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Organohalide-respiring microorganisms can use a variety of persistent pollutants, including trichloroethene (TCE), as terminal electron acceptors. The final two-electron transfer step in organohalide respiration is catalyzed by reductive dehalogenases. Here we report the x-ray crystal structure of PceA, an archetypal dehalogenase from Sulfurospirillum multivorans, as well as structures of PceA in complex with TCE and product analogs. The active site harbors a deeply buried norpseudo-B12 cofactor within a nitroreductase fold, also found in a mammalian B12 chaperone. The structures of PceA reveal how a cobalamin supports a reductive haloelimination exploiting a conserved B12-binding scaffold capped by a highly variable substrate-capturing region.

Composite of nanoscale Zero Valent Iron (nZVI) loaded on Biochar (BC) was prepared and characterized as hydrogen peroxide (H 2 O 2 ) activator for the degradation of trichloroethylene (TCE). nZVI is homogeneously loaded on lamellarly structured BC surfaces to form nZVI/BC with specific surface area (S BET ) of 184.91 m 2 g −1 , which can efficiently activate H 2 O 2 to achieve TCE degradation efficiency of 98.9% with TOC removal of 78.2% within 30 min under the conditions of 0.10 mmol L −1 TCE, 1.13 g L −1 nZVI/BC and 1.50 mmol L −1 H 2 O 2 . Test results from the Electron Spin Resonance (ESR) measurement and coumarin based fluorescent probe technology indicated that ∙OH radicals were the dominant species responsible for the degradation of TCE within the nZVI/BC-H 2 O 2 system. Activation mechanism of the redox action of Fe 2+ /Fe 3+ generated under both aerobic and anaerobic conditions from nZVI and single electron transfer process from BC surface bound C–OH to H 2 O 2 promoted decomposition of H 2 O 2 into ∙OH radicals was proposed.

In support of the Integrated Risk Information System (IRIS), the U.S. Environmental Protection Agency (EPA) completed a toxicological review of trichloroethylene (TCE) in September 2011, which was the result of an effort spanning > 20 years. We summarized the key findings and scientific issues regarding the human health effects of TCE in the U.S. EPA's toxicological review. In this assessment we synthesized and characterized thousands of epidemiologic, experimental animal, and mechanistic studies, and addressed several key scientific issues through modeling of TCE toxicokinetics, meta-analyses of epidemiologic studies, and analyses of mechanistic data. Toxicokinetic modeling aided in characterizing the toxicological role of the complex metabolism and multiple metabolites of TCE. Meta-analyses of the epidemiologic data strongly supported the conclusions that TCE causes kidney cancer in humans and that TCE may also cause liver cancer and non-Hodgkin lymphoma. Mechanistic analyses support a key role for mutagenicity in TCE-induced kidney carcinogenicity. Recent evidence from studies in both humans and experimental animals point to the involvement of TCE exposure in autoimmune disease and hypersensitivity. Recent avian and in vitro mechanistic studies provided biological plausibility that TCE plays a role in developmental cardiac toxicity, the subject of substantial debate due to mixed results from epidemiologic and rodent studies. TCE is carcinogenic to humans by all routes of exposure and poses a potential human health hazard for noncancer toxicity to the central nervous system, kidney, liver, immune system, male reproductive system, and the developing embryo/fetus.

Understanding the complex metabolisms of microbial communities in contaminated groundwaters is a challenge. PCE and TCE are among the most common groundwater contaminants in the United States that, when exposed to certain minerals, exhibit a unique abiotic degradation pathway in which C 2 H 2 is a product. In aquifers, acetylene (C 2 H 2 ) is a product of abiotic degradation of trichloroethene (TCE) catalyzed by in situ minerals. C 2 H 2 can, in turn, inhibit multiple microbial processes including TCE dechlorination and metabolisms that commonly support dechlorination, in addition to supporting the growth of acetylenotrophic microorganisms. Previously, C 2 H 2 was shown to support TCE reductive dechlorination in synthetic, laboratory-constructed cocultures containing the acetylenotroph Pelobacter sp. strain SFB93 and Dehalococcoides mccartyi strain 195 or strain BAV1. In this study, we demonstrate TCE and perchloroethene (PCE) reductive dechlorination by a microbial community enriched from contaminated groundwater and amended with C 2 H 2 as the sole electron donor and organic carbon source. The metagenome of the stable, enriched community was analyzed to elucidate putative community functions. A novel anaerobic acetylenotroph in the phylum Actinobacteria was identified using metagenomic analysis. These results demonstrate that the coupling of acetylenotrophy and reductive dechlorination can occur in the environment with native bacteria and broaden our understanding of biotransformation at contaminated sites containing both TCE and C 2 H 2 . IMPORTANCE Understanding the complex metabolisms of microbial communities in contaminated groundwaters is a challenge. PCE and TCE are among the most common groundwater contaminants in the United States that, when exposed to certain minerals, exhibit a unique abiotic degradation pathway in which C 2 H 2 is a product. C 2 H 2 can act as both an inhibitor of TCE dechlorination and of supporting metabolisms and an energy source for acetylenotrophic bacteria. Here, we combine laboratory microcosm studies with computational approaches to enrich and characterize an environmental microbial community that couples two uncommon metabolisms, demonstrating unique metabolic interactions only yet reported in synthetic, laboratory-constructed settings. Using this comprehensive approach, we have identified the first reported anaerobic acetylenotroph in the phylum Actinobacteria , demonstrating the yet-undescribed diversity of this metabolism that is widely considered to be uncommon.

Chlorinated hydrocarbons (CHCs) are often used in industrial processes, and they have been found in groundwater with increasing frequency in recent years. Several typical CHCs, including trichloroethylene (TCE), 1,1,1-trichloroethane (TCA), carbon tetrachloride (CT), etc., have strong cytotoxicity and carcinogenicity, posing a serious threat to human health and ecological environment. Advanced persulfate (PS) oxidation technology based on nano zero-valent iron (nZVI) has become a research hotspot for CHCs degradation in recent years. However, nZVI is easily oxidized to form the surface passivation layer and prone to aggregation in practical application, which significantly reduces the activation efficiency of PS. In order to solve this problem, various nZVI modification solutions have been proposed. This review systematically summarizes four commonly used modification methods of nZVI, and the theoretical mechanisms of PS activated by primitive and modified nZVI. Besides, the influencing factors in the engineering application process are discussed. In addition, the controversial views on which of the two (SO4·- and ·OH) is dominant in the nZVI/PS system are summarized. Generally, SO4·- predominates in acidic conditions while ·OH prefers neutral and alkaline environments. Finally, challenges and prospects for practical application of CHCs removal by nZVI-based materials activating PS are also analyzed.

Abstract Bioaugmentation is a promising strategy for enhancing trichloroethylene (TCE) degradation in fractured rock. However, slow or incomplete biodegradation can lead to stalling at degradation byproducts such as 1,2-dichloroethene (cis-DCE) and vinyl chloride (VC). Over the course of 7 years, we examined the response of groundwater microbial populations in a bioaugmentation test where an emulsified vegetable oil solution (EOS®) and a dechlorinating consortium (KB-1®), containing the established dechlorinator Dehalococcoides (DHC), were injected into a TCE-contaminated fractured rock aquifer. Indigenous microbial communities responded within 2 days to added substrate and outcompeted KB-1®, and over the years of monitoring, several other notable turnover events were observed. Concentrations of ethene, the end product in reductive dechlorination, had the strongest correlations (P< .05) with members of Candidatus Colwellbacteria but their involvement in reductive dechlorination is unknown and warrants further investigation.DHC never exceeded 0.6% relative abundance of groundwater microbial communities, despite its previously presumed importance at the site. Increased concentrations of carbon dioxide, acetic acid, and methane were positively correlated with increasing ethene concentrations; however, concentrations of cis-DCE and VC remained high by the end of the monitoring period suggesting preferential enrichment of indigenous partial dechlorinators over bioaugmented complete dechlorinators. This study highlights the importance of characterizing in situ microbial populations to understand how they can potentially enhance or inhibit augmented TCE degradation. Indigenous microbial populations outcompete bioaugmented reductive dechlorinators at a fractured rock site containing trichloroethylene.

Both trichloroethylene (TCE) and tetrachloroethylene (PCE) are high-priority chemicals subject to numerous human health risk evaluations by a range of agencies. Metabolism of TCE and PCE determines their ultimate toxicity; important uncertainties exist in quantitative characterization of metabolism to genotoxic moieties through glutathione (GSH) conjugation and species differences therein. This study aimed to address these uncertainties using novel liver models, interspecies comparison, and a sensitive assay for quantification of GSH conjugates of TCE and PCE, -(1,2-dichlorovinyl)glutathione (DCVG) and -(1,2,2-trichlorovinyl) glutathione (TCVG), respectively. Liver models used herein were suspension, 2-D culture, and micropatterned coculture (MPCC) with primary human, rat, and mouse hepatocytes, as well as human induced pluripotent stem cell (iPSC)-derived hepatocytes (iHep). We found that, although efficiency of metabolism varied among models, consistent with known differences in their metabolic capacity, formation rates of DCVG and TCVG generally followed the patterns , and primary . Data derived from MPCC were most consistent with estimates from physiologically based pharmacokinetic models calibrated to data. For TCE, the new data provided additional empirical support for inclusion of GSH conjugation-mediated kidney effects as critical for the derivation of noncancer toxicity values. For PCE, the data reduced previous uncertainties regarding the extent of TCVG formation in humans; this information was used to update several candidate kidney-specific noncancer toxicity values. Overall, MPCC-derived data provided physiologically relevant estimates of GSH-mediated metabolism of TCE and PCE to reduce uncertainties in interspecies extrapolation that constrained previous risk evaluations, thereby increasing the precision of risk characterizations of these high-priority toxicants. https://doi.org/10.1289/EHP12006.

The halogenated solvents trichloroethylene (TCE) and perchloroethylene (PCE; also called tetrachloroethylene) are high priorities for study owing to their adverse human health effects. Certain key facts regarding TCE and PCE toxicity and metabolism are well established and have not been in dispute; these include the widespread presence of these solvents in ground- and drinking water, the classification of TCE as a known human carcinogen with the kidney and liver as primary targets, the classification of PCE as a probable human carcinogen with the strongest evidence for bladder cancer, and the prominent role of cytochrome P450s (CYPs) in mediating oxidative metabolism in both chemicals. However, uncertainty remains regarding both the activity and the toxicological importance of glutathione (GSH) conjugation of TCE and PCE in the liver and kidney in humans and rodents. Although the kidney is a recognized and accepted target organ for these two compounds, it is unclear whether kidney effects should be used to support derivation of noncancer toxicity values. In a study reported in this issue of Environmental Health Perspectives, Valdiviezo et al.

Biochar (BC) was used to remove trichloroethylene (TCE) from soil and water phases, and BC modification changed the sorption behavior of pollutants. Microplastics are emerging pollutants in the soil and water phases. Whether microplastics can affect the sorption of TCE by modified BC is not clear. Thus, batch sorption kinetics and isotherm experiments were conducted to elucidate the sorption of TCE on BC, and BC combined with polyethylene (PE) or polystyrene (PS). The results showed that HCl and NaOH modification increased TCE sorption on BC, while HNO3 modification inhibited TCE sorption on BC. When PE/PS and BC coexisted, the TCE sorption capacity decreased significantly on BC-CK + PE, BC-HCl + PE, BC-HNO3 + PE, BC-NaOH + PE, and BC-NaOH + PS, which was likely due to the preferential sorption of PE/PS on BC samples. We concluded that microplastics can change TCE sorption behavior and inhibit TCE sorption on BC samples. Thus, the interaction of BC and microplastics should be considered when BC is used for TCE removal in soil and water remediation.

This study investigated the feasibility and mechanism of sulfide-modified nanoscale zero-valent iron supported on biochar (S-nZVI@BC) for the removal of TCE in the scenario of groundwater remediation. The effects of some critical factors, including pyrolysis temperature of biochar, mass ratio of S-nZVI to BC, initial pH, typical groundwater compositions, co-contaminants, and particle aging time, on the TCE removal were examined. The results revealed that the different pyrolysis temperatures could change physicochemical properties of BC, which influenced the TCE adsorption and degradation by S-nZVI@BC. The mass ratio of S-nZVI to BC could determine the extent of adsorption and degradation of TCE. The total removal of TCE was not significantly influenced by the initial pH (3.0–9.0), but the degradation of TCE was enhanced at higher pH. Notably, the typical anions (SO42−, HCO3−, and HPO42−), humic acid, and co-contaminants (Cr(VI) and NO3−) in groundwater all slightly influenced the total removal of TCE, but markedly inhibited its degradation. Additionally, after exposure to air over different times (5 days, 10 days, 20 days, and 30 days), the reactivity of S-nZVI@BC composites was apparently decreased due to surface passivation. Nevertheless, the aged S-nZVI@BC composites still maintained relative high removal and degradation of TCE when the reaction time prolonged. Overall, the results showed that the S-nZVI@BC, combining the high adsorption capacity of BC and the high reductive capacity of S-nZVI, had a much better performance than the single S-nZVI or BC, suggesting that S-nZVI@BC is one promising material for the remediation of TCE-contaminated groundwater.