环境科学与技术Pub Date : 2025-06-20DOI: 10.1021/acs.est.4c14481
Xintong Liu,Bo Liang,Siyu Yao,Anqi Xiong,Xiaohua Zhang,Yajing Sun,Li Zhang,Changchao Li,Yuefei Ruan,Meng Yan,Yuen-Wa Ho,James K H Fang,Bei Wang,Frederic D L Leusch,Daniel Schlenk,Wenhua Liu,Kenneth Mei Yee Leung,Ling N Jin
{"title":"Dissecting the Role of Natural Toxins and Anthropogenic Contaminants in Mixture Effects of Seawater Chemical Cocktails on Cetacean Skin Fibroblasts.","authors":"Xintong Liu,Bo Liang,Siyu Yao,Anqi Xiong,Xiaohua Zhang,Yajing Sun,Li Zhang,Changchao Li,Yuefei Ruan,Meng Yan,Yuen-Wa Ho,James K H Fang,Bei Wang,Frederic D L Leusch,Daniel Schlenk,Wenhua Liu,Kenneth Mei Yee Leung,Ling N Jin","doi":"10.1021/acs.est.4c14481","DOIUrl":"https://doi.org/10.1021/acs.est.4c14481","url":null,"abstract":"Marine mammal skin, in contact with seawater containing diverse chemicals, reflects species health and environmental quality. The contributions of natural toxins and anthropogenic contaminants to the effects of such chemical mixtures remain poorly quantified. Using skin fibroblast cells from the Indo-Pacific finless porpoise and humpback dolphin, we assessed the toxic potential of seawater extracts, focusing on cytotoxicity and intracellular reactive oxygen species (ROS) formation. Among the 38 studied chemicals prevalent in seawater, four algal toxins were 1-6 orders of magnitude more potent than 30 anthropogenic chemicals, including antibiotics, ultraviolet filters, per- and polyfluoroalkyl substances (PFASs), and polyaromatic hydrocarbons. Pectenotoxin-2 accounted for 92% of the cytotoxicity triggered by the mixture of all studied chemicals, which collectively explained 34% of seawater-induced cytotoxicity in porpoise cells. For ROS induction, although all studied chemicals collectively explained a small fraction (<1%) of the effects elicited by seawater extracts in both cell lines, okadaic acid and gymnodimine accounted for ∼80% of the mixture effects of all chemicals, with additional contributions from PFASs. Extending the approach to other coastal habitats where concentration data are available revealed algal toxins as dominant contributors among the known contaminant mixtures eliciting dermal toxic potential. This study provides novel insights to guide the identification of toxicity contributors across dermal health end points, with a balanced perspective on natural toxins and anthropogenic contaminants in addressing their mixture effects on sentinel species health.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"7 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144328859","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Chemoautotrophic Carbon Fixation Favors Iron-Bound Organic Carbon Formation in Estuarine and Coastal Sediments.","authors":"Boshuang Wu, Xiufeng Tang, Zhenyang Song, Mengting Qi, Min Liu, Xiaofei Li, Lijun Hou","doi":"10.1021/acs.est.5c00324","DOIUrl":"https://doi.org/10.1021/acs.est.5c00324","url":null,"abstract":"<p><p>Chemoautotrophic carbon fixation (CCF) is crucial for carbon sequestration; however, how the CCF process mediates carbon preservation remains poorly understood. Here, we investigated the CCF process, iron-bound organic carbon (Fe-OC), and chemoautotrophs through FeS-amended and <i>in situ</i> field samples in estuarine and coastal sediments. The CCF rates and Fe-OC concentrations were substantially enhanced by FeS addition and were significantly higher under anaerobic conditions than under aerobic conditions. Sulfide rather than Fe<sup>2+</sup> facilitated CCF rates, while more Fe-OC formation was caused by Fe<sup>2+</sup>. More humic substances, aromatic protein, and high diffraction intensity in the presence of FeS indicated that iron oxides protect organic carbon against microbial degradation. The enhanced abundance of functional genes in relation to nitrification, sulfide, and iron oxidation, as well as <i>cbbL</i> and <i>cbbM</i> genes synchronously, favored the CCF process and Fe-OC formation. The CCF rates and Fe-OC concentrations were also higher in Fe<sup>2+</sup>─and sulfide-enriched field sediments, and a positive feedback relationship was observed between Fe-OC formation and the CCF process. These results highlighted that the chemoautotrophic process favors Fe-OC formation, in which the enhanced Fe-OC may restrain microbial degradation of organic carbon, thereby facilitating carbon retention and preservation. This preservation mechanism provided a robust pathway for carbon sequestration in estuarine and coastal wetlands, representing a negative climate warming feedback loop.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144336117","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Production of the Neurotoxin BMAA by Marine Diatoms Drives Its Widespread Occurrence in Estuarine and Coastal Ecosystems.","authors":"Chao Wang,Mengsheng Xia,Yixi Su,Yuexuan Shu,Weizhao Meng,Jiahao Ma,Jiwei Chen,Pengbin Wang,Mathew Seymour,Weiqi Fu","doi":"10.1021/acs.est.5c00636","DOIUrl":"https://doi.org/10.1021/acs.est.5c00636","url":null,"abstract":"Phytoplankton are the primary producers of marine neurotoxins such as β-N-methylamino-l-alanine (BMAA), which cause seafood poisoning outbreaks in estuarine and coastal regions. BMAA has gained much attention for its pathogenic link to Alzheimer's and Parkinson's disease. However, whether BMAA accumulates in diatoms under fluctuations in estuarine and coastal areas remains largely unknown. In this study, we investigated BMAA biosynthesis in the model diatom Phaeodactylum tricornutum under simulated conditions of fluctuating nitrogen and salinity in estuarine regions. BMAA was detectable in P. tricornutum under all simulated seawater or hyper-eutrophic conditions, although nitrogen source and salinity interactively impact BMAA accumulation. In addition, high-nitrogen wastewater conditions promoted carbon metabolism, including the Calvin cycle, glycolysis, fatty acid biosynthesis, and decreased nitrogen metabolism and BMAA production. Finally, we proposed and elucidated a complete biosynthetic pathway of BMAA originating from glutamate, incorporating catalysis by S-adenosylmethionine (SAM)-dependent methyltransferases in diatoms, as inferred through artificial intelligence-based pathway analysis. This study marks the first attempt to decipher the BMAA metabolic pathway in diatoms, which provides a paradigm shift to identify conditions that trigger toxin production and also provides valuable metrics to address the complexity and unpredictability of monitoring and forecasting algal blooms.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"32 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144328858","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
环境科学与技术Pub Date : 2025-06-20DOI: 10.1021/acs.est.5c03323
Hai-Bo Wang, Xi-Peng Liu, Yu-Chen Shu, Gang Li, Cheng-Liang Sun, Davey L Jones, Yong-Guan Zhu, Xian-Yong Lin
{"title":"Molecular Composition of Exogenous Dissolved Organic Matter Regulates Dissimilatory Iron Reduction and Carbon Emissions in Paddy Soil.","authors":"Hai-Bo Wang, Xi-Peng Liu, Yu-Chen Shu, Gang Li, Cheng-Liang Sun, Davey L Jones, Yong-Guan Zhu, Xian-Yong Lin","doi":"10.1021/acs.est.5c03323","DOIUrl":"https://doi.org/10.1021/acs.est.5c03323","url":null,"abstract":"<p><p>Soil carbon (C) cycling under anoxic conditions is mechanistically linked to dissimilatory iron (Fe) reduction, potentially influenced by exogenous dissolved organic matter (DOM). However, the impact of complex exogenous DOM on soil microbial activity and C-Fe coupling in paddy soils remains underexplored. With a 100-day microcosm experiment, we found that biochar-DOM significantly promoted Fe reduction and accelerated CH<sub>4</sub> and CO<sub>2</sub> emissions, and manure-DOM increased soil CO<sub>2</sub> emissions. These effects may be caused by the following mechanisms: DOM molecules with high aromaticity and high double bond equivalence (DBE), including lignins-polyphenols, lignins-polycyclic aromatics, and condensed aromatics-polycyclic aromatics, promoted soil Fe reduction and CH<sub>4</sub> emissions with enrichment of soil Fe-reducing bacteria, r-strategists, and reduction of methanotrophs at the early stage of incubation. Conversely, DOM with low aromaticity, low DBE, and high H/C enhanced CO<sub>2</sub> emissions with the enhancement of recalcitrant C degradation and CH<sub>4</sub> oxidation at the late stage of incubation. In conclusion, our study highlights the importance of the molecular composition of organic amendment-derived DOM in regulating soil Fe reduction and greenhouse gas emissions. The findings offer novel insights into the effective utilization of agricultural resources and the potential mitigation of greenhouse gas production and emissions.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144336118","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
环境科学与技术Pub Date : 2025-06-20DOI: 10.1021/acs.est.5c02364
Elisabeth Woeldgen,Roger Teoh,Marc E J Stettler,Robert Malina
{"title":"Sustainable Aviation Fuel Deployment Strategies in Europe: Supply Chain Implications and Climate Benefits.","authors":"Elisabeth Woeldgen,Roger Teoh,Marc E J Stettler,Robert Malina","doi":"10.1021/acs.est.5c02364","DOIUrl":"https://doi.org/10.1021/acs.est.5c02364","url":null,"abstract":"Sustainable aviation fuel (SAF) could reduce aviation's CO2 and contrail climate forcing. This study quantifies the contrail mitigation potential and fuel supply chain costs of a uniform SAF distribution scenario, assuming all departing flights use a 10% SAF blend by mass. Building on this, we propose three SAF allocation strategies that optimize the same SAF supply to maximize contrail mitigation, while considering real-world supply chain constraints and additional costs. A seasonal strategy - providing SAF to all flights from October to February at higher blend ratios (28%) - achieves the highest benefit-to-cost ratio (1.7-7.2) and lowest abatement cost (€14-61/tCO2e). It raises annual reductions in contrail energy forcing (EFcontrail) from 7-8% (uniform vs no-SAF scenario) to 12-13%, with supply chain costs rising by 0.5% relative to the uniform scenario. Two diurnal strategies - one targeting flights after 16:00 local time and another adding a constraint of selecting flights with >250 km of persistent contrails - have lower benefit-to-cost ratios (0.2-2.4) and higher abatement costs (€42-675/tCO2e). Their 1-2% rise in supply chain costs relative to the uniform scenario outweighs the additional contrail climate benefits, as annual EFcontrail reductions only rise from 7-8% (uniform scenario) to 9-17%.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"15 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144328673","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
环境科学与技术Pub Date : 2025-06-20DOI: 10.1021/acs.est.4c11600
Silvia Dudášová,Urs Berger,Bettina Seiwert,Thorsten Reemtsma,Oliver J Lechtenfeld,Qiuguo Fu
{"title":"Retrospective Identification of Novel and Legacy Per- and Polyfluoroalkyl Substances in German Archived Fish Livers Using a Combined High-Resolution Mass Spectrometry Approach.","authors":"Silvia Dudášová,Urs Berger,Bettina Seiwert,Thorsten Reemtsma,Oliver J Lechtenfeld,Qiuguo Fu","doi":"10.1021/acs.est.4c11600","DOIUrl":"https://doi.org/10.1021/acs.est.4c11600","url":null,"abstract":"Per- and polyfluoroalkyl substances (PFAS) are persistent environmental pollutants with many unknown variants, posing potential ecosystem and human health risks. To comprehensively assess PFAS contamination and overcome the challenge of unknown PFAS identification, we combined Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) and liquid chromatography─quadrupole time-of-flight mass spectrometry (LC-QTOF MS) to identify novel and Legacy PFAS in archived bream liver samples collected in Germany between 1996 and 2020. By leveraging the ultrahigh resolution and mass accuracy of FT-ICR MS, we generated a mass list for cross-comparison with common precursor ion features from LC-QTOF MS. We identified 78 PFAS, including 68 classified into 12 homologue groups and 10 that did not fit into any homologue series, encompassing perfluoroalkyl acids, fluorotelomer-based substances, pentafluorosulfide perfluoroalkyl sulfonic acids, polyfluoroalkyl sulfinates, polyfluoroalkyl sulfonyl sulfonamides, and other novel compounds including ionic liquids. Spatial and temporal analysis revealed that perfluoroalkyl phosphinic acids (C6/C6, C6/C8) and polyfluoroalkyl sulfonic acids (n = 10) have a widespread presence, whereas tris(pentafluoroethyl)trifluorophosphate (FAP) and polyfluoroalkyl sulfonyl sulfonamides (n = 6) are more localized or have only recently emerged in specific regions. These findings underscore the need for continued monitoring to comprehensively understand exposure to PFAS and their long-term environmental impact.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"40 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144328860","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"A Hybrid Modeling Framework for Predicting Spatiotemporal Dynamics of Antimicrobial Resistance in Coastal Waters.","authors":"Xuneng Tong,Zhixin Xiang,Shin Giek Goh,Luhua You,Sanjeeb Mohapatra,Glendon Ong,Wei Ching Khor,Kyaw Thu Aung,Karina Yew-Hoong Gin","doi":"10.1021/acs.est.5c01927","DOIUrl":"https://doi.org/10.1021/acs.est.5c01927","url":null,"abstract":"Antimicrobial resistance (AMR) in aquatic environments poses a critical threat to both environmental and human health. This study presents a novel hybrid modeling framework that integrates a process-based hydrodynamic-environmental model with a data-driven approach to predict the spatiotemporal dynamics of AMR in coastal waters. Macrolide-related antimicrobial resistance genes (ARGs_Macro) were selected as representative markers. The model results were validated using data from a monthly sampling campaign conducted across Singapore's coastal waters, yielding a mean coefficient of determination (R2) of 0.693, a Nash-Sutcliffe efficiency (NSE) of 0.589, and a root-mean-square deviation (RMSE) of 0.0257 GC/16S rRNA across 12 sampling points. Lincomycin, pH, dissolved oxygen, zinc and temperature were identified as significant influencers of ARGs_Macro. Although Lincomycin is not classified as a macrolide, it ranks as the most important driver of ARGs_Macro due to its shared resistance mechanisms with macrolides, potentially facilitating cross-resistance. The spatiotemporal model results revealed that coastal areas, particularly in the northern part of Singapore, are vulnerable to significant ARG accumulation, with monsoon seasons amplifying the spread of AMR due to hydrodynamic conditions. This study highlights the development of a robust modeling framework that provides valuable insights into the environmental drivers of AMR in coastal waters, offering a foundation for regulatory strategies and future research aimed at mitigating the risks of antimicrobial resistance in aquatic environments.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"590 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144328684","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
环境科学与技术Pub Date : 2025-06-19DOI: 10.1021/acs.est.4c12633
Enrique E Rodriguez,Rebecca Dickman,Bradley Kennedy,Diana Aga,Abraham Noe-Hays,Krista R Wigginton,Olivier Jolliet,Nancy G Love
{"title":"Comparative Exposure Assessment of Crops Grown by Urine-Derived Fertilizer and Crops Irrigated with Reclaimed Water.","authors":"Enrique E Rodriguez,Rebecca Dickman,Bradley Kennedy,Diana Aga,Abraham Noe-Hays,Krista R Wigginton,Olivier Jolliet,Nancy G Love","doi":"10.1021/acs.est.4c12633","DOIUrl":"https://doi.org/10.1021/acs.est.4c12633","url":null,"abstract":"Urine-derived fertilizers (UDFs) are a sustainable alternative to energy-intensive and environmentally damaging synthetic fertilizers; however, contaminant concerns must be addressed. Source-separated urine contains pharmaceutical compounds that could pose a risk to the environment and public health. While treatment technologies that address pharmaceutical contamination in UDF have been proposed, little is known about the exposure and risk to public health that UDF-fertilized crops pose. We assessed pharmaceutical uptake by lettuce exposed to UDF spiked with pharmaceuticals at two levels: the highest reported concentrations from the literature and at a level 10 times this amount to represent a worst-case scenario for UDF application. Between 0.00004% and 0.0002% of the applied pharmaceutical mass was taken up by lettuce. Exposure to pharmaceuticals through the consumption of UDF-fertilized crops is not significantly different from exposure through crops irrigated with reclaimed water (RW). Compared to therapeutic doses, the cumulative pharmaceutical ingestion associated with consuming UDF-fertilized vegetables every day over 70 years is up to 2.5% of the therapeutic dose of pharmaceuticals considered in this study. Our comparative exposure assessment reveals minimal exposures associated with the consumption of crops that are either fertilized by UDF or irrigated with RW, providing key insights for various stakeholders.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"41 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144328780","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
环境科学与技术Pub Date : 2025-06-19DOI: 10.1021/acs.est.5c00871
Liuwei Wang,Caide Huang,Junhao Cao,Pingfan Zhou,Siqi Han,Guangyu Qu,Michael S Bank,Deyi Hou
{"title":"Polymer Type, Oxidation, Size, and Abundance of Microplastics in Subsoils versus Topsoils with Varying Land Use in Beijing, China.","authors":"Liuwei Wang,Caide Huang,Junhao Cao,Pingfan Zhou,Siqi Han,Guangyu Qu,Michael S Bank,Deyi Hou","doi":"10.1021/acs.est.5c00871","DOIUrl":"https://doi.org/10.1021/acs.est.5c00871","url":null,"abstract":"The occurrence of microplastics (MPs) in topsoil is well documented; however, recent evidence has also shown that MPs can reach the subsoil, which may eventually enter groundwater aquifers posing a potential threat to drinking water. In this study, we examined polymer-type specific, small-sized MPs (20-500 μm) in both topsoil (5 cm) and subsoil (50 and 100 cm) in the megacity of Beijing, China, using Laser Direct Infrared (LDIR) Chemical Imaging Spectroscopy, focusing on variation in abundance, size, polymer type, and oxidation characteristics across 6 land use types. A total of 6085 MP particles with 11 polymer types were identified. MP abundance in subsoils was significantly lower, and they were surprisingly larger in size and less oxidized. MP distribution in subsoils was enhanced in fine-textured and iron (Fe)-depleted soils. Based on these findings, we conducted additional column migration experiments using different textured vadose zones, either with or without hematite, as a typical Fe oxide. Two scenarios were set, including continuous water infiltration and wet-dry cycling conditions. Field data strongly reflected our lab experiments under wet-dry cycling, suggesting that preferential penetration rather than filtration served as the likely primary mechanism of MP occurrence in subsoil.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"15 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144328832","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
环境科学与技术Pub Date : 2025-06-19DOI: 10.1021/acs.est.5c04015
Xuemei Zhu,Chao Yang,Qing Du,Wenhan Wang,Changwei Lü,Hongwen Sun,Chengmei Liao,Xin Wang
{"title":"Breaking the Carbon-Fluorine Stronghold: Reductive Defluorination of PFASs.","authors":"Xuemei Zhu,Chao Yang,Qing Du,Wenhan Wang,Changwei Lü,Hongwen Sun,Chengmei Liao,Xin Wang","doi":"10.1021/acs.est.5c04015","DOIUrl":"https://doi.org/10.1021/acs.est.5c04015","url":null,"abstract":"Per/polyfluoroalkyl substances (PFASs), characterized by their ultrastable C-F bonds and pervasive environmental persistence, present critical remediation challenges due to their recalcitrance and bioaccumulative potential. Conventional oxidative degradation methods predominantly yield bioaccumulative short-chain fluorinated derivatives, failing to achieve molecular annihilation. We highlight reductive defluorination as a transformative strategy to directly cleave C-F bonds and mitigate toxicity through two distinct electron-transfer modalities: indirect routes mediated by reactive species (e.g., hydrated electrons/active hydrogen) contrasted with direct mechanisms employing biocatalytic or electrochemical systems for targeted electron injection. Mechanistic taxonomy and quantitative structure-reactivity analyses reveal that defluorination efficiency is governed by the molecular architecture (e.g., chain length and fluorination patterns) and operational parameters (e.g., pH, redox potentials, and solution matrices). While standalone reductive technologies face scalability constraints from energy intensity and secondary contamination risks, synergistic integration of bioremediation-electrochemical-photocatalytic systems demonstrates enhanced defluorination efficiency. By coupling molecular-level degradation mechanisms with modular engineering, we propose future directions for developing reductive defluorination, offering a sustainable pathway to eliminate environmental recalcitrance and comply with evolving global water quality mandates.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"44 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144328685","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}