IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-09-25 DOI: 10.1021/acs.est.5c03525

Yiling Xiong, Fang Wang, Peter Holzapfel, Matthias Finkbeiner, Ye Wu, Shaojun Zhang

{"title":"Well-to-Gate Greenhouse Gas Emissions of Petrochemical Products across the Supply Chain and Sources of Variability in China","authors":"Yiling Xiong, Fang Wang, Peter Holzapfel, Matthias Finkbeiner, Ye Wu, Shaojun Zhang","doi":"10.1021/acs.est.5c03525","DOIUrl":"https://doi.org/10.1021/acs.est.5c03525","url":null,"abstract":"The carbon-intensive petrochemical sector plays a critical role in numerous industrial supply chains. However, existing databases lack comprehensive carbon footprint profiles for petroleum products, hindering reliable assessments of greenhouse gas (GHG) emissions associated with derived chemicals and various downstream products. This study developed a quantification method that converts the material flows of oil refineries into input–output coefficient matrices using actual plant data, which further refined process-specific GHG emission estimates and identified key sources of variability across the full spectrum of petroleum products. The results show that inconsistent allocation methods lead to 40%–80% of the variation in emission estimates, while data uncertainty has a moderate influence. Configuration heterogeneity also affects GHG assessments by altering the process mix and upstream processes─specifically, a lower proportion of straight-run oil and deeper processing of heavier fractions result in higher emissions. Additionally, the aggregation of oil-based intermediates as chemical feedstocks introduces an uncertainty range of −19% to +44% in assessing the GHG emissions of major chemicals. This underscores the importance of comprehensive GHG emission profiles and variability analysis of petroleum products in advancing reliable emission assessments and decarbonization strategies for the petrochemical industry.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"18 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140906","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Human Internal Exposures of Bisphenol A and Six Data-Poor Analogs Predicted by Physiologically Based Kinetic Models with Multimodal Parametrization 基于多模态参数化的生理动力学模型预测双酚A和六种数据贫乏的类似物的人体内部暴露

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-09-25 DOI: 10.1021/acs.est.5c00513

Hélène Bigonne, Amrei Rolof, Inga Potapova, Shana J. Sturla, Georg Aichinger

{"title":"Human Internal Exposures of Bisphenol A and Six Data-Poor Analogs Predicted by Physiologically Based Kinetic Models with Multimodal Parametrization","authors":"Hélène Bigonne, Amrei Rolof, Inga Potapova, Shana J. Sturla, Georg Aichinger","doi":"10.1021/acs.est.5c00513","DOIUrl":"https://doi.org/10.1021/acs.est.5c00513","url":null,"abstract":"Bisphenols (BP) AF, B, E, F, M, and S are increasingly used as bisphenol A (BPA) substitutes. Despite widespread exposure and potential adverse health outcomes, they are poorly understood in terms of toxicokinetics, i.e., their absorption, distribution, metabolism, and excretion. We thus developed physiologically based kinetic models for different human physiological standards to predict internal concentrations of prevalent bisphenols following oral exposure. To address the imbalances in available human data among these chemicals, we used multimodal parametrization methods, including in vitro measurements of metabolism, computational prediction of gastrointestinal absorption, and rat–human extrapolation of enterohepatic circulation. Then, the models were evaluated against available human toxicokinetic data for BPA and BPS, revealing that 66% of predicted Cmax, tmax, and AUC values fell within a 2-fold difference from in vivo measures. Using environmentally relevant exposure levels to compare internal levels of all tested bisphenols, we observed significant differences in the toxicokinetic profiles. Concerning tissues of toxicological concern, BPS had the highest concentration in blood and testes, while BPM accumulated in the thyroid and BPAF in the breasts. The present models are expected to facilitate a more precise evaluation of health risks induced by BPA analogs, guiding their safer use.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"11 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145133455","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Examining the Compositional Selectivity of Hydrocarbon Oxidation Products Using Liquid–Liquid Extraction and Solid-Phase Extraction Techniques 采用液-液萃取和固相萃取技术研究烃类氧化产物的组分选择性

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-09-25 DOI: 10.1021/acs.est.5c07016

Phoebe Zito, Rana Ghannam, Maxwell L. Harsha, Barbara A. Bekins, David C. Podgorski

{"title":"Examining the Compositional Selectivity of Hydrocarbon Oxidation Products Using Liquid–Liquid Extraction and Solid-Phase Extraction Techniques","authors":"Phoebe Zito, Rana Ghannam, Maxwell L. Harsha, Barbara A. Bekins, David C. Podgorski","doi":"10.1021/acs.est.5c07016","DOIUrl":"https://doi.org/10.1021/acs.est.5c07016","url":null,"abstract":"The effect of extraction methods on detecting hydrocarbon oxidation products (HOPs) in groundwater remains unclear. HOPs are polar, water-soluble byproducts of petroleum biodegradation. Our previous work showed that liquid–liquid extraction (LLE), a method commonly used in regulatory monitoring, has a significantly lower extraction efficiency for HOPs compared to solid-phase extraction (SPE). In this study, we evaluate the analytical limitations and compositional selectivity of LLE and SPE using groundwater samples from the Bemidji, MN, crude oil spill site. Optical properties were characterized using excitation–emission matrix spectroscopy (EEMs), and a three-component PARAFAC model was validated, showing consistent trends across both extracts and whole water samples. Ultrahigh-resolution mass spectrometry (UHR-MS) revealed that LLE selectively recovered aliphatic-like compounds but underrepresented more polar oxygenated HOPs. In contrast, SPE methods were more effective at isolating highly oxidized compound classes. These differences were consistent across a gradient of contamination. Overall, the LLE was less precise and less representative of polar HOPs, introducing bias in the characterization of HOPs. This study is the first to quantitatively demonstrate the compositional selectivity and analytical bias of LLE versus SPE for HOPs using combined EEM-PARAFAC and UHR-MS techniques, with implications for long-term monitoring and site assessment protocols.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"18 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140911","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Climate Warming Increases Nitrate Export in High-Elevation Rivers: Divergent Temperature and Hydrological Controls across Basins 气候变暖增加了高海拔河流的硝酸盐出口：不同流域的温度和水文控制

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-09-25 DOI: 10.1021/acs.est.5c08510

Cai Li, Sen Xu, Fu-Jun Yue, Jun Zhong, Zhong-Jun Wang, Shuai Chen, Si-Liang Li

{"title":"Climate Warming Increases Nitrate Export in High-Elevation Rivers: Divergent Temperature and Hydrological Controls across Basins","authors":"Cai Li, Sen Xu, Fu-Jun Yue, Jun Zhong, Zhong-Jun Wang, Shuai Chen, Si-Liang Li","doi":"10.1021/acs.est.5c08510","DOIUrl":"https://doi.org/10.1021/acs.est.5c08510","url":null,"abstract":"The response of fluvial nitrate (NO3–) export to climate warming remains poorly constrained in high-elevation basins. Here, we integrate multi-decadal NO3– flux records with multi-year measurements of NO3– concentrations and dual-isotope signatures (δ15N–NO3– and δ18O–NO3–) from two contrasting rivers on the Qinghai–Tibetan Plateau, the permafrost-rich Jinsha River (JSR) and the permafrost-scarce Yalong River (YLR), to evaluate climate-driven shifts in NO3– dynamics. In the JSR, where sustained warming has driven widespread permafrost thaw, NO3– concentrations and fluxes increased by ∼190 and ∼220%, respectively, from 1993 to 2018. In contrast, the NO3– export in the YLR was primarily controlled by hydrological variability rather than temperature. In-soil nitrification is the dominant source of fluvial NO3–, with warming-enhanced nitrification emerging as the primary driver of increased NO3– flux, while runoff plays a minor role. Using the space-for-time substitution method, we infer that ongoing permafrost degradation may shift NO3– export from warming-driven to hydrology-driven controls. This transition is expected to enhance nitrogen leaching under warming and intensified precipitation, contributing to nitrogen limitation in high-elevation vegetation and weakening of CO2 uptake. These findings reveal a previously underappreciated climate-warming nitrogen–carbon feedback with implications for Earth system models in permafrost-affected regions.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"22 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140917","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Multiscale Regulation of Rhizosphere Microorganisms on the Spatiotemporal Variation of Soil Amino Acid Nitrogen During Plant Succession: A Case Study from the Desert Riparian Ecosystem 植物演替过程中根际微生物对土壤氨基酸氮时空变化的多尺度调控——以荒漠河岸生态系统为例

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-09-25 DOI: 10.1021/acs.est.5c06468

Wenyan Duan, Xiaojuan Yu, Xin Li, Chantal Hamel, Jie Yan, Ruonan Jing, Shuo Zhang, Xin Zhao, Jiaqi He, Ruiyang Guan, Nuo Yang, Min Sheng

{"title":"Multiscale Regulation of Rhizosphere Microorganisms on the Spatiotemporal Variation of Soil Amino Acid Nitrogen During Plant Succession: A Case Study from the Desert Riparian Ecosystem","authors":"Wenyan Duan, Xiaojuan Yu, Xin Li, Chantal Hamel, Jie Yan, Ruonan Jing, Shuo Zhang, Xin Zhao, Jiaqi He, Ruiyang Guan, Nuo Yang, Min Sheng","doi":"10.1021/acs.est.5c06468","DOIUrl":"https://doi.org/10.1021/acs.est.5c06468","url":null,"abstract":"Riparian zones in deserts are critical for water purification, habitat, and soil conservation, but most studies focus on vegetation zones without long-term monitoring, hindering the comprehensive assessment of their long-term benefits. This study on Yuangeda Lake in northwestern China’s desert used spatiotemporal substitution to convert soil spatial heterogeneity into a temporal gradient, analyzing soil properties across vegetation zones formed by lake expansion and microbial impacts on amino acid nitrogen. Results showed that rhizosphere soil amino acid nitrogen was higher in grass (Agropyron cristatum L. Gaertn.) and grass/shrub mixed (A. cristatum and Artemisia desertorum Spreng.) areas than in shrub areas (A. desertorum). As plant communities persisted, a distinct threshold in rhizosphere soil amino acid nitrogen emerged at approximately 11 years. Rhizosphere bacterial and fungal specific taxonomic units, microbial co-occurrence network topologies, and amino acid nitrogen-related bacterial functions differed between grass/grass-shrub-mixed and shrub areas, linked to plant community duration. Bacteria dominated amino acid nitrogen formation in grass areas, while bacteria and fungi contributed in the grass/shrub mixed area. Overall, water inflow promoted soil amino acid nitrogen accumulation, with microbial contributions varying by plant community duration. This study supports desert riparian soil restoration and management, advancing our understanding of amino acid nitrogen in the nitrogen cycle.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"2 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145133458","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

In-Sample Chemical Tracers for Quality Control in Environmental Samples: A Systematic Evaluation of Deuterated Pharmaceuticals for Sampling Campaigns. 用于环境样品质量控制的样品内化学示踪剂：用于采样活动的氘化药物的系统评价。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-09-24 DOI: 10.1021/acs.est.5c05862

Jianan Ren,Qiuda Zheng,Jiaying Li,Rory Verhagen,Phong K Thai,Jiuling Li,Jochen F Mueller,Ben J Tscharke

{"title":"In-Sample Chemical Tracers for Quality Control in Environmental Samples: A Systematic Evaluation of Deuterated Pharmaceuticals for Sampling Campaigns.","authors":"Jianan Ren,Qiuda Zheng,Jiaying Li,Rory Verhagen,Phong K Thai,Jiuling Li,Jochen F Mueller,Ben J Tscharke","doi":"10.1021/acs.est.5c05862","DOIUrl":"https://doi.org/10.1021/acs.est.5c05862","url":null,"abstract":"Understanding the integrity of water samples between collection and analysis is essential for the delivery of high-quality data. In this study, we evaluated the spiking of isotopically labeled chemicals into environmental samples postsampling as indicators of sample integrity. Our approach compared the ratio of unstable tracers (those sensitive to poor storage conditions or the matrix) to stable tracers (those insensitive to these factors) in samples to track sample integrity. We systematically evaluated 18 deuterium-labeled pharmaceuticals for this purpose in wastewater samples, classifying them into varying stability levels from highly stable to very unstable. Stability was determined under varying temperatures (37 °C, 20 °C, 4 °C, and -20 °C) for up to 84 days and using common preservation techniques (hydrochloric acid: HCl, sodium metabisulfite: SMS, and untreated). Based on our proposed selection criteria, of the 18 investigated, one was found suitable as an unstable tracer and 6 as stable tracers in acidified wastewater, while 3 unstable and 2 stable tracers were suitable for SMS-preserved wastewater and 4 unstable and 2 stable tracers when no preservatives are required. This study provides the first assessment of chemical tracers to measure the sample integrity for environmental sampling campaigns.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"40 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145127266","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Evaluating and Improving Light Absorption Retrievals of Black Carbon Using In Situ Polar Nephelometry 利用原位极化浊度法评价和改进黑碳的光吸收反演

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-09-24 DOI: 10.1021/acs.est.5c05919

Qizhi Xu, Barbara Bertozzi, Robin Lewis Modini, Benjamin Tobias Brem, Thomas Müller, Baseerat Romshoo, Claudia Mohr, Martin Gysel-Beer

{"title":"Evaluating and Improving Light Absorption Retrievals of Black Carbon Using In Situ Polar Nephelometry","authors":"Qizhi Xu, Barbara Bertozzi, Robin Lewis Modini, Benjamin Tobias Brem, Thomas Müller, Baseerat Romshoo, Claudia Mohr, Martin Gysel-Beer","doi":"10.1021/acs.est.5c05919","DOIUrl":"https://doi.org/10.1021/acs.est.5c05919","url":null,"abstract":"Black carbon (BC) is among the major contributors to global warming, yet significant uncertainties exist in remote sensing retrievals of BC light absorption. A key issue is the mismatch between the simplified spherical morphology assumption commonly used in these retrievals and the actual fractal-like morphology of BC particles. In situ polar nephelometry provides a unique opportunity to improve these retrieval algorithms. Laboratory-based polarimetric measurements allow for a comparison of retrieved and directly measured properties using independent instrumentation. In our experiments, bare BC aggregates were generated, and phase functions were measured using our newly developed polar nephelometer uNeph. Standard retrievals based on Lorenz-Mie theory poorly reproduced the phase function and polarized phase function of BC, leading to significant bias in retrieved properties beyond the uncertainty of independent measurements. Contrary to previous studies, we demonstrate a good closure between measured and simulated phase functions when using the Multi-Sphere T-Matrix (MSTM) method for BC aggregates in the accumulation size range. BC properties, particularly absorption coefficient and volume concentration, were accurately and precisely retrieved by accounting for the fractal-like morphology. Only two additional parameters were used in MSTM retrieval. This suggests that considering aggregates in remote sensing retrievals under real atmospheric conditions could be feasible.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"15 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145133506","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Comparison of Halophenol, Halonitrophenol, and Halosalicylic Acid Formation vs 1-2 Carbon DBP Formation during Chlorination and Chloramination of Surface Waters. 地表水氯化和氯胺化过程中卤代酚、卤代硝基酚和卤代水杨酸生成与1-2碳DBP生成的比较

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-09-24 DOI: 10.1021/acs.est.5c09818

Jiarui Han,Sungeun Lim,Vincent T DiPietri,Benjamin Najm,Xiangru Zhang,William A Mitch

{"title":"Comparison of Halophenol, Halonitrophenol, and Halosalicylic Acid Formation vs 1-2 Carbon DBP Formation during Chlorination and Chloramination of Surface Waters.","authors":"Jiarui Han,Sungeun Lim,Vincent T DiPietri,Benjamin Najm,Xiangru Zhang,William A Mitch","doi":"10.1021/acs.est.5c09818","DOIUrl":"https://doi.org/10.1021/acs.est.5c09818","url":null,"abstract":"Although haloaromatic disinfection byproducts (DBPs) are considered an important component of nonvolatile, high molecular weight DBPs, little research has compared haloaromatic DBP formation to the conventional 1-2 carbon DBPs during chlorination or chloramination of authentic surface waters. This study compared the concentrations of 15 halophenols, 5 halonitrophenols, and 8 halosalicylic acids to 28 1-2 carbon DBPs in samples collected in two rivers upstream and downstream of wastewater impacts, in a municipal wastewater effluent, and in five algal-impacted reservoirs treated with chlorine alone or chlorine for 1 h followed by chloramination. Halophenols and halosalicylic acids reached ∼10-600 ng/L within 2-12 h during chlorination. Halophenols degraded faster than halosalicylic acids thereafter, and ∼10-30 ng/L halosalicylic acids remained after 5 d. During chlorination/chloramination, both halophenols and halosalicylic acids remained near the levels formed during the first 1 h of chlorine contact. Halonitrophenols formed at ∼10-140 ng/L but were stable during chlorination and chlorination/chloramination. In contrast, 1-2 carbon DBPs formed at ∼50-820 μg/L, accumulating during chlorination but remaining at levels formed during the initial 1 h chlorine contact during chlorination/chloramination. The organic matter in the river samples was more potent at producing aromatic DBPs than the algal-impacted organic matter. Although the trends in halosalicylic acid concentrations during chlorination were consistent with previous observations of overall cytotoxicity, these specific haloaromatic DBPs contributed substantially less to cytotoxicity than the 1-2 carbon DBPs.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"10 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145127267","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Perfluorooctanoic Acid Can Increase Biofilm Resilience and Virulence in Drinking Water Distribution Systems. 全氟辛酸可以增加饮用水分配系统中生物膜的弹性和毒力。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-09-24 DOI: 10.1021/acs.est.5c07943

Haibo Wang,Yukang Li,Hui Chen,Pingfeng Yu,Baoyou Shi,Pedro J J Alvarez

{"title":"Perfluorooctanoic Acid Can Increase Biofilm Resilience and Virulence in Drinking Water Distribution Systems.","authors":"Haibo Wang,Yukang Li,Hui Chen,Pingfeng Yu,Baoyou Shi,Pedro J J Alvarez","doi":"10.1021/acs.est.5c07943","DOIUrl":"https://doi.org/10.1021/acs.est.5c07943","url":null,"abstract":"Despite the prevalence of perfluorooctanoic acid (PFOA) in drinking water distribution systems (DWDSs), its effects on biofilm formation and tolerance to residual disinfectants remain largely unknown. Here, we report that DWDS-relevant levels of PFOA (1-80 ng/L) promoted Pseudomonas aeruginosa biofilm formation (by 1.8- to 4.5-fold) and chlorine tolerance (by 7-22%). PFOA also enhanced biofilm tolerance to common antibiotics, increasing their minimum inhibitory concentrations by 25-67%. In a flow-through system, biofilm evolution toward higher resilience was attributed to PFOA-exerted oxidative stress, which fortuitously upregulated quorum sensing and stimulated extracellular polymeric substances production. PFOA exposure also increased bacterial chemotaxis and activated cyaA and cyaB genes, which enhanced the cAMP/Vfr signaling pathway, contributing to the upregulation of virulence factor genes. PFOA-induced chlorine and antibiotic resistance and increased virulence were also verified with a mesocosm system and a real DWDS pipeline biofilm. Overall, these results underscore the need for proactive microbial risk assessment associated with such indirect effects of emerging pollutants in DWDSs.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"1 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145127240","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Revisiting the Role of Tertiary Amines in Enhancing Aqueous Chlorination of Phenolic Compounds: Kinetic Modeling and Reaction Mechanisms. 叔胺在促进酚类化合物氯化反应中的作用：动力学模型和反应机理。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-09-24 DOI: 10.1021/acs.est.5c06728

Linke Jiang,Shuiqin Shi,Yuhang Li,Jiahui Hu,Junmei Yan,Xin Yu,Mingbao Feng

{"title":"Revisiting the Role of Tertiary Amines in Enhancing Aqueous Chlorination of Phenolic Compounds: Kinetic Modeling and Reaction Mechanisms.","authors":"Linke Jiang,Shuiqin Shi,Yuhang Li,Jiahui Hu,Junmei Yan,Xin Yu,Mingbao Feng","doi":"10.1021/acs.est.5c06728","DOIUrl":"https://doi.org/10.1021/acs.est.5c06728","url":null,"abstract":"Tertiary amines in dissolved organic nitrogen have been implicated for decades in mediating organic chlorination through the formation of reactive quaternary ammonium intermediates (R3N+-Cl), yet the mechanistic underpinnings of this process remain poorly understood. This study presents the first systematic investigation of structure-activity relationships (SARs) governing tertiary amine-enhanced chlorination using phenolic compounds as representative substrates. Through advanced kinetic analyses, we demonstrate that catalytic chlorination efficiency correlates directly with the Brønsted-Lowry basicity of tertiary amines, mechanistically linked to the stabilization of R3N+-Cl species. A MATLAB-based approach coupled with Kintecus modeling was used to quantify the R3N+-Cl reactivity with phenolics (2.86 × 104-2.29 × 105 M-1 s-1), previously uncharted kinetic parameters critical for predictive water treatment modeling. Environmental relevance was indicated through matrix interference studies, showing ∼10% reduction in phenol removal efficiency by Fe3+ or humic acid in the chlorine/trimethylamine system. Product analysis revealed conserved chlorination pathways without new byproduct formation, while the chlorinated bisphenol derivatives exhibited moderate-to-high endocrine-disrupting activity. This work fundamentally advances our understanding of amine-mediated chlorination mechanisms by revealing critical water quality implications through combined kinetic and toxicological assessments. The findings provide essential mechanistic insights for optimizing chlorination processes in tertiary amine-containing waters while highlighting previously underestimated risks from accelerated formation of bioactive chlorinated compounds.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"80 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145127241","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

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