Anne M. Riederer

Urinary Cadmium in the 1999–2008 U.S. National Health and Nutrition Examination Survey (NHANES)

Chronic low-level cadmium (Cd) exposure is linked to kidney and cardiovascular disease, fractures, and cancer. Diet and smoking are primary sources of exposure in the general population. We analyzed urinary Cd in NHANES 1999-2008 to determine whether levels declined significantly over the decade for U.S. children, teens, and adults (nonsmokers and smokers) and, if so, factors influencing the decline(s). For each subpopulation, we modeled log urinary Cd using variable-threshold censored multiple regression. Models included individual-level covariates (age, gender, BMI, income, race/ethnicity/country of origin, education, survey period), smoking, housing (home age, water source, filter use), and diet (supplement use; 24-h calorie, fat, protein, micronutrient, and Cd-containing food intakes), creatinine, and survey year variables. Geometric mean urinary Cd (ng/mL) declined 20-25% in these subpopulations, and the regressions showed statistically significant declines in later years for teens and adults. While certain covariates were significantly associated with Cd by subpopulation (creatinine; age; BMI; race/ethnicity/origin; education; smokers in the home; serum cotinine; 24-h fat, Mg, Fe intakes; use of dietary supplements), they did not help explain the declines. Instead, unidentified time-related factors appeared responsible. Despite the declines, millions of Americans remain potentially at risk of adverse outcomes associated with low-level Cd exposure.

Diet and Nondiet Predictors of Urinary 3-Phenoxybenzoic Acid in NHANES 1999-2002

Background 3-Phenoxybenzoic acid (3PBA), a pyrethroid metabolite, was detected in 75% of urine samples analyzed for pesticides in the U.S. National Health and Nutrition Examination Survey (NHANES) 1999–2002. NHANES also includes 24-hr diet data and information on household pesticide use, activities, occupation, demographics, and other exposure factors. Objectives The objective of our study was to explore the relative importance of diet versus nondiet predictors in explaining variability in urinary 3PBA. A secondary objective was to explore whether the NHANES data could be used to identify particular foods driving 3PBA levels. Methods We divided subjects into child (6–10 years of age), teen (11–18 years), and adult (≥ 19 years) age groups and restricted our analyses to subjects in the morning sampling session who fasted for ≥ 8 hr beforehand. Regression modeling consisted of several model-building steps and a final Tobit regression on the left-censored log 3PBA measurements. We also conducted bootstrap analyses to evaluate the stability of the regression parameters. Results Reported household pesticide use was not significantly associated with urinary 3PBA in any age group. Diet was significant for all three groups, and certain foods appeared to contribute more than others. Among adults, tobacco use was positively associated with 3PBA (p = 0.0326), and positive associations were suggested with the number of cytochrome p450–inhibiting medications taken (p = 0.0652) and minutes spent gardening (p = 0.0613) in the past month. Conclusions Although exploratory, our findings underline the importance of collecting accurate data on household pesticide use and dietary intake when evaluating pyrethroid exposure–biomarker relationships.

Method for the determination of organophosphorus and pyrethroid pesticides in food via gas chromatography with electron-capture detection.

We have developed a rapid, high-throughput, accurate, multiresidue method for the analysis of selected organophosphorus and pyrethroid pesticides in a variety of food samples suitable for use in public health and epidemiologic investigations of high-use pesticides using modifications of existing methods. The procedure involves a pesticide extraction from the food sample with acetonitrile followed by a salting-out with NaCl and cleanup of the extract with a multilayer solid-phase extraction cartridge composed of a Supelclean ENVI-CARB-II top layer and a primary-secondary amine bottom layer separated by a polyethylene frit. To evaluate the method, we performed fortification studies at 50, 100, and 200 ng/g for 3 organophosphorus and 4 pyrethroid pesticides in 16 different foods. Instrumental analysis was carried out by capillary gas chromatography with electron-capture detection (GC-ECD). Confirmatory analysis was performed by GC coupled with mass spectrometry (MS) in the selected-ion monitoring (SIM) mode. Average recoveries for each fortification level ranged from 49 to 146% with 80% of recoveries between 80 and 120%.

Method for the quantification of current use and persistent pesticides in cow milk, human milk and baby formula using gas chromatography tandem mass spectrometry

The aim of this study was to develop an analytical method for the quantification of organochlorine (OC), organophosphate (OP), carbamate, and pyrethroid insecticide residues in cow milk, human milk, and baby formula. A total of 25 compounds were included in this method. Sample extraction procedures combined liquid-liquid extraction, freezing-lipid filtration, dispersive primary-secondary amine cleanup, and solid-phase extraction together for effective extraction and elimination of matrix interferences. Target compounds were analyzed using gas chromatography with electron impact ionization-tandem mass spectrometry (GC-EI-MS/MS) in the multiple reaction monitoring (MRM) mode. Average extraction recoveries obtained from cow milk samples fortified at two different concentrations (10 ng/mL and 25 ng/mL), ranged from 34% to 102%, with recoveries for the majority of target compounds falling between 60% and 80%. Similar ranges were found for formula fortified at 25 ng/mL. The estimated limits of detection for most target analytes were in the low pg/mL level (range 3-1600 pg/mL). The accuracies and precisions were within the range of 80-120% and less than 15%, respectively. This method was tested for its viability by analyzing 10 human milk samples collected from anonymous donors, 10 cow milk samples and 10 baby formula samples purchased from local grocery stores in the United States. Hexachlorobenzene, p,p-dicofol, o,p-DDE, p,p-DDE, and chlorpyrifos were found in all samples analyzed. We found detectable levels of permethrin, cyfluthrin, and fenvalerate in some of the cow milk samples but not in human milk or baby formula samples. Some of the pesticides, such as azinphos-methyl, heptachlor epoxide, and the pesticide synergist piperonyl butoxide, were detected in some of the cow milk and human milk samples but not in baby formula samples.

Pyrethroid and organophosphorus pesticides in composite diet samples from Atlanta, USA adults.

Four pyrethroid (permethrin, cyfluthrin, cypermethrin, deltamethrin) and 3 organophosphorus (chlorpyrifos, diazinon, malathion) pesticides were measured in 4 days of 24 h duplicate diet samples collected from 12 Atlanta adults over two cycles (2005-2006). Samples were composited into 9 categories, by food type, to evaluate their contribution to daily intakes. The resulting 437 samples were analyzed using a multiresidue method using liquid-liquid and solid-phase extraction followed by quantification via gas chromatograph with electron-capture detection. Total daily intakes (mg/kg-d) were calculated by summing the mass of a pesticide in all composites collected that day and dividing by body weight. Chlorpyrifos, diazinon, and cypermethrin in were detected in a range of composite types at frequencies > or =30%, whereas other pesticides were detected at lower frequencies. Concentrations ranged from the detection limits (0.38-0.88 ng/g) to several hundred ng/g, exceeding U.S. tolerances in a few cases. We also detected pesticides in some foods labeled organic. Total daily intakes were below the U.S. Environmental Protection Agencys oral reference doses, except in 6% of cases when the organophosphorus concentrations were summed. Results show frequent dietary exposure of our participants to the target pesticides from a range of food types.

Predictors of blood trihalomethane concentrations in NHANES 1999-2006.

Background: Trihalomethanes (THMs) are water disinfection by-products that have been associated with bladder cancer and adverse birth outcomes. Four THMs (bromoform, chloroform, bromodichloromethane, dibromochloromethane) were measured in blood and tap water of U.S. adults in the National Health and Nutrition Examination Survey (NHANES) 1999–2006. THMs are metabolized to potentially toxic/mutagenic intermediates by cytochrome p450 (CYP) 2D6 and CYP2E1 enzymes. Objectives: We conducted exploratory analyses of blood THMs, including factors affecting CYP2D6 and CYP2E1 activity. Methods: We used weighted multivariable regressions to evaluate associations between blood THMs and water concentrations, survey year, and other factors potentially affecting THM exposure or metabolism (e.g., prescription medications, cruciferous vegetables, diabetes, fasting, pregnancy, swimming). Results: From 1999 to 2006, geometric mean blood and water THM levels dropped in parallel, with decreases of 32%–76% in blood and 38%–52% in water, likely resulting, in part, from the lowering of the total THM drinking water standard in 2002–2004. The strongest predictors of blood THM levels were survey year and water concentration (n = 4,232 total THM; n = 4,080 bromoform; n = 4,582 chloroform; n = 4,374 bromodichloromethane; n = 4,464 dibromochloromethane). We detected statistically significant inverse associations with diabetes and eating cruciferous vegetables in all but the bromoform model. Medications did not consistently predict blood levels. Afternoon/evening blood samples had lower THM concentrations than morning samples. In a subsample (n = 230), air chloroform better predicted blood chloroform than water chloroform, suggesting showering/bathing was a more important source than drinking. Conclusions: We identified several factors associated with blood THMs that may affect their metabolism. The potential health implications require further study. Citation: Riederer AM, Dhingra R, Blount BC, Steenland K. 2014. Predictors of blood trihalomethane concentrations in NHANES 1999–2006. Environ Health Perspect 122:695–702; http://dx.doi.org/10.1289/ehp.1306499

Mapping Global Environmental Lead Poisoning in Children

Background. Despite major reductions in environmental lead contamination and mean blood lead levels (BLLs) in children, hotspot lead exposure remains a concern for children globally. Recent mass lead intoxication events in Senegal (2008) and Nigeria (since 2010) illustrate the potential severity of such exposures in children. Objectives. The authors created a global map of childrens BLLs from the published literature and from sites where Blacksmith Institute has worked to remediate lead contamination. This project is intended to draw attention to the continued existence of lead hotspots in the developing world and to underline the need for investigation in regions where data is of poor quality or nonexistent. Methods. The authors collected data from the published literature through a PubMed literature search, and unpublished data from Blacksmith cleanup sites. Eligible studies measured blood lead levels in children (age < 18) using a standard laboratory method or the LeadCare® instrument and test kit, an...

Current and Historically Used Pesticides in Residential Soil from 11 Homes in Atlanta, Georgia, USA

We used a multiresidue, gas chromatography/mass spectrometry-based method to measure seven pyrethroid, five organophosphorus (OP), and six organochlorine pesticides in soil collected from 11 Atlanta homes in 2006. Our objective was to collect preliminary data for a larger study of pesticide exposures among Atlanta children. The pyrethroid insecticides (cis- and trans-permethrin, bioallethrin) were the most commonly detected analytes, giving evidence of widespread outdoor use among our study homes. Our pyrethroid insecticide detection frequencies were higher than those reported in a recent study of Ohio and North Carolina homes; however, our maximum values were approximately half of those reported. We detected the target OP pesticides in only a few samples, but we found two restricted-use OP pesticides—methyl parathion and terbufos—and thus possible evidence of illegal residential use or environmental persistence in soil. We also detected dichlorodiphenyltrichloroethane (DDT) and dichlorodiphenyldichloroethane (DDE) in samples from six homes. Although our small sample size limits comparison to other studies, our results provide evidence that residential soil is a potential source of human exposure to both current and historically used pesticides.

Associations of maternal organophosphate pesticide exposure and PON1 activity with birth outcomes in SAWASDEE birth cohort, Thailand

Prenatal organophosphate (OP) pesticide exposure has been reported to be associated with adverse birth outcomes and neurodevelopment. However, the mechanisms of toxicity of OP pesticides on human fetal development have not yet been elucidated. Our pilot study birth cohort, the Study of Asian Women and Offsprings Development and Environmental Exposures (SAWASDEE cohort) aimed to evaluate environmental chemical exposures and their relation to birth outcomes and infant neurodevelopment in 52 pregnant farmworkers in Fang district, Chiang Mai province, Thailand. A large array of data was collected multiple times during pregnancy including approximately monthly urine samples for evaluation of pesticide exposure, three blood samples for pesticide-related enzyme measurements and questionnaire data. This study investigated the changes in maternal acetylcholinesterase (AChE) and paraoxonase 1 (PON1) activities and their relation to urinary diakylphosphates (DAPs), class-related metabolites of OP pesticides, during pregnancy. Maternal AChE, butyrylcholinesterase (BChE) and PON1 activities were measured three times during pregnancy and urinary DAP concentrations were measured, on average, 8 times from enrollment during pregnancy until delivery. Among the individuals in the group with low maternal PON1 activity (n=23), newborn head circumference was negatively correlated with log10 maternal ∑DEAP and ∑DAP at enrollment (gestational age=12±3 weeks; β=-1.0 cm, p=0.03 and β=-1.8 cm, p<0.01, respectively) and at 32 weeks pregnancy (β=-1.1cm, p=0.04 and β=-2.6 cm, p=0.01, respectively). Furthermore, among these mothers, newborn birthweight was also negatively associated with log10 maternal ∑DEAP and ∑DAP at enrollment (β=-219.7 g, p=0.05 and β=-371.3g, p=0.02, respectively). Associations between maternal DAP levels and newborn outcomes were not observed in the group of participants with high maternal PON1 activity. Our results support previous findings from US birth cohort studies. This is the first study to report the associations between prenatal OP pesticide exposure and birth outcomes in Thailand.

A Method to screen U.S. environmental biomonitoring data for race/ethnicity and income-related disparity

BackgroundEnvironmental biomonitoring data provide one way to examine race/ethnicity and income-related exposure disparity and identify potential environmental justice concerns.MethodsWe screened U.S. National Health and Nutrition Examination Survey (NHANES) 2001–2008 biomonitoring data for 228 chemicals for race/ethnicity and income-related disparity. We defined six subgroups by race/ethnicity—Mexican American, non-Hispanic black, non-Hispanic white—and income—Low Income: poverty income ratio (PIR) <2, High Income: PIR ≥ 2. We assessed disparity by comparing the central tendency (geometric mean [GM]) of the biomonitoring concentrations of each subgroup to that of the reference subgroup (non-Hispanic white/High Income), adjusting for multiple comparisons using the Holm-Bonferroni procedure.ResultsThere were sufficient data to estimate at least one geometric mean ratio (GMR) for 108 chemicals; 37 had at least one GMR statistically different from one. There was evidence of potential environmental justice concern (GMR significantly >1) for 12 chemicals: cotinine; antimony; lead; thallium; 2,4- and 2,5-dichlorophenol; p,p’-dichlorodiphenyldichloroethylene; methyl and propyl paraben; and mono-ethyl, mono-isobutyl, and mono-n-butyl phthalate. There was also evidence of GMR significantly <1 for 25 chemicals (of which 17 were polychlorinated biphenyls).ConclusionsAlthough many of our results were consistent with the U.S. literature, findings relevant to environmental justice were novel for dichlorophenols and some metals.