Thermal treatment of perfluoroalkyl and polyfluoroalkyl substances (PFASs) presents a promising opportunity to halt the PFAS cycle. However, how co-occurring materials such as granular activated carbon (GAC) influence thermal decomposition products of PFASs, and underlying mechanisms remain unclear. We studied the pyrolysis of two potassium salts of perfluoroalkanesulfonates (PFSAs, CFSOK), perfluorobutanesulfonate (PFBS-K), and perfluorooctanesulfonate (PFOS-K), with or without GAC.
View Article and Find Full Text PDFUnlabelled: The acetogen couples caffeate reduction with ferredoxin reduction and NADH oxidation via electron bifurcation, providing additional reduced ferredoxin for energy conservation and cell synthesis. Caffeate is first activated by an acyl-CoA synthetase (CarB), which ligates CoA to caffeate at the expense of ATP. After caffeoyl-CoA is reduced to hydrocaffeoyl-CoA, the CoA moiety in hydrocaffeoyl-CoA could be recycled for caffeoyl-CoA synthesis by an ATP-independent CoA transferase (CarA) to save energy.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
July 2024
Per- and polyfluoroalkyl substances (PFAS), particularly the perfluorinated ones, are recalcitrant to biodegradation. By integrating an enrichment culture of reductive defluorination with biocompatible electrodes for the electrochemical process, a deeper defluorination of a C-perfluorinated unsaturated PFAS was achieved compared to the biological or electrochemical system alone. Two synergies in the bioelectrochemical system were identified: i) The in-series microbial-electrochemical defluorination and ii) the electrochemically enabled microbial defluorination of intermediates.
View Article and Find Full Text PDFEnzymatic cleavage of C─F bonds in per- and polyfluoroalkyl substances (PFAS) is largely unknown but avidly sought to promote systems biology for PFAS bioremediation. Here, we report the reductive defluorination of α, β-unsaturated per- and polyfluorocarboxylic acids by spp. The microbial defluorination products were structurally confirmed and showed regiospecificity and stereospecificity, consistent with their formation by enzymatic reactions.
View Article and Find Full Text PDFHydrogen-tuned 185 nm vacuum ultraviolet (VUV/H) photolysis is an emerging technology to destroy per- and polyfluoroalkyl substance (PFAS) in brine. This study discovered the promotive effects of two major brine anions, i.e.
View Article and Find Full Text PDFThe spread of antimicrobial resistance (AMR) in agricultural systems via irrigation water is a serious public health issue as it can be transmitted to humans through the food chain. Therefore, understanding the dissemination routes of antibiotic resistance genes (ARGs) in agricultural systems is crucial for the assessment of health risks associated with eating fresh vegetables such as spinach and radish irrigated with treated municipal wastewater (TMW). In this study, we investigated the bacterial community structure and resistome in the soil-plant-earthworm continuum after irrigation of spinach and radish with TMW containing the antibiotics trimethoprim (TMP), sulfamethoxazole (SMZ), and sulfapyridine (SPD) using 16S rRNA gene sequencing and high throughput quantitative PCR (HT-qPCR).
View Article and Find Full Text PDFThe total oxidizable precursor (TOP) assay has been extensively used for detecting PFAS pollutants that do not have analytical standards. It uses hydroxyl radicals (HO) from the heat activation of persulfate under alkaline pH to convert H-containing precursors to perfluoroalkyl carboxylates (PFCAs) for target analysis. However, the current TOP assay oxidation method does not apply to emerging PFAS because (i) many structures do not contain C-H bonds for HO attack and (ii) the transformation products are not necessarily PFCAs.
View Article and Find Full Text PDFChlorinated polyfluorocarboxylic acids (Cl-PFCAs) derived from the widely used chlorotrifluoroethylene (CTFE) polymers and oligomers may enter and influence the aquatic environment. Here, we report significant defluorination of Cl-PFCAs by an anaerobic microbial community via novel pathways triggered by anaerobic microbial dechlorination. Cl-PFCAs first underwent microbial reductive, hydrolytic, and eliminative dechlorination, and it was the hydrolytic dechlorination that led to significant spontaneous defluorination.
View Article and Find Full Text PDFEnzymatic cleavage of C-F bonds in per- and polyfluoroalkyl substances (PFAS) is largely unknown but avidly sought to promote systems biology for PFAS bioremediation. Here, we report the reductive defluorination of α, β-unsaturated per- and polyfluorocarboxylic acids by spp. Two critical molecular features in species enabling reductive defluorination are (i) a functional fluoride efflux transporter (CrcB) and (ii) an electron-bifurcating caffeate reduction pathway (CarABCDE).
View Article and Find Full Text PDFTreated municipal wastewater (TMW) can provide a reliable source of irrigation water for crops, which is especially important in arid areas where water resources are limited or prone to drought. Nonetheless, TMW may contain residual antibiotics, potentially exposing the crops to these substances. The goal of this study was to investigate the dissemination of antibiotics resistance genes (ARGs) in the soil-plant-earthworm continuum after irrigation of spinach and radish plants with TMW containing trimethoprim, sulfamethoxazole, and sulfapyridine in a greenhouse experiment, followed by feeding of earthworms with harvested plant materials.
View Article and Find Full Text PDFNanoscale Horiz
November 2023
The increasing prevalence of antibiotic-resistant bacterial infections, particularly methicillin-resistant (MRSA), presents a significant public health concern. Timely detection of MRSA is crucial to enable prompt medical intervention, limit its spread, and reduce antimicrobial resistance. Here, we introduce a miniaturized nano-sieve device featuring a pneumatically-regulated chamber for highly efficient MRSA purification from human plasma samples.
View Article and Find Full Text PDFThe increasing prevalence of antibiotic-resistant bacterial infections, particularly methicillin-resistant Staphylococcus aureus (MRSA), presents a significant public health concern. Timely detection of MRSA is crucial to enable prompt medical intervention, limit its spread, and reduce antimicrobial resistance. Here, we introduce a miniaturized nano-sieve device featuring a pneumatically-regulated chamber for highly efficient MRSA purification from human plasma samples.
View Article and Find Full Text PDFReliable chemical property data are the key to defensible and unbiased assessments of chemical emissions, fate, hazard, exposure, and risks. However, the retrieval, evaluation, and use of reliable chemical property data can often be a formidable challenge for chemical assessors and model users. This comprehensive review provides practical guidance for use of chemical property data in chemical assessments.
View Article and Find Full Text PDFGraphitic carbon nitride (g-CN) nanomaterials hold great promise in diverse applications; however, their stability in engineering systems and transformation in nature are largely underexplored. We evaluated the stability, aging, and environmental impact of g-CN nanosheets under the attack of free chlorine and reactive chlorine species (RCS), a widely used oxidant/disinfectant and a class of ubiquitous radical species, respectively. g-CN nanosheets were slowly oxidized by free chlorine even at a high concentration of 200-1200 mg L, but they decomposed rapidly when ClO· and/or Cl were the key oxidants.
View Article and Find Full Text PDFBenzimidazole fungicides are frequently detected in aquatic environments and pose a serious health risk. Here, we investigated the metabolic capacity of the recently discovered complete ammonia-oxidizing (comammox) Nitrospira inopinata and kreftii to transform a representative set of benzimidazole fungicides (i.e.
View Article and Find Full Text PDFUnder the ongoing climate change scenario, treated municipal wastewater (TMW) is a potential candidate for irrigated agriculture but may result in the exposure of agricultural environments to antibiotics. We studied the transfers of trimethoprim, sulfamethoxazole, and sulfapyridine in the TMW-soil-plant-earthworm continuum under greenhouse/laboratory conditions. Irrigation of potted spinach and radish with as-collected TMW resulted in no transfers of antibiotics into soil or plants owing to their low concentrations in the tertiary-treated TMW.
View Article and Find Full Text PDFIn most cases, point-of-use tap water quality is not routinely monitored due to widely-dispersed sampling sites and the costly tests. Although previous studies have revealed the variation of drinking water quality during distribution in municipal networks, the influence of aging pipes in buildings on quality is still unknown and this makes it difficult for water utilities to conduct regular maintenance. Herein, we have undertaken a survey of tap water samples across 8 districts in Beijing (China) to evaluate the potential effects of pipe age on point-of-use water quality, including turbidity, organic matter characteristics, and bacterial community.
View Article and Find Full Text PDFThe recently discovered microbial reductive defluorination of two C branched and unsaturated fluorinated carboxylic acids (FCAs) provided valuable insights into the environmental fate of per- and polyfluoroalkyl substances (PFASs) and potential bioremediation strategies. However, a systematic investigation is needed to further demonstrate the role of C═C double bonds in the biodegradability of unsaturated PFASs. Here, we examined the structure-biodegradability relationships of 13 FCAs, including nine commercially available unsaturated FCAs and four structurally similar saturated ones, in an anaerobic defluorinating enrichment and an activated sludge community.
View Article and Find Full Text PDFPer- and polyfluoroalkyl substances (PFAS) are a large group of manmade chemicals that impose emerging environmental concerns. Among them, short-chain per- and polyfluorinated carboxylic acids represent an important subgroup used as building blocks of biologically active chemicals and functional materials. Some are also considered PFAS alternatives, and some could be byproducts of the physicochemical treatment of PFAS.
View Article and Find Full Text PDFThe addition of iodide (I) in the UV/sulfite system (UV/S) significantly accelerated the reductive degradation of perfluorosulfonates (PFSAs, CFSO) and perfluorocarboxylates (PFCAs, CFCOO). Using the highly recalcitrant perfluorobutane sulfonate (CFSO) as a probe, we optimized the UV/sulfite + iodide system (UV/S + I) to degrade = 1-7 PFCAs and = 4, 6, 8 PFSAs. In general, the kinetics of per- and polyfluoroalkyl substance (PFAS) decay, defluorination, and transformation product formations in UV/S + I were up to three times faster than those in UV/S.
View Article and Find Full Text PDFSuperoxide and other reactive oxygen species (ROS) shape microbial communities and drive the transformation of metals and inorganic/organic matter. Taxonomically diverse bacteria and phytoplankton produce extracellular superoxide during laboratory cultivation. Understanding the physiological reasons for extracellular superoxide production by aerobes in the environment is a crucial question yet not fully solved.
View Article and Find Full Text PDFOmega-hydroperfluorocarboxylates (ω-HPFCAs, CF-(CF)-COO) are commercially available in bulk quantities and have been applied in agrochemicals, fluoropolymer production, and semiconductor coating. In this study, we used kinetic measurements, theoretical calculations, model compound experiments, and transformation product analyses to reveal novel mechanistic insights into the reductive and oxidative transformation of ω-HPFCAs. Like perfluorocarboxylates (PFCAs, CF-(CF)-COO), the direct linkage between CF- and -COO enables facile degradation under UV/sulfite treatment.
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