Silicone wristbands compared with traditional polycyclic aromatic hydrocarbon exposure assessment methods.

Currently there is a lack of inexpensive, easy-to-use technology to evaluate human exposure to environmental chemicals, including polycyclic aromatic hydrocarbons (PAHs). This is the first study in which silicone wristbands were deployed alongside two traditional personal PAH exposure assessment methods: active air monitoring with samplers (i.e., polyurethane foam (PUF) and filter) housed in backpacks, and biological sampling with urine. We demonstrate that wristbands worn for 48 h in a non-occupational setting recover semivolatile PAHs, and we compare levels of PAHs in wristbands to PAHs in PUFs-filters and to hydroxy-PAH (OH-PAH) biomarkers in urine. We deployed all samplers simultaneously for 48 h on 22 pregnant women in an established urban birth cohort. Each woman provided one spot urine sample at the end of the 48-h period. Wristbands recovered PAHs with similar detection frequencies to PUFs-filters. Of the 62 PAHs tested for in the 22 wristbands, 51 PAHs were detected in at least one wristband. In this cohort of pregnant women, we found more significant correlations between OH-PAHs and PAHs in wristbands than between OH-PAHs and PAHs in PUFs-filters. Only two comparisons between PAHs in PUFs-filters and OH-PAHs correlated significantly (rs = 0.53 and p = 0.01; rs = 0.44 and p = 0.04), whereas six comparisons between PAHs in wristbands and OH-PAHs correlated significantly (rs = 0.44 to 0.76 and p = 0.04 to <0.0001). These results support the utility of wristbands as a biologically relevant exposure assessment tool which can be easily integrated into environmental health studies. Graphical abstract PAHs detected in samples collected from urban pregnant women.

Chemical exposures in recently renovated low-income housing: Influence of building materials and occupant activities.

Health disparities in low-income communities may be linked to residential exposures to chemicals infiltrating from the outdoors and characteristics of and sources in the home. Indoor sources comprise those introduced by the occupant as well as releases from building materials. To examine the impact of renovation on indoor pollutants levels and to classify chemicals by predominant indoor sources, we collected indoor air and surface wipes from newly renovated "green" low-income housing units in Boston before and after occupancy. We targeted nearly 100 semivolatile organic compounds (SVOCs) and volatile organic compounds (VOCs), including phthalates, flame retardants, fragrance chemicals, pesticides, antimicrobials, petroleum chemicals, chlorinated solvents, and formaldehyde, as well as particulate matter. All homes had indoor air concentrations that exceeded available risk-based screening levels for at least one chemical. We categorized chemicals as primarily influenced by the occupant or as having building-related sources. While building-related chemicals observed in this study may be specific to the particular housing development, occupant-related findings might be generalizable to similar communities. Among 58 detected chemicals, we distinguished 25 as primarily occupant-related, including fragrance chemicals 6-acetyl-1,1,2,4,4,7-hexamethyltetralin (AHTN) and 1,3,4,6,7,8-hexahydro-4,6,6,7,8,8-hexamethylcyclopenta[g]-2-benzopyran (HHCB). The pre- to post-occupancy patterns of the remaining chemicals suggested important contributions from building materials for some, including dibutyl phthalate and xylene, whereas others, such as diethyl phthalate and formaldehyde, appeared to have both building and occupant sources. Chemical classification by source informs multi-level exposure reduction strategies in low-income housing.

Vinyl flooring in the home is associated with children's airborne butylbenzyl phthalate and urinary metabolite concentrations.

Prior studies have shown that vinyl flooring as well as the vinyl-softening plasticizers butylbenzyl phthalate (BBzP) and di(2-ethylhexyl) phthalate (DEHP) are associated with asthma and airway inflammation. Although DEHP exposure is primarily dietary, whether home vinyl flooring contributes to indoor air and urinary metabolite concentrations for these two phthalates is unclear. Exposures to BBzP and DEHP were examined in a prospective birth cohort of New York City children (n=239) using: (i) visual observation of potential phthalate containing flooring, (ii) a 2-week home indoor air sample, and (iii) concurrent urinary metabolites in a subset (n=193). The category "vinyl or linoleum" flooring was observed in 135 (56%) of monitored rooms; these rooms had statistically significantly higher indoor air geometric mean concentrations of BBzP (23.9 ng/m(3)) than rooms with wood or carpet flooring (10.6 ng/m(3)). Children from homes with "vinyl or linoleum" flooring also had significantly higher urinary BBzP metabolite concentrations than other children. Indoor air BBzP and urinary metabolite concentrations were correlated positively (Spearman's rho 0.40). By contrast, indoor air DEHP was not associated with flooring type nor with its urinary metabolite concentrations. Vinyl flooring in the home may be an important source of children's exposure to BBzP via indoor air.

Semivolatile organic compounds in homes: strategies for efficient and systematic exposure measurement based on empirical and theoretical factors.

Residential exposure can dominate total exposure for commercial chemicals of health concern; however, despite the importance of consumer exposures, methods for estimating household exposures remain limited. We collected house dust and indoor air samples in 49 California homes and analyzed for 76 semivolatile organic compounds (SVOCs)--phthalates, polybrominated diphenyl ethers (PBDEs), polychlorinated biphenyls (PCBs), polycyclic aromatic hydrocarbons (PAHs), and pesticides. Sixty chemicals were detected in either dust or air and here we report 58 SVOCs detected in dust for the first time. In dust, phthalates (bis(2-ethylhexyl) phthalate, benzyl butyl phthalate, di-n-butyl phthalate) and flame retardants (PBDE 99, PBDE 47) were detected at the highest concentrations relative to other chemicals at the 95th percentile, while phthalates were highest at the median. Because SVOCs are found in both gas and condensed phases and redistribute from their original source over time, partitioning models can clarify their fate indoors. We use empirical data to validate air-dust partitioning models and use these results, combined with experience in SVOC exposure assessment, to recommend residential exposure measurement strategies. We can predict dust concentrations reasonably well from measured air concentrations (R(2) = 0.80). Partitioning models and knowledge of chemical Koa elucidate exposure pathways and suggest priorities for chemical regulation. These findings also inform study design by allowing researchers to select sampling approaches optimized for their chemicals of interest and study goals. While surface wipes are commonly used in epidemiology studies because of ease of implementation, passive air sampling may be more standardized between homes and also relatively simple to deploy. Validation of passive air sampling methods for SVOCs is a priority.

Early-life cockroach allergen and polycyclic aromatic hydrocarbon exposures predict cockroach sensitization among inner-city children.

BACKGROUND: Sensitization to cockroach is one of the strongest identified risk factors for greater asthma morbidity in low-income urban communities; however, the timing of exposures relevant to the development of sensitization has not been elucidated fully. Furthermore, exposure to combustion byproducts, including polycyclic aromatic hydrocarbons (PAHs), can augment the development of allergic sensitization. OBJECTIVE: We sought to test the hypotheses that domestic cockroach allergen measured prenatally would predict cockroach sensitization in early childhood and that this association would be greater for children exposed to higher PAH concentrations. METHODS: Dominican and African American pregnant women living in New York City were enrolled. In the third trimester expectant mothers wore personal air samplers for measurement of 8 nonvolatile PAHs and the semivolatile PAH pyrene, and dust was collected from homes for allergen measurement. Glutathione-S-transferase µ 1 (GSTM1) gene polymorphisms were measured in children. Allergen-specific IgE levels were measured from the children at ages 2, 3, 5, and 7 years. RESULTS: Bla g 2 in prenatal kitchen dust predicted cockroach sensitization at the ages of 5 to 7 years (adjusted relative risk [RR], 1.15; P = .001; n = 349). The association was observed only among children with greater than (RR, 1.22; P = .001) but not less than (RR, 1.07; P = .24) the median sum of 8 nonvolatile PAH levels. The association was most pronounced among children with higher PAH levels and null for the GSTM1 gene (RR, 1.54; P = .001). CONCLUSIONS: Prenatal exposure to cockroach allergen was associated with a greater risk of allergic sensitization. This risk was increased by exposure to nonvolatile PAHs, with children null for the GSTM1 mutation particularly vulnerable.

Acetaminophen, pesticide, and diethylhexyl phthalate metabolites, anandamide, and fatty acids in deciduous molars: potential biomarkers of perinatal exposure.

The developing fetus is particularly vulnerable to adverse effects from pharmaceutical and exogenous chemical exposure. Deciduous teeth primarily form over specific periods from the second trimester in utero through the months after birth. We hypothesized that organic chemicals or their metabolites circulating in the bloodstream may sorb into forming dental tissues and remain stored in the tooth thereafter. Our aims were to devise analytical and preparation methods for potentially toxic or beneficial organic chemicals or metabolites in deciduous teeth and to estimate their detection frequencies. The analgesic acetaminophen was stored at greater concentration in a child's second molar than a first molar, consistent with intake, suggesting that acetaminophen concentration in molars may be a biomarker of acetaminophen exposure during molar formation. Chemicals detected by liquid chromatography/tandem mass spectrometry in molars of 21 typically developing children include the endocannabinoid anandamide (86% of children), acetaminophen (43%), and specific metabolites mono-2-ethylhexyl phthalate (MEHP, of plasticizer di-2-ethylhexyl phthalate, 29%), 3,5,6-trichloro-2-pyridinol (TCPy, of organophosphate (OP) insecticide chlorpyrifos, 10%), and 2-isopropyl-6-methyl-4-pyrimidinol (IMPy, of OP insecticide diazinon, 10%). None of these chemicals has previously been detected in human teeth. Molars from the two oldest subjects contained the largest concentrations of MEHP, TCPy, and IMPy. Potentially protective fatty acids detected by gas chromatography/mass spectrometry after derivatization include docosahexaenoic (19%), arachidonic (100%), and linoleic (100%). Validation studies are necessary to verify that each detected chemical in molars provides a biomarker of perinatal exposure.

Prenatal exposure to pesticide ingredient piperonyl butoxide and childhood cough in an urban cohort.

RATIONALE: Previously we reported that airborne concentrations of cis-permethrin, but not trans-permethrin, measured during pregnancy in an inner city pediatric cohort was associated with cough by age 5. However, the effect of subsequent exposures to both permethrins during early childhood, and to piperonyl butoxide (PBO, a synergist for residential pyrethroid insecticides) remains to be elucidated. We hypothesized that prenatal and age 5-6 year measures of PBO and permethrins would be associated with cough at age 5-6 years in this cohort. Further, we explored the associations between these pesticide measures and wheeze, asthma, seroatopy, and fractional exhaled nitric oxide (FeNO). METHODS: PBO and permethrins were measured in personal air during the third trimester of pregnancy and indoor residential air at age 5-6 years (n=224). Health outcome questionnaires were administered to the mothers of 5-6 year old children. Indoor allergen specific and total immunoglobulin (Ig) E production was measured from sera collected at age 5, and FeNO was measured at 5-6 years. The hypotheses were tested using regression models adjusting for common confounders. RESULTS: Noninfectious cough was reported among 14% of children at age 5-6 years. Measures of prenatal PBO, but not age 5-6 year PBO or permethrins, increased the odds of cough [OR (95% CI): 1.27 (1.09-1.48), p<0.01; n=217]. No significant associations were found for other measured health outcomes. CONCLUSIONS: Prenatal PBO exposure was associated with childhood cough. It is unclear whether the observed effect is due mainly to PBO itself or residential pyrethroids of which PBO is an indicator.

Comparison of wipe materials and wetting agents for pesticide residue collection from hard surfaces.

Different wipe materials and wetting agents have been used to collect pesticide residues from surfaces, but little is known about their comparability. To inform the selection of a wipe for the National Children's Study, the analytical feasibility, collection efficiency, and precision of Twillwipes wetted with isopropanol (TI), Ghost Wipes (GW), and Twillwipes wetted with water (TW), were evaluated. Wipe samples were collected from stainless steel surfaces spiked with high and low concentrations of 27 insecticides, including organochlorines, organophosphates, and pyrethroids. Samples were analyzed by GC/MS/SIM. No analytical interferences were observed for any of the wipes. The mean percent collection efficiencies across all pesticides for the TI, GW, and TW were 69.3%, 31.1%, and 10.3% at the high concentration, respectively, and 55.6%, 22.5%, and 6.9% at the low concentration, respectively. The collection efficiencies of the TI were significantly greater than that of GW or TW (p<0.0001). Collection efficiency also differed significantly by pesticide (p<0.0001) and spike concentration (p<0.0001). The pooled coefficients of variation (CVs) of the collection efficiencies for the TI, GW, and TW at high concentration were 0.08, 0.17, and 0.24, respectively. The pooled CV of the collection efficiencies for the TI, GW, and TW at low concentration were 0.15, 0.19, and 0.36, respectively. The TI had significantly lower CVs than either of the other two wipes (p=0.0008). Though the TI was superior in terms of both accuracy and precision, it requires multiple preparation steps, which could lead to operational challenges in a large-scale study.

Impact of prenatal exposure to piperonyl butoxide and permethrin on 36-month neurodevelopment.

OBJECTIVE: Recent pesticide-monitoring results suggest that a shift in residential pesticide exposure from organophosphorus insecticides to pyrethroid insecticides has occurred. Pyrethroid insecticides are potential neurodevelopmental toxicants and have not been evaluated for developmental toxicity. Our objective was to explore the association between prenatal exposure to permethrin (a common pyrethroid) and piperonyl butoxide (a pyrethroid synergist) and 36-month neurodevelopment. METHODS: Participants is this study were part of a prospective cohort of black and Dominican mothers and newborns living in low-income neighborhoods in New York City. We examined 36-month cognitive and motor development (using the Bayley Scales of Infant Development, second edition) as a function of permethrin levels measured in maternal and umbilical cord plasma collected on delivery and permethrin and piperonyl butoxide levels measured in personal air collected during pregnancy. All models were controlled for gender, gestational age, ethnicity, maternal education, maternal intelligence, quality of the home environment, and prenatal exposure to environmental tobacco smoke and chlorpyrifos. RESULTS: Prenatal exposure to permethrin in personal air and/or plasma was not associated with performance scores for the Bayley Mental Developmental Index or the Psychomotor Developmental Index. After data adjustment, children more highly exposed to piperonyl butoxide in personal air samples (>4.34 ng/m(3)) scored 3.9 points lower on the Mental Developmental Index than those with lower exposures (95% confidence interval: -0.25 to -7.49). CONCLUSIONS: Prenatal exposure to piperonyl butoxide was negatively associated with 36-month neurodevelopment.

Prenatal exposure to polycyclic aromatic hydrocarbons, environmental tobacco smoke and asthma.

BACKGROUND: Previously, we reported that prenatal exposures to polycyclic aromatic hydrocarbons (PAH) and postnatal environmental tobacco smoke (ETS) in combination were associated with respiratory symptoms at ages 1 and 2 years. Here, we hypothesized that children exposed to both prenatal PAH and ETS may be at greater risk of asthma and seroatopy at ages 5-6 years, after controlling for current pollution exposure. METHODS: Prenatal PAH exposure was measured by personal air monitoring over 48 h. ETS exposure, respiratory symptoms and asthma at ages 5-6 years were assessed through questionnaire. Immunoglobulin (Ig) E was measured by Immunocap. RESULTS: A significant interaction between prenatal PAH and prenatal (but not postnatal) ETS exposure on asthma (p < 0.05), but not IgE, was detected. Among children exposed to prenatal ETS, a positive nonsignificant association was found between prenatal PAH exposure and asthma (OR 1.96, 95% CI [0.95-4.05]). Among children without exposure to prenatal ETS, a negative nonsignificant association was found between prenatal PAH exposure and asthma (OR 0.65, 95% CI [0.41-1.01]). Prenatal PAH exposure was not associated with asthma or IgE at age 5-6 years. CONCLUSIONS: Combined prenatal exposure to PAH and ETS appears to be associated with asthma but not seroatopy at age 5-6. Exposure to PAH alone does not appear associated with either asthma or seroatopy at age 5-6 years. Discerning the differential effects between ETS exposed and ETS nonexposed children requires further study.

Semivolatile endocrine-disrupting compounds in paired indoor and outdoor air in two northern California communities.

Interest in the health effects of potential endocrine-disrupting compounds (EDCs) that are high production volume chemicals used in consumer products has made exposure assessment and source identification a priority. We collected paired indoor and outdoor air samples in 40 nonsmoking homes in urban, industrial Richmond, CA, and 10 in rural Bolinas, CA. Samples were analyzed by GC-MS for 104 analytes, including phthalates (11), alkylphenols (3), parabens (3), polybrominated diphenyl ether (PBDE) flame retardants (3), polychlorinated biphenyls (PCBs) (3), polycyclic aromatic hydrocarbons (PAHs) (24), pesticides (38), and phenolic compounds (19). We detected 39 analytes in outdoor air and 63 in indoor air. For many of the phenolic compounds, alkylphenols, phthalates, and PBDEs, these represent some of the first outdoor measures and the first analysis of the relative importance of indoor and outdoor sources in paired samples. Data demonstrate higher indoor concentrations for 32 analytes, suggesting primarily indoor sources, as compared with only 2 that were higher outdoors. Outdoor air concentrations were higher in Richmond than Bolinas for 3 phthalates, 10 PAHs, and o-phenylphenol, while indoor air levels were more similar between communities, except that differences observed outdoors were also seen indoors. Indoor concentrations of the most ubiquitous chemicals were generally correlated with each other (4-t-butylphenol, o-phenylphenol, nonylphenol, several phthalates, and methyl phenanthrenes; Kendall correlation coefficients 0.2-0.6, p<0.05), indicating possible shared sources and highlighting the importance of considering mixtures in health studies.

Urinary and air phthalate concentrations and self-reported use of personal care products among minority pregnant women in New York city.

Diethyl phthalate (DEP) and di-n-butyl phthalate (DnBP) are used extensively in personal care products, including fragrances (DEP) and nail polish (DnBP). Between May 2003 and July 2006, we gathered questionnaire data on the use of seven product categories (deodorant, perfume, hair spray, hair gel, nail polish/polish remover, liquid soap/body wash, and lotion/mist) over 48 h during the third trimester of pregnancy from 186 inner-city women. A 48-h personal air sample was collected and analyzed for DEP and DnBP; a maternal spot urine sample was collected and analyzed for their monoester metabolites, monoethyl phthalate (MEP) and mono-n-butyl phthalate (MnBP), respectively. In all, 97% of air samples and 84% of urine samples were collected within ±2 days of the questionnaire. During the 48 h, 41% of women reported perfume use and 10% reported nail polish/polish remover use. In adjusted analyses, no association was seen between nail product use and air DnBP or urine MnBP concentrations. Women reporting perfume use had 2.3 times higher (95% CI 1.6, 3.3) urinary MEP concentrations. Personal air DEP increased by 7% for each 25% increase in a composite indicator of the six other product categories (P<0.05), but was not associated with perfume use. Air DEP was correlated with urine MEP concentrations only among non-perfume users (r=0.51, P<0.001). Results suggest that perfume use is a significant source of DEP exposure.

Development of a personal dual-phase air sampling method for phthalate diesters.

Phthalates are used as plasticizers in many industrial and consumer products. Urinary biomonitoring has shown widespread human exposure to phthalates, with workers having especially high exposures. Phthalates can be present in workplace air as either aerosols or vapors depending on source materials, vapor pressure, and processing temperatures. We sought to develop a dual-phase air sampling method for 6 phthalates, dimethyl phthalate (DMP), diethyl phthalate (DEP), di-n-butyl phthalate (DBP), benzyl butyl phthalate (BzBP), di(2-ethylhexyl) phthalate (DEHP), and di-n-octyl phthalate (DnOP), adaptable to aerosol inlets with known particle collection characteristics. Collection media consisted of a quartz fiber filter and XAD-2 resin. Limit of detection (LOD) and limit of quantification (LOQ) were determined for each phthalate. Phthalate recoveries were evaluated at 3x, 10x and 30x the LOQ, and after storage at -21 degrees C and 21 degrees C. Media were Soxhlet extracted in 10% diethyl ether in hexanes along with an extraction surrogate, di-n-pentyl phthalate-d(4). Gas chromatography/mass spectrometry was performed to quantify the phthalate diesters using di(2-ethylhexyl) phthalate-d(4) as an internal standard. Estimated LODs were 1 microg per sample (BzBP, DEHP, and DnOP), 2 microg per sample (DMP and DBP), and 5 microg per sample (DEP). Mean recoveries under static conditions were 85-104% for DBP, BzBP, DEHP, and DnOP; but <70% for DMP and DEP at 3x and 10x the LOQ. After air was pulled through spiked samples, DMP and DEP recoveries improved to 74-81%. After storage for 62 days, phthalate recovery was better at -21 degrees C than at 21 degrees C. Method accuracy was best for DBP, BzBP, DEHP, and DnOP (range 11-18%), and less so for DMP (28%) and DEP (29%).

Prenatal di(2-ethylhexyl)phthalate exposure and length of gestation among an inner-city cohort.

OBJECTIVE: Our objective was to assess the relationship between di(2-ethylhexyl)phthalate (DEHP) exposure during pregnancy and gestational age at delivery among 311 African American or Dominican women from New York City. METHODS: Forty-eight-hour personal air and/or spot urine samples were collected during the third trimester. DEHP levels were measured in air samples and 4 DEHP metabolite levels were measured in urine. Specific gravity was used to adjust for urinary dilution. Gestational age was abstracted from newborn medical records (n = 289) or calculated from the expected date of delivery (n = 42). Multivariate linear regression models controlled for potential confounders. RESULTS: DEHP was detected in 100% of personal air samples (geometric mean: 0.20 microg/m(3) [95% confidence interval [CI]: 0.18-0.21 microg/m(3)]); natural logarithms of air concentrations were inversely but not significantly associated with gestational age. Two or more of the DEHP metabolites were detected in 100% of urine samples (geometric mean: 4.8-38.9 ng/mL [95% CI: 4.1-44.3 ng/mL]). Controlling for potential confounders, gestational age was shorter by 1.1 days (95% CI: 0.2-1.8 days) for each 1-logarithmic unit increase in specific gravity-adjusted mono(2-ethylhexyl)phthalate concentrations (P = .01) and averaged 5.0 days (95% CI: 2.1-8.0 days) less among subjects with the highest versus lowest quartile concentrations (P = .001). Results were similar and statistically significant for the other DEHP metabolites. CONCLUSIONS: Prenatal DEHP exposure was associated with shorter gestation but, given inconsistencies with previous findings for other study populations, results should be interpreted with caution, and additional research is warranted.

Monitoring and reducing exposure of infants to pollutants in house dust.

The health risks to babies from pollutants in house dust may be 100 times greater than for adults. The young ingest more dust and are up to ten times more vulnerable to such exposures. House dust is the main exposure source for infants to allergens, lead, and PBDEs, as well as a major source of exposure to pesticides, PAHs, Gram-negative bacteria, arsenic, cadmium, chromium, phthalates, phenols, and other EDCs, mutagens, and carcinogens. Median or upper percentile concentrations in house dust of lead and several pesticides and PAHs may exceed health-based standards in North America. Early contact with pollutants among the very young is associated with higher rates of chronic illness such as asthma, loss of intelligence, ADHD, and cancer in children and adults. The potential of infants, who live in areas with soil contaminated by automotive and industrial emissions, can be given more protection by improved home cleaning and hand washing. Babies who live in houses built before 1978 have a prospective need for protection against lead exposures; homes built before 1940 have even higher lead exposure risks. The concentration of pollutants in house dust may be 2-32 times higher than that found in the soil near a house. Reducing infant exposures, at this critical time in their development, may reduce lifetime health costs, improve early learning, and increase adult productivity. Some interventions show a very rapid payback. Two large studies provide evidence that home visits to reduce the exposure of children with poorly controlled asthma triggers may return more than 100% on investment in 1 yr in reduced health costs. The tools provided to families during home visits, designed to reduce dust exposures, included vacuum cleaners with dirt finders and HEPA filtration, allergy control bedding covers, high-quality door mats, and HEPA air filters. Infants receive their highest exposure to pollutants in dust at home, where they spend the most time, and where the family has the most mitigation control. Normal vacuum cleaning allows deep dust to build up in carpets where it can be brought to the surface and become airborne as a result of activity on the carpet. Vacuums with dirt finders allow families to use the three-spot test to monitor deep dust, which can reinforce good cleaning habits. Motivated families that receive home visits from trained outreach workers can monitor and reduce dust exposures by 90% or more in 1 wk. The cost of such visits is low considering the reduction of risks achieved. Improved home cleaning is one of the first results observed among families who receive home visits from MHEs and CHWs. We believe that proven intervention methods can reduce the exposure of infants to pollutants in house dust, while recognizing that much remains to be learned about improving the effectiveness of such methods.

A biomarker validation study of prenatal chlorpyrifos exposure within an inner-city cohort during pregnancy.

BACKGROUND: We previously documented significant decreases in chlorpyrifos concentrations in maternal personal and indoor air samples among pregnant African-American and Dominican women from New York City after the 2000-2001 restrictions on its residential use. OBJECTIVE: We undertook a biomarker validation study within the same cohort to evaluate trends over time in multiple biomarkers of prenatal chlorpyrifos exposure. METHODS: Subjects were enrolled between February 2001 and May 2004 (n = 102). We measured 3,5,6-trichloro-2-pyridinol (TCPy) in postpartum meconium (n = 83), repeat prenatal maternal spot urine samples (n = 253), and postnatal urine from the mothers (n = 73) and newborns (n = 59). We measured chlorpyrifos in postnatal maternal (n = 92) and umbilical cord (n = 65) blood. RESULTS: We did not detect TCPy in infant urine, but all other biomarkers showed a highly significant decrease in detection frequencies (chi2 = 7.8-34.0, p < or = 0.005) and mean ranks (p < or = 0.006, Kruskal-Wallis) among subjects enrolled in 2003-2004 compared with those enrolled in 2001-2002. Chlorpyrifos in maternal personal and indoor air declined 2- to 3-fold over the same period (p < 0.05). In 2001-2002 samples, TCPy levels in repeat prenatal urine were positively correlated (r = 0.23-0.56), but within-subject variability exceeded between-subject variability (intraclass correlation coefficient = 0.43); indoor air levels explained 19% of the variance in prenatal urine TCPy (p = 0.001). Meconium TCPy concentrations were positively correlated with chlorpyrifos in maternal and cord blood (r = 0.25-0.33, p < 0.05) and with TCPy in maternal urine (r = 0.31, p < 0.01). CONCLUSIONS: Results suggest the biomarkers are reliable dosimeters to differentiate between groups with prenatal chlorpyrifos exposures varying by a factor of 2 or more and vividly illustrate the efficacy of residential restriction on chlorpyrifos to reduce the internal dose during pregnancy.

Changes in pest infestation levels, self-reported pesticide use, and permethrin exposure during pregnancy after the 2000-2001 U.S. Environmental Protection Agency restriction of organophosphates.

BACKGROUND: Widespread residential pesticide use throughout the United States has resulted in ubiquitous, low-level pesticide exposure. The mix of active pesticide ingredients is changing in response to 2000-2001 regulations restricting use of the organophosphorus insecticides chlorpyrifos and diazinon. OBJECTIVES: We aimed to determine the impact of U.S. Environmental Protection Agency regulations on pest infestation levels, pesticide use, and pesticides measured in indoor air samples. METHODOLOGY: 511 pregnant women from inner-city New York were enrolled between 2000 and 2006. Permethrin, a pyrethroid insecticide; piperonyl butoxide (PBO), a pyrethroid synergist; chlorpyrifos; and diazinon were measured in 48-hr prenatal personal air samples. Data on pest infestation and pesticide use were collected via questionnaire. RESULTS: Eighty-eight percent of women reported using pesticides during pregnancy; 55% reported using higher-exposure pesticide applications (spray cans, pest bombs and/or professional pesticide applicators). Self-reported pest sightings and use of higher-exposure applications increased significantly after the regulations were implemented (p < 0.001). PBO, cis-, and trans-permethrin were detected in 75, 19, and 18% of personal air samples, respectively. Detection frequencies of PBO and cis- and trans-permethrin increased significantly over time (p < 0.05 controlling for potential confounders). Levels and/or detection frequencies of these compounds were significantly higher among mothers reporting use of high exposure pesticide applications (p < or = 0.05). Chlorpyrifos and diazinon levels decreased significantly over time (p < 0.001). CONCLUSION: In this cohort, pest infestations, use of pesticides, and use of permethrin appear to increase after the residential restriction of organophosphorus insecticides. This is one of the first studies to document widespread residential exposure to PBO.

Within- and between-home variability in indoor-air insecticide levels during pregnancy among an inner-city cohort from New York City.

BACKGROUND: Residential insecticide use is widespread in the United States, but few data are available on the persistence and variability in levels in the indoor environment. OBJECTIVE: The study aim was to assess within- and between-home variability in indoor-air insecticides over the final 2 months of pregnancy among a cohort of African-American and Dominican women from New York City. METHODS: Women not employed outside the home were enrolled between February 2001 and May 2004 (n = 102); 9 insecticides and an adjuvant were measured in 48-hr personal air samples and 2-week integrated indoor air samples collected sequentially for 7.0 +/- 2.3 weeks (n = 337 air samples). RESULTS: Sixty-one percent of the women reported using pest control during the air samplings. Chlorpyrifos, diazinon, and propoxur were detected in 99-100% of personal and indoor samples (range, 0.4-641 ng/m(3)). Piperonyl butoxide (a pyrethroid adjuvant) was detected in 45.5-68.5% (0.2-608 ng/m(3)). There was little within-home variability and no significant difference in air concentrations within homes over time (p > or = 0.2); between-home variability accounted for 88% of the variance in the indoor air levels of propoxur, 92% in chlorpyrifos, 94% in diazinon, and 62% in piperonyl butoxide (p < 0.001). Indoor and maternal personal air insecticide levels were highly correlated (r = 0.7-0.9, p < 0.001). Diazinon and chlorpyrifos levels declined 5-fold between 2001 and 2004 but were detected in all homes 1.5 and 2.5 years, respectively, after the U.S. Environmental Protection Agency ban on their residential use. CONCLUSION: Results showed that the insecticides were persistent in the home with little variability in air concentrations over the 2 months and contributed to chronic maternal inhalation exposures during pregnancy.

Personal exposure to fine particles and benzo[a]pyrene. Relation with indoor and outdoor concentrations of these pollutants in Kraków.

OBJECTIVES: This study assessed personal exposure of pregnant women to fine particles (PM(25)) and benzo[a]pyrene (B[a]P) and the relationship between pollutant concentrations in ambient and indoor air. MATERIALS AND METHODS: In a group of 78 pregnant women, simultaneous 48 h measurements of personal, indoor, and outdoor exposure to PM(25) and B[a]P were carried out in the second trimester of pregnancy. The results show that participants were exposed to varying concentrations of PM(25) and B[a]P, with higher exposure in the winter season. Overall, the mean personal PM(25) level was 30.4 microg/m(3) and B[a]P 2.1 ng/m(3). The winter/summer ratios for mean personal exposures were 1.4 (35.6 microg/m(3) vs. 25.8 microg/m(3)) and 5.4 (4.9 ng/m(3) vs. 0.9 ng/m(3)), respectively. As for indoor levels, the winter/summer ratios were 1.4 (33.2 microg/m(3) vs. 24.4 microg/m(3)) for PM(25) and 5.4 (4.3 ng/m(3) vs. 0.8 ng/m(3)) for B[a]P, and for outdoor concentrations, the respective values were 1.5 (40.3 microg/m(3) vs. 26.4 microg/m(3), and 6.8 (6.1 ng/m(3) vs 0.9 ng/m(3)). A stronger correlation was found between personal PM(25) exposure and the pollutant concentration indoors (r = 0.89; 95% CI: 0.83-0.93) than outdoors (r = 0.75; 95% CI: 0.64-0.83). The correlations between personal B[a]P exposure and its indoor or outdoor levels were similar (0.95-0.96) and significant. The markedly higher exposure to B[a]P in Kraków in winter than in summer can be explained by the massive use of coal for heating in the cold season. CONCLUSION: We conclude that although ambient PM(25) measurements provide an adequate indicator of outdoor air quality for use in epidemiologic studies, they may not be adequate for studies on relationship between non-ambient pollution and health effects. Since only about 20% of variability in personal B[a]P exposure could be explained by personal PM(25) level, the extrapolation of personal exposure to B[a]P from personal PM(25) data may be greatly underestimated.

An intervention to reduce residential insecticide exposure during pregnancy among an inner-city cohort.

BACKGROUND: We previously reported widespread insecticide exposure during pregnancy among inner-city women from New York City. Here we report on a pilot intervention using integrated pest management (IPM) to reduce pest infestations and residential insecticide exposures among pregnant New York City African-American and Latina women (25 intervention and 27 control homes). METHODS: The IPM consisted of professional cleaning, sealing of pest entry points, application of low-toxicity pesticides, and education. Cockroach infestation levels and 2-week integrated indoor air samples were collected at baseline and one month postintervention. The insecticides detected in the indoor air samples were also measured in maternal and umbilical cord blood collected at delivery. RESULTS: Cockroach infestations decreased significantly (p = 0.016) after the intervention among intervention cases but not control households. Among the intervention group, levels of piperonyl butoxide (a pyrethroid synergist) were significantly lower in indoor air samples after the intervention (p = 0.016). Insecticides were detected in maternal blood samples collected at delivery from controls but not from the intervention group. The difference was significant for trans-permethrin (p = 0.008) and of borderline significance (p = 0.1) for cis-permethrin and 2-isopropoxyphenol (a propoxur metabolite). CONCLUSION: To our knowledge, this is the first study to use biologic dosimeters of prenatal pesticide exposure for assessing effectiveness of IPM. These pilot data suggest that IPM is an effective strategy for reducing pest infestation levels and the internal dose of insecticides during pregnancy.