Table 2-4. Fluoride Levels in Infant Formulas Reconstituted with Deionized Water (Siew et al., 2009)
Formula type
Powdered concentrate
Liquid concentrate
Ready-to-feed
Overall mean
Base
Milk
Soy
Milk
Soy
Milk
Soy
Range of values
(ppm)
0.03-0.27
0.06-0.29
0.07-0.48
0.41-0.57
0.08-0.23
0.13-0.32
N
21
6
8
5
6
3
49
Mean ±SD
(ppm)a
0.12 ±0.08
0.16±0.09
0.27±0.18
0.50±0.08
0.15±0.06
0.21±0.10
0.1976 ±0.15
PValueb
0.44
0.01
0.46
SOURCE: Siew etal., 2009.
3Mean fluoride concentrations for milk-based formulas are compared with those for soy-based formulas.
bThe P value is based on a t test (unpaired data) comparing the mean values for milk and soy-based formulas.
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In general, soy-based formulas were higher in fluoride content than milk-based formulas. This
difference was not statistically significant for powdered concentrate and ready-to-feed
formulations; however, the fluoride concentration of the liquid concentrate soy formulas tested
was significantly higher than that of milk-based liquid concentrate formulas (P < 0.05, t test
analysis for unpaired data). The fluoride content in different batches of the same product was
fairly consistent.
Infant Foods. Singer and Ophaug (1979) measured fluoride levels in a variety of infant foods
including meats, vegetables, and fruits using a fluoride ion-specific electrode. Results are shown
in Table 2-5. The highest fluoride concentration was found in strained chicken with broth (mean
5.29 mg/kg; range 1.94-10.64 mg/kg). Mean F concentration in vegetables ranged from 0.15-
0.43 mg/kg, and those in fruits 0.017-0.078 mg/kg. Fluoride levels in dry cereal varied
depending on whether fluoridated water was used in the processing facility. Mixed cereals,
oatmeal, rice and barley cereals from facilities using non-fluoridated water contained 0.93, 0.98,
2.11, and 1.99 mg F/kg, respectively, whereas levels in the same types of cereals from plants
using fluoridated water were 3.85, 4.87, 6.35, and 4.30 mg/kg, respectively. Mean fluoride
levels in fruit juices made with non-fluoridated water ranged from 0.014 to 0.14 mg/L; juices
prepared with fluoridated water contained 0.15 to 1.48 mg F/L. Similarly, mean fluoride levels
in milk formulations were 0.08-0.31 mg/L when prepared with non-fluoridated water and 0.57-
0.66 mg/L when prepared with fluoridated water.
Table 2-5. Fluoride Concentrations in Infant Foods as Reported by Singer & Ophaug, 1979
Food Type
Strained meats
Chicken and broth
Turkey and broth
Beef and broth
Lamb and broth
Liver and broth
Veal and broth
Pork and broth
Overall mean
Vegetables
Carrots
Peas
Squash
Spinach
Green beans
Beets
Overall mean
Fruits
Pears
Peaches
Applesauce
Overall mean
Number of Plants
4
2
3
2
1
1
1
6
4
4
2
3
3
7
5
7
Fluoride Concentration (mg/kg food)
Mean
5.29
0.39
0.19
0.29
0.14
0.40
0.23
0.99
0.23
0.18
0.15
0.43
0.16
0.23
0.24
0.057
0.017
0.078
0.051
Range
1.94-10.64
0.34-0.43
0.17-0.21
0.16-0.42
0.14
0.40
0.23
0.022-0.53
0.038-0.34
0.046-0.34
0.18-0.67
0.036-0.33
0.13-063
0.012-0.13
0.003-0.034
0.016-0.23
SOURCE: Singer and Ophaug, 1979.
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December 2010
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A group of 206 commercially available, ready-to-eat infant foods purchased in Iowa City, Iowa,
were studied by Heilman et al. (1997) using a modified version of the Taves microdiffusion
method coupled with a fluoride ion-specific electrode. Fluoride levels ranged from 0.01 to 8.38
mg/kg. A summary of the results by food type is provided in Table 2-6.
Table 2-6. Fluoride Concentrations in Infant Foods as Reported by Heilman et al., 1997
Food Type
Fruits and desserts
Vegetables
Mixed foods
Meatsa
Chicken
Cereals
No. Samples
88
48
42
19
6
9
Fluoride Concentration (mg/kg food)
Range
0.01-0.49
0.01-0.42
0.01-0.63
0.01-8.38
1.05-8.38
0.01-0.31
Median
0.03
0.08
0.13
0.05
4.04
0.02
Mean
0.10
0.12
0.21
1.46
4.40
0.08
SOURCE: Heilman etal., 1997.
Includes poultry.
The highest fluoride concentrations were found in chicken (1.05-8.38 mg/kg); concentrations in
other meats ranged from 0.01 mg/kg in veal to 0.66 mg/kg in turkey. Heilman et al. (1997)
reported that the substantial variation in fluoride levels within a given type of food was due
primarily to different fluoride concentrations in the water used to process the foods. High
fluoride levels in chicken were attributed to the processing methods (mechanical deboning) that
leave some skin and residual bone particles in the meat. It was estimated that an infant
consuming 2 oz (about 60 g) of chicken containing 8 mg F/kg would have a fluoride intake of
about 0.48 mg (Heilman et al., 1997).
Heilman et al. (1997) also analyzed the fluoride content of 32 dry infant cereals and found that
the fluoride content ranged from 0.10-0.40 mg/kg. The study authors note that a considerable
amount of fluoride may be added to the cereal during manufacturing when the cereal is
processed as a slurry which is then dried, leaving any contained fluoride from the process-water
behind. Additional fluoride may be later added when the dry cereal is reconstituted with water
containing fluoride.
In 2005, the U.S. Department of Agriculture published a National Fluoride Database (USD A,
2005). This database summarizes and critically evaluates the quality of published and
unpublished information on the fluoride content of selected foods and beverages from a variety
of sources including data from some of the studies cited in this report. The database also
includes the results of USD A sampling of food and beverage products at 144 locations across the
U.S. (Pehrsson et al., 2000) as well as upublished data from several research projects. The
USDA samples were analyzed using a fluoride ion-specific electrode with direct readout for
clear liquids, and a microdiffusion method for other foods. The ranges of mean values for
various infant foods and beverages are shown in Table 2-7. The USDA data for foods consumed
by adults are given in Table 2-15.
14
December 2010
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Table 2-7. Fluoride Concentrations in Infant Foods as Summarized by USDA (2005)
Category/food group
Cereals
Desserts
Dinners
Fruit
Juice
Meat
Vegetables
Range of Mean Fluoride Concentrations
(mg/kg)
0.01-0.16
0.02-0.18
0.02-0.29
0.01-0.36
0.10-0.70
0.02-0.44
0.01-0.32
2.2.2. Fluoride in Foods of Children and Adults
San Filippo and Battistone (1971) calculated the fluoride content of representative food items
obtained in Baltimore, MD from an FDA "market basket program" on four separate occasions
(four diets) in 1967 and 1968. Each diet represented the 2-week food and beverage intake of 16-
19 year old males. The food items were placed into 12 commodity groups and analyzed on a
composite basis using microdiffusion and spectrophotometry (using erichrome cyanine R and
zirconyl chloride). Items were prepared in a manner representative of preparation in the home.
Fluoride concentrations are shown in Table 2-8. The highest fluoride levels were found in
beverages (beverages included tea, coffee, soft drinks and drinking water). Analysis of the
drinking water in the study area indicated that the fluoride level ranged from 0.99 to 1.0 mg/L.
Table 2-8. Fluoride Content of Food Commodity Groups
Commodity Group
Dairy products
Meat, fish and poultry
Grain and cereal products
Potatoes
Leafy vegetables
Legume vegetables
Root vegetables
Garden fruits
Fruits
Oils, fats, shortenings
Sugar and adjunct
Beverages*
Sample #1
(ppm)
0.19
0.55
0.49
0.13
0.46
0.24
0.08
0.41
0.11
0.45
0.44
1.22
Sample #2
(ppm)
0.22
1.00
0.44
0.17
0.15
0.19
0.06
0.09
0.10
0.24
0.30
1.07
Sample #3
(ppm)
0.15
1.04
0.26
0.17
0.13
0.24
0.07
0.07
0.11
0.25
0.33
1.10
Sample #4
(ppm)
0.11
0.42
0.59
0.45
0.85
0.25
0.22
0.18
0.10
0.12
0.56
1.10
SOURCE: San Filippo and Battistone, 1971.
aTea, coffee, soft drinks and drinking water.
15
December 2010
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Singer et al. (1980) evaluated fluoride concentrations in 117 food items placed in 12 composite
food groups for four geographic regions of the United States. Fluoride in the food items was
determined by four methods: ashed and unashed samples quantified using a fluoride ion-specific
electrode and colorimetric analysis (eriochromecyanine R procedure). The results from the ion-
specific electrode were found to be more accurate than the colorimetric method, especially for
unashed samples. Mean fluoride levels in the composite food groups are shown in Table 2-9.
Beverages represented the single highest source of fluoride (0.82-1.35 ppm).
Table 2-9. Fluoride Content of Composite Food Groups for Four Geographic Regions of the U.S.
Commodity
Group
Dairy
Meats, fish, poultry
Grain and cereal
products
Potatoes
Leafy vegetables
Legume vegetables
Root vegetables
Misc. vegetables
Fruits
Oils, fats
Sugars, adjuncts
Beverages*
San Francisco
ppm F
0.05
0.22
0.34
0.14
0.13
0.15
0.09
0.15
0.06
0.24
0.21
1.35
Buffalo
ppm F
0.05
0.22
0.39
0.08
0.13
0.24
0.10
0.14
0.13
0.13
0.24
0.82
Atlanta
ppm F
0.07
0.92
0.41
0.13
0.15
0.39
0.10
0.06
0.07
0.15
0.32
1.54
Kansas City
ppm F
0.05
0.32
0.29
0.14
0.10
0.31
0.09
0.17
0.06
0.15
0.35
0.83
SOURCE: Singer etal., 1980.
Includes tea, coffee, soft drinks, and water.
Food items in FDA toddler "Market Basket" collections made in 1977 and 1978 were analyzed
for fluoride by Ophaug et al. (1980b). The food items were placed in 11 composite groups for
four cities of the United States. Results are shown in Table 2-10. In all four locations, beverages
contained the highest concentrations of fluoride (0.54-1.19 ppm).
Taves (1983) measured fluoride levels in 93 foods and beverages included in a standard hospital
diet. The study authors note that the hospital was in a fluoridated area and consequently any
foods prepared with water reflect this factor. The concentration of fluoride in the tapwater was
not reported. Inorganic and total fluoride levels were determined on ashed and unashed samples
using the hexamethyldisiloxane (HMDS) microdiffusion (Taves) method coupled with a fluoride
ion-specific electrode. Range of mean levels in various food groups were reported as nanomole
per gram food and were converted to measures of mg/kg or mg/L by the IOM (1997). The
transformed results are given in Table 2-11. The highest fluoride concentration (144 nm/g; about
2.7 mg/L) was found in tea.
16
December 2010
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Table 2-10. Fluoride Content of Four Representative Diets for 2-Year-Olds
Commodity
Group
Drinking water
Whole milk
Other dairy
Meats, fish, poultry
Grain and cereal
products
Potatoes
Vegetables
Fruits and juices
Oils, fats
Sugars, adjuncts
Beverages3
Orlando
ppm F
0.67
0.02
0.10
0.48
0.23
0.04
0.24
0.22
0.29
0.24
0.94
Grand Rapids
ppm F
1.04
0.02
0.19
0.44
0.30
0.12
0.17
0.25
0.45
0.44
1.19
Philadelphia
ppm F
0.66
0.02
0.14
0.37
0.27
0.11
0.22
0.11
0.24
0.25
0.55
Los Angeles
ppm F
0.37
0.02
0.08
0.22
0.47
0.19
0.18
0.15
0.15
0.36
0.54
SOURCE: Ophaug et al., 1980b.
Includes carbonated and noncarbonated soft drinks, Kool-Aid, and tea.
Table 2-11. Fluoride Concentrations in Food Products
Category
Dairy products
Meat, fish and poultry
Grains and cereal products
Potatoes
Leafy vegetables
Legume vegetables
Root vegetables
Fruits
Sugars, etc.
Beverages3
Fats and oils
Miscellaneous
Fluoride Concentration (mg/kg or mg/L)
Mean
0.25
0.22
0.42
0.49
0.27
0.53
0.38
0.06
0.28
0.76
0.25
0.59
Range
0.02-0.82
0.04-0.51
0.08-2.01
0.21-0.84
0.08-0.70
0.49-0.57
0.27-0.48
0.02-0.08
0.02-0.78
0.02-2.74
0.02-0.44
0.29-0.87
SOURCE: Taves, 1983, as modified in IOM, 1997.
aDoes not include drinking water, but does include beverages made with tapwater.
Fluoride was determined with an ion-specific electrode after microdiffusion separation in various
foods obtained in 1987 in Winnipeg, Canada and reported in Dabeka and McKenzie (1995).
Mean fluoride levels for various food groups ranged from 0.095 mg/kg for fruits and fruit juices
to 2.1 mg/kg for fish (Table 2-12). The highest single items were cooked veal (1.2 mg/kg),
17
December 2010
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canned fish (4.6 mg/kg), shellfish (3.4 mg/kg), cooked wheat cereal (1.0 mg/kg), and tea (5.0
mg/kg). The mean for all samples was 0.325 mg/kg and the range was <0.011 to 4.97 mg/kg.
Table 2-12. Fluoride Concentrations in Foods Obtained in Winnipeg, Canada
Category
Milk and milk products
Meat and poultry
Fish
Soups
Vegetables
Fruits and fruit juices
Bakery goods and cereal
Fats and oils
Sugar and candies
Beverages
Miscellaneous3
Number of
Samples
12
17
4
4
38
25
24
o
J
1
1
7
Fluoride Concentration (mg/kg food)
Mean
0.189
0.251
2.118
0.606
0.146
0.095
0.402
0.096
0.111
1.148
0.564
Range
0.0 12-0.797
0.037-1.230
0.213-4.567
0.412-0.836
0.0 11-0.678
0.01 1-0.582
0.0 11-0.678
0.046-0.132
<0.0 16-0.275
0.213-4.970
0.075-1.000
SOURCE: Dabeka and McKenzie, 1995.
Includes tapwater (Dabeka and McKenzie, 1995, Table 2).
A recent study by Jackson et al. (2002) surveyed adolescents 12-14 years old to determine the
foods and beverages most commonly consumed by this age group. As a result, a total of 441
brand-name food items were purchased in both a non-fluoridated community (Connersville, IN;
fluoride 0.16 ±0.01 mg/L drinking water) and in a fluoridated community (Richmond, IN; 0.90
±0.05 mg/L). The foods and beverage items were placed into dietary groups according to USDA
guidelines, and the most up-to-date methods for analyzing for fluoride were used. Fluoride in
water and carbonated beverages was analyzed directly by using a combined fluoride ion-specific
electrode and pH/ion meter. Measurements were compared to a series of standards. Fluoride in
foods, juices and milk was analyzed with the HMDS silicon-facilitated microdiffusion method
of Taves (1968b) as modified by Rojas-Sanchez (1999). This method, which does not require
pre-ashing of the sample, was recommended in 1981 by the Association of Official Analytical
Chemists as the separation method of choice for analyzing fluoride in infant foods. The method
was validated in a series of spike and recovery tests. The Intraclass Correlation Coefficient of
the measurements was calculated to assess the reliability of the analyses (Bartko and Carpenter,
1976). The fluoride content of food and beverage items that were not cooked or reconstituted
with tap water did not vary significantly between the two towns; therefore, measurements of the
fluoride content of these items were assessed together (Table 2-13). However, fluoride content
of some food items reconstituted with or prepared in tap water (beverages and grain products)
was significantly different for several food categories (Table 2-14). The beverage items prepared
with the local Richmond tap water (0.9 mg/L) had significantly higher fluoride concentrations
then those prepared with the Connersville tap water (0.16 mg/L).
18
December 2010
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Table 2-13. Fluoride Concentrations of Noncooked and Nonreconstituted Foods and Beverages Consumed
by Adolescents 12-14 Years Old"
Category6
Grains and cereal
products
Vegetables0
Fruits
Dairy products
Meat, poultry
Nuts and seeds
Fats and oils
Sugars and sweets
Beverages
N
129
78
26
30
55
4
14
15
32
Fluoride Concentration (mg/kg)
Mean
0.49±0.25
0.25±0.28
0.12±0.21
0.31±0.29
0.36±0.30
0.16±0.03
0.24±0.17
0.29±0.19
0.55±0.26
Minimum
0.007
0.003
0.01
0.23
0.03
0.13
0.05
0.07
0.04
Maximum
1.36
1.93
0.84
1.36
1.41
0.19
0.62
0.60
0.93
95% CI
0.44, 0.53
0.18,0.31
0.04, 0.20
0.20, 0.42
0.28, 0.44
0.12,0.20
0.15,0.34
0.19,0.40
0.46, 0.65
SOURCE: Jackson et al., 2002.
aCombined data for foods and beverages purchased in Connersville and Richmond, IN.
'Excludes foods prepared with water.
"Excludes foods cooked with water.
dExcludes reconstituted and fountain beverages.
eUSDA food categories.
Table 2-14. Fluoride Concentrations (mg/kg) of Drinking Water and Foods and Beverages Reconstituted in
or Cooked in Tapwater
Food Group
Water6
Beverages
Bottled fruit drinks
Bottled carbonated
beverages
Reconstituted/fountain
carbonated beveragesa
Grain products
Vegetables0
Raw
Cooked
Connersville, IN
N
3
4
12
10
13
o
J
3
Mean
0.16
0.44
0.58
0.16
0.26
0.10
0.08
SD
0.01
0.40
0.21
0.04
0.11
0.06
0.06
Richmond, IN
N
3
4
12
12
11
o
J
3
Mean
0.90
0.65
0.53
0.78
0.86
0.10
0.73
SD
0.05
0.39
0.24
0.29
0.47
0.10
0.70
P value
0.01
0.49
0.59
o.or
o.or
0.99
0.18
SOURCE: Jackson et al., 2002.
"Includes juices, powdered drinks and fast food fountain drinks.
'includes cooked cereals, pastas, soups.
"Includes carrots, cauliflower, broccoli.
dUSDA food categories.
eSignificantly different between Connersville and Richmond.
19
December 2010
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The USDA (2005) database on foods provided information on foods consumed by the general
population as well data on infant foods (see Table 2-7). The ranges of mean values for various
food categories are shown in Table 2-15. The food categories in Table 2-15 are the headings
used in the database.
This database is the most comprehensive source of information on the concentrations of fluoride
in foods, but is incomplete because many foods found in an average U.S. diet are not included.
The database was developed from the data reported in many of the publications cited in this
report after critical review of the data and supplemented by data for foods collected and analyzed
by USDA (mostly beverages) during development of the database. USDA used a "key foods"
approach when selecting the materials they sampled for creation of the database; giving
consideration to previously published fluoride data for foods, beverages, and drinking water as
well as the respective patterns of consumption of these dietary items. Mean estimates of fluoride
concentration and variability in drinking water, beverages and foods that are the chief
contributors to dietary fluoride in the United States were developed from analyses of
representative samples.
Table 2-15. Fluoride Concentrations in Foods as Summarized by the USDA, 2005
Category/food group
Baked goods
Beef products
Breakfast cereals
Cereal grains and pastas
Dairy and egg products
Cream substitute-powdered
Fast foods
Fats and oils
Finfish and shellfish
Fruits and fruit products
Lamb, veal and game
Legume and legume products
Meals, entree, side-dishes
Nuts
Pork products
Poultry
Sausages and luncheon meats
Snacks
Soups, sauces and gravies
Spices and herbs
Sweets
Vegetables and vegetable products
Range of Mean Fluoride Concentrations
(mg/kg)
0.13-0.69
0.05-0.22
0.17-0.72
0.06-0.41
0.01-0.35
1.12
0.13-1.15
0.01-0.27
0.18-2.10
0.01-2.34
0.05-0.32
0.02-0.54
0.13-0.84
0.10
0.04-0.38
0.15-0.21
0.16-0.48
0.06-1.06
0.04-1.32
0.02-0.34
0.01-0.89
0.01-0.55
SOURCE: USDA, 2005.
20
December 2010
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2.2.3. Summary of the Data on Fluoride in Solid Foods
There is some consistency in the data on the concentrations of fluoride in foods despite the
differences in analytical methods, preparation, and sampling practices. The solid foods highest
in fluoride are fish and shellfish, reflective of the fluoride found in ocean water (-13 ppm). Most
samples offish and shellfish that have been analyzed contain greater than 1 ppm (Jackson et al.,
2002; Singer et al., 1980; USD A, 2005). More recent analyses offish samples are lower than
those from the early studies (range 0.18-2.10; USD A, 2005). Choice of analytical methods can
account for some of these differences as can the presence or absence of bone fragments in the
sample analyzed.
When foods were grouped for analysis, the inclusion offish in a grouping with meat and poultry
tended to lead to a higher mean value than found for meat or poultry alone or combined (Dabeka
and McKenzie, 1995; Jackson et al., 2002; USD A, 2005). Chicken had a relatively high fluoride
content (>1 ppm) in baby foods (1.20-8.38 ppm; Heilman et al., 1997). However, in the USDA
(2005) database chicken has a far lower average value (0.15 ppm) than reported in some of the
earlier studies. The USDA value for chicken is attributed to Featherstone (1988), Jackson (2002)
and Ophaug (1983-1987).
The majority of vegetables, be they leafy, root, legumes, green or yellow, have a relatively low
fluoride concentration (<0.5 ppm; IOM 1997; Singer et al., 1980; USDA, 2005). The
concentrations for fruits were generally lower than those in vegetables (< 0.2 ppm) in most
assays (IOM, 1997; Singer et al., 1980; Singer and Ophaug, 1979; USDA, 2005). Table 2-15
derived from the USDA database indicated a concentration range of 0.01 to 2.34 ppm for fruits.
However, in this case, the high end measure (raisins) was an outlier reflecting the use of cryolite
as a pesticide on grapes and concentration through drying. Fresh grapes had 0.08 ppm fluoride;
the concentration in all other fresh fruit was < 0.04 ppm.
Cereals, baked goods, breads, and other grain products tended to have fluoride concentrations
between about 0.5 and 1 ppm (IOM, 1997; Jackson et al., 2002; Singer et al., 1980). Dairy
product fluoride concentrations, as reported by IOM (1997), Singer et al. (1980), and USDA
(2005) were low (<0.5 ppm).
Infant foods have a tendency to have a higher liquid content than foods for toddlers through
adults in order to minimize chewing and increase the ease of swallowing. When fluoridated
water is used in their preparation, this can add to the total fluoride concentration. Most infant
foods studied had concentrations less than 0.5 ppm if they were cereal, fruit or vegetable based
and less than 1 ppm if they contained meat. Products containing chicken had a higher fluoride
concentration than those with meat or turkey in several studies (Heilman et al., 1997; Singer and
Ophaug, 1979). However, this was not the case with the meat and poultry containing infant foods
in the USDA (2005) database where concentrations were less than 0.5 ppm. The USDA data for
the meat and poultry-containing baby foods was attributed to unpublished data from Steven Levy
(University of Iowa).
In a study of maternal milk by Dabeka et al. (1986) fluoride levels were below detection in 56%
of the 210 samples tested and the mean concentration in areas without fluoridated water was
0.0044 mg/L while those receiving fluoridated water (1 mg/L) was 0.0098 mg/L. These
21 December 2010
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differences were significant (p = 0.007). The IOM (1997) reported that the fluoride concentration
in human breast milk ranged from 0.007 to 0.011 ppm.
The fluoride concentration in infant formula is difficult to assess and depends on the brand and
form of the formula product (i.e., liquid, concentrate, powder; Dabeka and McKenzie, 1987) and
the protein source (milk protein or soy protein; Van Winkle et al, 1995). In US products
analyzed by Dabeka and McKenzie (1987) the mean fluoride levels ranged from 0.23 mg/kg for
ready-to-serve products to 1.13 mg/kg for powdered formula concentrate. Fluoride from the
dilution water further increases the total fluoride from formula (as served) in the case of
concentrated and powdered products. For milk-based formulas Van Winkle et al. (1995)
reported mean values of 0.17 mg/L for ready-to-use products, 0.12 mg/L for liquid concentrates,
and 0.14 mg/L for powdered concentrates. In the case of soy formulas, the comparable values
were 0.30 mg/L (ready-to-use) and 0.24 mg/L (liquid and powdered concentrate. Distilled water
was used to prepare the samples for analysis.
In the most recent analysis of U.S. infant formula, Siew et al. (2009) reported mean values of
0.15, 0.27 and 0.12 ppm for milk-based, ready-to-use, liquid concentrates, and powdered
concentrates, respectively, and 0.21, 0.50, and 0.16 ppm for soy-based, ready-to-use, liquid
concentrates and powdered concentrates, respectively. The overall mean for all products
combined was 0.198 ppm.
It is difficult to tell if changes in analytical methods over time have influenced the results from
studies of fluoride in foods. Singer et al. (1980 found that the results with an ion-specific
electrode were more accurate than a colorimetric method and that ashed samples gave different
results from unashed samples for some food groups but not for others. Table 2-16 compares the
results from several studies conducted over the past 30 plus years that grouped the foods in the
same manner. No pattern is apparent in the results reported. The analytical results are likely
influenced by the products represented in a food group, food growth and preparation practices, as
well a variety of other variables that are difficult to quantify.
Table 2-16. Comparison of Food Group Measures over a 30-Year Period
Food group
Dairy products
Meat fish poultry
Grains and cereals
Leafy vegetables
Legume vegetables
Root vegetables
Fruits
San Filippo and
Battistone, 1971a'b
(mg/kg)
0.17
0.75
0.45
0.4
0.23
0.10
0.11
Singer et al.,
1980b
(mg/kg)
0.06
0.24
0.36
0.13
0.27
0.1
0.08
Taves, 1983/
IOM, 1997
(mg/kg)
0.25
0.22
0.42
0.27
0.53
0.38
0.06
Jackson et
al., 2002
(mg/kg)
0.31
0.36
0.49
0.25
0.12
USDA 2005
0.01-0.33
0.04-2.10
0.06-0.72
0.01-0.55
0.01-.0.13C
aAverage of 4 measurements.
bColorimetric method used by San Fillipo and Battistone (1971) has a tendency to give higher results than the ion-specific
electrode used by the other researchers (Singer et al., 1980).
°Raisins not included.
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Cooking and preparing foods with water that contains fluoride increases the fluoride content of
the food as served (Marier and Rose, 1966). This is true for home-prepared and commercial
foods. However, the uptake of fluoride from the process water varies with the food product. This
may relate to the presence of cations in the water that form poorly soluble fluoride salts such as
calcium fluoride reducing fluoride uptake into the finished product to a greater extent than those
like sodium that form soluble salts or from fluoride in the water reacting with these same ions in
the food and increasing the fluoride from water retained in the cooked product.
Maier and Rose (1966) analyzed the fluoride content of canned vegetables processed at plants
using low-fluoride water and plants using municipal water with 1 mg F/L using a micro-
distillation method coupled with colorimetric/spectrophotometric detection. Use of fluoridated
process water increased the fluoride content of the vegetables by 0.34 to 0.75 mg/kg (average
0.5 mg/kg) (Table 2-17). Although the values measured are likely to be high because of the
colorimetric quantification, they do illustrate the impact of processing foods with fluoridated
water. However, Ophaug (1985) reported that there was not a strong correlation between the
local fluoride drinking water concentration and total fluoride intake from solid foods in market
basket studies, most likely reflecting the combination of purchased and home prepared foods in a
normal diet.
Table 2-17. Fluoride Content of Canned Vegetables
Food
Mixed vegetables
Green beans
Whole potatoes
Diced carrots
Kernel corn
Green peas
Wax beans
Average Fluoride Content (mg/kg)
Non-fluoridated Process Water
Liquid
0.30
0.14
0.13
0.30
0.10
0.15
-
Solid
0.37
0.20
0.38
0.19
0.20
0.10
-
Fluoridated Process Water (1 mg F/L)
Liquid
1.03
0.71
0.87
0.55
0.48
-
0.49
Solid
1.05
0.89
0.76
0.61
0.56
-
0.60
SOURCE: Marier and Rose, 1966.
aResults are averages of single determinations for duplicate samples.
2.3. Fluoride in Beverages
Beverages are a major source of human dietary exposure to fluoride, especially after fluoridation
of public drinking water became widespread and before the growth in bottled water intake.
Exposure from plain (e.g., non-beverage) drinking water is summarized in Section 3 of this
report. Data on other beverages are presented below.
2.3.1. Non-Alcoholic Beverages
Clovis and Hargreaves (1988) published data (Table 2-18) from a study by Hargreaves which
measured fluoride levels in beverages in two towns in Canada. One town had a fluoridated water
supply (average adjusted fluoride concentration of 1.08 mg/L) and the other had a natural
fluoride level of 0.23 mg/L. Fluoride levels in commercially prepared beverages were similar in
23
December 2010
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the two towns; however, fluoride levels in home-prepared beverages were substantially higher in
the community with the fluoridated water supply.
Stannard et al. (1991) measured fluoride levels in 43 ready-to-drink fruit juices purchased in the
Boston area; however, the products were bottled in various locations around the U.S. Fluoride
was measured using a fluoride ion-specific electrode. Fluoride concentrations ranged from 0.15
to 6.80 ppm. Forty-two percent of the samples had a fluoride content of greater than 1 ppm.
Grape juice had the highest levels of fluoride (1.94-6.80 ppm), most likely reflecting the use of
cryolite as a pesticide on grapes.
Fluoride concentrations were measured in 532 different juices and juice-flavored drinks
(including five teas) purchased in Iowa City by Kiritsy et al. (1996). Many of the products were
distributed nationally or internationally. Frozen-concentrated beverages were reconstituted with
distilled water before analysis. The fluoride concentration ranged from 0.02 to 2.8 mg/L (mean,
0.56 mg/L). Upper limits on most kinds of juices exceeded 1.50 mg/L. The highest mean
fluoride concentration (1.45 mg/L) was found in white grape juice.
Table 2-18. Fluoride Concentrations in Beverages in Two Canadian Towns
Category
Milk
Carbonated beverages
Commercially prepared juice
Home prepared juice
Soups
Tea
Coffee
Other beverages prepared with tapwater
Misc., prepared with 0. 1 ppm water
Fluoride Concentration (ppm)
Town #1
(1.08 mg/L)
0.03
0.80
0.80
1.06
1.06
2.18
1.08
1.08
0.10
Town #2
(0.23 mg/L)
0.03
0.80
0.80
0.21
0.21
1.33
0.23
0.23
0.10
SOURCE: Hargreaves, unpublished, as cited in Clovis and Hargreaves, 1988.
The fluoride content of 332 carbonated beverages was measured by Heilman et al. (1999). The
beverages were purchased in Iowa, but produced at 17 different locations. Mean concentrations
of fluoride ranged from 0.04 mg/L to 1.06 mg/L (overall mean 0.72±0.34 mg/L).
Turner et al. (1998) reported fluoride levels of 0.68-0.91 ppm (mean 0.78±0.07 ppm) in
carbonated drinks bought in Houston, TX, and 0.0-0.73 ppm (mean 0.33±0.28 ppm) in
carbonated drinks bought in San Antonio, TX. Levels of fluoride in ready-to-drink juice drinks
were 0.28-1.08 ppm (mean 0.77 ±0.21 ppm) in Houston and 0.16-1.02 ppm (mean 0.58 ±0.38
ppm) in San Antonio. Fluoride determinations were made with a fluoride ion-specific electrode.
Various brands and kinds of coffee sold in the Houston area were analyzed for fluoride by
Warren et al. (1996). All samples were prepared with deionized distilled water. Fluoride levels
ranged from 0.10 to 0.58 mg/L. The mean concentration for decaffeinated coffee was 0.14 mg/L
and that for caffeinated 0.17 mg/L. Instant coffee had a mean fluoride content of 0.30 mg/L.
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The USD A (2005) database contains mean values for a variety of beverage categories as shown
in Table 2-19. The results are consistent with those reported in other publications. In order to
examine more closely the possible relationship between the concentrations of fluoride in
carbonated beverages and possible use of tap water containing fluoride in the production of such
beverages, the OW evaluated the mean and maximum concentration for the large sample sets
(28-72 samples/set) in the USD A (2005) fluoride database. The mean of the means for six
different carbonated beverage sets (4 colas) was 0.53 mg/L while the mean of the maximum
values was 0.97 mg/L. Since the ingredients other than water in such beverages are not notably
rich in fluoride, much of the fluoride present appears to come from the water component of the
beverage.
Table 2-19. Fluoride Levels in Beverages as Summarized by the USDA, 2005
Category/food group
Carbonated, non-alcoholic drinks
Carbonated flavored water
Chocolate, ready-to-drink
Coffee
Grain-based coffee substitute
Fruit juices and drinks
Range of Mean Fluoride Concentrations
(ppm)
0.14-0.84
0.84-1.05
0.87
0.52-0.91
1.25
0.08-1.09
Tea is a rich source of fluoride; concentrations vary depending on the type of tea, its source, and
the age of the leaves. The fluoride content of buds and young leaves ranges from 100 to 430
mg/kg, whereas that of older leaves ranges from 530 to 2350 mg/kg (Lu et al., 2004). Data on
the fluoride concentration of teas are summarized in Table 2-20.
Table 2-20. Fluoride Concentration in Tea as Served
Study
Cao et al., 2006
Chan and Koh, 1996
USDA, 2005
Whyte et al., 2005
Type
Black tea sticks
Black tea granules
Black tea bags
Caffeinated
Decaffeinated
Herbal
Caffeinated
Decaffeinated
Iced Tea
Green Tea
Herbal
Caffeinated and
decaffeinated
Concentration
(ppm)
0.95-1.41
0.7-2.44
1.15-6.01
0.34-3.71
1.10-5.2
0.02-0.14
3.10-3.93
2.47-2.93
0.72-1.23
1.15-2.72
0.13-0.90
1-6.5
Notes
Aged tea leaves
44 brands; brewed 5 to 120
minutes
Caffeinated and decaffeinated
Chamomile, peppermint
Prepared with distilled water
25
December 2010
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2.3.2. Alcoholic Beverages
Fluoride is present in a number of alcoholic beverages, especially wines, due to the use of
cryolite as a pesticide on grapes. Burgstahler and Robinson (1997) reported fluoride levels of
0.23-2.80 ppm (mean 1.02 ppm) in California wines. Seven of 19 samples tested above 1 mg/L.
Fluoride was determined using a fluoride ion-specific electrode. Martinez et al. (1998) reported
mean fluoride concentrations ranging from 0.08 to 0.68 mg/L in 70 wines from the Canary
Islands. The overall mean concentration was 0.16 mg/L. USDA (2005) found a mean
concentration of 1.05 ppm from 14 red wine samples and 2.02 ppm for 17 white wine samples.
Warnakulasuriya et al. (2002) reported mean fluoride concentrations of 0.08-0.71 mg/L in eight
kinds of beers available in Great Britain. The concentrations were the equivalent of 0.03-0.3 1
mg fluoride in one 440 mL can. USDA (2005) reported a mean of 0.45 ± 0.023 ppm for 142
light beer samples and 0.44±0.025 ppm for 102 regular beer samples. The average fluoride in
distilled alcoholic beverages was 0.08 ppm in the USDA (2005) database.
2.3.3. Summary for Fluoride in Beverages
The fluoride in commercial products tends to reflect the water source at the plant where juices
and carbonated beverages are processed. In most instances concentrations in carbonated
beverages ranged between 0.7 and 1 ppm, reflecting the concentrations in fluoridated water
(Clovis and Hargreaves, 1988; Heilman et al., 1999; Schulz et al., 1976; Turner et al., 1998,
USDA, 2005). Commercial fruit juices have the same or slightly lower means (Clovis and
Hargreaves, 1988; Kiritsy et al., 1996; Stannard et al., 1991, USDA, 2005), although the means
for grape-based products can be higher. USDA (2005) reported the mean concentration of grape
juice as 0.77 mg/kg for 20 samples of regular grape juice and 2.13 mg/kg for 12 samples of white
grape juice. Home-prepared products appear to reflect the concentration of the local water
supply (Clovis and Hargreaves, 1988; Jackson et al., 2002).
Tea is a rich source of fluoride, especially when made from aged leaves (Cao et al., 2006).
Herbal teas do not have the high fluoride content of real teas (Chan and Koh, 1996). All of the
samples of brewed black tea analyzed by USDA (2005) had a mean fluoride concentration of > 3
ppm. Brewed herbal teas and green teas had lower concentrations. Three popular brands of
bottled commercial ice teas had means between 0.72 and 1.23 mg/L (USDA, 2005).
Among alcoholic beverages, wines have the highest fluoride levels (usually 1-2 ppm) likely
reflecting the cryolite use in the growing of grapes (Burgstahler and Robinson, 1997; Martinez et
al., 1998; USDA, 2005). Levels of fluoride in distilled alcoholic beverages are low (<0.1 ppm;
USDA, 2005) and those in beer are intermediate, about 0.4 to 0.5 ppm for U.S. products (USDA,
2005).
2.4. Indirect Exposure from Pesticide Residues on Food
Cryolite. Cryolite (sodium aluminofluoride; NasAlFe) was first registered for use as a pesticide
in the U.S. in 1957 (U.S. EPA, 1996). It is used on fruits, vegetables and ornamental plants to
protect against leaf eating insects. The major products treated with cryolite are grapes, citrus
fruits, and potatoes. Applications rates are frequently high, and application can occur several
times during a growing season (U.S. EPA, 1996).
26 December 2010
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According to NRC (2006), the high fluoride content of grape juices (and grapes, raisins, and
wines), even when little or no manufacturing water is involved, is thought to be due to a cryolite
used in grape growing (Stannard et al., 1991; Kiritsy et al., 1996; Burgstahler and Robinson,
1997). The water-extractable fluoride in five brands of California raisins ranged from 0.83 mg/kg
to 5.20 mg/kg (mean 2.71 mg/kg). Soaking the raisins in distilled water for 1-2 hr resulted in the
release of 70-90% of the fluoride, suggesting that the fluoride was concentrated on the skin of
the fruit (Burgstahler and Robinson, 1997).
One study reported by Waldbott (1963) showed that celery leaves sprayed with cryolite had
fluoride residues of 77.0-135.0 ppm F whereas the normal levels of fluoride in celery were
reported to be 0.7-5.7 ppm. Similarly, 2.0-4.5 ppm F was found on sprayed apples compared
with 0.04-1.3 ppm F on unsprayed apples.
The market basket dietary data reported in this document include fluoride exposure from cryolite
because of its long history of use on a variety crops. To avoid counting the exposure to fluoride
from cryolite twice, the additional estimates of cryolite residue values provided by OPP (U.S.
EPA, 2009, see Appendix A) were not directly incorporated into the EPA exposure assessment.
There is uncertainty surrounding the OPP estimation of fluoride exposure through cryolite,
because the current analytical methods are unable to differentiate the various aluminum fluoride
species in each product and instead report total fluoride. Thus, it is possible that the residue
estimates could represent an overestimate. In the OPP assessment (U.S. EPA, 2009), the highest
level of fluoride residues was contributed by the OPP "other" food group which includes grape
and grape juice among other miscellaneous commodities such as coco beans, and coconut.
About 60% of the total fluoride residue in the "other" group comes from cryolite rather than
sulfuryl fluoride (See Appendix A).
Sulfuryl Fluoride. Sulfuryl fluoride, initially also known as Vikane, is a pesticide that was not
registered for food use when the studies reported in Section 2.2.2 were conducted. Therefore,
fluoride residues from its use are not included in the data presented. Sulfuryl fluoride was
developed by Dow Chemical in the late 1950s as a structural fumigant. It was first registered by
the OPP in December 1959 and first marketed in the United States in 1961. Sulfuryl fluoride is
now produced and sold by several manufacturers, under various brand names.
Sulfuryl fluoride is highly reactive and breaks down to form sulfate and fluoride anions. Parent
sulfuryl fluoride and the fluoride anion are the OPP's residues of concern for both tolerance
expression and risk assessment. It is considered to be an effective replacement for ozone
depleting methyl bromide, the conventional pesticide that had been used for structure fumigation.
On February 7, 2002 the Federal Register established temporary tolerances for residues of
sulfuryl fluoride and inorganic fluoride in or on walnuts and raisins. The temporary tolerances
were established to support an Experimental Use Permit (EUP) that involved testing a possible
alternative to methyl bromide in the post-harvest fumigation of stored walnuts and raisins (Fed
Reg. 67(59): 14713-14714). The temporary tolerances supported a 3-year EUP effective between
March 1, 2002 and March 1, 2005. There was no apparent exercise of the EUP. An 18-month
27 December 2010
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period was given to allow the treated commodities to clear commerce, meaning the temporary
tolerances expired on September 1, 2006.
The OPP was later petitioned by Dow AgroSciences (DAS) to register sulfuryl fluoride to
control pests in storage and processing facilities as well as to establish permanent tolerances for
residues of sulfuryl fluoride and the fluoride anion on cereal grains, dried fruits, and tree nuts. In
2004 the Health Effects Division (HED) of OPP conducted a human health risk assessment for
sulfuryl fluoride. Time-limited tolerances were granted for the requested commodities and
facilities, with the understanding that when the National Academies of Sciences (NAS) review of
fluoride for the OW was completed, the proposed tolerances were to be revisited.
In January of 2006, HED released a risk assessment that postdated a 2005 FR notice establishing
tolerances for residues of sulfuryl fluoride and fluoride resulting from fumigation of additional
foods (i.e. milk powder, eggs, cocoa, cheese, meat, coffee) and for food processing facilities.
Health-effects related limitations for fluoride exposure were based on the OW's MCLG for
fluoride in drinking water (4 mg/L and 2L drinking water per day). The MCLG was under
evaluation by NAS at that time. The OPP risk assessment stated that the tolerances would be
reevaluated once the NAS report was published.
HED performed a dietary exposure assessment for fluoride from treated food products for this
effort at the request of the OW (U.S. EPA, 2009). The analysis incorporates the most recent
residue data submitted to the agency by the registrant (Dow AgroSciences). The current analysis
is intended to replace the exposure projections from the 2006 OPP risk assessment. The HED
report to OW is found as Appendix A in this report.
The OPP report to the OW does not include any experimental data on residues in foods. The
OPP exposure analysis is based on residue data from select foods commodities extrapolated to
similar foods in deriving exposure estimates for humans. Intake data for food groups were
derived from the USDA's Continuing Survey of Food Intakes by Individuals (CSFII). All the
OPP exposure estimates utilize percent crop treated information.
The OPP analysis (U.S. EPA, 2009) used percent crops treated values for exposures during
fumigation that ranged from 0.1% to 100% for food fumigation based on reports of methyl
bromide usage by USDA. Use rate information was incorporated in the analysis to derive
anticipated residue values. One hundred percent of the dried beans and legumes (except chick
pea and cow pea) were assumed to be fumigated using sulfuryl fluoride as were cocoa beans and
a high percentage of walnuts, dates, prunes, raisins, and figs. The percent of crop treated for
coarse grains and wheat by-products such as flour was 0.1% and that for rice was 3%. For most
nuts, 10% of the crop was estimated to be treated based on the data for methyl bromide.
The OPP (U.S. EPA, 2009) food group exposure estimates are summarized in Table 2-21. Food
groups have been consolidated from the OPP tables to be consistent with groups reported in
other publications. Twenty-one food groups were reduced to twelve in this process. The values
reported are exposures of the general US population to fluoride from sulfuryl fluoride in each
food group. The "Other" group includes but is not limited to, cocoa beans, coconut, cranberry,
grape, and grape juice products. Based on the data from OPP, grains, legumes, and fruits
including fruit juices appear to be the major contributors of fluoride in the U. S. diet through the
28 December 2010
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tolerances granted to sulfuryl fluoride. The "other" food group is another large contributor but is
varied in its composition. The data from OPP were reported in units of mg/kg/day. They were
converted to mg/day values for this report using a 70 kg body weight consistent with OW
policies for the general U.S. population.
Table 2-21. Estimated Food Group Exposures of the General U.S. Population to Fluoride
from Sulfuryl Fluoride Tolerances
Food Groups
Dairy products
Meat & Poultry
Cereal Grains
Leafy vegetables
Legume vegetables
Root, tuber, bulb vegetables
Cucurbit and Fruiting Vegetables
Fruits & Fruit Juices
Tree nuts
Herbs and spices
Oil seeds
Otherb
mg/daya
0.0002
0.0007
0.0297
0.0016
0.0370
0.0015
0.0017
0.0044
0.0011
0.0002
O.0001
0.0646
SOURCE: U.S. EPA, 2009.
aBased on a 70 kg body weight.
bThe "other" category applies to foods not captured in one of the other groups including but not limited to
cocoa beans, coconut, cranberry, grapes and grape juice.
2.5. Estimates of Dietary Fluoride Intake
2.5.1. Exposure Assessment Methodologies
Estimates of dietary fluoride exposure are based on studies using several analytical approaches.
In reviewing the data it is important to understand the technical framework for each approach as
well as its strengths and limitations. The studies included in this Section have relied on
combinations of several methods for collecting dietary data for use in an exposure analysis:
Dietary records
Dietary recalls
Food frequency recall
Market Basket or Total Diet Study (TDS) surveys
Duplicate plate-type analyses.
The following paragraphs provide background information on each of the methods that were
used in generating the fluoride exposure estimates. To facilitate evaluation of the resultant
exposure estimate, the studies are grouped by method for three age groupings: infants, children <
14 years, adolescents and adults. Studies examining intakes for children less than 6 month of age
29 December 2010
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are not included because this age group was not identified as a sensitive population in the
fluoride dose-response assessment (U.S. EPA, 2010a).
Dietary Records. Dietary record studies require participants to keep a diary of the amounts and
kinds of foods they consume daily. This approach is useful for assessment of individual or group
intakes. Generally a minimum of three days is recommended (Guthrie, 1989), often two week
days and one week-end day. Compliance with recording intake tends to decline as the number of
days and complexity of record keeping increase.
The accuracy of dietary records is dependant on the literacy and commitment of the participants.
Failure to record condiments and other foods taken in small amounts is common. With busy
individuals, record keeping can regress to end of the day recall as the study progresses. Some
people may fail to record foods they think they should not be eating and favor recording intakes
of foods they feel are nutritious.
The dietary record is applicable to other groups who share the characteristics (i.e. age, sex, and
ethnicity) of the population that participated in the study, but not to groups with different
demographics. They provide information on nutrient intake when they are coupled with food
composition databases or analytical data on the amounts of a nutrient in specific foods. Three-
day records are best for studies of macronutrient intakes and less-well suited for studies of
micronutrients (Nutrition Quest, 2008).
Dietary Recall. Dietary recalls are the preferred method for population studies but can also be
used for evaluation of individual intakes. The difference between the recall and record approach
is the use of a trained interviewer for collection of the recall data. The interview is structured to
stimulate the responder's memory. The interviewer has a set of props to assist the respondent in
quantifying portion sizes. The use of the interview reduces the requirement for participant
literacy and widens the pool of potential participants.
Single 24-hour recalls can be used to describe the average intake of a group or to determine if
two groups have similar mean intakes. A single day 24-hour recall is not appropriate for
epidemiology studies or for assessing the quality of an individual's diet (Nutrition Quest, 2008).
Two- and three-day recalls are popular durations for the recall approach. As was the case for the
dietary record, a three-day recall will often target two week days and one weekend day.
Recall intake data are coupled with food composition information from nutrient databases or
food analysis information to generate exposure estimates. Studies show that large portion sizes
are generally underestimated and small portion sizes overestimated in recall studies (Guthrie,
1989). The recall approach lessens the record-keeping fatigue problems encountered with the
dietary record approach.
Two large-scale, recall-based studies in the United States are the National Health and Nutrition
Examinations Survey (NHANES) and the Continuing Survey of Food Intake by Individuals
(CSFII). NHANES is periodically updated by the National Center for Health Statistics of the
Centers for Disease Control and Prevention (CDC). In the NHANES, dietary data are gathered
through a 24-hour recall interviews conducted by a trained professional.
30 December 2010
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The CSFII was conducted by the U.S. Department of Agriculture on a periodic basis. One
purpose of this survey was to provide information on the kinds and amounts of food eaten by the
U.S. population. Each survey covered 3 years. In each of the survey years, a nationally
representative sample of the population was interviewed to provide information on 2 non-
consecutive days of food intake using the 24-hour recall approach. The direct tap water intake
data reported in USEPA (2000a, 2004) were derived from the CSFII.
Food Frequency Recall. In a food frequency recall the subject is asked how frequently foods
from a defined list are consumed over a specific time period (i.e. per day, week or month). The
list of foods is selected based on the objective of the study, generally targeting foods that are a
source of a particular nutrient or group of nutrients. The food frequency questionnaire can be
administered by an interviewer or self administered (Nutrition Quest, 2008). Frequency recall
data can be used in the development of analytical market baskets that reflect food preferences for
age groups of interest, but need to be combined with national intake data for foods or food
groups as collected by CSFII or NHANES in order to quantify food group intakes applicable to
the population studied.
Food frequency recalls are well suited to examining food preferences focused on intakes of
specific nutrients. For example, if there is concern about vitamin A intake of elderly adults, a
food frequency recall tool can be developed that focuses on foods know to be high in vitamin A.
The population status can be estimated by the frequency at which such foods are consumed (i.e.
daily vs. once per week). The food frequency tool is not as well suited to an evaluation of the
nutritional status of an average daily diet.
Market Basket Survey. A Market Basket Study relies on chemical analysis of a typical diet
using foods purchased (market baskets) at different locations and during different seasons of the
year. The U.S. Food and Drug Administration uses a Market-Basket approach to track the intake
of nutrients and contaminants in the U.S. diet in their Total Diet Study (TDS, Egan et al., 2007).
Several of the studies in Section 2.2 used a Market Basket approach for collecting and grouping
of foods. The results from those studies provided the data for some of the exposure estimates
reported in this section.
The Market Basket approach combines food recall data with chemical analysis of foods that are
representative of dietary intakes for different age/gender groups plus the geographic diversity
and seasonal influences that influence the foods purchased. The composition of representative
diets is derived from food intake studies such as the CSFII Survey. The foods are purchased in
different locations and prepared as they would be served. Individual food samples are pooled,
homogenized, and analyzed to obtain representative aliquots for the analytes of interest (Egan,
2002). Intake from water that does not become incorporated in the foods as served is not
captured by this analysis although analytes transferred to food from water during preparation are
captured. Foods can be analysed individually or in narrow food groups such as "white breads"
or "cooked apple products" (Egan et al., 2007). The most recent FDA TDS included 280 foods
from 12 broad food groups and covered 15 age/gender groupings (Egan et al., 2007).
The TDS represents the typical US diet. It does not provide estimates for individual or
population exposure distributions (Egan et al., 2007) unless coupled with the intake distributions
31 December 2010
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of a national survey such as NHANES or CSFII. The IDS data can identify the food groups that
are the major source of exposure to a nutrient or contaminant.
Duplicate Plate or Duplicate Diet Analysis. In a duplicate plate or duplicate diet study the
participants set aside an equivalent weighed portion of each of the foods they consume for
analysis. The plate terminology is appropriate in cases where two identical servings of each
meal are prepared in a food service setting such as a hospital kitchen. One plate is served and
consumed and the other is used for analysis. In the case of a duplicate diet study sometimes
duplicate portions of each food consumed are placed directly in one or more dedicated collection
vessels and preserved for later analysis (Thomas et al., 1997). Often there are separate collection
vessels for solid and liquid foods. At the end of the collection period the foods are homogenized
and several aliquots are harvested for chemical analysis of the analytes of interest.
The analyte concentration per mass of the aliquot when scaled to the mass of food
collected/consumed produces the estimate of the analyte intake for the day. The estimate of
intake is rather accurate for each individual and can be averaged for the participating group
providing a mean, median, standard deviation, and range for intake of the analyte. Intake from
direct tap water ingestion is not usually captured by this analysis.
The data from a duplicate diet study are limited if they do not identify and quantify the foods
contributing the analyte to the diet, and do not easily extrapolate to groups with other dietary
habits and/or demographic characteristics (age, gender, etc.). Intake estimates are also impacted
if the consumer eats more or less than was placed on the duplicate plate or in the collection
vessel.
Carrying out a duplicate diet study is resource intensive (Thomas et al., 1997; Martinez-Mier et
al., 2008). It requires dedicated participants if the collection period lasts for more than a day or
two. When participants are in a free-living setting they must prepare their foods, record and
weigh what they consume, collect the duplicate portion in the dedicated collections vessels and
keep the collected foods under conditions that will preserve the analytes and prevent spoilage.
Special plans must be made for measuring, collecting and preserving any foods consumed away
from the home setting.
Several exposure estimates reported in Section 2.2 involve plate analyses from hospital kitchens.
This type of analysis represents foods served but not necessarily food consumed unless there is a
correction for plate waste. The majority of duplicate plate or diet studies included in this report
did not require that the participants prepare, record, measure, and preserve the foods they ate for
later analysis in a free-living setting. Most of the studies cited were conducted in a hospital or
school-like setting.
There are strengths and weakness to each of the dietary methodologies that impact the study
outcomes. Martinez-Mier et al. (2008) conducted a pilot study that compared the results of 3-
day duplicate diets with 3-day diary records for 12 children (ages 18 to 25 months). Adults
(parents and/or caregivers) kept the diaries and collected the food and beverage samples. The 3-
day averages for each child differed for the two approaches with the differences ranging from
0.01 to 0.4 mg F/day. Both approaches suffered from protocol compliance problems, and large
32 December 2010
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variations in daily fluoride intake from both beverages and food were observed between and
within children.
The majority of the published studies that provided estimated oral fluoride intakes from the diet
for this report utilized a market basket approach coupled with recall records collected and
analyzed by the U.S. Departure of Agriculture. The date and title of the USD A study varies and
is provided in the study descriptions that follow. In one case the market basket was developed
from a food frequency recall but it too used food group intake values from USDA. Fewer studies
were identified that used a diary approach or a duplicate diet approach. In one instance the diary
record was used to construct a market basket for analysis.
The study summaries that follow, with the exception of some of the duplicate plate analyses, are
suitable for estimating dietary population intakes of fluoride within the limitations that apply to
the methods described in preceding paragraphs. Where possible, EPA chose to rely most heavily
on studies that obtained the fluoride concentration information from a market basket analysis
because such studies were considered to be more nationally representative than a study based
duplicate diet analyses.
2.5.2. Infants
Each of the studies assessing fluoride intake by infants used a market basket-type approach
where analysis of the fluoride content of foods was combined with estimates of food intake from
a recall, record, or intake recommendation, and measured or assumed drinking water
concentration, in order to arrive at an estimate for fluoride exposure.
Singer and Ophaug (1979) estimated maximum and minimum total fluoride intake of 6-month
old infants on diets prepared with fluoridated water or non-fluoridated water (Table 2-22).
Commercial manufacturers of infant foods provided samples of foods and milk formulations
produced at each of their domestic plants. Each sample was "closely examined for the fluoride
content of the water used in processing it" (actual fluoride concentrations in the processing water
were not reported). The food samples were fixed with magnesium oxide and then ashed. Fluoride
was isolated by diffusion and analyzed with a fluoride ion-specific electrode. Separate samples
were unashed and analyzed for fluoride by a colorimetric technique and an ion-specific
electrode. While the results with the electrode were in good agreement with both ashed and
unashed samples, the colorimetric method gave substantially higher fluoride readings-
presumably due to interfering substances.
Food consumption estimates (milk, formula, and "beikost") were based on the total caloric intake
for six month old infants according to the estimates of Fomon (1975). Beikost is a term that
refers to solid or semi-solid baby foods other than milk or formula. The quantity of each food
consumed was calculated by dividing the caloric intake supplied by each food item (kcal/day) by
average values of caloric density (kcal/gm) as given by Wiatrowski et al. (1975). The total
fluoride intake was calculated using the mean fluoride values for various food groups. In
estimating fluoride intakes, maximum values were based on foods obtained from the plant using
fluoridated water using the assumption that the infant's drinking water would contain 1.0 mg
F/L; minimum intake values were based on data from the non-fluoridated plant using the
assumption that the infant's drinking water would contain only 0.1 mg F/L. For 6-month-old
33 December 2010
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infants (bw 8.1 kg) the minimum fluoride intake was 0.153 mg/day, and the maximum intake
was 0.763 mg/day.
Table 2-22. Fluoride Intake of Infants 6 Months Old (Singer and Ophaug, 1979)
Food Item
Milk formula
Cereals
Fruits
Vegetables
Juices
Meats
Water
Total
Caloric
Intake3
(kcal)/day
444
57
93
62
22
62
740
Food
Consumption
(g)b
663
15
109
138
34
58
120
Maximum Fluoride
Intake0
mg/day
(mg/kg/day)
0.451
0.073
0.006
0.033
0.023
0.057
0.120
0.763 (0.094)
Minimum Fluoride
Intaked
mg/day
(mg/kg/day)
0.020
0.023
0.006
0.033
0.002
0.057
0.012
0.153 (0.019)
SOURCE: Singer and Ophaug, 1979.
"From Fomon, 1975.
bConsumption based on daily caloric intake and the following caloric densities (kcal/g): milk formula, 0.67;
cereals 3.74; fruits, 0.85; vegetables, 0.45; meats, 1.06; and juices, 0.65.
°Mean fluoride content were: milk formulations - 0.68 mg/L; cereal - 4.84 mg/kg, and juices - 0.67 mg/L
processed in plants using fluoridated water, and fruits - 0.051 mg/kg, vegetables - 0.24 mg/kg, meats - 0.99
mg/kg and water -1.0 mg/L.
dMean fluoride content of 1.5 mg/kg for cereal and 0.061 mg/L for juices processed in plants using
nonfluoridated water, and 0.03 mg/L for human or bovine milk , 0.051 mg/L for fruit, 0.24 mg/L, for
vegetables, 0.99 mg/kg for meats, and 0.1 mg/L for water.
Ophaug et al. (1980a) estimated the daily fluoride intake of 6-month-old infants for four
geographic regions of the United States. The study was based on the FDA market basket food
collections for 1977 and 1978. The foods were placed in 11 composite food groups. The
composites were prepared according to Shopping and Compositing Guides representing an
average 14-day consumption of a 6-month-old infant in Orlando, Philadelphia, Grand Rapids,
and Los Angeles. The first three cities reportedly had fluoridated water supplies (1.07 mg/L was
the maximum value reported, which was for Grand Rapids). The fluoride concentration in the
Los Angeles water system at the time of the study was reported to be 0.37 mg/L. The Shopping
and Composite Guides are based on data obtained by the U.S. Department of Agriculture survey
of food consumption made in 1965 to 1966 for each of the geographic regions (USD A, 1968).
The fluoride levels in all composites except one were analyzed by ashing, followed by diffusion
and detection by a fluoride ion-specific electrode. The oils and fats composite was analyzed by
an oxygen bomb reverse extraction procedure (Venkateswarlu, 1975). The total daily fluoride
intake ranged from a high of 0.541 mg/day in Orlando to a low of 0.207 mg/day in Grand Rapids
(Table 2-23). Using an estimated body weight of 8.1 kg for a 6-month-old infant, Ophaug et al.
(1980a) calculated a fluoride intake of 0.026 to 0.067 mg/kg/day.
34
December 2010
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Table 2-23. Fluoride Intake (mg F/day) by Infants 6 Months Old in Four Regions of the U.S.
Food Item
Water
Milk
Other dairy and
formula
Meats, fish,
poultry
Grains/cereals
Potatoes
Vegetables
Fruits/juices
Oils/fats
Sugars, etc.
Beverages
Total
South
(Orlando)
0.295
0.013
0.060
0.024
0.077
0.000
0.026
0.028
-
0.002
0.016
0.541
North central
(Grand Rapids)
0.092
0.015
0.024
0.006
0.011
0.001
0.044
0.014
-
0.000
-
0.207
Northeast
(Philadelphia)
0.077
0.017
0.016
0.009
0.026
0.001
0.057
0.011
0.005
0.008
0.045
0.272
West
(Los Angeles)
0.108
0.007
0.073
0.022
0.102
-
0.021
0.012
-
0.001
0.008
0.354
SOURCE: Ophaug, 1980a.
Ophaug et al. (1985) estimated dietary fluoride intake of 6-month-old infants in 20 cities across
the U.S. The cities were grouped in one of four geographic regions. The survey used the same
market basket and same composite food groupings as those used in the authors' 1980
publication. Fluoride levels were determined with a fluoride ion-specific electrode in all but one
case; fluoride level in oils and fats was determined using the oxygen bomb reverse extraction
procedure. Dietary fluoride intake from each composite was calculated by multiplying its
fluoride content by an estimate of the amount consumed daily. The fluoride content of the
drinking water in the cities where the market baskets were collected ranged from 0.05 to
1.04 mg/L. Specific information on food and drinking water intakes was not reported.
A summary of the estimated fluoride intakes for 6-month-old infants for each of the study sites in
the Ophaug et al. (1985) study is shown in Table 2-24. Fluoride intake for infants was estimated
from an analysis of commercial infant foods processed in fluoridated and non-fluoridated plants.
Within each region total fluoride intake was correlated with water fluoride concentration. The
highest dietary intake of fluoride occurred in the southern region. The daily fluoride intake from
foods (total intake minus that from water and beverages) averaged 0.171 ±0.012 (SE) mg/day
and was not correlated with water fluoride level.
Ophaug et al. (1985) assessed their results by concentration of fluoride in drinking water. The
mean total dietary intake of fluoride (including beverages) for 6-month old infants ranged from
0.226 mg/day where the fluoride level in drinking water was less than 0.3 mg/L to 0.418 mg/day
in areas where the fluoride level was greater than 0.7 mg/L (Table 2-25).
35
December 2010
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Table 2-24. Estimated Fluoride Intake of 6-Month Old Infants in Different Regions of the U.S.
Region/city
(year of sample)
Northeast:
Boston, MA (1980)
Hartford, CT( 1978)
Philadelphia, PA (1977)
Boston, MA (1977)
Manchester, NH (1980)
North Central:
Grand Rapids, WI( 1978)
Akron, OH (1981)
Fargo, ND (1981)
Kansas City, KS (1982)
South:
Louisville, KY (1980)
Chattanooga, TN (1982)
Columbia, SC (1979)
Orlando, FL (1976)
Baton Rouge, LA (1980)
West:
Boise, ID (1979)
Boise ID (1980)
Denver, CO (1977)
Phoenix, AZ( 1982)
Los Angeles, CA( 1977)
Fresno, CA( 1981)
Tacoma,WA(1981
Sacramento, CA( 1980)
OVERALL MEAN
Water F Level
mg/L
1.00
0.93
0.66
0.10
0.10
1.04
1.01
0.91
0.54
1.00
1.00
0.80
0.67
0.30
1.00
1.00
0.71
0.50
0.37
0.10
0.05
0.05
Total F intake
mg/day
0.307
0.369
0.272
0.305
0.220
0.207
0.251
0.178
0.097
0.642
0.650
0.582
0.541
0.265
0.549
0.504
0.456
0.354
0.354
0.239
0.204
0.163
mg/kg
0.038
0.033
0.034
0.038
0.027
0.026
0.031
0.022
0.012
0.079
0.080
0.072
0.068
0.033
0.068
0.062
0.056
0.044
0.044
0.030
0.025
0.020
F Intake in Foods
mg/day
0.130
0.091
0.150
0.227
0.140
0.115
0.162
0.098
0.049
0.164
0.188
0.208
0.230
0.123
0.257
0.210
0.242
0.205
0.238
0.201
0.179
0.147
0.171
SOURCE: Ophaug etal, 1985.
Table 2-25. Mean Dietary Fluoride Intake of 6-Month-Old Infants (Ophaug et al., 1985)
Fluoride
Cone.
<0.3 ppm
0.3-0.7 ppm
>0.7 ppm
n
5
6
11
mg/day
0.2263
0.314
0.4183
SEM
±0.023
±0.059
±0.054
n
5
6
11
mg/kg/day
0.028b
0.039
0.052b
SEM
±0.003
±0.007
±0.007
SOURCE: Ophaug etal., 1985.
Statistically different at p <0.025.
bStatistically different at p <0.025.
Fomon and Ekstrand (1999) estimated fluoride intakes of infants from birth to age 10 months.
Fluoride concentrations in infant foods were derived from an earlier study (Fomon and Ekstrand,
1993b), as were estimates of mean energy intakes for specific age groups (Fomon and Ekstrand,
36
December 2010
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1993a). Fomon and Ekstrand (1999) give an estimate of 120 mL/kg/day for milk or formula
intake by "older infants" (although a specific age range is not given, the implication in the text is
that these are infants 4-10 months old). The study authors note that the older infants would also
be consuming a small amount of beikost (weaning food) which they estimated would increase in
fluoride intake by an average 20 |ig/kg/day in most cases. Estimates of fluoride intake from milk
and formulas only are shown in Table 2-26.
Table 2-26. Estimated Fluoride Intake of 4-10 Month Old Infants with Varying Intakes of Milk or
Formula
Milk/
Formula
Human milk
Cow's milk
Formula:
Ready to feed-milk-based
Cone, liquid-milk-based
Isolated soy protein-based
Powdered milk-based
F Concentration (jig/L)
Formula
200
200
200
240
240
690a
690
690
Water
-
200
1000
200
1000
200
600
1000
As Fed
6
40
200
200
600
270
620
276b
700
980
F Intake (jig/kg/day) for a
Formula Intake of
120 mL/kg/day
1
5
24
24
72
22
74
33
84
118
SOURCE: Fomon and Ekstrand, 1993b; as modified by Fomon and Ekstrand, 1999.
aug/kg of formula powder.
bAssumes that 145 g of formula diluted with 880 mL of water to make 1 liter.
Fomon and Ekstrand (1999) note that infant feeding patterns have changed from the 1960s and
70s to the 1980s and 90s with a trend toward more extended feeding of formula. As a result,
prolonged intake of fluoride from formula became more common. A comparison of infant
fluoride intakes during these two periods for infants from 4 to 10 months old is shown in Table
2-27. The study authors note that the estimates for the 1960s and early 1970's were based on
measurements of fluoride levels in milk and formula made by Fomon and Ekstrand (1993b); and
not on measurements from the 1960s and 1970s, and that values are therefore somewhat less than
would be the case if calculations had been based on concentrations of fluoride in formulas
actually marketed in the 1960s and 1970s.
Table 2-27. Dietary Fluoride Intake of Infants 4-10 Months Old from the 1960s to the 1990s
Diet
Human milk
Infant formula
Cow's milk
1960s-and Early 1970s3
F Intakeb
(jig/kg/day)
-
24-1 18a
5
Estim. % of
Infants
-
<20
>80
1980s and Early 1990s
F Intakeb
(jig/kg/day)
1-37
24-118
5
Estim. % of
Infants
15
55
30
SOURCE: Fomon and Ekstrand, 1999.
aBased on measurements of fluoride levels in milk and formula made by Fomon and Ekstrand (1993); and not on measurements
from the 1960s and 1970s. The study authors note that the values listed are therefore somewhat less than would be the case if
calculations had been based on concentrations of fluoride in formulas actually marketed in the 1960s and 1970s.
'Fluoride intakes by exclusively breast-fed infants do not exceed 1 ug/kg/day; however, many breast-fed infants also receive
formula and the range of intakes in the table includes those of partially breast-fed infants.
37
December 2010
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Using the same assumptions concerning energy intakes of infants and energy equivalents of
infant foods, Fomon et al. (2000) updated the estimates of fluoride intake by infants that were
reported by Fomon and Ekstrand (1999). The study authors also included estimates of fluoride
intake from formulas prepared at home with evaporated milk. These estimates are shown in
Table 2-28.
Table 2-28. Updated Estimated Fluoride Intake of 4-10 Month Old Infants with Varying Intakes of
Milk and Formula (Fomon et al., 2000)
Milk/
Formula
Human milk
Cow's milk
Formulas:
Home prepared evaporated
milk formula3
Ready to feed-milk-based
Cone, liquid-milk-based
Isolated soy protein-based
Powdered milk-based
F Concentration (jig/L)
Formula
90
90
-
200
200
250
250
690b
690b
Water
200
1000
-
200
1000
200
1000
200
1000
As Fed
6
40
155
632
200
200
600
225
625
262C
966C
F Intake (jig/kg/day)
120 mL/kg/day
1
5
19
76
24
24
72
27
75
31
116
aAssumes 0.39L of evaporated milk to 0.57 L of water (also includes formulas made with fresh milk)
Vg/kg of formula powder.
°Assumes that 125 g of formula diluted with 880 mL of water makes 1 liter of formula as fed.
Siew et al. (2009) measured fluoride levels in different types of infant formula (see Table 2-4),
and estimated the daily fluoride intake for age-groups from birth to 12 months. Based on body
weight and formula intake data for male and female infants (Table 2-29), Siew et al. (2009)
reported that female infants would have a slightly greater intake of fluoride than male infants.
Table 2-29. Volume of Formula Consumed and Body Weights from Birth to 12 Months
(Siew et al., 2009)
Age
(months)
0-4
4-6
6-9
9-12
Formula
intake
(ounces)3
21-29
29-32
30-32
24-30
Body weights (kg)
Girls
10th Percent.
2.7-5.2
5.2-6.2
6.2-7.4
7.4-8.3
50th Percent.
3.4-6.2
6.2-7.2
7.2-8.5
8.5-9.5
90th Percent.
4.0-7.1
7.1-8.4
8.4-9.8
9.8-11.0
Boys
10th Percent.
2.8-5.7
5.7-6.8
6.8-8.0
8.0-9.0
50th Percent.
3.6-6.7
6.7-7.9
7.9-9.3
9.3-10.3
90th Percent.
4.2-7.8
7.8-9.2
9.2-10.8
10.8-11.9
SOURCE: Siew et al. 2009.
a Derived from Hendricks and Duggan's Manual of Pediatric Nutrition.
Total fluoride intake for female infants was then calculated from both the amount of fluoride
ingested from the water used to reconstitute the formula (0.0, 0.4, 0.5, 0.7 or 1.0 ppm fluoride)
and from the formula itself. Results showed that the formulas themselves did not contain
fluoride at levels high enough to exceed an intake of 0.10 mg/kg/day with normal consumption.
38
December 2010
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It was estimated that a minimal risk of exceeding 0.1 mg/kg/day would exist with a fluoride
drinking water level of 0.5 ppm. If the drinking water contained 1 ppm fluoride, infants
consuming powdered formula reconstituted with this water would exceed a fluoride intake of 0.1
mg/kg/day. However, it should be recognized that fluoride is a nutrient and reconstitution of
infant formulas with water containing lower levels of fluoride may result in infants not
consuming the Adequate Intake for fluoride (0.5 mg/day) established by the Institute of Medicine
(1997). The American Dental Association (2007) recommends "Parents and caregivers should
consult with their dentist, pediatrician or family physician regarding the most appropriate water
to use in their area to reconstitute infant formula". The ADA (2007) publication informs users of
liquid concentrate or powdered infant formula as the primary source of nutrition that can "be
mixed with water that is fluoride free or contains low levels of fluoride to reduce the risk of
fluorosis".
2.5.3. Children to 14 Years of Age
The fluoride exposure estimates for children up to 14 years of age come from three types of
studies. Most have used the Market Basket approach but there are also two that use dietary
records of beverage intake to estimate the fluoride from beverages only and two that employed a
duplicate plate methodology. The Market Basket-type studies are presented first followed by the
two using the dietary records and then the duplicate plate studies.
Market Basket Studies. Ophaug et al. (1980b) estimated the daily fluoride intake of 2-year-old
children residing in four regions of the United States (Table 2-30).
Table 2-30. Fluoride Intake (mg F/day) by Children 2 Years Old in Four Regions of the U.S.
Food Item
Water
Milk
Other dairy and formula
Meats, fish, poultry
Grains/cereals
Potatoes
Vegetables
Fruits/juices
Oils/fats
Sugars, etc.
Beverages
Totals (mg/day)
(mg/kg/day)
South
(Orlando)
0.274
0.009
0.005
0.060
0.023
0.001
0.016
0.021
0.004
0.008
0.133
0.554
0.044
North central
(Grand Rapids)
0.302
0.011
0.013
0.051
0.042
0.005
0.011
0.042
0.008
0.014
0.111
0.610
0.049
Northeast
(Philadelphia)
0.206
0.011
0.011
0.057
0.029
0.004
0.016
0.020
0.002
0.008
0.046
0.410
0.033
West
(Los Angeles)
0.136
0.010
0.006
0.023
0.055
0.006
0.016
0.020
0.002
0.010
0.031
0.315
0.025
SOURCE: Ophaug, 1980b.
This study was identical in methodology to that conducted by Ophaug et al. (1980a) for 6-month-
old infants, but was based on the FDA toddler market basket food collections for 1977 and 1978.
39
December 2010
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The foods were placed in the same 11 composite food groups according to Shopping and
Compositing Guides representing an average 14-day consumption of 2-year-old children. The
Shopping and Composite Guides were based on data obtained by the U.S. Department of
Agriculture survey of food consumption made in 1965 to 1966 for each of the geographic
regions. The fluoride levels in all composites except one were analyzed by ashing, followed by
diffusion and detection by a fluoride ion-specific electrode. The oils and fats composite was
analyzed by an oxygen bomb reverse extraction procedure (Venkateswarlu, 1975). The total
daily fluoride intake ranged from a low of 0.315 mg/day for Los Angeles to a high of 0.610
mg/day for Grand Rapids. The intake per unit body weight ranged from 0.025 mg/kg/day to
0.049 mg/kg/day.
Ophaug et al. (1985) continued the studies of Ophaug et al. (1980b) by evaluating dietary
fluoride intake of 2-year-old children in 20 cities across the U.S. (Table 2-31).
Table 2-31. Dietary Fluoride Intake of an Average 2-Year-Old Child
City (year of sample)
Water F Level
(mg/L)
Total F intake
(mg/day)
(mg/kg)
Foods
(mg/day)
Northeast:
Boston, MA (1980)
Hartford, CT (1978)
Philadelphia, PA (1977)
Boston, MA (1977)
Manchester, NH (1979)
1.00
0.93
0.66
0.10
0.10
0.475
0.507
0.410
0.348
0.182
0.038
0.041
0.033
0.028
0.014
0.125
0.141
0.158
0.314
0.132
North Central:
Grand Rapids, WI (1978)
Akron, OH (1981)
Fargo, ND (1981)
Kansas City, KS (1982)
1.04
1.01
0.91
0.54
0.607
0.682
0.504
0.376
0.049
0.055
0.040
0.040
0.194
0.190
0.155
0.150
South:
Louisville, KY (1980)
Chattanooga, TN (1982)
Columbia, SC (1979)
Orlando, FL (1976)
Baton Rouge, LA (1980)
1.00
1.00
0.80
0.67
0.30
0.880
0.784
0.718
0.554
0.310
0.070
0.063
0.057
0.044
0.025
0.150
0.191
0.211
0.147
0.107
West:
Boise, ID (1979)
Boise ID (1980)
Denver, CO (1977)
Phoenix, AZ (1982)
Los Angeles, CA (1977)
Fresno, CA (1981)
Tacoma, WA (1981
Sacramento, CA (1980)
OVERALL MEAN
1.00
1.00
0.71
0.50
0.37
0.10
0.05
0.05
0.537
0.568
0.566
0.350
0.315
0.197
0.162
0.146
0.043
0.045
0.045
0.028
0.025
0.016
0.013
0.012
0.127
0.173
0.244
0.138
0.148
0.144
0.116
0.124
0.163
SOURCE: Ophaug etal., 1985.
40
December 2010
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This study was based on FDA market food basket collections obtained during 1977-1982. The
methodology was the same as that described above. The fluoride content of the drinking water
in the cities where the market baskets were collected ranged from 0.05 to 1.04 mg/L. A
summary of the fluoride intakes is given in Table 2-31. Fluoride dietary intake was highly
correlated with water fluoride level with correlation coefficients > 0.72. The highest dietary
intake occurred in the southern region, and was reported to be a reflection of greater
consumption of water and beverages (551 g/day vs. 383-426 g/day in the other regions). The
daily fluoride intake from foods (total intake minus that from water and beverages) averaged
0.161±0.010 (SE) mg/day, and was not correlated with water fluoride level.
Mean total dietary intakes (including beverages) based on fluoride levels in drinking water are
shown in Table 2-32. Mean fluoride intake increased with increase in fluoride concentration in
drinking water.
Table 2-32. Mean Dietary Fluoride Intake of 2-Year-Olds
Fluoride Concentration in
Drinking Water
<0.3 ppm
0.3-0.7 ppm
>0.7 ppm
n
5
6
11
mg/day
0.207b'c
0.386a'c
0.62 la'b
SEM
±0.036
±0.037
±0.039
n
5
6
11
mg/kg/day
0.017e'f
0.03 ld'f
O.OSO46
SEM
±0.003
±0.003
±0.003
SOURCE: Ophaug etal., 1985.
"Statistically different at the p <0.0025.
bStatistically different at the p <0.0005.
"Statistically different at the p <0.005.
Statistically different at the p <0.0025.
"Statistically different at the p <0.0005.
^Statistically different at the p <0.005.
Dabeka and McKenzie (1995) surveyed fluoride levels in various foods obtained in 1987 in
Winnipeg, Canada. The foods were prepared for consumption and combined into 113
composites and 39 composite subsets using a Total Diet Study approach. The water used to
prepare the foods contained 1 mg F/L. Fluoride was determined with a fluoride ion-specific
electrode after microdiffusion. As reported in Dabeka et al. (1993), food intake data
(g/person/day) for each of food composites was obtained from the Nutrition Canada Survey
(Bureau of Nutritional Sciences, 1977) for the age groups of 1-4, 5-11, and 12-19 yr. Total
dietary intake of fluoride (excluding plain drinking water) was estimated to be 0.353 mg/day for
boys and girls 1-4 years old; 0.530 mg/day for boys and girls 5-11 years old; 1.025 mg/day for
boys 12-19 years old; and 0.905 mg/day for girls 12-19 years old.
The fluoride content of 441 brand-name food items purchased in both a non-fluoridated
community (Connersville, IN, fluoride 0.16 ±0.01 mg F/L) and in a fluoridated community
(Richmond, IN, 0.90 ±0.05 mg F/L) (see Section 3.1.2) were evaluated by Jackson et al. (2002).
A modified validated Food Frequency Questionnaire was administered to determine the 75 foods
and beverages most commonly eaten by adolescents (ages 12-14) in these communities.
Frequency of ingestion was weighted from 1 for less than monthly to 9 for two or more times per
day. Parents of the children were interviewed to determine the outcome of the Frequency Recall
and asked to identify the brand names of the foods and beverages most often purchased. Food
samples were purchased in each community (grocery stores and restaurants) and prepared using
41
December 2010
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community water in cases where preparation was necessary. Foods were grouped for analysis
based on the USDA classification (1998). [Note: According to USDA (1998), the beverages
group excludes plain water and noncarbonated bottled water]. Homogenates of each food group
were analyzed for their fluoride content and used to estimate exposure for 3-5 year old children.
Mean fluoride intakes were derived from the fluoride content of each food group homogenate
using age and gender-specific mean food intakes from the Midwest regional data from the USDA
(1998) CSFII survey (Table 2-33). Mean fluoride intake was 0.454 mg/day in Connersville, IN
and 0.536 mg in Richmond, IN (Note: fluoride intake from consumption of drinking water was
not included in the calculation).
Table 2-33. Estimated Fluoride Intake of 3- to 5-Year-Old Children Living in a Nonfluoridated and
Fluoridated Community
Food Category
Grains and cereal
products
Vegetables
Fruits
Dairy Products
Meat, poultry
Nuts and seeds
Fats and oils
Sugars and sweets
Beverages0
Total
Food
intake
(g/day)a
264
90
213
387
64d
5
5
45
291
1010
Connersville, IN (F = 0.16 mg/L)
F Content
(Mg/g)b
0.44
0.26
0.13
0.35
0.35
0.14
0.24
0.24
0.40
F Intake
(Mg/day) b
116.16
23.40
27.69
135.45
22.40
0.70
1.20
10.80
116.40
454.20
Richmond, IN (F = 0.9 mg/L)
F Content
(ng/g)b
0.55
0.28
0.11
0.28
0.37
0.18
0.25
0.35
0.66
F Intake
(Mg/day) b
145.20
25.20
23.43
108.36
23.68
0.90
1.25
15.75
192.06
535.83
SOURCE: Jackson et al., 2002.
aUSDA, 1998.
'Mean values.
"Plain drinking water is not included in the category according to USDA (1998).
dUSDA (1998) lists 99 grams/day for this age group for the mid-west region of the US; however, in Jackson et al. (2002) it is
given as 64 grams/day.
Since the USDA (1998) percentile intake distributions for food groups were not available to the
researchers, an upper bound estimate of fluoride intake was calculated using the mean intake and
the 90th percentile data for fluoride concentration in each food group. Jackson et al. (2002)
calculated that the upper bound fluoride intake would be 0.925 mg/day (0.058 mg/kg/day) in
Connersville and 0.999 mg/day (0.062 mg/kg/day) in Richmond.
Jackson et al. (2002) determined exposure data only for the 3-5 year old age group because of
their vulnerability to dental fluorosis. However, because the food frequency recall data that
supported the market baskets were collected from adolescents, the analytical data on fluoride
levels in the food groups can be combined with food group intake information from USDA
(1998) to provide estimates for the 6-11 and 12-19 year age groups. Tables 2-34 and 2-35
42
December 2010
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below provide the results of these calculations for Connersville and Richmond. The extrapolated
estimates for both age groups are supported by the results from the Dabeka and McKenzie
(1995) Canadian Study.
Table 2-34. Estimated Fluoride Intake of 6 to 11 and 12 to 19 Year Olds Living in a Nonfluoridated
Community
Food Category"
Grains/cereal products
Vegetables
Fruits
Dairy Products
Meat, poultry
Nuts and seeds
Fats and oils
Sugars and sweets
BEVERAGES6
Mean
F Content
(Mg/g)b
0.44
0.26
0.13
0.35
0.35
0.14
0.24
0.24
0.40
6-11 yrolds
(average for males and females
Food intake0
(g/day)
309
119
163.5
435
139.5
5
8.5
53
407.5
TOTAL F INTAKE
F INTAKE FROM FOOD [(Total) - (beverages)]
Fluoride Intaked
(Hg/day)
136
31.0
21.3
152.3
48.8
0.7
2.0
12.7
163
567.9
404.8
12-19 yr olds
(average for males and females)
Food Intake0
(g/day)
363
170.5
144.5
403.5
227
3
11.5
42.5
959.5
Fluoride Intaked
(jig/day)
159.7
44.3
18.8
141.2
79.5
0.4
2.8
10.2
383.7
840.7
457
aFood categories of eggs and legumes are listed in USDA (1998), but are not included in Jackson et al. (2002)
kMean values (Jackson et al., 2002).
°USDA (1998; survey data from 1994-1996; mean food intake values).
dFluoride intake calculated as fluoride concentration in food category (|ig/g) multiplied by food intake (g/day).
ePlain drinking water is not included in the beverage category according to USDA (1998).
Dietary Record Studies. Three-day beverage records of Grade 6 children (average age 11.94
yr) in two towns in Canada were used to document daily means of the highest and lowest
fluoride intake from beverages (Clovis and Hargreaves, 1988). The study was conducted in a
town with a fluoridated water supply (average adjusted fluoride concentration of 1.08 mg/L) and
in one without fluoride added to the water (0.23 mg F/L). The three highest and three lowest
beverage intakes (including drinking water) were used to estimate the range of fluoride intakes in
the two communities. In the nonfluoridated community, the probable fluoride intake ranged
from 0.00-0.03 mg from milk, 0.02-0.43 mg from water, 0.08-0.69 mg from carbonated
beverages; 0.01-0.14 mg from reconstituted juices; and 0.08-0.09 mg from other types of drinks.
The total fluoride intake from beverages ranged from 0.02 to 0.82 mg. For the fluoridated
community, the probable fluoride intake ranged from 0.00-0.05 mg from milk, 0.07-0.25 mg
from water, 0.1-0.93 mg from carbonated beverages; 0.21-0.35 mg from reconstituted juices;
and 0.07-1.76 mg from other types of drinks. The total fluoride intake from beverages ranged
from 0.40 to 2.45 mg.
43
December 2010
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Table 2-35. Estimated Fluoride Intake of 6 to 11 and 12 to 19 Year Old Children Living in a Fluoridated
Community
Food Category"
Grains/cereal products
Vegetables
Fruits
Dairy products
Meat, poultry
Nuts and seeds
Fats and oils
Sugars and sweets
BEVERAGES6
Mean
F Content
(ng/g)b
0.55
0.28
0.11
0.28
0.37
0.18
0.25
0.35
0.66
6-11 yrolds
(average for males and females)
Food intake0
(g/day)
309
119
163.5
435
139.5
5
8.5
53
407.5
TOTAL F INTAKE
F INTAKE FROM FOOD [(Total) - (beverages)]
Fluoride
Intaked
(jig/day)
170.0
33.3
18.0
121.8
51.6
0.9
2.1
18.6
269.0
685.3
416.3
12-19 yr olds
(average for males/females)
Food
Intake0
(g/day)
363
170.5
144.5
403.5
227
3
11.5
42.5
959.5
Fluoride Intaked
(jig/day)
199.7
47.7
15.9
113.0
84.0
0.5
2.9
14.9
633.3
1111.9
478.6
aFood categories of eggs and legumes are listed in USDA (1998), but are not included in Jackson et al. (2002)
bMean values (Jackson et al., 2002).
°USDA (1998; survey data from 1994-1996; mean food intake values).
dFluoride intake calculated as fluoride concentration in food category (|ig/g) multiplied by food intake (g/day).
ePlain drinking water is not included in the beverage category according to USDA (1998).
Pang et al. (1992) studied fluoride intake of 225 children, ages 2-10 years, living in North
Carolina. Data on beverage intake was collected by means of three-day diary records kept
during April, May or June, 1990. Concentrated fruit juices, fruit drinks, and teas were prepared
with deionized water. Total fluid intake was 970-1,240 mL/day, and consumption of soft drinks,
juices, tea, and other beverages 585-756 mL/day. Of the total fluid consumption, milk and water
constituted 36-40%. Fluoride was determined by the microdiffusion method and a fluoride ion-
specific electrode. Fluoride concentrations in the beverages ranged from nondetectible to 6.7
mg/L; mean concentrations were 0.74 mg/L for soda, 0.36 mg/L for juices, 0.33 mg/L for
punches, 2.56 mg/L for teas, and 0.85 mg/L for Gatorade. The estimated average fluoride intake
(±SD) from beverages (excluding milk, plain water and beverages listed less than five times in
the diaries) for children ages 2-3, 4-6, and 7-10 years were 0.36±0.31, 0.54±0.52, and
0.60±0.48 mg/day, respectively. The maximum fluoride intakes for individual children within
these groups were 1.40, 2.39, and 2.00 mg/day, respectively. The study authors note that
fluoride levels were high in grape juice (maximum 1.6 ppm) and also in teas (mostly 2-3 ppm,
and with a maximum of 6.5 ppm).
Levy et al. (2003a) estimated an average fluoride intake of 0.2 mg/day from beverages, not
including plain drinking water, for 785 three to six year olds. Parents were asked to periodically
44
December 2010
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complete modified food frequency questionnaires which assessed numbers and sizes of daily
servings of different categories of beverages and foods made with water.
There was no direct verification of the data reported by the parents in the questionnaires. The
90th percentile estimate was about 0.5 mg/day.
Duplicate Diet/Plate Analyses. Rojas-Sanchez et al. (1999) estimated fluoride intakes from
foods and beverages (and dentifrice) consumed by children (16-40 months old; about 1.3 to 3.3
years old) living in three different communities using a duplicate plate methodology. The three
communities differed in the fluoride concentration of their water supply: 1) a low-fluoride
community (San Juan, Puerto Rico; <0.3 mg F/L); 2) a fluoridated community (Indianapolis, IN,
0.8-1.2 mg F/L); and 3) a "halo" community (Connersville, IN, <0.3 mg F/L) in the distribution
region for Indianapolis). All participating children were required to be healthy, attend a
certified, commercial-, community- or church-based day-care center on a full-time basis, and
have parental consent and cooperation. The day-care water source was required to have a
fluoride concentration similar to the community water supply. Duplicate plate samples of all
foods consumed (after visual adjustment for plate waste) on one or two day-care days and one
weekend home day were collected and conglomerated for analysis. Beverages were kept
separate from solid foods.
Water samples were analyzed for fluoride using a combined fluoride ion-specific electrode and
pH/ion meter calibrated with a series of standards. Food samples were analyzed for fluoride
using the HMDS-microdiffusion method of Taves (1968b) as modified by Dunipace et al.
(1995). All samples were analyzed in duplicate, and the reliability of measurements was
determined using the Intraclass Correlation Coefficient, the values of which were estimated from
the variance components of an ANOVA model. Mean fluoride intake from food was 0.116-
0.146 mg/day (Table 2-36) with no significant difference between communities. Intake from
beverages (including drinking water) was estimated to be 0.103, 0.257, and 0.396 mg/day for the
low-fluoride, halo, and fluoridated communities; differences between the towns were statistically
significant (p < 0.05) as determined by one-way ANOVA. Based on mean values, total dietary
fluoride intake (including drinking water) was 0.219 mg/day in San Juan, 0.389 mg/day in
Connersville, and 0.544 mg/day in Indianapolis.
Table 2-36. Dietary Fluoride Intake of 16-40 Month Old Children
City
San Juan, PR
Connersville, IN
Indianapolis, IN
FinDW
<0.3 mg/L
<0.3 mg/L
0.8-1.2 mg/L
N
11
14
29
F Intake" from
Foods
(Mg/day)
116±24b
132±16b
146±17b
F Intake" from
Beverages
(Mg/day)
103±22C
257±59C
396±52C
Total Dietary F
Intake
(jig/day)d
219
389
542
SOURCE: Rojas-Sanchez et al., 1999.
aMean±SEM.
''Not significantly different from each other (p > 0.05; one-way ANOVA).
"Significantly different, p < 0.05.
dTotal of mean values.
Using a duplicate plate method, Brunetti and Newbrun (1983), evaluated the fluoride dietary
intake and output of a group of 10 children (4 boys and 6 girls) ages 3 and 4 years, living in an
45
December 2010
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optimally fluoridated community (study location and fluoride concentration in drinking water not
reported). The diet of the children was unrestricted except that they were not allowed to chew
gum. Duplicates of all food and fluid served and any leftovers by each child were collected and
pooled every 24 hr. Intake was measured by subtracting leftovers from food served. Samples
were assayed for fluoride using a diffusion method. The reported average dietary intake of
fluoride was 0.33 (±0.14) mg F/day (food and beverage). Fluoride output (assumed to be based
on urinary excretion) was reported to be 0.28 (±0.08) mg F/day.
2.5.4. Older Children and Adults
Exposure estimates for older children and adults are based on market basket and duplicate-plate
types of studies. As was the case in Sections 2.5.2 and 2.5.3, the data from Market Basket-type
analyses are presented first. Summaries that utilized the duplicate plate-type of approach follow.
Market Basket Studies. San Filippo and Battistone (1971) calculated the fluoride content of
representative diets of 16-19 year-old males. Food items were obtained in Baltimore, MD from
a market basket program conducted by the FDA on four separate occasions in 1967 and 1968.
The food items were purchased in local supermarkets and prepared "in a manner representative
of preparation at home" using the local fluoridated water. The food items for a two-week period
were weighed to the nearest gram (wet weight) and then separated into 12 commodity groups.
The commodity groups were homogenized and analyzed on a composite basis using
microdiffusion and a colorimetric analysis. For most groups, the final values were averages of
triplicate analyses. Results are shown in Table 2-37. Analysis of the Baltimore water supply
indicated that the fluoride level ranged from 0.99 to 1.1 mg/L.
The daily contribution of each commodity group was an average of the two-week content. The
data indicated an average total daily intake of 2.09-2.34 mg fluoride. Beverages contributed
61% to the total (1.28-1.46 mg/day), and all other food stuffs including those prepared with milk
or water contributed 39% (0.78-0.9 mg/day). San Filippo and Battistone (1971) note that in their
study the fluoride intake from the food ranged from 0.8 to 0.9 mg/day, an increase of about 0.5
mg over the intake from areas containing low fluoride in the drinking water reported in other
studies (McClure, 1949 and Cholak, 1959).
Singer et al. (1980) evaluated the total daily dietary fluoride intake of 16-19 year-old males
living in four geographic regions of the United States. Fluoride content of FDA composite
"market basket collections" made in 1975 and 1977 were used in the analysis (USFDA, 1977).
Food collections consisted of 117 items placed in 12 composite groups. The diets were based on
Department of Agriculture (USDA, 1968, 1972) regional food consumption surveys. Fluoride in
the food items was determined for ashed and unashed samples using ion-specific electrode and
colorimetric (eriochromecyanine R) procedures. Total daily dietary fluoride intake, excluding
drinking water (see Singer et. al., 1985), ranged from 0.912 mg in Kansas City to 1.720 mg in
Atlanta (Table 2-38). Average and total mean fluoride intake for all four cities combined is
1.211 mg/kg/day (Table 2-39). Beverages contributed 65% of the total.
46 December 2010
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Table 2-37. Fluoride Content of Four Two-week Representative Diets for Teens 16-19 Years Old
Commodity
Group
Dairy
Meats, fish, poultry
Grain and cereal
products
Potatoes
Leafy vegetables
Legume vegetables
Root vegetables
Garden fruits
Fruits
Oils, fats and
shortening
Sugar, salt, candy
Beverages: tea,
coffee, soft drinks,
water
Totals
Diet #1
mgF
/2wk
2.47
2.03
3.06
0.34
0.52
0.28
0.09
1.11
0.43
1.27
0.53
20.38
32.51
mgF
/day
0.18
0.15
0.22
0.02
0.04
0.02
0.01
0.08
0.03
0.09
0.04
1.46
2.34
Diet #2
mgF
/2wk
2.66
4.20
2.77
0.49
0.37
0.14
0.05
0.19
0.50
0.34
0.83
17.89
30.43
mgF
/day
0.19
0.30
0.20
0.04
0.03
0.01
0.01
0.01
0.04
0.02
0.06
1.28
2.18
Diet #3
mgF
/2wk
1.86
4.38
1.64
0.49
0.34
0.18
0.07
0.14
0.56
0.36
0.92
18.31
29.25
mgF
/day
0.13
0.31
0.12
0.04
0.02
0.01
0.01
0.01
0.04
0.03
0.07
1.31
2.09
Diet #4
mgF
/2wk
1.34
1.52
4.09
1.32
0.94
0.28
0.27
0.45
0.49
0.18
0.68
18.51
30.07
mgF
/day
0.10
0.11
0.29
0.09
0.07
0.02
0.02
0.03
0.04
0.01
0.05
1.32
2.15
SOURCE: SanFilippo and Battistone, 1971.
Table 2-38. Average Daily Fluoride Intake of 16-19 Year Olds Residing in Four Cities
Commodity
Group
Dairy
Meats, fish, poultry
Grain and cereal products
Potatoes
Leafy vegetables
Legume vegetables
Root vegetables
Misc. vegetables
Fruits
Oils, fats
Sugars, adjuncts
Beverages
Totals"
San Francisco,
CA
mg F/day
0.035
0.058
0.138
0.022
0.007
0.011
0.003
0.011
0.013
0.017
0.018
0.882
1.215
Buffalo, NY
mg F/day
0.039
0.058
0.167
0.013
0.007
0.017
0.004
0.011
0.031
0.011
0.020
0.610
0.988
Atlanta, GA
mg F/day
0.052
0.239
0.168
0.021
0.009
0.032
0.003
0.011
0.015
0.011
0.026
1.133
1.720
Kansas City, KS
mg F/day
0.040
0.084
0.126
0.022
0.005
0.023
0.003
0.013
0.013
0.011
0.028
0.544
0.912
SOURCE: Singer etal., 1980.
aSinger et al., 1985, state that the total daily fluoride intake reported in Singer et al., 1980, did not include fluoride ingested in
drinking water.
47
December 2010
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Table 2-39. Daily Fluoride Intake Based on Composite Diets
Category
Dairy products
Meat, fish and poultry
Grains and cereal products
Potatoes
Leafy vegetables
Legume vegetables
Root vegetables
Garden Fruits
Fruits
Oils and fats
Sugars, etc.
Beverages
Total Intake
Fluoride Intake (nig/day)
Mean
0.042
0.110
0.150
0.020
0.007
0.021
0.003
0.012
0.018
0.013
0.023
0.792
1.211
SD
0.007
0.087
0.021
0.004
0.002
0.009
0.001
0.001
0.009
0.003
0.005
0.270
SOURCE: Singer etal., 1980.
In a continuation of the studies of Singer et al. (1980), Singer et al. (1985) utilized 24 FDA
market basket collections made between 1975 and 1982 to again evaluate total daily fluoride
intake of 15-19 year-olds living in the same four geographic regions of the United States. Food
collections (24 "market baskets") consisted of 117 items placed in the same 12 composite
groups. The diets used by Singer et al. (1985) were based on the USDA's Food Consumption
Surveys of 1968 and 1972, and the USFDA (1977) Compliance Program Guidance Manual,
extrapolated to reflect the Recommended Daily Allowance (RDA) for the average young adult
male (2800 kcal). Fluoride in the composites was determined on diffusates of ashed samples
with a fluoride ion-specific electrode.
Total fluoride intake ranged from 0.46 to 2.04 mg/day in eight cities in the West; 0.93 to 2.45
mg/day for four cities in the South; 0.80 to 1.92 mg/day for four cities in the North Central part
of the country; and 1.47 to 1.94 mg/day for 3 cities in the North East. Singer et al. (1985)
separated their data on the basis of the fluoride level in the municipal drinking water of each city
to determine the impact of fluoride concentration in tap water on total fluoride intake
(Table 2-40). Foods, exclusive of beverages and drinking water, contributed a mean fluoride
intake of 0.27-0.37 mg/day (overall mean 0.33 mg/day). Singer et al. (1985) noted that a basal
diet in a nonfluoridated region of the United States contained 0.43 mg of fluoride as reported by
Maheshwari etal., 1981.
48
December 2010
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Table 2-40. Average Daily Fluoride Intake (mg/day) of 16-19 Year Olds
Commodity
Group
Total dietary
Beverages and
Water
Food only
Fluoride Concentration of Municipal Water
< 0.3 mg/L
(0.14 ±0.03)a
(n = 5)b
0.86 ±0.14
0.59 ±0.12
0.27 ±0.03
0.3-0.7 mg/L
(0.56 ±0.05)a
(n = ll)b
1.39 ±0.13
1.06 ±0.11
0.33 ±0.03
>0.7 mg/L
(1.04 ±0.05)a
(n = 8)b
1.85 ±0.11
1.48 ±0.08
0.37 ±0.05
<0.1 to 1.3 mg/L
(n =24)b
NR
NR
0.33 ±0.02
SOURCE: Singer etal., 1985.
NR. Not reported.
aMean F concentration ±SEM.
'Number of market baskets.
Based on a 6-day survey of a regular hospital diets (location not specifically mentioned, but
presumed to be in the Rochester, NY area, as the affiliation of the researchers was the University
of Rochester), and using information on fluoride levels in 93 foods and beverages (see Section
2.2.2), Taves (1983) calculated a mean total daily fluoride intake of 1.783 mg, of which 1.383
mg (78%) was provided by beverages (Table 2-41). Tea was the major contributor to the intake
from beverages. The author notes that drinking water was not taken into account in the study, but
that the tap water used in the preparation of the hospital foods was fluoridated. The fluoride
level in the tap water was not reported.
Table 2-41. Daily Fluoride Intake based on 6-day Hospital Diets
Category
Dairy Products
Meat, fish and poultry
Grains and cereal products
Potatoes
Leafy vegetables
Legume vegetables
Root vegetables
Garden Fruits
Fruits
Oils and fats
Sugars, etc.
Beverages
Total Intake
Fluoride Intake (mg/day)
Mean
0.013
0.044
0.241
0.018
0.027
0.037
0.010
0.000
0.006
0.003
0.001
1.383
1.783
SD
0.000
0.035
0.153
NR
0.019
NR
NR
NR
NR
0.001
0.000
0.041
SOURCE: Taves, 1983.
NR, Not reported
49
December 2010
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Dabeka and McKenzie (1995) surveyed fluoride levels in various foods obtained in 1987 in
Winnipeg, Canada. The foods were prepared for consumption and combined into 113
composites and 39 composite subsets using a Total Diet Study approach. The concentration of
fluoride in tapwater was reported to be 1 mg/L. Fluoride was determined with a fluoride ion-
specific electrode after microdiffusion. As reported in Dabeka et al. (1993), food intake data
(g/person/day) for each of composites was obtained from the Nutrition Canada Survey (Bureau
of Nutritional Sciences, 1977) for the age groups of 1-4, 5-11, and 12-19, and 20+ years. Total
dietary fluoride intake was 1.025 mg/day for 12-19 yr old males and 0.905 mg/day for 12-19
year old females. For the age groups of 20+ years, the fluoride intake ranged from 2.17 to 3.03
mg/day. Over all ages (including the 20+ yr groups) and both sexes, the estimated average
dietary intake of fluoride was 1.76 mg/day; the food category contributing most to the estimated
intake was beverages (80%).
Duplicate Diet/Plate Methods. The fluoride content of the strictly controlled metabolic diets
that were used over a six-year period at a VA hospital in the Chicago area during 1967-72 were
analyzed by Osis et al. (1974b). The house diets served to patients in the same hospital were also
analyzed using the same approach. Fluoride concentrations were determined by the diffusion
method of Singer and Armstrong (1965) with spectrophotometric analysis. Osis et al. (1974a)
reported a coefficient of variation of 4.3% for this method. The daily intake of fluoride of
individuals on the metabolic diet, as shown in Table 2-42, averaged 1.56-1.91 mg/day. During
the course of the study, fluoridation of the tap water was temporarily discontinued. As a result, it
was possible for the study authors to compare the fluoride content of the general hospital diet
when "non-fluoridated" water (0.27 mg F/L) was used in the preparation of meals with that
prepared with fluoridated water (about 0.9 mg F/L). The results, shown in Table 2-43, indicate
that the average fluoride intake was reduced more than 50% when the "nonfluoridated" water
was used in the preparation of the meals.
Table 2-42. Fluoride Intake of Individuals on a Metabolic Diet over a Six- Year Period
Year
1967
1968
1969
1970
1971
1972
Average ±SD (mg/day)a
1.91 ±0.42
1.60 ±0.15
1.56 ±0.18
1.76 ±0.15
1.74 ±0.16
1.60 ±0.15
Range
1.47-3.08
1.26-1.83
1.21-2.30
1.46-2.06
1.28-2.07
1.33-1.88
SOURCE: Osis etal.,1974b.
aWater used in the preparation of the meals contained about 0.9 mg/L fluoride.
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Table 2-43. Fluoride Intake from a General Hospital Diet Prepared with and without Fluoridated Water
Meal
No.
Average ±SD
(mg/day)
Range
Diet prepared with fluoridated water"
Breakfast
Lunch
Dinner
Total F (mg/day)b
5
5
5
0.65 ±0.17
0.75 ±0.28
0.57 ±0.15
1.96 ±0.48
0.47-0.86
0.42-1.16
0.34-0.71
1.23-2.41
Diet prepared with non-fluoridated water0
Breakfast
Lunch
Dinner
Total F (mg/day)b
5
5
5
0.29 ±0.06
0.32 ±0.06
0.25 ±0.02
0.86 ±0.08
0.21-0.37
0.25-0.37
0.22-0.27
0.73-0.94
SOURCE: Osis et al., 1974b.
aWater used in the preparation of the meals contained 0.9 mg F/L.
bThe total daily dietary fluoride represents the range from the lowest to the highest intakes per day, and does not represent the
sum of the individual meals listed.
"Water used in the preparation of the meals contained about 0.27 mg F/L.
Kramer et al. (1974) analyzed the fluoride content of diets obtained from hospitals in 16 cities in
the United States, 12 cities where the drinking water was fluoridated and 4 cities where the
drinking water was not fluoridated (Table 2-44). The diets were normal in composition and
provided 2,400 to 2,600 kcal/day. Most of the diets were collected as separate, individual meals,
breakfast, lunch and dinner; although in some cases the food items making up the diet for the
entire day were obtained. The compositions of each individual meal and of the total diet were
determined. Beverages, including coffee and tea, were included, but not plain drinking water.
Fluoride was analyzed by the method of Singer and Armstrong (1965). Dietary fluoride was
lowest in those communities having the lowest fluoride levels in drinking water. The mean
fluoride content of the diet was generally greater in fluoridated areas than in nonfluoridated
areas, however, there was not a linear relationship between the fluoride concentration of the
drinking water supply and that of the diet. The highest level of dietary fluoride was that for a
community with a 0.6 mg/L fluoride concentration, not the system with the highest drinking
water fluoride concentration (1.27 mg/L).
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Table 2-44. Dietary Fluoride Intake in Sixteen U.S. Cities
City
Birmingham, AL
Iron Mountain, MI
Chicago, IL
Houston, TX
Durham, NC
Corvallis, OR
Tuscaloosa, AL
Martinez, CA
Milwaukee, WI
New York, NY
St. Louis, MO
Chicago, IL
Madison, WI
Louisville, KY
Lexington, KY
Cleveland, OH
F in Drinking water
(mg/L)
0.08
0.08
0.33
0.44
0.53
0.60
0.76
0.81
0.85
0.88
0.91
0.95
1.11
1.14
1.15
1.27
Daily Dietary F Intake
(mg)
0.78
1.03
0.86a
0.95
2.62
3.44
2.94
1.73
3.41
2.55
2.10
1.97
2.88
1.98
2.84
3.05
SOURCE: Kramer etal., 1974.
aAverage of five diets analyzed at a time when the water was not fluoridated.
2.5.5. Combined Exposure Estimates for Age Groups of Concern
The OW has used the dietary exposure data to estimate fluoride intakes for the age groups
identified in the OW dose-response assessment (U.S. EPA, 2010a). The data summarized in
Table 2-45 come from the U.S. assessments discussed in Section 2.5.2 through 2.5.4 that were
based on analytical data from foods and TDS or duplicate diet estimates. Table 2-45 does not
include intake from drinking water or the beverage grouping where possible. The beverage data
are summarized in Table 2-46. Study conditions are described in the notes field of the table.
Evaluation of the food and exposure data support several conclusions related to fluoride intake
via the diet.
The use of fluoridated water in processing and preparing food increases the fluoride
content of the diet for both home prepared and commercial foods but not in predictable
linear fashion (Maier and Rose, 1966; Ophaug et al., 1985).
The relationship between the fluoride in local tap water and intake from beverages
displays a linear relationship (> 0.72 correlation coefficient; Ophaug et al., 1985).
Analytical methods influence the results. The older colorimetric methods appear to be
less reliable than more recent methods (Singer at al., 1980).
52
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Concentration of fluoride appears to be related to food group as follows: protein foods >
grains and vegetables, > fruits, > beverages.
Table 2-45. Summary of Daily Dietary Fluoride Intakes for Age Groups of Concern
Age
years
0.5 -<1
l-<4
4-<7
7-14
Fluoride
Exposure
Estimate
(mg/day)
0.171 ±0.012
0.161 ±0.010
0.1 16 ±0.024
0.132 ±0.016
0.146 ±0.017
0.33 ±0.14
0.33 ±0.14
0.338
0.344
0.35
0.405
0.83
0.424
0.33
0.403
Notes
Ophaug et al., 1985 - Overall mean of 44 market baskets, and national food intake
data; does not include F from water and beverages; 6 months old age group.
Ophaug et al., 1985 - Overall mean of 22 market baskets, and national food intake
data; does not include water and beverages; 2 years old age group.
Rojas-Sanchez et al., 1999 - Duplicate plate analysis (n=54; mean ±SEM ) for three
cities; excludes beverages and drinking water (<0.3 mg F/L DW in 2 cities and 0.8-1 .2
mg F/L DW in the third); 1 .3-3.3 year old age group.
Brunetti andNewbrunn, 1983 - Duplicate plate analysis (n=10, for 1-4 days); estimate
for all foods and fluids consumed 3-4 year old age group
Brunetti andNewbrunn, 1983 - Duplicate plate analysis (n=10, for 1-4 days); estimate
for all foods and fluids consumed; 3-4 year old age group.
Jackson et al. , 2002 - Analysis of 75 most commonly consumed foods and beverages
of 12-14 yr olds placed in 9 composites and USDA food consumption data for 3-5
year olds. Does not include water and beverages; 0. 16 mg F/L DW; fluoridated water
concentration 0. 16 mg/L.
Jackson et al. , 2002 - Analysis of 75 most commonly consumed foods and beverages
of 12-14 yr olds placed in 9 composites and USDA food consumption data for 3-5
year olds. Does not include water and beverages; fluoridated water concentration 0.9
mg/L
No U.S. data for age group. The estimate is based on the analytical food group
fluoride data from Jackson et al., (2002) and USDA data on food group intakes for 6-
1 1 year olds. Does not include water and beverages; fluoridated water concentration
0.9 mg/L.
No U.S. data for age group. The estimate is based on the analytical food group
fluoride data from Jackson et al., (2002) and USDA data on food group intakes for 12-
19 year olds. Does not include water and beverages; fluoridated water concentration
0.9 mg/L
San Filippo and Battistone, 1 971 - Four market baskets, and FDA food intake data;
does not include water and beverages; 16-19 years old.
Singer et al., 1980. Market baskets from 4 regions of the country; beverages and plain
drinking water not included; 16-19 years old.
Singer et al., 1985. 24 market baskets from different areas of the country; beverages
and plain drinking water not included; 16-19 years old.
Taves, 1983 - Six-day hospital diet; does not include beverages and plain drinking
water; Adults.
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Table 2-46. Estimates of Daily Dietary Fluoride from Beverages for Age Groups of Concern
Age
(yr)
0.5- <1
0.5-1
l-<4
4-<7
7-14
Fluoride
Exposure
Estimate
(mg/day)
0.14(mg/L)
0.09-0.12
0.36 ±0.31
0.257 ±0.059
0.396 ±0.052
0.54 ±0.52
0.116
0.192
0.2
0.60±0.48
0.216
0.509
1.34
0.792
0.59
1.383 ±0.041
Notes
Van Winkle et al., 1995. Concentration for powdered formula prepared with distilled
water.
Siew et al. 2009. Estimates (from graphical presentation of data) of range of fluoride
intake from powdered formula prepared with distilled water, based on estimates of
formula intake for female infants 6 to 12 months old.
Pang et al., 1992 - Three-day drink diaries (n=57); beverages only, excluding milk,
water and those listed fewer than five times; home-prepared beverages made with de-
ionized water; 2-3 years old.
Rojas-Sanchez et al., 1999 - Duplicate plate study (n=14; mean ±SEM); beverages
and drinking water; <0.3 mg F/L DW; 1.3-3.3 years old.
Rojas-Sanchez et al., 1999 - Duplicate plate study (n=29; mean ±SEM); beverages
and drinking water; 0.8 mg F/L DW; 1.3-3.3 years old.
Pang et al., 1992 - Three-day drink diaries (n=79); beverages only, excluding milk,
water and those listed fewer than five times; home-prepared beverages made with de-
ionized water; 4-6 years old.
Jackson et al. , 2002 - Analysis of 75 most commonly consumed foods and beverages
of 12-14 yr olds placed in 9 composites and USDA food consumption data for 3-5 yr
olds; beverages only, plain DW not included; low F location (0.16 mg/L); 3-5 years
old.
Jackson et al. , 2002 - Analysis of 75 most commonly consumed foods and beverages
of 12-14 yr olds placed in 9 composites and USDA food consumption data for 3-5 yr
olds; beverages only, plain drinking water not included; fluoridated location (0.9
mg/L); 3-5 years old.
Levy et al., 2003a. Estimate of average intake from beverages, not including plain
drinking water for 3-6 year olds derived from questionnaires completed by the parents
and historical data on fluoride concentrations in the beverages. The 90th percentile
estimate was 0.5 mg/day.
Pang et al., 1992 - Three-day drink diaries (n=89); beverages only, excluding milk,
water and those listed fewer than five times; home-prepared beverages made with de-
ionized water; 7-10 years old.
This estimate is based on the means from two market baskets in the study by Jackson
et al. (2002) and USDA data on beverage intakes. It does not include drinking water.
Ages 6-11.
This estimate is based on the means from two market baskets in the study by Jackson
et al. (2002) and USDA data on beverage intakes. It does not include drinking water.
Ages 12-19. It is supported by the average (0.51 mg/L) from a Canadian dietary
record survey by Clovis and Hargreaves (1988); (range 0.02-0.82 mg/day).
San Filippo and Battistone, 1971 - Four market baskets, and FDA intake data;
includes beverages and plain drinking water; 16-19 years old.
Singer et al., 1980. Market baskets from 4 regions of the country 16-1 9 years old.
Singer et al., 1985. 5 Market baskets from different areas of the country; plain
drinking water not included. Drinking water used to prepare beverages low in
fluoride (0.14 mg/L ± 0.03); 15-19 years old.
Taves, 1983 - beverages; does not including plain drinking water; derived from a
duplicate plate hospital study; adults.
The U. S. EPA assessment of dose-response for severe dental fluorosis (U.S. EPA, 2010a)
divided the population into age groups that correlate with those used in the Ershow and Cantor
(1989) analysis of drinking water intakes because they represented the water intake data that
54
December 2010
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were closest (1977-1978) to those likely to have occurred at the time of the Dean (1942)
publication. The age groupings reported in the published papers summarized above are not
always congruent with those used by EPA (2010a). For this reason Tables 2-45 and 2-46 array
the published data according to the age groups used for the dose-response assessment. As a
result, each study was placed according to its best fit with the drinking water age groups.
Except for Brunetti and Newbrun (1983), Table 2-45 on intakes from solid foods does not
include intakes from beverages. Milk and fruit juices are included in the solid foods grouping
because of their placement in a market basket survey in the dairy and fruit groups, respectively.
Table 2-46 is a summary of the data reported for other beverages as a separate market basket
item. In Table 2-46, no attempt was made to separate fluoride that may have originated from
local tap water used in making tea, coffee or powdered juice drinks from the commercial
beverages. Two of the studies (Pang et al., 1992; Van Winkle et al., 1995) used deionized water
in the home preparation of beverages.
There is variability in the results reported for the fluoride in beverages with Pang et al. (1992)
generally reporting higher levels for the 4 to <7 year old group and the 7 to < 11 year old group
than other studies. The Pang et al. (1992) study used a record keeping approach (3-days) to
determining the kinds and amounts of beverages consumed by children in North Carolina in
April, May and June. The ages of the participants, diary approach, location (southern U.S.), and
time of year (Spring and early Summer) could have influenced these results.
In order to refine the fluoride estimate from beverage ingestion, EPA examined the list of market
basket foods and their categories in the 1990 and 2003 FDA market basket lists (Egan, 2009).
Most fruit juices were included in the fruit rather than the beverage group. The beverage group
included carbonated beverages, coffee, tea products reconstituted or prepared using tap water,
and alcoholic beverages. Based on information obtained from FDA, beverages containing
commercial water contributed 53 to 74 % of the total mass intake from the beverage category in
the TDS based on the 1987-1988 CSFII and 65 to 77 % for the TDS based on the 1994-1998
CSFII (bottled water and alcoholic beverages excluded) for the age groups of interest. The
remainder would be contributed by the indirect use of tap water explaining the strong correlation
between local levels in drinking water and the market basket results for beverages. In general,
the commercial water contribution to a market basket beverage intake increases with age (Egan,
Personal Communication, 2009). This is consistent with the higher intakes of carbonated and
other commercial beverages by the older age groups.
The San Filippo and Battistone (1971) results for those >14 include plain drinking water but are
similar to the Taves (1983) results which do not. However, Taves (1983) explains that the
hospital diets studied included orange juice, coffee, and two servings of tea on a daily basis as
well as other juices. The analytical data from the Taves (1983) study show that the tea was the
major contributor to the fluoride from beverages. For that reason the Singer et al. (1980, 1985)
results are considered to be more representative of the general population when plain drinking
water is excluded.
55 December 2010
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2.5.6. Fluoride Exposures from Sulfuryl Fluoride Use
At the request of the Office of Water, OPP (U.S. EPA, 2009, 201 Ob) provided estimates of
exposures to fluoride from the tolerances granted to sulfuryl fluoride (SuF in Table 2-47). The
OPP data were generated using the DEEM exposure program that integrates residue data from
representative commodities with age-specific food group intakes from CSFII (1998). Exposure
estimates were provided by age group and whether the residues were the result of fumigation of
food storage facilities or fumigation of food processing structures (U.S. EPA, 201 Ob).
Table 2-47. Summary of Pesticidal Fluoride Contributions to Dietary Fluoride Exposure
Population Group
0.5-1 year
Children l-<4yrs
Children 4-<7 yrs
Children 7-14
Exposure Estimates, mg/day
SuF Structural
Fumigations
0.0087
0.0121
0.0153
0.0170
0.0182
0.0187
SuF Food
Fumigations
0.0213
0.0329
0.0466
0.0544
0.0675
0.0576
Total
0.0300
0.0450
0.0619
0.0714
0.0857
0.0763
SOURCE: U.S. EPA, 2010b
The age groups generated by the OPP exposure assessment (U.S. EPA, 201 Ob) are congruent
with those used by OW for this report. OPP (U.S. EPA, 2010b) also reported the exposure
estimates in terms of mg/day. The 11 to <14 year age group appears to have the highest
estimated total exposure from sulfuryl fluoride residues.
56
December 2010
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3. Exposure from Drinking Water
Fluoride occurs naturally in water. Levels in drinking water can range from insignificant to
unacceptably high depending on the water source and the extent of treatment. In many locations
where the fluoride levels are naturally low, fluoride is intentionally added to water supply
systems to reduce the occurrence and severity of dental caries in children. Community water
fluoridation at a concentration of about 1 ppm was initiated in 1945 (Ripa, 1993). Based on data
collected in 1999 from 24 locations nation-wide, Miller-Ihli et al. (2003) concluded that 40% of
the U.S. water supplies were fluoridated (mean concentration 1.01±0.15 mg/L). Currently CDC
(2008) records indicate that about 69% of the population obtains its water from systems that
fluoridate.
3.1. Analytical Methods
Methods used to analyze for fluoride in drinking water have changed over time. In the 1930s
and early 1940s, colorimetric methods required visual comparison of the color of samples with a
set of standard solutions to identify the fluoride concentration in the sample. In the Elvove
(1933) method, water samples were acidified with hydrochloric acid and mixed with a dye
complex such as zirconium oxychloride and alizarin sodium monosulphonate mixed to produce a
colored solution from binding of the fluoride with the reagent. A series of solutions containing
varying known amounts of sodium fluoride are mixed with the reagent to produce a series of
colored standards. The test samples were then visually compared to the standards (in "Nessler"
tubes) to estimate the concentration by a match of the sample color with that of the color of the
closest standard. Elvove (1933) reported that as little as 0.01 mg of fluorine in 50 cc, or 0.2
mg/L could be differentiated from a corresponding control with this method. This method was
used by Dean (1942) in evaluating the fluoride content in water supplies of 22 U.S. cities. The
Dean (1942) report states that the sensitivity of the analytical method was about 0.1 mg/L. The
Dean (1942) study is the basis of the dose-response assessment for severe dental fluorosis in U.S.
EPA(2010a).
The Elvove (1933) colorimetric method is subject to error caused by interfering substances such
as sulfate, chloride, bicarbonate, iron, manganese, and aluminum when these substances exceed
specific concentrations. Nevertheless, colorimetric methods for fluoride determination are still
considered Standard methods today, albeit using spectrophotometric instrumentation and
standard curves for determining concentrations.
The most recent standard colorimetric methods employ two reagents related to those used by
Elvove (1933). One employs an acidic reagent containing zirconyl chloride and the complexing
agent SPADNS [sodium 2-(parasulfophenylazo)-l, 8-dihydroxy-3, 6-naphthalene disulfonate]
(APHA/AWWA/WEF, 2005). The other employs both alizarin and lanthanum nitrate to form a
blue complex in an automated system.
In the mid-1960s a fluoride ion-specific electrode was developed which allowed direct detection
and measurement of fluoride concentrations in water by means of a potentiometer (see Section
2.1.3 for further discussion). The concentration of the fluoride ion was in direct proportion to the
current generated. Compared to colorimetric methods, the fluoride ion-specific electrode
exhibits superior selectivity when challenged with chloride, chlorine, color and turbidity, iron,
57 December 2010
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phosphate, sulfate, and aluminum (StandardMethods, APHA/AWWA/WEF, 2005). Standard
Methods clearly indicates the electrode and colorimetric methods are most satisfactory
Ion-specific chromatography can also be used to analyze fluoride in aqueous solution, and
although this method has a high level of sensitivity and specificity for fluoride, it has only rarely
been used in the studies discussed in this report.
3.2. Natural Sources
Drinking water can be obtained from non-fluoridated municipal systems, private wells, cisterns,
springs, or from bottled water. The fluoride levels in these sources may vary considerably
depending on the source, time of year, and the level of treatment. Certain geological formations
are rich in fluoride-containing minerals from which fluoride can leach into surrounding
groundwater or surface water. According to Fleischer et al. (1974), some groundwaters average
as much as 8 ppm of fluoride or more. Groundwater from the Wilcox Basin in Southeastern
Arizona can contain up to 282 ppm fluoride (Kister et al., 1966). Most water from this basin is
used primarily for irrigation. However, it is also the water source for several public drinking
water systems (Towne and Freark, 2001).
Fluoride levels in groundwater in the coterminous United States were mapped by the U.S.
Geological Survey (see Figure 3-1). Some of the areas indicated in Figure 3-1 correspond to
areas of aridity as shown in Figure 3-2 (McGinnies et al., 1968). In these areas drinking water
consumption rates may be greater than average, and combined with the high levels of fluoride in
groundwater, may contribute to higher than normal exposures to fluoride from private drinking
water systems and more frequent exceedences of the SMCL. States that have reported MCL
violations most frequently to the Safe Drinking Water Information System - Federal
(SDWIS/FED) during the period from 1998 to 2006 are Arizona, Florida, Montana, New
Mexico, Texas and Virginia. All states have some areas with high levels of geological fluoride.
In 1993, the CDC reported on naturally occurring fluoride levels in U.S. water sources.
Although there is a range in fluoride concentrations within each state, in most cases the
maximum reported concentrations correspond fairly well with the areas predicted to have high
levels of fluoride in groundwater (Fig. 3-1). According to CDC (1993), maximum
concentrations of 7 mg/L or greater were reported for Arizona, Colorado, Idaho, Iowa, Montana,
New Mexico, North Dakota, Oklahoma, and Texas. Seventeen states had maximum
concentrations exceeding 4.0 mg/L, and 32 states had maximum concentrations >2.0 mg/L in
some localities. In most cases only a small proportion of the total sampled population was
located in areas where the fluoride levels were high. The CDC (1993) estimated that of the
approximately 10 million people in the U.S. with naturally fluoridated public drinking water,
approximately 67% had fluoride concentrations of < 1.2 mg/L; about 14% had concentrations of
1.3-1.9 mg/L; 14% had concentrations of 2.0-3.9 mg/L and 2% had levels of >4.0 mg/L.
Due to the differences in groundwater fluoride, private water sources (particularly well-water)
are likely to have highly variable fluoride concentrations. Felsenfeld and Roberts (1991)
reported one case of fluoride-associated osteosclerosis in an individual whose drinking water
well had an average concentration of about 8 mg F/L.
58 December 2010
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EXPLANATION
^H1 5 PPm F or highu
1.0-1 4 ppmF
05-0 9 ppm F
0-04 ppm F
I NO dam
Figure 3-1. Fluoride Levels in Groundwater in the U.S. (Fleischer et al., 1974).
semi arid
arid
hyperarid
Figure 3-2. Arid Regions in the U.S. (McGinnies et al., 1968).
59
December 2010
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3.3. Public Drinking Water Systems
Public drinking water systems are required to monitor finished water for fluoride on defined
schedules determined by whether or not the level detected exceeds the MCL, and to report the
results to the state. If there is no exceedence of the MCL, surface water systems monitor once a
year while groundwater systems monitor only once every three years unless granted a waiver by
States to further reduce monitoring. The monitoring identifies whether or not there has been an
exceedence of the MCL and SMCL. Exceedences are reported to consumers in their required
yearly drinking water quality Consumer Confidence Report and trigger a return to quarterly
monitoring. When the yearly average fluoride concentration exceeds the MCL (4 mg/L) the
Consumer Confidence Report is required to include the following language regarding health
effects:
Some people who drink water containing fluoride in excess of the MCL over many
years could get bone disease, including pain and tenderness of the bones.
Fluoride in drinking water at half the MCL or more may cause mottling of teeth,
usually in children less than nine years old. Mottling, also known as dental
fluorosis, may include brown staining and/or pitting of the teeth and occurs only
in developing teeth before they erupt from the gums. (40CFR141, subpart O, App.
A).
In cases where the yearly average fluoride concentration exceeds the SMCL (2 mg/L), the
following message must be sent to consumers within 12 months of the exceedence. This can be
accomplished by including the warning in the annual Consumer Confidence Report. Exceedence
of the SMCL is more frequent than exceedence of the MCL; ground water systems are affected
to a greater extent than surface water systems. Exceeding the SMCL does not require a return to
quarterly monitoring.
This is a notification about your drinking water and a cosmetic dental problem
that might affect children under nine years of age. At low levels fluoride can help
prevent cavities, but children drinking water containing more than 2 mg/L of
fluoride may develop cosmetic discoloration of their permanent teeth (dental
fluorosis). The drinking water provided by your community water system [name]
has a fluoride concentration of [insert number] mg/L.
Dental fluorosis, in its moderate or severe forms, may result in brown staining or
pitting of the permanent teeth. This problem occurs only in developing teeth
before they erupt from the gums. Children under nine should be provided with
alternative sources of drinking water or water that has been treated to remove the
fluoride to avoid the possibility of staining and pitting of the permanent teeth.
You may also want to contact your dentist about proper use by young children of
fluoride-containing products. Older children and adults may safely drink the
water.
Drinking water containing more than 4 mg/L fluoride (the U.S. Environmental
Protection Agency's drinking water standard) can increase your risk of
developing bone disease. Your drinking water does not contain more than 4 mg/L
60 December 2010
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fluoride, but we are required to notify you when we discover fluoride levels in
your drinking water that exceed 2 mg/L because of this cosmetic dental problem.
(40CFR141.208).
In conjunction with the second six-year review of the National Primary Drinking Water
Regulations, EPA conducted an Information Collection Request (ICR). Through this process
EPA asked that all States and primacy entities voluntarily submit their SDWA compliance
monitoring data. This request was for the submission of compliance monitoring data collected
between January 1998 and December 2005 for 79 regulated contaminants. A total of 52 States
and entities provided compliance monitoring data that included all analytical detection and non-
detection records. These data represent the national occurrence of regulated contaminants in
public drinking water systems. Through extensive data management efforts, quality assurance
evaluations, and communications with State data management staff, EPA established a high
quality dependable contaminant occurrence database consisting of data from 46 States. Details
of the data management and data quality assurance evaluations are available in the supporting
document (U.S. EPA, 2008b).
The contaminant occurrence data from the States and entities comprise more than 17 million
analytical records from approximately 136,000 public water systems. Approximately 265
million people are served by these public water systems nationally. The number of States and
public water systems represented in the data set varies across contaminants because of variability
in voluntary State data submissions and contaminant monitoring schedules. This is the largest,
most comprehensive set of drinking water compliance monitoring data ever compiled and
analyzed by EPA.
EPA used a two-stage analytical approach to analyze these data and characterize the national
occurrence of contaminants. The first stage of analysis provides a straightforward evaluation of
contaminant occurrence. This stage is a simple, non-parametric count of occurrence for
regulated contaminants in public water systems. A typical stage 1 occurrence analysis generates
a count of the number (or percentage) of systems with at least one analytical detection of a
specific contaminant at a concentration above the concentration of interest (i.e., the SMCL).
This approach generates a conservative (i.e., upwardly biased) estimate of the number of
potential systems having contaminant occurrence at levels of interest. It is the appropriate metric
for a contaminant such as fluoride where intakes above the threshold of concern over even a
limited period of time can have an impact on the development of enamel on the secondary teeth
forming only during the time of the exposure.
ICR data for fluoride were examined on the basis of all samples and all systems as well as for
only those systems that reported at least one sample with a concentration >2 mg/L during the 8-
year reporting period. The results are summarized in Tables 3-1 and 3-2, and include
conservative estimates of the total populations exposed during the monitoring period. According
to information extracted from the U.S. Census Bureau's web site, there were 60.3 million
children under the age 14 in the U.S. in 2010, approximately 21.4% of the total U.S. population.
The period from 6 months to 14 years is the age period for enamel formation for secondary teeth,
including the third molars (Massler and Schour, 1958).
61 December 2010
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The data set for fluoride included some entries with apparent unit discrepancies. Fluoride
concentrations were designated as mg/L values but appear to have actually been ug/L values
based on the other reported measures from the same utility. If the actual levels were truly mg/L
measures, the high fluoride concentrations would have caused adverse effects among the
exposed population (gastrointestinal irritation; see NRC, 2006 for review).
Values for detections reported as < 0.002 mg/L and greater than 40 mg/L were considered as
outliers and eliminated from the analysis. Values reported as greater than 20 mg/L are also
suspect based on historic records for the United States, but have been included in the analysis
presented in Tables 3-1 and 3-2. A total of 426 entries were considered as anomalously high and
eliminated from the analysis; six values between 40 and 100 mg/L and 420 values equal to or
greater than 100 mg/L.
The ICR data set also included results from some transient noncommunity systems. The Agency
excluded these samples from the analysis presented in Tables 3-1 and 3-2 because federal
fluoride regulations do not apply. The Agency also excluded all samples that could be identified
as source water quality samples that do not represent water quality at the entry point to the
distribution system (e.g., water quality prior to treatment or fluoridation). The data in Tables 3-1
and 3-2 also do not include samples reporting fluoride as not detected in the determination of
mean, median and 90th percentile values. There are variations in the number of samples and
systems across the monitoring period. These variations reflect differences in the monitoring
schedule and the number of States providing data. Systems that fluoridate are required to report
fluoride levels monthly to the appropriate organization within their state (often the state dental
officer) but have no obligation to report those monthly measurements to EPA.
The number of quarterly samples analyzed over the 8 years of monitoring ranged from about
7,000 to 12,000, with 2.3 to 5.6 % of these samples > 2 mg/L. Monitoring data were analyzed
for four quarters per year, but the data have been compressed in Table 3-1 and 3-2 to show only
the range across the four quarters. The systems reporting each quarter are not consistent because
surface water systems with mean average annual concentrations below 4 mg/L have to report
only once per year or once every three years for a groundwater system.
Table 3-1 suggests the possibility of a trend towards an increase in the percent of samples with
detections of 2 mg/L or higher across the 8-year monitoring period. In the first 4 years the
percent of detections for the subset > 2 mg/L exceeded 4% for two of the 16 quarters. In the
second 4 years, the frequency increased to all 16 quarters. The percent of systems reporting a
concentration of >2 mg/L ranged from 4.1 % to 5.6 % in the first four years of monitoring and
4.6% to 8.3% in the second four years. Close inspection of the ICR results indicates that the
apparent trend was the result of an increase in the number of states included in the data set. The
later years include states with high geological levels of fluoride (Florida, Texas, and Virginia)
that did not submit data for the early years of the monitoring period.
The mean, median, and 90th percentile concentrations were determined for each of the
monitoring quarters. Over the first four years of monitoring the high end of the range for the
mean was 0.85 or 0.86 mg/L while in the second 4 years it increased to a maximum of 0.95
mg/L. In the last four years, the range for the means is consistently higher than that for the
medians reflecting positively skewed distribution (i.e., having a longer right tail with higher F
62 December 2010
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concentrations). A similar trend is reflected in the 90th percentile values, which have also
increased over the 8 years of monitoring. The means and medians remain at a concentration
within the recommended range for fluoridation and the 90th percentile value, although
consistently above the upper end of the fluoridation range, never exceeded the 2 mg/L SMCL.
The average quarterly mean for the 8 years reported is 0.85 mg/L and that for the 2002-2005
period is 0.87 mg/L. The corresponding average quarterly 90l percentile values are 1.39 mg/L
and 1.43 mg/L, respectively.
Table 3-2 represents only the systems that were at 2 mg/L or higher for at least one quarter
during the eight year monitoring period. In parallel with the pattern observed in Table 3-1, Table
3-2 shows that the number of systems that measure a concentration of 2 mg/L or above in a given
year is increasing from around 500 in the early years of the ICR time span to above 800 in the
last two years. This too reflects an increase in the number of states reporting. The samples from
systems that have reported levels > 2 mg/L come from 26 to 46% of the systems in each quarter.
This difference between the percent of systems affected and percent of samples can reflect
sampling at multiple entry points for the system or the taking of a second sample for
confirmation of the original result. It is important to remember when looking at the percent data,
that the reporting of a value of >2 mg/L does not require a system to begin monitoring on a
quarterly basis. The system can maintain their yearly or triennial monitoring schedule, but are
required to report the exceedence of the SMCL in their consumer confidence report. Some
systems may increase their monitoring for fluoride when the concentration reaches 2 mg/L.
In examining the mean and median of the concentrations reported by the systems that had at least
1 sample with a concentration of 2 mg/L or higher, all of the median values are still within the
fluoridation range, while all of the means lie above the fluoridation range but are lower than the
SMCL. The ranges for the 90th percentile values are consistently above the SMCL but below
the MCL. For the last four years of the ICR monitoring (2001-2005) the average quarterly
fluoride concentration was 1.76 mg F/L and the 90th percentile value was 3.84 mg F/L. Over the
ICR reporting period from 1.8 million to 6.4 million individuals could have been exposed in a
given year to a concentration of 2 mg/L or higher for at least a short period of time. It is not
possible to estimate how many of these individuals may have been exposed during a period of
vulnerability for severe dental fluorosis.
62 December 2010
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Table 3-1. Public Water System Monitoring Data 1998-2005
Ranges Across Quarterly Data in Each Year; Nondetect Values Not Included in Samples, Mean, Median and 90th Percentile
Year
Samples
% samples
>2mg/L
Systems
% systems
>2mg/L
Mean (mg/L)a
Median
(mg/L)a
90th percentile
(mg/L)a
Population
1998
6,566 - 7,288
3. 2% -3. 6%
3,263 - 3,973
4.8% - 5.6%
0.81-0.85
0.83-0.86
1.32-1.36
40,455,048 -
52,890,715
1999
6,783-6,991
2.8% -3.0%
3,134-3,322
4.5% - 4.9%
0.83-0.85
0.88-0.92
1.34-1.37
41,810,370 -
70,262,253
2000
6,990 - 8,049
2.7% -3. 3%
3,489 - 3,873
4.1% -4.7%
0.82-0.86
0.87-0.90
1.30-1.38
43,543,007 -
70,200,938
2001
6,559 - 8,961
3.1% -4.5%
3,972 - 4,480
4.5% - 5.5%
0.81-0.86
0.77 - 0.87
1.33 - 1.40
45,062,700 -
82,331,386
2002
6,126-8,295
4.0% -5.1%
3,541-4,563
4.6% - 5.8%
0.78-0.89
0.70-0.85
1.40 - 1.44
50,333,719-
82,609,244
2003
6,910-8,562
5.2% - 6.2%
4,054-4,981
6.1% -7.2%
0.86-0.93
0.80-0.85
1.40-1.47
44,398,104-
87,126,153
2004
8,231-9,580
4.9% - 6.4%
5,007 - 5,700
5.6% - 7.7%
0.80-0.90
0.69-0.80
1.40-1.50
47,726,060 -
86,715,548
2005
7,051-9,635
5.4% - 6.8%
3,869 - 5,472
6.9% - 8.3%
0.84-0.95
0.75 - 0.86
1.40-1.50
58,824,170 -
102,533,400
SOURCE: The monitoring data used in this analysis were collected through information collection request for EPA's second Six-Year Review under the provisions of the
Paperwork Reduction Act, 44 U.S.C. 3501 et seq.; Office of Management and Budget (OMB) control number 2040-0275.
aMean, median and 90th percentile based on all detections (modal minimum reporting level (MRL) = 0.1 mg/L).
-------
Table 3-2. A Summary of Public Water System Fluoride Monitoring Data from Systems for Systems with at Least One Detection of 2 mg/L or
Higher during the Year of Monitoring
Ranges Across Quarterly Data in Each Year; Nondetect Values Not Included in the Sample, Mean, Median and 90th Percentile
Year
Samples from systems
that ever had a
detection > 2 mg/L
% samples with at least
one detection >2 mg/L
Systems that ever had a
detection > 2 mg/L
% systems with at least
one detection>2 mg/L
Mean (mg/L)
Median (mg/L)
90th percentile (mg/L)
Population-served by
systems that ever had a
detection > 2 mg/L
1998
1,380-1,513
15. 3% -17.4%
499 - 563
32.3% -36.9%
1.27-1.43
1.05-1.10
2.40-2.65
2,513,263-
3,887,873
1999
1,372-1,494
13. 3% -14.7%
528 - 549
26.5% -29.5%
1.32-1.37
1.10-1.10
2.20 - 2.40
1,864,149-
4,703,418
2000
1,432-1,527
14.5% -
16.5%
541 - 586
27.3% -
32.0%
1.32-1.43
1.10-1.11
2.21-2.46
2,429,353 -
3,215,929
2001
1,225-1,762
16.4%-
24.0%
563 - 656
31.4%-
36.3%
1.33-1.60
1.10-1.20
2.60-3.10
3,088,021 -
4,450,151
2002
1,138-1,473
24.9% -27.5%
579 - 668
32.3% -35.6%
1.60-1.69
1.20-1.29
3.10-3.40
3,563,761 -
5,402,152
2003
1,409-1,603
29.6% -3 1.8%
687 - 763
40.5% - 44.3%
1.75-1.84
1.20-1.30
3.80-4.39
3,820,278 -
4,793,365
2004
1,557-
1,951
27.7% -
33.9%
756 - 843
42.3%-
48.3%
1.65-1.86
1.15-1.30
3.70-4.18
3,849,780 -
5,242,650
2005
1,521 -
1,713
30.5% -
31.8%
754 - 822
42.6% -
45.9%
1.73-1.86
1.20-1.23
3.90-4.24
4,326,194-
6,405,661
SOURCE: The monitoring data used in this analysis were collected through information collection request for EPA's second Six-Year Review under the provisions of the
Paperwork Reduction Act, 44 U.S.C. 3501 et seq.; Office of Management and Budget (OMB) control number 2040-0275.
aMean, median and 90th percentile based on only detections from systems that ever had a sample detection of 2 mg/L or higher (modal minimum reporting level (MRL) = 0.1
mg/L).
-------
3.4. Fluoridation Contributions
The U.S. Public Health Service (CDC, 1995) recommends that fluoride levels in municipal
drinking water be maintained in the range of 0.7 to 1.2 mg/L. The exact level is determined by
the annual average of maximum daily ambient air temperatures (Table 3-3). The linkage
between fluoridation levels and ambient air temperatures was based on the hypothesis that
drinking water intake is increased in areas with warmer climates requiring less fluoride in the
water to achieve the same average population dose.
Table 3-3. CDC Recommendations for Optimal Fluoride Concentrations in Public Water Supply
Systems
Annual Average of Maximum Daily Air
Temperatures"
50.0-53.7°F
53.8-58.3°F
58.4-63. 8°F
63.9-70.6°F
70.7-79.2°F
79.3-90.5°F
Community Water Systems
Fluoride Concentration
(mg/L)
1.2
1.1
1.0
0.9
0.8
0.7
SOURCE: Adapted from CDC, 1995.
aBased on 5 years of temperature data.
In the past, school drinking water fluoridation programs targeted areas where the municipal
water was not fluoridated (naturally or intentionally). CDC (2001) updated the school
fluoridation recommendation because of the widespread use of fluoride toothpaste and,
availability of other fluoride-treatment modalities that can be delivered in the school setting.
CDC (2001) recommends that decisions to initiate or continue school fluoridation programs be
based on an assessment of present caries risk in the target school(s) and alternative preventive
modalities that might be available accompanied by periodic evaluation of program effectiveness.
Several studies have indicated that current drinking water consumption rates may not be as
affected by climatic conditions as they once were thought to be, suggesting that the temperature-
related guidelines for fluoride concentrations in drinking water may need to be reevaluated
(NRC, 2006). Heller et al. (1999) examined drinking water intake estimates documented in the
1994-1996 CSFII and compared these data to information from the 1977-78 Nationwide Food
Consumption Survey and found no "obvious strong or consistent association between water
intake and month or season."
Using 24-hr recall data from the third National Health and Nutrition Examination Survey
(NHANES III, 1988-1994), Sohn et al. (2001), reported that for children aged 1-10 years there
was no significant relationship (based on multiple regression analysis) between total fluid intake
or plain water intake and mean daily maximum temperature, either before or after controlling for
sex, age, socioeconomic status, and race or ethnicity. Fluid intake was significantly associated
with age, sex, socioeconomic status, and race and ethnicity. Estimates of total fluoride intake
and plain water intake by geographic region are shown in Table 3-4. However, the NHANES
survey was designed to avoid interviewing people in extremely hot or cold weather conditions.
66 December 2010
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This could be a limitation on the applicability of results from this analysis to the entire U. S.
population. The mean maximum temperatures used in the analysis (based on the average of
daily maximum temperatures during 1960-1990 for the survey month) ranged from 53.4°F to
89.3°F. The majority of temperatures were distributed within the range of 65.0° to 85°F.
Table 3-4. Estimated Daily Fluid and Plain Water Regional Intake in Children 1-10 Years Old
Region
Northeast
Midwest
South
West
No.
679
699
869
1,622
Total Fluid Intakeb
mL/day±SE
1,734.8 ±30.7
1,734.4 ±45.3
1,739.4 ±31.2
1,737.4 ±24.5a
mL/kg/day±SE
86.9 ±2.3
83.7 ±1.5
83.2 ±2.2
81.1 ±1.7
Plain Water Intake
mL/day±SE
568.2 ±52.1
639.7 ±53.8
612.9 ±24.1
624.4 ±44.2
mL/kg/day±SE
26.4±2.1
28.9 ±1.8
27.6 ±1.3
27.0 ±1.9
SOURCE: Sohn et al., 2001; NHANES III, 1988-1994.
aA value of 734.4 is given in Sohn et al., 2001; however, based on the consumption per unit body weight, it appears that this
data point should actually be 1,737.4 mL/day, as shown here.
It should be noted that the CDC recommendations for temperature-dependent optimal fluoride
concentrations in municipal drinking water are still in effect (CDC, 1995) but are an issue of
current interest as indicated by Heller et al. (1999) and Sohn et al. (2001). NRC (2006) and CDC
(2001) have also recommended a reevaluation of the ambient air temperature-based guidelines.
3.5. Bottled Water
Fluoride content of bottled water varies considerably with brand, source, and time of packaging.
Nowak and Nowak (1989) analyzed the fluoride content of 19 types of bottled water obtained in
the Iowa City area using a fluoride ion-specific electrode and found that the F concentration
ranged from 0.004 to 0.33 mg/L. Chan et al. (1990) analyzed the fluoride content of twenty-two
types of bottled water originating from nine different regions of the US and three regions of
France. Eighteen of the samples had fluoride levels below 0.3 mg/L; and the highest fluoride
level was 0.79 mg/L. Stannard et al. (1990) tested 24 brands of domestic and imported bottled
waters for fluoride using an ion-specific electrode. The fluoride levels ranged from a trace
amount (two samples less than 0.1 mg/L) to 1.25 mg/L. The average was calculated to be 0.33
mg/L, assuming the two samples to have 0 mg/L fluoride.
Among 78 commercially available bottled waters sampled in Iowa, Van Winkle et al. (1995)
found that fluoride levels ranged from 0.2 mg/L to 1.36 mg/L with a mean of 0.18 mg/L; 83%
ranged from 0.02 to 0.16 mg/L, 7% from 0.34 to 0.56 mg/L, 1% had a fluoride level of 0.88
mg/L and 9% had levels >1 mg/L. Van Winkle et al. (1995) reported that 340 of 1308 homes
(26%) used bottled water.
Allen et al. (1989) analyzed the chemical composition of 37 brands of imported and domestic
bottled mineral water. Fluoride was analyzed with an ion-selective electrode. Fluoride
concentrations ranged from <0.01 mg/L to 7.9 mg/L. In an earlier study MacFadyen et al. (1982)
reported fluoride levels of <0.1 mg/L to 5.8 mg/L in 26 bottled spring waters.
67
December 2010
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The National Fluoride Database (USDA, 2005) includes data on the concentrations of fluoride in
several brands of bottled water. Samples were collected in up to 144 locations across the
country, depending on the level of contribution to fluoride intake as previously determined by
the USDA. Differences in geographical location were incorporated into the sampling strategy.
Fifteen brands and one to 20 samples per brand were assayed using a fluoride ion-specific
electrode. The range of mean values for various types of bottled water was 0.02-0.78 mg/L. The
one brand containing fluoride at a level within the fluoridation range was a product intended to
supply fluoride. The mean concentration for most of the remaining samples tended to be below
0.2 mg/L F. According to U.S. EPA (2004), bottled water accounts for 3 mL/kg/day of total
ingested water from all sources (equal to 210 mL/day for a 70 kg adult), or about 18 % of mean
adult total water intake.
The fluoride concentrations in bottled water products vary substantially. Some products can
contain fluoride at levels that exceeded the levels recommended for fluoridation; a few mineral
or spring waters exceeded the MCL for fluoride.
3.6. Exposure from Drinking Water
Estimated exposures from public drinking water sources have been calculated using the average
and 90th percentile age-related water consumption estimates derived from U.S. EPA (2004), and
the average national concentration of fluoride reported in the ICR monitoring data (Section 3.3).
The average water concentration used for this calculation, 0.87 mg/L, is the average of the
averages from the data submitted to EPA for the 16 monitoring quarters from 2002 through
2005. The data used to determine the average concentration are reported in Table 3-1.
Mean water consumption (direct and indirect) and mean fluoride intake for all individuals
(consumers and nonconsumers) for specific age groups and the entire population, using the
average fluoride concentration of 0.87 mg/L, are shown in Table 3-5.
Table 3-5. Fluoride Intake from Consumption of Municipal Water (Direct and Indirect") at the Average
Concentration ( 0.87 mg/L) Determined from Monitoring Records for 2002 through 2005
Group
Infants <0.5 yr
0.5-0.9
1-3 yrs
4-6 yrs
7-10 yrs
11-14 yrs
15-19
20+
Total Pop.
Water Consumption (mL/day)b
Mean
296
360
311
406
453
594
761
1,098
926
90 % C.I. Upper bound
329
392
324
426
485
642
823
1127
949
Fluoride Intake (mg/day)b
Mean
0.26
0.31
0.27
0.35
0.39
0.52
0.66
0.96
0.81
90% C.I. Upper bound
0.29
0.34
0.28
0.37
0.42
0.56
0.72
0.98
0.83
SOURCE: Adapted from U.S. EPA, 2004. Table 5.1 Al.
Indirect consumption refers to intake through beverages and foods that include fluoridated drinking water as an ingredient.
bBased on an average fluoride concentration of 0.87 mg/L.
68
December 2010
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U.S. EPA (2004) reported that during a 2-day survey period for the CSFII survey, it was
determined that 5% of the individuals older than 1 year and 25% of infants younger than 1 yr did
not drink community water. If these individuals are excluded from the average intake
calculations, then the average amounts of municipal water consumed increase as do the fluoride
exposures. U.S. EPA (2004) calculated water consumption levels for the group "consumers
only" in order to adjust for those that did not report drinking water intake during the two days of
dietary data reported. These data are most important for infants who consume formula
reconstituted using tap water on a daily basis but whose formula intake is not recognized as a
source of tap water in the survey records. Estimated fluoride exposure at the mean fluoride
concentration (0.87 mg/day) and the consumer-only mean and 90th percentile intakes for the six
month to < 1 year age group are 0.41 mg/day and 0.84 mg/day (water intake = 971 mL) ,
respectively (see Table 3-6). For the 1 to < 3 year old group they are 0.30 mg/day and
0.63 mg/day (water intake = 723 mL), respectively.
For comparison with the estimates in Table 3-5, Table 3-7 presents the estimated average
fluoride exposures for all individuals (consumers and nonconsumers) with average drinking
water consumptions of direct and indirect water who consume water that is at the 90th percentile
fluoride concentration (1.43 mg/L) for a sustained period of time. The 90th percentile
concentration used for this analysis is the average of the 90th percentile values for the 16 quarters
reported to EPA between 2002 and 2005. Average consumers of drinking water from public
systems representative of the 90th percentile fluoride concentration have higher daily intakes of
fluoride from drinking water than those with 90th percentile intakes of drinking water at an
average fluoride concentration. However, only ten percent of the population will have water at
or greater than the 90th percentile concentration.
Table 3-6. Consumers Only Fluoride Intake from Consumption of Municipal Water (Direct and
Indirect") at the Average Concentration (0.87 mg/L) Determined from Monitoring Records for 2002
through 2005
Group
Infants <0.5 yr
0.5-0.9
1-3 yrs
4-6 yrs
7-10 yrs
11-14 yrs
15-19
20+
Total Pop.
Water Consumption1"
(mL/day)
Mean
548
467
349
442
487
641
817
1176
1000
90% Percentile
985
971
723
943
993
1415
1671
2284
2069
Fluoride Intakeb
(mg/day)
Mean
0.48
0.41
0.30
0.38
0.42
0.56
0.71
1.02
0.87
90% Percentile
0.86
0.84
0.63
0.82
0.86
1.23
1.45
1.99
1.80
SOURCE: Adapted from U.S. EPA, 2004. Table 5.2.A1.
Indirect consumption refers to intake through beverages and foods that include fluoridated drinking water as an ingredient.
bBased on an average fluoride concentration of 0.87 mg/L .
69
December 2010
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Table 3-7. Fluoride Intake From Average Drinking Water Consumption and 90th
Percentile Fluoride Concentration (1.43 mg/L) Determined from Monitoring
Records for 2002 through 2005
Group
Infants <0.5 yr
0.5-0.9
l-3yrs
4-6yrs
7-10 yrs
ll-14yrs
15-19
20+
Total Pop.
Water Consumption
Average
Total mL
296
360
311
406
453
594
761
1098
926
Fluoride Intake
mg/day
total
0.42
0.51
0.44
0.58
0.65
0.85
1.09
1.57
1.32
SOURCE: Adapted from U.S. EPA, 2004, Table 5.1.A1.
As noted by NRC (2006), fluoride exposures from drinking water depend on individual water
intakes, fluoride concentration in the water, and whether water purification or filtration systems
are used to remove fluoride. Some individuals may have substantially higher intakes of fluoride
from their drinking water as a result of specific types of activities that increase water intake (e.g.,
athletes or outdoor laborers in warm climates), life stage (e.g., pregnant or lactating women), or
as a result of medical conditions such as diabetes mellitus, diabetes insipidus, or renal problems.
70
December 2010
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4. Fluoride in Dental Products
4.1. Toothpaste
According to Newbrun (1992), more than 95% of all toothpaste sold in the United States
contains fluoride. Results of the 1983 National Health Interview Survey showed that 67.8% of
children younger than 5 years old used fluoridated tooth paste and 95.5% of those 5-9 years old
(Ismail et al., 1987). As many as 15% to 20% of children in some age groups studies by
Wagener et al., (1992) used fluoride supplements or mouth rinses.
The total daily amount of fluoride ingested and systemically absorbed following tooth brushing
with a fluoride toothpaste will vary with: 1) the concentration of fluoride in the toothpaste, 2) the
amount of toothpaste used; 3) the frequency of brushing; 4) the amount of rinsing; 5) the
swallowing control of the individual; and 6) the time of brushing relative to the time the last
meal was eaten. Most toothpaste sold in North America contains fluoride ion at a concentration
of 1000-1100 ppm (Levy, 1993). Toothpastes with lower concentrations of fluoride (250-500
ppm) are sold specifically for use by children (Newbrun, 1992) in other countries but are not
generally available in the United States. Some products without added fluoride are available in
the United States,
Fluoridated toothpastes (gel or paste products) in the United States are required to include
guidance to users on their product label (USFDA, 2009). Children under the age of 6 are to be
instructed in "good brushing and rinsing habits to minimize swallowing" and supervised "as
necessary until capable of using without supervision". It is recommended that a dentist or
pediatrician be consulted about toothpaste use for children under 2. The label should identify
toothpaste as a product intended for adults and children 2-years of age and older. Brushing is
recommended after every meal or twice per day. In a study discussed later, Levy et al. (1997)
found that 31.7% of parents surveyed reported use of fluoridated toothpaste by their children by
the time they were one year old, suggesting that many individuals do not follow the label
guidance.
The amount of toothpaste used per brushing, the frequency of brushing and the amount of rinsing
are expected to be highly variable factors which can substantially impact the amount of
toothpaste ingested. In studies conducted in Europe, Cochran et al. (2004) and O'Mullane et al.
(2004) found that 60% of 1.5-2.5 year-olds swallowed between 70% and 100% of the toothpaste
placed on the brush. Borysewicz-Lewicka et al., (2007) reported that children swallowed on
average 17% of the fluoride used in brushing with a gel containing 1.25% fluoride. Baxter
(1980) reported that children 5-6 years of age ingested an average of about 0.27 g per brushing;
older children ingested less.
Levy (1993) noted that a full strip of toothpaste covering a child's size toothbrush is 0.75 to 1.0 g
which could result in a fluoride intake as high as 1 mg per brushing. Based on the literature
available at the time, Levy (1993, 1994) estimated that children 2-3 years old would ingest about
0.3 g per brushing, equivalent to 59-65% of the amount used. At one time a complete ribbon of
toothpaste across the surface of the toothbrush was recommended. However, more recent
guidelines stress the application of a pea-sized portion. Levy et al. (1992) found that children
71 December 2010
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using flavored toothpastes marketed specifically for children used higher amounts of toothpaste
than those using regular toothpaste.
Levy (1993) also reported that 49% of 59 children aged 1-4 years did not rinse or expectorate
when brushing and an additional 27% rinsed but ingested almost all of the rinse water. Only 5%
of the children under the age of 2.5 years spit after brushing. In reviewing the available
literature, Levy (1993, 1994) noted that children who did not rinse after tooth brushing ingested
75% more toothpaste than those who rinsed. Swallowing control is especially weak in younger
children, and Levy et al. (2001) note that several studies have shown that younger children may
ingest more than half of the toothpaste used per brushing. In studies on young adults, Sjogren
and Melin (2001) found that oral retention of fluoride following brushing can be substantially
reduced by more than 50% by increased rinsing.
Following ingestion, fluoride absorption in the GI tract has been found to be close to 100%
(Ekstrand and Ehrnebo, 1980); however, the total amount absorbed can be affected by the
presence of certain foods in the stomach. Ekstrand and Ehrnebo (1979) reported that the
absorption of fluoride from sodium fluoride tablets was reduced to 50-79% when co-
administered with milk products. Cury et al. (2005) conducted a double-blind crossover study on
eleven volunteers (six women and five men aged 17-20 yrs) who ingested toothpastes with
fluoride concentrations of 0, 550 or 1100 jig F/g. The toothpastes were administered as a slurry
(45 mg/kg body weight) while fasting or 15 min after a meal (breakfast or lunch). Fluoride
levels were measured in unstimulated whole saliva for up to 3 hours post-exposure and in urine
24 hour pre-exposure and 24 hr post-exposure using an ion-selective electrode. Bioavailability
was 61% and 71% after lunch and breakfast, respectively, compared to an assumed 100% after
fasting for a toothpaste containing 1100 jig F/g, and 78% and 65%, respectively, for a toothpaste
with 550 |igF/g.
Osuji et al. (1988) conducted a case-control study of children 8-10 years old (34 children with
fluorosis and 34 controls) living in East York, Ontario, to determine the risk factors for dental
fluorosis. Factors evaluated included: prematurity, low birth weight, breastfeeding, use of
fluoride mouth rinses or supplements, residence history, medical and dental history (including
history of tooth brushing), and consumption of formula, tea, fish, soft drinks, milk, water, and
reconstituted juices. The only factors showing a significant association with fluorosis were
ingestion of infant formula and early use of fluoride tooth paste. Children who brushed their
teeth before age 25 months had 11 times the odds of developing fluorosis as those who began
tooth brushing at a later age. Prolonged use of infant formulas (>13 months) was associated with
3.5 times the risk of fluorosis compared with no or shorter duration of formula use. The odds
ratio for developing fluorosis was 7.1 (95% C.L. = 1.14-44.45) for children with prolonged
formula use, 13.8 (95% C.L. = 5.12-37.38) for children who had started brushing early, and 37.9
(95% C.L. = 10.60-134.52) for children who were in both groups.
Simard et al. (1989) evaluated tooth brushing habits, toothpaste use and its ingestion in a group
of Canadian children 2 to 5 years old. All but one of the children used a fluoridated toothpaste.
The majority (71.4%) brushed twice daily, 23.8% brushed three times daily, and 4.8% brushed
only once daily. The study was conducted at a day care center where the children brushed with a
toothpaste containing 0.24% NaF (1100 ppm F). Brushing habits at home were determined by a
questionnaire filled out by the parents. The quantity of toothpaste used and ingested and the
72 December 2010
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estimated amount of fluoride ingested are shown in Table 4-1. For all age groups combined the
amount of fluoride ingested was 0.329 mg per brushing.
Table 4-1. Toothpaste Use and Estimated Fluoride Ingestion by Children 2-5 Years Old
Age
(yr)
2-3
4
5
All
No of
Subjects
5
9
9
23
Toothpaste Used Per
Brushing (g)
Mean
0.464
0.783
0.651
0.662
SD
±0.19
±0.28
±0.34
±0.30
Toothpaste Ingested Per
Brushing (g)
Mean
0.278
0.390
0.221
0.299
SD
±0.13
±0.25
±0.12
±0.19
Estimated Fluoride Ingested
Per brushing (mg)
Mean
0.304
0.429
0.243
0.329
SD
±0.15
±0.27
±0.13
±0.20
SOURCE: Simard et al., 1989.
Fluoride retention following tooth brushing in nineteen 3-10-year-old children was evaluated by
Salama et al. (1989). Each child brushed with 1.8 g of toothpaste (1043 ppm F as MFP).
Fluoride recovered on the toothbrush and in expectorant was analyzed with a fluoride ion-
specific electrode after FDVIDS diffusion. The average quantity of fluoride not recovered was
0.36 ± 0.05 mg (range 0.08 to 0.82 mg). The study authors concluded that fluoride intake from a
single tooth brushing exceeds dietary intake in non-fluoridated areas and is equivalent to about
75% of dietary intake in fluoridated areas.
A pilot study was conducted to determine the tooth brushing habits of children 12-24 months old
and used to estimate the quantity of fluoride that children in this age group would ingest during
brushing (Simard et al., 1991). The study was conducted in the Quebec City region and involved
15 children. The authors used information from their earlier study (Simard et al., 1989) which
indicated that children 2-3 years of age ingested about 60% of the toothpaste used to estimate
fluoride exposures. A survey of the parents indicated that 60% of the children had their teeth
cleaned once a day, 32% twice a day and 8% three or four times per day. The average amount of
toothpaste used was 0.160 g. The assumption was made that the mean NaF concentration in the
toothpaste was 0.243%. The amount of fluoride ingested was calculated by taking 60% of the
quantity of toothpaste used per brushing per day multiplied by a conversion factor of 1.09 (to
convert from NaF to mg F/g of toothpaste) multiplied by the number of times the child brushed
each day. The estimated amount of fluoride ingested per day ranged from 0.02 to 0.33 mg (N=8)
for those whose teeth were cleaned once, and from 0.05 to 0.55 mg (N=6) for those whose teeth
were cleaned twice per day. The amount ingested by the one child who brushed three times per
day was 0.07 mg. Simard et al. (1991) reported that 20% of the children ingested more than 0.25
mg of fluoride per day. The average amount of fluoride ingested by all 15 children was 0.15
mg/day.
Levy et al. (1995) summarized the results of studies conducted up to 1993 which evaluated the
amounts of toothpaste ingested during tooth brushing for various age groups. Toothpaste
ingestion per brushing for children 1-9 years old ranged from 0.11 to 0.39 g, with 90th percentile
levels ranging from 0.08 to 0.73 g. Assuming 1.1 mg F/g toothpaste, this amount of toothpaste
ingestion would result in a consumption of 0.12-0.43 mg F (90l percentile range of 0.09 to 0.8
73
December 2010
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mg F). Levy et al. (1995) estimated a mean fluoride intake from toothpaste of 0.01 mg (range 0-
0.04 mg) for infants 6 months old, 0.07 mg (range 0.03-0.66 mg) for children 12 months old,
and 0.25 mg (range 0.01-1.50 mg) for children 2 and 3 years old.
In a later study Levy et al. (1997) surveyed by questionnaire the parents of children born in
eastern Iowa on the tooth brushing practices of their children up to 1 year of age (Table 4-2). If
it is assumed that about 62.45% of the toothpaste reported as used in the 1997 paper is ingested,
then the estimated amount of fluoride ingested is 0.13 mg for 6-mo-olds, 0.12 mg for 9-mo-olds;
and 0.12 mg for 12-mo-olds. The estimate for ingestion comes from a Levy et al. (2000) study of
3-4 year old subjects. The percent of children who were reported as having their teeth brushed
increased from 12.9% at six months to 64.5% at one year. The percent of parents that reported
using fluoride-containing toothpaste increased from 1.9% at six months to 31.7 % at one year.
Table 4-2. Toothpaste Use by Children 6 to 12 Months Old
Parameter
Number of children
Percentage with erupted teeth
Percentage whose teeth were brushed
Percentage using fluoridated toothpaste
Mean amount of fluoride used per brushing
Mean amount of fluoride used per day
Age Groups
6 Months
899
34.6%
12.9%
1.9%
0.11 mg
(0.02-0.05)3
0.21 mg
(0.02-1. 50)a
9 Months
665
83.6%
36.7%
11.7%
0.14mg
(0.02-0.88)3
0.20
(0.01-1.75)3
'12 Months
508
98.0%
64.5%
31.7%
0.17
(0.02-0.88)3
0.19
(0.01-1.75)3
Frequency of cleaning/brushing
Less than once per day
Once per day
Twice per day
Three times per day
More than three times per day
31.4%
41.2%
16.9%
6.3%
6.3%
33.2%
45.5%
17.0%
3.1%
1.1%
37.0%
44.8%
14.7%
3.5%
-
SOURCE: Levy etal., 1997.
aRange.
Levy et al. (2000) further evaluated the tooth brushing habits of 28 U.S. preschoolers (3-4 years
old; mean age 44 months). The average amount of toothpaste applied to the toothbrush was
0.256 g (range 0.035-0.620 g, SD = 0.177 g). The estimated mean amount of ingested fluoride
was determined by subtracting the estimated amount expectorated from the amount of toothpaste
applied to the brush. Fluoride was determined with a fluoride ion-specific electrode after
diffusion using a modified Taves microdiffusion method. The mean amount of fluoride ingested
was 0.17 mg per brushing (SD 0.15 mg; range 0.00-0.52 mg), equivalent to 62.45% of the initial
amount in the toothpaste.
Only a few studies have given 90th and 95th percentile estimates for toothpaste and/or fluoride
ingestion. Barnhart et al. (1974) measured toothpaste use and ingestion in four age groups; 2-4
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December 2010
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yr olds (N=68), 5-7 yr olds (N=4); 11-13 yr olds (N=98); and 20-35 yr olds (N=70) under
simulated home-use conditions. Chronic usage conditions were simulated with a statistical
model to obtain realistic estimates of the 90th and 95th percentile ingestion. The mean amount of
toothpaste used per brushing was 0.86 g for the 2-4 yr olds, 0.94 g for the 5-7 yr olds and 1.10 g
for the 11-13 yr olds. Ingestion rates among the four groups are summarized in Table 4-3.
Assuming 1000 ppm F in the toothpaste, these toothpaste ingestion rates would correspond to
mean fluoride ingestion rates of 0.3 mg for the 2-4 yr olds, 0.13 mg for the 5-7 yr olds and 0.07
mg for the 11-13 yr olds.
Table 4-3. Age-Related Estimates of Fluoride Ingestion from Toothpaste Use
Age
(yr)
2-4
5-7
11-13
20-35
No. of
Subjects
62
56
73
60
Toothpaste
Used
Per Brushing
(grams)3
0.86
0.94
1.10
1.39
Toothpaste Ingestion
(g)
Mean
0.30
0.13
0.07
0.04
90th
Percentile
0.73
0.27
012
0.12
95th
Percentile
0.82
0.44
0.21
0.13
Estimated Fluoride Ingestion
(mg)b
Mean
0.3
0.13
0.07
0.04
90th
Percentile
0.73
0.27
0.12
0.12
95th
Percentile
0.82
0.44
0.21
0.13
SOURCE: Bamhart et al., 1974.
aMean value.
bAssumes 1000 ppm F in toothpaste.
Environment Canada/Health Canada (1993) estimated the daily intake of fluoride from
toothpaste (products for home use) for different age groups. Based on a mean inorganic fluoride
concentration of 1000 ppm in most toothpaste products (Beltran and Szpunar, 1988; Whitford,
1987), and an estimated toothpaste intake of 0.26-0.78 g/day for children 7 months to 4 years of
age, 0.22-0.54 g/day for children 5 to 11 years of age, 0.14 g/day for adolescents 12-19 years of
age, and 0.08 g/day for adults 20+ years of age (Levy, 1993), and assuming an average of two
brushing per day, the fluoride intakes for these age groups was estimated to be 0.02-0.06 mg/kg
bw/day, 0.008-0.02, 0.00246, and 0.00114 mg/kg bw/day, respectively. Using an average body
weight of 57 kg for the 12-19 yr-olds and 70 kg for the adults, the daily fluoride intakes for these
two age groups can be calculated as 0.14 mg/day and 0.0798 mg/day, respectively.
The most important factor determining the quantity of fluoride ingested by children during tooth-
brushing was the amount of toothpaste used according to a study of 405 children, ages 2-7 yr,
enrolled in Quebec City schools (Naccache et al., 1992). The estimated amount of toothpaste
used per brushing was determined by the difference between the amount used and the amount
recovered from the toothbrush and rinse water. Fluoride was analyzed with an ion-specific
electrode. The toothpaste contained 0.24% NaF. The amount of toothpaste used, the age of the
children and the amount of rinsing were analyzed by multiple regression analysis. The amount
of toothpaste used and the amount of fluoride ingested are shown in Table 4-4. On average, the
amount of toothpaste used was 0.5 g per brushing. The mean amount of fluoride ingested was
0.229 mg per brushing. The amount ingested decreased with increasing age.
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December 2010
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Table 4-4. Toothpaste Use and Fluoride Ingestion in Children Two to Seven Years Old
Age
(yr)
2
3
4
5
6
7
Total
No of
Subjects
36
56
81
77
78
77
405
Toothpaste Used
(grams)3
Mean
0.618
0.529
0.446
0.516
0.484
0.497
0.503
SD
0.976
0.424
0.269
0.366
0.254
0.401
0.401
Estimated Fluoride Ingested
(mg per brushing)
Mean
0.358
0.280
0.241
0.227
0.180
0.175
0.229
SD
0.363
0.218
0.184
0.174
0.127
0.194
0.195
SOURCE: Naccache et al, 1992.
Rojas-Sanchez et al. (1999) estimated fluoride intake from toothpaste in groups of children, aged
16-40 months, from three communities; San Juan, Puerto Rico (n=l 1), Connersville, IN (n=14)
and Indianapolis, IN (n=29). Intake was determined by subtracting the amount of toothpaste
expelled and the amount left on the toothbrush from the amount initially placed on the
toothbrush. The concentration of fluoride in the toothpaste was 0.10-0.11% (theoretical).
Samples were analyzed for fluoride using the hexamethyldisiloxane microdiffusion method of
Taves (1968b) as modified by Dunipace et al. (1995). Frequency of brushing equal to or greater
than two times per day was 91% (n=l 1) in San Juan; 67% (n = 14) in Connersville; and 46% (n
= 29) in Indianapolis. The mean amount (± SEM) of fluoride ingested in toothpaste each day
was estimated to be 548 ±62 jig in San Juan, 576 ±86 jig in Connersville, and 424 ±73 jig in
Indianapolis.
The patterns of fluoride ingestion from toothpaste use in children from shortly after birth (1.5
months) to an age of 36 months were reported by Levy et al. (2001). Information was obtained
from questionnaires as part of the longitudinal Iowa Fluoride Survey. Estimates of the amount of
toothpaste used were based on the parents selecting from pictures depicting children's
toothbrushes with different quantities of toothpaste on them, and the amount ingested were based
on estimates made by the parents. Estimates of the fluoride ingested were based on the
manufacturers indication of the fluoride content of the toothpaste used (in most cases 1000-1100
ppm). Results are shown in Table 4-5.
Using the same methodology as that for children 0-36 months old (Levy et al., 2001, see above),
Levy et al. (2003a) calculated fluoride ingestion from toothpaste use in children aged 36 to 72
months old. Results of the survey by fluoride source were presented by Levy et al. (2003a) in
graphical form. As estimated from the graphical data, mean fluoride intake from toothpaste was
about 0.28 mg/day at 36 months, 0.27 mg/day at 48 months, 0.20 mg/day at 60 months, and 0.17
mg/day at 72 months. Estimates of 90th percentile intakes from toothpaste ingestion for these
same age groups were 0.76, 0.76, 0.50, and 0.50 mg/day, respectively.
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December 2010
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Table 4-5. Estimated Fluoride Intake from Toothpaste" in Children 1.5 to 36
Months Old
Age
(months)
1.5
3.0
6.0
9.0
12.0
16.0
20.0
24.0
28.0
32.0
36.0
Intake (mg)
Mean (SD)
0.000
0.000
0.002 (0.041)
0.013 (0.081)
0.038(0.136)
0.102(0.207)
0.191 (0.270)
0.257(0.312)
0.267 (0.305)
0.290(0.315)
0.278 (0.292)
90th Percentile
0.000
0.000
0.000
0.000
0.109
0.250
0.500
0.656
0.750
0.750
0.750
SOURCE: Levy et al., 2001.
aPortion of toothpaste ingested estimated from parent's report.
Participants in the Iowa Fluoride Study were evaluated to determine the effect of fluoride
toothpaste ingestion on the occurrence of dental fluorosis (Franzman et al., 2006). The study
utilized information derived from questionnaires filled out by the participants' parents
concerning fluoride exposures and toothbrushing at ages 16, 24, and 36 months. The results of
the survey on toothpaste use are shown in Table 4-6. The estimated percent of individuals
ingesting 75% or more of the toothpaste was 82% at age 16 months, 85% at age 24 months, and
66% at age 36 months.
Table 4-6. Toothpaste Use and Ingestion by Children Ages 16 to 36 Months
Parameter
Individuals who brash teeth
Use of fluoridated toothpaste
Brash teeth less than once/day
Brash teeth once/day
Brash teeth twice/day
Brash teeth more than twice /day
<25% toothpaste swallowed
50% toothpaste swallowed
>75 toothpaste swallowed
Percentage of Children (n = 343)
16 Months Old
90
65
35
48
14
4
13
5
82
24 Months Old
100
90
25
51
23
2
7
9
85
36 Months Old
100
96
18
57
24
1
21
13
66
SOURCE: Franzman et al., 2006.
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In an earlier study (Franzman et al., 2004) estimated that 51-59% of children 9-32 months old
ingested 0.125-0.25 g of toothpaste per brushing, declining to 28% at 60 months. 12% ingested
0.5-0.75 g at 9 months, increasing to 64% at 60 months. The percentage using 0.875-1.0 g per
brushing was <3% up to 28 months, 3-5% at 32-54 months and 7% at 60 months. Using the
information from Franzman et al. (2004), Franzman et al. (2006) estimated the amount of
fluoride ingested (per kg body weight) by children who were showing definitive signs of
fluorosis on the incisors and those not showing signs of fluorosis. Results are presented in Table
4-7. Average body weights for each age group were not reported. For all but the 16-month
children the fluoride ingestion per unit of body weight was higher for the children with dental
fluorosis than those without.
Table 4-7. Fluoride Ingestion from Toothpaste Use and Fluorosis
Age
16 mo
24 mo
36 mo
16-36 AUCC
Fluorosis Absent
Number
220
220
220
220
Median Daily
Fluoride Ingestion
(mg/kg bw)
0.002
0.010
0.012
0.011
Fluorosis Present"
Number
89
89
89
89
Median Daily
Fluoride Ingestion
(mg/kg bw)
0.002
0.017
0.016
0.013
P Valueb
0.61
0.02
0.02
0.02
SOURCE: Franzman et al., 2006.
aTwo or more incisors with definitive fluorosis (fluorosis risk index of 2).
bBased on Wilcoxon rank sum test.
°AUC = Area under the curve, a measure of cumulative exposure.
Bohaty et al. (1989) evaluated topical and systemic fluoride supplement use and the prevalence
of dental fluorosis in 300 children, aged 6-13 from 6 elementary schools, living in areas with
optimal water fluoridation (location of the study sites and the fluoride level in the drinking water
were not reported). Fluorosis was scored using Dean's system (subjects with fluorosis were
considered those with a Dean score of 0.5 or higher). The data were categorized according to
fluoride use, residential history, age, sex and geographic location. Differences in frequency of
the categorized data were evaluated statistically with Chi-square analysis where the differences
were considered significant at p < 0.05. There were no differences between tooth brushing
frequency and fluorosis scores in any group.
4.2. Topical Applications and Mouth Rinses
Several studies have evaluated use of topical fluoride products and mouth-rinses. According to
Levy and Zarei-M (1991), the Dental Care Supplement of the 1983 National Health Information
survey found that 5% of children under age 5 yr and 17% of children 5-17 years old reportedly
were using fluoride mouth-rinses.
Data from the 1986-87 National Institute of Dental Research U.S. Children's Survey revealed
that 54% of children 5-17 years old without access to fluoridated drinking water received topical
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December 2010
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fluoride treatments at a dentist's office and 22% had received topical fluoride treatments through
school-based programs. From data complied in the Iowa Fluoride Study, Levy et al. (2003b)
found that only 6% of children surveyed had a fluoride treatment by age 3, 27% by age 4, 44%
by age 5 and 66% by age 6 (Table 4-8). Children with dental caries were more likely to have had
such a treatment.
Table 4-8. Percentage of Children Receiving Fluoride Treatments by Age Groups
Age
(yr)
-------
(2006) concluded that intakes from topical fluorides during professional treatment were unlikely
to be significant contributors to chronic fluoride exposures because they are used only a few
times per year.
4.3. Summary of Fluoride Exposure from Dental Products
Table 4-9 is a summary of studies that examined exposure to fluoride from toothpaste. With few
exceptions all of these studies were published in the early to mid-1990s and are likely to not
reflect changes in guidance on the amounts of toothpaste recommended for brushing (a pea-sized
portion rather than a ribbon). Accordingly, they may overestimate current fluoride intakes from
toothpaste. The data provided in Table 4-9 come only from studies that measured ingested
fluoride by comparing the amount placed on the toothbrush to that left on the toothbrush and
expectorated. Many of other studies reported estimates of ingestion based on questionnaires from
parent reporting on toothpaste use. Data on ingestion estimates are not included in Table 4-9.
Use of fluoridated mouth washes on a daily basis in the home setting is likely to increase the
daily dose of fluoride from dental products. Unfortunately no primary data on exposures from
mouthwashes were identified. In 1983 less than 20% of children in the 6 months to 14 year age
range of concern used mouthwashes. However, these data may very well not reflect current use
patterns.
Fluoride is released from a number of dental devices, including composite resins, resin-based
cements, resin-bonding agents, orthodontic bracket adhesives, pit and fissure sealants, glass
ionomer cements, and cavity varnishes. However, the exposure dose is probably small (HHS,
2010).
Table 4-9. Age-Related Exposure Estimates for Fluoride From Toothpaste
Age
(yr)
0.5 <1
1<4
4<7
7<11
11-14
>14
Fluoride Intake"
(mg/day)
0.01
0.07
0.358 ±0.363
0.280 ±0.218
0.25
0.424,
0.576
0.17
0.241 ±0.184
0.227 ±0.174
0.180 ±0.127
0.175 ±0.194
0.2
No data
Notes
Levy et al, 1995 - mean; 6 month olds
Levy et al., 1995 - mean; 12 month olds
Nacchache et al., 1992 - 2 year olds
Nacchache et al., 1992 - 3 year olds
Levy et al., 1995; 2-3 year olds
Rojas-Sanchez et al., 1999; 1.3-3.3 year olds. Average of values
for two different locations
Levy et al., 2000; 3-4 year olds.
Nacchache et al., 1992; 4 year olds
Nacchache et al., 1992; 5 year olds
Nacchache et al., 1992; 6 year olds
Nacchache et al., 1992; 7 year olds
Levy et al., 1995 - as adjusted by NRC; 13-19 year olds
No data
"Fluoride values represent one brushing per day.
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December 2010
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Surveys of fluoride ingestion from tooth brushing are indicative of wide individual variability
with standard deviations that are frequently greater than the mean values (Naccache et al., 1992).
The studies are generally consistent in showing that mean fluoride intake from toothpaste
decreases with age. This is likely due in some part to maturation of the swallowing reflex as
well as improved rinsing and expectoration practices.
The number of times a child or adult brushes their teeth per day is an important variable in
determining the fluoride ingested because of toothpaste use. Table 4-10 summarizes the data
available from studies in children that recorded this parameter. Three of the studies were
conducted in the United States (Levy et al., 1997; Rojas-Sanchez et al., 1999; Franzman et al.,
2006) and two in Canada (Simard et al., 1989, 1991). In all the studies but 2 (Rojas-Sanchez et
al., 1999, at one location; Simard et al., 1989), the percentage brushing their teeth one time per
day was greater than that for more frequent brushings. The Simard et al., 1989 study covered the
largest age range (2 to 5 years), suggesting that those results may easily have been influenced by
a high representation of older children who brushed two or three times per day. Based on these
data, the OW chose to use the data for one brushing per day to represent fluoride exposure from
ingestion of toothpaste. There are no ingestion data for elementary-school age children,
adolescents or adults. Although some of the cited data are from Canada, the values reported
suggest that the FDA (2009) guidance that children younger than 2 years in age should not use
toothpaste when brushing their teeth is not practiced by many.
Table 4-10. Number of Tooth Brushings Per Day Reported for Children (Six Months to Five Years Old)
Study
Simard etal, 1989
Simard etal. 1991
Levy etal., 1997
Rojas-Sanchez etal., 1999
Franzman et al., 2006
N =
23
15
899
665
508
14
29
90
100
100
Age
(years)
2 to 5
Ito2
0.5
0.75
1
2.25
2.3
1.3
2
3
Percentages"
1 time/day
4.8
60
41.2
33.2
37
33b
54b
48
51
51
2 times/day
71.4
32
16.9
17
14.7
3 times/day
23.8
8
6.3
3.1
3.5
67C
46C
14
23
24
4
2
1
aSome studies also reported those brushing their teeth less than once per day and more than three times per day. In these cases
the percentages do not add up to 100%.
bLess than or equal to 1 time per day
"Equal to or greater than 2 times per day
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December 2010
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The presence of food in the gastrointestinal tract decreases the bioavailability of fluoride from 30
to 40 % based on studies in which adults ingested a toothpaste slurry after eating a meal or after
fasting (Cury et al., 2005). In the fasted state, bioavailability was assumed to be close to 100%,
deceasing to 61 to 71% after meals if the toothpaste has the current conventional 1100 ppm
fluoride concentration. These data are supported by a study of fluoride absorption after ingestion
of tablets (2 mg) of sodium fluoride and sodium monofluorophosphate (Trautner and Einwag,
1989); both chemicals are used in toothpaste. Ingestion of the tablet with milk reduced peak
plasma fluoride levels to 70% of the level when the tablet was taken with water (Trautner and
Einwag, 1989).
82 December 2010
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5. Other Sources of Exposure
5.1. Exposure from Air
As noted by NRC (2006), fluoride is released to the atmosphere by natural sources such as
volcanoes and also by various anthropogenic sources. Atmospheric releases of inorganic fluoride
to the atmosphere can come from power plants burning coal, aluminum production plants,
phosphate fertilizer plants, chemical production facilities, steel mills, magnesium plants, and
manufacturers of brick and structural clay (ATSDR, 2003).
5.1.1. Monitoring Data
Cholak (1960) reviewed pre-1951 data on atmospheric levels of fluoride ion in several non-
industrial areas of the United States. Average concentrations ranged from 0.02 ppb in Logan,
Utah, to 2 ppb in New York.
Thompson et al. (1971) reported on water-soluble fluoride concentrations in ambient air
collected by the National Air Surveillance Network in 1966, 1967, and 1968. Fluoride levels
were measured in water-extracted samples using a fluoride ion-specific electrode. Of a total of
9175 urban air samples, only 18 (2%) exceeded 1.0 ug/m3, and the maximum concentration
recorded was 1.89 ug/m3 (mean concentrations were not reported). Of 2164 non-urban samples
only 3 (1%) exceeded 0.1 ug/m3, and the maximum concentration recorded was 0.16 ug/m3.
Thompson et al (1971) also summarized the results of the Continuous Air Monitoring Project
conducted in 1967 and 1968 in six major US cities (Chicago, Cincinnati, Denver, Philadelphia,
St. Louis, and Washington, DC). Over 110 samples were analyzed from each city. The
percentage of 1967 samples in which no fluoride could be detected (minimum detection limit
0.05 ug/m3) ranged from 58% in Chicago to 98% in Washington, DC. The percentage of 1968
samples in which no fluoride could be detected ranged from 42% in St Louis to 84% in
Cincinnati. The maximum recorded values were 1.90 ug/m3 in St. Louis in 1967 and 0.55 ug/m3
in Chicago in 1968.
Kelly et al. (1993) reported that ambient concentrations of hydrogen fluoride in the United
States, as measured around 1983, ranged from 1.0 to 7.5 ug/m3 (ATSDR, 2003).
Atmospheric concentrations of fluoride in most parts of Canada are generally low or
undetectable (<0.05 ug/m3) (Environment Canada/Health Canada, 1993). Atmospheric levels in
a residential area near Toronto averaged (monthly) 0.03 ug/m3.
Fluoride levels in the atmosphere can be unusually high in certain locations due to industrial
activity and/or the burning of fluoride-rich coal. Ernst et al. (1986) reported that in 1981 the
Surveillance Division of the Air Pollution Control Directorate-Canada measured an average
atmospheric fluoride concentration (particulate and gaseous) of about 0.6 mg/m3 downwind from
an aluminum smelter located in a rural inhabited area on the U.S.-Canadian border.
83 December 2010
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5.1.2. Exposure to Airborne Fluoride
According to NRC (2006), exposure to airborne fluoride for most individuals in the United
States is expected to be low compared with ingested fluoride as reported by U.S. EPA, (1988),
with exceptions being populations living in heavily industrialized areas or having occupational
exposure. Using inhalation rates of 10 mVday for children and 20 m3/day for adults, NRC (2006)
calculated that fluoride inhalation exposures in rural areas (<0.2 ug/m3 fluoride) would be less
than 2 ug/day for a child and 4 ug/day for an adult. In urban areas (<2 ug/m3), fluoride
exposures would be less than 20 ug/day for a child and 40 ug/day for an adult. Most of the data
that support these estimates are 30 to 40 years old and were collected before restrictions were
placed on many industrial releases of gases and particulate matter to ambient air. The NRC
estimates are consistent with the older monitoring data reported in Section 5.1.1 but the 1993
Canadian data cited above suggest that ambient air concentration in the U.S. may now be lower
than the values used by NRC (2006) in their assessment.
Airborne fluoride can indirectly contribute to human exposure as a result of secondary
contamination of edible fruits and vegetables. In reviewing the data available at the time,
Waldbott (1963) reported that peaches grown near an aluminum plant in Oregon contained 3.2-
21.9 ppm fluoride, whereas those grown in an uncontaminated area contained only 0.21 ppm F.
Similarly, carrots grown near an aluminum plant in Switzerland contained 5.0 ppm F, whereas
uncontaminated carrots contained 0.22-2.0 ppm F. High levels of fluoride were also reported for
orange juice (0.05-3.12 ppm F), milk (3.2 ppm F) and spinach (16.0 ppm F) obtained in Tampa,
FL, near a phosphate fertilizer plant. The normal levels of fluoride in orange juice were reported
to be 0.07-0.17 ppm, and that in milk 0.1-0.3 ppm.
5.2. Oral Supplements
Oral fluoride supplements are prescribed by physicians and dentists for children living in areas
where the drinking water contains low levels of fluoride. The daily doses of supplemental
fluoride recommended by the American Dental Association (as revised in 1994) call for no
supplement use for children less than 6 months old and none for any child whose water contains
more than 0.6 mg F/L (Table 5-1). Guidelines for other age groups and drinking water fluoride
concentrations are summarized in Table 5-1.
Table 5-1. Daily Fluoride Supplementation Recommended by the ADA and the American Academy of
Pediatric Dentistry
Age
0-6 months
6-36 months
3-6 years
6-16 yr
Fluoride Concentration in Local Water Supply
<0.3 ppm
None
0.25 mg
0.50 mg
1.00 mg
0.3-0.6 ppm
None
None
0.25 mg
0.50 mg
>0.6 ppm
None
None
None
None
SOURCE: ADA (..http://www.ada.org/3088.aspx.).
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The Dental Care Supplement of the 1989 National Health Interview Survey reported that
approximately 10.5% of 31,446 children under 18 yr of age had used fluoride supplements
(CDC, 1989).
Levy and Muchow (1992) evaluated patterns of fluoride supplement use among 446 children and
their siblings living in either Iowa or North Carolina. Fluoride intake through the use of
supplements was compared to the fluoride levels of the municipal drinking water in the areas
where the children lived. Results suggested that approximately one-third of the primary children
and 42% of the siblings did not receive an adequate amount of fluoride.
A survey conducted by Pendrys and Morse (1990) of seventh and eighth grade children living in
Massachusetts and Rhode Island found that 35.1% of 74 children who had lived in a fluoridated
community for at least 3 years during their first 6 years of life were given fluoride supplements.
As reported in Section 4, the patterns of fluoride ingestion from toothpaste use in children from
shortly after birth (1.5 months) to an age of 36 months were reported by Levy et al. (2001).
Using information from the questionnaires provided by the parents, Levy et al., (2003a)
calculated fluoride ingestion from dietary supplements in children ages 36 to 72 months old.
Results were presented in graphic form. The estimates of mean fluoride intakes from
supplements were less than 0.05 mg/day for all age groups (Table 5-2).
Table 5-2. Fluoride Intake from Supplements in Children 1.5 to 36 Months Old
Age
(months)
1.5
3.0
6.0
9.0
12.0
16.0
20.0
24.0
28.0
32.0
36.0
Intake (mg/day)
Mean (SD)
0.014 (0.045)3
0.018 (0.060)
0.019 (0.063)
0.014 (0.052)
0.015 (0.054)
0.011(0.054)
0.008 (0.038)
0.008 (0.052)
0.012 (0.068)
0.013 (0.079)
0.013 (0.079)
Maximum
0.375
0.833
1.000
0.500
0.500
1.000
0.250
1.000
1.000
1.000
1.000
SOURCE: Levy etal., 2001.
Trautner and Einwag (1986) measured the bioavailability of fluoride in three health food
products recommended for children. The net urinary excretion of fluoride in six children ages
15-16 years was measured after ingestion of bone meal tablets, calcium earth tablets or siliceous
earth tablets with fluoride contents of 520, 100, and 115 mg F/kg. Urinary fluoride was
measured with an ion-specific electrode. Mean relative bioavailability was found to be 53.9
85
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±21.6% from bone meal tablets, 64.8 ±23.6% from calcium tablets, and 38.9 ±20.5% from
siliceous earth tablets.
In a later study Trautner and Einwag (1989) measured the bioavailability of fluoride when
administered as NaF or sodium monofluorophosphate tablets (2 mg F). The test subjects were 7-
19 years old and were given the supplements while fasting, or with milk or with milk and food.
Fluoride levels in blood samples were measured using an ion-specific electrode. In fasting
subjects equal levels of bioavailability were seen for both fluoride compounds and assumed to be
100%. Ingestion of milk reduced peak plasma fluoride levels by 30% compared to that for
fasting individuals, but this effect was not seen when the milk was consumed with food.
Bohaty et al. (1989) evaluated both topical and systemic fluoride supplement use and the
prevalence of dental fluorosis in 300 children, aged 6-13 from 6 elementary schools, living in
areas with optimal water fluoridation (location of the study sites and the fluoride level in the
drinking water were not reported). Fluorosis was scored using Dean's system (subjects with
fluorosis were considered those with a Dean score of 0.5 or higher). The data were categorized
according to fluoride use, residential history, age, sex and geographic location. Differences in
frequency of the categorized data were evaluated statistically with Chi-square analysis where the
differences were considered significant at p < 0.05. Although there were no significant
associations between the frequency of tooth brushing and dental fluorosis, for subjects from four
schools (n = 206), the frequency of using fluoride supplements was significantly associated with
fluorosis. Similarly, for subjects of three of these four schools, the use of fluoride gels and rinses
was significantly associated with dental fluorosis.
5.3. Soil Ingestion by Children
Fluoride ranks 13th or 14th in terms of its elemental abundance in the earth's crust. Thus, fluoride
in soil could be a source of inadvertent exposure, primarily for children. Typical fluoride
concentrations in soil in the United States range from very low (<10 ppm) to as high as 7%
(70,000 ppm) in some areas with high concentrations of fluorine-containing minerals (ATSDR,
2003). Mean or typical concentrations in the United States are on the order of 300-430 ppm.
Soil fluoride content may be higher in some areas due to use of fluoride containing phosphate
fertilizers or to deposition of airborne fluoride released from industry.
The EPA (2008) Child-Specific Exposure Factor's Handbook recommends use of a combined
soil and outdoor dust ingestion rate of 60 mg/day for children < 1 year old and 100 mg/day for
children 1 to < 21 years of age. Using an average fluoride concentration of 400 ppm, the oral
intake from soils for an infant (<1 year) would be 0.02 mg/day and that for older children and
adolescents would be 0.04 mg/day. The estimated intake for adults in the EPA (1997) Exposure
Factors Handbook is 50 mg/day and equivalent to 0.02 mg F/day from soils with an average
concentration of 400 ppm. Erdal and Buchanan (2005) estimated intakes of 0.0025 and 0.01
mg/kg/day for children (3-5 years), for mean and reasonable maximum exposures, respectively,
based on a fluoride concentration in soil of 430 ppm. In their estimates, fluoride intake from soil
was 5-9 times lower than that from fluoridated drinking water.
For children with pica (a condition characterized by consumption of nonfood items such as dirt
or clay), an estimated value for soil ingestion is 10 g/day (U.S. EPA, 1997). For a 20-kg child
86 December 2010
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with pica, the fluoride intake from soil containing fluoride at 400 ppm would be 4 mg/day or 0.2
mg/kg/day. Although pica in general is not uncommon among children, the prevalence is not
known (U.S. EPA, 1997). Pica behavior specifically with respect to soil or dirt appears to be
relatively rare but is known to occur (U.S. EPA, 1997). Fluoride intake from soil for a child with
pica could be a significant contributor to total fluoride intake. For most children and for adults,
fluoride intake from soil probably would be important only in situations in which the soil
fluoride content is high, whether naturally or due to industrial pollution.
5.4. Pharmaceuticals
As noted by Miiller et al. (2007), since 1957, over 150 fluorine-containing drugs have come to
the marketplace and now make up about 20% of all pharmaceuticals. The presence of fluorine in
a drug can enhance binding efficacy and selectivity (Miiller et al., 2007). Typical fluorine-
containing drugs include fluoxetine (antidepressant Prozac), atorvastatin (cholesterol-lowering
drug Lipitor), and ciprofloxacin (antibacterial drug Ciprobay). Waldbott (1963) reported that
certain fluoride-containing tranquilizers and steroids, when taken three times per day, can result
in a daily intake of 0.8-1.0 mg F. Fluoride in such drugs is organically bound to carbon atoms.
The extent that the fluoride becomes bioavailable as a result of the metabolism of these drugs is
likely to vary from drug to drug. To assess the contribution of fluorine-containing drugs to the
total body pool of fluoride ion, information is needed on the changes in concentration of fluoride
ion in blood serum following ingestion of such drugs. NRC (2006) reported that there are slight,
but not significant increases of inorganic fluoride in serum after ingestion of several
organofluorine pharmaceuticals but only a limited number of such products have been evaluated.
Oral electrolyte solutions were sampled for fluoride and found to contain 0.01-0.15 mg F/kg by
Dabeka and McKenzie (1987). Electrolyte solutions are used to replenish the fluids lost during
episodes of severe diarrhea in children.
5.5. Occupational Exposures
Inhalation exposures to fluoride in the workplace are limited by regulations established by the
Occupational Safety and Health Administration (OSHA). The OSHA 8-hr TWA exposure limit
of for fluoride is 2.5 mg/m3 (ATSDR, 2003). A person breathing at an average rate of 20 m3 per
day would inhale 16.8 mg during one 8-hr working shift (equivalent to 0.24 mg/kg/day for a 70
kg man).
5.6. Smoking
As noted by NRC (2006), heavy cigarette smoking could contribute as much as 0.8 mg of
fluoride per day to an individual (0.01 mg/kg/day for a 70-kg person) (U.S. EPA, 1988).
87 December 2010
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6. Exposure Assessment Summary
As mentioned in the preceding sections of this report, fluoride concentrations in different media
and resultant fluoride exposures vary for a number of reasons including the following:
The methodologies used in conducting the studies differ in the ways the data were
gathered, grouped and analyzed
The size and composition of the study populations differ between studies.
The analytical methods used to determine the concentration of fluoride in media of
interest have evolved over time with the evolution of new methods that improved
fluoride recovery and detection levels as well as reduced interference from other
ions
The amounts of fluoride present in the drinking water supply and soils differ with
local geology and fluoridation practices.
Available commercial food and beverage products and population dietary preferences
are not constant over time
Use of fluoridated water as process water by commercial food and beverage facilities
can increase fluoride content to levels above that in the unprocessed product.
Home cooking of foods in fluoride-containing water increases the fluoride content of
the finished product but the increase varies with the food material prepared.
Each of these factors contributes to the differences observed when comparing data from the
studies included in this report and to the uncertainty inherent in establishing an RSC for fluoride.
In developing the RSC for the fluoride from drinking water, EPA chose to focus on the following
media as the major contributors to total intake:
Drinking water from public drinking water systems.
Solid foods from the diet including milk and juices not made from concentrate.
Residues of the recently registered pesticide, sulfuryl fluoride.
Beverages, both commercial and home-prepared using tap water (i.e. coffee, tea.
reconstituted juices and powdered beverage mixes).
Infant formula made from powdered concentrate for the six-month to less than one-
year age group.
Toothpaste swallowed during tooth brushing.
Incidental ingestion of soil and outdoor dust.
There are other sources of fluoride exposure such as ambient air, dietary supplements,
professional dental treatment products, and some pharmaceuticals. These sources make minimal
contributions to daily intakes during the period of dental fluorosis vulnerability. NRC (2006)
estimated that average exposures from ambient air would be 2 micrograms per day for children
and 4 micrograms per day for adults. Supplements are not recommended for use in cases where
water is fluoridated, and thus, would not be appropriate at the 0.87 mg/L concentration that
represents the national average fluoride concentration for public water systems (Section 3.3)
because it falls within the recommended fluoridation range. Professional dental fluoride
treatments are episodic and do not contribute greatly to the average daily intake when normalized
88 December 2010
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across time. The major chronic-use, fluoride-containing pharmaceuticals (i.e. Zocor and Prozac)
do not include young children among their target population. Intakes of the antibiotic
Ciptoflaxozin (Cipro) by children would be episodic rather than chronic. In addition, the
covalently-bound fluoride in pharmaceuticals does not appear to be bioavailable (NRC, 2006).
After consideration of the strengths and weaknesses of the studies presented in the preceding
sections of this report, EPA selected the data from one or two studies to represent the fluoride
intake for each of the age groups used in assessing the dose-response for severe dental fluorosis
(U.S. EPA, 2010a). In making the selection of the representative study EPA applied the
following guidelines:
Where possible a study from the United States was selected over a study from
Canada.
The publication had to report that plain water was not included in the market basket
or duplicate diet.
Where there was no study that clearly eliminated plain water from the market basket
in the study description, the study location with the lowest drinking water fluoride
concentration was selected and the uncertainty introduced noted.
Market basket approaches were preferred over duplicate diet or recall studies because
they were considered to be more geographically representative.
Studies considered for use as representative for toothpaste were those where the
ingested toothpaste was measured.
The study methodology and the ages of the children studied were both considered:
methodology was given a higher weight in the selection process than age in
situations where there were several study options for an age range.
The value selected and the rationale for its selection are provided in Tables 6-1, 6-2, 6-3, and 6-4
for solid foods, beverages, plain drinking water, and toothpaste, respectively. Soil ingestion by
young children was determined using an average soil concentration of about 400 ppm (see
Section 5.3) and the EPA estimates of 60 or 100 mg/day for soil ingestion by young children
(U.S. EPA, 2008). Each value is reported to a hundredth of a mg/day due to the analytical
limitations inherent in the representative values.
6.1. Dietary Intake
Foods. The food category includes milk and fruit and vegetable juices that are not made from
concentrate. Milk and such juices are not categorized as beverages by the FDA Total Diet Study
(Egan et al., 2007).
Data from Ophaug et al., (1985) and Jackson et al. (2002) were selected as representative for all
but adults in Table 6-1 below. These studies used a market basket approach in the analysis of
food for their fluoride content. Intakes for the non-beverage food groups come from the USDA
(1998) Continuing Survey of Food Intakes by Individuals (Jackson et al., 2002) or its precursor
USDA (1968) survey of food consumption. The Ophaug et al. (1985) data are used for the 0.5-
to
-------
than the data selected because of the study design and the small number of participants. In
addition, Brunetti and Newbrunn (1983) did not separate the fluoride from beverages from that
for solid foods.
Table 6-1. Estimated Daily Dietary Fluoride Intakes from Solid Foods for Age Groups of Concern
Age
(years)
0.5 -<1
l-<4
4-<7
7-14
Exposure
Estimate
(mg/day)
0.25
0.16
0.35
0.41
0.47
0.38
Rationale
Ophaug et al., 1985 - Overall mean (0.17 mg/day) from 22 market baskets, and
national food intake data (Table 2-24); does not include F from plain water and
beverages. These data were adjusted by subtracting the average for the milk and the
average for formula and other dairy products of 0.06 mg/day from (Ophaug, 1980a
Table 2-23) and replacing it with 0.14 mg/day from the powdered formula (Van
Winkle et al., 1995) [ 0.17 - 0.06 + 0.14 = 0.25]. The Ophaug et al. (1985) data apply
to 6-month-old infants.
Ophaug et al., 1985 - Overall mean of 22 market baskets, and national food intake
data; does not include plain water and beverages (see Table 2-31). Based on 2-year-old
children. This value is slightly greater than the average of the means (0. 13 mg/day)
from the less representative Rojas-Sanchez et al. (1999) duplicate plate analysis using
data for 54 children from three cities covering a larger segment of the age range 1 .3-
3.3 years. The Ophaug et al. (1985) estimate, although an older study, had a broader
geographic representation.
Jackson et al. (2002). Average of 2 market basket values (0.350 and 0.357 mg/day)
excluding plain drinking water and beverages. Based on 3- to 5-year-old children.
The estimate for this age group is based on the mean F concentration for food groups
from two market baskets in the study by Jackson et al. (2002) and USDA (1998) data
on food group intakes for the 6-1 1 year age group. It does not include plain drinking
water or beverages.
The estimate for this group is based on the mean F concentration for food groups from
two market baskets in the study by Jackson et al. (2002), and USDA ( 1 998) data on
food group intakes for the 12-19 year age group. It does not include plain drinking
water or beverages.
Average of the exposure estimates of Singer etal., (1980, 1985) andTaves (1983). All
estimates but Taves (1983) are based on 15- or 16- to 19-year-old males. The Taves
study was a six-day duplicate diet type representing an adult regular hospital diet.
In the case of the 0.5 to one year old group, the exposure value for foods applies to formula-fed
children in cases where the formula is a powdered product reconstituted with tap water. Only the
fluoride in the powdered formula, not that in the tap water used to reconstitute the formula, is
included in the food value in Table 6-1. Powdered formula is the most prevalent product chosen
(-90%) by parents who use formula according to the HHS Infant Feeding Practices Study (Table
3-15, CDC, 2009).
As described in the table, the food value for this age group was calculated by adding the average
of the four city average intakes from milk to the average of the four city average intakes from
other dairy products and formula (0.06 mg/day; Table 2-23) and subtracting the sum from the
food total (0.17 mg/day; Table 2-24), and then adding the amount from the powdered formula
(0.14 mg). The water added to reconstitute the formula is included in the drinking water
exposure (Table 6-3). The relative contribution of fluoride in the powdered formula versus the
added water depends on the concentration present in the water as well as the concentration in the
powder. When the water is fluoridated it accounts for more of the exposure than the powdered
formula.
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December 2010
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The reported food value in Table 6-1 represents a child with no intake of fluoride from milk or
other dairy products. In many cases children begin to consume milk rather than formula as they
approach their first birthday. Total fluid feeding of infants begins to decline at about 5-months as
the intake of solid foods increases; at 9 months only about 10% of infants are being given a fluid-
only diet. (Grummer-Strawn et al., 2008) This is not reflected in Table 6-1 making the estimate a
conservative one.
Using the data from Van Winkle et al. (1995 Table 2-3) to represent a soy-based powdered
formula will increase the fluoride intake for soy-based, formula-fed children 0.5 to 1 years old by
0.1 mg/day to 0.36 mg/day. The mean value for powdered soy-formula preparations reported by
Siew et al. (2009, Table 2-4) had lower fluoride concentration and would lower the total fluoride
from the powdered concentrate by 0.03 mg/day.
There is a lack of appropriate data from published studies of the 7- to <11-year and 11- to 14-
year age groups. Accordingly, local fluoride food-group concentrations from the Jackson et al.
(2002) study were combined with national USDA (1998) food intake data for the closest age
range and used to represent these age groups (Tables 2-34). Food product information in the
USDA (2005) database is too limited to support OW development of a market basket to apply
with age groups that lack primary data. The value for the 11 to <14 year old age group is a
conservative estimate since the USDA (1998) food intake data apply to the 12 to 19 year age
group. High food intakes associated with the teenage growth spurt will tend to cause averages
for 12-19 year old children to be higher than those for 11 to <14 year old children.
The adult data available for fluoride intake from foods were limited to an analysis based on
hospital diets of limited scope (Taves, 1983) and three market basket surveys (San Filippo and
Battistone, 1971, Singer et al., 1980, 1985). Each of the market basket surveys was based on
teen-aged male adolescents as the population of interest. This age group tends to have a higher
caloric and food intake than adults > 20 years old. Singer at al. (1980) found that the colorimetric
method used for fluoride analysis by San Filippo and Battistone (1971) produced higher fluoride
concentrations than those obtained for the same homogenates using an ion-specific electrode.
This is likely the reason that the San Filippo and Battistone results are about 0.3 to 0.4 mg/day
higher than those from the other three studies. Because of the weaknesses in the San Filippo and
Battistone (1971) data, EPA chose to average the results of the other three studies together as
representative of average adult intakes from foods (0.40 + 0.42 + 0.33 mg/day + 3 = 0.38
mg/day).
The uncertainties in the exposure estimates in Table 6-1 are acknowledged. However, despite
the limitations found in the available data set, the pattern of fluoride intake is consistent with the
expected pattern for food and calorie intakes that apply to the individual age groups. The
mg/day intake for infants whose primary food source is formula made from a powdered
concentrate was higher than that for the 1-3 years age group with a more mixed diet. The
estimates for the other age groups were higher than that for infants, increasing with age as caloric
requirements and food intake levels increase.
Beverages. As was the case for the food estimates, EPA selected a single value from the
beverage data (Table 2-46) to represent the intakes for each age group of interest. The values
selected and selection rationales are presented in Table 6-2. Estimates represent a combination
91 December 2010
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of fluoride from commercial beverages and beverages prepared at home using tap water. As was
the case for the food, the beverage estimates are given to the hundredth of a mg/day in
recognition of the analytical limitations for the studies that provided the representative values.
Table 6-2. Estimated Daily Fluoride Intake from Beverages Only for Age Groups of Concern
Age
(years)
0.5 -<1
l-<4
4-<7
7-14
Exposure
Estimate
(mg/day)
-
0.36
0.54C
0.60
0.38
0.59
Rationale
No value. All fluoride intake was considered to be from powdered formula (Table 6-1)
prepared with tap water (The tap water fluoride concentration is in Table 6-3).
Mean value from Pang et al., (1992); 3-day drink diaries (n=57); beverages store-bought or
made with de-ionized water. Milk and plain drinking water were excluded. Based on 2-3
year olds.
Mean value from Pang et al., (1992); 3-day drink diaries (n=79); beverages store-bought or
made with de-ionized water. Milk and plain drinking water were excluded. Based on 4-6
year olds.
Mean value from Pang et al., (1992); 3-day drink diaries (n=89); beverages store-bought or
made with de-ionized water. Milk and plain drinking water were excluded. Based on 7-10
year olds.
Derived from Jackson et al. (2002). Data for fluoride in the beverage food group were
combined with USDA (1998) data on beverage intakes to estimate fluoride exposure. Does
not include plain drinking water. Applies to ages 12-19. The Jackson et al. (2002) estimate
is supported by the Clovis and Hargreaves (1988) data from a dietary record Canadian
study covering six-grade students, average age -12 years (range of 0.02 to 0.82 mg/day).
Singer et al., (1985); based on 5 market baskets from different areas of the country and
excluding plain drinking water. The average water fluoride level was 0.14 mg/1 ± 0.03.
Based on data for 15-19 year-olds.
There is no beverage intake estimate for the 0.5 to
-------
0.12 mg/day for the 4 to < 7 year age group and a value of 0.22 mg/day for the 7 to < 11 year age
group. The Pang et al. (1992) exposure estimate falls above the mean and 90th percentile levels in
the Levy et al. (2003a) study and above the average values from Jackson et al. (1995).
Accordingly it is a conservative value for fluoride intake from beverages.
The average male/female fluoride intake from beverages in the low fluoride town (0.16 mg/L;
Connorsville, IN; Table 2-34) studied by Jackson et al. (2002) is used for the 11 to 14-year age
group in the absence of other data. The Jackson data do not include fluoride from plain drinking
water but do include fluoride from bottled water. This estimate may be slightly high since the
beverage intakes apply to 12 to 19 year old adolescents and the local water was not totally free of
fluoride. Inclusion of bottled water is expected to have a minimal impact on the fluoride intake.
The USDA (2005) database indicates that commercial bottled waters are low in fluoride.
The beverage exposure estimate for adults is from Singer et al. (1985) for the 5 cities with the
lowest drinking water fluoride levels (average 0.14 mg/L). It was selected as representative of
intakes in communities with low fluoride in their drinking water and therefore in home prepared
beverages. The Taves (1983) estimate of (1.38 mg/day) and that of San Fillipe and Battistone
(1971; 1.34 mg/day) were higher. The San Fillipe and Battistone data were not selected because
it included plain drinking water and used a colorimetric assay for fluoride analysis which is less
accurate than the ion-specific electrode used by Singer et al. (1985). The Taves (1983) estimate
was based on house diets for adults in a hospital setting. Taves (1983) attributed the high fluoride
levels to the fact that the hospital diets included daily servings of orange juice, coffee, and two
servings of tea, as well as other juices. The Taves data demonstrate that tea was the major
contributor to the fluoride intake from beverages. All of the adult data are from studies where
tap water was used for home beverage preparation.
6.2. Drinking Water
Table 6-3 provides the estimates for fluoride intakes from plain drinking water and the indirect
water that is used in the home preparation of beverages and foods when it is part of a standard
recipe. Following the RSC policy, the drinking water contribution is determined from the
average fluoride concentration from public drinking water systems as reported to EPA through
the ICR for the second six-year review of regulations combined with 90th percentile drinking
water intakes. The data apply to consumers only at the 90th percentile intake level. The average
water concentration (0.87 mg/L) was derived from 16 monitoring quarters covering the years
2002 through 2005 as described in Section 3.3. The drinking water intake data come from EPA
(2004) rather than the EPA (2008) Child-Specific Exposure Factors Handbook because the age
ranges in EPA (2004) match those used in the EPA (2010a) dose-response assessment for severe
dental fluorosis while those in EPA (2008) do not. Both EPA (2004) and EPA (2008) are based
in CSFII 1994-1998 water intake data.
93 December 2010
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Table 6-3. Fluoride Intake from Consumption of Municipal Water (Direct and
Indirect") at the Average Concentration (0.87 mg/L) Determined from Monitoring
Records for 2002 through 2005
Group
(yr)
0.5-0.9
1-3
4-6
7-10
11-14
14+
Water Consumption"
90th Pecentile Intake
Total mL
971
723
943
993
1415
2000b
Fluoride Intake"
mg/day
total
0.84
0.63
0.82
0.86
1.23
1.74b
SOURCE: Adapted from U.S. EPA, 2004.
Consumers only value.
bValue for the 14+ age group - EPA policy for adults.
6.3. Toothpaste
There are a number of studies that report on toothpaste use and resultant potential total exposure
from fluoridated dentifrice. A more limited set of data are available from studies where the
ingestion of toothpaste during tooth brushing was measured. In the toothpaste ingestion studies,
the toothpaste placed on the toothbrush was measured and corrected for that left on the
toothbrush after brushing and that expectorated during post-brushing rinsing of the mouth. The
difference was assumed to be swallowed. The data from these studies are summarized in Table
6-4. Each estimate is highly uncertain since the confidence bounds around the mean values are
indicative of high inter-individual variability (See Table 4-9). Estimates may be high because the
studies were conducted before the recommendation became widely publicized for children to use
only a pea-sized amount of toothpaste when brushing.
Table 6-4. Age-Related Exposure Estimates for Fluoride from Toothpaste
Age
(yr)
0.5 -<1
l-<4
4-<7
7-
-------
Fluoride intakes represent one brushing per day, a value that is applicable to about half the
population for children < 3 years old according to the data collected by Franzman et al. (2006),
Levy et al. (1997), and Simard et al. (1991). The number of brushings appears to increase to
twice a day for older children (Simard et al., 1989) but this estimate lacks confirmation from
other studies. Increasing the number of brushings per day for children to 2 would double the
intake estimates.
6.4. Soils
Although concentration varies with local geological conditions, 400 ppm was been identified as a
reasonable estimate for an average fluoride concentration in soils (ATSDR, 2003). Based on this
concentration and a combined soil and outdoor dust ingestion rate of 60 mg/day for children < 1
year old (U.S.EPA, 2008) the fluoride intake for an infant (<1 year) would be 0.02 mg/day. The
comparable fluoride intake for the 0-14 year age groups would be 0.04 mg/day using the 100
mg/day estimate for intakes of soil and indoor dusts (U.S. EPA, 2008). The fluoride RSC
assessment considers children older than 14 to be grouped with adults since they are no longer
vulnerable to severe dental fluorosis. The estimated intake for adults in the EPA (1997)
Exposure Factors Handbook is 50 mg/day and equivalent to a 0.02 mg/day intake from soils with
an average concentration of 400 ppm. Lower fluoride concentrations in soil are likely the norms
for areas of the country with minimal geological fluoride.
6.5. Uncertainty
There are many uncertainties in the estimates EPA selected for the RSC analysis related to
analytical methods and study protocols. In addition, the food preferences and food intakes of the
U.S. population shift as new products are introduced into the market-place and the dietary
intakes change. The past thirty years have seen an increase in the use of pre-prepared
commercial foods by the average consumer, increased imports of fresh produce from foreign
countries, and more frequent eating of meals away from home at restaurants, schools and daycare
facilities. Accordingly, the data from the selected studies (published between 1980 and 2002) are
not necessarily representative of current food preferences and intakes.
Additional uncertainties in the exposure estimates are due to the lack of published studies that
provide an exact match to the age ranges used in this analysis. Some of the data come from very
localized areas whereas other studies collected food and beverage samples representing different
geographical areas across the country. The concentrations of fluoride in the water used in food
preparation were not always identified; in cases where the fluoride in the water was identified,
the resultant concentrations in the finished foods did not always show a consistent relationship to
the drinking water concentration. Each of these factors contributes to the uncertainty in the
representative values chosen.
In recognition of the multiple uncertainties affecting the data, EPA has selected values that are
representative of average to slightly above average fluoride intakes for the RSC analysis. EPA
believes that these are reasonable estimates.
In addition to the methodological variables influencing the intake assessment, there are also
uncertainties about the bioavailability of fluoride in the diet. The solubility product constants for
95 December 2010
-------
calcium and magnesium fluoride are low and can limit fluoride absorption from foods that
contain these cations. Spak et al. (1982) found that 72% of the fluoride in milk and 65% of the F
in formula were bioavailable by measuring the fluoride levels in plasma after ingestion. Cury et
al. (2005) found the gastrointestinal absorption of fluoride in an ingested toothpaste slurry was
lower when slurry ingestion occurred directly after a meal than when it was consumed after
fasting. Hydroxyfluoroapatite, the form of fluoride found in bone, has a low solubility product
constant. Thus, when ashed for analysis, any meat, poultry, or fish products that may have
contained bone fragments would contribute to an overestimate of the bioavailable fluoride in the
product as consumed.
One major limitation with the food and beverage data reported in Tables 6-1 and 6-2 is the
studies were all conducted before the approval of sulfuryl fluoride as a fumigant for food storage
facilities and food processing plants. Accordingly, any fluoride currently in the food supply
because of sulfuryl fluoride fumigation is not reflected in those data. The OPP (U.S. EPA,
201 Ob; see Appendix B) provided OW with estimated contributions of fluoride to the food
supply from sulfuryl fluoride data (Table 6-5). As was the case for Tables 6-1 through 6-4,
fluoride residues are reported to the hundredth of a mg/day.
Table 6-5. Sulfuryl Fluoride Contributions to Dietary Fluoride Exposure.
Population Group
0.5- <1 year
Children 1 - <4 yrs
Children 4 - <7 yrs
Children 7 -<11 yrs
Youth 11-<14 yrs
Adults >14
Exposure Estimates, mg/day
Structural
Fumigations
0.01
0.01
0.02
0.02
0.02
0.02
Food
Fumigations
0.02
0.03
0.05
0.05
0.07
0.06
Total
0.03
0.05
0.06
0.07
0.09
0.08
SOURCE: U.S. EPA, 2010b
96
December 2010
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7. Relative Source Contribution (RSC)
The OW has followed the general principles for RSC determination outlined in the Ambient
Water Quality Criteria Human Health Methodology (U.S. EPA, 2000b) when determining the
RSC from drinking water intake for fluoride. According to OW policies, the subtraction
approach to RSC determination is not appropriate because of the OPP registration of pesticides
(cryolite, sulfuryl fluoride) that limit fluoride residues on treated food products (See Section 1.2
of this report). Accordingly, the percentage approach was applied.
The RSC for water from public systems is calculated using the following equation:
DWI x 100
DWI + FI + BI + DI + SI
where:
DWI = Intake from consuming water (direct and indirect) with an average of 0.87 mg/L F (see
Section 3.3) by the 90th percentile consumer
FI = Average intake of F from dietary foods except for beverages
BI = Average intake of F from beverages (commercial and prepared with tap water)
DI = Average intake of F from toothpaste use
SI = Average intake from soils and outdoor dust
Exposures from ambient air are not included in the RSC equation because they are a minor
contributor (< 4 jig/day) to the total exposure estimate (Section 5.1.2). Based on the NRC
estimated urban air concentration, the contribution of fluoride from air is <0.3% of the total
exposure for a young child and < 0.1% of the total for an adult. Fluoride intakes from
supplements are also not included because the average drinking water concentration falls within
the recommended range for fluoridation of drinking water, and supplements are not
recommended for those who receive fluoridated drinking water (see Section 5.2).
Table 7-1 provides the representative values for intakes of fluoride through each quantified
medium for each age group of interest as well as the total fluoride intake and the percentage
contributed by direct and indirect drinking water residential tap water. The 90th percentile
drinking water intakes (consumers only) are used for all age groups as it is U.S. EPA policy to
protect the majority of the population. The drinking water fluoride concentration is the average
for all systems detecting fluoride. Average values are used for the fluoride contributions from
the other media as required by (EPA, 2000b). Exposure estimates are presented at the one
hundredth of a milligram intake level because of the analytical uncertainties surrounding the
representative data selected.
97 December 2010
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Table 7-1. Representative Values for Fluoride Intakes Used in Calculation of the Relative Source
Contribution for Drinking Water
Age
Group
(years)
0.5- <1
1- <4
4- <7
7- <11
11-14
>14
DWF
(mg/day)
0.84
0.63
0.82
0.86
1.23
1.74
FI
(mg/day)
0.25b
0.16
0.35
0.41
0.47
0.38
BI
(mg/day)
-
0.36
0.54
0.60
0.38
0.59
TI
(mg/day)
0.07
0.34
0.22
0.18
0.20
0.10C
SI
(mg/day)
0.02
0.04
0.04
0.04
0.04
0.02
Total
(mg/day)
1.19
1.53
1.97
2.09
2.32
2.83
RSC
(%)
71
41
42
41
53
61
Consumers only; 90th percentile intake except for >14 years. The > 14 year value is based on the OW policy of 2 L/day.
blncludes foods, F in powdered formula, and fruit juices; no allocation for other beverages.
"Assumed to be 50% of the value for the 11-14 year old age group.
DWI = Drinking Water Intake (see Table 6-3).
FI = Food Intake (Solid Foods) (see Table 6-1).
BI = Beverage intake (see Table 6-2).
TI = Toothpaste Intake (see Table 6-4).
SI = Soil Intake (see Section 6.4).
Table 7-1 does not include consideration of any residues from the use of sulfuryl fluoride, a
fumigant that was approved for use on food products after all of the dietary data used for this
report were collected (U.S. EPA, 2009b). A separate calculation that includes estimation of
fluoride residues from sulfuryl fluoride (SuF) is provided in Table 7-2. Sulfuryl fluoride
decomposes in the environment to produce sulfate and fluoride ions. The OPP (U.S. EPA, 2009;
201 Ob) has provided the OW with estimates of fluoride residues from the currently approved
uses of this product which include fumigation of food storage facilities and processing plants, as
well as direct fumigation of some foods for pest control purposes. Table 7-2 shows the results of
the RSC calculation when sulfuryl fluoride residue is included in the RSC analysis.
Table 7-2. Representative Values for Fluoride Intakes (Including Sulfuryl Fluoride) Used in Calculation
of the Relative Source Contribution from Drinking Water
Age
Group
(years)
0.5 -<1
1- <4
4-<7
7- <11
11-14
>14
owr
(mg/day)
0.84
0.63
0.82
0.86
1.23
1.74b
FI
(mg/day)
0.25b
0.16
0.35
0.41
0.47
0.38
SuF
(mg/day)
0.03
0.05
0.06
0.07
0.09
0.08
BI
(mg/day)
0.36
0.54
0.60
0.38
0.59
TI
(mg/day)
0.07
0.34
0.22
0.18
0.20
0.10C
SI
(mg/day)
0.02
0.04
0.04
0.04
0.04
0.02
Total
(mg/day)
1.21
1.58
2.03
2.16
2.41
2.91
RSC
(%)
70
40
40
40
51
60
Consumers only; 90th percentile intake except for >14 years. The > 14 year value is based on the OW policy of 2 L/day.
blnchides foods, F in powdered formula, and fruit juices; no allocation for other beverages.
"Assumed. 50% of the 11-14 year old age group.
DWI = Drinking Water Intake (see Table 6-3).
FI = Food Intake (Solid Foods) (see Table 6-1).
SuF = Sulfuryl Fluoride Intake (see Table 6-5)
BI = Beverage Intake (see Table 6-2).
TI = Toothpaste Intake (see Table 6-4).
SI = Soil Intake (see Section 6.4).
98
December 2010
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Figure 7-1 illustrates the percentage contributed by each of the media in Table 7-2 to daily total
fluoride intake. It is apparent that, for most individuals in the population, the contribution from
drinking water is substantially less than the 100% assumed in the EPA 1986 derivation of the
MCLG for crippling skeletal fluorosis. However, the contribution from drinking water for adults
who are not at risk for dental fluorosis (60%) is greater than the limiting value for children (40%)
who are susceptible to severe dental fluorosis.
100%
90% -
80% -
70% -
60% -
50% -
40% -
30% -
20% -
10% -
0.5 to
1 to <4
4to<7
7to<11
11 to 14
Years
DWater BFood DBeverages DSulfuryl fluoride DToothpaste DSoils
Figure 7-1. Percentage Media Contribution to Total Daily Fluoride Intake: 90th Percentile
Drinking Water Intakes for Consumers Only and a Fluoride Concentration of 0.87 mg/L
Drinking water contributes the highest percentage of the total fluoride intake (70%) for infants
six months to one year old. However, the high percentage contribution of drinking water for this
age group is partially a consequence of the use of the intakes for infants fed exclusively with
powdered formula reconstituted with tap water containing 0.87 mg/L fluoride for this analysis.
The food intake data for the 0.5 to 1 year old age group came from a study of six-month old
infants (Ophaug et al., 1985) as described in Table 6-1). This intake value also contributes to the
high percent of the total coming from drinking water because, at this stage of development, the
intake of formula is higher than that at one year when the typical infant's diet has expanded to
include a variety of solid foods and juices.
The diet (solid foods, beverages, and sulfuryl fluoride) is another major contributor to total
fluoride intake with sulfuryl fluoride making a minor contribution to the total. It is the largest
contributor for children ages 4 to <1 1. However, dietary fluoride is indirectly impacted by the
99
December 2010
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fluoride in drinking water because cooking and preparing foods in fluoride-containing water
increases the fluoride content of the prepared food (Maier and Rose, 1966; Ophaug et al., 1985).
Many food and beverage production facilities use fluoride-containing water in food preparation.
When there is fluoride in the water supply, some of it will end up in the food supply. This is
particularly true for beverages. The work by Ophaug et al. (1985) found that correlation
coefficients between beverage fluoride and the drinking water fluoride concentration ranged
from 0.72 to 0.98 for the four quadrants of the country. There was not a strong correlation
between the drinking water fluoride and the fluoride content of solid foods (Ophaug et al., 1985)
although cooking studies have shown uptake from the preparation water (Martin, 1951).
As discussed in Section 6, there are alternative estimates for the contribution of fluoride from
beverages, excluding plain drinking water, for children in the 4 through <11 year age groups.
The alternative estimates are lower than the values from the Pang et al. (1999) diary-based study
selected by EPA. They are 0.2 mg/day from Levy (2003a) and 0.12 from Jackson et al (1995)
for the 4 through <7 year group and 0.22 from Jackson et al. (1995) for the 7 to <11 year age
group. When the RSCs for drinking water were calculated with these values in place of the Pang
et al. (1999) data, the RSC values changed from 40 and 39% to 49/51 and 48%.
The relative source for drinking water would also be affected by the use of a soy-based powdered
formula rather than a milk-based powdered formula by children in the 0.5 to 1 year old age
group. Under this circumstance the drinking water RSC will decline from 70% to 64% if the
soy-formula data from Van Winkle et al. (1995) are used.
Geologically, one-third to one-half of the U.S. has access to ground water containing less than
0.5 ppm fluoride (See Figure 3-1), while surface waters exhibit lower geochemical fluoride
levels. However, currently, about 69% of U.S. population receives fluoridated water (CDC,
2008), where the natural fluoride level has been augmented through the addition of certified
fluoridation chemicals to attain final fluoride concentrations that range between 0.7 and 1.2
mg/L. Consequently, the average fluoride concentration in the nation's drinking water has
increased from what it was before systems began the practice of fluoridating drinking water on
an experimental basis in 1945 as a public health measure to lower cavities for children and adults
(CDC, 1999).
Figure 7-1 indicates that existing data and estimates regarding sulfuryl fluoride in food items
support a determination that sulfuryl fluoride is a minor contributor to the diet at current use
levels. Recent identification of sulfuryl fluoride as a greenhouse gas (Papadimitriou et al., 2008;
Anderson et al., 2009; Miihle et al., 2009) could limit future projected increases in SuF use.
After drinking water and diet, third in contribution to total fluoride intake for humans is
toothpaste (Figure 7-1). Most recently introduced in 1955 as a measure to increase protection
against dental cavities (Procter and Gamble, 2009), fluoridation of toothpaste with sodium
fluoride, monofluorophosphate, or stannous fluoride has grown so that by 1989 almost 95% of
the toothpaste sold to the U.S. market was fluoridated (Newbrun, 1989). The relative
contribution of fluoride in toothpaste to total intake is highest (21%) for children in the 1- to 3-
year age group. This is a consequence of poor swallowing control by children in this age range
(Levy et al., 2001). Ingestion of fluoride from toothpaste decreases linearly with increased age as
control of swallowing and expectoration reflexes mature (Figure 7-1).
100 December 2010
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The estimates of average ingestion of fluoride from toothpaste are more uncertain than those for
food and drinking water. There are several factors that contribute to the uncertainty including
frequency of brushing, the amount of toothpaste used, and individual variability in use. The data
in Figure 7-1 represent average values per brushing and a single brushing per day. In U.S.
studies of the 1-3 year age group (Levy et al., 1997; Franzman et al., 2006) about 20 to 30 % of
children brushed more frequently (Table 4-9). Estimates for population groups greater than 3-
years also assume one brushing per day. Data on the frequency of brushing were not identified
for school-aged children and adults but a substantial portion of those groups is likely to brush
their teeth at least twice a day. Increased brushing frequency would increase intake contributed
by toothpaste and its percent of the total. When the data were analyzed using estimates for two
brushings per day for all age groups >7 years of age, the RSC values for drinking water
decreased from 40, 40, 51 and 60% to 36, 37, 47 and 58%. None of these changes was
substantial.
Another variable impacting the estimate is the amount of toothpaste placed on the toothbrush.
The studies used to quantify the intake were conducted before the guidance (ADA, 1991) to
reduce the toothpaste applied from a ribbon to a pea-sized portion was publicized and do not
reflect the FDA (2009) recommendation that children younger than 2 years not use toothpaste
when brushing their teeth. Decreasing the amounts of toothpaste applied to the toothbrush
decreases the fluoride ingested. Finally, all of the dentifrice studies showed that there was high
inter-individual variability among the subjects as indicated by the wide confidence bounds on the
average values (see Table 4-8). Thus, there is considerable uncertainty in the toothpaste
estimates.
Normalized daily intakes of fluoride from soils, indoor dust, ambient air, fluoride-containing
Pharmaceuticals, episodic dental treatments, and cigarette smoke are minor contributors to total
exposures for the average children and adults. Use of fluoride-containing mouthwashes,
particularly by children in the 1-7 year age group, is an unquantified exposure that could
measurably increase the total estimates from Table 7-2. Mouthwash contributions were not
quantified because of a lack of data. In 1983, the now dated National Health Interview Survey
found that 5% of children under 5 used mouth rinses, as did 17% of children ages 5 to 17.
However, this survey did not estimate fluoride intakes from such products and intakes from
fluoridated mouthwashes are not included in the RSC analysis.
101 December 2010
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8. Relationship of Exposure Estimates to Dietary Guidelines
Although, the contributions of various individual media to total fluoride intakes are important,
the total intake is even more important from a public health perspective. Fluoride is a
nutritionally-active substance with beneficial properties for both teeth and bone (IOM, 1997).
Accordingly, total intakes should provide adequate fluoride to meet dietary guidelines without
leading to severe dental fluorosis in children and skeletal problems in adults.
8.1. Estimates of Daily Dietary Needs.
The National Academy of Sciences (NAS) provided dietary guidelines for fluoride beginning in
1989 (NRC, 1989). The most recent guidelines (Dietary Reference Intakes; IOM, 1997)
established Adequate Intake (AI) recommendations for age groupings from infants through
adults. The AI is the recommended average daily intake based on observed or experimentally
determined approximations, or estimates of adequate nutrient intakes by a group (or groups) of
apparently healthy people. The AI is used when a Recommended Dietary Allowance (RDA)
cannot be determined because the data are not sufficient to establish average dietary needs based
on a biological measure of a person's nutritional status. In the case of fluoride, an easily
monitored biological measure of adequacy has not been established.
The AI for fluoride was based on the estimated dietary intakes that have been shown "to reduce
the occurrence of dental cavities maximally in a population without causing unwanted side
effects including moderate dental fluorosis." IOM (1997) determined that the role of fluoride in
protecting tooth enamel, stimulating bone growth, and preventing calcification of soft tissues
justified the development of dietary guidelines.
Table 8-1 provides the AI values for each age grouping targeted by IOM and compares the AI
levels to the total dietary fluoride intake estimates from Table 7-2. The AI estimates for fluoride
include drinking water and identify it as a major contributor to total fluoride (IOM, 1997). It is
clear from these data that EPA estimates of current total F intakes meet the AI recommendations
for infants, children through age 14, and females, but are below the AI recommendation for adult
males.
IOM (1997) did not consider dental decay as a biomarker for low fluoride exposure because
decay is associated with a variety of factors and cannot be attributed solely to low fluoride
intakes. The AI for infants is based on the daily mean intake of a nutrient from human milk by
exclusively breast-fed, healthy infants (IOM, 1997). Intakes from drinking water are included in
the AI for fluoride for other age groups; in fact, the IOM (1997) considered ingested drinking
water to be the major contributor to total dietary intake.
102 December 2010
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Table 8-1. Comparison of Total Fluoride Intake Estimates to the Dietary
Adequate Intake (AI).
Age Range"
(years)
0.5 -<1
l-<4
4-<7
7-
-------
mg/kg/day. A 0.01 mg/kg/day contribution from the diet, as derived from McClure (1943), was
added to the drinking water component to yield the 0.08 mg/kg/day RfD. The RfD derivation can
be found in the EPA (2010a) companion document, Fluoride: Dose-Response Analysis for Non-
cancer Effects.
The RfD (mg/kg/day) was converted to age-specific oral exposure benchmarks (mg/day) that
should be protective for severe dental fluorosis in most children and skeletal effects in most
adults using mean bodyweights for each age group from (EPA, 2004) as reported in Table 8-2.
They are compared in the table to both the IOM (1997) UL guidelines and the OW total daily
intake estimates from this document.
Table 8-2. Comparison of Total Fluoride Intake Estimates to the IOM (1997) Tolerable Upper
Intake Level and the OW Age-Specific Benchmarks
Age Group
(years)
0.5 -<1
l-<4
4-<7
7-8 year olds
(skeletal fluorosis)d
10
(skeletal fluorosis)
10
(skeletal fluorosis)
10
(skeletal fluorosis)
Intake Estimate
(mg/day)c
1.21
1.58
2.03
2.16
2.41
2.91
2.91
aThe OW benchmarks were established to protect against severe dental fluorosis in children up to age 14 and to
protect against skeletal fractures and skeletal fluorosis in adults.
bIOM UL values were established to protect against dental fluorosis up to age 8.
"From Table 7-2.
dThe IOM values for ages > 8 years were established to protect against skeletal fluorosis.
8.3. Exposure Profiles
-,th
The data in Table 8-2 indicate that some children drinking water at the 90 percentile intake
level up to about age 7 are being exposed to fluoride on a daily basis at levels at or higher than
estimated acceptable intake levels when the concentration of fluoride in their drinking water is at
or above 0.87 mg/L. Figure 8-1 shows the relationship between current intake estimates
(drinking water intake at the 90th percentile level) and the OW RfD-derived benchmarks in units
of mg/day. The RfD-derived benchmarks for each age group are shown as the solid black line in
Figures 8-1 through 8-4. When examining Figure 8-1 it is important to remember that the RfD
represents an exposure that is estimated to provide the anticaries benefits from fluoride without
causing severe dental fluorosis in 99.5% of the children who drink water with 0.87 mg/L F at a
90th percentile intake level and have average intakes from other media during the period of
secondary tooth formation. Based on the dose-response for severe dental fluorosis in EPA
(2010a) only 0.5% or fewer of children consistently ingesting fluoride at a levels equivalent to
104
December 2010
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the RfD for a several month period would be at risk of experiencing severe dental fluorosis in
two or more teeth.
0.5to<1
1 to<4
4 to <7
7to<11
Age Range in Years
Figure 8-1. Total Daily Fluoride Intake Estimates Relative to the Proposed RfD Using 90th Percentile
Drinking Water Intake Data for Consumers Only and the Mean Drinking Water Fluoride Concentration
(0.87 mg/L)
If the drinking water intake level is adjusted to an average intake to match the average values
used for the other exposure media, the relationship between exposure intakes and the RfD-
equivalent intake changes (Figure 8.2). Children with average intake of all media in the younger
age groups would still be slightly over exposed if the drinking water concentration were 0.87
mg/L. At higher concentrations in drinking water, the number of children at risk for severe
dental fluorosis would likely increase. Risk would also increase if the fluoride from any other
exposure media were greater than the values utilized by EPA in this assessment.
The OW RfD identifies a level of exposure that is considered to be acceptable for the general
population. Levels above the RfD are not necessarily unacceptable but risk is considered to
increase as the difference between the RfD-equivalent and the dose increases.
105
December 2010
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0.5 to
7to<11
Age Range in Years
Figure 8-2. Total Daily Fluoride Intake Estimates Relative to the Proposed RfD Using the Mean Drinking
Water Intake Data for Consumers Only and the Mean Drinking Water Fluoride Concentration (0.87 mg/L)
In any population, dietary intakes and food choices change from day to day. Each person's daily
fluoride exposure will be influenced by what they eat each day and how they brush their teeth.
No one is average on a continuous basis. Many people will consistently be exposed to higher
levels of each fluoride-containing medium others will consistently be exposed to lower levels
than depicted. Children in communities that routinely exceed the current SMCL for fluoride
during the period when their teeth are forming will be particularly vulnerable to developing
severe dental fluorosis. Figure 8-3 depicts the impact of an average drinking water intake for
consumers only and the 90th percentile fluoride concentration for all systems reporting
detections of fluoride. Figure 8-4 depicts the age-specific intakes for populations where drinking
water intakes are at the 90th percentile level and the fluoride concentration (1.76 mg/L) is the
average for those systems that reached or exceeded the SMCL of 2 mg/L at least once during the
last 4 years of the ICR monitoring period for the second six-year review of regulations (Table 3-
2). Children in areas of the country with high geological levels of fluoride and resultant higher
levels in their drinking water who are also at the high end of the drinking water intake
distribution are those with the greatest risk for severe dental fluorosis.
106
December 2010
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4to<7 7to<11
Age Range in Years
Figure 8-3. Total Daily Fluoride Intake Estimates Relative to the Proposed RfD using Mean Drinking
Water Intakes for Consumers Only and the 90th percentile Fluoride Concentration for all Systems
Reporting Detections of Fluoride.
4to<7 7to<11 11 to 14
Age Range in Years
Figure 8-4. Total Daily Fluoride Intake Estimates Relative to the Proposed RfD using 90th Percentile
Drinking Water Intakes for Consumers Only and Average Concentration (1.76 mg/L) for those
Systems that Reached or Exceeded the SMCL of 2 mg/L at Least Once During the ICR Monitoring
Period for the Second Six-year Review.
In the case of fluoride, there are data on prevalence of dental fluorosis to support a conclusion
that fluoride exposure levels among the population have increased in the last 40 to 50 years
107 December 2010
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resulting in an increase in dental fluorosis (lida and Kumar, 2009; CDC, 2005). The prevalence
of dental fluorosis has increased from 10-12% in the areas with about 1 mg/L in drinking water
at the time of Dean (NRC, 1993) to 23 % in 1986/87 (NRC, 1993; lida and Kumar, 2009) and to
32% in the 1999-2002 NHANES survey (CDC, 2005). The 1986/1987 data come from the
National Survey of Oral Health of U.S. School Children, which examined 40,693 subjects. The
NHANES survey included a smaller set of subjects (17,092) at ages greater than 2 years (CDC,
2005). Comparable data are not available for severe dental fluorosis.
The CDC (2005) report found that the prevalence of fluorosis was higher in the 12-15 and 16-19
year age groups during the 1999-2002 survey than in the 20-39 year old age groups, which may
be a reflection of recent increases in total fluoride exposure. The data also indicated that
posterior teeth were impacted to a greater extent than the visible anterior teeth and that there was
a higher prevalence among the Non-Hispanic African Americans than Non-Hispanic Caucasian
Population. Most of the fluorosis reported in the CDC (2005) report was very-mild or mild,
conditions that are associated with decreases in tooth decay. However, there were cases of
moderate/severe dental fluorosis combined and the percentages reported were higher for the age
groups younger than 20 years old than for older individuals indicating that increases in total
fluoride intakes may be relatively recent.
8.4. Summary of findings
The OW conducted the Exposure and Relative Source Contribution assessment in order to
determine the relationship of total fluoride intakes to the inorganic fluoride RfD from the
companion dose-response assessment (U.S. EPA, 2010a). The relative contribution of ingested
drinking water from public drinking water systems to total exposures was also examined.
The EPA MCLG/MCL for fluoride was established in 1986 and determined to be protective for
Stage III (crippling) skeletal fluorosis. The determination of the MCLG/MCL included an
assumption that drinking water contributed 100% of the exposure because the data used for
quantification were derived from measures of the fluoride in the drinking water among the cases
of Stage III skeletal fluorosis that provided the point of departure for the calculation.
The NRC (2006) examination of the MCL/MCLG for fluoride was an outgrowth of the first six-
year review of the 1986 fluoride drinking water regulation as mandated by the 1996 SDWA and
recognition by EPA of the number of scientific studies on the bone and dental effects of fluoride
that were published after the regulation (U.S. EPA, 2003). The NRC published the report of their
effort in 2006 as: Fluoride in Drinking Water: A Scientific Review of EPA 's Standards. The
NRC committee concluded that EPA's current MCLG of 4 mg/L for fluoride should be lowered
to reduce the risk of severe enamel fluorosis and minimize the risk for bone fractures and skeletal
fluorosis in adults. It charged the OW with conducting a dose-response assessment for the
critical noncancer effects of fluoride on teeth and bone (U.S. EPA, 2010a) and the exposure and
relative source assessment presented in this report. Through this effort, EPA has concluded that:
Some young children are being exposed to fluoride up to about age 7 at levels that
increase the risk for severe dental fluorosis.
The contribution of residential tap water to total ingested fluoride is lower that it was in
the past.
108 December 2010
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Use of fluoridated water for commercial beverage production has likely resulted in
increased dietary fluoride in purchased beverages, adding to the risk for over-exposure.
The increase of fluoride in solid foods because of fluoridated commercial process water
is more variable than that for beverages.
Incidental toothpaste ingestion is an important source of fluoride exposure in children up
to about 4 years of age. However, use of fluoridated toothpaste is not recommended for
children under age 2 according to FDA guidance and package labeling suggesting the
need for greater parental awareness of the FDA (2009) recommendations.
Ambient air, soils, and sulfuryl fluoride residues in foods are minor contributions to total
fluoride exposure.
Based on the data collected and evaluated by the OW, it is likely that most children, even those
that live in fluoridated communities, can be over-exposed to fluoride at least occasionally.
Children who live in communities where the fluoride concentration routinely falls between 2
mg/L and 4 mg/L have an even greater opportunity for over-exposure unless parents follow the
EPA public notification advice not to allow their children to routinely drink the tap water until
they are nine years of age (the upper age limit for the current public notification), and consult
with their dental professions regarding use of fluoridated dental products. The impact of the
elevated intakes on the risk for severe dental fluorosis in one or more teeth depends on the
timing, frequency and duration of the over-exposures.
The data from this report and its companion dose-response assessment (U.S. EPA, 2010a) will be
used by the EPA in order to determine whether lowering the MCLG and/or MCL for fluoride
will provide a meaningful opportunity to reduce the risk for severe dental fluorosis and skeletal
effects among populations served by public drinking water systems. The EPA is required to
consider whether the costs of reducing fluoride in public water supplies are justified by the
health benefits accrued through such a change. Regulatory decisions related to the MCLG and
MCL are separate from the assessment of hazard in the NRC (2006) report, the OW dose-
response report (U.S. EPA, 2010a), and this exposure and RSC document.
The OW's exposure and relative source contribution analysis accomplished each of its desired
objectives within the limitations of the data provided in the published literature and the
monitoring information from the second six-year review ICR data. The output of the analysis is
age-group specific for children at risk of developing severe dental fluorosis and is presented in a
format that will aid the OGWDW in characterizing opportunities for reducing population risk
from fluoride in public drinking water systems. The data are intended as a resource for
facilitating any necessary adjustment in the regulatory nonenforceable MCLG and enforceable
MCL.
It is important to remember, however, that the exposure quantification provided follows the
policy guidelines from EPA (2000b) using average exposure estimates for all media other than
drinking water, the average drinking water concentration for systems that detect fluoride, and
90th percentile drinking water intakes. Thus, the intake estimates are more representative of
average consumers than they are for individuals residing in areas of the country where the
average drinking water concentration falls between the 2 mg/L and 4 mg/L concentrations
allowed by the NPDWR rather than the 0.87 mg/L that is representative of the country as a
109 December 2010
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whole and for those where the drinking water has very low fluoride concentrations (< 0.1 mg/L).
For children residing in areas where the fluoride levels are close to the MCL (4 mg/L) the risk
for severe dental fluorosis is considerably higher. Some adolescents and adults receiving
drinking water that is consistently close to the MCL can easily exceed the 6 mg/day where the
risk for effects on bone are considered to be a concern (WHO, 2001).
110 December 2010
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APPENDICES
Appendix A: Fluoride Chronic Dietary Exposure Analysis
Appendic B: Sulfuryl Fluoride: Estimates of Fluoride Exposure from
Pesticidal Sources - Customized Age Groups
128 December 2010
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UNITED STATES ENVIRONMENTAL PROTECTION AGENCY
WASHINGTON, D.C. 20460
£
OFFICE OF PREVENTION, PESTICIDE
AND TOXIC SUBSTANCES
MEMORANDUM
Date: 6 May 2009
SUBJECT: Fluoride Chronic Dietary Exposure Analysis
PC Code: None
MRIDNo.: 47594701
Petition No.: None
Assessment Type: Single Chemical
TXRNo.: None
DP Barcode: 362183
Registration No.: None
Regulatory Action: None
Registration Case No.: None
CAS No.: 16984-48-8
FROM:
THROUGH:
Michael A. Doherty, Ph.D., Senior Chemist
Risk Assessment Branch II
Health Effects Division (7509P)
TO:
Background
Thurston Morton, Chemist
Mohsen Sahafeyan, Chemist
Dietary Exposure Science Advisory Council
Health Effects Division (7509P)
Christina Swartz, Branch Chief
Risk Assessment Branch II
Health Effects Division (7509P)
Michael A. Doherty, Ph.D., Senior Chemist
Risk Assessment Branch II
Health Effects Division (7509P)
The Agency's Office of Water (OW) is currently examining its drinking water standard for
fluoride (F). As part of that examination, they are determining relative source contributions for
fluoride exposure (i.e., how much fluoride comes from various sources such as toothpaste,
natural residues in foods, etc.). The Office of Pesticide Programs (OPP) has been asked to
supply OW with estimates of dietary exposure to fluoride that results from the use of pesticides.
OPP has identified two pesticides, cryolite and sulfuryl fluoride (SF), whose use results in
fluoride levels which may be elevated above background levels in treated foods. In 2006, OPP
completed an aggregate human health risk assessment for fluoride that addressed dietary
exposure to F from these two sources (M. Doherty, D312659, 18 January 2006). Since that time,
the registrant (Dow AgroSciences; DAS) for sulfuryl fluoride has provided the Agency with
Page 1 of30
-------
information that will support a more refined estimate of F exposure attributable to the use of
sulfuryl fluoride. This assessment incorporates refinements to fluoride residue levels, taking into
account the information from DAS, and examines the contribution of various crops and crop
groups to pesticidal F exposure. Note that because of the purpose of this assessment and the on-
going work by OW, this document presents exposure estimates for fluoride and not risk
estimates.
Executive Summary
Chronic dietary (food only) exposure assessments were conducted using the Dietary Exposure
Evaluation Model DEEM-FCID, Version 2.03 which use food consumption data from the U.S.
Department of Agriculture's Continuing Surveys of Food Intakes by Individuals (CSFII) from
1994-1996 and 1998. Two analyses have been completed for sulfuryl fluoride, the first to
address the structural fumigation uses, wherein foods may receive inadvertent treatment, and the
second to obtain estimates for the food uses of the product, wherein foods are intentionally
fumigated to treat pest problems. An additional, third analysis was conducted to determine the
food-specific contributions to F exposure due to the use of cryolite.
All analyses include the use of percent crop treated (% CT) information and incorporate
anticipated residues. The % CT and anticipated-residue values represent a range of refinements
in which some conservatism remains. As more data become available and are validated by the
Agency, further refinement to the exposure estimates may be possible. On the other hand, this
assessment departs to some extent from regular HED practice by using very low percent crop
treated estimates and anticipated residues predicted from data bearing on historical application
rates. Regulatory measures, such as frequent mandatory reporting, may be appropriate to insure
that usage and application rates do not change. Fluoride exposure estimates from pesticidal
sources range from 0.0015 to 0.0063 mg/kg/day, depending on the population subgroup.
I. Residue Information
Fluoride from Cryolite. Residue and % CT estimates in the cryolite assessment are identical to
those used in the previous assessment (M. Doherty, D309013, 12 October 2004). That
assessment is based on average residue values from field trials and incorporates %CT estimates
for the majority of the foods in the analysis. The resulting exposure estimates are considered to
be moderately refined. OPP notes that the analytical method used to obtain the residue estimates
in the cryolite field trials reports total fluoride and does not differentiate between the various
aluminum-fluoride species that may be present in the treated commodities. Therefore, the
residue estimates associated with the use of cryolite likely represent an overestimate of fluoride
anion residues resulting from cryolite use.
Fluoride from Sulfuryl Fluoride. As in previous assessments {e.g.., M. Doherty, D317731, 18
January 2006), average residue values from fumigation trials conducted at the maximum total
application rate of sulfuryl fluoride (1500 mg-h/L) were used to assess dietary exposure, except
as noted below. OPP has received a significant amount of data depicting F residues in foods at
various treatment rates, and for many foods there is a relationship between treatment rate and
terminal F residues. Dow AgroSciences maintains a database which tracks sites where sulfuryl
fluoride is used as well as various parameters associated with each fumigation, including the
actual treatment rates. For foods with demonstrable rate/residue relationships, the average
Page 2 of 30
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residues from trials at the maximum rate have been adjusted to their average-fumigation-rate
equivalent using linear regression (Table 1). The regression analysis, as described in the
submission, is as follows and is in line with OPP guidance for deriving anticipated residues
(USEPA/OPP, 15 June 2000):
[Regressions] were based on relative concentrations and relative dose levels. Specifically, within each
commodity, one or more samples treated at dose levels closest to the maximum label rate (1500 oz-hr) were
designated as "reference samples". Reference dose levels and reference concentrations were derived as the
average dose levels and concentrations associated with these reference samples. The dose levels and
concentrations associated with all samples were then expressed as relative dose level and relative
concentrations (percent of the reference dose level and of the reference concentration), and these relative
values were used in the linear regression models of the form:
Relative Concentration = a + b x Relative dose,
where a and b are the intercept and slope. The regression models described above were used to estimate the
anticipated concentration at the average (historical) dose levels summarized above. In addition, predicted
levels at the maximum dose rate of 1,500 oz-hr were also derived. Specifically, the concentration at dose
level D was derived as:
Concentration at Dose D = Reference concentration x [a + (b x Dose D/Reference dose)],
where a and b are the intercept and slope from the corresponding regression model. Note that regression
models were used only for commodities with more than two data points which spanned a range of at least
600 oz-hr and for which the regression p-value was 20% or lower. [The p-value of 20% was footnoted as
follows: The regression models for four commodities (cornflour, figs, raisins and white rice) hadp-values
lower than 20% but higher than the 5% level typically used to represent statistical significance.
Nevertheless, the regression models were used to predict concentration levels for these four commodities
because a visual examination of the data indicated a linear relationship between [dose] and residues. The
regression models produced conservative estimates of anticipated residues at the average [dose], since the
estimates were comparable to, if not higher than, the observed residues at the maximum [dose].}
For all foods in the analysis, DAS has used a correction factor to account for the inability of the
analytical method to measure total fluoride. The correction factor is commodity-specific and the
values range from 0.37 to 1.0. Residue estimates are divided by the correction factor to obtain an
estimated total fluoride concentration. The data used to obtain the correction factors are not
available to OPP at this time and therefore the factors cannot be verified. The factors, being < 1,
result in residue estimates that are greater than or equal to prior OPP assessments; therefore, OPP
is accepting them at this time without further review. The study should be submitted for review
by the Agency. EPA will revise residue estimates, as needed, following review of these data.
HED has verified the regression parameters and analysis presented by DAS and, except for
hazelnuts (filberts), concurs that the anticipated residues are not likely to underestimate actual
residues resulting from the use of SF at the average dose levels reported to date. Hazelnuts are
reported as having a regression with a negative intercept. Conceptually, the intercept represents
the background residue in the untreated matrix; therefore, a negative intercept does not make
sense from a residue perspective and is considered to be an artifact of the regression process.
Therefore, for hazelnuts, OPP has recalculated the anticipated residues assuming an intercept of
zero (the slope was not recalculated).
Sulfuryl fluoride currently has two use strategies (1) pest control in structures via structural
fumigations and (2) control of pests in foods via direct fumigation of foods. During structural
Page 3 of 30
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fumigation, facilities are to be emptied of foods to the extent possible. Nevertheless, there will
be some foods that remain in the structure and that will be inadvertently treated with SF. OPP is
assessing these two uses separately. Residue data are not available for a number of commodities
that may be treated with SF. For those commodities surrogate data have been used (e.g., the
residue estimate for figs is used for a number of other dried fruits). Residue estimates are
summarized in Table 5 for both the structural and food fumigation uses. As previously noted,
the residue estimates for fluoride coming from cryolite are identical to those used in the previous
assessment. A complete listing of the residue inputs is included in Attachments 1-3.
Table 1. Reference Values and Regression Parameters for Determination of Fluoride Anticipated Residues.
Food
Barley
Cocoa Beans
Corn
Corn Flour
Corn, Popcorn
Dates
Dried Plums
Figs
Oats
Pistachios
Raisin
Rice, Brown
Wheat Flour
Wheat Germ
Wheat Grain
Rice, White
Almonds
Pecans
Walnuts
Hazelnutst (Space)*
Hazelnutst (Food)
Reference
Dose,
mg-hr/L
1628
1483
1549
1573
1505
1484
1543
1524
1534
1517
1545
1558
1533
1512
1539
1509
1539
1533
2460
1576
1576
Residue at
Reference
Dose,
ppm
2.95
5.12
1.78
21.73
0.95
0.70
0.85
1.14
7.90
4.10
0.05
5.68
25.93
67.95
2.92
1.90
4.70
8.55
2.25
2.32
1.81
Slope
1.149
1.082
0.868
0.340
0.801
0.333
0.470
0.239
0.859
1.248
1.033
0.892
0.770
0.700
0.382
1.290
0.470
0.831
1.939
2.014
2.749
Intercept
0.611
0.034
0.383
0.694
0.513
0.748
0.537
0.657
0.408
0.094
14.612
0.250
0.550
0.220
0.669
0.987
0.610
0.091
0.336
-0.179
-0.861
Average Rate,
mg-hr/L
Structural
590
790
670
670
1340
380
380
380
560
350
380
620
590
590
590
620
350
350
350
350
~
Food
610
790
390
390
1340
380
380
380
560
540
380
960
610
610
610
960
540
540
540
540
Residue at Average
Rate, ppm
Structural
3.03
3.12
1.35
18.22
1.16
0.58
0.56
0.81
5.70
1.56
0.74
3.43
21.96
33.50
2.38
2.88
3.37
2.40
1.38
1.03
~
Food
3.07
3.12
1.07
16.91
1.16
0.58
0.56
0.81
5.70
2.21
0.74
4.54
22.22
34.13
2.39
3.44
3.64
3.28
1.71
1.70
calculated residues assume the intercept is zero.
* Data are from hazelnuts without shell
II.
Use Information
Food Fumigations. Information regarding % CTp (% CT for food fumigations) was submitted to
the Agency by DAS. OPP's Biological and Economic Analysis Division (BEAD) has examined
the information submitted by DAS and has derived recommended %CTp values for use in the
dietary exposure analysis for food fumigations (C. Cook and E. Rim, D361041, 30 April 2009).
The recommendations from BEAD are summarized in Table 2.
Table 2. Summary of Revised Estimates of Percent Commodity Directly Treated with Sulfuryl Fluoride.
BEAD Commodity
Grouping
Meats and Cheese
Commodity
Cheese1
Ham1
Percent Commodity Treated
DAS
0.0 %
0.0 %
BEAD
Estimate
0.0 %
0.0 %
Recommended
0.0 %
0.0 %
Page 4 of 30
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Table 2. Summary of Revised Estimates of Percent Commodity Directly Treated with Sulfuryl Fluoride.
BEAD Commodity
Grouping
Quarantined Uses2
Coarse Grains
Processed Commodities
Stored Commodities
Nuts4
Methyl Bromide
Critical Use Exemption
Commodities
Commodity
Beef (Dried)
Coconut
Coffee Bean
Macadamia Nut
Ginger
Barley3
Corn6
Cottonseed3
Millet3
Oats6
Rice Hulls3
Sorghum6
Triticale3
Corn - Flour, Grits, Meal
Herbs And Spices
Popcorn
Rice - Flour, Bran
Wheat - Flour, Germ, Bran, Shorts, Milled
Byproducts
Peanut6
Wheat6
Rice6
Wild Rice
Almonds
Beechnut
Brazil Nut
Butternut
Cashew
Chestnut
Chinquapin
Filbert
Hickory Nut
Pecans
Pine Nut
Pistachio1
Walnuts1
Dates1
Prunes, Raisins, Figs1
Other Dried Fruit5'7
Dried Beans 1
Legumes (Dried, except Chickpea & Cowpea) 5> 7
Cocoa Beans1
Percent Commodity Treated
DAS
0.0 %
0.1%
0.1%
0.1%
0.1%
0.1%
0.1%
0.1%
0.0 %
0.1%
0.0 %
0.1%
0.0 %
0.1%
0.1%
0.1%
3.0%
0.1%
0.1%
0.1%
3.0%
10.0 %
0.0 %
0.1%
0.0 %
0.1%
0.1%
0.0 %
0.1%
0.1%
0.1%
0.1%
0.1%
20.0 %
40.0 %
40.0 %
0.1%
100.0 %
0.1%
100.0 %
BEAD
Estimate
0.0 %
0.0 %
0.0 %
0.0 %
0.0 %
0. %
0. %
0. %
0. %
0. %
0. %
0. %
0. %
0.0 %
-------
Structural Fumigations. As in previous assessments, information regarding the percentage of
facilities treated, the number of days the facilities are in operation, and the amount of material
onsite during fumigation has been used to obtain % CT estimates associated with structural
fumigations (% CTS). The estimate is calculated as follows:
% CTS = % facilities treated x number of days production held during fumigation x number
of fumigations per year H- number of operating days per year,
where the percent of both the grain mills and processing facilities treated equals 40%, the
number of days production held in the facility during a fumigation is 2 days for grain mills and 1
day for processing facilities, the number of fumigations per year is 3 for grain mills and 2.5 for
processing facilities, and both grain mills and processing facilities are in operation for 300 days
per year. These values give a % CTs of 0.8 for grain mills and a % CTs of 0.4% for processing
facilities. Given knowledge of industry practices, EPA believes this to be a conservative manner
of estimating residues resulting from structural fumigation; however, with the current label
directions, further refinement is not appropriate.
There is the potential for "sequential" treatment of certain foods. For example, wheat grain
could be inadvertently during a structural fumigation, that grain milled into flour, and then a
portion of that same flour could be inadvertently treated during a mill fumigation. Past
assessments have taken the extremely conservative assumption that the probability of sequential
treatment occurring is 100%. This assessment uses % CTS information to derive a more realistic
picture of the likelihood of sequential treatments. There are four scenarios that describe the
sequential treatment possibilities associated with structural fumigations:
1. Flour is incidentally treated, source grain is incidentally treated
2. Flour is incidentally treated, source grain is not incidentally treated
3. Flour is not incidentally treated, source grain is incidentally treated
4. Flour is not incidentally treated, source grain is not incidentally treated.
The likelihood of each scenario can be estimated by multiplying the % CTS estimates for the
various combinations (Table 3).
Table 3. Likelihood of Sequential Treatment with Sulfuryl Fluoride from Structural Fumigations.
Grain Treated (0.8%)
Grain Not Treated (99.2%)
Flour Treated (0.4%)*
0.0032% (Scenario 1)
0.397% (Scenario 2)
Flour Not Treated (99.6%)
0.797% (Scenario 3)
98.8% (Scenario 4)
Parenthetical values are % of facilities treated. Values in the table are obtained by multiplying the % of facilities
treated for each scenario (e.g., % of flour bearing residues from both mill fumigation and grain fumigation = 0.004 *
0.008 = 0.000032 = 0.0032%).
Combining the scenario likelihood values, residue estimates for flours, and empirical factors for
processing grains into flours (0.38 for wheat, 0.73 for other grains) gives the weighted average
residue values presented in Table 4. These values are used to estimate the exposure from grain
flour as a result of structural fumigations. Flour residue estimates for food fumigations are based
on the regression analyses discussed above. Exposure estimates from the inadvertent treatments
Page 6 of 30
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and food treatments are added together in a separate step in the assessment process to provide
estimates of overall dietary exposure from the uses of SF.
Table 4. Weighted average residue estimates for grain flours resulting from structural treatment.
Flour
Source
Barley
Corn
Oats
Rice
Wheat
Treated
Grain
Residue,
ppm
3.03
1.35
5.70
2.88
2.38
Analytical
Correction
Factor
0.83
1.00
0.70
0.56
0.83
Corrected
Treated
Grain
Residue,
ppm
3.65
1.35
8.14
5.14
2.90
Flour Residue, ppm
Processed
from Treated
Grain3
(0.797%)*
2.66
0.99
5.94
3.75
1.10
Treated
Flour
(0.397%)
33.70
18.22
72.28
32.50
31.40
Processed
from Treated
Grain +
Treated Flour
(0.0032%)
36.36
19.21
78.22
36.25
32.50
Weighted
Average,
ppmb
0.156
0.081
0.337
0.160
0.134
a Grain residue x processing factor (0.38 for wheat, 0.73 for others)
b Weighted Average = £ (Flour Residue x % Likelihood from Table 3 + 100). The contribution from Scenario 4 to
the weighted average is zero since no treatments were involved (flour residue = 0 ppm).
* Parenthetical values are % likelihood estimates from Table 3.
Table 5 summarizes the inputs used for the dietary exposure assessment for fluoride coming
from the uses of sulfuryl fluoride. Where appropriate, the regression parameters (Table 1) were
applied to the available residue data to obtain residue estimates based on actual use patterns. The
%CT information (Table 2) is also summarized in Table 5, and was used to derive weighted
averages (Tables 3 and 4) for residues associated with structural fumigations and processed grain
commodities.
Table 5. Summary of Analytical Correction Factors, Percent Crop Treated, and Residue Estimates for the Dietary
Exposure Analysis of Fluoride from Use of Sulfuryl Fluoride.
Food
Alfalfa, seed
Almond
Almond, oil
Amaranth, grain
Apple, dried
Apricot, dried
Arrowroot, flour
Banana, dried
Barley, pearled barley
Barley, flour
Barley, bran
Basil, fresh leaves
Basil, dried leaves
Bean, black, seed
Bean, broad, seed
Bean, cowpea, seed
Bean, great northern, seed
Bean, kidney, seed
Bean, lima, seed
Bean, mung, seed
Bean, navy, seed
Bean, pink, seed
Analytical
Correction
Factor
0.51
0.37
0.78
0.51
0.79
0.79
0.70
0.79
0.83
0.83
0.83
0.69
0.69
0.69
0.69
0.69
0.69
0.69
0.69
0.69
0.69
0.69
Structural
Residue Value Data
Source
See sorghum
Regression*
!/2 LOQ
See sorghum
See figs
See figs
Non-mixed wheat flour
See figs
Regression*
Wtd avg (see text)
See Barley, pearled
Avg @ 1569-1 596 rate§
Avg @ 1569- 1596 rate
Cocoa beans (3) avg rate
Cocoa beans (3> avg rate
Cocoa beans @ avg rate
Cocoa beans @ avg rate
Cocoa beans @ avg rate
Cocoa beans (a), avg rate
Cocoa beans (3> avg rate
Cocoa beans @ avg rate
Cocoa beans @ avg rate
%
CTS*
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.8
tt
0.8
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
Residue,
ppm*
20.4
9.2
1.5
20.4
1.0
1.0
31.4
1.0
3.65
0.156
3.65
67.1
67.1
4.5
4.5
4.5
4.5
4.5
4.5
4.5
4.5
4.5
Food
Residue Value Data
Source
Regression
See figs
See figs
See figs
Regression*
Regression* with 0.73X
factor
Regression* with 2.56X
factor
Avg@ 1569- 1596 rate
Cocoa beans (a), avg rate
Cocoa beans (3> avg rate
Cocoa beans @ avg rate
Cocoa beans @ avg rate
Cocoa beans @ avg rate
Cocoa beans (a), avg rate
Cocoa beans (3> avg rate
Cocoa beans @ avg rate
Cocoa beans @ avg rate
% CTF*
10
69
69
69
0.1
0.1
0.1
0.1
100
100
100
100
100
100
100
100
100
Residue,
ppm*
9.7
1.0
1.0
1.0
3.7
3.7
3.7
67.1
4.5
4.5
4.5
4.5
4.5
4.5
4.5
4.5
4.5
Page 7 of 30
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Table 5. Summary of Analytical Correction Factors, Percent Crop Treated, and Residue Estimates for the Dietary
Exposure Analysis of Fluoride from Use of Sulfuryl Fluoride.
Food
Bean, pinto, seed
Beef, meat, dried
Beet, sugar, molasses
Brazil nut
Buckwheat
Buckwheat, flour
Butternut
Cashew
Chestnut
Chickpea, seed
Chickpea, flour
Chicory, roots
Chive
Chrysanthemum, garland
Cinnamon
Cocoa bean, chocolate
Cocoa bean, powder
Coconut, meat
Coconut, dried
Coconut, milk
Coconut, oil
Coffee, roasted bean
Coffee, instant
Coriander, leaves
Coriander, seed
Com, field, flour
Com, field, meal
Com, field, bran
Com, field, starch
Com, field, syrup
Com, field, oil
Com, pop
Cottonseed, oil
Cranberry, dried
Currant, dried
Date
Dill, seed
Dillweed
Egg (dried)
Fig, dried
Filbert
Filbert, oil
Flaxseed, oil
Garlic, dried
Ginger
Ginger, dried
Ginseng, dried
Grape, raisin
Guar, seed
Herbs, other
Hickory nut
Lemongrass
Lentil, seed
Lychee, dried
Macadamia nut
Mango, dried
Analytical
Correction
Factor
0.69
0.69
0.69
0.62
0.83
0.70
0.62
0.62
0.62
0.69
0.69
0.69
0.69
0.69
0.69
0.69
0.69
0.69
0.69
0.69
0.78
0.69
0.69
0.69
0.69
1.00
1.00
1.00
0.80
0.78
0.78
0.69
0.78
0.79
0.79
0.69
0.69
0.69
0.69
0.79
0.69
0.78
0.78
0.69
0.69
0.69
0.69
0.72
0.69
0.69
0.62
0.69
0.69
0.79
0.62
0.79
Structural
Residue Value Data
Source
Cocoa beans @ avg rate
Avg @ 1573-1658 rate
Avg @ 1454-1523 rate
See pecans
See wheat grain
See wheat flour
See pecans
See pecans
See pecans
Cocoa beans @ avg rate
Cocoa beans @ avg rate
Avg @ 1616-1658 rate
See dried parsley
See dried parsley
Avg @ 1573-1580 rate
Cocoa beans @ 1 500 rate
Cocoa beans (3) 1500 rate
Avg @ 1596- 1607 rate
Avg @ 1596- 1607 rate
Avg @ 1596- 1607 rate
!/2 LOQ
Avg @ 1573-1580 rate
Avg @ 1610-1658 rate
See dried parsley
See pepper, black/white
Wtd avg (see text)
Avg @ 1573- 1590 rate
Avg @ 1573- 1590 rate
Avg@ 1534-1573 rate
Com grain x 0.17
Avg @ 1540- 1580 rate
Regression
!/2 LOQ
See figs
See figs
Regression
See pepper, black/white
See dried parsley
Avg @ 1414-1580 rate
Regression
Regression
!/2 LOQ
!/2 LOQ
Avg @ 1414-1446 rate
See garlic
See garlic
Regression
Cocoa beans @ avg rate
See dried parsley
See pecans
See dried parsley
Cocoa beans @ avg rate
See figs
See pecans
See figs
%
CTS*
0.4
0.4
0.4
0.4
0.8
m
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
m
0.8
0.8
0.8
0.8
0.8
0.8
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
0.4
Residue,
ppm^
4.5
58.4
1.2
3.9
2.9
0.112
3.9
3.9
3.9
4.5
4.5
13.9
63.5
63.5
73.5
8.4
8.4
49.1
49.1
49.1
1.5
7.1
13.9
63.5
7.1
0.081
14.0
14.0
6.6
0.6
0.4
1.7
1.5
1.0
1.0
0.9
7.1
63.5
402.5
1.0
1.5
1.5
1.5
10.9
10.9
10.9
1.0
4.5
63.5
3.9
63.5
4.5
1.0
3.9
1.0
Food
Residue Value Data
Source
Cocoa beans @ avg rate
See pecans
See pecans
See pecans
See pecans
Cocoa beans @ avg rate
Cocoa beans @ avg rate
See dried parsley
Avg @ 1573- 1580 rate
Cocoa beans @ 1 500 rate
Cocoa beans (3> 1 500 rate
Avg @ 1596- 1607 rate
Avg @ 1596- 1607 rate
Avg @ 1596- 1607 rate
Avg@ 1573- 1580 rate
Avg @ 1610-1658 rate
See dried parsley
See pepper, black/white
Regression
Com grain x 0.78
Com grain x 0.78
Corn grain x 0.17
Corn grain x 0.17
Regression
See figs
See figs
Regression
See pepper, black/white
See dried parsley
Regression
Regression
Avg @ 1414-1446 rate
See garlic
See garlic
Regression
Cocoa beans @ avg rate
See dried parsley
See pecans
See dried parsley
Cocoa beans @ avg rate
See figs
See pecans
See figs
% CTF*
100
10
10
10
10
100
100
0.1
0.1
100
100
0.1
0.1
0.1
0.1
0.1
0.1
0.1
0.1
0.1
0.1
0.1
0.1
0.1
10
10
42
0.1
0.1
69
10
0.1
0.1
0.1
69
100
0.1
10
0.1
100
69
0.1
69
Residue,
ppm^
4.5
5.3
5.3
5.3
5.3
4.5
4.5
63.5
73.5
8.4
8.4
49.1
49.1
49.1
7.1
13.9
63.5
7.1
16.9
2.8
2.8
0.6
0.6
1.7
1.0
1.0
0.9
7.1
63.5
1.0
2.5
10.9
10.9
10.9
1.0
4.5
63.5
5.3
63.5
4.5
1.0
5.3
1.0
Page 8 of 30
-------
Table 5. Summary of Analytical Correction Factors, Percent Crop Treated, and Residue Estimates for the Dietary
Exposure Analysis of Fluoride from Use of Sulfuryl Fluoride.
Food
Maple, sugar
Maple syrup
Marjoram
Milk (powdered)
Milk (cured; cheese)
Millet, grain
Oat, bran
Oat, flour
Oat, groats/rolled oats
Olive, oil
Onion, dry bulb, dried
Palm, oil
Papaya, dried
Parsley, dried leaves
Pea, dry
Pea, pigeon, seed
Peach, dried
Peanut
Peanut, butter
Peanut, oil
Pear, dried
Pecan
Pepper, bell, dried
Pepper, nonbell, dried
Pepper, black/white
Peppermint, oil
Pine nut
Pineapple, dried
Pistachio
Plantain, dried
Plum, prune, dried
Potato, chips
Potato, dry
Potato, flour
Psyllium, seed
Pumpkin, seed
Quinoa, grain
Rapeseed, oil
Rice, white
Rice, brown
Rice, flour
Rice, bran
Rye, grain
Rye, flour
Safflower, oil
Savory
Sesame, seed
Sesame, oil
Sorghum, grain
Sorghum, syrup
Soybean, flour
Soybean, soy milk
Soybean, oil
Spearmint, oil
Spices, other
Analytical
Correction
Factor
0.69
0.69
0.69
0.69
0.69
0.83
0.52
0.70
0.83
0.78
0.69
0.78
0.79
0.69
0.69
0.69
0.79
0.69
0.69
0.78
0.79
0.62
0.69
0.69
0.69
0.78
0.69
0.79
0.69
0.79
0.82
0.69
0.69
0.70
0.69
0.69
0.51
0.78
0.75
0.36
0.56
0.69
0.83
0.70
0.78
0.69
0.69
0.78
0.51
0.78
0.70
0.69
0.78
0.78
0.69
Structural
Residue Value Data
Source
Avg @ 1454-1523 rate
Avg @ 1454-1523 rate
See basil
Avg @ 1414-1580 rate
Avg @ 1414-1446 rate
See wheat grain
See wheat bran
Wtd avg (see text)
See pearled barley
!/2 LOQ
Control value; treated
samples avg rate
See figs
Avg@ 1569- 1596 rate
Avg @ 1569- 1596 rate
See figs
Regression
Avg@ 1454-1523 rate
Avg @ 1573- 1580 rate
See figs
Regression
See figs
Regression
Regression
Regression
Avg@ 1573- 1580 rate
Avg @ 1573 rate
See dried parsley
Avg @ 1573- 1580 rate
See pepper, black/white
% CTF*
0.1
0.1
0.1
0.1
0.1
69
0.1
100
100
69
0.6
0.6
69
10
0.1
10
69
27
69
69
3
3
3
3
0.1
0.1
0.1
Residue,
ppm^
67.1
2.9
18.5
18.5
18.5
1.0
63.5
4.5
4.5
1.0
16.4
16.4
1.0
5.3
7.1
8.8
1.0
3.2
1.0
0.7
4.5
12.5
32.5
37.5
63.5
20.4
7.1
Page 9 of 30
-------
Table 5. Summary of Analytical Correction Factors, Percent Crop Treated, and Residue Estimates for the Dietary
Exposure Analysis of Fluoride from Use of Sulfuryl Fluoride.
Food
Sugarcane, sugar
Sugarcane, molasses
Sunflower, seed
Sunflower, oil
Tea, dried
Tea, instant
Tomato, dried
Triticale, flour
Turmeric
Walnut
Wheat, grain
Wheat, flour
Wheat, germ
Wheat, bran
Wild rice
Analytical
Correction
Factor
0.69
0.69
0.69
0.78
0.69
0.69
0.79
0.70
0.69
0.70
0.83
0.70
0.62
0.52
0.36
Structural
Residue Value Data
Source
Avg @ 1454-1523 rate
Avg @ 1454-1523 rate
Cocoa beans (5> avg rate
!/2 LOQ
See basil
See basil
See figs
See wheat flour
See pepper, black/white
Regression
Regression
Wtd avg (see text)
Regression
Avg @ 1573-1717 rate
See rice, brown
%
CTS*
0.4
0.4
0.4
0.4
0.4
0.4
0.4
"
0.4
0.4
0.8
0.8
0.8
0.8
Residue,
ppm^
1.2
1.2
4.5
1.5
67.1
67.1
1.0
0.134
7.1
2.0
2.9
0.134
54.0
74.2
9.4
Food
Residue Value Data
Source
Wheat with 0.3 8 factor
See pepper, black/white
Regression
Regression
Regression
Wheat grain x 4.8
Avg@ 1573- 171 7 rate
See rice, brown
% CTF*
0.1
0.1
99
0.4
0.1
0.1
0.1
3
Residue,
ppm^
2.9
7.1
2.4
2.9
31.4
13.9
74.2
12.5
% CTS = percent crop treated for structural fumigations. % CTF = percent crop treated for food fumigations.
t Residue values include the analytical correction factor.
* Residue values are from Table 1, after application of the analytical correction factor.
§ Avg @ rate = the average residue value from the listed application rate
% CTS estimates associated with grain flours are incorporated into the residue estimate directly and are, therefore, not used as a
modifying factor for these commodities. For the DEEM input file, the value is set at 1.00.
For grains, the current label for sulfuryl fluoride allows for fumigation of corn, rice, and wheat
processed commodities. Fumigation of processed commodities of other grains (e.g., barley, oats,
and triticale) is not permitted. The entries in Table 4 associated with the food fumigation of the
processed commodities for these other grains include factors of 0.38 for flour and 2.56 for bran.
These factors are from a study (MRTD 45396301) in which wheat was fumigated with sulfuryl
fluoride and then processed into flour, bran, germ, etc. using simulated commercial practices. A
processing factor for chickpea flour is not available. FED has assumed that there is no
concentration of fluoride residue during the processing of chickpeas into flour, and believes that
this is a conservative assumption given the processing factors for wheat flour (0.38) and corn
flour (0.73).
III. DEEM-FCID Program and Consumption Information
These dietary exposure assessments were conducted using the Dietary Exposure Evaluation
Model software with the Food Commodity Intake Database DEEM-FCID, Version 2.03 which
incorporates consumption data from USDA's Continuing Surveys of Food Intakes by Individuals
(CSFII), 1994-1996 and 1998. The 1994-96, 98 data are based on the reported consumption of
more than 20,000 individuals over two non-consecutive survey days. Foods "as consumed"
(e.g., apple pie) are linked to EPA-defined food commodities (e.g. apples, peeled fruit - cooked;
fresh or N/S; baked; or wheat flour - cooked; fresh or N/S, baked) using publicly available recipe
translation files developed jointly by USDA/ARS and EPA. For chronic exposure assessment,
consumption data are averaged for the entire U.S. population and within population subgroups,
but for acute exposure assessment are retained as individual consumption events. Based on
analysis of the 1994-96, 98 CSFII consumption data, which took into account dietary patterns
and survey respondents, HED concluded that it is most appropriate to report risk for the
following population subgroups: the general U.S. population, all infants (<1 year old), children
Page 10 of 30
-------
1-2, children 3-5, children 6-12, youth 13-19, adults 20-49, females 13-49, and adults 50+ years
old.
For chronic dietary exposure assessment, an estimate of the residue level in each food or food-
form (e.g., orange or orange juice) on the food commodity residue list is multiplied by the
average daily consumption estimate for that food/food form to produce a residue intake estimate.
The resulting residue intake estimate for each food/food form is summed with the residue intake
estimates for all other food/food forms on the commodity residue list to arrive at the total
average estimated exposure. Exposure is expressed in mg/kg body weight/day. This procedure
is performed for each population subgroup.
IV. Results/Discussion
Chronic dietary exposure estimates are summarized in Table 6 for each source and each
population subgroup noted above. The estimated contributions from the various crop subgroups
to total fluoride exposure from the currently registered uses of cryolite and sulfuryl fluoride are
provided in Table 7. The results of the commodity contribution analysis for each source are
summarized in Attachments 7 through 9. The complete commodity contribution reports have not
been included in this document due to their excessive length. These reports are available upon
request. Overall exposure is estimated to be greatest for the age group consisting of 1-2 year
olds; however, 3-5 year olds have higher exposure for certain food groups (e.g., leafy vegetables,
cucurbit vegetables, citrus fruits, pome fruits, and tree nuts; Table 7).
Table 6. Summary of Pesticidal Fluoride Contributions to Dietary Fluoride Exposure.
Population Group
U.S. Population (total)
All infants (< 1 year)
Children 1-2 yrs
Children 3 -5 yrs
Children 6-12 yrs
Youth 13-19 yrs
Adults 20-49 yrs
Adults 50+ yrs
Females 13-49 yrs
Exposure Estimates, mg/kg/day
Cryolite
0.000682
0.000956
0.003275
0.002112
0.000885
0.000346
0.000445
0.000547
0.000473
SF Structural Fumigations
0.000336
0.000505
0.000827
0.000800
0.000543
0.000320
0.000272
0.000215
0.000249
SF Food Fumigations
0.001023
0.001071
0.002169
0.002293
0.001743
0.001032
0.000814
0.000719
0.000799
Total
0.002041
0.002532
0.006271
0.005205
0.003171
0.001698
0.001531
0.001481
0.001521
V. Characterization of Inputs/Outputs
The residue estimates for most of the commodities in these analyses are moderately to highly
refined. Data reflecting residues of F at various fumigation rates could be used to further refine
residue estimates for a number of commodities. However, such data are not expected to result in
significant changes to the exposure estimates presented in Section IV. Percent CT estimates
have been used for both the structural and food fumigation uses. The % CT values used by OPP
are considered to be highly refined, although certain conservatism remains in the values in that
where there are discrepancies between the estimates from BEAD and Dow AgroSciences, the
higher value was used.
Page 11 of 30
-------
Table 7. Summary of Fluoride Exposure Estimates by Age Group and Crop/Food Group.
Group*
(O) Other1
(M) Meat
(P) Poultry
(D) Dairy Products
(1) Root and Tuber Vegetables
(3) Bulb Vegetables
(4) Leafy Vegetables (except Brassica)
(5) Brassica Leafy Vegetables
(6) Legume Veg. (Succulent or Dried)
(8) Fruiting Vegetables
(9) Curcurbit Vegetables
(10) Citrus
(11) Pome Fruits
(12) Stone Fruits
(13) Berries
(14) Tree Nuts
(15) Cereal Grains
(19) Herbs and Spices
(20) Oilseeds
Fruit Juices*
Total
Exposure, mg/kg/day
U.S. Pop.
0.0009222
0.0000004
0.0000103
0.0000032
0.0000218
0.0000002
0.0000077
0.0000148
0.0005292
0.0000153
0.0000091
0.0000462
0.0000013
0.0000091
0.0000061
0.0000163
0.0004246
0.0000026
0.0000003
0.0002769
0.0020407
Grouping by Age (Years)
<1
0.0009517
0.0000000
0.0000055
0.0000684
0.0000216
0.0000002
0.0000000
0.0000082
0.0003465
0.0000062
0.0000110
0.0000159
0.0000017
0.0000503
0.0000117
0.0000013
0.0010255
0.0000016
0.0000039
0.0007996
0.0025312
1-2
0.0037942
0.0000009
0.0000296
0.0000135
0.0000509
0.0000007
0.0000040
0.0000313
0.0010570
0.0000284
0.0000162
0.0001014
0.0000027
0.0000401
0.0000147
0.0000257
0.0010501
0.0000092
0.0000004
0.0022384
0.0062710
3-5
0.0028948
0.0000002
0.0000210
0.0000096
0.0000470
0.0000006
0.0000061
0.0000230
0.0009845
0.0000260
0.0000186
0.0001027
0.0000030
0.0000179
0.0000147
0.0000262
0.0010019
0.0000072
0.0000004
0.0012761
0.0052054
6-12
0.0016121
0.0000006
0.0000118
0.0000031
0.0000310
0.0000004
0.0000063
0.0000167
0.0006567
0.0000188
0.0000121
0.0000544
0.0000023
0.0000114
0.0000093
0.0000190
0.0007000
0.0000044
0.0000004
0.0004614
0.0031708
13-19
0.0006471
0.0000011
0.0000079
0.0000017
0.0000224
0.0000002
0.0000075
0.0000094
0.0005222
0.0000140
0.0000074
0.0000298
0.0000012
0.0000035
0.0000049
0.0000113
0.0004035
0.0000026
0.0000003
0.0001593
0.0016980
20-50
0.0005932
0.0000004
0.0000102
0.0000011
0.0000181
0.0000002
0.0000088
0.0000131
0.0004703
0.0000145
0.0000068
0.0000305
0.0000009
0.0000049
0.0000042
0.0000150
0.0003361
0.0000020
0.0000002
0.0001053
0.0015305
>50
0.0006092
0.0000002
0.0000068
0.0000014
0.0000164
0.0000002
0.0000077
0.0000161
0.0004453
0.0000129
0.0000098
0.0000614
0.0000011
0.0000100
0.0000056
0.0000171
0.0002590
0.0000014
0.0000002
0.0000941
0.0014818
Females
13-49
0.0006484
0.0000004
0.0000110
0.0000011
0.0000171
0.0000002
0.0000094
0.0000134
0.0004313
0.0000134
0.0000074
0.0000322
0.0000010
0.0000055
0.0000046
0.0000150
0.0003077
0.0000020
0.0000002
0.0001126
0.0015213
For crops, the groups correspond to OPP crop groupings. Groups 7, 16, 17, and 18 do not consist of commodities for human
consumption and are not included in this table.
^ Foods not captured in one of the listed groups, including, but not limited to,
Use of cryolite is the predominant source of fluoride for this group.
* The exposure contributions from fruit juices are included in the overall total
do not include the specific exposure estimate from fruit juices.
cocoa beans, coconut, cranberry, grape, and grape juice.
via the crop groups; therefore, the values listed as total
Page 12 of 30
-------
Attachments
1. Inputs for the chronic dietary exposure analysis of fluoride from cryolite
2. Inputs for the chronic dietary exposure analysis of fluoride from structural fumigation with
sulfuryl fluoride
3. Inputs for the chronic dietary exposure analysis of fluoride from food fumigation with
sulfuryl fluoride
4. Results of the chronic dietary exposure analysis of fluoride from cryolite
5. Results of the chronic dietary exposure analysis of fluoride from structural fumigation with
sulfuryl fluoride
6. Results of the chronic dietary exposure analysis of fluoride from food fumigation with
sulfuryl fluoride
7. Commodity contribution summary for the chronic dietary exposure analysis of fluoride from
cryolite
8. Commodity contribution summary for the chronic dietary exposure analysis of fluoride from
structural fumigation with sulfuryl fluoride
9. Commodity contribution summary for the chronic dietary exposure analysis of fluoride from
food fumigation with sulfuryl fluoride
Page 13 of 30
-------
Attachment 1. Inputs for the chronic dietary exposure analysis of fluoride from cryolite
U.S. Environmental Protection Agency Ver. 2.00
DEEM-FCID Chronic analysis for CRYOLITE 1994-98 data
Residue file: C:\Documents and Settings\mdoherty\My Documents\Chemistry Reviews\!DEEM
Runs\Sulfuryl Fluoride\Cryolite-AR-CT new raisin factor.R98
Adjust. #2 used
Analysis Date 02-19-2009 Residue file dated: 06-24-2004/10:05:08/8
Food Crop
EPA Code Grp
Food Name
Adj.Factors
#1 #2
Comment
13B
Apricot
Apr!cot-babyfood
Apricot, dried
Apricot, juice
Apricot, juice-babyfood
Blackberry
Blackberry, juice
Blackberry, juice-babyfood
Blueberry
Blueberry-babyfood
Boysenberry
Broccoli
Broccoli-babyfood
Brussels sprouts
Cabbage
Cabbage, Chinese, bok choy
Cantaloupe
Casaba
Cauli flower
Citrus citron
Collards
Cranberry
Cranberry-babyfood
Cranberry, dried
Cranberry, juice
Cranberry, juice-babyfood
Cucumber
Currant
Currant, dried
Dewberry
Eggplant
Elderberry
Gooseberry
Grape
Grape, juice
j uice-babyfood
leaves
raisin
Grape, wine and sherry
Grapefruit
Grapefruit, juice
Honeydew melon
Huckleberry
Kale
Kiwi fruit
Kohlrabi
Kumguat
Lemon
Lemon, juice
Lemon, juice-babyfood
Lemon, peel
Lettuce, head
Lettuce, leaf
Lime
Lime, j uice
Lime, juice-babyfood
Loganberry
Nectarine
Orange
8.000000
13.500000
13.500000
2.500000
000000
13.500000
13.500000
13.500000
0.250000
4.500000
8.000000
1
1.000
1.000
6.000
1. 000
1. 000
1. 000
1. 000
1.000
1.000
1.000
1.000
1. 000
1. 000
1. 000
1.000
1.000
1.000
1.000
1. 000
1. 000
1. 000
1. 000
1.000
1.000
1.100
1.100
1.000
1. 000
1. 000
1. 000
1. 000
1.000
1.000
1.000
0. 830
0. 830
1. 000
1.350
0.830
1.000
0. 026
1.000
1. 000
1. 000
1. 000
1. 000
1.000
1.000
0. 024
0. 024
0.280
1. 000
1. 000
1. 000
0. 024
0. 024
1.000
1.000
1.000
0.010
0.010
0.010
0. 010
0.010
1. 000
1. 000
1.000
1.000
1.000
1.000
0.020
0. 020
0.020
0.010
0.010
0.010
0.010
0.020
0.040
0.020
1. 000
1.000
1.000
1.000
1.000
0.010
1. 000
1. 000
1. 000
0. 010
1.000
1.000
0.330
0.330
0.330
0.330
0.330
0.330
0.040
0.040
0.010
1. 000
0.020
0.140
0.020
0.040
0.020
0.020
0.020
0.020
0. 010
0.010
0.040
0.040
0.040
1.000
0.010
0.020
Page 14 of 30
-------
10002410
10002411
10002420
12002600
12002601
12002610
12002611
12002620
12002621
08002700
08002701
08002710
08002711
08002720
08002721
08002730
95002750
95002760
12002850
12002851
12002860
12002861
12002870
12002871
12002880
12002881
01032960
01032970
01032971
01032980
01032981
01032990
01032991
01033000
01033001
10003070
09023080
09023090
13013200
13013201
13013210
13013211
95003520
95003530
09023560
09023561
09023570
09023571
95003590
95003591
95003600
95003601
10003690
10003700
08003750
08003751
08003760
08003761
08003770
08003771
08003780
08003781
08003790
09013990
09014000
10
10
10
12
12
12
12
12
12
Orange, juice
Orange, juice-babyfood
Orange, peel
Peach
Peach-babyfood
Peach, dried
Peach, dried-babyfood
Peach, juice
Peach, juice-babyfood
Pepper, bell
Pepper, bell-babyfood
Pepper, bell, dried
Pepper, bell, dried-babyfood
Pepper, nonbell
Pepper, nonbell-babyfood
Pepper, nonbell, dried
Peppermint
Peppermint, oil
Plum
Plum-babyfood
Plum, prune, fresh
Plum, prune, fresh-babyfood
Plum, prune, dried
Plum, prune, dried-babyfood
Plum, prune, juice
Plum, prune, juice-babyfood
Potato, chips
Potato, dry (granules/ flakes)
Potato, dry (granules/ flakes)-b
Potato, flour
Potato, flour-babyfood
Potato, tuber, w/peel
Potato, tuber, w/peel-babyfood
Potato, tuber, w/o peel
Potato, tuber, w/c
Pummelo
Pumpkin
Pumpkin, seed
Raspberry
Raspberry-babyfood
Raspberry, juice
Raspberry, juice-babyfood
Spearmint
Spearmint, oil
Sguash, summer
Sguash, summer-babyfood
Squash, winter
Squash, winter-babyfood
Strawberry
Strawberry-babyfood
Strawberry, juice
Strawberry, juice-babyfood
Tangerine
Tangerine, juice
Tomato
Tomato-babyfood
Tomato, paste
Tomato, paste-babyfood
Tomato, puree
Tomato, puree-babyfood
Tomato, dried
Tomato, dried-babyfood
Tomato, juice
Watermelon
Watermelon, juice
8.
8.
8.
4 .
4 .
4 .
4 .
4 .
4 .
3.
3.
3.
3.
3.
2
3 .
19.
19.
0 .
0 .
0 .
2.
2 .
2 .
2 .
2.
0 .
0 .
0 .
0.
0.
0.
0.
0 .
0 .
9 .
2.
2.
0.
0.
0.
0.
19.
19.
2.
2.
2 .
2 .
1.
1.
1.
1.
8.
8.
1.
1.
1.
1.
1.
1.
1.
1.
1.
2 .
2 .
.000000
000000
. 000000
500000
. 500000
.500000
.500000
.500000
.500000
. 500000
. 500000
. 500000
500000
. 500000
.500000
.500000
.500000
.500000
. 500000
500000
. 500000
. 000000
.000000
.000000
.000000
. 000000
. 650000
. 650000
. 650000
.650000
.650000
.650000
.650000
. 650000
. 650000
. 000000
. 500000
500000
.250000
.250000
.250000
.250000
500000
. 500000
500000
. 500000
.500000
.500000
.000000
. 000000
. 000000
. 000000
. 000000
.000000
.500000
.500000
.500000
. 500000
. 500000
. 500000
. 500000
. 500000
.500000
.160000
.160000
0.
0 .
0 .
1.
1.
-j
-J
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
0.
1.
1.
1.
1.
5 .
5 .
1.
1.
1.
6 .
6 .
6.
6.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
0 .
1.
1.
1.
1.
1.
1.
1.
1.
1.
0.
1.
1.
1.
1.
1.
1.
14 .
14 .
1.
1.
1.
.022
. 022
.280
. 000
. 000
.000
.000
.000
.000
. 000
. 000
. 000
. 000
. 000
.000
.000
.000
. 026
. 000
. 000
. 000
. 000
.000
.000
.400
. 400
. 000
. 500
. 500
.500
.500
.000
.000
. 000
. 000
. 000
. 000
. 000
.000
.000
.000
.000
. 000
. 026
. 000
. 000
.000
.000
.000
. 000
. 000
. 000
. 000
.028
.000
.000
.500
. 500
. 000
. 000
.300
.300
.500
.000
.000
0.
0 .
0 .
0 .
0 .
0.
0.
0.
0.
0 .
0 .
0 .
0 .
0 .
0.
0.
1.
1.
0 .
0 .
0 .
0 .
0.
0.
0.
0 .
0 .
0 .
0 .
0.
0.
0.
0.
0 .
0 .
0 .
0 .
0 .
1.
1.
1.
1.
1.
1.
0 .
0 .
0.
0.
0.
0 .
0 .
0 .
0 .
0.
0.
0.
0.
0 .
0 .
0 .
0 .
0 .
0.
0.
0.
.020
. 020
. 020
. 010
. 010
.010
.010
.010
.010
. 010
. 010
. 010
. 010
. 010
.010
.010
.000
.000
. 010
. 010
. 010
. 010
.010
.010
.010
. 010
. 030
. 030
. 030
.030
.030
.030
.030
. 030
. 030
. 040
. 010
. 010
.000
.000
.000
.000
. 000
. 000
. 010
. 010
.010
.010
.020
. 020
. 020
. 020
. 040
.040
.010
.010
.010
. 010
. 010
. 010
. 010
. 010
.010
.010
.010
Page 15 of 30
-------
Attachment 2. Inputs for the chronic dietary exposure analysis of fluoride from structural
fumigation with sulfuryl fluoride
U.S. Environmental Protection Agency Ver. 2.00
DEEM-FCID Chronic analysis for FLUORIDE 1994-98 data
Residue file: C:\Documents and Settings\mdoherty\My Documents\Chemistry Reviews\!DEEM
Runs\Sulfuryl Fluoride\F Space Fumigation - 2009 - 5-1.R98
Adjust. #2 used
Analysis Date 05-06-2009 Residue file dated: 05-06-2009/13:52:45/8
Reference dose (RfD) = 0.114 mg/kg bw/day
Adj.Factors
#1 #2
18000020
14000030
14000031
14000040
14000041
95000060
11000090
11000091
12000130
01030150
01030151
95000240
95000241
15000250
15000251
15000260
15000261
15000270
19010280
19010281
19010290
19010291
06030300
06030320
06030340
06030350
06030360
06030380
06030390
06030400
06030410
06030420
21000450
01010530
01010531
14000590
15000650
15000660
14000680
14000810
14000920
06030980
06030981
06030990
01011000
19011030
04011040
19021050
19021051
95001090
95001100
95001110
95001111
95001120
95001130
95001140
18
14
14
14
14
O
11
11
12
1CD
1CD
O
O
15
15
15
15
15
19A
19A
19A
19A
6C
6C
6C
6C
6C
6C
6C
6C
6C
6C
M
1A
1A
14
15
15
14
14
14
6C
6C
6C
1AB
19A
4A
19B
19B
O
O
O
O
O
O
O
Alfalfa, seed
Almond
Almond -baby food
Almond, oil
Almond, oil-babyfood
Amaranth, grain
Apple, dried
Apple, dried-babyf ood
Apricot, dried
Arrowroot, flour
Arrowroot, f lour-babyf ood
Banana, dried
Banana, dried-babyf ood
Barley, pearled barley
Barley, pearled barley-babyf ood
Barley, flour
Barley, f lour-babyf ood
Barley, bran
Basil, fresh leaves
Basil, fresh leaves-babyf ood
Basil, dried leaves
Basil, dried leaves-babyf ood
Bean, black, seed
Bean, broad, seed
Bean, cowpea, seed
Bean, great northern, seed
Bean, kidney, seed
Bean, lima, seed
Bean, mung, seed
Bean, navy, seed
Bean, pink, seed
Bean, pinto, seed
Beef, meat, dried
Beet, sugar, molasses
Beet, sugar, molasses-babyf ood
Brazil nut
Buckwheat
Buckwheat, flour
Butternut
Cashew
Chestnut
Chickpea, seed
Chickpea, seed-babyf ood
Chickpea, flour
Chicory, roots
Chive
Chrysanthemum, garland
Cinnamon
Cinnamon -baby food
Cocoa bean, chocolate
Cocoa bean, powder
Coconut, meat
Coconut- meat-babyfood
Coconut, dried
Coconut, milk
Coconut, oil
20.
9 .
9 .
1.
1.
20.
1.
1 .
1.
31.
31.
1.
1.
3 .
3.
0 .
0 .
3.
67.
67 .
67.
67 .
4 .
4 .
4 .
4 .
4 .
4 .
4 .
4 .
4 .
4 .
58.
1.
1.
3.
2 .
0.
3.
3.
3.
4 .
4 .
4 .
13.
63.
63.
73.
73.
8 .
8.
49.
49.
49.
49.
1 .
. 400000
. 200000
. 200000
.500000
.500000
.400000
.000000
. 000000
. 000000
. 400000
. 400000
.000000
.000000
.650000
. 650000
. 156000
. 156000
. 650000
.100000
.100000
.100000
.100000
. 500000
. 500000
. 500000
. 500000
. 500000
.500000
.500000
.500000
.500000
. 500000
. 400000
. 200000
. 200000
. 900000
. 900000
.134000
. 900000
. 900000
. 900000
. 500000
.500000
.500000
. 900000
.500000
. 500000
. 500000
. 500000
. 400000
. 400000
.100000
.100000
.100000
.100000
. 500000
1. 000
1 . 000
1. 000
1.000
1.000
1.000
1.000
1 . 000
1 . 000
1. 000
1 . 000
1.000
1.000
1.000
1. 000
1 . 000
1. 000
1. 000
1.000
1.000
1.000
1.000
1 . 000
1 . 000
1 . 000
1 . 000
1 . 000
1.000
1.000
1.000
1.000
1. 000
1. 000
1 . 000
1. 000
1.000
1.000
1.000
1 . 000
1. 000
1 . 000
1 . 000
1.000
1.000
1.000
1.000
1 . 000
1 . 000
1 . 000
1 . 000
1. 000
1.000
1.000
1.000
1.000
1 . 000
004
004
004
0.004
0.004
0.004
0.004
0 . 004
0 . 004
0 . 004
0 . 004
0.004
0.004
0.008
0. 008
1. 000
1. 000
0 . 008
0.004
0.004
0.004
0.004
0 . 004
0 . 004
0 . 004
0 . 004
0 . 004
0.004
0.004
0.004
0.004
0 . 004
0 . 004
0 . 004
0 . 004
0.004
0.008
1.000
0 . 004
0 . 004
0 . 004
0 . 004
0.004
0.004
0.004
0.004
0 . 004
0 . 004
0 . 004
0 . 004
0 . 004
0.004
0.004
0.004
0.004
0 . 004
Page 16 of 30
-------
95001141 0
95001150 O
95001160 O
19011180 19A
19011181 19A
19021190 19B
19021191 1 9B
15001200 15
15001201 15
15001210 15
15001211 15
15001220 15
15001230 15
15001231 15
15001240 15
15001241 15
15001250 15
15001251 15
15001260 15
95001280 O
95001281 O
95001310 O
13021370 13B
95001410 0
19021430 19B
19011440 19A
70001450 P
Coconut, oil-babyfood
Coffee, roasted bean
Coffee, instant
Coriander, leaves
Coriander, leaves-babyf ood
Coriander, seed
Coriander, seed-babyf ood
Corn, field, flour
Corn, field, f lour-babyf ood
Corn, field, meal
Corn, field, meal-babyf ood
Corn, field, bran
Corn, field, starch
Corn, field, starch-babyf ood
Corn, field, syrup
Corn, field, syrup-babyf ood
Corn, field, oil
Corn, field, oil-babyfood
Corn, pop
Cottonseed, oil
Cottonseed, oil-babyfood
Cranberry, dried
Currant, dried
Date
Dill, seed
Dillweed
Egg, whole
110-Uncooked; Fresh or N/S
120-Uncooked; Frozen; Cook
210-Cooked; Fresh or N/S;
211-Cooked; Fresh or N/S;
212-Cooked; Fresh or N/S;
213-Cooked; Fresh or N/S;
214-Cooked; Fresh or N/S;
215-Cooked; Fresh or N/S;
221-Cooked; Frozen; Baked
223-Cooked; Frozen; Fried
1.500000
7 . 100000
13. 900000
63 . 500000
63 . 500000
7.100000
7 . 100000
0.081000
0.081000
14 . 000000
14 . 000000
6 . 600000
6 . 600000
0.600000
0.600000
0.400000
0.400000
1 . 700000
1 . 500000
1 . 500000
1 . 000000
1.000000
0. 900000
7.100000
63 . 500000
; Cook Meth N/S
0 . 000000
Meth N/S
0.000000
Cook Meth N/S
0.000000
Baked 0 . 000000
Boiled
0 . 000000
Fried 0.000000
Fried/baked
0.000000
Boiled/baked
0.000000
0.000000
0 . 000000
224-Cooked; frozen; fried/baked 0.000000
230-Cooked; Dried; Cook Meth N/S
1.000
1 . 000
1. 000
1 . 000
1 . 000
1.000
1.000
1.000
1.000
1 . 000
1. 000
1 . 000
1 . 000
1 . 000
1.000
1.000
1.000
1.000
1 . 000
1 . 000
1 . 000
1. 000
1.000
1.000
1.000
1 . 000
1 . 000
1.000
1.000
1 . 000
1. 000
1 . 000
1.000
1.000
1.000
1 . 000
1 . 000
402.500000
Dried; Boiled 402.500000
Dried; Fried 402.500000
Cook Meth N/S
0.000000
Boiled
Canned;
0 .
242-Cooked
252-Cooked
253-Cooked
Egg, white
110-Uncooked; Fresh or N/S; Cook Meth N/S
0.000000
120-Uncooked; Frozen; Cook Meth N/S
130-Uncooked; Dried; Cook Meth N/S
402.500000
Cook Meth N/S
Baked 0.000000
Boiled
210-Cooked; Fresh or
Fried
Fried/baked
0.000000
Frozen; Baked 0.000000
Frozen; Fried 0.000000
Page 17 of 30
-------
70001461
95001540
14001550
14001560
20001630
03001650
03001651
01031670
01011680
95001780
06031820
06031821
19011840
19011841
14001850
19012020
06032030
95002120
14002130
95002160
95002180
95002190
19012200
19012201
27002220
P
O
14
14
20
3
3
1CD
1AB
O
6C
6C
19A
19A
14
19A
6C
O
14
O
O
O
19A
19A
D
Canned; Cook Meth N/S
ed;
ed;
Egg, white (sc
Fig, dried
Filbert
Filbert, oil
Flaxseed, oil
Garlic, dried
Garlic, dried-
Ginger, dried
Ginseng, dried
Grape, raisin
Guar, seed
Guar, seed-ba
Herbs, other
Herbs, other-
Hickory nut
Lemongrass
Lentil, seed
Lychee, dried
Macadamia nut
Mango, dried
Maple, sugar
Maple syrup
Marj oram
Marj oram-babyfood
Milk, fat
110-Uncooked
0 . 000000
Canned; Boiled 0.000000
Cured etc; Cook Meth N/S
0.000000
lids) -babyfood 402.500000
1.000000
1.500000
1 . 500000
1 . 500000
10. 900000
babyfood 10.900000
10. 900000
10.900000
1.000000
4.500000
yfood 4.500000
63 . 500000
>abyfood 63.500000
3. 900000
63. 500000
4.500000
1.000000
3. 900000
1 . 200000
1 . 200000
67 . 100000
ood 67.100000
.; Fresh or N/S; Cook Meth N/S
0.000000
.; Frozen; Cook Meth N/S
.; Dried; Cook Meth N/S
5 . 400000
.; Cured etc; Cook Meth N/S
3. 900000
Fresh or N/S; Cook Meth N/S
0.000000
Fresh or N/S; Baked 0.000000
Fresh or N/S; Boiled
Fresh or N/S; Fried 0.000000
Fresh or N/S; Fried/baked
0.000000
Fresh or N/S; Boiled/baked
0.000000
Frozen; Cook Meth N/S
Frozen; Baked 0.000000
Frozen; Boiled 0.000000
Frozen; Fried 0.000000
Frozen; Fried/baked 0.000000
Dried; Cook Meth N/S
5.400000
Dried; Baked 5.400000
Dried; Boiled 5.400000
1. 000
1 . 000
1.000
1.000
1.000
1.000
1 . 000
1. 000
1. 000
1 . 000
1. 000
1.000
1.000
1.000
1.000
1 . 000
1.000
1. 000
1. 000
1.000
1.000
1.000
1 . 000
1 . 000
1. 000
1 . 000
1.000
1.000
1 . 000
1. 000
1.000
1.000
1.000
1 . 000
1 . 000
1.000
1.000
1 . 000
1 . 000
1 . 000
1.000
1.000
1.000
1. 000
1 . 000
0 .
0 .
0.
0.
0.
0.
0 .
0 .
0 .
0 .
0 .
0.
0.
0.
0.
0 .
0
0 .
0 .
0.
0.
0.
0 .
0 .
0 .
0 .
0.
0.
0 .
0 .
0.
0.
0.
0 .
0 .
0.
0.
0 .
0 .
0 .
0.
0.
0.
0 .
0 .
. 004
. 004
.004
.004
.004
.004
. 004
. 004
. 004
. 004
. 004
.004
.004
.004
.004
. 004
,004
. 004
. 004
.004
.004
.004
. 004
. 004
. 004
. 004
.004
.004
. 004
. 004
.004
.004
.004
. 004
. 004
.004
.004
. 004
. 004
. 004
.004
.004
.004
. 004
. 004
Dried; Fried 5
Canned; Cook Meth N/S
.400000
1. 000
Canned; Boiled 0.000000
Cured etc; Cook Meth N/S
3.900000
Cured etc; Fried 3.900000
Cured etc; Boiled/baked
3.900000
Milk, nonfat solids
110-Uncooked; Fresh or N/S; Cook Meth N/S
0.000000
120-Uncooked; Frozen; Cook Meth N/S
0.000000
0 . 004
Page 18 of 30
-------
255-
Uncooked; Dried; Cook Meth N/S
5.400000
Uncooked; Cured etc; Cook Meth N/S
3.900000
Cooked; Fresh or N/S; Cook Meth N/S
0.000000
Cooked; Fresh or N/S; Baked 0.000000
Cooked; Fresh or N/S; Boiled
0.000000
Cooked; Fresh or N/S; Fried 0.000000
Cooked; Fresh or N/S; Fried/baked
Cooked; Fresh or N/S; Boiled/baked
Cooked; Frozen; Cook Meth N/S
0.000000
Cooked; Frozen; Baked 0.000000
Cooked; Frozen; Boiled 0.000000
Cooked; Frozen; Fried 0.000000
Cooked; Frozen; Fried/baked 0.000000
Cooked; Dried; Cook Meth N/S
5.400000
Cooked; Dried; Baked 5.400000
Cooked; Dried; Boiled 5.400000
Cooked; Dried; Fried 5.400000
Cooked; Canned; Cook Meth N/S
0.000000
Cooked; Canned; Boiled 0.000000
Cooked; Canned; Boiled/baked
0.000000
Cooked; Cured etc; Cook Meth N/S
3.900000
Cooked; Cured etc; Fried 3.900000
Cooked; Cured etc; Boiled/baked
3.900000
nonfat solids-baby food/infant
Uncooked; Fresh or N/S; Cook Meth N/S
0.000000
Uncooked; Dried; Cook Meth N/S
5.400000
Cooked; Fresh or N/S; Baked 0.000000
Cooked; Canned; Cook Meth N/S
0.000000
water
Uncooked; Fresh or N/S; Cook Meth N/S
Uncooked; Frozen; Cook Meth N/S
0.000000
Uncooked; Dried; Cook Meth N/S
5.400000
Uncooked; Cured etc; Cook Meth N/S
3.900000
Cooked; Fresh or N/S; Cook Meth N/S
0.000000
Cooked; Fresh or N/S; Baked 0.000000
Cooked; Fresh or N/S; Boiled
0.000000
Cooked; Fresh or N/S; Fried 0.000000
Cooked; Fresh or N/S; Fried/baked
Cooked; Fresh or N/S; Boiled/baked
Cooked; Frozen; Cook Meth N/S
0.000000
Cooked; Frozen; Baked 0.000000
Cooked; Frozen; Boiled 0.000000
Cooked; Frozen; Fried 0.000000
Cooked; Frozen; Fried/baked 0.000000
Cooked; Dried; Cook Meth N/S
5.400000
Cooked; Dried; Baked 5.400000
Cooked; Dried; Boiled 5.400000
Cooked; Dried; Fried 5.400000
Page 19 of 30
-------
15002260
15002310
15002320
15002321
15002330
15002331
95002360
03002380
03002381
95002440
95002441
95002460
190124 90
19012491
06032560
06032561
06032580
12002610
12002611
95002630
95002640
95002650
11002670
14002690
08002710
08002711
08002730
19022740
19022741
95002760
95002780
95002800
14002820
95002840
12002870
12002871
01032960
01032970
01032971
01032980
01032981
95003060
09023090
95003110
20003190
20003191
15003230
15003231
15003240
15003241
15003250
15003251
15
15
15
15
15
15
O
3
3
O
O
O
19A
19A
6C
6C
6C
12
12
O
O
O
11
14
8
8
8
19B
19B
O
O
O
14
O
12
12
1C
1C
1C
1C
1C
O
9B
O
20
20
15
15
15
15
15
15
Canned; Cook Meth N/S
0.000000
Canned; Boiled 0.000000
Cured etc; Cook Meth N/S
3.900000
Cured etc; Fried 3.900000
Cured etc; Boiled/baked
3.900000
Milk, sugar (lactose)-baby food/infa
110-Uncooked; Fresh or N/S; Cook Meth N/S
0.000000
130-Uncooked; Dried; Cook Meth N/S
5.400000
Fresh or N/S; Cook Meth N/S
0.000000
Fresh or N/S; Boiled
0.000000
Dried; Cook Meth N/S
240-Cooked; Canned; Cook Meth N/S
Millet, grain
Oat, bran
Oat, flour
Oat, flour-babyfood
Oat, groats/rolled oats
Oat, groats/rolled oats-babyfood
Olive, oil
Onion, dry bulb, dried
Onion, dry bulb, dried-babyfood
Palm, oil
Palm, oil-babyfood
Papaya, dried
Parsley, dried leaves
Parsley, dried leaves-babyfood
Pea, dry
Pea, dry-babyfood
Pea, pigeon, seed
Peach, dried
Peach, dried-babyfood
Peanut
Peanut, butter
Peanut, oil
Pear, dried
Pecan
Pepper, bell, dried
Pepper, bell, dried-babyfood
Pepper, nonbell, dried
Pepper, black and white
Pepper, black and white-babyfood
Peppermint, oil
Pine nut
Pineapple, dried
Pistachio
Plantain, dried
Plum, prune, dried
Plum, prune, dried-babyfood
Potato, chips
Potato, dry (granules/ flakes)
Potato, dry (granules/ flakes)-b
Potato, flour
Potato, flour-babyfood
Psyllium, seed
Pumpkin, seed
Quinoa, grain
Rapeseed, oil
Rapeseed, oil-babyfood
Rice, white
Rice, white-babyfood
Rice, brown
Rice
Rice, flour
Rice
0 .
2.
4 .
0.
0.
.8.
.8.
1.
1.
1.
1.
1.
1.
,3.
S3.
4 .
4 .
4 .
1.
1.
.6.
.6.
1.
1.
3.
;6.
!6.
16.
7 .
7 .
1.
8.
1.
2 .
1.
0.
0.
7 .
:5.
ii.
ii.
7 .
8.
:o.
1.
1.
3.
3.
9 .
9
0.
0.
. 000000
. 900000
.200000
.337000
.337000
. 500000
500000
. 500000
. 700000
.700000
.500000
.500000
.000000
500000
. 500000
. 500000
. 500000
500000
.000000
.000000
.400000
.400000
500000
. 000000
. 900000
. 100000
.100000
.100000
.100000
. 100000
. 500000
. 800000
. 000000
.300000
.000000
.700000
.700000
. 100000
. 600000
. 600000
. 400000
. 400000
.100000
.800000
.400000
.500000
. 500000
. 900000
. 900000
. 400000
.400000
.160000
.160000
1. 000
1. 000
1.000
1.000
1.000
1. 000
1 . 000
1. 000
1 . 000
1.000
1.000
1.000
1.000
1 . 000
1. 000
1. 000
1. 000
1 . 000
1.000
1.000
1.000
1.000
1 . 000
1. 000
1 . 000
1. 000
1.000
1.000
1.000
1. 000
1. 000
1 . 000
1. 000
1.000
1.000
1.000
1.000
1. 000
1 . 000
1. 000
1. 000
1. 000
1.000
1.000
1.000
1.000
1. 000
1 . 000
1. 000
1 . 000
1.000
1.000
1.000
0 .
0 .
0.
1.
1.
0 .
0 .
0 .
0 .
0.
0.
0.
0.
0 .
0 .
0 .
0 .
0 .
0.
0.
0.
0.
0 .
0 .
0 .
0 .
0.
0.
0.
0 .
0 .
0 .
0 .
0.
0.
0.
0.
0 .
0 .
0 .
0 .
0 .
0.
0.
0.
0.
0 .
0 .
0 .
0 .
0.
1.
1.
. 004
. 008
.008
.000
.000
. 008
. 008
. 004
. 004
.004
.004
.004
.004
. 004
. 004
. 004
. 004
. 004
.004
.004
.004
.004
. 004
. 004
. 004
. 004
.004
.004
.004
. 004
. 004
. 004
. 004
.004
.004
.004
.004
. 004
. 004
. 004
. 004
. 004
.004
.004
.004
.004
. 004
. 008
. 008
. 008
.008
.000
.000
Page 20 of 30
-------
Rice, bran
Rice, bran-babyfood
Rye, grain
Rye, flour
Safflower, oil
Safflower, oil-babyfood
Savory
Sesame, seed
Sesame, seed-babyfood
Sesame, oil
Sesame, oil-babyfood
Sorghum, grain
Sorghum, syrup
S o yb ean, flour
Soybean, flour-babyfood
Soybean, soy milk
Soybean, soy milk-babyfood or in
Soybean, oil
Soybean, oil-babyfood
Spearmint, oil
Spices, other
Spices, other-babyfood
Sugarcane, sugar
Sugarcane, sugar-babyfood
Sugarcane, molasses
Sugarcane, molasses-babyfood
Sunflower, seed
Sunflower, oil
Sunflower, oil-babyfood
Tea, dried
Tea, instant
Tomato, dried
Tomato, dried-babyfood
Triticale, flour
Triticale, flour-babyfood
Turmeric
Walnut
Wheat, grain
Wheat, grain-babyfood
Wheat, flour
Wheat, flour-babyfood
Wheat, germ
Wheat, bran
Wild rice
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
Page 21 of 30
-------
Attachment 3. Inputs for the chronic dietary exposure analysis of fluoride from food fumigation
with sulfuryl fluoride
U.S. Environmental Protection Agency Ver. 2.00
DEEM-FCID Chronic analysis for FLUORIDE 1994-98 data
Residue file: C:\Documents and Settings\mdoherty\My Documents\Chemistry Reviews\!DEEM
Runs\Sulfuryl Fluoride\F Food Fumigation - 2009 RevisedCT - 4-28 Strict Label.R98
Adjust. #2 used
Analysis Date 05-06-2009 Residue file dated: 05-06-2009/13:54:06/8
Reference dose (RfD) = 0.114 mg/kg bw/day
Food Crop
EPA Code Grp
14000030
14000031
11000090
11000091
12000130
95000240
95000241
15000250
15000251
15000260
15000261
15000270
19010290
19010291
06030300
06030320
06030340
06030350
06030360
06030380
06030390
06030400
06030410
06030420
14000590
14000680
14000810
14000920
06030980
06030981
06030990
19011030
19021050
19021051
95001090
95001100
95001110
95001111
95001120
95001130
95001150
95001160
19011180
19011181
19021190
19021191
15001200
15001201
15001210
15001211
15001220
15001230
15001231
15001240
15001241
15001260
14
14
11
11
12
O
O
15
15
15
15
15
19A
19A
6C
6C
6C
6C
6C
6C
6C
6C
6C
6C
14
14
14
14
6C
6C
6C
19A
19B
19B
O
O
O
O
O
O
O
O
19A
19A
19B
1 9B
15
15
15
15
15
15
15
15
15
15
Food Name
Almond
Almond -baby food
Apple, dried
Apple, dried-babyfood
Apricot, dried
Banana, dried
Banana, dried-babyfood
Barley, pearled barley
Barley, pearled barley-babyf ood
Barley, flour
Barley, flour babyf ood
Barley, bran
Basil, dried leaves
Basil, dried leaves-babyf ood
Bean, black, seed
Bean, broad, seed
Bean, cowpea, seed
Bean, great northern, seed
Bean, kidney, seed
Bean, lima, seed
Bean, mung, seed
Bean, navy, seed
Bean, pink, seed
Bean, pinto, seed
Brazil nut
Butternut
Cashew
Chestnut
Chickpea, seed
Chickpea, seed-babyf ood
Chickpea, flour
Chive
Cinnamon
Cinnamon -baby food
Cocoa bean, chocolate
Cocoa bean, powder
Coconut, meat
Coconut- meat-babyfood
Coconut, dried
Coconut, milk
Coffee, roasted bean
Coffee, instant
Coriander, leaves
Coriander, leaves-babyf ood
Coriander, seed
Coriander, seed-babyf ood
Corn, field, flour
Corn, field, f lour-babyf ood
Corn, field, meal
Corn, field, meal-babyf ood
Corn, field, bran
Corn, field, starch
Corn, field, starch-babyf ood
Corn, field, syrup
Corn, field, syrup-babyf ood
Corn, pop
Residue
(ppm)
9 .
9 .
1 .
1.
1.
1.
1.
3.
3.
3.
3.
3 .
67 .
67.
4 .
4 .
4 .
4 .
4 .
4 .
4 .
4 .
4 .
4 .
5
5 .
5.
5 .
4 .
4 .
4 .
63.
73.
73.
8.
8.
49.
49.
49.
49.
7 .
13.
63.
63.
-j
16.
16.
2.
2.
2.
0.
0.
0.
0.
1 .
. 700000
. 700000
. 000000
.000000
.000000
.000000
.000000
. 700000
. 700000
. 700000
700000
.700000
.100000
.100000
. 500000
. 500000
. 500000
. 500000
.500000
.500000
.500000
.500000
. 500000
. 500000
. 300000
. 300000
. 300000
.300000
.500000
.500000
.500000
. 500000
. 500000
. 500000
. 400000
.400000
.100000
.100000
. 100000
. 100000
. 100000
. 900000
.500000
.500000
.100000
. 100000
. 900000
. 900000
. 800000
. 800000
. 800000
.600000
.600000
.600000
.600000
. 700000
Adj . Fa
#1
1. 000
1 . 000
1 . 000
1.000
1.000
1.000
1.000
1 . 000
1 . 000
0. 730
0. 730
2.560
1.000
1.000
1 . 000
1 . 000
1 . 000
1. 000
1.000
1.000
1.000
1.000
1 . 000
1 . 000
1 . 000
1. 000
1 . 000
1.000
1.000
1.000
1.000
1. 000
1 . 000
1 . 000
1. 000
1.000
1.000
1.000
1 . 000
1. 000
1 . 000
1. 000
1.000
1.000
1.000
1.000
1. 000
1 . 000
1. 000
1 . 000
1. 000
1.000
1.000
1.000
1.000
1 . 000
ctors Comment
#2
0 .
0 .
0 .
0.
0.
0.
0.
0 .
0 .
0 .
0 .
0.
0.
0.
1 .
1.
1 .
1.
1.
1.
1.
1.
1.
1 .
0 .
0 .
0 .
0.
1.
1.
1.
0 .
0 .
0 .
1.
1.
0.
0.
0 .
0 .
0 .
0 .
0.
0.
0.
0 .
0 .
0 .
0 .
0 .
0 .
0.
0.
0.
0.
0 .
.100
. 100
. 690
.690
.690
.690
.690
. 001
. 001
. 001
. 001
.001
.001
.001
. 000
. 000
. 000
. 000
.000
.000
.000
.000
. 000
. 000
. 100
.100
. 100
.100
.000
.000
.000
. 001
. 001
. 001
. 000
.000
.001
.001
. 001
. 001
. 001
. 001
.001
.001
.001
.001
. 001
. 001
. 001
. 001
. 001
.001
.001
.001
.001
. 001
Page 22 of 30
-------
Cranberry, dried
Currant, dried
Date
130-Uncooked; Dried;
000000
oooooo
19021430
19011440
95001540
14001550
03001650
01031660
01031661
01031670
95001780
06031820
06031821
19011840
19011841
14001850
19012020
06032030
95002120
14002130
95002160
19012200
19012201
15002260
15002310
15002320
15002321
15002330
15002331
95002460
19012490
19012491
06032560
06032561
06032580
12002610
12002611
95002630
95002640
11002670
14002690
19022740
19022741
95002780
95002800
14002820
95002840
12002870
12002871
15003230
15003231
15003240
15003241
15003250
15003251
15003260
15003261
19013340
15003440
19023540
19023541
15003810
15003811
19B
19A
O
14
^
1CD
1CD
1CD
O
6C
6C
19A
19A
14
19A
6C
O
14
O
19A
19A
15
15
15
15
15
15
O
19A
19A
6C
6C
6C
12
12
O
O
11
14
19B
19B
O
O
14
O
12
12
15
15
15
15
15
15
15
15
19A
15
19B
19B
15
15
Cook Meth N/S
0 .
Fresh or N/S; Cook Meth
0.
Fresh or N/S; Baked 0.
Fresh or N/S; Boiled
230-Cooked; Dried; Cook Meth N/S
Dill, seed
Dillweed 6
Fig, dried
Filbert
Garlic, dried 1
Ginger 1
Ginger-babyfood 1
Ginger, dried 1
Grape, raisin
Guar, seed
Guar, seed-babyfood
Herbs, other 6
Herbs, other-babyfood 6
Hickory nut
Lemongrass 6
Lentil, seed
Lychee, dried
Macadamia nut
Mango, dried
Marjoram 6
Marjoram-babyfood 6
Millet, grain
Oat, bran 1
flour 1
flour-babyfood 1
Oat, groats/rolled oats 1
Oat, groats/rolled oats-babyfood 1
Papaya, dried
Parsley, dried leaves 6
Parsley, dried leaves-babyfood 6
Pea, dry
Pea, dry-babyfood
Pea, pigeon, seed
Peach, dried
Peach, dried-babyfood
Peanut 1
Peanut, butter 1
Pear, dried
Pecan
Pepper, black and white
Pepper, black and white-babyfood
Pine nut
Pineapple, dried
Pistachio
Plantain, dried
Plum, prune, dried
Plum, prune, dried-babyfood
Rice, white
Rice, white-babyfood
Rice, brown 1
Rice, brown-babyfood 1
Rice, flour 2
Rice, bran
Rice, bran-babyfood
Savory
Sorghum, grain
Spices, other
Spices, other-babyfood
Triticale, flour
Triticale, flour-babyfood
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
560
730
730
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
380
1
0. 420
0 . 001
0. 001
0.690
0.100
0.001
0.001
0. 001
0 . 001
0. 690
1 . 000
000
0.001
0.001
0.100
0 . 001
1. 000
0.690
0.001
0.690
0.001
0.001
0 . 001
0. 001
0 . 001
0. 001
0 . 001
0.001
0.690
0.001
0.001
1 . 000
1. 000
1 . 000
0. 690
0.690
0.006
0.006
0.690
0.100
0 . 001
0. 001
0.100
0.690
0.270
0.690
0. 690
0.690
0. 030
0 . 030
0. 030
0.030
0.030
0.030
0.030
0. 030
0 . 001
0. 001
0 . 001
0.001
0.001
0.001
Page 23 of 30
-------
Walnut
Wheat, grain
Wheat, grain-babyfood
Wheat, flour
Wheat, flour-babyfood
Wheat, germ
Wheat, bran
Wild rice
Page 24 of 30
-------
Attachment 4. Results of the chronic dietary exposure analysis of fluoride from cryolite
U.S. Environmental Protection Agency Ver. 2.00
DEEM-FCID Chronic analysis for CRYOLITE (1994-98 data)
Residue file name: C:\Documents and Settings\mdoherty\My Documents\Chemistry Reviews\!DEEM
Runs\Sulfuryl Fluoride\Cryolite-AR-CT new raisin factor.R98
Adjustment factor #2 used.
Analysis Date 02-19-2009/14:16:56 Residue file dated: 06-24-2004/10:05:08/8
Total exposure by population subgroup
U.S. Population (total)
U.S. Population (spring season)
U.S. Population (summer season)
U.S. Population (autumn season)
U.S. Population (winter season)
Northeast region
Midwest region
Southern region
Western region
Hispanics
Non-hispanic whites
Non-hispanic blacks
Non-hisp/non-white/non-black
All infants (< 1 year)
Nursing infants
Non-nursing infants
Children 1-6 yrs
Children 7-12 yrs
Females 13-19 (not preg or nursing)
Females 20+ (not preg or nursing)
Females 13-50 yrs
Females 13+ (preg/not nursing)
Females 13+ (nursing)
Children 1-2 yrs
Children 3-5 yrs
Children 6-12 yrs
Youth 13-19 yrs
Adults 20-49 yrs
Adults 50+ yrs
Females 13-49 yrs
Page 25 of 30
-------
Attachment 5. Results of the chronic dietary exposure analysis of fluoride from structural
fumigation with sulfuryl fluoride
U.S. Environmental Protection Agency Ver. 2.00
DEEM-FCID Chronic analysis for FLUORIDE (1994-98 data)
Residue file name: C:\Documents and Settings\mdoherty\My Documents\Chemistry Reviews\!DEEM
Runs\Sulfuryl Fluoride\F Space Fumigation - 2009 - 5-1.R98
Adjustment factor #2 used.
Analysis Date 05-06-2009/13:56:30 Residue file dated: 05-06-2009/13:52:45/8
Reference dose (RfD, Chronic) = .114 mg/kg bw/day
Total Exposure
Population
Subgroup
Population (spring season)
Population (summer season)
Population (autumn season)
Population (winter season)
Northeast region
Midwest region
Southern region
Western region
Hispanics
Non-hispanic whites
Non-hispanic blacks
Non-hisp/non-white/non-black
All infants (< 1 year)
Nursing infants
Non-nursing infants
Children 1-6 yrs
Children 7-12 yrs
Females 13-19 (not preg or nursing)
Females 20+ (not preg or nursing)
Females 13-50 yrs
Females 13+ (preg/not nursing)
Females 13+ (nursing)
Children 1-2 yrs
Children 3-5 yrs
Children 6-12 yrs
Youth 13-19 yrs
Adults 20-49 yrs
Adults 50+ yrs
Females 13-49 yrs
Page 26 of 30
-------
Attachment 6. Results of the chronic dietary exposure analysis of fluoride from food fumigation
with sulfuryl fluoride
U.S. Environmental Protection Agency Ver. 2.00
DEEM-FCID Chronic analysis for FLUORIDE (1994-98 data)
Residue file name: C:\Documents and Settings\mdoherty\My Documents\Chemistry Reviews\!DEEM
Runs\Sulfuryl Fluoride\F Food Fumigation - 2009 RevisedCT - 4-28 Strict Label.R98
Adjustment factor #2 used.
Analysis Date 05-06-2009/13:57:26 Residue file dated: 05-06-2009/13:54:06/8
Reference dose (RfD, Chronic) = .114 mg/kg bw/day
Total exposure by population subgroup
U.S.
Population
Subgroup
U.S. Population (total)
Total Exposure
Northeast region
Midwest region
Southern region
Western region
Hispanics
Non-hispanic whites
Non-hispanic blacks
Non-hisp/non-white/non-black
All infants (< 1 year)
Nursing infants
Non-nursing infants
Children 1-6 yrs
Children 7-12 yrs
Females 13-19 (not preg or nursing)
Females 20+ (not preg or nursing)
Females 13-50 yrs
Females 13+ (preg/not nursing)
Females 13+ (nursing)
Children 1-2 yrs
Children 3-5 yrs
Children 6-12 yrs
Youth 13-19 yrs
Adults 20-49 yrs
Adults 50+ yrs
Females 13-49 yrs
Page 27 of 30
-------
Attachment 7. Commodity contribution summary for the chronic dietary exposure analysis of fluoride from cryolite
Crop Group = (O) Other
Crop Group = (1) Root and Tuber Vegetables
Crop Group = (1C) Tuberous and Corm Vegetables
Crop Group = (4) Leafy Vegetables (except Brassica)
Crop Group = (4A) Leafy Greens
Crop Group = (5) Brassica (Cole) Leafy Vegetables
Crop Group = (5A) Brassica: Head and Stem
Crop Group = (5B) Brassica: Leafy Greens
Crop Group = (8) Fruiting Vegetables
Crop Group = (9) Curcurbit Vegetables
Crop Group = (9 A) Melons
Crop Group = (9B) Squash/Cucumbers
Crop Group = (10) Citrus Fruits
Crop Group = (12) Stone Fruits
Crop Group = (13) Berries
Crop Group = (13A)Berries: Caneberry Group
Crop Group = (13B)Berries: Bushberry Group
Ex
U.S.
0.0005567
0.0000189
0.0000189
0.0000077
0.0000077
0.0000148
0.0000135
0.0000013
0.0000149
0.0000091
0.0000052
0.0000039
0.0000462
0.0000073
0.0000061
0.0000041
0.0000020
Infants
0.0008359
0.0000169
0.0000169
0.0000000
0.0000000
0.0000082
0.0000080
0.0000002
0.0000059
0.0000110
0.0000017
0.0000094
0.0000159
0.0000502
0.0000117
0.0000050
0.0000067
Kl-2
0.0030082
0.0000430
0.0000430
0.0000040
0.0000040
0.0000313
0.0000287
0.0000026
0.0000274
0.0000162
0.0000109
0.0000052
0.0001014
0.0000294
0.0000147
0.0000088
0.0000059
K3-5
0.0018675
0.0000388
0.0000388
0.0000061
0.0000061
0.0000230
0.0000201
0.0000029
0.0000251
0.0000186
0.0000133
0.0000054
0.0001027
0.0000159
0.0000147
0.0000096
0.0000051
posure, mg/kg/day
K6-12
0.0007324
0.0000260
0.0000260
0.0000063
0.0000063
0.0000167
0.0000157
0.0000011
0.0000182
0.0000121
0.0000080
0.0000041
0.0000544
0.0000092
0.0000093
0.0000062
0.0000030
Y13-19
0.0002507
0.0000195
0.0000195
0.0000075
0.0000075
0.0000094
0.0000073
0.0000021
0.0000136
0.0000074
0.0000043
0.0000031
0.0000298
0.0000033
0.0000049
0.0000035
0.0000014
A20-50
0.0003483
0.0000157
0.0000157
0.0000088
0.0000088
0.0000131
0.0000122
0.0000009
0.0000141
0.0000068
0.0000034
0.0000034
0.0000305
0.0000039
0.0000042
0.0000027
0.0000015
A50+
0.0004115
0.0000150
0.0000150
0.0000077
0.0000077
0.0000161
0.0000146
0.0000015
0.0000127
0.0000098
0.0000057
0.0000041
0.0000614
0.0000073
0.0000056
0.0000043
0.0000013
Fern 13-49
0.0003740
0.0000147
0.0000147
0.0000094
0.0000094
0.0000134
0.0000123
0.0000010
0.0000131
0.0000074
0.0000041
0.0000033
0.0000322
0.0000046
0.0000046
0.0000028
0.0000017
Page 28 of 30
-------
Attachment 8. Commodity contribution summary for the chronic dietary exposure analysis of fluoride from structural fumigation with
sulfuryl fluoride
Crop Group = (O) Other
Crop Group = (M) Meat
Crop Group = (P) Poultry
Crop Group = (D) Dairy Products
Crop Group = (1) Root and Tuber Vegetables
Crop Group = (1A) Root Vegetables
Crop Group = (IB) Root Vegetables (exc sugar beet) subgroup
Crop Group = (1C) Tuberous and Corm Vegetables
Crop Group = (ID) Tuberous/Corm Vegetables (exc sugar beet)
Crop Group = (3) Bulb Vegetables
Crop Group = (4) Leafy Vegetables (except Brassica)
Crop Group = (4A) Leafy Greens
Crop Group = (6) Legume Vegetables (Succulent or Dried)
Crop Group = (6C) Dried Shelled Pea/Bean (exc Soybean)
Crop Group = (8) Fruiting Vegetables
Crop Group = (9) Curcurbit Vegetables
Crop Group = (9B) Squash/Cucumbers
Crop Group = (11) Pome Fruits
Crop Group = (12) Stone Fruits
Crop Group = (13) Berries
Crop Group = (13B)Berries: Bushberry Group
Crop Group = (14) Tree Nuts
Crop Group = (15) Cereal Grains
Crop Group = (19) Herbs and Spices
Crop Group = (19A)Herbs
Crop Group = (19B)Spices
Crop Group = (20) Oilseeds
Ex)
U.S.
0.0000126
0.0000004
0.0000103
0.0000032
0.0000029
0.0000000
0.0000000
0.0000029
0.0000000
0.0000002
0.0000000
0.0000000
0.0000063
0.0000021
0.0000004
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000003
0.0002967
0.0000021
0.0000017
0.0000004
0.0000003
Infants
0.0000145
0.0000000
0.0000055
0.0000684
0.0000047
0.0000000
0.0000000
0.0000047
0.0000000
0.0000002
0.0000000
0.0000000
0.0000318
0.0000013
0.0000003
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0003739
0.0000013
0.0000011
0.0000002
0.0000039
Kl-2
0.0000255
0.0000009
0.0000296
0.0000135
0.0000079
0.0000000
0.0000000
0.0000079
0.0000000
0.0000006
0.0000000
0.0000000
0.0000141
0.0000042
0.0000010
0.0000000
0.0000000
0.0000000
0.0000001
0.0000000
0.0000000
0.0000003
0.0007256
0.0000074
0.0000067
0.0000007
0.0000004
K3-5
0.0000293
0.0000002
0.0000210
0.0000096
0.0000082
0.0000000
0.0000000
0.0000082
0.0000000
0.0000005
0.0000000
0.0000000
0.0000126
0.0000039
0.0000009
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000004
0.0007112
0.0000058
0.0000049
0.0000009
0.0000004
josure, mg/kg/day
K6-12
0.0000196
0.0000006
0.0000118
0.0000031
0.0000050
0.0000000
0.0000000
0.0000050
0.0000000
0.0000003
0.0000000
0.0000000
0.0000083
0.0000026
0.0000006
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000003
0.0004892
0.0000035
0.0000027
0.0000008
0.0000004
Y13-19
0.0000098
0.0000011
0.0000079
0.0000017
0.0000029
0.0000000
0.0000000
0.0000029
0.0000000
0.0000002
0.0000000
0.0000000
0.0000056
0.0000021
0.0000004
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000002
0.0002876
0.0000021
0.0000017
0.0000005
0.0000003
A20-50
0.0000101
0.0000004
0.0000102
0.0000011
0.0000024
0.0000000
0.0000000
0.0000024
0.0000000
0.0000002
0.0000000
0.0000000
0.0000050
0.0000019
0.0000004
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000003
0.0002397
0.0000016
0.0000013
0.0000004
0.0000002
A50+
0.0000103
0.0000002
0.0000068
0.0000014
0.0000014
0.0000000
0.0000000
0.0000014
0.0000000
0.0000002
0.0000000
0.0000000
0.0000044
0.0000018
0.0000002
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000003
0.0001887
0.0000011
0.0000007
0.0000003
0.0000002
Feml3-49
0.0000095
0.0000004
0.0000110
0.0000011
0.0000024
0.0000000
0.0000000
0.0000023
0.0000000
0.0000002
0.0000000
0.0000000
0.0000046
0.0000017
0.0000003
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000000
0.0000003
0.0002171
0.0000016
0.0000012
0.0000003
0.0000002
Page 29 of 30
-------
Attachment 9. Commodity contribution summary for the chronic dietary exposure analysis of fluoride from food fumigation with
sulfuryl fluoride
Crop Group = (O) Other
Crop Group = (1) Root and Tuber Vegetables
Crop Group = (1C) Tuberous and Corm Vegetables
Crop Group = (ID) Tuberous/Corm Vegetables (exc sugar beet)
Crop Group = (3) Bulb Vegetables
Crop Group = (6) Legume Vegetables (Succulent or Dried)
Crop Group = (6C) Dried Shelled Pea/Bean (exc Soybean)
Crop Group = (11) Pome Fruits
Crop Group = (12) Stone Fruits
Crop Group = (13) Berries
Crop Group = (13B)Berries: Bushberry Group
Crop Group = (14) Tree Nuts
Crop Group = (15) Cereal Grains
Crop Group = (19) Herbs and Spices
Crop Group = (19A)Herbs
Crop Group = (19B)Spices
Ex)
U.S.
0.0003529
0.0000000
0.0000000
0.0000000
0.0000000
0.0005229
0.0005229
0.0000013
0.0000018
0.0000000
0.0000000
0.0000160
0.0001279
0.0000005
0.0000004
0.0000001
Infants
0.0001013
0.0000000
0.0000000
0.0000000
0.0000000
0.0003147
0.0003147
0.0000017
0.0000001
0.0000000
0.0000000
0.0000013
0.0006516
0.0000003
0.0000003
0.0000001
Kl-2
0.0007605
0.0000000
0.0000000
0.0000000
0.0000001
0.0010429
0.0010429
0.0000027
0.0000106
0.0000000
0.0000000
0.0000254
0.0003245
0.0000018
0.0000017
0.0000002
K3-5
0.0009980
0.0000000
0.0000000
0.0000000
0.0000001
0.0009719
0.0009719
0.0000030
0.0000020
0.0000000
0.0000000
0.0000258
0.0002907
0.0000014
0.0000012
0.0000002
josure, mg/kg/day
K6-12
0.0008601
0.0000000
0.0000000
0.0000000
0.0000001
0.0006484
0.0006484
0.0000023
0.0000022
0.0000000
0.0000000
0.0000187
0.0002108
0.0000009
0.0000007
0.0000002
Y13-19
0.0003866
0.0000000
0.0000000
0.0000000
0.0000000
0.0005166
0.0005166
0.0000012
0.0000002
0.0000000
0.0000000
0.0000111
0.0001159
0.0000005
0.0000004
0.0000001
A20-50
0.0002348
0.0000000
0.0000000
0.0000000
0.0000000
0.0004653
0.0004653
0.0000009
0.0000010
0.0000000
0.0000000
0.0000147
0.0000964
0.0000004
0.0000003
0.0000001
A50+
0.0001874
0.0000000
0.0000000
0.0000000
0.0000000
0.0004409
0.0004409
0.0000011
0.0000027
0.0000000
0.0000000
0.0000168
0.0000703
0.0000003
0.0000002
0.0000001
Feml3-49
0.0002649
0.0000000
0.0000000
0.0000000
0.0000000
0.0004267
0.0004267
0.0000010
0.0000009
0.0000000
0.0000000
0.0000147
0.0000906
0.0000004
0.0000003
0.0000001
Page 30 of 30
-------
UNITED STATES ENVIRONMENTAL PROTECTION AGENCY
WASHINGTON, D.C. 20460
OFFICE OF CHEMICAL SAFETY AND
POLLUTION PREVENTION
MEMORANDUM
Date: 1 July 2010
SUBJECT:
Sulfuryl Fluoride: Estimates of Fluoride Exposure from Pesticidal Sources
Customized Age Groups
PC Code: 078003 (Sulfuryl Fluoride)
MRIDNo.: None
Petition No.: None
Assessment Type: Single Chemical
TXRNo.: None
DP Barcode: D379854
Registration No.: None
Regulatory Action: None
Registration Case No.: None
CAS No.: 16984-48-8
FROM: Michael A. Doherty, Ph.D., Senior Chemist
Risk Assessment Branch II
Health Effects Division (7509P)
THROUGH:
TO:
Christina Swartz, Branch Chief
Douglas A. Dotson, Ph.D., Senior Chemist
Risk Assessment Branch II
Office of Pesticide Programs
Health Effects Division (7509P)
Elizabeth Doyle, Branch Chief
Human Health Risk Assessment Branch
Office of Water
Office of Science and Technology (4304T)
In May 2009, the EPA's Office of Pesticide Programs (OPP) provided the Office of Water (OW)
with estimates of exposure to fluoride from use of the pesticides cryolite and sulfuryl fluoride
(Memorandum from M. Doherty to E. Doyle, DP Number D362184, 6 May 2009). Those
estimates were for the populations and sub-populations typically addressed by OPP dietary risk
assessments; namely the general U.S. population, all infants (< 1 year), children 1-2 years,
children 3-5 years, children 6-12 years, youth 13-19 years, adults 20-49 years, adults 50+ years,
and females 13-49 years. Exposure estimates were presented in units of mg/kg body weight/day.
The 2009 exposure estimates were developed for use by the OW in their relative source
contribution (RSC) analysis for fluoride. A draft RSC analysis document was provided by the
OW to the OPP, at which time it became apparent that the OW is focusing on different
population subgroups and that exposure estimates are being presented in units of mg/day. The
Page 1 of 38
-------
OPP is providing new exposure estimates in order to match the population groups and exposure
units of primary interest to the OW.
The OPP has used the same input files that were used to estimate the exposures reported in the
May 2009 memorandum (included in Attachments 1-3 for reference). Rather than use the
chronic dietary exposure module in the Dietary Exposure Evaluation Model (DEEM), the OPP
has used the acute dietary exposure module, which provides a mechanism to (1) specify
customized population groupings and (2) leave body weight out of the exposure estimates to give
exposure in units of mg/day. Average exposure estimates from the acute module are identical to
the exposure estimates given by the chronic module. Average exposure estimates for the
customized population groups are summarized in Table I. Complete outputs of the three
analyses, including error estimates, are included as Attachments 4, 5, and 6.
Table 1. Summar
Age Range,
years
0.5 -<1
1 - <4
4-<7
7-
-------
CC:
Steve Bradbury (OPP/IO)
Ephraim King (OW/IO)
Tina Levine (OPP/HED)
Edward Ohanian (OW/HECD)
Steve Knizner (OPP/HED)
Richard Keigwin (OPP/SRRD)
Lois Rossi (QPP/RD)
Jon Fluechaus (OGC)
Attachments:
1. Inputs for cryolite fluoride exposure estimates
2. Inputs for sulfuryl fluoride food fumigation exposure estimates
3. Inputs for sulfuryl fluoride structural fumigation exposure estimates
4. Results of cryolite fluoride exposure analysis
5. Results of sulfuryl fluoride food fumigation exposure analysis
6. Results of sulfuryl fluoride structural fumigation exposure analysis
Page 3 of38
-------
Attachment 1. Inputs for cryolite fluoride exposure estimates
Filename: C:\Documents and Settings\MDOHERTY\My Documeats\Cheinistry Reviews\DEEM Runs\Sulfuryl
Fluoride\Cryolite-AR-CT new raisin factor.R98
Chemical: Cryolite
R£D(Chronic): .114 mg/kg bw/day HOEL(Chronic): 0 mg/kg bw/day
RfD(Acute): 0 mg/kg bw/day NOEL(Acute): 0 mg/kg bw/day
Date created/last modified: 05-24-2004/10:05:08/8 Program ver. 2.03
EPA
Code
12000120
12000121
12000130
12000140
12000141
13010550
13010560
13010561
13020570
13020571
13010580
05010610
05010611
05010640
05010690
05020700
09Q1Q7SO
09010800
05010830
10001060
05021170
95001300
95001301
9S001310
95001320
9SQQ1321
090213SO
13021360
13021370
13011420
08001480
13021490
13021740
95001750
95001760
95001761
95001770
95001780
95001790
10001800
10001810
09011870
13021910
05021940
95001950
05011960
10001970
10001990
10002000
10002001
10002010
04012040
04012050
10002060
1.0002070
10002071
13012080
12002300
10002400
10002410
Crop
Grp
12
12
12
12
12
13A
13A
13A
13B
13B
13A
5A
5A
5A
5A
SB
9A
9A
5A
10
SB
0
0
O
O
O
9B
13B
13B
13A
8
13B
13B
O
O
0
O
0
0
10
10
9A
13B
SB
0
5A
10
10
10
10
10
4A
4A
10
10
10
13A
12
10
10
Commodity Name
Apricot
Apricot -babyfood
Apricot, dried
Apricot, juice
Apricot, juice -babyfood
Blackberry
Blackberry, juice
Blackberry, juice-babyfood
Blueberry
Blueberry- baby food
Boysenberry
Broccoli
Broccoli -baby food
Brussels sprouts
Cabbage
Cabbage, Chinese, bok choy
Cantaloupe
Casaba
Cauliflower
Citrus citron
Collards
Cranberry
Cranberry-babyfood
Cranberry, dried
Cranberry, juice
Cranberry, juice-babyfood
Cucumber
Currant
Currant, dried
Dewberry
Eggplant
Elderberry
Gooseberry
Grape
Grape, juice
Grape, juice-babyfood
Grape, leaves
Grape, raisin
Grape, wine and sherry
Grapefruit
Grapefruit, juice
Honey dew melon
Huckleberry
Kale
Kiwif ruit
Kohlrabi
Kumguat
Lemon
Lemon, juice
Lemon, juice-babyfood
Lemon, peel
Lettuce, head
Lettuce, leaf
Lime
Lime, juice
Lime, juice-babyfood
Loganberry
Nectarine
Orange
Orange, juice
Def Res
(ppm)
4 .
4 .
4 .
4 .
4 .
0.
0,
0.
0,
0.
0,
5 ,
5
4
1
4
2
2
3
8
4
0.
0
0
0
0
2
0
0
0
1
0
0
3
3
3
3
3
3
9
9
2
0
4
4
5
8
13
13
13
13
2
15
13
13
13
0
4
a
8
500000
500000
500000
.500000
.500000
250000
,250000
,250000
.110000
.110000
,250000
,000000
.000000
.000000
.500000
.000000
.160000
.160000
.000000
.000000
. 000000
. 500000
. 500000
.500000
.500000
.500000
.500000
.110000
.110000
.250000
.500000
.110000
.110000
.500000
.500000
.500000
.500000
.500000
.500000
.000000
.000000
.160000
.110000
.000000
.500000
.000000
.000000
.500000
. 500000
.500000
.500000
.500000
.000000
.500000
.500000
.500000
.250000
.500000
.000000
.000000
Ad j . Factors Comment
#1 1*2
1.
1.
6 .
1.
1.
1.
1.
1.
1,
1.
1.
1
1.
1
1
1
1.
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
0
0
1
1
0
1
0
1
1
1
1
1
1
1
0
0
0
1
1
1
0
0
1
1
1
0
000
000
000
000
,000
,000
,000
,000
,000
,000
,000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
. 000
,100
.100
.000
.000
.000
.000
.000
.000
.000
.000
.830
.830
.000
.350
.830
.000
.026
.000
.000
.000
.000
.000
.000
.000
.024
.024
.280
.000
.000
.000
.024
.024
.000
, 000
.000
.022
0.
0.
0.
0 .
0.
1.
1.
1.
1
I.
1.
0.
0.
0.
0 .
0.
0.
0 .
0.
0.
0 .
1.
1 .
1,
1,
1.
0.
1.
1,
1,
0.
1
1
0,
0.
0,
0
0 .
0 .
0,
0
0,
1,
0 ,
0,
0
0
0
0
0
0.
0
0
0
0
0.
1
0
0
0
010
010
010
010
010
000
000
000
000
000
000
020
020
020
010
010
010
010
020
040
020
000
000
000
000
000
,010
.000
,000
,000
.010
.000
,000
,330
.330
.330
.330
.330
,330
.040
.040
.010
.000
.020
.140
.020
.040
.020
.020
.020
.020
.010
.010
.040
.040
.040
.000
.010
.020
.020
Page 4 of 3 8
-------
10002411
10002420
12002600
12002601
12002610
12002611
12002620
12002621
08002700
08002701
08002710
08002711
08002720
08002721
08002730
95002750
950Q276Q
12002850
12002851
12002860
12002861
12002870
12002871
12002880
12002881
01032960
01032970
01032971
01032980
01032981
01032990
01032991
01033000
01033001
10003070
09023080
09023090
13013200
13013201
13013210
13013211
95003520
95003530
09023560
09023561
09023570
09023571
95003590
95003591
95003600
95003601
10003690
10003700
08003750
08003751
08003760
08003761
08003770
08003771
08003780
08003781
08003790
09013990
09014000
10
10
12
12
12
12
12
12
8
8
8
8
8
8
8
O
O
12
12
12
12
12
12
12
12
1C
1C
1C
1C
1C
1C
1C
1C
1C
10
9B
9B
13A
13A
13A
13A
O
O
9B
9B
9B
9B
0
O
0
0
10
10
8
8
8
8
8
8
8
8
8
9A
9A
Orange, juice -baby food
Orange , peel
Peach
Peach- babyfood
Peach, dried
Peach, dried- babyfood
Peach, juice
Peach, juice-babyfood
Pepper, bell
Pepper, bell -babyfood
Pepper, bell, dried
Pepper, bell, dried-babyf ood
Pepper, nonbell
Pepper, nonbell -baby food
Pepper, nonbell, dried
Peppermint
Peppermint, oil
Plum
PI urn -baby food
Plum, prune, fresh
Plum, prune, f resh-babyfood
Plum, prune, dried
Plum, prune, dried-bafoyfood
Plum, prune, juice
Plum, prune, juice-babyfood
Potato, chips
Potato, dry {granules/ flakes)
Potato, dry (granules/ flakes) -b
Potato, flour
Potato, flour-babyfood
Potato, tuber, w/peel
Potato, tuber, w/peel -babyfood
Potato, tuber, w/o peel
Potato, tuber, w/o peel-babyfood
Pummel o
Pumpkin
Pumpkin, seed
Raspberry
Raspberry -babyfood
Raspberry, juice
Raspberry, juice-babyfood
Spearmint
Spearmint, oil
Squash, summer
Squash, summer-babyfood
Squash, winter
Squash, winter -babyfood
Strawber*"y
Strawberry -babyfood
Strawberry, juice
Strawberry, juice-babyfood
Tangerine
Tangerine, juice
Tomato
Tomato-babyfood
Tomato, paste
Tomato, paste -babyfood
Tomato, puree
Tomato, puree -babyfood
Tomato, dried
Tomato, dried-babyfood
Tomato, juice
Watermelon
Watermelon, juice
8
8
4
4
4
4
4
4
3
3
3
3
3
3
3
19
19
0
0
0
2
2
2
2
2
0
0.
0
0
0.
0.
0.
0,
0,
9,
2.
2 .
0.
0.
0 .
0 .
19.
19.
2 .
2 .
2.
2,
1 .
1.
1 .
1.
8.
8.
1.
1.
1.
1.
1.
1.
1.
1 .
1.
2 .
2 .
.000000
.000000
.500000
.500000
.500000
.500000
.500000
.500000
.500000
.500000
.500000
.500000
.500000
.500000
.500000
.500000
.500000
.500000
.500000
.500000
.000000
. 000000
.000000
. 000000
.000000
.650000
.650000
.650000
.650000
.650000
.650000
.650000
.650000
.650000
,000000
.500000
500000
250000
250000
250000
250000
500000
500000
500000
500000
500000
SOOOOO
000000
000000
000000
000000
000000
000000
500000
500000
500000
500000
500000
500000
500000
500000
500000
160000
160000
0
0
1
1
7
7
1
1
1
1
1
1
1
1
1
1
0
1
1
1
1.
s.
5.
1.
1.
1.
6.
6.
6.
6.
1.
1,
1 .
1,
1 .
1 .
1 .
1 .
1.
1.
1.
1.
0 .
I.
1 .
1.
1.
1.
1.
1 .
1.
1.
0.
1.
1 .
1.
1.
1.
1.
14.
14.
1.
1.
1.
.022
.280
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.026
.000
.000
.000
,000
.000
,000
,400
.400
,000
,500
,500
500
,500
000
000
000
000
000
000
000
000
000
000
000
000
026
000
000
000
000
000
000
000
000
000
028
000
000
500
500
000
000
300
300
500
000
000
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
1
1
0
0
0
0
0
0.
0,
0.
0,
0.
0,
0.
0.
0.
0.
0.
0.
0.
0.
0.
1.
1.
1.
1.
1.
1.
0 .
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
0.
.020
.020
.010
.010
.010
.010
.010
.010
.010
.010
.010
.010
.010
.010
.010
.000
.000
.010
.010
.010
.010
.010
.010
.010
.010
.030
.030
,030
,030
.030
,030
,030
,030
.030
.040
010
010
000
000
000
000
000
000
010
010
010
010
020
020
020
020
040
040
010
010
010
010
010
010
010
010
010
010
010
Page 5 of 38
-------
Attachment 2. Inputs for sulfuryl fluoride food fumigation exposure estimates
U.S. Environmental Protection Agency Ver. 2.00
DEEM-FCID Chronic analysis for FLUORIDE . 1934-98 data
Residue file: C:\Documents and Settings\mdoherty\My Docuraents\Chemistry ReviewsX!DEEM
Runs\Sul£uryl Fluoride\F Food Fumigation - 2009 RevisedCT - 4-28 Strict Label.R98
Adjust. #2 used
Analysis Date 05-06-2009 Residue file dated: 05-06-2009/13:54:06/8
Reference dose (RfD) = 0.114 mg/kg bw/day
Food Crop
EPA Code Grp
14000030
14000031
11000090
11000091
12000130
95000240
95000241
15000250
15000251
15000260
15000261
15000270
19010290
19010291
OS030300
OS030320
06030340
06030350
06030360
06030380
06030390
06030400
06030410
06030420
14000590
14000680
14000810
14000920
06030980
06030981
06030990
19011030
19021050
19021051
95001090
95001100
95001110
95001111
95001120
95001130
95001150
95001160
19011180
19011181
19021190
19021191
15001200
15001201
15001210
15001211
15001220
15001230
15001231
15001240
15001241
15001250
95001310
14
14
11
11
12
O
0
15
15
15
15
15
19A
19A
SC
6C
6C
6C
6C
6C
6C
6C
SC
SC
14
14
14
14
6C
6C
6C
19A
19B
19B
0
O
0
0
0
0
0
O
19A
19A
19B
19B
15
15
15
15
15
15
15
15
15
15
0
Food Name
Almond
Almond- babyfood
Apple, dried
Apple, dried-babyfood
Apricot, dried
Banana, dried
Banana, dried-babyfood
Barley, pearled barley
Barley, pearled barley-babyf ood
Barley, flour
Barley, flour-babyfood
Barley, bran
Basil, dried leaves
Basil, dried leaves-babyf ood
Bean, black, seed
Bean, broad, seed
Bean, cowpea, seed
Bean, great northern, seed
Bean, kidney, seed
Bean, lima, seed
Bean, mung, seed
Bean, navy, seed
Bean, pink, seed
Bean, pinto, seed
Brazil nut
Butternut
Cashew
Chestnut
Chickpea, seed
Chickpea, seed-babyf ood
Chickpea, flour
Chive
Cinnamon
Ci nnaraon - babyfood
Cocoa bean, chocolate
Cocoa bean, powder
Coconut , meat
Coconut- meat -baby food
Coconut, dried
Coconut, milk
Coffee, roasted bean
Coffee, instant
Coriander, leaves
Coriander, leaves -babyfood
Coriander, seed
Coriander, seed-babyf ood
Corn, field, flour
Corn, field, flour-babyfood
Corn, field, meal
Corn, field, meal -babyfood
Corn, field, bran
Corn, field, starch
Corn, field, starch-babyf ood
Corn, field, syrup
Corn, field, syrup -baby food
Corn, pop
Cranberry, dried
Residue
(ppm>
9.
9 .
1.
1,
1.
1 ,
1 .
3.
3
3
3
3.
67
67
4
4
4
4
4
4
4
4
4
4
5
5.
5
5
4
4
4
63
73
73
8
8
49
49
49
49
7
13
63
63
7
7
16
16
2
2
2
0
0
0
0
1
1
700000
700000
.000000
,000000
.000000
.000000
.000000
.700000
.700000
.700000
.700000
.700000
.100000
. 100000
.500000
.500000
.500000
.500000
. 500000
. 500000
.500000
. 500000
.500000
.500000
. 300000
.300000
. 300000
. 300000
.500000
.500000
.500000
.500000
.500000
.500000
.400000
.400000
.100000
.100000
.100000
.100000
.100000
.900000
.500000
.500000
.100000
. 100000
.900000
.900000
.800000
.800000
.800000
.600000
.600000
.600000
.600000
.700000
.000000
Adj . Factors Comment
#1 #2
1.
1 ,
1.
1,
1,
1 ,
1.
1
1.
0
0
2
1
1
j_
1
1
1
1.
T_
1
1 .
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
000
.000
.000
,000
,000
.000
.000
.000
.000
.730
.730
.560
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
. 000
. 000
. 000
.000
.000
. 000
. 000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
0.
0.
0,
0.
0.
0.
0.
0,
0,
0.
0.
0,
0
0,
1.
1
1
1
1
1
1
1
1
1
0
0
0
0
1
1
1
0
0
0
1
1
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
,100
,100
690
,690
,690
.690
.690
.001
.001
.001
.001
.001
.001
.001
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.100
.100
. 100
. 100
.000
.000
.000
.001
.001
.001
.000
.000
.001
.001
.001
.001
.001
.001
.001
.001
.001
.001
.001
.001
.001
.001
.001
.001
.001
.001
.001
.001
.100
Page 6 of 38
-------
13021370 13B Currant, dried 1.000000 1,000
95001410 O Date
130-Uncooked; Dried; Cook Meth N/S
0.900000 1.000
210-Cooked; Fresh or N/S; Cook Meth N/S
211-Cooked; Fresh or N/S; Baked
0
0
.000000
.000000
1
1
.000
.000
212-Cooked; Fresh or N/S; Boiled
0
.000000
1
.000
230 -Cooked; Dried; Cook Meth N/S
19021430
19011440
95001540
14001550
030016SO
01031660
01031661
01031670
95001780
06031820
06031821
19011840
19011841
14001850
19012020
06032030
95002120
14002130
95002160
19012200
19012201
15002260
15002310
15002320
1S002321
1S002330
15002331
95002460
19012490
19012491
06032560
06032561
06032580
12002610
12002611
95002630
95002640
11002670
14002690
19022740
19022741
95002780
95002800
14002820
95002840
12002870
12002871
15003230
15003231
15003240
15003241
15003250
150032S1
15003260
15003261
19013340
15003440
19023540
19023541
15003810
1S003811
01033870
19B
19A
0
14
3
1CD
1CD
1CD
O
6C
6C
19A
19A
14
19A
6C
O
14
O
19A
19A
15
15
15
15
15
IS
O
19A
19A
6C
6C
6C
12
12
O
O
11
14
19B
19B
O
0
14
O
12
12
15
IS
15
15
IS
15
15
IS
19A
15
19B
19B
15
15
1CD
Dill, seed
Dillweed
Fig, dried
Filbert
Garlic, dried
Ginger
Ginger - babyf ood
Ginger, dried
Grape, raisin
Guar, seed
Guar, seed-babyfood
Herbs, other
Herbs, other -babyf ood
Hickory nut
Lemongrass
Lentil, seed
Lychee, dried
Macadamia nut
Mango, dried
Marjoram
Mar j oram- babyf ood
Millet, grain
Oat , bran
Oat, flour
Oat, f lour-babyf ood
Oat, groats/rolled oats
Oat, groats/rolled oats -baby food
Papaya, dried
Parsley, dried leaves
Parsley, dried leaves-babyf ood
Pea, dry
Pea, dry-baby food
Pea, pigeon, seed
Peach, dried
Peach, dried-babyf ood
Peanut
Peanut, butter
Pear, dried
Pecan
Pepper, black and white
Pepper, black and white -babyf ood
Pine nut
Pineapple, dried
Pistachio
Plantain, dried
Plum, prune, dried
Plum, prune, dried-babyf ood
Rice, white
Rice, white -babyf ood
Rice, brown
Rice, brown-babyfood
Rice, flour
Rice, flour -babyf ood
Rice, bran
Rice, bran-babyf ood
Savory
Sorghum, grain
Spices, other
Spices, other-babyfood
Triticale, flour
Triticale, f lour-babyf ood
Turmeric
0
1
63
1.
2
10
10
10
10
1.
4
4
63
63
5
63
4
1
5
1,
67,
67.
2.
18.
18.
18,
18.
18.
1.
63 .
63 .
4 .
4 .
4 .
1.
1 ,
16.
16.
1 .
5 .
7 .
7 .
8 .
1.
3 .
1.
0.
0.
4 .
4.
12.
12.
32.
32.
37.
37.
63 .
20.
7 .
7 .
2.
2.
7.
.900000
.100000
.500000
.000000
.500000
.900000
. 900000
. 900000
. 900000
.000000
.500000
. 500000
.500000
.500000
.300000
. SOOOOO
.500000
.000000
.300000
.000000
.100000
.100000
.900000
.500000
.500000
.500000
.500000
.SOOOOO
.000000
,500000
500000
500000
.500000
500000
.000000
,000000
400000
400000
000000
300000
100000
100000
800000
000000
200000
000000
700000
700000
500000
500000
500000
500000
500000
SOOOOO
500000
500000
500000
400000
100000
100000
900000
900000
100000
1
1
1
1
1
J.
1
1
1
J.
1
1
X
i
1
1
1
1
1
1
1.
1.
1
2.
0 .
0
1,
1.
1.
1,
1,
1,
1.
1.
1.
1.
1.
1.
1 ,
1.
1.
1.
1 .
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1,
1.
1.
1.
1.
1.
0.
0.
1.
.000
.000
.000
. 000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.560
,730
.730
.000
.000
.000
.000
.000
,000
,000
.000
.000
,000
,000
,000
,000
,000
.000
.000
000
.000
000
000
.000
.000
000
000
.000
.000
000
000
000
000
000
000
000
000
380
380
000
0.100
0.420
0.000
0.000
0.000
0.420
0.001
0.001
0.690
0.100
0.001
0.001
0 .001
0.001
0.690
1. 000
1.000
0.001
0.001
0. 100
0.001
1.000
0.690
0 .001
0 .690
0 .001
0 .001
0 .001
0 .001
0.001
0.001
0.001
0.001
0.690
0.001
0.001
1.000
1. 000
1.000
0.690
0.690
0.006
0.006
0.690
0.100
0 .001
0 .001
0.100
0 .690
0 .270
O.S90
0 .690
0 .690
0.030
0.030
0.030
0.030
0.030
0.030
0.030
030
001
001
001
001
0.001
0.001
0.001
Page 7 of 38
-------
14003910 14 Walnut
15004010 15
15004011 15
15004020 15
15004021 15
15004030 15
Wheat,
wheat ,
Wheat ,
wheat ,
Wheat,
grain
grain-babyfood
flour
flour-babyfood
germ
15004040 IS Wheat, bran
15004050 IS Wild rice
2.400000
2.900.000
2.900000
31.400000
31.400000'
13,900000
74,200000
12.500000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
0.990
0.004
0.004
0.001
0.001
0.001
0.001
0.030
Page 8 of38
-------
Attachment 3. Inputs for sulfuryl fluoride structural fumigation exposure estimates
U.S. Environmental Protection Agency Ver. 2.00
DEEM-FCID Chronic analysis for FLUORIDE 1994-98 data
Residue file: C:\Documents and Settings\!rsdoherty\My Documents\Cheinistry Reviews\ IDEEM
Runs\Sulfuryl Fluoride\F Space Fumigation - 2009 - S-1.R98
Adjust. $2 used
Analysis Date 05-06-2009 Residue file dated: 05-06-2009/13:52:45/8
Reference dose (RfD) = 0.114 mg/kg bw/day
Food Crop
EPA Code Grp Food Name
18000020
14000030
14000031
14000040
14000041
95000060
11000090
11000091
12000130
01030150
01030151
9S000240
95000241
15000250
15000251
1S000260
15000261
15000270
19010280
19010281
19010290
19010291
OS030300
OS030320
06030340
06030350
06030360
OS030380
06030390
06030400
06030410
06030420
21000450
01010530
01010531
14000590
15000650
1S000660
14000680
14000810
14000920
06030980
06030981
06030990
01011000
19011030
04011040
19021050
19021051
95001090
95001100
95001110
95001111
9S001120
95001130
95001140
95001141
18
14
14
14
14
0
11
11
12
1CD
1CD
0
o
15
15
15
15
IS
19A
19A
19A
19A
6C
6C
6C
6C
6C
6C
6C
SC
6C
6C
M
1A
1A
14
IS
15
14
14
14
6C
6C
6C
1AB
19A
4A
198
19B
0
0
0
0
0
0
0
O
Alfalfa, seed
Almond
Almond- baby food
Almond, oil
Almond, oil-babyfood
Amaranth, grain
Apple, dried
Apple, dried-babyfood
Apricot, dried
Arrowroot, flour
Arrowroot, f lour-babyfood
Banana, dried
Banana, dried-babyfood
Barley, pearled barley
Barley, pearled barley-babyfood
Barley, flour
Barley, f lour-babyfood
Barley, bran
Basil, fresh leaves
Basil, fresh leaves -baby food
Basil, dried leaves
Basil, dried leaves-babyf ood
Bean, black, seed
Bean, broad, seed
Bean, cowpea, seed
Bean, great northern, seed
Bean, kidney, seed
Bean, lima, seed
Bean, mung, seed
Bean, navy, seed
Bean, pink, seed
Bean, pinto, seed
Beef, meat, dried
Beet, sugar, molasses
Beet, sugar, molasses -babyf ood
Brazil nut
Buckwheat
Buckwheat, flour
Butternut
Cashew
Chestnut
Chickpea, seed
Chickpea, seed-babyf ood
Chickpea, flour
Chicory, roots
Chive
Chrysanthemum, garland
Cinnamon
Cinnamon-baby food
Cocoa bean, chocolate
Cocoa bean, powder
Coconut , meat
Coconut- raeat-taabyfood
Coconut, dried
Coconut, milk
Coconut, oil
Coconut, oil-babyfood
Residue
(ppm)
20
9
9
1
1
20
1
1
1
31
31
1
1
3
3
0
0.
3
67
67
67
67
4
4
4
4
4
4
4
4
4
4
58
1.
1
3 ,
2.
0.
3,
3 .
3 ,
4 ,
4 .
4 ,
13 .
63 .
63.
73.
73 .
8,
8.
49.
49.
49,
49.
1.
1.
.400000
.200000
.200000
.500000
.500000
.400000
.000000
.000000
.000000
.400000
.400000
.000000
.000000
.650000
.650000
.156000
.156.000
.650000
. 100000
.100000
. 100000
. 100000
.500000
. 500000
.500000
.500000
. 500000
.500000
.500000
.500000
.500000
.500000
,400000
.200000
.200000
. 900000
, 900000
.134000
.900000
.900000
.900000
.500000
.500000
.500000
.900000
.500000
.500000
,500000
,500000
.400000
,400000
,100000
.100000
,100000
,100000
,500000
500000
Adj . Factors Comment
#1 #2
1
1
1
1
1
1
1
1
1
1
1 .
1
1 .
1,
1,
1,
1 ,
1 .
j_
1,
1 ,
1.
X -
1.
X
1 .
]_ 4
1 .
1. ,
1.
1 .
1.
1.
1 .
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
,000
.000
.000
,000
.000
.000
.000
.000
,000
,000
,000
,000
,000
,000
,000
,000
,000
,000
,000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
000
0
0
0
0
0
0
0
0
0
0
0
0.
0,
0,
0,
1
1
0
0.
0.
0
0,
0
0,
0
0,
0.
0.
0.
0.
0 ,
0 .
0 .
0 .
0 ,
0 .
0 ,
1 .
0 .
0 ,
0 ,
0.
0,
0.
0.
0,
0.
0.
0.
0,
0,
0.
0.
0.
0.
0.
0.
.004
.004
. 004
.004
.004
.004
.004
.004
.004
.004
.004
.004
.004
.008
.008
.000
.000
,008
.004
.004
.004
.004
.004
.004
.004
.004
.004
.004
.004
. 004
,004
.004
,004
.004
.004
.004
,008
,000
,004
,004
,004
,004
,004
.004
,004
,004
004
,004
,004
004
,004
,004
,004
004
004
004
004
Page 9 of38
-------
95001150
95001160
19011180
19011181
19021190
19021191
15001200
15001201
15001210
15001211
15001220
15001230
15001231
15001240
15001241
15001250
15001251
15001260
95001280
95001281
95001310
13021370
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15
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Coffee, roasted bean
Coffee, instant
Coriander, leaves
Coriander, leaves -baby food
Coriander, seed
Coriander,
Corn, field
Corn, field
Corn, field
Corn, field
Corn, field
Corn, field
Corn, field
Corn, field
Corn, field
Corn, field
Corn, field
Corn, pop
Cottonseed,
Cottonseed,
Cranberry,
seed-babyfood
, flour
, f lour -babyfood
, meal
, meal -babyfood
, bran
, starch
, starch-babyf ood
, syrup
, syrup -baby food
, oil
, oil -babyfood
oil
oil -babyfood
dried
Currant, dried
Date
Dill, seed
Dillweed
Egg, whole
110 -Uncooked; Fresh or N/S;
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Cook Meth N/S
0.000000
120-Uncooked; Frozen; Cook Meth N/S
0.000000
210-Cooked; Fresh or N/S; Cook Meth N/S
0.000000
211-Cooked; Fresh or N/S; Baked 0.000000
212-Cooked; Fresh or N/S; Boiled
0.000000
213-Cooked; Fresh or N/S; Fried 0.000000
214-Cooked; Fresh or N/S; Fried/baked
0.000000
215-Cooked; Fresh or N/S; Boiled/baked
0.000000
221-Cooked; Frozen; Baked 0,000000
223-Cooked; Frozen; Pried 0.000000
224-Cooked; Frozen; Fried/baked 0,000000
230-Cooked; Dried; Cook Meth N/S
402.500000
232-Cooked; Dried; Boiled 402,500000
233-Cooked; Dried; Fried 402,500000
240-Cooked; Canned; Cook Meth N/S
0.000000
Canned; Boiled
Cured etc; Boiled
Cured etc; Fried
0.000000
0 .000000
0 .000000
242-Cooked
252-Cooked
253-Cooked
70001460 P Egg, white
110-Uncooked; Fresh or N/S; Cook Meth N/S
0 .000000
120-Uncooked; Frozen; Cook Meth N/S
0 .000000
130-Uncooked; Dried; Cook Meth N/S
402 .500000
210-Cooked; Fresh or N/S; Cook Meth N/S
0.000000
211-Cooked; Fresh or N/S; Baked 0.000000
212-Cooked; Fresh or N/S; Boiled
0.000000
213-Cooked; Fresh or N/S; Fried 0.000000
214-Cooked; Fresh or N/S; Fried/baked
0.000000
0,000000
0.000000
221-Cooked;
223-Cooked.r
230-Cooked;
232-Cooked;
Frozen,- Baked
Frozen; Fried
Dried; Cook Meth N/S
402.500000
Dried; Boiled 402,500000
233-Cooked; Dried; Fried
402.500000
1. 000
1. 000
1.000
1.000
1.000
1.000
1.000
1.000
1. 000
1. 000
1.000
1.000
1.000
1.000
1.000
1.000
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1.000
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1 .000
1.000
1.000
1.000
1.000
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0.004
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0.004
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0.004
0.004
0,004
Page 10 of 38
-------
70001461
95001540
14001550
14001560
20001630
03001650
03001651
01031670
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95001780
06031820
06031821
19011840
19011841
14001850
19012020
06032030
95002120
14002130
95002160
95002180
95002190
19012200
19012201
27002220
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0
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240-Cooked; Canned; Cook Meth N/S
0.000000
242-Cooked; Canned; Boiled 0.000000
250-Cooked; Cured etc; Cook Meth N/S
0.000000
Egg, white (solids) -babyfood 402.500000
Fig, dried 1.000000
Filbert 1.500000
Filbert, oil 1.500000
Flaxseed, oil 1.500000
Garlic, dried 10.900000
Garlic, dried-babyfood 10.900000
Ginger, dried 10.900000
Ginseng, dried 10.900000
Grape, raisin 1.000000
Guar, seed 4.500000
Guar, seed-babyfood 4.500000
Herbs, other 63.500000
Herbs, other-babyfood 63.500000
Hickory nut 3.900000
Lemongrass 63.500000
Lentil, seed 4.SOOOOO
Lychee, dried 1.000000
Macadamia nut 3.900000
Mango, dried 1.000000
Maple, sugar 1.200000
Maple syrup 1.200000
Marjoram 7.100000
Mar jorara- baby food 67.100000
Milk, fat
110 -Uncooked; Fresh or N/S; Cook Meth N/S
0.000000
120 -Uncooked; Frozen; Cook Meth N/S
0.000000
130 -Uncooked; Dried; Cook Meth N/S
S .400000
150 -Uncooked; Cured etc; Cook Meth N/S
3.900000
210-Cooked; Fresh or N/S; Cook Meth N/S
0.000000
211-Cooked; Fresh or N/S; Baked 0.000000
212-Cooked; Fresh or N/S; Boiled
0.000000
213 -Cooked; Fresh or N/S; Fried 0.000000
2 14 -Cooked; Fresh or N/S; Fried/baked
0.000000
2 15 -Cooked; Fresh or N/S; Boiled/baked
0.000000
220 -Cooked; Frozen; Cook Meth N/S
0.000000
221 -Cooked; Frozen; Baked 0.000000
222-Cooked; Frozen; Boiled 0.000000
223-Cooked; Frozen; Fried 0.000000
224-Cooked; Frozen; Fried/baked 0.000000
230-Cooked; Dried; Cook Meth N/S
5.400000
231-Cooked; Dried; Baked 5.400000
232-Cooked; Dried; Boiled 5.400000
233-Cooked; Dried; Fried 5.400000
240-Cooked; Canned; Cook Meth N/S
0. 000000
242-Cooked; Canned; Boiled 0.000000
250-Cooked; Cured etc; Cook Meth N/S
3.900000
253 -Cooked; Cured etc; Fried 3.900000
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3.900000 1.000 0.004
27012230 D Milk, nonfat solids
110-Uncooked; Fresh or N/S; Cook Meth N/S
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120-Uncooked; Frozen; Cook Meth N/S
0.000000 1.000 0.004
130-Uncooked; Dried; Cook Meth N/S
Page 11 of38
-------
27012231 D
27022240 D
5.400000
150 -Uncooked; Cured etc; Cook Meth N/S
3 ,900000
210-Cooked; Fresh or N/S; Cook Meth N/S
0.000000
211-Cooked; Fresh or N/S; Baked 0.000000
212-Cooked; Fresh or N/S; Boiled
0.000000
2 13 -Cooked; Fresh or N/S; Fried 0.000000
214-Cooked; Fresh or N/S; Fried/baked
0 .000000
215-Cooked; Fresh or N/S; Boiled/baked
0 .000000
220 -Cooked; Frozen; Cook Meth N/S
0.000000
221 -Cooked; Frozen; Baked 0.000000
222-Cooked; Frozen; Boiled 0.000000
223-Cooked; Frozen; Fried 0.000000
224 -Cooked; Frozen; Fried/baked 0.000000
230-Cooked; Dried; Cook Meth N/S
5.400000
231-Cooked; Dried; Baked 5.400000
232-Cooked; Dried; Boiled S. 400000
233-Cooked; Dried; Fried 5.400000
240 -Cooked; Canned; Cook Meth N/S
0.000000
242 -Cooked; Canned; Boiled 0.000000
24 5 -Cooked; Canned; Boiled/baked
0 .000000
250-Cooked; Cured etc,- Cook Meth N/S
3 .900000
253 -Cooked; Cured etc; Fried 3.900000
255-Cooked; Cured etc; Boiled/baked
3 . 900000
Milk, nonfat solids-baby food/ infant
110 -Uncooked; Fresh or N/S;. Cook Meth N/S
0 .000000
130 -Uncooked; Dried; Cook Meth N/S
5 .400000
211-Cooked; Fresh or N/S; Baked 0.000000
240-Cooked; Canned; Cook Meth N/S
0. 000000
Milk, water
110-Uncooked; Fresh or N/S; Cook Meth N/S
0. 000000
120 -Uncooked; Frozen; Cook Meth N/S
0. 000000
130-Uncooked; Dried; Cook Meth N/S
5.400000
150-Uncooked; Cured etc; Cook Meth N/S
3.900000
210-Cooked; Fresh or N/S; Cook Meth N/S
0,000000
211-Cooked; Fresh or N/S; Baked 0.000000
212-Cooked; Fresh or N/S; Boiled
0.000000
213-Cooked; Fresh or N/S; Fried 0.000000
214-Cooked; Fresh or N/S; Fried/baked
0,000000
215-Cooked; Fresh or N/S; Boiled/baked
0,000000
220 -Cooked; Frozen; Cook Keth N/S
0.000000
221 -Cooked; Frozen; Baked 0.000000
222-Cooked; Frozen; Boiled 0,000000
223-Cooked; Frozen; Fried 0.000000
224-Cooked; Frozen,- Fried/baked o. 000000
230-Cooked; Dried; Cook Meth N/S
S. 400000
231-Cooked; Dried; Baked S. 400000
232-Cooked; Dried; Boiled 5.400000
233 -Cooked; Dried; Fried 5.400000
240-Cooked; Canned; Cook Meth N/S
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Page 12 of 38
-------
210-cooked,-
212-Cooked;;
230-Cooked;r
240-Cooked;
242-Cooked; Canned; Boiled
2SO-Cooked; Cured etc; Cook Meth N/S
253-Cooked; Cured etc; Fried
255-Cooked; Cured etc; Boiled/baked
3
27032251 D Milk, sugar (lactose)-baby food/infa
110-Uncooked; Fresh or N/S; Cook Meth N/S
0
130-Uncooked; Dried; Cook Meth N/S
Fresh or N/S; Cook MI
Fresh or N/S; Boiled
Dried; Cook Meth N/S
Canned; Cook Meth N/S
15 Millet, grain
15 Oat, bran
15 Oat, flour
15 Oat, flour-babyfood
15 Oat, groats/rolled oats
15 Oat, groats/rolled oats-babyfood
O Olive, oil
3 Onion, dry bulb, dried
3 Onion, dry bulb, dried-babyfood
O Palm, oil
O Palm, oil-babyfood
0 Papaya, dried
19A Parsley, dried leaves
19A Parsley, dried leaves-babyfood
6C Pea, dry
6C Pea, dry-babyfood
6C Pea, pigeon, seed
12 Peach, dried
12 Peach, dried-babyfood
O Peanut
O Peanut, butter
O Peanut, oil
11 Pear, dried
14 Pecan
8 Pepper, bell, dried
8 Pepper, bell, dried-babyfood
8 Pepper, nonbell, dried
19B Pepper, black and white
19B Pepper", black and white-baby food
0 Peppermint, oil
O Pine nut
O Pineapple, dried
14 Pistachio
0 Plantain, dried
12 Plum, prune, dried
12 Plurn, prune, dried-babyfood
1C Potato, chips
1C Potato, dry (granules/ flakes)
1C Potato, dry (granules/ flakes)-b
1C Potato, flour
1C Potato, flour-babyfood
0 Psylliura, seed
9B Pumpkin, seed
O Quirioa, grain
20 Rapeseed, oil
20 Rapeseed, oil-babyfood
15 Rice, white
15 Rice, white-babyfood
15 Rice, brown
15 Rice, brown-babyfood
15 Rice, flour
15 Rice, flour-babyfood
15
15002260
15002310
15002320
15002321
15002330
15002331
95002360
03002380
03002381
95002440
95002441
95002460
19012490
19012491
06032S60
06032561
06032580
12002510
12002611
9S002630
95002640
95002650
11002670
14002690
08002710
08002711
08002730
19022740
19022741
95002760
9S002780
95002800
14002820
95002840
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12002871
01032960
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01032981
95003060
09023090
95003110
20003190
20003191
15003230
15003231
15003240
15003241
15003250
15003251
15003260
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0
0
.000000
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1.000
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3
3
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16
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36
36
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25
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.000000
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.700000
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.160000
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1.000
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1.000
1.000
1.000
1.000
1.000
1 .000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
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1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
1.000
0.004
0.004
0.004
0.004
0.004
0.004
0.004
0.004
0.004
0.004
0.004
0 .008
0 .008
1.000
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0 .008
0 .008
0 .004
0 .004
0.004
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0.004
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Page 13 of38
-------
15003261
15003280
15003290
20003300
20003301
19013340
9S003360
9S003361
95003370
95003371
1S003440
15003450
06003480
06003481
06003490
06003491
06003500
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19023541
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95003630
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15004050
15
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20
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0
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0
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15
6
6
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20
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Rice, bran-babyfood
Rye, grain
Rye, flour
Safflower, oil
Saf flower, oil-babyfood
Savory
Sesame, seed
Sesame, seed-babyfood
Sesame, oil
Sesame, oil-babyfood
Sorghum, grain
Sorghum , syrup
Soybean, flour
Soybean, f lour-babyf ood
Soybean, soy milk
Soybean, soy mi Ik -baby food or in
Soybean, oil
Soybean, oil-babyfood
Spearmint, oil
Spices, other
Spices, other-baby£ood
Sugarcane, sugar
Sugarcane, sugar -babyf ood
Sugarcane, molasses
Sugarcane, molasses -babyf ood
Sunflower, seed
Sunflower, oil
Sunflower, oil-babyfood
Tea, dried
Tea, instant
Tomato, dried
Tomato, dried-babyfood
Triticale, flour
Triticale, f lour-babyfood
Turmeric
Walnut
Wheat , grain
Wheat, grain-babyf ood
Wheat, flour
Wheat, f lour-babyf ood
Wheat, germ
wheat , bran
wild rice
37.
2.
0 .
1.
i.
63.
7.
7.
1.
1.
20,
0.
0.
0.
2,
2.
1 ,
1,
1.
7 .
7.
1
1
1
1
4
1
1
67
67
1
1
0
0.
7
2
2
2
0
0
54
74
9
500000
900000
134000
500000
500000
500000
100000
100000
500000
,500000
.400000
.600000
.081000
.081000
.400000
.400000
.500000
,500000
.500000
.100000
.100000
.200000
.200000
.200000
.200000
. 500000
. 500000
.500000
. 100000
. 100000
.000000
. 000000
.134000
.134000
.100000
.000000
.900000
.900000
,134000
,134000
.000000
.200000
.400000
1 .
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1.
1,
1.
1.
1 .
1.
1 .
1
1
1
1
1
1
1
1
1.
1
1
1
1
1
1
1
1
1
1
000
000
000
000
000
,000
000
000
000
000
,000
,000
,000
,000
,000
,000
,000
.000
.000
.000
.000
,000
.000
.000
.000
.000
.000
.000
.000
.000
. 000
. 000
. 000
.000
.000
.000
.000
.000
.000
.000
.000
.000
.000
0.
0.
1.
0.
0.
0.
0.
0.
0.
0.
0.
0.
1.
1.
0.
0.
0.
0.
0.
0.
0.
0.
0
0.
0,
0.
0
0.
0
0
0
0
1
1
0
0
0
0
1
1
0.
0
0
008
008
000
004
004
004
004
004
,004
004
008
,008
,000
.000
,004
,004
,004
.004
.004
.004
, 004
.004
.004
.004
.004
.004
.004
.004
.004
.004
.004
.004
.000
.000
.004
.004
.008
.008
.000
.000
.008
.008
.008
Page 14 of38
-------
Attachment 4. Results of cryolite fluoride exposure analysis
U.S. Environmental Protection Agency Ver. 2.02
DEEM-FC1D ACUTE Analysis for CRYOLITE (1994-98 data)
Residue file: Cryolite-AR-CT new raisin factor.R98
Adjustment factor #2 used.
Analysis Date: 06-03-2010/13:01:11 Residue file dated: 05-24-2004/10:05:08/8
No body weight adjustment; Toxicology endpoiixts not used
Daily totals for food and foodform consumption used.
Run Comment: ""
Summary calculations (per capita):
95th Percentile
Exposure
All infants:
0.048374
Custom demographics 1: 0.5 - <1:
0.175850
Custom demographics 2: 1 - <4:
0.202992
Custom demographics 3: 4 - <~i
0.1S9838
Custom demographics 4:7- <11:
0.126163
Custom demographics 5: 11 - <14:
0.11.3618
Custom demographics 6: 14+:
0.179623
99th Percentile
Exposure
0.1801S3
0.367189
0.443950
0.313532
0.332575
0.324475
0.425648
99.9th Percentile
Exposure
0.437825
0.703934
0.921210
0.737197
0.741806
0.733375
0.861668
Page 15 of 38
-------
U.S. Environmental Protection Agency Ver. 2,02
DEEM-FCID ACOTE Analysis for CRYOLITE ' (1994-98 data)
Residue file: Cryolite-AR-CT new raisin factor.R98
Adjustment factor #2 used.
Analysis Date: 06-03-2010/13:01:11 Residue file dated: 05-24-2004/10:05:08/8
Mo body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: ""
All infants
Daily Exposure Analysis /a
(rag/day)
per Capita per User
Mean 0.008410 0.016502
Standard Deviation 0.035543 0.048427
Standard Error of mean 0.000652 0.001252
Percent of Person-Days that are User-Days = 50.9"?%
Estimated percentile of user-days falling below calculated exposure
in rag/day
Percentile
Exposure
10
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0
0
0
0
0
0
0
0
.000113
.000331
.000635
.001133
.001882
.002814
.004828
.009149
Percentile Exposure
90.00
95. 00
97.50
99.00
99.50
99. 7S
99.90
0.047259
0. 102587
0. 126726
0.243049
0.2S9194
0.366479
0.481071
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile
Exposure
Percentile
Exposure
10 .
20 .
30 .
40.
50.
60.
70.
80
.00
.00
.00
,00
.00
. 00
, 00
.00
0.
0 .
0,
0,
0.
0.
0.
0
.000000
.000000
.000000
.000000
.000021
.000370
.001204
.002981
90,
95
97
99
99
99
99
.00
.00
.SO
.00
.50
.75
.90
0 ,
0,
0,
0
0.
0
0
.009432
.048374
.104997
.180153
.243227
.289300
.437825
a/ Analysis based on all two-day participant records in CSFII 1994-98 survey.
1
Page 16 of38
-------
U.S. Environmental Protection Agency Ver, 2.02
D1EM-FCID ACUTE Analysis for CRYOLITE (1994-98 data)
Residue file: Cryolite-AR-CT new raisin factor.R98
Adjustment factor #2 used.
Analysis Date: 06-03-2010/13:01:11- Residue file dated: 05-24-2004/10:05:08/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: ""
Custom demographics 1: O.S -
-------
U.S. Environmental Protection Agency Ver. 2,02
DEEM-FCID ACUTE Analysis for CRYOLITE .(1994-98 data)
Residue file: Cryolite-AR-CT new raisin factor.R98
Adjustment factor #2 used.
Analysis Date: 06-03-2010/13:01:11 Residue file dated: 06-24-2004/10:05:08/8
Ho body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: ""
Custom demographics 2 : 1 - <4
All Seasons
All Regions
Sex: M/F-all/
All Races
Nursing and Non-Nursing (Ages <= 3)
Age-Low: 1 yrs High: 4 yrs
Daily Exposure Analysis
(rag/day)
per Capita per User
Mean 0.040443 0.041017
Standard Deviation 0.090977 0.091492
Standard Error of mean 0.000857 0.000867
Percent of Person-Days that are User-Days = 98.60%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile Exposure
Percentile Exposure
10
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0
0
0
0
0
0
0
0
.000553
.001268
.002092
.003407
.006150
.012014
.023498
.050975
90,00
95.00
97.50
99.00
99 .50
99.75
99.90
0,121346
0.205310
0.287423
0,445745
0 .527179
0.634370
0.924251
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
Percentile Exposure
10,
20
30.
40.
50.
60.
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0
0.
0,
0.
0.
0.
0.
0
.000463
,001185
.001996
.003255
.005910
.011640
.023114
.050184
90 .00
95 .00
97.50
99.00
99.50
99.75
99.90
0. 1.20416
0 .202992
0 .284998
0 .443950
0.523800
0.632941
0.921210
Page 18 of 38
-------
U.S. Environmental Protection Agency Ver, 2.02
DEEM-FCID ACUTE Analysis for CRYOLITE {1994-98 data)
Residue file: Cryolite-AR-CT new raisin factor,R98
Adjustment factor #2 used,
Analysis Date: 06-03-2010/13:01:11 Residue file dated: 06-24-2004/10:05:08/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: ""
Custom demographics 3: 4
All Seasons
All Regions
Sex: M/F-all/
All Races
Age-Low: 4 yrs High: 7 yrs
Mean
Standard Deviation
Standard Error of mean
Daily Exposure Analysis
(rug/day)
per Capita per Dser
0.031330 0.031550
0.070270 0.070467
0.000841 0.000846
Percent of Person-Days that are User-Days = 99.30%
Estimated percentile of user-days falling below calculated exposure
in rag/day
Percentile Exposure
10
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0,
0,
0.
0,
0,
0,
0.
0.
.000698
,001433
.002307
.003723
.006322
.011540
.021241
.037074
Percentile Exposure
90.00
93.00
97.50
99 .00
99 .SO
99.75
99. 90
0.090283
0.160747
0.231215
0.313832
0.440487
0.577595
0.737251
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
10
20
30
40
SO
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0.
0,
0.
0.
0.
0.
0.
0 .
,000656
.001389
.002246
.003648
.006191
.011397
,021063
.036609
Percentile Exposure
90.00
95.00
97.50
99.00
99.50
99.75
99.90
0.089739
0.159838
0.229675
0.313532
0.439401
O.S76810
0.737197
Page 19 of38
-------
U.S. Environmental Protection Agency Ver, 2.02
DEEM-FCID ACOTE Analysis for CRYOLITE {1994-98 data)
Residue file: Cryolite-AR-CT new raisin factor.R98
Adjustment factor #2 used.
Analysis Date: 06-03-2010/13:01:11 Residue file dated; 06-24-2004/10:05:08/8
So body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: ""
Custom demographics 4:7- <11
All Seasons
All Regions
Sex: M/F-all/
All Races
Age-Low: 7 yrs High: 11 yrs
Daily Exposure Analysis
(rag/day)
per Capita per User
Mean 0.028471 0.028704
Standard Deviation 0.069277 0.069512
Standard Error of mean 0.001337 0.001347
Percent of Person-Days that are User-Days = 99.19%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile
Exposure
10
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0.
0.
0
0
0
0
0
0
.000759
.001569
,002533
.003744
.005884
.010417
.017264
,028363
Percentile Exposure
90.00
95.00
97,50
99.00
99.50
99.75
99.90
O.Q7454
0.126652
0.225153
0.333141
0.485657
0.671155
0.741857
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
10
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0
0
0
0
0
0
0
0
.000703
.001513
.002456
.003685
.005711
.010173
.017039
.028166
Percentile Exposure
90.00
95.00
97.50
99.00
99.50
99.75
99.90
0. 074291
0.126163
0.224248
0.332575
0.484766
0.671024
0.741806
Page 20 of 3 8
-------
0.S. Environmental Protection Agency Ver, 2,02
DEEM-FCID ACUTE Analysis for CRYOLITE {1994-98 data)
Residue file: Cryolite-AR-CT new raisin factor,R98
Adjustment factor #2 used.
Analysis Date: 06-03-2010/13:01:11 Residue file dated: 06-24-2004/10:05:08/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: ""
Custom demographics 5: 11 - <14
All Seasons
All Regions
Sex: M/F-all/
All Races
Age-Low: 11 yrs High: 14 yrs
Daily Exposure Analysis
(mg/day)
per Capita per User
Mean 0.024786 0.025056
Standard Deviation 0.061571 0.061850
Standard Error of mean 0.001524 0.001540
Percent of Person-Days that are User-Days = 98.92%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile Exposure
10.00
20.00
30. 00
40. 00
50.00
60.00
70.00
80.00
0.000871
0.001695
0.002571
0.003537
0.005329
0.008325
0.014132
0.025251
Percentile
Exposure
90.00
95. 00
97.50
99.00
99.50
99.75
99. 90
0.059909
0.115049
0.188393
0.324694
0.425857
0.489522
0.733597
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
10
20.
30,
40,
50
60,
70,
80,
.00
.00
.00
.00
.00
.00
.00
,00
0
0
0,
0,
0,
0,
0,
0,
.000773
.001634
.002497
.003503
.005215
.008098
.013948
.025070
Percentile Exposure
90.00
95.00
97.50
99.00
99.50
99.75
99. 90
0.059621
0. 113618
0, 188208
0.324475
0.425786
0.489044
0.733375
Page 21 of38
-------
U.S. Environmental Protection Agency Ver. 2.02
DEEM-FCID ACUTE Analysis for CRYOLITE {1994-98 data)
Residue file: Cryolite-AR-CT new raisin factor.R98
Adjustment factor #2 used.
Analysis Date: 06-03-2010/13:01:11 Residue file dated: 06-24-2004/10:05:08/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodforns consumption used.
Run Comment: ""
Custom demographics 6: 14+
All Seasons
All Regions
Sex: M/F-all/
All Races
Age-Low: 14 yrs High: 99 yrs
Daily Exposure Analysis
(mg/day)
per Capita per User
Mean 0.032704 0.033291
Standard Deviation 0.084056 0.084692
Standard Error of mean 0.000584 0.000594
Percent o£ Person-Days that are User-Days =. 98.24% .
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile Exposure
10.
20
30
40
50
60.
70
80.
.00
.00
.00
.00
.00
.00
.00
.00
0.
0
0.
0.
0
0.
0.
0
.000863
.001938
.0030S8
.004460
.006449
.009821
.016997
.029959
Percentile
Exposure
90.00
95 .00
97.50
99. 00
99. 50
99. 75
99.90
0 .078174
0 .182131
0.278982
0 .427729
0 . 533164
0.681739
0 . 872898
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
10 ,
20 .
30 .
40.
50.
60.
70.
80.
.00
.00
.00
.00
,00
. 00
.00
.00
0
0
0
0
0
0
0
0
.000684
.001796
.002912
.004277
.006224
.009528
.016530
.029249
Percentile
Exposure
90.00
95.00
97.50
99.00
99.50
99.75
99.90
0. 07S275
0.179623
0.276623
0.425648
0.530005
0.681273
0.861668
Page 22 of 3 8
-------
Attachment 5. Results of sulfuryl fluoride food fumigation exposure analysis
U.S. Environmental Protection Agency Ver, 2.02
DEEM-FC1D ACUTE Analysis for FLUORIDE (1994-98 data)
Residue file: F Food Fumigation - 2009 RevisedCT - 4-28 Strict Label.R9S
Adjustment factor #2 used.
Analysis Date: 06-03-2010/12:59:31 Residue file dated: 05-06-2009/13:54:06/8
Ho body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: "RfO is converted Fluoride MCL and for adult pops only."
Summary calculations (per capita):
95th Percentile
Exposure
All infants:
0.039579
Custom demographics 1: 0.5 - <1:
0.096990
Custom demographics 2: 1 - <4:
0.140401
Custom demographics 3: 4 - <7:
0.176854
Custom demographics 4:7- <11:
0.204775
Custom demographics 5: 11 - <14:
0.291818
Custom demographics 6: 14+:
0.273986
99th Percentile
Exposure
0.098237
0.226422
0.282132
0.355497
0.406162
0.602765
O.S63283
99.9th Percentile
Exposure
0.230985
0.429346
0.528114
0.663533
0.744262
0.981154
1.122529
Page 23 of 3 8
-------
U.S. Environmental Protection Agency Ver. 2.02
DEEM-FCID ACUTE Analysis for FLUORIDE {1934-98 data)
Residue file; F Food Fumigation - 2009 RevisedCT - 4-28 Strict Label.R98
Adjustment factor #2 used.
Analysis Date: 06-03-2010/12:59:31 Residue file dated: '05-06-2009/13:54 = 06/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: "RfD is converted Fluoride MCL and for 'adult pops only."
All infants
Daily Exposure' Analysis
(rag/day)
per Capita per Oser
/a
Mean 0.009074 0.012660
Standard Deviation 0.020369 0.023098
Standard Error of mean 0.000374 0.000500
Percent of Person-Days that are User-Days = 71.67%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile Exposure
10
20
30
40.
50.
SO
70
80,
.00
.00
.00
.00
,00
.00
.00
.00
0
0
0.
0
0.
0.
0.
0
.000096
.000323
,000933
.002440
.004827
,007798
.011819
.019633
Percentile
Exposure
90.00
95.00
97. 50
99.00
99.50
99.75
99. 90
0 .033116
0.048078
0 .073765
0 . 108894
0.135625
0 . 197544
0 .274808
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
10.00
20.00
30.00
40.00
50.00
60.00
70 .00
80.00
Percentile Exposure
0.000000
0.000000
0.000022
0.000214
0.000957
0.003358
0.007314
0.013155
90. 00
95.00
97.50
99.0.0
99.50
99.75
99.90
0.027144
0.039579
0.057927
0.098237
0.124019
0.159292
0.230985
a/ Analysis based on all two-day participant records in CSFII 1994-98 survey.
1
Page 24 of 3 8
-------
U.S. Environmental Protection Agency
DEEM-FCID ACUTE Analysis for FLUORIDE
Residue file: F Food Fumigation - 2009 RevisedCT
Adjustment factor #2 used.
Analysis Date: 06-03-2010/12:59:31 Residue file dated
No body weight adjustment; Toxicology endpoints- not used
Daily totals for food and foodform consumption used.
Run Comment: "RfD is converted Fluoride MCL and for adult pops only."
Ver. 2.02
(1994-98 data)
4-28 Strict Label-R98
05-06-2009/13:54:06/8
Custom demographics 1: 0.5 - <1
All Seasons
All Regions
Sex: M/F-all/
All Races
Nursing and Non-Nursing (Ages <-
Age-Low: 6 in High: 1 yrs
3)
Daily Exposure Analysis
(rag/day)
per Capita per User
Mean 0.021276 0.021691
Standard Deviation 0.041194 0.041486
Standard Error of mean 0.000696 0.000709
Percent of Person-Days that are User-Days = 98.08%
Estimated pereentile of user-days falling below calculated exposure
in rag/day
Percentile Exposure
10
20
30
40
SO
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0,
0.
0.
0.
0,
0.
0.
0.
.000713
.001437
.002363
.003805
.006416
.010962
.018673
.029818
Percentile
Exposure
90 .00
95 .00
97.50
99.00
99. SO
99. 7S
99.90
0.053524
0.097690
0.132S6S
0.227504
0.273936
0.324460
0.429503
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
10
20
30
40
SO
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0.
0.
0
0
0
0.
0
0
.000592
.001332
.002232
.003620
.005965
.010310
.018080
.029392
Percentile Exposure
90.00
95.00
97.50
99.00
99.50
99.75
99.90
0.052671
0.096990
0.131812
0.226422
0.273629
0.323589
0.429346
Page 25 of 38
-------
Ver. 2.02
(1994-98 data)
28 Strict Label.R98
U.S. Environmental Protection Agency
DEEM-FCID ACOTE Analysis for FLUORIDE
Residue file: F Food Fumigation - 2009 RevisedCT - 4
Adjustment factor #2 used.
Analysis Date: 06-03-2010/12:59:31 Residue file dated
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: "RfD is converted Fluoride MCL and for adult pops only."
05-06-2009/13:54:06/8
Custom demographics 2: 1 - <4
All Seasons
All Regions
Sex: M/F-all/
All Races
Nursing and Non-Nursing (Ages <= 3}
Age-Low: 1 yrs High: 4 yrs
Daily Exposure Analysis
(rag/day)
per Capita per User
Mean 0.032891 0.032958
Standard Deviation 0.059247 0.059289
Standard Error of mean 0.000558 0.000559
Percent of Person-Days that are User-Days = 99.79%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile Exposure
10
20
30
40
50
60
70
80
.00
.00
,00
,00
,00
.00
.00
.00
0
0.
0
0
0.
0
0
0
.001493
.002474
.003756
.005811
.010068
.017265
.028945
.045984
Percentile Exposure
90.00
95.00
97.50
99.00
99. 50
99.75
99.90
0,088963
0.140511
0.198017
0.282227
0.359262
0.443445
0.528153
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
10
20
30
40.
SO,
60
70
80
, 00
.00
.00
.00
.00
.00
.00
.00
0,
0
0.
0.
0.
0.
0
0.
.001475
.002457
. 003733
.005780
.009990
.017173
.028867
.045864
Percentile
Exposure
90 .00
95 .00
97.50
99.00
99.50
99. .75
99.90
0 .088844
0 .140401
0.197707
0.282132
0 .358994
0 .443314
0.528114
Page 26 of 38
-------
Ver. 2.02
U994-98 data)
RevisedCT - 4-28 Strict Label.R98
U.S. Environmental Protection Agency
DEEM-FCID ACUTE Analysis for FLUORIDE
Residue file: F Food Fumigation - 2009
Adjustment factor #2 used.
Analysis Date: 06-03-2010/12:59:31 Residue file dated: 05-06-2009/13:54:06/8
No body weight adjustment; Toxicology-endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: "RfD is converted Fluoride MCL and for adult pops only."
Custom demographics 3: 4 - <7
All Seasons
All Regions
Sex: M/F-all/
All Races
Age-Low: 4 yrs High: 7 yrs
Mean
Standard Deviation
Standard Error of mean
Daily Exposure Analysis
(trig/day)
per Capita per User
0.046643 0.046649
0.073659 0.073662
0.000881 0.000881
Percent of Person-Days that are User-Days = 99.99%
Estimated percentile of user-days falling below calculated exposure
in rag/day
Percentile Exposure
10
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0,
0,
0.
0,
0,
0,
0 .
0,
.002394
.004068
.006915
.012303
.021403
.032227
.044555
.067720
Percentile
Exposure
90 .00
95. -00
97.50
99 .00
99.50
99.75
99 .90
0.121850
0.176863
0.266527
0.355504
0.487238
0.534215
0.663534
Estimated percentile of per-capita days falling below calculated exposure
in nig/day
Percentile Exposure
10
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0
0
0
0
0
0
0
0
.002392
.004066
.006911
.012297
.021396
.032222
.044549
.067714
Percentile
Exposure
90.00
95.00
97.50
99.00
99.50
99.75
99.90
0. 121841
0.176854
0.266522
0.35S497
0.487227
0.534211
0.663533
Page 27 of 3 8
-------
U.S. Environmental Protection Agency Ver. 2.02
DEEM-FCID ACUTE Analysis for FLUORIDE (1994-98 data)
Residue file: F Food Fumigation - 2009 RevisedCT - 4-.2S Strict Label,R98
Adjustment factor #2 used.
Analysis Date: 06-03-2010/12:59:31 Residue file dated: 05-06-2009/13:54:06/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: "RfD is converted Fluoride MCL and for adult pops only."
Custom demographics 4: 7 - <11
All Seasons
All Regions
Sex: M/F-all/
All Races
Age-Low: 7 yrs High: 11 yrs
Daily Exposure Analysis
(mg/day)
per Capita per User
Mean 0.054355 0.054355
Standard Deviation 0.089280 0.089280
Standard Error of mean 0.001723 0.001723
Percent of Person-Days that are User-Days ='100.00%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile
Exposure
10
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0.
0
0
0
0
0
0
0.
.002781
.005067
.009619
.017785
.028257
.037462
.050645
.076801
Percentile Exposure
90.00
95. 00
97.50
99. 00
99. 50
99.75
99.90
0 . 130309
0 .204775
0 ,297045
0.406162
0. 539413
0.639542
0. 744262
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
Percentile Exposure
10 .
20.
30.
40.
50.
60.
70.
80
.00
.00
. 00
. 00
. 00
,00
,00
.00
0.
0,
0,
0.
0 ,
0,
0
o
,002781
.005067
.009619
.017785
.028257
.037462
.050645
.076801
90.00
95.00
97.50
99.00
99.50
99.75
99 .90
0.130309
0.204775
0.297045
0.406162
0.539413
0.639542
0.744262
Page 28 of 38
-------
Ver, 2.02
(1994-98 data)
RevisedCT - 4-28 Strict Label.R98
U.S. Environmental Protection Agency
DEEM-FCID ACUTE Analysis for FLUORIDE
Residue file: F Food Fumigation - 2009
Adjustment factor t2 used.
Analysis Date: 06-03-2010/12:59:31 Residue file dated: 05-06-2009/13:54:06/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: "RfD is converted Fluoride MCL and for adult pops only."
Custom demographics 5: 11 - <14
All Seasons
All Regions
Sex: M/F-all/
All Races
Age-Low: 11 yrs High: 14 yrs
Daily Exposure Analysis
(rag/day)
per Capita per User
Mean 0,067522 0,067522
Standard Deviation 0,127399 0.127399
Standard Error of mean 0.003154 0.003154
Percent of Person-Days that are User-Days = 100.00%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile Exposure
10,
20,
30.
40,
50.
60.
70.
80.
.00
.00
,00
.00
,00
.00
.00
.00
0,
0.
0,
0 .
0,
0.
0,
0.
,002472
.004212
.006674
.014134
.027275
.040233
.057641
.092775
Percentile
Exposure
90 .00
,95.00
97.50
99.00
99.50
99 .75
99 .90
0.179495
0.291818
0.400124
0.602765
0.792960
0.827384
0. 981154
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
10
20
30,
40,
50,
60,
70,
80,
.00
.00
.00
.00
.00
.00
.00
.00
0
0
0
0
0.
0,
0,
0,
.002472
.004212
.006674
.014134
.027275
.040233
.057641
,092775
Percentile
Exposure
90.00
95.00
97. 50
99.00
99.50
99.75
99.90
0. 179495
0.291818
0.400124
0,602765
0.792960
0.827384
0. 981154
Page 29 of 3 8
-------
U.S. Environmental Protection Agency Ver, 2.02
DEEM-FCID ACUTE Analysis for FLUORIDE (1994-98 data)
Residue file: F Food Fumigation - 2009 RevisedCT - 4-28 Strict Label.R98
Adjustment factor f2 used.
Analysis Date: 06-03-2010/12:59:31 Residue file dated: 05-06-2009/13:54:06/8
Ho body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: "RfD is converted Fluoride MCL and for adult pops only."
Custom demographics 6: 14+
All Seasons
All Regions
Sex: M/F-all/
All Races
Age-Low: 14 yrs High: 99 yrs
Daily Exposure Analysis
(mg/day)
per Capita per User
Mean 0.057620 0.057768
Standard Deviation 0.117804 0.117919
Standard Error of mean 0.000819 0.00.0821
Percent of Person-Days that are User-Days =. 99.74%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile
Exposure
10
20
30
40
BO
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0
0
0
0
0
0
0
0
.001770
.002968
,004572
.007237
.012067
.021400
.039452
.074577
Percentile Exposure
90.00
95.00
97.50
99.00
99.50
99.75
99,90
0.1S8094
0.274313
0.395651
0.563477
0.747002
0,883365
1.122607
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile
80. 00
Exposure
10 .00
20 .00
30 .00
40.00
50.00
60.00
70.00
0.001744
0.002939
0.004537
0.007181
0.011979
0.021271
0.039263
0.074327
Percentile
Exposure
90.00
95.00
97. SO
99.00
99. SO
99.75
99.90
0,157643
0.273986
0 .395310
0.563283
0,746855
0.883065
1.122529
Page 3 Oof 3 8
-------
Attachment 6. Results of sulfuryl fluoride structural fumigation exposure analysis
U.S. Environmental Protection Agency Ver, 2,02
DEEM-FCID ACUTE Analysis for FLUORIDE (1994-98 data)
Residue file: F Space Fumigation - 2009 - 5-1.R98 Adjustment factor #2 used.
Analysis Date: 06-03-2010/12:57:19 Residue file dated: 05-06-2009/13:52:45/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodforrn consumption used.
Run Comment: "RfD is converted Fluoride HCL and is valid for adult pops, only"
Summary calculations (per capita):
93th Percentile
Exposure
All infants:
0.012880
Custom demographics 1: 0.5 -
-------
U.S. Environmental Protection Agency Ver, 2.02
DEEM-FCID ACUTE Analysis for FLUORIDE (1994-98 data)
Residue file: F Space Fumigation - 2009 - 5-1.R98 Adjustment factor 12 used.
Analysis Date: 06-03-2010/12:57:19 Residue file dated: 05-06-2009/13:52:45/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodforra consumption used.
Run Comment: "RED is converted Fluoride MCL and is valid for adult pops, only"
All infants
Daily Exposure Analysis /a
(mg/day)
per Capita per User
Mean 0.004162 0.004671
Standard Deviation 0.005018 0.005087
Standard Error of mean 0.000092 0.000099
Percent of Person-Days that are User-Days = 89.10%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile Exposure
10
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0
0.
0
0
0
0
0
0
.000287
.001141
.001796
.002352
.003240
.004202
.005457
.007331
Percentile
Exposure
90.00
95.00
97.50
99.00
99.50
99.75
99.90
0. 010182
0.013552
0.017857
0.022398
0.032183
0.041136
0.047989
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
Percentile- Exposure
10
20
30
40
50
SO
70
80
.00
.00
.00
.00
.00
.00
.00
. 00
0
0
0
0
0
0
0
0
.000000
.000296
.001279
.001912
.002668
.003716
.004955
. 006913
90
95.
97,
99
99
99
99
.00
.00
.50
.00
.SO
.75
. 90
0.
0.
0.
0 .
0.
0,
0.
.009705
.012880
.017653
.021374
.032032
.040955
.046940
a/ Analysis based on all two-day participant records in CSFII 1994-98 survey.
1
Page 32 of 3 8
-------
U.S. Environmental Protection Agency Ver. 2.02
DEEM-FCID ACUTE Analysis for FLUORIDE {1994-98 data)
Residue file: F Space Fumigation - 2009 - 5-1.R98 Adjustment factor #2 used.
Analysis Date; 06-03-2010/12:57:19 Residue file dated: 05-06-2009/13:52:45/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: "RfD is converted Fluoride MCL and is valid for adult pops, only"
Custom demographics 1: 0.5 - <1
All Seasons
All Regions
Sex: M/F-all/
All Races
Nursing and Non-Nursing (Ages <= 3)
Age-Low: 6 m High: 1 yrs
Daily Exposure Analysis
(mg/day)
per Capita per User
Mean 0.008687 0.008742
Standard Deviation 0.006490 0.006473
Standard Error of mean 0.000110 0.000110
Percent of Person-Days that are User-Days = 99.37%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile Exposure
10
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0.
0,
0.
0.
0
0,
0
0
.002317
.003754
.004835
.006085
.007295
.008688
.010478
.012723
Percentile
Exposure
90.00
95.00
97.50
99.00
99.50
99.75
99.90
0.016759
0.020288
0.024883
0.032100
0.038552
0 .041749
0.050424
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
10
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0.
0.
0.
0,
0,
0,
0.
0.
.002228
.003685
.004790
,006034
.007254
.008650
.010442
.012683
Percentile
Exposure
90.00
95.00
97.50
99 .00
99.50
99.75
99.90
0.016715
0.020257
0.024758
0.032080
0.038501
0.041724
0.050413
Page 33 of 38
-------
U.S. Environmental Protection Agency Ver. 2,02
DEEM-FCID ACUTE Analysis for FLUORIDE ' {1994-98 data)
Residue file: P Space Fumigation - 2009 - 5-1.R98 Adjustment factor #2 used.
Analysis Date: 06-03-2010/12:57:19 Residue file dated: 05-06-2009/13:52:45/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: "RfD is converted Fluoride MCL and is valid for adult pops, only"
Custom demographics 2: 1 - <4
All Seasons
All Regions
Sex: M/F-all/
All Races
Nursing and Non-Nursing (Ages <-. 3)
Age-Low: 1 yrs High: 4 yrs
Daily Exposure Analysis
(rag/day)
per Capita per User
Mean 0.012080 0.012093
Standard Deviation 0.007781 0.007776
Standard Error of mean 0.000073 0.000073
Percent of Person-Days that are User-Days = 99,89%
Estimated percentile of user-days falling below calculated exposure
in rag/day
Percentile Exposure
10.
20.
30,
40.
50.
60.
70,
80,
.00
.00
, 00
,00
. 00
.00
,00
.00
0.
0,
0,
0.
0.
0,
0,
0.
.0042S4
.006188
.007792
.009186
.010638
.012244
.014101
.016786
Percentile Exposure
90.00
95.00
97.50
99.00
' 99 .50
99 .,75
99.90
0.021199
0.025862
0.030621
0.039299
0 .047837
0.054314
0.062737
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
10
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0
0
0
0
0
0
0
0
.004233
.006169
.007783
.009178
.010629
.012237
.014095
.016780
Percentile Exposure
90. 00
95. 00
97.50
99,. 00
99.50
99.75
99.90
0.021193
0. 025853
0.030615
0.039290
0.047830
0.054306
0-.062731
Page 34 of 38
-------
U.S. Environmental Protection Agency Ver, 2.02
DEEM-FCID ACUTE Analysis for FLUORIDE (1994-98 data)
Residue file: F Space Fumigation - 2009 - 5-1..R9S Adjustment factor #2 used.
Analysis Date: 06-03-2010/12:57:19 Residue file dated: 05-06-2009/13:52:45/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: "RfD is converted Fluoride MCL and is valid for adult pops, only"
Custom demographics 3: 4 - <7
All Seasons
All Regions
Sex: M/F-all/
All Races
Age-Low: 4 yrs High: 7 yrs
Mean
Standard Deviation
Standard Error of mean
Daily Exposure Analysis
(rag/day)
per Capita per User
0.015334 0.015335
0.008582 0.008582
0.000103 0.000103
Percent of Person-Days that are User-Days = 100.00%
Estimated percentile of user-days falling below calculated exposure
in nig/day
Percentile Exposure
10
20
30
40
50.
60.
70,
80.
.00
.00
.00
.00
.00
.00
.00
. 00
0
0.
0.
0.
0
0,
0 .
0,
.006783
.008838
.010475
.012192
.013877
. 015620
.017752
.020477
Percentile
Exposure
90.00
95.00
97.50
99.00
99.50
99.75
99, 90
0.025067
0.030101
0.036002
0,045022
0.054278
0.062688
0.076356
Estimated percentile of per-capita days falling below calculated exposure
in rag/day
Percentile Exposure
10
20
30
40
SO
60
70.
80
.00
.00
.00
.00
.00
.00
.00
.00
0,
0.
0.
0.
0.
0.
0.
0.
,006782
,008837
010475
,012192
013876
015620
017752
020476
Percentile Exposure
90.00
95.00
97.50
99.00
99.50
99,75
0.025067
0.030100
0.036002
0.045022
0.054278
0.062687
99.90
0.076355
Page 35 of 38
-------
U.S. Environmental Protection Agency Ver. 2,02
DEEM-FCID ACUTE Analysis for FLUORIDE (1994-98 data)
Residue file: F Space Fumigation - 2009 - 5-1,R98 Adjustment factor #2 used.
Analysis Date: 06-03-2010/12:57:19 Residue file dated: 05-06-2009/13:52:45/8
No body weight adjustment; Toxicology, endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: "RfD is converted Fluoride MCL and is valid for adult pops, only"
Custom demographics 4:7- <11
All Seasons
All Regions
Sex: M/F-all/
All Races
Age-Low: 7 yrs High: 11 yrs
Daily Exposure Analysis
(rag/day)
per Capita per User
Mean 0.016963 0.016963
Standard Deviation 0.009573 0.009573
Standard Error of mean 0.000185 0.000185
Percent of Person-Days that are User-Days = 100.00%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile
Exposure
10.
20.
30.
40
50.
60.
70.
80.
.00
.00
.00
.00
.00
.00
.00
.00
0.
0.
0,
0.
0,
0
0,
0,
.007496
.009838
.011950
.013499
.015090
.016983
.019627
. 022463
Percentile
Exposure
90.00
95.00
97.50
99.00
99. 50
99.75
99. 90
0 .027494
0.034938
0 .041059
0 .050785
0 .064499
0 .071295
0 .074763
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile Exposure
10
20.
30
40
50.
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0.
0
0
0
0
0
0.
0.
.007496
.009838
.011950
.013499
.015090
.016983
.019627
.022463
Percentile Exposure
90.00
95.00
97.50
99.00
99.50
99.75
99.90
0.027494
0.034938
0.041059
0.050785
0.064499
0.071295
0.074763
Page 36 of 38
-------
U.S. Environmental Protection Agency Ver. 2.02
DEEM-FCID ACUTE Analysis Cor FLUORIDE (1994-98 data)
Residue file: F Space Fumigation - 2009 - 5-1.R98 Adjustment factor #2 used.
Analysis Date: 06-03-2010/12t57:19 Residue file dated: 05-06-2009/13:52:45/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodfortn consumption used.
Run Comment: "RfD is converted Fluoride MCL and is valid for adult pops, only"
Custom demographics 5: 11 - <14
All Seasons
All Regions
Sex: M/F-all/
All Races
Age-Low: 11 yrs High: 14 yrs
Daily Exposure Analysis
(mg/day)
per Capita per User
Mean 0.018195 0.018195
Standard Deviation 0.010600 0.010600
Standard Error of mean 0.000262 0.000262
Percent of Person-Days that are User-Days = 100.00%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile Exposure
Percentile Exposure
10
20
30
40.
50.
SO,
70.
80.
.00
.00
.00
.00
. 00
.00
.00
.00
0
0.
0
0,
0.
0.
0.
0.
.007430
.009973
.011986
.014242
.016293
,018556
.021368
.024821
90.00
95.00
97.50
99.00
99.50
99.75
99. 90
0.031142
0.0371S1
0.044191
0.051720
0.065023
0.074234
0.089794
Estimated percentile of par-capita days falling below calculated exposure
in mg/day
Percentile
Exposure
10.
20.
30.
40.
50.
60.
70.
80.
.00
.00
.00
,00
.00
.00
.00
.00
0.
0,
0,
0,
0.
0.
0.
0.
.007430
.009973
.011986
.014242
.016293
.018556
.021368
.024821
Percentile
Exposure
90.00
95.00
97. 50
99.00
99.50
99.75
99 .90
0.031142
0.037161
0.044191
0.051720
0.065023
0.074234
0.089794
Page 37 of 38
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U.S. Environmental Protection Agency Ver. 2.02
DEBM-FCID ACUTE Analysis for FLUORIDE (1994-98 data)
Residue file: F Space Fumigation - 2009 - 5-1.R98 Adjustment factor #2 used.
Analysis Date: 06-03-2010/12:57:19 Residue file dated: 05-06-2009/13:52:45/8
No body weight adjustment; Toxicology endpoints not used
Daily totals for food and foodform consumption used.
Run Comment: "RfD is converted Fluoride MCL and is valid for adult pops, only"
Custom demographics 6: 14+
All Seasons
All Regions
Sex: M/F-all/
All Races
Age-Low: 14 yrs High: 99 yrs
Daily Exposure Analysis
(mg/day)
per Capita per User
Mean 0.018672 0.018711
Standard Deviation 0.014970 0.014961
Standard Error of mean 0.000104 0.000104
Percent of Person-Days that are User-Days = 99.79%
Estimated percentile of user-days falling below calculated exposure
in mg/day
Percentile Exposure
10.
20
30
40
50
60
70
80
.00
.00
.00
.00
.00
.00
.00
.00
0.
0.
0.
0.
0.
0.
0.
0
.005648
.008329
.010533
.012727
.015106
.017760
.021331
.026257
Percentile
Exposure
90 .00
95 . 00
97.50
99. 00
99.50
99.75
99. -90
0 .035058
0.045280
0.057802
0. 074405
0. 087706
0.11044S
0.135358
Estimated percentile of per-capita days falling below calculated exposure
in mg/day
Percentile
Exposure
10,
20.
30.
40,
50.
60.
70.
80,
.00
,00
.00
.00
,00
.00
.00
,00
0
0
0
0
0
0
0
0
.005592
.008289
.010499
.012698
.015084
.017733
.021308
.026235
Percentile Exposure
90.00
95.00
97.50
99 .00
99.50
99.75
99.90
0 .035028
0.04S247
0 .057763
0 .074354
0 .087587
0 .110395
0.13S312
Page 38 of 38
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