r/EPA
              United States
              Environmental Protection
              Agency
              Office of
              Toxic Substances
              Washington, D.C. 20460
EPA 560/13-80-024
November 1980
              Office of Toxic Substances
Mirex Residue  Levels
in Human Adipose Tissue
                *
A Statistical  Evaluation

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                                    EPA 560/13-80-024
                                    November, 1980
                final Report

               RTI/1864/17-OOF
Mirex Residue Levels in Human Adipose Tissue:
          A Statistical Evaluation

                     by

               Carol Leininger
              Donna Lucas Watts
              Charles Sparacino
              Stephen Williams
         Research Triangle Institute
           Research Triangle Park
            North Carolina  27709
         Contract Number 68-01-5848
         Task Manager:   Cindy Stroup
       Project Officer:   Joseph Carra
        Design and Development Branch
        Exposure Evaluation Division
         Office of Toxic Substances
    U.  S. Environmental Protection Agency
              401 M Street, SW
           Washington,  D.C.  20460

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                            DISCLAIMER NOTICE

This  report was  prepared under  contract  to  an  agency of  the  United
States Government.  Neither  the  United States Government nor any of its
employees,  contractors,  subcontractors, or  their employees, makes  any
warranty, expressed or implied, nor assumes any legal liability or respon-
sibility  for  any third  party's  use or  the results of  such  use  of any
information, apparatus, product or process disclosed in this report, nor
represents that its use by such third party would not infringe privately
owned rights.

Publication of the  data in  this  document  does  not  signify  that  the
contents necessarily reflect the joint or separate views and policies of
each  sponsoring  agency.   Mention of trade names  or  commercial  products
does not constitute endorsement or recommendation for use.

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                             ACKNOWLEDGEMENT
     The  authors  acknowledge  the  cooperation  of  Dr.  Frederick Kutz,
Ms. Sandra Strassman-Sundy,  and Ms.  Madeline O'Neill Dean of  the  U.S.
Environmental Protection Agency, Washington, D.C.,  in providing informa-
tion  on the  sample design  and data collection for the  Mirex Special
Study.  The authors appreciate the assistance of Dr.  Robert Welch of the
Michigan Department of  Public Health in supplying  information about the
chemical analysis techniques employed.  Special thanks go to Ms. Martha
Clegg and Ms. Pat Parker for an excellent job of typing.
                                   -1-

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                            TABLE OF CONTENTS
1.   INTRODUCTION AND CONCLUSIONS 	  1

     1.1  Introduction	1
          1.1.1  Foreward	1
          1.1.2  Summary of Study	1
     1.2  Conclusions 	  2
          1.2.1  Survey Design	2
          1.2.2  Chemical Analysis	2
          1.2.3  Exploratory Data Analysis	2
                 1.2.3.1  Introduction	2
                 1.2.3.2  Unweighted Analysis 	  3
                 1.2.3.3  Weighted Analysis 	  3

2.   THE NATIONAL HUMAN MONITORING PROGRAM'S MIREX
       SPECIAL STUDY	5

     2.1  Detailed Description of Study 	  5
          2.1.1  Introduction 	  5
          2.1.2  Sample Design	5
     2.2  National Human Monitoring Program 	  6
          2.2.1  Introduction 	  6
          2.2.2  Strata	8
          2.2.3  Eligible Places	8
          2.2.4  Pathologists and Medical Examiners 	  8
          2.2.5  Quotas	8
     2.3  Selection Weight Construction 	  9

3.   EVALUATION OF CHEMICAL ANALYSIS	13

     3.1  Introduction	13
     3.2  Discussion	13

4.   UNWEIGHTED ANALYSIS	24

     4.1  Data Description	•  .  .	24
     4.2  Data Analysis	25
          4.2.1  Data Distribution	25
          4.2.2  Proportions of Positive Values  	 32
          4.2.3  Quantifiable Positive Values 	 40
          4.2.4  Unweighted Analysis Conclusions	40

5.   WEIGHTED ANALYSIS	43

     5.1  Introduction	43
     5.2  Weight Formation	43
     5.3  Estimates of Positive Mirex Detection 	 43
     5.4  Estimates of Quantifiable Positive Values 	 48
     5.5  Weighted Analysis Conclusions 	 49
                               -ii-

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                        TABLE OF CONTENTS (Cont.)

                                                                 Page

REFERENCES	54

APPENDIX A:     State Maps Showing Counties Where Federally
               Assisted Mirex was Applied at Some Time During
               1965-1974	A-55

APPENDIX B:     Counties Where Federally Assisted Mirex was
               Applied at Some Time During 1965-1974	B-65

APPENDIX C:     Definition of Mirex Treated Areas	C-71

APPENDIX D:     MSS Sample Site Selection Method 	 D-73

APPENDIX E:     List of MSS Collection Sites	E-79

APPENDIX F:     Quotas for Mirex Special Study Specimens 	 F-82

APPENDIX G:     Instructions to Pathologists 	 G-86

APPENDIX H:     Modification of Mirex Analysis Protocol -
               GC Column Temperature	H-95

APPENDIX I:     Confirmation Analyses of Mirex in Human Adipose
               Tissue Extracts	1-97
                                  -iii-

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                             LIST OF TABLES

Table                                                            Page

3.1  Comparison of Mirex Peak Heights (mm) and Calculated
     Amounts (pg) as Determined by Michigan Department of
     Public Health and Quality Control Checks 	    22

3.2  Interperson Comparison of Mirex Peak Height Measurements .    23

4.1  Specimens Collected for Each Census Division by Age, Race,
     and Sex	    26

4.2  Detection of Mirex Residue by State:  Number of Specimens
     with Positive and Zero Detectable Levels	    34

4.3  Detection of Mirex Residue by Race and Age:  Number of
     Specimens with Positive and Zero Detectable Levels ....    35

4.4  Chi-Square Analysis Results for Zero Detectable/Positive
     Values:  Geographic and Demographic Variables	    36

4.5  Regression Model for Race, Age, Sex, and State:  Zero
     Detectable/Positive Residue Values 	    38

4.6  Regression Model for Race, Age, Sex, and Census Division:
     Zero Detectable/Positive Residue Values	    39

4.7  Summary Statistics for Quantifiable Positive Residue
     Values:  Geometric Means and Standard Errors 	    41

4.8  Summary Statistics for Quantifiable Positive Residue
     Values:  Geometric Means and Standard Errors 	    42

5.1  Weighted Chi-Square Analysis Results for Zero Detectable/
     Positive Values:  Geographic and Demographic Variables . .    45

5.2  Weighted Regression Model for Race, Age, Sex, and Census
     Division:  Zero Detectable/Positive Residue Values ....    46

5.3  Weighted Regression Model for Race, Age, Sex, and State:
     Zero Detectable/Positive Residue Values	    47

5.4  Estimated Summary Statistics for Quantifiable Positive Residue
     Values:  Weighted Geometric Means and Standard Errors. . .    50

5.5  Estimated Summary Statistics for Quantifiable Residue Values:
     Weighted Geometric Means and Standard Errors 	    51

5.6  Weighted Regression Model for Location, Age, Race, and Sex
     Versus Quantifiable Positive Residue Amounts of Mirex. . .    52

5.7  Weighted Regression of Quantifiable Positive Residue
     Amounts:  Location, Age, Race, and Sex	    53
                             -iv-

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                             LIST OF FIGURES

Figure

 2.1      Sampling frame and selection procedures for Mirex
          Special Study 	    7

 3.1      Gas chromatogram - Aroclor 1260 standard	   15

 3.2      Gas chromatogram - mirex standard	   16

 3.3      Gas chromatogram - mixture of Aroclor 1260 and mirex
          standards	   17

 3.4      Gas chromatogram - mirex containing specimen (moderate
          level) with interference peak (moderate level). ...   18

 3.5      Gas chromatogram - mirex containing specimen (low
          level) with interference peak (low level)	    19

 3.6      Gas chromatogram - mirex containing specimen (moderate
          level) with interference (high level) 	   20

 4.1      Frequency Distribution for Raw Values of Residue
          Amount	   28

 4.2      Frequency Distribution for transformed values of
          wet weight mirex residue	   30

 4.3      Frequency Distribution of lipid adjusted mirex
          residue amounts and transformed values (n = 123
          quantifiable positives) 	   31
                                 -v-

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1.        INTRODUCTION AND CONCLUSIONS
1.1.      Introduction
1.1.1.    Foreword
     This  report presents  a statistical  evaluation of  data  collected
under  the  Environmental  Protection  Agency  National Human  Monitoring
Program's Mirex  Special Study,  which was begun  in 1975.  The  primary
objectives of  this  effort  were  to investigate, document, and assess the
survey design, to verify the chemical analysis results, and to calculate
estimates of  the  prevalence of  mirex residues in  human  adipose  tissues
in a defined section of the southern United States.  Several demographic
variables were included in  exploratory analyses  to  determine  if there
were any identifiable factors contributing or otherwise related to mirex
residues in humans.
     Chapter  2 of this report  describes the  survey  design employed in
the  Mirex Special  Study  and  includes  a  rationale of  the statistical
analysis approach.   Chapter 3  is a discussion of the chemical analysis.
Chapters 4 and 5 are presentations of unweighted and weighted statistical
analyses, respectively.
1.1.2.    Summary of Study
     Mirex is  an  organochlorine  insecticide  widely used for the control
of the  imported  fire ant  in large areas  of  the  southern United States.
It  is  persistent,  which,  in combination with  the  substance's  pharraaco-
dynamics,  leads  to  environmental  mobility and potential incorporation
into various food chains.
     Mirex  residues  found  in specimens of human  adipose  tissue  led to
the Mirex Special Study (MSS) conducted by the National Human Monitoring
Program (NHMP).  The study area,  sample design, sample selection,  speci-
fication of the procedures  for collecting specimens in the field and for
chemical analysis were  defined by the NHMP.    From October 1975  through
September  1976,  a  sample   of  630 human  adipose   tissue  specimens  were
collected from selected surgical patients and cadavers.   The sample was
selected within a  study area defined as all  counties having some  feder-
ally  assisted application  of  the  insecticide mirex  between 1965  and
1974.   Mirex   residues  were found in 141 of  the  624 tissue  specimens
analyzed  (six of the 630  specimens  were not  analyzed  because  of  the
inadequate amount of extractable  lipid).  The convention of referring to
a single  sampling  unit, i.e.,  adipose tissue from a surgical patient or
                                 -1-

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cadaver, as  a  specimen,  and a collection of sampling units or specimens
as a sample is used throughout this report.
1.2.      Conclusions
1.2.1.    Survey Design
     The  limitations  and  assumptions  of  the  MSS  survey design  are
described in detail  in Chapter 2 and in sections 4.1, 4.2, and 5.2.   In
brief,  the  major  limitation  of  this particular  survey design  is  the
method of sample  selection.  The sample selection did not include prob-
ability  sampling  at each  step of the selection process.   Any estimate
for a population  made  from a  small number  of  people or things selected
from  the larger  group  is  based  on  the assumption  that anyone  can be
selected  and that  the probability,  or chance,  of  that  selection is
known.   Residue  levels  and other pertinent population  values  cannot be
accurately estimated  with  any  assurance  unless the  probabilities with
which a  given  tissue  specimen was chosen for the MSS can be calculated.
This  limitation  should be  recognized in the  interpretation  and  use of
the findings in this report.
1.2.2.    Chemical Analysis
     Raw mirex analytical  data,  in the form of  gas  chromatograms, were
examined in  order  to  assess the reliability of  the  final results.  For
those chromatograms  made available for study,  good  analytical practice
was indicated  in virtually all  cases.  The analytical system remained
stable  over  the  period  of study, overall sensitivity  was  more  than
adequate, and  peak area  measurements were accurate  and  precise  in  the
vast  majority  of  cases.    The  results were  thus  deemed  reliable  and
amenable to detailed statistical treatment.
1.2.3.    Exploratory Data Analysis
1.2.3.1.  Introduction
     Two methods  of analysis  were used for  the  exploratory  analyses:
unweighted and weighted  analyses.   The unweighted analysis can  only be
used  to  describe  the  624  specimens  in the MSS sample.   The  weighted
analysis is  an  attempt to  estimate the patterns  influencing  prevalence
of mirex residues  in  the target population.  The target population here
consists of  all human  residents  of all counties where mirex was applied
during  a ten  year period  in eight  southern  States.   The process of
adjusting the information  contained  in the sample so that it represents
                                 -2-

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the target population is called weighting; the methodology and justifica-
tion are  described in  greater detail in  section 2.3.   Any  inferences
about a study population that are based on a sample from that population
need to be  based on data that have  been adjusted or weighted according
to rules or assumptions of probability.
1.2.3.2   Unweighted Analysis
     The results  of  the unweighted analysis on the sample of 624 speci-
mens indicate that the geographic location of the collection site is the
most important  factor studied for explaining the  differences  in number
of positive detections of mirex in these particular human adipose tissue
specimens.   Some results  from  the  unweighted  analyses  of  the entire
sample and  of  the 123 quantifiable observations are  listed below.   The
results describe  only the specific group of human adipose tissue speci-
mens analyzed.
     For all 624 specimens,
          the   proportion  of  positive   detections   is   significantly
          different  (p £ 0.0001)  among States  and  Census  Divisions.
          there are marginally significant (p £ 0.10) differences related
          to the factors age and race.
     For the 123 quantifiable observations,
          demographic and geographic  factors  did not show any effect in
          degree of mirex concentration in sample specimens.
1.2.3.3.  Weighted Analysis
     In the weighted  analysis,  location of the  selection site  is again
the most significant  variable of those studied for explaining variation
in mirex residues.   The results  of the weighted analyses  for the entire
sample and for the quantifiable observations are listed below.
     For the total sample,
          State is a  significant (p < 0.0001)  factor  in  explaining the
          variation of positive mirex detection.
          Mississippi  is  the  State  in  which  the proportion  of mirex
          residues is extremely high (51.1 percent).
     For the quantifiable residue amounts,
          there is a significant interaction between geographic location
          and race.   This  suggests  that there is possibly a race effect
          for some geographic  divisions  that is not particularly strong
          or consistent throughout the mirex treated area.
                                 -3-

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     It must be  emphasized  that the limitations of the sample selection
methodology restrict the  interpretation  of any results.  These findings
can be  interpreted  only as  indications of trends  or  patterns which may
exist in the population living in the mirex treated region.
                                 -4-

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2.        THE  NATIONAL HUMAN MONITORING  PROGRAM'S MIREX  SPECIAL STUDY
2.1.      Detailed Description of the Study
2.1.1.    Introduction
     Human  adipose tissue  specimens  for  the  Mirex Special  Study were
collected from October 1,  1975  through September  30,  1976 (FY76).  The
target population  was the  human population of  all counties  with some
federally assisted application  of mirex at any  time  during the 10-year
period  1965 to  1974  (Kutz  and  Strassman undated).   A  list  of these
counties was provided to the NHMP by the U.S.  Department of Agriculture.
Maps of the eight southern States containing these counties are displayed
in  Appendix A.  A  list of  the  mirex counties,  by State,  is  given in
Appendix B.   The pattern  of mirex use  can be  charted  directly to the
areas of infestation of imported fire ants in this country.  This infes-
tation pattern does  not conform to large-scale  geographic or political
boundaries, such as Census Divisions or States, as can be seen by examin-
ing the maps  in  Appendix A.  No information was provided concerning the
amount or frequency  of mirex application over the 10-year period.  Such
information might be extremely important in determining levels of expect-
ed  exposure to this  insecticide;  for further discussion  of this point
see Appendix C.
2.1.2.    Sample Design
     Mirex residues were found in human adipose tissue specimens submit-
ted to the NHMP,  which was designed to provide estimates at the national
level.  There were eight cities  in mirex areas where established contacts
(hospital. pathologists or  medical examiners)  were  already submitting
adipose tissue specimens  for the NHMP.  A special study was designed to
increase representation  from mirex regions by increasing  the number of
sample  sites  in  mirex areas.   32 supplementary sites were selected,
bringing the total number of sites contacted in the MSS to 40.
     To select  the 32  supplementary  areas for  the MSS,  a listing was
made of all  1974  Ranally Metropolitan Areas (RMA's)  in  the mirex area:
RMA's were  defined on a township and  locality basis.   All areas with a
total population of  50,000  or more were considered to be  RMA's.  Other
areas that  presently had populations  close to  50,000,  had populations
greater than  50,000  in  the  past,  or had  special  significance  in their
States were also defined  as RMA's (Rand  McNally 1974).   The  complete
                                 -5-

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listing of the population from which a sample will be selected is called
a frame.  The  8  NHMP sites were on the frame of 68 RMA's located in the
mirex area.   These 8 cities were not included as possible selections for
the  mirex supplementary  sample because they  were already  included as
part  of  the MSS  sample by virtue  of their initial  selection into the
NHMP.
     Of the 60 RMA's in the mirex supplementary list, 32 were apparently
selected by  simple  random sampling (SRS).   The 60  RMA's were listed in
alphabetical order  (not pertinent to the selection process), and then a
SRS was selected  from  the list.  See Appendix D for a discussion of the
site selection methodology employed.  Nine additional sites were select-
ed, in the same manner, to be used as alternates in case there were non-
responding  sites.   These  alternates were  to  be   substituted  for non-
responding sites in the order in which they were selected.  One site was
replaced by  an alternate  selection.   A list of the  selected sites and
alternates is given in Appendix E.
     The selection of sites within mirex areas produced 40 sample RMA's.
Of  these,  5 of  the 8  NHMP  sites and 23 of the  32 mirex supplementary
sample RMA's  responded with  valid  tissue specimens.   The treatment of
nonresponding  sites  is described  in section 2.3.   Figure 2.1 outlines
the path of  the  sample selection procedures for obtaining tissue speci-
mens for the MSS.
     Data collection for  the  MSS  after  the  selection  of  first-stage
RMA's follows the methods  used in the Adipose Tissue Survey (ATS) of the
NHMP.  For  the convenience  of  the  readers,  a  brief  discussion of the
NHMP is now included; a more detailed description is contained in a 1979
EPA document (Hartwell et  al. 1979).
2.2.      National Human Monitoring Program
2.2.1.    Introduction
     The statistical design used to collect data for the ATS of the NHMP
has two stages.   The contiguous 48 states were stratified into several
regions.   Sampling  sites  were  selected  from a list  of eligible places
with probability proportional to population.   Within the sampling sites,
the  subsampling  was performed  by cooperating pathologists  and medical
examiners.
                                 -6-

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    23,557,425
    17,085,700
    13,486,900
    unknown
       624
Target population*—total population of counties
  where mirex has been used.
                                       Purposive exclusions of cities and towns not
                                          defined as RMA's.
1st stage sampling frame and inference population—
   the human population of 68 RMA's.
                                       Selection of a subset of 40 of the 68 RMA's.
                                                               / *
1st stage sample of RMA's.
                                       Purposive exclusion of some hospitals, pathologist*
                                          and medical examiners, selection of only
                                          cadavers and surgical patients.
Sampled population—includes a subset of only
   surgical patients and persons who died  in FY76.
                                       Subsampling of surgical patients and cadavers
                                          by cooperating professionals.
Sample.
       Figure 2.1.  Sampling frame and selection procedures for Mirex Special Study.


Source:  Based on information contained in Kutz and Strassman undated, and Rand McNally and Co., 1974.

'Population values based on 1970 census data.
                                             -7-

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2.2.2.    Strata
     In FY70-FY72,  the contiguous  48  states were  stratified  by Census
Region.  Beginning in FY73, the strata were changed to Census Divisions.
In the  earlier  period,  the number of sites selected within each stratum
was determined  by  its  population as given in the 1960 Census.   In FY73,
the allocations were revised based on 1970 Census data.
2.2.3.    Eligible Places
     In FY70-72, the eligible places were cities with populations greater
than 25,000 persons  based on the 1960 Census.  In FY73-76, the eligible
places were cities greater than 25,000 based on the 1970 Census.  Sample
sites were selected in FY73 and followed through FY76.  The sample sites
were  independently  selected from each stratum  with probability propor-
tional  to size  of  the  city.   This was  done  by  listing the  sites  in
random order along with their cumulative population totals.  An interval
for each stratum was calculated by dividing the total population for all
sites  listed  by the number  of  sites  to be selected  in  the  stratum.   A
random number was  obtained between zero and  the  length  of the interval
to give  a starting  point.   The  sites  were  selected  by matching their
cumulative totals  with the  starting  point or  integer multiples  of the
interval plus the starting point.
2.2.4.    Pathologists and Medical Examiners
     The subsampling within each site was done by a cooperating patholo-
gist  or  medical examiner.   When no cooperative pathologist or medical
examiner  could  be  found  in a  selected  site,  an  alternate   site  was
selected.   Alternate  sites were  chosen  by position  in  the listing  of
eligible sites with respect to the nonrespondent site.  The first alter-
nate was  the  site  immediately  below the originally  selected  site,  the
second alternate the one  immediately  above, the third alternate was the
second site following,  and so on.
2.2.5.    Quotas
     Each site was assigned a quota based on the demographic characteris-
tics of  age,  sex, and  race.   The ages were  grouped  into  three ranges:
0-14,   15-44,  and greater  than  44.   The races were  classified  as white
and nonwhite.   The  quotas  for  FY70-FY72  were based on the  national
demographic characteristics  according  to  the 1960 Census.  The  quotas
for FY73-FY76 were determined by the appropriate demographic characteris-
tics for each Census Division,  based on the 1970 Census.   The MSS quotas
are given in Appendix F.
                                 -8-

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     There was no  probability structure below the sample city level for
obtaining the participants  in the survey.  The hospitals, pathologists,
and medical  examiners  were  selected subjectively.  Also, the samples of
cadavers and surgical patients were selected subjectively by the cooper-
ating professionals.   Appendix  G contains a copy of the EPA letter sent
to  each  cooperating professional  stating the guidelines  for screening
specimens and the types of individuals from whom tissue specimens should
not be  obtained  (for example, suspected  victims  of pesticide poisoning
and institutionalized patients).
2.3.      Selection Weight Construction
     In order to use the information obtained in the MSS to estimate the
level of  mirex concentration  in the population of RMA's  in the target
area and to account for disproportionate sampling rates, it is necessary
to  weight  the  original  values  before analysis.   This presents  some
problems, for  the nature of the selection of sites,  which includes at
some  points  purposive  selection  (subjective,  not based on  any  known
probability of selection), is incompatible with the formation of statis-
tically valid sampling weights.   A method of "quasi" weighting has been
devised and used for the weighted analyses.  A simple method of weighting
was chosen  to facilitate the  weighted analyses,  but  it  is  by no  means
necessarily  the  best  or  only way  to  weight the  data.  The  method of
weighting chosen  and  some  of that particular method's limitations are
described here.
     The first stage  selection frame,  consisting of 68  1974 RMA's from
the designated  mirex  counties  in  eight  southern States,  was  actually
split between two lists, which were considered separately in constructing
weights.   One list consisted of eight mirex area cities that were origi-
nally part of the NHMP, and the second list consisted of 60 sites (RMA's),
from which  the  supplementary  MSS sample was  drawn.   The  eight cities
that  had  been part of  the  NHMP were included  with  certainty in the
sample.   These eight  cities  are in RMA's, but were not considered  among
the possible selections for the supplementary sample.
     Even if  one  assumes the  selection process within  sample  sites is
approximately random, the sample design of the MSS does not assign  equal
"probabilities"  of selection  to  all elements (cadavers and surgical pa-
                                 -9-

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tients) in the sample.  This introduces the possibility of sampling bias
in  calculating population  estimates.   Bias  refers  to  the  difference
between an estimated population value and the true population value.  It
can  occur as  a  result  of  sampling error or  measurement error,  or a
combination of both.   To facilitate bias reduction in this situation, a
sample  weight  for  each observation  was  calculated  that attempts  to
reflect its approximate  probability of selection.  Including weights in
the analysis should reduce bias in estimating means or proportions.  For
probability sampling this results  in strictly unbiased  estimators for
such  statistics   as  means,  proportions, and  totals.    In  the following
paragraphs, procedures  are  given  for computing  weights for  the MSS.
Again, note that true sampling weights cannot be calculated because some
stages of selection involve non-probability sampling.
     The population from which tissue specimens might be obtained is not
actually all people  residing in a  selected RMA;  only surgical patients
or individuals who die from certain  causes at  the selected hospital in
any sample RMA  have a chance of being selected.   The surgical patients
and  cadavers  that are  available  to  the  selected pathologist  may not
necessarily be residents of the RMA that they are purported to represent,
because individuals  may travel  to  another city  for  medical  treatment.
The possibility  of medical  care migration is  particularly problematic
for RMA's  that  are located on or near the  borders of mirex areas (such
as Dallas).
     To estimate  the probability of a  given  individual  being selected
within a sample site,  one might use the number of pathologists and hos-
pitals, so that the  probability of selecting any one  pathologist at any
hospital in an RMA could be estimated.  Then the population of suitable
surgical patients  and cadavers to which the pathologist had access would
need to be estimated,  so  that  a probability of  selection of a tissue
specimen by that pathologist could be estimated.  Even with this type of
information,  the  estimates of  selection probability would be  very rough
because the pathologists and tissue  specimens  in the MSS were  not select-
ed in  any random  or systematic method but by  purposive  selection.   At
this time,  there   is no  reasonable  adjustment that can be made  to take
the above  facts into consideration.  Hence, equal probability of selec-
tion  is  assumed  for  the  within-site  stage  of sampling.  This  method
involves dividing  the  number of specimens  received by the population of
the RMA.
                                 -10-

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      The probability  of an  RMA  being selected in the MSS  is dependent
 upon the study  for which the site was  originally  selected.   The selec-
 tion  criteria  for  the  sites that were already part  of the NHMP  were
 different  from  those  for  the  sites  that were  sampled  specifically for
 the MSS.
      The probability  of selection of  a site at the first  stage  is the
 number of  selections  made  divided by the number of possible selections;
 this is the  number of selected RMA's divided by  the number of RMA's on
 the frame,  or

      p       ( 1st stage }   _ number (n) of sample  RMA's
              (selection/     number (N) of RMA'S on the iist
      For each  of the eight RMA's  that  are part of the NHMP,  the prob-
 ability of  selection  is  equal to 8/8,  or  a  probability of selection of
 one.   These eight  sites were  included with  certainty  in the  sample
 because data collection systems already existed at these locations.  For
 RMA's that  were  selected as part of the supplementary or additional MSS
 sample, the probability  of  selection is 32/60, or 0.53.  The supplemen-
 tary  sites  were  selected by  simple random sampling,  which  does  not
 consider the size of the population of the  RMA's in the selection process.
 When equal selection probability is used at the first stage and approxi-
 mately equal sample sizes are selected from each of the primary sampling
 units, this can result in oversampling small RMA's and cause underrepre-
 sentation of RMA's that have large populations.
      Weighting the observations within the  sample site is used  to adjust
 for this.   The weight of a given  sampling unit is the  inverse  of the
 "quasi" sampling  rate.   Hence,  the  weight  for  a given  observation  is
c ,   . .      ...   number of RMA's on list         population of RMA
Selection weight = - r - j - ; — srrn -  x — *-r£ - j - : -
             °     number of sample RMA s        number of specimens
                                                   selected in RMA

      In  this   study,  as  noted  previously, some  of  the sample  sites
 selected did not  submit  valid tissue samples  for  analysis.  To  compen-
 sate for  this  nonresponse, the  inverse of  the proportion  of  selected
 sample sites that responded was used to  adjust the weights.  For example,
                                  -11-

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data were submitted from five of the eight NHMP sites (5/8 or 62.5 percent
responded), which  results  in a nonresponse adjustment factor of 1.6 for
NHMP sites.  The nonresponse adjustment for supplementary RMA's is 1.23,
the inverse of  26/32.   This factor, multiplied by  the  selection weight
for an  observation,  produces  a weight adjusted for  nonresponse at the
first stage level.  This technique is designed to reduce bias that might
result  from  this nonresponse.   There  was no  information  upon which to
base any adjustments for the sampling bias which might occur as a result
of  the  subjective selection of tissue specimens within selected sites.
                                 -12-

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3.        EVALUATION OF CHEMICAL ANALYSIS
3.1.      Introduction
     The objective of  this  portion of the study  is  to assess the reli-
ability of  the  results obtained from the chemical analytical procedures
employed in the MSS.   The analysis of adipose tissue specimens for mirex
was  carried out  by  the  Michigan Department  of Public  Health  (MDPH).
     The analytical procedure used for the determination of mirex is de-
scribed  in the  EPA  Pesticides Methods  Manual (USEPA  1974).   Specific
details  regarding the  collection,  storage,  and shipping  of  specimens
were described  in the  NHMP study report for mirex  (Kutz and Strassman
undated).  A number  of raw mirex  chromatograms,  supplied by MDPH,  were
examined in sufficient detail  to  allow for a meaningful assessment of
the quality of reported mirex levels.
3.2.      Discussion
     The method  used for  the determination of mirex levels was based on
the  use of  an  external  standard.   Reference  standards  were injected
before, during,  and  at the end of each mirex specimen group.  The stan-
dard  consisted,  usually,  of a mixture  of known amounts of  mirex  and
Aroclor 1260.   This mixture served not only for purposes of quantitation,
but also provided  a  constant check on the degree of separation between
mirex and  a late-eluting  Aroclor  peak.  This peak  represents  an inter-
ference found in most  tissue specimens due to the  ubiquitous  nature of
the Aroclors.   In an effort to maximize the separation of the two peaks,
the  gas chromatographic  procedure was modified,  and the  analysis  was
conducted  at   a   temperature  slightly  below  that  recommended  in  the
Pesticides  Manual.   This  procedure  was approved by memo  (Appendix H)
prior to chemical analysis.  Chromatograms of Aroclor 1260, mirex,  and a
mixture of 1260/mirex are depicted in Figures 3.1 through 3.3.   Baseline
separation  was  achieved  for  mirex and the Aroclor  1260  peak,  and  this
separation was maintained throughout the analysis period covered by the
chromatograms  examined (May 1976-November 1977).
     The same quantity of Aroclor 1260 and mirex was  injected for each
check.   Thus,  a measure  of the reproducibility  of injection  could be
determined by measuring detector  response (peak height) for these stan-
dards.   A  check  of 17  such injections showed acceptably close agreement
(differences  <  10 percent)  between  injections  for  a  given  specimen
                                 -13-

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group.  This agreement and the reproducible retention times observed for
the compounds over a period of several months are indicative of a stable
analytical system.
     For  a significant  number  of  chromatograms,  an  interference  peak
other than Aroclor  1260  was noted.  Of some 50 chromatograms from which
a  quantitative  assessment  of mirex was  made, approximately  half  (26)
showed  mirex. peak   interference.   The  degree  of  interference  varied
(Figures 3.4 through 3.6) but was not so severe as to prevent estimation
of levels  of target compound.
     Of  the  chromatograms   examined,  only  one  blank  and two  control
specimens  were   included.    These  specimens  were  not  described so  no
significance could be  attached to them, except that the blank chroraato-
gram was "clean" in the area of interest.
     To assess  the  reliability of the chromatographic and, to a limited
extent, the quantitative procedures  used, all mirex peaks were measured
(peak  heights)  and  the  results  compared with  the peak  height values
denoted on the  chromatograms.   Comparisons were also made of the amount
of mirex as calculated from the MDPH peak height values and as determined
by  the  measurements.  These data are  shown in Table  3.1.   As  can  be
seen, the  results are  consistent with average absolute errors and stan-
dard errors (A%,  see Table  3.1) of 9.2  + 2.1% for peak height measure-
ments, and 8.1  +  1.2% for calculated amounts.  A check on the interper-
sonal variability was determined by independent measurements and calcula-
tions of  the  same parameters,  i.e.,  peak  height  and  amount  of mirex.
Some 10  percent of  the  measured chromatograms were  replicated  in  this
manner.   These  results are  shown in Table 3.2.  Again the data are  very
consistent, with the average absolute error and standard error calculated
at 3.0 + 1.0 %.   Thus,  the measurement of mirex peaks and the calculation
of raw mirex amounts were straightforward, and, at least for the chroma-
tograms examined,  no gross errors (inaccurate measurement, faulty calcu-
lation,  peak assignment error) were evident.
     As no completely adequate method exists for the quantitative statis-
tical treatment  of  "trace"  levels  of  compound,  an  attempt was  made  to
ascertain  the minimum  detectable quantity (MDQ)  of mirex as analyzed by
the MDPH.   Since  the  MDQ was not available,  an approximation was  made
adopting the  usual  assumption  of  MDQ =  3  (signal/  noise).   Since two
                                 -14-

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Figure 3.1.  Gas chromatogram - Aroclor 1260 standard.

-------
"(*>
>\
                  Figure  3.2.   Gas chromatograra - tnlrex standard.   Conditions as in Figure 3.1.

-------
Figure 3.3.  Gas chromatogram - mixture of Aroclor 1260  and mirex
             standards.   Conditions as in  Figure  3.1 except chart
             speed is 0.5X.
                                    -17-

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oo
                    Figure  3.4.   Gas chromatogram - mirex containing specimen (moderate level)
                                  with interference peak (moderate level).  Conditions
                                  as in Figure 3.1.

-------
I
H1
          Figure  3.5.  Gas chromatogram  - mirex  containing specimen (low level)  with interference peak

                       (low level).  Conditions  as  in  Figure 3.1.

-------
I
to
                u~~n
                Figure  3.6.  Gas  chromatogram - mirex  containing specimen (moderate level)  with

                             interference  (high level).  Conditions as in Figure 3.1.

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detection systems were used in this study, MDQs were determined for each
at the beginning  of the analytical runs (May 1976) and again at the end
(November 1977).  For  system  one,  the MDQ's were 16 pg at the beginning
and 20 pg  at the end of the  study;  for system two, the MDQ's were 9 pg
and 12  pg at  the beginning  and  end, respectively.   The similarity of
these values  bespeaks  an extremely stable  analytical  system,  with more
than  adequate  sensitivity for these  types  of analyses.   Unfortunately,
these values could not be translated into the concentration values (ppm)
reported on  the  data file.   This was due to the inability to relate the
specimen identifiers (specimen numbers) on the sample chromatograms with
the identifiers   (patient  numbers) reported  on the  raw data  file.  In
addition, information  was  not available  regarding  the exact analytical
procedures followed (e.g.,  analyte solution  volume,  dilution factors);
thus,  specimen dilution factors  could not be ascertained.  The absolute
amounts  of  mirex,  as   shown  on  most  of  the chroma tograms,  could not,
therefore, be converted to ppm fat.
     Although  a  check  on the reliability  of the  final  reported mirex
concentration levels could not be made, the raw data indicate that sound
analytical quantitation procedures were followed, and the results are of
acceptable quality.   Further  assurance  of  the  quality  of the  data  is
provided  by   independent   confirmation   of  the  mirex  levels  using,
primarily,  gas  chromatography/mass  spectrometry  (GC/MS).   Results  of
analyses of some 23 specimens  (Appendix I) showed good agreement between
the values reported by MDPH and those reported by the confirming labora-
tories.
     The  quality of  the raw data,   the  results of  the confirmational
analyses, and  the  stability of the analytical system  are taken as good
indicators of  reliable  and  accurate results.  Although  every  aspect of
the analysis could  not  be  checked (for example,  calculations leading to
concentration values),  no errors  were noted from the available chemical
analytical data.   There is no  indication that the information as reported
on the raw data file is suspect.
                                 -21-

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Table 3.1.   Comparison of Mirex  Peak Heights  (mm)  and Calculated
            Amounts  (pg)  as  Determined  by Michigan Department  of
            Public Health and Quality Control Checks
Specimen
1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23
24
25
26
27
28
29
30
31
32
33
34
35
36
37
* A% =
Ht (MDPH)
17
108
19
54
58
43
13
75
75
20
20
78
15
98
28
0
0
0
0
15.5
32.5
118
6.5
22
0
32
12
60
21
71
124
56
107
15
18
12
54
X (QCC)
Ht (QCC)
16.5
113.0
20.5
57.0
77.0
43.5
13.0
76.5
82.0
20.0
20.0
81.5
15.0
99.5
33.0
0
0
0
0
15.0
32.5
119.0
6.5
23.5
0
32.5
16.5
67.0
23.0
80.0
126.5
60.0
120.0
11.0
17.5
17.0
70.5
- X (MDPH)
A%*
-2.9
4.6
7.9
5.6
32.8
1.2
0
2.0
9.3
0
0
4.5
0
1.5
17.9
-
-
-
-
-3.2
0
0.8
0
6.8
-
1.6
37.5
11.7
9.5
12.7
2.0
7.1
12.4
-26.7
- 2.8
41.7
30.6
nnm
Amt (MPDH)
187
2967
284
?
X
X
236
X
986
213
274
829
221
2020
412
0
0
0
0
470
198
2450
198
224
0
327
102
254
244
602
1442
577
973
7
?
120
378

Amt (QCC)
159
2729
271
1326
488
423
236
1855
982
185
240
755
190
2020
418
0
0
0
0
458
198
2466
198
209
0
289
115
205
217
557
1193
517
906
282
280
142
400

A%*
-15.0
- 8.0
- 4.6
-
-
-
0
-
- 0.4
-13.1
-12.4
- 8.9
-14.0
0.5
2.5
-
-
-
-
- 2.6
0
0.7
0
- 6.7
-
-11.6
12.7
-19.5
-11.1
- 7.5
-17.3
-10.4
- 6.9
-
-
18.3
5.8

             X (MDPH)

                            -22-

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Table 3.2.  Interperson Comparison of Mirex Peak Height
            Measurements
                         Peak height (mm)
Specimen             A              B              A %
   1                85.0           82.0            3.7

   2                21.0           20.0            5.0

   3                20.0           20.0            0

   4                79.5           81.5           -2.5

   5                22.5           23.0           -2.2

   6                25.5           23.5            8.5

   7                60.0           60.0            0

   8                29.0           29.0           -1.7
                            -23-

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4.        UNWEIGHTED ANALYSIS
4.1.      Data Description
     The  MSS  data  consisted  of  664 observations  from  31  responding
sites.  40 observations were excluded from analysis:  34 records were of
specimens  collected outside  the reference  time  period,  and  the lipid
extractable  amount for 6 observations was  less  than 10 percent.   There
were  no  data  exclusions  on the basis  of  inadequate  chemical analysis
confidence codes.   After  exclusions,  there were 624 observations avail-
able for statistical analysis.
     In Chapter  2,  there  is brief mention of desired specimen quotas by
age,  race, and sex (Appendix F).  These quotas guided the field contact
in  submitting  specimens  from a range of individuals.  It  should be kept
in  mind that representativeness  for factors of occupation and length of
residence in an area is not accomplished through balancing on age, race,
and  sex  information.   The  quotas  were  established in  an attempt  to
obtain information that would reflect the age, race, and sex distribution
of  the living population.
     Tissue specimens that fit the quota specifications were referred to
as  design  specimens; tissue  specimens  received in  excess of  the quota
guidelines were  called  surplus  specimens.   None  of  the sites  filled
their quota  of 27  design specimens  even though 6  of  the  31  responding
sites  submitted  27  or more  tissue  specimens.   There were 479  design
specimens and 145 surplus specimens.  There is no difference in methodol-
ogy of selection or collection between the design and surplus specimens;
the designation was made in order of date of receipt and processing of a
valid  specimen as  the study  year progressed.   There  seems  to be  no
obvious reason to  exclude the surplus tissue specimens (23.2 percent of
the data)  from weighted analysis  and probably not from unweighted analy-
sis because design quotas were never satisfied.
     Table 4.1 contains  classifications  for all tissue specimens within
Census Divisions by age,  race,  and sex.  The  desired  quotas  for racial
representation were  met  reasonably well  within the South Atlantic and
West South Central  Census Divisions and almost exactly  within the  East
South Central Census Division.  The Census Division level  desired distri-
bution by  age group was  not met;  the  0-14 age  group  was consistently
underrepresented in all three divisions.   This is to be expected because
                                 -24-

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children do not die or undergo surgery in proportion to their representa-
tion in the population.  The actual distribution of specimens classified
by  sex was  roughly  in keeping  with the desired  quotas on  the  Census
Division level.
     For the various  sample sites the number of valid tissue specimens
submitted ranged from 1 to 37.  Dallas, Texas, one of the NHMP sites and
the  largest  RMA in  the  MSS  (2,455,000  people),  was  the  location that
contributed only one  tissue specimen.   Dallas presents further analysis
problems because  of its location, for  it  falls on the  edge  of  a mirex
area and part  of  the defined RMA  including  Dallas  falls outside of the
mirex area boundary.  Because Dallas is the largest city in that part of
Texas  (see maps, Appendix  A), the population that relies on the medical
facilities  in  Dallas  extends far beyond the  boundaries  of  the mirex
counties.  Houston and San Antonio are similarly situated in both geogra-
phical and medical  terms.   The locations of  other  RMA's are subject to
the  same cautions  in interpreting the residence of the individuals from
whom adipose tissue  specimens were obtained.  Some sites,  such as those
in Louisiana, are clearly located in a heavily fire ant-infested region,
and for these,  little ambiguity exists about the potential mirex exposure
of the population.
     In future  investigations  it would be useful to obtain the zip code
of the home  address  of the patients from whom  the tissue specimens are
obtained so  that  residence  in a mirex area  can be verified.   However,
this still would not give any indication of the length of time an indivi-
dual resided in an area  exposed to mirex.   Level of exposure and inten-
sity of  application  of mirex to an  area  are also not  known  but  are of
interest.
4.2.      Data  Analysis
4.2.1.     Data  Distribution
     In the  interpretation of estimates  and statistical  tests  in this
section,  which  are based  on unweighted analyses of MSS data, it must be
recognized that at least two categories of individuals are not as preva-
lent (underrepresented) in  the sample  as in  the population.   These are
people under age 15  and  residents of the larger RMA's.  In light of the
correlations between geographic location and mirex positives, the latter
imbalance  may   cause  unweighted  analysis to be  seriously biased  for
                                 -25-

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         Table 4.1  Specimens Collected for Each Census Division
                           By Age, Race, and Sex*
East South Central:  Alabama and Mississippi

                            Number of Specimens
                     Caucasian
Non-Caucasian
Age Group
  0-14
 15-44
   >45
Male
5
22
36
63
Female
7
29
43
79
                        142
Male
1
6
7
14
Female
2
5
12
19
                       Total
                         15
                         62
                         98
      33
175
          desired non-Caucasian quota = 5/27 = 18.5%
          actual non-Caucasian representation = 33/175 = 18.9%
South Atlantic:  Florida, Georgia, North Carolina, and South Carolina
Number of
Caucasian
Age Group
0-14
15-44
>45
Male
13
35
55
103
Female
8
29
52
89
Specimens
Non-Caucasian
Male
6
25
18
49
Female
10
11
20
41
Total
37
100
145
                        192
      90
282
          desired non-Caucasian quota = 6/27 = 22.2%
          actual non-Caucasian representation = 90/282 = 31.9%
West South Central:  Louisiana and Texas
                            Number of Specimens
                     Caucasian
Non-Caucasian
Age Group
  0-14
 15-44
   >45
Male
7
18
28
53
Female
9
34
41
84
Male
2
7
7
16
Female
0
8
6
14
                       Total
                         18
                         67
                         82
                        137
      30
167
          desired non-Caucasian quota = 4/27 = 14.8%
          actual non-Caucasian representation = 30/167 = 18.0%
      Based on the results of the MSS and information in Appendix F.

                                 -26-

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purposes of extending the results to all persons in the study population.
The weighted analyses  in the following chapter should  reduce  this risk
of bias.
     In examining the data, it is important to consider the distribution
of mirex levels before choosing summary statistics or conducting descrip-
tive  analyses.   Of the  624  specimens,  141  (22.6 percent)  contained
detectable amounts of mirex.  Eighteen (12.8 percent) of the 141 detect-
able values were trace quantities of mirex, present but not in sufficient
quantity  to  be  accurately measured  (see  discussion  in  section 3.2).
These  trace  quantities  were  included  in analyses where presence  or
absence  of mirex  was  measured  but not  included in  those statistical
analyses where a specific numerical value was required.
     The two histograms in Figure 4.1 illustrate the distribution of the
frequency  of  mirex residue  values  (in parts  per million)  for all 624
specimens and for the 123 specimens for which there were definite measur-
able quantities.   It is  obvious  that the  levels  of mirex in the sample
do not  follow a  normal  distribution  (example  at the  bottom  of Figure
4.1),  even when  the  501  zero  (nondetectable)  and  trace values  are
excluded.  The skewing of  the distribution to  the  right  indicates that
the residue amounts  follow a lognormal or exponential  distribution, and
that a  transformation  of the data might yield  a  distribution  of values
that would be  more appropriate for meeting the assumption of  normality
underlying many  statistical tests.   Figure 4.2 contains  a histogram of
the  result  of  a  natural log  (log  )  logarithmic  transformation  of the
measurable positive  raw  (wet  weight)  residue  amounts.  It can  be seen
that the  distribution  of  the  123  transformed  values  in  Figure 4.2 is
much closer to normal than the distribution of the same 123 untransformed
values  in  Figure  4.1.    Log   is  usually  used  for  biological  data
transformation.
     It  should  be noted that  the  actual  distribution of  mirex levels
contained in human adipose tissues probably consists of fewer true zeros
than  current   analytical  techniques  indicate.   That   is,  if  it  were
possible to analyze the exact same 624 specimens using  improved technol-
ogy,   there would  probably be  fewer zeros  reported and  more positive
detections of  some minute  amounts  of  mirex.   The  skewing to  the right
would still  exist, but  the distribution of  values would  more closely
                                 -27-

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          500 -
number of
specimens 400 -

          300 -

          200 -

          100 -
                         n = 624 sample values:
                             zeros,  traces,  and
                             quantifiable positive
                             values
               zeros and traces '    0.5      1.0

                                Residue Amount, ppm
                        1.5
 2.0
  2.5
90 •
80 •
70 -
number of
specimens 60 •
50 -
40 •
30 -
20 -
10 -









n = 123 quantifia
positive valu




.A. 	 .
                 <0.4
0.8     1.6     2.4     3.2

  Residue Amount, ppm
4.0
4.8
                                        68% of
                                        values
                                     normal curve
  Figure 4.1  Frequency distribution for raw values of residue amount
*Based on results of Mirex Special Study, FY76.
                                    -28-

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resemble a true  continuous  distribution if the presence of mirex in any
quantity, however small, could be measured.
     The average minimum detectable quantity (using techniques available
in 1975-1977) estimated for mirex in human adipose tissues is within the
range  0.05  to  0.10 ppm.   However, no  specific numerical  value  could
reasonably be substituted  or inserted  for  the 18  trace observations.
The  483  zero values  could  be transformed  to a logarithmic  scale  if a
constant term was  added to  all values before  transformation.   This was
not done for the MSS because there are so many nondetectable values that
means and standard  deviations of specific levels of  mirex  residues for
the  entire  sample  would  provide little information.  Instead, it was
decided  to  look  at the proportion  of  detectable versus nondetectable
values and at the quantifiable residue  amounts.  From  this information
estimates can be made  of  the levels  of definitely  quantifiable  mirex
residues  in  the  proportion  of  the  sample  that  has  some  discernible
quantity of mirex in their adipose tissues.
     Both the  proportion of  positive  values and the geometric mean of
the  transformed  quantifiable data  were  used  as  summary  statistics.
Statistical tests are based on the simple arithmetic mean of the logari-
thmically transformed  quantifiable  data.  Summary statistics  are  given
in terms of  the  geometric  mean,  which is an appropriate summary statis-
tic for  logarithmic  data.   A geometric mean is the antilogarithm of the
arithmetic mean of  logarithms.   It  is a good estimator of the median of
the underlying distribution of this data (Hartwell et al.  1979).
     It has been specified by EPA that part of the analysis in this task
is to be carried out on the raw residue amount divided by the proportion
lipid  extractable  material  (LEM) in  the  specimen.   This  quantity is
indicated by  the  term  Y in the following pages.  The natural log,  log ,
was  obtained  for all  123  quantifiable  positive  values of  Y.   The two
histograms in Figure 4.3  are the distributions  of  Y  and log  Y.   It
should be  noted here  that  the adjustment  of wet weight values by the
proportion of LEM  does  not  affect the proportion of positive detections
of mirex residues  in the  sample.   Presence or absence of mirex is  inde-
pendent of the LEM adjustment.
                                 -29-

-------
60
50
number of
specimens 40
30
20
10
•
•
•













__, 	 ,__., ^ 1 , _
                  -4
-3
-2
-1
                              log  mirex residue amounts
Figure 4.2.  Frequency distribution for transformed values of wet
                                 *
             weight mirex residue
 #
  Based on results of Mirex Special Study, FY76.
                               -30-

-------



number of
specimens


80 -
70 -
60 -
50' -
40 -
30 -
20 -
10 -

















AAA . . 1 . 1 . 1 i
<0.5 "'123456
Y
50
40
30
number of
Specimens 20
i n
iU
.
•

'












                         -4
-3
                        -2     -1     0     123


                           Y


Y = Mirex Residue Amount (ppm)/% Lipid Extractible Material
Figure 4.3   Frequency distributions of lipid adjusted mirex residue amounts
             and transformed values (n=123 quantifiable positives)*

     *
      Based on results of Mirex Special Study, FY 76.
                                    -31-

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4.2.2.    Proportions of Positive Values
     In Tables 4.2 and 4.3 are some simple classifications of the number
of  detectable and  nondetectable values  by demographic  and geographic
categories.   In  Table  4.2,  which is a  summary by State, the two States
with the  largest percent of detectable mirex  levels are Mississippi and
Louisiana,  46.3  and 35.7  percent positive, respectively.   Georgia has
the third largest percentage of detectable mirex levels, at 20.9 percent.
The percentage of detectable mirex values drops  to  less than 8 percent
for  the  5  remaining  States.   There  were no positive values  for the
specimens submitted from North Carolina and Texas.
     This  information  by State  suggests  a possible  connection between
residence  in  a   widespread  mirex-treated  area  with  detectable  mirex
levels in human adipose tissue.  This is borne out by the highly signifi-
cant results of a chi-square test on the zero  detectable/positive values
by  State  in Table  4.4.   The empty cells  for  positive  values for Texas
and North Carolina  make the chi-square test results  less  reliable than
if  there  were  some  positive values for these  states.  However, the test
can still be used to infer that there are significant differences in the
percent of positive mirex residues detected by State.
     Census Division was the only other variable investigated that shows
significant results  in  the  chi-square test.  Race, age, and sex did not
show  significant  differences   in the  percent  positive mirex  residue
values for the chi-square test results in Table 4.4.
     The  information  in Table 4.3, which  is a three-way classification
by  race,  age,  and detectable mirex residues,  is  less  easily summarized
than the data in the two-way classification in Table 4.2.  When consider-
ing  additional  categories,  it becomes  necessary to  consider possible
interactions between variables as well as simple main effects.  This can
be  done  by computing  an analysis of  variance (ANOVA)  or  a regression
equation.   A model such as the following can be used.
               P. ....   = |J + A. + S. + R.  + L0 + e. ., „
                         r    i    j    k    8,    ijk£m
where
          P. ....  =  mirex level in tissue for the m   individual, the
                                                                 '
                    3,   location, in the (ijk) age-race-sex group;
                 =  mean mirex level;
                                 -32-

-------
              A. =  age effect for the i   age group;
              S. =  sex effect for the j   sex group;
               J
              R, =  race effect for the k   race group;
               1C
              I- =  location effect of the &   location;
          £..,,,  =  random error.
           ijkJtrn
     In the above model, testing for age, sex, race, and location effects
corresponds to testing the equality of the A., S., R, ,  and L0.  Standard
                                            1   J   K       *
statistical computer  software  was  used to carry out these tests for un-
weighted data, and specialized software is available at RTI for carrying
out the analyses  for  weighted data (see Chapter 5).  A model similar to
the above  is  used for testing the proportion of positive values and the
arithmetic means  of  the positive  values for  mirex residues  found in
human tissue.
     A  regression model was  tested for the main effects  of race,  age,
sex, and  location,  with location being alternately  defined  as  State or
Census  Division.   Then the  model  was expanded  to  include all  possible
interaction terms.  The dependent variable for  this model was  presence
or absence of mirex, indicated as 0 or 1 in the model.   It is recognized
that log linear models are generally more appropriate than linear regres-
sion models for binomial  (0,1) dependent variables.  In the case of the
MSS data,  there  are  so  few specimens in some of the  subgroups (cells)
that it is necessary  to combine, or collapse, across subgroups  to avoid
the problem of  empty  cells  in the analysis.   As illustration, the vari-
able age  has  three subgroups,  which  could  be  collapsed  into  two  sub-
groups or  into  one  group,  which would then  involve simply dropping age
from the analysis.  This collapsing would result in positive proportions
of  presence  or  absence of  mirex  that  could then be analyzed  by log
linear  analysis.   This defeats  the purpose  of  the analysis;  the  sub-
groups that could be  collapsed are the ones for which bias reduction is
sought and for which adjustment is being made.
     The robustness of  the  regression technique should hold up  in light
of  the  overall  proportion   of  positives  (22.6%)  detected for  the MSS
sample.   This is  based on the tendency of the  binomial distribution to
approach  approximate   normality  for  measures of  central tendency for
                                 -33-

-------
 Table 4.2.  Detection of Mirex Residue by State:   Number of   j
             Specimens with Positive and Zero Detectable Levels
State/number of responding RMA's
Number of Specimens

Alabama (3)
Florida (6)
Georgia (5)
Louisiana (5)
Mississippi (6)
North Carolina (1)
Texas (3)
South Carolina (2)
Zero
Detectable
36
129
72
83
73
18
38
34
483
Positive
3
8
19
46
63
0
0
2
141
Total
39
137
91
129
136
18
38
36
624
Percent
Positive
7.7
5.8
20.9
35.7
46.3
0.0
0.0
5.6
22.6
Based on results of the Mirex Special Study,  FY 76.
                           -34-

-------
     Table 4.3.  Detection of Mirex Residue by Race and Age:  Number
                 of Specimens with Positive and Zero Detectable Levels*
Number of Specimens
Race
Caucasian


Non-Caucasian


Age
Group
0-14
15-44
>45
Total
0-14
15-44
>45
Zero
Detectable
42
128
202
372
19
44
48

Positive
7
39
53
151
2
18
22

Total
49
167
255
624
21
62
70

                         Total
111
 42
153
Total over race and age
483
141
624
                                 -35-

-------
     Table 4.4  Chi-Square Analysis Results for Zero Detectable/Positive
                Values:  Geographic and Demographic Variables*
2
Variable Number of % Positive within x df Significance
specimens each level level (p)**
AGE
0-14
15-44
>45
CENSUS DIVISION
East South Central
South Atlantic
West South Central
RACE
Caucasian
Non-Caucasian
SEX
Male
Female
STATE
Alabama
Florida
Georgia
Louisiana
Mississippi
North Carolina
South Carolina
Texas
70
229
325
175
282
167
471
153
298
326
39
137
91
129
136
18
36
38
12.7 4.53 2 0.103
24.5
23.1
37.7 49.65 2 0.0001
10.3
27.5
21.0 2.73 1 0.098
27.5
24.2 0.80 1 0.371
21.2
7.7 105.8 7 0.0001***
5.8
20.9
35 . 7
46.3
0.0
5.6
0.0
      Total number of specimens (n) = 624.
    VWr                    o
      Probability that a x  this large or larger might occur by chance, under
the assumption of no difference among categories.
   ***
      Apparently highly significant, but over 5% of the cells have expected counts
less than 5.   Sparse table indicates chi-square may not be a valid test.
                                      -36-

-------
large  samples   (Snedecor  and Cochran  1967).   Therefore, the  ANOVA,  or
regression, model  is  appropriate in this case for analysis of detection
of mirex residues.
     The results  of  this  analysis are summarized in Tables 4.5 and 4.6.
When State was  the location factor, the model gave a strong main effect
(p<0.0001) for location, even considering interaction effects.  Mississippi
and Louisiana are  the States which have significantly different propor-
tions of mirex detections from the remaining six States.  When interaction
terms were  not considered,  race and  sex were  both significant.   After
interaction  terms were  included in the  model, these  significant main
effects for  race  and sex disappeared.   When Census Division was used as
the location factor, Census Division  was highly significant (p<0.0001)
for the main effects of the all possible interaction terms model.  Race
was the only other significant effect in either model  involving Census
Division,   and  there  were no  significant  interaction terms.   The East
South Central Census  Division (which contains Mississippi) and the West
South Central Census  Division (containing Louisiana) have significantly
different proportions of positive mirex detections from the South Atlantic
Census Division.
     In addition  to  examining the significance levels of the individual
F ratios,  the fit of the model to the data overall should be considered.
              2
The value of R  is one indication of the appropriateness of the model to
                                                           2
describe the data.   In general,  the larger the value for R , the better
the model  is  as   a  description  of the  relationship of  the dependent
variable  (in this case,  presence or absence of mirex  residue in human
                                                                       2
tissue) to the  independent  factors (age, race,  sex,  and location).   R
can range from  zero  to one; a good fit is generally indicated by values
     2                                              2
for R  that  are greater than 0.4.  The  value  for  R  within a series of
models of the  same variable will always increase as more interaction or
                                                                2
quadratic terms  are added.   This  change  in the magnitude of  R  can be
used to determine  the relative contribution of  an  addition  or deletion
                                              2
of a term  to the  model.  In  this  case,  the R  values  for the 4 models
                                                                2
fitted are small;  the two models including State  have  higher R  values
than do the  models including Census Division as the geographic boundary
of interest.  This  is logical, as the Census  Division  boundaries group
States on a proximity basis that does not necessarily reflect concentrated
                                 -37-

-------
        Table 4.5  Regression Model for Race, Age, Sex, and State:*
                   Zero Detectable/Positive Residue Values
Source
df
F Value'
   Pr>F
Significance
Model             11
Error            612
Corrected Total  623
State
Race
Age
Sex
  7
  1
  2
  1
Model             73
Error            550
Corrected Total  623
              12.92
 18.89
    .48
    ,45
    ,64
               2.46
                    0.0001
   0.0001
   0.006
   NS
   0.057

   0.0001
                    0.188
                                     0.246
State
Race
Age
Sex
St x R
St x A
St x Sx
R x A
R x Sx
A x Sx
St x R x A
St x R x Sx
St x A x Sx
R x A x Sx
7
1
2
1
7
13
7
2
1
2
10
7
11
2
6.85
1.12
1.18
0.21
0.80
0.37
0.21
0.60
0.00
0.58
1.02
0.89
0.37
0.53
0.0001
NS
NS
NS
NS
NS
NS
NS
NS
NS
NS
NS
NS
NS
     *
      Calculations unweighted and ignoring design effect.

      Ratios of sampling variances used to test factor effects follow the F
distribution of the population variances are equal (null hypothesis).
     #*
       Probability that this might occur by chance under the assumption of
no difference among categories.
                                 -38-

-------
            Table 4.6  Regression Model for Race, Age, Sex, and Census
                       Division:  Zero Detectable/Positive Residue Values*
Source
df
F Value1
  Pr>F**
Significance
Model              6
Error            617
Corrected Total  623

Census Division    2
Race               1
Age                2
Sex                1
              11.45
              29.86
               8.05
               1.74
               2.54
                    0.0001
                    0.0001
                    0.005
                    NS
                    NS
                   0.100
Model
Error
Corrected Total
Census Division
Race
Age
Sex
CD x R
CD x A
CD x S
R x A
R x S
A x S
CD x R x A
CD x R x S
CD x A x S
R x A x S
CD x R x A x S
34
589
623
2
1
2
1
2
4
2
2
1
2
4
2
4
2
3
2.73


20.07
6.82
0.46
0.78
1.10
0.89 '
0.59
0.19
0.50
1.11
0.98
0.23
0.35
0.41
1.64
0.0001 0.136


0.0001
0.0009
NS
NS
NS
NS
NS
NS
NS
NS
NS
NS
NS
NS
NS
      Calculations unweighted and ignoring design effect.

      Ratios of sampling variances used to test factor effects follow the F
distribution if the population variances are equal (null hypothesis).

      Probability that this might occur by chance under the assumption of
no difference among categories.
                                   -39-

-------
mirex treatment area divisions.  If percentage of a State's area treated
by mirex were considered, it would be more reasonable to group Louisiana
and Mississippi together  for analysis than the Census Division grouping
of Louisiana and Texas.
4.2.3.    Quantifiable Positive Values
     The summary statistics for the 123 quantifiable positive values are
displayed in Tables  4.7  and 4.8.  The data  in these two tables are the
summary statistics for the  log  of both  the  raw residue amount and the
lipid extractable material (LEM) adjusted residue amount (Log  Y).   Both
of these values were analyzed in an unweighted regression analysis.  The
model for this  analysis  is  similar to the model used to detect differ-
ences  in  the presence or absence  of mirex  in  the entire  sample (624
observations).
     The  unweighted  regression  analysis did not show  any significant
differences either in  a  simple main effects  model  or in examination of
interaction terms  in  the model.   This indicates that  if  there are any
statistically significant differences  for the level of concentration of
mirex residues  among  the  categories of age,  race,  sex,  and location of
selection sites, these difference do not fit a linear model.
4.2.4.    Unweighted Analysis Conclusions
     For  this  section,  the  results  do  not  generalize  to the  target
population  but  reflect  only the  actual  sample  selected.   Within this
group,  it  is  observed that the most important  factor  in  an individual
showing mirex residues in adipose tissue is the location of the selection
site.   There  were  no significant  differences  found  among any of the
demographic and geographic  factors examined,  in  analysis  of  the 123
observations in this sample with quantifiable levels of mirex.
                                 -40-

-------
Table 4.7.  Summary Statistics for Quantifiable Positive Residue
            Values:  Geometric Means and Standard Errors*
Factor
All
AGE


CENSUS


RACE

SEX

STATE







Factor
Levels

0-14
15-44
>45
East South Central
South Atlantic
West South Central
Caucasian
Non-Caucasian
Male
Female
Alabama
Florida
Georgia
Louisiana
Mississippi
North Carolina
South Carolina
Texas
n
123
8
47
68
61
23
34
86
37
65
58
3
30
14
39
58
0
1
0
LOG Y**
Geometric Mean (ppm)
0.319
0.226
0.290
0.356
0.278
0.368
0.365
0.299
0.372
0.362
0.278
0.340
0.262
0.419
0.365
0.275
-
0.897
™
Standard Error
0.029
0.084
0.041
0.044
0.035
0.098
0.050
0.032
0.065
0.049
0.033
0.280
0.116
0.148
0.050
0.035
-
-
V
 Calculations unweighted and ignoring design effect.

**
  LEM adjusted values.
                                 -41-

-------
Table 4.8.  Summary Statistics for Quantifiable Positive Residue
            Values:  Geometric Means and Standard Errors*
Factor
All
AGE


CENSUS


RACE

SEX

STATE







Factor
Levels

0-14
15-44
>45
East South Central
South Atlantic
West South Central
Caucasian
Non-Caucasian
Male
Female
Alabama
Florida
Georgia
Louisiana
Mississippi
North Carolina
South Carolina
Texas
n
123
8
47
68
61
23
34
86
37
65
58
3
30
14
39
58
0
1
0
Log Residue Amount**
e
Geometric Mean (ppm)
0.220
0.117
0.205
0.250
0.190
0.237
0.267
0.211
0.245
0.239
0.201
0.290
0.177
0.269
0.267
0.186
-
0.420
™*
Standard Error
0.011
0.019
0.012
0.013
0.010
0.026
0.016
0.010
0.017
0.013
0.010
0.106
0.033
0.039
0.016
0.010
-
-
™
*
 Calculations unweighted and ignoring design effect,

  Wet weight residue values.
                                 -42-

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5.        WEIGHTED ANALYSIS
5.1.      Introduction
     The  analyses  presented  in  this  chapter are  weighted to  offset
disproportionate  sampling  rates and, hence, to  unbiasedly estimate for
the target population.  Quasi-selection weights were calculated for each
observation  and  used to  estimate  population  totals.   Several  software
programs  developed  specifically for weighted  analysis  of sample survey
data were used  to obtain the summary statistics and regression analyses
(Holt 1977, Shah 1979).
5.2.      Weight Formation
     Weights are numerical values that are used to adjust sample data to
estimate  information about the target  population.   Weights  were calcu-
lated  separately for  each (geographic)  site,  as described  in section
2.3.  The observations within  each site have the same  weight, with no
adjustments  for  age, race,  and sex distribution within the site.   The
quotas established for each site are intended to create a self-weighting
sample with  respect to  age,  race, and  sex  distribution.   These quotas
were based on  the demographic distribution of the  living population of
the Census Divisions in which the sample sites were located, rather than
on  the  distribution of  the  population within  the individual  sites.
These quotas  were not  achieved within  geographic  site, although  on  a
Census Division level  the  desired  proportions  of  race  and  sex  were
approximately met  (see Table  4.1).   The age  distribution  was  not met,
and this  undoubtedly reflects  the source of  the selection population;
the younger population is not proportionately represented in the segment
of the  population that  undergoes  surgery or dies in a  large hospital.
     After weights were  calculated and added to  the data file  for each
observation,  the  weighted  analyses were carried  out.   The  estimates of
the proportion  of  positive  mirex detections  are presented  in section
5.3.   The  estimates of  the  quantifiable mirex  residues  for the target
population are presented in section 5.4.
5.3.       Estimates of Positive Mirex Detection
     The  parameters  and  statistical tests  used are  the same  for the
weighted and unweighted analyses.   The use of weights to produce popula-
tion-based estimates  affects  the  calculation of  statistics  in  a manner
that allows  generalization of the statistics  to  the target population.
                                 -43-

-------
Otherwise,  the  interpretation of  the  statistics  is  similar  for  the
weighted and unweighted test results.
     A weighted chi-square test was used to examine the estimated propor-
tion  of  the  target  population  with detectable  mirex residues.   The
weighted chi-squares were produced by a weighted chi-square SAS procedure
(Barr  1979).   This produced an inflated  (artifically large)  statistic.
To adjust  for  this inflation before evaluating the resulting statistic,
the  computed chi-squares were multiplied by  the  sampling fraction and
then divided by the design effect (Fellegi 1980).  The sampling fraction
is the number of specimens in the sample divided by the target population
estimate.  In this case, the sampling fraction = 624/23,371,372 = 2.67 x
10   .   The design effect  (DEFF)  is  the  ratio of the  variance for the
design  employed to  the variance  that would  be  obtained  for  a simple
random  sample.   For the  MSS,  the DEFF  was 7.99.  This means  that the
effective sample size here was equivalent to 78 observations selected by
SRS.
     The results of this analysis are shown in Table 5.1.  State was the
only significant factor  for explaining differences in the proportion of
the  target  population  that  has  detectable  mirex  residue  in adipose
tissue.   Mississippi  was  the  State  that  had  a  statistically  signifi-
cantly larger proportion of positive mirex detection.
     A linearized weighted least squares analysis was used that incorpo-
rates  the sampling  structure into  the  regression  model  calculations
(Shah  1979).   This analysis will not compute  valid  F  statistics  (for
testing factor  effects  on a continuous variable) if the number of PSU's
is smaller than the combined levels of the factors in the model.  In the
case of a  model that  included State as the location factor, there are 8
levels  for the factor  State.   When  interaction  terms  are included  in
this model,  the sum  of levels in the  analysis  rapidly  increases beyond
the  limits imposed by the sampling structure.   Consequently,  only main
effects models involving State as the  location variable  were computed at
this time.
     The  interpretation  of the weighted  regression model  requires  some
caution.  The presence  of significant main effects can be  misleading in
some cases.  It is  important to consider possible interaction effects in
the model as  well.   Significant main effects in the presence of signifi-
                                 -44-

-------
     Table 5.1  Weighted Chi-Square Analysis  Results  for Zero Detectable/
                Positive Values:   Geographic  and Demographic Variables*
 Variable
Estimates
% Estimated Positive
     within each
df
Significance

AGE
0-14
15-44
>45
CENSUS DIVISION
East South Central
South Atlantic
West South Central
RACE
Caucasian
Non-Caucasian
SEX
Male
Female
STATE
Alabama
Florida
Georgia
Louisiana
Mississippi
North Carolina
South Carolina
Texas
of N.
i

6,606,385
7,529,303
9,235,645

1,727,307
9,726,438
11,917,587

18,517,425
4,853,897

8,653,061
14,718,264

503,079
2,477,302
5,642,299
3,229,595
1,224,229
210,692
1,396,152
8,687,994
level

1.6
11.3
15.4

37.6
13.3
3.6

9.8
11.5

16.1
6.7

4.6
5.4
19.6
13.4
51.1
0.0
3.9
0.0
level (p)**

2.72 • 2 0.257



2.6 2 0.273



0.04 1 . 0.844


1.8 1 0.180


32.8 7 0.0001***







      Estimate of N = 23,371,332 for the MSS target population.
refers to the subgroup i for a given variable.
                                            The ith subscript
     Probability that a X  this large or larger might occur by chance,  under
the assumption of no difference among categories.   Significance is  often
considered to be p < 0.05.
   ***
      Apparently highly significant,  but over 5% of the original cells have expected
counts less than 5.   Sparse table indicates chi-square may not be a valid test.
                                      -45-
                                         V

-------
            Table 5.2  Weighted Regression Model for Race, Age, Sex, and
                       Census Division:  Zero Detectable/Positive Residue
                       Values*
                Degrees of                  u.              Pr>F**
Source           freedom             F Value            Significance
Overall Model         6              9.30                 0.0001

Census Division       2              3.53                 0.042
Race                  1              0.14                 NS
Age                   2              1.93                 0.162
Sex                   1              3.03                 0.092

Overall Model        19             46.41                 0.0001
Census Division
Race
Age
Sex
CD x R
CD x A
CD x S
R x A
R x S
A x S
2
1
2
1
2
4
2
2
1
2
/*/>/*
0~UJL
t\ t\ 4\
***
***
0.26
1.13
3.45
0.28
0.11
1.22



NS
NS
0.044
NS
NS
NS
      Based on the results of the MSS FY76.
    JLJU
      Probability that this might occur by chance under the assumption of
no difference among categories.
      Not testable in the presence of interactions.

      Ratios of sampling variances used to test factor effects follow the F
distribution if the population variances are equal (null hypothesis).
                                  -46-

-------
               Table 5.3  Weighted Regression Model for Race, Age, Sex,
                          and State:  Zero Detectable/Positive Residue
                          Values*

Source
Overall Model
Total
State
Race
Age
Sex
Degrees of
freedom
11
30
7
1
2
1
f
F Value1
11.38

16.11
0.23
0.91
2.72
Pr>F**
Significance
0.0001

0.0001
NS
NS
0.109
     *
      Based on the results of the MSS FY76.
    j-jf
      Probability that this might occur by chance under the assumption of
no difference among categories.  Significance is often considered to be
p < 0.05.

      Ratios of sampling variances used to test factor effects follow the
F distribution if the population variances are equal (null hypothesis).
                                   -47-

-------
cant  interaction  terms  involving the same factors  that  are in the main
effects  can not be interpreted  independently  of  the interaction terms.
     The  results  for a  weighted regression analysis  for the estimated
presence  or absence of  mirex when  Census  Division is  the location of
interest  are in  Table  5.2.   A model  containing  all possible  two-way
interactions produced a  significant sex and Census Division interaction
relating  to  percent positive  (p<0.017).  In this interaction, there are
no  significant  differences  in  the East  South Central  or West  South
Central Census Divisions between the proportion of males and females who
have  detectable mirex  residues, but  there  is a  significantly higher
proportion  of  males than  females  with positive mirex detection in the
South Atlantic Census Division.
     The  model  containing State was limited  to  a  simple  main  effects
model, due  to  the restrictions noted above.  Results for this model are
shown in Table 5.3.  The significant main effect for State  (p<0.0001) in
this  analysis   confirms  the  results of the weighted  chi-square,  which
also  shows  that the States have significantly different proportions of
their population with positive mirex residues.   Mississippi is the State
that has a significantly greater proportion of positive mirex detections
than  the  seven  other States.   The main effect for sex in this model is
marginally significant (p£0.109).  There may be some interaction between
sex  and  State;  however, this  could not be tested  within  the  limits of
the software program used.
5.4.      Estimates of Quantifiable Positive Values
     The  estimates  of the geometric means and standard  errors  for the
log   of  the lipid  extractable material  (LEM)  adjusted  residue  amounts
and  the  the log  raw residue  amount are  in Tables  5.4  and 5.5.  These
variables  are  also  analyzed  by  the  weighted  regression  technique
described in section 5.2.
     The variable of  most  interest is the LEM adjusted  residue  amount;
three models involving this variable are listed in Table 5.6.  The first
two models  in the table are  main effects  models,  one  with State as the
location  factor and one with Census Division.   Neither model  has  any
significant  main  effects.   The  third  model in  Table  5.6  contains  all
possible  second order interactions.   There are marginally significant
interactions for  Census  Division by age group  (p<0.069)  and for Census
                                 -48-

-------
Division by  race  (p<0.0106).   This indicates that there  may be differ-
ences  in  levels of  mirex concentraction among  subgroups  of the target
population.  However,  these  differences  are not straight-forward in the
sense  that it  can  be assumed  that the  same  subgroup had  the highest
mirex  levels  in every Census Division.  For example,  Caucasians in the
East South Central  and West South  Central  Census  Divisions  have higher
levels  of mirex  concentrations than  do  non-Caucasians.   In  the South
Atlantic Census Division non-Caucasians have higher mirex residue levels
than do Caucasians.
     The same  three  models were analyzed for the unadjusted (wet weight
or raw) residue amount values.   These results are  in Table  5.7.  There
is a significant effect for State (p<0.0027) and for age group  (p<0.0138)
when  State is  the   location  tested.  In  the  second  order  interaction
model, with Census Division as the location factor, the interactions are
similar to  those obtained  when the LEM adjusted  residue  amount is the
dependent variable in the same model.
5.5    Weighted Analysis Conclusions
     The two  weighted analyses  are presented so that  inferences can be
made about  the population  of  the  mirex  treated areas.  The use of two
different analyses provides a check on the test results.
     The  chi-square  statistic is relatively assumption-free,  but it is
less  sensitive  to   differences  than  regression  analysis.   Regression
analysis,  in  turn,  requires  more assumptions to be met about the under-
lying  structure of  the data before it can  be  considered  an appropriate
test.
     It appears  that geographic location is an important variable for
explaining percentage presence  or absence  of  mirex  in  human adipose
tissue.  Mississippi  is  the  State  that shows the  largest  proportion of
presence  of  mirex  in human  adipose  tissue.  There  is less  clear cut
evidence that there are any large differences in level of residue amount
in  any particular category  studied,  although marginally  statistically
significant results  are found for several categories.
                                 -49-

-------
Table 5.4  Estimated Summary Statistics for Quantifiable Positive Residue Values:
           Weighted Geometric Means and Standard Errors*
Factor
All
AGE
CENSUS
RACE
SEX
STATE

Estimate of
population
Factor positives,
Levels N**
1
0-14
15-44
>45 1
East South Central
South Atlantic .
West South Central
Caucasian
Non-Caucasian
Male
Female
Alabama
Florida
Georgia
Louisiana
Mississippi
North Carolina
South Carolina
Texas
,919,220
88,474
504,045
,326,701
621,846
924,120
373,254
1,427,135
492,085
1,033,219
886,001
23,193
132,962
764,235
373,254
598,654
***
26,923
T^rA*
LOG Y - LEM adjusted Standard
Geometric Mean (ppm) Error
0.286
0.172
0.283
0.297
0.292
0.266
0.331
0.252
0.406
0.322
0.249
0.340
0.298
0.250
0.331
0.290
***
0.897
***
0.048
0.037
0.039
0.077
0.018
0.083
0.049
0.030
0.102
0.085
0.023
JUJt«JU
/\ f\ n
0.105
0.085
0.049
0.019
Jl~l~£.
***
***
  ***
 Based on the results of the MSS FY76.
IL
'*
 Estimate of total population for the mirex region = 23,371,372.


No information in sample on which to base estimate.
                                    -50-

-------
Table 5.5  Estimated Summary Statistics for Quantifiable Positive Residue Values:
           Weighted Geometric Means and Standard Errors*
Factor
All
AGE
CENSUS
RACE
SEX
STATE

Estimate of
Population
Factor positives Log Residue Amount
Levels N** Geometric Mean (ppm)

0-14
15-44
>45
East South Central
South Atlantic
West South Central
Caucasian
Non-Caucasian
Male
Female
Alabama
Florida
Georgia
Louisiana
Mississippi
North Carolina
South Carolina
Texas
1,919,220
88,474
504,045
1,326,701
621,846
924,120
373,254
1,427,135
492,085
1,033,219
886,001
23,193
132,962
764,235
373,254
598,654
***
26,923
***
0.197
0.095
0.192
0.209
0.189
0.187
0 . 244
0.184
0.240
0.208
0.186
0.290
0.190
0.181
0.244
0.185
***
0.420
***
Standard Error
0.010
0.009
0.012
0.017
0.003
0.017
0.014
0.011
0.020
0.018
0.006
-Hr*
0.030
0.018
0.014
0.003
***
***
***
  ***
 Based on the results of the MSS FY76.
i_
 Estimate of total population for the mirex region = 23,371,372.
                           c
No information in sample on which to base estimate.
                                  -51-

-------
     Table 5.6  Weighted Regression Model for Location, Age, Race, and
                Sex Versus Quantifiable Positive Residue Amounts of Mirex*
Source
Degrees of
 freedom
 F Value1
  Pr>F**
Significance
Overall Model***
                       7.42
                     0.0001
State
Age
Race
Sex

Overall Model
    5
    1
    1
    2
   1.34
   0.66
   1.65
   2.22
                       6.25
  NS
  NS
  NS
  0.1322

  0.006
Census Division
Age
Race
Sex
    2
    2
    1
    1
   0.85
   2.02
   2.25
   0.77
  NS
  0.1561
  0.1481
  NS
Overall Model***
   18
129409
  0.0001
Census Division
Age
Race
Sex
CD X A
CD X R
CD X S
A X R
A X S
R X S
2
2
1
1
3
2
2
2
2
1
Not Testable
Not Testable
Not Testable
Not Testable
2.72
5.63
0.43
0.55
0.50
2.17




0.0690
0.0106
NS
NS
NS
0.155
      Dependent variable in model is the log  LEM adjusted mirex residue amount.

      Ratios of sampling variances used to test factor effects follow the F
distribution if the population variances are equal (null hypothesis).
    **•
      Probability that this might occur by chance under the assumption of
no difference among categories.  Significance is often considered to be
represented by p £ 0.05.
   ***
      Full higher order interaction models not estimable.
                                  -52-

-------
          Table 5.7  Weighted Regression of Quantifiable Positive
                     Residue Amounts:  Location, Age, Race, and Sex*
Source
Degrees of
 freedom
F Value1
  Pr>F**
Significance
Overall Model***      9

State                 5
Age                   1
Race                  1
Sex                   2

Overall Model         6

Census Division       2
Age                   2
Race                  1
Sex                   1

Overall Model***
                      34.18

                       5.20
                       5.24
                       1.34
                       0.01

                      13.70

                       1.31
                       4.
                       1.
    83
    70
                       0.02
  0.0001

  0.0027
  0.0138
  NS
  NS

  0.001

  NS
  0.0182
  NS
  NS
Census Division
Age
Race
Sex
CD X A
CD X R
CD X S
A X R
A X S
R X S




3
2
2
2
2
1
Not Testable
Not Testable
Not Testable
Not Testable
4.03
6.59
0.84
1.34
0.43
1.70




0.020
0.0057
NS-
NS
NS
NS
      Variable log  raw residue amount.

      Ratios of sampling variances used to test factor effects follow the F
distribution if the population variances are equal (null hypothesis).
    **
      Probability that this might occur by chance under the assumption of
no difference among categories.  Significance is often considered to be
represented by p £ 0.05.

   ***Models containing higher level interactions not computed.
                                  -53-

-------
                               References

Barr AJ  et  al.   1979.   A User's Guide  to  SAS-79.   North Carolina:   SAS
     Institute, Inc.
BC.  1972.  Bureau of the Census.  1970 Census of Population.
     Characteristics of the Population (Volume I, Part A, Sections 1 and
     2).  Washington, DC:  U.S. Department of Commerce.
Fellegi  IP.   1980.   Approximate tests  of independence  and  goodness of
     fit based on stratified  multistage samples.  JASA 75(370):261-268.
Hartwell T, Piserchia P, White SB et al. 1979.  Analysis of EPA
     Pesticides Monitoring Networks.  Washington, DC:  U.S. Environmental
     Protection Agency. EPA-560/13-79-014.
Hartwell T, Piserchia P, White SB et al. 1979.  Analysis of EPA
     Pesticides  Monitoring  Networks.   ADDENDA.   Washington,  DC:   U.S.
     Environmental Protection Agency.  EPA-560/13-79-014.
Holt MM. May 1977.   SURREGR:  Standard Errors of Regression Coefficients
     From  Sample Survey  Data.  Research  Triangle Park,  NC:   Research
     Triangle Institute.
Kutz FW  and Strassman SC.  Undated.  National Human Monitoring  Program
     Study Plan for Mirex Special Project.   Internal document.   Washington,
     DC:  Office of  Pesticides and Toxic Substances, U.S.  Environmental
     Protection Agency.
Rand McNally and Co.  1974.   Commercial Atlas and  Marketing  Guide.   New
     York, New York:  Rand McNally and Co.  Shah BV.  June 1979.  SESUDAAN:
Standard Errors Program for Computing
     of  Standardized  Rates  from Sample Survey Data.   Research Triangle
     Park, NC:   Research Triangle Institute.   RTI/1789/00-01F.
Snedecor  GW and Cochran WG.   1967.   Statistical Methods.    Ames,  Iowa:
     Iowa Press.
Thompson JF,  ed.   1974.  Analysis  of Pesticide Residues  in  Human  and
     Environmental  Samples.   Section 5A.  Research Triangle  Park,  NC:
     U.S. Environmental Protection Agency.
                                -54-

-------
                     APPENDIX A

State Maps Showing Counties Where Federally Assisted
Mirex Was Applied At Some Time During 1965-1974
                      A-55-

-------
Shaded areas had some application of mirex during the
period 1965-1974

-------
AfcBAMA
Counties, Standard  Metropolitan Statistical Areas, and Selected  Places
  I
                                                                                              COLUMBUS
                                                                                                KUtCOGCC
                                                                                                  OIUMBUS
                                                                                    LEGEND
                                                                         ®   Places of 100,000 or more'inhabitants
                                                                         •   Places of 50,000 to  100.000 inhabitants
                                                                         O   Places of 25,000  to 50,000 inhabitants outside SMSA's
                                                                                    Standard Metropolitan
                                                                                    Statistical Areas (SMSA's)
M
                                                            A-57

-------
                                                                                                                                                                 14
OO
                                                                                                                                                                            IS
                                   LEGEND

                       (•)   PUces ol 100.000 01 more inhabitants

                       •    Places ol 50.000 to 100.000 inhabitants

                       O    Places ol 25.000 to 50.000 inhabitants outside SMSA's
                               •:*ri Slandatd Metropolitan
                                    Statistical Areas ISMSA's)
                                                                                                                                 FORT  LAUDERDALE HOLL'
WEST  PALM BEACH

    p?  V^..^rr|

.YWOOD   »,,..„     ./
                                                                                                                        10
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                                                                                                                                                                                                                           2.
                                                                                                                                                                                                                           s
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                                                                                                                                                                                                                           3
                                                                                                                                                                                                                           Q>
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                                                                                                                                                                                                                           05
                                                                                                                                                                                                                           CO
Q>
3
Q.

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-------
1
 I
EORGIA
 unties, Standard Metropolitan Statistical Areas, and  Selected Places
i
            -,';   CHATTANOOGA
              '        »
            ,  ©CHATTANOOGA
                                                                                            LEGEND

                                                                                 ®   Places of 100,000 or more inhabitants

                                                                                 •   Places of 50.000 to 100,000 inhabitants

                                                                                 O   Places of 25.000 to 50.000 inhabitants outside SMSA's
                                                                                         J—1 Standard Metropolitan
                                                                                            Statistical Areas (SMSA's)


                                                                          KS^S^;&V%s*'^&Jf£&K^-Vi&i\';;'"i^?T*~~"(*


                                                                                   ^%ve>«
-------
  10
               11
12
                                        13

             LEGEND


®   Places ol 100.000 or more inhabitants

•   Places of SO.OOO to 100.000 inhabitants

O   Places ol 25.000 to SO.OOO inhabitants outside SMSA's
           PI Standard Metropolitan
              Statistical Areas I SMSA's)
                                                                               CD
                                                                               3-

                                                                               Q.
                                                                               Q>
                                                    CD
                                                    i-f

                                                    s
                                                    T3
                                                    O_

                                                    r*
                                                    0)
                                                    =1

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                                                    ET
                                                                               S
                                                                               (D
                                                                               0)
                                                                               in

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                                                                               O.
                                                                               W
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                                                                               0)
                                                                               O
                                                                               (D
                                                                               (A
                                                                                       CO

-------
*
SISSIPPI
Counties, Standard  Metropolitan Statistical Areas, and Selected Places
                    LEGEND

         ®   Places of 100,000 or more inhabitants
         Q   Central cities of SMSA's with fewer than 50,000 inhabitants
         O   Places of 25,000 to 50,000 inhabitants outside SMSA's
                    Standard Metropolitan
                     Statistical Areas (SMSA's)
                                                                                                                    H
                                                                                                                   Mi
                                                                                                10
                                                             A-61

-------
                                                                                       10       11       12       13     14
                                                                                   15
16       17       18


                          STOMS | 1KXHINCMAM I CASWIU I KRSON
                 WIN^Tpf^SALEM-HIGHl POINT
»»i«u«i \   WIL« »   Kz^vvmym
H
                                LEGEND
                   ®   Places of  100,000 or more inhabitants
                   •    Places of 50,000 to 100,000 inhabitants
                   D    Central cities of SMSA's with fewer than 50,000 inhabitants
                   O    Places of  25,000 to 50,000 inhabitants outside SMSA's
                                Standard Metropolitan
                                 Statistical Areas (SMSA's)
                                                                                                                        H
                                                                                                                                                                                    a
                                                                                                                                                                                    s
                                                                                                                                                                                    3
                                                                                                                                                                                    C/J
                                                                                                                                                                                    sr
                                                                                                                                                                                    o
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                                                                                                                                                                                    0)
                                     Q)
                                     Q.
                                     ay
                                     CD.
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                                     Jl
                                     8.
                                     33
                                     Q)
                                                                                                                                  O   IO  2O  3O  40 9O MILCS
                                                                                                                                  I •  I   I   I    I —<
                                                                                       10       11       12       13       14       15       16       17
                                                                                                               18

-------
                                                                                                                         10
               11
                                                                                                                                                     12
                13
to
                      LEGEND


        ®    Places of 100,000 or more inhabitants

         •    Places of 50.000 to 100.000 inhabitants

         O    Places of 25.000 to 50,000 inhabitants outside SMSA's
                     Standard Metropolitan
                      Statistical Areas (SMSA's)
                                                                                                                                  CHARLESTON
                                                                                                                                          IO     O     IO    «O    *O     4O Mil
                                                                                                                                                                                                     CO
                                                                                                                                                                                                     f-+
                                                                                                                                                                                                     Q)
                                                                                                                                                                                                     3
                                                                                                                                                                                                     Q.
                                                                                                                                                                                                     CO
                                                                                                                                                                                                     2-
                                                                                                                                                                                                     3
                                                                                                                                                                                                    T3
                                                                                                                                                                                                     Q)
                                                                                                                                                                                                     3
                                                                                                                                                                                                     Q>
                                                                                                                                                                                                     o
                                                                                                                                                                                                     D)
                                                                                                                                                                                                     (D
                                                                                                                                                                                                     Q)
                                                                                                                                                                                                     Q)


                                                                                                                                                                                                     Q.

                                                                                                                                                                                                     CO
                                                                                                                                                                                                     O>
                                                                                                                                                                                                     O
                                                                                                                                                                                                     CO
                                                                                                                                                                                                     o
                                                                                                                                                                                                     (D
                                                                                            8
10
                                                                                                                                      11
12
13

-------
                                                                                          10
                                                                                                   II
                                                                                                           12
                                                                                                                    13
                                                                                                                             14
                                                                                                                                              16
                                                                                                                                                      17
                                                                                                                                             TEXARKANA
                                                                                                                                                     .BEAUMONT-

                                                                                                                                                   PORT.ARTHUR

                                                                                                                                                          ORANGE
                                                                                                                                                          OUNCf

                                                                                                                                                          I AITNUI
                                                                                                                                          GALVESTON TEXAS  CITY
            LEGEND

(•)   Places ol 100.000 ot more inhabitants
•    Places of 50.000 to 100.000 inhabitants
O   Central Cities ol SMSA's with fewer than 50000 inhabitants

O   Places of 25.000 to 50.000 inhabitants outside SMSA's
         "—i Standard Metropolitan
             Statistical Areas ISMSA's)
                                                                                                                       BROWNSVILLE  HARLINGEN SAN BENITO



                                                                                                                                    15       16      17
 C

 i-f
 (D*
 tn
                                                                                                                                                                                              Q)
                                                                                                                                                                                              =1
                                                                                                                                                                                              Q.
                                                                                                                                                                                              0)
                                                                                                                                                                                              (D
                                                                                                                                                                                              !-*•
                                                                                                                                                                                              s
                                                                                                                                                                                             T3
                                                                                                                                                                                              D)
                                                                                                                                                                                              =1

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                                                                                                                                                                                              <-^
                                                                                                                                                                                              Q)
                                                                                                                                                                                             >
                                                                                                                                                                                             0>

-------
                                APPENDIX B


        Counties  Where Federally  Assisted  Mirex  was  Applied at  Some
        Time During 1965-1974
Note:     Population values based on 1970 Census Data
                               B-65

-------
Alabama
          Total Population 3,444,165
All counties except

     Colbert
     Lauderdale
     Lawrence
     Limestone
     Madison
     Morgan
     Marshall
     Jackson
     DeKalb
     Cherokee
     Mirex Area Popultation
Population

   49,632
   68,111
   27,281
   41,699
  186,540
   77,306
   54,211
   39,202
   41,981
   15,606
  601,569

2.842.596
Florida
          Total Population 6,789,443
All counties except

     Monroe
     Dade
     Collier
     Broward
     Hendry
     Palm Beach
     Glades
     Martin
     St. Lucie
     Indian River
Mirex Area Population
Population

   52,586
1,267,792
   38,040
  620,100
   11,859
  348,753
    3,669
   28,035
   50,836
   35.992
2,457,662

4,331,781
                             B-66

-------
Georgia
               Total Population 4,589,575
All counties except

     Dade
     Walker
     Catoosa
     Whitfield
     Murray
     Fannin
     Gilmer
     Union
     Towns
     Rabun
     Habersham
     White
     Lumpkin
     Dawson
     Pickens
     Gordon
     Chattooga
     Floyd
     Polk
     Haralson
     Carroll
     Douglas
     Paulding
     Bartow
     Cherokee
     Forsyth
     Hall
     Banks
     Stephens
     Franklin
     Hart
     Elbert
     Madison
     Jackson
     Barrow
     Walton
     Morgan
     Oconee
     Clarke
     Oglethorpe
     Wilkes
     Lincoln
     Columbia
     McDuffie
     Warren
     Taliaferro
     Greene
     Hancock
     Glascock
Population

    9,910
   50,691
   28,271
   55,108
   12,986
   13,257
    8,956
    6,811
    4,565
    8,327
   20,691
    7,742
    8,728
    3,639
    9,620
   23,570
   20,541
   73,742
   29,656
   15,927
   45,404
   28,659
   17,520
   32,663
   31,059
   16,928
   59,405
    6,833
   20,331
   12,784
   15,814
   17,262
   13,517
   21,093
   16,859
   23,404
    9,904
    7,915
   61,177
    7,598
   10,184
    5,895
   22,327
   15,276
    6,669
    2,423
   10,212
    9,019
    2,280
Jefferson
Burke
Jenkins
Emanuel
Candler
Mirex Area
Population
Population

   17,174
   18,255
    8,332
   18,189
    6.412
1,031,614
3.557.961
                              B-67

-------
Louisiana
     Total Population 3,641,306
All counties mirex treated
     Population
     3,641,306
Mississippi
     Total Population 2,216,912
All counties except

     Sunflower
     Leflore
     Humphreys
     Sharkey
     Issaquena
     Bolivar
     Coahoma
     Quitman
     Tallahatchie
     Tunica
     Panola
     Tate
     DeSoto
     Marshall
     Benton
     Tippah
     Alcorn
     Prentiss
     Tishomingo
     Carroll
     Holmes
     Attala
     Clarke
     George
     Stone
     Pearl River
     Hancock
     Mirex Area Population
Population

   37,047
   42,111
   14,601
    8,937
    2,737
   49,409
   40,447
   15,888
   19,338
   11,854
   26,829
   18,544
   35,885
   24,027
    7,505
   15,852
   27,179
   20,133
   14,940
    9,397
   23,120
   19,570
   15,049
   12,459
    8,101
   27,802
   17,387
  566,148

1,650,764
                         B-68

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North Carolina
          Total Population 5,082,059
     New Hanover
     Brunswick
     Columbus
     Robeson
     Bladen
     Duplin
     Onslow
     Lenoir
     Jones
     Craven
     Pamlico
     Cateret
Population
 82,996
 24,223
 46,937
 84,342
 26,477
 38,015
103,126
 55,204
  9,779
 65,554
  9,467
 31,603
     Mirex Area Population    578,223
South Carolina
          Total Population 2,590,516
     Marlboro
     Dillon
     Marion
     Horry
     Georgetown
     Williamsburg
     Florence
     Clarendon
     Sumter
     Kershaw
     Fairfield
     Richland
     Calhoun
     Orangeburg
     Berkeley
     Charleston
     Dorchester
     Colleton
     Bamberg
     Barnwell
     Aiken
     Allendale
     Edgefield
     Lexington
     Hampton
     Jasper
     Beaufort Point
Population
   27,151
   28,838
   30,270
   69,992
   33,500
   34,243
   89,636
   25,604
   79,425
   34,727
   19,999
  233,868
   10,780
   69,789
   56,199
  247,650
   32,276
   27,622
   15,950
   17,176
   91,023
    9,692
   15,692
   89,012
   15,878
   11,885
   51,136
     Mirex Area Population    1,469.023
                          B-69

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Texas
          Total Population 11,196,730
     Denton
     Collin
     Dallas
     Bowie
     Harrison
     Smith
     Orange
     Jefferson
     Polk
     San Jacinto
     Walker
     Madison
     Grimes
     Harris
     Galveston
     Brazoria
     Fort Bend
     Waller
     Austin
     Washington
     Wharton
     Lavaca
     DeWitt
     Victoria
     Bexar
     Nueces
     Montgomery
     Brazos
Population
   75,633
   66,920
1,327,321
   67,813
   44,841
   97,096
   71,170
  244,733
   14,457
    6,702
   27,680
    7,693
   11,855
1,741,912
  169,812
  108,312
   52,314
   14,285
   13,831
   18,842
   36,729
   17,903
   18,660
   53,766
  830,460
  237,544
   49,479
   57,978
     Mirex Area Population    5,485,781
                          B-70

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           APPENDIX C
Definition of Mirex Treated Areas
          C-71

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                    Definition of Mirex-Treated Areas

     For purposes of the MSS, a mirex treated county is a county includ-
ing  an area having  any application  of  mirex during  a 10-year period.
This  definition does  not take  into  consideration factors  of repeated
applications, amount of active substance displaced, or land area covered.
     Before being banned  from sale and use in 1977, mirex was sold over
the  counter to  private  individuals  and  applied  by both  State  action
agencies and the States and Federal Government working together.  It may
be possible to obtain mirex use information from individual State action
agencies  and  from the United States  Department  of Agriculture's  Animal
and Plant Health Inspection Service (USDA, APHIS) that would help answer
some of  the above questions about the frequency and intensity of mirex
application.   For example,  this  kind  of historical  information about
mirex  application  in the  State of North  Carolina  can  be gathered from
existing  records  in  the North Carolina Department of Agriculture's Pest
Control  Division.-    Information from the APHIS of USDA concerning the
number of mirex-treated acres by State is available; this only includes
those  acres treated  from  1964  to  1973   by  the Federal  Government  in
                                        21
connection  with the  individual States.-   Additional  mirex treatment
must have  varied from  State to State, dependent  upon  the magnitude  of
the fire ant problem and the resources of  the State.
     It would be inconclusive, however, to attempt to correlate detailed
information  about  mirex  use  with  this human  adipose  tissue  data.
Specific  residence  information was  not  obtained  about  the individuals
from whom specimens were collected.  In an epidemiological study such as
this,  it  is more important to verify the  residence of study individuals
than to  form a  better  definition  of the  area in  which the individuals
can only be assumed to reside.
     - Singletary HM.  May 8, 1980.  Personal communication, C. Leininger.
Raleigh,  North  Carolina:   Pesticide  Division,  North  Carolina  State
Department of Agriculture.

     2/
     -Table  of  Aggregate   Acres  Treated,  provided to  EPA  by  APHIS.
Revised date 8/1/73.
                                C-72

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           APPENDIX D
MSS Sample Site Selection Method
           D-73

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                    MSS Sample Site Selection Method
D.I.      Introduction
     In  order to  calculate  appropriate  weights  that can  be  used  in
making population  estimates  from sample data, the method used to select
the sample must  be known.  This appendix  is  a discussion of the method
used to  select  the sample RMA's for  the  MSS.   For the NHMP, the method
used to select sites involved selection with probability proportional to
the size  of  the  site's population (PPS) and with replacement.  The NHMP
study plan  for  the MSS-  is  not clear as to  the method  used to select
sites for the MSS.  The selection procedure  for the  MSS was checked by
calculating the expected outcome of selecting 32 out of 60 RMA's by both
PPS and simple random sampling (SRS).  It was concluded that SRS was the
method used.
D.2.      The NHMP and Probability Proportional to Size
     The  method  of  sample  selection used in the NHMP  was systematic
selection with probability  proportional to size (PPS) from a stratified
sampling frame.  This  means  that the population of a city was a factor
in the possibility of the city being selected in a sample.  When n areas
are to  be selected  systematically with  PPS,  the  selection probability
for a  given  area  is calculated by  dividing n  times  the population of
that  area  by the  total  population  of all  the  areas in  the  sampling
frame.  This  is expressed as
                                                                  i
  ,  ..       , v-i  -4.  /T.T.OA  c      -i    n x population of area i
selection probability (PPS) of area i' =  - *-*• -  ,
                                             N
                                             I  population of area i
where N  is the  number of  areas  in the sampling  frame.   If some units
have a size measure  greater than the sampling interval, this expression
should  be  termed expected number  of  hits  as   opposed  to  selection
probabilities.
     NHMP  cities  were  selected by PPS, within strata  defined  by Census
Divisions.  As discussed  in Chapter 2, the 8 NHMP cities located in the
mirex area were   included  in the MSS.   This was  an effort to  use the
                               D-74

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existing tissue  collection network.   The  MSS supplementary  sample was
selected from  60 RMA's not  in the NHMP.  The majority  of  the existing
documentation  of  the MSS  indicates  that SRS was used to select  the 32
MSS sites.
D.3.      Simple Random Sampling
     In SRS, any  RMA has  the same chance of being selected as any other
RMA in the list of 60 RMA's in the mirex area.  A listing of the eligible
sites might be made  and a consecutive number  assigned  to  each site.  A
sample of sites can then be selected by drawing numbers (sites) from the
list using a table of random numbers.
     If SRS  was  used  to  choose  the  32  RMA's, then any one  RMA  was as
likely as any other to be chosen.  To test this,  the 60 RMA's were first
ordered by population size, and then divided into 4 groups,  each with 15
RMA's.  There  were 32  RMA's actually selected.   Under  SRS  it would be
expected that  approximately  the same number of RMA's would  be selected
from  each  of  the  4 divisions  that have been arbitrarily  made  in the
ordered listing.   This  can be seen more easily in the line chart below,
where the 4  segments  or groups are  indicated  by  Roman numerals,  with a
subscript "s"  or  "f"  to   indicate  membership in the  sample or  in the
frame.
1
1
I
s
:f
8
15
II
s
Hf
16
30
III
III
s
f
24
45
IV
s
IVf
32 =
60 =
sample
frame
RMA's
RMA's
     In repeated sampling, the average proportion of selected RMA's from
a segment of the frame will be one-fourth.  Since it is a random process,
there  will  be  some  variation in  the number of  selected RMA's  from a
segment of  the frame.   A 95 percent confidence interval  (C.I.)   will
give the  range  of  values that will be encountered 95 out of 100 times a
given  sample  selection  procedure  is used.  The expected number of sites
selected by SRS  in any of the 4  segments of the frame is one-fourth of
32, or 8.   To find a 95  percent   confidence interval for the number of
sites  chosen  from  each segment,  computations were based on the variance
of  the number of  sites  selected  per segment and the  properties  of the
normal  curve.   These calculations  are  given in detail  in  section D.6.
For this  case,  where 8 is the expected  number  of sites selected from a
segment, the 95 percent C.I.  is 8 + 1.96V 6  = 8 ± 4.8.
                               D-75

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        The number of  sites  selected  under SRS can range  from  3.2  to  12.8
   sites within a 95 percent C.I.   This agrees with the actual distribution
   of sites among  the  arbitrary segments,  as indicated in the chart below.

                      I          II        III         IV
                       s           s          s          s
Expected number
of sites (SRS)      8 ± 4.8    8+4.8   8 ± 4.8    8 + 4.8
and the 95% C.I,    	.
Number of sites       8         5         8        11
actually in the MSS 	
        Another method  that can be  used to  check  the observed number  of
   sites selected  against the number  of sites  expected  under SRS  is  the
                2
   chi-square  (x )  test.   This  test  compares the expected results  (F)  to
   the actual results (f)  under the hypothesis of no  significant difference
                                                             2
   between expected and observed result.   The value  of the x  statistic  is
   computed using the following formula.

                            ,  *
                  X
                                  F.
                                   i
                   2
   where          x    =    chi-square statistic ,
                  f.   =    observed number of sites  for the  ith segment ,
   and            F.   =    expected number of sites  for the  ith segment .
        Any standard statistical text will contain  a  more detailed description
   of this simple test.   A thorough explanation is  given in Chapter 3  of
   Statistical Methods by Snedecor and Cochran (1967).
                                        2
        For these  data, the value of x   under the assumption of SRS  is
   2.25, which with  3  degrees  of freedom  (number of  segments (4)  minus  1 =
   3) has  a p-value  of 0.522.   This  is  not at all significant;  the test
   hypothesis  of no  difference  between the expected results  under  SRS  and
   the observed results cannot  be rejected as false.
   D.4  Probability Proportional to Size
        The same arbitrary segments were created, and 95 percent C.I.'s  for
   the number  of sites selected from each  segment were  calculated,  assuming
   selection  PPS.   The  selection  rates  varied  from  segment  to  segment,
                                 D-76

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   because the combined population of the areas within a segment determined
   the sampling rate for that segment.  The combined population for each of
   the four divisions  varied considerably:   I_ = 730.600, II,, = 1,159,800,
                                              r              r
   IIIF = 2,124,100,  and IVp = 6,779,200, for a frame total of 10,793,700.
   The selection probabilities  also  varied accordingly, from Pr(I ) =0.07
                                                                  s
   to  Pr(IV ) = 0.63.   C.I.'s for the number of  selected sites from each
            S
   segment under  PPS were  computed  and are displayed  in  the chart below.
Expected number
of sites (PPS)
and the 95% C.I.
Actually selected       8           5           8            11
for MSS
s
2.2 ± 2.8
II
s
3.4 ± 3.5
III
s
6.3 ± 4.4
IV
s
20.1 ± 5.4
        The number of  sites  actually selected in 2 of the 4 segments falls
   outside the 95% C.I.  for  number of selected sites from the segment when
   selection  is  PPS.  The  result is  in  agreement with  the results  of  a
   chi-square test for expected  number of sites under PPS  to the observed
                                                    2
   number of  sites selected  for  the sample.  The  x  in  this case is 20.6,
   which with 3 degrees of freedom has a p value of 0.0001.   This is highly
   significant and indicates  that the hypothesis of no difference cannot be
   accepted as true.
   D.5.  Conclusions
        Based  on  the  computations described  in  Section D.3 and  D.4,  it
   appears that the MSS sample sites were selected by simple random sampling.
   Therefore,  the  selection  rates used in  computing the  quasi  selection
   weights were calculated under  the assumption of SRS.
   D.6. Calculations
        This section contains a  detailed  description of  the calculation of
   confidence intervals for  the  number of sites selected per segment when
   selecting  32 of  60 RMA's  by  SRS.   The method  used to determine C.I.'s
   when using  PPS  sampling  is  similar to  that used in  SRS, and  will be
   described briefly.
        Confidence intervals  are  calculated using  the  properties  of the
   normal curve and  the variance of a random variable.   In this case, the
                                 D-77

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   random variable, which can be called y, is the number of sites that will
   be  selected  from a  given segment.   The distribution of  y is binomial.
   Variances  are  calculated for  binomial random variables  (in this case,
   the Bernoulli  event  is  that a site is selected in a given segment or it
   is  not selected  in that  segment)  by multiplying  the  total  number of
   sites  selected  by  the  probability (p) that  the  selected  site is in the
   segment by the  probability (q) that it is not.  Thus, the variance of y
   can be expressed as V(y) = npq.
        The probability that a  selected site falls in  a  given segment is
   8/32 = 1/4 = p.  The value of q is then 24/32 or 3/4.  The variance will
   be  the  same   for  the  number  of  sites  selected  in  each  segment:
   32(l/4)(3/4)=6.  To  find  the  95  percent  C.I.  for  y  (where y  is  the
   number of  sites selected for a segment) requires multiplying the square
   root  of  the  variance  (this  is the  standard  deviation)  by  1.96.   The
   constant  1.96   is a  value (called  a  z  score)  which corresponds  to 95
   percent  of the area under  the normal  curve.  Other  constants,  which
   correspond to  different percentages  of the area under the normal curve,
   can be found in a table of  z scores  in any standard statistical text.
   In  this  case,   where the probability  that a selected site  falls  in the
   given segment is the same for all segments, the 95 percent
   C.I. is 8 ± 1.96V~1T~  =  8 ± 4.8 for each segment.
        To find  the 95%  confidence  interval for number of  selected sites
   falling in a given segment, assuming PPS, the same procedure is followed
   as  for SRS,  except  that the probability of a selected site falling in a
   given  segment  is different  for each segment.  This reflects the differ-
   ence in the population size of the sites in the frame.  To calculate the
   expected number of sites in a segment, the probability of selection for
   a  segment  is multiplied by the number  of  sites  desired in  the  final
   sample.  As  an example,  for segment  If, with Pr(selection)  = 730,600/
   10,793,700 =  0.07,   the  expected  value  of y =  (0.07)(32) =2.2.   The
   variance of y was calculated separately for each segment,  and the C.I.'s
   computed for each segment as was done when assuming SRS.
- Kutz F W and Strassman S C. undated.  National Human Monitoring
Program Study Plan for Mirex Special Project.  EPA internal document.
Washington, DC:  Office of Pesticides and Toxic Substances, U.S.
Environmental Protection Agency.
                                 D-78

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         APPENDIX E
List of MSS Collection Sites
            E-79

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                               COLLECTION SITES
Alabama

  Anniston
0 Birmingham
  Dothan
°*Mobile
0 Montgomery
* Tuscaloosa
Florida

  Fort Myers
  Fort Walton Beach
  Lakeland
  Orlando
°*Panama City
  Sarasota
0 St. Petersburg
  Tallahassee
°*Tampa

Georgia

  Atlanta
0 Brunswick
  Columbus
  Ma con
  Savannah
x Valdosta

Louisiana

  Alexandria
0 Lafayette
  Lake Charles
  Monroe
* New Orleans
  Shreveport
Albany, Georgia
Opelika, Alabama
Melbourne, Florida
Bryan, Texas
RMA Population-'
93,100
679,000
51,200
312,500
201,000
106,300


83,500
76,500
97,000
473,000
72,000
222,000 '
625,000
121,500
495,000


1,720,000
54,300
226,700
219,500
184,000
50,100
97,500
128,800
128,500
110,800
1,126,000
282,000
Mississippi RMA Population-
Columbus 43,200
0 Greenville 51,100
Hattiesburg 57,200
Jackson 258,000
Laurel 41,000
Meridian 56,200
Pascagoula 74,900
North Carolina
Wilmington 91,300


South Carolina

Charleston 290,000
Columbia 315,000

Texas
* Dallas 2,455,000
* Houston 2,085,000
* San Antonio 890,000



••'-'.-"







ALTERNATE COLLECTION SITES -/
94,800
46,700
100,000
60,700

Gadsden, Alabama 79,000
Jacksonville, Florida 585,000
Baton Rouge, Louisiana 361,000
Pensacola, Florida .217,000
Gulfport, Mississippi 173,500
*
X
o
1
2
National Human Monitoring Site
Replaced by Albany, Georgia, in survey
Nonresponding Site
1974 Rand McNally Population Estimates
Listed in Order of Selection
                              E-80

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                    RMA Remainder Frame  After Selection of
                        Collection Sites and Alternates
Florida

Cocoa
Daytona Beach
Gainesville
Titusville
Winter Haven

Georgia

Augusta

Louisiana

Houma
New Iberia

North Carolina

Jacksonville

South Carolina

Florence
Sumter
RMA
Population —
Texas
RMA Population -'
                                                                           I/
      87,000
     117,000
      97,000
      39,000
      64,800
     215,500
      53,000
      40,500
      71,000
      49,600
      69,600
                     Beaumont-Port Arthur     226,000
                     Corpus Christi           257,000
                     Freeport-Lake Jackson     58,700
                     Galveston-Texas City     135,000
                     Orange                    51,600
                     Texarkana                 75,000
                     Tyler         •            79,200
                     Victoria                  45,400
     1974 Rand McNally Population Estimates
     Remainder Frame:  The sites remaining .after sample selection has been
     made from the frame of target sites.
                               E-81

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               APPENDIX F






Quotas for Mirex Special Study Specimens

-------
               NATIONAL HUMAN MONITORING PROGRAM
              U. S. ENVIRONMENTAL PROTECTION AGENCY
                   WASHINGTON, D. C.  20460
                QUOTA FOR MIREX SPECIAL PROJECT

Each collection site in the states of Alabama and Mississippi is
requested to collect human adipose tissue from the following
age/sex/race groups:
QUOTA                    AGE GROUP               SEX
4                        0-14                    Male
4                        0-14"                    Female
5                        15-44                   Male
6                        15-44                   Female
4                        45 and above            Male
4                        45 and above            Female
Quota of 27 samples should include 5 non-Caucasian specimens.
Proportional  distribution of these non-Caucasian specimens
among the age/sex groups is preferable but not required.
                          F-83

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             NATIONAL HUMAN MONITORING PROGRAM
           U. S. ENVIRONMENTAL PROTECTION AGENCY
                 WASHINGTON, D. C.  20460
             QUOTA FOR MIREX SPECIAL PROJECT

Each collection site in the states of Louisiana and Texas
is requested to collect human adipose tissue from the following
age/sex/race groups:
QUOTA                    AGE GROUP               SEX
4                        0-14                    Male
4                        0-14                    Female
6                        15-44                   Male
6                        15-44                   Female
3                        45 and above            Male
4                        45 and above            Female
Quota of 27 samples should include 4 Non-Caucasian specimens.
Proportional distribution of these non-Caucasian soecimens aroono
the age/sex groups  is preferable but not required.
                           F-84

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              NATIONAL HUMAN MONITORING PROGRAM
             U. S. ENVIRONMENTAL PROTECTION AGENCY
                    WASHINGTON, D. C.  20460

              QUOTA FOR MIREX SPECIAL PROJECT

Each collection site in the states of North Carolina, South Carolina,
Georgia and Florida is requested to collect human adipose tissue from
the following age/sex/race groups:
QUOTA                    AGE GROUP               SEX
4                        0-14                    Male
4                        0-14                    Female
5                        15-44~                  Male
6                        15-44                   Female
4                        45 and above            Male
4                        45 and above            Female
Quota of 27 samples should include 6 non-Caucasian specimens.  Proportional
distribution of these non-Caucasian specimens among the age/sex groups
is preferable but not required.

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         APPENDIX G






Instructions to Pathologists
         G-86

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Dear	:
     	 has been selected as one of 40
representative cities in which the U. S. Environmental-Protection
Agency would like to conduct a special research study to determine
the frequency of finding residues of the insecticide, mi rex in
humans.  This letter is an invitation to you to participate
in this study.  This project is an activity of the National
Human Monitoring Program for Pesticides and will be ongoing for
the next 6 to 9 months.
     Mirex is an organochlorine insecticide which has been used
for the control of the imported fire ant in large areas of the
southern United States.  Our information indicates that over
14 million acres have been treated to date.  Mirex is extremely
resistant to chemical degradation and thus its persistence enables
it to accumulate in certain organisms in the food chain.  As you
will note from the enclosed reprint, mirex has been found in
humans.  We now need to make a more precise estimate of the
epidemiology of this chemical.
     As a mechanism for estimating exposure to mirex, samples of
human adipose tissue will be chemically analyzed in our laboratories.
Reports of findings will be furnished to each participating physician.
Data from these analyses are useful in evaluating various factors
and conditions pertaining to human health and pesticide regulation.
                       G-87

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     We will need samples of human adipose tissue from previously
excised surgical specimens and/or postmortem examinations.   The
samples should be collected in accordance with the enclosed
guidelines.  Each participant is being asked to collect specimens
according to the enclosed age/sex/race quota form.  We furnish
all supplies (mailers, forms, bottles, postage-paid address cards,
etc.) and are able to remunerate you or your designee for professional
services at the rate of $10.00 per acceptable sample.
     We hope that you will help in this study by providing selected
adipose tissues obtained during routine pathology.  We will telephone
you about this in a few days.
                                   Sincerely yours,
                                   Frederick W. Kutz, Ph.D.
                                      Project Officer
                            National Human Monitoring Program (WH-569)
Enclosures
                            G-88

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            INSTRUCTIONS FOR THE COLLECTION OF
             HUMAN ADIPOSE TISSUE FOR MIREX
                    ANALYSIS
     Mi rex is an organochlorine insecticide used for the control
of the imported fire ant in large areas of southern United States.
The chemical is extremely resistant to degradation and this
persistence and its chemical characteristics enable it to
accumulate in certain organisms in the food chain.
     The objective of this special environmental study is to
determine the incidence and levels of mi rex in human adipose
tissue collected from areas which have been treated with this
chemical.  The results from the program are used in evaluating
various factors and conditions pertaining to human health and effective
pesticide regulation.
     The adipose tissue for this project is secured through the
cooperation of participating pathologists located throughout
southern United States.  The tissue is obtained from surgical
specimens previously excised for pathological examination and from
postmortem examinations.  The specimens are sent to the program
office in Washington, D. C., from which they are then forwarded to
contract laboratories for chemical analysis.  Periodic reports of
the laboratory results are sent to each participating pathologist
for the tissues which were submitted under his auspices.  Summaries
comparing results with other regions are also provided as they become
available.

-------
     In order to develop precise epidemiologic data, collections
must be made according to an experimental design which dictates
the number of samples required according to the demographic
distribution of the population of your area.  You should have a
copy of the quota of samples expected to be collected from your
location on a fiscal year basis.  All collections should be made
according to this age/sex/race distribution.  You should be able
to collect the number of samples required in each category in the
next 6 months.  If you feel that you will be unable to collect the
number of samples required, please let us know.
Criteria for Selection of Patients to be Sampled
     Since the program objective is to reflect pesticide incidences
and levels in the general (man-on-the-street) population, a few
suggestions are listed here for your guidance:
     .  The highest priority should be given to satis-
        fying the number and demographic distribution
        of your quota.  This quota should be completed
        as soon as possible after the start of the project.
     .  Patients having known or suspected pesticide
        poisoning should not be sampled.  If you are
        involved with a potential pesticide poisoning,
        we would like to assist you in any way possible.
        However, samples should not be taken for the
        National Human Monitoring Program.
                            fSr-fO

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        .  Patients with cachexia or who have been institu-
          tionalized for long periods should not be sampled
          for the national program.
Collection of Surgical Adipose Tissue
     Collect samples of adipose tissue from living patients from
unfixed specimens which have been surgically excised for therapeutic
reasons.  Take special care to keep samples from different patients
separate and correctly and securely labeled and to avoid their con-
tact with other chemicals such as paraffin, disinfectants or plastics.
     At least five grams of good quality (subcutaneous, perl renal,
mesenteric) adipose tissue should be collected from any part of the
specimen; avoid fibrous or connective tissue, I.e., omentum.  Place
the fat, without any fixatives or preservatives, Into the chemically-
cleaned container that you have been given and legibly complete, in
ball-point pen or pencil, and attach the self-adhesive label.  The
bottle labels should be affixed before freezing.  Store the specimens
up-right in a freezer at -4°F (-20°C) until shipment.
Collection of Postmortem Adipose Tissue
     Adipose tissue samples must be obtained only from unembalmed
cadavers.  The interval between death and the collection of tissue
should be as short as possible and must not exceed 24 hours,
assuming refrigeration during the interval.  Samples of adipose
tissue must weigh at least five grams and should be placed in the
                             (3-91
                                 •v

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supplied chemically-clean container with a completed label  affixed.
Specimens should be stored at -4°F (-20°C) without any fixative or
preservative until shipment.  Submit only good quality fat; do not
submit omentum as it contains too much connective tissue for satis-
factory analysis.
     Adipose should be taken dry, and should not be rinsed before
placing in the containers provided.  Many water supplies contain
materials which would interfere with chemical analysis.
     Instruments should be well-rinsed with distilled water and
dried before taking the adipose sample.
Completion of the Patient Summary Report
     A Patient Summary Report should be completed for each patient
from whom a sample was taken.  Special attention should be given to
the completeness of the information.  First and last Initials, in
that order, should be used instead of the complete name to insure
that confidentiality is maintained.  The Initials, along with the
date of birth, sex, and race, are used 1n this office to compose the
AMA identification number.  The patient's Identification number and/or
the pathology department's accession number are for your Information
in referring back to the individual patient when you receive the
results of the pesticide analysis.
     Confirmed diagnosis should be detailed in the spaces provided.
Only the major ones should be supplied.

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     Other information required should be completed as accurately
as possible.  The completed forms should be held and sent under the
lid of the insulated container when shipment is made.
Packing and Shipping
     Tighten all lids on the specimen bottles carefully.  This is
important since we are required to use special aluminum foil  cap
liners which make tightening a little difficult.  Be certain  that
a completed bottle label is firmly attached to each specimen  bottle.
Wrap each bottle in gauze or paper to prevent breakage during ship-
ment and to keep the label on the container.  Place the specimen
bottles in the insulated mailer and fill it wi.th dry ice.  If you
have difficulty obtaining dry ice, please call us and we can  arrange
alternative methods of refrigeration for you.
     .A franked addressed label is on the reverse side of the  address
card.  This card is marked AIR MAIL - SPECIAL DELIVERY.  (Do  not
send Air Express, please).  There is no cost to the sender because
of the franked label.  All insulated mailers should have a PERISHABLE
PACKED IN DRY ICE label visible from all sides on the outside.
                                                                     i
     Specimens should be mailed on a Monday or Tuesday of a week with
no federal holidays.  This assures that they will arrive before the
end of the work week on Friday.
                            G-93

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     Patient Summary Reports should be sent in the carton with
the specimens when possible.  They can be folded and placed on
the top of the styrofoam lid.
     Only samples which meet our criteria and are handled according
to the guidelines can be accepted.  No substitute containers will
be accepted.
For Further Information
     If you have any questions or comments, please contact us.
Telephone (collect):  202-755-8060.
                                   Frederick W. Kutz, Ph.D.
                                   Sandra C. Strassman
                                   National Human Monitoring Program
                           ..G-94

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               APPENDIX H

Modification of Mirex Analysis Protocol
GC Column Temperature
               H-95

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                           ENVIRONMENTAL TOXICOLOGY DIVISION
                           HEALTH  EFFECTS  RESEARCH LABORATORY
                  UNITED STATES ENVIRONMENTALPROTECTION AGENCY
                     Research Triangle Park, North Carolina  27711

SUBJECT-.  Multiresidue Analysis  of Adipose Tissue with          DATE:  March 1, 1976
          Emphasis on Mi rex and  Chlordane/HeptacJilor Derivatives
FROM:
TO:
          Chief, Quality Assurance Section, ETD, EPA, HERL,
          Research Triangle Park, N.C.
          Michigan  Project, Mr. R. L. Welch

              After receiving a copy of Bob Welch's letter to Dr..Kutz (2/11/76)
         we  cranked up a straight 5% OV-210 and a mixture column of 1.5/1.95,
         OV-17/OV-210 and ran some chromatograms in the appropriate concentration
         ranges incorporating the derivatives of heptachlor/chlordane, mirex, and
         Aroclor 1260.
                                                        V
              Frankly, we were not overjoyed by the elution patterns produced
         by  Aroclor 1260 and Mirex.  As Bob commented in his letter, at 200°C
         Mirex overlaps nearly completely with the next to last Aroclor peak
         (a  major one).  However, at 195°, although the separation is slightly
         better, we could not agree that it was anything remarkable on our
         column.  Our separation was not nearly as good as the separation
         in  Bob's chromatogram.  We dropped the column temp, to 190°, and while
         the mirex peak was clearly visible on the early side of the Aroclor, it
         was not a quantifiable separation.

              Undoubtedly, the relative efficiency of his column vs. ours was a
         factor.  We estimated his column to be yielding about 3,200 T.P. with
         his carrier flow obviously cranked down.  To compensate for the exces-
         sive time consumption at 190°, we raised the flow to 80 ml  with a -   .
         resulting EFF. of about 2,700 T.P.  Undoubtedly, our resolution
         characteristics suffered accordingly.

              Just so long as Bob's column holds up and he can continue to
         obtain the separations shown in his sample chromatograms, we see no
         objection at all  to making temperature and/or carrier flow adjustments
         in  any way that it will  best get the job done.   There is nothing
         sanctified in the recommended parameters in the manual.   They were
         written for a shotgun approach to general  multiresidue work, but if
         some other combination is more suitable for special purposes, then  by
         all means, appropriate modifications should be made.

              Even with our poor separation, I believe the chromatographer would
         be  alerted to the possible presence of mirex, then by further confirmation
         via ECD and GC/MS the final  answers can be obtained.

              I'm sure we  will  want to get together for further discussions
         of  this topic the week of the chemists'  meeting.

         cc:  Dr.  F.  W.  Kutz, Washington
              Dr.  H.  F.  Enos, Athens
EPA Form 1320-6 (Rav. £.72)
                                        ,#-96

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                         APPENDIX I





Confirmation Analyses of Mirex Human Adipose Tissue Extracts
                         1-97

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                        Analytical Results


                    Confirmational Analyses for
              Mirex in Human Adipose Tissue Extracts
                    Analytical Chemistry Branch
                 Environmental Toxicology Division
                Health Effects Research Laboratory
           Research Triangle Park, North Carolina  27711
Date:  30 November 1976
                           1-98

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                        Health Effects  Research  Laboratory
                   Research Triangle Park, North Carolina  27711
                    UNITED STATES ENVIRONMENTAL PROTECTION AGENCY

  DATE:    November 30, 1976

SUBJECT:    Confirmational Analyses for Mirex in Human Adipose Tissue Extracts
  FROM:     Dr. Edward 0. Oswald, Chief
           Analytical Chemistry Branch, ETD  (MD-69)

    TO:     Dr. Frederick W. Kutz
           Ecological Monitoring Branch (WH-569)
           OPP, Headquarters

  THRU:     Director, HERL  (MD-51)
                Attached you will find the results of confirmational analyses  for
           Mirex as generated by members of the Analytical Chemistry Branch, ETD,
           HERL, RTP on extracts of human adipose tissue which were received from
           the Michigan OPP lab on the 2 September 1976.  Three  (3) separate mass
           spectrometry groups analyzed selected extracts by gas liquid chroma-
           tography interfaced either with low resolution or with high resolution
           mass spectrometry in the electron impact mode.

                The results of the present report confirm both the qualitative and.
           the comparable quantitative presence of Mirex in human adipose  tissue as
           indicated by the electron capture results from the Michigan lab.

                As indicated to you in a similar report of the 23 June 1976, the
           GC/EC results agree quite favorably with the confirmational analyses by
           GC/MS.          .            .                  '

                If additional GC/MS confirmational analyses are needed by  OPP  for
           Mirex in human adipose tissue, then I would suggest that only about 10%
           of the total extracts be analyzed.

                If I or other members of the Branch can be of assistance on this or
           other matters, please feel free to contact me.

           Enclosure
 EPA Form 1320-t (Rc». 3-76)

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              Mirex in Human Adipose Tissue Extracts

       (Concentrations expressed in parts per million—ppm)
   Sample
Identification
*GC/EC Analyses
  (Michigan)
Confirmational GC/MS Analyses
Research Triangle Park, N. C.

0.10
0.20
0.39
0.16
0.20
0.07
Negative
0.09
^) 0.09
i Negative
LU 0.12
ijj 0.22
^ 1.10
0.11
0.15
0.12
1.13
0.16
.
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                      Analytical Methodology


                    Confintiational Analyses for
              Mirex in Human Adipose Tissue Extracts
                    Analytical Chemistry Branch
                 Environmental Toxicology Division
                Health Effects Research Laboratory
           Research Triangle Park, North Carolina  27711
Date:  30 November 1976
                               I-K31L

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Methods




     Extracts of human adipose tissue were received in.sealed glass




ampules.  At the time that the sample vial was opened, aliquots of each




selected sample extract were prepared for analysis by the various mass




spectrometry groups.  All samples were analyzed by.at least two (2)




of the analytical teams which generated multiple analyses.  All




quantitative results are expressed as mean concentrations in parts per




million (ppm) for each analytical team.  The three (3) mass spectrometry




teams were coordinated by:  (a) Mr. Robert Harless; (b) Dr. Wayne Sovocool




and (c) Dr. Lynn Wright.




     Below are listed the detailed analytical conditions utilized for




the GC/MS confirmational analyses of Mirex in extracts of human adipose




tissue.
                         1-102

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Group A.

           Low Resolution GC/MS

Instrument:  Hewlett Packard 5930A Mass Spectrometer equipped with a
             Hewlett Packard 5700 gas chromatograph

GC Column:  183 cm x 2 mm (i.d.) glass column packed with 3% OV-17 on
            100/120 mesh Gas Chrom Q.

Column temperature:  235°C

Injector temperature:  235°C

Transfer line temperature:  250°C

Membrane separator temperature:  235°C

Carrier gas:  Helium

Flow rate:  42 ml/min

lonization voltage:  70 eV

Criteria for Analyses:

     These low resolution mass spectrometric analyses  (GC-LRMS) are
based upon:   (a) correct absolute retention time as compared to Mirex;
(b) presence of intense fragments at m/e 270 with a 6-chlorine isotope
cluster and at m/e 235 with a 5-chlorine cluster (corresponding to the
main electron impact ion fragments of Mirex); and (c)  the proper ratios
of the m/e 270 and m/e 235 ion clusters.

     Quantitative GC-LRMS measurements were accomplished by single ion
monitoring of the m/e 272 ion in comparison to an external Mirex standard
and to internal spiked samples.  All samples were analyzed in at least
duplicates.
                           I-.1Q3

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Group B.

          Low Resolution GC/MS

Instrument:  Finnigan 3200 Mass Spectrometer equipped with a Finnigan
             6100 data system and Finnigan 9500 gas chromatograph

GC Column:  122 cm x 2 mm (i.d.) glass column packed with 3% OV-17
            on 100/120 mesh Gas Chrom Q

Column temperature:  240°C

Injector temperature:  240°C

Transfer line temperature:  240°C

Glass jet separator temperature:  240°C .

Carrier gas:  Helium

Flow rate:  20 ml/min

lonization voltage:  70eV

Criteria for Analyses:

     These low resolution mass spectrometric analyses  (GC-LEMS) are
based upon:   (a) correct absolute retention time as compared to Mirex;
and (b) presence of intense fragments in the m/e 270 region representing
the most prominent ions of the C_C1   cluster.
                                5  o
     The mass spectrometer was operated in the multiple ion detection
mode monitoring the three (3) most prominent ions of the C^Cl.  cluster—
m/e 270, m/e  272, and m/e 274.  A fourth ion m/e 405—not present in the
spectrum of Mirex—was monitored to provide a background.  Any sample
which gave a  negative or trace response upon the initial dilution
conditions was then further reduced in volume to approximately 1/10 of
its original  volume.  The sample was then reanalyzed.  Negative responses
to the latter conditions were reported as negative.

     Samples  were quantitated by summating the areas the mass chromato-
grams for m/e 270, 272, and 274 and comparisons of these values with the
average response obtained for an external Mirex standard which was
injected either before or after each residue sample.

           High Resolution GC/MS

Instrument:   Varian MAT 311A Mass Spectrometer equipped with a Varian
              2700 gas chromatograph and a Varian C-1024 time averaging
              computer  (CAT).

GC Column:  91 cm x 2 mm  (i.d.) glass column packed with 2% Dexil 410
            on 90/100 mesh Anakrom Q.
                          I-104-,

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Column temperature:  243°C

Injector port temperature:  255°C

Transfer line temperature:  255°C

Slit separator temperature:  2559C

Carrier gas:  Helium

Flow rate:  10-12 ml/min

lonization voltage:  70eV

Criteria for Analyses:

     The high resolution mass spectrometric analyses  (GC-HRMS) are based
upon:  (a) correct absolute retention time as compared to Mirex;  (b)
isotope ratios of two fragments of the molecular ion  cluster—m/e 539.6262
    •jt                           *3 C    ^/
(C1Q  C112) and m/e 543.6203 (C1Q  CllQ  Cl.); and  (c) analysis with
internal and external standards of Mirex.

     The mass spectrometer was operated at a high sensitivity in order
to observe the molecular ion .m/e 543.6203 (C    CLm  c^ with a mass
resolution capability of 7200-8500.  Using the time averaging computer
(CAT) system, the mass spectrometer was operated in a double ion moni-
toring mode for the molecular ion m/e 539.6262 and m/e 543.6203.  The
quantitative analyses were accomplished by the use of internal and
external standards of Mirex combined with the double  ion monitoring of
two specific ion fragments in the molecular cluster of Mirex in the high
resolution GC/MS mode.
                             I-

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                        Health Effects Research Laboratory
                           Environmental Research Center
                  UNITED STATES ENVIRONMENTAL PROTECTION AGENCY
                      Research Triangle Park, North Carolina

SUBJECT: Confirmation  of Mirex in Human Adipose Tissue          DATE: June 23, 1976
        Extracts
FROM:    Dr.  Robert G. Lewis, Chief
         Chemical Characterization Section, ACB/ETD  (MD-69)

TO:      Dr.  Frederick W. Kutz
         Ecological Monitoring Branch  (WH-569)
         OPP, Headquarters
             This  is  to  confirm my telephone transmittals to you of the results
         of  our confirmatory  analysis of mirex in human adipose tissue extracts
         received from the Michigan project on June  15, 1976.  Mirex was confirmed
         qualitatively and determined quantitatively in all five samples by each
         of  three independent methods; i.e. , photochemical, GC-low resolution
         mass spectrometry  (GC-LRMS) and GC-high resolution mass spectrometry
         (GC-HRMS) .  Data are presented below:

                       GC-ECD                   Mirex Concentration, ppm
         Sample I.D.   (Michigan)     Photochem. GC-ECD     GC-LRMS     GC-HRMS

                         0.5                0.4              0.5          0.7

             ^           1.3                0.8              0.7          0.9
            A
            jU           1.3             -  1.3              1.2          1.6

             j           0.4                0.3              0.2          0.4
             ui
            <3  .         1.2                0.4              0.8          1.2

             Samples  were received in .glass vials sealed with Teflon- lined caps.
         Volumes ranged from  3.6 to 14.6 ml.  Aliquots of 1 to 4.5 ml were with-
         drawn  for  photochemical confirmation.  In this procedure, the aliquot
         was added  to  10% diethylamine in hexane sufficient to make a total
         volume of  5 ml.  These solutions were analyzed for GC-ECD before and
         after  100  min. exposure in quartz tubes to  a 275W sunlamp.  Analytical
         conditions were  as follows:

             Instrument  — Tracer 222 -   Ni ECD

             Column — 183-cm x 4-mm  (i.d.) glass,  packed with 1.5% OV-17/1.95%
             OV-210 on 80/100 mesh Gas Chrom Q
                              2
             Attenuation —  10  x 8

             Carrier  Gas —  Ar/CH , 95:5

             Carrier  Flow — 75 ml/min

             Column temp —  200°C

             Detector temp — 270°C

             Inlet temp  — 225°C
EPA Form 1320-6 (Rev. 6-72)


                                     1-106

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     B.C. Current — 46% f.s.d. @ 102 x 128 D.C.

     Voltage — 50v
     Pulse Width — 5 ysec
     Pulse Rate — 150 usec
     Photochemical confirmation work was performed by R. C. Hanisch.

     Portions of each sample were taken for GC-LRMS analysis.  These
were concentrated to 100 pi by evaporation under a gentle stream of
nitrogen at room temperature.  Portions corresponding to ca. 50 ng of
mirex were injected into the GC-LRMS for determination of mass spectra
over the 195 to 560 amu range.  GC-LRMS confirmation was based on  (1)
correct absolute retention time; (2) presence of intense fragments at
270 m/e with 6-chlorine isotope cluster and at 235 m/e with 5-chlorine
isotope cluster (corresponded to the main electron impact fragments of
mirex); (3) presence of other fragments derivable from mirex; (4) absence
of possible interferring compounds; and (5) proper ratios of the 270 and
235 m/e clusters.  Quantitative GC-LRMS measurements were accomplished
through single ion monitoring of the 272 m/e peak and the use of an
external mirex standard.  All samples were analyzed in duplicate or
better.  Precision with standards was +10 to 15%.  GC-LRMS parameters
were as follows:

     Instrument:  Hewlett Packard 5930A quadrapole focusing mass spec-
     trometer equipped with an HP 5700A gas chromatograph and an HP
     5932A data system.                              _

     Column:  183-cm x 2-mm (i.d.) glass, packed with 3% OV-17 on 100/120
     mesh Gas Chrom Q.
     Carrier Gas:  Helium

     Flow rate:  41 ml/min
     Injection port temperature:  200°C

     Column temperature:  230°C
     Transfer line temperature:  250°C

     Membrane separator temperature:  230°C

     Ion source temperature:  190°C
     Mass filter temperature:  120°C

     lonization voltage:  70eV

     Filament emission:  160 yamp

     Ion source pressure:  2 x 10   mm Hg

-------
     Scan rate:  360 amu/sec

     GC-LRMS measurements were performed by G. W. Sovocool and M.
Simpson.

     The same concentrated samples used for GC-LRMS were also used for
GC-HRMS.  The mass spectrometer was operated at extreme sensitivity in
order to observe the molecular ion at 543.6203 m/e (corresponding to
C1035C11037C12).  Qualitative and quantitative analyses were performed
by double ion monitoring of the 539.6262 and molecular ions.  GC retention
times and internal standards were used for identification and quantifi-
cation.  GC-HRMS parameters are given below:

     Instrument:  Varian MAT 311A double focusing mass spectrometer
     equipped with a Varian gas cnromatograph and a Varian data system.

     Column:  91-cm x 2-mm (i.d.) glass, packed with 5% OV-101 on Gas
     Chrom Q.
     Carrier gas:  Helium

     Flow rate:  15 ml/min

     Column temperature:  235°C

     •Injection port, transfer line and separator temperatures:  250°C

     Ion source temperature:  220°C
     Ion source pressure:  5 x 10   mm Hg

     GC-HRMS measurements were performed by R. L. Harless.

     I trust that you will find these data useful.  If we can be of
further assistance, please call on us.
                            1-108

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                                   TECHNICAL REPORT DATA
                            (Please read Instructions on the reverse before completing)
1. REPORT NO.
 EPA 560/13-80-024
                              2.
                          3. RECIPIENT'S ACCESSION NO.
4. TITLE AND SUBTITLE
 Mirex Residue Levels in Human Adipose Tissue:
 Statistical Evaluation
                          5. REPORT DATE
                           November,
198$
ate of
Pfepara-
          r.on;
                          6. PERFORMING ORGANIZATION CODE
7. AUTHOR(S)
  Carol Leininger, Donna Lucas Watts,  Charles Sparacino,
  and Stephen^Williams
                          8. PERFORMING ORGANIZATION REPORT NO.
                           RTI/1864/17-01I
9. PERFORMING ORGANIZATION NAME AND ADDRESS
  Research Triangle Institute
  P.  0.  Box 12194
  Research Triangle Park,  NC  27709
                           10. PROGRAM ELEMENT NO.
                           11. CONTRACT/GRANT NO.

                           EPA contract 68-01-5848
12. SPONSORING AGENCY NAME AND ADDRESS
  Design and Development  Branch
  Exposure Evaluation  Division, Office of
  Toxic Substances,    U.S.  Environmental Protection Agencj
  401 M Street, SW, Washington, DC  20460
                           13. TYPE OF REPORT AND PERIOD COVERED
                               Final Report
                           14. SPONSORING AGENCY CODE
15. SUPPLEMENTARY NOTES
16. ABSTRACT
       Mirex is an  insecticide which has a specific geographic region  of  application
  in the United States.   The Mirex Special Study was undertaken in  1975 by the
  National Human Monitoring Program in an attempt to obtain information about the
  prevalence and levels  of mirex in human adipose tissues in areas  in  mirex application.
  A sample of human adipose tissue specimens was selected from mirex treated areas in
  eight southern States.   Detectable levels of mirex were found in  141 of 624 human
  adipose tissue specimens in the sample.  The data were analyzed with respect to three
  demographic variables  (race, age, and sex) and two geographic variables (Census
  Division and State).   Geographic divisions appear to be the most  salient factors in
  levels of concentration of mirex in the sample studied.
 7.
                                KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
                                              b.lDENTIFIERS/OPEN ENDED TERMS
                                        c.  COSATI Field/Group
  mirex
  fire ant control pesticides
  human  adipose tissues
  sample design
  gas chromatography
  regression analysis
  chi square analysis
unweighted
 statistical
  analysis
weighted
 statistical
  analysis
18. DISTRIBUTION STATEMENT
                                              19. SECURITY CLASS (This Report)
                                               unclassified
                                                                          21. NO. OF PAGES
                                              20. SECURITY CLASS (This page)
                                                unclassified
                                                                          22. PRICE
EPA Form 2220-1 (Rev. 4-77)   PREVIOUS EDITION is OBSOLETE

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        Include ZIP code.

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        Indicate interim final, etc., and if applicable, dates covered.

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        Insert appropriate code.

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        Enter information not included elsewhere but useful,  such as: Prepared  in cooperation with, Translation of, Presented'at conference of.
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        Include a brief (200 words or less) factual summary of the most significant information contained in the report. If the report contains a
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        (a) DESCRIPTORS - Select from the Thesaurus of Engineering and Scientific Terms the proper authorized terms that identify the major
        concept of the research and are sufficiently specific and precise to be used as index entries for cataloging.

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EPA Form 2220-1  (Rev. 4-77) (Reverse)

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