EPA/600/R-95/098
August 1996
THE PARTICLE TEAM (PTEAM) STUDY:
ANALYSIS OF THE DATA
FINAL REPORT
VOLUME DDE
by
H. Ozkaynak, J. Xue, R. Weker, D. Butler,
P. Koutrakis, and J. Spengler
Harvard University School of Public Health
Boston, MA 02115
Contract Number: 68-02-4544
Project Officer: A. Lindstrom
Atmospheric Research and Exposure Assessment Laboratory
Human Exposure and Field Research Division
Task Manager: L. Wallace
Atmospheric Research and Exposure Assessment Laboratory
Human Exposure and Field Research Division
Prepared for
Atmospheric Research and Exposure Assessment Laboratory
Office of Research and Development
United States Environmental Protection Agency
Research Triangle Park, NC 27711
Printed on Recycled Paper
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PREFACE
This is the final volume of a three-volume report on
exposures to inhalable particles of residents of the City of
Riverside, California. Volume Ia, prepared by Research Triangle
Institute (RTI), Research Triangle Park, NC, presented the study
design, methodology, and basic population-weighted statistics for
the particle and elemental concentrations. Volume IIb, prepared
by RTI for the Air Resources Board (ARE), State of California,
dealt with the polyaromatic hydrocarbon and phthalate results.
Volume III, prepared by the Harvard School of Public Health,
presents statistical and physical models for all physical
parameters monitored during the study.
a Pellizzari, E.D., Thomas, K.W., Clayton, C.A., Whitmore, R.W.,
Shores, R.C., Zelon, H.S., and Perritt, R.L. Particle Total
Exposure Assessment Methodology (PTEAM); Riverside, California
Pilot Study. Volume I. NTIS # PB 93-166-/957/AS. Springfield,
VA, 1993a.
b Sheldon, L., Clayton, A. Keever, J., Perritt, R. and Whitaker,
D. PTEAM; Monitoring of Phthalates and PAHs ih Indoor and
Outdoor Air Samples in Riverside, California. Volume II.
California Air Resources Board/ Sacramento, CA, 1992.
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ABSTRACT
The US EPA and the California Air Resources Board sponsored
the first probability-based survey of personal exposure to
inhalable particles (PM10) in Riverside, CA, in the fall of 1990.
178 participants, representing 139,000 nonsmoking Riverside
residents, carried newly-designed personal monitors for a day to
measure their exposure to particles, elements, and nicotine.
Concurrently, nearly identical monitors measured indoor and
outdoor concentrations of PM10, fine particles (PM2 5) , elements,
polyaromatic hydrocarbons (PAHs), and phthalates.
Population-weighted results for particles and elements were
reported in Volume I of this series, and for PAHs and phthalates
in Volume II. This volume is the third and last of the series.
It provides a statistical analysis of all the data, including the
nicotine and air exchange data.
The monitors displayed excellent precision, with median
relative standard deviations of 3-4%. The PM10 monitors had a
sharp cutpoint at 11 jLtm, and the PM2.5 monitors had a sharp
cutpoint at exactly 2.5 jum.
Daytime personal exposures to PM10 were more than 50% higher
than concurrent indoor or outdoor concentrations. Overnight
personal exposures were similar to the indoor and outdoor
concentrations. The increased personal exposures were not due to
exposures encountered while commuting or at work. Therefore it
is concluded that a "personal cloud" of particles can be created
iii
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by personal activities at home.' The composition of the personal
cloud was studied using x-ray fluorescence (XRF) and scanning
electron microscopy (SEM). The XRF analysis showed that 14 of 15
elements were elevated by large amounts (50-100%) in the personal
cloud. The SEM analysis indicated that skin flakes were
prevalent in many cases, but it is unclear how much they
contribute to the observed increase in mass.
A nonlinear method of solving the mass-balance indoor air
equation was developed and employed for the first time. The
method employed nonlinear least squares regression analysis to
estimate indoor penetration factors and decay rates for particles
and elements. The method was also used to estimate the strengths
of important indoor sources. According to this analysis, outdoor
sources contributed on average about 2/3 of the PMi0 mass
measured indoors, and about 3/4 of the indoor PM2.5. Most of the
remaining mass was supplied by unidentified indoor sources. The
two main identified indoor sources were smoking and cooking.
Each provided an average of about 20-30% of the total particle
mass in homes where the activity took place.
Indoor sources accounted for about half of the observed
variance in personal exposures, but outdoor sources could explain
only about 16% of the variance. Thus it does npt seem possible
to use outdoor measurements alone to reliably predict personal
exposure to PM10. Another investigation in a different part of
the country is desirable to test the accuracy and
generalizability of these conclusions.
iv
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TABLE OF CONTENTS
Preface iii
Abstract iv
Figures vii
Tables xvi
Abbreviations .... ...... xxv
Acknowledgements xxvi
1. Introduction 1-1
Major findings from Volume I 1-3
Major findings from Volume II 1-5
Objectives of Volume III 1-6
2. Conclusions 2-1
3. Recommendations 3-1
4. Survey Design, Methods, and Quality Assurance . . . 4-1
Survey design 4-1
Monitoring methods ...... 4-4
Quality of the data 4-11
Particles 4-11
Elements 4-19
PAHs and phthalates 4-32
Nicotine 4-35
Air exchange .,, 4-35
5. Statistical Analysis: Particles, Elements,
Nicotine, Air Exchange Rates 5-1
Description of data 5-1
Summary statistics . 5-8
Particles 5-8
Nicotine 5-17
Elements . 5-31
Air exchange 5-67
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Correlations 5-91
Analysis of variance ..... ............ 5-109
Simple regressions ............... 5-113
Multiple regressions .............. 5-123
Stepwise regressions 5-134
Particles and nicotine ........... 5-134
Elements 5^-146
Indoor source models .............. 5-154
"Personal cloud" calculations . . . . , . . . . . 5-170
6. Statistical Analysis: PAHs and Phthalates ..... 6-1
Frequencies of detection ............ 6-2
Summary statistics ............... 6^-6
Temporal trends and high values 6-32
Effect of activities .............. 6^54
Correlations .................. 6-^82
Factor analyses ... ..... 6-99
Analysis of variance .............. 6-102
Regressions . ............ 6-110
Physical model ................. 6-114
References ........................ 7-1
Appendices .
A. Comparison of PM10 monitoring methods ....... A-l
B. Study of storage stability of nicotine . ...... B-l
C. SEM screening of PTEAM samples ........... C-l
D. Air exchange data ................. D-l
E. Nicotine data ........... ^ E-l
F. Elemental data ... F-l
vx
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FIGURES
Figure Caption
2-1 Population-weighted inhalable particle (PM10)
concentrations 2-3
2-2 Increased concentrations of elements in
personal vs indoor filters . . 2-5
2-3 Proportion of PM10 and PM2.5 concentrations
due to various sources: all homes 2-7
2-4 Proportion of PM10 and PM2>5 concentrations
due to various sources: homes with smoking ...'... 2-8
2-5 Proportion of PM10 and PM2.5 concentrations
due to various sources: homes with cooking 2-9
2-6 Central-site vs residential outdoor monitors . . . . 2-12
2-7 Indoor vs outdoor PM10 concentrations ........ 2-13
2-8 Personal vs outdoor PM10 .............. 2-15
2-9 Personal vs indoor PM10 . 2-16
4-1
4-2
4-3
4-4
4-5
4-6
Duplicate measurements of residence times: ND = LOD . 4-40
Duplicate measurements of residence times: ND = LOD/2 4-41
Duplicate .measurements of air exchange: ND = LOD . . 4-42
Duplicate measurements of air exchange: ND = LOD/2 . 4-43
Duplicate measurements of air exchange
rates (logarithms) : ND = LOD ......
4-45
Duplicate measurements of air exchange
rates (logarithms) : ND = LOD/2 4-46
vii
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5-1
5-2
5-3
5-4
5-5
5-6
5-7
5-8
5-9
5-10
5-11
5-12
5-13
5-14
5-15
5-16
5-17
5-18
Population-weighted PM10 exposures compared to
unweighted data: cumulative frequency distributions of
12-hour average concentrations measured by Personal
Exposure Monitor (PEM) 5-7
Outdoor PM10 concentrations measured near homes by
Stationary Ambient Monitor (SAM) ..... 5-11
Indoor'PM10 concentrations measured in home by
Stationary Indoor Monitor (SIM) .... 5-11
Personal PM10 concentrations 5-12
Outdoor PM2.S concentrations 5-13
Indoor PM2.5 concentrations 5-13
Daytime personal, indoor, and outdoor PM10
concentrations: cumulative frequency distributions . 5-14
Overnight personal, indoor, and outdoor PM10
concentrations: cumulative frequency distributions . 5-14
Daytime indoor and outdoor PM2.5 concentrations:
cumulative frequency distributions 5-15
Overnight indoor and outdoor PM2.5 concentrations:
cumulative frequency distributions . 5-15
24-h personal, indoor, and outdoor PM10
concentrations: cumulative frequency distributions
5-16
24-h indoor and outdoor PM2.5 concentrations:
cumulative frequency distributions .... 5-16
Central-site particle concentrations compared to
those measured near residences using Stationary
Ambient Monitor (SAM) ...... ... 5-18
Nicotine: all measurements. Cumulative frequency
distribution 5-21
Nicotine: indoor measurements 5-22
Nicotine: personal measurements . . 5-23
Nicotine: personal and indoor measurements ..... 5-24
Personal nicotine distributions for persons
reporting exposure to environmental tobacco smoke
(ETS) vs those not reporting exposure 5-27
Vlll
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5-19
5-20
5-21
5-22
5-23
5-24
5-25
5-26
5-27
5-28
5-29
5-30
5-31
5-32
5-33
5-34
5-35
5-36
5-37
5-38
5-39
5-40
Indoor nicotine distributions for homes where smoking
was reported vs those with no smoking reported . . .
5-27
Regression on personal nicotine concentrations of
number of minutes exposed to ETS 5-29
Regression on indoor nicotine concentrations of
number of cigarettes smoked in house
during monitoring period 5-30
Boxplot: particles . . . 5-39
Boxplot: aluminum ..... 5-39
Boxplot: bromine .... .......... 5-40
Boxplot: calcium ...... 5-40
Boxplot: chlorine 5-41
Boxplot: copper .-....• 5-41
Boxplot: iron 5-42
Boxplot: potassium > • • • • 5-42
Boxplot: manganese 5-43
Boxplot: phosphorus . . ......... 5-43
Boxplot: lead 5-44
Boxplot: sulfur . 5-44
Boxplot: silicon 5-45
Boxplot: strontium 5-45
Boxplot: titanium . . . . . . • • •• • • 5-46
Boxplot: zinc 5-46
Aluminum: central-site concentrations compared
to those measured near residences 5-48
Bromine: central-site concentrations compared
to those measured near residences . 5-49
Calcium: central-site concentrations compared
to those measured near residences .......... 5-50
IX
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5-41 Chlorine: central-site concentrations compared
to those measured near residences ^ .. ^ ...... 5-51
5-42 Copper: central-site concentrations compared
to those measured near residences .......... 5-52
5-43 Iron: central-site concentrations compared
to those measured near residences . 5-53
5-44 Potassium: central-site concentrations compared
to those measured near residences .......... 5-54
5-45 Manganese: central-site concentrations compared
to those measured near residences ... . . 5-55
5-46 Phosphorus: central-site concentrations compared
to those measured near residences 5-56
5-47 Lead: central-site concentrations compared
to those measured near residences 5-57
5-48 Sulfur: central-site concentrations compared
to those measured near residences * 5-58
5-49 Silicon: central-site concentrations compared
to those measured near residences . . . 5-59
5-50 Strontium: central-site concentrations compared
to those measured near residences 5-60
5-51 Titanium: central-site concentrations compared
to those measured near residences 5-61
5-52 Zinc: central-site concentrations compared
to those measured near residences .......... 5-62
5-53 24-hour average air exchange rates: cumulative
frequency distributions employing two conventions
for treating values below the limit of detection . . 5-72
5-54 24-hour average residence times: cumulative frequency
distributions employing two conventions for treating
values below the limit of detection 5-72
5-55 Daytime and overnight air exchange rates, setting
undetected values equal to the limit of detection . . 5-76
5-56 Daytime and overnight air exchange rates,
setting undetected values equal to half
the limit of detection 5-76
x
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5-57
5-58
5-59
5-60
5-61
5-62
5-63
5-64
5-65
5-66
Daytime and overnight residence times, setting
undetected values equal to the limit of detection
5-77
5-67
5-68
5-69
5-70
Daytime and overnight residence times, setting
undetected values equal to half
the limit of detection 5-77
Daytime air exchange rates, employing two conventions
for treating values below the limit of detection . . 5-78
Overnight air exchange rates, employing two conventions
for treating values below the limit of detection . . 5-78
Daytime residence times, employing two conventions
for treating values'below the limit of detection . . 5-79
Overnight residence times, employing two conventions
for treating values below the limit of detection . . 5-79
Log-normal fit to 24-h average air exchange
rates: ND = LOD 5-81
Log-normal fit to 24-h average residence
times: ND = LOD 5-82
Gamma function fit to 24-h average air exchange
rates: ND = LOD 5-83
Normal fit to the logarithms of the daytime air
exchange rates: ND = LOD. The geometric
mean = e~°-u = 0.87. The geometric standard
deviation = e°-78 = 2.18 5-84
Normal fit to the logarithms of the overnight
air exchange rates: ND = LOD. The geometric
mean = e"°-25 = 0.78. The geometric standard
deviation = e°-68 =1.97 5-85
Normal fit to the logarithms of the 24-hour
air exchange rates: ND = LOD. The geometric
mean = e~0-14 = 0.87. The geometric standard
deviation = e°-66 =1.93 ,„.,-„. 5-86
Normal fit to the logarithms of the overnight
air exchange rates: ND = LOD/2. The geometric
mean = e"°-026 = 0.97. The geometric standard
deviation = e°-78 = 2.18 5-87
Air exchange rates: day, night and 24-hour
cumulative frequency distributions . 5-89
XI
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5-71
5-72
5-73
5-74
5-75
5-76
5-77
5-78
5-79
5-80
5-81
6-1
6-2
6-3
6-4
6-5
6-6
6-7
6-8
6-9
6-10
6-11
Air exchange rates: individual measurements
(N = 735) compared to 24-h averages (N = 175) .... 5-90
Indoor vs outdoor PM10 concentrations. Rz = 27% . . . 5-118
Personal vs indoor PM10. R2 = 49% .......... 5-121
Personal vs outdoor PM10. R2 = 16% 5-122
Central-site vs residential outdoor monitors.
R2 = 57% 5-124
Air exchange rates vs house volumes. R2 — 12% ... 5-125
Residence times vs house volumes. R2 — 10% ..... 5-126
Elements in the personal cloud ........... 5-174
Scanning electron microscopy (SEM) photograph
of a personal filter ................ 5-175
Scanning electron microscopy (SEM) photograph
of an indoor air filter ............... 5-176
Regression on personal PM10 exposure of ^number of skin
flakes counted on 138 personal filters ....... 5-181
Detection frequencies for nine PAHs . . . . . . . . . . 6-4
Detection frequencies for four PAHs
and five phthalates 6-5
Boxplot: acenapthylene . . ..... 6-10
Boxplot: phenanthrene ..... 6-10
Boxplot: anthracene ................. 6-11
Boxplot: fluoranthene 6-11
Boxplot: pyrene .......... 6-12
Boxplot: benzo(a)anthracene ............. 6-12
Boxplot: chrysene ..... 6-13
Boxplot: benzo(k)fluoranthene 6-13
Boxplot: benzo(e)pyrene * ..... 6-14
XII
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6-12
6-13
6-14
6-15
6-16
6-17
6-18
6-19
6-20
6-21
6-22
6-23
6-24
6-25
6-26
6-27
6-28
6-29
6-30
6-31
6-3-2
6-33
6-34
6-35
6-36
6-37
Boxplot: benzo(a)pyrene 6-14
Boxplot: indeno[123-cd]pyrene .... 6-15
Boxplot: benzo(ghi)perylene 6-15
Boxplot: coronene . 6-16
Boxplot: diethyl phthalate 6-16
Boxplot: di-n-butyl phthalate . 6-17
Boxplot: benzyl butyl phthalate 6-17
Boxplot: di-2-ethylhexyl phthalate .... 6-18
Boxplot: di-n-octyl phthalate 6-18
Histograms: acenapthylene . . . 6-19
Histograms: phenanthrene .... 6-20
Histograms: anthracene 6-21
Histograms: fluoranthene . . •» 6-22
Histograms: pyrene . .' . 6-23
Histograms: benzo(a)anthracene . 6-24
Histograms: chrysene 6-25
Histograms: benzo(e)pyrene . . 6-26
Histograms: benzo(a)pyrene . 6^27
Histograms: benzo(ghi)perylene 6-28
Histograms: coronene . • 6-29
Concentrations by monitoring period: acenapthylene . 6-33
Concentrations by monitoring period: phenanthrene . . 6-34
Concentrations by monitoring period: anthracene . . . 6-35
Concentrations by monitoring period: fluoranthene . . 6-36
Concentrations by monitoring period: pyrene . .... 6-37
Concentrations by monitoring period:
benzo(a)anthracene . 6-38
xiii
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6-38
6-39
6-40
6-41
6-42
6-43
6-44
6-45
6-46
6-47
6-48
6-49
6-50
6-51
6-52
6-53
6-54
6-55
6-56
6-57
6-58
6-59
6-60
Concent:
Concent]
Concent]
Concent]
indeno [ :
Concent]
benzo(gl
Concenti
Concenti
diethyl
Concenti
di-n-but
Concenti
benzyl 1
Concenti
di-2-etl
Boxplot
Boxplot
Boxplot
Boxplot
Boxplot
Boxplot
Boxplot
Boxplot
Boxplot
Boxplot
Boxplot
Boxplot
Boxolot
rati
rati
rati
rati<
L23-<
rati<
ii)p<
ratic
rati(
phtl
:ati(
:yl ]
:ati(
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ratic
iylh«
(by
(by
(by
(by
(by
(by
(by
(by
(by
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fbv
ons by m
ons by m
ons by m
Dns by m
3d]pyren<
Dns by m<
srylene
Dns by me
ans by m<
Dns by me
Dhthalat*
Dns by nu
L phthal<
Dns by me
sxyl phtl
smoking
smoking
smoking
smoking
smoking
smoking
smoking
smoking
smoking
smoking
smoking
smoking
smokincr
onitoring period: chrysene ....
onitoring period: benzo(e)pyrene .
onitorihg period: benzo(a)pyrene .
Dnitoring period:
a
Dnitoring period:
Dnitoring period: coronene ....
Dnitoring period:
Dnitoring period:
a
Dnitoring period:
ate *
Dnitoring period:
category)
category)
category)
category)
category)
category)
category)
category)
category)
category)
category)
category)
catecrorv)
acenapthylene ....
anthracene . . . .
f luorartthene
benzo( a) anthracene . .
benzo(k) fluoranthene .
benzo(e)pyrene ....
benzo(a)pyrene ....
indeno[123-cd]pyrene .
benzo(ghi)perylene . .
coronene
6-39
6-40
6-41
6-42
6-43
6-44
6-45
6-46
6-47
6-48
6-70
6-70
6-71
6-71
6-72
6-72
6-73
6-73
6-74
6-74
6-75
6-75
6-76
xiv
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6-61
6-62
6-63
6-64
6-65
Boxplot (by smoking category): diethyl phthalate
Boxplot (by smoking category): di-n-butyl phthalate
Boxplot (by smoking category):
benzyl butyl phthalate
Boxplot (by smoking category):
di-2-ethylhexyl phthalate . .
Boxplot (by smoking category):
di-n-octyl phthalate ....
6-76
6-77
6-77
6-78
6-78
xv
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TABLES
Table Title Page
4-1 Household Enumeration Sample Results 4-3
4-2 Monitoring Sample Results 4-5
4-3 Summary of Response Rates ..... 4-6
4-4 Change in Mass of Blank Filters and
Limits of Detection ...... 4-16
4-5 Distributions of Relative Standard Deviations (%)
of Duplicate Particle Samples ....... 4-18
4-6 Background Levels of Elements on
Field Blanks (ng/m3) 4-21
4-7 Weighted Estimates of Percent Measurable for
Individual (PEM) and Household
(SIM and SAM) Populations, by
Time of Day: Primary Elements ....... 4-23
4-8 Weighted Estimates of Percent Measurable for
Individual (PEM) and Household
(SIM and SAM) Populations, by
Time of Day: Secondary Elements 4;~24
4-9 Estimates off Percent Measurable for Temporal
Site Samples, by Time of Day:
Primary Elements . 4-25
4-10 Estimates off Percent Measurable for Temporal
Site Samples, by Time of Day:
Secondary Elements ....... 4-26
4-11 Duplicate Elemental Analyses: Median Relative
Standard Deviations (%) 4-29
4-12 PAHs and Phthalates: Blanks, Spikes,
and Duplicates . 4-33
4-13 Nicotine Duplicates (jug/m3) 4-36
4-14. Duplicate Air Exchange Rates:
Relative Standard Deviations and
Ratios to the Geometric Mean 4-37
xvi
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5-1
5-2
5-3
5-4
5-5
5-6
5-7
5-8
5-9
5-10
5-11
5-12
5-13
5-14
5-15
5-16
Number of Samples to Be Collected 5-3
Sample Collection Status . 5-4
Quality of 12-hr Aerosol Samples ... 5-6
Particle Concentrations (/zg/m3) . . . 5-9
Nicotine Concentrations (jug/m3) by Exposure to
Tobacco Smoke ....... 5-19
Particle and Nicotine concentrations (jug/m3) in
Homes with and Without Smokers: Day .... 5-32
Particle and Nicotine concentrations (/zg/m3) in
Homes with and Without Smokers: Night . . . 5-33
Nicotine and Particle Ratios: Day 5-34
Nicotine and Particle ratios: Night . . . . . . . 5-35
Concentrations of Particles (/zg/m3) and
Elements (ng/m3) 5-36
Median Mass and Elemental concentrations (ng/m3)
in Homes with and without Smokers: Night .
Median Mass and Elemental concentrations (ng/m3)
in Homes with and without Smokers: Day . .
Mean Mass and Elemental Concentrations (ng/m3)
in Homes with and without Smokers: Night .
Mean Mass and Elemental Concentrations (ng/m3)
in Homes with and without Smokers: Day . .
Ratios of Mean Elemental Concentrations in
Homes with and without Smokers
24-hr Air Exchange Rates and Residence Times
Using Different Conventions for Values
Below the LOD ,
5-63
5-64
5-65
5-66
5-68
5-71
XVI1
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5-17 12-hr Air Exchange Rates and Residence Times:
Day and Night (ND = LOD) 5-73
5-18 12-hr Air Exchange Rates and Residence Times:
Day and Night (ND = LOD/2) 5-74
5-19 Correlations of Outdoor Particles and Elements
Between Homes and the Central Site ..... 5-92
5-20 Correlations of Central-Site Particle and Element
Concentrations with Those Measured Outdoors
at Residences: PM2_5 Overnight . . . • . . . . 5-93
5-21 Correlations of Central-Site Particle and Element
Concentrations with Those Measured Outdoors
at Residences: PM2-5 Daytime 5-94
5-22 Correlations of Central-Site Particle and Element
Concentrations with Those Measured Outdoors
at Residences: PM10 Overnight 5-95
5-23 Correlations of Central-Site Particle and Element
Concentrations with Those Measured Outdoors
at Residences: PM10 Overnight ....... 5-96
5-24 Correlations between Nicotine Levels and Personal
and Indoor Concentrations of Particles and
Associated Elements 5-97
5-25 Correlations between Particle and Nicotine Levels
and Household Activities and
Characteristics: Daytime 5-99
5-26 Correlations between Particle and Nicotine Levels
and Household Activities and
Characteristics: Overnight • 5-100
5-27 Correlations between Particle and Nicotine
Levels and Household Activities and
Characteristics 5-101
5-28 Correlations of Covariates: Daytime . 5-103
5-29 correlations of Covariates: Overnight 5-105
xvnx
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5-30
5-31
5-32
5-33
5-34
5-35
5-36
5-37
5-38
5-39
Correlation Matrix of Covariates . 5-107
Correlations between Particle and Nicotine Levels
and Meteorological Variables (March AFB),
Activities, and Some Household
Characteristics: Daytime . 5-110
Correlations between Particle and Nicotine Levels and
and Meteorological Variables (March AFB),
Activities, and Some Household
Characteristics: Overnight ......... 5-m
Correlations between Particle and Nicotine Levels
and Activities, Household Characteristics,
and Meteorological Variables (March AFB) . . 5-112
Univariate ANOVA Results (Controlling for
Day-Night Effect) . . .
Multivariate ANOVA Results (Controlling for
Day-Night Effect)
Regression of Outdoor on Indoor PM10:
Particles and Elements ....
Regression of Outdoor on Indoor PM2.5:
Particles and Elements (ng/m3)
5-114
5-115
5-117
5-119
5-40
Regression on Personal Exposures of Time-Weighted
Indoor and Outdoor Concentrations of PM10
Particles and Associated Elements (ng/m3) . 5-129
Regression on Personal Exposures (For Persons
Spending >80% of Time at Home) of Indoor
and Outdoor Concentrations of PM10 Particles
and Associated Elements . 5-131
Regression on Personal Exposures (For Persons
Spending >50% of the Day Away from Home and
>20% of the Night Away from Home) of Indoor
and Outdoor Concentrations of PM10 Particles
and Associated Elements 5-132
xix
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5-41
5-42
5-43
5-44
5-45
5-46
5-47
5-48
5-49
5-50
5-51
5-52
Regression on Personal Exposures of Indoor and
Outdoor Concentrations of PMi0 Particles and
Associated Elements ............ 5-133
Stepwise Regression on Personal Exposures of Indoor
and Outdoor Concentrations of PM10
Particles and Elements 5-135
Stepwise Regression on Personal Exposure of Indoor
and Outdoor Concentrations of M10 and Elements
Weighted by Time Spent Indoors and Outdoors
Near Home 5-137
Stepwise Regression on Daytime Personal Exposure
of Indoor and Outdoor concentrations for
Persons Away from Home Most of Day ......
Stepwise Regression on Particles and Nicotine
of Activities, Household Characteristics,
and Meteorological Variables
Stepwise Regression on Particles and Nicotine of
Activities, Household Characteristics,, and
Meteorological Variables: Day and Night . .
Stepwise Regression on Particles and Nicotine of
Activities, Household Characteristics,
Meteorology, and Particle Concentrations . .
Stepwise Regression on Particles and Nicotine of
Activities, Household Characteristics,
Meteorology, and Indoor and Outdoor
Levels: Day and Night
Stepwise Regression on Particles and Nicotine of
Activities, Household Characteristics,
Meteorology, and Central Site Particle
Levels: Day and Night ...........
Stepwise Regression: Lead . .
Stepwise Regression: Sulfur .
Stepwise Regression: Bromine
5-138
5-139
5-141
5-142
5-144
5-145
5-147
5-148
5-150
xx
-------
5-53
5-54
5-55
5-56
5-57
5-58
5-59
5-60
5-61
5-62
5-63
5-64
5-65
5-66
5-67
Stepwise Regression: Silicon 5-151
Stepwise Regression: Chlorine 5-152
Stepwise Regression: Titanium . 5-153
Penetration Factors, Decay Rates, and
Source Strengths: Nonlinear Estimates . . . 5-157
Estimated Penetration Factors, Decay Rates
and Source Strengths: Daytime ....... 5-159
Estimated Penetration Factors, Decay Rates
and Source Strengths: Overnight 5-160
Percent of Particle and Elemental Mass Due to
All Sources in All Homes 5-162
Percent of Particle and Elemental Mass Due to
All Sources in Homes with Smoking 5-164
Percent of Particle and Elemental Mass Due to
All Sources in Homes with Cooking 5-165
Percent of Particle and Elemental Mass Due to
"Other" Sources in Homes with
No Smoking or Cooking 5-166
Fine Particle and Elemental Emission Rates
from Indoor Sources Calculated Using
the Koutrakis Model 5-169
Comparison of Estimated Source Strengths Due
to Cigarettes: PTEAM Results vs.
New York State . 5-171
Regression on Personal Cloud of Fine and
Coarse Fractions 5-181
Regression on Personal Cloud of Time in
Microenvironments: Daytime 5-184
Regression on Personal Cloud of Time in
Microenvironments: Overnight 5-185
xxi
-------
5-68
5-69
6-1
6-2
6-3
6-4
6-5
6-6
6-7
6-8
6-9
6-10
6-11
6-12
6-13
Particle concentrations in Homes with and
without Pets: Overnight .... 5-186
Particle concentrations in Homes with and
without Pets: Daytime 5-187
Frequencies of Detection of PAHs and Phthalates
PAH and Phthalate Concentrations (ng/m3) . . .
6-3
6-7
Homes with High PAH and Phthalate
Concentrations (ng/m3) 6-49
/
Homes with High PAH and Phthalate Concentrations 6-52
PAH and Phthalate Concentrations (ng/m3)
by Cooking Status 6-55
Homes Using Aerosol Sprays vs No-Spray Homes:
PAH and Phthalate Concentrations (ng/m3)
6-57
PAH and Phthalate concentrations (ng/m3) by
House Cleaning Status . 6-59
Homes with and without Reported Cooking: Student's
t Test on Indoor Concentrations (ng/m3) . .
6-61
Homes with and without Aerosol Spray
Activities: Student's t Test on Indoor
Concentrations (ng/m3) 6-62
Homes with and without House Cleaning Activities:
Student's t Test on Indoor
Concentrations (ng/m3) . . 6-63
PAH and Phthalate Concentrations (ng/m3) by
Reported In-Home Smoking Status ...... 6-64
Homes with and without Smoking: Student's t Test
on Indoor Concentrations (ng/m3) . . . . . . 6-66
PAH and Phthalate Concentrations (ng/m3) by
Proximity to Busy Roadways 6-68
xxi i
-------
6-14 Homes with Cooking vs Homes without Cooking:
Student's t Test on Ratios of
Indoor/Outdoor Concentrations 6-79
6-15 Homes Using Aerosol Sprays vs No-Spray Homes:
Student's t Test on Ratios of
Indoor/Outdoor Concentrations 6-80
6-16 Homes with and without House Cleaning Activities:
Student's t Test on Ratios of
Indoor/Outdoor Concentrations 6-81
6-17 Homes with Smokers vs Homes without Smokers:
Student's t Test on Ratios of
Indoor/Outdoor Concentrations . . 6-83
6-18 Correlations between Indoor and Outdoor PAH
Phthalate Concentrations . . . . 6-84
6-19 Pearson Correlations of Logarithms of Indoor PAH
and Phthalate Concentrations: Overnight . . 6-85
6-20 Pearson Correlations of Logarithms of Indoor PAH
and Phthalate Concentrations: Daytime . . . 6-88
6-21 Pearson Correlations of Logarithms of Indoor PAH
and Phthalate Concentrations with PM2-5 Mass
and Elements: Overnight 6-91
6-22 Pearson Correlations of Logarithms of Indoor PAH
and Phthalate Concentrations with PM2-5 Mass
and Elements: Daytime 6-93
6-23 Pearson Correlations of Logarithms of Indoor PAH
and Phthalate Concentrations with PM10 Mass
and Elements: Overnight 6-95
6-24 Pearson Correlations of Logarithms of Indoor PAH
and Phthalate Concentrations with PM10 Mass
and Elements: Daytime 6-97
6-25 Factor Loadings of Indoor PAHs and Phthalates . . 6-100
6-26 Factor Loadings of Indoor PAHs and Phthalates
(Day and Night Combined) 6-101
xxi 11
-------
6-27
6-28
6-29
6-30
6-31
6-32
6-33
6-34
6-35
6-36
6-37
Factor Loadings of Indoor PAHs, Phthalates, and
PM2>5 Mass and Elements: Daytime 6-103
Factor Loadings of Indoor PAHs, Phthalates, and
PM2.s Mass and Elements: Overnight 6-104
Factor Loadings of Indoor PAHs, Phthalates, and
PM10 Mass and Elements: Overnight ..... 6-105
Factor Loadings of Indoor PAHs, Phthalates, and
PM10 Mass and Elements: Overnight 6-106
ANOVA Analyses of PAH and Phthalate Data .... 6-107
Simple Regression of Outdoor PAH and
Phthalate Concentrations on Indoor
Concentrations (ng/m3) . 6-111
Simple Regression of Smoking on PAH and Phthalate
Concentrations (ng/m3) . . . 6-112
Multiple Regression of Outdoor Concentrations
(ng/m3) and Smoking Indicator (No. of
Cigarettes Smoked In Home) on Indoor PAH and
Phthalate Concentrations . . 6-113
Physical Model for Estimating Indoor Penetration
Decay Rates, and Source Strengths for
PAHs and Phthalates 6-115
Penetration Efficiencies, Decay Rates, and Indoor
Source Strengths for PAHs and Phthalates . . 6-116
Estimated Percent Contributions to PAH
Concentrations from Various Sources .... 6-119
xxiv
-------
Variables used in Statistical Analysi
H—
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outdoor particle concentration near home (Station?
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indoor particle concentration at home (Stationary 1
personal concentration (Personal Exposure Monitc
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outdoor particle concentration at the central (or ter
particle PM 10 concentration at the central site
time weighted PM10 concentration near home
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presence or absence of pets at home
measured air exchange rate
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number of cigarettes smoked during monitoring at
total time of house activities during monitoring
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in minutes (including vacuuming, dusting, cleanin
age of house
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vacuuming during monitoring at home in minutes
house volume (m3)
VACUUM
VOLUME
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dusting during monitoring at home in minutes
cooking during monitoring at home in minutes
dirt factor (0: very clean home, 1 : clean, 2: somew
DUST
COOK
DIRTLVL
percentage of floor coverage by carpets
temperature at March AFB in degrees Fahrenheit
1—
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dew point at March AFB in degrees Fahrenheit
inverse of house volume (1/m3)
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XXV
-------
ACKNOWLEDGEMENTS
Many scientists and technicians were required to carry out a
study of the magnitude of the Particle TEAM Study. Most of these
persons have been individually acknowledged in Volumes I and II.
The field portion of this study was conducted collaboratively
between Research Triangle Institute, Harvard University, and
Accurex, Inc. We are grateful to Robert Stevens and his
colleagues at EPA's Atmospheric Research and Exposure Assessment
Laboratory and Mantech, Inc. for providing the XRF analysis and
the SEM screening.
xxvi
-------
INTRODUCTION
A full description of the PTEAM study design and monitoring
methods is provided in Volume I. Briefly, a newly-designed
personal exposure monitor (PEM) was developed and tested in a
1989 pilot study (Anderson et al., 1989; Clayton et al., 1991;
Ozkaynak et al., 1990; Research Triangle Institute and Harvard
School of Public Health 1990a,b,c; Spengler et al., 1989; Wiener
1988, 1989; Wiener et al., 1990). The redesigned monitor was
then provided to 178 Riverside residents in the period Sept. 22,
1990 through Nov. 9, 1990. The residents wore the monitor for
two consecutive 12-hour periods (day and night). The PEM
collected inhalable particles (less than 10 /zm aerodynamic
diameter) on a Teflon filter. Inhalable particles, or PM10, is
the size fraction that is regulated (Federal Register, 1987) by
the Environmental Protection Agency (EPA).
Concurrently, nearly identical monitors collected both the
inhalable (PM10) and fine (PM2-5) particle fractions indoors at the
subject's home and outdoors near his or her home. The indoor and
outdoor monitors were identical, and differed from the PEM only
in the type of pump employed. The indoor monitor was dubbed the
SIM (for stationary indoor monitor), and the outdoor monitor was
called the SAM (for stationary ambient monitor). All filters
were weighed to determine the mass of particles collected, and
1-1
-------
were subsequently analyzed by x-ray fluorescence (XRF) to
determine concentrations of elements.
The PEM and SIM monitors included an extra filter treated
with citric acid to trap nicotine in both the vapor and particle
phase.
At 120 homes, indoor samples of air were collected over the
two 12-h periods and analyzed for polyaromatic hydrocarbons
(PAHs) and phthalates. At 60 of these homes, concurrent outdoor
samples were collected and analyzed.
Air exchange measurements were made at all homes using
multiple perfluorocarbon tracers (PFTs).
A central location in Riverside was equipped with a pair of
the newly-designed monitors (one PEM and one SAM); a pair of
high-volume Wedding samplers; and a pair of moderate-volume
dichotomous samplers. The Weddings and dichots were equipped
with size-selective inlets to collect inhalable particles. These
samplers operated throughout the 48 days of the study, collecting
96 12-hour samples each. This allowed an extensive side-by-side
field comparison of the newly designed monitors with existing
reference monitors.
Over 95% of the personal and stationary particle, nicotine
and air exdhange samples were successfully collected, and over
90% of the PAH/phthalate samples were collected. The population-
weighted summary statistics for particles and elements are
provided in Volume I, and for PAH/phthalates in Volume II.
1-2
-------
MAJOR FINDINGS FROM VOLUME I
The newly-designed personal monitors were found to be highly
precise (median 4% relative standard deviation), with a 10%
positive bias compared to the dichotomous reference sampler,
based on 96 consecutive 12-hour samples collected by two of the
new monitors collocated with two dichots.
The major finding from Volume I was significantly increased
daytime personal exposures compared to indoor and outdoor
concentrations. Population-weighted personal air concentrations
of PM10 averaged 150 + 9 (SE) /Ltg/m3 during the day, compared to
values of 95 ± 6 fJ>g/m3 for both the indoor and outdoor
concentrations. At night, the personal concentrations were
similar to indoor and outdoor levels, suggesting that daytime
activities caused the increase in some way. A similar increase
was noted for 14 of the 15 elements, suggesting that at least a
portion of the "personal cloud" was made up of an aerosol similar
in composition to the indoor and outdoor aerosols. Another
portion of the personal cloud could be due to the shedding of
skin flakes from the subject or fibers from his or her clothes.
This possibility was investigated by scanning electron microscopy
(SEM) of several filters. SEM microphotographs detected flakes
but not fibers on most filters. However, the contribution to the
1-3
-------
mass of these skin flakes is difficult to estimate, due to their
unknown thickness and density.
Another significant finding was that about 25% of the
volunteers were exposed to 24-h average PM10 values exceeding 150
ftg/m3, although none of the central-site monitors recorded a 24-
hour outdoor average exceeding the NAAQS.
Personal PM10 concentrations were fairly well correlated
with indoor levels (Spearman r « 0.7), and indoor levels were
somewhat less well correlated with outdoor levels (r « 0.5).
However, personal levels were not well correlated with outdoor
levels (r ~ 0.4). A linear regression of the personal exposures
on the outdoor (back yard) concentrations yielded a large nonzero
intercept, a slope of about 0.5, and an jR2 of only 16%. It was
concluded that measurements of ambient air would be unable to
predict personal exposure to PM10 for most persons.
Although only about 22 of the 178 homes included smokers, it
was possible to detect an increase of about 30 jug/m3 in the PM1Q
levels in those homes. Indoor concentrations were also increased
in homes where some cooking occurred.
Several peer-reviewed journal articles discussing these and
other findings from Volume I have appeared (Clayton et al.,,
1993; Thomas et al., 1993). Results have also been presented at
national and international meetings (Ozkaynak et al., 1993;
Perritt et al., 1991; Wallace et al., 1991a,b, 1993). A summary
of Volume I is available from EPA (Pellizzari et al., 1993b).
1-4
-------
MAJOR FINDINGS FROM VOLUME II
Both indoor and outdoor levels for the PAHs were generally
very low. The more volatile 3- and 4-ringed PAHs
(acenaphthylene, fluoranthene, and pyrene) had median
concentrations in the 1-10 ng/m3 range, whereas the less volatile
5- to 7-ringed species were an order of magnitude lower.
Benzo[a]pyrene, for example, had median outdoor levels of 0.1
ng/m3 during the day, and 0.2 ng/m3 at night. In general,
overnight ambient concentrations were considerably higher than
daytime levels, perhaps due to photodegradation occurring during
the day. Indoor source strengths for all the PAHs were very low,
with median values of 0.01 to 0.2 ng/h. Homes with smokers had
significantly elevated levels of some PAHs.
By contrast, four of the five phthalates were elevated
indoors by factors of 2 (diethylphthalate) to 16 (di-n-
butylphthalate). Only di-n-octylphthalate had median
indoor/outdoor ratios close to 1. Estimated median indoor source
strengths for the four prevalent phthalates ranged from 7-92
jitg/h. No activities could be identified as potential sources of
the higher concentrations.
As yet, no peer-reviewed articles have been prepared on the
results of Volume II. Results were presented at one
international meeting (Sheldon et al., 1993) and one regional
meeting (Jenkins et al., 1992).
1-5
-------
OBJECTIVES OF VOLUME III
The overall goal of the work reported on here was to
determine the most important relationships between the physical
parameters, indoor-outdoor locations, and personal activities.
The individual objectives supporting that goal were
1) Complete the chemical analysis of the nicotine filters
and the tracer gas passive samplers (to measure air
exchange rates).
2) Determine correlations among the physical and chemical
parameters.
3) Statistically analyze relations between the parameters
and indoor-outdoor locations and personal activities.
4) Identify the most important sources of indoor
particles, elements, nicotine, PAHs and phthalates.
5) Use a physical model to determine decay rates,
penetration coefficients, and source strengths for
those sources identified in (4) above for particles,
elements, PAHs and phthalates.
1-6
-------
CONCLUSIONS
The PTEAM Study is the first probability-based study of
personal exposure to particles. The 178 participants represented
139,000 nonsmoking residents of Riverside, CA over the age of 10.
The primary objective of the study was to determine the
distribution of personal exposures to particles in a community.
To achieve this objective, it was necessary to design and
construct a personal monitor that could be worn comfortably for
up to 14 hours by persons from 10 to 80 years old. The monitor
consists of a 4L/minute battery-operated Casella pump, with a
lightly greased impactor plate and a sampling nozzle designed to
give a sharp cut at 10 /zm aerodynamic diameter (PM10) . The
actual cutpoint was found to be 11 im. A backup filter treated
with citric acid is used to collect vapor-phase nicotine. The
monitor is contained in a soft pack that can be adjusted to be
worn on the side, back, or front. The sampling head is mounted
at chest height on a Sam Browne shoulder belt. Sixteen such
monitors were constructed and employed in the study. The
monitors were both rugged and precise. Over 95% of the planned
samples were collected, with a median precision of 4%.
Nearly identical monitors were employed to collect
concurrent indoor and outdoor samples. They differed from the
personal monitors only in the type of pump, which was operated
from line current. Also, a second sampling nozzle was supplied
2-1
-------
to give a sharp cut at 2.5 jum aerodynamic diameter (fine
particles, or PM2.5) .
These indoor and outdoor monitors provided similar
dependable and precise collection characteristics. More than
2750 particle samples were collected, about 96% of those
attempted. More than 550 nicotine samples were collected. More
than 1000 12-h average air exchange rate measurements were made,
including 273 duplicate pairs, with a median precision of 8%.
The personal exposures of the community were determined for
the period from late September to early November, 1990.
Population-weighted daytime personal exposures averaged 150 ± 9
(SE) jug/m3, compared to concurrent indoor and outdoor
concentrations of 95 + 6 jig/m3 (Figure 2-1) . Overnight personal
exposures, which included the sleeping period (the monitor was
placed on the bedside table), were much more similar to the
indoor and outdoor concentrations (77 ±4, 63+3, and 87+4
/ig/m3, respectively) . (Similar results were obtained for the
unweighted data, reported in this volume.) About 25% of the
population were estimated to have 24-h personal exposures in
excess of 150 jug/m3, even though no outdoor sample exceeded this
value during the 48 days of the study.
The more than 50% increase in daytime personal exposures
compared to concurrent indoor or outdoor concentrations suggested
that personal activities were important determinants of exposure.
However, the nature of this "personal cloud" of particles has not
yet been determined. Scanning electron microscopy was undertaken
2-2
-------
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2-3
-------
on 138 personal filters. Skin flakes were common on many
filters. A preliminary analysis suggested that the average
number of skin flakes per filter was 120,000-150,000. The mass
of some personal filters may have been considerably increased by
unusually large numbers of skin flakes. However, attempts to
calculate the mass of skin flakes from estimates of their volume
and density suggest an average contribution to the mass of only
about 4 #g/m3, less than 10% of the mass of the average personal
cloud.
Another approach to the composition of the personal cloud is
elemental analysis, using x-ray fluorescence. Analysis of all
personal and indoor filters showed that 14 of 15 elements were
elevated, by values of 50-100%, in the personal filters compared
to the indoor filters (Figure 2-2). This observation suggests
that a component of the personal cloud is an aerosol of the same
general composition as the indoor aerosol. This could be
particles created by activities (e.g., cooking) or re-entrained
household dust from motion (walking across carpets, sitting on
upholstered furniture).
The existence of the personal cloud is the major finding
from the PTEAM study, and the determination of its composition is
one of the major research needs emanating from the study.
A nonlinear mass-balance method to estimate penetration
factors, decay rates, and source strengths for particles and
elements from both size fractions was developed and applied for
the first time. This method improved on previous formulations in
2-4
-------
M
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2-5
-------
making fewer arbitrary assumptions and solving for all unknown
parameters simultaneously. An interesting result from this
effort was the finding that the penetration factor was very close
to 1 for nearly all particles and elements. Decay rates were
0.39 ± 0.17 h"1 for fine particles and 0.65 ± 0.28 h"1 for PM10.
Outdoor air was the major source of indoor particles,
providing about 3/4 of fine particles and 2/3 of inhalable
particles in the average home (Figure 2-3). It was also the
major source for most elements, providing 70-100% of the observed
indoor concentrations for 12 of the 15 elements. Only copper and
chlorine were predominantly due to indoor sources in both the
fine particle and inhalable particle fractions.
Unidentified indoor sources accounted for most of the
remaining particle and elemental mass collected on the indoor
monitors. The nature of these sources is not yet understood.
They do not include smoking, other combustion sources, cooking,
dusting, vacuuming, spraying, or cleaning, since all these
sources together account for less than the unidentified sources.
For example, the unidentified sources accounted for 26% of the
average indoor PM10 particles, whereas smoking accounted for 4%
and cooking for 5%.
Of the identified indoor sources, the two most important
were smoking and cooking (Figures 2-4 and 2-5). Smoking was
estimated to increase 12-h average indoor concentrations of PM10
and PM2.S by 2 and 1.5 /ig/m3 per cigarette, respectively. Homes
with smokers averaged about 30 ]ug/m3 higher levels of PM10 than
2-6
-------
INDOOR FINE PARTICLE MASS
IN ALL HOMES
Outdoor
76%
Cooking
4%
Other indoor
Smoking
5%
N • 352 samples from 178 homes
INDOOR PM-10 MASS
IN ALL HOMES
Outdoor
66%
Cooking
5%
Other indoor
26%
Smoking
4%
' • 350 Samples from 178 homes
Figure 2-3. Sources of-particles: all homes.
2-7
-------
r
INDOOR FINE PARTICLE MASS
IN HOMES WITH SMOKING
Cooking
indoor
7%
Outdoor
60%
Smoking
30%
N • 61 Samples from 31 homes
INDOOR PM-10 MASS
IN HOMES WITH SMOKING
Cooking
3%
Outdoor
56%
Other indoor
16%
Smoking
24%
N » 61 Samples from 31 homes
Figure 2-4. Sources of particles: homes with smoking.
2-8
-------
INDOOR FINE PARTICLE MASS
IN HOMES WITH COOKING
Outdoor
62%
Cooking
25%
Other indoor
8%
Smoking
5%
N » 62 Samples from 33 homes
INDOOR PM-10 MASS
IN HOMES WITH COOKING
Outdoor
56%
Cooking
25%
Other indoor
16%
Smoking
4%
N • 82 Samples from 33 homes
Figure 2-5. Sources of particles: homes with cooking.
2-9
-------
homes without smokers. Most of this increase was in the fine
fraction. Cooking increased indoor concentrations of PM10 by
about 6 /ng/m3 per hour, with most of the increase in the coarse
particles.
Emission profiles for elements were obtained for smoking and
for cooking. Major elements emitted by cigarettes were potassium
and chlorine, with smaller amounts of bromine and sulfur, as
determined in previous studies. Calcium was also indicated as a
possible constituent of cigarette smoke.
Elements associated with cooking included aluminum, iron,
calcium, and chlorine. This appears to be the first study to
obtain emission profiles for cooking.
Other household activities such as vacuuming and dusting
appeared to make smaller contributions to indoor particle levels.
An interesting finding was that commuting and working outside the
home resulted in lower particle exposures than for persons
staying at home.
A central site was maintained with two pairs of reference
method monitors (Sierra-Anderson dichotomous samplers and Wedding
high-volume samplers) operated side by side with the newly-
designed personal and indoor samplers for the 48 days of the
study. This allowed a test of the accuracy of the new samplers
as well as a test of the ability of one central station to
characterize outdoor concentrations throughout a neighborhood.
The results of the side-by-side methods comparison are
provided in an Appendix to this report. Briefly, the dichotomous
2-10
-------
and personal-indoor samplers showed good precision/ with the new
samplers having a positive bias of about 12% compared to the
dichotomous samplers. This bias may be partly due to somewhat
different outpoints (about 11.0 jum for the new samplers, 9.5 ^m
for the dichotomous inlets) and partly to a small amount of
particle "bounce" from the impactor plates on the new samplers
(measured at about 9% in laboratory studies). No effects of
temperature, wind speed, or other phenomena were noted on these
two types of monitors. However, an effect of temperature was
seen on the Wedding instruments, which showed an increase in
concentrations of about 1% per °F. The Weddings also appeared to
respond adversely to cleaning, with concentrations dropping by an
average of 14% after cleaning and then building up again until
the next cleaning (done at 5-day intervals in this study.) These
two effects should be further studied.
The central site appeared to be a moderately good estimator
of outdoor concentrations throughout the city. Spearman
correlations of the central-site concentrations measured by all
three methods with outdoor near-home concentrations as measured
by the new samplers ranged from 0.8 to 0.85 (p<0.00001). Linear
regressions indicated that the central-site readings could
explain about 60% of the variance observed in the near-home
outdoor concentrations (Figure 2-6).
Outdoor concentrations could explain about 25-30% of the
variance observed in indoor concentrations (Figure 2-7).
Spearman correlations of near-home outdoor concentrations with
2-11
-------
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2-13
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indoor concentrations ranged from 0.5 to 0.6. Spearman
correlations of the central-site outdoor concentrations with
indoor concentrations were reduced somewhat (about 0.45 to 0.55).
Outdoor concentrations were able to account for only about
16% of the variance in personal exposures (Figure 2-8). This is
understandable in view of the importance of indoor activities
such as smoking, cooking, dusting, and vacuuming on exposures to
particles. The higher daytime exposures were even less well
represented by the outdoor concentrations, whether measured near
the home or at the central site.
Indoor concentrations accounted for about half of the
variance in personal exposures (Figure 2-9). However, neither
the indoor concentrations alone, nor the outdoor concentrations
alone, nor time-weighted averages of indoor and outdoor
concentrations could do more than explain about 2/3 of the
observed variance in personal exposures. The remaining portion
of personal exposure must arise from personal activities or
unmeasured microenvironments that are not well represented by
fixed indoor or outdoor monitors.
2-14
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2-16
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Note Added in Proof.
Possible Explanation of Low Nicotine Readings
Following completion of this report, a paper was published
(Lofroth, 1995) that showed considerable losses of nicotine to
the first (particle) filter if the cigarette smoke was aged and
if the initial filter was slightly acidic. It is thought that
nicotine in aged cigarette smoke may not be as overwhelmingly in
the vapor phase as in fresh cigarette smoke. Since the tandem
filters used in the PTEAM Study were tested in chambers employing
fresh cigarette smoke, no losses were observed. However, in view
of the Lofroth paper, it is possible that the nicotine values
reported in Section 5 are erroneously low. The magnitude of the
error cannot be estimated; however, Lofroth reported losses
greater than 50% in some of the typical indoor microenvironments
he tested.
Lofroth, G. "Phase distribution of nicotine in real environments
as determined by two sampling methods." Environ. Sci. Tech.
29:975-978, 1995.
2-17
-------
-------
RECOMMENDATIONS
This initial study of personal exposure to particles has
resulted in a number of interesting findings. However, which of
these are truly general and which are particular to the southern
California area studied cannot be determined until a second study
is carried out in a different region of the country. In
particular, since Riverside has one of the highest outdoor
concentrations of inhalable particles in the country, how would
the findings be affected if a study were carried out in a region
with a more nearly typical outdoor air PM10 concentration?
It may be speculated that in such more nearly typical
regions, the effect of the personal cloud on total exposure would
be enhanced. Moreover, the effect of indoor air sources such as
cooking and smoking should also be enhanced compared to the
effect of outdoor sources. However, the extent of these effects
can only be determined by carrying out a study.
The second PTEAM study should probably be carried out in an
Eastern city, since much of the urban population resides in the
East. Also, the nature of the atmospheric pollution is
different, including much more effect of sulfates, and perhaps
less of secondary aerosol production, than in the West. In view
of the recent findings of an effect on daily mortality of
atmospheric particles, the study could be situated in a city of
sufficient population size to have a fairly large and stable
number of deaths per day. A city with a record of daily outdoor
3-1
-------
measurements would be preferable to one with only every-sixth-day
measurements. One city that meets these requirements is
Philadelphia, where the effect of outdoor particles on daily
mortality has already been studied, and where an EPA research
program has collected daily outdoor concentrations for more than
one year.
It is recommended thai: consideration be given to mounting a
second PTEAM study in an Eastern city to verify and extend the
conclusions of the first PTEAM study.
The major finding of the PTEAM Study was the existence of
the "personal cloud," a significant source of additional personal
exposure over and above the concurrent indoor air concentrations.
The source and composition of the "personal cloud" remains
unclear. Two possible sources are re-entrained household dust
and skin flakes.
It is recommended that targeted studies to characterize the
source and composition of the "personal cloud" be carried out.
These studies should include investigations of the influence of
re-entrained household dust, and the mass associated with human
dander. The latter study could profitably employ scanning
electron microscopy or other advanced methods to determine the
mass of a single skin flake.
3-2
-------
Indoor sources contributed substantially to the total indoor
air concentration, even in Riverside, where outdoor air levels
"were extremely high. However, the exact nature of the indoor
sources remains unclear. Two important sources were cooking and
smoking; however, together they accounted for less than 25% of
the total mass due to indoor sources. Other identified sources,
such as dusting, vacuuming, cleaning, and spraying, accounted for
much less of the total. Therefore the source or sources for the
bulk of the indoor source-related concentrations remains to be
identified.
It is recommended that special studies be carried out to
determine the main indoor source of indoor air particles in homes
without cooking, smoking, or other identified sources.
The 48-day side-by-side test of the Wedding hi-volume
samplers suggested that they respond adversely to temperature
changes and to the intensive cleaning cycle adopted for the
study. These findings need to be validated and investigated to
understand the physical principles at work.
It is recommended that the Wedding hi-volume samplers be
studied for an effect of temperature and cleaning on performance.
3-3
-------
-------
SURVEY DESIGN, MONITORING METHODS, AND QUALITY ASSURANCE
In this section, brief discussions will be provided of the
survey design and monitoring methods employed in the PTEAM Study.
More complete descriptions are provided in Volume 1. These brief
discussions are included to make Vol. 3 more nearly self-
contained.
Volume 1 also includes full descriptions of the quality
control and quality assurance procedures and results for most of
the measurement methods. The main results for the particles and
elements will be presented here. However, results from the
nicotine and air exchange methods were not available when Volume
1 was written; therefore they will be discussed at greater length
here. Also, an extensive comparison of the three particle
monitoring methods employed at the central site for the 48 days
of the study has been undertaken and is included in this section.
Finally, a nicotine storage stability study was undertaken
following the completion of the field study and results are
reported here.
SURVEY DESIGN
The PTEAM Study was based on a probability sampling design.
Probability sampling methods are the only accepted approach for
making inferences from a sample to the target population (Hansen
4-1
-------
et al., 1983; Williams et al., 1983). Probability sampling also
provides the basis for calculating the standard errors of survey
statistics.
Nonsmokers above the age of 10 in the city of Riverside were
included. Smokers were excluded because their particle exposures
would be overwhelmed by the particles in mainstream cigarette
smoke. Children under 10 were excluded because of the burden of
carrying the personal monitor.
A multistage area household sampling design was used. In
the first stage, 36 geographic areas were selected randomly on
the basis of population size using a probability minimum
replacement sequential sampling algorithm (Chromy, 1979). The
sampling frame was stratified by geographic area, housing unit
values, and prevalence of detached, single-family dwellings.
Four geographic strata were defined using the Riverside Freeway
as one boundary and a north-south line through the middle of the
city as the other. Housing unit values were determined by
combining the 1980 Census data for owned and rented housing
units. The proportion of detached single-family dwellings was
also determined from Census data.
In the second stage, 780 dwellings were selected from the 36
areas. These were contacted in "waves", such that a total of 175
target dwellings would be attained. The full sample was obtained
early, and only 680 dwellings were contacted. Of these, 632
eligible sample housing units were identified, with 443 (70.1%)
completing the initial screening interview (Table 4-1).
4-2
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In the final stage, 257 sample persons were selected for
particle and element monitoring. (A subsample of 181 housing
units were selected for indoor phthalate and PAH monitoring, and
of these, a subsubsample of 98 units were selected for outdoor
phthalate and PAH monitoring.) Of the 257 persons, 191 (74.3%)
completed their questionnaires and consented to monitoring (Table
4-2). However, only 178 (69.3%) were monitored, owing to cost
considerations and to an incident of threatened violence that
resulted in not completing work in one section of the city.
The overall response rate is the product of the two rates
(70.1% X 69.3%): 48.5% (Table 4-3). Although this rate is low
for opinion surveys, which place much less burden on the
recipient than monitoring studies, it is similar to the rates
observed in previous monitoring studies (Hartwell et al., 1986,
1987; Immerman and Schaum, 1990; Pellizzari et al., I986a,b and
1988a,b,c; Wallace 1987).
MONITORING METHODS
All of the monitoring methods employed in the PTEAM Study
are described fully in Volume I. A brief description is provided
here.
Personal Exposure Monitor (PEM)
A Personal Exposure Monitor (PEM) was used for collecting
inhalable particles PM10. The PEM employs a flow-controlled
4-4
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battery-operated Casella pump to sample air through a nozzle
containing an impactor plate. The sampling nozzle contains a set
of 1.9-mm holes in a circular design. A 37-mm diameter Teflon
filter with 2-/tm pore size is mounted behind the impactor plate.
The lightly greased impactor plate intercepts particles having an
aerodynamic diameter larger than 10 /*m. (Laboratory studies have
established that the actual cutpoint is about 11 /im and is very
sharp.) Behind the filter is a second citric acid treated filter
to collect vapor-phase nicotine. A constant flow rate of 4 L/min
was used to sample over periods of approximately 12 hours.
The PEM sampling nozzle was worn on the participant's lapel
(in the participant's breathing zone) while being shielded from
direct impacts of clothing fibers and dander using a leather hood
in the shape of a traffic blinker. The pump was worn in a pack
that was designed to slide around the waist as desired for
sitting, walking, etc. During certain activities such as
sleeping or showering, the PEM was kept as near to the person as
practical.
Only technical staff involved in observing field activities
wore duplicate PEMs. One PEM impactor was worn approximately
10 cm under the normally situated PEM impactor for duplicate
sample collection.
Stationary Monitors (SIM and SAM)
For collecting inhalable (PM10) and fine (PM2.5) particles
indoors and outdoors at or near the participants' homes, the
4-7
-------
Stationary Indoor Monitor (SIM) and the Stationary Ambient
Monitor (SAM) were used. The SIM and SAM monitors were
identical, each consisting of a flow-controlled Medo pump used to
draw air through stationary impactors. Sampling nozzles with
holes 1.4 mm in diameter were used to collect the fine fraction.
Laboratory studies of these nozzles indicate that the actual
outpoint is very close to 2.5 jum.
Nicotine
Nicotine samples were collected to evaluate the contribution
of particles due to environmental tobacco smoke. All PEM, SIM
and SAM sampling heads contained a glass fiber backing filter
(40 mm) to support the Teflon filter. These backing filters were
impregnated with citric acid to capture nicotine. Only the
filters from the PEM and lti-/im SIM monitors were analyzed *
PAHs and Phthalates .
Polycyclic aromatic hydrocarbons (PAHs) and phthalates were
collected indoors at 125 homes, and both indoors and outdoors at
65 homes. The monitor consisted of a sampling pump and a
cartridge containing a sorbent bed of XAD-2 («5 g) preceded by a
quartz fiber filter. The XAD bed was 22 mm in diameter and was
inside a glass sampling heeid connected to a sampling box
containing four Medo pumps (operated in opposing phases for noise
dampening). The pump sampled air at a constant flow rate of
approximately 18 L/min over periods of approximately 12 hours.
4-8
-------
The sampling head was placed in a box for protection in both
indoor and outdoor locations. The sampling head was located
approximately l to 1.5 m above ground or floor level.
Air Exchange
Air exchange rates were measured at participant homes to aid
particle source modeling. The measurement involved the constant
release of perfluoromethylcyclohexane, a "perfluorotracer" (PFT),
while simultaneously collecting the tracer with a sorbent. Four
to eight PFT emitters (depending on home volume) were put into
each home 24 hours prior to the first sample collection visit.
Each PFT source was continually heated to 40°C and was located
0.5 to 1.5 m above the floor. At the initial visit when PFT
sources were deployed, the interior dimensions of each home were
measured and recorded. At each of the subsequent two visits
capillary adsorption tubes (CATS) were placed in the home at
three sites and were situated 1 to 1.5 m above the floor. Two
CATS were placed in the main living area, one in the bedroom, and
one near the center of the home. The CATS passively collected
the PFT onto their specially activated charcoal-type substrate
for periods of approximately 12 hours, in conjunction with the
other sampling activities.
Central-site Methods
A central site was maintained throughout the 48 days of the
study. One purpose was to compare the new instruments developed
4-9
-------
for this study (PEM and SAM) to the reference monitoring methods
accepted by the EPA (dichotomous and high-volume samplers). A
second purpose was to determine how well a central site could
characterize particle concentrations in a neighborhood (as
measured by the SAMs near the participants' homes).
The site selected was near the California School for the
Deaf/ close to the geographic center of Riverside. The school
bordered a segment (neighborhood) used for sampling homes. It
was only about 1/2 mile from the freeway, but this is similar to
many residential neighborhoods in Riverside. The central site
was at a slightly higher elevation than much of the city.
The samplers Were placed on a platform approximately 2 m
above ground so that the sampling height was 3.4 m. The platform
was located approximately 1*5 building-heights away from the
school building and was in a grassy area at least 15 m from any
trees.
PEM and SAM. One PEM and one SAM were mounted at the
central site. The SAM collected both the fine and inhalable
fractions, since the PEM and the SAM-10 were identical except
for the pump, their concentrations were averaged when comparing
to the other methods.
Dichotomous samplers. Two virtual-impactor dichotomous
samplers were operated at the central site. The Sierra
dichotomous sampler consisted of a tripod holding a sampling head
connected to an air sampling pump. The air sampling head
fractionated the particulate so that particles up to 2.5 /tm in
4-10
-------
aerodynamic diameter were collected by one filter (37 mm) and
particles up to 10 ^m in aerodynamic diameter were collected by
the other filter (37 mm). Studies indicate that the actual
cutpoint of the inlet employed here is close to 9.5 jttm. No
impactor is employed, thus eliminating the possibility of
particles bouncing off the impactor and being collected by the
filters. Filters were replaced at the end of each monitoring
period of approximately 12 hours.
High Volume PMlfl Sample Collection. Two Wedding reference
method high-volume PM10 monitors were operated at the central
site. The Wedding sampler consisted of a large air sampling pump
and a sampling head that trapped particles up to 10 jon in aerody-
namic diameter onto an 8" x 10" glass fiber filter with a 2-/*m
pore size. The air sampling system used a volumetric flow
control system and maintained a constant flow rate of 1.13
m3/min. The sampling head used a cyclonic fractionation
technique for collection of the particles of interest. This
technique produces a cutpoint that is less sharp than the other
samplers. The estimated cutpoint for these samplers is about 9
jitm. As with the other 'samplers, the period of collection was
approximately 12 hours. Both Wedding samplers were disassembled
and cleaned every five days.
Meteorological Data Collection. Attempts to collect
meteorological data at the central site were unsuccessful.
Meteorological data were subsequently obtained from three
4-11
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airports in and near Riverside: the March Air Force Base, the
Riverside Airport, and the Orange County Airport.
Weigh Trailer Operations. The weigh trailer was designed
for weighing filters in a stable environment (temperature and
humidity) with minimal vibration at the balance. The balances
were placed on tables with legs extending through the trailer-
floor to the ground. The trailer interior was maintained at 21
+3°C and relative humidity was maintained at 50 ±2 percent. A
steam humidifier was used to help maintain the humidity level as
part of the HVAC system. The floor, shelves and other surfaces
were cleaned with a damp mop or rag to reduce dust. Anti-static
measures were used to prevent erroneous weighings. All filters
were subjected to at least 24-hour exposure to the trailer
atmosphere prior to tare and final weighings.
Weighing- Methods
Two weighing methods were employed: one for the high-volume
filters and the other for all the smaller filters.
PEM. SAM. SIM and Dichotomous Sampler Filters. The PEMf
SAM, SIM and dichotomous samplers all used 37-mm Teflon filters,
and their weighing procedures were identical. The balance used
was a Cahn Model 30 microbalance with an accuracy of 1.0 pig. It
was connected to a microcomputer with weighing software developed
for this program. Once tared, all filters were inspected for
holes or other imperfections prior to use and were kept in a
barcode-labelled Petri dish., Filters were equilibrated in the
4-12
-------
weigh trailer for 24 hours prior to being weighed (e.g. taring,
reweighing or at any other weighing).
A set of 10 filters was weighed using the following steps.
First the balance was zeroed and the calibration checked using
NIST traceable masses. Then each filter was weighed and the
weight recorded once the computer recognized a stable reading (1-
2 min). After each set of 10 filters was weighed, the zero was
checked to within ±0.004 mg and a 200 mg weight to within ±0.002
mg. If either zero or the 200 mg weighing failed their test then
the zero/calibration was repeated and the previous set of filters
was reweighed. Otherwise weights for the 10 filters were
accepted.
High-Volume Filters. The high-volume filters were weighed
in a somewhat different manner, using a Mettler HIS balance with
an accuracy of ±0.1 mg and an upper mass limit of 200 g. A set
of up to ten filters was weighed using the following steps.
First the balance was zeroed and the calibration checked with an
NIST traceable 5 g weight. Then each filter was weighed,
allowing settling of the balance for a set period, and the weight
was manually recorded. After each set of filters was weighed,
the zero was checked. If the zero was outside of a ±0.3 mg
limit, then the balance was re-zeroed, the calibration weight was
reweighed and the previous set of filters was reweighed.
Quality Control Procedures. The primary quality control
procedure, as mentioned above, was to bracket any set of 10 (or
fewer) filters with zeroes and mass readings which were within
4-13
-------
specifications. The other procedure used was the reweighing of
filters by a different operator. One filter was selected from
each set of 10 to be reweighed. This applied to all filter
types. All procedures used were identical to original weighing
and were carried out for tare and final weighings. For the 37-mm
Teflon filters, the reweighing had to agree to within +4 /tg of
the original weight to be accepted. If any filter fell outside
of this limit, the set of 10 filters from which it was taken was
reweighed by the primary weighing person. No data were accepted
until this reweighing procedure was carried out.
QUALITY OF THE DATA
Quality assurance activities for the PTEAM study included
systems and performance audits in the field and audits of
database quality before statistical analysis began. The audits
of data quality documented the completeness of sample
acquisition, precision, accuracy, and detection limits. Results
are described fully in Volume I, and are briefly summarized in
this section.
Particles
Blanks. Blank filters were used during this study to
evaluate potential problems of filter contamination during
handling. Two types of blanks were used; field blanks and
4-14
-------
special blanks. Field blank filters were pre-weighed and
assembled into impactors with greased impactor plates, just as
was done for the sample filters. These impactor assemblies were
carried from the workroom to the field monitoring sites along
with the samples. The impactors were then returned to the
workroom and the filters were removed and reweighed along with
sample filters. During the course of the field monitoring it was
observed that increases in field blank filter masses were
typically in the 0 to 15 jug range, up to a maximum of 34 jug. One
potential contaminant was the grease applied to impactor plates.
Nine special blanks were prepared that were identical to the
field blanks except that no grease was applied to the impactor
plates.
Blank filters used for PEM, SIM, and SAM measurements showed
small increases in mass with a median of 9 jug per filter (Table
4-4). This median value was used to adjust the particle catches
of all PEM, SIM, and SAM sample filters. Special blanks had
similar increases with a median of 5 /zg.
The lower value for the special blanks suggests that grease
contamination may have been responsible for some, but not all, of
the filter contamination. Other potential contaminant sources
include airborne dust, dander from persons handling the filters,
and small metal particles from the impactor assemblies. Over 90%
of the PM2-S samples and 98% of the PM10 samples had particle
catches greater than 40 jug, so the impact of the filter
contamination on the results of this study are small. However,
4-15
-------
TABLE 4-4. CHANGE IN MASS OF BLANK
FILTERS AND LIMITS OF DETECTION
PEM.SIM.SAM Dichotomous Wedding hi-vol
Number of blanks
Mass increase (ug)
Median
Mean
SD
t-statistic
(0.99 level)
Nominal volume (m3)
LOD (ug/m3)
51
9
9.5
9.9
2.4
2.88
7.5
37
4
5.4
3.8
2.4
1.15 (coarse)
11.5 (fine)
8.0
0.8
43
100
200
500
2.4
815
1.5
4-16
-------
the level of background contamination may be important if similar
monitoring is conducted with small air volumes (approximately 3
m3) in locations with lower particle concentrations than were
observed in Riverside. In general, filter contamination was very
small, especially considering that a true clean-room environment
could not be maintained for filter handling operations during the
field study.
Blank dichotomous and Wedding filters showed a median
increase in mass of 4 ng and 100 jug., respectively (Table 4-4).
These median increases were all judged to be small in comparison
to the observed net magnitudes and ranges of aerosol masses found
for exposed filters. Dichot and Wedding samples were not
adjusted for the observed background.
Duplicates. In order to characterize the precision of the
aerosol measurements, collocated samples were collected
periodically for some sample types and routinely for other sample
types. Relative standard deviations (RSDs) for the particulate
concentrations were calculated for each pair using the following
expression for the RSD:
where x{ and x2 denote the two observed concentrations. The
distributions of these'RSDs are characterized by the results
presented in Table 4-5, which shows the number of pairs for which
4-17
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RSDs were calculated, along with the mean, median, maximum, and
standard deviation of the RSDs. The results are given by
particle size (2.5 or 10 jum) and sample type. The results imply
excellent agreement (high precision) between the collocated
samples, with very few exceptions. For instance, the median
relative standard deviations varied from about 2% to 5%,
depending on the sample type.
Elements
All PEM, SIM, SAM and dichotomous filters were analyzed for
42 elements by X-ray fluorescence (XRF). All of the
approximately 2500 filters were analyzed once by XRF at the EPA
facility in the Research Triangle Park. A subset of filters was
subjected to a second analysis to evaluate analysis precision and
the potential for bias over analysis time. A second subset of
filters was analyzed at the Lawrence Berkeley Laboratories (LBL)
for quality assurance purposes.
Blanks. Some filter blanks were analyzed by XRF prior to
beginning field monitoring to ensure that background elemental
concentrations were low and that the filters were acceptable.
One filter blank was then included with each set of 35 sample
filters analyzed by XRF at the EPA facility, for a total of 62
blanks for PEM/SIM/SAMs and 12 blanks for dichots. Fifty-one
field blanks were deployed during the study for PEM/SIM/SAM
4-19
-------
samples and all were analyzed by XRF. Eight dichot field blanks
were analyzed by XRF. Results are summarized in Table 4r-6.
In general, elemental background concentrations were very
low. Only mean iron concentrations were greater than the mean
uncertainty limit. In the case of iron, lab blank concentrations
were higher than either the field blank or special blank
concentrations, suggesting that contamination did not occur
during filter handling and may have been lowered by the tapping
procedure prior to weighing (the lab blank filters were not
weighed). Iron concentrations on the field blanks were 4 to 100
times lower than the mean sample iron concentrations.
Spikes. Quality control samples were also used to evaluate
the accuracy of the elemental analysis. Two types of quality
control samples were used during this study to evaluate accuracy:
1. NIST SRM
NIST Standard Reference Materials (SRMs) nos. 1833 and
1832, containing known elemental concentrations, were
analyzed along with each set of 35 sample filters.
2. Interlaboratory Duplicate Analyses
Sample filters ansilyzed first at the EPA facility and
then at Lawrence Berkeley Laboratories (LBL).
The SRM analyses provided a measure of analytical accuracy
over time with each group of samples analyzed. Interlaboratory
analyses were conducted by energy-dispersive XRF at LBL on
approximately 100 PEM/SIM/SAM filters and 20 dichot filters.
4-20
-------
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4-21
-------
Overall, the XRF system accuracy appeared to be very good
for the 12 elements contained in the SRM spiked samples. Median
percent biases ranged from -5.5% to +7.0% for 36 PEM-SAM-SIM
samples, and -4.4% to 7.1% for 8 dichotomous samples.
The XRF analyses provided data for 42 elements. These 42
elements consisted of 13 primary elements designated as of a
priori interest due to knowledge concerning their most
significant sources:
Primary Sources
Crustals/soils:
Industrial:
Combustion —•
Wood:
Coal:
Oil:
Vehicle Emissions
Tobacco:
Toxic Metals:
There were also 29 secondary elements identifiable by XRF.
Percentage Measurable. The proportions of samples with
measurable concentrations for each of the 42 elements are given
in Tables 4-7 through 4-10:
Table 4-7: Primary elements — residence data
Table 4-8: Secondary elements — residence data
Table 4-9: Primary elements — central site data
Table 4-10: Secondary elements — central site data.
Elements
Si, Al, Ca
Fe, Mn, Ni
K
Se
V
Br
Cd
Pb, As
4-22
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4-26
-------
the populations of individuals (PEM samples) or households (SIM
or SAM samples).
The classification of the elements is depicted below:
Percent Measurable
High
Low
Primary
Si, Al, Ca, Fe,
Mn, K, Br, Pb
Ni, SE, V, Cd,
As
Secondary
S, Zn, Cl, Ti,
Cu, Sr, P
Cr, Ba, Rb, Sn, Zr,
La, Co, Ga, Y, Au,
Hg, W, Sb, Ag, Ge,
Cs, Mo, Rh, Pd, Sc,
Te, I
"High percent measurable" elements are defined as those that
exhibited over 50% measurable for either the daytime or nighttime
PEM PM10 samples, where the measurability threshold is defined as
three times the reported uncertainty in the XRF measurement.
This threshold level is referred to as an uncertainty limit (UL).
Uncertainty limits were associated with each reported element
concentration and were dependent on the magnitude of the
concentration. As expected (due to the higher flow rate), the
dichot samplers generally produced higher percentage measurable
values than the corresponding PEMs and SAMs at the central site.
Eight of the 13 primary elements were generally found in
measurable quantities in the residence samples (PEM/SIM/SAM
samples), and, in particular, were measurable in over 50% of the
daytime or nighttime personal (PEM) PM10 samples. Of the 29
secondary elements, seven met this same criterion. These 15
elements are the only ones included in the subsequent statistical
analysis reported in this volume.
4-27
-------
elements are the only ones included in the subsequent statistical
analysis reported in this volume.
Duplicates
Numbers of collocated sample pairs, by particle size and
type, are given below:
Locations of Sampling
Size Sample
Cut (/im) Type
2.5 SIM
SAM
Dichot
10 SIM
SAM
PEM
Dichot
Homes
15
17
17
18
Central
Site
3
90
4
3
90
Pro j ect
Staff
15
Table 4-11 provides the median relative standard deviations
for each of the above types of collocated samples (except those
with only 3 or 4 duplicate pairs). For those pairs with both
values measurable, the table gives the number of such pairs and
the median RSD. The results are presented for those 15 elements
with high percentage measurable values. For most types of
samples and most elements in which reasonable sample sizes were
attained, the median RSDs were less than 15% and in many cases
(especially for the 10 pro. samples), they were less than 5%. The
major departure from rthis was for the SAM 2.5 jwm samples, for
4-28
-------
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which six elements had median RSDs greater than 15%. The
dichotomous samplers also showed high median RSDs of 26-30% for
copper. This observation was investigated further by recording
whether one of the two samplers was consistently associated with
higher values of any element. Since members of each pair of
dichot samples are distinguishable by sampler (B or C), the
direction of concentration differences between the two can be
determined. The results indicate that the median percentage
difference for the 10 /tin samples was less than 10% for 14 of the
15 elements; however, copper had a median percent difference of
-33.9% (i.e., generally a lower Cu concentration for Sampler C
than Sampler B). Copper concentrations also showed a median
percent difference of -40.8% for the 2.5 /xm samples. There
appears to have been a source of copper contamination, possibly
from wear of brass fittings, in Sampler B.
In general, both SRM and duplicate analyses indicate a small
downward trend in reported concentrations of several elements
over analysis time. It appears that a change in instrument
response may have resulted in elemental concentrations for batch
C samples (analyzed last) that were 2% to 5% lower than would
have been reported if they had been analyzed in batches A or B.
It is possible that small decreases in elemental concentrations
over analysis time could be due to particle loss from the filters
during handling. However, the magnitude of these differences is
in most cases less than the uncertainties associated with
reported concentrations for all elements except chlorine.
4-30
-------
Chlorine is an interesting case; reported concentrations
decreased throughout the course of the study. Twenty-six filters
were first analyzed by wavelength-dispersive XRF; the chlorine
concentration's median difference was -120% when the same filters
were analyzed at EPA several weeks later. Chlorine
concentrations of different samples decreased 13% to 26% between
duplicate analyses at EPA over the course of about three months.
These data are suggestive of losses due to volatilization from
the sample filter during analysis or over time. However, median
chlorine concentrations analyzed at LBL were 27% higher than
concentrations measured at an earlier time at EPA. Reported
chlorine concentrations may not accurately reflect actual
concentrations in the air at the time of sample collection.
An interlaboratory comparison of some of the filters was
supplied by LBL. The filters were first analyzed by EPA and then
were sent as blind samples to LBL. Results for the analysis of
approximately 100 PEM, SIM, and SAM sample filters were reported
in volume 1. Except for chlorine and manganese the absolute
percent differences were 21% or less. For all cases except
aluminum, median elemental concentrations measured at LBL were
higher than those measured at EPA even though the samples were
analyzed at LBL at a later time. Standard reference materials
1832 and 1833 were not analyzed at LBL so no direct comparison of
potential instrument bias is possible. Ten sets of dichot filter
sets (coarse/fine pairs) were also analyzed at LBL after an
initial analysis at EPA. Median percent differences were
4-31
-------
generally less than 22%. High manganese and titanium
concentrations were measured in the fine (PM2.5) fraction at LBL,
but there was only one measurable pair in each case. Chlorine
was consistently lower at LBL for the fine filters but higher
than EPA on the coarse filters.
Another type of duplicate analysis involved a second
interlaboratory comparison. A subset of 26 of the filters
analyzed by EPA using ED-XRF were also analyzed by WD-XRF at
another facility. Median percent differences greater than ±25%
were observed for Si, Al, and Cl. The use of different particle
size attenuation correction factors may have been responsible for
the differences in Si and Al, while chemical reaction or
volatility losses of Cl may have occurred between the initial
analysis by WD-XRF and the later analysis by ED-XRF.
PAHs and Phthalates
These two chemical groups were collected at a subset of 120
homes (indoors at all 120 homes and outdoors at 60 of these
homes). As with the particle samples, two 12-hour average
samples were collected at each home.
Blanks. Fourteen field blanks and 16 method blanks were
analyzed. Twelve of the 13 PAHs had very low field blank levels
ranging from ND to 1.7 ng/cartridge (the equivalent of 0.1
ng/m3) . Phenanthrene had a higher level of 9.4 ng/cartridge, but
this was still well below the levels found in most field samples
(Table 4-12).
4-32
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Three of the five phthalates had much higher method and
field blank levels of 64-220 and 94-266 ng/cartridge,
respectively. However, these amounts were still approximately an
order of magnitude lower than amounts found in indoor air
samples.
Spikes. A method of preparing control samples went through
several stages, as documented in Volume 1. Eventually, filters
embedded with NIST certified urban dust were used as laboratory
control samples. Recoveries of five 4-6-ringed PAHs ranged from
61% for benzo[a]anthracene to 126% for indeno[l,23-cd]pyrene
(Table 4-12). Recoveries of more volatile 3- and 4-ringed PAHs
spiked directly onto the XAD resin in field control cartridges
ranged from 75% (anthracene) to 96% (pyrene). No method capable
of emulating chemical behavior during collection, storage, and
analysis was developed for the particle-bound 5- to 7-ringed
PAHs. Recoveries of the phthalates were more variable, due to
probable background contamination of the field and laboratory
controls. Recoveries for diethylphthalate (the most common
contaminant) were 56% for the 25 laboratory controls and 65% for
the 14 field controls (Table 4-12). Field control recoveries for
the other phthalates ranged from 80% for butylbenzyl phthalate to
110% for di-n-butylphthalate.
Field samples were not corrected for recoveries.
Duplicates. Median relative standard deviations for 14
duplicate pairs were less than 10% for all target chemicals with
4-34
-------
the exception of di-n-octylphthalate (17% based on three pairs),
which was seldom detected in field samples (Table 4-12).
Nicotine
A filter to collect nicotine was mounted on all personal and
indoor monitors. All the personal nicotine filters were
examined, and all indoor filters in homes with reported cigarette
smoking. Due to fiscal restraints, some indoor filters collected
in homes without reported cigarette smoking were not analyzed.
Thirty-one duplicate pairs of nicotine samples were
analyzed, 20 of these at a quality assurance laboratory (K.
Hammond, Univ. of ,Amherst). Only six pairs exceeded the LCDs of
each laboratory; relative standard deviations (RSDs) for five of
these six pairs were lower than 10% (Table 4-13).
Air exchange
Air exchange rates were measured using the perfluorotracer
(PFT) method. The collection and analytic methods are discussed
fully in Vol. I. The gas used was PMCH. House volumes were
determined by measurements of each room by a technician.
Depending on house volume, between four and eight sources were
placed in each home the day before monitoring began, to allow the
gas to approach equilibrium. Two or three collecting tubes
(CATs) were exposed during each 12-hour monitoring period. At
least two rooms in the house had a CAT deployed during each
monitoring period. Duplicate tubes were placed in at least one
4-35
-------
TABLE 4-13. NICOTINE DUPLICATES (ug/m3)
NICID1 CONC1
N7586
N7135
N7663
N7795
N7851
N7785
N7322
N7813
N7796
N7804
N7699
N7839
N7557
N7693
N7373
N7292
N7318
N7869
N7221
N7495
N7194
N7463
N7162
N7383
N7338
N7337
N7402
N7333
N7726
N7153
N7150
1.00
0.84
0.23
0.21
0.18
0.07
0.07
0.08
0.06
0.06
0.08
0.06
0.08
0.08
0.08
0.06
0.08
0.09
0.07
0.06
0.08
O.Q7
0.12
0.08
0.07
0.07
0.07
0.07
0.07
0.05
0.05
ND1
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
LAB1
old
Old
new
new
new
new
new
new
new
new
new
new
new
new
new
new
new
new
new
new
new
new
old
old
old
old
old
old
old
old
old
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
HSPH
NICID2 CONC2
N7575
N7125
N7662
N7752
N7843
N7781
N7321
N7805
N7743
N7800
N7695
N7811
N7553
N7692
N7346
N7286
N7314
N7864
N7220
N7492
N7187
N7459
N7163
N7387
N7334
N7339
N7403
N7414
N7736
N7152
N7151
1.02
0.95
0.23
0.22
0.27
0.07
0.06
0.06
0.05
0.04
0.04
0.03
0.03
0.03
0.03
0.02
0.02
0.01
0.01
0.01
0.01
0.01
0.07
0.08
0.07
0.07
0.07
0.07
0.06
0.05
0.06
ND2
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
LAB2
Old HSPH
Old HSPH
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
Hammond
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
RSD
0.011
0.089
0.013
0.014
0.297
0.025
HSPH: Harvard School of Public Health
old HSPH: old laboratory analytic method
new HSPH: new laboratory analytic method
Hammond: laboratory of K. Hammond at Univ. Mass. Amherst
4-36
-------
of the two rooms, preferably the living room, family room, or
den.
58 blank tubes were either taken to the homes but remained
capped, or were left in the laboratory and remained capped. The
limit of detection (LOD) was normally 3 picoliters of PMCH,
although for some tubes it ranged up to 7.2 PI. All blank tubes
were below the LOD.
A measure of precision for the air exchange measurements can
be determined by calculating the relative standard deviation
(RSD) of each pair. The RSD of a duplicate pair is calculated by
multiplying the absolute value of the difference between one
observation and the mean of the pair by the square root of two
and dividing by the mean of the pair. Since about 20% of the
observations were below the limit of detection (LOD), some
convention must be adopted to assign numbers to these
unmeasurable values. One convention is to assign the LOD itself
to these observations; another is to assign one half the LOD.
Using the first of these conventions, the median RSD was 8.2%,
and the 75th percentile was 16.7%. Using the second convention,
the median RSD was 8.6%, and the 75th percentile was 17.4%.
Since the air exchange measurements involve products of
estimated volumes and estimated emission rates of the tubes,
errors are likely to be multiplicative rather than additive.
Therefore a better measure of precision than the RSD might be the
ratio of one member of a duplicate pair to the geometric mean of
the pair. ,Using this measure, about 70% of the 273 pairs were
4-37
-------
within 10% of the geometric mean of the pair, and nearly 90% were
within 20%.
The percentiles for the RSDs and ratios are provided for the
273 duplicate pairs of air exchange rates and residence times in
Table 4-14.
Since the air exchange rate is inversely related to the
amount of PMCH on the tubes, those tubes below the LOD are
associated with the largest air exchange rates. Assigning a
value of 1/2 the LOD to those tubes results in multiplying the
air exchange rates by a factor of 2. This leads to large
variability when the air exchange rates are graphed in a
scatter.plot. Therefore, a more appropriate parameter to compare
is the inverse of the air exchange rate, which is the average
residence time of a parcel of air in the home. The residence
times of the duplicate pairs are compared in Figure 4-1. The
slope of the linear regression is 0.965, with an R2 of 93%, for
the residence times when the ND = LOD convention is observed.
The slope and R2 values change very little (0.966 and 93%,
respectively) when the alternative convention (ND = LOD/2) is
substituted (Figure 4-2). The intercept is also unchanged, at
0.04 in both regressions. This behavior is in contrast to the
poor and variable R2 values observed when the air exchange rates
are compared. The R2 value is only 77% using the first
convention (Figure 4-3), and worsens to 65% using the second
convention (Figure 4-4). The slopes are only about 0.8 in each
case, and the intercept varies from 0.18 to 0.33. Agreement of
4-38
-------
TABLE 4-14. DUPLICATE AIR EXCHANGE RATES:
RELATIVE STANDARD DEVIATIONS AND
RATIOS TO THE GEOMETRIC MEAN
AIR EXCHANGE RATE
N
GEOM MEAN
GEOM ST DEV
MEAN
SD
PERCENTILE:
1
2
5
10
16
25
50
75
84
90
95
98
99
RSD
273
*
*
0.134
0.167
0
0
0.00
0.00
0.02
0.03
0.08
0.17
0.25
0.32
0.45
0.68
0.99
RATIO
273
1.002
1.100
1.011
0.139
0.67
0.71
0.81
0.87
0.91
0.94
1.00
1.06
1.11
1.17
1.26
1.40
1.55
RESIDENCE
RSD
273
*
*
0.126
0.136
0
0
0.00
0.00
0.02
0.03
0.08
0.17
0.25
0.32
0.42
0.53
0.60
TIME
RATIO
273
0.998
1.100
1.007
0.142
0.65
0.71
0.79
0.85
0.90
0.95
1.00
1.06
1.10
1.14
1.24
1.40
1.48
* Undefined: RSD for at least one pair = 0
RSD = ABS(D1 -[D1 +D2]/2)*SQRT(2)/[(D1 +D2)/2j
RATIO m D1/[SQRT(D1 *D2)] = SQRT(D1/D2)
Non-detects assigned value of LOD
4-39
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level of the residence time analyses, by plotting the logarithms
of the rates (Figures 4-5 and 4-6) . The R2 value increases to
89% and 87% for the two cases: the slopes are 0.92 and 0.93; and
the intercepts are small at -0.01 and 0.006, respectively.
Considering only the 221 pairs of observations that were
both measurable, the total amount of tracer collected on the
tubes followed log-normal distributions for each member of the
pair of observations (MI = 15.45 pi, ax = 11.87 PI, x2 = 12-2 with
8 d.f., p = 0.14; Mz = 15.32 pL, (72 = 11.84 pL, X2 = 8.7 with 8
d.f., p - 0.37). The Spearman rank correlation for these 221
pairs was 0.922.
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STATISTICAL ANALYSIS: PARTICLES, ELEMENTS,
NICOTINE, AIR EXCHANGE RATES
DESCRIPTION OF DATA
A target of 175 participants was set for the PTEAM Study.
Each participant was to collect two (day and night) 12-h
integrated personal air samples of inhalable particulates (PM10) .
Concurrent indoor and outdoor air samples were also to be
collected for both inhalable and fine (PMg 5) particles. Thus a
total of 1750 personal, indoor, and outdoor particle samples were
scheduled for collection. All these filters were to be analyzed
by XRF for 42 target elements.
Nicotine samples were to be collected with each particle
sample, but only the personal and some of the indoor filters were
to be analyzed, since the great majority of samples would contain
no or vanishingly small amounts of nicotine.
Air exchange samples were scheduled for both the day and
night period at each home. Three samples were to be collected at
each home for a total of 1050 (3 X 175 X 2) samples.
120 homes were scheduled for indoor air monitoring of PAHs
and phthalates. Half of these were scheduled for concurrent
outdoor air monitoring.
5-1
-------
The study was scheduled to last 44 days. A central site
containing two pairs of EPA reference method samplers
(dichotomous and hi-vol) together with the PEM and SAM samplers
developed for this study was planned. Each sampler was to
i
collect 88 12-hour. PM10 samples. In addition, the two
dichotomous samplers and the SAM sampler were each scheduled to
collect 88 12-hour PM2.5 samples as well.
Duplicate and blank samples were scheduled for all types of
samples. Since wearing two samplers was felt to be too much of a
burden for the participants, 20 pairs of duplicate samples were
scheduled to be collected in Riverside by project staff.
The total numbers of field, duplicate, and blank samples
scheduled for the residential and central-site monitors are
summarized in Table 5-1.
In the event, somewhat more samples were attempted than were
originally scheduled. The study ran for 48 days instead of 44,
and 178 residents participated instead of 175. This led to a
small increase in the number of residential field samples (1764
collected vs 1750 planned) and a nearly 10% increase in the
number of central site samples (576 collected vs. 528 planned).
Table 5-2 provides the numbers of samples originally scheduled,
those attempted, and those collected. More than 2700 ,(97%) of
the approximately 2800 particle samples attempted were
successfully collected. Due apparently to frequent short power
outages in Riverside, which caused the pumps on line current to
shut down before completing the 12-hour sampling period, a lower
5-2
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proportion of PAH/phthalate samples were successfully completed
(242 of 278 indoor samples and 108 of 144 outdoor samples).
Particle data were flagged according to problems encountered
in the field or during the weighing, as discussed more fully in
Volume I. In the Volume I analysis, flags 1 (no problems); 3
(questionable); 6 (some problems, considered usable); and 8
(outlier, considered usable) were included in the analysis. For
the analysis in Volume 3, data flagged as 3 (questionable) were
not employed. Thus the total numbers of samples are slightly
smaller (generally 2-5%) than the totals in Volume I. Table 5-3
provides the number of samples with each type of flag, and the
total number of each type used in the Volume 3 analysis.
All data in this volume are analyzed without the population
weights employed in Volume I. Those weights were proper in
estimating the frequency distribution of exposures for the target
population, but in this volume we will be concerned with physical
relationships (indoor-outdoor comparisons, source strength
calculations, etc.) that cannot be weighted by selection
probabilities. Since all data are unweighted, table titles will
not explicitly employ the term "unweighted;" this is to be
understood throughout the volume.
The differences between the weighted and unweighted data are
not expected to be large. As an example, the weighted and
unweighted distributions of personal exposures to PM10 are
plotted in Figure 5-1. As can be seen, the distributions lie
very close to one another.
5-5
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The convention adopted for the plotting was as described in
Wallace (1987). For the valid unweighted measurements (N = 171),
the percentile Pt for the kth ordered point (1 < k < N) is
Pk = (k - 1/2)/N
One can visualize this convention as follows: The N data points
can be associated with N equally spaced percentile ranges. A
reasonable plotting position would be the midpoint of each range.
For weighted data, there are again N data points. However,
each point i has a weight W, associated with it, such that the
sum of the weights Wt equals the target population N^ (here N^ =
132,000). We may visualize the N data points as associated with
N unequally spaced percentile ranges. A natural choice for the
plotting percentile of the Jcth ordered observation is the
midpoint of the "width" Wk associated with the Jtth weighted
observation:
SUMMARY STATISTICS
Particles
Summary statistics for the particle data are presented in
Table 5-4. The unweighted data show a large daytime increase in
5-8
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personal (PEM) PM10 exposures compared to the indoor (SIM) and
outdoor (SAM) concentrations. The magnitude of the increase
(mean personal exposure nearly 50% greater than mean indoor and
outdoor concentrations) is similar to that shown by the weighted
distributions (see Table 9^-17 of Volume I). Overnight personal
PM10 exposures are similar to the indoor and outdoor
concentrations, as was also the case with the population-weighted
values. Frequency distributions of outdoor, indoor, and personal
PM10 results are provided in Figures 5-2 to 5-4 for the daytime
and overnight concentrations;. The longer "tail" of the daytime
values is evident for both the personal and indoor values.
Fine particle (PM2.5) concentrations indoors are similar to
the outdoor levels in daytime, and fall somewhat below outdoor
levels at night. Frequency distributions of outdoor and indoor
PM2.s results are provided in Figures, 5-5 and 5-6. Again the
daytime indoor values are higher than overnight.
Nine of these 10 distributions could be fit by log-normal
distributions (x2 test, p > 0.05). These 10 distributions are
graphed on log-normal probability paper in Figures 5-7 to 5-10.
A perfectly log-normal distribution would appear as a straight
line on this paper. The GSDs for PM10 varied from 1.7 to .1.9.
The GSDs for the fine particles (PM2.5) were generally larger: 2.1
to 2.3.
The distributions of 24-h average concentrations are
displayed in Figures 5-11 and 5-12. The GSDs decline slightly,
as would be expected.
5-10
-------
Frequency Distribution of SAM10 in Residence Data
10 SO GOTO 90 HO 130 150 170 190 210
250 390 E1O
Nighttime
(~~1 Daytime
IFVequency Distribution of SIM10 in Residence Data
10 30 5070 9O 110 130 ISO 170 ISO 210
250 350 GiO
HI Nighttime I I Daytime
Figure 5—2. Outdoor PM10 concentrations measured near homes.
Figure 5-3. Indoor PM10 concentrations measured in homes.
5-11
-------
R^quency Distribution of PEM10 in Residence Data
40.
30-
20-
10-
I
n n
f-l l-l 1-1
SO GO TO 90 HO 330 ISO 170 190 ZtO 230 260 270 290 310 330 370 8SO 430 460
Nighttime
I—| Daytime
Figure 5-4. • Personal PM10 concentrations.
5-12
-------
Frequency Distribution of SAM2.5 in Residence Data
30-
20-
10-
I
U
Jltl.nl Li^
Nigiittime
I—| Daytime
Frequency Distribution of SIM2.5 in Residence Data
50
40-
30-
20-
10-
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Figure 5-5. Outdoor PM2.5 concencrations.
Figure 5—6. Indoor PM2-S concentrations.
5-13
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Both PM10 and PM2.5 values at the outdoor central, or temporal
(TEM), site agree well with outdoor values at the residences,
except for the overnight PM10 values, which appear to be somewhat
higher at the residences than at the central site (Figure 5-13).
Nicotine
A total of 334 valid measurements were obtained for the
personal samples, and 230 for the indoor samples.
Only about 30% (176) of the 564 analyzed nicotine samples
exceeded the limit of detection (LOD) of 0.15 jug/filter
(corresponding to a nominal value of about 0.05 /zg/m3) . Most of
these were from personal or indoor samples associated with
exposure to cigarette smoke. Mean personal and indoor nicotine
concentrations were on the order of 1 fJ.g/m3 for, those samples
associated with reported exposure to tobacco.smoke, but were only
0.1 Mg/m3 for those samples with no reported exposure (Table 5-
5).
Since about 70% of samples were below the detection limit,
various statistics such as the geometric mean are dependent on
the choice made for assigning a value to these samples. If the
mathematical form of the distribution of the samples is known or
can be guessed, it is sometimes possible to estimate a geometric
mean and geometric standard deviation (GSD) by plotting those
samples above the LOD and extending the plot by graphical or
numerical fitting processes. Since many environmental pollutants
have been found to follow log-normal or near log-normal
5-17
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5-18
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5-19
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'distributions, the combined personal and indoor nicotine values
have been plotted on log-normal probability paper (Figure 5-14).
The results appear to be close to log-normal between the 50th and
95th percentiles. Below the 50th percentile, nearly all values
are below the LOD. Above the 95th percentile, the distribution
departs from log-normality in the direction of smaller
concentrations than expected at the highest percentiles.
Plots have also been prepared for the indoor concentrations
by day and night (Figure 5-15) and the personal concentrations by
day and night (Figure 5-16) ., In both cases, little difference
between the day and night concentrations is discernible. To
compare the personal and indoor concentrations, these last two
figures were combined into one (Figure 5-17). This figure
suggests that little difference between the personal exposures
and the indoor concentrations exists.
On these plots, only the upper 30% or so of the values
exceed the LOD. Extending the values downward from, say, the
95th percentile through the 75th percentile would clearly result
in much lower values below the median than those shown, which
result from the convention of assigning the LOD value to
undetectable concentrations,, The GSDs determined by the ratio of
the 97.5th percentile (z=2) to the 84th percentile (z=l) are in
the range of 8-12. GSDs determined by the ratio of the 99.9th
percentile (z=3) to the 97.5th percentile are considerably lower,
in the range of 2-3. GSDs determined by the square root of the
ratio of the 99.9th percentile to the 84th percentile are at
5-20
-------
NICOTINE IN RIVERSIDE
(N = 565)
ug/m3
1
0.1
0.01
q10
1
0.1
255075 9599%
0.01
Figure 5—14. Nicotine: all measurements. Cumulative frequency distribution.
5-2-1
-------
NICOTINE IN RIVERSIDE
INDOOR 12-H CONCENTRATIONS
10F
ug/m3
1
0.1
0.01
NT (120)
DAY (111)
255075 9599%
q 1.0
1
0.1
0.01
Figure 5—15. Nicotine: indoor measurements.
NT = overnight samples. DAY = daytime samples.
5-22
-------
NICOTINE IN RIVERSIDE
PERSONAL 12-H EXPOSURES
10
ug/m3
1
0.1
0.01
NT (170)
DAY (166)
255075 9599%
10
1
0.1
0.01
Figure 5—16. Nicotine: personal measurements.
NT = overnight samples. DAY = daytime samples.
5-23
-------
NICOTINE IN RIVERSIDE
PERSONAL AND INDOOR SAMPLES
10F
ug/m3
1
0.1
0.01
PNT (170)
INT (120)
PDAY (165)
I DAY (111)
10
1
0.1
255075 9599%
0.01
Figure 5—17* Nicotine: personal and indoor measurements.
PNT = personal overnight samples. PDAY = personal
daytime samples. INT = indoor overnight samples.
IDAY « indoor daytime samples. No. of samples in
parentheses.
5-24
-------
intermediate levels of 4-5. Because of the large number of
undetectable values and the lack of stability of the calculated
GSDs, it appears difficult to estimate the true geometric mean
and GSD of the nicotine distributions with any confidence.
A second way to account for the large number of samples
below the detection limit is to assign the highest and lowest
possible values to them, thus establishing limits for such
statistics as the arithmetic mean. In this case, all samples
below the LOD were first assigned the LOD value (about 0.05
jitg/m3, depending on the volume of air sampled) and then a value
of 0. The resulting range of the arithmetic mean was 0.34 to
0.39 pg/m3 for the 230 indoor nicotine samples, and 0.26. to 0.32
)ug/m3 for the 334 personal nicotine samples. Assigning a value
of half the LOD to all samples below the LOD results in an
intermediate estimate of 0.37 jug/m3 for the indoor nicotine
samples, and 0.29 fJ-g/ra3 for the personal nicotine samples. The
overall arithmetic mean for 564 nicotine samples using this
convention was 0.32 /Ltg/m3.
Approximately 40 of the 178 participants reported one or
more cigarettes smoked in their homes during either the daytime
or overnight monitoring periods. About 52 participants, reported
being exposed to environmental tobacco smoke (ETS) at some point
during the 24-hour monitoring period. The total time exposed for
these 52 persons was 3840 minutes (70 minutes per person per 24-
hour day), or about 5% of the total time monitored. About 1/3 of
the exposure (1230 minutes) took place at night and two/thirds
5-25
-------
(•2610 minutes) during the day. This ratio is similar to the
ratio of waking hours in each monitoring period (about 10 hours
in the day period and five or six in the night period.)
A total of 80 personal nicotine samples were collected from
persons reporting one or more minutes of exposure to cigarette
smoke. Of these, 76% (61) exceeded the LOD. By contrast, of the
254 personal nicotine samples collected from persons reporting no
exposure to cigarette smoke, less than 15% (36) exceeded the LOD.
The difference in the means of the personal nicotine samples for
those reporting exposure to cigarette smoke vs. those reporting
no exposure is highly significant (p < 0.0001). Personal
nicotine levels were correlated with the number of minutes of
exposure to cigarette smoke (Spearman correlation coefficient r =
0.38; p < 0.001; N = 334). The distributions of measurable
personal nicotine concentrations for these two groups (reporting
ETS exposure and reporting no exposure) are shown in Figure 5-18.
As can be seen, the distributions are markedly different.
Out of 230 indoor nicotine samples, 72 were collected in
homes where at least one cigarette was smoked during either of
the two 12-hour monitoring periods. Again the difference in the
means for indoor samples in homes where cigarettes were smoked
vs. those with no cigarette smoking reported is significant (p <
0.0001). There was also a moderate correlation (Spearman
correlation coefficient r = 0.52; p < 0.0001; N = 230) between
indoor nicotine levels and the number of cigarettes reported
smoked during the monitoring period. The distribution of
5-26
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measurable indoor nicotine levels for samples collected during
the monitoring periods in which cigarettes were reported as
smoked is compared to the distribution for samples collected
during periods in which no cigarettes were smoked (Figure 5-19).
As in Figure 5-18, the distributions are very well separated.
A regression of personcil nicotine levels on minutes exposed
to cigarette smoke is shown in Figure 5-20. The personal
nicotine value increased by about 0.013 Mg/m3 per minute of
reported exposure to cigarette smoke. The J?2 value is 36.6% (N -
334). A second regression of personal nicotine on a binary
variable indicating whether any exposure to cigarette smoke or
smoker in the home was reported suggested that nicotine exposures
went up by about 0.85 jig/m3 for persons exposed during the
monitoring period; however, this relationship had a somewhat
smaller Rz value of 22.6%.
A regression of indoor nicotine concentrations on the number
of cigarettes smoked in the home during the monitoring period is
illustrated in Figure 5-21. Indoor nicotine values increased by
about 0.12 ng/Tfi3 for each cigarette reported smoked during the
monitoring period. The Rz value is 35.4% (N = 227). A second
regression was run on a binary variable indicating whether any
cigarettes were smoked in the home during the monitoring period;
this regression suggested that nicotine concentrations increased
by an average of 0.964 jug/m3 in homes with smoking, but the R
value was only 28.4%.
5-28
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Mean indoor PM10 (SIM10) concentrations were elevated by
about 40 jug/m3 in the homes with smokers (Tables 5-6 and 5-7) .
Fine particle (SIM2.5) levels were also greater (by about 30
/zg/m3) in the homes with smokers. (At night, a portion of this
increase may have been due to higher outdoor particle levels near
homes with smokers.)
Ratios of various combinations of particle and nicotine
concentrations are provided in Tables 5-8 and 5-9 for homes with
smoking compared to homes without smoking. Elevated ratios of
indoor to outdoor particles (SIM/SAM) and of fine to inhalable
particles (SIM2.5/SIM10) occur in the smoking homes.
Elements
Volume I provides a full discussion of the methods, quality
assurance results, and population-weighted statistics for the 15
elements that were measurable in at least 20% of the samples.
Mean concentrations of the two particle sizes and associated
elements are provided in Table 5-10. The unweighted
distributions of the particles and the 15 elements are shown in
Figures 5-22 to 5-37. The figures illustrate that daytime
personal exposures to 14 of the 15 elements are increased by
considerable amounts over concurrent indoor or outdoor
concentrations; only sulfur is an exception. The side-by-side
box plots for PM2.5 and PM10 also show which elements are mostly
in the coarse fraction (very low PM2.5 values) and which are
\,
mostly in the fine fraction (PM2.S values approximately equal to
5-31
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5-35
-------
TABLE 5-10. CONCENTRATIONS OF
PARTICLES (fjg/mS) AND ELEMENTS (ng/m3)
DAYTIME
NAME
PERSONAL
PEM10
Al
Br
Ca
Cl
Cu
Fe
K
Mn
P
Pb
S
Si
Sr
Ti
Zn
N
PM10
159
159
159
159
159
159
159
159
159
159
159
159
159
159
159
159
MEAN
143.9
4386.3
24.8
4056.8
790.6
42.7
3205.6
1799.4
64.0
254.5
42.4
1809.2
11228.2
23.8
366.9
152.0
SD
79.6
4508.5
34.0
2896.6
551.7
32.7
3163.8
1392.5
60.9
168.1
45.1
1161.1
10038.1
15.7
327.6
102.7
OVERNIGHT
N
166
166
166
166
166
166
166
166
166
166
166
166
166
166
166
166
MEAN
78.6
1629.1
14.4
1659.5
435.7
20.3
1173.9
819.6
24.8
166.1
27.1
1535.3
4286.7
11.6
135.3
70.0
SD
42.3
1121.6
12.8
1118.9
315.3
26.4
811.2
524.3
16.0
107.5
30.7
967.5
3056.8
5.3
80.1
43.2
INDOOR PM10
SIM10
Al
Br
Ca
Cl
Cu
Fe
K
Mn
P
Pb
S
Si
Sr
Tf
Zn
165
165
165
165
165
165
165
165
165
165
165
165
165
165
165
165
98.3
2606.9
13.6
2520.0
437.0
23.0
1881.9
1129.2
39.7
185.7
29.2
1710.9
6638.9
16.2
200.7
90.0
64.9
2233.3
7.8
2890.4
384.9
18.7
1666.7
847.3
35.1
106.2
15.f
1310.9
5499.3
10.3
161.6
64.6
162
162
162
162
162
162
162
162
162
162
162
162
162
162
162
162
65.2
1441.6
12.1
1253.0
314.1
16.0
1023.1
672.9
22.8
142.2
28.6
1523.0
3484.4
10.5
111.0
63.0
38.8
777.4
6.6
812.0
268.7
11.4
669.5
430.8
14.8
79.7
32.5
1005.4
2165.5
4.3
63.8
41.3
(cont.)
5-36
-------
TABLE 5-10. CONCENTRATIONS OF
PARTICLES (A/g/m3) AND ELEMENTS (ng/m3)
DAYTIME
NAME
INDOOR
SIM2.5
Al
Br
Ca
Cl
Cu
Fe
K
Mn
P
Pb
S
Si
Sr
Ti
Zn
N
PM2.5
167
167
167
167
167
167
167
167
167
167
167
167
167
167
167
167
MEAN
48.6
559.3
10.7
413.7
143.2
14.3
356.6
275.1
12.7
117.8
22.6
1303.5
741.0
8.5
66.5
43.5
SD
40.9
206.9
5.4
496.3
187.7
12.2
346.9
247.6
7.5
18.2
11.6
1186.0
744.0
1.9
25.0
28.0
OVERNIGHT
N
165
165
165
165
165
165
165
165
165
165
165
165
165
165
165
165
MEAN
37.2
445.1
10.0
210.6
112.8
12.1
212.0
206.9
10.5
102.7
22.8
1270.8
388.7
7.2
53.4
34.4
SD
30.5
54.6
5.7
117.4
157.2
9.6
117.3
211.1
4.1
15.9
30.3
954.9
202.5
1.1
8.7
26.8
OUTDOOR PM10
SAM 10
Al
Br
Ca
Cl
Cu
Fe
K
Mn
P
Pb
S
Si
Sr
Ti
Zn
162
162
162
162
162
162
162
162
162
162
162
162
162
162
162
162
96.9
3224.7
12.1
2339.7
244.4
16.2
2398.8
1111.6
52.8
152.9
33.1
1808.7
7878.2
18.2
215.0
66.6
59.2
2708.3
5.4
1402.8
274.4
7.8
1598.7
633.0
36.7
23.2
21.8
1546.1
5458.7
8.4
143.5
34.1
159
159
159
159
159
159
159
159
159
159
159
159
159
159
159
159
87.1
2084.3
13.9
1592.2
503.2
18.4
1701.6
808.6
37.6
134.0
32.8
1858.7
5160.3
14.1
143.9
56.4
48.8
1024.0
7.5
875.8
457.0
17.9
819.0
329.7
19.4
26.1
22.4
1288.9
2441 .5
5.4
68.5
36.6
(cont.)
5-37
-------
TABLE 5-10. CONCENTRATIONS OF
PARTICLES (//g/m3) AND ELEMENTS (ng/m3)
DAYTIME
NAME
OUTDOOR
SAM2.5
Al
Br
Ca
Cl
Cu
Fe
K
Mn
P
Pb
S
Si
Sr
Ti
Zn
N
PM2.5
159
159
159
159
159
159
159
159 ,
159
159
159
159
159
159
159
159
MEAN
48.1
536.4
10.7
298.8
97.7
11.5
383.3
212,5
13.7
118.4
23.9
1540.7
677.3
8.5
63.8
43.1
SD
36,2
88.8
4.9
177.3
141,1
5,0
205.1
108.9
5,8
17,6
11.3
1347.7
425.3
1,5
11.0
38.5
OVERNIGHT
N
160
160
160
160
160
160
160
160
160
160
160
160
160
160
160
160
MEAN
51.9
438,8
11.6
171.3
183.2
12.6
265.8
149.8
12.1
102.6
24.6
1570.3
391.0
7.2
53.4
38,1
SD
41.5
53.7
6.6
114.9
271.5
14.4
162.3
85.5
5.6
14.6
18,2
114Q.1
232,1
1.3
8.4
30.3
5-38
-------
Figure 5 — 22 Distribution of Particle Cone, for Residence Samples
350
300
250
200-
150
100-
X ^
I
r
SAM25 SIM26 SAM10 SIM10 PEM10
SAM26 SIM25 SAM10 SIM10 PEM10
DAYTIME
NIGHTTIME
Figure 5 — 23 Distribution of AT Cone, for Residence Particle Samples
12000
10000
8000
6000
40OO-
2000-
ng/m3
0
SAM25 SIM25 SAMtO SIM10 PBM10
DAYTIME
SAM26 SIM25 SAM10 SIM10 PEM10
NIGHTTIME
5-39
-------
Figure 5 — 24 Distribution of Br Cone, for Residence Particle Samples
ng/m3
50-
40-
80-
20-
10-
I
^^
1
T
J~
SAM25 SIM2S SAM10 SIM10 PEM10
DAYTIME
SAM25 SIM2S SAM10 SIM10 PEM10
NIGHTTIME
Figure 5 — 25 Distribution of Ca Cone, for Residence Particle Samples
32000
ng/m3
10000-
8000-
6000-
4000-
2000-
T
I
SAM2S 3IM2S SAM10 SIM10 PBIillO
SAM2S SIM26 SAM10 SIM10 PEM10
DAYTIME
NIGHTTIME
5-40
-------
Figure 5 — 26 Distribution of Cl Cone, for Residence Particle Samples
ng/m3
ZiUW
1800
1600-
1400-
3200-
1000
800
600-
400-
200-
n-
§
s
-1—
*
*
1
-1-"
jjj.
^>
^-^-^
-[-
4
i
#
*
i _L _L • • J-
SAM25 SIM25 SAM10 SIM10 PEM10
DAYTIME
SAM25 SIM2S SAM10 SIM10 PEM10
NIGHTTIME
Figure 5 — 27 Distribution of Cu Cone, for Residence Particle Samples
320
ng/m3
100
80-
60-
40-
20
IT
SAM25 SIM25 SAM10 SIM10 PEM10
SAM2S SIM25 SAM10 SIM10 PEM10
DAYTIME
NIGHTTIME
5-41
-------
Figure 5-28 Distribution of Fe Cone, for Residence Particle Samples
ng/m3
8000-
7000-
6000-
6000-
Annn-
8000-
2000-
1000-
n.
_^
F^3 Him
4
»
<
N
-------
Figure 5 — 30 Distribution of Mn Cone, for Residence Particle Samples
ng/m3
O.OU
140
120-
100-
fin -
60
40
20-
n-
-,-
^£S% \
^^ ^^
*
I
4
i
_J
i
4
1
A
T
H-i T T
' i rn
"T" — i — * *
J^ T -1 _
£^*'
-------
Figure 5-32 Distribution of Pfo Cone, for Residence Particle Samples
ng/m3
120
100 H
80
60
40
20 -\
3AM2S SIM26 SAM10 SIM10 PEM10
DAYTIME
SAM26 SIM26 SAM10 SIMlO PEM10
NIGHTTIME
'Figure 5 — 33 Distribution of S Cone, for Residence Particle Samples
5000
ng/m3
4000-
3000-
2000-
1000
I
m
T
1
m
T T
SAM25 SIM25 SAM10 SIM10 PEldlO
DAYTIME
SAM2S SIM26 SAM10 SIM10 PBM10
NIGHTTIME
5-44
-------
Figure 5 — 34 Distribution of Si Cone, for Residence Particle Samples
30000
26000
20000
16000
10000-
6000
T
i
I
SAM26 SIM25 SAM10 SIM10 PEM10
DAYTIME
SAM25 SIM26 SAM10 SIM10 PEM10
NIGHTTIME
Figure 5 —35 Distribution of Sr Cone, for Residence Particle Samples
70
60
50
40
30
20-
10
ng/m3
0
T
X
T
SAM25 SIM25 SAM10 SIM10 PEM10
DAYTIME
SAM2S SIM26 SAM1O SIM10 PBM10
NIGHTTIME
5-45
-------
Figure 5 — 36 Distribution of Ti Cone, for Residence Particle Samples
ng/m3
9OO-
800-
700-
600-
600-
400-
300-
200-
IOO-
n.
I
*
±
4t
_L
*
i
T T
_L -j- -=-| —
SAM2S SIM25 SAMIO SIM10 PEM10
SAM26 SIM26 SAMIO SIM10 PEM10
DAYTIME
NIGHTTIME
Figure 5 — 37 Distribution of Zn Cone, for Residence Particle Samples
4UU-
360-
300-
260-
200-
150-
100-
60-
n.
T
1
&&2
i&?
&&',
— « —
J_
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H
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J
* i
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,__,>-,
II . • -*- .
'OZZ- r-'\---'\ — i —
5&Z if&Z l__^ | _L
'^S^. ^^'' 1 -J—
SAM2S SIM25 SAMIO SIM1O PEM10
SAM25 SIM2S SAMIO SIM10 PEM10
DAYTIME
NIGHTTIME
5-46
-------
PM.,0 values). Five elements were associated mostly with the fine
fraction: bromine, phosphorus, lead, strontium, and sulfur.
The outdoor (backyard) concentrations of the 15 elements are
compared to the concurrent outdoor concentrations measured by the
SAM at the central site in Figures 5-38 to 5-52. The elemental
concentrations associated with the fine fraction (PM25) and with
the inhalable particles (PM10) are shown separately, as are the
daytime and overnight values. Excellent agreement is noted for
sulfur, and good agreement is seen for most elements in the
daytime. Some elements (Ca, Cl, Fe, K, Mn, Si) show occasional
overnight peaks at the residential sites that are not reflected
at the central site, for unknown reasons. The greatest
consistent disagreement is shown for copper, with central site
values often two- or threefold higher than backyard
concentrations. It is possible that the copper brushings on the
large amount of air monitoring equipment located at the central
site were elevating the local copper concentration. Additional
comparisons between samplers and locations are provided in
Appendix F.
Cigarette smoke has been found to be a source of certain
elements such as potassium and chlorine (Koutrakis et al., 1990).
Tables 5-11 and 5-12 provide median concentrations of 15 elements
in homes with smokers compared to homes without smokers. Large
increases in particle mass, potassium and chlorine are noted in
both size fractions in the homes with smokers. Tables 5-13 and
5-14 provide mean values for the same elements. The ratios of
5-47
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these mean values (for homes with smokers compared to homes
without smokers) are provided in Table 5-15. The largest ratios
are for potassium, chlorine, and bromine. Ratios of these
elements and of particle mass tend to be larger in the fine
fraction than in the PM10 fraction, supporting previous
conclusions that cigarette smoke makes a larger relative
contribution to the fine fraction than to the total PM10 mass.
Air exchange
A total of 1010 samples were collected. There were 273
duplicate pairs and 464 single observations. Two observations
were outliers, resulting in 735 values after averaging the
duplicates. These were split evenly between night (W = 368) and
day (N = 367) .
Considering all 735 individual air exchange rates, the
median air exchange rate is close to 1 h"1, corresponding to a
residence time of one hour. The 25th percentile air exchange rate
is 0.5 h"1 and the 75th percentile air exchange rate is 1.7 h"1.
The 25th percentile residence time is 0.44 h and the 75th
percentile residence time is 2.00 hours. Higher percentiles than
the 80th (for the air exchange rates) or lower percentiles than
the 20th (for the residence times) are uncertain due to the fact
that 165 measurements (about 20% of the total) were below the
LOD.
In order to estimate the upper 20% of the air exchange rates
associated with tracer measurements below the LOD, an effort was
5-67
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made to fit the distribution suggested by the 616 values > LOD.
The hypotheses that the distribution arose from a normal or a
log-normal distribution were rejected by a x2 test (p < io"7 and p
< .00012, respectively). However, the distribution was fit by a
gamma distribution, with a = 1.25 and j3 = 0.86 (x2 = 17 with 14
d.f., p = 0.25). Assuming that the gamma distribution represents
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of the individual measured air exchange rates will be about 2.8
h"1, and that the 95th percentile will be about 3.5 h"1.
The above analysis was done on all individual air exchange
rates as if they were independent. However, most of the measured
values were associated with at least one other measurement in the
same house (but a different room) at the same time. Therefore an
analysis of the air exchange rates or residence times averaged
over all measurements in a given house and during the same time
period is appropriate.
A convention for averaging air exchange rates is required.
Since what is measured is the amount of tracer gas on a tube,
which is proportional to the residence time and inversely
proportional to the air exchange rate, it is more appropriate to
average residence times than air exchange rates for two or more
samples in a home during the same time period. Then the
"average" air exchange rate is found by taking the inverse of the
mean residence time. This is equivalent to determining the
harmonic mean of the air exchange rates measured by the different
tubes. Since the harmonic mean is always less than or equal to
5-69
-------
the arithmetic mean, this convention results in slightly smaller
air exchange rates than would otherwise be calculated. The
average difference in the air exchange rates calculated by the
two methods amounted to about 5%.
i
This convention does not apply to averaging across different
time periods. For example, the average 24-h air exchange rate is
found by a normal average (eirithmetic mean) of the two 12-h air
exchange rates, even though each of the 12-h rates may be a
harmonic average of the rates measured by different tubes.
Using the above averaging conventions, the 24-h average air
exchange rates and residence times are provided (Table 5-16) for
175 Riverside homes using the two "LOD" conventions (ND = LOD; ND
= LOD/2). The geometric mean of the air exchange rates by these
conventions is 0.78 and 0.84 h"1, with a GSD of 1.9 and 2.1. The
cumulative frequency distributions are pictured in Figures 5-53
and-5-54. Figure 5-54 suggests that the LOD/2 convention matches
the slope of the measured residence times more nearly than the
LOD convention.
At night, 175 homes had at least one valid air exchange rate
measurement; during the day 174 homes had at least one
measurement. (The three homes with no measurements at all were
#'s 110, 117, and 126. Home # 90 had no daytime measurements.)
The summary statistics for the air exchange rates averaged over
the homes are affected by the convention chosen for treating
measurements below the LOD. Therefore two tables (5-17 and 5-18)
using the two "LOD conventions" are provided for the day and
5-70
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5-74
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night air exchange rates and residence times. As before, the
residence times are less affected by the different "LOD
conventions" than the air exchange rates. For example, the
standard deviation for the daytime air exchange rates increases
from 0.8 to 1.5, (nearly (100%) when the conventional value for a
nondetectable concentration is changed from LOD to LOD/2; the
corresponding SD for the residence times changed by only a small
amount (1.30 to 1.34, or less than 5%).
The cumulative frequency distributions for the day and night
air exchange rates and residence times are provided in Figures 5-
55 to 5-58. To see more clearly the effect of the different "LOD
conventions," the cumulative frequency distributions using the
different conventions are plotted side by side in Figures 5-59 to
5-62.
Using the convention of assigning the LOD to the not-
detected values, the geometric mean of the harmonic mean air
exchange rates was 0.87 h"1 during the day and 0.78 h"1 at night.
These differences, though small, were statistically significant.
The higher air exchange rates in the daytime are likely to be
associated with increased activity (using doors, kitchen and
bathroom exhaust fans, opening and closing windows, etc.). The
alternative convention (ND =1/2 LOD) resulted in geometric means
of 0.98 and 0.84 h"1, respectively.
Log-normal and gamma distributions were fit to the
untransformed daytime, overnight, and 24-hour air exchange rate
and residence time measurements. Log-normal distributions were
5-75
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rejected for the daytime air exchange rates, but were not
rejected for all other air exchange rate and residence time
distributions. Gamma distributions were also rejected for the
daytime residence times, but were not rejected for all other
combinations. Two examples of log-normal fits are presented for
the 24-hour air exchange rates (Figure 5-63) and the 24-hour
residence times (Figure 5-64). The log-normal fit for the 24-
hour average air exchange rate values had an arithmetic mean of
1.079 IT1 and an SD of 0.800 h"1 (x2 value =• 9.9 with 8 d.f.; p =
0.27). The log-normal fit for the 24-hour average residence
times had an arithmetic mean of 1.585 and an SD of 1.170 (x2
value =10.9 with 7 d.f.; p = 0.14). An example of a best-fit
gamma function (a = 2.6, 0 == 2.45; x2 = 8.3 with 8 d.f.; p -
0.40) is provided for the 24-hour air exchange rates in Figure 5-
65. -
When all data were transformed by taking the logarithms, the
data fit a normal distribution (p-value of the x2 test >0.05) for
all 12 (22 X 3) combinations of air exchange rate vs. residence
time, day vs. night vs. 24-h average, and LOD vs. LOD/2
convention. Examples of the normal fits to log-transformed data
are provided for the day and night air exchange rates using the
ND=LOD convention in Figures 5-66 and 5-67; and for the 24-hour
air exchange rates using both conventions in Figures 5-68 and 5-
69. By exponentiating the means and standard deviations of the
log-transformed data shown in the figures, the geometric means
and GSDs of the best-fitting log-normal distributions can be
5-80
-------
tO
LU
OH
LLl
35
25
20
15
10
0
0
AIR EXCHANGE RATES BY HOME CN = 175)
/'
LOG-NORMAL FIT: MEAN = 1.08 SD * 0.80
24-h AVERAGE AIR EXCHANGE RATE (i/h)
Figure 5-63. Log-normal fit to 24-h average air exchange rates: ND - LOD.
5-81
-------
50
40
CO
LU
30
RESIDENCE: TIMES BY HOME CN = 175)
Log-Normal Fit. Mean =1.58. SD = 1.17.
•
» ' - 1 — -i
24-h AVERAGE RESIDENCE TIME'
-------
en
u.
o
10 -
5 -
0 -
AIR EXCHANGE RATES BY HOME
-------
DAYTIME AIR EXCHANGE RATES CLOGS)
NORMAL FIT: MEAN = -0.14 SO = 0.78
en
LU
en
u.
CD
Oi
LJ
IS
15
12
0 -
1 1—i 1 1 1 1—i 1 i 1 1 1—I—r—i 1
-2.1
-1.1
-0.1
0.9
1.9
LN AIR 'EXCHANGE RATE Cl/h)
Figure 5—66. Normal fit to the logarithms of the daytime air exchange rates:
ND — LOD. The geometric mean — e"0-1* = 0.87. The geometric standard
deviation - e°-78 - 2.18.
5-84
-------
OVERNIGHT AIR EXCHANGE RATES (LOGS)
NORMAL FIT: MEAN = -0.25 SD = 0.68
CO
UJ
CO
U.
o
cz
111
03
] 1 i 1—i j 1 1 1—i j 1 1 1 1 j—i 1 1
4 -
0 -
-2.1
-1.1
-0.1
0.9
1.9
LN AIR EXCHANGE RATE
Figure 5—67. Normal fit to the logarithms of the overnight air exchange
rates: ND - LOD. The geometric mean = e~°-25 = 0.78. The geometric standard
deviation =* e°-68 - 1.97.
5-85
-------
AIR EXCHANGE RATES BY HOME CLOGS) N=175
NORMAL FIT: MEAN = -0.14 SD * 0.66
1
ffi
i—i—i—i—i—r—i—i—i—T—i—i—i 1—1—r—-1 i
i i—i 1—i—i—i
-2.1
-1.1
-0.1
0.9
1.9
LN 24-h AIR EXCHANGE RATE Cl/h)
Figure 5-68. Normal fit to the logarithms of the .24-hour air exchange rates:
ND - LOD. The geometric mean - e~°-14 - 0.87. The geometric standard
deviation - e°-66 - 1.93.
5-86
-------
AIR EXCHANGE RATES BY HOME CLOGS) N=175
NORMAL FIT: MEAN = -0.026 SO = 0.78
CO
Stf
o
•E
20 -
' .ill 1 I 1 !
-2.1 -1.1
-0.1
0.9
1.9
2.9
LOG 24-h AVERAGE AIR EXCHANGE RATE
Figure 5-69 Normal fit to the logarithms of the overnight air exchange
rates: ND - LOD/2. The geometric mean - e'0-026 - 0.97. The geometric
standard deviation - e°-78 - 2.18.
5-87
-------
obtained. Because of the likelihood that errors are
multiplicative rather than additive, and distributed log-normally
rather than normally, the practice of transforming the data first
and using a least-squares fit to a normal distribution may be
more appropriate than that of fitting a log-normal distribution
to the untransformed data. (%2 scores were consistently better
for the normal fits to log-transformed data than for log-normal
fits to untransformed data.) In both cases it is a log-normal
distribution that results, but the calculated GMs and GSDs are
somewhat different.
The GSD for the air exchange rates (using the "ND = LOD"
convention) was 2.2, 2.0 and 1.9. for the day, night, and 24-hour
distributions, respectively. The decline in GSD with the longer
averaging time can be seen in Figure 5-70. Since the geometric
means were 0.87, 0.78, and 0.78 h'1, respectively, this
corresponds to a predicted two-sigma (97.5th percentile) air
exchange rate of 4.1, 3.1, and 2.9 h'1, respectively.
A comparison of the cumulative frequency distributions of
all 735 individual 12-h air exchange rate measurements with the
175 24-h averages is provided in Figure 5-71. The decline of the
GSD with the combination of averaging across homes and averaging
across time periods is somewhat more evident in this figure than
in the preceding one.
5-88
-------
AIR EXCHANGE RATES
RIVERSIDE: FALL 1990
10
ACH
0.1
1 2 5 10 25 50 75 90 95 98 99%
DAY
NIGHT -*- 24-HR
Non-detects assigned value of LOD
Figure 5-70. Air exchange rates: day, night and 24-hour cumulative frequency
distributions.
5-89
-------
AIR EXCHANGE RATES
RIVERSIDE: FALL 1990
10
ACH
0.1
1 2 5 10 25 50 75 9095 9899%
AITSamples
Non-detects assigned value of LOD
24-h Avgs
Figure 5-71. Air exchange rates: individual measurements (N -. 735) compared
to 24-h averages (N - 175).
5-90
-------
CORRELATIONS
Correlations between the centrally-located outdoor monitors
(SAM) and those in the backyards of the residences are provided
in Table 5-19 for particles and 15 elements. Correlation
coefficients are very high for sulfur (0.98 to 0.99), indicating
that it is well-mixed throughout the region. Correlation
coefficients for most other elements range from 0.5 to 0.9, with
one major exception: copper. Since the central site included a
number of monitors, copper components may have contributed to the
loadings on the central-site SAM. Three other elements had low
correlations in the fine fraction: aluminum, strontium, and
titanium. Cross-correlations between all mass and elemental
concentrations at the central site and those at the backyard
sites are provided in Tables 5-20 to 5-23.
Nicotine was significantly associated with personal and
indoor PM10, and especially with indoor PM2.5, suggesting that
environmental tobacco smoke made important contributions to
personal exposure and indoor air (Table 5-24). Nicotine was also
significantly correlated with potassium and chloride, and to some
extent for calcium, suggesting that these elements are markers
for environmental tobacco smoke.
Correlations between particle and elemental concentrations
and some activities are presented in Tables 5-25 to 5-27. House
cleaning activities were more common in homes with higher
nicotine levels (r — 0.24; p < 0.01).
5-91
-------
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-------
TABLE 5-20. CORRELATIONS OF CENTRAL-SITE PARTICLE
AND ELEMENT CONCENTRATIONS WITH THOSE
MEASURED OUTDOORS AT RESIDENCES: PM2.5 OVERNIGHT
PM_C
AL_C
BR_C
CA_C
CL_C
CU_C
FE_C
K_C
MN_C
P_C
PB_C
S_C
SI_C
SR_C
TI_C
ZN_C
PM
0.96
0.00
145
0.03
0.72
145
0.91
0.00
145
-0.21
0.01
145
0.66
0.00
145
-0.07
0.37
145
0.16
0.06
145
0.18
0.03
145
0.51
0.00
145
0.70
0.00
145
0.69
0.00
145
0.78
0.00
145
-0.22
0.01
145
0.16
0.05
145
-0.01
0.92
145
0.57
0.00
145
AL
0.26
0.00
145
0.08
0.34
145
0.19
0.02
145
0.06
0.50
145
0.17
0.04
145
-0.03
0.68
145
0.22
0.01
145
0.17
0.04
145
0.33
0.00
145
0.15
0.08
145
0.22
0.01
145
0.10
0.21
145
0.08
0.35
145
0.25
0.00
145
0.04
0.64
145
0.29
0.00
145
BR
0.84
0.00
145
0.00
0.97
145
0.85
0.00
145
-0.22
0.01
145
0.56
0.00
145
-0.08
0.35
145
0.11
0.18
145
0.12
0.14
145
0.35
0.00
145
0.61
0.00
145
0.60
0.00
145
0.67
0.00
145
-0.27
0.00
145
0.13
0.13
145
-O.04
0.60
145
0.51
0.00
145
CA
0.08
0.32
145
0.25
0.00
145
0.00
0.97
145
0.47
0.00
145
-0.06
0.48
145
-0.14
0.08
145
0.58
0.00
145
0.44
0.00
145
0.35
0.00
145
-0.17
0.04
145
0.11
0.18
145
-0.28
0.00
145
0.47
0.00
145
0.25
0.00
145
0.04
0.63
145
0.17
0.05
145
CL
0.51
0.00
145
-0.04
0.61
145
0.49
0.00
145
-0.11
0.19
145
0.36
0.00
145
-0.12
0.16
145
0.09
0.31
145
0.19
0.02
145
0.24
0.00
145
0.26
0.00
145
0.29
0.00
145
0.35
0.00
145
-0.11
0.19
145
-0.01
0.90
145
-0.04
0.67
145
0.25
0.00
145
CU
0.14
0.09
145
-0.07
0.41
145
0.13
0.12
145
-0.10
0.21
145
0.09
0.29
145
0.00
0.99
145
0.02
0.84
145
-0.04
0.60
145
0.18
0.03
145
0.06
0.49
145
0.15
0.07
145
0.10
0.25
145
-0.13
0.12
145
-0.04
0.63
145
-O.12
0.16
145
0.10
0.21
145
FE
0.31
0.00
145
0.20
0.01
145
0.20
0.02
145
0.33
0.00
145
0.04
0.63
145
-0.21
0.01
145
0.58
0.00
145
0.45
0.00
145
0.51
0.00
145
-0.02
0.78
145
0.26
0.00
145
-0.10
0.24
145
0.33
0.00
145
0.18
0.03
145
0.04
0.66
145
0.36
0.00
145
K
0.32
0.00
145
0.12
0.15
145
0.28
0.00
145
0.24
0.00
145
0.10
0.24
145
-0.25
0.00
145
0.44
0.00
145
0.60
0.00
145
0.37
0.00
145
-0.02
0.80
145
0.15
0.08
145
-0.05
0.53
145
0.28
0.00
145
0.06
0.45
145
0.03
0.74
145
0.22
0.01
145
MN
0.45
0.00
145
0.03
0.69
145
0.37
0.00
145
0.15
0.07
,145
0.18
0.03
145
-0.11
0.20
145
0.37
0.00
145
0.36
0.00
145
0.55
0.00
145
0.15
0.07
145
0.36
0.00
145
0.09
0.28
145
0.04
0.67
145
0.27
0.00
145
0.03
0.73
145
0.50
0.00
145
P
0.54
0.00
145
-0.05
0.56
145
0.52
0.00
145
-0.36
0.00
145
0.45
0.00
145
0.07
0.40
145
-0.10
0.22
145
-0.07
0.38
145
0.31
0.00
145
0.58
0.00
145
0.40
0.00
145
0.63
0.00
145
-0.34
0.00
145
0.16
0.06
145
-0.02
0.85
145
0.36
0.00
145
PB
0.50
0.00
145
-0.02
0.80
145
0.45
0.00
145
-0.02
0.86
145
0.41
0.00
145
-0.01
0.90
145
0.17
0.05
145
0.12
0.14
145
0.42
0.00
145
0.25
0.00
145
0.61
0.00
145
0.25
0.00
145
-0.11
0.20
145
0.13
0.12
145
0.04
0.61
145
0.43
0.00
145
S
0.70
0.00
145
-0.03
0.68
145
0.73
0.00
145
-0.55
0.00
145
0.64
0.00
145
0.11
0.17
145
-0.28
0.00
145
-0.20
0.01
145
0.12
0.17
145
0.83
0.00
145
0.47
0.00
145
0.97
0.00
145
-0.47
0.00
145
0.01
0.87
145
-0.02
0.82
145
0.27
0.00
145
SI
-0.03
0.72
145
0.41
0.00
145
-0.10
0.22
145
0.55
0.00
145
-0.10
0.23
145
-0.17
0.04
145
0.68
0.00
145
0.50
0.00
145
0.23
0.01
145
-0.25
0.00
145
0.06
0.50
145
-0.37
0.00
145
0.70
0.00
145
0.19
,0.02
145
0.05
0.57
145
0.06
0.45
145
SR
0.14
0.08
145
-0.09
0.31
145
0.09
0.26
145
-0.05
0.52
145
0.13
0.13
145
-0.02
0.85
145
0.06
0.49
145
-0.01
0.94
145
0.17
0.04
145
0.03
0.76
145
0.15
0.07
145
0.05
0.55
145
-0.04
0.67
145
0.20
0.02
145
-0.04
0.60
145
0.26
0.00
145
TI
0.09
0.30
145
0.00
0.98
145
0.06
0.48
145
0.04
0.61
145
0.04
0.61
145
0.03
0.73
145
0.07
0.43
145
0.02
0.79
145
0.24
0.00
145
0.11
0.19
145
0.09
0.28
145
0.05
0.55
145
-0.01
0.94
145
0.20
0.02
145
0.05
0.56
145
0.19
0.02
145
ZN
0.34
0.00
145
-0.05
0.52
145
0.29
0.00
145
0.02
0.84
145
0.19
0.02
145
-0.08
0.33
145
0.27
0.00
145
0.24
0.00
145
0.58
0.00
145
0.07
0.39
145
0.35
0.00
145
0.05
0.54
145
-0.09
0.29
145
0.18
0.04
145
-0.07
0.41
145
0.52
0.00
145
5-93
-------
TABLE 5-21. CORRELATIONS OF CENTRAL-SITE PARTICLE
AND ELEMENT CONCENTRATIONS WITH THOSE
MEASURED OUTDOORS AT RESIDENCES: PM2.5 DAYTIME
PM_c
ALjC
BRjC
CA_C
CL_C
CU_C
F5_C
K_C
MN_C
P_C
PB_C
S_C
si_c
SRjC
WA>_N*
TL.C
**mr^
ZN_C
0.92
0.00
138
0.01
0.86
138
0.83
0.00
138
-O.08
0.33
138
0.76
0.00
138
0.28
0.00
138
0.00
0.97
138
0.24
0.01
138
0.10
0.2S
138
0.68
0.00
138
0.45
0.00
138
0.78
0.00
138
-0.08
0.33
138
0.05
0.56
138
0.08
0.34
138
0.39
0.00
138
0.00
0.99
138
0.19
0.02
138
-0.03
0.70
138
0.21
0.01
138
-0.04
0.63
138
-0.02
0.78
138
0.25
0.00
138
0.26
0.00
138
0.12
0.15
138
0.07
0.42
138
-0.05
0.59
138
-0.07
0.42
138
0.28
0.00
138
0.19
0.03
138
0.26
0.00
138
-0.03
0.70
138
0.74
0.00
138
-0.09
0.27
138
0.74
0.00
138
-0.18
0.03
138
0.63
0.00
138
0.23
0.01
138
-0.12
0.18
138
0.12
0.16
138
-0.01
0.88
138
0.64
0.00
138
0.37
0.00
138
0.74
0.00
138
-0.17
0.04
138
-0.03
0.72
138
0.02
0.82
138
0.30
0.00
138
0.03
0.72
138
0.37
0.00
138
-0.13
0.13
138
0.44
0.00
138
-0.17
0.05
138
0.03
0.75
138
0.51
0.00
138
0.43
0.00
138
0.47
0.00
138
-0.03
0.72
138
0.19
0.02
138
-0.30
0.00
138
0.50
0.00
138
0.31
0.00
138
0.40
0.00
138
0.20
0.02
138
0.66
0.00
138
-0.06
0.46
138
0.71
0.00
138
-0.13
0.12
138
0.90
0.00
138
-0.10
0.23
138
-0.16
0.05
138
-0.02
0.81
138
-0.16
0.06
138
0.51
0.00
138
0.01
0.92
138
0.74
0.00
138
-0.14
0.09
138
-0.11
0.21
138
-0.02
0.83
138
0.15
0.07
138
0.18
0.03
138
0.00
0.96
138
0.16
0.06
138
-0.02
0.82
138
-0.01
0.87
138
0.18
0.04
138
0.05
0.53
138
0.08
0.35
138
0.17
0.05
138
0.14
0.10
138
0.34
0.00
138
0.09
0.28
138
0.01
0.95
138
-0.03
0.73
138
0.07
0.43
138
0.30
0.00
138
O.JO
0.22
133
0.43
0.00
138
-0.05
0.52
138
0.53
0.00
138
-0.12
0.18
138
-0.01
0.89
138
0.58
0.00
138
0.49
0.00
138
0.54
0.00
138
0.02
OJ78
138
0.18
0.03
138
-0.23
0.01
138
0.56
0.00
138
0.41
0.00
138
0.45
0.00
138
0.24
0.00
138
0.36
0.00
138
0.27
0.00
138
0.21
0.01
138
0.28
0.00
138
-0.01
0.93
138
0.17
0.05
138
0.41
0.00
138
0.54
0.00
138
0.39
0.00
138
0.23
0.01
138
0.46
0.00
138
0.02
0.77
138
0.31
0.00
138
0.32
0.00
138
0.29
0.00
138
0.39
0.00
138
0.14
0.10
138
0.15
0.07
138
0.08
0.33
138
0.21
0.01
138
-0.01
0.87
138
0.10
0.22
138
0.35
0.00
138
0.29
0.00
138
0.36
0.00
138
-0.01
0.89
138
0.31
0.00
138
-0.12
0.17
138
0.24
0.00
138
0.15
0.07
138
0.13
0.13
138
0.38
0.00
138
0.52
0.00
138
-0.09
0.32
138
0.61
0.00
138
-0.19
0.03
138
0.46
0.00
138
0.18
0.03
138
-0.17
0.04
138
0.07
0.38
138
-0.10
0.24
138
0.60
0.00
138
0.17
0.05
138
0.67
0.00
138
-0.17
0.05
138
-0.06
0.52
138
0.07
0.40
138
0.09
0.29
138
0.30
0.00
138
-0.05
0.57
138
0.29
0.00
138
-0.01
0.93
138
0.04
0.67
138
0.21
0.02
138
0.13
0.11
138
0.25
0.00
138
0.30
0.00
138
0.15
0.08
138
0.57
0.00
138
'0.13
0.14
138
0.02
0.82
138
-0.06
0.46
138
0.06
0.46
138
0.57
0.00
138
0.71
0.00
138
-0.16
0.06
138
0.81
0.00
138
-0.32
0.00
138
0.77
0.00
138
0.10
0.22
138
-0.33
0.00
138
-0.06
0.45
138
-0.22
0.01
138
0.77
0.00
138
0.11
0.18
138
0.99
0.00
138
-0.32
0.00
138
-0.15
0.07
138
-0.06
0.49
138
• 0.13
0.12
138
-0.04
0.61
138
0.56
0.00
138
-0.22
0.01
138
0.63
0.00
138
-0.17
0.05
138
-0.11
0.20
138
0.62
0.00
138
0.51
0.00
138
0.48
0.00
138
-0.06
0.50
138
-0.05
0.52
138
-0.33
0.00
138
0.68
0.00
138
0.48
OJOO
138
0.54
0.00
138
-0.01
0.95
138
0.05
0.58
138
-0.10
0.27
138
0.12
0.17
138
-0.10
0.23
138
-0.07
0.44
138
.0.10
0.26
138
-0.08
0.36
138
0.04
0.67
. 138
-0.11
0.21
138
0.10
0.24
138
0.04
0.66
138
0.07
0.43
138
-0.09
0.29
138
-0.03
0.69
138
-0.04
0.65
138
-0.03
0.72
138
0.01
0.91
138
0.17
0.05
138
0.01
0.95
138
0.15
0.08
138
-0.06
0.45
138
0.01
0.89
138
0.12
0.15
138
0.15
0.09
138
"0.09
0.27
138
0.10
0.25
138
0.00
0.99
138
-0.03
0.76
138
0.17
0.04
138
0.13
0.13
138
0.20
0.02
138
-0.06
0.49
138
0.15
0.09
138
-0.02
0.80
138
0.19
0.03
138
-0.01
0.89
138
0.06
0.49
138
0.16
0.06
138
0.07
0.43
138
0.09
0.31
138
0.15
0.08
138
0.08
0.33
138
0.31
0.00
138
0.07
0.41
138
-0.03
0.73
138
-0.05
0.59
138
0.00
0.98
138
0.37
0.00
138
5-94
-------
TABLE 5-22. CORRELATIONS OF CENTRAL-SITE PARTICLE
AND ELEMENT CONCENTRATIONS WITH THOSE
MEASURED OUTDOORS AT RESIDENCES: PM10 OVERNIGHT
PM_C
AL_C
BR_C
CA_C
CL_C
CU_C
FB_C
K_C
MN_C
P_C
PB_C
S_C
SLC
SR_C
TLC
ZN_C
PM
0.93
0.00
148
-0.04
0.65
148
0.89
0.00
148
-0.09
0.27
148
-0.05
0.54
148
0.27
0.00
148
0.26
0.00
148
0.18
0.03
148
0.30
0.00
'148
0.63
0.00
148
0.65
0.00
148
0.76
0.00
148
0.05
0.53
148
0.05
0.55
148
0.20
0.01
148
0.49
0.00
148
AL
0.13
0.12
148
0.50
0.00
148
0.00
0.97
148
0.37
0.00
148
0.08
0.31
148
-0.02
0.85
148
0.62
0.00
148
0.50
0.00
148
0.64
0.00
148
0.02
0.78
148
0.15
0.08
148
-0.20
0.01
148
0.57
0.00
148
0.59
0.00
148
0.58
0.00
148
0.26
0.00
148
BR
0.82
0.00
148
-0.19
0.02
148
0.84
0.00
148
-0.17
0.04
148
0.01
0.88
148
0.21
0.01
148
0.07
0.41
148
0.04
0.67
148
0.13
0.12
148
0.55
0.00
148
0.54
0.00
148
0.71
0.00
148
-O.12
0.13
148
-0.07
0.43
148
0.02
0.81
148
0.38
0.00
148
CA
0.18
0.03
148
0.30
0.00
148
0.08
0.35
148
0.26
0.00
148
0.15
0.06
148
0.03
0.74
148
0.46
0.00
148
0.41
0.00
148
0.49
0.00
148
0.11
0.18
148
0.18
0.03
148
-0.08
0.31
148
0.38
0.00
148
0.47
0.00
148
0.41
0.00
148
0.27
0.00
148
CL
0.16
0.05
148
-0.17
0.04
148
0.17
0.04
148
-0.16
0.05
148
0.52
0.00
148
0.02
0.77
148
-0.04
0.63
148
0.07
0.38
148
0.02
0.82
148
0.03
0.71
148
0.04
0.67
148
0.12
0.14
148
-0.09
0.27
148
-0.04
0.59
148
-0.11
0.18
148
-0.06
0.47
148
cu
0.16
0.05
148
-0.02
0.84
148
0.15
0.06
148
-0.01
0.92
148
-0.12
0.16
148
-0.04
0.66
148
0.10
0.22
148
-0.04
0.60
148
0.10
0.21
148
-0.03
0.68
148
0.32
0.00
148
0.01
0.87
148
-0.02
0.78
148
0.00
0.99
148
-0.04
0.60
148
'0.27
0.00
148
FE
0.31
0.00
148
0.32
0.00
148
0.22
0.01
148
0.23
0.00
148
0.09
0.28
148
0.06
0.46
148
0.56
0.00
148
0.41
0.00
148
0.59
0.00
148
0.14
0.10
148
0.30
0.00
148
-0.04
0.64
148
0.42
0.00
148
0.47
0.00
148
0.48
0.00
148
0.37
0.00
148
K
0.28
0.00
148
0.27
0.00
148
0.19
0.02
148
0.17
0.05
148
0.18
0.03
148
0.01
0.87
148
0.46
0.00
148
0.46
0.00
148
0.49
0.00
148
0.18
0.03
148
0.20
0.02
148
0.03
0.72
148
0.38
0.00
148
0.44
0.00
148
0.39
0.00
148
0.22
0.01
148
MN
0.34
0.00
148
0.29
0.00
148
0.25
0.00
148
O.23
0.00
148
0.11
0.18
148
0.08
0.35
148
0.52
0.00
148
0.38
0.00
148
0.57
0.00
148
0.15
0.06
148
0.32
0.00
148
-O.01
0.91
148
0.38
0.00
148
0.46
0.00
148
0.46
0.00
148
0.37
0.00
148
P
0.45
0.00
148
-0.03
0.72
148
0.41
0.00
148
-0.06
0.50
148
0.07
0.38
148
0.08
0.33
148
0.11
0.18
148
0.15
0.06
148
0.13
0.13
148
0.42
0.00
148
0.31
0.00
148
0.41
0.00
148
0.02
0.84
148
0.15
0.08
148
0.12
0.15
148
0.27
0.00
148
PB
0.56
0.00
148
0.00
0.98
148
0.53
0.00
148
0.01
0.93
148
-0.07
0.41
148
0.14
0.10
148
0.21
0.01
148
0.05
0.56
148
0.29
0.00
148
0.25
0.00
148
0.72
0.00
148
0.29
0.00
148
0.01
0.89
148
0.07
0.40
148
0.17
0.04
148
0.48
0.00
148
S
0.73
0.00
148
-0.27
0.00
148
0.78
0.00
148
-0.35
0.00
148
-0.04
0.67
148
0.24
0.00
148
-0.14
0.08
148
-0.06
0.45
148
-0.17
0.04
148
0.68
0.00
148
0.37
0.00
148
0.97
0.00
148
-0.23
0.00
148
-0.25
0.00
148
-0.11
0.20
148
0.17
0.04
148
SI
0.18
0.03
148
0.49
0.00
148
0.06
0.45
148
0.33
0.00
148
0.13
0.11
148
-0.01
0.86
148
0.62
0.00
148
0.54
0.00
148
0.63
0.00
148
0.09
0.30
148
0.18
0.03
148
-0.13
0.12
148
0.58
0.00
148
0.60
0.00
148
0.58
0.00
148
0.25
0.00
148
SR
0.24
0.00
148
0.28
0.00
148
0.14
0.08
148
0.14
0.08
148
0.18
0.03
148
0.08
0.33
148
0.45
0.00
148
0.40
0.00
148
0.46
0.00
148
0.18
0.03
148
0.15
0.07
148
0.02
0.77
148
0.38
0.00
148
0.46
0.00
148
0.42
0.00
148
0.28
0.00
148
TI
0.17
0.04
148
0.37
0.00
148
0.07
0.41
148
0.25
0.00
148
0.15
0.06
148
0.01
0.88
148
0.54
0.00
148
0.45
0.00
148
0.57
0.00
148
0.06
0.44
148
0.14
0.09
148
-0.12
0.15
148
0.46
0.00
148
0.53
0.00
148
0.49
0.00
148
0.27
0.00
148
ZN
0.39
0.00
148
0.05
0.55
148
0.35
0.00
148
0.01
0.92
148
-0.09
0.29
148
0.06
0.46
148
0.28
0.00
148
0.09
0.26
148
0.31
0.00
148
0.13
0.10
148
0.49
0.00
148
0.11
0.17
148
0.05
0.52
148
0.09
0.26
148
0.17
0.04
148
0.52
0.00
148
5-95
-------
TABLE 5-23. CORRELATIONS OF CENTRAL-SITE PARTICLE
AND ELEMENT CONCENTRATIONS WITH THOSE
MEASURED OUTDOORS AT RESIDENCES: PM10 DAYTIME
PM_C
AI<_C
BR_C
CA_C
CL_C
CU_C
FE_C
K_C
MN_C
P_C
PB_C
S_C
SI_C
SR_C
TLC
ZN_C
PM
0.64
0.00
131
0.19
0.03
131
0.50
0.00
131
0.14
0.11
131
0.32
0.00
131
0.02
0.86
131
0.24
0.01
131
0.26
0.00
131
0.24
0.01
131
0.48
0.00
131
0.23
0.01
131
0.45
0.00
131
0.23
0.01
131
0.18
0.04
131
0.24
0.01
131
0.31
0.00
131
AL
0.21
0.02
131
0.62
0.00
131
-0.21
0.02
131
0.52
0.00
131
-0.22
0.01
131
-0.10
0.26
131
0.60
0.00
131
0.59
0.00
131
0.60
0.00
131
0.26
0.00
131
0.01
0.89
131
-0.30
0.00
131
0.64
0.00
131
0.55
0.00
131
0.62
0.00
131
0.15
0.09
131
BR
0.62
0.00
131
-0.25
0.00
131
0.85
0.00
131
-0.21
0.02
131
0.57
0.00
131
0.17
0.06
131
-0.15
0.08
131
-0.12
0.17
131
-0.15
0.09
131
0.42
0.00
131
0.37
0.00
131
0.81
0.00
131
-0.22
0.01
131
-0.21
0.02
131
-0.17
0.05
131
0.34
0.00
131
CA
0.24
0.01
131
0.49
0.00
131
-0.10
0.25
131
0.40
0.00
131
-0.19
0.03
131
0.03
0.77
131
0.54
0.00
131
0.51
0.00
131
0.54
0.00
131
0.26
0.00
131
0.23
0.01
131
-0.25
0.00
131
0.54
0.00
131
0.46
0.00
131
0.53
0.00
131
0.31
0.00
131
CL
0.38
0.00
131
-0.16
0.07
131
0.53
0.00
131
-0.14
0.12
131
0.81
0.00
131
-O.24
0.01
131
-0.15
0.09
131
-0.13
0.15
131
-0.15
0.08
131
0.24
0.01
131
0.02
0.83
131
0.61
0.00
131
-0.16
0.07
131
-0.13
0.15
131
-0.20
0.02
131
0.06
0.50
131
CU
0.02
0.86
131
0.01
0.89
131
0.06
0.53
131
0.00
0.99
131
-0.12
0.16
131
0.07
0.40
131
0.10
0.27
131
0.05
0.56
131
0.10
0.25
131
0.09
0.31
131
0.35
0.00
131
-0.06
0.51
131
0.04
0.66
131
0.00
0.99
131
0.04
0.68
131
0.29
0.00
131
FE
0.2S
0.00
131
0.53
0.00
131
-0.12
0.17
131
0.44
0.00
131
-0.19
0.03
131
-0.04
0.61
131
0.56
0.00
131
0.53
0.00
131
0.55
0.00
131
0.27
0.00
1311
0.12
0.16
131
-0.25
0.00
131
0.57
0.00
i3i
0.49
0.00
131
0.55
0.00
131
0.24
0.01
131
K
0.29
0.00
131
0.51
0.00
131
-0.06
0.52
131
0.43
0.00
131
-0.18
0.04
131
-0.04
0.68
131
0.54
0.00
131
0.53
0.00
131
0.54
0.00
131
0.32
0.00
131
0.13
0.14
131
-0.19
0.03
131
0.55
0.00
131
0.48
0.00
131
0.54
0.00
131
0.22
0.01
131
MN
0.24
0.01
131
0.51
0.00
131
-0.11
0.20
131
0.42
0.00
131
-0.17
0.05
131
0.00
0.96
131
0.54
0.00
131
0.50
0.00
131
0.53
0,00
131
0.26
0.00
131
0.16
0.07
131
-0.24
0.01
131
0.54
0.00
131
0.47
0.00
131
0.53
0.00
131
0.26
0.00
131
P
0.44
0.00
131
0.12
0.19
131
0.40
0.00
131
0.08
0.36
131
0.17
0.05
131
0.04
0.64
131
0.17
0.05
131
0.20
0.02
131
0.17
0.06
131
0.41
0.00
131
0.19
0.03
131
0.31
0.00
131
0.16
0.06
131
0.13
0.14
131
0.18
0.04
131
0.20
0.02
131
PB
0.20
0.02
131
-0.05
0.57
131
0.34
0.00
131
-0.04
0.67
131
0.05
0.56
131
0.27
0.00
131
0.08
0.35
131
0.04
0.68
131
0.08
0.37
131
0.16
0.06
131
0.61
0.00
131
0.14
0.10
131
-0.01
0.93
131
-O.03
0.77
131
0.01
0.92
131
0.45
0.00
131
S
0.55
0.00
131
-0.32
0.00
131
0.85
0.00
131
-0.29
0.00
131
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In the daytime samples (Table 5-25), the strongest
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with both inhalable and fine particles indoors (p < 0.0001) and
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positive correlation with indoor PM10. Again homes with larger
air exchange rates showed a positive correlation with indoor
particles.
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smokers continued to show the strongest positive associations
with nicotine and indoor particles. Cooking also had significant
associations with indoor and personal particle levels, and also
with personal, but not indoor, nicotine levels. Vacuuming and
dusting showed significant positive correlations with both
5-98
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outdoor and indoor particle levels. Homes with higher air
exchange rates had significantly higher indoor and personal
particle concentrations.
Since some of the above variables may be covariates, a
correlation matrix of covariates was calculated for daytime
(Table 5-28), overnight (Table 5-29) and combined (Table 5-30)
samples. Two new variables (area coverage by carpets and
technicians' estimates of dirt level in the homes) are included.
The area covered by carpets was calculated from responses to
questions on the questionnaire. The technicians' estimate of
dirt level was made while measuring each room to determine the
house volume. Two technicians carried out all the measurements.
They estimated dirt and dust levels on a 7-point scale, and
"calibrated" themselves by experimenting on several Boston homes
before going to Riverside. Dusting was highly correlated with
vacuuming; air exchange rate was significantly positively
correlated with house age and negatively correlated with house
volume; dirt level was positively correlated with home age; and
home age was negatively correlated with house volume.
Correlations between particle and nicotine levels and
between the two new variables (carpet coverage and dirt level)
and three meteorological variables (temperature, dewpoint, and
wind speed, all measured at the nearby March Air Force Base) are
provided in Tables 5-31 to 5-33.
During the day (Table 5-31) , personal and indoor PM10 were
significantly correlated with estimated household dirt level. No
5-102
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significant (p < 0.01) correlations appeared with temperature or
with wind speed. Both outdoor and indoor fine particles were
positively correlated with dewpoint; indoor nicotine was
negatively associated.
In the overnight samples (Table 5-32) personal and indoor
particles and nicotine were all significantly associated with
estimated dirt level. Indoor nicotine was negatively associated
with temperature and dewpoint, and positively associated with
wind speed. Outdoor particle levels were positively associated
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associated with wind speed.
In the combined day-night samples (Table 5-33), personal and
indoor particles and indoor nicotine continued to be
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temperature.
ANALYSIS OF VARIANCE
Based on the correlations above, variables were selected for
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night effect. Results (Table 5-34) indicate that cooking,
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and indoor PM10 concentrations. Older homes and those with
smokers and with higher air exchange rates were also associated
5-109
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with higher particle concentrations. Only homes with smokers
were associated with higher nicotine concentrations.
Next, a multivariate ANOVA was carried out on the same
variables (Table 5-35). In this analysis, dusting and home age
no longer had a significant effect on any measured indoor
concentrations, and vacuuming had a weak effect only on indoor
fine particles. The effect of cooking was restricted to indoor
PM10. The associations with air exchange rates and with smoking
continued to be significant.
SIMPLE REGRESSIONS
Simple regressions of indoor PM10 mass and elemental
concentrations on outdoor levels were carried out. The model
fitted is
where
C,, = indoor concentration (PM2.5, PM10, or elements)
C^ = outdoor concentration
j80 = concentration due to indoor sources
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measures contribution of outdoor constituent
to indoor air concentrations
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5-113
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intercept (/30) not significantly different from zero. The
intercept for PM10 was higher in the daytime (51 jug/m3) than at
night (20 /ig/m3), suggesting the importance of daytime activities
in elevating indoor concentrations. Daytime intercepts for most
of the elements were also higher than the overnight values.
Sulfur had the highest R2 values (84-88%) and the highest slopes
(0.72-0.8), suggesting a relative lack of indoor sources and good
penetration (since sulfur hcis the smallest mass median diameter
of the targeted elements).
The slopes of the regression lines (/?!) were generally in
the range of 0.3 to 0.7 (mean values of 0.41 at night and 0.53 in
the day), suggesting an overall contribution to indoor air of
about half the outdoor concentrations of PM10 particles and
elements.
A simple regression of the combined day and night 12-h
indoor PM10 concentrations on the concurrent outdoor (backyard)
levels showed that outdoor concentrations explained only 27% of
the variance observed in the* indoor levels (Figure 5-72) . Very
similar results (R2 = 25-28%) were obtained if the backyard
concentrations were replaced by the concentrations at the central
site/ as measured by any one of the three methods (SAM,
dichotomous, or high-volume samplers) employed there.
Results from similar regressions for fine (PM2.5) particles
and the associated elements are summarized in Table 5-37. Two
elements, titanium and sulfur, had high R2 values and intercepts
not significantly different from zero, suggesting no indoor
5-116
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sources. The daytime intercept did not exceed the overnight
value for fine particle mass, but some elements (calcium,
aluminum, potassium) showed higher daytime j80 values than
overnight.
The slopes associated with the fine particles and elements
were generally in the range of 0.4 to 0.8 (mean values of 0.54 at
night and 0.61 in the daytime) suggesting a slightly higher
contribution (nearly 0.6) for outdoor fine (PM2.5) particles than
for outdoor inhalable (PM10) particles. The models explained
about 50% of the indoor fine particle variance.
Simple regressions of personal exposures on indoor and on
outdoor concentrations were also carried out. Results are
summarized in Figures 5-73 and 5-74. Indoor concentrations alone
explained about 49% of the variance in personal exposures, but
outdoor concentrations alone explained only 16% of the variance
in personal exposures. These results were nearly unchanged when
the regressions were carried out on the logarithms of the
personal indoor, and outdoor concentrations. Similarly, the
results were nearly unchanged (R2 values of 16-18%) when the
backyard concentrations were replaced by the central site
concentrations measured by any of the three methods.
To test how well the central site can represent neighborhood
exposures, central site concentrations as measured by the mean of
the two dichotomous reference samplers were regressed on the
backyard concentrations. The results are summarized in Figure 5-
5-120
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5-121
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5-122
-------
75. The central site explained about 57% of the observed
variance in the backyard concentrations.
A simple regression of 12-h average (harmonic mean) air
exchange rates on house volumes indicated that air exchange rates
were lower in larger homes (Figure 5-76). The regression was
limited to those homes in which all measurements in a given 12-
hour period exceeded the limit of detection. A total of 258
observations were available for the regression. The air exchange
rate dropped by 0.056 h"1 for every additional 1000 ft3 of house
volume (R2 = 12%) .
A corresponding regression of 12-h average (arithmetic mean)
residence times • (Figure 5-77) showed an increase in the residence
time of 0.12 h per 1000 cubic feet, or about six minutes per 100
square feet of house area.
As mentioned above in the section on correlations, the
larger homes were also newer homes. Since newer homes employ
construction methods that lead to a tighter seal, it might be
expected that they would have lower air exchange rates. Larger
(more expensive) homes may also be better constructed than some
smaller (less expensive) homes.
MULTIPLE REGRESSIONS
Personal exposures to particles and elements were modeled
using a simple time-weighted average of concentrations indoors
and outdoors:
5-123
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5-126
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where the new parameters are
personal concentration (PM2.5/ PM^, or
elements)
concentration due to personal activities not
affecting indoor or outdoor monitors
factor multiplying concentration measured
indoors, weighted by fraction of time person
spent indoors
factor multiplying concentration measured
outdoors, weighted by fraction of time person
spent outdoors
fraction of monitoring period spent indoors
fraction of monitoring period spent outdoors
In the ideal case (the person stays at home, either indoors
or in his yard, for the entire monitoring period), the
coefficients /?! and j82 would both equal 1, and exposure would be
a time-weighted average of the indoor and outdoor concentrations
(plus the personal contribution /30) .
This model is more appropriately applied to the overnight
values, since the measured concentrations (Cto and C^) are more
likely to be those actually experienced by the respondent, most
of whom spent the entire overnight period at or near their homes.
5-127
-------
In fact, the model is able to explain 66% of the variance in
personal PM10 concentrations at night, compared to only 39%
during the day, when many participants were away from their homes
(Table 5-38). The proportions of the variance explained for most
of the elemental concentrations are generally smaller than for
particle mass, but show the same relative increase during the
night compared to the daytime values. A singular exception is
sulfur, personal exposure to which is explained very well by the
model (Rz - 89% at night, 85% during the day). This suggests
that few or no sources of sulfur are provided by personal
activities. By contrast, no other element exceeded 40% Rz values
for both day and night monitoring periods. The fact that
intercept terms are generally significantly different from zero
implies that some portion of total exposure is due to personal
activities not impacting the indoor monitors. For PM10 mass, the
daytime intercept of 65 jug/ra3 greatly exceeds the overnight
intercept of 21 ^g/m3, again suggesting the importance of waking
activities in contributing to personal exposure. Values of /30
are significantly different from zero for all elements except
bromine, lead, and phosphorus in the daytime, and all except
bromine at night.
Values for Pi often range between 0.7 and 0.9 at night, and
between 0.6 and 0.8 in the daytime. Since time spent indoors
(£,„) greatly exceeds time spent outdoors (£„„) , these high values
suggest a strong influence of indoor particle and elemental
concentrations on personal exposure. Values of j82 are also high,
5-128
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but the much smaller values of f^ result in a smaller
contribution of outdoor air to personal exposure than indoor air.
When the model is restricted to persons who were close to
their homes (more than 80% of the monitoring period), a dramatic
improvement in the daytime performance is apparent (Table 5-39);
the Rz value for PM10 is 66% (N =35) compared to the 39% when all
respondents are included. The overnight performance of the model
improves only slightly (from 66% to 68%).
When the model is applied only to persons who spent a large
proportion of time away from home (Table 5-40), its predictive
power falls off sharply. R2 values are less than 20% for most
elements, and range between 25% and 42% for particle mass.
Results of applying the model to fine particles and
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to 17 A"3/ra3 at night. The intercepts of 12 of the 15 elements
were also significantly positive,, attesting to the presence of
personal sources of exposure over and above the indoor sources.
However, indoor sources were also significant during the day-—
indoor concentrations of particles and all 15 elements made
significant contributions to personal exposures. By contrast,
none of the outdoor concentrations contributed significantly in a
positive way. This suggests that daytime outdoor fine particle
5-130
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5-133
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concentrations do not contribute substantially to personal
exposure, except by their contribution to the
indoor concentrations.
At night, when the personal monitor was placed on the
bedside table and thus became a fixed indoor monitor for much of
the monitoring period, the results were markedly different. Less
than half of the elements had significant intercepts, suggesting
no particular personal sources or contributions from unmeasured
microenvironments. However, all but one of the elements
associated with the indoor samples made significant contributions
to exposure, and more than half of the outdoor elements also made
significant contributions.
STEPWISE REGRESSIONS
Particles and Nicotine
A series of stepwise regressions were performed on the
personal particle mass and elemental concentrations as dependent
variables. The independent variables included particle
concentrations indoors and outdoors, as well as concentrations
weighted by the time spent in each microenvironment.
The stepwise regressions selected indoor particle mass as
the most important variable in every instance (Table 5-42).
Outdoor concentrations were also significant in more than half of
the runs. When the model was restricted to persons near home
most of the time, again the indoor concentrations were selected
5-134
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5-135
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in every case as the most important variable (Table 5-43). In
only a few cases was the outdoor concentration significant.
Applying the model to only those persons away from home a
substantial amount of time, there were a few cases (aluminum,
iron/ silicon) in which the outdoor concentration was significant
(Table 5-44); in all these cases, the indoor concentration at
home was not significant.
Stepwise regressions were also run on the personal, indoor,
and outdoor particle and nicotine concentrations as dependent
variables, with questionnaire and meteorological results as
independent variables, but excluding particle concentrations as
independent variables to simulate the case in which no
information is available on outdoor air particle concentrations
(Table 5-45). The proportion of the variance explained was small
for most variables (as low as 7% for outdoor PM10) but reached
moderate levels for personal PM10 (27%) and indoor nicotine
(48%).
Personal PM10 exposures were increased by vacuuming, by
increased air exchange rates, and by decreased wind speed.
Indoor PM10 concentrations were increased by cooking, smoking,
and increased air exchange rates. . Indoor PM2-5 concentrations
were increased by smoking, vacuuming, decreased house volume, and
increased dewpoint. Outdoor PM10 and PM2.5 concentrations were
inversely related to wind speed. Personal, indoor, and outdoor
PM10 concentrations were all significantly lower at night.
5-136
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5-137
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5-138
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5-139
-------
Nicotine concentrations were significantly increased in
homes with smokers.
A set of stepwise regressions was performed on the day and
night concentrations separately (Table 5-46). Personal exposures
were increased by reported smoking at home during the night but
not during the day. Outdoor concentrations at night were
inversely related to outdoor temperature and wind speed, and
directly to dewpoint temperature (R2 = 25-30%).
When particle concentrations were included as independent
variables, the proportion of the variance explained increased,
ranging between 30 and 60% for indoor and personal particle and
nicotine variables (Table 5-47).
For personal PM10 exposures, the single variable of
significance (other than the day-night effect) was indoor PM10
concentration, which had a slope of 0.86. Indoor PM10
concentrations were increased by increased outdoor
concentrations, increased air exchange rates and the number of
cigarettes smoked in the home. For indoor fine particles, the
outdoor fine particle concentration was a significant contributor
(slope = 0.64), as well as increased air exchange rates, number
of cigarettes smoked in the house, and outdoor temperature.
Indoor nicotine levels were significantly affected by number
of cigarettes smoked in the home, and personal nicotine levels
were in turn significantly affected by indoor nicotine. Indoor
nicotine was also affected by air exchange rate.
5-140
-------
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5-142
-------
Stepwise regressions were also run on the daytime and
overnight data sets separately to remove the day-night effect
(Table 5-48). Relatively high R2 values of 43-69% were noted for
the overnight personal and indoor particle and nicotine results.
R2 values during the day were reduced, ranging between 25% and
57%.
Personal exposure to PM10 depended primarily on indoor
concentrations. Indoor PM10 and PM2.5 concentrations depended
primarily on outdoor concentrations and on household smoking
(both day and night). A dependence on air exchange rate was
noted at night but not during the day for both size fractions.
Outdoor particle levels were dependent only on meteorological
variables, and in one case, home age.
Personal nicotine exposures (both day and night) were
dependent on indoor nicotine concentrations. Indoor nicotine
(day only) was dependent on household smoking status.
Since particle concentrations are normally available only
from a central monitoring station, similar stepwise regressions
were performed by replacing the residential outdoor
concentrations by those measured at the central site (Table 5-
49) . R2 values for the indoor inhalable and fine particles were
barely affected, providing further evidence that a single central
site monitor can provide a good indication of outdoor
concentrations throughout the area. However, R2 values were
reduced for personal particle exposure estimates.
5-143
-------
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5-145
-------
Elements
Similar stepwise regressions were performed on the
concentrations of six elements in personal, indoor, cind outdoor
samples (Tables '5-50 to 5-55).
Lead. At night, personal exposures to lead could be
predicted well (Rz = 95%) by indoor and outdoor concentrations
(Table 5-50). During the day, when people are using motor
vehicles away from the PTEAM measuring instruments, personal lead
exposures could hardly be predicted at all (R2 = 5%) , with only
outdoor concentrations contributing to exposure estimates.
Overnight indoor concentrations were well explained (R2 = 72-79%)
by outdoor levels and by air exchange rates. Daytime indoor lead
concentrations were moderately well explained (R2 = 50-65%) by
outdoor concentrations and by air exchange rates. Dusting and
vacuuming were also associated with increased levels of indoor
lead concentrations during the day. Lead levels were higher in
older homes. Outdoor concentrations were not well explained (R2
= 3-14%) by any variables.
Sulfur. Personal exposures to sulfur were very well
predicted (R2 = 88-89%) by indoor and (night only) outdoor
concentrations (Table 5-51). Indoor concentrations were well
explained (R2 = 88-94%) by outdoor concentrations and air
exchange rates. Outdoor concentrations were not explained well
by any variables (R2 = 5-7%) . Older homes were located in areas
with higher outdoor sulfur concentrations.
5-146
-------
TABLE 5-50. STEPWISE REGRESSION: LEAD (ng/m3)
DEPENDENT VARIABLES
PEM10
SIM10
SIM25 SAM10
SAM25
Overnight
N
R2
INTERCEPT
SIM10
SAM10
SAM25
AER_AVG
COOK
HOUSE
SMOKE
HOMEAGE
MAR_AMBT
MAR_DWPT
MSPDJNV
120
0.95
-1.19
0.82
0.20
-0.82
125
0.72
-13.60
1.31
-0.27
126 134
0.79 0.04
-15.33 31.02
1.56
. 0.25
134
0.03
23.52
0.16
Daytime
N
R2
INTERCEPT
SIM10
SAM10
SAM25
AER_AVG
COOK
DUST
HOUSE
SMOKE
VACUM
HOMEAGE
MAR_AMBT
MAR_DWPT
MSPDJNV
118
0.05
18.87
0.72
133
0.50
5.34
0.48
3.73
0.39
3.22
127 139
0.65 0.14
6.50 -73.03
0.62
0.15
1.4
134
0.09
-18.67
0.56
5-147
-------
TABLE 5-51. STEPWISEE REGRESSION: SULFUR
DEPENDENT VARIABLES
PEM10
SIM10
SIM25 SAM10
SAM25
Overnight
N
R2
INTERCEPT
SIM10
SAM10
SAM25
NICJ
AER_AVG
COOK
HOUSE
SMOKE
HOMEAGE
120
0.89
172.52
0.68
0.18
125
0.88
-49.23
0.72
200.39
126 134
0.92 0.06
-132.97 1508.95
0.80
175.20
633.06
134
0.07
1226.13
626.97
Daytime
N
R2
INTERCEPT
SIM 10
SAM10
SAM25
NICJ
AER_AVG
COOK
DUST
HOUSE
SMOKE
VACUM
HVOLUME
HOMEAGE
118
0.88
375.85
0.89
2.37
-46.27
133
0.92
-50.69
0.78
200.09
1.11
26.12
127 139
0.94 0.05
1371.81
0.82
121.91
647.94
134
0.06
1187.32
31 .79
466.36
5-148
-------
Bromine. Personal exposures to bromine (Table 5-52) were
dependent on indoor concentrations, with only moderate values of
R2 (32-40%). Indoor concentrations showed significant effects
both of outdoor concentrations and number of cigarettes smoked.
Outdoor concentrations showed a moderate dependence on
meteorological variables, particularly the dewpoint temperature
(R2 = 16-30%).
Silicon. Personal exposures to this crustal element were
somewhat related (R2 = 15-36%) to indoor concentrations and
(overnight only) outdoor concentrations (Table 5-53). Indoor
levels were related to outdoor concentrations only at night, but
to outdoor concentrations household activities, vacuuming, and
meteorological variables in the daytime. Outdoor concentrations
were related to meteorological variables at moderate levels (R2 =
13-38%).
Chlorine. Personal exposures to chlorine were related to
indoor concentrations, with an R2 of 33-61% (Table 5-54). Indoor
concentrations of chlorine were related to household smoking for
both size fractions and both time periods.
Titanium. Personal exposures to titanium at night (Table 5-
55) were fairly well explained by indoor and outdoor
concentrations (R2 = 47%) , but were not explained well by outdoor
concentrations during the day (R2 = 9%). Vacuuming was selected
as one of two variables contributing to daytime indoor fine
particle concentrations of Ti (R2 = 40%) .
5-149
-------
TABLE 5r52. STEPWISE REGRESSION: BROMINE
PEM10
SIM10 SIM25 SAM10
SAM25
Overnight
N 120
R2 0.40
INTERCEPT -0.96
SIM10 1.35
SAM10
SAM25
NICJ
AER.AVG
COOK
HOUSE
SMOKE
HOMEAGE
MAR.AMBT
MARJDWPT
MSPD INV
125 126 134
0.43 0.42 0.30
3.91 3.24 24.96
0.54
0.54
0.67 0.69
-0.36
0.23
0.17
134
0.28
25.94
2.3
-0.39
0.16
0.13
Daytime
N 118
R2 0.32
INTERCEPT 5.04
SIM10 3.59
SAM10 -2.16
SAM25
NICJ
AER_AVG
COOK
. DUST
HOUSE
SMOKE
VACUM
HVJNV
HOMEAGE
MAR_AMBT
MAR.DWPT
MSPDJNV
133 127 139
0.42 0.36 0.22
1.71 1-50 4.41
0.94
0.65
0.29 0.32
445.24
0.19
134
0.16
4.59
0.15
5-150
-------
TABLE 5-53. STEPWISE REGRESSION: SILICON
DEPENDENT VARIABLES
PEM10 SIM10
SIM25 SAM10
SAM25
Overnight
N
R2
INTERCEPT
SIM10
SAM10
SAM25
NICJ
AER_AVG
COOK
HOUSE
SMOKE
HOMEAGE
MARJ3WPT
, 120 125
0.36 0.10
205.66 1907.24
0.77
0.31 0.26
126 134
0.15 0.13
244.28 7529.00
0.35
-60.89
134
0.38
777.22
f
-9.58
Daytime
N
R2
INTERCEPT
SIM10
SAM10
SAM25
NICJ
AER_AVG
COOK
DUST
HOUSE
SMOKE
VACUM
HOMEAGE
MAR_AMBT
MARJDWPT
MSPDJNV
118 133
0.15 0.49
5331.00 8783.76
0.97
0.46
1260.14
16.02
-106.84
127 139
0.32 0.30
547.79 21523.00
0.42
15.12
-6.26 -225.58
-21081.28
134
0.29
1502.95
77.39
-15.67
-1377.16
5-151
-------
TABLE 5-54. STEPWISE REGRESSION: CHLORINE
DEPENDENT VARIABLES
PEM10
SIM10
SIM25
SAM 10 SAM25
Overnight
N 120
R2 0.61
INTERCEPT 202.01
S1M10 0.92
SAM10
SAM25
NICJ
AER_AVG
COOK
HOUSE
SMOKE
HOMEAGE
MAR_DWPT
MSPDJNV
N 118
R2 0.33
INTERCEPT 766.98
SIM10 0.72
SAM10
SAM25
NICJ
AER_AVG
COOK
DUST
HOUSE
SMOKE
VACUM
HVOLUME
HOMEAGE
MAR_DWPT -7.57
MAR_AMBT
125
0.24
481.06
0.09
40,72
-6.19
133
0.27
438.12
0.70
16.05
^5.33
126
0.24
171.41
2.14
29.01
-2.22
Daytime
127
0.38
32.36
0.95
12.57
134 134
0.03 0.09
451,23
103.93
4.13 3.04
139 134
0.16 0.11
725.52 250,14
1,99
-2.24
5.81
5.65 2.42
-9.66 -3.45
5-152
-------
TABLE 5-55. STEPWISE REGRESSION: TITANIUM
DEPENDENT VARIABLES
PEM10
SIM10 SIM25
SAM10
SAM25
Overnight
N 120
R2 0.47
INTERCEPT 17.16
SIM10 0.70
SAM 10 0.28
SAM25
AER_AVG
COOK
HOUSE
SMOKE
HOMEAGE
MAR_AMBT
MAR_DWPT
MSPDJNV 0.63
124 162
0.11 0.71
63.09 8.48
"
0.29
-0.39
134
0.17
358.04
13.61
-3.19
-1.06
0.00
Daytime
N 118
R2 0.09
INTERCEPT 219.03
SIM10 0.83
SAM10
SAM25
AER_AVG
COOK
DUST
HOUSE
SMOKE
VACUM
HOMEAGE
MAR_AMBT
MAR_DWPT
MSPDJNV
133 127
0.34 0.40
46.52 20.93
0.42
0.65
32.83
0.45
0.38
139
0.27
552.61
-5.51
-532.51
134
0.22
-1.07
-25.33
5-153
-------
INDOOR SOURCE MODEL
Ultimately, we would like to identify important sources of
particles and elements and estimate the relative contribution of
each to personal exposure. To do so, we must determine the
emission rates associated with each source. We utilize a model
developed in Koutrakis et al. (1990) to calculate fine particle
and elemental emission rates for several indoor sources. In this
model, derived from a basic mass balance model, the indoor
concentration of particles or elements is given by
where
+ QJV
a + k
[1]
Cta = indoor concentration (ng/m3 for elements,
particles)
P = penetration coefficient
a = air exchange rate (IT1)
C^ = outdoor concentration (ng/m3 or jug/m3)
Qti - mass flux generated by indoor sources (ng/h or
V = volume of room or house (m3)
k - decay rate due to diffusion or sedimentation (IT1)
From the initial multivariate analyses (ANOVA and regression
analysis) described above, the most important indoor sources
5-154
-------
appeared to be smoking and cooking. Therefore the indoor source
term Qto was replaced by the following expression:
where
t
Nd
3.,
T.
coat
'cock
tether
= duration of the monitoring period (h)
= number of cigarettes smoked during monitoring period
= mass of elements or particles generated per cigarette
smoked (ng/cig or ng/cig)
— time spent cooking (h) during monitoring period
= mass of elements or particles generated per hour
of cooking (ng/h or Mg/h)
= mass flux of elements or particles from all other
indoor sources (ng/h or
With these changes, the equation for the indoor
concentration due to these indoor sources becomes
PaC
a + k
(a + k)Vt
(a + k)V
[2J
The indoor and outdoor concentrations, number of cigarettes
smoked, monitoring duration, time spent cooking, house volumes,
and air exchange rates were all measured or recorded. The
penetration factor, decay rates, and source strengths for
5-155
-------
smoking, cooking, and all other indoor sources (Q^) were
estimated using a nonlinear model (NLIN in SAS software). The
Gauss-Newton approximation technique was chosen to regress the
residuals onto the partial derivatives of the model with respect
to the unknown parameters until the estimates converge. On the
first run, the penetration coefficients were allowed to "float"
(no requirement was made that they be < 1). Since nearly all
coefficients came out close to one, a second run was made
bounding them from above by 1.
Results are presented in Table 5-56 for the combined day and
night samples. Penetration factors are very close to 1 for
nearly all particles and elements. The calculated decay rate for
fine particles is 0.39 + 0.16 h"1, and for PM10 is 0.65 + 0.28 h"1.
Each cigarette emits 22 + 8 mg of PM10 on average, about two-
thirds of which (14+4 mg) is in the fine fraction. Cooking
emits 4.1 + 1.6 mg/h of inhalable particles, of which about 40%
(1.7 +0.6 mg/h) is in the fine fraction. All elements emitted
by cooking were limited almost completely to the coarse fraction.
Sources other than cooking and smoking emit about 5.6 mg/h of
PMio, of which only about 1.1 mg/h (20%) is in the fine fraction.
Decay rates for elements associated with the fine, fraction
were generally lower than for elements associated with the coarse
fraction, as would be expected. For example, sulfur, which has
the lowest mass median diameter of all the elements, had
calculated decay rates of 0.16 and 0.21 h"1 for the PM2.5 and PM10
5-156
-------
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fractions, respectively. The crustal elements (Ca, Al, Mn, Fe),
on the other hand, had decay rates ranging from 0.6 to 0.8 h'1.
Estimates of decay rates and source strengths are also
provided for the- daytime (Table 5-57) and overnight (Table 5-58)
samples separately.
The decay rate k may be represented as a surface-to-volume
ratio a times a deposition velocity ud (see Koutrakis et al*>
1992 for a derivation):
ou.
The surface-to-volume ratio of an unfurnished 3X3X4
meter room is 1.8. Furnishings would increase the ratio. Using
an assumed value for cr of 2 m"1, we can calculate a deposition
velocity for each element associated with the fine particle and
PM10 size fractions by simply dividing the decay rate by 2. This
provides a deposition velocity for the fine particles of about
0.19 m/h, which is similar to the 0.18 m/h observed by Sinclair
et al., 1988 but larger than the value of 0.065 m/h calculated
from the value of k of 0.13 h"1 reported by Lewis et al., 1991.
Sinclair et al (1990) calculated deposition velocities for
sulfate, potassium, and calcium ions associated with fine (PM2.5)
and coarse (PM15-PM2.5) particles in four buildings used for
telephone switching purposes. In the fine particle mode,
observed deposition velocities were 0.004-0.005 cm/s for sulfate
ions, 0.004-0.03 cm/s for potassium ions, and 0.006-0.06 cm/s for
5-158
-------
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5-160
-------
calcium ions. The PTEAM estimates were 0.002, 0.002, and 0.008
cm/s, respectively.
The deposition velocity for the PM10 size fraction is
estimated using this approach as about 0.32 m/h. For sulfur,
potassium, and calcium, the estimated deposition velocities are
0.003, 0.006, and 0.009 cm/sec, respectively. These values are
considerably smaller than the range reported in Sinclair et al.,
(1990) for the three ions associated with the coarse fraction
between PM2.5 and PM15: 0.1-1.8, 0.2-3.8, and 0.07-2.2 cm/s,
respectively. However, the PM10 size fraction includes the
slower-settling fine particles, and the coarse particles in the
Sinclair study go up to 15 ,/im in diameter and would thus be
expected to settle faster.
We can apply these results to homes with different particle
sources (e.g., smoking or cooking) to determine their relative
contributions to particle and elemental concentrations. The
average percent contributions from all sources for all homes are
provided for both particle fractions in Table 5-59. Outdoor air
provided three quarters of the fine particle concentrations and
two thirds of the inhalable particle concentrations. Outdoor air
was also the dominant source for most elements. Only copper and
chlorine had the major portion of their indoor concentrations
provided by indoor sources. Smoking and cooking provided only 4-
5% each of the PM2.S and PM10 concentrations. "Other"
(unidentified) indoor sources provided 14% of the PM2 5
concentration and 26% of the PM10 concentration. These unknown
5-161
-------
TABLE 5-59. PERCENT OF PARTICLE AND ELEMENTAL
MASS DUE TO ALL SOURCES IN ALL HOMES
Source contribution
Var
PM2.5
Al
Mn
Br
Pb
Tl
Cu
Sr
P
Si
Ca
Fe
K
S
Zn
C!
PM10
Al
Mn
Br
Pb
Ti
Cu
Sr
P
Si
Ca
Fe
K
S
Zn
Cl
Size,
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
10
10
10
10
10
10
10
10
10
10
10
10
10
10
10
10
Outdoor
76
100
77
71
37
90
95
59
50
63
92
99
41
29
66
70
97
80
98
71
45
71
78
87
96
73
87
59
26
Smoking
5
0
0
3
3
0
1
0
7
0
8
1
0
8
4
0
0
3
2
0
3
3
0
6
0
4
2
0
5
Cooking
4
0
0
0
0
0
0
0
0
0
0
0
0
5
5
3
3
2
0
3
0
2
3
6
4
2
0
0
6
Other indoor
14
0
23
25
59
10
4
41
44
32
0
0
59
58
26
27
0
15
0
26
52
23
19
0
0
21
11
41
63
5-162
-------
sources also provided a larger fraction of most of the elemental
concentrations than either smoking or cooking.
Even in homes with smoking (N = 61 samples), the outdoor
contribution remained paramount (Table 5-60). However, about 30%
of fine particles in these samples was due to smoking, and about
24% of PM10. About 39-48% of the calcium, potassium, and
chlorine in the fine particles was attributed to smoking.
Smaller amounts of bromine and copper (19-21%) were associated
with smoking in this fine particle fraction. Similar amounts
(19-39%) of the same elements were provided in the PM10 fraction.
Lead, strontium, and sulfur in the PM10 fraction also appeared to
be associated with smoking.
Samples from homes with cooking (N = 62) showed increased
levels of a number of elements in the PM10 fraction, but only
chlorine was associated with cooking in the PM2-5 fraction (Table
5-61). Cooking provided about 25-26% of the total mass of both
PM2.5 and PM10. The main elements associated with cooking (30-34%
of the PM10 fraction) were calcium and chlorine. Lesser amounts
(10-20%) of aluminum, manganese, bromine, titanium, strontium,
silicon, iron, and potassium were noted in the PM10 fraction.
Samples from homes with no smoking or cooking (N = 244)
showed that other indoor sources contributed about 17% of the
total observed fine particle concentration and about 30% of the
inhalable particle concentration (Table 5-62). Substantial
portions (21-68%) of many of the other elements were also
contributed by these unknown indoor sources. A major exception
5-163
-------
TABLE 5-60. PERCENT OF PARTICLE AND ELEMENTAL
MASS DUE TO ALL SOURCES IN HOMES WITH SMOKING
Source contribution
Var
PM2.5
At
Mn
Br
Pb
Ti
Cu
Sr
P
Si
Ca
Fe
K
S
Zn
Cl
PM10
Ai
Mn
Br
Pb
Ti
Cu
Sr
P
Si
Ca
Fe
K
S
Zn
Cl
Size
2.5
2.5
2.5
2.5
2.5
2,5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
10
10
10
10
10
10
10
10
10
10
10
10
10
10
10
10
Outdoor
60
1 00
80
62
32
91
93
.63
37
72
52
92
46
20
56
73
97
70
87
74
40
62
80
57
97
60
81
63
21
Smoking
30
0
0
21
19
0
4
0
39
0
48
8
0
46
24
0
0
19
13
0
19
19
0
39
0
25
11
0
32
Cooking
3
0
0
0
0
0
0
0
0
0
0
0
0
3
3
3
3
1
0
3
0
2
3
4
3
2
0
0
4
Other indoor
7
0
20
17
49
9
3
37
24
28
0
0
54
30
16
25
0
9
0
23
42
17
17
0
0
14
8
37
42
5-164
-------
TABLE 5-61. PERCENT OF PARTICLE AND ELEMENTAL
MASS DUE TO ALL SOURCES IN HOMES WITH COOKING
Source contribution
Var
PM2.5
Al
Mn
Br
Pb
Ti
Cu
Sr
P
Si
Ca
Fe
K
S
Zn
Cl
PM10
Al
Mn
Br
Pb
Ti
Cu
Sr
P
Si
Ca
Fe
K
S
Zn
Cl
Size
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
10
10
10
10
10
10
10
10
10
10
10
10
10
10
10
10
Outdoor
62
100
82
75
42
92
96
66
56
73
92
98
45
24
56
65
82
76
98
68
48
69
71
61
80
69
87
64
21
Smoking
5
0
0
4
4
0
1
0
7
0
8
2
0
8
4
0
0
3
2
0
3
3
0
5
0
4
2
0
5
Cooking
25
0
0
0
0
0
0
0
0
0
0
0
0
26
25
17
18
10
0
15
0
12
17
34
20
13
0
0
30
Other indoor
8
0
18
21
54
8
3
34
37
27
0
0
55
41
16
17
0
11
0
17
49
16
12
0
0
14
10
36
44
5-165
-------
TABLE 5-62. PERCENT OF PARTICLE AND ELEMENTAL
MASS DUE TO "OTHER" SOURCES
IN HOMES WITH NO SMOKING OR COOKING
Source contribution
Var
PM2.5
AI
Mn
Br
Pb
Ti
Cu
Sr
P
Si
Ca
Fe
K
S
Zn
Cl
PM10
AI
Mn
Br
Pb
Ti
Cu
Sr
P
Si
Ca
Fe
K
S
Zn
CI
Size
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
2.5
10
10
10
10
10
10
10
10
10
10
10
10
10
10
10
10
Outdoor
83
100
76
72
37
89
96
57
51
65
100
100
39
32
70
71
100
83
100
72
45
74
79
100
100
76
88
57
28
Smoking
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
Cooking
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
Other indoor
17
0
24
28
63
11
4
43
49
35
0
0
61
68
30
29
0
17
0
28
55
26
21
0
0
24
12
43
72
5-166
-------
was sulfur, which was entirely due to outdoor sources in the fine
fraction, and about 88% due to outdoor sources in the inhalable
fraction. Phosphorus was also mostly (96%) due to outdoor
sources in the fine fraction, and could not be characterized in
the inhalable fraction. Chlorine (68% of the total associated
with the fine particle fraction, 72% of the total associated with
the inhalable fraction), copper (63% in PM2.S, 55% in PM10), and
zinc (61% and 43%) were mostly due to these unknown indoor
sources.
In order to compare these results to those obtained by
Koutrakis et al. (1992), we have, also calculated the source
strengths using the method outlined in that publication. In this
method, indoor concentrations of PM2.5 and associated elements
measured in New York State homes in which no combustion source
was present were regressed on outdoor concentrations to obtain
the coefficient of the outdoor concentration in equation [1]
above. The regression was successful in obtaining this
coefficient for eight elements. Since this coefficient includes
two unknowns (P and k), Koutrakis et al. assumed a value for k of
0.36. (Actually, the authors assumed a value for the deposition
velocity ud of 0.18 m/h and a surface-to-volume ratio a of 2 m"1,
which leads to a value for k of 0.36 h"1.) The resulting values
of P were then employed in equation [2] for those homes with only
one type of combustion source to determine the strength for that
source.
5-167
-------
Note that the fundamental difference in the Koutrakis method
from the PTEAM method is that an arbitrary value of k was assumed
in order to determine a value of P; these values were then
inserted into the equivalent of equation [2], which was solved
sequentially for each type of combustion source (smoking, wood
stove, etc.) to obtain the individual source strength. In the
method employed in PTEAM, the values of k, P, and all source
strengths are solved for simultaneously using a nonlinear
approach.
The Koutrakis method was applied to the PTEAM data to
determine the fine particle and elemental source strengths from
smoking, cooking, and "other" indoor sources. The estimated
emission rates for smoking, cooking, and "other" are displayed in
Table 5-63. Smoking emits fine particles at the rate of about 11
mg/cigarette. (This estimate using the Koutrakis method agrees
fairly well with the estimate of 13.9 mg/cigarette using the
PTEAM method.) Calcium, potassium, and chlorine are emitted at
rates of about 250, 130, and 63 pig/cigarette, respectively.
Cooking emits fine particles at the rate of about 110 mg/h.
Calcium, iron, chlorine, and copper are emitted at rates of about
870, 630, 318, and 36 jug/h, respectively.
A comparison of estimated smoking emission rates from the
PTEAM data (using both the PTEAM and Koutrakis models) with the
New York State data using the Koutrakis model is provided in
Table 5-64. Good agreement is seen for fine particle mass for
all three cases (11.4 mg/cig for the Riverside data using the
5-168
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Koutrakis model, 13.8 mg/cig for the Riverside data using the
PTEAM model, and 12.7 mg/cig for the New York State data using
the Koutrakis model). Bromine and potassium also show fair
agreement in all three cases. Sulfur and chlorine emission rates
agree well for the Koutrakis model in both sets of data, but are
in disagreement with the PTEAM model. On the other hand, the
PTEAM model agrees with the Koutrakis model (as applied to the
New York State data) in attributing no silicon to cigarette
smoke, but the Koutrakis model applied to Riverside data suggests
silicon as an element emitted by cigarettes.
Another way to compare the two models is to examine the
coefficients determined for the contribution of the outdoor air.
Four of the eight elements whose coefficient was determined by
Koutrakis et al., 1992 were included in the PTEAM study. Three
of the four coefficients agreed quite well (Mn: 0.52 in
Koutrakis, 0.50 in this study; Pb: 0.52, 0.57; and Ca: 0.59,
0.52). Only the coefficient determined for bromine disagreed
(0.35, 0.56). Also, the average of the eight coefficients in
Koutrakis was 0.49; the average for the 15 elements in this study
was 0.56.
"PERSONAL CLOUD" CALCULATIONS
A large daytime difference between personal and indoor
concentrations of inhalable particles was noted. One possible
reason for this difference could be that people who were away
5-170
-------
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5-171
-------
from their homes (in their cars or at work) were exposed to
higher concentrations of particles. However, such persons were
actually exposed to significantly smaller particle concentrations
than those who stayed at home. Moreover, many persons who stayed
at home the entire day had higher exposures than the fixed indoor
sampler recorded. For these persons at least, and possibly for
most of the participants, these findings can be interpreted as
evidence of a "personal cloud" of particles—a local increase in
particles due to unknown sources. Several hypotheses have been
raised to explain the personal cloud:
1) The apparent increase is an artifact due to differences
in operation of the personal monitor and the fixed
monitor.
2) The increase is due to skin scales, hairs, fibers from
clothes, or other contamination from the person wearing
the monitor.
3) The increase is due to a cloud of particles, either
raised by personal activities, or somehow attracted to
the person or the monitor by static electricity or
other forces.
The first possibility has been studied in the laboratory.
The only difference between the personal PEM and fixed indoor and
5-172
-------
outdoor monitors (SIM/SAM) was the pump and type of current
employed. The personal monitor had a battery-operated Casella
pump whereas the indoor monitor used line current through Medo
pumps. Side-by-side comparison of the pumps detected no
difference in operation. The possibility remains.that the
physical motion (jiggling, changes in orientation) of the
personal monitors caused different inlet collection
characteristics.
The second possibility was investigated by exploring three
filter triplets (personal, indoor, outdoor) by scanning electron
microscopy (SEM). Although skin scales were seen in abundance in
the personal and indoor samples in one triplet, and were also
found in lesser amounts in the remaining two triplets, the
contribution of the skin scales to total mass was estimated to be
relatively low (Mamane, 1992). Also, if these carbon-based
materials were supplying significant mass to the personal
samples, the abundance of the remaining elements should be
lowered relative to the indoor samples; however, the XRF analyses
of hundreds of filters showed that 14 of 15 elements were
elevated in personal samples in about the same (or greater—50%
or more) ratio as the total particle mass (Figure 5-78).
Microphotographs of an additional 140 personal filters
showed an average of about 4 skin flakes visible at the 500x
magnification, equivalent to roughly 120,000 skin flakes on a
typical PEM filter (Figures 5-79 and 5-80). The number of skin
flakes visible on the 500x microphotographs was correlated
5-173
-------
1
CO
M
-------
Figure 5--79. Photomicrograph showing the particle loading
on the PEM-10 filter, Participant 131A. Sample is highly
enriched with skin particles of organic composition.
5-175
-------
Figure 5-80. Close-up micrograph of the unique particles
found in personal and indoor samples.
5-176
-------
significantly with total particle mass on the filter. A
regression of PM10 mass on number of skin flakes per photo
resulted in each flake visible in the 500x photo accounting for
an increase in mass of about 10 Mg/m3 (Figure 5-81) . (That is,
30,000 flakes account for about 30,000 ng/filter; one flake would
thus weigh 1 ng.) Thus, this analysis suggests that skin flakes
could account for most of the observed mass (about 40 /ug/m3) of
the personal cloud.
However, another method of analysis suggests that an
individual skin flake is unlikely to weigh more than 0.1 ng, and
that skin flakes would thus account for no more than 10% of the
personal cloud mass. This analysis rests on the observed area of
about 300 /zm2 for the skin flakes. The thickness is difficult to
determine from the photographs, since the flakes normally come to
rest showing only the two larger dimensions. Based on
measurements of a few curled-up .flakes that display the
thickness, the thickness is estimated to be about 0.2 jum.
Assuming a maximum density of 1 (if dried up, the flake would
have a density less than 1) results in a mass estimate of only
0.06 ng/flake, a factor of 16 below the amount estimated from the
linear regression.
At present, the discrepancy between these two results
remains unexplained.
The third possibility—that the personal cloud is due to
personal activities — has been investigated by the statistical
work described above, with the finding that indoor
5-177
-------
en
§
2
1
o
u
a.
c.
a
o
at
ai
a.
Personal PM-10 levels vs. skin flakes
PERS = 9.5*FLAKES + 105
500 -
400 —
300 -
200
100
I i i t i I i i i i I ' '' ' I
! :
» 34% N = 138
L.I ' ' ' ' ' ' '—111''
0
is
20
25
No. of skin flakes at 500X magnification
Figure 5-81. Regression of personal PM10 exposure vs. number of skin flakes
counted on 138 personal filters. Rz - 34%.
5-178
-------
concentrations, and possibly a portion of the increased personal
concentrations, are affected by smokers in the home and by
cooking, with a possibility that dusting and vacuuming contribute
in lesser amounts. However, even larger (relative) personal
clouds are noted in persons who did not engage in any of the
above activities, suggesting other unknown sources of the
personal cloud. These could include simple activities not
analyzed in the questionnaire, such as walking on carpet or
sitting on upholstered furniture. Alternatively, an
electrostatic attraction could possibly be occurring.
As a further attempt to characterize the personal cloud, we
investigated its partitioning into two size fractions. The
personal cloud is defined as the difference between the personal
exposure and the time-weighted indoor and outdoor concentrations:
Pers Cloud = PEM - Jfta SIM10 - £M SAM:
10
where
and
fft = fraction of monitoring period indoors
£„., = fraction of monitoring period outdoors
Since the exposure during the time spent away from home will
not necessarily be well characterized by the home-based SIM and
SAM monitors, this relationship was investigated first using all
5-179
-------
possible subjects, and then (for particle mass only) using only
those who were at or near home a large fraction of the time.
The results using all subjects are provided in Table 5-65.
Since a small fraction of participants had negative values for
the personal cloud, the regressions were also run on those with
positive values only. Most elements appeared to make a positive
contribution to the personal cloud, with crustal elements (Al,
Si, Ca, Fe) making the largest and most significant
contributions. At night, fine particles contributed more than
coarse to the personal cloud; during the day, the reverse was
suggested .
Another approach was to compare the personal cloud with the
various microenvironments and the time spent in each as reported
by the subjects in their activity diaries. In this model,
Pers Cloud = PEM -
SIM10 -
SAM
10,
as above, but the fractions of time indoors and outdoors are
split into the five microenvironments reported by the subjects:
where
-fh = durl + dur2
£<* = dur3 + dur4 + dur5
durl = percent time indoors at home
dur2 = percent time indoors away from home
<,i
dur3 = percent time outdoors near home
5-180
-------
TABLE 5-65. REGRESSION OF PERSONAL CLOUD
ON FINE AND COARSE FRACTIONS
Nighttime
all obs. positive
only
Particle
Al
Mn
Br
Pb
Ti
Cu
Sr
intercept
a (SIM2.5)
j5 (SIM10-SIM2.5)
intercept
a (SIM2.5)
0 (SIM10-SIM2.5)
intercept
a(SIM2.5)
/? (SIM10-SIM2.5)
intercept
a (SIM2.5)
0 (SIM10-SIM2.5)
intercept
a(SIM2.5)
& (SIM10-SIM2.5)
intercept
a (SIM2.5)
j8 (SIM10-SIM2.5)
intercept
a (SIM2.5)
0 (SIM10-SEM2.5)
intercept
a (SIM2.5)
/3 (SIM10-SIM2.5)
23.54 **
-0.04
-0.30 *
11.07 *
0,96
-0.24 *
6.82 *
-0.13
-0.26
0.30
0.03
1.18 **
3.68 **
-0.04
-0.70 **
47.87
-0.25
-0.18 *
11.96 **
-0.37
-0.64 **
1.16
0.16
-0.34 **
15.93 **
0.15
0.07
404.10
-0.08
0.36
3.05
0.36
0.24
-0.60
0.33
2.39 **
0.82
0.26 *
-0.09
41.40
-0.05
0.15
14.23
-0.19
-0.20
-3.11
0.90
0.20
Daytime
all obs. positive
only
68.09 **
-0.36 *
-0.02
3443.25 **
-2.52
-0.10
14.83
1.88 *?
-0.56 *
-1.30
0.73
2.48 **
22.97 *
-0.47
-0.04
376.77 **
-3.14 *
0.08
28.86 **
-0.25
-0.55 **
19.81 **
-1.36 *
-0.08
48.93 **
0.11
0.19
6332.85 *
-7.62
0.28
5.74
3.38 **
-0.35
-10.12
1.91 **
3.34 **
21.24
-0.08
0.19
620.80 **
-6.53 *
0.29
23.20 **
0.29
0.25
20.79 **
-1.35
0.45 •*'
1. all: all observations are included
2. positive: all observations of positive mass of personal cloud are included.
3. mass of personal cloud=pemlO-homep*simlO/100-outp*samlO/100
4. homep:fraction of time inside home, outp:fraction time outside home (homep+outp=100).
(cont.)
5-181
-------
TABLE 5-65. REGRESSION OF PERSONAL CLOUD
ON FINE AND COARSE FRACTIONS
Nighttime
all obs. , positive
only
P
Si
Ca
Fo
K
S
Zn
Cl
intercept
a (SIM2.5)
P (SEM10-SIM2.5)
intercept
a (SIM2.5)
0 (SIM10-SIM2.5)
intercept
a (SIM2.5)
& (SIM10-SIM2.5)
intercept
a (SIM2.5)
j8 (SIM10-SIM2.5)
intercept
a (SIM2.5)
/3 (SIM10-SIM2.5)
intercept
a (SIM2.5)
/5 (SIM10-SIM2.5)
intercept
a (SIM2.5)
0 (SIM10-SIM2.5)
intercept
a (SIM2.5)
/3 (SM10-SIM2.5)
-19.34
0.61
-0.55 **
1408.25 **
-0.60
-0.11
406.05 **
2.96 **
-0.56 **
389.19 **
-0.46
-0.17
221.72 **
0.08
-0.20
75.32
-0.11 **
0.36
30.63 **
-0.25 *
-0.46 **
149.25 **
-0.19
-0.07
-49.28
0.86
0.36
244.13
4.07
0.08
373.08 *
3.60 **
-0.42
237.61
0.10
0.28
52.23
0.55 *
0.34
137.66 *
0.03
0.10
14.85 *
0.36 *
0.07
104.55 **
0.34
0.28 *
Daytime
all obs. positive
only
85.87
-0.05
0.03
5533.04 **
-3.89
0.31
2776.94 **
-1.49
-0.28
1662.55 **
-0.39
-0.13
926.65 **
-1.01
0.08
489.73 **
-0.19 **
-0.23
76.96 **
-0.32
0.08
428.05 **
-0.90 **
0.23
-0.98
0.77
0.24
6537.46 **
4.01
0.49
1874.30 **
1.45
-0.10
1586.23 **
2.39
-0.33
880.18 **
-0.89
0.34
314.67 '.**
0.00
0.21
54.62 **
0.07
0.49
416.66 **
-0.47
0.40 *
1. all: all observations are included
2. positive: all observations of positive mass of personal cloud are included.
3. mass of personal cloud==pemlO-homep*simlO/100-outp*samlO/100
4. homep:fraction of time inside home, outp:fraction time outside home (homep+outp=100).
5-182
-------
dur4 = percent time outdoors away from home
dur5 = percent time in transit
The regressions (Tables 5-66 and 5-67) resulted in very
little evidence that the time-weighted concentrations in
microenvironments 2 (which includes work) and 5 (which includes
commuting) had any appreciable effect on the mass of the personal
cloud or on any of the elemental compositions.
On the other hand, microenvironment 4 (outdoors away from
home) had a positive effect on PM10 mass and most associated
elements, suggesting that outdoor activities either occur in
elevated microenvironmental concentrations or can increase the
personal cloud effect. However, the amount of time spent
outdoors away from home is so small (less than 10% of the daytime
monitoring period for more than 75% of the respondents) that the
total contribution of this microenvironment to the personal cloud
is small.
A possible source of airborne particles is pets; however,
Tables 5-68 and 5-69 show no increase in indoor fine or inhalable
particles in homes with pets.
5-183
-------
TABLE 5-66. REGRESSION ON PERSONAL CLOUD
OF TIME IN M1CROENVIRQNMENTS: DAYTIME
Variable
PM10
Al
Mn
Br
Pb
Ti
Cu
Sr
P
Si
Ca
Fe
K
S
Zn
Cl
R2
0.06
0.07
0.10
0.11
0.04
0.10
0.07
0.06
0.07
0.09
0.09
0.08
0.14
intercept
41
1190
14
2
7
71
15
6
3292
575
842
527
48
dur2 dur4 dur5
110
8724
123
134
63
228 593
62
24
17792
2549 4453
6373
2598
244
Personal cloud=PEM-T_in*SIM+T_out*SAM (T_in+T_out - 100%)
durl: % indoor time at home
dur2: % indoor time away from home
dur3: % outdoor time near home
dur4: % outdoor time away from home
dur5: % time in transit
5-184
-------
TABLE 5-67. REGRESSION ON PERSONAL CLOUD
OF TIME IN MICROENVIRONMENTS: OVERNIGHT
Variable R2 intercept dur2 dur4 dur5
PM10
AI
Mn
Br
Pb
Ti
Cu
Sr
P
Si
Ca
Fe
K
S
Zn
Cl
0.06
12
49
0.04
15
764
0.04
0.09
20
120
-503
-1241
Personal cIoud=PEM-T_in*SIM+T_out*SAM (T_in+T_out = 100%)
durl:% indoor time at home
dur2: % indoor time away from home
dur3: % outdoor time near home
dur4: % outdoor time away from home
dur5: % time in transit
5-185
-------
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STATISTICAL ANALYSIS: PAHS AND PHTHALATES
Polyaromatic hydrocarbons (PAHs) and phthalates were
collected from 120 homes and 60 outdoor locations in Riverside,
CA. The analysis included
1) Exploratory data analysis and summary statistics of
unweighted data on PAHs and phthalates, including analysis
of variance by home categories (homes with smoking, cooking,
household cleaning activities, use of aerosol sprays, and
proximity to highways).
2) Correlation analysis, including factor analysis of PAHs and
phthalates and comparisons with particles and elements.
3) Regression analyses of PAHs and phthalates on independent
variables, including household cleaning, cooking or smoking
activities.
4) Application of factor analysis (PCA with varimax rotation)
methods to identify sources of particles, elements, PAHs and
phthalates.
5) Determination of indoor penetration factors, decay rates,
*
and source profiles for PAHs and phthalates, using a revised
version of the physical modeling approach published by
Koutrakis et_al., 1992.
6-1
-------
FREQUENCIES OF DETECTION
Table 6-1 and Figures 6-1 and 6-2 present the detection
frequencies of 13 PAHs and five phthalates. Four of the five
phthalates had very high frequencies of detection indoors (95-
100%) and lower frequencies outdoors (12-58%). Di-n-octyl
phthalate had the lowest detection frequency (< 40% indoors, < 3%
outdoors) among the phthalates. Most of the PAHs had fairly high
detection frequencies of 70-100%. Benzo(k)fluoranthene had the
lowest detection frequency (< 40%) among the PAHs. These two
compounds were thus excluded from further analyses because of too
few detected values.
The convention was adopted of assigning half the median
method quantifiable limit (MQL) to observations that were
reported at less than the analytical detection limits. These
median MQLs ranged from 1-3 ng/sample (0.08 to 0.24 ng/m3) for 10
of the PAHs, and slightly higher levels of 12, 13, and 33
ng/sample (1, 1, and 2.8 ng/m3) for acenaphthylene, fluoranthene,
and phenanthrene, respectively (Table 7-12, Volume II). The
median MQLs for the phthalates ranged from 38 to 290 ng/sample (3
to 24 ng/m3) for four phthalates, and 950 ng/sample (80 ng/m3)
for diethyl phthalate.
6-2
-------
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6-5
-------
SUMMARY STATISTICS
Univariate statistics (Table 6-2) and box plots (Figures 6-3
to 6-20) are presented for indoor and outdoor PAH and phthalates.
Histograms of phthalates and PAHs showed that all these compounds
were highly skewed to the right. (This is illustrated for 11 of
the PAHs in Figures 6-21 to 6-31.) This was the basis for the
logarithmic transformations employed later in some of the
statistical analyses.
These observations are summarized by compound.
Acenaphthvlene
This volatile 3-ringed PAH was measured in 70-80% of the
samples and had the highest maximum value observed for any of the
PAHs: 2900 ng/m3. There were five extremely high concentrations
measured indoors. Due to these few high values, the day and
night mean concentrations were several times higher than the
outdoor means; however, for most (95%) of the distribution,
little day-night or indoor-outdoor difference could be observed.
Overnight, indoor and outdoor concentrations were higher than the
daytime values.
Phenanthrene
This volatile 3-ringed PAH was measured in 99-100% of the
indoor samples and 90-95% of the outdoor samples. Phenanthrene
had the highest mean concentrations of all the PAHs, and was the
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6-6
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ng/m
50-
Acenaphthylene
40-
80-
20-
10-
Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME
DAYTIME
50-
Phenanthrene
40-
so-
20-
10-
Outdoor
Indoor
Outdoor
Indoor
6-3. Boxplot: acenapthylene.
Figure 6—4. Boxplot: phenanthrene.
6-10
-------
3.0
Anthracene
2JS
2.0
LO
0.5
0.0-
Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME
DAYTIME
Fluoranthene
4-
3
2-
1
Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME DAYTIME
Figure 6—5. Boxplot: anthracene.
Figure 6—6. Boxplot: fluoranthene.
6-11
-------
Fyrene
6-
B-
S-
2-
1.0-
0.9-
OS-
0.7-
0.6-
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0.4-
0^-
02-
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Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME
DAYTIME
Benzo(a)anthracene
Outdoor
•Indoor
Outdoor
NIGHTTIMB " , DATTIME
Figure 6-7.. Boxplot: pyrene.
Figure 6-8. Boxplot: benzo(a)anthracene.
6-12
-------
1.4
L2
LO
O.S
0.6-
0.4-
0.2-
0.0-
Chrysene
3.0
Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME
DAYTIME
Benzo(k)£luoranthene
ZJ5
2.0
us-
0.0-
Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME DAYTIME
Figure 6-9. Boxplot: chrysene.
Figure 6-10. Boxplot: benzo(k)fluoranthene.
6-13
-------
12-
10-
0.6-
0.4-
02-
0.0-
Benzo(e)pyrene
2.0-
L8-
1.6-
14-
12-
10-
OJ&-
0.6-
0.4-
0^-
0.0-
Outdoor
Outdoor
Itidoor
NIGHTTIME
DAYTIME
Benzo(a)pyrene
^Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME^ ,, , . . , DAYTIME
Figure 6-11. Boxplot: benzo(e)pyrene.
Figure 6—12. Boxplot: benzo(a)pyrene.
6-14
-------
3.0
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ZJ5
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Indoor
Outdoor
Indoor
NIGHT-TIME
DAYTIME
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0.0 -
Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME DAYTIME
Figure 6-13. Boxplot: indeno[1.2.3-cd]pyrene.
Figure 6-14. . Boxplot: benzo(ghi)perylene.
6-15
-------
6-
3-
Coronene
Outdoor
Indoor
Outdoor
Indoor
NIGJbiTi'JLME
DAYTIME
Diethyl phthalate
1400-
1200-
1000-
800-
600-
400-
200-
0
Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME DAYTIME
Figure 6-15. Boxplot: coronene.
Figure 6-16. Boxplot: diethyl phthalate.
6-16
-------
Di—n—butyl phthalate
2000
1800
1600
1400
1200
1000
80O
600
400
200
0
Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME
DAYTIME
Benzyl butyl phttialate
220
200
180
160
140
320
100 H
80
60-
40-
20-
0
Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME DAYTIME
Figure 6—17. Boxplot: di—n—butyl phthalate.
Figure 6-18. Boxplot: benzyl butyl phthalate.
6-17
-------
25-
Di—2 — ethylhexyl phthalate
sso-
soo-
250-
200-
3BO-
100-
50-
Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME
DAYTIME
Di—ai—octyl phthalate
30-
20-
IB-
ID-
Outdoor
Indoor
Outdoor
Indoor
NIGHTTIME
DAYTIME
Figure 6-19. Boxplot: di-2-ethylhexyl phthalate.
Figure 6-20. Boxplot:.di-n-octyl phthalate.
-------
6-19
-------
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6-27
-------
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6-29
-------
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Benzofa)anthracene and chrysene
The last two of the 4-ringed PAHs were less commonly found
than the first two, and were at concentrations about an order of
magnitude less.
Other PAHs
Indoor and outdoor concentrations of the less volatile 5- to
7-ringed PAHs (benzo(k)fluoranthene, benzo(e)pyrene,
benzo(a)pyrene, indeno(l,2,3,cd)pyrene, benzo(ghi)perylene and
coronene) were quite similar. Concentrations were also quite
low, with 95th percentile values in the range of 1-4 ng/m3.
Overnight concentrations, particularly outdoors, were usually
higher than daytime levels.
Diethvl phthalate
This compound was found in 96-98% of the indoor samples, but
only 17-19% of the outdoor samples. The indoor concentrations
were 5-10 times higher than the outdoor levels. The day and
night concentrations were similar. - ,
Di-n-butyl phthalate ,
This was found in virtually all (99-100%) of the indoor
samples and about half (50-58%) of the outdoor samples. Indoor
concentrations were 20-30 times higher than the outdoor
concentrations. Differences between the daytime and the
nighttime concentrations were negligible.
6-31
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examined but no apparent or possible sources of PAHs were
identified from the completed questionnaires except for smoking,
which was reported in both of the homes. Strong indoor sources
of PAHs in these homes, though not obvious from the
questionnaires, made these homes clearly different from the rest
of the homes in terms of the PAH concentration distributions.
Therefore, these two homes were excluded in most of the
statistical analyses.
Other homes with high PAH and phthalate concentrations were
identified by the following technique. Four concentration means
were calculated: indoor night, indoor day, outdoor night and
outdoor day. For each compound the highest of these means was
selected as a reference to identify the high values for
phthalates and PAHs in these homes. Five homes had extremely
high diethyl phthalate concentrations and eight had high
concentrations of di-n-butyl phthalate both during the day and
night (Table 6-4). Although some other homes appear in this
table, the extremely high PAH concentrations were clustered
mainly in the two homes (ID numbers 116A and 167A) identified
above; therefore none of the other homes in Table 6-4 were
excluded from subsequent statistical evaluations.
The geographical distribution of the homes in this table was
checked by plotting the sampling clusters (1 through 36)
associated with each of these homes, but no distinct or close
spatial clusters were visually detected for these extremely high
values.
. 6-51
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6-53
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TABLE 6-5. PAH AND PHTHALATE CONCENTRATIONS
(ng/m3) BY COOKING STATUS
NAME
Acenaphthylene
Acenaphthylene
Acenaphthylene
Acenaphthylene
Phenanthrene
Phenanthrene
Phenanthrene
Phenanthrene
Anthracene
Anthracene
Anthracene
Anthracene
Fluoranthene
Fluoranthene
'Fluoranthene
Fluoranthene
Pyrene
Pyrene
Pyrene
Pyrene
Benzo[a]anthracene
Benzo[a]anthracene
Benzo[a]anthracene
Benzo[a]anthracene
Chrysene
Chrysene
Chrysene
Chrysene
Benzojejpyrene
Benzo[e]pyrene
Benzo[e]pyrene
Benzo[e]pyrene
Benzo[a]pyrene
Benzo[a]pyrene
Benzo{a]pyrene
Benzo[alpyrene
ROUND
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
;Day
Night
Night
Day
Day
COOK
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
N
96
11
91
20
100
11
90
22
98
11
87
22
100
11
89
22
100
11
90
22
91
10
87
20
94
10
84
21
98
10
87
21
99
11
86
22
MEAN
6.31
5.39
7.07
5.49
17.02
15.56
18.11
17.47
0.88
0.59
0.79
0.55
1.73
1.72
1.93
2.04
1.92
1.69
2.06
2.47
0.13
0.14
0.15
0.15
0.26
0.20
0.27
0.25
0.21
0.23
0.24
0.20
0.29
0.31
0.27
0.18
STD
6.94
4.57
13.84
5.06
8.41
5.09
8.63
10.62
3.02
0.38
2.55
0.32
0.96
0.57
1.09
1.19
1.55
0.57
1.17
2.92
0.13
0.06
0.14
0.12
0.31
0.10
0.30
0.20
0.20
0.17
0.25
0.18
0.35
0.25
0.34
0.16
P5
0.50
0.50
0.50
0.50
6.15
7.20
7.20
7.40
0.09
0.09
0.09
0.28
0.55
1.10
0.55
0.55
0.78
0.94
0.91
0.98
0.06
0.06
0.06
0.06
0.05
0.05
0.05
0.05
0.04
0.04
0.04
0.04
0.04
0.04
0.04
0.04
P50
3.70
4.45
3.70
3.25
16.00
16.00
16.50
15.00
0.47
0.49
0.42
0.41
1.60
1.60
1.70
1.80
1.60
1.50
1.90
1.85
0.06
0.14
0.06
0.12
0.17
0.19
0.17
0.19
0.13
0.23
0.17
0.14
0.18
0.24
0.14
0.14
P95
19.0
16.0
25.0
16.5
31.0
25.0
38.0
27.0
2.3
1.5
1.3
1.3
3.3
2.7
3.6
4.5
3.9
2.7
4.8
4.0
0.4
0.3
0.5
0.4
0.9
0.4
1.0
0.6
0.6
0.5
0.8
0.7
1.0
0.7
0.9
0.4
(cont.)
6-55
-------
-------
TABLE 6-6. HOMES USING AEROSOL SPRAYS VS NO-SPRAY
HOMES: PAH AND PHTHALATE CONCENTRATIONS (ng/m3)
NAME
Acenaphthylene
Acenaphthylene
Acenaphthylene
Acenaphthylene
Phenanthrene
Phenanthrene
Phenanthrene
Phenanthrene
Anthracene
Anthracene
Anthracene
Anthracene
Fluoranthene
Fluoranthene
Fluoranthene
Fluoranthene
Pyrene
Pyrene
Pyrene
Pyrene
Benzo[a]anthracene
Benzo[a]anthracene
Benzo[a]anthracene
Benzo[a]anthracene
Chrysene
Chrysene
Chrysene
Chrysene
Benzo[e]pyrene
Benzo[e]pyrene
Benzo[e]pyrene
Benzo[e]pyrene
Benzo[a]pyrene
Benzo[a]pyrene
Benzo[a]pyrene
Benzo[a]pyrene
ROUND
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
SPRAY
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No ,
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
N
84
23
83
28
88
23
84
28
87
22
83
26
88
23
84
27
88
23
84
28
81
20
81
26
82
22
77
28
85
23
82
26
87
23
81
27
MEAN
6.28
5.97
6.71
7.01
17.20
15.67
18.26
17.16
0.93
0.56
0.82
0.49
1.77
1.56
1.96
1.92
1.98
1.59
2.03
2.47
0.14
0.11
0.14
0.17
0.28
0.19
0.27
0.27
0.21
0.20
0.22
0.27
0.30
0.27
0.24.
0.29
STD
6.93
6.04
14.21
6.74
8.67
5.67
8.99
9.17
3.20
0.55
2.61
0.33
0.98
0.69
1.17
0.92
1.63
Or57
1.16
2.63
0.14
0.07
0.14
0.13
0.32
0.14
0.30
0.22
0.21
0.17
0.25
0.22
0.35
0.29
0.30
0.33
P5
0.50
0.50
0.50
0.50
7.20
6.40
7.20
8.60
0.09
0.20
0.09
0.09
0.55
0.55
0.55
0.55
0.78
0.76
0.93
0.91
0.06
0.06
0.06
0.06
0.05
0.05
0.05
0.05
0.04
0.04
0.04
0.04
0.04
0.04
0.04
0.04
P50
3.85
4.20
3.40
4.70
16.00
15.00
16.00
16.50
0.52
0.39
0.45
0.40
1.60
1.35
1.70
1.90
1.60
1.50
1.80
1.95
0.08
0.11
0.06
0.13
0.17
0.16
0.16
0;20
0.13
0.16
0.14
0.21
0.20
0.18
0.12
0.18
P95
18.0
16.0
17.0
21.0
31.0
25.0
38.0
32.0
1.7
1.5
1.3
1.2
3.3
2.7
4.5
2.8
4.0
2.5
4.0
5.8
0.4
0.3
0.5
0.4
0.9
0.5
1.0
0.8
0.6
0.6
0.7
0.7
0.9
0.8
0.9
0.9
6-57
(cont.)
-------
-------
TABLE 6-7. PAH AND PHTHALATE CONCENTRATIONS (ng/m3)
BY HOUSE CLEANING (VACUUMING, DUSTING...) STATUS
NAME
Acenaphthylene
Acenaphthyiene
Acenaphthylene
Acenaphthylene
Phenanthrene
Phenanthrene
Phenanthrene
Phenanthrene
Anthracene
Anthracene
Anthracene
Anthracene
Fluoranthene
Fluoranthene
Fluoranthene
Fluoranthene
Pyrene
Pyrene
Pyrene
Pyrene
Benzo[a]anthracene
Benzo[a]anthracene
Benzo[a]anthracene
Benzo[a]anthracene
Chrysene
Chrysene
Chrysene
Chrysene
Benzo[e]pyrene
Benzo[e]pyrene
Benzo(e]pyrene
Benzo[e]pyrene
Benzo[a]pyrene
Benzo[a]pyrene
Benzo[a]pyrene
Benzo[a]pyrene
ROUND
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
CLEAN
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
N
98
9
80
31
102
9
80
32
100
9
77
32
102
9
79
32
102
9
80
32
92
9
77
30
95
9
74
31
100
8
79
29
101
9
76
32
MEAN
6.13
7.15
6.72
6.93
16.88
16.90
18.63
16.37
0.87
0.66
0.83
0.52
1.73
1.66
1.96
1.93
1.92
1.67
2.23
1.91
0.13
0.14
0.14
0.16
0.25
0.36
0.25
0.30
0.21
0.20
0.23
0.25
0.29
0.33
0.25
0.26
STD
6.87
5.08
14.58
5.73
8.33
5.87
9.87
6.18
2.98
0.75
2.71
0.31
0.94
0.75
1.18
0.93
1.53
0.63
1.89
0.80
0.12
0.18
0.13
0.15
0.27
0.55
0.29
0.26
0.20
0.12
0.24
0.24
0.35
0.29
0.31
0.31
P5
0.50
0.50
0.50
0.50
6.40
7.60
7.35
6.70
0.09
0.20
0.09
0.09
0.55
0.55
0.55
0.55
0.78
0.89
0.92
0.91
0.06
0.06
0.06
0.06
0.05
0.05
0.05
0.05
0.04
0.04
0.04
0.04
0.04
0.04
0.04
0.04
P50
3.80
6.50
3.30
5.00
15.50
18.00
16.00 -
16.50
0.48
0.40
0.45
0.42
1.60
1.60
1.70
2.05
1.60
1.90
1 .90
1.85
0.11
0.06
0.10
0.06
0.16
0.19
0.16
0.19
0.13
0.21
0.14
0.20
0.20
0.27
0.13
0.16
P95
19.0
15.0
26.0
17.0
31.0
28.0
40.5
27.0
1.6
2.6
1.4
1.2
3.2
2.8
4.9
3.3
3.7
2.5
5.5
3.3
0.3
0.6
0.4
0.5
0.8
1.8
1.0
0.9
0.6
0.4
0.7
0.8
0.9
0.9
0.9
0.9
6-59
(cont.)
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TABLE 6-11. PAH AND PHTHALATE CONCENTRATIONS (ng/m3)
BY REPORTED IN-HOME SMOKING STATUS
NAME
Benzo[ghi]perylene
Benzo[ghi]perylene
Benzo[ghi]perylene
Benzo[ghi]perylene
Coronene
Coronene
Coronene
Coronene
Diethyl phthalate
Diethyl phthalate
Diethyl phthalate
Diethyl phthalate
Di-n-butyl phthalate
Di-n-butyl phthalate
Di-n-butyl phthalate
Di-n-butyl phthalate
Benzyl butyl phthalate
Benzyl butyl phthalate
Benzyl butyl phthalate
Benzyl butyl phthalate
Di2ethyl hexyl phthalate
Di2ethyl hexyl phthalate
Di2ethyl hexyl phthalate
Di2ethyl hexyl phthalate
ROUND
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
Night
Night
Day
Day
SMOKE
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
No
Yes
N
88
21
95
18
90
21
95
18
90
21
95
17
90
21
95
17
90
21
95
18
90
21
95
18
MEAN
0.9
1.3
1.0
1.6
0.8
1.3
0.9
1.6
430.5
443.6
433.0
610.9
597.4
353.0
629.3
427.6
54.0
39.3
63.4
63.7
107.5
107.1
131.6
210.6
STD
0.9
0.9
1.0
1.4
0.9
1.0
0.9
1.4
320.0
445.1
336.8
629.9
490.3
217.8
552.9
415.5
52.0
34.7
75.9
54.1
60.1
45.7
77.0
209.9
P5
0.1
0.4
0.1
0.2
0.1
0.3
0.1
0.1
120.0
120.0
40.0
140.0
150.0
66.0
160.0
110.0
6.9
6.4
2.6
6.9
39.0
43.0
49.0
75.0
P50
0.5
1.1
0.5
1.3
0.5
1.1
0.5
1.4
350.0
300.0
340.0
430.0
437.5
340.0
440.0
330.0
37.0
22.0
33.0
54.5
92.5
110.0
110.0
150.0
P95
2.7
2.6
3.7
5.3
2.5
2.8
3.1
5.0
1100.0
930.0
1300.0
2800.0 •
1800.0
730.0
2000.0
1900.0
160.0
100.0
200.0
210.0
235.0
160.0
310.0
1000.0
6-65
-------
-------
difference between the geometric mean concentrations in smoking
vs. non-smoking homes was statistically significant, usually at p
< 0.000-1.
Overnight outdoor concentrations of acenaphthylene,
benzo(e)pyrene, benzo(a)pyrene and benzo(ghi)perylene near homes
within 100 yards of a "busy road" were somewhat higher than those
near homes located further away (Table 6-13).
Since smoking was the only activity found to be strongly
associated with increased concentrations of some of the target
PAHs and phthalates, box plots of PAH and phthalate
concentrations in smoking and nonsmoking homes were prepared
(Figures 6-48,to 6-65). These figures show that not only were
the indoor PAH concentrations in homes with smoking higher than
in homes without smoking, but also the outdoor PAH concentrations
were higher near homes with smoking. (This is especially
apparent for acenaphthylene, anthracene, fluoranthene,
benzo(a)anthracene, chrysene, benzo(e)pyrene, and
benzo(a)pyrene.) Therefore, a new set of t-tests were performed
using the ratios between the indoor and outdoor concentrations to
adjust for any effects of outdoor concentrations on the indoor
levels. There were still few or no detectable effects of
cleaning, cooking, or spraying activities (Tables 6-14 to 6-16),
except that benzo(ghi)perylene had higher geometric means in
homes with cooking (p < 0.005), and several PAHs had lower
geometric means in homes reporting aerosol spray use. However,
the ratios of 6 out of 12 PAHs (acenaphthylene,
6-67
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3
2
1-
Outdoor
Indoor
Outdoor
Indoor
NONSMOKE
SMOKE
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8
7
6
5
4-
3
2
1
0-
Outdoor
Indoor
Outdoor
Indoor
NONSMOKE SMOKE
Figure 6-50. Boxplot (by smoking category): anthracene.
Figure 6-51. Boxplot (by smoking category): fluoranthene.
6-71
-------
-------
Chrysene
1.6
1.4
12
uo-
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Outdoor
Outdoor
Indoor
NONSMOKE
SMOKE
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4-
s
2
1
Outdoor
Indoor
Outdoor
NONSMOKE SMOKE
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Figure 6—55. Boxplot (by smoking category): benzo(k)fluoranthene.
6-73
-------
-------
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4-
3
2
1
Outdoor
Indoor
Outdoor
Indoor
NONSMOKE
SMOKE
Benzo(ghOperylene
4
3
2
1-
Outdoor
Indoor
Outdoor
Indoor
NONSMOKE SMOKE
Figure 6—58. Boxplot (by smoking category): indeno[1.2.3—cdjpyrene.
Figure 6-59. Boxplot (by smoking category): benzo(ghi)perylene.
6-75
-------
-------
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360
800
260
200
150-
100
50
0
16
14
32
ID-
S'
6
4
2-
0-
Outdoor
Indoor
Outdoor
Indoor
NONSMOKE
SMOKE
Di — n—octyl phthalate
Outdoor
Indoor
Outdoor
NONSMOKE^ t SMOKE
Figure 6-64. Boxplot (by smoking category): di-2-ethylhexyl phthalate.
Figure 6-65. Boxplot (by smoking category): di-n-octyl phthalate.
6-77
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2) Phenanthrene was correlated with 3- and 4-ringed PAHs
and highly correlated with anthracene, fluoranthene and
pyrene (correlation coefficients ranging from 0.46 to
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3) Fluoranthene and pyrene were highly correlated with 3-
and 4-ringed PAHs.
4) Benzo(a)anthracene and chrysene were highly correlated
with 5- to 7-ringed PAHs and also with acenaphthylene.
5) 5- to 7-ringed PAHs were highly correlated among
themselves and also with acenaphthylene.
6) Diethyl phthalate was correlated with di-n-butyl
phthalate and di-2-ethylhexyl phthalate and also
correlated with some of the 3- and 4-ringed PAHs
(phenanthrene, anthracene, fluoranthene and pyrene).
7) Di-n-butyl phthalate was correlated with diethyl
phthalate and di-2-ethylhexyl phthalate.
8) Benzyl butyl phthalate was weakly correlated with only
anthracene and di-2-ethylhexyl phthalate.
9) Di-2-ethylhexyl phthalate was correlated with other
phthalates and also with 4-ringed PAHs.
Similar correlation patterns were observed for the daytime
phthalates and PAH measurements (Table 6-20).
6-87
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During the day, again only one of the phthalates—di-2-
ethylhexyl phthalate—was correlated with PM10 mass or with PM10
elemental concentrations.
i
FACTOR ANALYSES
Factor analyses (Principal Component Analysis with Varimax
Rotation) were used to identify the common factors for
phthalates, PAHs, PM2.5 and PM10 mass and elemental concentrations.
Results for the indoor samples (Table 6-25) showed that for the
overnight period, four principal factors explaining 82% of the
total variance were identified for phthalates and PAHs. The
first factor included one 3-ringed PAH (acenaphthylene) and 4- to
7-ringed PAHs (benzo(a)anthracene, chrysene, benzo(e)pyrene,
benzo(a)pyrene, indeno(l,2,3-cd)pyrene, benzo(ghi)perylene and
coronene). The second factor included two 3-ringed PAHs
(phenanthrene and anthracene) and two 4-ringed PAHs (fluoranthene
and pyrene). Benzyl butyl phthalate formed a separate factor
(factor 4) and the other three phthalates were associated
together in factor 3. A similar pattern was also seen for the
daytime indoor samples.
For the outdoor samples, PAH and phthalate concentrations
for both time periods were combined because of sample size
limitations (Table 6-26). Three factors explained 81% of the
total variance. Volatile (3- to 4-ringed) PAHs formed one factor
6-99
-------
-------
TABLE 6-26. FACTOR LOADINGS OF OUTDOOR
PAHS AND PHTHALATES (day and night combined)
COMPOUND
Acenaphthylene
Phenanthrene
Anthracene
Fluoranthene
Pyrene
Benzo(a)anthracene
Chrysene
Benzo(e)pyrene
Benzo(a)pyrene
lndeno[1 ,2,3-cd]pyrene
Benzo(ghi)perylene
Coronene
Diethyl phthalate
Di-n-butyl phthalate
Benzyl butyl phthalate
Di-2-ethylhexyl phthalate
factor!
0.47
0.37
0.48
0.60
0.63
0.91
0.91
0.92
0.89
0.92
0.85
0.84
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-0.17
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0.78
0.63
0.66
0.25
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0.30
0.30
0.25
0.37
0,38
0.21
0.31
-0.08
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factors
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0.15
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0.01
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0.59
0.79
0.88
0.74
6-101
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TABLE 6-35. PHYSICAL MODEL FOR ESTIMATING
INDOOR PENETRATION, DECAY RATES, AND
SOURCE STRENGTHS FOR PAHS AND PHTHALATES
c,-
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decay rate (h"1)
air exchange rate (h'1)
house volume (m3)
duration (h) of monitoring period
number of cigarettes smoked during monitoring
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flux of unknown indoor sources (ng/h or
6-115
-------
-------
The estimated average decay rates for PAHs ranged from 0.4
to 1.6 h"1 with sizeable variation. No apparent dependence on
volatility was noted. The two phthalates had decay rates of 0.7
(di-n-butyl phthalate) and 1.5 (diethyl phthalate) per hour.
Estimated indoor source strengths for smoking for
benzo(a)anthracene, chrysene, benzo(e)pyrene, benzo(a)pyrene,
benzo(ghi)perylene, and coronene were 122, 192, 86, 264, 244, and
245 ng/cigarette, respectively. Smoking was not indicated as an
indoor source for phthalates.
Other (unidentified) indoor sources were found to be very
important for both of the phthalates and for the volatile PAHs,
but the estimates of source strengths were highly uncertain.
The physical models had reasonably good fit to particulate
PAHs, and coefficients between model predicted concentrations and
observed concentrations averaged about 0.7.
These results differ from the preliminary results reported
in Volume II. As explained in that volume, the modeling
attempted was only preliminary, and involved several assumptions
that are known to be unlikely on physical grounds. For example,
the decay rates k were set equal to zero, whereas we have noted
that they range from 0.4 to 1.6 h"1, making them comparable to
the average air exchange rate of about 0.8 h"1. Also the
penetration coefficient P (called f in Volume II) was set equal
to 0.5 in one set of calculations, and ranged from 0.4 to 0.6 in
another set employed in Volume II, whereas our calculations
indicate that this coefficient is very close to 1. This led to a
6-117
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-------
REFERENCES
Anderson, R., Kamens, R., and Rodes, C. A Collocation Study of
PM-10 and PM-2.5 Inertial Impactors for Indoor Aerosol Exposure
Assessment. In: Proceedings of EPA/AWMA Symposium on Measurement
of Toxic and Related Air Pollutants. Air and Waste Management
Association (VIP-13) Pittsburgh, PA, pp. 464-469, 1989.
Chromy, J. R.. Sequential Sample Selection Methods. In:
Proceedings of the American Statistical Association Section on
Survey Research Methods, 1979. pp. 401-406.
Clayton, C.A., Perritt, R.L. Pellizzari, E.D., Thomas, K.W.,
Whitmore, R.W., Ozkaynak, H., Spengler, J.D., and Wallace, Lance
A. Particle Total Exposure Assessment Methodology (PTEAM) Study:
Distributions of Aerosol and Elemental concentrations in
Personal, Indoor, and Outdoor Air Samples in a Southern
California Community. J Exposure Analysis and Environmental
Epidemiology 3:227-250, 1993.
Clayton, C.A., Pellizzari, E.D., and Wiener, R.W. Use of a Pilot
Study for Designing a Large-scale Probability Study of Personal
7-1
-------
-------
Communities in Northern and Southern California. Atmos.
Environ., 21:1995-2004, 1987.
Immerman, F. W. and Schaum, J. L. Nonoccupational Pesticide
Exposure Study: Final Report. EPA/600-3-90-003.- U.S.
Environmental Protection Agency, Washington, DC, 1990.
Jenkins, P.L., Hui, S.P., Phillips, T.J. and Lum, S.B. Toxic Air
Pollutants in California Residences. In: Edwards, L. (ed)
Current Issues in Air Toxics: Proceedings of the Third Annual
West Coast Regional Air and Waste Management Association
Conference Nov. 9-10, 1992. Air and Waste Management
Association, Pittsburgh, PA.
Kamens, R., Lee, C. T., Weiner, R., and Leith, D. A Study to
Characterize Indoor Particles in Three Non-Smoking Homes. Atmos.
Environ. 25:939-948, 1991.
Koutrakis, P., Briggs, S.L.K. and Leaderer, B.P. Source
Apportionment of Indoor Aerosols in Suffolk and Qnondaga
i
Counties, New York. Environ. Sci. Tech. 26:521-27, 1992.
Lewis, C.W. Sources of Air Pollutants Indoors: VOC and Fine
Particulate Species. J Exposure Analysis and Environmental
Epidemiology 1:31-44, 1991.
7-3
-------
-------
Pellizzari, E.D., Thomas, K.W. , Clayton, C.A., Whitmore, R.W.,
Shores, R.C., Zelon, H.S., and Perritt, R.L. Project Summary.
Particle Total Exposure Assessment Methodology (PTEAM):
Riverside, California Pilot Study. Volume I. EPA/600/SR-93/050.
US EPA, Research Triangle Park, NC, I993b.
Pellizzari, E. D., Perritt, K., Hartwell, T. D., Michael, L. C.,
Sparacino, C. M., Sheldon, L. S., Whitmore, R., Leininger, C.,
Zelon, H., Handy, R. W., and Smith D. Total Exposure Assessment
Methodology (TEAM) Study: Elizabeth and Bayonne, New Jersey,
Devils Lake, North Dakota, and Greensboro, North Carolina, Volume
II, Final Report. EPA Contract No. 68-02-3679, 1986a.
Pellizzari, E. D., Perritt, K. , Hartwell, T. D., Michael, L. C.,
Whitmore, R., Handy, R. W., Smith D., and Zelon H. Total
Exposure Assessment Methodology (TEAM) Study: Selected
Communities in Northern and Southern California, Volume III,
Final Report. EPA Contract No. 68-02-3679, I986b.
Pellizzari, E. D., Hartwell, T. D., Zelon, H., Perritt, R.,
Sebestik, J., Williams, W., Smith D. J., Keever, J., Decker, C.
E., Jayanty, R. K. M., Thomas, K., Whitaker, D. A., arid Michael,
L. C. Baltimore Total Exposure Assessment Methodology (TEAM)
Study, Final Report. EPA Contract No. 68-02-4406, 1988a.
7-5
-------
-------
Research Triangle Institute and Harvard School of Public Health.
Particle Total Exposure Assessment Methodology (PTEAM): Pilot
Study Volume III: Quality Assurance Project Plan, Workplan for
EPA Contract No. 68-02-4544, EPA Work Assignment 67 and CARB
Agreement No. A833-060. Environmental Protection Agency,
Research Triangle Park, NC, 199Ob.
Research Triangle Institute and Harvard School of Public Health.
Nine-Home Particle TEAM Study, Final Report for EPA Contract No.
68-02-4544, Work Assignment 11-66. U. S. Environmental
Protection Agency, Research Triangle Park, NC, 1990c.
Sheldon, L., Clayton, A. Keever, J., Perritt, R. and Whitaker, D.
PTEAM: Monitoring of Phthalates and PAHs in Indoor and Outdoor
Air Samples in Riverside, California. Volume II. California Air
Resources Board, Sacramento, CA, 1992.
Sheldon, L., Whitaker, D., Keever, J. , Clayton, A. and Perritt,
R. Phthalates and PAHs in Indoor and Outdoor Air in a Southern
California Community. In: Indoor Air '93: Proceedings of the 6th
International Conference on Indoor Air Quality and Climate vol.
3i pp. 109-114. Helsinki University of Technology. Espoo,
Finland, 1993.
Sinclair, J. D., Psota-Kelty, L. A., and Weschler, C. J.
Indoor/Outdoor Ratios and Indoor Surface Accumulations of Ionic
7-7
-------
-------
J. Exposure Analysis and Environmental Epidemiology., 3:203-226,
1993.
Wallace, L. A. The Total Exposure Assessment Methodology (TEAM)
Study: Summary and Analysis, Volume I. EPA/600/6-87/002a.
Office of Research and Development, U.S. Environmental Protection
Agency, Washington, DC, 1987.
Wallace, Lance A., Pellizzari, E.D., Spengler, J.D., Jenkins, P.
et al. Initial Results from the PTEAM Study: Survey Design,
Population Response Rates, Monitor Performance, and Quality
Control Results. In: Proceedings of the EPA-AWMA Symposium on
Measurement of Toxic Chemicals, Vol. 2. Air and Waste Management
Association (VIP-21), Pittsburgh, PA. pp. 659-664, 1991a.
Wallace, Lance A., Pellizzari, E.D., Spengler, J.D., Jenkins, P.
et al. The US EPA TEAM Study of Inhalable Particles (PM-10) : ..
Study Design, Response Rate, and Sampler Performance. Paper #91-
171.3 presented at the 84th Annual Meeting of the Air and Waste
Management Association, Vancouver, BC, June .199Ib. NTIS # PB91-
182873.
Wallace, L., Ozkaynak, H., Spengler, J.D., Pellizzari, E.D., and
Jenkins, P. Indoor, Outdoor, and Personal Air Exposures to
Particles, Elements, and Nicotine for 178 Residents of Riverside,
California. In: Indoor Air '93: Proceedings of the 6th
7-9
-------
-------
APPENDIX A
COMPARISON OF PM10 MONITORING METHODS
-------
-------
ABSTRACT
A comparison of three methods for measuring inhalable
particles (PM-g) was carried out as part of EPA's PTEAM Study in
Riverside, California. The instruments included two Wedding
high-volume samplers, two Sierra dichotomous samplers, and two
portable monitors developed for the PTEAM study. All instruments
were collocated at a single site and were operated over 48 days
between Sept. 22, 1990 and Nov. 9, 1990. All samples were 12-
hour samples collected between 7AM and 7PM (day) and 7PM to 7AM
(night).
In general, all instruments performed well, with few invalid
samples and very high median precisions of 3-5%. A day-night
difference was noted betwen the Wedding and the other two types
of samplers, with the Wedding decreasing by about 13% relative to
the others at night.
Since the data were rejected as being drawn from a normal
distribution, but were not rejected for log-normality,
statistical analyses were performed on the logarithms of the
concentrations. Multiple and stepwise regressions were carried
out on the differences between the logarithms of the
concentrations measured by each pair of methods. The independent
variables included temperature; wind speed; wind direction; dew
point; concentration; composition of the aerosol, as reflected by
the coarse (PM10 - PM ? 5) fraction; cleaning frequency of the
Wedding; sampling period; and a "diurnal oscillation" step
function identified from analyses of the residuals of earlier
multiple regressions. These nine variables explained 42-73%
(adjusted Rz) of the observed variance in the comparisons
involving the Wedding sampler, but only 0-14% of the variance in
the comparison of the dichotomous sampler with the portable
samplers.
The day-night difference observed earlier appeared to be
associated with the temperature; concentrations measured by the
Wedding increased relative to the other two methods by about 1%
per °F rise in temperature. Cleaning of the Wedding was followed
by an average 14% decrease in the immediately succeeding 12-hour
measurement period (relative to the dichotomous sampler), with a
"recovery" over the next few periods. The reason for the
temperature effect is presently unclear. The cleaning effect may
be due to removal of particles from the vanes of the cyclone,
followed by interception of particles from the airstream until an
equilibrium layer of soiling is attained. Both effects should be
studied further.
A-3-
-------
-------
Dichotomous samplers.
Two medium-volume (1.0 m3/h) dichotomous samplers (Sierra
Series 244E) were employed. Following impaction in the Andersen
Model 246B inlet, particles less than 10 jum in aerodynamic diameter
are separated into fine (< 2.5A«n) and coarse (between 2.5 and 10
Aim) fractions using a virtual impaction method. An accelerator
nozzle provides a cutpoint of about 9.5 /*m, according to the
manufacturers. No maintenance was undertaken on the dichots for
the length of the study.
Personal samplers.
Two low-volume (0.24 m3/n) samplers developed for this study
were collocated at the central site. The personal exposure monitor
(PEM) includes a PM10 impaction inlet (Marple et al.,), together
with a battery-operated Casella pump. The stationary ambient
monitor (SAM) employs two inlets of the same design but different
cutpoints: 2.5/z and 10/Lt. The pump is a Medo pump operated off line
current. Particles less than 10 urn (or less than 2.5 jum, in the
case of the SAM2 5) are collected on Teflon filters after removal of
larger particles using a lightly greased impaction plate. The 10-fj,
SAM and the PEM have identical circular inlets with 1.9-mm holes.
When both are employed as fixed monitors, they differ only in the
type of pump—thus they can be treated as members of a pair in the
same way as the Wedding and dichotomous samplers. The cutpoint for
the PEM, as determined in laboratory tests, is 11.0 jura (USEPA,
1990). The cutpoint for the SAM was not determined, but previous
A-5
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1) The concentrations measured by the method selected as the
independent variable are measured without error;
2) The concentrations are drawn from a normal distribution;
3) The errors are additive and normally distributed.
All three assumptions are often false. That is, all
measurement methods have errors; environmental concentrations are
seldom normal; errors are often multiplicative and seldom
distributed normally. As an example of the last point, measurement
method errors are usually described in terms of a percent of the
reported concentration (implying multiplicative errors) rather than
as an absolute amount (which would imply additive errors).
A number of different approaches may be adopted to circumvent
these problems. For example, orthogonal regression allows both
measurement methods to have errors. Transformations of the data
may achieve more normal distributions. If the errors are
multiplicative and log-normally distributed, then their logarithms
are additive and normally distributed (Wallace, 1987).
Theoretical considerations indicate that many environmental
parameters should follow log-normal distributions (Ott, 1990).. If
the measured concentrations are drawn from a log-normal
distribution, and if the major measurement errors are
multiplicative and log-normally distributed, then least-squares
regressions on the logarithms•of the concentrations would meet the
last two assumptions above. Since the difference of two normal
distributions is also normal, the regression may be run on the
A-7
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for the PEMSAM-dichot comparisons, for both the day and night
values (Fig. 1).
The concentrations measured by the three methods were tested
for normality and for log-normality using the ^-square test (Table
3) . In all three cases, the observed distribution was rejected for
normality at the p < 0.001 level, but could not be rejected for
log-normality. This indicates that regressions should not be
carried out on the untransformed concentrations; however,
regressions on the logarithms of the concentrations, or on the
differences of the logarithms of the concentrations would be
allowed. Therefore, three sets of multiple regressions were
carried out on the differences of the logarithms of the
concentrations as measured by the three pairs of samplers: Wedding
vs. dichot, Wedding vs. PEM-SAM, and dichot vs. PEM-SAM.
Independent variables
Particle samplers could conceivably be differentially affected
by the following variables:
1) wind speed
2) wind direction
3) temperature
4) dewpoint
5) concentration of the aerosol
6) composition of the aerosol
7) maintenance schedule
8) calculational errors
A-9
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noticeable effect of cleaning the Wedding; the period immediately
following the cleaning showed a decrease of about 14% (compared to
the dichot) followed by a roughly linear recovery (Table 4).
Therefore a cleaning frequency (CLEANFREQ) variable was employed,
which took on values of unity for the four 12-h periods immediately
following a cleaning and zero thereafter.
Finally, another inspection of residuals following regressions
using the above variables indicated that a diurnal effect existed,
which, however, changed sign at period 60 (Fig. 2) . It is
suspected that some form of calculational error may have occurred,
but the exact cause remains undiscovered. However, this effect can
be modeled by a variable (DIURNAL) having the value of unity during
the day and zero at night for the first 60 periods, and the reverse
values for the final 36 periods.
Thus the final set of regressions includes nine variables that
are closely related to the eight factors listed above:
1) wind speed
2) wind direction
3) temperature
4) dewpoint
5) concentration of the aerosol
6) coarse fraction of the.aerosol
7) period
8) cleaning frequency of the Wedding (CLEANFREQ)
9) the diurnal oscillatory function (DIURNAL)
A-ll
-------
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significant variables were wind speed (day) and concentration
(night). The complete results of the stepwise regressions for the
day, night, and combined day-night periods are in Appendix 2.
PEMSAM vs. Wedding.
The dependent variable in this case was log (PEMSAM) - log
(Wedding). For the combined day-night data, again five variables
were significant. Four of these were the same variables (and had
the same direction relative to the Wedding instrument) as in the
Wedding-dichot comparison: temperature, concentration, the cleaning
frequency of the Wedding, and the diurnal oscillation. The fifth
significant variable was windspeed, which increased the difference
with increasing windspeed. Together these five variables explained
42% of the observed variance in the combined day-night data set.
Separate regressions on the day and night data explained 49% and
47% of the variance (Appendix 2). Highly significant variables
were the dewpoint and temperature (day) and the cleaning frequency
of the Wedding instrument (night).
PEMSAM vs. dichot.
The dependent variable in these regressions was log (PEMSAM) -
log (dichot). For the combined day-night observations, none of the
nine independent variables affected the PEMSAM/dichot ratio
(adjusted R2 = 0) . A similar result was found for the overnight
data. For the daytime data, an effect of windspeed was noted,
explaining 14% of the variance (Appendix 2).
A-13
-------
-------
instrument, such as temperature, concentration, and composition of
the aerosol had little or no effect on the PEMSAM vs. dichot
comparison. The "diurnal oscillation" variable also appeared in
both comparisons involving the Wedding instrument but not in the
comparison of the other two methods.
Main explanatory variables.
Cleaning frequency. The effect of cleaning the Wedding is
significant. It appears likely that the readings of the Wedding
immediately after cleaning are underestimates produced by some
unintended effect of cleaning. The instrument appears to "recover"
steadily, regaining its previous relationship with the other
samplers after about four 12-hour periods. Since the cleaning
i
includes the vanes of the cyclone, which are in the direct path of
the sampled aerosol, it may be that the vanes remove enough aerosol
during the period following cleaning to affect the total mass.
Recovery would then occur as the vanes again become coated with the
aerosol to some equilibrium level.
Temperature. Temperature increases the Wedding/dichot and
Wedding/PEMSAM ratios by about 1% per °F. This effect continued to
be evident, at about the same magnitude, when the daytime data were
analyzed separately, thus confirming that the effect is due to
temperature and not to some third variable (e.g. fine-coarse ratio)
that covaries with the day-night periods. No particular
temperature dependence was noted for the PEM-SAM/dichot ratios.
These observations could indicate that the Wedding instrument reads
A-15
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night comparison of the PEMSAM and Wedding. As the wind speed
increases, the dichot reads higher with respect to the PEMSAM,
which in turn reads higher with respect to the Wedding.
Previous Comparisons of Methods
Several previous studies have compared reference methods for
PM-10. Rodes et al. (1985) compared the Sierra-Andersen Model 321A
with the General Metal Works 9000 (using a PM-10 inlet designed by
Wedding) in four cities. Disagreement was substantial, with the
Sierra-Andersen reaching as much as 36% higher concentrations in
one of the cities (Phoenix, AZ) . Rodes attributed the cause of the
bias to undercollection by the Wedding instrument due to build-up
of particles on the oiled internal collection surface of the inlet.
Wedding et al. (1985a,b) countered that the Sierra-Andersen
instrument was overestimating PM-10 concentrations because of
particle bounce, and that the bounce effect could be minimized by
oiling the impaction surface.
An experiment by EPA in Phoenix (Purdue et al. , 1986)
suggested that both of these explanations were correct, and that
the undercollection by the Wedding instrument could be minimized by
periodic cleaning whereas the overestimation by the S/A 321A could
be minimized by oiling the impaction stages of the inlet. Even
properly maintained instruments continued to show a 10-15%
difference, however, with the Sierra-Andersen providing the higher
readings. It was concluded that this difference would likely be an
A-17
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collection, <0.5 /xm changes in D50 cutpoint) are expected at wind
speeds of 2, 8, and 24 km/h/ which span the observed wind speeds in
Riverside.
The wind tunnel tests do little to explain the much larger
differences observed in the field. Perhaps this is because the
wind tunnel tested only one variable (wind speed), whereas
temperature, concentration, composition, and cleaning frequency all
had important effects on one or more of the sampling methods.
SUMMARY
In a general sense, all methods performed well. Few samples
of any type were lost due to equipment failure. All three methods
showed excellent precision, with median RSDs of 3-5%. The
differences between the methods were no greater than has been
observed in previous comparisons of reference methods.
Several new findings have emerged. One is that cleaning the
Wedding often results in readings over the next 12-hour period that
are sharply lower (by 14%) compared to the dichotbmous sampler,
with an apparent "recovery" period of two days. This effect may be
due to the vanes of the cyclone intercepting a portion of the
aerosol until an equilibrium loading is achieved. The effect
should be studied further.
A second finding is that temperature has a strong differential
effect on the methods. This finding was made possible by the 12-
hour sampling, which showed a significant 13% day-night difference
A-19
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REFERENCES
Environmental Monitoring Systems Laboratory (1989). Operating
Procedure for the Sierra Series 244E dichotomous sampler equipped
with the Andersen model 246B PM10 Inlet.
Federal Register (July 1, 1987). Ambient Air Quality Standards
for Particulate Matter; Final Rules. 40 CFR Parts 50, 51, 52, 53,
and 58; Appendices J and K.
Hoffman, A.J., Purdue, L.J., Rehme, K.A., and Holland, D.M. (1988).
1987 PM10 Sampler Intercomparison Study. Internal EPA report.
Kashdan, R.R., Ranade, M.B., Purdue., L.J., and Rehme, K.A. (1986).
Interlaboratory Evaluation of Two Inlets for Sampling Particles
Less than 10 /im. Envir. Sci. Tech. 20:911-916.
Marple, V.A., Rubow, K.L., Turner, W. and Spengler, J.D. (1987) Low
flow rate sharp cut impactors for indoor air sampling: design and
calibration, J. Air Pollut. Control Assoc. 37:1303-7.
McFarland, A.R. and Ortiz, C.A. (February, 1984) Characterization
of Sierra-Andersen PM-10 inlet model 246b. Air Quality Laboratory,
Texas ASM. Report #4716/02/02/84/ARM. Revised.
Ott, W.R. (1990). A Physical Explanation of the Lognormality of
Pollutant Concentrations. J. Air Waste Manage. Assoc. 40:1378-83.
Pellizzari, E.D., Thomas, K.W., Clayton, C.A., Whitmore, R.W.,
Shores, R.C., Zelon, H.S. and Perritt, R.L. (1992). Particle Total
Exposure Assessment Methodology (PTEAM). Final Report. Vol. I.
EPA Contract # 68-02-4544.
Purdue, L.J. (1985). US EPA PM10 Methodology Review. Internal
report. USEPA. Environmental Monitoring Systems Laboratory.
Research Triangle Park, NC.
Purdue, L.J., Rodes, C.E., Rehme, K.A., Holland, D.M. and Bond,
A.E. (1986). Intercomparison of High-Volume PM10 Samplers at a
Site with High Particulate Concentrations, JAPCA 36:917.
Ranade, M.B., Woods, M.C., Chen, FL. Purdue, L.J. and Rehme, K.A.
(1990). Wind Tunnel Evaluation of PM10 Samplers. Aerosol Sci.
13:54-71.
Rodes, C.E.,.Rehme, K.A., and Purdue, L.J., (Feb. 1982). Particle
Collection Criteria for 10 Micrometer Samplers. Internal report.
US EPA. Environmental Monitoring Systems Laboratory. Research
Triangle Park, NC.
Rodes, C. E. Holland, D.M., Purdue, L.J.. and Rehme, K.A., (1985).
A Field Comparison of PM10 Inlets at Four Locations. JAPCA 35:345.
A-21
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Wedding, J.B., Weigand, M.A., Kim, Y.J., Swift, D.L. and Lodge,
J.P. Jr., (1987) . A Critical Flow Device for Accurate PM1p Sampling
and Correct Indication of PM10 Dosage to the Thoracic Region of the
Respiratory Tract. JAPCA 37:254-258.
A-23
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Table 2. Comparison of ratios of the three methods.
Statistic
Arith. mean of logs
of the ratios
St. Dev. of logs
Geom. mean ratio
Geom. stand, dev.
Upper 97.5% ratio8
Lower 2.5% ratio3
Time
Day
Night
D
N
D
N
D
N
D
N
D
N
PEMSAM
Dichot
0.12
0.12
0.10
0.09
1.13
1.13
1.11
1.09
1.39
1.34
0.92
0.95
Dichot
Wedding
0.00
0.14
0.16
0.17
1.00
1 . 15
1.17
1.18
1.37
1.60
0.73
0.83
a Calculated values two standard deviations above and below
the mean (GM X GSD2 and GM/GSD2)
A-25
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Table 4. Effect of cleaning on Wedding sampler
Ratio of concentration (Wedding/dichotomous)
n n+2 n+4 n+6
Period :
cleaned
Rati<
n n-2
10
19
28
40
49
59
69
79
89
Normalized
mean
St . error
1.13
0.97
1.30
0.96
1.00
1.08
0.94
0.87
0.90
1.0
,
1.13
0.97
1.30
0.96
1.00
1.08
0.94
0.87
0.90
0.98
0.80
0.92
1.17
0.75
0.72
1.03
0.74
0.72
1.00
0.84
0.96
1.03
0.68
0.93
1.22
0.77
0.74
1.29
0.98
0.75
0.94
0.67
0.98
1.12
0.78
0.76
1.04
1.01
0.98
1.00
0.77
0.99
1.09
0.87
0.92
0.86
0.06
0.91
0.04
0.92
0.05
0.99
0.04
A-27
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Figure Captions
Figure 1. Distribution of ratios of PM10 concentrations at the
central site, as measured by the three measurement
methods employed. (Top) Average of two dichotomous
samplers compared to the average of the personal exposure
monitor (PEM) and Stationary Ambient Monitor (SAM)
deployed at the site. (Middle) Average of two Wededing
high-volume instruments compared to the two dichotomous
samplers. (Bottom) Wedding compared to PEMSAM average.
Distributions are broader for the two comparisons
involving the Wedding sampler.
Figure 2. Differences in residuals from successive 12-h periods
(calculated from a model comparing the Wedding and
dichotomous samplers) are here fitted by a "diurnal
oscillation" step function. The 48 days are followed by
the 48 nights on the x-axis. The function takes on one
set of values during the first 30 days (nights) and the
opposite set during the last 18 days (nights).
A-29
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A-31
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A-33
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Appendix 2
RESULTS FROM STEPWISE REGRESSIONS USING NINE VARIABLES,
Symbols Definition
Dependent variables
Igwddi
Igpswd
Igpsdi
Log10 (Wedding) - Iog10 (dichot)
Log10 (average of PEM and SAM) -
Log1Q (PEMSAM) - Iog10 (dichot)
(Wedding)
Independent variables
avtemp
avwndir
avwindsp
avdewpt
avdic
avpemsam
avwed
cleanfreq
diurnal
period
samcoarse
dicoarse
Average temperature (°F) from local airports
Average (airport) wind direction (°) ("0" = North)
Average (airport) wind speed (knots)
Average dewpoint (°F)
Average concentration of dichots "B" & "C" (/ig/m3)
Average concentration of PEM and SAM (/ig/m3)
Average concentration of Weddings "A" & "D" (jug/m3)
Cleaning frequency for Wedding samplers. "1" = cleaned
less than 2 days before; "0" = not cleaned for 2 days
or more.
"Diurnal oscillation" step function. "1" for first 30
days and last 18 nights; "0" otherwise,
12-h period since monitoring began: "1" = overnight
sampling period beginning at 7 PM on Sept. 22, 1990;
"96" = Daytime sampling period beginning at 7 AM on
Nov. 9, 1990.
coarse fraction (PM10 - PM., 5) measured by SAM.
coarse fraction (PM10 - PMj'g) measured by dichot.
A-35
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Stepwise Selection for l^(wd/di) YYA'i 5:44:50p
eeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeee4iseeeeeeeeeeeeeeeeeee
Selection: Forward Maximum steps: 500 F-to-enter: 4.00
Step: 3 F-to-remove: 4.00
Control: Manual
R-squared: .75185
Adjusted: .73324
MSE: 1.2646E-3
d.f.: 40
Variables in Model Coeff. F-Remove Variables Not in Model P.Corr. F-Enter
adaaaaaaadaaadaaaaddaaaaaaaaaaaaaaaadadaaaaaaaaaaaaaaaaaaaaaaaaadaadaaaadddaaaaa
4. avwindsp
5. avtemp
6. avdewpt
-0.00969
0.00448
0.00169
24.6972
24.0409
11.0464
1.
2.
3.
7.
8.
cleanfreq
diurnal
avwndir
period
avpemsam
9. dicoarse
.0141
.0170
.1463
.0620
.0795
.0013
.0077
.0112
.8534
.1503
.2479
.0001
Final model selected. Press F5 for options or ENTER to continue.
IHelp 2Edit SSavscr 4Prtscr 50pts 6Go 7Vars 8Cmd 9Review lOQuit
INPUT 8/14/91 17:44 STATGRAPHICS Vers. 2,1. STEP
Model fitting results for: ln(wd/di) 5:45:59p
eeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeee
Independent variable coefficient std. error t-value sig.level
daadadaddaaadadaaadaadaaaaaaaaaaaaaaaaaaaaaaaaaaaaadaaaaaadaaaaaaaaaaaaaaaaaaaad
CONSTANT -0.341387 0.081785 -4.1742 0.0002
avwindsp -0.009694 0.001951 -4.9696 0.0000
avtemp 0.004481 0.000914 4.9031 0.0000
avdewpt 0.001692 0.000509 3.3236 0.0019
aaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaadaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaadaaaaaaaadd
R-SQ. (ADJ.) - 0.7332 SE- 0.035561 MAE- 0.028320 DurbWat- 1.644
Previously; 0.1485 0.040643 0^ 028449 1.354
44 observations fitted, forecast(s) computed for 2 missing val. of dep. var.
A-37
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Stepwise Selection for Iwpswd /T// 6:49:48p
eeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeee
Selection: Forward Maximum steps: 500 F-to-enter: 4.00
Control: Manual Step: 5 F-to-remove: 4.00
R-squared: .45515
Adjusted: .42233
MSE: 3.31655E-3
d.f.: 83
Variables in Model Coeff. F-Remove Variables Not in Model P.Corr. F-Enter
aaaaadaaaaaaaaadddaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaadaaaddaaaad
1.
2.
4.
5.
cleanfreq
diurnal
avwindsp
avtemp
8. avdic
0.04112
0.05042
0.00466
-0.00408
-0.00032
10.4830
16.5914
7.5652
29.1234
4.2333
3 . avwndir
6 . avdewp t
7. VARO
9. dicoarse
.0859
.1248
.0273
.0970
.6094
1.2978
.0611
.7795
Final model selected. Press F5 for options or ENTER to continue.
IHelp 2Edit SSavscr 4Prtscr SOpts 6Go ' 7Vars 8Cmd 9Review lOQuit
INPUT 8/14/91 18:49 STATGRAPHICS Vers. 2.1 STEP
Model fitting results for: Inpswd 6:51:31p
eeeeeeeeeeeeeeeee'eeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeegeeeeeeeeeeeeeeeee
Independent variable coefficient std. error t-value sig.level
aaaaaaaaaadaaaaaaaaaaaaaaaaaaadaaaaaaaaaaaaaadaaaaaaaaaaaaaaaaaaaaaaadaaaaaaaaad
CONSTANT
cleanfreq
diurnal
avwindsp
avtemp
avdic
0.320119
0.041122
0.050425
0.004662
-0.004083
-0.000318
0.05198
0.012701
0.012379
0.001695
0.000757
0.000155
6.1585
3.2377
4.0733
2.7505
-5.396.6
-2.0575
0.0000
0.0017
0.0001
0.0073
0.0000
0.0428
R-SQ. (ADJ.) - 0:4223 SE= 0.057590 MAE= 0.040182 DurbWat- 2.106
Previously: 0.0000 0.000000 0.000000 0.000
89 observations fitted, forecast(s) computed for 6 missing val. of dep. var.
A-39
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Stepwise Selection for ln,(ps/wd) l^j" 6:ll:19p
eeeeeeeegeeeeeeeSeeeeeeeeeeeeeeeegeeeeeeeeeSeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeeee
Selection: Forward Maximum steps: 500 • F-to-enter: 4.00
Control: Manual Step: 3 F-to-remove: 4.00
R-squared: .50707
Adjusted: .47100
MSE: 3.32695E-3
d.f.: 41
Variables in Model Coeff. F-Remove Variables Not in Model P.Corr. F-Enter
aaaaaaaaaaaaaaaaaaaadaadaaaaaaaaaaaaaaaaaadaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaa
1. cleanfreq
6. avdewpt
8. avdic
0.08447
0.00187
-0.00085
22.3841
6.4571
13.3681
2.
3.
4.
5.
7.
9.
diurnal
avwndir
avwindsp
avterap
period
dicoarse
.0394
.0676
.2825
.2092
.2406
.2725
.0622
.1835
3.4683
1.8302
2.4584
3.2092
Final model selected. Press F5 for options or ENTER to continue.
IHelp 2Edit SSavscr 4Prtscr SOpts 6Go 7Vars . 8Cmd 9Review lOQuit
INPUT 8/14/91 ' 18:11 STATGRAPHICS Vers. 2.1 STEP
Model fitting results for: ln(ps/wd) 6:12:17p
geeeeee§eeee§eee§eeeeeeeee§geeeeeeeeeeeegeeee§ee§eeeeeeegeeeeeeee§eeeeeeeeeeeeee
Independent variable coefficient std. error t-value sig.level
daaaaaaaaaaaaaaaaaaaaaadaaaaaaaaaaaaaaadadaaaaaaaaaaaaaaaaaaaaaaaaaaaadaaaaaadaa
CONSTANT 0.051111 0.032324 1.5812 0.1215
cleanfreq 0.08447 0.017854 4.7312 0.0000
avdewpt 0.001868 0.000735 2.5411 0.0149
avdic -0.000847 0.000232 -3.6562 0.0007
aaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaadaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaaad
R-SQ. (ADJ.) - 0.4710 SE- 0.057680 MAE= 0.041101 DurbWat- 1.041
Previously: 0.6281 0.042562 0.032090 0.953
45 observations fitted, forecast(s) computed for 3 missing val. of dep. var.
A-41
-------
-------
Stepwise Selection for lo.(ps/di) Qft V 5:40:15p
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Selection: Forward Maximum steps: 500 F-to-enter: 4.00
Control: Manual Step: 1 F-to-remove: 4.00
R-squared: .16829
Adjusted: .14848
MSE: 1.65186E-3
d.f.: 42
Variables in Model Coeff. F-Remove Variables Not in Model P.Corr. F-Enter
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Final model selected. Press F5 for options or ENTER to continue.
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INPUT 8/14/91 17:36 STATGRAPHICS Vers. 2.1 STEP
Model fitting results for: ln(ps/di) 5:40:49p
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Independent variable coefficient std. error t-value sig.level
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avwindsp -0.005493 0.001884 -2.9152 0.0057
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R-SQ. (ADJ.) - 0.1485 SE- 0.040643 MAE= 0.028449 DurbWat- 1.354
Previously: 0.0000 0.000000 0.000000 0.000
44 observations fitted, forecast(s) computed for 1 missing val. of dep. var.
A-43
-------
-------
APPENDIX 8
STUDY.OP STORAGE STABILITY OP NICOTINE
ON PERSONAL EXPOSURE MONITOR FILTERS
B-l
-------
-------
STUDY OF STORAGE STABILITY OF NICOTINE ON FILTERS
WANO. IV-139
Objectives of the Work Assignment
Although storage stability of nicotine has been established for periods of up to a
month, many of the Particle Total Exposure Assessment Methodology(PTEAM) study
filters were stored for longer periods of time, up to three months. Therefore it is
important to establish the storage stability of nicotine on the filters used in the PTEAM
Study in order to interpret PTEAM data and also to plan for future studies of personal
exposure to particles and environmental tobacco smoke. In this study, Harvard
researchers exposed a number of filters in the home of a cigarette smoker, stored the
filters under the same conditions as in the PTEAM Study, and analyzed the filters, using
the same analysis methods as in PTEAM, after 0, 4, and 6 weeks in order to determine
storage stability. An additional set of filters were also archived for possible analysis at
a much later date (eg. 26 weeks after collection). A set of filters were also spiked with
2, 5 and 15 ^g of nicotine in the lab and stored at two different temperatures, and then
analyzed after 0, 4, and 6 weeks to examine the storage stability under controlled
conditions. The details of the nicotine storage study QA/QC and analyses procedures
are provided in Appendix I.
Description of Storage Study
The nicotine storage study consists of two sets of samples: first a series of
artificially prepared filter samples which have been treated with known amounts of
nicotine, and second a series of filter samples obtained in a home setting with active
cigarette smoking. (All filters were pretreated with known amounts of citric acid to trap
nicotine.) Each set was further subdivided into two storage temperature groups of 4°C.
and 25°C. These subdivisions have been undergoing analysis at different storage times
which include a time zero or analysis immediately after collection or preparation, at
approximately 4 weeks of storage, and at approximately 6 weeks of storage. A sufficient
number of samples were obtained so that another analysis could be conducted at the
sixth month mark if funds are available in the future.
Description of "Spiked Filters"
The artificially treated samples were made from a carefully prepared aqueous
solution of nicotine salicylate. Concentrations were adjusted to produce filter sets with
2 |j.g, 5 jxg, and 15 p.g of nicotine. Nicotine salicylate was used because it is a salt
which can be obtained in purer form than nicotine liquid, has less decomposition in
storage than the pure liquid, and consequently has less loss of nicotine by volatilization.
The latter point is very important for the preparation of filters containing small amounts
of nicotine because there can be very significant losses of nicotine when it is added to
B-3
-------
-------
stored at 4°C.; and since each data point is an average of two samples, it is noteworthy
that in this case one determination gave 5.3 p.g of nicotine and the other gave 4.59 ^g
for an average of 4.94 p.g. In fact this was the largest deviation for any of the "spiked
samples" analyzed to date and clearly stands out as unusual. Values for the 2 pg
loading are speculative because the nicotine loadings for the time 0 samples were
obtained when the GC was erratic; at a later time we will try to reanalyze these if
sufficient volume remains. Nevertheless, the nominal value of 2 p.g is not unjustified
since the same solution which was used to prepare the 5 and 15 |j.g loadings was also
used to prepare the 2 ^g samples. (At time 0, the 5 and 15 gave averages of 4.77 and
14.6 respectively.) The obtained recoveries ranged from 93% to 99% and if the 2 jig
loading followed the trend of the 5 and 15 jig loadings, the true recovery would be much
closer to 100% average.
The data obtained in the residence contains more variability under all conditions.
To help explain this, the data are shown in a form which schematically represents their
physical position during sampling. Also, the average(% recovery) and coefficient of
variation are given for each time period for each experiment. The recoveries range from
59% to 153%, the large deviations from 100% are probably the result of spatial variation.
The average and coefficient of variation are also shown for each experiment regardless
of storage time. These last data show that there is no significant difference between
storage at 4°C. and 25°C. Observation of the data for GS3-01, CS3-02, and for CS2-02
suggests that samples in the A and B position may have had a tendency to collect more
nicotine, i.e. more cigarette smoke possibly because of their location which was slightly
closer to the source(s) than positions D or E. However, values obtained in positions F
and H also appear larger but still less than those in A or B. This reasoning is obviously
not consistent with the data obtained for CS1 -01 but it should be noted that at the level
of a 1 ng loading, the analytical RSD is greater than at higher levels and the higher level
data also indicates spatial variation; both of these factors may contribute to the 4 and
6 week losses shown. The apparent anomaly for the 4 week sample average.for CS3-01
is clearly traced to one sample with an unexplainably high reading.
Comparing the positionally related data within any experiment shows differing
implications. For example, in CS1-02, there is a decrease in nicotine from position C to
D to E then a reversal in position F; E and F are both 6 week storage at 4°C. In CS3-01
there is a decrease going from E to D but the opposite occurs in CS3-02 going from D
to C. In these cases neither the storage temperature nor time can ,be clearly shown to
be causative agents. Since the analytical technique, the sample flow rates, and the
storage times have relatively low RSDs, the variation seen may indeed be caused by
spatial considerations of sampling. This can be the case if the smoke does not disperse
completely uniformly in the room. Even though gas phase nicotine may be expected to
disperse uniformly more quickly than paniculate matter, neither has a large diffusion
coefficient and there was not very much air movement in the room except for the
sampling units themselves.
B-5
-------
-------
None of the models tested resulted in a significant effect estimate for the class
variables selected. In other words, analysis time, storage temperature, nicotine
loading level or location of the sampler did not statistically significantly influence or
affect the nicotine concentration measurements. The p-values for the estimated class
effects were found to be greater than >0.2 for most of these design factors.
(However, the temperature effect at ~ 20 p.g loading reached near significance in
Model 9 with p = 0.055.)
Even though the sample size was limited, we can conclude from this more
formal analysis that the results support the observations reported earlier in that over
the six-week storage time, the nicotine concentrations did not vary by time of storage,
temperature or nicotine level. Even though location differences were not found to be
statistically significant because of variability in the data, nevertheless nicotine mass
measured at position B vs D at each nicotine level suggests spatial trends in the data
as a consequence of sampler orientation and proximity to the nicotine source.
Summary
Nicotine stability experiments were carried out successfully. Laboratory spiked
samples and field samples were analyzed after 0, 4, and 6 weeks of collection. Blank
samples were also obtained and analyzed. Within experimental variability, results
indicate good stability of nicotine samples over different storage times using the
same field collection and analysis techniques employed in the PTEAM study.
The data obtained indicate that for "spiked" samples, no appreciable loss of
nicotine can be determined after 4 weeks at 25°C. The data obtained from a real
residential situation also do not indicate that there is detectable loss of nicotine but
the large associated uncertainty which is observed may be related more to spatial
variation as opposed to actual losses during storage.
B-7
-------
-------
Home Data for PTEAM nicotine storage study.
The values given below are micrograms of nicotine found.
Within comparative groupings, the sample volumes are equivalent
14 April 1993 Robert A. Weker
filename=c:\pteamnic\mcg_nic.wk1 and b:\mcg_nic.wk1
Expt. Storage Storage
Temp. Time
CS1 -01 25 °C.
CS1 -02 4 °C.
CS3-01 25 °C.
CS3-02 4 °C.
CS2-01 25 °C.
CS2-02
~ 20 UCL
4°C.
Position
BCD
Group
H Avg. RSD Avg. &
RSD
0 weeks
4 weeks
6 weeks
0 weeks
4 weeks
6 weeks
0 weeks
4 weeks
6 weeks
0 weeks
4 weeks
6 weeks
0 weeks
4 weeks
6 weeks
0 weeks
4 weeks
6 weeks
I
0.99
8.65
24.4
26.2
i
0.73
13.5
9-.4
19
30
1.03
0.98
5.91
7.73
19.9
0.68
!
0.86
6.46
6.56
16.2
23.6
0.82
8.43
8.44
18.9
1.28
0.95
20.6
-•
0.72 1
0.71
7.51
17.6
0.79
6.44
10.8
19.6
23.4
1.18 8.5 0.88
0.76 3.9 25.25
0.70 2.9
0.80 16.0 0.89
0.92 7.0 11.28
0.88 7.3
6.98 7.7 8.04
11 23.1 32.04
6.18 4.4
7.5 12.5 8.60
9.26 16.6 15.33
9.02 4.2
19.3 1.8 19.28
17.6 8.0 13.20
21 16.2
25 20.2 23.95
23.4 12.0 14.23
23.5 0.4
B-9
-------
-------
A copy of PROCEDURE TO ANALYZE FILTERS FOR NICOTINE CONTENT is
attached. This was substantially followed for analysis of the storage study samples.
Standards were injected onto the GC at the beginning and end of each run as well as
interspersed between about every six to ten samples.
Although the procedure calls for 10% reanalysis, almost every sample was reanalyzed
twice'because the numbers of samples being analyzed per run was small. If the-
reanalysis was not within 15%, then the sample was injected a third time; an average
was always used unless the chromatogram clearly indicated an anomaly.
For the spike test samples, 2 lab blanks were run for each test configuration. For the
samples exposed to nicotine in the field, 2 field blanks were carried through the entire
process for each test configuration. Both field and lab blanks usually produced zero
readings; the exception would occur sometimes if the blank were injected after a high
standard, but the immediately subsequent reinjection would be zero.
A strict cleaning procedure was maintained at ail times to insure that contamination was
minimized. This consisted of routine washing and rinsing with high purity water and/or
rinsing with pretested ammoniated heptane. All vials were rinsed with ammoniated
heptane and the rinses checked for nicotine contamination; similar treatment was applied
to extraction vials, standard bottles, and GC syringes, etc.
B-ll
-------
-------
3. Vials may be ultrasonically cleaned with water
and laboratory detergent, followed by several
rinses with Milli-Q water and ultrasonication, and
finally overnight "air' drying with some dust
protection in place.
4. Syringes are maintained by rinsing carelfully
with ammoniated heptane before and after each
usage.
II Extraction of Filters
A. With a clean SS tweezers, remove the filter from its Petri
dish by grasping the edge only, then on a clean surface cut it
into 6-10 narrow strips using a clean SS scissors. Carefully
transfer the strips to a clean 50 ml Erlenmeyer flask fitted
with a Caplug.
B. Add 500 pl'of ethanol from an automatic pipette directly
to the filter material to wet it thoroughly.
C. Carefully transfer an appropriately sized magnetic
stirring bar to the flask.
D. With an automatic syringe, add 5 ml of ION NaOH to the
flask and loosely place the Caplug in the neck.
E. Stir gently for 5 minutes (timer). Turn the stirrer off.
F. Add 5 ml of ammoniated heptane with an accurate glass
transfer pipette.
G. Continue stirring for an additional 10 minutes (timer).
Turn the stirrer off.
H. Carefully decant ca. 2-3 ml of the organic supernatant
into a clean 4 ml vial.
NOTES: .1. Exposed filters must be stored in a
refrigerator at 4°C.
2. All vials are to be pretested for nicotine
contamination by testing on the GC a combined rinse
(ammoniated heptane) from each batch of. 10 or less
vials.
3. At least 10% of filters to be analyzed should
be lab blanks.
4. At least 10% of filters to be analyzed should
be field blanks.
B-13
-------
-------
8
Frequently check the hydrogen regulator secondary
pressure, guage and ensure that it is reading exacti.y 3.5
psx. If not, it may be adjusted very carefully as needed
to _ maintain the reading at 15 psi - the regulator
adjusting handle is very sensitive! Perform this
adjustment between GC runs ' and allow a few minutes
equilibration time; a very small change in the hydrogen
pressure causes a very large change in the detector
output. NOTE: When the GC is being operated routinely
from early morning to late afternoon or early evening
then for overnight shutdown, the hydrogen regulator
needle valve may be closed (fully CW) while the tank
valve and the regulator valve are left ON; of course
this assumes there are no leaks. This can help to
minimize the regulator valve equilibration time.
Depress [SIG1] [ZERO] 6.0 [ENTER]. This operation causes
the GC to subtract the [ZERO] value shown (in this case,
6.0) from the [SIG1] valuebefore the signal is sent to
its output (the recorder); it is a sophisticated method
to both keep the recorder pen on scale and at the same
time allow full exploitation of the. GC's output
capabilities. *
9. 'Proceed to inject standards and samples. Some adjustment
of the RANGE 2t will be necessary to keep the larger
nicotine peaks on scale. NOTE: Prior to every injection
.check the value of SIGNAL i. If it is not 7.1 ± o.i'
then first check the hydrogen regulator guage for an
output pressure of 15 psi and adjust accordingly (see
•above); second, adjust the NPD bead power (this knob is
also a very sensitive adjusting mechanism) until a stable
baseline is maintained at 7.0 ± o.l; after approximately"
three or four hours, the baseline is usually stable
however, if the usage has been heavy, then the detector
will produce a signal greater than 7.1. This is not the
result of change in inherent detector sensitivity but
rather a temporary change in output due to phenomena
occuring at the detector from small amounts of lingering
compounds from previous injections. In time, if no
further injections were to be made, the baseline would
smoothly and slowly return to 7.0. Running quality
assurance injections of nicotine standards on some
schedule, say one out of every five or six injections,
will help to reveal the cause of baseline changes.
Experience gained with detector operation is a very big
help in this situation.
10. Calibration
A. Use the working standards labelled 0.0 (pure
ammoniated heptane), 0.10. 0.25, 0.50, 1.0, 2.5,
and 5.0 ppm nicotine. (i ppm =
B-15
-------
-------
SEM SCREENING OF PTEAM SAMPLES
John Miller and Bob Willis
March 5, 1993
Contact Bob Willis for more information: 919-541-2809
C-l
-------
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INDEX TO MICROGRAPHS
PERSONAL ID
1
1
1
17
17
35
35
35
42
42
55
55
55
64
64
64
69
69
71
71
105
105
108
108
122
122
FILTER ID
F4693 PEM
F4643 SIM
F4644 SAM
F4777 PEM
F4816 SIM
F4874 PEM
F4903 SIM
F4878 SAM
F4987 PEM
F4983 SIM
F5431 PEM
F5438 SIM
F5453 SAM
F5383 PEM
F5400 SIM
F5224 SAM
F4957 PEM
F4958SIM
F5241 PEM
F5240 SIM
F6052 PEM
F6053 SIM
F5875 PEM - NIGHT
F6033 SIM - NIGHT
F5829 PEM - NIGHT
F5786 SIM - NIGHT
PAGE NUMBER
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APPENDIX D
AIR EXCHANGE DATA
D-l
-------
Explanation of Headings in Appendix D
PID
LOG
Amt PFT
(PD
LOD
house vol
(ft3)
elapsed time
(hr)
AER (hr'1)
Period
Time of day
Dup
Personal identification Number: 001A-184A
Only one participant from each house;
therefore the ;PID is also the House ID
Location of PFT Collector tubes.
BED •= toedroom
LIV = living room
FAM = family room
DEN = den
KIT = kitchen
Amount of PFT collected in picoliters
limit of Detection
blank = measurable
< = below the LOD
Volume of house in cubic feet
Duration of PFT collection period
Air exchange rate (air changes per hour)
Day and time of day of monitoring.
1 = overnight; Sept. 22-23, 1990
96 = daytime; Nov. 9,, 1990
Time of day of monitoring.
Duplicate collector tube for PFT: 1 = duplicate
D-2
-------
PTEAM Pilot Study -Euations Used to Calculate Air Exchane Rate
The air exchange rate (AER) is calculated as follows:
where n: number of PFT sources
S: emission rate (pL/hr)
V: house volume (m3)
C: PFT concentration (pL/L)
The emission rate is defined by the equation:
g 350\ig
where E is PFT emission rate (g/hr) and the other quantities are physical constants. Two
emission rates are used: 4.57xlO"5 for sources labeled by HSPH as "NN" series and 4.92xlO"5
for all other sources. The emission rate used in the equation is the weighted average of
these, i.e.:
E=4.57xlQ-5x(% NN series sources)+4.92xlO~5x(l - % NN series sources)
.There are typically either six or eight sources per household. House volume was estimated
in ft3 in the field; this is converted to m3 using the relationship 28.31685 cubic feet = 1 cubic
meter.
The PFT concentration is calculated as:
ELPxSR
where P: amount of PFT collected by the CAT (pL)
ELP: elapsed time CAT was exposed (hr)
SR: CAT sampling rate = 0.00892 L/hr
D-3
-------
Amt PFT • house vol elapsed
PID
001A
001A
001A
001A
001A
001A
002A
002A
002A
002A
002A
002A
OOSA
OOSA
003A
003A
OOSA
OOSA
004A
004A
004A
004A
004A
OOSA
OOSA
OOSA
OOSA
OOSA
006A
006A
006A
006A
006A
006A
007A
007A
007A
007A
007A
007A
OOSA
OOSA
OOSA
OOSA
008A
009A
009A
009A
009A
009A
009A
010A
010A
010A
010A
010A
011A
011A
011A
011A
LOG
BED
BED
LIV
LIV
LIV
LIV
BED
BED
FAM
FAM
FAM
FAM
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
BED
BED
LIV
LIV
(pL) LOD
3.00 <
4.90 <
17.80
12.50
17.10
12.40
28.10
6.96
3.00
6.98
6.58
5.48
3.00 <
3.00
5.50 <
Void
5.50 <
5.90
11.22
4.28
5.50 <
Void
3.00 <
13.49
17. '60 .
15.50
13.30
45.50
3.33
3.00 <
9.53
3.24
3.00 <
7.91
6.60 <
5.41
3.00 <
3.00 <
3.00 <
3.93
11.80
10.50
12.00
7.70
15.40
6.70 <
10.20
3.00
11.25
Void
4.90 <
3.00 <
3.00 <
3.00 <
3.00 <
6.60 <
47.30
11.50
55.50
47.00
(ft3) time (hr)
4,940
4,940
4,940
4,940
4,940
4,940
10,350
10,350
10,350
10,350
10,350
10,350
22 , 614
22 , 614
22,614
22,614
22,614
22,614
5,148
5,148
5,148
5,148
5,148
8,012
8,012
8,012
8,012
8,012
7,752
7,752
7,752
7,752
7,752
7,752
6,052
6,052
6,052
6,052
6,052
6,052
7,048
7,048
7,048
7,048
7,048
6,624
6,624
6 , 624
6,624
6,624
6,624
5,832
5,832
5,832
5,832
5,832
6,720
6,720
6,720
6,720
13.5
8.1
13.5
8.1
13.5
8.1
10.9
9.5
10.9
10.9
9.5
9.5
13.1
9.4
9.4
13.0
13.0
9.4
11.2
10.5
11.2
10.5
11.2
11.3
10.0
11.2
11.2
9.9
9.5
11.4
11.4
9.4
9.4
11.4
9.4
10.6
10.5
10.5
9.4
9.4
11.3
11.1
11.2
11.1
11.2
8.9
11.9
8.9
11.9
11.9
8.9
11.8
10.9
11.8
11.8
10.9
11.7
11.0
11.7
11.7
AER
Time
(hr-1) Period of day
5.50
2.03
0.93
0.79
0.96
0.80
0.23
0.80
2.12
0.91
0.85
1.02
1.18
0.84
0.46
0.64
0.43
1.17
2.87
2.38
V
4.36
0.63
0.43
0.55
0.64
0.16
2.21
2.97
0.93
2.27
2.45
1.12
1.43
1.96
3.51
3.51
3.12
2.38
0.82
0.91
0.80
1.23
0.62
1.21
1.06
2.70
0.96
1.65
4.08
3.76
4.07
4.07
1.72
0.22
0.86
0.19
0.22
1
2
1
2
1
2
1
2
1
1
2
2
3
4
4
3
3
4
3
4
3
4
3
3
4
3
3
4
4
3
3
4
4
3
6
5
5
5
6
6
6
5
6
5
6
5
6
5'
6
6
5
6
5
6
6
5
8
7
8
8
night
day
night
day
night
day
night
day
night
night
day
day
night
day
day
night
night
day
night
day
night
day
night
night
day
night
night
day
day
night
night
day
day
night
day
night
night
night
day
day
day
night
day
night
day
night
day
night
day
day
night
day
night
day
day
night
day
night
day
day
Dup
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-4
-------
011A LIV
011A LIV
012A BED
012A BED
012A DEN '
012A DEN
012A KIT
013A BED
013A BED
013A FAM
013A FAM
013A FAM
013A FAM
013 A KIT
013A KIT
014A BED
014A BED
014A FAM
014A FAM
014A FAM
014A FAM
014A OTH
015 A BED
015A BED
015A KIT
015A KIT
015A LIV
015A LIV
015A LIV
015A LIV
016A BED
016A LIV
016A LIV
016A LIV
016A LIV
017A BED
017A BED
017A LIV
017A LIV
017A LIV
018A BED
018A BED
018A LIV
018A LIV
018A LIV
019A BED
019A BED
019A DEN
019A DEN
019A DEN
019A DEN
020A BED
020A BED
020A KIT
020A KIT
020A LIV
020A LIV
020A LIV
020A LIV
020A OTH
021A BED
021A BED
24.60
25.40
3.00 •
7.20 •
3.00 •
4.30 •
3.00 •
6.04
6.36
6.13
4.81
6.18
5.07
8.21
6.14
17.90
13.20
15.50
22.30
17.00
19.80
3.00
8.78
14.70
•16.20.
21.90
14 ".50
7.92
19.00
21.70
10.10
18.60
14.60
11.70
12.72
3.00
3.77
9.12
9.60
9.30
31.40
11.25
4.30
35.20
29.50
.3.00
9.26
3.00
3.65
3.00
4.30
8.88
3.00
8.96
4.54
9.38
3.84
8.82
5.45
3.00
3.00
4.60
6,720
6,720
16,155
16,155
16 , 155
16,155
16,155
15 , 348
15,348
15,348
15,348
15,348
15,348
15,348
15 , 348
13,360
13,360
13,360
13,360
13,360
13,360
13,360
12,785
12,785
12,785
12,785
12,785
12,785
12,785
12,785
6,500
6,500
6,500
6,500
6,500
4,770
4,770
4,770
4,770
4,770
6,060
6,060
6,060
6,060
6,060
12,029
12,029
12,029
12,029
12,029
12,029
7,040
7,040
7,040
7,040
7,040
7,040
7,040
7,040
7,040
10,150
10,150
11.1
11.1
11.9
8.4
8.4
8.4
11.9
8.5
13.2
8.4
13.2
13.2
8.4
13.2
8.4
10.8
14.9
10.7
14.9
10.7
14.9
10.7
11.3
10.0
11.2
10.0
11.2
11.2
9 . 9
9.9
8.0
13.2
13.2
8.0
8.0
.-. 9.7
11.7
11.7
9.6
9.6
11 ..9
9.8
9.8
'-.-12.0
12.0
9.9
11.5
9.8
11.6
11 .6
9.8
11.7
8.4
11.7
8.4
11.7
8.4
11.7
8.4
8.4
10.8
12.0
0.40
0.39
1.50
0.44
1.06
'0.74
1.51
0.74
1.09
0.72
1.44
1.12
0.87
0.84
0.72
0.27
0.51
0.31
0.30
0.29
0.34
1.62
0.81
0.43
0.44
0.29
0.49
0.89
0.33
0.29
0.74
0.66
0.84
0.64
0.58
4.09
3.94
1.62
1.27
1.31
0.38
0.87
2.27
0.34
•0.40
1.65
0.63
1.65
1.59
1.94
1.15
1.13
2.39
1.12
1.58
1.07
1.87
1.14
1.32
2.39
3.05
2.21
7
7
7
8
8
8
7
10
9
10
9
9
10
9
10
10
9
10
9
10
9
10
9
10
9
10
9
9
10
10
12
11
11
12
12
11
12
12
11
11
11
12
12
11
11
12
11
12
11
11
12
13
14
13
14
13
14
13
14
14
14
13
night
night
night
day
day
day
night
day
night .
day "
night
night
day
night
day
day
night
day
night
day
night
day
night
day
night
day
night
night
day
day
day
night
night
day
day
night
day
day
night
night
night
day
day
night
night
day
night
day
night
night
day
night
day
night
day
night
day
night
day
day
day
night.
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-5
-------
021A
021A
021A
022A
022A
022A
022A
022A
022A
022A
022A
023A
023A
023A
023A
023A
024A
024A
024A
024A
024A
025A
025A
025A
025A
025A
025A
026A
026A
026A
026A
026A
026A
027A
027A
027A
027A
027A
027A
028A
028A
028A
028A
028A
028A
029A
029A
029A
029A
029A
029A
029A
029A
030A
030A
030A
030A
030A
030A
030A
030A
031A
LIV
LIV
LIV
BED
BED
KIT
KIT
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
DEN
DEN
DEN
DEN
BED
BED
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
BED
BED
KIT
KIT
LIV
LIV
LIV
LIV
BED
BED
DIN
DIN
DIN
DIN
KIT
KIT
BED
3.04
4.56
3.73
5.06
Void
17.00
7.98
5.30
13.80
14.20
Void
6.98
16.10
6.64
3.79
19.10
13.40
9.75
12.73
12.30
12.14
3.00 <
3.00 <
4.45
3'. 00 <
6.60 <
5.10 <
5.76
10.00
5.69
14.40
15.50
1.50
10.80
12.80
12.90
15.40
13.40
3.00 <
15.10
25.40
25.30
25.30
26.30
23.00
3.00 <
Void
6.05
3.00 <
Void
1.49
3.99
Void
4.07
3.25
3.98
8.84
7.21
6.35
3.58
5.83
11.72
10,
10,
10,
4,
4,
4,
4,
4,
4,
4,
4,
4,
4,
4,
4,
4,
7,
7,
7,
7,
7,
7,
7,
7,
7,
7,
7,
15,
15,
15,
15,
15,
15,
2,
2,
2,
2,
2,
2,
11,
11,
11,
11,
11,
11,
13,
13,
13,
13,
13,
13,
13,
13,
6,
6,
6,
6,
6,
6,
6,
6,
8,
150
150
150
136
136
136
136
136
136
136
136
136
136
136
136
136
415
415
415
415
415
604
604
604
604
604
604
243
243
243
243
243
243
964
964
964
964
964
964
707
707
707
707
707
707
509
509
509
509
509
509
509
509
936
936
936
936
936
936
936
936
509
10.
12.
10.
9.
13.
13.
9;
9.
13.
13.
9.
8.
12.
8.
8.
7
0
7
1
3
3
2
1
3
3
1
8
0
8
8
12.0
12.
8.
8.
12.
8.
9.
12.
12.
9.
12.
9.
11.
9.
9.
11.
11.
9.
13.
9.
9.
13.
13.
8.
12.
10.
10.
12.
12.
10.
11.
9.
9.
11.
9.
11.
9.
11.
12.
10.
10.
12.
12.
10.
10.
12.
8.
5
0
0
5
0
7
8
8
7
8
7
3
0
0
2
2
0
6
3
3
5
5
3
0
1
1
0
0
1
5
7
7
5
7
5
7
5
4
3
2
3
4
2
3
4
6
2
2
2
2
1
1
2
1
1
1
1
1
3
0
0
0
0
0
0
2
3
2
2
1
1
1
0
0
0
0
3
2
1
.99
.24
.44
.71
.17
.72
.58
.44
,40
.87
.10
.97
.45
.93
.76
.67
.51
.83
.54
.74
.60
.43
.73
.64
.60
.03
.47
.83
.41
.38
.16
.59
.51
1.49
1
2
"5
0
0
0
0
0
0
2
0
2
4
1
2
2
2
1
1
1
2
1
0
.81
.09
.74
.56
.28
.28
.33
.32
.31
.29
.95
.29
.60
.44
.65
.75
.24
.22
.49
.40
.49
.85
.52
14
13
14
14
13
13
14
14
13
13
14
14
13
14
14
13
15
16
16
15
16
16
15
15
16
15
16
15
16
16
15
15
16
15
16
16
15
15
16
17
18
18
17
17
18
18
17
.17
18
17
18
17
18
17
18
18
17
17
18
18
17
18
day
night
day
day
night
night
day
day
night
night
day
day
night
day
day
night
night
day
day
night-.
day
day
^night
night
day
night
day
night
day
day
night
night
day
night
day
day
night
night
day
night
day
day
night
night
day
day
night
night
day
night
day
night
day
night
day
day
night
night
day
day
night
day
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
.1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-6
-------
031A
031A
031A
031A
03 2 A
032A
032A
032A
032A
032A
032A
033A
033A
033A
03 3A
033A
033A
034A
034A
034A
034A
034A
035A
035A
035A
035A
035A
035A
03 5A
03 5A
036A
03 6A
036A
03 6A
036A
036A
036A
03 6A
036A
037A
037A
037A
037A
037A
037A
037A
038A
038A
038A
038A
038A
039A
039A
039A
039A
039A
040A
040A
040A
040A
040A
040A
BED
DEN
DEN
DEN
BED
BED
FAM
FAM
FAM
FAM
OTH
BED
BED
LIV
LIV
LIV
LIV
BED
BED
FAM
FAM
FAM
BED
BED
KIT
KIT
LIV
LIV
LIV
LIV
BED
BED
FAM
FAM
FAM
FAM
KIT
KIT
OTH
BED
BED
LIV
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
BED
BED
FAM
FAM
FAM
BED
BED
LIV
LIV
LIV
OTH
5
5
4
4
6
13
13
3
11
3
3
3
6
3
6
6
3
21
18
15
14
4
6
20
7
23
21
5
5
24
11
10
5
17
7
3
32
8
26
10
12
28
3
7
8
7
9
3
386
3
3
6
7
5
3
7
4
3
.30
.50
.23
.62
.60 <
.23
.18
.00 <
.10
.00 <
.00 <
.00 <
.11
.00 <
.60 <
.60 <
.29
.00
.40
.80
.30
Void
.98
.38
.00
.49
.20
.60
.96
.87
Void
.50
Void
.20
.80
.84
.00
.27
.00
.10
.44
.90
.10
.54
.80
.00 <
.77
.65
Void
.30
.44
.00 <
.60
.00 <
.00 <
.02
.27
.50 < -
.00 <
.20 <
.60
.00 <
8,
8,
8,
8,
11,
11,
11,
11,
11,
11,
11,
10,
10,
10,
10,
10,
10,
10,
10,
10,
10,
10,
9,
9,
9,
9,
9,
9,
9,
9,
9,
9,
9,
9,
9,
9,
9,
9,
9,
10,
10,
10,
10,
10,
10,
10,
7,
7,
7,
7,
7,
11,
11,
11.
11,
11,
9,
9,
9,
9,
9,
9,
509
509
509
509
118
118
118
118
118
118
118
494
494
494
494
494
494
010
010
010
010
010
936
936
936
936
936
936
936
936
162
162
162
162
162
162
162
162
162
114
114
114
114
114
114
114
413
413
413
413
413
331
331
331
331
331
182
182
182
182
182
182
11
8
11
11
10
10
10
10
10
10
10
9
11
11
9
9
11
9
11
11
--.'- 9
11
11
9
11
9
11
11
9
9
11
9
9
11
11
9
11
9
9
12
9
12
9
9
12
12
10
10
10
10
10
10
12
9
12
12
8
13
13
13
8
8
.9
.6
.9
.9
.9
,8
.7
.9
.7
.9
.7
.4
.7
.7
.4
.4
.7
.6
.4
.4
.6
.4
.8
.9
.8
.9
.8
.7
.9
.9
.8
.8
.8
.8
.8
.8
.8
.8
.8
.0
.7
.0
.7
.7
.0
,0
.8
.1
.0
.0
.8
.0
.6
.9
.5
.5
.3
.7
.7
.7
.3
.3
1.59
1 . 11
1.99
1.82 '
0 . 9.1
0.45
0.45
1 . 99
0.53
1 . 9.9
1.97
1.93
1.17
2.39
0.88
0.88
2.18
0.37
0 . 50
0.59
0.54
1.48
.0.97
0.37
0.83
0.32
0.34
1.04
1.0.6
0.35
0.94
0.97
1.49
0.62
1.19
2.90
0.24
0 . 74
0.29
0.62
0.50
0,27
2.57
1.14
0.95
1.12
0.94
1.78
0.02
1.77
2.23
1.11
0.76
1.66
3.04
1.27
1.20
1.83
17
18
17
17
19
20
20
19
20
19
20
20
19
19
20
20
19
19
20
20
19
20
19
20
19
20
19
19
20
20
21
22
22
21
21
22
21
22
22
62
61
62
61
61
62
62
21
22
- 22
22
21
22
21
22
21
21
24
23
23
23
24
24
night
day
night
night
night
day
day
night
day
night
day
day
night
night
day
day
night
night
day
day
night
day
night
day
night
day
night
night
day
day
night
day
day
night
night
day
night
day
day
day
night .
day
night
night
day
day
night
day
day
day
night
day
night
day
night
night
day
night
night
night
day
day
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
> 1
1
1
: i
i
i
i
i
i
i
i
i
i
i
i
i
i
i
i
i
D-7
-------
041A
041A
041A
041A
041A
041A
042A
042A
042A
042A
042A
042A
042A
042A
043A
043A'
043A
043A
043A
043A
043A
043A
043A
044A
044A
044A
044A
044A
044A
044A
045A
045A
045A
045A
045A
046A
046A
046A
046A
046A
046A
047A-
047A
047A
047A
047A
047A
048A
048A
048A
048A
048A
048A
049A
049A
049A
049A
049A.
049A
049A
050A
050A
BED
BED
LIV
LIV
LIV
LIV
BED
BED
KIT
KIT
LIV
LIV
LIV
LIV
BED
BED
KIT
KIT
LIV
LIV
LIV
LIV
OTH
BED
BED
FAM
FAM
FAM
FAM
OTH
BED
BED
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
OTH
BED
BED
25.80
16.70
18.70
25.90
17.90
14.30
10.10
4.12
4.13
9.79
10.60
9.53
4.83
5.04
Void
6.48
8.68
7.31
9.17
Void
7.29
6.97
3.00
3.00 <
3.00 <
3.00 <
7.97
3.00 <
8.00
4.30 <
9.85
8.89
8.50
11.40
11.70
9.34
5.42
5.81
4.01
16.30
3.00 <
14.70
16.80
14.60
14.10
18.30
12.20
18.10
9.85
24.70
11.40
26.70
13.10
10.60
8.10
15.30
14.30
13.80
14.90
3.00 <
3.00 <
23.20
7
7
7
7
7
7
9
9
9
9
9
9
9
9
8
8
8
8
8
8
8
8
8
7
7
7
7
7
7
7
4
4
4
4
4
5
5
5
5
5
5
4
4
4
4
4
4
6
6
6
6
6
6
6
6
6
6
6
6
6
11
11
,696
,696
,696
,696
,696
,696
,868
,868
,868
,868
,868
,868
,868
,868
,593
,593
,593
,593
,593
,,593
, 593
,593
,593
,736
,736-
,736
,736
,736
,736
,736
, 636
,636
,636
,636
,636
,760
,760
,760
,760
,760
,760
,032
,032
,032
,032
,032
,032
,100 -
,100
,100
,100
,100
,100
,100
,100
,100 .
,100
,100
,100
,100
,320
,320
11.6
9.9
9.9
11.6
11.6
9.9
10.7
11.1
11.1
10,7
10.7
10.7
11.1
11.1
10.9
10.4
10.8
10.4
10.8
10.8
10.4
10.4
10.8
, 11.7
8.6
8.6
11.7
8.6
11.7
8.6
10.9
12.0
11.9
11.9
10.9
13.5
a.4
9.3
9.3
13.5
9.3
10.5
11.0
10.5
11.0
. 10.5
11.0
11.2
9.4
11.2
9.4
11.2
9.4
9.2
13.4
13.4
13.4
9.2
9.2
9.2
7.3
13.1
0.36
0.48
"0.43
0.36
0.52
.0.56
0.87
2.21
2.20
0.90
0.83
0.92
1.88
1.80
1.13
G . 88
1.00
0.83
1.00
1.05
2.52
3.16
2.33
2.33
1.19
2.33
1.18
1.62
1.47
1.78
1.86
1.38
1.23
1.57
1.68
1.75
2.53
,0.90
3.40
1.10
1.01
1.10
1.20
0.88
1.38
0.61
0.95
0.45
0.82
0.41
0.71
0.87
1.66
0. 88
0.94
0.67
0.62
3.08
1.76
0.41
24
23
23
24
'24
23
24
23
23
24
24
24
23-
23
24
23
24
23
24
24
23
23
24
25
26
26
25
26
25
26
25
26
26
26
25
25
26
26
'26
25
26
26
25
26
25
26
25
27
28
27
28
27
28
28
27
27
27
28
28
28
28
27
day
night
night
day
day
night
day-
night
night ;.
day
day
day
night
night
day
night
day-
night
day
day
night
night
day-
night
day
day
night
day
night
day
night
day
day
day-
night
night
day
day
day
night
day
day
night
day-
night
day
night
night
day
night
day
night
day
day-
night
night
night
day
day
day
day
night
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
I
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-8
-------
050A
050A
050A
051A
051A
051A
051A
051A
051A
052A
05 2A
052A
052A
052A
052A
052A
053A
05 3A
053A
053A
053A
053A
054A
054A
054A
054A
054A
054A
055A
055A
05 5A
055A
055A
055A
056A
05 6A
056A
056A
056A
056A
057A
057A
057A
057A
057A
057A
05 7A
05 7A
057A
058A
058A
058A
058A
058A
05 8A
059A
059A
059A
059A
05 9A
05 9A
060A
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV.
LIV
OTH
BED
BED
BED
BED
DIN
DIN
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
.LIV
BED
BED
KIT
KIT
LIV
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
21.50
3.00
21.90
11.60
10.95
7.15
4.57
20.90
21.40
9.09
20.20
4.30
6.24
9.02
7.20
27 .20
6.11
27.20
28.20
6.12
4.30
7.80
19.90
-3.36
3.00
15.90
10.61
7.31
3.00
8.77
4.20
5.50
4.30
3.00
3.00
3.00
3.00
3.00
10.90
18.90
9.22
9.42
11.00
10.10
9.49
3.00
5.10
7.20
5.50
3.64
3.00
3.00
27.50
7.70
7.32
21.80
87.40
24.90
5.60
Void
Void
Void
11,320
11,320
11,320
9,480
9,480
9,480
9,480
9,480
9,480
5,220
5,220
5,220
5,220
5,220
5,220
5,220
8,876
8,876
8,876
8 , 876
8,876
8,876
14,622
14,622
14,622
14,622
14,622
14,622
7,052
7,052
7,052
7,052
7,052
7,052
9,548
9,548
9,548
9,548
9,548
9,548
12,860
12,860
12,860
12,860
12, -860
12,860
12,860
12,860
12,860
4,860
4,860
4,860
4,860
4,860
4,860
8,992
8,992
8,992
8,992
8,992
8,992
11,248
13.1
7.3
13.1
9.7
13.3
9.7
9.7
13.3
13.3
11.7
9.9
11.7
10.0
11.7
9.9
9.9
10.9
10.3
10.3
10.9
10.9
10.3
8.5
13.4
13.3
8.4
8.5
13.3
11.1
10.4
10.4
11.1
: io.4
7.2
11.8
10.1
11.4
10.1
11.4
10.0
10.9
11.9
11.9
10.9
11.9
11.9
10.9
10.9
10.9
9.4
13.0
12.9
13.0
9.4
9.4
11.1
9.4
9.4
11.1
9.4
11.1
10.6
0.44
1.76
0.43
0.54
0.79
0.87
1.37
0.41
0.40
1.53
0.58
3.24
1.90
1 . 31
1.63
0.28
1.17
0.28
0.27
1.18
1.09
0.94
0.37
1.39
1.56
0.46
0.89
1.22
2.96
1.08
2.12
1.12
1.87
2.29
2.59
2.30
2.59
2.28
0.64
0.40
0.82
0.74
0.69
0.69
0.73
2.32
2.41
2.35
3.07
4;65
4.11
4.10
0.28
0.83
0.87
0.35
0.07
0 . 30
1.41
27
28
27
28
27
28
28
27
27
29
30
29
30
29
30
30
29
30
30
29
29
30
30
29
29
30
30
29
29
30
30
29
30
30
50
49
50
49
50
49
32
31
31
32;
31
31
32
32
32
32
31
31
31
32
32
31
32
32
31
32
31
34
night
day
night
day
night
day
day
night
night
night
day
night
day
night
day
day
night
day
day
night
night
day
day
night
night
day
day
night
night
day
day
night
day
day
day
night
day
night
day
night
day
night
night
day
night
night
day
day
day
day
night
night
night
day
day
night ,
day
day
night
day
night
day
1
1
i
i
i
i
i
i
i
i
i
" i
i
i
i
i
i
i
i
i
: 1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-9
-------
060A
060A
060A
060A
060A
060A
060A
060A
061A
061A
061A
061A
061A
061A
061A
061A
062A
062A
062A
062A
062A
064A
064A
064A
064A
064A
064A
064A
064A
065A
065A
065A
065A
065A
065A
066A
066A
06 6A
066A
06 6A
066A
067A
067A
067A
067A
067A
067A
068A
068A
068A
068A
068A
069A
069A
069A
069A
069A
070A
070A
070A
070A
070A
BED
DEN
DEN
DEN
DEN
KIT
KIT
OTH
BED
BED
FAM
FAM
FAM
FAM
LIV
LIV
BED
BED
LIV
LIV
LIV
BED
BED
KIT
KIT
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
LIV
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
15.00
6.34
10.80
15.20
5.58
13.80
7.30
3.00
21.20
9.47
13.10
19.20
4.40
3.00- «
15.20
8.35
13.10
9.20
17.80
11.30
10.50
6.82
4.00
• 3.00 •
3.00
3.00
3.00 •
3.00
3.00
4.60
34.00
5.50
20.80
18.80
4.90.
3.00
13.80
3.00
11.70
3.00
15.40
•7.59
3.00
6.60
6.60
3.00
3.00
13.46
8.36
8.02
9.74
3.00
22.90
26.50
12.12
10.49
17.70
3.00
3.00
7.33
7.37
6.45
11,248
11,248
11 , 248
11,248
11,248
11,248
11,248
11,248
16 , 273
16,273
16,273
16,273
16,273
16,273
16,273
16,273
5 , 824
5,824
5 824
5,824
5,824
12,786
12,786
12,786
12,786
12,786
12,786
12,786
12,786
12,540
12,540
12 , 540
12 , 540
12 , 540
12 , 540
9,534
9 534
9,534
J
9,534
9,534
9,534
8,514
8,514
8,514
8,514
8,514
8,514
4,361
4 , 361
4,361
4,361
4,361
6,608
6,608
6^608
6,608
6,608
4^860
4,860
4,860
4 860
4,860
11.0
10.6
11.0
11.0
10.6
11.0
10.6
10.5
10.9
15.0
10.9
10.9
15.0
15.0
1 10.9
15.0
9.9
11.2
9.9 .
11.2
9.3
12.0 -
9.9
9.9
12.0
10.0
12 .0
12.0
10.0
9.5
12.1
9.4
12.1
12.1
12.1
11.9
9.8
11.9
9.8
11.9
9.8
10.7
10.2
10.2
10.7
10.7
10.2
11.0
10.7
10, 7
11.1
10.7
10,9
10.9
10.9
10.9
10.9
11.8
9.4
11.8
11.8
9.4
0.54
1.24
0 . 76
0.54
1.42
. 0.59
1.08
2.60
0.19
0.59
0.31
0.21
1.26
1.85
0.27
0.67
0 . 79
1.26
0.58
1.03
0.92
0.88
1.24
1,65
1.99
1.66
1.99
1.99
1.65
1.00
0.17
0,84
0.28
0 . 31
1.20
2.57
0.46
2.57
0.54
2,57
0.41
1.01
2.45
1.11
1.16
2.56
2.45
0.76
1.18
' 1.23
1.05
3.30
0.45
0.39
0.84
0.98
0.58
4.90
3.89
2.00
2.00
1.82
33 night
34 day
33 night
33 night
34 day
33 night
34 day
34 day
S3 night
34 day
33 night
33 night
34 day
34 day
33 night
34 day
36 day
35 night
36 day
35 night
35 night
35 night
36 day
36 day
35 night.
36 day
35 night
35 night
36 day
35 night
36 day
35 night
36 day
36 day.
36 day
35 night
36 day
35 night
36 day
35 night
36 day
37 night
38 day
38 day
37 night
37 night
38 day
37 night
38 day
38 day
37 night
38 day
37 night
38 day
37 night
37 night
38 day
37 night
' 38 day
37 night
37 night
38 day
1
1
1
1
1
1
1
1
1
1
1
1
1
L
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-10
-------
070A
070A
071A
071A
071A
071A
071A
073A
073A
073A
073A
073A
074A
074A
074A
074A
074A
074A
075A
075A
07 5A
075A
075A
075A
075A
075A
076A
07 6 A
076A
076A
07 6A
.076A
076A
077A
077A
077A
077A
077A
077A
078A
078A
078A
078A
078A
079A
079A
07 9A
079A
079A
079A
079A
08 OA
080A
080A
080A
08 2A
082A
082A
08 2A
082A
08 2A
08 3A
LIV
OTH
BED
BED
KIT
LIV
LIV
BED
BED
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
KIT
KIT
LIV
LIV
LIV
LIV
BED
BED
DEN-
DEN
DEN
DEN
DIN
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
BED
BED
DIN
LIV
LIV
LIV
OTH
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
OTH
BED
6.63
3.00
5.37
8.60
3.00
4.60
5.50
43.60
18.80
4.77
9.05
13.90
15.40
21.80-
7.84
13.70
15.90
11.79
14.10
12.60
15.50
13.50
9.22
16.20
12.70
61.30
16.90
3.00
11.60
3.00
11.50
14.10
11.50
21.00
10.50
4.42
3.83
10.10
26.50
17.90
23.90
29.00
18.10
12.80
26.40
7.05
9.75
26.40
9.35
3.00
15.00
13.70
15.40
12.30
8.40
9.30
4.45
7.20
3.00
3.00
8.83
Void
4,860
4,860
7 , 300
7,300
7,300
7,300
7,300
5,824
5 , 824
5,824
5,824
5,824
5,824
5,824
5,824
5,824
5,824
5,824
5,916
5,916
5,916
5,916
5,916
5,916
5,916
5,916
11,708
11,708
11,708
11,708
11,708
11,708
11,708
8,942
8,942
8 , 942
8,942
8,942
8,942
4,032
4,032
4,032
4,032
4,032
6 , 740
6 , 740
6,740
6,740
6,740
6,740
6,740
3,092
3,092
3,092
3,092
4,860
4,860
4,860
4,860
4,860
4,860
18,346
9.4
9.4
10.9
10.6
10.6
10.9
10.9
10.0
12.4
10.0
12.4
12.4
10.0
10.4
10.4
10.1
10.0
10.4
13.4
8.3
13.4
8.3
13.4
8.3
13.4
8.3
13.2
8.4
8.4
13.2
8.4
13.2
13.2
10.2
10.9
10.9
10.2
10.2
11.0
9.9
11.3
9.9
9.9
11.3
13.0
9.5
12.9
13.0
9.5
13.0
9.5
11.2
9.8
11.2
9.9
9.5
12.5
9.4
12.5
9.4
9.4
11.9
1.77
3.90
1.79
1.08
• 3.10
2.09
1.75
0.24
0.70
2.20
1.44
0.94
0.69
0.51
1.41
0.78
0.67
0.94
0.97
0.68
0.55
1.01
0,92
0.:84
0.67
0.12
0.27
1.50
0.61
1.50
0.61
0.50
0.60
0.35
0.70
1.55
1.80
0.73
0.60
1.01
0.67
0.55
1.01
0.94
0.34
1.71
1.24
0,33"
1.29
2.94
1.45
1.40
1.42
' 1.57
1.41
1.67
2.63
2.15
3.90
3.90
0.60
38
38
39
40
40
39
39
39
40
39
40
40
39
40
40
39
39
40
39
40
39
40
39
40
39
40
41
42
42
41
42
41
41
42
41
.41
42
42
41
58
57
58
58
57
41
42
41
41
42
41
42
43
44
43
44
44
43
44
43
44
44
43
day
day
night
day
day
night
night
night
day
night
day
day
night
day
day
night
night
day
night
day
night
day
night
day
night
day
night
day
day
night
day
night
night
day
night
night
day
day
night
day
night
day
day
night
night
day
night
night
day
night
day
night
day
night
day
day
night
day
night
day
day
night
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-ll
-------
083A BED
083A LIV
083A LIV
083A LIV
083A LIV
084A BED
084A BED
084A KIT
084A KIT
084A LIV
084A LIV
084A LIV
084A LIV
085A BED
085A BED
085A LIV
085A LIV
085A LIV
086A BED
086A BED
086A KIT
086A KIT
086A LIV
086A LIV
086A LIV
086A LIV
08 6A OTH
087A BED
087A BED
087A LIV
087A LIV
087A LIV
08 7A LIV
088A BED
088A BED
088A LIV
088A LIV
088A LIV
08 8A LIV
088A OTH
089A- BED
089A BED
089A LIV
089A LIV
089A LIV
089A LIV
090A BED
090A LIV
090A LIV
091A BED
091A BED
09 1A LIV
091A LIV
091A LIV
092A BED
092A BED
092A DEN
092A DEN
092A DEN
092A DEN
093A BED
093A BED
3.00
3.00
5.06
4.90
3.00
17.40
14.00
10.30
7.50
4.41
6.03
8.68
8.40
52.00
15.10
16.40
7.95
14.50
12.50
12.00
5.53
4.58
4.48
5.08
5.22
5.38
3.00
, 3.00
3.00
3.00
3.00
6.70
4.90
23.60
22.60
19.40
22.90
27.80
3.00
24.00
26.80
18.30
12.20
22.30
15.50
5.55
15.00
10.70
14.30
31.20
23.30
16.40
28.10
10.90
25.90
9.90
16.90
16.60
8.16
61.90
70.00
Void
18,346
18 , 346
18,346
18,346
18,346
8,560
8,560
8,560
8,560
8,560
8,560
8,560
8,560
8,640
8,640
8,640
8,640
8 , 640
12,212
12,212
12,212
12,212
12,212
12,212
12,212
12,212
12,212
8,056
8,056
8,056
8,056
8,056
8,056
8,692
8,692
8,692
8,692
8,692
8,692
8,692
10,930
10,930
10,930
10,930
10,930
10,930
5,760
5,760
5,760
4,032
4,032
4,032
4,032
4,032
13,164
13,164
13,164
13,164
13,164
13,164
7,228
7,228
9.4
9.4
11.9
9.4
11.9
10.7
10.9
10.9
10.7
10.7
10.7
10.9
10.9
10.3
,11.3
11,3
10.3
11.3
10.5
10.0
9.9
10.5
10.5
9.9
9.9
10.5
9.9
10.9
12.1
10.9
10.9
12.0
12.0
11.1
11.8
11.8
11. S
11.1
11.0
11.8
9.8
10.2
9.8
10.2
9.8
, 10.2
11.3
11.3
11.3
9.5
11.7
11.7
9.4
11.6
8.6
13.5
8.5
13.5
13.5
8.5
11.0
11.7
1.40
1.40
1.04
0.86
1.76
0.47
0.59
0.80
1.09
1.85
1.36
0.96
0.99
0.15
0.57
0.52
0.97
0.59
0.60
0.59
1,28
1.63
1.67
1.39
1.35
1.38
2.35
2,94
3.26
2.93
2.93
1.45
1.98
0.38
0.39
0.46
0.36
0,30
2.95
0.24
0.23
0.32
0.50
0.26
0.39
2.31
0.85
1.20
1.07
0.60
0.81
0.93
0,67
0.39
0.26
0.43
0.40
0.40
0.52
0.16
0.15
44
44
43
44
43
46
45
45
46
46
46
45
45
46
45
45
46
,45
45
46
46
45
45
46
46
45
46
45
46
45
45
46
46
47
48
48
48
47
47
.48
47
48
47
48
47
48
47
47
47
48
47
47
48
47
50
49
50
49
49
50
50
49
day
day
night
day
night
day
night
night
day
day
day
night
night
day
night
night
day
night
night
day
day
night
night
day
day
night
day
night
day
night
night
day
day
night
day
day
day
night
night
day
night
day
night
day
night
day
night
night
night
day
night
night
day
night
day
night
day
night
night
day
day
night
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-12
-------
09 3A LIV
093A LIV
09 3A LIV
093A LIV
093A OTH
094A BED
094A BED
094A KIT
094A LIV
094A LIV
094A LIV
094A LIV
09 5A BED
095A BED
095A FAM
095A FAM
09 5A FAM
095A FAM
09 6A BED
096A BED
09 6A KIT
09 6A LIV
09 6 A LIV
09 6A OTH
097A BED
09 7A BED
097A LIV
097A LIV
097A LIV
097A LIV
097A OTH
098A BED
09 8A BED
09 8 A LIV
09 8A LIV
098A LIV
09 8 A OTH
099A BED
099A BED
09-9A LIV
09 9A LIV
099A LIV
100A BED
100A BED
100A LIV
100A LIV
100A LIV
100A LIV
100A OTH
101A BED
10 1A BED
10 1A LIV
10 1A LIV
10 1A LIV
101A LIV
10 2A BED
102A BED
102A LIV
10 2A LIV
102A LIV
102A LIV
103A BED
55.80
48.70
43.60
56.90
3.00
45.50
8.10
3.00
5.23
4.70
7.12
4.74
9.60
13.70
8.70
14.10
15.00
8.70
9.12
14.00
3.00
3.00
5.10
28.90
22.70
13.30
18.90
23.30
11.90
6.20
12.60
4.60
6.85
6.20
3.15
4.60
3.00
9.04
8.37
3.00
3.00
18.70
20.10
16.30
20.60
15.10
17.70
3.00
11.80
23.60
3.00
5.50
23.80
25.50
54.80
37.00
43.00
29.20
47.60
29.10
13.10
Void
7,228
7,228
7,228
7,228
7,228
6,612
6,612
6,612
6,612
6,612
6,612
6,612
16,292
16,292
16,292
16,292
16,292
16,292
7,096
7,096
7,096
7,096
7,096
7,096
12,524
12,524
12,524
12,524
12,524
12,524
12,524
7,416
7,416
7,416
7,416
7,416
7,416
12,371
12,371
12,371
12,371
12,371
7,708
7,708
7,708
7,708
7,708
7,708
7,708
4,860
4,860
4,860
4,860
4,860
4,860
10,312
10,312
10,312
10,312
10,312
10,312
6,212
10.9
11.7
11.7
11.0
11.0
11.8
8.7
8.6
11.8
8.6
8.6
11.8
11: 9
11.0
11.8
11.0
11.0
11.8
9.1
10.9
9.1
10.9
10.9
11.0
10.9
12.8
10.9
" 12 . 8
12.8
10.9
12.8
11.9
8.4
11.9
8.5
8.5
8.5
8.8
12.2
12 . 3
8.9
8.8
10.5
9.7
10.5
9.7
9.7
10.5
10 .5
10.2
11.0
10.1
10.1
11.0
11.0
12.1
9.3
12.0
9.3
12.0
9.3
10.6
0.18
0.22
0.24
0.17
3.29
0.25
1.05
2.83
2.22
1.81
1.19
2.45
0.66
0.43
0.72
0.42
0.39
0.72
1.07
0.58
3.26
3.26
1.92
0.20
0.29
0.43
0.35
0.29
0.48
1.08
0.81
1.57
1.49
1.17
2.30
1.58
1.55
0.71
0.77
1.56
1.55
0.48
0.41
0.55
0.40
0.54
0.50
2.97
1.16
0.62
4.52
2.47
0.62
0.58
0.14
0.16
0.18
0.20
0.16
0.20
0.85
50
49
49
50
50
49
50
50
49
50
50
49
51
52
51
52
52
51
51
52
51
52
52
52
51
52
51
52
52
51
52
51
52
51
52
52
52
54
53
53
54
54
54
53
54
53
53
54
54
54
53
54
54
53
53
54
53
54
53
54
53
56
day
night
night
day
day
night
day
day
night
day
day
night
night
day
night
day
day
night
night
day
night
day
day
day
night
day
night
day
day
night
day
night
day
night
day
day
day
day
night
night
day
day
. day
night
day
night
night
day
day
day
night
day
day
night
night
day
.night •
day
night
day
night
day
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-13
-------
103A
103A
103A
103A
103A
104A
104A
104A
104A
104A
104A
105A
105A
105A
105A
105A
105A
106A
106A
106A
106A
106A
106A
107A
107A
107A
107A
107A
107A
108A
108A
108A
108A
108A
108A
109A
109A
109A
109A
109A
109A
111A
111A
111A
111A
111A
111A
112A
112A
112A
112A
112A
112A
112A
112A
112A
113A
113A
113A
113A
113A
113A
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
FAM
FAM
FAM
OTH
BED
BED
DEN
DEN
DEN
DEN
BED
BED
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
BED
BED
KIT
KIT
LIV
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
17.50
18.80
8.64
18.10
9.59
3.00 <
23.50
24.80
3.00 <
22.30
3.00 <
19.30
8.53
14.50
14.10
6.80 <
5.50 <
18.20
14.60
4.51
12.80
5.66
11.80
12.20
3.00 <
17.40
19.20
3.00 <
3.00 <
15.00
20.60
11.70
17.00
19.70
10.80
27.60
29.90
3.00 <
9.87
8.44
6.80 <
41.00
30.30
25.30
31.00
32.30
31.30
27.40
4.48
47.10
11.30
36.80
6.58
32.80
8.33
3.00
18.90
30.10
7.53
8.12
12.20
12.20
6,212
6,212
6,212
6,212
6,212
6,180
6,180
6,180
6,180
6,180
6,180
10,484
10,484
10,484
10,484
10,484
10,484
13,115
13,115
13,115
13 , 115
13 , 115
13,115
12,498
12,498
12,498
12,498
12,498
12,498
8,250
8,250
8,250
8,250
8,250
8,250
12,728
12,728
12,728
12,728
12,728
12,728
7,209
7,209
7,209
7,209
7,209
7,209
5,956
5,956
5,956
5,956
5,956
5,956
5,956
5,956
5,956
14,298
14,298
14,298
14,298
14,298
14,298
12.2
11.9
10.6
11.9
10.6
8.3
11.9
11.9
8.3
11.9
8.3
11.5
9.9
11.5
11.5
9.9 .
9.9
13.5
8.4
8.4
13.5
8.4
13.5
12.3
10.3
12.3
12.3
10.3
10.3
8.6
11.7
8.6
11.7
11.7
8.6
9.9
11.8
9.9
11.8
11.8
9.9
9.7
11.7
11.7
9.6
9.7
11.7
12.0
10.8
12.0
10.9
12.0
10.9
12.0
10.9
12.0
8.4
11.9
11.9
11.9
8.4
8.4
0.73
0.67
1.28
0.69
1.15
2.91
0.53
0.50
2:90
0.56
2.90
0.37
0.72
0.49
0.50
-0.90
1.12
0.37
0.29
0.92
0.52
0.74
0.57
0.53
1.78
0.37
0.33
1.79
1.79
0.45
0.45
0.58
0.54
0.47
0.63
0.18
0.20
1.69
0.61
0.72
0.75
0.21
0.35
0.42
0.28
0.27
0.34
0.48
2.64
0.28
1.05
0.36
1.80
0.40
1.42
4.37
0.20
0.18
0.72
0.67
0.31
0.31
55
55
56
55
56
56
55
55
56
55
56
55
56
55
55
56
56
55
56
56
55
56
55
57
58
57
57
58
58
58
57
58
57
57
58
58
57
58
57
57
58
60
59
59
60
60
59
60
59
60
59
60
59
60
59
60
60
59
59
59
60
60
night
night
day
night
day
day
night
night
day
night
day
night
day
night
night
day
day
night
day
day
night
day
night
night
day
night
night
day
day
day
night
day
night
night
day
day
night
day
night
night
day
day
night
night
day
day
night
day
night
day
night
day
night
day
night
day
day
night
night
night
day
day
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-14
-------
113A
114A
114A
114A
114A
114A
114A
115A
115A
115A
115A
115A
116A
116A
116A
116A
116A
118A
118A
118A
118A
118A
118A
118A
118A
118A
119A
119A
119A
119A
119A
119A
120A
120A
120A
120A
120A
120A
121A
•121A
121 A
12 1A
121A
121A
122A
12 2A
122A
122A
12 2A
123A
12 3A
123A
123A
12 3 A
123A
124A
124A
124A
124A
124A
124A
125A
OTH
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
BED
BED
KIT
KIT'
LIV
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
BED
3.00
8.43
9.30
3.00
8.28
8.60
7.40
17.60
36.90
32.00
13.20
35.10
12.60
11 . 80
12.17
5.43
5.99
19.40
49.30
22.40
37.60
18.10
13.80
44.20
42.50
3.00
23.70
26.70
8.43
12.00
16.30
10.74
6.52
3.00
3.00
3.96
4.19
6.20
20.70
15.60
14.50
12.68
16.90
4.30
13.00
15.50
14.30
12.10
13.00
7.70
6.01
3.09
3.47
9.32
3.00
10.50
3.00
5.34
6.73
6.85
4.44
13.20
14,298
5,328
5,328
5,328
5,328
5,328
5,328
10,253
10,253
10,253
10,253
10,253
4,864
4,864
4,864
4,864
4,864
9,564
9,564
9,564
9,564
9,564
9,564
9,564
9,564
9,564
13,811
13,811
13,811
13,811
13,811
13,811
13,602
13,602
13,602
13,602
13 , 602
13,602
6,909
6,909
6,909
6,909
6,909
6,909
8,074
8,074
8,074
8,074
8,074
4,784
4,784
4,784
4,784
4,784
4,784
5,916
5,916 ,
5 , 916
5,916
5,916
5,916
9,338
8.4
9.8
11.7
11.7
9.8
9.8
11.7
9.1
12.0
12.0
9.1
12.0
9.9
11.6
11.6
9.9
9.9
9.5
11 . 0
9.5
11.0
9.5
9.5
10 . 9
11.0
11.0
10.6
11.4
11.4
10.5
10.5
11.4
10.9
10.5
10.9
-. 10.4
10.4
10.9
13.3
11.9
11.9
13.3
11.8
11.9
8.7
12.0
11.9
8.7
8.7
11.7
11.1
11 .0
11.1
11.7
11.7
12.0
8.8
8.8
12.0
12.0
8.8
11.0
1.27
1.43
1.54
4.77
1.45
1.40
1.93
0.33
0.21
0.24
0.44
0.22
1.05
1 . 32
1.28
2.44
2.21
0.33
0.15
0.29
.0.20
0.36
0.47
0.17
0.18
2.49
0.21
0.20
0.64
0.41
0.30
0.50
- 0 . 80
1.67
1.74
1.26
1.19
0.84
0.61
0.72
0.77
0.99
0.66
2.60
0.54
0.62
0.67
0.58
0.54
2.06
2.50
4.86
4.34
1.71
5.31
1.26
3.24
1.82
1.96
1.93
2.18
0.58
60
62
61
61
62
62
61
61
62
62
61
62
62
61
61
62
62
63
64
63
64
63
63
64
64
64
64
63
63
64
64
63
63
64
63
64
64
63
65
66
66
65
66
66
65
66
66
65
65
66
65
65
65
66
66
65
66
66
65
65
66
68
day
day
night
night
day
day
night
night
day
day
night
day
day
night
night
day ,
day
night
day
night
day
night
night
day
day
day
day
night
night
day
day
night
night
day
night
day
day
night
night
day
day
night
day
day
night
day
day
night
night
day
night
night
night
day
day
night
day
day
night
night
day
day
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
'l
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-15
-------
125A
125A
125A
125A
125A
125A
127A
127A
127A
127A
127A
127A
128A
128A
128A
128A
128A
128A
128A
128A
129A
129A
129A
129A
129A
129A
130A
130A
130A
130A
130A
130A
131A
13 1A
13IA
131A
131A
131A
132A
132A
• 132A
'132A
132A
132A
133A
133A
133A
133A
133A
133A
133A
134A
134A
134A
134A
134A
134A
134A
134A
135A
135A
135A
BED
LIV
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
BED
BED
KIT
KIT
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
OTH
BED
BED
KIT
KIT
LIV
LIV
LIV
LIV
BED
BED
FAM
11.90
8.40
8.92
10.90
12,60
6.60
4.74
11.20'
3.00.
3.00
8.08
9.43
4.13
6.06
3,00
5.64
6.05
3.00
3.00
11.60
7.06
6.47
10.70
10.60
7.17
16.80
12.10
16.20
8.70
8.90
10.90
46.40
57.00
48.40
42.50
54.10
6.70
3.00
7.84
9.48
9.80
6.27
7.95
5.72
3.00
3.23
3.00
3.00
3.00
3.00
20.30
7.90
17,50
5,77
16.90
14.00
6.31
3.00
74.50
65.50
Void
Void
9,338
J
9,338
9,338
9,338
9,338
9,338
8,846
8r846
8,846
8,846
8,846
8 , 846
16,419
16r419
16,419
16,419
16,419
16 ,419
16,419
16 ,419
9,420
9,420
9,420
9,420
9,420
9,420
11,604
11,604
11,604
11,604
11,604
11,604
12,288
12,288
12,288
12,288
12,288
12,288
11,208
11,208
11,208
11,208
11,208
11,208
4,488
4,488
4,488
4,488
4,488
4,488
4,488
6,848
)
6,848
6,848
6,848
6 , 848
6,848
6,848
6,848
10,528
10,528
10,528
11.2
11.3
11.2
11.0
11.0
11.0
10.0
11.7
10.0
10,0
11.8
11.8
11.0
11.5
11.5
11.0
11.5
11.5
11.0
11.0
13.4 .
8.4
8.4
13.4
13.4
8.4
10.5
10.9
10,5
10.9
10.9
10.5
9.9
11.8
11.8
9,8
11.8
9,8
11.4
9.8
9.9
9.9
11.4
11:4
13,2
8.3
13.1
8.3
13.2
8.3
8.3
13.2
10.3
13.2
10,4
10.3
13,2
13.2
10.4
8,3
14.4
14.5
0,66
0.93
0.88
0.71
0.61
1,17
1.55
0.77
2.45
2.45
1.07
0,92
1.41
1.00
1.94
1.07
1.00
1.94
1.94
1.06
1.10
1.20
1.15
1.16
1.09
0.35
0.50
0,36
0.70
0.69
0.54
0.15
0.15
0.17
0.16
0,15
1.04
2.21
0.73
0,60
0,58
1.05
0.83
3.34
4.02
5.91
4.01
6.37
4.02
4.01
0.82
1.66
0.96
2,27
0.99
1.20
2.08
2.27
0.16
0.18
67
67
67
68
68
68
68
67
68
68
67
67
67
68
68
67
68
68
67
67
69
70^
70
69
69
70
70
69
70
69
69
70
70
69
69
70
69
70
69
70
70
70
69
69
71
72
71
72
71
72
72
71
72
71
72
72
71
71
72
72
71
71
night
night
night
day
day
day
day
night
day
day
night
night
night
day
day
night
day
day
night
night
night
day
day
night
night
day
day
night
day
nigrit
night
day
day
night
night
day
night
day
night
day
day
day
night
night
night
day
night
day
night
day
day
night
day
night
day
day
night
night
day
day
night
night
1
1
1
I
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-16
-------
13 5 A FAM
135A FAM
13 5A FAM
13 5A KIT
135A KIT
13 5A OTH
13 6 A BED
136A BED
13 6 A LIV
13 6 A LIV
136A LIV
137A BED
137A BED
137A FAM
137A FAM
137A FAM
13 7A FAM
13 7A KIT
13 7A KIT
138A BED
13 8 A BED
13 8A LIV
138A LIV
138A LIV
13 8 A LIV
138A OTH
139A BED
13 9 A BED
13 9A LIV
13 9 A LIV
139 A LIV
139A OTH
140A BED
140A BED
140A LIV
140A LIV
140A LIV
141A BED
141A BED
141A KIT
141A KIT
141A LIV
14 1A LIV
141A LIV
141A LIV
142A BED
142A BED
142A LIV
142A LIV
142A LIV
142A LIV
143A BED
USA BED
143A LIV
143A LIV
143A LIV
143A LIV
143A OTH
144A BED
144A BED
144A LIV
144A LIV
20.20
22.60
• 63.20
61.90
24.00
3.00
5.63
13.70
3.00
9.80
13.00
12.10
24.90
31.00
32.30
28.60
31.70
26.40
31.00
4.30
13.37
7.20
5.50
5.50
4.30
3.00
8.50
5.35
25.00
26.80
24.70
3.00
34.00
22.70
20.60
23.00
14.30
54.30
3.00
44.30
55.50
3.00
58.00
3.00
3.00
3.00
9.69
3.00
3.00
9.00
13.90
8.20
11.50
19 . 70
19.50
10.30
3.00 •
6.15
6.70 •
3.00 •
4.94
Void
10,528
10,528
10,528
10,528
10,528
10,528
6,909
6,909
6,909
6,909
6,909
9,122
9,122
9,122
9,122
9,122
9,122
9,122
9,122
7,740
7,740
7,740
7,740
7,740
7,740
7,740
6,664
6,664
6,664
6,664
6,664
6,664
10,270
10,270
10,270
10,270
10,270
6,832
6,832
6,832
6,832
6,832
6,832
6,832
6,832
6 , 944
6,944
6 , 944
6 , 944
6,944
6 , 944
9,680
9,680
9,680
9,680
9,680
9,680
9,680
13,509
13,509
13,509
13,509
8.3
8.3
14.4
14.4
8.3
8.2
10.4 :
11.8
10 . 3 '
11.8
11.8
11.9
11.0
11.9
11.0
11.0
11 .9
11.0
11.9
9.9
10.8
9.8
10.8
9.9
10.8
10.8
10.5
12.2
10.6
12.2
10 . 6
10.5
10.5
9.5
9.5
9.5
10.5
9.4
12.0
9.4
12.0
12.0
9.4
12.0
9.5
9.5
12.4
12 .4
9.5
9.5
12.4
12.4
9.4
9.4
12.5
12.5
9.4
9.4
12.4
9.0
9,0
12.4
0.34
0.30
0.19
0.19
0.28
2.25
1.74
0.81
3.23
1 . 14
0.86
0.70
0.31
0.27
0.24
0.27
0.27
0.30
0.27
1.93
0.68
1.15
1.65
1.51
2.11
3.02
1.21
2.23
0.41
0.45
0.42
3.44
0.26
0.35
0.39
0.35
0.62
0.21
3.00
0 . 26
0.21
3.00
0.20
3.01
2.97
3,88
1.20
2.97
2.96
1.29
0.60
0.77
0.55
0.43
0.43
0.61
2.11
1.29
0.86
1.92
1.61
72 day
72 day
71 night
71 night
72 day
72 day
72 day
71 night
72 day
71 night
71 night
73 night
74 day
73 night
74 day
74 day
73 night
74 day
73 night
73 night
74 day
73 night
74 day
73 night
74 day
74 day
74 day
73 night
74 day
73 night
74 day
74 day
74 .day
73 night
73 night
73 night
74 day
76 day
75 night
76 day
75 night
75 night
76 day
75 night
76 day
76 day
75 night
75 night
76 day
76 day
75 night
75 night
76 day
76 day
75 night
75 night
76 day
76 day
75 night
76 day
76 day
75 night
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-17
-------
144A LIV
USA BED
USA BED
USA LIV
USA LIV
USA LIV
USA LIV
146A BED
U6A BED
146A DIN
146A DIN
146A KIT
USA BED
USA BED
USA LIV
USA LIV
USA LIV
USA OTH
U9A BED
149A BED
149A LIV
149A LIV
149A LIV
U9A OTH
151A BED
151A BED
151A FAM
151A FAM
151A FAM
151A FAM
151A KIT
151A KIT
152A BED
152A BED
152A LIV
152A LIV
152A LIV
152A LIV
152A OTH
153A BED
15 3 A BED
153A OTH
154A BED
154A BED
154A FAM
154A FAM
154A FAM
154A FAM
154A KIT
154A KIT
155A BED
155A BED
155A FAM
155A FAM
155A FAM
155A FAM
155A KIT
155A KIT
155A OTH
15 6A BED
156A BED
156A FAM
3.00
12.40
3.38
12.70
15.00
24.00
11.50
6.70
4.28
19.90
24.80
3.00
3.00
3.00
5.72
4.17
3.61
3.00
6.19
3.00
7.72
9.43
17.20
3.00
15.90
5.32
3.34
3.66
14.20
14.60
13.60
3.93
34.20
18.40
30.50
22.90
33.50
22.10
3.00
23.10
26.10
3.00
3.64
6.04
4.30
5.82
5.99
3.95
3.53
3.00
11.60
16.20
5.39
5.25
8.99
10.60
7.46
3.00
9.19
14.70
12.81
Void
13,509
8,200
8,200
8,200
8,200
8,200
8,200
8,200
8,200
8,200
8,200
8,200
8,928
8,928
8,928
8,928
8,928
8,928
6,350
6,350
6,350
6,350
6,350
6,350
17,654
17,654
17,654
17,654
17,654
17,654
17,654
17,654
10,129
10,129
10,129
10,129
10,129
10,129
10,129
1,664
1,664
1,664
15,696
15,696
15,696
15,696
15,696
15,696
15,696
15,696
13 , 134
13,134
13,134
13,134
13,134
13,134
13,134
13,134
13,134
15,627
15,627
15,627
9.0
8.8
12.0
8.8
12.0
12.0
8.8
12.5
10.3
12.5
12.5
10.3
9.4
11.8
9.4
11.8
11.8
9.4
9.9
11.4
9.9
9.9
11.4
9.9
12.0
8.5
8.5
8.5
12.0
12.0
12.0
8.5
13.9
9.0
13.9
9.0
13.9
9.0
13.9
12.3
8.9
9,0
8.9
12.9
8.9
12.9
12.9
8.9
12.9
8.9
9.2
12.0
12.0
9.2
9.2
12.0
12.0
9.2
9.2
11.4
12.9
11.4
1.92
0.56
2.82
0.55
0.64
0.40
0.61
1.48
1.91
0.50
0.40
2.73
2.29
2.86
1.20
2.06
2.38
2.29
1.64
3.91
1.32
1.08
0.68
3.39
0.37
0.78
1.24
1.14
0.41
0.40
0.43
1.06
0.35
0.42
0.39
0.34
0.36
0.35
3.98
0.69
0.45
3.89
1.35
1.18
1.14
1.23
1.19
1.24
2.02
1.64
0.39
0.37
0.85
0.87
0.66
0.56
0.61
1.52
0.69
0.49
0.49
76
78
77
78
77
77
78
77
78
77
77
78
78
77
78
77
77
78
80
79
80
80
79
80
79
80
80
80
79
79
79
80
80
79
80
79
80
79
80
81
82
82
82
81
82
81
81
82
81
82
82
81
81
82
82
81
81
82
82
82
81
82
day
day
night
day
night
night
day
night
day
night
night
day
day
night
day
night
night
day
day
night
day
day
night
day
night
day
day
day
night
night
night
day
day
night
day
night
day
night
day
night
day
day
day
night
day
night
night
day
night
day
day
night
night
day
day
night
night
day
day
day
night
day
' 1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1.
1
1
1
1
1
1
1
1
1
D-18
-------
156A FAM
15 6A FAM
15 7A BED
15 7A LIV
15 7A LIV
157A LIV
15 7 A LIV
15 8A BED
15 8A BED
15 8A BED
158A BED
15 8 A BED
15 8A OTH
15 9A BED
159A BED
159A LIV
15 9A LIV
15 9A LIV
160A BED
160A BED
160A FAM
160A FAM
160A FAM
160A FAM
160A OTH
16 1A BED
161A BED
161A DEN
16 1A DEN
161A DEN
16 1A OTH
162A BED
16 2 A BED
16 2 A LIV
16 2A LIV
162A LIV
163A BED
16 3A BED
16 3 A LIV
16 3 A LIV
163A LIV
16 3A OTH
164A' BED
164A BED
164A KIT
164A KIT
164A LIV
164A LIV
164A LIV
164A LIV
16 6 A BED
166A BED
16 6A LIV
166A LIV
16 6 A LIV
166A LIV
16 6 A OTH
167A BED
16 7A BED
167A LIV
167A LIV
16 7A LIV
16.50
12.74
4.35
18.60
4.90 <
3.00 <
17.00
7.63
9.20
11.10
5.45
15.00
3.00 <
14.40
30.20
20.70
11.13
20.00
6.68
3.00 <
13.50
3.46
4.30
11.50
3.00 <
7.94'
9.43
9.35
7.99
14.80
3.00 <
29.60
27.30
22.40
19.70
23.30
11.80 loose
37.40
30.70
16.20
36.30
3.00 <
4.73
6.83
15.00
Void
4.22
3.51
Void
Void
34.60
30.60
41.00
37.70
36.20
41.20
3.00 <
27.90
30.60
9.29
3.13
3.15
15,627
15,627
8,200
8,200
8,200
8 , 200
8,200
15,192
15,192
15,192
15 ; 192
15,192
15,192
4,032
4,032
4,032
4,032
4,032
13,509
13,509
13,509
13,509
13,509
13,509
13,509
13 , 201
13,201
13,201
13,201
13,201
13,201
12,860
12,860
12,860
12,860
12,860
6,664
6,664
6,664
6,664
6,664
6,664
8,089
8,089
8,089
8,089
8,089
8,089
8,089
8,089
8,992
8,992
8,992
8,992
8,992
8,992
8,992
8,908
8,908
8,908
8,908
8,908
12.9
11.4
8.4
13 . 5
8.4
8.4
13.5
11.3
10.1
11.3
11.3
10.1
10.1
12.3
10.5
10.5
12.3
10.6
11.6 .
8.7
11.6
8.8
8.8
11.5
8.8
10.7
9.5
9.4
9.5
10.7
9.5
13.4
9.6
9.6
. 9.6
13.4
10.7
12.2
12.2
10.7
12.2
10.7
9.1
11.1
11.1
9.0
9.1
9.1
11.1
11.1
10.9
10.6
10.9
10.6
10.9
10.6
10.9
10.0
11.3
11.3
10.0
10.0
0.43
0.50
1.54
0.57
1.36
2.23
0.63
0.63
0.47
0.44
0.89
0.29
1.44
0.92
0.38
0.55
1.18
0.57
0.83
1.40
0.41
1.22
0.98
0.48
1.41
0.88
0.66
0.66
0.78
0.47
2.08
0.31
0.24
0.29
0.33
0.39
0.89
0.32
0.39
0.65
0.33
3.49
1.55
1.31
0.60
1.73
2.08
0.23
0.25
0.19
0.20
0.22
0.19
2.63
0.35
0.36
1.19
3.11
3.08
81
82
84
83
84
84
83
83
84
83
83
84
84
83
84
84
83
84
83
84
83
84
84
83
84
85
86
86
86
85
86
85
86
86
86
85
86
85
85
86
85
86
86
85
85
86
86
86
85
85
88
87
88
87
88
87
88
88
87
87
88
88
night
day
day
night
day
day
night
night
day
night
night
day
j •>
day
night
O
day
day
night
day
night
day
night
O
day
, J
day
night
day
night
day
^ J
day
day
night
day
night
day
, J
day
j J
day
night
day
night
night
day
night
day
day
night
night
day
v*o.jr
day
day
night
night
day
night
day
night
O
day
night
day
day-
night
night
day
day
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1 .
1
D-19
-------
167A LIV
167A OTH
168A BED
168A BED
168A LIV
168A LIV
168A LIV
169A BED
169A BED
169A LIV
169A LIV
169A LIV
169A LIV
170A BED
170A BED
170A KIT
170A KIT
170A LIV
170A LIV
170A LIV
170A LIV
170A OTH-
171A BED,
171A BED"
171A LIV
171A LIV
171A LIV
171A LIV
172A BED
172A BED
172A LIV
172A LIV
172A LIV
173A BED
173A BED
17 3A KIT
173A KIT
173A LIV
173A LIV
173A LIV
173A LIV
173A OTH
174A BED
174A BED
174A LIV
174A LIV
175A BED
175A BED
175A LIV
175A LIV
175A LIV
175A LIV
175A OTH
176A BED
176A BED
176A LIV
176A LIV
176A LIV
176A LIV
177A BED
177A BED
177A LIV
8.52
5.50 <
16.20
27.70
12.60
24.00
8.70
4.25
14.60
5.09
4.79
24.00
21.00
8.97
17.60
13.20
4.51
12.80
3.70
15.00
4.34
3.00
4.96
5.50 <
13.30
13.70
10.60
10.30
37.20
13.90
7.84
3.98
34.60
25.30
3.00
19.30
25.60
24.40
26.10
21.00
23.10
3.00 <
13.90
11.69
9.99
3.94
5.54
3.32
3.81
8.93
3.89
8.42
3.00 <
3.00 <
16.90
5.68
14.50
3.40
13.20
17.80
13.00
17.50
8,908
8 908
7,708
7,708
7,708
7,708
7,708
8,330
8,330
8,330
8,330
8,330
8,330
8,722
8,722
8,722
8,722
8,722
8,722
8,722
8,722
8,722
5,760
5,760
5,760
5,760
5,760
5,760
4,860
4,860
4,860
4,860
4,860
5,586
5,586
5,586
5,586
5,586
5,586
5,586
5,586
5,586
5,104
5,104
5,104 '
5,104
6,248
6,248
6,248
6,248
6,248
6,248
6 , 248
3,900
3,900
3,900
3,900
3,900
3,900
10,201
10,201
10,201
11.3
9.9
9.5
12,0
9.5
12.0
9.5
8.9
11.6
8.9
8.9
11.6
11.6
10.8
11.9
11.9
10.8
11.9
10.8
11.9
10.8
10.8
12.0
9.4
9.4
9.4
12.0
12.0
13.4
8.5
8.6
8.6
13.4
12.0
9.6
12.0
9,6
12.0
9.6
12.0
9.6
12.0
9.3
12.7
9.3
9.3
11.3
10.8
10.8
11.3
10.8
11.3
10.8
9.6
9.8
9.6
9.9
9.6
9.9
9.4
11.8
11.9
1.29
1.76
0.50
0.37
0.64
0.42
0.92
1.64
0.62
1.37
1.45
0.38
0.43
1.20
0.67
0.90
2.38
0.93
2.91
0.79
2.47
3.58
2.72
1.94
0.80
0.77
1.27
1.31
0.48
0.82
1.46
2.88
0.52
0.55
3.72
0.72
0.44
0.57
0.43
0.67
0.48
4.65
0.85
1.38
1.19
3.00
2.13
3.38
2.94
1.32
2.88
1.40
3.74
3.56
0.65
1.88
0.76
3.14
0.83
0.34
0.58
0.43
87
88
87
88
87
88
87
90
89
90
90
89
89
90
89
89
90
89
90
89
90
90
90
89
89
89
90
90
89
90
90
90
89
92
91
92
91
92
91
92
91
92
91
92
91
91
91
92
92
91
92
91
92
92
91
92
91
92
91
94
93
93
night
day
night
day
night
day
night
day
night
day
day
night
night
day
night
night
day
night
day
night
day
day
day
night
night
night
day
day
night
day
day
day
night
day
night
day
night
day
night
day
night
day
night
day
night
night
night
day
day
•night
day
night
day
day
night
day
night
day
night
day
night
night
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
D-20
-------
177A
177A
178A
178A
178A
178A
178A
178A
179A
179A
179A
179A
179A
17 9A
17 9A
180A
180A
180A
180A
180A
180A
181A
181A
181A
18 1A
181A
181A
182A
182A
182A
182A
182A
18 2 A
182A
183A
183A
183A
183A
183A
183A
.184A
184A
184A
184A
184A
184A
???
LIV
LIV
BED
BED
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
BED
BED
LIV
'LIV
LIV
LIV
BED
BED
LIV
LIV
LIV
LIV
OTH
BED
BED
LIV
LIV
LIV
LIV
.BED
BED
LIV
LIV
LIV
LIV
???
20.20
18.70
14.60
27.00
17.10
23.10
18.80
6.60
29.30
15.40
30.40
23.50
31.60
23.00
3.00
7.21
8.64
5.20
3.00
3.00
5.88
16.10
22.40
19.50
17.60
16.90
16.10
3.00
3.00
2.05
3.00
8.22
8.30
3.00
29.10
30.00
29.10
36.10
21.50
27.40
15.40
20.30
19.40
4.60
18.80
Void
Void
10,201
10,201
7,526
7,526
7,526
7,526
7,526
7,526
7,961
7,961
7,961
7,961
7,961
7,961
7,961
10,886
10,886
10,886
10,886
10,886
10,886
6,832
6,832
6,832
6,832
6,832
6,832
7,252
7,252
7,252
7,252
7,252
7,252
7,252
4,032
4,032
4,032
4,032
4,032
4,032
6,048
6,048
6,048
6,048
6,048
6,048
9.4
11.9
10.6
10.9
10.6
10.9
10.9
10.8
11.4
9.9
11.4
9.9
11.4
9.9
11.4
9.0
12.8
9.0
12.8
9.0
12.8
11.6
10.5
10.5
11.6
10.5
11.6
9.8
11.4
11.4
11.4
9.8
9.8
11.4
13.4
8.6
8.6
8.6
13.4
13.4
10.6
10.6
10.6
10.6
10.6
10.6
0.30
0.40
0.63
0.35
0.53
0.41
0.50
1.42
0.32
0.53
0.31
0.35
0.30
0.35
3.10
0.75
0.88
1.04
2.54
1.79
1.30
0.69
0.44
0.51 :
0.63
0.59
0.69
2.92
3.42
5.00
3.42
1.07
1.06
3.42
0.50
0.31
0.32
0.26
0.67
0.53
0.74
0.56
0.59
2.48
94
93
93
94
93
94
94
94
94
93
94
93
94
93
94
94
93
94
93
94
93
96
95
95
96
95
96
95
96
96
96
95
95
96
95
96
96
96
95
95
95
96
95
95
96
96
day
night
night
day
night
day
day
day
day
night
day
night
day
night
day
day
night
day
night
day
night
day
night
night
day
night
day
night
day
day
day
night
night
day
night
day •
day
day
night
night
night
day
night
night
day
day
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
1
AER - (n * S)/(V * C)
S = E * lE+6ug/g * 24.5uL/350ug * !E+6pL/uL
D-21
-------
-------
APPENDIX E
NICOTINE DATA
E-l
-------
Explanation of Headings in Appendix E
NICID
FLTII>
BID
LOC
PER
UP
VOL
MASS
CONC
ND;
LAB
FLAG-
AWCOK
Nicotine filter identification number
Particle filter identification number
Personal identification number
Location o£ monitor:
PER ~ participant
LI^T =* living? room
BED - bedroom
EAK — family room'
Period: Day and time ofT day of monitoring;.
1 = overnightr Sept. 22-23, 19&&
9 & = daytime; Nov^ ^ 19 ^0;
DupJLlcates H - duplicate monitor
\fbltune eollectedl (liters^
Mass of nicotine collected £ng;]f
Concentration ([ng/E or fi^/T^l
Not detected?
blanlc = measurable
ND- = not detected
Laboratory wftere analysis toolc place.
There were two main laboratories at the
Harvard School of Public Healthi ("old
and li;newir) ; the quality assurance lab
was at the University of Massachusetts
at Amherst CKathy Hammond)
Flag? for gusli ty of
no, proMems
below' detection limit
If duplicates were collected^ the average o€ the
two values is listed, here
E-2
-------
NICID
N7006
N7002
N7001
N7005
N7007
N7003
N7021
N7022
N7008
N7004
N7027
N7018
N7009
N7010
N7028
N7017
N7020
N7019
N7029
N7025
N7024
N7023
N7030
N7026
N7031
N7032
N7050
N703S
N7036
N70S1
N7034
N7039
N7048
N7047
N7040
N7033
N7045
N7046
N7049
N7044
N7076
N7053
N7054
N7069
N7068
N70S7
N707S
FLTID
F4651
F4745
F4693
F4643
F4748
F4656
F4690
F4642
F4747
F4598
F4595
F4591
F4692
F4S71
F4645
F4647
F4740
F4640
F4649
F4599
F4737
F4650
F4648
F4623
F4717
F4710
F46S5
F4652
F471S
F4677
F4712
F4772
F4767
F4684
F4718
F4682
F4756
F4773
F4803
F4679
F4734
F4674
F4805
F4636
F4S60
F4618
F4631
PID
001 A
001A
001 A
001A
002A
002A
002A
002A
003A
003A
003A
003A
004A
004A
004A
004 A
005A
005A
005A
005A
006A
006A
006A
006A
007A
007A
007A
008A
008 A
008A
009A
009A
009A
009A
010A
010A
010A
010A
011A
011A
011 A
012A
012A
012A
012A
013A
013A
LOG
PAR
LIV
PAR
UV
FAM
PAR .
PAR
FAM
LIV
PAR
PAR
LIV
PAR
LIV
PAR
LIV
LIV
PAR
LIV
PAR .
PAR
UV
LIV
PAR
PAR
LIV
PAR
LIV
PAR
PAR
LIV
PAR
LIV
PAR
PAR
LIV
PAR
LIV
PAR
LIV
PAR
PAR
OEN
DEN
PAR
PAR
FAM
PER UP L
1
1
2
2
1
1
2
2
3
3
4
4
3
3
4
4
3
3
4
4
3
3
4
4
5
5
6
5
5
6
S
5
6
6
5
5
6
6
7
.7
8
7.
7
8
8
9
10
1
- 2
1
2
2
1
1
2
2
1
, 1
2
1
2
1
2
2
1
2
1
1
2
2
1
1
2
1
2
1
1
2
1
2
1
1
2
1
2
1
2
1
1
2
2 -•
1
1
2
VOL MASS CONG ND
1.763
3.102
1.826
1.954
2.554
2.458
2.322
, 2.264
3.077
3.135
2.227
2.263
2.535
2.602
2.447
. 2.578
2.678
2.625
2.272
2.426
2.759
1.767
2.090
2.226
2.464
2.473
2.236
2.664
2.607
2.701
2.089
2.047
2.851
2.797
2.610
2.558
2.818
2.813
2.507
2.571
2.800
2.805
2.788
2.023
1.968
3.109
1.993
0.15
0.15
0.15
0.15,
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.54
0.15
0.15
0.15
0.15
0.15
0.64
0.15
0.56
0.95
0.43
1.63
0.15
0.15
0.15
0.15
0.15
0.15
0.15
1.24
7.3
4.31
0.44
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.11 NO
0.06 NO
0.11 ND
0.10 ND
0.08 NO
0.08 NO
0.08 NO
0.09 ND
0.06 ND
0.06 ND
0.09 ND
0.09 ND
0.08 ND
0.07 ND
0.29
0.08 ND
0.07 ND
0.07 ND
0.09 ND
0.08 NO
0.30
0.11 ND
0.35
0.55
0.23
0.86
0.09 ND
0.07 ND
0.07 ND
0.07 ND
0.09 ND
0.10 ND
0.07 ND
0.58
3.64
2.19
0.20
0.07 ND
0.08 ND
0.08 ND
0.07 ND
0.07 ND
0.07 ND
0.10 ND
0.10 ND
0.06 ND
0.10 ND
LAB
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
new HSPH
old HSPH
old HSPH
new HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH .
old HSPH
old HSPH
old HSPH
old HSPH
new HSPH
old HSPH
old HSPH
old HSPH
old HSPH
new HSPH
old HSPH
FLAG
04
04
04
04
04
04
04
04
04
04
04
04
04
04
01
04
04
04
04
04
01
04
01
01
01
01
04
04
04
04
04
04
04
01
01
01
01
04
04
04
04
04
04
04
04
04
04
AVCON
0.11
0.06
0.11
0.10
0.08
0.08
0.08
0.09
0.06
0.06
0.09
0.09
0.08
0.07
0.29
0.08
0.07
0.07
0.09
0.08
0.30
0.11
0.35
0.55
0.23
0.86
0.09
0.07
0.07
0.07
0.09
0.10
0.07
0.58
3.64
2.19
0.20
0.07
0.08
0.08
0.07
0.07
0.07
0.10
0.10
0.06
0.10
E-3
-------
NICID
N7071
N7073.
N7088
N7084
N7062
N7066
N7078
N7059
N7098
N7097
N7095
N7089
N7100
N7101
N7082
N7081
N7079
N7093
N7090
N7080
N7085
N7091
N7092
N7089
N7122
N7123
N7083
N7098
N7124 '
N7121
N7107
N7108
N7111
N7112
N7109
N7110
N7113
N7114
N7148
N7140
N7140
N7141
N7120
N7110
N7134
N7142
N7118
FLTID
F4S97
F4707
F4685
F4708
F4B08
F4587
F4614
F4811
F4813
F4783
F4S07
F4814
F45S5
F4619
F4777
F4873
F.4798
F4925
F4928
F4829
F4828
F4870
F47B8
F4853
F4821
F4822
F4820
F4857
F4861
F4845
F4580
F4S81
F4839
F4832
F4858
F4S38
F4B60
F4855
F5289
F527B
F5089
F5294
F5291
F5290
F5092
F50S6
F5303
PID
013A
014A
014A
014A
015A
01SA
015A
015A
01 6A
016A
016A
01 6A
017A
017A
017A
018A
018A
018A
018A
019A.
019A
01 9A
019A
020A
020A
020A
021A
021A
021A
021A
022A
022A
022A
022A
023A
023A
023A
023A
024A
024A
024A
024A
025A
025A
025A
025A
026A
LOG
PAR
PAR
PAR
FAM
PAR
L1V
PAR
LIV
PAR
UV
PAR
UV
UV
PAR
PAR
UV
PAR
LIV
PAR
PAR
DEN
PAR
DEN
PAR
PAR
LIV
PAR
UV
UV
PAR
UV
PAR
LIV
PAR
PAR
UV
UV
PAR
PAR
UV
PAR
UV
PAR
UV
UV
PAR
PAR
PER UP L
10
9
10
10
9
9
10
10
11
11
12
12
11
11
12
11
11
12
12
11
11
• 12
12
13
14
14
13
13
14
14
13
13
14
14
13
13
14
14
15
15
' 16
16
15
15
16
16
15
1
1
1
2
1
2
1
2' ;
1
2
1
' 2
' >Z '
1
1
2
1
2
1
1
2
1
2
1
1
2
1
2
2
1
2
1
2
1
1
2
2
1
1
2
1
2
1
2
2
1
1
VOL MASS CONG NO .
2.001
3.370
2.548
2.426
2.624
2.669
2.367
2.391
3.100
3.123
1.891
1.874
2.148
2.168
2.698 '
2.797
2.828
2.278
2.313"
2.661
2.622
2.302
2.374
2.722
1.942
1.977
2.864
2.808
2.559
2.564
3.144
3.212
2.174
2.204
2.760
2.536
2.086
2.076
2.881
2.890
1.888
1.870
2.990
2.951
2.272
2.248
3.038
0.15
0.15
0.15
0.15
0.15
0.15
1.59
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.5
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15.
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
1.62
0.15
0.15
0.15
0.15
0.15
1.25
0.10 ND
0.06 ND
0.08 ND
0.08 ND
0.07 ND
0.07 ND
0.87
0.08 ND
, 0.06 ND
0.06 ND
0.10 ND
0.10 ND
0.09 ND
0.09 ND
0.24
0.07 ND
0.07 ND
0.09 ND
0.08 ND
0.07 ND
0.07 ND
0.08 ND
0.08 ND
0.07 ND
0.10 ND
0.10 ND
0.07 ND
0.07 ND
0.08 ND
0.08 ND
0.06 ND
0.06 NO
0.09 ND
0.09 ND
0.07 ND
0.08 ND
0.09 ND
0.09 ND
0.07 ND
0.07 ND
1.12
0.10 ND
0.07 ND
0.07 ND
0.09 ND
0.09 ND
0.53
LAB
old HSPH
old HSPH
old HSPH
old HSPH
new HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH .
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
FLAG
04
04
04
04
04
04
01
04
04
04
04
04
04
04
01
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04,
04
04 .
04
04
04
04
04
04
04
04
01
04
04
04
04
04
01
AVCON
0.10
0.06
0.08
0.08
0.07
0,07
0.87
0.08
0.06
0.06
0.10
0.10
0.09
0.09
0.24
'0.07
0.07
0.09
0.08
0.07
0.07
0.08
,0.08
0.07
0.10
0.10
0.07
0.07
0.08
0.08
0.06
0.06
0.09
0.09
0.07
0.08
0.09
0.09
0.07
0.07
1.12
0.10
0.07
, 0.07
0.09
0.09
0.53
E-4
-------
NICID
N7115
N7127
N7138
N7117
N7118
N7135
N7126
N7136
N7132
N7158
N71S4
N7139
N7133
N7160
N715S
N7129
N7130
N7171
N7170
N7137
N7131
N7173
N7172
N7178
N7177
N7194
N7195
N7176
N7175
N7193
N7174
N7168
N7190
N7169
N7167
N7192
N7189
N7180
N7181
N7199
N7198
N7S58
N7554
N7627
N7639
N7182
N7179
FLT1D
F5091
F5081
F5071
F5299
F5304
F5075
FS288
F5141
F5098
F5087
F5102
F4962
F4961
F5138
F5139
, FS069
F5070
F506S
F5064
F5119
F5118
F4966
F5122
F4881
F4883
F5019
F5014
F4941
F4944
F4876
F4922
F5143
F4913
F4887
F5017
F4874
F4903
F4908
F4904
F4849
F4862
F6169
F6171
F6173
F6164
F4889
F4909
FID
026A
026A
026A
027A
027A
027A
027A
028A
028A
028A
028A
029A
029A
029A
029A
030A
030A
030A
030A
031 A
031 A
031 A
031 A
032A
032A
032A
032A
033A
033A
033A
034A
034A
034A
035A
035A
035A
035A
036A
036A
036A
036A
037A
037A
037A
037A
038A
038A
LOG
DEN
PAR
DEN
L!V
PAR
LIV
PAR
PAR
LIV
PAR
LIV
PAR
LIV
PAR
LIV
PAR
DIN
DIN
PAR
PAR
DEN
DEN
PAR
FAM
PAR
FAM
PAR
LIV
PAR
PAR
PAR
FAM
PAR
PAR
LIV
PAR
LIV
FAM
PAR
PAR
FAM
LIV
PAR
PAR
LIV
PAR
LIV
PER UP
15
16
16
15
15
16 1
16
17
17
18
18
17
17
18 '
18
17
17
18
18
17
17
18
18
19
19
20 1
20
19
19
20
19
19
20
19
19
20
20
21
21
22
22
61
61
62
62
21
21
L
2
1
2
2
1
2
1
1
2
1
2
1
2
1
2
1
2
2
1
1
2
2
1
2
1
2
1
2
1
1
1
2
1
1
2
1
2
2
1
1
2
2
1
1
2
1
2
VOL MASS CONC ND
2.582
2.092
2.134
3.087
3.173
2.219
2.238
2.835
2.761
2.396
2.424
2.205
1.383
2.694
2.725
2.824
2.879
2.404
2.394
2.770
2.751
2.010
2.056
2.563
2.589
2.520
2.600
2.778
2.700
2.179
2.254
. 2.204
2.664
2.703
2.695
2.305
2.320
2.715
2.726
2.310
2.314
2.251
2.193
2.869
2.811
2.570
2.556
0.15
0.15
0.15
0.15
0.15
1.43
1.69
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.3
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.25
0.38
0.08 ND
0.09 ND
0.09 ND
0.06 ND
0.06 ND
0.84
0.98
0.07 ND
0.07 ND
0.08 ND
0.08 ND
0.09 ND
0.14 ND
0.07 ND
0.07 ND
0.07 ND
0.07 ND
0.08 ND
0.08 ND
0.07 ND
0.07 ND
0.10 ND
0.09 ND
0.08 ND
0.08 ND
0.08 ND
0.08 ND
0.07 ND
0.07 ND
0.09 ND
0.09 ND
0.09 ND
0.07 ND
0.07 ND
0.07 ND
0.17
0.08 ND
0.07 ND
0.07 ND
0.08 ND
0.08 ND
0.09 ND
0.09 ND
0.07 ND
0.07 ND
0.13
0.19
LAB
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
new HSPH
new HSPH
old HSPH
old HSPH
new HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
new HSPH
new HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
FLAG
04
04
04
04
04
01
01
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
04
01
04
04
04
04
04
04
04
04
04
01
01
AVCON
0.08
0.09
0.09
0.06
0.06
0.89
0.98
0.07
0.07
0.08
0.08
0.09
0.14
0.07
0.07
0.07
0.07
0.08
0.08
0.07
0.07
0.10
0.09
0.08
0.08
0.01
0.08
0.07
0.07
0.09
0.09
0.09
0.07
0.07
0.07
0.17
0.08
0.07
0.07
0.08
0.08
0.09
0.09
0.07
0.07
0.13
0.19
E-5
-------
N1CID
N7204
N7200
N7188
N7196
N7212
N7208
N7217
N7216
N7224
N7202
N7201
N7230
N7209
N7206
N7223
N7222
N7205
N7213
N7218
N7221
N7239
N7246
N7226
N7244
N7242
N7232
N722S
N7237
N7240
N7229
N7241
N7247
N7253
N7269
N7249
N7252
N7263
N7264
N7287
N72B9
N7261
N7256
N7265
N7254
N7281
N7280
N7248
FLTID
F4897
F4889
F4930
F4934
F4937
F4938
F5018
F5022
F4894
F4a7Z
F4791
F4801
F4931
F4988
F4983
F4987
F4980
F4991
F4995
FS237
F5225
F5223
FS193
F5203
F4817
F516S
FS168
F5330
F5038
F4935
F5367
F5322
F5321
F5339
F5369
F5374
F5354
F53S5
F5336
F5318
FS329
F49S9
FS363
FS348
FS173
F5174
FS300
PID
038A
038A
039A
039A
039A
039A
040A
040A
040A
041 A
041 A
041 A
042A
042A
042A
042A
043A
043A
043A
044A
044A
044A
045A
045A
04SA
046A
046A
046A
. 046A
047A
047A
048A
048A
049A
049A
049A
050A
050A
050A
050A
051 A
051 A
052A
052A
052A
052A
053A
LOG
LIV
PAR
FAM
PAR
PAR
FAM
LIV
PAR
PAR
LIV
PAR
PAR
PAR
LIV
LIV
PAR
PAR
LIV
PAR
DEN
PAR
PAR
PAR
PAR
LIV
LIV
PAR
LIV
PAR
PAR
PAR
PAR
PAR
LIV
LIV
PAR
LIV
PAR
PAR
LIV
PAR
PAR
LIV
PAR
PAR
LIV
PAR
PER UP
22
22
21
21
22
22
23
23
24
23
23
24
23
23
24
24
23
23
24
25 1
25
26
25
26
26
25
25
26
26
25
26
27
28
27
28
28
27
27
28
28
27
28
29
29
30
30
29
L
2
1
2
1
1
2
2
1
1
2
1
1
1
2
2
1
1
2
1
2
1
1
1
1
2
2
1
2
1
1
1
1
1
2
2
1
2
1
1
2
1
1
2
1
1
2
1
VOL MASS CONG
2.363
2.350
2.939
2.919
2.312
2.308
3.133
3.153
1.980
2.199
2.265
2.729
2.525
2.521
2.514
2.564
2.381
2.409
2.559
2.742
2.734
2.013
2.463
2.522
2.762
3.181
3.105
1.973
2.014
2.528
2.415
2.516
2.208
3.086
2.144
2.148
2.969
3.017
1.735
1.713
3.091
2.247
2.813
2.757
2.234
2.469
2.634
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.4
0.4
0.15
0.15
0.15
0.15
1.58
. 0.15
0.15
0.15
0.15
10.5
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.58
2.18
1.26
0.69
0.74
0.38
0.15
0.15
0.15
0.15
1.3
3
5.42
5.34
0.72
0.08
0.08
0.07
0.07
0.08
0.08
0.06
0.06
0.10
0.09
0.09
0.07
0.21
0.21
0.08
0.08
0.08
0.08
0.80
0.07
0.07
0.10
0.08
5.41
0.07
0.06
0.06
0.10
0.10
0.08
0.08
0.08
0.34
0.92
0.76
0.42
0.32
0.16
0.11
0.11
.0.06
0.09
0.60
1.41
3.15
2.81
0.36
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
LAB
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
new HSPH
old HSPH
old HSPH
new HSPH
old HSPH
old HSPH
new HSPH
new HSPH
old HSPH
old HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
FLAG
04
04
04
04
04
04
04
04
04
04
04
04
01
01
04.
04
04
04
01
04
04
04
04
01
04
04
04
04
04
04
04
04
01
01
01
01
01
01
04
04 '
04
04
01
01
01
.01
01
AVCON
0.08
0.08
0.07
0.07
0.08
0.08
0.06
0.06
0.10
0.09
0.09
0.07
0.21
0.2.1
0.08
0.08
0.08
0.08
0.80
0.01
0.07
0.10
0.08
5.41
0.07
0.06
0.06
0.10
0.10
0.08
0.08
0.08
0.34
0.92
0.76
0.42
0.32
0.16
0.11
0.11
0.06
0.09
0.60
1.41
3.15
2.81
0.36
E-6
-------
NICID
N7251
N7285
N7286
N7277
N7258
N727S
N7462
N7468
N7278
N7316
N7313
N7317
N7272
N7297
N7318
N7299
N7311
N7348
N7380
N7372
N7368
N7307
N731S
N7364
N7360
N73S2
N7384
N7369
N7361
N7392
N7396
N7353
N7357
N7354
N7326
N7373
N7347
N7323
N7335
N7330
N7419
N7342
N734S
N7413
N7408
N7365
N7349
FLTID
F5296
FS265
F5264
F5433
F5474
F5431
F5728
F5664
F5496
F5516
F5501
F5502
F5472
F5169
F5130
F5148
F5219
F5221
F5190
F5383
F5400
F5414
FS214
F5129
FS147
F5534
F5282
F5490
F5482
FS387
F5380
F4954
F4953
F4711
F50S2
F4958
F4957
F5379
F5183
F5181
F5241
F5430
F5428
FS426
F5420
FS7S1
F574S
FID
053A
054A
OS4A
054A
05SA
055A
OS6A
056A
057A
OS7A
058A
OS8A
OS9A
OS9A
060A
060A
061 A
062A
062A
064A
064A
065A
066A
065A
065A
066A
067A
067A
067A
068A
068A
068A
068A
069A
069A
069A
069A
070A
071 A
071 A
071 A
073A
073A
073A
073A
074A
074A
LOO
UV
PAR
LIV
PAR
PAR
PAR
PAR
LIV
PAR
PAR
LIV
PAR
PAR
PAR
DEN
PAR
PAR
PAR
PAR
PAR
LIV
LIV
PAR
LIV
PAR
PAR
PAR
LIV
PAR
PAR
LIV :
LIV
PAR
LIV
PAR
LIV
PAR
PAR
PAR
LIV
PAR
PAR
LIV
PAR
LIV
PAR
LIV
PER UP
29
29
29 1
30
29
30
49
49
31
32
32
32
31
32
34 1
34
34
35
36
36
36
35
. 35
36
36
36
37
38
38
37 .
37
38
38
37
37
38 1
38
37
39
39
40
39
39
40
40
39
39
L
2
1
2
1
1
1
1
2
1
1
2
1
1
1
2
1
1
1
1
1
2
2
1
2
1
1
1
2
1
1
2
2
1
2
1
2
1
1
1
2
1
1
2
1
2
1
2
VOL MASS CONG ND
2.S7S
3.119
3.035
1.981
2.520
2.463
2.463
2.310
2.684
2.574
2.186
2.226
2.493
2.234
2.386
2.545
2.372
2.618
2.327
2.314
2.258
2.240
2.190
2.754
2.772
2.350
2.506
2.443
2.447
2.526
2.490
2.466
2.616
2.524
2.493
2.491
2.551
2.761
2.555
2.482
2.479
2.198
2.301
2.904
2.863
2.250
2.367
0.65
0.15
0.04
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15 .
0.15
1.93
0.21
0.22
0.17
3.92
1.09
2.69
0.54
0.15
0.15
0.32
0.3
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.33
0.15
0.15
0.15
0.15
0.15
0.15
0.15 '
0.15
1.16
0.98
0.33
0.06 ND
0.02
0.10 ND
0.08 ND
0.08 ND
0.08 ND
0.08 ND
0.07 ND
0.08 ND
0.09 ND
0.09 ND
0.08 ND
0.09 ND
0.08 ND
0.08 ND
0.08 ND
0.96
0.12
0.12
0.10
2.28
0.65
1.27
0.25
0.08 ND
0.08 ND
0.17
0.16
0.08 ND
0.08 ND
0.08 ND
0.07 ND
0.08 ND
0.08 ND
0.08 ND
0.17
0.07 ND
0.08 ND
0.08 ND
0.08 ND
0.09 ND
0.08 ND
0.07 ND
0.07 ND
0.67
0.54
LAB
new HSPH
new HSPH
Hammond
new HSPH
new HSPH
new HSPH
old HSPH
old HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
old HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
old HSPH
old HSPH
new HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
FLAG
01
04
01
04
04
04
04
04
04
04
04
04
04
04
04
04
04
01
01
01
01
01
01
01
01
04
04
01
01
04
04
04
04
04
04
04
01
04
04
04
04
04
04
04
04
01 ,
01
AVCON
0.33
0.06
0.02
0.10
0.08
0.08
0.08
0.08
0.07
0.08
0.09
0.09
0.08
0.09
0.02
0.08
0.08
0.96
0.12
0.12
0.10
2.28
0.65
1.27
0.25
0.08
0.08
0.17
0.16
0.08
0.08
0.08
0.07
0.08
0.08
0.03
0.17
0.07
0.08
0.08
0.08
0.09
0.08
0.07
0.07
0.67
0.54
E-7
-------
NICID FLTID
N7409
N7410 ,
N7331
N7412
N7405
N7408
N7404
:N7407
M7411
N7400
N7503
N7499
;N7524
N7525
N7415
N73S5
N7351
•N7363
N7375
N7379
N7387
N7378
N7397
N7371
N7383
N7390
N7424
N7421
N7386
N7423
N7422
N7362
N7391
N7394
N7420
N7368
N7383
N7382
N7432
•N7428
N7437
N7472
N743B
N7440
N7480
N7441
N7433
F5251
F5744
F5234
F5233
F5199
F5457
F5740
FS211
F5207
F.5514-
FSS48
F6007
F59T4
F5853
1=5003
F4663
FS012
F5039
F5689
FS70B
F5688
FS573
FS038
"F5011
FS672
F5671
FS635
F56S7
F46S8
F5634
F5652
F5580
FS608
F5700
FS702
F5707
FS417
F5385
F5269
F5271
F5398
F5397
FS267
F5257
F5255
F52SS
F5532
PID
074A
074A
075A
075A
076A
078A
076A
077A
077A
077A-
078A
078A
078A
078A
07SA
079A
080A
080A
080A
080A
082A
082A
083A
083A
084A
OS4A
084A
084A
085A
085A
085A
086A
O86A
086A
086A
087A
087A
087A
088 A
088A
088A
088A
089A
089A
089A
089A
090A
toe
LIV
PAR
PAR
PAR
DEN
PAR
PAR
PAR
LIV
UV
LIV
PAR
UV
PAR
PAR
PAR
PAR
L1V
PAR
UV
PAR
PAR
PAR
PAR
UV
PAR
PAR
LIV
PAR
PAR
UV
PAR
LIV
PAR
UV
PAR
UV
PAR
PAR
.LIV
PAR
UV
UV
PAR
PAR
LIV
PAR
PER UP
40
40
30
40
41
41
42
41
41
42
57
57
58
£8
41
42
43
43
44
44
43
44
43
44
45 1
45
46
46
45
46
46
45
45
46
46
45
46
48
' 47
47
48
48
47
47
48
48
47
L
2
1
1
1
2
1
]
1
2
2
2
1
2
1
1
1
1
2
1
2
1
1
1
"I
2
t
1
2
1
1
2
1
2
1
2
1
2
1
'1
2
1
2
' 2
1
-I
2
1
VOL MASS CONC .NO
2.424
2.526
3.103
1.927
3.123
3.055
1.995
2.579
2.419
2.458
2.792
2.748
2.349
2.409
3.163
2230
2.707
2,529
2.201
2278
3.067
2217
2.749
2.202
2.558
2.598
2.485
2.484
2.620
2.364
2.466
2.422
2.418
2275
2.292
2.613
2.791
2.767
2.533
2.554
2^71
2.719
2.309
2200
2.390
2.377
2.686
0.76
8.47
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.58
0.15
0.15 -
fl;21
0.22
0.15
0.15
1.14
OJS4
0.38
0.48
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.5
0.3
2.2
0.94
3.98
0.15
1.83
0.15
0.15
0.15
4J51
426
0.67
2.03
0.62
0.31
0.55
0.35
0.15
O.41
4.36
0.06 ND
0.10 ND
0.06 ND
0.06 ND
0.10 ND
O.OB ND
0.08 ND
0.31
0^)7 ND
0.07 ND
0.12
0.12
0.06 ND
0.09 ND
0.55
0.33
022
027
0.06 ND
0.09 ND
0.07 ND
0.09 ND
0.08 ND
' 0.08 ND
0.08 ND
0.08 ND
0.25
0.16
1.16
0;50
2.14
0.09 ND
1.04
0.07 ND
0.07 tJD
0.07 WD
2.31
2.17
0.30 .
0.97
0.35
0.18
0.30
0.19
0.07 ND
UVB
oldHSPH
oldHSPH
newHSPH
newHSPH
.oldHSPH
oldHSPH
newHSPH
oldHSPH
old HSPH
new HSPH
newHSPH
newHSPH
newHSPH
newHSPH
newHSPH,
newHSPH
newHSPH
new HSPH
-newHSPH
newHSPH
newHSPH
newHSPH
newHSPH
new HSPH
oldHSPH
oldHSPH
oldHSPH
old HSPH
sold HSPH
old HSPH
oldHSPH
new«SPH
newMSPH
oldHSPH
oldHSPH
new HSPH
old HSPH
oldHSPH
newHSPH
newHSPH
o!d«SPH
old .HSPH
newHSPH
newHSPH
old HSPH
oldHSPH
oldHSPH
FLAG AVCON
B1
01, ,
04
;04
04
04
04
O4
04
01
04
04
01
01
04.
04
01
01
01
01
04
04
04 .
04;
O4
'O4
04
04
01
01
01
01
01
04
01
04
04
04
01
01
01
01
,01
01
01
01
04 .
0;41
4.36
0.06
0.10
0.06
0.06
0.10
O.08
0.08
0.31
0.07
O.O7.
0.12
0.12
0.06
0.09
0:55
0.33
0.22
0-27
0.06
0.09
0.07
0.09
0.08
0.08
0.08
0,08
025
«.16
1.16
0.50
.2.14
0.09
1i04
0.07
10.07
0.07
2.31
2.17
0.30
0.97
J0.35
D.18
0.30
O.19
0;07
E-8
-------
NICID
N7429
N7464
N7425
N7476
N7445
N7449
N7450
N7454
N7455
N7456
N7452
N7435
N7453
N7465
N7477
N7473
N7478
N7459
N7426
N7427
N7431
N7466
N7438
N7442
N7474 (
N7470
N7493
N7486
N7496
N7497
.N7485
N7482
N7471
N7484
N7488
N7479
N7319
N7480
N7483
N7508
N7500
N7512
N7491
N7502
N7492
N7481
N7518
FLTID
F5451
F5716
F5717
F5723
F5712
F5713
F5663
F5660
F5520
F5525
F5524
F5695
F5680
F5631
F5821
F5808
F5817
F5802
F5990
F5668
F5598
F5733
F5555
F5732
F5611
F5586
F5616
F5613
F5644
F5639
F6015
F6014
F5866
F5915
F5654
F5963
F5979
F5969
F5641
F5788
F5999
F5806
F6055
F6052
F6054
F6022
F5636
PID
090A
090A
091 A
091 A
091 A
091 A
092A
092A
092A
093A
093A
093A
094A
094A
095A
095A
095A
095A
096A
096A
097A
097A
098A
098A
098A
098A
099A
099A
100A
100A
100 A
100A
101A
101A
101A
102A
102A
102A
103A
103A
104A
104A
105A
105A
106A
106A
106A
LOG
LIV
LIV
PAR
LIV
PAR
LIV
DEN
PAR
PAR
LIV
PAR
PAR
PAR
PAR
FAM
PAR
PAR
FAM
PAR
PAR
PAR
PAR
PAR
LIV
PAR
LIV
PAR
PAR
PAR
LIV
LIV
PAR
PAR
PAR
LIV
PAR
LIV
PAR
PAR
PAR
PAR
PAR
PAR
PAR
FAM
PAR
PAR
PER UP
47
48
47
47
48
48
49
49
50
49
49
50
49
50
51
51
52
52 1
51
52
51
52
51
51
52
52
53
54
53
53
54
54
53
54
54
53
54
54
55
56
55
56
55
56
55 1
55
56
L '
2
2
1
2
1
2
2
1
1
2
1
1
1
1
2
1
1
2
1
1
1
1
1
2
1
2
1
1
1
2
2
1
1
1
2
1
2
1
1
1
1
1
1
1
2 .
1
1
VOL MASS CONG ND
2.682
2.327
2.633
2.640
2.143
2.265
3.085
3.131
1.939
2.726
2.749
2.535
2.733
2.125
2.815
2.772
2.634
2.558
2.158
2.549
2.502
2.940
2.882
2.754
2.054
1.987
2.877
2.098
2.185
2.278.
2.517
2.448
2.585
2.361
2.359
2.227
2.795
2.906
2.818
2.465
2.760
1.897
2.603
2.297
3.069
3.232
2.040
0.15
0.15
0.57
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.17
0.15
0.15
0.15
0.15
0.15
0.91
0.01
0.15
0.15
0.15
0.15
0.44
0.23
0.18
0.25
0.15
0.15
0.63
2.63
1.3
0.84
0.15
0.41
0.15
0.15
0.15
1.39
0.15
0.15
0.15
0.15
0.15
0.15
0.02
0.15
0.15
0.07 ND
0.08 ND
0.28
0.07 ND
0.09 ND
0.09 ND
0.06 ND
0.06 ND
0.10 ND
0.07 ND
0.08
0.08 ND
0.07 ND
0.09 ND
0.07 ND
. 0.07 ND
0.45
0.01 ND
0.09 ND
0.08 ND
0.08 ND
0.07 ND
0.20
0.11
0.11
0.16
0.07 ND
0.09 ND
0.37
1.50
0.67
0.45
0.08 ND
0.23
0.08 ND
0.09 ND
0.07 ND
0.62
0.07 ND
0.08 ND
0.07 ND
0.10 ND
0.07 ND
0.08 ND
0.01
0.06 ND
0.10 ND
LAB
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
Hammond
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
Hflfnmond
new HSPH
new HSPH
FLAG
04
04
01
04
04
04
04
04
04
04
01
04
04
04
04
04
01
04
04
04
04
04
01
01
01
01
04
04
01
01
01
01
04
01
04
04
04
01
04
04
04
04
04
04
01
04
04
AVCON
0.07
0.08
0.28
0.07
0.09
0.09
0.06
0.06
0.10
0.07
0.08
0.08
0.07
0.09
0.07
0.07
0.45
0.01
0.09
0.08
0.08
0.07
0.20
0.11
0.11
0.16
0^07
0.09
0.37
1.50
0.67
0.45
0.08
0.23
0.08
0.09
0.07
0.62
0.07
0.08
0.07
0.10
0.07
0.08
0.01
0.06
0.10
E-9
-------
NICID
M7513
N751S
N7511
N7507
N7S19
N7501
N7S08
N7510
N7523
N7505
N7532
N7533
N7538
N7537
N7558
N7553
N7544
N753S
N7552
N7530
N7534
N754S
N7607
N7B03
N7538
N7542
N761S
N7611
N7546
N7S50
N7631
N7635
N7S31
N7S27
N75B8
N7590
N7543
N7S59
N75S2
N7563
N7SS1
N7547
N7555
N7539
N7819
N7C23
N75S9
FLTID
F5823
F5831
F5S14
F5S18
F587S
FS87B
F6039
F5860
F5856
F5876
F5684
F5978
F59S1
F5865
F6072
F583S
F5833
F6152
F6156
F5864
F6135
F6139
F6124
F5953
F6229
F6239
F6242
F6233
F5941
F5949
F5780
F56SS
F6128
F5874
F6048
F5902
F5828
F5933
F5923
F5924
FS882
F5898
F6042
F5890
F6047
F5728
F6104
PID
107A
107A
107A
107A
108A
108 A
109A
109A
109A
109 A
110A
110A
111A
111A
112A
112A
112A
112A
113A
113A
114A
114A
114A
114A
115A
115A
115A
1T5A
116A
116A
116A
116A
117A
117A
117A
117A
11 8A
118A
118A
118A
11SA
119A
119A
119A
120A
120A
120A
LOO
FAM
PAR
FAM
PAR
PAH
PAR
PAR
LIV
PAR
LIV
PAR
PAR
PAR
PAR'
PAR
LIV
PAR
LIV
PAR
PAR
LIV
PAR
PAR
LIV
PAR
LIV
LIV
PAR
11V
PAR
PAR
LIV
LIV
PAR
LIV
PAR
LIV
PAR
LIV
PAR
PAR
LIV
UV
PAR
PAR
LIV
PAR
PER
67
57
58
58
57
58
57
57
58
58
59
60
59
60
59
59
60
£0
£9
60
61
61
62
62
61
61
62
62
61
81
62
62
63
63
64
64
63
63
64
64
63
63
64
64
63
63
64
UP L
2
1
3.
1
1
1
1
2
1
-2
1
1
1
1
1
1 .2
1
2
1
1
2
1
1
2
1
2
2
1
2
1
1
2
2
1
1 2
1
2
1
2
1
1
2
2
1
1
2
1
VOL MASS CONC ND
2.883
2.906
2.393
2.426
2.754
2.010
2.773
2.851
2.329
2.366
2.201
2.856
2.656
2.345
2.519
2.577
:3.634
2.867
2.782
1.938
2.726
2.679
2.274
2.306
2.186
2.107
2.782,
2.813
2.548
2.703
2.303
2.390
2.711
2.843
2.640
,2.631
2.187
2.198
2.668
2.563
2.719
2.645
2.834
2.897
2.489
2.494
2.461
0.15
7.18
0.15
0.3
0.15
0.15
0.27
2.04
1
6.1
0,15
0.15
0.15
0.15
0.15
0.06
3.91
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.78
0.18
129
1.56
1.15
1.2
2.04
1.47
0.15
0.15
0.15
0.15
;2.81
9.05
13.61
6.02
0.15
0.15
0.95
0.07 ND
321
0.08 ND
0.16
0.07 ND
0.10 ND
0.13
0.93
0.56
3.35
0.09 ND
0.07 ND
0.07 NO
0.08 ND
0.08 ND
0.03
1.40
0.07 ND
0.07 ND
0.10 ND
0.07 ND
0.07 ND
0.09 ND
0.08 ND
0.09 ND
0.09 ND
,6.07 ND
0.07 ,ND
(0.40
0.09
0.73
0.85
0.55
0.55
1.00
0.73
0.09 ND
0.09 ND
0.07 ND
0.08 ND
1.34
4.45
6.24
2.70
0.08 ND
0.08 ND
0.50
LAB
newHSPH
newHSPH
new HSPH
newHSPH
new HSPH
new HSPH
newHSPH
new HSPH
new HSPH
new,HSPH
newHSPH
newHSPH
newHSPH
new HSPH
newHSPH
^Hammond
newHSPH
newHSPH
new HSPH
newHSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old:HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
»ld HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
OldWSPH
old HSPH
old HSPH
«ld HSPH
old HSPH
FLAG
04
01
04
01
04
04
01
01
01
01
04
04
04
04
04.
01
01
04
04
04
04
04
04
04
04
04
04
04
01
01
01
O1
01
01
01
01
04
04
04
04
01
01
01
01
04
04
01
AVCON
0.07
-321
0.08
0.16
0.07
0.10
0.13
0.93
0.56
3.35
0.09
0.07
0;07^
0.08
0.08
0.03
1.40
0.07
0.07
0.10
B.07
0.07
0.09
0.08
0.09
0.09
0.07
0.07
0.40
0.09
0.73
0.85
0.55
6.55
1.01
0.73
0.09
0.09
0.07
0.08
1.34
4.45
6.24
2.70
0.08
0.08
0.50
E-10
-------
NICID
N7505
N7638
N7587
N7588
N7602
N7634
N7630
N7S91
N7594
N7567
N7618
N7614
N7606
N7626
N7622
N7571
N7589
N7573
N7601
N7570
N7564
N7568
N7605
N7S97
N7566
N7577
N7574
N7578
N7583
.N7S79
N7609
N758S
N7637
N7633
N7565
N7562
N7581
N7S13
N7596
N7569
N7617
N7621
N7616
N7612
N7629
N762S
N7604
FLTID
F5773
F5779
F5775
F5770
FS626
FS786
F5829
FS774
F5740
F5804
F5784
F5801
F5789
F6119
F6114
F5843
F6154
F5958
F5956
F5946
F6158
F6082
FS917
F5926
FS964
FS959
F6149
FS962
F5921
F5920
F6077
F6079
F6115
F6041
F6123
FS730
F6122
FS727
F6121
FS724
F55S2
F5553
F57S2
F5747
F5912
F5927
F5754
PID
120A
121A
121 A
121A
121A
122A
122A
122A
122A
123 A
123A
123A
123A
124A
124A
124A
125A
12SA
125A
125A
126A
126A
126A
126A
127A
127A
127A
127A
128 A
128A
128A
128A
129A
129A
129A
129A
130 A
130 A
130A
130 A
131A
131A
131A
131A
132A
132A
132A
LOG
LIV
LIV
PAR
LIV
PAR
LIV
PAR
LIV
PAR
LIV
PAR
PAR
LIV
LIV
PAR
PAR
PAR
LIV
LIV
PAR
LIV
PAR
PAR
LIV
LIV
PAR
LIV
PAR
PAR
LIV,
PAR
LIV
LIV
PAR
LIV
PAR
PAR
LIV
PAR
LIV
LIV
PAR
LIV
PAR
LIV
PAR
PAR
PER UP L
64
65
65
66
66
65
65
66
66
65
65
60
66
65
65
66
67 •
67
68
68
67
67
68
68
67
67
68
68
67
67
68
68
69
69
70
70
69
69
70
70 1
69
69
70
70
69
69
70
2
2
1
2
1
2
1
" 2
1
- 2
1
1
2
2
1
1
1
2
2
1
2
1
1
2
2
1
2
1
1
2
1
2
2
1
2
1
1
2
1
2
2
1
2
1
2
1
1
VOL MASS CONC ND
2.453
3.016
3.125
2.758
2.782
1.930
1.944
2.739
2.810
2.518
2.650
2.760
2.768
2.745
2.798
2.062
2.551
2.581
2.561
2.554
2.337
2.316
2.239
2.234
2.709
2.778
2.439
2.308
2.643
2.595
2.780
2.672
3.243
3.082
2.049
1.992
2.515
2.566
2.511
2.485
2.812
2.806
2.331
2.260
2.603
2.288
2.291
0.15
0.15
0.15
0.15
0.15
4.82
5.21
3.56
12.49
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.25
0.28
0.25
0.15
0.15
0.15
0.15.
0.15
0.15
0.15
0.15
0.15
0.24
0.55
0.15
0.15
5.53
3.3
0.25
0.75
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.54
3.75
1.63
0.08 ND
0.06 ND
0.06 ND
0.07 ND
0.07 ND
3.25
3.48
1.69
5.78
0.08 ND
0.07 ND
0.07 ND
0.07 ND
0.07 ND
0.07 ND
0.09 ND
0.13
0.14
0.13
0.08 ND
0.08 ND
0.08 ND
0.09 ND
0.09 ND
0.07 ND
0.07 ND
0.08 ND
0.08 ND
0.12
0.28
0.07 ND
0.07 ND
2.22
1.39
0.16
0.49
0.08 ND
0.08 ND
0.08 ND
0.08 ND
0.07 ND
0.07 ND
0.08 ND
0.09 ND
0.27
2.13
0.92
LAB
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
new HSPH
new HSPH
old HSPH
old HSPH
new HSPH
new HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
old HSPH
. old HSPH
old HSPH
FLAG
04
04
04
04
04
01
01
01
01
04
04
04
04
04
04.
04
01
01
01
04
04
04
04
04
04
04
04
04
01
01
04
04
01
01
01
01
04
04
04
04
04
04
04
04
01
01
01
AVCON
0.08
0.06
0.06
0.07
0.07
3.25
3.48
1.69
5.78
0.08
0.07
0.07
0.07
0.07
0.07
0.09
0.13
0.14
0.13
0.08
0.08
0.08
0.09
0.09
0.07
0.07
0.08
0.08
0.12
0.28
0.07
0.07
2.22
1.39
0.16
0.49
0.08
0.08
0.08
0.08
0.07
0.07
0.08
0.09
0.27
2.13
0.92
E-ll
-------
NICID
N760S
N7600.
N75B2
N7714
N770fl
N7588
N75S4
N7708
N7715
N7560
N7632
N7624
N7620
N7638
N7628
N7716
N7717
N7710
N7711
N7689
N7680
N7706
N7707
N7700
N7704
N7685
N7697
N7705
N7701
N7698
N7694
N7683
N7692
N7660
N7677
N7678
N7661
N7656
N7685
N7678
N7684
N7668
N7673
N7675
N7687
N7649
N7B50
FLTID
F5750
F6456
F6420
F6447
F6449
F6454
F6436
F6394
F6432
.F6329.
F6459
F6324
F6335
F6438
F6439
F6448
F6321
F6103
F6102
F6344
F6203
F6463
F6298
F6380
F6318
F6319
F6354
F6360
F6458
F6341
F6336
F6305
F6290
F6258
F6285
F6172
F6180
F6178
F6089
F6094
F6106
F6095
F6184
F6185
F6078
F6343
F6362
PID
132A
133A
133A
133A
133A
134A
134A
134A
134A
135A
135A
135A
13SA
136A
138A
136A
136A
137A
137A
137A
137A
138A
138A
139A
139A
139A
139A
140A
14QA
140A
140A
141A
141A
141A
142A
142A
142A
142A
143A
143A
143A
143A
144A
144A
145A
145A
145A
LOG
LIV
LIV
PAR
PAR
LIV
LIV
PAR
LIV
PAR
FAM
PAR
PAR
FAM
PAR
UV
PAR
UV
FAM
PAR
FAM
PAR
UV
PAR
LIV
PAR
UV
PAR
UV
PAR
PAR
LIV
UV
PAR
PAR
UV
PAR
PAH
LIV
UV
PAR
LIV
PAR
PAR
PAR
PAR
PAR
LIV
PER UP
70
71
71
72
72
71
71
72
72
71
71
72
72
71
71
72
72
73
73
,74
74
73
73
73
73
74 1
74
73
73
74
74
75
75
76
75
75
76
76
75
75
76
76
75
76
77
78
78
L
'9
2
1
1
2
2
•J
2
1
2
1
1
2
1
2
1
2
2
1 ,
2
1
2
1
"• 2
1
2
1
2
1
1
2
2
1
1
2
1
1
2
2
1
2
1
1
1
1
1
2
VOL MASS CONG ND .
2.301
3.140
3.148
2.004
1.930
3.068
3.045
2.450
2.445
3.427
3.388
2.018
1.978
2.762
2.767
2.429
2.419
2.741
2.794
2.551
2.611
2.306
2.314
2.846
2.828
2.440
2.480
2.185
2.208
2.449
2.511
2.802
2.794
2.192
2.903
2.854
2.200
2.229
2.896
2.885
2.164
2.234
2.941
2.070
2.759
2.038
2.026
1.1
O.15 ,
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15 "
0.15
0.15
0.15
1.05
0.25
0.74
0.15
0.15.
0.15
0.15
0.15
0.07
0.15
0.15
0.15
0.15
0.15
0.15
0.25
0.15
0.15
0.15
0.15
0.15
0.99
0.28
1.97
0.4
0.15
0.15
0.15
0.6
0.15
0.62
0.06 ND
0.06 ND
0.10 ND
0.10 ND
0.06 ND
0.06 ND
0.08 ND
0.08 ND
0.06 ND
0,06 ND
0.10 ND
0.10 ND
0.07 ND
0.07 ND
0.08 ND
0.08 ND
. 0.50
0.12
0.38
0.07 ND
0.08 ND
0.08 ND
0.07 ND
. 0.07 ND
0.04
0.08 ND
0.09 ND
0.09 ND
0.08 ND
0.08 ND
0.07 ND
0.12
0.09 ND
0.07 ND
0.07 ND
0.09 ND
0.09 ND
0.44
0.13
1.18
0.23
0.07 ND
0.09 ND
0.07 ND
0.38
0.10 ND
LAB FLAG AVCON
oldHSPH
old HSPH
old HSPH
old HSPH
oldHSPH
old HSPH
oldHSPH
oldHSPH
old HSPH
old HSPH
old HSPH
oldHSPH
oldHSPH
oldHSPH
" old HSPH
oldHSPH
old HSPH
old HSPH
old HSPH
new HSPH
.new HSPH
old HSPH
old HSPH
old HSPH
oldHSPH
Hammond
new.HSPH
old HSPH
old HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
01
04
04
04
.04
04
04
04
04
04
04
04
04
04
04
04
04
01
01
01
04
04
.04
04
04
01
04
04
04
04
04
04
01
04
04
04
04
04
01
01
01
01
04
04
04
01
04
0.62
0.06
0.06
0.10
0.10
0.06
. 0.06
0.08
0.08
0.06
0.06
fl.10
0.10
0.07
0.07
0,08
0.08
0.50
0.12
0.38
0.07
0,08
. 0.08
0.07
O.07
0.04
0.08
0,09
- 0.09
0.08
0.08
BX>7
0,12
0.09
,0.07
0.07
0.09
0.09
0.44
0.13
1,18
0.23
0.07
0.09
0.07
0.38
0.10
E-12
-------
NICID
N7662
N76S2
N7655
N7648
N76S3
N7658
N7645
N7798
N7641
N7640
N7722
N7723
N7643
N7642
N772S
N7724
N7720
N7721
N7729
N7733
N7651
N7723
N7732
N7728
N7797
N7727
N7737
N7726
N773S
N7751 .
N7789
N7756
N7794
N7783
N7753
N7744
N7738
N7754
N7747
N7742
N7746
N7779
N7791
N7784
N7785
N7786
N7755
FLTID
F6000
F6001
F6214
F6213
F6247
F6289
F8741
F6756
F6524
F6S1S
F6636
F6632
F6S07
F6487
F6634
F6415
F6744
F6582
F6588
F6S85
F6726
F6721
F6704
F6859
F6712
F6710
F6652
F6815
F6714
F627S
F62S4
F6471
F6413
F6384
F6385
F6522
F6520
F6592
F6387
F6536
F6353
F6666
F6695
F6482
F8405
F6475
F6314
PID
146A
146A
146A
146A
148 A
148A
149A
149A
1S1A
151A
151A
151A
152A
152 A
152 A
152A
153A
153A
154A
154A
154A
154A
155A
155 A
155A
155A
156A
156A
156 A
157A
157A
157A
158A
158 A
158A
159A
159A
159 A
159A
160 A
160 A
161A
162 A
162 A
163 A
163A
164A
LOG PER UP L
DIN
PAR
DIN
PAR
PAR
PAR
PAR
PAR
FAM
PAR
FAM
PAR
LIV
PAR
PAR
LIV
PAR
BED
PAR
FAM
PAR
FAM
PAR
FAM
FAM
PAR
PAR
FAM
PAR
PAR
LIV
LIV
PAR
BED
PAR
LIV
PAR
LIV
PAR
PAR
PAR
PAR
PAR
PAR
LIV
PAR
LIV
77 1
77
78
78
77
78
79
80
79
79
80
80
79
79
80
80
81
81
81
81
82
82
81
81
82
82
81
81 1
82
83
83
84
83
84
84
83
83
84
84
83
84
85
85
86
86 1
86
85
2
1
2
1
1
1
1
1
2
1
2
1
2
1
1
2
1
2
1
2
1
2
1
2
2
1
1
2
1
1
2
2
1
2
1
2
1
2
1
1
1
1
1
1
2
1
2
VOL MASS CONC ND
2.810
1.824
2.485
3.477
2.825
2.239
2.619
2.295
2.811
2.842
1.913
1.974
2.062
2.106
3.315
3.222
2.918
2.894
3.072
3.106
2.103
2.089
2.773
2.780
2.201
2.252
3.006
2.992
2.083
3.147
3.132
1.966
2.638
2.413
2.404
2.937
2.922
2.328
2.438
2.712
„ 2.049
2.535
3.140
2.282
2.604
2.510
2.701
0.5
0.15
0.15
14.9
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
1.34
1.29
0.25
0.78
0.15
0.15
0.15
0.15
0.15
0.15
1.5
9.14
6.09
1.53
0.15
0.15
0.15
7.2
8.1
0.99
0.15
0.15
1.67
0.53
0.48
1.16
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
4.4
0.23
0.11 ND
0.08 ND
5.57
0.07 ND
0.09 ND
0.07 ND
0.08 ND
0.07 ND
0.07 ND
0.10 ND
ND
0.84
0.80
0.10
0.31
0.07 ND
' 0.07 ND
0.06 ND
0.06 ND
ND
ND
0.70
4.27
3.60
0.88
0.06 ND
0.07 ND,
0.09 ND
2.97
3.36
0.65
0.07 ND
• 0.08 ND
0.90
0.23
0.21
0.65
0.08 ND
0.07 ND
0.10 ND
0.08 ND
0.06 ND
0.09 ND
0.07
0.08 ND
2.12
LAB
Hammond
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
newHSPH
new HSPH
new HSPH
new HSPH
old HSPH
new HSPH
new HSPH
new HSPH
old HSPH
old HSPH
old HSPH
old HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
old HSPH
old HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
FLAG
01
04
04
01
04
04
04
04
04
04
04
02
01
01 .
01.
01
04
04
04
04
02
02
01
01
01
01
04
04
04
01
01
01
04
04
01
01
01
01
04
04
04
04
04
04
01
04
01
AVCON
0.23
0.11
0.08
5.57
0.07
0.09
0.07
0.08
0.07
0.07
0.10
0.84
0.80
0.10
0.31
0.07
0.07
0.06
0.06
0.70
4.27
3.60
0.88
0,06
0.06
0.09
2.97
3.36
0.65
0.07
0.08
0.90
0.23
0.21
0.65
0.08
0.07
0.10
0.08
0.06
0.09
0.07
0.08
2.12
E-13
-------
NICIO
N7759
N7766
N774S
-N7762
N7771
N7769
N7782
N7767
N7757
N7770
N7831
N7827
N7869
N7860
N781S
N7819
N7873
N7877
N7872
N7863
N7823
N785S
N7879
N7S71
N785S
N7807
N7844
N7B61
N7862
N7870
N7S66
N784S
N7837
N7824
N7828
N7841
N7829
N7833
N7838
N7820
N7850
N7816
N7854
N7S30
N7834
N7SU
N7810
FLTID
F6403
F6288
F6263
FC181
F6376
F6372
FB3S3
F6377
FB367
F6231
F6811
F6881
F6757
F6309
F6S42
F6878
F6767
F6800
F6S84
F6887
F6601
F6762
F6796
F6846
F6731
F6577
F6857
F6782
F6540
F6722
F6725
F6062
F6648
F6663
F6S10
F6065
F6249
F6867
F6834
FC681
F6839
F6837
F6799
F6784
F6780
F6791
F6789
PID
164A
164A
164 A
166A
166A
167A
167A
167A
167A
168A
169A
169A
189 A
169A
170A
170A
170A
170A
171A
171A
172A
172A
173A
173A
173A
174A
174A
175A
17SA
176A
176A
177A
178A
178A
179A
179A
180 A
180A
180A
180A
181A
181A
182A
183A
183A
183A
183A
LOG PER UP
PAR
PAR
UV
PAR
PAR
PAR
UV
PAR
LIV
PAR
PAR
UV
LIV
PAR
UV
PAR
UV
PAR
PAR
PAR
PAR
PAR
PAR
LIV
LIV
PAR
PAR
PAR
PAR
PAR'
PAR
PAR
PAR
PAR
PAR
PAR
PAR
LIV
PAR
UV
PAR
PAR
PAR
UV
PAR
LIV
PAR
.85
86
86
' 87
88
87
, 87
88
88
88
89
89
90 1
:, 90
89
89
90
90
89
90
89
90
91
91
92
91
92
91
92
91
92
93
93
94
93
94
93
93
94
94
" 95
-96
95
' 95
95
96
96
L
1
1
2
1
1
1
2
1
2
1
1
2
2
1
2
1
2
-1
1
1
1
1
1
2
2
1
1
1
1
1
1
1
1
1
1
1
1
2
1
2
1
1
1
2
1
2
1
VOL
2.671
2.104
1.988
2.481
2.594
2.708
2.723
2.398
2.366
2.796
2.686
2.683
2.111
2.093
2.822
2.806
2.505
2.487
2.182
2.789
3.157
2.053
2.388
2.154
2.828
2.260
' 3.034
2.659
2.576
2.301
2.284
2.801
2.482
2.524
2.333
2.719
I 2.971
3.037
2.111
2.070
2.452
2.714
2.312
3.009
3.139
2.054
2.006
MASS CONC NO
2.49
0.17
0.32
0.15 ' •••
0.15
3.92
1.38
1.9
0.94
0.43
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.15
0.91
0.28
0.46
1.8
0.7
0.15
0.15
0.15
0.15 -
0.15
0.7
0.15
0.15
0.29
0.15
0.15
7.74
5.81
1.67
2.53
0.15
0.71
0.15
0.15
0.15
0.15
0.15
1.21
. 0.11
0,08 NO
0.08 NO
1.88
0.66
1.03
0.52
0.20
0.07 NO
0.07 NO
0.09 NO
0.09 NO
0.07 NO
0.07 NO
0.08 NO
0.08 NO
0.09 NO
0.07 NO
0.37
0.18
0.25
1.09
0.32
0.09 NO
0.06 NO
0.07 NO
0.08 NO
0.08 NO
0.40
0.07 NO
0.08 NO
0.15
0.08 NO
0.07 NO
3.39
2.49
1.03
1.59
0.08 NO
0.34
0.08 NO
0.06 NO
0.06 NO
0.09 NO
0.10 NO
LAB
new HSPH
newHSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
hew HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
new HSPH
old HSPH
FLAG AVCON
01
01
02
04
04,
01..
01
01
01
01
04
04
04
04 •„
04 ;
04
04
04
04
04
01
01
01
01 •
01
04
04
04
04
04
01
04
04
01
04
04
01
01
01
01
04
01
04
04
04
04 ,
04
1.21
0.11
0.08
0.08
1.88
0.66
1.03
0.52
0-20
0.07
0.07
0.01
0.09
0.07
0.07
0.08
0.08
0.09
0.07
0.37
0.18
0.25
1.09
0.32
0.09
0.06
0.07
0.08
0.08
0.40
0.07
0.08
0.15
0.08
0.07
3.39
2.49
1.03
1.59
0.08
0.34
0.08
0.06
0.06
0.09
0.10
E-14
-------
NICID FLTIO
N7826 F6829
N7821 F6831
N7808 F6784
N7809 F679S
PID LOG PER UP L
184A LIV 95 2
184 A PAR 95 1
184A LIV 06 2
184A PAR 96
1
VOL MASS CONC ND
2.407 0.15 0.08 NO
2.509 0.15 0.08 ND
2.559 0.15 0.08 ND
2.524 0.15 0.08 ND
LAB FLAG AVCON
new HSPH 04 0.08
new HSPH 04 0.08
new HSPH 04 0.08
new HSPH 04 0.08
E-15
-------
-------
APPENDIX F
ELEMENTAL DATA
F-l
-------
ELEMENTAL DATA
In this Appendix, elemental concentrations as measured by
different monitors at the central sitey or by the same monitors
at the central site and at the residences, are compared. In all
cases, the estimated value from the^X&Franalysis is provided
unchanged, without reference to whether it was above or below the
detection limit. For some of the elements that were not detected
a high percentage of the time (e.g., barium, rubidium,
strontium), this leads to apparently poor agreement, and
sometimes negative concentrations.
The first set of 16 graphs (pp. F-l to F-8) compare the
elemental concentrations associated with PM1Q as measured at the
central site by the PEM and SAM10 monitors ;(average values) vs.
the sum of the fine,and coarse fractions as measured at the
central site by the dichotomous sampler (average of two
samplers). The second set of graphs (pp. F-9 to F-16) compare
the central-site dichot fine fraction to the SAKL, 5 results at the
central site, and the third set of graphs (pp. F-17 to F-25)
compare the central-site dichot coarse fraction to the difference
of the SAM10 and SAM^g at the central site.
The next set of graphs (pp. F-26 to F-31) compares the
average of the davtime average PEM-SAM10 readings at the central
site to the outdoor SAM10 values at the residences. Agreement is
generally good (two-sample analyses do not reject the null
F-2
-------
hypothesis of no difference between locations) except for copper,
which apparently had a source'at "the central site. However, many
of the same elements compared at night (pp. F-32 to F-39) show
significant differences, with residential values higher than the
central site.
The next set of graphs provides similar comparisons for the
fine fraction elements measured by the SAM2>5 monitors at the
central site and at the residences. For the daytime comparisons
(pp.F-40 to F-47), again no difference is seen with the exception
of copper. But for the overnight comparisons, the residences
often show higher values than the central site.
The central site was in a well-shielded and mostly grassy
area. This may explain why PM10 concentrations were lower at the
central site, by about 6% during the day and 12% at night.
(Windspeeds were lower at night, which might account for the
increased overnight difference.) However, the fine particle
difference was much smaller (about 6% lower during the day and 4%
lower at night). Thus the much larger differences observed in
the elemental concentrations, particularly in those associated
with the fine fraction, can apparently not be completely
explained by lower particle concentrations at the central site.
F-3
-------
9
8
7
tls
NiX *O
1 J4
1^3
2
1
0
0
5 ;, ,Jft .i5
-SAM concentration; (ng/m3): Aluminum
20
200
150
100
+-»
1 50
3
0
-50
0
• I*
50 100 150 200 250 300
PEM-SAM concentration (ng/m3): Barium
350
F-4
-------
30
25
co
t
c
20
15
o
•s
Q 10
5
0
* .
-50 5 10 15 20 25 30 35
PEM-SAM concentration (ng/m3): Bromine
H
c
¥
5
11
10
9
8
•8 7
1 6
1 5
H 4
3
2
1
n
•
-
-
•
-
-
"•
• •
- «JP*
idF-
i i . . 1 .
0
5 10 15
Thousands
PEM-SAM concentration (ng/m3): Calcium
20
F-5
-------
6
5
t2>
-8
3
2
1
0
0
2 345 67
. Thousands
PEM-SAM concentration (ng/m3): Iron
8
2500
2000
1 1500
WJ
•§ 1000
•-^
Q
500
0
0
1 2 3
Thousands
PEM-SAM concentration (ng/m3): Potassium
F-6
-------
co
I
2000
1500
1000
500
0
0
200 400 600 800 1000
PEM-SAM concentration (hg/m3): Chlorine
1200
500
400
CO
,8 300
o
o
S
• 200
100
0
10 20 30 40 50 60 70 80 90
PEM—SAM concentration (ng/m3): Copper
100 110
F-7
-------
140
120
100
80
1 60
o
3
40
20
0
0 50 100 150
PEM-SAM concentration (ng/m3): Manganese
200
co"
I
c
o
•g
3
1UU
90
80
70
60
50
40
30
20
10
n
-
-,
_
-
• . B
• •
••• *
• • m ^
• • • " "
- ^.itrj51^^ * *
. j^pz >
,
0
20 40 60 80
PEM-SAM concentration (ng/m3): Lead
100
120
F-8
-------
15
10
co
I
o
3
0
* vV-1
'•*&•'
05 10 15 20 25
PEM—SAM concentration (ng/m3): Rubidium
30
co
Sen
"O
bZ) C
G wj
O O
5
6
w
5
4
3
2
1
n
•
' . •
• •
• .
• m • • * *
. "/' .**' -
••.„ . > .-. ' '
i 1-- .' '..
^*""A". •
0
2 3.4 5
Thousands
PEM-SAM concentration (ng/m3): Sulfur
F-9
-------
CO
Q
20
15
10
0
0
10
25
15 20
Thousands
PEM-SAM concentration (ng/m3): Silicon
30
35
50
40
30
* 20
10
0
o
o
5
0
" f iZ
"
10 20 30 40 50
PEM—SAM concentration (ng/m3): Strontium
60
70
F-10
-------
CO
t
a
600
500
400
300
o
•s •
S 200
100
0
0 100 200 300 400 500 600 700
PEM-SAM concentration (ng/m3): Titanium
800 900
300
250
--200
t
^ 150
o
•S-
5 100
50
0
•
H
•
..-"•"•"
^H
— f r i
0
50 100 150
PEM-SAM concentration (ng/m3): Zinc
200
F-ll
-------
1200
1000
800
f
•§> 600
N&
2 400
.2
Q
200
0
-200
-500 0 500 1000
SAM-2.5 concentration (ng/m3): Aluminum
1500
50
40
en
S 30
w>
•§ 20
5
10
0
-100
•• WL
0 100 200 300
SAM-2.5 concentration (ng/m3): Barium
400
500
F-12
-------
25
20
c
•*-»
o
•5 10
5
0
-10
".*
0 10 20 30
SAM—2.5 concentration (ng/m3): Bromine
40
1500
CO
I
1000
o
•S
5 500
0
0
500 1000 1500 2000
SAM—2.5 concentration (ng/m3): Calcium
2500
F-13
-------
y*j\j
800
700
^600
|500
o 400
0
S 300
200
100
0
-1
-
-
—
-
-
1
* * • , •
m ' m '
j£^
00 0 100 200 300 400 500 600 700 80
SAM—2.5 concentration (ng/m3): Chlorine
350
300
250
cr?
"I, 200
••*
P
150
100
50
0
-.
0 10 20 30 40 50 60
SAM—2.5 concentration (ng/m3): Copper
70
80
:F-14
-------
o
"6
1200
1000
800
600
400
200
0
0
500 1000 1500
SAM-2.5 concentration (ng/m3): Iron
2000
500
400
co
4s 300
aft
•S 200
100
0
•
m • •
0 100 200 300 400 500
SAM-2.5 concentration (ng/m3): Potassium
600
700
:F-15
-------
25
20
CO
15
-
I 10
S
o
-10
• "•* *
mm~ •*•
* •
•• «i-.-
#• • •
• •
0 10 20 30 40
SM-2.5 concentration (ng/m3): Manganese
50
90
80 h
70
"|>50
|40
Q 30
20
10
0
-10 0
10 20 30 40 50 60 70
SAM-2.5 concentration (ng/m3): Lead
80
90
F-16
-------
/^-N
n
e
o
41!
O
3
z.
1.5
1
0.5
0
-0.5
1
-
•
• * B"
"-. Ti -i
• • "i
• i
• " • • *
• •"*
• i
i
• •
.
• _ *
* • m m
,•* •• • •
i • •
* • • * " • •
• «
• • u m m
1 ' """ .=
i
-5 05
SAM—2.5 concentration (ng/m3): Rubidium
10
.7
8
1
to* 6
f 5
I4
5 3
2
1
n
-
-
_
-
•
•
•
•
•
•
•
•
*"" ... . "A ""
• • ••• _ * ** m
•" " ¥
-10
-5 0 5 10 15
!!AM—2.5 concentration (ng/m3): Strontium
20
F-17
-------
1 «
5 1
o |
p
0
5
4
3
2
1
n
•
•
. "
« •
• _ •
a • ' "
U<>
. Mr*
Bl ••i ^
J^1^
f*^ ......
0
2 34 5
Thousands
SAM—2.5 concentration (ng/m3): Sulfur
6
2500
2000
1 1500
feb
c
v—^
4-*
1 1000
3
500
0
0
1 .2 3
Thousands
SAM-2.5 concentration (ng/m3): Silicon
F-18
-------
90
80
70
^ 60
co
J 50
c Ar.
^ 40
o
•S 30
B 20
10
0
10
-
-
_
-
"•• v
r
B-
•* * "*•-
^#v
-200 -150 -100 -50 0 50
SAM-2.5 concentration (ng/m3): Titanium
100
150
200
150
1
•—
O
:§
Q
100
50
0
•
.. "f m
• • .
fmm
0 10 20 30 40 50 60 70 80 90
SAM-2.5 concentration (ng/m3): Zinc
100 110
F-19
-------
8
7
6
C^ f
5 -8 5
w) C
^ « 4
o o
"o H 3
S
2
1
0
-50 5 10
Thousands
SAM (coarse) concentration (ng/m3): Aluminum
15
J.Z
10
8
en
C3 ^
bb O
4->
^ 4
o
s
2
0
o
-
-
-
m
Jg •
»
.
• M
1
if"w/r"-'i""- * - j
"•""«*•-"•
•
, •
-10
-50 5 10 15
SAM (coarse) concentration (ng/m3): Bromine
20
F-20
-------
tr?
6 CO
-O
C «
~" 5
o jo
5
9
j
8
7
6
5
4
3
2
1
0
-
_
_
-
-
•
•
•
•
•
M^^H
^^^^^^
L 1
-5 0 5 10
Thousands
SAM (coarse) concentration (ng/m3): Calcium
15
2000
1500
t
o
•5
1000
500 -
0
-500
0 500 1000
SAM (coarse) concentration (ng/m3): Chlorine
1500
F-21
-------
200
150
o
100
50
0
40 -30 -20 -10 0 10 20 30 40 50
SAM (coarse) concentration (ng/m3): Copper
60 70
en
ee/J ft
_ TJ 3
^b G
C CO
N^/ CO
S §
Q
0
-1 0 1 2 34 5
Thousands
SAM (coarse) concentration (ng/m3): Iron
F-22
-------
2000
1500
co
t
c
o
•s
1000
500
0
-500
0 500 1000 1500 2000 2500 3000
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3500
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200
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10
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100
120
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1500
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25
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300
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25
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35
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50
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700
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60 70
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80
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80
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80
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80
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