Person: Herrick, Robert
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Herrick
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Herrick, Robert
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Publication An Unrecognized Source of PCB Contamination in Schools and Other Buildings(National Institue of Environmental Health Sciences, 2004) Herrick, Robert; McClean, Michael D.; Meeker, John D.; Baxter, Lisa K.; Weymouth, George A.An investigation of 24 buildings in the Greater Boston Area revealed that one-third (8 of 24) contained caulking materials with polychlorinated biphenyl (PCB) content exceeding 50 ppm by weight, which is the U.S. Environmental Protection Agency (U.S. EPA) specified limit above which this material is considered to be PCB bulk product waste. These buildings included schools and other public buildings. In a university building where similar levels of PCB were found in caulking material, PCB levels in indoor air ranged from 111 to 393 ng/m3; and in dust taken from the building ventilation system, < 1 ppm to 81 ppm. In this building, the U.S. EPA mandated requirements for the removal and disposal of the PCB bulk product waste as well as for confirmatory sampling to ensure that the interior and exterior of the building were decontaminated. Although U.S. EPA regulations under the Toxic Substances Control Act stipulate procedures by which PCB-contaminated materials must be handled and disposed, the regulations apparently do not require that materials such as caulking be tested to determine its PCB content. This limited investigation strongly suggests that were this testing done, many buildings would be found to contain high levels of PCBs in the building materials and potentially in the building environment. The presence of PCBs in schools is of particular concern given evidence suggesting that PCBs are developmental toxins.Publication Soil Contamination from PCB-Containing Buildings(National Institute of Environmental Health Sciences, 2006) Herrick, Robert; Lefkowitz, Daniel J.; Weymouth, George A.Background: Polychlorinated biphenyls (PCBs) in construction materials, such as caulking used around windows and expansion joints, may constitute a source of PCB contamination in the building interiors and in surrounding soil. Several studies of soil contamination have been conducted around buildings where the caulking has been removed by grinding or scraping. The PCBs in soil may have been generated in the process of removing the caulking, but natural weathering and deterioration of the caulking may have also been a source. Objectives: The objectives of this study were to measure PCB levels in soil surrounding buildings where PCB-containing caulk was still in place, and to evaluate the mobility of the PCBs from caulking using the Toxicity Characteristic Leaching Procedure (U.S. Environmental Protection Agency Method 1311). Discussion: We found soil PCB contamination ranging from 3.3 to 34 mg/kg around buildings with undisturbed caulking that contained 10,000–36,200 mg/kg PCBs. The results of the Toxicity Characteristic Leaching Procedure (leachate concentrations of 76–288 mg PCB/L) suggest that PCBs in caulking can be mobilized, apparently as complexes with dissolved organic matter that also leach off the caulking material. Conclusions and Recommendations: Although these new findings are based on a small sample size, they demonstrate the need for a national survey of PCBs in building materials and in soil surrounding these buildings. Because the buildings constructed during the time the PCB caulking was in use (1960s and 1970s) include schools, hospitals, and apartment buildings, the potential for exposure of children is a particular concern. It is necessary to reconsider the practice of disposing of old PCB caulking removed during building renovations in conventional landfills, given the apparent mobility of PCBs from the caulking material. Disposal of some caulking material in nonhazardous landfills might lead to high PCB levels in landfill leachate.Publication Serum PCB levels and congener profiles among US construction workers(BioMed Central, 2007) Herrick, Robert; Meeker, John D; Hauser, Russ; Altshul, Larisa; Weymouth, George ABackground: The presence of PCB in caulking (sealant) material found in masonry buildings has been well-documented in several countries. A recent investigation of 24 buildings in the greater Boston area found that 8 buildings had high PCB levels in caulking materials used around window frames and in joints between masonry blocks. Workers removing caulking material have been shown to have elevated serum PCB levels. Methods: This project compared serum PCB levels among male workers who installed and/or removed PCB-containing caulking material from buildings in the greater Boston area with reference serum PCB levels from 358 men from the same area. Serum PCB levels were measured in the same laboratory by liquid-liquid extraction, column chromatography clean-up and dual capillary column GC/microECD analysis. Results: When the congener profiles were compared between the reference population and the construction workers, the serum levels of the more volatile, lighter PCBs (di-, tri-and tetrachloro, sum of IUPAC# 6–74) were substantially higher among the construction workers. One of the youngest workers had the lowest total serum PCB levels (sum of 57 congeners) of all 6 workers, but the contribution of more volatile (less chlorinated) PCB congeners (#16, 26,28,33,74,66, and 60) was markedly higher than in other 5 workers and reference men. Only this worker was working on a job that involved removing PCB caulking at the time of the blood sampling. Conclusion: While the results of this pilot study are based upon small numbers (6 construction workers who handled PCB caulking), the serum PCB levels among the construction workers exceed the referents. Comparison of the congener profiles suggests that there are substantial differences between the construction workers and the general population samples. These differences, and the similarities of profiles among the construction workers strongly suggest that occupational contact with caulking material can be a major source of PCB exposure for construction workers.Publication The Relationship of Urinary Metabolites of Carbaryl/Naphthalene and Chlorpyrifos with Human Semen Quality(The National Institute of Environmental Health Sciences, 2004) Meeker, John D.; Ryan, Louise; Barr, Dana B.; Herrick, Robert; Bennett, Deborah H.; Bravo, Roberto; Hauser, RussMost of the general population is exposed to carbaryl and other contemporary-use insecticides at low levels. Studies of laboratory animals, in addition to limited human data, show an association between carbaryl exposure and decreased semen quality. In the present study we explored whether environmental exposures to 1-naphthol (1N), a metabolite of carbaryl and naphthalene, and 3,5,6-trichloro-2-pyridinol (TCPY), a metabolite of chlorpyrifos and chlorpyrifos-methyl, are associated with decreased semen quality in humans. Subjects (n = 272) were recruited through a Massachusetts infertility clinic. Individual exposures were measured as spot urinary concentrations of 1N and TCPY adjusted using specific gravity. Semen quality was assessed as sperm concentration, percent motile sperm, and percent sperm with normal morphology, along with sperm motion parameters (straight-line velocity, curvilinear velocity, and linearity). Median TCPY and 1N concentrations were 3.22 and 3.19 μg/L, respectively. For increasing 1N tertiles, adjusted odds ratios (ORs) were significantly elevated for below-reference sperm concentration (OR for low, medium, and high tertiles = 1.0, 4.2, 4.2, respectively; p-value for trend = 0.01) and percent motile sperm (1.0, 2.5, 2.4; p-value for trend = 0.01). The sperm motion parameter most strongly associated with 1N was straight-line velocity. There were suggestive, borderline-significant associations for TCPY with sperm concentration and motility, whereas sperm morphology was weakly and nonsignificantly associated with both TCPY and 1N. The observed associations between altered semen quality and 1N are consistent with previous studies of carbaryl exposure, although suggestive associations with TCPY are difficult to interpret because human and animal data are currently limited.Publication PM\(_{2.5}\) metal exposures and nocturnal heart rate variability: a panel study of boilermaker construction workers(BioMed Central, 2008) Cavallari, Jennifer M; Eisen, Ellen; Fang, Shona C; Schwartz, Joel; Hauser, Russ; Herrick, Robert; Christiani, DavidBackground: To better understand the mechanism(s) of particulate matter (PM) associated cardiovascular effects, research priorities include identifying the responsible PM characteristics. Evidence suggests that metals play a role in the cardiotoxicity of fine PM (PM\(_{2.5}\)) and in exposure-related decreases in heart rate variability (HRV). We examined the association between daytime exposure to the metal content of PM\(_{2.5}\) and night HRV in a panel study of boilermaker construction workers exposed to metal-rich welding fumes. Methods: Twenty-six male workers were monitored by ambulatory electrocardiogram (ECG) on a workday while exposed to welding fume and a non-workday (baseline). From the ECG, rMSSD (square root of the mean squared differences of successive intervals) was summarized over the night (0:00–7:00). Workday, gravimetric PM\(_{2.5}\) samples were analyzed by x-ray fluorescence to determine metal content. We used linear mixed effects models to assess the associations between night rMSSD and PM\(_{2.5}\) metal exposures both with and without adjustment for total PM\(_{2.5}\). Matched ECG measurements from the non-workday were used to control for individual cardiac risk factors and models were also adjusted for smoking status. To address collinearity between PM\(_{2.5}\) and metal content, we used a two-step approach that treated the residuals from linear regression models of each metal on PM\(_{2.5}\) as surrogates for the differential effects of metal exposures in models for night rMSSD. Results: The median PM\(_{2.5}\) exposure was 650 μg/m\(^3\); median metal exposures for iron, manganese, aluminum, copper, zinc, chromium, lead, and nickel ranged from 226 μg/m\(^3\) to non-detectable. We found inverse linear associations in exposure-response models with increased metal exposures associated with decreased night rMSSD. A statistically significant association for manganese was observed, with a decline of 0.130 msec (95% CI: -0.162, -0.098) in night rMSSD for every 1 μg/m\(^3\) increase in manganese. However, even after adjusting for individual metals, increases in total PM\(_{2.5}\) exposures were associated with declines in night rMSSD. Conclusion: These results support the cardiotoxicity of PM\(_{2.5}\) metal exposures, specifically manganese. However the metal component alone did not account for the observed declines in night HRV. Therefore, results suggest the importance of other PM elemental components.Publication Characterization of Phthalate Exposure among Pregnant Women Assessed by Repeat Air and Urine Samples(National Institute of Environmental Health Sciences, 2008) Adibi, Jennifer J.; Whyatt, Robin M.; Calafat, Antonia M.; Camann, David; Nelson, Heather; Bhat, Hari K.; Perera, Frederica P.; Silva, Manori J.; Williams, Paige; Herrick, Robert; Hauser, RussBackground: Although urinary concentrations of phthalate metabolites are frequently used as biomarkers in epidemiologic studies, variability during pregnancy has not been characterized. Methods: We measured phthalate metabolite concentrations in spot urine samples collected from 246 pregnant Dominican and African-American women. Twenty-eight women had repeat urine samples collected over a 6-week period. We also analyzed 48-hr personal air samples (n = 96 women) and repeated indoor air samples (n = 32 homes) for five phthalate diesters. Mixed-effects models were fit to evaluate reproducibility via intraclass correlation coefficients (ICC). We evaluated the sensitivity and specificity of using a single specimen versus repeat samples to classify a woman’s exposure in the low or high category. Results: Phthalates were detected in 85–100% of air and urine samples. ICCs for the unadjusted urinary metabolite concentrations ranged from 0.30 for mono-ethyl phthalate to 0.66 for monobenzyl phthalate. For indoor air, ICCs ranged from 0.48 [di-2-ethylhexyl phthalate (DEHP)] to 0.83 [butylbenzyl phthalate (BBzP)]. Air levels of phthalate diesters correlated with their respective urinary metabolite concentrations for BBzP (r = 0.71), di-isobutyl phthalate (r = 0.44), and diethyl phthalate (DEP; r = 0.39). In women sampled late in pregnancy, specific gravity appeared to be more effective than creatinine in adjusting for urine dilution. Conclusions: Urinary concentrations of DEP and DEHP metabolites in pregnant women showed lower reproducibility than metabolites for di-n-butyl phthalate and BBzP. A single indoor air sample may be sufficient to characterize phthalate exposure in the home, whereas urinary phthalate biomarkers should be sampled longitudinally during pregnancy to minimize exposure misclassification.Publication The relationship between environmental exposures to phthalates and DNA damage in human sperm using the neutral comet assay.(2003) Duty, Susan M.; Singh, Narendra P; Silva, Manori J; Barr, Dana B; Brock, John W; Ryan, Louise; Herrick, Robert; Christiani, David; Hauser, RussPhthalates are industrial chemicals widely used in many commercial applications. The general population is exposed to phthalates through consumer products as well as through diet and medical treatments. To determine whether environmental levels of phthalates are associated with altered DNA integrity in human sperm, we selected a population without identified sources of exposure to phthalates. One hundred sixty-eight subjects recruited from the Massachusetts General Hospital Andrology Laboratory provided a semen and a urine sample. Eight phthalate metabolites were measured in urine by using high-performance liquid chromatography and tandem mass spectrometry; data were corrected for urine dilution by adjusting for specific gravity. The neutral single-cell microgel electrophoresis assay (comet assay) was used to measure DNA integrity in sperm. VisComet image analysis software was used to measure comet extent, a measure of total comet length (micrometers); percent DNA in tail (tail%), a measure of the proportion of total DNA present in the comet tail; and tail distributed moment (TDM), an integrated measure of length and intensity (micrometers). For an interquartile range increase in specific gravity-adjusted monoethyl phthalate (MEP) level, the comet extent increased significantly by 3.6 micro m [95% confidence interval (95% CI), 0.74-6.47]; the TDM also increased 1.2 micro m (95% CI, -0.05 to 2.38) but was of borderline significance. Monobutyl, monobenzyl, monomethyl, and mono-2-ethylhexyl phthalates were not significantly associated with comet assay parameters. In conclusion, this study represents the first human data to demonstrate that urinary MEP, at environmental levels, is associated with increased DNA damage in sperm.Publication Placental biomarkers of phthalate effects on mRNA transcription: application in epidemiologic research(BioMed Central, 2009) Adibi, Jennifer J; Hauser, Russ; Williams, Paige; Whyatt, Robin M; Thaker, Harshwardhan M; Nelson, Heather; Herrick, Robert; Bhat, Hari KBackground: CYP19 and PPARγ are two genes expressed in the placental trophoblast that are important to placental function and are disrupted by phthalate exposure in other cell types. Measurement of the mRNA of these two genes in human placental tissue by quantitative real-time polymerase chain reaction (qPCR) offers a source of potential biomarkers for use in epidemiologic research. We report on methodologic challenges to be considered in study design. Methods: We anonymously collected 10 full-term placentas and, for each, sampled placental villi at 12 sites in the chorionic plate representing the inner (closer to the cord insertion site) and outer regions. Each sample was analyzed for the expression of two candidate genes, aromatase (CYP19) and peroxisome proliferator activated receptor protein gamma (PPARγ) and three potential internal controls: cyclophilin (CYC), 18S rRNA (18S), and total RNA. Between and within placenta variability was estimated using variance component analysis. Associations of expression levels with sampling characteristics were estimated using mixed effects models. Results: We identified large within-placenta variability in both transcripts (>90% of total variance) that was minimized to <20% of total variance by using 18S as an internal control and by modelling the means by inner and outer regions. 18S rRNA was the most appropriate internal control based on within and between placenta variability estimates and low correlations of 18S mRNA with target gene mRNA. Gene expression did not differ significantly by delivery method. We observed decreases in the expression of both transcripts over the 25 minute period after delivery (CYP19 p-value for trend = 0.009 and PPARγ (p-value for trend = 0.002). Using histologic methods, we confirmed that our samples were comprised predominantly of villous tissue of the fetal placenta with minimal contamination of maternally derived cell types. Conclusion: qPCR-derived biomarkers of placental CYP19 and PPARγ gene expression show high within-placental variability. Sampling scheme, selection of an appropriate internal control and the timing of sample collection relative to delivery can be optimized to minimize within-placenta and other sources of underlying, non-etiologic variability.Publication Association of Expired Nitric Oxide with Occupational Particulate Exposure(2003) Kim, Jee Young; Wand, Matthew P; Hauser, Russ; Mukherjee, Sutapa; Herrick, Robert; Christiani, DavidParticulate air pollution has been associated with adverse respiratory health effects. This study assessed the utility of expired nitric oxide to detect acute airway responses to metal-containing fine particulates. Using a repeated-measures study design, we investigated the association between the fractional concentration of expired nitric oxide (F\(_E\)NO) and exposure to particulate matter with an aerodynamic mass median diameter of less than or equal to 2.5 micro m (PM\(_{2.5}\)) in boilermakers exposed to residual oil fly ash and metal fumes. Subjects were monitored for 5 days during boiler repair overhauls in 1999 (n = 20) or 2000 (n = 14). The Wilcoxon median baseline F\(_E\)NO was 10.6 ppb [95% confidence interval (CI): 9.1, 12.7] in 1999 and 7.4 ppb (95% CI: 6.7, 8.0) in 2000. The Wilcoxon median PM\(_{2.5}\) 8-hr time-weighted average was 0.56 mg/m(3) (95% CI: 0.37, 0.93) in 1999 and 0.86 mg/m(3) (95% CI: 0.65, 1.07) in 2000. F\(_E\)NO levels during the work week were significantly lower than baseline F\(_E\)NO in 1999 (p < 0.001). A significant inverse exposure-response relationship between log-transformed F\(_E\)NO and the previous workday's PM\(_{2.5}\) concentration was found in 1999, after adjusting for smoking status, age, and sampling year. With each 1 mg/m\(^3\) incremental increase in PM\(_{2.5}\) exposure, log F\(_E\)NO decreased by 0.24 (95% CI: -0.38, -0.10) in 1999. The lack of an exposure-response relationship between PM\(_{2.5}\) exposure and F\(_E\)NO in 2000 could be attributable to exposure misclassification resulting from the use of respirators. In conclusion, occupational exposure to metal-containing fine particulates was associated with significant decreases in F\(_E\)NO in a survey of workers with limited respirator usage.