Fan Fan, Fu Liu, Qingmiao Yu, Ran Yi, Hongqiang Ren, Jinju Geng
Identifying primary estrogen receptor (ER) agonists in municipal sewage is essential for ensuring the health of aquatic environments. Given the complex and variable chemical composition of sewage, the predominant ER agonists remain unclear. High-resolution mass spectrometry (HRMS)-based models have been developed to predict compound bioactivity in complex matrices, but further optimization is needed to effectively bridge HRMS features with ER agonists. To address this challenge, an FT-GNN (fragmentation tree-based graph neural network) model was proposed. Given limited data and class imbalance, data augmentation was performed using model predictions within the applicability domain (AD) and oversampling technique (OTE). Model development results demonstrated that integrating the FT-GNN with data augmentation improved the balanced accuracy (bACC) value by 6%–31%. The developed model, with a high bACC to identify more true ER agonists, efficiently classified tens of thousands of unidentified HRMS features in sewage, reducing postprocessing workload in nontargeted screening. Analysis of ER agonist transformation during sewage treatment revealed the anaerobic stage as key to both their removal and formation. Estrogenic effect balance analysis suggests that α-E2 and 9,11-didehydroestriol may be two previously overlooked key ER agonists. Collectively, the development and application of the FT-GNN model are crucial advancements toward credible tracking and efficient control of estrogenic risks in water.
{"title":"FT-GNN Tool for Bridging HRMS Features and Bioactivity: Uncovering Unidentified Estrogen Receptor Agonists in Sewage","authors":"Fan Fan, Fu Liu, Qingmiao Yu, Ran Yi, Hongqiang Ren, Jinju Geng","doi":"10.1021/acs.est.5c02324","DOIUrl":"https://doi.org/10.1021/acs.est.5c02324","url":null,"abstract":"Identifying primary estrogen receptor (ER) agonists in municipal sewage is essential for ensuring the health of aquatic environments. Given the complex and variable chemical composition of sewage, the predominant ER agonists remain unclear. High-resolution mass spectrometry (HRMS)-based models have been developed to predict compound bioactivity in complex matrices, but further optimization is needed to effectively bridge HRMS features with ER agonists. To address this challenge, an FT-GNN (fragmentation tree-based graph neural network) model was proposed. Given limited data and class imbalance, data augmentation was performed using model predictions within the applicability domain (AD) and oversampling technique (OTE). Model development results demonstrated that integrating the FT-GNN with data augmentation improved the balanced accuracy (bACC) value by 6%–31%. The developed model, with a high bACC to identify more true ER agonists, efficiently classified tens of thousands of unidentified HRMS features in sewage, reducing postprocessing workload in nontargeted screening. Analysis of ER agonist transformation during sewage treatment revealed the anaerobic stage as key to both their removal and formation. Estrogenic effect balance analysis suggests that α-E2 and 9,11-didehydroestriol may be two previously overlooked key ER agonists. Collectively, the development and application of the FT-GNN model are crucial advancements toward credible tracking and efficient control of estrogenic risks in water.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"1 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143805979","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}
Rahel Mesfin Ketema, Yu Ait Bamai, Houman Goudarzi, Takeshi Yamaguchi, Yi Zeng, Ayaka Yasuda, Megasari Marsela, Satoshi Konno, Reiko Kishi, Atsuko Ikeda
Phthalate exposure is linked to asthma and allergic symptoms, yet their individual and combined effects on symptoms and inflammatory biomarkers, type 2 (T2) and non-T2, remain unexplored. This study examined the association of phthalate metabolites with allergic symptoms (wheeze, allergic rhinoconjunctivitis, and eczema), T2 biomarker (fraction of exhaled nitric oxide (FeNO), blood eosinophil count, and total immunoglobulin E (IgE)), and non-T2 biomarker (absolute neutrophil count (ANC)) and also their association with oxidative stress biomarkers, such as 4-hydroxynonenal, hexanoyl-lysine, and 8-hydroxy-2-deoxyguanosine. Ten urinary phthalate metabolites were measured using UPLC-MS/MS in 421 children (aged 9–12 years) from The Hokkaido Cohort, Japan. Symptoms were defined using the International Study of Asthma and Allergies in Childhood questionnaire, and biomarkers were measured in blood. Logistic regression assessed individual metabolites, while quantile-g computation and Bayesian kernel machine regression analyzed mixture effects on binary outcomes. Individual analysis showed that MnBP (mono-n-butyl phthalate) was positively associated with allergic rhinoconjunctivitis and eosinophil ≥ 300 cells/μL, while ∑DBP (dibutyl phthalate) and OH-MiNP (mono-hydroxy-isononyl phthalate) were linked with FeNO ≥ 35 ppb. DEHP (di(2-ethylhexyl) phthalate) metabolites were associated with a high prevalence of blood eosinophils ≥ 300 cells/μL. We found a positive association between phthalates and oxidative stress markers, but no link was observed between oxidative stress and inflammatory markers. Mixture analysis identified MnBP as a major contributor to the high FeNO level, with di-n-butyl phthalate (DnBP) and DEHP metabolites contributing to eosinophil count ≥ 300 cells/μL and ANC ≥ 4400 cells/μL. These findings suggest that phthalate exposure from DnBP and DEHP is associated with immune dysregulation by triggering both T2 and non-T2 inflammatory responses.
{"title":"Association of Phthalate Exposure with Respiratory and Allergic Symptoms and Type 2 and Non-Type 2 Inflammation: The Hokkaido Study","authors":"Rahel Mesfin Ketema, Yu Ait Bamai, Houman Goudarzi, Takeshi Yamaguchi, Yi Zeng, Ayaka Yasuda, Megasari Marsela, Satoshi Konno, Reiko Kishi, Atsuko Ikeda","doi":"10.1021/acs.est.4c14579","DOIUrl":"https://doi.org/10.1021/acs.est.4c14579","url":null,"abstract":"Phthalate exposure is linked to asthma and allergic symptoms, yet their individual and combined effects on symptoms and inflammatory biomarkers, type 2 (T2) and non-T2, remain unexplored. This study examined the association of phthalate metabolites with allergic symptoms (wheeze, allergic rhinoconjunctivitis, and eczema), T2 biomarker (fraction of exhaled nitric oxide (FeNO), blood eosinophil count, and total immunoglobulin E (IgE)), and non-T2 biomarker (absolute neutrophil count (ANC)) and also their association with oxidative stress biomarkers, such as 4-hydroxynonenal, hexanoyl-lysine, and 8-hydroxy-2-deoxyguanosine. Ten urinary phthalate metabolites were measured using UPLC-MS/MS in 421 children (aged 9–12 years) from The Hokkaido Cohort, Japan. Symptoms were defined using the International Study of Asthma and Allergies in Childhood questionnaire, and biomarkers were measured in blood. Logistic regression assessed individual metabolites, while quantile-g computation and Bayesian kernel machine regression analyzed mixture effects on binary outcomes. Individual analysis showed that MnBP (mono-<i>n</i>-butyl phthalate) was positively associated with allergic rhinoconjunctivitis and eosinophil ≥ 300 cells/μL, while ∑DBP (dibutyl phthalate) and OH-MiNP (mono-hydroxy-isononyl phthalate) were linked with FeNO ≥ 35 ppb. DEHP (di(2-ethylhexyl) phthalate) metabolites were associated with a high prevalence of blood eosinophils ≥ 300 cells/μL. We found a positive association between phthalates and oxidative stress markers, but no link was observed between oxidative stress and inflammatory markers. Mixture analysis identified MnBP as a major contributor to the high FeNO level, with di-<i>n</i>-butyl phthalate (DnBP) and DEHP metabolites contributing to eosinophil count ≥ 300 cells/μL and ANC ≥ 4400 cells/μL. These findings suggest that phthalate exposure from DnBP and DEHP is associated with immune dysregulation by triggering both T2 and non-T2 inflammatory responses.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"31 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806048","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}
Julie Beth Zimmerman, Gregory Lowry, Fernando Rosario-Ortiz, Paul Westerhoff, Daniel Alessi, Pedro Alvarez, Alexandra Boehm, Ian Cousins, Jordi Dachs, Matthew Eckelman, Imad El Haddad, Pablo Gago-Ferrero, Jorge Gardea-Torresdey, Jacqueline MacDonald Gibson, Keri Hornbuckle, Heileen Hsu-Kim, Juliane Hollender, Atsuko Ikeda, Frederic Leusch, Melissa Maurer-Jones, James Mihelcic, Shelly Miller, Lutgarde Raskin, Z. Jason Ren, Susan Richardson, Daniel Schlenk, Huahong Shi, Paul Tratnyek, David Waite, Shuxiao Wang, Zhanyun Wang, Michael Wong, Sukhwan Yoon
There is an old saying that “facts do not need you to believe them to be true”. This has never been more relevant. In an era where scientific research, particularly in environmental, health, and climate science, faces mounting political challenges, we must reaffirm that our work is not contingent on ideology but on the immutable laws of nature. A molecule of carbon dioxide does not recognize political debates over international climate agreements. It will, however, contribute to climate change because of the fundamental physics governing the carbon–oxygen double bond. A molecule of methylene chloride does not consider economic arguments about regulatory limits, yet it will still be capable of causing cancer when it enters the human body. Per- and polyfluoroalkyl substances, PCBs, pesticides, and heavy metals do not change their toxicity based on geopolitical preferences. The virulence of a pathogen is not determined by socially acceptable risk standards. The dangers these and other substances and organisms pose are dictated by their physical and chemical properties, indifferent to political rhetoric, economic debates, or national borders. Science-based environmental policies have delivered tangible benefits. The United States’ Clean Water and Air Acts dramatically improved water and air quality, preventing disease and mortality while saving billions in healthcare costs. Many countries use the World Health Organization’s health-based drinking water quality standards as the basis for their own national standards, which have significantly reduced infant mortality from infectious diseases. The Montreal Protocol has meaningfully benefited the planet by protecting the ozone layer and mitigating climate change. Multilateral agreements such as the Stockholm Convention on Persistent Organic Pollutants and the Minamata Convention on mercury have curtailed our exposure to hazardous chemicals. China’s clean air action plans have achieved remarkable air quality improvements in record time, demonstrating that environmental progress is possible even amid rapid economic expansion. Today’s environmental crises continue to defy geopolitical boundaries and the politics that compound them. Mercury pollution in tuna, plastics in the ocean, and chemical contaminants in Arctic and Antarctic wildlife are a few examples illustrating that no single country or continent can confront these challenges alone. The increasing frequency and intensity of environmental disasters due to climate change, from record-breaking wildfires to catastrophic flooding, further underscore the urgency for global, coordinated actions. As environmental scientists and engineers, our mandate is clear: we must remain steadfast in our commitment to truth and scientific integrity. We must amplify our voices, educating, informing, and engaging with decision-makers and the public and insisting that scientific facts underpin policy decisions. More than ever, it is crucial to share our findings effectivel
{"title":"Apolitical Science","authors":"Julie Beth Zimmerman, Gregory Lowry, Fernando Rosario-Ortiz, Paul Westerhoff, Daniel Alessi, Pedro Alvarez, Alexandra Boehm, Ian Cousins, Jordi Dachs, Matthew Eckelman, Imad El Haddad, Pablo Gago-Ferrero, Jorge Gardea-Torresdey, Jacqueline MacDonald Gibson, Keri Hornbuckle, Heileen Hsu-Kim, Juliane Hollender, Atsuko Ikeda, Frederic Leusch, Melissa Maurer-Jones, James Mihelcic, Shelly Miller, Lutgarde Raskin, Z. Jason Ren, Susan Richardson, Daniel Schlenk, Huahong Shi, Paul Tratnyek, David Waite, Shuxiao Wang, Zhanyun Wang, Michael Wong, Sukhwan Yoon","doi":"10.1021/acs.est.5c03696","DOIUrl":"https://doi.org/10.1021/acs.est.5c03696","url":null,"abstract":"There is an old saying that “facts do not need you to believe them to be true”. This has never been more relevant. In an era where scientific research, particularly in environmental, health, and climate science, faces mounting political challenges, we must reaffirm that our work is not contingent on ideology but on the immutable laws of nature. A molecule of carbon dioxide does not recognize political debates over international climate agreements. It will, however, contribute to climate change because of the fundamental physics governing the carbon–oxygen double bond. A molecule of methylene chloride does not consider economic arguments about regulatory limits, yet it will still be capable of causing cancer when it enters the human body. Per- and polyfluoroalkyl substances, PCBs, pesticides, and heavy metals do not change their toxicity based on geopolitical preferences. The virulence of a pathogen is not determined by socially acceptable risk standards. The dangers these and other substances and organisms pose are dictated by their physical and chemical properties, indifferent to political rhetoric, economic debates, or national borders. Science-based environmental policies have delivered tangible benefits. The United States’ Clean Water and Air Acts dramatically improved water and air quality, preventing disease and mortality while saving billions in healthcare costs. Many countries use the World Health Organization’s health-based drinking water quality standards as the basis for their own national standards, which have significantly reduced infant mortality from infectious diseases. The Montreal Protocol has meaningfully benefited the planet by protecting the ozone layer and mitigating climate change. Multilateral agreements such as the Stockholm Convention on Persistent Organic Pollutants and the Minamata Convention on mercury have curtailed our exposure to hazardous chemicals. China’s clean air action plans have achieved remarkable air quality improvements in record time, demonstrating that environmental progress is possible even amid rapid economic expansion. Today’s environmental crises continue to defy geopolitical boundaries and the politics that compound them. Mercury pollution in tuna, plastics in the ocean, and chemical contaminants in Arctic and Antarctic wildlife are a few examples illustrating that no single country or continent can confront these challenges alone. The increasing frequency and intensity of environmental disasters due to climate change, from record-breaking wildfires to catastrophic flooding, further underscore the urgency for global, coordinated actions. As environmental scientists and engineers, our mandate is clear: we must remain steadfast in our commitment to truth and scientific integrity. We must amplify our voices, educating, informing, and engaging with decision-makers and the public and insisting that scientific facts underpin policy decisions. More than ever, it is crucial to share our findings effectivel","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"1 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798315","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}
Pranav Nair, Holly Barrett, Kaylin Tanoto, Linna Xie, Jianxian Sun, Diwen Yang, Han Yao, Datong Song, Hui Peng
Distinct from other nontoxic phenyl-p-phenylenediamine (PPD) quinones, N-(1,3-dimethylbutyl)-N′-phenyl-p-phenylenediamine-quinone (6PPD-Q) was recently discovered to be regioselectively metabolized to alkyl hydroxylated metabolites (alkyl–OH-6PPD-Q) in rainbow trout. It remains unknown whether the unique alkyl–OH-6PPD-Q contributes to the toxicity of 6PPD-Q. To test this, we herein synthesized chemical standards of alkyl–OH-6PPD-Q isomers and investigated their metabolic formation mechanism and toxicity. The predominant alkyl–OH-6PPD-Q was confirmed to be hydroxylated on the C4 tertiary carbon (C4–OH-6PPD-Q). The formation of C4–OH-6PPD-Q was only observed in microsomal but not in cytosolic fractions of rainbow trout (O. mykiss) liver S9. A general cytochrome P450 (CYP450) inhibitor fluoxetine inhibited the formation of hydroxylated metabolites of 6PPD-Q, supporting that CYP450 catalyzed the hydroxylation. This well-explained the compound- and regio-selective formation of C4–OH-6PPD-Q, due to the weak C–H bond on the C4 tertiary carbon. Surprisingly, while cytotoxicity was observed for 6PPD-Q and C3–OH-6PPD-Q in a coho salmon (O. kisutch) embryo (CSE-119) cell line, no toxicity was observed for C4–OH-6PPD-Q. To further confirm this under physiologically relevant conditions, we fractionated 6PPD-Q metabolites formed in the liver microsome of rainbow trout. Cytotoxicity was observed for the fraction of 6PPD-Q, but not the fraction of C4–OH-6PPD-Q. In summary, this study highlighted the C4 tertiary carbon as the key moiety for both metabolism and toxicity of 6PPD-Q and confirmed that alkyl hydroxylation is a detoxification pathway for 6PPD-Q.
{"title":"Structure and Toxicity Characterization of Alkyl Hydroxylated Metabolites of 6PPD-Q","authors":"Pranav Nair, Holly Barrett, Kaylin Tanoto, Linna Xie, Jianxian Sun, Diwen Yang, Han Yao, Datong Song, Hui Peng","doi":"10.1021/acs.est.4c11823","DOIUrl":"https://doi.org/10.1021/acs.est.4c11823","url":null,"abstract":"Distinct from other nontoxic phenyl-<i>p</i>-phenylenediamine (PPD) quinones, <i>N</i>-(1,3-dimethylbutyl)-<i>N</i>′-phenyl-<i>p</i>-phenylenediamine-quinone (6PPD-Q) was recently discovered to be regioselectively metabolized to alkyl hydroxylated metabolites (alkyl–OH-6PPD-Q) in rainbow trout. It remains unknown whether the unique alkyl–OH-6PPD-Q contributes to the toxicity of 6PPD-Q. To test this, we herein synthesized chemical standards of alkyl–OH-6PPD-Q isomers and investigated their metabolic formation mechanism and toxicity. The predominant alkyl–OH-6PPD-Q was confirmed to be hydroxylated on the C<sub>4</sub> tertiary carbon (C<sub>4</sub>–OH-6PPD-Q). The formation of C<sub>4</sub>–OH-6PPD-Q was only observed in microsomal but not in cytosolic fractions of rainbow trout (<i>O. mykiss</i>) liver S9. A general cytochrome P450 (CYP450) inhibitor fluoxetine inhibited the formation of hydroxylated metabolites of 6PPD-Q, supporting that CYP450 catalyzed the hydroxylation. This well-explained the compound- and regio-selective formation of C<sub>4</sub>–OH-6PPD-Q, due to the weak C–H bond on the C<sub>4</sub> tertiary carbon. Surprisingly, while cytotoxicity was observed for 6PPD-Q and C<sub>3</sub>–OH-6PPD-Q in a coho salmon (<i>O. kisutch</i>) embryo (CSE-119) cell line, no toxicity was observed for C<sub>4</sub>–OH-6PPD-Q. To further confirm this under physiologically relevant conditions, we fractionated 6PPD-Q metabolites formed in the liver microsome of rainbow trout. Cytotoxicity was observed for the fraction of 6PPD-Q, but not the fraction of C<sub>4</sub>–OH-6PPD-Q. In summary, this study highlighted the C<sub>4</sub> tertiary carbon as the key moiety for both metabolism and toxicity of 6PPD-Q and confirmed that alkyl hydroxylation is a detoxification pathway for 6PPD-Q.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"244 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798193","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}
Pablo A. Lara-Martín, Lena Schinkel, Yves Eberhard, Walter Giger, Michael Berg, Juliane Hollender
The increasing amount of sewage sludge generated during wastewater treatment poses both growing management challenge and environmental issues. Sludge with many co-occurring contaminants is often destined to land application which raises concern regarding human and environmental health. It is also a good integrator in time and space and can provide valuable information on consumption pattern and change over time. Here, we have conducted suspect and nontarget screening (SNTS) in sludge from 29 wastewater treatment plants (WWTPs) covering 30% of the Swiss population. Over 500 contaminants were identified and up to 382 quantified, with concentrations ranging from a few ng/g to several thousand ng/g, which translated into total annual loads of approximately 5 g of micropollutants per Swiss citizen. The distribution of detected substances was dominated by pharmaceuticals in terms of number of compounds (>250) and personal care products in terms of concentration (e.g., 75 μg/g for linoleic acid). Homologous series analysis revealed the presence of multiple classes of surfactants among those compounds with the highest signal intensities in sludge. Principal component analysis and hierarchical clustering showed that spatial distribution of contaminants across Switzerland was not homogeneous, while Pearson correlation indicated that changes can be attributed to different anaerobic digestion times in WWTPs.
{"title":"Suspect and Nontarget Screening of Organic Micropollutants in Swiss Sewage Sludge: A Nationwide Survey","authors":"Pablo A. Lara-Martín, Lena Schinkel, Yves Eberhard, Walter Giger, Michael Berg, Juliane Hollender","doi":"10.1021/acs.est.4c13217","DOIUrl":"https://doi.org/10.1021/acs.est.4c13217","url":null,"abstract":"The increasing amount of sewage sludge generated during wastewater treatment poses both growing management challenge and environmental issues. Sludge with many co-occurring contaminants is often destined to land application which raises concern regarding human and environmental health. It is also a good integrator in time and space and can provide valuable information on consumption pattern and change over time. Here, we have conducted suspect and nontarget screening (SNTS) in sludge from 29 wastewater treatment plants (WWTPs) covering 30% of the Swiss population. Over 500 contaminants were identified and up to 382 quantified, with concentrations ranging from a few ng/g to several thousand ng/g, which translated into total annual loads of approximately 5 g of micropollutants per Swiss citizen. The distribution of detected substances was dominated by pharmaceuticals in terms of number of compounds (>250) and personal care products in terms of concentration (e.g., 75 μg/g for linoleic acid). Homologous series analysis revealed the presence of multiple classes of surfactants among those compounds with the highest signal intensities in sludge. Principal component analysis and hierarchical clustering showed that spatial distribution of contaminants across Switzerland was not homogeneous, while Pearson correlation indicated that changes can be attributed to different anaerobic digestion times in WWTPs.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"36 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798196","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}
Teng Wang, Dongxiang Liu, Rongze Liu, Feng Yuan, Yongcheng Ding, Jianguo Tao, Yaping Wang, Wenwen Yu, Yining Fang, Baojie Li
Coastal wetlands function as critical retention zones for environmental microplastics, potentially accelerating their degradation through unique hydrological conditions. This study conducted a comprehensive 24-month in situ experiment at the Chongming Dongtan National Nature Reserve, examining the weathering processes of five morphologically distinct polyethylene (PE), polypropylene (PP), and polystyrene (PS) microplastics. Quarterly analyses revealed progressive surface deterioration in all microplastics after initial exposure, followed by polymer-specific fragmentation patterns and environmental pollutant adherence. Surface elemental analysis showed rising O/C ratios, with intertidal zones exhibiting higher variance (0.0014–0.0096 vs 0.0006–0.0028 supratidal). Carbonyl index (CI) displayed fluctuating increases, with PS showing the highest CI rise (75.75%/year intertidal vs 61.77%/year supratidal). Systematic comparisons identified three weathering determinants: enhanced intertidal degradation from mechanical-photochemical synergy; spherical particles degrading faster than films via larger surface area; and polymer vulnerabilities dictating PS > PP > PE degradation rates. These findings demonstrate that microplastic weathering in coastal wetlands is collectively governed by hydrological conditions, particle morphology, and polymer composition, providing crucial quantitative parameters for assessing environmental persistence and ecological risks in these sensitive transition ecosystems.
{"title":"Weathering Process and Characteristics of Microplastics in Coastal Wetlands: A 24-Month In Situ Study","authors":"Teng Wang, Dongxiang Liu, Rongze Liu, Feng Yuan, Yongcheng Ding, Jianguo Tao, Yaping Wang, Wenwen Yu, Yining Fang, Baojie Li","doi":"10.1021/acs.est.4c12140","DOIUrl":"https://doi.org/10.1021/acs.est.4c12140","url":null,"abstract":"Coastal wetlands function as critical retention zones for environmental microplastics, potentially accelerating their degradation through unique hydrological conditions. This study conducted a comprehensive 24-month in situ experiment at the Chongming Dongtan National Nature Reserve, examining the weathering processes of five morphologically distinct polyethylene (PE), polypropylene (PP), and polystyrene (PS) microplastics. Quarterly analyses revealed progressive surface deterioration in all microplastics after initial exposure, followed by polymer-specific fragmentation patterns and environmental pollutant adherence. Surface elemental analysis showed rising O/C ratios, with intertidal zones exhibiting higher variance (0.0014–0.0096 vs 0.0006–0.0028 supratidal). Carbonyl index (CI) displayed fluctuating increases, with PS showing the highest CI rise (75.75%/year intertidal vs 61.77%/year supratidal). Systematic comparisons identified three weathering determinants: enhanced intertidal degradation from mechanical-photochemical synergy; spherical particles degrading faster than films via larger surface area; and polymer vulnerabilities dictating PS > PP > PE degradation rates. These findings demonstrate that microplastic weathering in coastal wetlands is collectively governed by hydrological conditions, particle morphology, and polymer composition, providing crucial quantitative parameters for assessing environmental persistence and ecological risks in these sensitive transition ecosystems.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"13 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806046","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}
Pranav Nair, Jianxian Sun, Linna Xie, Lisa Kennedy, Derek Kozakiewicz, Sonya M. Kleywegt, Chunyan Hao, Hannah Byun, Holly Barrett, Joshua Baker, Joseph Monaghan, Erik T. Krogh, Datong Song, Hui Peng
N-(1,3-Dimethylbutyl)-N′-phenyl-p-phenylenediamine-quinone (6PPD-Q), the tire rubber-derived transformation product of 6PPD, was recently discovered to cause the acute mortality of coho salmon (Oncorhynchus kisutch). Aiming to identify potential replacement antiozonants for 6PPD that do not produce toxic quinones, seven PPD-quinones with distinct side chains were synthesized to investigate their structure-related toxicities in vivo using rainbow trout (Oncorhynchus mykiss). While 6PPD-Q exerted high toxicity (96 h LC50 = 0.35 μg/L), toxicity was not observed for six other PPD-quinones despite their similar structures. The fish tissue concentrations of 6PPD-Q after sublethal exposure (0.29 μg/L) were comparable to the other PPD-quinones, which indicated that bioaccumulation levels were not the reason for the selective toxicity of 6PPD-Q. Hydroxylated PPD-quinones were detected as the predominant metabolites in fish tissue. Interestingly, a single major aromatic hydroxylation metabolite was detected for the alternate PPD-quinones, but two abundant OH-6PPD-Q isomers were detected for 6PPD-Q. MS2 spectra confirmed that hydroxylation occurred on the alkyl side chain for one isomer. The structurally selective toxicity of 6PPD-Q was also observed in a coho salmon (CSE-119) cell line, which further supports its intrinsic toxicity. This study reported the selective toxicity of 6PPD-Q and pinpointed the possibility for other PPDs to be applied as potential substitutes of 6PPD.
{"title":"Synthesis and Toxicity Evaluation of p-Phenylenediamine-Quinones","authors":"Pranav Nair, Jianxian Sun, Linna Xie, Lisa Kennedy, Derek Kozakiewicz, Sonya M. Kleywegt, Chunyan Hao, Hannah Byun, Holly Barrett, Joshua Baker, Joseph Monaghan, Erik T. Krogh, Datong Song, Hui Peng","doi":"10.1021/acs.est.4c12220","DOIUrl":"https://doi.org/10.1021/acs.est.4c12220","url":null,"abstract":"<i>N</i>-(1,3-Dimethylbutyl)-<i>N′</i>-phenyl-<i>p</i>-phenylenediamine-quinone (6PPD-Q), the tire rubber-derived transformation product of 6PPD, was recently discovered to cause the acute mortality of coho salmon (<i>Oncorhynchus kisutch</i>). Aiming to identify potential replacement antiozonants for 6PPD that do not produce toxic quinones, seven PPD-quinones with distinct side chains were synthesized to investigate their structure-related toxicities <i>in vivo</i> using rainbow trout (<i>Oncorhynchus mykiss</i>). While 6PPD-Q exerted high toxicity (96 h LC<sub>50</sub> = 0.35 μg/L), toxicity was not observed for six other PPD-quinones despite their similar structures. The fish tissue concentrations of 6PPD-Q after sublethal exposure (0.29 μg/L) were comparable to the other PPD-quinones, which indicated that bioaccumulation levels were not the reason for the selective toxicity of 6PPD-Q. Hydroxylated PPD-quinones were detected as the predominant metabolites in fish tissue. Interestingly, a single major aromatic hydroxylation metabolite was detected for the alternate PPD-quinones, but two abundant OH-6PPD-Q isomers were detected for 6PPD-Q. MS<sup>2</sup> spectra confirmed that hydroxylation occurred on the alkyl side chain for one isomer. The structurally selective toxicity of 6PPD-Q was also observed in a coho salmon (CSE-119) cell line, which further supports its intrinsic toxicity. This study reported the selective toxicity of 6PPD-Q and pinpointed the possibility for other PPDs to be applied as potential substitutes of 6PPD.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"38 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798194","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}
Pub Date : 2025-04-08DOI: 10.1021/acs.est.5c0369610.1021/acs.est.5c03696
Julie Beth Zimmerman*, Gregory Lowry, Fernando Rosario-Ortiz, Paul Westerhoff, Daniel Alessi, Pedro Alvarez, Alexandra Boehm, Ian Cousins, Jordi Dachs, Matthew Eckelman, Imad El Haddad, Pablo Gago-Ferrero, Jorge Gardea-Torresdey, Jacqueline MacDonald Gibson, Keri Hornbuckle, Heileen Hsu-Kim, Juliane Hollender, Atsuko Ikeda, Frederic Leusch, Melissa Maurer-Jones, James Mihelcic, Shelly Miller, Lutgarde Raskin, Z. Jason Ren, Susan Richardson, Daniel Schlenk, Huahong Shi, Paul Tratnyek, David Waite, Shuxiao Wang, Zhanyun Wang, Michael Wong and Sukhwan Yoon,
Jian Sun, Zezhuang Liu, Fan Xia, Yilu Gu, Xiaofeng Gao, Sha Lu, Yang Xu, Feidan Meng, Qian Zhang, Tao Zhou
Rapid urbanization in China has exacerbated the urban heat island (UHI) effect, posing considerable challenges to urban sustainability and public health. Most UHI studies have focused on the impacts of two-dimensional (2D) urbanization, which involves outward city expansion and increased built-up area. However, as cities mature, they typically transition from horizontal expansion to vertical densification (3D urbanization), leading to increased material stock density. The implications of this shift for the UHI effect remain underexplored. This study compared the 2D and 3D urbanization–induced impacts on UHI across 384 Chinese cities from 2000 to 2020, using impervious surface and gridded material stocks. Our results surprisingly indicated that 2D urbanization lost explanatory power of the UHI intensity when the impervious surface area percentage exceeded 87%. Relative importance analysis utilizing a random forest algorithm revealed that the population, vegetation abundance, and precipitation significantly moderated the effects of 3D urbanization, emphasizing the crucial role of urban green spaces in mitigating thermal stress. This study examined the spatiotemporal dynamics of the UHI effect in China, emphasizing the key role of 3D urbanization. Our findings highlight the urgent need to incorporate 3D urbanization characteristics when devising UHI mitigation strategies.
{"title":"Uncovering the Impacts of 2D and 3D Urbanization on Urban Heat Islands in 384 Chinese Cities","authors":"Jian Sun, Zezhuang Liu, Fan Xia, Yilu Gu, Xiaofeng Gao, Sha Lu, Yang Xu, Feidan Meng, Qian Zhang, Tao Zhou","doi":"10.1021/acs.est.4c12689","DOIUrl":"https://doi.org/10.1021/acs.est.4c12689","url":null,"abstract":"Rapid urbanization in China has exacerbated the urban heat island (UHI) effect, posing considerable challenges to urban sustainability and public health. Most UHI studies have focused on the impacts of two-dimensional (2D) urbanization, which involves outward city expansion and increased built-up area. However, as cities mature, they typically transition from horizontal expansion to vertical densification (3D urbanization), leading to increased material stock density. The implications of this shift for the UHI effect remain underexplored. This study compared the 2D and 3D urbanization–induced impacts on UHI across 384 Chinese cities from 2000 to 2020, using impervious surface and gridded material stocks. Our results surprisingly indicated that 2D urbanization lost explanatory power of the UHI intensity when the impervious surface area percentage exceeded 87%. Relative importance analysis utilizing a random forest algorithm revealed that the population, vegetation abundance, and precipitation significantly moderated the effects of 3D urbanization, emphasizing the crucial role of urban green spaces in mitigating thermal stress. This study examined the spatiotemporal dynamics of the UHI effect in China, emphasizing the key role of 3D urbanization. Our findings highlight the urgent need to incorporate 3D urbanization characteristics when devising UHI mitigation strategies.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"108 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789701","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}
Jingyang Song, Xiaoke Su, Lijing Hou, Chunli Chu, Tongyuan Wu, Hancheng Dai, Yang Ou, Osamu Nishiura, Zhi Cao, Meiting Ju
In the global effort to mitigate climate change, the cement sector remains highly emission-intensive and hard-to-decarbonize. Previous research has highlighted material efficiency strategies─including more intensive use, lifetime extension, material-efficient design, and end-of-life processes, as demand-side options for reducing emissions. However, unintended effects and supply side responses, such as shifts in technological portfolios and investment trends, remain underexplored. This study develops a framework that couples detailed stock-flow modeling and a bottom-up energy system optimization model, a subcategory of integrated assessment models. Taking China’s cement sector as a pilot case, our framework projects comprehensive decarbonization pathways for cement-based materials. The results show that material efficiency strategies could reduce cement demand by 57%, significantly decreasing reliance on supply side technologies required for net-zero emissions, with these strategies contributing nearly 50% of the cumulative decarbonization effort. The material efficiency strategies also reduce the incremental total production costs associated with low-carbon technologies in upstream sectors. When combined with CO2 uptake from cement-based materials, this study offers a cost-effective pathway for achieving net-zero emissions in the cement sector, lowering both costs and CO2 emissions without heavy dependence on carbon capture and storage.
{"title":"Integrating Stock-Flow Modeling and Energy System Optimization to Explore Decarbonization Pathways for China’s Cement Industry","authors":"Jingyang Song, Xiaoke Su, Lijing Hou, Chunli Chu, Tongyuan Wu, Hancheng Dai, Yang Ou, Osamu Nishiura, Zhi Cao, Meiting Ju","doi":"10.1021/acs.est.4c14724","DOIUrl":"https://doi.org/10.1021/acs.est.4c14724","url":null,"abstract":"In the global effort to mitigate climate change, the cement sector remains highly emission-intensive and hard-to-decarbonize. Previous research has highlighted material efficiency strategies─including more intensive use, lifetime extension, material-efficient design, and end-of-life processes, as demand-side options for reducing emissions. However, unintended effects and supply side responses, such as shifts in technological portfolios and investment trends, remain underexplored. This study develops a framework that couples detailed stock-flow modeling and a bottom-up energy system optimization model, a subcategory of integrated assessment models. Taking China’s cement sector as a pilot case, our framework projects comprehensive decarbonization pathways for cement-based materials. The results show that material efficiency strategies could reduce cement demand by 57%, significantly decreasing reliance on supply side technologies required for net-zero emissions, with these strategies contributing nearly 50% of the cumulative decarbonization effort. The material efficiency strategies also reduce the incremental total production costs associated with low-carbon technologies in upstream sectors. When combined with CO<sub>2</sub> uptake from cement-based materials, this study offers a cost-effective pathway for achieving net-zero emissions in the cement sector, lowering both costs and CO<sub>2</sub> emissions without heavy dependence on carbon capture and storage.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"89 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789703","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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