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Journal of Exposure Analysis and Environmental Epidemiology (1999) 9, 535 ± 545

# 1999 Stockton Press All rights reserved 1053- 4245/99/$12.00

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Estimating environmental exposures to sulfur dioxide from multiple


industrial sources for a case±control study
J. FELIX ROGERS,a GEORGE G. KILLOUGH,b SHIRLEY J. THOMPSON,c CHERYL L. ADDY,c
ROBERT E. MCKEOWNc AND DAVID J. COWENd

a
Centers for Disease Control and Prevention, National Center for Environmental Health, Radiation Studies Branch, 4770 Buford Highway, NE, Atlanta,
Georgia 30341 - 3742
b
Hendecagon Corporation, 105 Netherlands Road, Oak Ridge, Tennessee 37830
c
Department of Epidemiology and Biostatistics, School of Public Health, University of South Carolina, Columbia, South Carolina 29298
d
Department of Geography, University of South Carolina, Columbia, South Carolina 29208

This paper first discusses how population exposures to environmental pollutants are estimated from environmental monitoring data and the problems that are
encountered in estimating risk from pollutants on the basis of ecologic studies. We then present a technique of estimating individualized exposures to an
atmospheric pollutant, sulfur dioxide ( SO2 ) , through atmospheric transport modeling for a case ± control study. The transport model uses the quantities of SO2
released from 30 geographically identified industrial facilities and meteorological data ( wind speed and direction ) to predict the downwind ground - level
concentrations of SO2 at geographically identified residences, receptors, of 797 study subjects. A distribution of facility SO2 emissions, uncertainties in
effective stack height, and model uncertainty are incorporated to examine the uncertainty in the predicted versus ambient monitoring SO2 levels, and to
generate an exposure uncertainty distribution for both the cases and controls. The transport model's accuracy is evaluated by comparing recorded ambient
measurements of SO2 with the model's predicted SO2 estimates at geographically identified ambient monitoring stations.

Keywords: atmospheric pollution, environmental, exposure, SO2, transport modeling.

Introduction product of fossil fuel combustion. SO2 is a common air


pollutant in areas surrounding coal -fired electric generating
Air pollution has been linked to increased mortality and plants, smelters, sulfuric acid factories and other industries.
respiratory symptoms in a number of studies both in the Electric generating plants are the primary source of SO2 in
United States and Europe ( Abbey et al., 1993, 1995; Ito et industrialized countries (Petruzzi et al., 1994 ).
al., 1993; PoÈnkaÈ and Virtanen, 1994; Xiping et al., 1995; Numerous federal agencies in the U.S. have established
Ballester et al., 1996; Wojtyniak and Piekarski, 1996 ). standards for air pollutants based upon the pollutants'
Sulfur dioxide (SO2 ) is one of the components of air potential for adverse health effects or damage to the
pollution resulting from industrial processes and a source of environment (Sanders, 1986 ) . The U.S. Environmental
sulfate ( SO4 ) in the atmosphere. Atmospheric sulfates Protection Agency (EPA ) has set the primary National
promote the production of acid rain and reduce atmospheric Ambient Air Quality Standards ( NAAQS ) for SO2
visibility ( Shprentz et al., 1996 ). SO2 itself is a non- exposure at 78 g/ m3. The annual average ambient
flammable, nonexplosive, irritant colorless gas that is a concentration of SO2 in the U.S. is 15 g / m3. Ambient
concentrations of SO2 tend to be highest in the summer
1. Abbreviations: AOD, airway obstructive disease; CO, carbon mon- months (40 ±50 g/m3 ) when the demand for electricity is
oxide; EPA, Environmental Protection Agency; GAEPD, Georgia greatest (National Air Quality and Emissions Trends
Environmental Protection Division; GHD9, Georgia Health District 9; Report, 1995 ) .
km2, square kilometer; g / m3, micrograms / cubic meter; NAAQS,
National Ambient Air Quality Standards; NCDC, National Climatic Data
This investigation reviews recent studies that estimate
Center; NO2, nitrogen dioxide; SO2, sulfur dioxide; SO4, sulfate; TSP, environmental exposures to atmospheric pollutants and
total suspended particulate matter; UTM, Universal Transverse Mercator; demonstrates how misclassification errors in exposure
VOCs, volatile organic compounds. assessment occur and the impact these errors have on
2. Address all correspondence to: Felix Rogers, PhD, Centers for Disease inferences made from these studies. Finally, this study
Control and Prevention, National Center for Environmental Health,
Radiation Studies Branch ( MS F - 35 ) , 4770 Buford Highway, NE,
presents a method that improves assessment of individual
Atlanta, GA 30341 - 3742. Tel.: ( 770 ) 488 - 7099. E-mail: fxr3@cdc.gov exposures to atmospheric pollutants for case± control
Received 12 November 1997; accepted 24 January 1999. epidemiological studies.
Rogers et al. Estimating environmental exposures to SO2

Background (1996) included meteorological data such as daily mean


temperatures and humidity in addition to ambient 24 -
Estimating environmental exposures to atmospheric pollu- measurements of SO2 for generating an exposure
tants is difficult in epidemiologic studies, and, at present, estimate.
such studies rely on crude methodologies. Obtaining Other environmental exposure investigations have ge-
information about the sources of the pollutants, including nerated exposure estimates expressed as categories of
the kinds of emissions and emission rates, determining the exposure based on census tracts (Shaw et al., 1992 ) or
effect that weather plays upon the dispersion of pollutants exposure risk indexes incorporating distance from a waste
from the sources, identifying the locations where an site and a hazard ranking score ( Geschwind et al., 1992 ).
individual exposure may occur, and quantifying individual Marshall et al. ( 1993 ) estimated potential exposure scores
exposures are difficult and time consuming. As a result, for hazardous waste sites within a 1 -mile radius by using a
environmental studies generally have been designed as template originating at the waste site. The template was
inexpensive ecologic studies (Morgenstern and Thomas, divided into 25 sectors extending from the waste site. The
1993 ) that make no attempt to estimate individual exposure score was based on the probability of exposure
exposures. As surrogates of exposure, environmental (i.e., the degree to which a residence in a sector was in the
epidemiologic studies have used air quality monitoring data path of offsite migration of contamination ) . The exposure
obtained from sampling networks that were established for metric used in these studies was not related to any specific
purposes other than health -related research. In areas pollutant.
without monitoring systems, researchers have attempted to A weakness common to all ecologic studies is that the
interpolate measurements collected from monitored areas to researchers cannot identify study subjects as exposed or
unmonitored areas. The ecological design ignores the unexposed. All study subjects may be regarded as exposed,
locations of pollutant sources and the atmospheric influence and those with health effects from the exposure are
upon the dispersion and ultimate concentrations of these generally reflected in increases in the number of hospital
pollutants. In ecologic studies researchers assign a crude admissions, reported deaths, and reported asthma attacks. In
estimate of exposure to large population areas such census essence, an ecologic study's use of ambient exposure
tracts, counties, or postal zip code areas. measures results in a nondifferential exposure misclassifica-
Several attempts have been made to associate sulfur- tion bias. This bias may lead to an overestimation of effect
containing pollutants with adverse health effects ( Abbey et (Brenner et al., 1992 ) , or an underestimation of effect
al., 1993, 1995; Ito et al., 1993; Xu et al., 1995; Ballester et (Morgenstern and Thomas, 1993) depending on the study
al., 1996; PoÈnkaÈ and Virtanen, 1996; Wojtyniak and design and response rates. Furthermore, any causal
Piekarski, 1996 ). In studies of respiratory symptoms and inferences suggested from ecologic studies fail to demon-
exposure to a variety of pollutants, Abbey et al. (1993, strate the true effect at the individual level ( Morgenstern
1995 ) used SO2 cut -points from 10- year cumulative and Thomas, 1993 ) . Attempts to associate exposure with
ambient measurements that ranged from 2 to 14 parts -per- outcome at the individual level in ecologic studies is known
hundred -million (pphm ) . Xu et al. ( 1995 ) used mean as the ecologic fallacy (Morgenstern, 1982 ) .
ambient concentrations of SO2 measured in two residential We found no study in which individualized environ-
areas in Beijing, China, to study the effect that exposure to mental exposures were modeled from a point source to a
SO2 had on gestational age in four residential areas. The geographically identified receptor, a residence, through the
exposures, annual mean concentrations of SO2, were from use of an atmospheric transport model. A few studies,
93 to 108 g / m3. In their study of mortality and air however, have used an atmospheric transport model to
pollution in the city of London, England, Ito et al. (1993 ) estimate exposures in regions that ranged in sizes from 1
used daily averages of SO2 measurements from seven km2 to zip code areas, from which exposure estimates were
sampling sites with ambient exposures of 100 to 1000 interpolated across larger areas (Brown et al., 1984; Hatch
g/ m3 while in their study of low- level air pollution and et al., 1990 ) . Although exposure estimates based on
asthma in Helsinki, Finland, PoÈnkaÈ and Virtanen (1994 ) residential locations have not been used in transport
used eight ambient sampling sites with ambient exposures modeling techniques, residential locations have been used
ranging from 13 to 25 g / m3. to estimate individual external exposures from nuclear
Another series of more recent ecologic studies that bomb test fallout (Lloyd et al., 1990 ). However, in the
evolved from the multinational European air pollution Lloyd et al. ( 1990 ) study, residence was defined in terms of
health effects study also relied on ambient measurements a geographical area that contained the true residence. In the
of pollutants for exposure estimates ( Ballester et al., studies by Brown et al. ( 1984 ) , Hatch et al. (1990) and
1996; PoÈnkaÈ and Virtanen, 1996; Wojtyniak and Lloyd et al. ( 1990 ) the study subjects that lived within
Piekarski, 1996 ). The air pollution± mortality study of specific areas received the same exposure estimate and
Ballester et al. ( 1996 ) and Wojtyniak and Piekarski therefore were subject to exposure misclassification.

536 Journal of Exposure Analysis and Environmental Epidemiology (1999) 9(6)


Estimating environmental exposures to SO2 Rogers et al.

The Gaussian environmental transport model (Meade


and Pasquill, 1958 ) presented below is used to estimate
ground -level SO2 concentrations at residences of case and
control subjects when SO2 originates from multiple
geographically identified SO2 release points. The ground -
level concentration estimate is a summation of the model
SO2 concentration estimates for the residence from each
release point. Exposure predictions obtained in this manner
will provide an individualized external exposure estimate
that will reduce the probability of exposure misclassifica-
tion. In this study, we used our estimates of residential SO2
concentrations to test the association between exposure to
environmental SO2 and the birth of very low birthweight
babies in Georgia Health District 9 (GHD9 ) between April
1, 1986 and March 31, 1988.
The model described below was chosen on the basis of
several general assumptions. First, we assumed that the
model is suitable for this type of study. This assumption is
based on the demonstrated reliability of the Gaussian
atmospheric transport model in predicting downwind
concentrations of material released into the atmosphere,
given certain parameter limitations ( Vesper, 1992 ). Second,
we assumed that the use of annual industrial emissions and
meteorological data in the model will provide good
estimates of annual SO2 concentrations at the locations of
interest. Third, we assumed that annual ambient monitoring
data that are used to validate the model estimates are
accurate and represent the true annual ambient SO2
concentrations for the monitored regions. The limitations
of using annual meteorological and monitoring data in
estimating exposures are discussed below.

Methods Figure 1. ( a ) Industrial sulfur dioxide emission locations ( o ) in


Georgia Health District 9 counties. ( b ) Sulfur dioxide emission sites
( o ) and ambient monitoring sites ( M ) in Chatham County,
Study Area Georgia.
The study area is Georgia Health District 9 ( GHD9 ), which
is composed of 24 counties in the southeastern coastal
region of Georgia (USA ) . This largely rural region of monitored by the GAEPD. According to the GAEPD these
Georgia consists primarily of small towns, although it facilities account for between 90% and 95% of the 50,500
contains two moderately sized cities, Savannah and tons per year of SO2 emissions in the area. The GAEPD
Brunswick. The entire area encompasses approximately emissions data included the quantity (in tons ) of the
38,000 km2 (Figure 1a ). estimated annual emissions of SO2 (the source term ),
facility geocodes, and stack data (stack height, stack
Emission Site Data diameter, gas temperature, and gas flow rate ) . No informa-
Emissions data for 1986 ±1988 (Table 1 ) on 30 industrial tion was available to describe the variation in stack releases
facilities within GHD9 were obtained from the Georgia over the reported time period. In order to establish some
Environmental Protection Division (GAEPD ) 1 of the degree in the uncertainty of the annual SO2 releases, we
Georgia Department of Natural Resources. The emissions incorporated a uniform distribution with a 40% variation,
from these industries, whose products include chemicals, above and below, the reported release estimates greater than
plastics, fertilizers, asphalt, wood, paper, and gypsum, are 1000 tons per year (Table 1 ) for stochastic sampling. Of the
30 point sources located within the study area, 14 are
1
Georgia Environmental Protection Division, Georgia Department of located in 10 of the 24 counties ( Figure 1a ), and 16 are
Natural Resources, Atlanta, GA, 30354. within a single county, Chatham (Figure 1b ).

Journal of Exposure Analysis and Environmental Epidemiology (1999) 9(6) 537


Rogers et al. Estimating environmental exposures to SO2

Table 1. Point source emission data: county, annual release ( tons ) , Ambient Monitoring Data
geocode, Universal Transverse Mercator ( UTM ) , and physical stack
Data for five ambient monitoring stations within GHD9
heights ( meters ) .
were obtained from the GAEPD for 1986 ±1988. The data
included mean annual SO2 concentrations and geocodes of
County Release Northing Easting Stack
( UTM ) ( UTM ) height the monitoring stations. Four monitoring sites are located
within the city of Savannah (Chatham County, Figure 1b)
Ware 2 3457188.34 365306.95 8
and the fifth site is located 114 km southeast of Savannah in
Chatham 5 3548806.06 495101.77 10
Brunswick (Glynn County ). The monitoring data will be
Chatham 11 3551191.09 482987.58 15
used to test the accuracy of the atmospheric transport model
Evans 13 3558595.75 413411.23 17
in predicting ground -level concentrations of SO2 at
Chatham 20 3554880.15 484201.07 47
Chatham 34 3549989.55 485901.53 11
unmonitored residences.
Bryan 53 3572400.04 455820.06 20
Glynn 77 3443993.31 453598.88 32
Residence Data
Chatham 79 3552603.44 487395.77 18
The residences outside Savannah ( those of 140 case and
Chatham 90 3551191.09 482987.58 26
360 control subjects ) were geocoded ( latitude/longitude )
Chatham 102 3552292.35 487999.2 33
with USGS topographic maps and on- site surveillance.
Chatham 148 3552602.71 487999.57 42
Residences within Savannah ( those of 98 case and 199
Pierce 153 3464903.78 381900.58 10
control subjects ) were geocoded by street address matching
Glynn 218 3453185.44 447904.73 62
of residences to degrees latitude and longitude with the
Chatham 220 3557902.8 486506.55 17
geographic software Maptitude.3 All geographic latitude
Charlton 221 3407999.31 403510.98 20
and longitude coordinates were converted to universal
Chatham 427 3555985.66 486192.77 47
transverse Mercator ( UTM ) coordinates for modeling
Chatham 517 3496505.42 490808.09 59
purposes using the software Geocalc.4
Liberty 518 3510794.92 460999.74 49
Chatham 631 3548285.47 494393.65 20
Environmental Transport Model
Glynn 633 3447802.23 454416.2 60
The Gaussian plume atmospheric transport model used in
Glynn 645 3439591.38 440702.97 40 this study was first introduced by Holland (1953 ) and
Chatham 1946 3549490.62 486004.65 20 Meade and Pasquill ( 1958 ). The sector-averaged form of
Chatham 2336 3556917.28 485797.97 80 the model used in this study is given by:
p  
Wayne 3535 3502404.34 420416.46 80 Q 2=f h2e
Chatham 5860 3551704.32 488498.57 100
ˆ exp …1†
…2x=16†z u 22z
Effingham 6491 3579797.95 484108.21 40
Glynn 7343 3448718.11 450389.02 90 where u= the wind speed ( m /s ), f =the fraction of the time
Camden 7453 3401284.17 448204.93 90 the wind blows into the receptor sector, x =the distance (m )
Chatham 10762 3556794.95 486090.14 90 from the source to the receptor,  z = the vertical dispersion
coefficients (m ) as a function of downwind distance from
the source ( Hanna et al., 1982 ), 2 /16 = the angular width
Meteorological Data of a standard windrose sector of 22.58, h e = effective stack
Meteorological data for Savannah was obtained from the height of the source ( m ). Q = the release rate of SO2 from
National Climatic Data Center ( NCDC ) , Asheville, NC.2 the source ( g /s ), and  = the average ground - level
Savannah was the only location within GHD9 where concentration ( g / m 3).
meteorological data is collected by the NCDC. These data, This model is designed to estimate the average ground -
for 1986 ± 1988, were annualized and included a frequency level concentration over long periods of time such as a
distribution of six wind speed categories over a 16- sector season or a year. The model concentrations are estimated by
windrose for six atmospheric stability classes defined as weighting the predicted concentration at a receptor by the
follows: A Ð extremely unstable, B Ð moderately frequency f that the wind blows from a point source into the
unstable, C Ð slightly unstable, D Ð neutral, E Ð 22.58 sector containing the receptor according to climato-
slightly stable, and F Ð moderately stable conditions. This logical records (the windrose) . The Gaussian model
stability - typing classification is known as the Pasquill ± predicts the averaged concentration along an arc within
Gifford scheme (Hanna et al., 1982 ) . the sector at the calculated distance from a source. Two

2 3
National Climatic Data Center, Federal Building, Ashville, NC 28801 - Caliper Corporation, 1172 Beacon St., Newton, MA 02161.
4
2696. Blue Marble Geographics, 46 Water Street, Gardiner, ME 04345.

538 Journal of Exposure Analysis and Environmental Epidemiology (1999) 9(6)


Estimating environmental exposures to SO2 Rogers et al.

residences at the same radial distance from a source within executed on an Excel5 spread sheet. Stochastic sampling
the same sector would receive the same estimated exposure was achieved with the software Crystal Ball6 to estimate the
from that source, but two residences at different distances exposure distributions.
within the same sector or two residences in different sectors
would, in general, receive different exposures from the Model Bias
source. This model allowed us to estimate individualized To test the accuracy of the environmental transport model,
exposures, since no two birth homes will fall along the same we compared the model -predicted concentrations with the
arc. environmentally monitored (observed ) ambient concentra-
tions. When the annual source term ( SO2 release data ) from
the industrial facilities is known, model performance can be
Transport Model Uncertainty validated by comparing how well the model predicts a
We implemented uncertainty in the transport model, after downwind concentration at a receptor to the observed
Miller and Hively (1987) , by multiplying the predicted ambient monitoring data at that receptor. In order to validate
exposure concentrations for each source ± receptor pair by a the model used in this study we obtained ambient
lognormally distributed factor with geometric mean 1.0 and monitoring data (see Ambient Monitoring Data above )
geometric standard deviation 1.52. The lognormal distribu- for the five locations within the study area that recorded
tion with these parameters has its 5th percentile at 1 /2 and ambient SO2 levels.
its 95th percentile at 2; thus, the factor is between these two There are several ways to compare predicted with
values with probability 0.90) . This factor is assumed to be observed SO2 concentrations. One simple way is to examine
stochastically independent of other sources of uncertainty, the trend of concentrations over distances. However, it is
such as the release rate and the parameters affecting plume useful to quantify the difference between the model -
rise. The choice of a factor of 2 for model uncertainty is predicted and measured concentrations. Bias can be
discussed below. expressed in terms of a predicted -to - observed ratio (P / O
The effective stack height h e ( Hanna et al., 1982 ) is ratio ) where:
estimated from: P /O = 1 exact agreement,
 v 1:4  T

P /O > 1 overprediction,
he ˆ h ‡ d 1‡ ; …2† P /O < 1 underprediction.
u T
When a number of locations are being examined, the
where h =the physical stack height (m ), u= the wind speed geometric bias is used. The geometric bias is the geometric
( m / s ), v =the stack gas velocity ( m /s ), T= the stack gas mean of the individual P /O ratios, given by
temperature ( 8F) , T= the difference in stack gas tempera- 0P n 1
ture and ambient temperature (8F ), and d= the stack ln…Pi =Oi †
Biˆ1 C
diameter ( m ) . Geometric bias ˆ expB @
C;
A …3†
n
The effective stack height thus takes into account plume
rise height as a result of the exit velocity and temperature of
the effluent gas. Uncertainties in the effective stack height where P i = predicted concentration at location i, O i =ob-
were propagated by sampling from a normal ambient served concentration at location i, and n = the number of
temperature distribution ( mean = 658, standard devia- locations being compared.
tion = 108) , and the meteorological wind speed distribution.
Results
Exposure Calculations
For this study, estimates of ground -level concentrations of Model Performance
SO2 at a receptor were obtained by summing the ground - Table 2a ( physical stack heights, h ) and b (effective stack
level concentrations estimated from Equation 1 over each of height ( plume rise ) , h e ) show both the measured
the 30 SO2 point sources. The source term for the (observed ) and model - predicted SO2 concentrations at
deterministic model with plume rise used the reported the GAEPD ambient monitoring stations obtained from the
annual SO2 facility releases ( Table 1 ), an ambient deterministic model. The predicted values are the sums of
temperature of 658, and a wind speed of 1 km /s for the model -predicted downwind SO2 concentrations over
calculating the effective stack height. The stochastic model the 30 point sources. The effect of using plume rise to
sampled from the source term distributions described above establish the effective stack height, h e, is to move the model
for the release points, incorporating the uncertainty in the
effective stack height discussed above. The program for the 5
Excel97, Microsoft Corporation.
exposure model was written in a Visual Basic module and 6
Crystal Ball, Decisioneering, 1515 Araphahoe Street, Denver, Colorado.

Journal of Exposure Analysis and Environmental Epidemiology (1999) 9(6) 539


Rogers et al. Estimating environmental exposures to SO2

Table 2. Observed ( measured ) and predicted ( estimated ) SO2 concen- per year ) located in Chatham County, estimated from the
trations at ambient monitoring sites with predicted - to - observed ratios,
deterministic model. The closest monitoring station at 3218
geometric bias, and correlation coefficient, r, for models with and without
plume rise ( deterministic model ) . m, Savannah Water Works, was predicted to receive
approximately two- thirds of GAEPD measured atmos-
Observed Predicted P/O pheric SO2 concentration from this single release site. The
g / m3 g / m3 other ambient monitoring stations within the city of
a. Model without plume rise a Savannah and Brunswick receive increasingly smaller
Savannah Water Works 17.40 50.15 2.88 predictions of SO2 concentrations from this single SO2
Savannah Farmers Market 15.70 116.33 7.71 source as distance from the release point increased.
Savannah Electric 16.31 51.68 3.17
Savannah E. President St. 13.07 49.73 3.81 Exposure Estimates
Brunswick, GA 5.23 14.91 2.85 The exposure estimates for the cases gave a lognormal
distribution with a mean of 7.64 and a standard deviation of
b. Model with plume rise ( effective stack height ) b 10.87 while the exposure estimates for the controls resulted
Savannah Water Works 17.40 18.75 1.08 in a lognormal distribution with a mean of 5.71 and a
Savannah Farmers Market 15.70 23.04 1.47 standard deviation of 7.92. Figure 2 shows the percentile
Savannah Electric 16.31 12.95 0.79 distribution for the case and control residential SO2. The 5th
Savannah E. President St. 13.07 11.44 0.88 percentile of the two groups were essentially the same, 0.88
Brunswick, GA 5.23 6.15 1.18 versus 0.89 g/ m3. The percentile estimates for the case and
a
Geometric bias = 3.74 ( r = 0.29 ) . control residences begin to separate starting at the 25th
b
Geometric bias = 1.05 ( r = 0.78 ) . percentile. Figure 3 shows the uncertainty in SO2 exposure
for the cases and controls from their exposure distributions.

predictions toward the GAEPD observed values (Table


2b ). The estimated bias of the model is 3.74 when physical Discussion
stack height is used in the transport model and 1.05 when
the effective stack height is used in the transport model. Model Accuracy
Therefore, effective stack height was used in calculating the Hanna et al. ( 1977 ) described the Gaussian transport model
exposure estimates described below. as ``the basic workhorse'' for dispersion calculations
Table 3 shows the uncertainty in the ambient monitor because of the model's good agreement with experimental
estimates generated by the stochastic model and the data, ease of operation, conceptional appeal, and reflection
distribution in the model bias when estimating ground - of the random nature of atmospheric turbulence. The
level concentrations at the monitoring stations for the 30 ground -level concentration estimates from the Gaussian-
release sites. After 1000 simulations the model bias was plume model are responses to a number of clearly visible
shown to fluctuate between a 5th percentile of 0.47 and a parameters. The predicted concentration at a receptor from a
95th percentile of 1.99, with the median estimate being source is directly proportional to the release rate at the
0.99. source ( Equation 1) . Distance from the source to the
Table 4 shows the ground -level SO2 concentrations at receptor also plays a major role in the exposure estimate. As
the GAEPD ambient monitoring stations within the city of seen in Figure 4, the exposure estimate declines approxi-
Savannah and the monitoring station at Brunswick mately logarithmically as distance from the source in-
attributable to the largest point source (10,762 tons SO2 creases. Meteorological parameters such as wind speed,

Table 3. Uncertainty distribution ( percentiles ) of ground - level concentrations of SO2 ( g / m3 ) at the ambient monitoring stations with predicted - to -
observed ratios ( P / O ) , and percentile geometric bias ( stochastic model ) .

Monitor location 5th 25th 50th 75th 95th


Water Works 8.05 ( 0.46 ) 12.77 ( 0.73 ) 17.49 ( 1.01 ) 23.40 ( 1.34 ) 35.84 ( 2.06 )
Farmers Market 10.10 ( 0.64 ) 15.91 ( 1.01 ) 21.58 ( 1.37 ) 28.61 ( 1.82 ) 43.26 ( 2.76 )
Savannah Electric 5.78 ( 0.35 ) 9.23 ( 0.57 ) 12.43 ( 0.76 ) 16.39 ( 1.00 ) 24.90 ( 1.53 )
Savannah East President 5.07 ( 0.39 ) 8.14 ( 0.62 ) 10.94 ( 0.84 ) 14.47 ( 1.11 ) 21.72 ( 1.66 )
Brunswick, GA 2.82 ( 0.54 ) 4.32 ( 0.83 ) 6.05 ( 1.10 ) 7.80 ( 1.49 ) 11.87 ( 2.27 )

Geometric bias 0.47 0.74 0.99 1.32 1.99

540 Journal of Exposure Analysis and Environmental Epidemiology (1999) 9(6)


Estimating environmental exposures to SO2 Rogers et al.

Table 4. Contribution of the largest point source to the ambient monitoring stations. This table reflects the effect of distance ( meters ) on SO2 concentration
at ambient monitoring sites from the largest SO2 emission site ( deterministic model ) .

Source North East Height Monitor location North East Distance Direction g / m3
( tons ) ( UTM ) ( UTM ) (m) ( UTM ) ( UTM ) (m)
10762 3556794 486090 90 Water Works 3556814 482872 3218 SE 10.53
Farmers Market 3550696 485748 6109 SE 5.74
Savannah Electric 3546000 488600 11083 SE 2.54
Savannah East President 3547850 495375 12893 SE 2.08
Brunswick, GA 3446292 454522 114944 SSW 0.18

direction, and atmospheric stability class ( A ±F ) also affect could be attributable to the Gaussian -plume model in this
model estimates. For example, two locations equidistant study would approximate that seen in flat terrain, or a factor
from a source but lying in different directional sectors may of 2.
experience different concentrations because of a combina- The height of the release of a source also has a strong
tion of different average wind speeds, directional frequen- impact on exposure estimates as shown in Table 2a and b.
cies, and stability classes for the two sectors. When the physical stack height was modeled as the release
Miller and Hively (1987 ) investigated the uncertainty of point of emissions (Table 2a) , predicted -to -observed
the Gaussian -plume model by summarizing ratios of model ratios at the ambient monitoring stations ranged from
predictions with corresponding experimental observations approximately 3 to 7 with a model bias of 3.74 ( r= 0.29 ).
( P /O ratios ) from numerous studies. Their data indicated However, when plume rise was incorporated into the model
that for annual average predictions for landscapes with flat (Table 2b ), the predicted -to -observed ratios at the ambient
terrain and receptors located within 10 km of the source, the monitoring stations ranged from 0.79 to 1.47, with a model
uncertainty attributed to the Gaussian plume model was bias of only 1.05 (r =0.78 ). Plume rise effectively raises the
approximately a factor of 2 ( i.e., P / O is between 1/2 and 2 release point of stack emissions, and the higher the release
with probability 0.90 ). This model uncertainty increased to point, the smaller the ground -level concentration at the
a factor of 4 when the distance exceeded 10 km (up to 150 ambient monitoring sites. Data such as stack gas tempera-
km ) . ture, gas velocities, and diameters also affect the release
Based on a small number of studies for complex terrain point as calculated by Equation 2. This additional informa-
or coastal meteorology (the latter is the case for the region tion improved the accuracy of the model in predicting SO2
under study ), the Gaussian -plume estimate of uncertainty concentrations at the known ambient monitoring stations.
for long -term releases ranged from 0.1 to 10, or two orders Thus our stochastic model with a median geometric bias of
of magnitude. Because of the small variation in the P / O 0.99 (Table 3 ) would be considered a good predictor of
ratios (Table 2b ), approximately 30%, obtained from local SO2 concentrations at geographically known but unmoni-
monitoring data, and the fact that our study area was tored locations.
basically flat terrain, we considered the factor of 10 unduly
pessimistic for this work. Our deterministic model appeared
to behave more like that seen in flat terrain validation
studies. We therefore assumed that the uncertainty that

Figure 2. Percentile distribution of estimated SO2 exposures for cases Figure 3. Uncertainty distribution of SO2 exposures for cases and
and controls. controls.

Journal of Exposure Analysis and Environmental Epidemiology (1999) 9(6) 541


Rogers et al. Estimating environmental exposures to SO2

of other pollutants that are a part of the same continuum of


exposures. For example, because particulate matter has been
associated with adverse health outcomes (Abbey et al.,
1993; Ito et al., 1993; PoÈnkaÈ and Virtanen, 1996) , the
researcher must consider the potential of one pollutant
acting as a surrogate for another pollutant which has a direct
impact upon the health of individuals.
Lippmann and Thurston (1996 ) demonstrated that the
quantity of total particulate matter (TSP ) in the atmosphere
is closely correlated with the sulfate ion (SO4 2 ) and
suggested that since TSP has a major impact on public
health and quality of life, SO4 2 should be monitored as a
Figure 4. Logarithmic decline of exposure estimates with distance. metric for ambient TSP. Moreover, in studies in which
associations between an exposure and outcome are
significant, investigators may question the association as
Exposure Estimate one representing that of a surrogate exposure. This problem
The uncertainty distribution of exposures presented in was seen by Abbey et al. ( 1993 ), when, using ambient data,
Figure 3 represents a broad range of estimated ground - level they found a significant association between SO4 2 and
SO2 concentrations that may be seen over a 24- county area airway obstructive disease ( AOD ). However, when the
in south Georgia as a result of industrial emissions. Whereas association between TSP and AOD, and SO4 and AOD were
the annual averages of ambient SO2 from GAEPD tested together, only TSP was found to be associated with
( observed ) data ranged from 5.23 to 17.4 g/ m3 (Table AOD. Abbey et al. ( 1993 ) concluded that SO4 2 was a
2 ), with an average of approximately 14 g / m3, the surrogate pollutant that whose apparent effect was actually
variation in the stochastic model predicted exposures for attributable to TSP. These kinds of problems involving
both the case and control subjects ( Figure 3) , demonstrate multiple exposures seen by Abbey et al. ( 1993 ) and
how misclassification of exposure occurs in an ecologic Lippmann and Thurston ( 1996 ) could be resolved with
study. better descriptions of an individual's exposure to multiple
The exposure distribution shown in Figure 3 represent an pollutants.
environmental transport model - predicted estimate of an
external exposure at a specific location, a study subject's Model Limitations
residence. However, the use of such modeling techniques is There are five major limitations to the model estimates
usually only a first step in exposure assessment for developed for this study. First, the exposure estimates are
epidemiologic studies. Environmental pollutants to which based on annual source term data ( i.e., they assume that
the individual is exposed may take many pathways, and releases are constant over a year ) , and annual meteo-
estimating an individual's exposure requires assessing other rological data. We were not able to consider peak daily
potential pathways through which that person might be emission releases and daily changes in meteorology that
exposed. For example, in the study of exposures to may have increased a subject's chance for higher or lower
radionuclides, geographic and lifestyle parameters such as exposure. We did, however, attempt to incorporate some
time spent indoors versus time spent outdoors, time spent at uncertainty in our model that would express some
specific locations such as work or home or school, extremes in exposures. In addition, we are not able to
migration into and out of a study area, farming practices, define a critical time of exposure. Such information about
milk consumption, consumption of garden - fresh or canned time of exposure would strengthen the association
foods, and decay of the radionuclide all influence the between exposure and outcome in an epidemiologic study
exposure estimate (Lloyd et al., 1990; Stevens et al., 1990 ). (Rothman and Poole, 1988 ).
Second, factors such as chemical conversions of SO2 to
Multipollutants/ Surrogates SO4 2 and wet and dry deposition for chemicals such as
In studying exposures from industrial releases, researchers SO2, which generally take a few days ( Hanna et al., 1982 ),
must discriminate between the effects of multiple pollutants. were not modeled. Atmospheric transport models that
The industrial -emissions data obtained that we obtained include chemical conversions and deposition of SO2 have
from GAEPD included information on volatile organic been written and tested (Andresen and Tha Paw, 1985 ) and
compounds (VOCs), nitrogen dioxide ( NO2 ) , carbon could be used with enhanced data. However, as shown
monoxide (CO ), and total particulate matter (TSP ), as above, the model we used proved to be a good estimator of
well as information on SO2. To determine a pollutant's SO2 concentrations at the ambient monitoring stations
effect upon an outcome, one needs to investigate the effects without these additional parameters.

542 Journal of Exposure Analysis and Environmental Epidemiology (1999) 9(6)


Estimating environmental exposures to SO2 Rogers et al.

Third, parameters that were not modeled in this study application, which includes Savannah and Brunswick,
may also account for some uncertainty in the model. For Georgia.
example, the model bias at the 50th percentile ranged about
30% ( Table 3 ). Part of the discrepancy between the Statistical Questions
predicted and observed concentrations may be due to the The problem addressed here concerns the correlation matrix
effect of city buildings on wind patterns Savannah. Our that should be assigned to the Gaussian plume uncertainty
model does not account for changes in dispersion patterns as component when applied to multiple exposure locations.
the plume moves alternately through urban and rural The question is not of primary importance for the
regions. Neither does the model consider building wake predictions we have examined in this paper, but it could
effects and downwash (Hanna et al., 1982 ). However, these play a major role in studies where uncertainty distributions
phenomena are of greater concern for predictions near a involving multiple locations are crucial to estimates
source than for locations a few kilometers away. It would expected numbers of excess cases, given an exposure, or
have been advantageous to have more ambient monitoring test statistics.
data from more than five ambient monitoring sites in the Correlations among model uncertainties at different
study area. Additional monitoring data could have provided locations are induced by the distributions of release rates
a more complete evaluation of our model performance, but and plume rise parameters. These correlations will be
we were limited to the number of available SO2 monitoring affected by what is assumed about the joint distribution of
sites located within the study area. the model uncertainty. Intuition suggests that model
Fourth, the summary emissions data obtained from the uncertainties for nearby residences (e.g., next door ) should
GAEPD suggest that emissions from the monitored point be highly correlated. Therefore the model will tend to be in
sources in south Georgia have not fluctuated much in the error by about the same amount at the two locations when
last decade. These source - term data, however, may contain estimating annual average exposures. Those correlations for
some error that would directly affect the modeling exposure residences at great distances from each other may ( at least
estimates. We have attempted to account for this potential in some circumstances ) be uncorrelated and the model error
source of error by incorporating an uncertainty distribution differ for the two locations. Unfortunately we know of no
in the reported release estimate. Our source terms also are convincing quantification of such a correlation pattern.
based on data recorded for environmental monitoring However, it is possible to perform exposure calculations
purposes. Thus, we have no information on SO2 entering twice to answer the above question by assuming first that all
the environment from sources that are exempt from pairs of model uncertainties have correlation coefficient
maintaining data on emissions. Additional SO2 from = 1 ( highly correlated hypothesis ) and second that all
background sources such as automobiles and small pairs of model uncertainties are uncorrelated ( uncorrelated
industries would presumably add to ambient SO2 concen- hypothesis ). Sums of exposures have a larger variance
trations and would, if incorporated in our model, increase under the highly correlated hypothesis than under the
our estimates of SO2 concentrations to which residents were uncorrelated hypothesis ( Wilks, 1962 ). Presumably, it may
exposed. However, SO2 concentrations that the model occur that under one hypothesis a test statistic gives
predicts at the monitoring stations closely approximates significant results, but fails to do so under the other
what is being recorded at these stations, and the monitored hypothesis.
concentrations should include any background contribu- The handling of correlations is an unresolved question
tions of SO2. that requires attention for most environmental assessments
Fifth, the meteorological data used in this study come involving airborne transport of pollutants. If the structure of
from the only meteorological recording station in the area. the correlation matrix were known, and if the number of
This limited set of meteorological data has been used to receptors is moderately large, the size of the correlation
portray the weather patterns of a large area of south Georgia. matrix can be a barrier to the Monte Carlo calculations. For
There are no available monitoring data to test the accuracy example, to implement the desired simulations for 1000
of the model for the inland areas of south Georgia. Also, the locations, a matrix of 500,000 pairs of correlated samples
Gaussian plume model is known to have less predictive must be generated. However, given the structure of the
capability in coastal regions ( Miller and Hively, 1987 ) than matrix and the nature of the statistical estimates and tests to
in inland areas with flat terrain. However, the stochastic be carried out, there may be approximations that can give
model predictions of all available monitoring locations, with some information, if not everything the investigator might
a geometric bias of 0.99, suggests that factor-of -ten desire. For example, if the purpose is to estimate numbers of
uncertainties generally applicable to a Gaussian plume's health effects as being proportional to collective exposure,
usage in coastal regions might be overly pessimistic in this then the variable of interest is the sum of exposure over all
case, and within this resolution we believe the model should locations. Even if the correlation matrix is unknown, it is
be considered reasonably accurate for the present domain of possible to show that the coefficient of variation of the sum

Journal of Exposure Analysis and Environmental Epidemiology (1999) 9(6) 543


Rogers et al. Estimating environmental exposures to SO2

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