James J Quackenboss

Distributions, associations, and partial aggregate exposure of pesticides and polynuclear aromatic hydrocarbons in the Minnesota Children's Pesticide Exposure Study (MNCPES).

The Minnesota Childrens Pesticide Exposure Study (MNCPES) provides exposure, environmental, and biologic data relating to multipathway exposures of children for four primary pesticides (chlorpyrifos, malathion, diazinon, and atrazine), 14 secondary pesticides, and 13 polynuclear aromatic hydrocarbons (PAHs). Monitoring was performed on a probability-based sample of 102 children aged 3–12 in Minneapolis/St. Paul and in a nearby rural area (Goodhue and Rice counties). This paper provides estimated distributions of this populations exposures and exposure-related measurements and examines associations among the various measures via rank (Spearman) correlations. In addition, it provides some aggregate and cumulative exposure estimates for pesticides, and compares the relative intakes from inhalation and dietary ingestion. Intakes for the four primary pesticides appeared to come principally from the ingestion rather than the inhalation route; this was clearly true for chlorpyrifos but was less certain for the other three primary pesticides because of their higher degree of nondetects. Solid food rather than beverages was clearly the main contributor to the ingestion intake. Despite the dominance of the ingestion route, the urinary metabolite of chlorpyrifos exhibited a stronger association with the air measurements than with the dietary measures. Personal-air samples exhibited strong rank correlations with indoor air samples for chlorpyrifos, malathion, and diazinon (0.81, 0.51, and 0.62, respectively), while personal-air atrazine levels correlated well with outdoor levels (0.69); personal-air diazinon levels also correlated well with outdoor levels (0.67). For the PAHs, many significant associations were evident among the various air samples and for the air samples with the dust samples, especially for those compounds with consistently high percent measurable values (particularly fluoranthene, phenanthrene, and pyrene).

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-chlorophenoxy] 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.

Determinants of temporal variability in NHEXAS-Maryland environmental concentrations, exposures, and biomarkers

The longitudinal NHEXAS-Maryland study measured metals, PAHs, and pesticides in several media to capture temporal variability. Questionnaires were concurrently administered to identify factors that influenced changes in contaminant levels over time. We constructed mixed-effects regression models for lead, phenanthrene, and chlorpyrifos (including metabolites) in indoor air, dust, dermal wipes, and biological fluids. Significant predictors represented time-varying activities as well as unchanging housing and demographic factors. There was little overlap among the models, with predictors generally reflecting the diverse characteristics of the target compounds. We estimated between- and within-person variance components to evaluate the reliability of the measurements. While only one measurement of lead in blood or chlopyrifos in dust was needed for a dependable estimate of an individuals average level, three to eight measurements were needed for most other compound/exposure medium combinations because of considerable temporal variability. Measurements in biological fluids and dust were generally more consistent than those in indoor air. The significant covariates in the full models preferentially reduced the between-person variance component. Since the regression models explained only 1–37% of the within-person variance, the questionnaires in this study provided only modest insight into the factors responsible for the temporal variability in the contaminant levels.

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).

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 Childrens 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, Wainman 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 childs 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 ≥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) µg/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.

Responses to the region 5 NHEXAS time/activity diary. National Human Exposure Assessment Survey:

The time/activity diary developed for use in the National Human Exposure Assessment Survey (NHEXAS) was completed by 249 participants in the Research Triangle Institute/Environmental and Occupational Health Sciences Institute (RTI/EOHSI) NHEXAS population-based pilot project conducted in the upper Midwest (EPA Region 5). The majority of participants successfully completed the diary during the 6-day study period. Participant responses showed internal consistency between related questions within the diary and between instruments used within the study. Comparison of response rates with the National Human Activity Pattern Survey, a nationwide population-based study, found consistent results when the same questions were used in both studies. Several questions identified age-specific activities. The value of the 6-day diary over 1-day surveys was apparent in discriminating between episodic and regularly conducted activities and in identifying subpopulations whose behavior may contribute to exposure to environmental pollutants.

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 Childrens 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 childrens 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 childrens 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.

An assessment of the data quality for NHEXAS - Part I: exposure to metals and volatile organic chemicals in Region 5

A National Human Exposure Assessment Survey (NHEXAS) was performed in U.S. Environmental Protection Agency (U.S. EPA) Region V, providing population-based exposure distribution data for metals and volatile organic chemicals (VOCs) in personal, indoor, and outdoor air, drinking water, beverages, food, dust, soil, blood, and urine. One of the principal objectives of NHEXAS was the testing of protocols for acquiring multimedia exposure measurements and developing databases for use in exposure models and assessments. Analysis of the data quality is one element in assessing the performance of the collection and analysis protocols used in NHEXAS. In addition, investigators must have data quality information available to guide their analyses of the study data. At the beginning of the program quality assurance (QA) goals were established for precision, accuracy, and method quantification limits. The assessment of data quality was complicated. First, quality control (QC) data were not available for all analytes and media sampled, because some of the QC data, e.g., precision of duplicate sample analysis, could be derived only if the analyte was present in the media sampled in at least four pairs of sample duplicates. Furthermore, several laboratories were responsible for the analysis of the collected samples. Each laboratory provided QC data according to their protocols and standard operating procedures (SOPs). Detection limits were established for each analyte in each sample type. The calculation of the method detection limits (MDLs) was different for each analytical method. The analytical methods for metals had adequate sensitivity for arsenic, lead, and cadmium in most media but not for chromium. The QA goals for arsenic and lead were met for all media except arsenic in dust and lead in air. The analytical methods for VOCs in air, water, and blood were sufficiently sensitive and met the QA goals, with very few exceptions. Accuracy was assessed as recovery from field controls. The results were excellent (≥98%) for metals in drinking water and acceptable (≥75%) for all VOCs except o-xylene in air. The recovery of VOCs from drinking water was lower, with all analytes except toluene (98%) in the 60–85% recovery range. The recovery of VOCs from drinking water also decreased when comparing holding times of <8 and >8 days. Assessment of the precision of sample collection and analysis was based on the percent relative standard deviation (% RSD) between the results for duplicate samples. In general, the number of duplicate samples (i.e., sample pairs) with measurable data were too few to assess the precision for cadmium and chromium in the various media. For arsenic and lead, the precision was excellent for indoor, and outdoor air (<10% RSD) and, although not meeting QA goals, it was acceptable for arsenic in urine and lead in blood, but showed much higher variability in dust. There were no data available for metals in water and food to assess the precision of collection and analysis.

Contributions of a Child’s Built, Natural, and Social Environments to Their General Cognitive Ability: A Systematic Scoping Review

The etiology of a child’s cognitive ability is complex, with research suggesting that it is not attributed to a single determinant or even a defined period of exposure. Rather, cognitive development is the product of cumulative interactions with the environment, both negative and positive, over the life course. The aim of this systematic scoping review was to collate evidence associated with children’s cognitive health, including inherent factors as well as chemical and non-chemical stressors from the built, natural, and social environments. Three databases were used to identify recent epidemiological studies (2003–2013) that examined exposure factors associated with general cognitive ability in children. Over 100 factors were evaluated from 258 eligible studies. We found that recent literature mainly assessed the hypothesized negative effects of either inherent factors or chemical exposures present in the physical environment. Prenatal growth, sleep health, lead and water pollutants showed consistent negative effects. Of the few studies that examined social stressors, results consistently showed cognitive development to be influenced by both positive and negative social interactions at home, in school or the community. Among behavioral factors related to diet and lifestyle choices of the mother, breastfeeding was the most studied, showing consistent positive associations with cognitive ability. There were mostly inconsistent results for both chemical and non-chemical stressors. The majority of studies utilized traditional exposure assessments, evaluating chemical and non-chemical stressors separately. Collective evidence from a limited number of studies revealed that cumulative exposure assessment that incorporates multiple chemical and non-chemical stressors over the life course may unravel the variability in effect on cognitive development and help explain the inconsistencies across studies. Future research examining the interactions of multiple stressors within a child’s total environment, depicting a more real-world exposure, will aid in understanding the cumulative effects associated with a child’s ability to learn.

Cost/variance optimization for human exposure assessment studies

The National Human Exposure Assessment Survey (NHEXAS) field study in EPA Region V (one of three NHEXAS field studies) provides extensive exposure data on a representative sample of 249 residents of the Great Lakes states. Concentration data were obtained for both metals and volatile organic compounds (VOCs) from multiple environmental media and from human biomarkers. A variance model for the logarithms of concentration measurements is used to define intraclass correlations between observations within primary sampling units (PSUs) (nominally counties) and within secondary sampling units (SSUs) (nominally Census blocks). A model for the total cost of the study is developed in terms of fixed costs and variable costs per PSU, SSU, and participant. Intraclass correlations are estimated for media and analytes with sufficient sample sizes. We demonstrate how the intraclass correlations and variable cost components can be used to determine the sample allocation that minimizes cost while achieving pre-specified precision constraints for future studies that monitor environmental concentrations and human exposures for metals and VOCs.