Fine and ultrafine particle exposures on 73 trips by car to 65 non-smoking restaurants in the San Francisco Bay Area.

A number of studies indicate cooking is a major source of exposure to particulate matter, but few studies have measured indoor air pollution in restaurants, where cooking predominates. We made 73 visits by car to 65 different non-smoking restaurants in 10 Northern California towns while carrying portable continuous monitors that unobtrusively measured ultrafine (down to 10 nm) and fine (PM2.5 ) particles to characterize indoor restaurant exposures, comparing them with exposures in the car. The mean ultrafine number concentrations in the restaurants on dinner visits averaging 1.4 h was 71 600 particles/cm3 , or 4.3 times the mean concentration on car trips, and 12.3 times the mean background concentration in the residence. Restaurants that cooked dinner in the same room as the patrons had higher ultrafine concentrations than restaurants with separate kitchens. Restaurant PM2.5 mass concentrations averaged 36.3 µg/m3 , ranging from 1.5 to 454 µg/m3 , but were relatively low on most visits: 43% of the indoor means were below 10 µg/m3 and 66% were below 20 µg/m3 , with 5.5% above 100 µg/m3 . Exposure to fine and ultrafine particles when visiting a restaurant exceeded the exposure a person received while traveling by car to and from the restaurant.

Ultrafine particles from electric appliances and cooking pans: experiments suggesting desorption/nucleation of sorbed organics as the primary source.

Ultrafine particles are observed when metal surfaces, such as heating elements in electric appliances, or even empty cooking pans, are heated. The source of the particles has not been identified. We present evidence that particles >10 nm are not emitted directly from the heating elements or the metal surfaces. Using repeated heating of an electric burner, several types of cooking pans, and a steam iron, the increase in the number of particles (>10 nm) can be reduced to 0. After the devices are exposed to indoor air for several hours or days, subsequent heating results in renewed particle production, suggesting that organic matter has sorbed on their surfaces. Also, after a pan has been heated to the point that no increase in particles is observed, washing with detergent results in copious production of particles the next time the pan is heated. These observations suggest that detergent residue and organics sorbed from indoor air are the sources of the particles. We hypothesize that organic compounds are thermally desorbed from the hot surface as gaseous molecules; as they diffuse from the hot air near the pan into cooler air, selected compounds exceed their saturation concentration and nucleation occurs.

Identifying and quantifying secondhand smoke in source and receptor rooms: logistic regression and chemical mass balance approaches.

Identifying and quantifying secondhand tobacco smoke (SHS) that drifts between multiunit homes is critical to assessing exposure. Twenty-three different gaseous and particulate measurements were taken during controlled emissions from smoked cigarettes and six other common indoor source types in 60 single-room and 13 two-room experiments. We used measurements from the 60 single-room experiments for (i) the fitting of logistic regression models to predict the likelihood of SHS and (ii) the creation of source profiles for chemical mass balance (CMB) analysis to estimate source apportionment. We then applied these regression models and source profiles to the independent data set of 13 two-room experiments. Several logistic regression models correctly predicted the presence of cigarette smoke more than 80% of the time in both source and receptor rooms, with one model correct in 100% of applicable cases. CMB analysis of the source room provided significant PM2.5 concentration estimates of all true sources in 9 of 13 experiments and was half-correct (i.e., included an erroneous source or missed a true source) in the remaining four. In the receptor room, CMB provided significant estimates of all true sources in 9 of 13 experiments and was half-correct in another two.

Controlled experiments measuring personal exposure to PM2.5 in close proximity to cigarette smoking.

Few measurements of exposure to secondhand smoke (SHS) in close proximity to a smoker are available. Recent health studies have demonstrated an association between acute (<2 h) exposures to high concentrations of SHS and increased risk of cardiovascular and respiratory disease. We performed 15 experiments inside naturally ventilated homes and 16 in outdoor locations, each with 2-4 non-smokers sitting near a cigarette smoker. The smoker's and non-smokers' real-time exposures to PM2.5 from SHS were measured by using TSI SidePak monitors to sample their breathing zones. In 87% of the residential indoor experiments, the smoker received the highest average exposure to SHS, with PM2.5 concentrations ranging from 50-630 µg/m(3) . During the active smoking period, individual non-smokers sitting within approximately 1 m of a smoker had average SHS exposures ranging from negligible up to >160 µg/m(3) of PM2.5 . The average incremental exposure of the non-smokers was higher indoors (42 µg/m(3) , n = 35) than outdoors (29 µg/m(3) , n = 47), but the overall indoor and outdoor frequency distributions were similar. The 10-s PM2.5 averages during the smoking periods showed great variability, with multiple high concentrations of short duration (microplumes) both indoors and outdoors.

Radioactive materials in biosolids: dose modeling.

The Interagency Steering Committee on Radiation Standards (ISCORS) has recently completed a study of the occurrence within the United States of radioactive materials in sewage sludge and sewage incineration ash. One component of that effort was an examination of the possible transport of radioactivity from sludge into the local environment and the subsequent exposure of humans. A stochastic environmental pathway model was applied separately to seven hypothetical, generic sludge-release scenarios, leading to the creation of seven tables of Dose-to-Source Ratios (DSR), which can be used in translating from specific activity in sludge into dose to an individual. These DSR values were then combined with the results of an ISCORS survey of sludge and ash at more than 300 publicly owned treatment works, to explore the potential for radiation exposure of sludge workers and members of the public. This paper provides a brief overview of the pathway modeling methodology employed in the exposure and dose assessments and discusses technical aspects of the results obtained.

The National Human Activity Pattern Survey (NHAPS): a resource for assessing exposure to environmental pollutants.

Because human activities impact the timing, location, and degree of pollutant exposure, they play a key role in explaining exposure variation. This fact has motivated the collection of activity pattern data for their specific use in exposure assessments. The largest of these recent efforts is the National Human Activity Pattern Survey (NHAPS), a 2-year probability-based telephone survey (n=9386) of exposure-related human activities in the United States (U.S.) sponsored by the U.S. Environmental Protection Agency (EPA). The primary purpose of NHAPS was to provide comprehensive and current exposure information over broad geographical and temporal scales, particularly for use in probabilistic population exposure models. NHAPS was conducted on a virtually daily basis from late September 1992 through September 1994 by the University of Maryland's Survey Research Center using a computer-assisted telephone interview instrument (CATI) to collect 24-h retrospective diaries and answers to a number of personal and exposure-related questions from each respondent. The resulting diary records contain beginning and ending times for each distinct combination of location and activity occurring on the diary day (i.e., each microenvironment). Between 340 and 1713 respondents of all ages were interviewed in each of the 10 EPA regions across the 48 contiguous states. Interviews were completed in 63% of the households contacted. NHAPS respondents reported spending an average of 87% of their time in enclosed buildings and about 6% of their time in enclosed vehicles. These proportions are fairly constant across the various regions of the U.S. and Canada and for the California population between the late 1980s, when the California Air Resources Board (CARB) sponsored a state-wide activity pattern study, and the mid-1990s, when NHAPS was conducted. However, the number of people exposed to environmental tobacco smoke (ETS) in California seems to have decreased over the same time period, where exposure is determined by the reported time spent with a smoker. In both California and the entire nation, the most time spent exposed to ETS was reported to take place in residential locations.

Mathematical models for predicting indoor air quality from smoking activity.

Much progress has been made over four decades in developing, testing, and evaluating the performance of mathematical models for predicting pollutant concentrations from smoking in indoor settings. Although largely overlooked by the regulatory community, these models provide regulators and risk assessors with practical tools for quantitatively estimating the exposure level that people receive indoors for a given level of smoking activity. This article reviews the development of the mass balance model and its application to predicting indoor pollutant concentrations from cigarette smoke and derives the time-averaged version of the model from the basic laws of conservation of mass. A simple table is provided of computed respirable particulate concentrations for any indoor location for which the active smoking count, volume, and concentration decay rate (deposition rate combined with air exchange rate) are known. Using the indoor ventilatory air exchange rate causes slightly higher indoor concentrations and therefore errs on the side of protecting health, since it excludes particle deposition effects, whereas using the observed particle decay rate gives a more accurate prediction of indoor concentrations. This table permits easy comparisons of indoor concentrations with air quality guidelines and indoor standards for different combinations of active smoking counts and air exchange rates. The published literature on mathematical models of environmental tobacco smoke also is reviewed and indicates that these models generally give good agreement between predicted concentrations and actual indoor measurements.

Investigations of the proximity effect for pollutants in the indoor environment.

More than a dozen indoor air quality studies have reported a large discrepancy between concentrations measured by stationary indoor monitors (SIMs) and personal exposure monitors (PEMs). One possible cause of this discrepancy is a source proximity effect, in which pollutant sources close to the respondent cause elevated and highly variable exposures. This paper describes three sets of experiments in a home using real-time measurements to characterize and quantify the proximity effect relative to a fixed distant location analogous to a SIM. In the first set of experiments, using sulfur hexafluoride (SF6) as a continuously emitting tracer pollutant from a point source, measurements of pollutant concentrations were made at different distances from the source under different air exchange rates and source strengths. A second set of experiments used a continuous point source of carbon monoxide (CO) tracer pollutant and an array of high time resolution monitors to collect simultaneous concentration readings at different locations in the room. A third set of experiments measured particle count density and particle-bound polycyclic aromatic hydrocarbon (PAH) concentrations emitted from a continuous particle point source (an incense stick) using two particle counters and two PAH monitors, and included human activity periods both before and during the source emission period. Results from the SF6 and CO experiments show that while the source is emitting, a source proximity effect can be seen in the increases in the mean and median and in the variability of concentrations closest to the source, even at a distance of 2.0 m from the source under certain settings of air exchange rate and source strength. CO concentrations at locations near the source were found to be higher and more variable than the predictions of the mass balance model. For particles emitted from the incense source, a source proximity effect was evident for the fine particle sizes (0.3 to 2.5 microm) and particle-bound PAH up to at least 1.0 m from the source. Analysis of spatial and temporal patterns in the data for the three tracer pollutants reveal marked transient elevations of concentrations as seen by the monitor, referred to as "microplumes," particularly at locations close to the source. Mixing patterns in the room show complex patterns and directional effects, as evidenced by the variable intensity of the microplume activity at different locations. By characterizing the spatial and temporal variability of pollutant concentrations in the home, the proximity effect can be quantified, leading to improved indoor monitoring designs and models of human exposure to air pollutants.

The effect of cigar smoking on indoor levels of carbon monoxide and particles.

To provide new information on environmental tobacco smoke (ETS) levels from cigars, we conducted three types of experiments: (1) Measurements of carbon monoxide (CO) during 15 controlled experiments in an office where several cigar brands were machine-smoked; (2) Measurements of CO or respirable suspended particles (RSP) and particle-bound polycyclic aromatic hydrocarbons (PAH) in a residence where two cigars were smoked by a person; and (3) Measurements of CO during two studies at cigar social events (where there were up to 18 cigars being smoked at a time) in which an investigator wore a concealed personal exposure monitor. Average concentrations of CO at the cigar social events were comparable to, or larger than, those observed on a freeway during rush hour traffic. A mass balance model that has been used successfully to predict ETS from cigarettes is used in this paper to obtain CO, RSP, and PAH emission factors (emission rate [mg/min], total mass emitted [mg], and emissions per mass smoked [mg/g]). The calculated emission factors show that the cigar can be a stronger source of CO than the cigarette. In contrast, the cigar may have fewer emissions of RSP and PAH per gram of consumed tobacco than the cigarette, but its size and longer smoking time results in greater total RSP and PAH emissions than for a single cigarette.

A quantitative definition of exposure and related concepts.

This paper develops a unified theoretical framework for understanding exposure to environmental pollutants and other agents. It reviews the scientific literature to describe the many diverse and often confusing ways in which the term "exposure" is being used. Using six criteria proposed for a useful framework, a set of quantitative definitions, which encompass and expand upon existing definitions, is developed. After "agent" (e.g., a pollutant) and "target" (e.g., a person's hand) are defined, "exposure" is defined as the contact between an agent and a target. An "instantaneous point exposure" is defined as the joint occurrence of two events: 1) point i of a target is located at (xi, yi, zi) at time t, and 2) an agent of concentration Ci is present at location (xi, yi, zi) at time t. It is shown that the definition of instantaneous point exposure is fundamental in that all other functions of exposure with respect to space or time-such as the average exposure and the integrated exposure-can be derived from it. Because exposure and dose are closely related and often confused, our framework also includes a general definition of dose that is consistent with common usage. Finally, the definitions in this unified theoretical framework are shown to apply to inhalation exposure, dermal exposure, and ingestion exposure. In addition to the literature review and the quantitative definitions of exposure, this paper includes a glossary of terms that are proposed to help establish a common language for the exposure sciences.

A mathematical model for predicting trends in carbon monoxide emissions and exposures on urban arterial highways.

The roadway is one of the most important microenvironments for human exposure to carbon monoxide (CO). To evaluate long-term changes in pollutant exposure due to in-transit activities, a mathematical model has been developed to predict average daily vehicular emissions on highways. By utilizing measurements that are specific for a given location and year (e.g., traffic counts, fleet composition), this model can predict emissions for a specific roadway during various time periods of interest, allowing examination of long-term trends in human exposure to CO. For an arterial highway in northern California, this model predicts that CO emissions should have declined by 58% between 1980 and 1991, which agrees fairly well with field measurements of human exposure taken along that roadway during those two years. An additional reduction of up to 60% in CO emissions is predicted to occur between 1991 and 2002, due solely to the continued replacement of older cars with newer, cleaner vehicles.

Human exposure assessment: the birth of a new science.

I am honored to have been selected to receive the 1995 Weselowski Award for Career Achievement in Exposure Assessment. When I think back to my friendship with Jerry Weselowski, I remember our discussions in 1991 about the need to define exposure rigorously and quantitatively. In fact, I sent Jerry a letter on that topic--the quantitative definition of exposure--on November 7, 1991. I think it is fitting, therefore, that I select one of the topics in my talk today from that letter. Jerry always welcomed full and open scientific debate and discussion, and I feel that the need to define exposure and to understand what it means is a topic of great importance in exposure assessment. I also want to offer some observations about the importance of our field for the public and the regulatory community and to suggest the directions that exposure assessment might take as it evolves as a profession. Finally, I hope to provide an up-to-date listing of some selected scientific papers that are relevant to our field.

Residential air exchange rates for use in indoor air and exposure modeling studies.

Data on air exchange rates are important inputs to indoor air quality models. Indoor air models, in turn, are incorporated into the structure of total human exposure models. Fragmentary data on residential ventilation rates are available in various governmental reports, journal articles, and contractor reports. Most of the published papers present data on only a few homes to answer very specialized questions, and none of these publications summarize the ventilation rates of a large population of homes across the United States. Brookhaven National Laboratory (BNL) has conducted more than 4000 residential perfluorocarbon tracer (PFT) measurements and brought them together into a large data base from about 100 studies in the United States and elsewhere. This paper analyzes the BNL PFT data base to generate frequency distributions and summary statistics for different regions of the United States, different seasons, and different levels within the homes. The data analyses suggest that residential ventilation rates are similar in the northeastern and northwestern states but higher in the southwestern states. Winter and fall ventilation rates are similar, but the rates are slightly higher in spring, and much higher in summer. Multi-level residences have higher air exchange rates than single-level residences. Although the BNL data are not a representative sample of homes in the United States, these analyses give insight into the range of air exchange rates found in the United States under a great variety of conditions and are intended for use by developers of models of indoor air quality and total human exposure.

Comparison of microenvironmental CO concentrations in two cities for human exposure modeling.

The microenvironmental components of the CO concentration in two cities are compared by subtracting the ambient background concentration from personal exposures measured in Denver, Colorado, and Washington, DC. Two surrogate measures for the ambient background concentration are tested. Both improve the similarity of the means in the two cities, but the Denver standard deviations are higher than those in Washington, DC. Microenvironments containing the internal combustion engine have both higher means and standard deviations in Denver compared with Washington, DC. The Washington, DC, mean concentration for automobiles, for example, was 59% of the Denver mean (2.0 ppm versus 4.9 ppm). Washington, DC, had approximately 57% of the Denver emissions, and the difference in mean CO concentrations is roughly consistent with the lower emissions in Washington, DC, due to lower elevation. A surprising finding is that mean CO exposure levels caused by cooking with gas stoves in Washington, DC, were only 58% of the levels in Denver (1.9 ppm and 3.3 ppm, respectively). This result suggests that elevation may exert an influence on gas stove emissions that is similar to its influence on internal combustion engines. Using an averaging time model, analysis of the autocorrelation of sleeping and office microenvironments suggests that considerable serial dependency exists. The microenvironmental data and findings in this paper have important implications for constructing human exposure-activity pattern models. For future human exposure field studies, the findings emphasize the importance of measuring background values in a location that is extremely close to each microenvironment studied.

Averaging time modeling of exposure simulation with application to the El Camino Real vehicle data.

When profiles of activity patterns are used to generate time series of simulated exposure, one typically samples from exposure distributions which are microenvironment-specific to each activity. If the simulation time step is short, then independent sampling at each time step, ignoring autocorrelation, will result in aggregates with too little variability from one simulation to another. Autocorrelation can often be modeled with one or two extra parameters and then used in the simulation. Furthermore, one may substantially reduce computation by generating a single averaged exposure for each activity segment whose distribution depends in a simple way on the activity duration and the modeled autocorrelation. The process is illustrated using the El Camino Real commuting exposure study data of Ott, Switzer, and Willits.

A physical explanation of the lognormality of pollutant concentrations.

Investigators in different environmental fields have reported that the concentrations of various measured substances have frequency distributions that are lognormal, or nearly so. That is, when the logarithms of the observed concentrations are plotted as a frequency distribution, the resulting distribution is approximately normal, or Gaussian, over much of the observed range. Examples include radionuclides in soil, pollutants in ambient air, indoor air quality, trace metals in streams, metals in biological tissue, calcium in human remains. The ubiquity of the lognormal distribution in environmental processes is surprising and has not been adequately explained, since common processes in nature (for example, computation of the mean and the analysis of error) usually give rise to distributions that are normal rather than lognormal. This paper takes the first step toward explaining why lognormal distributions can arise naturally from certain physical processes that are analogous to those found in the environment. In this paper, these processes are treated mathematically, and the results are illustrated in a laboratory beaker experiment that is simulated on the computer.

Total human exposure: basic concepts, EPA field studies, and future research needs.

Historically, environmental regulatory programs designed to protect public health have monitored pollutants only in geophysical carrier media (for example, outdoor air, streams, soil). Field studies have identified a gap between the levels observed in geophysical carrier media and the concentrations with which people actually come into contact: their daily exposures. A new approach--Total Human Exposure (THE)--has evolved to fill this gap and provide the critical data needed for accurately assessing public health risk. The THE approach considers a three-dimensional "bubble" around each person and measures the concentrations of all pollutants contacting that bubble, either through the air, food, water, or skin. Two basic THE approaches have emerged: (1) the direct approach using probability samples of populations and measuring pollutant concentrations in the food eaten, air breathed, water drunk, and skin contacted; and (2) the indirect approach using human activity pattern-exposure models to predict population exposure distributions. Using the direct approach, EPA has conducted over 20 field studies for pollutants representing four groups--volatile organic compounds, carbon monoxide, pesticides, and particles--in 15 cities in 12 states. The indirect modeling approach has been applied to several of these pollutants. Additional research is needed in a great variety of areas. Even from the few projects completed thus far, the THE approach has yielded a rich new data base for risk assessments and has provided many surprises about the relative contribution of various pollutant sources to public health risk.