Shihao Zhu,Junhui Wang,Junfeng Li,Yuquan Li,Zhiguo Wen,Hengchao Sun,Yong Liu,Zeqiu Chen,Likun Pan
Faradaic capacitive deionization (Faradaic CDI) is a promising technology for tackling the global water crisis through efficient desalination. However, its practical implementation has been hindered by inherent challenges, such as sluggish reaction kinetics and limited mass transfer, especially under low-salinity conditions. To address these issues, this study proposes an induced-charge Faradaic CDI (IC-Faradaic CDI) system. The key innovation lies in the strategic integration of Faradaic CDI with an electric double-layer mechanism through a wireless induced-charge IC unit. This design modulates the electric field and ion transport, optimizes the concentration distribution, and establishes a universal pathway to reconcile the trade-off between kinetics and capacity. As a result, the IC-Faradaic CDI system delivers a desalination capacity of 0.269 mg cm–2 and an outstanding average desalination rate of 0.027 mg cm–2 min–1, surpassing most existing Faradaic CDI systems. Furthermore, to validate its real-world applicability, a larger-scale system (324 cm2) was constructed, achieving 77% salt removal from simulated brackish water and the effective desalination of real brackish water from the Yangtze River estuary. This work provides a novel and universal strategy to alleviate the kinetic limitations of Faradaic CDI and offers a low-cost, membrane-free, and energy-efficient solution for high-performance water treatment.
{"title":"Induced-Charge Assisted Faradaic Capacitive Deionization: A New Paradigm to Break the Capacity-Rate Trade-off","authors":"Shihao Zhu,Junhui Wang,Junfeng Li,Yuquan Li,Zhiguo Wen,Hengchao Sun,Yong Liu,Zeqiu Chen,Likun Pan","doi":"10.1021/acs.est.5c16428","DOIUrl":"https://doi.org/10.1021/acs.est.5c16428","url":null,"abstract":"Faradaic capacitive deionization (Faradaic CDI) is a promising technology for tackling the global water crisis through efficient desalination. However, its practical implementation has been hindered by inherent challenges, such as sluggish reaction kinetics and limited mass transfer, especially under low-salinity conditions. To address these issues, this study proposes an induced-charge Faradaic CDI (IC-Faradaic CDI) system. The key innovation lies in the strategic integration of Faradaic CDI with an electric double-layer mechanism through a wireless induced-charge IC unit. This design modulates the electric field and ion transport, optimizes the concentration distribution, and establishes a universal pathway to reconcile the trade-off between kinetics and capacity. As a result, the IC-Faradaic CDI system delivers a desalination capacity of 0.269 mg cm–2 and an outstanding average desalination rate of 0.027 mg cm–2 min–1, surpassing most existing Faradaic CDI systems. Furthermore, to validate its real-world applicability, a larger-scale system (324 cm2) was constructed, achieving 77% salt removal from simulated brackish water and the effective desalination of real brackish water from the Yangtze River estuary. This work provides a novel and universal strategy to alleviate the kinetic limitations of Faradaic CDI and offers a low-cost, membrane-free, and energy-efficient solution for high-performance water treatment.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"57 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111179","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}
Yu Wang, Qiongqiong Yang, Jiaxin Chen, Qi Chen, Nengwang Chen, Chen He, Quan Shi, Ta-Hui Lin, Yu Cong, Nianzhi Jiao, Alexandra Z Worden, Qiang Zheng
Subtropical coastal bays significantly mediate land-ocean carbon fluxes, yet their responses to concurrent warming and intensified river discharge remain unclear. Using monthly observations over a decade in Xiamen Bay and integrating flow cytometry, high-throughput sequencing, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), and NanoSIMS carbon tracing, we explored how microbially driven carbon cycling responds to these dual forces. Our findings reveal that under present-day conditions, a +4 °C warming would increase the abundances of Synechococcus (∼19%) and microeukaryotic algae (∼5%), suggesting an enhanced potential for labile dissolved organic matter (LDOM) production. NanoSIMS experiments showed a 5-fold increase in heterotrophic bacterial assimilation of phytoplankton-derived carbon at elevated temperatures (30 °C versus 22 °C). Concurrently, intensified riverine discharge delivered terrestrial recalcitrant DOM (RDOM), altering DOM molecular composition and decreasing overall bioavailability. These combined stressors restructured microbial communities, accelerating heterotrophic carbon processing and reducing the ratio of ecologically persistent DOM to recalcitrant dissolved black carbon. We propose a Dual-DOM Forcing framework that formalizes how thermal (autochthonous LDOM) and hydrological (allochthonous RDOM) drivers jointly regulate microbial carbon processing, DOM persistence, and coastal carbon sequestration potential. This framework provides a transferable basis for assessing the vulnerability of coastal blue carbon sinks to concurrent warming and altered river discharge.
{"title":"Warming and River Discharge Accelerate Coastal Heterotrophy and Increase Dissolved Organic Matter Recalcitrance.","authors":"Yu Wang, Qiongqiong Yang, Jiaxin Chen, Qi Chen, Nengwang Chen, Chen He, Quan Shi, Ta-Hui Lin, Yu Cong, Nianzhi Jiao, Alexandra Z Worden, Qiang Zheng","doi":"10.1021/acs.est.5c17340","DOIUrl":"https://doi.org/10.1021/acs.est.5c17340","url":null,"abstract":"<p><p>Subtropical coastal bays significantly mediate land-ocean carbon fluxes, yet their responses to concurrent warming and intensified river discharge remain unclear. Using monthly observations over a decade in Xiamen Bay and integrating flow cytometry, high-throughput sequencing, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), and NanoSIMS carbon tracing, we explored how microbially driven carbon cycling responds to these dual forces. Our findings reveal that under present-day conditions, a +4 °C warming would increase the abundances of <i>Synechococcus</i> (∼19%) and microeukaryotic algae (∼5%), suggesting an enhanced potential for labile dissolved organic matter (LDOM) production. NanoSIMS experiments showed a 5-fold increase in heterotrophic bacterial assimilation of phytoplankton-derived carbon at elevated temperatures (30 °C versus 22 °C). Concurrently, intensified riverine discharge delivered terrestrial recalcitrant DOM (RDOM), altering DOM molecular composition and decreasing overall bioavailability. These combined stressors restructured microbial communities, accelerating heterotrophic carbon processing and reducing the ratio of ecologically persistent DOM to recalcitrant dissolved black carbon. We propose a Dual-DOM Forcing framework that formalizes how thermal (autochthonous LDOM) and hydrological (allochthonous RDOM) drivers jointly regulate microbial carbon processing, DOM persistence, and coastal carbon sequestration potential. This framework provides a transferable basis for assessing the vulnerability of coastal blue carbon sinks to concurrent warming and altered river discharge.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":11.3,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146117121","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}
Kai Zhang,Qianyi Wang,Bo Fu,Runmei Ma,Xiangtao Zhang,Le Zhang,Tiantian Li,Bin Wang
{"title":"Toward an AI Foundation Model Integrating Climate Change, Air Pollution, Socioeconomics, and Human Health","authors":"Kai Zhang,Qianyi Wang,Bo Fu,Runmei Ma,Xiangtao Zhang,Le Zhang,Tiantian Li,Bin Wang","doi":"10.1021/acs.est.5c16891","DOIUrl":"https://doi.org/10.1021/acs.est.5c16891","url":null,"abstract":"","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"31 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111176","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}
Jiwon Park,Eunhye Bae,Hee-Jin Park,Yeonjeong Ha,Beate I. Escher,Jung-Hwan Kwon
Water-soluble polymers (WSPs) represent a key class of polymers widely employed in liquid formulations across diverse industries. We investigated their interactions with synthetic lipid membranes, as well as cytotoxicity triggered by membrane disruption. Zwitterionic 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC) and negatively charged 1,2-dioleoyl-sn-glycero-3-phosphoglycerol (DOPG) liposomes were utilized as lipid membrane models for assessing fluorescence leakage caused by two positively charged, two negatively charged, and one neutral WSPs. Positively charged WSPs induced substantial leakage in DOPG liposomes with increasing polymer concentrations, whereas the negatively charged WSP caused only minor leakage in DOPC liposomes at high concentrations, and nonionic WSPs did not cause significant disruption. Quantification of in vitro cytotoxicity on one human (MCF7) and one fish (RTgill-W1 from Oncorhynchus mykiss) cell line confirmed the WSP’s ability to disrupt membrane integrity. Cationic WSPs also caused cytotoxicity in both cell lines at similar concentrations, distinguishing them from negatively charged and neutral WSPs. These findings highlight the pivotal role of electrostatic interactions between charge characteristics of WSPs and phospholipid headgroups of biological membranes. Although WSPs are often exempted for toxicity tests in chemicals regulations such as the European Union’s REACH, further evaluation is necessary to understand their toxic potential and modes of toxic action.
{"title":"Disruption of Lipid Membrane Integrity by Synthetic Water-Soluble Polymers: Effects of Lipid Headgroup","authors":"Jiwon Park,Eunhye Bae,Hee-Jin Park,Yeonjeong Ha,Beate I. Escher,Jung-Hwan Kwon","doi":"10.1021/acs.est.5c15107","DOIUrl":"https://doi.org/10.1021/acs.est.5c15107","url":null,"abstract":"Water-soluble polymers (WSPs) represent a key class of polymers widely employed in liquid formulations across diverse industries. We investigated their interactions with synthetic lipid membranes, as well as cytotoxicity triggered by membrane disruption. Zwitterionic 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC) and negatively charged 1,2-dioleoyl-sn-glycero-3-phosphoglycerol (DOPG) liposomes were utilized as lipid membrane models for assessing fluorescence leakage caused by two positively charged, two negatively charged, and one neutral WSPs. Positively charged WSPs induced substantial leakage in DOPG liposomes with increasing polymer concentrations, whereas the negatively charged WSP caused only minor leakage in DOPC liposomes at high concentrations, and nonionic WSPs did not cause significant disruption. Quantification of in vitro cytotoxicity on one human (MCF7) and one fish (RTgill-W1 from Oncorhynchus mykiss) cell line confirmed the WSP’s ability to disrupt membrane integrity. Cationic WSPs also caused cytotoxicity in both cell lines at similar concentrations, distinguishing them from negatively charged and neutral WSPs. These findings highlight the pivotal role of electrostatic interactions between charge characteristics of WSPs and phospholipid headgroups of biological membranes. Although WSPs are often exempted for toxicity tests in chemicals regulations such as the European Union’s REACH, further evaluation is necessary to understand their toxic potential and modes of toxic action.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"105 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111178","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}
Sergio Ibarra-Espinosa,Edmilson Dias de Freitas,Benjamin Gaubert,Pablo Lichtig,Karl Ropkins,Iara da Silva,Guilherme Martins Pereira,Daniel Schuch,Janaina Nascimento,Leonardo Hoinaski,Leila Droprinchinski Martins,Mario Gavidia-Calderón,Angel Vara-Vela,Taciana Toledo de Almeida Albuquerque,Rita Yuri Ynoue,Sebastian Diez,Zamir Mera,Alejandro Casallas,Fidel Vallejo,Valeria Diaz,Rizzieri Pedruzzi,Rosana Abrutzky,Marco A. Franco,Nicolas Huneeus,Hector Jorquera,Luis Carlos Belalcázar-Cerón,Néstor Y. Rojas,Maria de Fatima Andrade,Louisa Emmons,Guy Brasseur
Global emission inventories often fail to capture the complexities of vehicular pollution in regions with unique fuel mixes, such as Brazil’s extensive biofuel use, leading to significant uncertainties in atmospheric modeling. This study presents a century-long (1960–2100) bottom-up vehicular emission inventory for Brazil, leveraging locally derived emission factors. Our estimates reveal substantial discrepancies in magnitude, timing, and speciation of non-CO2 pollutants (CO, NMHC, PM2.5) compared to leading global inventories (EDGAR, CEDS, CAMS), highlighting critical inaccuracies in widely used data sets. More critically, future projections under Shared Socioeconomic Pathways (SSPs) uncover a novel positive feedback mechanism: rising temperatures significantly enhance vehicular evaporative nonmethane hydrocarbon (NMHC) emissions. This temperature-dependent increase and subsequent NMHC oxidation to CO2 suggest an overlooked pathway that could amplify climate warming and air pollution globally, particularly after a breakpoint around 2050 (p < 0.05). While historical emissions peaked in the 1990s–2000s, nonexhaust PM becomes increasingly important. Air quality simulations using our inventory in the MUSICA model show good regional PM2.5 agreement but highlight challenges in resolving local primary pollutant peaks. This comprehensive inventory provides crucial data for Brazil and uncovers globally relevant climate–chemistry interactions, urging a re-evaluation of regional specificities in global emission assessments.
{"title":"A Century of Vehicular Emissions in Brazil: Unveiling the Impacts of Unique Fuel Mix on Air Quality","authors":"Sergio Ibarra-Espinosa,Edmilson Dias de Freitas,Benjamin Gaubert,Pablo Lichtig,Karl Ropkins,Iara da Silva,Guilherme Martins Pereira,Daniel Schuch,Janaina Nascimento,Leonardo Hoinaski,Leila Droprinchinski Martins,Mario Gavidia-Calderón,Angel Vara-Vela,Taciana Toledo de Almeida Albuquerque,Rita Yuri Ynoue,Sebastian Diez,Zamir Mera,Alejandro Casallas,Fidel Vallejo,Valeria Diaz,Rizzieri Pedruzzi,Rosana Abrutzky,Marco A. Franco,Nicolas Huneeus,Hector Jorquera,Luis Carlos Belalcázar-Cerón,Néstor Y. Rojas,Maria de Fatima Andrade,Louisa Emmons,Guy Brasseur","doi":"10.1021/acs.est.5c08400","DOIUrl":"https://doi.org/10.1021/acs.est.5c08400","url":null,"abstract":"Global emission inventories often fail to capture the complexities of vehicular pollution in regions with unique fuel mixes, such as Brazil’s extensive biofuel use, leading to significant uncertainties in atmospheric modeling. This study presents a century-long (1960–2100) bottom-up vehicular emission inventory for Brazil, leveraging locally derived emission factors. Our estimates reveal substantial discrepancies in magnitude, timing, and speciation of non-CO2 pollutants (CO, NMHC, PM2.5) compared to leading global inventories (EDGAR, CEDS, CAMS), highlighting critical inaccuracies in widely used data sets. More critically, future projections under Shared Socioeconomic Pathways (SSPs) uncover a novel positive feedback mechanism: rising temperatures significantly enhance vehicular evaporative nonmethane hydrocarbon (NMHC) emissions. This temperature-dependent increase and subsequent NMHC oxidation to CO2 suggest an overlooked pathway that could amplify climate warming and air pollution globally, particularly after a breakpoint around 2050 (p < 0.05). While historical emissions peaked in the 1990s–2000s, nonexhaust PM becomes increasingly important. Air quality simulations using our inventory in the MUSICA model show good regional PM2.5 agreement but highlight challenges in resolving local primary pollutant peaks. This comprehensive inventory provides crucial data for Brazil and uncovers globally relevant climate–chemistry interactions, urging a re-evaluation of regional specificities in global emission assessments.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"41 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111204","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}
Yang Chen, Shirui Yan, Yaliang Hou, Yongxiang Lin, Kexin Liu, Dingfan Cao, Yuxuan Xing, Daizhou Zhang, Wei Pu, Xin Wang
Black carbon in seasonal snow (BCS) critically influences the Earth system by reducing surface albedo (snow darkening), perturbing radiative balance, and accelerating snowmelt. However, its climatic and hydrological impacts remain poorly quantified because high-quality data sets are scarce. This study introduces a novel Dual Random Forest (DRF) framework that synergistically constrains BCS concentration estimates through both physical mechanisms and observational fidelity. By pretraining with six spatiotemporally complete Earth System Model (ESM) simulations, driven by multisource reanalysis data, and fine-tuning against global field observations, the DRF generates a 44-year (1981-2024) global monthly BCS data set at 0.5° × 0.625° resolution. This data set achieves higher accuracy in BCS patterns and concentrations compared with observations (spatial correlation R = 0.92; normalized mean error NME = 31%), outperforming both single-constrained machine learning approaches (ESM- or observation-only) and traditional methods (CMIP5, CMIP6, and MODIS; R = 0.07-0.82, NME = 51%-1951%). It also excels in capturing seasonal variations and long-term annual trends, better reproducing increasing trends driven by anthropogenic forcing and decadal variability modulated by natural climate variability. This data set is hence valuable for robust quantification of BCS-induced radiative forcing and attribution of snowmelt acceleration to snow darkening versus climate warming on a global scale.
季节性雪(BCS)中的黑碳通过降低地表反照率(雪变暗)、扰乱辐射平衡和加速融雪对地球系统产生重大影响。然而,由于缺乏高质量的数据集,其气候和水文影响的量化仍然很差。本研究引入了一种新的双随机森林(Dual Random Forest, DRF)框架,该框架通过物理机制和观测保真度协同约束BCS浓度估计。DRF利用6个时空完整的地球系统模型(ESM)模拟进行预训练,在多源再分析数据的驱动下,对全球野外观测数据进行微调,生成了一个44年(1981-2024年)的0.5°× 0.625°分辨率的全球月度BCS数据集。与观测数据相比,该数据集在BCS模式和浓度方面具有更高的精度(空间相关R = 0.92,归一化平均误差NME = 31%),优于单约束机器学习方法(ESM或仅观测)和传统方法(CMIP5, CMIP6和MODIS; R = 0.07-0.82, NME = 51%-1951%)。它还擅长捕捉季节变化和长期年度趋势,更好地再现由人为强迫驱动的增加趋势和由自然气候变率调节的年代际变率。因此,该数据集对于bcs引起的辐射强迫的可靠量化以及全球范围内融雪加速归因于雪变暗与气候变暖的关系具有重要价值。
{"title":"Global Quantification of Black Carbon in Seasonal Snow: A Physically and Observationally Constrained Machine-Learning Framework.","authors":"Yang Chen, Shirui Yan, Yaliang Hou, Yongxiang Lin, Kexin Liu, Dingfan Cao, Yuxuan Xing, Daizhou Zhang, Wei Pu, Xin Wang","doi":"10.1021/acs.est.5c09936","DOIUrl":"https://doi.org/10.1021/acs.est.5c09936","url":null,"abstract":"<p><p>Black carbon in seasonal snow (BCS) critically influences the Earth system by reducing surface albedo (snow darkening), perturbing radiative balance, and accelerating snowmelt. However, its climatic and hydrological impacts remain poorly quantified because high-quality data sets are scarce. This study introduces a novel Dual Random Forest (DRF) framework that synergistically constrains BCS concentration estimates through both physical mechanisms and observational fidelity. By pretraining with six spatiotemporally complete Earth System Model (ESM) simulations, driven by multisource reanalysis data, and fine-tuning against global field observations, the DRF generates a 44-year (1981-2024) global monthly BCS data set at 0.5° × 0.625° resolution. This data set achieves higher accuracy in BCS patterns and concentrations compared with observations (spatial correlation <i>R</i> = 0.92; normalized mean error NME = 31%), outperforming both single-constrained machine learning approaches (ESM- or observation-only) and traditional methods (CMIP5, CMIP6, and MODIS; <i>R</i> = 0.07-0.82, NME = 51%-1951%). It also excels in capturing seasonal variations and long-term annual trends, better reproducing increasing trends driven by anthropogenic forcing and decadal variability modulated by natural climate variability. This data set is hence valuable for robust quantification of BCS-induced radiative forcing and attribution of snowmelt acceleration to snow darkening versus climate warming on a global scale.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":11.3,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146117106","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}
Introducing environmentally benign Zn single-atom catalysts (SACs) in Fenton-like reactions to induce electron transfer processes (ETP) holds great potential in advanced water remediation technologies. However, precise coordination of Zn SACs is highly required to selectively trigger the ETP pathway. Herein, under the guidance of density functional theory (DFT) predictions, we constructed asymmetric Zn–N3Cl sites on N-doped carbon (NC) to unlock the electron-transfer reactivity of redox-inert Zn while maintaining structural robustness. Compared with the symmetric Zn–N4 system, the Zn–N3Cl system achieved a higher sulfamethoxazole (SMX) removal rate and PMS utilization efficiency by 4.4 and 2.3 times, respectively. Mechanism studies revealed that Cl doping significantly altered the electronic structure of Zn sites, thereby promoting their electron transfer capacity. The strongly polarized Zn–N3Cl sites exhibited a notably enhanced interaction with PMS, facilitating the formation of Zn–N3Cl/PMS* with high redox potential and lowering the energy barrier of the rate-determining step (RDS) for ETP. The Zn–N3Cl system demonstrated outstanding catalytic reactivity toward various environmental interferences over a wide pH range. Notably, this system remained effective for the continuous flow-through treatment of pharmaceutical wastewater, coupling high catalytic reactivity and structural robustness. Our rational design of environmentally benign materials offers a blueprint for sustainable water remediation.
{"title":"Tailoring the Interfacial Microenvironment of Atomically Dispersed Zinc to Boost Electron Transfer Process for Water Purification","authors":"Zhiyuan Huang,Qi Hao,Songru Xie,Chaoyi Huang,Li Jin,Rui Li,Linxuan Xie,Qi Tang,Jiang Xu,Kai Liu","doi":"10.1021/acs.est.5c18038","DOIUrl":"https://doi.org/10.1021/acs.est.5c18038","url":null,"abstract":"Introducing environmentally benign Zn single-atom catalysts (SACs) in Fenton-like reactions to induce electron transfer processes (ETP) holds great potential in advanced water remediation technologies. However, precise coordination of Zn SACs is highly required to selectively trigger the ETP pathway. Herein, under the guidance of density functional theory (DFT) predictions, we constructed asymmetric Zn–N3Cl sites on N-doped carbon (NC) to unlock the electron-transfer reactivity of redox-inert Zn while maintaining structural robustness. Compared with the symmetric Zn–N4 system, the Zn–N3Cl system achieved a higher sulfamethoxazole (SMX) removal rate and PMS utilization efficiency by 4.4 and 2.3 times, respectively. Mechanism studies revealed that Cl doping significantly altered the electronic structure of Zn sites, thereby promoting their electron transfer capacity. The strongly polarized Zn–N3Cl sites exhibited a notably enhanced interaction with PMS, facilitating the formation of Zn–N3Cl/PMS* with high redox potential and lowering the energy barrier of the rate-determining step (RDS) for ETP. The Zn–N3Cl system demonstrated outstanding catalytic reactivity toward various environmental interferences over a wide pH range. Notably, this system remained effective for the continuous flow-through treatment of pharmaceutical wastewater, coupling high catalytic reactivity and structural robustness. Our rational design of environmentally benign materials offers a blueprint for sustainable water remediation.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"41 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111175","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}
Sustainable generation of ferrous iron (Fe(II)) through engineered zero-valent iron (ZVI, Fe(0)) offers an innovative strategy for efficient pollutant reduction. This study presents a wet ball milling-surface engineering strategy for synthesizing low-molecular-weight organic acid (LMWOA)-modified ZVI, which enables a novel dual redox activation mechanism for Fe(II)─a functionality that cannot be achieved by conventional wet ball milling or external LMWOA addition. X-ray absorption fine structure spectroscopy and density functional theory calculations demonstrate that α-hydroxy carboxylic acids (e.g., citric, tartaric, and malic acids) form five-membered chelate rings via hydrogen bonding, thereby significantly enhancing electron transfer kinetics from Fe(0) to Fe(II). Meanwhile, non-α-hydroxy carboxylic acids (e.g., succinic/acetic/formic acids) promote Fe(III) adsorption–reduction cycles, thus sustaining Fe(II) regeneration. Notably, ZVI modified with oxalic acid or ascorbic acid exhibited a synergistic effect of both pathways, resulting in the highest Cr(VI) removal capacities, with 19.7- and 22.6-fold increases in Cr(VI) removal and Fe(III) recovery rates of 81.7% and 108.9% relative to unmodified ZVI, respectively. This enhanced performance can be attributed to the improved dissolution of Fe(II) and the elevated levels of structurally bound Fe(II), which collectively promote sustained electron generation and effective transfer to Cr(VI). These findings indicate that LMWOA-modified ZVI establishes a tunable Fe(II) activation system, thereby positioning LMWOA as a promising strategic platform for groundwater remediation.
{"title":"Dual Activation of Ferrous Iron via Surface Engineering of Zero-Valent Iron with Low-Molecular-Weight Organic Acids","authors":"Linbo Qian,Zhenyu Kang,Hangyu Li,Zhen Ni,Hongtao Sheng,Yuqing Wang,Xiaoqi Long,Mengfang Chen,Baoliang Chen","doi":"10.1021/acs.est.5c14314","DOIUrl":"https://doi.org/10.1021/acs.est.5c14314","url":null,"abstract":"Sustainable generation of ferrous iron (Fe(II)) through engineered zero-valent iron (ZVI, Fe(0)) offers an innovative strategy for efficient pollutant reduction. This study presents a wet ball milling-surface engineering strategy for synthesizing low-molecular-weight organic acid (LMWOA)-modified ZVI, which enables a novel dual redox activation mechanism for Fe(II)─a functionality that cannot be achieved by conventional wet ball milling or external LMWOA addition. X-ray absorption fine structure spectroscopy and density functional theory calculations demonstrate that α-hydroxy carboxylic acids (e.g., citric, tartaric, and malic acids) form five-membered chelate rings via hydrogen bonding, thereby significantly enhancing electron transfer kinetics from Fe(0) to Fe(II). Meanwhile, non-α-hydroxy carboxylic acids (e.g., succinic/acetic/formic acids) promote Fe(III) adsorption–reduction cycles, thus sustaining Fe(II) regeneration. Notably, ZVI modified with oxalic acid or ascorbic acid exhibited a synergistic effect of both pathways, resulting in the highest Cr(VI) removal capacities, with 19.7- and 22.6-fold increases in Cr(VI) removal and Fe(III) recovery rates of 81.7% and 108.9% relative to unmodified ZVI, respectively. This enhanced performance can be attributed to the improved dissolution of Fe(II) and the elevated levels of structurally bound Fe(II), which collectively promote sustained electron generation and effective transfer to Cr(VI). These findings indicate that LMWOA-modified ZVI establishes a tunable Fe(II) activation system, thereby positioning LMWOA as a promising strategic platform for groundwater remediation.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"20 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111181","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}
Adam P Sibal, Rachel N Gaines, Bridget E Friel, Paul J A Kenis, Ashlynn S Stillwell
The U.S. biodiesel industry faces significant economic challenges, exacerbated by declining glycerol coproduct values and rising feedstock costs and leading to numerous plant closures. In this study, we investigate the technoeconomic and environmental viability of electrochemically upcycling low-value industrial-grade crude glycerol (50 wt % glycerol) and methanol-depleted crude glycerol (80 wt % glycerol) into formic acid, a valuable chemical commodity. Through process modeling, we assess purification processes and electrochemical oxidation pathways for these waste glycerol streams. Our findings indicate that utilizing low-value crude glycerol can produce formic acid at competitive costs, contingent upon advancements in catalyst efficiency and reactor design. Life cycle assessments reveal that this approach could reduce environmental impacts compared to traditional formic acid production, especially as the U.S. electricity grid decarbonizes through additional renewable energy deployment. State-level analyses highlight the influence of regional electricity prices, water costs, policies, and incentives on economic feasibility. By enabling the circular use of biodiesel-derived waste, this work supports more resilient renewable fuel systems and advances sustainable chemical manufacturing.
{"title":"Turning Waste into Value: Technoeconomic Analysis and Life Cycle Assessment of Biodiesel-Derived Crude Glycerol Electrooxidation.","authors":"Adam P Sibal, Rachel N Gaines, Bridget E Friel, Paul J A Kenis, Ashlynn S Stillwell","doi":"10.1021/acs.est.5c16857","DOIUrl":"https://doi.org/10.1021/acs.est.5c16857","url":null,"abstract":"<p><p>The U.S. biodiesel industry faces significant economic challenges, exacerbated by declining glycerol coproduct values and rising feedstock costs and leading to numerous plant closures. In this study, we investigate the technoeconomic and environmental viability of electrochemically upcycling low-value industrial-grade crude glycerol (50 wt % glycerol) and methanol-depleted crude glycerol (80 wt % glycerol) into formic acid, a valuable chemical commodity. Through process modeling, we assess purification processes and electrochemical oxidation pathways for these waste glycerol streams. Our findings indicate that utilizing low-value crude glycerol can produce formic acid at competitive costs, contingent upon advancements in catalyst efficiency and reactor design. Life cycle assessments reveal that this approach could reduce environmental impacts compared to traditional formic acid production, especially as the U.S. electricity grid decarbonizes through additional renewable energy deployment. State-level analyses highlight the influence of regional electricity prices, water costs, policies, and incentives on economic feasibility. By enabling the circular use of biodiesel-derived waste, this work supports more resilient renewable fuel systems and advances sustainable chemical manufacturing.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":11.3,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146117132","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}
Tingting Zhang, Zhou Qi, Yunfei Teng, Zhao Duan, Han Dai, Dong Cheng, Jie Han, Ming Liu
The neurotoxic effects of pesticide residues on nontarget organisms, particularly pregnant women and fetuses, represent a critical concern in environmental and health research. In this study, dimethomorph (DMM) was detected in human cord blood in normal pregnancies at term (without maternal-fetal complications). And neurotoxicity of the fungicide DMM through integrated single-cell RNA sequencing (scRNA-seq) and metabolomic profiling in pregnant mice brain tissue. Our results demonstrate that DMM exposure induces significant alterations in both the proportions and functions of multiple neural cell populations, including microglia, oligodendrocytes, astrocytes, and endothelial cells, accompanied by metabolic reprogramming and blood-brain barrier (BBB) dysfunction. Single-cell analysis revealed cell subtype-specific transcriptional changes and aberrant activation of metabolic pathways (e.g., PI3K-AKT-mTOR signaling), while metabolomic profiling further identified substantial disturbances in amino acid, lipid, and energy metabolism. Furthermore, cell–cell communication analysis indicated enhanced pathological signaling network interactions under DMM exposure. These findings not only elucidate the mechanisms underlying DMM-induced neurotoxicity but also highlight the potential risks of pesticide exposure during pregnancy to maternal and fetal health, providing critical insights for pesticide safety assessment and the development of neuroprotective strategies.
{"title":"Single-Cell Dissection of Dimethomorph-Induced Neurotoxicity in the Gestational Brain: Metabolic Disruption and Blood–Brain Barrier Dysfunction","authors":"Tingting Zhang, Zhou Qi, Yunfei Teng, Zhao Duan, Han Dai, Dong Cheng, Jie Han, Ming Liu","doi":"10.1021/acs.est.5c11595","DOIUrl":"https://doi.org/10.1021/acs.est.5c11595","url":null,"abstract":"The neurotoxic effects of pesticide residues on nontarget organisms, particularly pregnant women and fetuses, represent a critical concern in environmental and health research. In this study, dimethomorph (DMM) was detected in human cord blood in normal pregnancies at term (without maternal-fetal complications). And neurotoxicity of the fungicide DMM through integrated single-cell RNA sequencing (scRNA-seq) and metabolomic profiling in pregnant mice brain tissue. Our results demonstrate that DMM exposure induces significant alterations in both the proportions and functions of multiple neural cell populations, including microglia, oligodendrocytes, astrocytes, and endothelial cells, accompanied by metabolic reprogramming and blood-brain barrier (BBB) dysfunction. Single-cell analysis revealed cell subtype-specific transcriptional changes and aberrant activation of metabolic pathways (e.g., PI3K-AKT-mTOR signaling), while metabolomic profiling further identified substantial disturbances in amino acid, lipid, and energy metabolism. Furthermore, cell–cell communication analysis indicated enhanced pathological signaling network interactions under DMM exposure. These findings not only elucidate the mechanisms underlying DMM-induced neurotoxicity but also highlight the potential risks of pesticide exposure during pregnancy to maternal and fetal health, providing critical insights for pesticide safety assessment and the development of neuroprotective strategies.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"34 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146102003","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}