Liang Tang, Bin Lu, Honghong Chen, Haodong Cheng, Jason T. Magnuson, Xinyuan Kang, Shusheng Luo, Wenhui Qiu
Butylated hydroxytoluene (BHT), a widely used synthetic phenolic antioxidant, undergoes metabolic transformation in aquatic environments and organisms. However, the immunotoxic potential of its metabolites remains largely unexplored. Here, we combined density functional theory calculations, chemical analyses, and zebrafish bioassays to investigate the metabolism and immunotoxicity of BHT and its representative metabolites. Gas chromatography–mass spectrometry confirmed the presence of 3,5-ditert-butyl-4-hydroxybenzoic acid (BHT-COOH) and 2,6-ditert-butyl-p-benzoquinone (BHT-Q) in exposure water and larvae, whereas 2,6-ditert-butyl-4-hydroxymethylphenol (BHT-OH) was primarily detected in larvae. Exposure to environmentally relevant concentrations of BHT, BHT-COOH, and BHT-Q significantly increased macrophage and neutrophil numbers, weakened antibacterial resistance against Vibrio parahemolyticus, and induced oxidative stress with dysregulated immune markers and elevated tumor necrosis factor-α (TNF-α) levels. Comparative analyses showed that BHT-COOH and BHT-Q induced stronger immunotoxic responses than the parent compound, BHT. Additionally, high-throughput screening of the immune-related receptors using molecular docking identified the Interleukin-1β (IL-1β) signaling pathway as a critical mediator of these effects, as coexposure with an IL-1β inhibitor markedly attenuated immune disruption. Collectively, these findings demonstrate that BHT metabolites, especially BHT-COOH and BHT-Q, exhibit stronger immunotoxic responses than the parent compound, highlighting the importance of incorporating metabolite pathways into ecological risk assessments of synthetic phenolic antioxidants.
{"title":"Characterization of the Immunotoxic Effects and Underlying Mechanism of Butylated Hydroxytoluene and Its Metabolites to Early Life Stage Fish","authors":"Liang Tang, Bin Lu, Honghong Chen, Haodong Cheng, Jason T. Magnuson, Xinyuan Kang, Shusheng Luo, Wenhui Qiu","doi":"10.1021/acs.est.5c14000","DOIUrl":"https://doi.org/10.1021/acs.est.5c14000","url":null,"abstract":"Butylated hydroxytoluene (BHT), a widely used synthetic phenolic antioxidant, undergoes metabolic transformation in aquatic environments and organisms. However, the immunotoxic potential of its metabolites remains largely unexplored. Here, we combined density functional theory calculations, chemical analyses, and zebrafish bioassays to investigate the metabolism and immunotoxicity of BHT and its representative metabolites. Gas chromatography–mass spectrometry confirmed the presence of 3,5-di<i>tert</i>-butyl-4-hydroxybenzoic acid (BHT-COOH) and 2,6-di<i>tert</i>-butyl-p-benzoquinone (BHT-Q) in exposure water and larvae, whereas 2,6-di<i>tert</i>-butyl-4-hydroxymethylphenol (BHT-OH) was primarily detected in larvae. Exposure to environmentally relevant concentrations of BHT, BHT-COOH, and BHT-Q significantly increased macrophage and neutrophil numbers, weakened antibacterial resistance against <i>Vibrio parahemolyticus</i>, and induced oxidative stress with dysregulated immune markers and elevated tumor necrosis factor-α (TNF-α) levels. Comparative analyses showed that BHT-COOH and BHT-Q induced stronger immunotoxic responses than the parent compound, BHT. Additionally, high-throughput screening of the immune-related receptors using molecular docking identified the Interleukin-1β (IL-1β) signaling pathway as a critical mediator of these effects, as coexposure with an IL-1β inhibitor markedly attenuated immune disruption. Collectively, these findings demonstrate that BHT metabolites, especially BHT-COOH and BHT-Q, exhibit stronger immunotoxic responses than the parent compound, highlighting the importance of incorporating metabolite pathways into ecological risk assessments of synthetic phenolic antioxidants.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"7 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728911","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}
When communities are exposed to environmental chemicals, the federal government’s response relies on scientific evidence to prove that adverse health conditions were caused by the particular chemical exposure. However, the lack of robust exposure information and a minimal understanding of cumulative effects means critical information required to prove causation is rarely available. As a result, the government often fails to adequately protect public health. We propose a response model based on presumptive association that would allow government to act in the absence of community-specific data linking cause and effect after community-wide chemical exposures. In this model, when a community is exposed to a chemical of concern, agencies would review scientific information about the health effects of exposure to that chemical. If the evidence indicates the chemical could cause a certain health condition, then the government would take action to benefit community members who were exposed and who have that condition. They would not have to prove that their health condition was caused by exposure to the chemical of concern. Adopting a presumptive association model for federal responses to chemical exposures would create a clear, fair, standardized, and timely approach that protects public health.
{"title":"Need for a New Federal Approach for Responding to Chemical Exposure Caused by Community-Wide Contamination","authors":"Mihir Vohra, Stephen Lester","doi":"10.1021/acs.est.5c04498","DOIUrl":"https://doi.org/10.1021/acs.est.5c04498","url":null,"abstract":"When communities are exposed to environmental chemicals, the federal government’s response relies on scientific evidence to prove that adverse health conditions were caused by the particular chemical exposure. However, the lack of robust exposure information and a minimal understanding of cumulative effects means critical information required to prove causation is rarely available. As a result, the government often fails to adequately protect public health. We propose a response model based on presumptive association that would allow government to act in the absence of community-specific data linking cause and effect after community-wide chemical exposures. In this model, when a community is exposed to a chemical of concern, agencies would review scientific information about the health effects of exposure to that chemical. If the evidence indicates the chemical could cause a certain health condition, then the government would take action to benefit community members who were exposed and who have that condition. They would not have to prove that their health condition was caused by exposure to the chemical of concern. Adopting a presumptive association model for federal responses to chemical exposures would create a clear, fair, standardized, and timely approach that protects public health.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"11 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728852","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}
Sohyeon Choi, Aram Lee, Jae-Eun Lim, Sungkyoon Kim, Kyungho Choi, Hyo-Bang Moon, Younglim Kho, Jeongim Park
Phthalic acid esters (PAEs) and alternative plasticizers (APs) are commonly found in food packaging. We quantified diet-only exposure to twenty-one plasticizers (16 PAEs and 5 APs) in 124 Korean adults by GC-MS/MS in 370 duplicate-diet composites (representing three nonconsecutive 24-h collections per participant). Total plasticizer concentrations ranged from 103 to 240,000 ng/g dry weight (median 414 ng/g). DEHP predominated among PAEs (median 106 ng/g). Among APs, DEHTP, ATBC, and DINCH showed comparable medians (approximately 22 ng/g). The AP fraction rose significantly with increasing exposure: APs constituted 57% of the total in the highest quartile (Q4) versus 20% in the lowest quartile (Q1) (p < 0.001), with DINCH markedly enriched in Q4. Food-intake diaries indicated higher consumption of food delivery, packaged meals, and dining out in Q4, consistent with greater plastic contact. Estimated daily intakes for individual analytes were below their respective reference doses. However, 17.5% of samples exceeded the cumulative antiandrogenic reference dose. These findings suggest a compositional shift from PAEs toward APs, coupled with right-tail signals for cumulative antiandrogenic risk. Duplicate-diet coprofiling paired with body weight and 24 h diaries provides a baseline for surveillance of plasticizer shifts and for prioritizing candidate sources for follow-up measurement.
{"title":"Phthalates and Alternative Plasticizers in Duplicated Diet Samples from Korea","authors":"Sohyeon Choi, Aram Lee, Jae-Eun Lim, Sungkyoon Kim, Kyungho Choi, Hyo-Bang Moon, Younglim Kho, Jeongim Park","doi":"10.1021/acs.est.5c09984","DOIUrl":"https://doi.org/10.1021/acs.est.5c09984","url":null,"abstract":"Phthalic acid esters (PAEs) and alternative plasticizers (APs) are commonly found in food packaging. We quantified diet-only exposure to twenty-one plasticizers (16 PAEs and 5 APs) in 124 Korean adults by GC-MS/MS in 370 duplicate-diet composites (representing three nonconsecutive 24-h collections per participant). Total plasticizer concentrations ranged from 103 to 240,000 ng/g dry weight (median 414 ng/g). DEHP predominated among PAEs (median 106 ng/g). Among APs, DEHTP, ATBC, and DINCH showed comparable medians (approximately 22 ng/g). The AP fraction rose significantly with increasing exposure: APs constituted 57% of the total in the highest quartile (Q4) versus 20% in the lowest quartile (Q1) (<i>p</i> < 0.001), with DINCH markedly enriched in Q4. Food-intake diaries indicated higher consumption of food delivery, packaged meals, and dining out in Q4, consistent with greater plastic contact. Estimated daily intakes for individual analytes were below their respective reference doses. However, 17.5% of samples exceeded the cumulative antiandrogenic reference dose. These findings suggest a compositional shift from PAEs toward APs, coupled with right-tail signals for cumulative antiandrogenic risk. Duplicate-diet coprofiling paired with body weight and 24 h diaries provides a baseline for surveillance of plasticizer shifts and for prioritizing candidate sources for follow-up measurement.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"7 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718250","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}
Jinshuai Li, Tianxiang Hao, Mousong Wu, Meng Yang, Zhi Chen, Guirui Yu, Hyun Seok Kim, Sara H. Knox
Understanding the link between wetland gross primary productivity (GPP) and methane (CH4) emissions is crucial for global carbon cycle modeling, yet this coupling remains poorly constrained at a global scale due to data limitations. To address this critical gap, we compiled and analyzed the most comprehensive daily scale eddy covariance data set of GPP and CH4 fluxes. In this analysis, we define this coupling as the slope of the linear fit between carbon fixed by ecosystems and carbon emitted as CH4. Results indicate that the median lag time between CH4 emissions and GPP is 24.8 days. In terms of their coupling, for every gram of carbon fixed in wetlands, 0.03 (interquartile range: 0.02–0.05) grams of carbon are released into the atmosphere as CH4. The upscaling results indicate that the coupling in tropical wetlands is typically larger than in temperate and boreal wetlands, and the CO2-equivalent emissions of CH4 surpass the amount of CO2 absorbed through photosynthesis. These results enhance our understanding of the complex biogeochemical processes that drive CH4 emissions, offering valuable insights into the interplay between carbon fixation and emissions dynamics in wetland ecosystems.
{"title":"Linking Freshwater Wetland Productivity and Methane Emissions: A Global Perspective","authors":"Jinshuai Li, Tianxiang Hao, Mousong Wu, Meng Yang, Zhi Chen, Guirui Yu, Hyun Seok Kim, Sara H. Knox","doi":"10.1021/acs.est.5c10778","DOIUrl":"https://doi.org/10.1021/acs.est.5c10778","url":null,"abstract":"Understanding the link between wetland gross primary productivity (GPP) and methane (CH<sub>4</sub>) emissions is crucial for global carbon cycle modeling, yet this coupling remains poorly constrained at a global scale due to data limitations. To address this critical gap, we compiled and analyzed the most comprehensive daily scale eddy covariance data set of GPP and CH<sub>4</sub> fluxes. In this analysis, we define this coupling as the slope of the linear fit between carbon fixed by ecosystems and carbon emitted as CH<sub>4</sub>. Results indicate that the median lag time between CH<sub>4</sub> emissions and GPP is 24.8 days. In terms of their coupling, for every gram of carbon fixed in wetlands, 0.03 (interquartile range: 0.02–0.05) grams of carbon are released into the atmosphere as CH<sub>4</sub>. The upscaling results indicate that the coupling in tropical wetlands is typically larger than in temperate and boreal wetlands, and the CO<sub>2</sub>-equivalent emissions of CH<sub>4</sub> surpass the amount of CO<sub>2</sub> absorbed through photosynthesis. These results enhance our understanding of the complex biogeochemical processes that drive CH<sub>4</sub> emissions, offering valuable insights into the interplay between carbon fixation and emissions dynamics in wetland ecosystems.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"8 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718402","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}
Blood levels of the pollutants benzene, toluene, xylene (i.e., the sum of ortho-, meta-, and para-xylene isomers), and ethylbenzene (BTEX) are associated with an increased incidence of cardiovascular diseases. However, the underlying mechanisms are unknown. Here, we tested the hypothesis that BTEX accumulate in human atherosclerotic plaque, promoting local proinflammatory responses within atheroma tissues. To this aim, we retrospectively analyzed carotid plaque samples from 147 individuals from a cohort of people with asymptomatic carotid stenosis undergoing carotid endarterectomy. In atheroma specimens, we quantified BTEX and 1,4-benzoquinone, a benzene metabolite, through flame ionization detector gas chromatography and by high-performance liquid chromatography, respectively. We categorized individuals as BTEX-positive or BTEX-negative and compared the expression of plaque inflammatory markers in these two groups. To explore the mechanistic basis for our clinical observations, we also treated human monocytes with relevant concentrations of the four BTEX and evaluated their possible proinflammatory effect. Among the 147 plaques analyzed, 93 had evidence of at least one BTEX pollutant. Benzene was the most abundant, and its levels were positively correlated to those of 1,4-benzoquinone. Patients with evidence of BTEX within the atheroma, compared with those without, showed higher levels of CD68, MMP9, NLRP3, IL-1β, and TNF-α within the plaque but also of systemic markers of inflammation such as the white blood cell count and neutrophil-to-lymphocyte ratio. BTEX levels were positively correlated with NLRP3 and IL-1β levels as well as with triglyceride. BTEX levels were higher in people with a prior diagnosis of dyslipidemia and with a subsequent major cardiovascular event. Treatment of monocytes for 5 days with benzene, xylene, and ethylbenzene, but not toluene, fostered a consistent proinflammatory response, an effect observed in the absence of cytotoxicity and phenocopied by the treatment with 1,4-benzoquinone. BTEX and 1,4-benzoquinone also promoted foam cell formation in monocytes differentiated into macrophages. These data represent the first evidence that BTEX pollutants accumulate within the carotid plaque tissue. This phenomenon is associated with increased local inflammation, possibly suggesting the activation of proatherogenic pathways at the local level.
{"title":"Detection and Proinflammatory Effects of BTEX within the Human Atherosclerotic Plaque.","authors":"Raffaele Marfella,Francesca Carreras,Francesco Prattichizzo,Rosalba La Grotta,Valeria Pellegrini,Celestino Sardu,Nunzia D'Onofrio,Michelangela Barbieri,Maurizio Municinò,Mario Siniscalchi,Fabio Spinetti,Gennaro Vigliotti,Carmine Vecchione,Albino Carrizzo,Giulio Accarino,Antonio Squillante,Giuseppe Spaziano,Davida Mirra,Renata Esposito,Angelo Fenti,Simona Galoppo,Silvana Canzano,Ludovica Vittoria Marfella,Giovanni Falco,Maria Luisa Balestrieri,Ciro Mauro,Antonio Ceriello,Philip J Landrigan,Bruno D'Agostino,Pasquale Iovino,Giuseppe Paolisso","doi":"10.1021/acs.est.5c04941","DOIUrl":"https://doi.org/10.1021/acs.est.5c04941","url":null,"abstract":"Blood levels of the pollutants benzene, toluene, xylene (i.e., the sum of ortho-, meta-, and para-xylene isomers), and ethylbenzene (BTEX) are associated with an increased incidence of cardiovascular diseases. However, the underlying mechanisms are unknown. Here, we tested the hypothesis that BTEX accumulate in human atherosclerotic plaque, promoting local proinflammatory responses within atheroma tissues. To this aim, we retrospectively analyzed carotid plaque samples from 147 individuals from a cohort of people with asymptomatic carotid stenosis undergoing carotid endarterectomy. In atheroma specimens, we quantified BTEX and 1,4-benzoquinone, a benzene metabolite, through flame ionization detector gas chromatography and by high-performance liquid chromatography, respectively. We categorized individuals as BTEX-positive or BTEX-negative and compared the expression of plaque inflammatory markers in these two groups. To explore the mechanistic basis for our clinical observations, we also treated human monocytes with relevant concentrations of the four BTEX and evaluated their possible proinflammatory effect. Among the 147 plaques analyzed, 93 had evidence of at least one BTEX pollutant. Benzene was the most abundant, and its levels were positively correlated to those of 1,4-benzoquinone. Patients with evidence of BTEX within the atheroma, compared with those without, showed higher levels of CD68, MMP9, NLRP3, IL-1β, and TNF-α within the plaque but also of systemic markers of inflammation such as the white blood cell count and neutrophil-to-lymphocyte ratio. BTEX levels were positively correlated with NLRP3 and IL-1β levels as well as with triglyceride. BTEX levels were higher in people with a prior diagnosis of dyslipidemia and with a subsequent major cardiovascular event. Treatment of monocytes for 5 days with benzene, xylene, and ethylbenzene, but not toluene, fostered a consistent proinflammatory response, an effect observed in the absence of cytotoxicity and phenocopied by the treatment with 1,4-benzoquinone. BTEX and 1,4-benzoquinone also promoted foam cell formation in monocytes differentiated into macrophages. These data represent the first evidence that BTEX pollutants accumulate within the carotid plaque tissue. This phenomenon is associated with increased local inflammation, possibly suggesting the activation of proatherogenic pathways at the local level.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"148 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728472","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}
Converting sludge to high-value resources is a sustainable strategy. Recent advances in alkaline thermal hydrolysis (ATH) technology have revealed its potential for phytohormone synthesis by leveraging the inherent complexity of sludge, offering an innovative approach to resource recovery. While previous studies focused on optimizing yields and agronomic applications of sludge-derived phytohormones, mechanistic investigations into their molecular transformation pathways are lacking. This study systematically compares residual activated sludge (RAS) and anaerobic digestion sludge (ADS) to unravel phytohormone generation mechanisms during ATH. Using metabolomic analysis and molecular energy calculations, we clarified the phytohormone distribution and differential characteristics between the two sludges. Key findings reveal that ATH amplifies the inherent precursor advantages of specific sludge types: RAS shows superior auxin production (1.58 × 104 to 7.93 × 104 ng/mL), whereas ADS preferentially synthesizes jasmonic acids (6.61 to 2.56 × 103 ng/mL). Indole-3-acetic acid synthesis in RAS is driven by tryptophan-mediated pathways, where decarboxylation and aromatic substitution dominate precursor conversion; jasmonic acid in ADS forms via cyclization and oxidation of anaerobic-stress-induced linolenic acid derivatives. The favorable thermodynamics of both pathways was confirmed by Gibbs free energy calculations. Establishing relationships between sludge composition and phytohormone characteristics, this work provides molecular evidence to guide the agricultural application of sludge-derived phytohormones.
{"title":"Differential Molecular Transformation Mechanisms of Phytohormones in Activated Sludge and Anaerobic Digestion Sludge: The Precursor Roles of Tryptophan and Linolenic Acid","authors":"Shuxian Chen, Yu Hua, Chong Chen, Yue Zhang, Nina Duan, Boyuan Zou, Lihua Wang, Xiaohu Dai","doi":"10.1021/acs.est.5c11385","DOIUrl":"https://doi.org/10.1021/acs.est.5c11385","url":null,"abstract":"Converting sludge to high-value resources is a sustainable strategy. Recent advances in alkaline thermal hydrolysis (ATH) technology have revealed its potential for phytohormone synthesis by leveraging the inherent complexity of sludge, offering an innovative approach to resource recovery. While previous studies focused on optimizing yields and agronomic applications of sludge-derived phytohormones, mechanistic investigations into their molecular transformation pathways are lacking. This study systematically compares residual activated sludge (RAS) and anaerobic digestion sludge (ADS) to unravel phytohormone generation mechanisms during ATH. Using metabolomic analysis and molecular energy calculations, we clarified the phytohormone distribution and differential characteristics between the two sludges. Key findings reveal that ATH amplifies the inherent precursor advantages of specific sludge types: RAS shows superior auxin production (1.58 × 10<sup>4</sup> to 7.93 × 10<sup>4</sup> ng/mL), whereas ADS preferentially synthesizes jasmonic acids (6.61 to 2.56 × 10<sup>3</sup> ng/mL). Indole-3-acetic acid synthesis in RAS is driven by tryptophan-mediated pathways, where decarboxylation and aromatic substitution dominate precursor conversion; jasmonic acid in ADS forms via cyclization and oxidation of anaerobic-stress-induced linolenic acid derivatives. The favorable thermodynamics of both pathways was confirmed by Gibbs free energy calculations. Establishing relationships between sludge composition and phytohormone characteristics, this work provides molecular evidence to guide the agricultural application of sludge-derived phytohormones.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"113 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718251","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}
Yuren Feng,Xiaochuan Huang,Ze He,Tsai-Hsuan Chen,Matthew D Meyer,Yifan Zhu,Yunhao Zhang,Chia-Hung Hou,Kuichang Zuo,Qilin Li
Ion exchange membranes (IEMs) separate ions of opposite charges, enabling a variety of applications, including desalination and mineral recovery via electrodialysis (ED). ED is uniquely suited for ion separation and recovery from high-salinity waters, especially for ions of low concentrations, as ions, instead of water, are transported in an electrical field. However, the application of ED is limited by the lack of selectivity of the counterions in the existing IEMs. Here, we developed a thin-film composite cation exchange membrane (TFC-CEM) consisting of an ultrathin polyamide coating, a porous polysulfone support, and a dense cation exchange polymer layer, which provides excellent separation between divalent and monovalent cations, high mechanical strength, and effective separation between cations and anions. At a constant current of 0.24 mA cm-2, the TFC-CEM demonstrated monovalent over divalent cation selectivity of 49.32-136.79 in mixed cation solutions with a divalent to monovalent cation molar ratio of 25. The selectivity increased with increasing divalent to monovalent cation concentration ratios and correlated strongly with the difference in the hydrated size of the cations. Furthermore, the asymmetric structure of the TFC-CEM led to unique limiting current density behaviors, revealing that ion transport through the polyamide coating was rate-limiting. Finally, TFC-CEM demonstrated great potential for lithium extraction from hypersaline brines.
离子交换膜（IEMs）可以分离带相反电荷的离子，从而实现多种应用，包括通过电渗析（ED）进行海水淡化和矿物回收。ED特别适合于从高盐度水中分离和回收离子，特别是低浓度离子，因为离子而不是水在电场中传输。然而，由于现有的IEMs中对离子缺乏选择性，限制了ED的应用。在此，我们开发了一种薄膜复合阳离子交换膜（TFC-CEM），该膜由超薄聚酰胺涂层、多孔聚砜载体和密集的阳离子交换聚合物层组成，具有良好的二价和一价阳离子分离，高机械强度和有效的阳离子和阴离子分离。在恒定电流为0.24 mA cm-2时，TFC-CEM在二价与一价阳离子摩尔比为25的混合阳离子溶液中表现出一价阳离子对二价阳离子的选择性为49.32 ~ 136.79。选择性随二价与单价阳离子浓度比的增加而增加，并与阳离子水合尺寸的差异密切相关。此外，TFC-CEM的不对称结构导致了独特的极限电流密度行为，表明离子通过聚酰胺涂层是限速的。最后，TFC-CEM显示了从高盐盐水中提取锂的巨大潜力。
{"title":"Scalable Thin-Film Composite Cation Exchange Membrane for Separation of Monovalent and Divalent Cations in Electrodialysis.","authors":"Yuren Feng,Xiaochuan Huang,Ze He,Tsai-Hsuan Chen,Matthew D Meyer,Yifan Zhu,Yunhao Zhang,Chia-Hung Hou,Kuichang Zuo,Qilin Li","doi":"10.1021/acs.est.5c14380","DOIUrl":"https://doi.org/10.1021/acs.est.5c14380","url":null,"abstract":"Ion exchange membranes (IEMs) separate ions of opposite charges, enabling a variety of applications, including desalination and mineral recovery via electrodialysis (ED). ED is uniquely suited for ion separation and recovery from high-salinity waters, especially for ions of low concentrations, as ions, instead of water, are transported in an electrical field. However, the application of ED is limited by the lack of selectivity of the counterions in the existing IEMs. Here, we developed a thin-film composite cation exchange membrane (TFC-CEM) consisting of an ultrathin polyamide coating, a porous polysulfone support, and a dense cation exchange polymer layer, which provides excellent separation between divalent and monovalent cations, high mechanical strength, and effective separation between cations and anions. At a constant current of 0.24 mA cm-2, the TFC-CEM demonstrated monovalent over divalent cation selectivity of 49.32-136.79 in mixed cation solutions with a divalent to monovalent cation molar ratio of 25. The selectivity increased with increasing divalent to monovalent cation concentration ratios and correlated strongly with the difference in the hydrated size of the cations. Furthermore, the asymmetric structure of the TFC-CEM led to unique limiting current density behaviors, revealing that ion transport through the polyamide coating was rate-limiting. Finally, TFC-CEM demonstrated great potential for lithium extraction from hypersaline brines.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"10 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728631","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}
Xinfei Ge, Wenjun Zhang, Lijun Wang, Christine V. Putnis
Phosphorus (P) is a nonrenewable macronutrient essential for agriculture, yet its availability is often constrained by the formation of mineral–P associations (MPAs) at soil–mineral interfaces. Soil organic carbon (SOC), however, can dynamically transform these MPAs, mobilizing the associated P. This critical review synthesizes the interface processes and mechanisms governing the formation and transformation of MPAs, linking them to farmland P availability. We first outline the specific characteristics of minerals and P phases that lead to the formation of MPAs via adsorption and precipitation. We then introduce a novel conceptual framework in which SOC drives the transformation of MPAs through desorption and dissolution. This framework emphasizes how the specific reactive SOC compounds target mineral-associated P (MAP), with efficacy contingent on MPA inherent properties. We propose a trade-off between the formation and transformation dynamics of MPAs, which governs the legacy P pool and its varying availability. A holistic understanding of these dynamic interactions operating at mineral–organic carbon interfaces will enhance predictions of long-term P fertility and inform the development of innovative SOC-based P management strategies for sustainable agriculture and environment.
{"title":"Dynamic Phosphorus Interactions at Soil Mineral–Organic Carbon Interfaces: A Critical Review","authors":"Xinfei Ge, Wenjun Zhang, Lijun Wang, Christine V. Putnis","doi":"10.1021/acs.est.5c14215","DOIUrl":"https://doi.org/10.1021/acs.est.5c14215","url":null,"abstract":"Phosphorus (P) is a nonrenewable macronutrient essential for agriculture, yet its availability is often constrained by the formation of mineral–P associations (MPAs) at soil–mineral interfaces. Soil organic carbon (SOC), however, can dynamically transform these MPAs, mobilizing the associated P. This critical review synthesizes the interface processes and mechanisms governing the formation and transformation of MPAs, linking them to farmland P availability. We first outline the specific characteristics of minerals and P phases that lead to the formation of MPAs via adsorption and precipitation. We then introduce a novel conceptual framework in which SOC drives the transformation of MPAs through desorption and dissolution. This framework emphasizes how the specific reactive SOC compounds target mineral-associated P (MAP), with efficacy contingent on MPA inherent properties. We propose a trade-off between the formation and transformation dynamics of MPAs, which governs the legacy P pool and its varying availability. A holistic understanding of these dynamic interactions operating at mineral–organic carbon interfaces will enhance predictions of long-term P fertility and inform the development of innovative SOC-based P management strategies for sustainable agriculture and environment.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"112 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718403","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}
Yan Zhu,Shihao Wang,Yong Han,Yao Lu,Anqi Xiong,Shulan Qiu,Ling N Jin,Weixiong Zhang
Air pollution poses a critical global public health challenge. Molecular-level initiating events, such as pollutant-protein interactions, can trigger cascades of biological responses that may contribute to adverse health effects. However, current methods are limited in their ability to systematically identify these early binding events, particularly for emerging airborne pollutants, which hinders mechanistic understanding and risk assessment of pollution-related toxicity. To address this, we developed tipFormer (pollutant-protein interaction prediction based on transformer), a novel deep learning approach for predicting interactions between airborne organic pollutants and human proteins. The model incorporates dual pretrained language models to encode proteins and organic pollutants, coupled with cross-attention mechanisms to learn intricate interaction patterns underlying pollutant-protein binding. Rigorous validation demonstrated that tipFormer achieves state-of-the-art performance, with an AUC of 0.9787 on a test set. Furthermore, genome-wide transcriptomic analysis using human bronchial epithelial cells exposed to three representative airborne pollutants revealed significant concordance between tipFormer's predicted targets and the experimentally responsive genes, thereby supporting the model's biological relevance. By bridging large-scale computational predictions with transcriptomic validation, this study provides deeper mechanistic insight into the molecular basis of air pollution-related adverse outcomes.
{"title":"A Transformer-Based Deep Learning Approach to Predicting Air Organic Pollutant-Human Protein Interactions.","authors":"Yan Zhu,Shihao Wang,Yong Han,Yao Lu,Anqi Xiong,Shulan Qiu,Ling N Jin,Weixiong Zhang","doi":"10.1021/acs.est.5c12915","DOIUrl":"https://doi.org/10.1021/acs.est.5c12915","url":null,"abstract":"Air pollution poses a critical global public health challenge. Molecular-level initiating events, such as pollutant-protein interactions, can trigger cascades of biological responses that may contribute to adverse health effects. However, current methods are limited in their ability to systematically identify these early binding events, particularly for emerging airborne pollutants, which hinders mechanistic understanding and risk assessment of pollution-related toxicity. To address this, we developed tipFormer (pollutant-protein interaction prediction based on transformer), a novel deep learning approach for predicting interactions between airborne organic pollutants and human proteins. The model incorporates dual pretrained language models to encode proteins and organic pollutants, coupled with cross-attention mechanisms to learn intricate interaction patterns underlying pollutant-protein binding. Rigorous validation demonstrated that tipFormer achieves state-of-the-art performance, with an AUC of 0.9787 on a test set. Furthermore, genome-wide transcriptomic analysis using human bronchial epithelial cells exposed to three representative airborne pollutants revealed significant concordance between tipFormer's predicted targets and the experimentally responsive genes, thereby supporting the model's biological relevance. By bridging large-scale computational predictions with transcriptomic validation, this study provides deeper mechanistic insight into the molecular basis of air pollution-related adverse outcomes.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"15 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728471","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}
Zeya Li, Xun Wang, Huizhong Li, Zi Yan, Xin Zhou, Zhiquan Hou, Lu Wei, Jiguang Deng, Hongxing Dai, Yuxi Liu
Chlorinated volatile organic compounds (CVOCs) exert a big hazard to public health and the atmosphere environment. The conventional way of eliminating CVOCs at the emission source is by exhausting liquid recovery. Owing to the complexity and cost of purification, however, the collected CVOCs are difficult to reuse as raw materials. Herein, this study puts forward an innovative approach for enhancing the usage efficiencies of recovered CVOCs that converted the CVOCs into syngas through catalytic steam reforming and employed the yielded syngas as clean and value-added chemicals. To study the feasibility of such a technique, steam reforming of 1,2-dichloroethane (1,2-DCE) was performed over the supported intermetallic compound catalyst (Pd5Ga3/TiO2), which exhibited a remarkable catalytic efficiency with a 1,2-DCE conversion of 88.9% at 550 °C and a carbon monoxide selectivity of 77.8%. Moreover, no distinct change in catalytic activity over the bimetallic catalyst during the stability test at 550 °C indicated its excellent chlorine and coke resistance ability. The synergistic interaction of the Pd5Ga3 greatly promoted the adsorption and activation of H2O to form distinctive hydrogen-bond hydroxyl groups, which could be exchanged with a Cl atom that promoted the rupture of C–Cl bonds. The Pd5Ga3/TiO2 catalyst converted both trichloroethylene (TCE) and chlorobenzene (CB) with conversion efficiencies of above 99.8% and 82.0% at 600 °C, while maintaining remarkable (CO + H2) yields. This work opens a promising pathway for developing antichlorine and coke poisoning catalyst and related technology for the resource utilization of CVOCs.
{"title":"Palladium–Gallium Intermetallic Compound with Unique Ability to Activate Water for Catalytic Steam Reforming of 1,2-Dichloroethane","authors":"Zeya Li, Xun Wang, Huizhong Li, Zi Yan, Xin Zhou, Zhiquan Hou, Lu Wei, Jiguang Deng, Hongxing Dai, Yuxi Liu","doi":"10.1021/acs.est.5c08172","DOIUrl":"https://doi.org/10.1021/acs.est.5c08172","url":null,"abstract":"Chlorinated volatile organic compounds (CVOCs) exert a big hazard to public health and the atmosphere environment. The conventional way of eliminating CVOCs at the emission source is by exhausting liquid recovery. Owing to the complexity and cost of purification, however, the collected CVOCs are difficult to reuse as raw materials. Herein, this study puts forward an innovative approach for enhancing the usage efficiencies of recovered CVOCs that converted the CVOCs into syngas through catalytic steam reforming and employed the yielded syngas as clean and value-added chemicals. To study the feasibility of such a technique, steam reforming of 1,2-dichloroethane (1,2-DCE) was performed over the supported intermetallic compound catalyst (Pd<sub>5</sub>Ga<sub>3</sub>/TiO<sub>2</sub>), which exhibited a remarkable catalytic efficiency with a 1,2-DCE conversion of 88.9% at 550 °C and a carbon monoxide selectivity of 77.8%. Moreover, no distinct change in catalytic activity over the bimetallic catalyst during the stability test at 550 °C indicated its excellent chlorine and coke resistance ability. The synergistic interaction of the Pd<sub>5</sub>Ga<sub>3</sub> greatly promoted the adsorption and activation of H<sub>2</sub>O to form distinctive hydrogen-bond hydroxyl groups, which could be exchanged with a Cl atom that promoted the rupture of C–Cl bonds. The Pd<sub>5</sub>Ga<sub>3</sub>/TiO<sub>2</sub> catalyst converted both trichloroethylene (TCE) and chlorobenzene (CB) with conversion efficiencies of above 99.8% and 82.0% at 600 °C, while maintaining remarkable (CO + H<sub>2</sub>) yields. This work opens a promising pathway for developing antichlorine and coke poisoning catalyst and related technology for the resource utilization of CVOCs.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"20 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718401","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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