IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-26 DOI: 10.1021/acs.est.4c07159

Bifeng Zhang, Jiawei Yang, Yibo Mu, Xiaoyu Ji, Yandi Cai, Nan Jiang, Shaohua Xie, Qiuhui Qian, Fudong Liu, Wei Tan, Lin Dong

{"title":"Fabrication of Highly Dispersed Ru Catalysts on CeO2 for Efficient C3H6 Oxidation","authors":"Bifeng Zhang, Jiawei Yang, Yibo Mu, Xiaoyu Ji, Yandi Cai, Nan Jiang, Shaohua Xie, Qiuhui Qian, Fudong Liu, Wei Tan, Lin Dong","doi":"10.1021/acs.est.4c07159","DOIUrl":"https://doi.org/10.1021/acs.est.4c07159","url":null,"abstract":"Emissions of volatile organic compounds (VOCs) threaten both the environment and human health. To realize the elimination of VOCs, Ru/CeO2 catalysts have been intensively investigated and applied. Although it has been widely acknowledged that the catalytic performance of platinum group metal catalysts was highly determined by their dispersion and coordination environment, the most reactive structures on Ru/CeO2 catalysts for VOCs oxidation are still ambiguous. In this work, starting from Ce-BTC (BTC = 1,3,5-benzenetricarboxylic acid) materials, atomically dispersed Ru catalysts and agglomerated Ru catalysts were successfully created via one-step hydrothermal method (Ru-CeO2-BTC) and conventional incipient wetness impregnation method (Ru/CeO2-BTC), respectively. In a typical model reaction of C3H6 oxidation, atomically dispersed Ruδ+ species with the formation of abundant Ru–O–Ce linkages on Ru-CeO2-BTC were found to perform much better than agglomerated RuOx species on Ru/CeO2-BTC. Further characterizations and mechanism study disclosed that Ru-CeO2-BTC catalyst with atomically dispersed Ru ions and more superior low temperature redox performance compared to Ru/CeO2-BTC could better facilitate the adsorption/activation of C3H6 and the decomposition/desorption of intermediates, thus exhibiting superior C3H6 oxidation activity. This work elucidated the reactive sites on Ru/CeO2 catalysts in the C3H6 oxidation reaction and provided insightful guidance for designing efficient Ru/CeO2 catalysts to eliminate VOCs.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325700","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

The Pivotal Role of Heavy Terpenes and Anthropogenic Interactions in New Particle Formation on the Southeastern Qinghai-Tibet Plateau 青藏高原东南部新粒子形成过程中重萜烯和人为相互作用的关键作用

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-26 DOI: 10.1021/acs.est.4c04112

Yuliang Liu, Wei Nie, Ximeng Qi, Yuanyuan Li, Tao Xu, Chong Liu, Dafeng Ge, Liangduo Chen, Guangdong Niu, Jinbo Wang, Liwen Yang, Lei Wang, Caijun Zhu, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Qiaozhi Zha, Chao Yan, Chunxiang Ye, Guoxian Zhang, Renzhi Hu, Ru-Jin Huang, Xuguang Chi, Tong Zhu, Aijun Ding

{"title":"The Pivotal Role of Heavy Terpenes and Anthropogenic Interactions in New Particle Formation on the Southeastern Qinghai-Tibet Plateau","authors":"Yuliang Liu, Wei Nie, Ximeng Qi, Yuanyuan Li, Tao Xu, Chong Liu, Dafeng Ge, Liangduo Chen, Guangdong Niu, Jinbo Wang, Liwen Yang, Lei Wang, Caijun Zhu, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Qiaozhi Zha, Chao Yan, Chunxiang Ye, Guoxian Zhang, Renzhi Hu, Ru-Jin Huang, Xuguang Chi, Tong Zhu, Aijun Ding","doi":"10.1021/acs.est.4c04112","DOIUrl":"https://doi.org/10.1021/acs.est.4c04112","url":null,"abstract":"Aerosol particles originating from the Qinghai-Tibet Plateau (QTP) readily reach the free troposphere, potentially affecting global radiation and climate. Although new particle formation (NPF) is frequently observed at such high altitudes, its precursors and their underlying chemistry remain poorly understood. This study presents direct observational evidence of anthropogenic influences on biogenic NPF on the southeastern QTP, near the Himalayas. The mean particle nucleation rate (J1.7) is 2.6 cm–3 s–1, exceeding the kinetic limit of sulfuric acid (SA) nucleation (mean SA: 2.4 × 105 cm–3). NPF is predominantly driven by highly oxygenated organic molecules (HOMs), possibly facilitated by low SA levels. We identified 1538 ultralow-volatility HOMs driving particle nucleation and 764 extremely low-volatility HOMs powering initial particle growth, with mean total concentrations of 1.5 × 106 and 3.7 × 106 cm–3, respectively. These HOMs are formed by atmospheric oxidation of biogenic precursors, unexpectedly including sesquiterpenes and diterpenes alongside the commonly recognized monoterpenes. Counterintuitively, over half of HOMs are organic nitrates, mainly produced by interacting with anthropogenic NOx via RO2+NO terminations or NO3-initiated oxidations. These findings advance our understanding of NPF mechanisms in this climate-sensitive region and underscore the importance of heavy terpene and NOx-influenced chemistry in assessing anthropogenic-biogenic interactions with climate feedbacks.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325926","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

Revisiting Contrail Ice Formation: Impact of Primary Soot Particle Sizes and Contribution of Volatile Particles 重新审视烟霞冰的形成：原生烟尘颗粒大小的影响和挥发性颗粒的贡献

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-26 DOI: 10.1021/acs.est.4c04340

Fangqun Yu, Bernd Kärcher, Bruce E. Anderson

{"title":"Revisiting Contrail Ice Formation: Impact of Primary Soot Particle Sizes and Contribution of Volatile Particles","authors":"Fangqun Yu, Bernd Kärcher, Bruce E. Anderson","doi":"10.1021/acs.est.4c04340","DOIUrl":"https://doi.org/10.1021/acs.est.4c04340","url":null,"abstract":"Aircraft contrails, formed largely on soot particles in current flights, are important for aviation’s non-CO2 climate impact. Here we show that the activation of nonvolatile soot particles during contrail formation is likely determined by the sizes of primary soot particles rather than the effective sizes of soot aggregates as assumed in previous studies, which can explain less-than-unity fractions of soot particles forming contrail ice particles as recently observed during ECLIF (Emission and CLimate Impact of alternative Fuels) campaigns. The smaller soot primary sizes compared to aggregate sizes delay the onset of contrail ice formation, increase the maximum plume supersaturation reached in the contrail plume, and thus increase the probability of small volatile particles contributing to the total contrail ice particle number. This study suggests that the range of conditions for volatile plume particles to contribute significantly to the contrail ice number budget is wider than previously thought. As the aviation industry is moving toward sustainable aviation fuel and/or lean-burning engine technology, which is expected to reduce not only the emission index of nonvolatile soot particles but also the sizes of primary soot particles, this study highlights the need to better understand how the combined changes may affect contrail formation, contribution of volatile particles, and climate impacts.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321630","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

Occurrence and Ecological Risk Assessment of Highly Toxic Halogenated Byproducts during Chlorination Decolorization of Textile Printing and Dyeing Wastewater 纺织印染废水氯化脱色过程中高毒性卤化副产物的出现及生态风险评估

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-26 DOI: 10.1021/acs.est.4c07888

Yukun Zhou, Tianyu Chen, Xiang Zhang, Ruiqing Chen, Nali Zhu, Lingxiangyu Li, Lixia Zhao, Zhigang Li, Yawei Wang, Guibin Jiang

{"title":"Occurrence and Ecological Risk Assessment of Highly Toxic Halogenated Byproducts during Chlorination Decolorization of Textile Printing and Dyeing Wastewater","authors":"Yukun Zhou, Tianyu Chen, Xiang Zhang, Ruiqing Chen, Nali Zhu, Lingxiangyu Li, Lixia Zhao, Zhigang Li, Yawei Wang, Guibin Jiang","doi":"10.1021/acs.est.4c07888","DOIUrl":"https://doi.org/10.1021/acs.est.4c07888","url":null,"abstract":"Textile printing and dyeing wastewater is a substantial source of highly toxic halogenated pollutants because of the chlorination decolorization. However, information on the occurrence and fate of the highly toxic halogenated byproducts, which are produced by chlorination decolorization of the textile printing and dyeing wastewater, is very limited. In this study, the occurrence of six categories of halogenated byproducts (haloacetic acids (HAAs), haloacetonitriles (HANs), N-nitrosamines (NAs), trihalomethanes, halogenated ketones, and halonitromethanes) was investigated along the full-scale treatment processes of textile printing and dyeing wastewater treatment plants. Furthermore, the ecological risk of the halogenated byproducts was evaluated. The results showed that the total concentration of halogenated byproducts increased significantly after chlorination. Large amounts of HAAs (average 122.1 μg/L), HANs (average 80.9 μg/L), THMs (average 48.3 μg/L), and NAs (average 2314.3 ng/L) were found in the chlorinated textile wastewater, and the results showed that the generations of HANs and NAs were positively correlated with the BIX and β/α index, indicating that the HANs and NAs might form from the microbial metabolites. In addition, HAAs and HANs exhibited high ecological risk quotients (>1), suggesting their high potential ecological risk. The results also demonstrated that most halogenated byproducts could be effectively removed by reverse osmosis treatment processes except NAs, with a lower removal rate of 18%. This study is believed to provide an important theoretical basis for controlling and reducing the ecological risks of halogenated byproducts in textile printing and dyeing wastewater effluents.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325711","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

River Damming Impacts on Carbon Emissions Should Be Revisited in the Context of the Aquatic Continuum Concept 应在水生连续体概念的背景下重新审视河坝对碳排放的影响

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-25 DOI: 10.1021/acs.est.4c09286

Xingcheng Yan, Yuchen Chen, Hao Sun, Qiuwen Chen, Jianyun Zhang, Wei Zhi

{"title":"River Damming Impacts on Carbon Emissions Should Be Revisited in the Context of the Aquatic Continuum Concept","authors":"Xingcheng Yan, Yuchen Chen, Hao Sun, Qiuwen Chen, Jianyun Zhang, Wei Zhi","doi":"10.1021/acs.est.4c09286","DOIUrl":"https://doi.org/10.1021/acs.est.4c09286","url":null,"abstract":"Figure 1. A conceptual schematic illustrating the effects of river damming on downstream hydrological and nutrient regimes, and how these changes further impact carbon cycling processes in downstream aquatic ecosystems, including rivers, connected lakes, and estuarine ecosystems. Before-D and After-D denote conditions before and after river damming. Dr. Xingcheng Yan earned his PhD in Geosciences, Natural Resources, and Environment from Sorbonne University, Paris, in 2022. He currently serves as a senior engineer in the Eco-Environmental Research Department at the Nanjing Hydraulic Research Institute. He leads the Young Scientist Project under the National Key Research and Development Program, as well as the Young Foundation Project of the National Natural Science Foundation of China. His research primarily focuses on the eco-environmental impacts of river damming, with particular attention to the biogeochemical cycling of carbon, nitrogen, phosphorus, and silicon. Dr. Qiuwen Chen is currently the head of Eco-Environmental Research Department of Nanjing Hydraulic Research Institute (NHRI). He received Ph.D. degree from Delft University of Technology in 2004. Then, he worked in RCEES Chinese Academy of Science from 2004 to 2013, and joined NHRI in 2014. He has been long engaged in Eco-environmental conservation for hydraulic engineering and hydropower development. He has published more than 400 international peer-reviewed papers. He was awarded the 20th Arthur Thomas Ippen Award from the International Association for Hydro-Environment Engineering (IAHR) and the Xplore Prize. He is now the chairman of Global Water Security of IHAR, and an associate editor of 2 international journals. This work was supported by the National Key R&D Program of China (2023YFC3210000), the National Natural Science Foundation of China (52121006, 52309097). This article references 8 other publications. 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":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142317211","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

Reactivity, Pathways, and Iodinated Disinfection Byproduct Formation during Chlorination of Iodotyrosines Derived from Edible Seaweed 食用海藻中提取的碘酪氨酸氯化过程中的反应性、途径和碘化消毒副产物的形成

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-25 DOI: 10.1021/acs.est.4c03542

Shunke Ding, Zhenqi Du, Ruixin Qu, Menglin Wu, Rong Xiao, Pin Wang, Xiaoyan Chen, Wenhai Chu

{"title":"Reactivity, Pathways, and Iodinated Disinfection Byproduct Formation during Chlorination of Iodotyrosines Derived from Edible Seaweed","authors":"Shunke Ding, Zhenqi Du, Ruixin Qu, Menglin Wu, Rong Xiao, Pin Wang, Xiaoyan Chen, Wenhai Chu","doi":"10.1021/acs.est.4c03542","DOIUrl":"https://doi.org/10.1021/acs.est.4c03542","url":null,"abstract":"Iodine derived from edible seaweed significantly enhances the formation of iodinated disinfection byproducts (I-DBPs) during household cooking. Reactions of chlorine with monoiodotyrosine (MIT) and diiodotyrosine (DIT) derived from seaweed were investigated. Species-specific second-order rate constants (25 °C) for the reaction of hypochlorous acid with neutral and anionic MIT were calculated to be 23.87 ± 5.01 and 634.65 ± 75.70 M–1 s–1, respectively, while the corresponding rate constants for that with neutral and anionic DIT were determined to be 12.51 ± 19.67 and 199.12 ± 8.64 M–1 s–1, respectively. Increasing temperature facilitated the reaction of chlorine with MIT and DIT. Based on the identification of 59 transformation products/DBPs from iodotyrosines by HPLC/Q-Orbitrap HRMS, three dominant reaction pathways were proposed. Thermodynamic results of computational modeling using density functional theory revealed that halogen exchange reaction follows a stepwise addition–elimination pathway. Among these DBPs, 3,5-diiodo-4-hydroxy-benzaldehyde and 3,5-diiodo-4-hydroxy-benzacetonitrle exhibited high toxic risk. During chlorination of MIT and DIT, iodinated trihalomethanes and haloacetic acids became dominant species at common cooking temperature (80 °C). These results provide insight into the mechanisms of halogen exchange reaction and imply important implications for the toxic risk associated with the exposure of I-DBPs from household cooking with iodine-containing food.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321634","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

Enhanced Extracellular Electron Transfer in Magnetite-Mediated Anaerobic Oxidation of Methane Coupled to Humic Substances Reduction: The Pivotal Role of Membrane-Bound Electron Transfer Proteins 磁铁矿介导的甲烷厌氧氧化与腐殖质还原过程中的细胞外电子传递增强：膜结合电子传递蛋白的关键作用

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-25 DOI: 10.1021/acs.est.4c05543

Lianfu Liang, Zhen Jin, Yang Tao, Yang Li, Zhiqiang Zhao, Yaobin Zhang

{"title":"Enhanced Extracellular Electron Transfer in Magnetite-Mediated Anaerobic Oxidation of Methane Coupled to Humic Substances Reduction: The Pivotal Role of Membrane-Bound Electron Transfer Proteins","authors":"Lianfu Liang, Zhen Jin, Yang Tao, Yang Li, Zhiqiang Zhao, Yaobin Zhang","doi":"10.1021/acs.est.4c05543","DOIUrl":"https://doi.org/10.1021/acs.est.4c05543","url":null,"abstract":"Humic substances are organic substances prevalent in various natural environments, such as wetlands, which are globally important sources of methane (CH4) emissions. Extracellular electron transfer (EET)-mediated anaerobic oxidation of methane (AOM)-coupled with humic substances reduction plays an important role in the reduction of methane emissions from wetlands, where magnetite is prevalent. However, little is known about the magnetite-mediated EET mechanisms in AOM-coupled humic substances reduction. This study shows that magnetite promotes the reduction of the AOM-coupled humic substances model compound, anthraquinone-2,6-disulfonate (AQDS). 13CH4 labeling experiments further indicated that AOM-coupled AQDS reduction occurred, and acetate was an intermediate product of AOM. Moreover, 13CH313COONa labeling experiments showed that AOM-generated acetate can be continuously reduced to methane in a state of dynamic equilibrium. In the presence of magnetite, the EET capacity of the microbial community increased, and Methanosarcina played a key role in the AOM-coupled AQDS reduction. Pure culture experiments showed that Methanosarcina barkeri can independently perform AOM-coupled AQDS reduction and that magnetite increased its surface protein redox activity. The metatranscriptomic results indicated that magnetite increased the expression of membrane-bound proteins involved in energy metabolism and electron transfer in M. barkeri, thereby increasing the EET capacity. This phenomenon potentially elucidates the rationale as to why magnetite promoted AOM-coupled AQDS reduction.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321635","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

Wastewaters Coproduced with Shale Gas Drive Slight Regional Salinization of Groundwater 页岩气产生的废水导致区域性地下水轻微盐碱化

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-25 DOI: 10.1021/acs.est.4c03371

Samuel W. Shaheen, Tao Wen, Zhong Zheng, Lingzhou Xue, Jennifer Baka, Susan L. Brantley

{"title":"Wastewaters Coproduced with Shale Gas Drive Slight Regional Salinization of Groundwater","authors":"Samuel W. Shaheen, Tao Wen, Zhong Zheng, Lingzhou Xue, Jennifer Baka, Susan L. Brantley","doi":"10.1021/acs.est.4c03371","DOIUrl":"https://doi.org/10.1021/acs.est.4c03371","url":null,"abstract":"While unconventional oil and gas (UOG) development is changing the world economy, processes that are used during UOG development such as high-volume hydraulic fracturing (“fracking”) have been linked with water contamination. Water quality risks include leaks of gas and salty fluids (brines) that are coproduced at wellpads. Identifying the cause of contamination is difficult, however, because UOG wells are often colocated with other contaminant sources. We investigated the world’s largest shale gas play with publicly accessible groundwater data (Marcellus Shale in Pennsylvania, U.S.A. with ∼29,000 analyses) and discovered that concentrations of brine-associated barium ([Ba]) and strontium ([Sr]) show small regional increases within 1 km of UOG development. Higher concentrations in groundwaters are associated with greater proximity to and density of UOG wells. Concentration increases are even larger when considering associations with the locations of (i) spill-related violations and (ii) some wastewater impoundments. These statistically significant relationships persist even after correcting for other natural and anthropogenic sources of salts. The most likely explanation is that UOG development slightly increases salt concentrations in regional groundwaters not because of fracking but because of the ubiquity of wastewater management issues. These results emphasize the need for stringent wastewater management practices across oil and gas operations.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142317169","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

First Insight into the Mobilization and Sequestration of Arsenic in a Karstic Soil during Redox Changes 首次揭示氧化还原变化过程中岩溶土壤中砷的迁移和螯合作用

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-25 DOI: 10.1021/acs.est.4c02989

Jianxu Wang, Sabry M. Shaheen, Ann-Christin Swertz, Chengshuai Liu, Christopher W.N. Anderson, Scott Fendorf, Shan-Li Wang, Xinbin Feng, Jörg Rinklebe

{"title":"First Insight into the Mobilization and Sequestration of Arsenic in a Karstic Soil during Redox Changes","authors":"Jianxu Wang, Sabry M. Shaheen, Ann-Christin Swertz, Chengshuai Liu, Christopher W.N. Anderson, Scott Fendorf, Shan-Li Wang, Xinbin Feng, Jörg Rinklebe","doi":"10.1021/acs.est.4c02989","DOIUrl":"https://doi.org/10.1021/acs.est.4c02989","url":null,"abstract":"Karst terrains provide drinking water for about 25% of the people on our planet, particularly in the southwest of China. Pollutants such as arsenic (As) in the soil can infiltrate groundwater through sinkholes and bedrock fractures in karst terrains. Despite this, the underlying mechanisms responsible for As release from karst soils under redox changes remain largely unexplored. Here, we used multiple synchrotron-based spectroscopic analyses to explore As mobilization and sequestration in As-polluted karstic soil under biogeochemical conditions that mimic field-validated redox conditions. We observed that As in the soil exists primarily as As(V), which is mainly associated with Fe(oxyhydr)oxides. The concentration of the dissolved As was high (294 μM) and As(III) was dominant (∼95%) at low Eh (≤−100 mV), indicating the high risk of As leaching under reducing conditions. This As mobilization was attributed to the fact that the dissolution of ferrihydrite and calcite promoted the release and reduction of associated As(V). The concentration of the dissolved As was low (17.0 μM) and As(V) was dominant (∼68%) at high Eh (≥+100 mV), which might be due to the oxidation and/or sequestration of As(III) by the recrystallized ferric phase. Our results showed that the combined effects of the reductive release of As(V) from both ferric and nonferric phases, along with the recrystallization of the ferric phase, govern the redox-induced mobilization and potential leaching of As in soils within karst environments.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142317303","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

How Does Triclocarban Affect Sulfur Transformation in Anaerobic Systems? 三氯卡班如何影响厌氧系统中的硫转化？

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-25 DOI: 10.1021/acs.est.4c07825

Qizi Fu, Xuemei Li, Yunhao Xu, Xingyu Ma, Yan Wang, Sha Long, Xuran Liu, Dongbo Wang

{"title":"How Does Triclocarban Affect Sulfur Transformation in Anaerobic Systems?","authors":"Qizi Fu, Xuemei Li, Yunhao Xu, Xingyu Ma, Yan Wang, Sha Long, Xuran Liu, Dongbo Wang","doi":"10.1021/acs.est.4c07825","DOIUrl":"https://doi.org/10.1021/acs.est.4c07825","url":null,"abstract":"Triclocarban (TCC), as a typical antimicrobial agent, accumulates at substantial levels in natural environments and engineered systems. This work investigated the impact of TCC on anaerobic sulfur transformation, especially toxic H2S production. Experimental findings revealed that TCC facilitated sulfur flow from the sludge solid phase to liquid phase, promoted sulfate reduction and sulfur-containing amino acid degradation, and largely improved anaerobic H2S production, i.e., 50–600 mg/kg total suspended solids (TSS) TCC increased the cumulative H2S yields by 24.76–478.12%. Although TCC can be partially biodegraded in anaerobic systems, the increase in H2S production can be mainly attributed to the effect of TCC rather than its degradation products. TCC was spontaneously adsorbed by protein-like substances contained in microbe extracellular polymers (EPSs), and the adsorbed TCC increased the direct electron transfer ability of EPSs, possibly due to the increase in the content of electroactive polymer protein in EPSs, the polarization of the amide group C═O bond, and the increase of the α-helical peptide dipole moment, which might be one important reason for promoting sulfur bioconversion processes. Microbial analysis showed that the presence of TCC enriched the organic substrate-degrading bacteria and sulfate-reducing bacteria and increased the abundances of functional genes encoding sulfate transport and dissimilatory sulfate reduction.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321636","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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