环境科学与技术最新文献_第10页

Sulfur-Intercalated Layered Double Hydroxides Minimize Microbial Mercury Methylation: Implications for In Situ Remediation of Mercury-Contaminated Sites 硫钙化层状双氢氧化物可将微生物的汞甲基化作用降至最低：汞污染场地原位修复的意义

IF 10.8 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-16 DOI: 10.1021/acs.est.4c0687010.1021/acs.est.4c06870

Xin Tong, Zhanhua Zhang, Xiaoyin Dong, Wenyu Guan, Zhenhai Liu, Jiubin Chen, Pedro J. J. Alvarez, Wei Chen and Tong Zhang*,

{"title":"Sulfur-Intercalated Layered Double Hydroxides Minimize Microbial Mercury Methylation: Implications for In Situ Remediation of Mercury-Contaminated Sites","authors":"Xin Tong, Zhanhua Zhang, Xiaoyin Dong, Wenyu Guan, Zhenhai Liu, Jiubin Chen, Pedro J. J. Alvarez, Wei Chen and Tong Zhang*, ","doi":"10.1021/acs.est.4c0687010.1021/acs.est.4c06870","DOIUrl":"https://doi.org/10.1021/acs.est.4c06870https://doi.org/10.1021/acs.est.4c06870","url":null,"abstract":"Conventional approaches for in situ remediation of mercury (Hg)-contaminated soils and sediments rely mostly on precipitation or adsorption. However, this can generate Hg-rich surfaces that facilitate microbial production of methylmercury (MeHg), a potent, bioaccumulative neurotoxin. Herein, we prove the concept that the risk of mercury methylation can be effectively minimized by adding sulfur-intercalated layered double hydroxide (S-LDH) to Hg-contaminated soils. Hg bound to S-LDH has minimal methylation potential when incubated with model methylating bacteria Pseudodesulfovibrio mercurii ND132 and Geobacter sulfurreducens PCA. With a combination of spectroscopic and microscopic evidence, as well as theoretical calculations, we confirm that dissolved Hg(II) tends to enter the interlayers of S-LDH to bind to the sulfur groups intercalated within, leading to the formation of nanoscale metacinnabar (β-HgS). This not only physically blocks the contact of methylating microorganisms but also inhibits secondary release of bound mercury in the presence of strong binding ligands in porewater. This study highlights the promising concept of in situ risk reduction of heavy metal contamination by inducing precipitation within (nano)confined domains, achieving a sustainable outcome of enhanced removal and reduced bioaccessibility for pollutants that may otherwise be bioavailable in the form of nanoprecipitates.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142310043","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}

引用次数: 0

Correction to “Multiomic Signatures of Traffic-Related Air Pollution in London Reveal Potential Short-Term Perturbations in Gut Microbiome-Related Pathways” 对 "伦敦交通相关空气污染的多组学特征揭示了肠道微生物相关途径的潜在短期干扰 "的更正

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-16 DOI: 10.1021/acs.est.4c09132

Sibo Lucas Cheng, Michael Hedges, Pekka Keski-Rahkonen, Anastasia Chrysovalantou Chatziioannou, Augustin Scalbert, Kian Fan Chung, Rudy Sinharay, David C. Green, Theo M. C. M. de Kok, Jelle Vlaanderen, Soterios A. Kyrtopoulos, Frank Kelly, Lützen Portengen, Paolo Vineis, Roel C. H. Vermeulen, Marc Chadeau-Hyam, Sonia Dagnino

{"title":"Correction to “Multiomic Signatures of Traffic-Related Air Pollution in London Reveal Potential Short-Term Perturbations in Gut Microbiome-Related Pathways”","authors":"Sibo Lucas Cheng, Michael Hedges, Pekka Keski-Rahkonen, Anastasia Chrysovalantou Chatziioannou, Augustin Scalbert, Kian Fan Chung, Rudy Sinharay, David C. Green, Theo M. C. M. de Kok, Jelle Vlaanderen, Soterios A. Kyrtopoulos, Frank Kelly, Lützen Portengen, Paolo Vineis, Roel C. H. Vermeulen, Marc Chadeau-Hyam, Sonia Dagnino","doi":"10.1021/acs.est.4c09132","DOIUrl":"https://doi.org/10.1021/acs.est.4c09132","url":null,"abstract":"The Acknowledgments and the authors’ affiliation have been corrected. Joint first authors. Joint last authors. This study was funded through a UK British Heart Foundation project grant number PGF/10/82/28608. It was also supported by the Imperial College/Kings College MRC-PHE for Environment and Health and the National Institute for Health Research (NIHR) Respiratory Disease Biomedical Research Unit at the Royal Brompton NHS Foundation Trust and Imperial College London. K.F.C. is a Senior Investigator of NIHR. This work was supported by the grant FP7 of the European Commission ‘Enhanced exposure assessment and omic profiling for high priority environmental exposures in Europe’ (EXPOsOMICS grant 308610 to P.V.). The Centre for Environment and Health is supported by the Medical Research Council and Public Health England (MR/ L01341X/1). We also acknowledge the EXPANSE (EU-H2020 grant 874627 to R.V.). This study was funded by the National Institute for Health Research (NIHR) Health Protection Research Unit for Chemical and Radiation Threats and Hazards at Imperial College London, a partnership between UK Health Security Agency (UKHSA) and Imperial College London. The views expressed are those of the authors and not necessarily those of the NIHR, UKHSA, or the Department of Health and Social Care. This article has not yet been cited by other publications.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142234257","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}

引用次数: 0

Methanogenic Potential of Sewer Microbiomes and Its Implications for Methane Emission 下水道微生物群的产甲烷潜力及其对甲烷排放的影响

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-16 DOI: 10.1021/acs.est.4c04005

Yuqing Yan, Jun-Jie Zhu, Harold D. May, Cuihong Song, Jinyue Jiang, Lin Du, Zhiyong Jason Ren

{"title":"Methanogenic Potential of Sewer Microbiomes and Its Implications for Methane Emission","authors":"Yuqing Yan, Jun-Jie Zhu, Harold D. May, Cuihong Song, Jinyue Jiang, Lin Du, Zhiyong Jason Ren","doi":"10.1021/acs.est.4c04005","DOIUrl":"https://doi.org/10.1021/acs.est.4c04005","url":null,"abstract":"The sewer system, despite being a significant source of methane emissions, has often been overlooked in current greenhouse gas inventories due to the limited availability of quantitative data. Direct monitoring in sewers can be expensive or biased due to access limitations and internal heterogeneity of sewer networks. Fortunately, since methane is almost exclusively biogenic in sewers, we demonstrate in this study that the methanogenic potential can be estimated using known sewer microbiome data. By combining data mining techniques and bioinformatics databases, we developed the first data-driven method to analyze methanogenic potentials using a data set containing 633 observations of 53 variables obtained from literature mining. The methanogenic potential in the sewer sediment was around 250–870% higher than that in the wet biofilm on the pipe and sewage water. Additionally, k-means clustering and principal component analysis linked higher methane emission rates (9.72 ± 51.3 kgCO2 eq m–3 d–1) with smaller pipe size, higher water level, and higher potentials of sulfate reduction in the wetted pipe biofilm. These findings exhibit the possibility of connecting microbiome data with biogenic greenhouse gases, further offering insights into new approaches for understanding greenhouse gas emissions from understudied sources.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142234254","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}

引用次数: 0

Sulfur-Intercalated Layered Double Hydroxides Minimize Microbial Mercury Methylation: Implications for In Situ Remediation of Mercury-Contaminated Sites 硫钙化层状双氢氧化物可将微生物的汞甲基化作用降至最低：汞污染场地原位修复的意义

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-16 DOI: 10.1021/acs.est.4c06870

Xin Tong, Zhanhua Zhang, Xiaoyin Dong, Wenyu Guan, Zhenhai Liu, Jiubin Chen, Pedro J. J. Alvarez, Wei Chen, Tong Zhang

{"title":"Sulfur-Intercalated Layered Double Hydroxides Minimize Microbial Mercury Methylation: Implications for In Situ Remediation of Mercury-Contaminated Sites","authors":"Xin Tong, Zhanhua Zhang, Xiaoyin Dong, Wenyu Guan, Zhenhai Liu, Jiubin Chen, Pedro J. J. Alvarez, Wei Chen, Tong Zhang","doi":"10.1021/acs.est.4c06870","DOIUrl":"https://doi.org/10.1021/acs.est.4c06870","url":null,"abstract":"Conventional approaches for in situ remediation of mercury (Hg)-contaminated soils and sediments rely mostly on precipitation or adsorption. However, this can generate Hg-rich surfaces that facilitate microbial production of methylmercury (MeHg), a potent, bioaccumulative neurotoxin. Herein, we prove the concept that the risk of mercury methylation can be effectively minimized by adding sulfur-intercalated layered double hydroxide (S-LDH) to Hg-contaminated soils. Hg bound to S-LDH has minimal methylation potential when incubated with model methylating bacteria Pseudodesulfovibrio mercurii ND132 and Geobacter sulfurreducens PCA. With a combination of spectroscopic and microscopic evidence, as well as theoretical calculations, we confirm that dissolved Hg(II) tends to enter the interlayers of S-LDH to bind to the sulfur groups intercalated within, leading to the formation of nanoscale metacinnabar (β-HgS). This not only physically blocks the contact of methylating microorganisms but also inhibits secondary release of bound mercury in the presence of strong binding ligands in porewater. This study highlights the promising concept of in situ risk reduction of heavy metal contamination by inducing precipitation within (nano)confined domains, achieving a sustainable outcome of enhanced removal and reduced bioaccessibility for pollutants that may otherwise be bioavailable in the form of nanoprecipitates.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142234085","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}

引用次数: 0

Generational Specific Recruitment of Arsenic- and Antimony-Reducing Microorganisms in Plant Root-Associated Niches for Adapting to Metalloid-Metal Pollution 植物根系相关生境中砷和锑还原微生物的代际特异性招募，以适应金属类金属污染

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-16 DOI: 10.1021/acs.est.4c05291

Huang Yu, Shengwei Liu, Wanlin Weng, Yijun Peng, Xinqi Cai, Yu Zhu, Pubo Chen, Dandan Zhang, Huanping Liu, Jiaxiong Zeng, Songfeng Liu, Zhili He, Qingyun Yan

{"title":"Generational Specific Recruitment of Arsenic- and Antimony-Reducing Microorganisms in Plant Root-Associated Niches for Adapting to Metalloid-Metal Pollution","authors":"Huang Yu, Shengwei Liu, Wanlin Weng, Yijun Peng, Xinqi Cai, Yu Zhu, Pubo Chen, Dandan Zhang, Huanping Liu, Jiaxiong Zeng, Songfeng Liu, Zhili He, Qingyun Yan","doi":"10.1021/acs.est.4c05291","DOIUrl":"https://doi.org/10.1021/acs.est.4c05291","url":null,"abstract":"The recruitment of microorganisms by plants can enhance their adaptability to environmental stressors, but how root-associated niches recruit specific microorganisms for adapting to metalloid-metal contamination is not well-understood. This study investigated the generational recruitment of microorganisms in different root niches of Vetiveria zizanioides (V. zizanioides) under arsenic (As) and antimony (Sb) stress. The V. zizanioides was cultivated in As- and Sb-cocontaminated mine soils (MS) and artificial pollution soils (PS) over two generations in controlled conditions. The root-associated microbial communities were analyzed through 16S rRNA, arsC, and aioA gene amplicon and metagenomics sequencing. V. zizanioides accumulated higher As(III) and Sb(III) in its endosphere in MS in the second generation, while its physiological indices in MS were better than those observed in PS. SourceTracker analysis revealed that V. zizanioides in MS recruited As(V)- and Sb(V)-reducing microorganisms (e.g., Sphingomonales and Rhodospirillaceae) into the rhizoplane and endosphere. Metagenomics analysis further confirmed that these recruited microorganisms carrying genes encoding arsenate reductases with diverse carbohydrate degradation abilities were enriched in the rhizoplane and endosphere, suggesting their potential to reduce As(V) and Sb(V) and to decompose root exudates (e.g., xylan and starch). These findings reveal that V. zizanioides selectively recruits As- and Sb-reducing microorganisms to mitigate As–Sb cocontamination during the generational growth, providing insights into novel strategies for enhancing phytoremediation of metalloid-metal contaminants.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142234255","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}

引用次数: 0

Seasonal Controls on Microbial Depolymerization and Oxidation of Organic Matter in Floodplain Soils 洪泛区土壤中微生物解聚和有机物氧化的季节性控制因素

IF 10.8 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-15 DOI: 10.1021/acs.est.4c0510910.1021/acs.est.4c05109

Cam G. Anderson, Malak M. Tfaily, Rosalie K. Chu, Nikola Tolić, Patricia M. Fox, Peter S. Nico, Scott Fendorf and Marco Keiluweit*,

{"title":"Seasonal Controls on Microbial Depolymerization and Oxidation of Organic Matter in Floodplain Soils","authors":"Cam G. Anderson, Malak M. Tfaily, Rosalie K. Chu, Nikola Tolić, Patricia M. Fox, Peter S. Nico, Scott Fendorf and Marco Keiluweit*, ","doi":"10.1021/acs.est.4c0510910.1021/acs.est.4c05109","DOIUrl":"https://doi.org/10.1021/acs.est.4c05109https://doi.org/10.1021/acs.est.4c05109","url":null,"abstract":"Floodplain soils are vast reservoirs of organic carbon often attributed to anaerobic conditions that impose metabolic constraints on organic matter degradation. What remains elusive is how such metabolic constraints respond to dynamic flooding and drainage cycles characteristic of floodplain soils. Here we show that microbial depolymerization and respiration of organic compounds, two rate-limiting steps in decomposition, vary spatially and temporally with seasonal flooding of mountainous floodplain soils (Gothic, Colorado, USA). Combining metabolomics and -proteomics, we found a lower abundance of oxidative enzymes during flooding coincided with the accumulation of aromatic, high-molecular weight compounds, particularly in surface soils. In subsurface soils, we found that a lower oxidation state of carbon coincided with a greater abundance of chemically reduced, energetically less favorable low-molecular weight metabolites, irrespective of flooding condition. Our results suggest that seasonal flooding temporarily constrains oxidative depolymerization of larger, potentially plant-derived compounds in surface soils; in contrast, energetic constraints on microbial respiration persist in more reducing subsurface soils regardless of flooding. Our work underscores that the potential vulnerability of these distinct anaerobic carbon storage mechanisms to changing flooding dynamics should be considered, particularly as climate change shifts both the frequency and extent of flooding in floodplains globally.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142310199","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}

引用次数: 0

Seasonal Controls on Microbial Depolymerization and Oxidation of Organic Matter in Floodplain Soils 洪泛区土壤中微生物解聚和有机物氧化的季节性控制因素

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-15 DOI: 10.1021/acs.est.4c05109

Cam G. Anderson, Malak M. Tfaily, Rosalie K. Chu, Nikola Tolić, Patricia M. Fox, Peter S. Nico, Scott Fendorf, Marco Keiluweit

{"title":"Seasonal Controls on Microbial Depolymerization and Oxidation of Organic Matter in Floodplain Soils","authors":"Cam G. Anderson, Malak M. Tfaily, Rosalie K. Chu, Nikola Tolić, Patricia M. Fox, Peter S. Nico, Scott Fendorf, Marco Keiluweit","doi":"10.1021/acs.est.4c05109","DOIUrl":"https://doi.org/10.1021/acs.est.4c05109","url":null,"abstract":"Floodplain soils are vast reservoirs of organic carbon often attributed to anaerobic conditions that impose metabolic constraints on organic matter degradation. What remains elusive is how such metabolic constraints respond to dynamic flooding and drainage cycles characteristic of floodplain soils. Here we show that microbial depolymerization and respiration of organic compounds, two rate-limiting steps in decomposition, vary spatially and temporally with seasonal flooding of mountainous floodplain soils (Gothic, Colorado, USA). Combining metabolomics and -proteomics, we found a lower abundance of oxidative enzymes during flooding coincided with the accumulation of aromatic, high-molecular weight compounds, particularly in surface soils. In subsurface soils, we found that a lower oxidation state of carbon coincided with a greater abundance of chemically reduced, energetically less favorable low-molecular weight metabolites, irrespective of flooding condition. Our results suggest that seasonal flooding temporarily constrains oxidative depolymerization of larger, potentially plant-derived compounds in surface soils; in contrast, energetic constraints on microbial respiration persist in more reducing subsurface soils regardless of flooding. Our work underscores that the potential vulnerability of these distinct anaerobic carbon storage mechanisms to changing flooding dynamics should be considered, particularly as climate change shifts both the frequency and extent of flooding in floodplains globally.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142234258","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}

引用次数: 0

Rapid and Highly Selective Fe(IV) Generation by Fe(II)-Peroxyacid Advanced Oxidation Processes: Mechanistic Investigation via Kinetics and Density Functional Theory 通过 Fe(II)-Peroxyacid 高级氧化过程快速、高选择性生成 Fe(IV)：通过动力学和密度泛函理论进行机理研究

IF 10.8 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-14 DOI: 10.1021/acs.est.4c0523410.1021/acs.est.4c05234

Junyue Wang, Juhee Kim, Jiaqi Li, Caroline Krall, Virender K. Sharma*, Daniel C. Ashley* and Ching-Hua Huang*,

{"title":"Rapid and Highly Selective Fe(IV) Generation by Fe(II)-Peroxyacid Advanced Oxidation Processes: Mechanistic Investigation via Kinetics and Density Functional Theory","authors":"Junyue Wang, Juhee Kim, Jiaqi Li, Caroline Krall, Virender K. Sharma*, Daniel C. Ashley* and Ching-Hua Huang*, ","doi":"10.1021/acs.est.4c0523410.1021/acs.est.4c05234","DOIUrl":"https://doi.org/10.1021/acs.est.4c05234https://doi.org/10.1021/acs.est.4c05234","url":null,"abstract":"High-valent iron (Fe(IV/V/VI)) has been widely applied in water decontamination. However, common Fe(II)-activating oxidants including hydrogen peroxide (H2O2) and persulfate react slowly with Fe(II) and exhibit low selectivity for Fe(IV) production due to the cogeneration of radicals. Herein, we report peroxyacids (POAs; R–C(O)OOH) that can react with Fe(II) more than 3 orders of magnitude faster than H2O2, with high selectivity for Fe(IV) generation. Rapid degradation of bisphenol A (BPA, an endocrine disruptor) was achieved by the combination of Fe(II) with performic acid (PFA), peracetic acid (PAA), or perpropionic acid (PPA) within one second. Experiments with phenyl methyl sulfoxide (PMSO) and tert-butyl alcohol (TBA) revealed Fe(IV) as the major reactive species in all three Fe(II)-POA systems, with a minor contribution of radicals (i.e., •OH and R–C(O)O•). To understand the exceptionally high reactivity of POAs, a detailed computational comparison among the Fenton-like reactions with step-by-step thermodynamic evaluation was conducted. The high reactivity is attributed to the lower energy barriers for O–O bond cleavage, which is determined as the rate-limiting step for the Fenton-like reactions, and the thermodynamically favorable bidentate binding pathway of POA with iron. Overall, this study advances knowledge on POAs as novel Fenton-like reagents and sheds light on computational chemistry for these systems.This paper systematically studied the Fenton-like reactions of three different peroxyacids (performic acid, peracetic acid, and perpropionic acid) and elucidated their high reactivity from experimental and computational perspectives.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.est.4c05234","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142310197","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Rapid and Highly Selective Fe(IV) Generation by Fe(II)-Peroxyacid Advanced Oxidation Processes: Mechanistic Investigation via Kinetics and Density Functional Theory 通过 Fe(II)-Peroxyacid 高级氧化过程快速、高选择性生成 Fe(IV)：通过动力学和密度泛函理论进行机理研究

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-14 DOI: 10.1021/acs.est.4c05234

Junyue Wang, Juhee Kim, Jiaqi Li, Caroline Krall, Virender K. Sharma, Daniel C. Ashley, Ching-Hua Huang

{"title":"Rapid and Highly Selective Fe(IV) Generation by Fe(II)-Peroxyacid Advanced Oxidation Processes: Mechanistic Investigation via Kinetics and Density Functional Theory","authors":"Junyue Wang, Juhee Kim, Jiaqi Li, Caroline Krall, Virender K. Sharma, Daniel C. Ashley, Ching-Hua Huang","doi":"10.1021/acs.est.4c05234","DOIUrl":"https://doi.org/10.1021/acs.est.4c05234","url":null,"abstract":"High-valent iron (Fe(IV/V/VI)) has been widely applied in water decontamination. However, common Fe(II)-activating oxidants including hydrogen peroxide (H2O2) and persulfate react slowly with Fe(II) and exhibit low selectivity for Fe(IV) production due to the cogeneration of radicals. Herein, we report peroxyacids (POAs; R–C(O)OOH) that can react with Fe(II) more than 3 orders of magnitude faster than H2O2, with high selectivity for Fe(IV) generation. Rapid degradation of bisphenol A (BPA, an endocrine disruptor) was achieved by the combination of Fe(II) with performic acid (PFA), peracetic acid (PAA), or perpropionic acid (PPA) within one second. Experiments with phenyl methyl sulfoxide (PMSO) and tert-butyl alcohol (TBA) revealed Fe(IV) as the major reactive species in all three Fe(II)-POA systems, with a minor contribution of radicals (i.e., •OH and R–C(O)O•). To understand the exceptionally high reactivity of POAs, a detailed computational comparison among the Fenton-like reactions with step-by-step thermodynamic evaluation was conducted. The high reactivity is attributed to the lower energy barriers for O–O bond cleavage, which is determined as the rate-limiting step for the Fenton-like reactions, and the thermodynamically favorable bidentate binding pathway of POA with iron. Overall, this study advances knowledge on POAs as novel Fenton-like reagents and sheds light on computational chemistry for these systems.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142231883","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}

引用次数: 0

Deciphering the Novel Picolinate-Mn(II)/peroxymonosulfate System for Sustainable Fenton-like Oxidation: Dominance of the Picolinate-Mn(IV)-peroxymonosulfate Complex 解密可持续芬顿氧化作用的新型烟酸锰（II）/过氧单硫酸盐体系：烟酸锰（IV）过氧化单硫酸盐复合物的优势

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-14 DOI: 10.1021/acs.est.4c05482

Lijun Niu, Zhipeng Luo, Wenzheng Chen, Xinyang Zhong, Huabin Zeng, Xin Yu, Mingbao Feng

{"title":"Deciphering the Novel Picolinate-Mn(II)/peroxymonosulfate System for Sustainable Fenton-like Oxidation: Dominance of the Picolinate-Mn(IV)-peroxymonosulfate Complex","authors":"Lijun Niu, Zhipeng Luo, Wenzheng Chen, Xinyang Zhong, Huabin Zeng, Xin Yu, Mingbao Feng","doi":"10.1021/acs.est.4c05482","DOIUrl":"https://doi.org/10.1021/acs.est.4c05482","url":null,"abstract":"A highly efficient and sustainable water treatment system was developed herein by combining Mn(II), peroxymonosulfate (PMS), and biodegradable picolinic acid (PICA). The micropollutant elimination process underwent two phases: an initial slow degradation phase (0–10 min) followed by a rapid phase (10–20 min). Multiple evidence demonstrated that a PICA-Mn(IV) complex (PICA-Mn(IV)*) was generated, acting as a conductive bridge facilitating the electron transfer between PMS and micropollutants. Quantum chemical calculations revealed that PMS readily oxidized the PICA-Mn(II)* to PICA-Mn(IV)*. This intermediate then complexed with PMS to produce PICA-Mn(IV)-PMS*, elongating the O–O bond of PMS and increasing its oxidation capacity. The primary transformation mechanisms of typical micropollutants mediated by PICA-Mn(IV)-PMS* include oxidation, ring-opening, bond cleavage, and epoxidation reactions. The toxicity assessment results showed that most products were less toxic than the parent compounds. Moreover, the Mn(II)/PICA/PMS system showed resilience to water matrices and high efficiency in real water environments. Notably, PICA-Mn(IV)* exhibited greater stability and a longer lifespan than traditional reactive oxygen species, enabling repeated utilization. Overall, this study developed an innovative, sustainable, and selective oxidation system, i.e., Mn(II)/PICA/PMS, for rapid water decontamination, highlighting the critical role of in situ generated Mn(IV).","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142231884","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}

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