Assessing the Impact of Wildfires on the Use of Black Carbon as an Indicator of Traffic Exposures in Environmental Epidemiology Studies.

Epidemiological studies frequently use black carbon (BC) as a proxy for traffic-related air pollution (TRAP). However, wildfire smoke (WFS) represents an important source of BC not often considered when using BC as a proxy for TRAP. Here, we examined the potential for WFS to bias TRAP exposure assessments based on BC measurements. Weekly integrated BC samples were collected across the Denver, CO region from May to November 2018. We collected 609 filters during our sampling campaigns, 35% of which were WFS-impacted. For each filter we calculated an average BC concentration. We assessed three GIS-based indicators of TRAP for each sampling location: annual average daily traffic within a 300 m buffer, the minimum distance to a highway, and the sum of the lengths of roadways within 300 m. Median BC concentrations were 9% higher for WFS-impacted filters (median = 1.14 µg/m3, IQR = 0.23 µg/m3) than nonimpacted filters (median = 1.04 µg/m3, IQR = 0.48 µg/m3). During WFS events, BC concentrations were elevated and expected spatial gradients in BC were reduced. We conducted a simulation study to estimate TRAP exposure misclassification as the result of regional WFS. Our results suggest that linear health effect estimates were biased away from the null when WFS was present. Thus, exposure assessments relying on BC as a proxy for TRAP may be biased by wildfire events. Alternative metrics that account for the influence of "brown" carbon associated with biomass burning may better isolate the effects of traffic emissions from those of other black carbon sources.

Metabolites of a tobacco-specific lung carcinogen in the urine of elementary school-aged children.

Limited data are available in the literature on carcinogen uptake by children exposed to environmental tobacco smoke (ETS). In this study, we quantified metabolites of the tobacco-specific lung carcinogen 4-(methylnitrosamino)-1-(3-pyridyl)-1-butanone (NNK) in the urine of elementary school-aged children participating in the School Health Initiative: Environment, Learning, Disease study, a school-based investigation of the environmental health of children. The metabolites of NNK are 4-(methylnitrosamino)-1-(3-pyridyl)-1-butanol (NNAL) and its glucuronide (NNAL-Gluc). We also measured cotinine and its glucuronide (total cotinine). Urine samples were collected from 204 children. Seventy (34.3%) of these had total cotinine > or =5 ng/ml. NNAL or NNAL-Gluc was detected in 52 of 54 samples with total cotinine > or =5 ng/ml and in 10 of 20 samples with total cotinine < 5 ng/ml. Levels of NNAL plus NNAL-Gluc and total cotinine were significantly higher when exposure to ETS was reported than when no exposure was reported. However, even when no exposure to ETS was reported, levels of NNAL, NNAL-Gluc, and NNAL plus NNAL-Gluc were higher than in children with documented low exposure to ETS, as determined by cotinine levels < 5 ng/ml. Levels of NNAL, NNAL-Gluc, and cotinine were not significantly different in samples collected twice from the same children at 3-month intervals. Levels of NNAL plus NNAL-Gluc in this study were comparable with those observed in our previous field studies of adults exposed to ETS. There was a 93-fold range of NNAL plus NNAL-Gluc values in the exposed children. The results of this study demonstrate widespread and considerable uptake of the tobacco-specific lung carcinogen NNK in this group of elementary school-aged children, raising important questions about potential health risks. Our data indicate that objective biomarkers of carcinogen uptake are important in studies of childhood exposure to ETS and cancer later in life.

Measurement of children's exposure to pesticides: analysis of urinary metabolite levels in a probability-based sample.

The Minnesota Children's Pesticide Exposure Study is a probability-based sample of 102 children 3-13 years old who were monitored for commonly used pesticides. During the summer of 1997, first-morning-void urine samples (1-3 per child) were obtained for 88% of study children and analyzed for metabolites of insecticides and herbicides: carbamates and related compounds (1-NAP), atrazine (AM), malathion (MDA), and chlorpyrifos and related compounds (TCPy). TCPy was present in 93% of the samples, whereas 1-NAP, MDA, and AM were detected in 45%, 37%, and 2% of samples, respectively. Measured intrachild means ranged from 1.4 microg/L for MDA to 9.2 microg/L for TCPy, and there was considerable intrachild variability. For children providing three urine samples, geometric mean TCPy levels were greater than the detection limit in 98% of the samples, and nearly half the children had geometric mean 1-NAP and MDA levels greater than the detection limit. Interchild variability was significantly greater than intrachild variability for 1-NAP (p = 0.0037) and TCPy (p < 0.0001). The four metabolites measured were not correlated within urine samples, and children's metabolite levels did not vary systematically by sex, age, race, household income, or putative household pesticide use. On a log scale, mean TCPy levels were significantly higher in urban than in nonurban children (7.2 vs. 4.7 microg/L; p = 0.036). Weighted population mean concentrations were 3.9 [standard error (SE) = 0.7; 95% confidence interval (CI), 2.5, 5.3] microg/L for 1-NAP, 1.7 (SE = 0.3; 95% CI, 1.1, 2.3) microg/L for MDA, and 9.6 (SE = 0.9; 95% CI, 7.8, 11) microg/L for TCPy. The weighted population results estimate the overall mean and variability of metabolite levels for more than 84,000 children in the census tracts sampled. Levels of 1-NAP were lower than reported adult reference range concentrations, whereas TCPy concentrations were substantially higher. Concentrations of MDA were detected more frequently and found at higher levels in children than in a recent nonprobability-based sample of adults. Overall, Minnesota children's TCPy and MDA levels were higher than in recent population-based studies of adults in the United States, but the relative magnitude of intraindividual variability was similar for adults and children.

Quantitative analysis of children's microactivity patterns: The Minnesota Children's Pesticide Exposure Study.

The National Human Exposure Assessment Survey (NHEXAS)/Minnesota Children's Pesticide Exposure Study (MNCPES) was a population-based study designed to characterize children's exposure to residential pesticides and to evaluate the contribution of residential and children's activities to children's exposure. Families of 168 children were surveyed for residential use of pesticides and children's activities. From these homes, families of 102 children between the ages of 3 and 13 years participated in a week-long intensive exposure study. Of the 102 children, 19 children were videotaped for four consecutive hours in their normal daily activities. The survey responses indicated that the youngest children were more likely to exhibit behaviors that would foster exposure to environmental contaminants. Comparison of questionnaire responses indicated that the videotaped subsample was representative of the exposure study population. The microactivities of the videotaped children that might contribute to their exposure via ingestion or dermal routes were quantified. Hand-to-mouth and object-to-mouth activities were observed most frequently among the youngest children. The youngest children were also most likely to be barefoot both indoors and outside. Gender differences were found in mouthing behavior and the proportion of observed time spent outdoors.

House dust levels of selected insecticides and a herbicide measured by the EL and LWW samplers and comparisons to hand rinses and urine metabolites.

During the Minnesota Children's Pesticide Exposure Study (MNCPES), comparisons were made between the insecticide/herbicide loadings obtained with two household dust/insecticide or herbicide samplers: the Edwards and Lioy (EL) press sampler (used for dust collection from carpets or other surfaces) and the Lioy, Waimnan and Weisel (LWW) surface wipe sampler. The results were compared with hand rinse levels, and urine metabolite levels obtained from 102 children (ages 3-13). All measurements were made during a 1-week sampling period, and information was obtained on household pesticide use and each child's activities. Of the homes, <5% had recent spot uses of a pesticide but none had recent general applications. The analyses focused primarily on atrazine (a herbicide), and malathion, diazinon, and chlorpyrifos (insecticides). Metabolites were measured for atrazine, malathion and chlorpyrifos. The atrazine levels obtained using the EL indicate that this compound was transported into the home by an unquantified transport mechanism (e.g. tracking of soil). Two malathion hand rinse values exceeded >170 ng/cm2, suggesting that since indoor surface levels were low, these children had other sources of exposure. Atrazine, chlorpyrifos and malathion were detectable in >30% of the homes by the EL, LWW or hand rinse. Only chlorpyrifos had detectable levels in > or = 50% of the samples for all types, i.e. compound or metabolite, which is consistent with it being a common household pesticide. The median (and maximum) chlorpyrifos levels for the EL surface, EL carpet, LWW surface (two rooms), hand rinse, and urine metabolites were: 0.07 (32.6) ng/cm2; 0.07 (44.5) ng/cm2; 0.34 (3.64) ng/cm2; 0.42 (14.4) ng/cm2; 0.03 (2.14) ng/hand and 6.9 (59.0) microg/g, respectively. A strong correlation was found for chlorpyrifos between the EL surface and carpet samples. Chlorpyrifos levels detected by LWW had a different distribution and concentration range than the EL, indicating that it collected more than the surface dislodgeable insecticide. EL was directly comparable to the hand rinse or urine levels, but only the LWW had a weak correlation with hand rinse levels, suggesting that the children had other sources of chlorpyrifos exposure. Thus, mechanistic exposure studies are needed to more accurately establish exposure dose relationships in residential settings.

Comparison of short-term variations (15-minute averages) in outdoor and indoor PM2.5 concentrations.

Measurements of 15-min average PM2.5 concentrations were made with a real-time light-scattering instrument at both outdoor (central monitoring sites in three communities) and indoor (residential) locations over two seasons in the Minneapolis-St. Paul metropolitan area. These data are used to examine within-day variability of PM2.5 concentrations indoors and outdoors, as well as matched indoor-to-outdoor (I/O) ratios. Concurrent gravimetric measurements of 24-hr average PM2.5 concentrations were also obtained as a way to compare real-time measures with this more traditional metric. Results indicate that (1) within-day variability for both indoor and outdoor 15-min average PM2.5 concentrations was substantial and comparable in magnitude to day-to-day variability for 24-hr average concentrations; (2) some residences exhibited substantial variability in indoor aerosol characteristics from one day to the next; (3) peak values for indoor short-term (15-min) average PM2.5 concentrations routinely exceeded 24-hr average outdoor values by factors of 3-4; and (4) relatively strong correlations existed between indoor and outdoor PM2.5 concentrations for both 24-hr and 15-min averages.

Design strategy for assessing multi-pathway exposure for children: the Minnesota Children's Pesticide Exposure Study (MNCPES).

Although children are exposed to a variety of environmental hazards, including pesticides, there is a scarcity of information available to estimate exposures realistically. This article reports on one of the first attempts to measure multi-pathway pesticide exposures in a population-based sample of urban and non-urban children. A design strategy was developed to assess multi-pathway pesticide exposures in children using personal exposure measurements in combination with complimentary measurements of biological markers of exposure, concentrations in relevant environmental media, and time spent in important microenvironments and participating in exposure-related activities. Sample collection and analysis emphasized measurement of three insecticides (i.e., chlorpyrifos, diazinon, and malathion) and one herbicide (i.e., atrazine). These compounds were selected because of their frequent use, presence in multiple environmental media, expected population exposures, and related hazard/toxicity. The study was conducted during the summer of 1997 in Minnesota and involved a stratified sample of households with children ages 3-12 years. Participants resided in either (a) the cities of Minneapolis and St. Paul (urban households), or (b) Rice and Goodhue Counties just south of the metropolitan area (non-urban households). Results from a residential inventory documenting storage and use of products containing the target pesticides were used to preferentially select households where children were likely to have higher exposures. The study successfully obtained pesticide exposure data for 102 children, including measurements of personal exposures (air, hand rinse, duplicate diet), environmental concentrations (residential indoor/outdoor air, drinking water, residential surfaces, soil), activity patterns (obtained by questionnaire, diary, videotaping), and internal dose (metabolites in urine).

Pesticide storage and use patterns in Minnesota households with children.

As part of the National Human Exposure Assessment Survey (NHEXAS), residential pesticide storage and use patterns were evaluated in a population-based sample of Minnesota households with children aged 3-13. In-home interviews and inventories were conducted to identify pesticide products stored and used in and around 308 households. This statistically based sample represents more than 49,000 urban and rural households in the census tracts sampled. More than 850 unique products were identified using Environmental Protection Agency (EPA) registration numbers. Pesticide products were found in 97% and reported used in 88% of study households. Population-weighted mean values for pesticide storage and use were 6.0 and 3.1 products per household, respectively. The most common active ingredients found were diethyl toluamide (DEET) and related compounds, piperonyl butoxide, pyrethrins, dimethylamine 2-[2-methyl-4-chlorophenoxyl propionate (MCPA) and chlorpyrifos. Household socio-demographic characteristics explained little of the variability in pesticide storage and use patterns, and there were no significant differences in residential storage and use patterns between households located in urban versus non-urban census tracts. Although the prevalence of households with pesticide products was similar to recent national surveys, observed storage and use rates were almost twice those obtained in recent national studies, reflecting improved inventory techniques used by this study and/or increased rates of pesticide presence and use in study households.

Measurement of multi-pollutant and multi-pathway exposures in a probability-based sample of children: practical strategies for effective field studies.

The purpose of this manuscript is to describe the practical strategies developed for the implementation of the Minnesota Children's Pesticide Exposure Study (MNCPES), which is one of the first probability-based samples of multi-pathway and multi-pesticide exposures in children. The primary objective of MNCPES was to characterize children's exposure to selected pesticides through a combination of questionnaires, personal exposure measurements (i.e., air, duplicate diet, hand rinse), and complementary monitoring of biological samples (i.e., pesticide metabolites in urine), environmental samples (i.e., residential indoor/outdoor air, drinking water, dust on residential surfaces, soil), and children's activity patterns. A cross-sectional design employing a stratified random sample was used to identify homes with age-eligible children and screen residences to facilitate oversampling of households with higher potential exposures. Numerous techniques were employed in the study, including in-person contact by locally based interviewers, brief and highly focused home visits, graduated subject incentives, and training of parents and children to assist in sample collection. It is not feasible to quantify increases in rates of subject recruitment, retention, or compliance that resulted from the techniques employed in this study. Nevertheless, results indicate that the total package of implemented procedures was instrumental in obtaining a high percentage of valid samples for targeted households and environmental media.

A school-based strategy to assess children's environmental exposures and related health effects in economically disadvantaged urban neighborhoods.

The School Health Initiative: Environment, Learning, Disease (SHIELD) study is a novel school-based investigation of children's environmental health in economically disadvantaged urban neighborhoods of Minneapolis. This article describes the study design and summarizes lessons learned about recruiting and monitoring this historically understudied population. The SHIELD study focused on measuring children's exposures to multiple environmental stressors [volatile organic chemicals (VOCs), environmental tobacco smoke, allergens, bioaerosols, metals, pesticides, polychlorinated biphenyls (PCB), phthalates] and exploring related effects on respiratory health (e.g., lung function) and learning outcomes (e.g., standardized test scores, academic achievement). It involved intensive exposure monitoring, including environmental measurements inside and outside the children's schools and inside their homes, personal measurements with passive dosimeters worn by the children, and biological marker measurements in blood and urine. The SHIELD participants comprised a stratified random sample of 153 "index" children and 51 of their siblings enrolled in grades 2-5 at two adjacent elementary schools. The Minneapolis Public Schools (MPS) assisted with identifying, contacting, recruiting, and monitoring this population, which traditionally is difficult to study because families/children are highly mobile, speak a diversity of languages, frequently do not have a telephone, endure economic hardships, often do not trust researchers, and have a spectrum of unconventional lifestyles and living arrangements. Using a school-based approach, the overall SHIELD enrollment (response) rate was 56.7%, with a wide disparity between English-speaking (41.7%) and non-English-speaking (71.0%) families/children. Most children remained involved in the study through both monitoring sessions and exhibited an acceptable degree of compliance with study protocols, including providing blood and urine samples. Results indicate that it is both practical and affordable to conduct probability-based exposure studies in this population, but that it is also important to improve our understanding of factors (e.g., cultural, economic, psychological, social) affecting the willingness of families/children to participate in such studies, with special emphasis on developing cost-effective recruitment methods.

Looking at environmental justice from an environmental health perspective.

Although scientific evidence is scarce and uneven, there are mounting concerns that environmental health risks are borne disproportionately by members of the population who are poor and nonwhite. From an environmental health perspective, research to reduce critical uncertainties in health risk assessment must necessarily be at the heart of efforts to evaluate and resolve issues of environmental justice--helping to define the dimensions of the problem, understand its causes, and identify effective and efficient solutions. The full range of environmental health sciences, including exposure analysis, epidemiology, toxicology, biostatistics, and surveillance monitoring, is needed to build a strong scientific foundation for informed decision making. This is the best and surest way to promote health and safety for all members of our society, regardless of age, ethnicity, gender, health condition, race, or socioeconomic status.

The use of isotope ratios to apportion sources of lead in Jersey City, NJ, house dust wipe samples.

Lead stable isotope ratio (IR) analysis by inductively coupled plasma mass spectrometry was used to examine the relationship between sources of Pb in 22 dust wipe samples collected from 10 homes in Jersey City, NJ. Common lead sources examined included interior lead-based paints, exterior soils and street dusts, and indoor air. High correlations between IRs of wipe samples and both street dusts and exterior soils indicated these two exterior sources were indistinguishable. They were treated as a single exterior source in a source apportionment using IR matching and a simple mixing model. The upper-bound estimate of the contribution of interior lead-based paints to 10 floor- and eight sill-wipe samples was 56% and 50%, respectively. It was not possible to apportion sources in four of the 22 samples because wipe sample IRs were outside the range of measured sources. Examination of means obscures the variability in the data, however, as eight of the 18 apportioned samples matched interior or exterior source media. In most cases, however, sources from outside the home contribute as much Pb to house dust wipe samples as interior lead-based paints.

Lead in house dust: relationships between exposure metrics.

This paper examines the quantitative relationships between dust loading, lead loading, and lead concentration in house dust. Bare floor, interior sill, and carpet dust samples were collected in 216 Jersey City, New Jersey, homes using quantitative wipe and vacuum sampling techniques. Comparison of wipe and vacuum sample distributions for these homes indicated that lead loading was more variable than dust loading or lead concentration measured on floors, sills, or carpets. These data also indicated that increased lead loading on carpets relative to sills or floors was due to higher dust loading on carpets. Correlation analysis of wipe samples indicated that dust loading was more strongly correlated with lead loading on floors (r = 0.73) than on sills (r = 0.53), that dust loading was not correlated with lead concentration on either surface, and that lead loading and lead concentration were more strongly correlated in samples collected from sills (r = 0.81) than from floors (r = 0.65). Most importantly, carpets and rugs served as large reservoirs for house dust and consequently were a large potential source of dust exposure in children's common microenvironments.

Nitrogen dioxide exposure and urinary excretion of hydroxyproline and desmosine.

The relationship between average and peak personal exposure to nitrogen dioxide and urinary excretion of hydroxyproline and desmosine was investigated in a population of preschool children and their mothers. Weekly average personal nitrogen dioxide exposures for subjects who resided in homes with one or more potential nitrogen dioxide source (e.g., a kerosene space heater, gas stove, or tobacco smoke) ranged between 16.3 and 50.6 ppb (30.6 and 95.1 micrograms/m3) for children and between 16.9 and 44.1 ppb (12.8 and 82.9 micrograms/m3) for mothers. In these individuals, the hydroxyproline-to-creatinine and desmosine-to-creatinine ratios were unrelated to personal nitrogen dioxide exposure--even though continuous monitoring documented home nitrogen dioxide concentration peaks of 100-475 ppb lasting up to 100 h in duration. Significantly higher hydroxyproline-to-creatinine and desmosine-to-creatinine ratios were observed in children, compared with mothers (p < .001 and .003, respectively).