环境科学与技术最新文献

{"title":"Dynamic Surface Incorporation of Pb²⁺ Ions at the Actively Dissolving Calcite (104) Surface.","authors":"Bektur Abdilla, Sang Soo Lee, Paul Fenter, Neil C Sturchio","doi":"10.1021/acs.est.4c03567","DOIUrl":"10.1021/acs.est.4c03567","url":null,"abstract":"<p><p>The reaction of dissolved Pb²⁺ with calcite surfaces at near-equilibrium conditions involves adsorption of Pb²⁺ and precipitation of secondary heteroepitaxial Pb-carbonate minerals. A more complex behavior is observed under far-from-equilibrium conditions, including strong inhibition of calcite dissolution, development of microtopography, and near-surface incorporation of multiple monolayers (ML) of Pb²⁺ without precipitation of secondary phases [where 1 ML ≡ 1 Ca/20.2 Ų, the crystallographic site density of the calcite (104) lattice plane]. However, the mechanistic controls governing far-from-equilibrium reactivity are not well understood. Here, we observe the interfacial incorporation of dissolved Pb²⁺ during the dissolution of calcite (104) surfaces at pH ∼ 3.7 in a flow-through reaction cell, revealing the formation of a ∼1 nm thick Pb-rich calcite layer with a total Pb coverage of ∼1.4 ML. These observations of the sorbed Pb distribution used resonant anomalous X-ray reflectivity, X-ray fluorescence, and nanoinfrared atomic force microscopy. We propose that this altered surface layer represents a novel sorption mode that is stabilized by conditions of sustained disequilibrium. This behavior may significantly impact the transport of dissolved metals during disequilibrium processes occurring in acid mine drainage and subsurface CO₂ injection and, if appropriately accounted for, could improve the predictive capability of geochemical reactive-transport models.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142131157","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}

{"title":"Impacts on Atlantic Killifish from Neurotoxicants: Genes, Behavior, and Population-Relevant Outcomes","authors":"Janice L. Albers, Lori N. Ivan, Bryan W. Clark, Diane E. Nacci, Rebekah H. Klingler, Adam Thrash, Juan P. Steibel, Natalia Garcia-Reyero Vinas, Michael J. Carvan, Cheryl A. Murphy","doi":"10.1021/acs.est.4c04207","DOIUrl":"https://doi.org/10.1021/acs.est.4c04207","url":null,"abstract":"Molecular, cellular, and organismal alterations are important descriptors of toxic effects, but our ability to extrapolate and predict ecological risks is limited by the availability of studies that link measurable end points to adverse population relevant outcomes such as cohort survival and growth. In this study, we used laboratory gene expression and behavior data from two populations of Atlantic killifish <i>Fundulus heteroclitus</i> [one reference site (SCOKF) and one PCB-contaminated site (NBHKF)] to inform individual-based models simulating cohort growth and survival from embryonic exposures to environmentally relevant concentrations of neurotoxicants. Methylmercury exposed SCOKF exhibited brain gene expression changes in the si:ch211–186j3.6, si:dkey-21c1.4, scamp1, and klhl6 genes, which coincided with changes in feeding and swimming behaviors, but our models simulated no growth or survival effects of exposures. PCB126-exposed SCOKF had lower physical activity levels coinciding with a general upregulation in nucleic and cellular brain gene sets (BGS) and downregulation in signaling, nucleic, and cellular BGS. The NBHKF, known to be tolerant to PCBs, had altered swimming behaviors that coincided with 98% fewer altered BGS. Our models simulated PCB126 decreased growth in SCOKF and survival in SCOKF and NBHKF. Overall, our study provides a unique demonstration linking molecular and behavioral data to develop quantitative, testable predictions of ecological risk.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142235532","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}

{"title":"Crystal Water in Minerals Modulates Oxygen Activation for Hydrogen Peroxide Photosynthesis.","authors":"Chao Xing, Yunjie Zou, Mingkai Xu, Lan Ling","doi":"10.1021/acs.est.4c04691","DOIUrl":"10.1021/acs.est.4c04691","url":null,"abstract":"<p><p>Sunlight-responsive minerals contribute significantly to biogeochemical cycles by activating oxygen (O₂) to generate reactive oxygen species (ROS). However, the role of crystal water, incorporated into minerals through hydration during rock cycles, in O₂ activation remains largely unexplored. Here, we construct tungstite models containing oxygen vacancies to elucidate the modulation of mineral-based ROS dynamics by the synergy between oxygen vacancy and crystal water. Crystal water promotes the protonation process of superoxide anion radicals to produce hydrogen peroxide (H₂O₂) and alleviates its decomposition. This mineral-based H₂O₂ photosynthesis system efficiently eliminates organic pollutants in a sequential light-dark reaction. Furthermore, this synergy effect can extend to other metal oxide minerals such as TiO₂, SnO₂, CuO, ZnO, and Bi₂O₃. Our results illuminate an overlooked pathway for modulating the protonation process by immobilized water in hydrous minerals, playing a crucial role in ROS storage and migration and pollutant dynamics in a natural environment throughout the day/night cycle.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142015471","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}

{"title":"Rising Alkali-to-Acid Ratios in the Atmosphere May Correspond to Increased Aerosol Acidity.","authors":"Guangjie Zheng, Hang Su, Ruilin Wan, Xiaolin Duan, Yafang Cheng","doi":"10.1021/acs.est.4c06860","DOIUrl":"10.1021/acs.est.4c06860","url":null,"abstract":"<p><p>Aerosol acidity (or pH) is one central parameter in determining the health, climate, and ecological effects of aerosols. While it is traditionally assumed that the long-term aerosol pH levels are determined by the relative abundances of atmospheric alkaline to acidic substances (referred to as <i>R</i>_C/A hereinafter), we observed contrasting pH─<i>R</i>_C/A trends at different sites globally, i.e., rising alkali-to-acid ratios in the atmosphere may unexpectedly lead to increased aerosol acidity. Here, we examined this apparently counterintuitive phenomenon using the multiphase buffer theory. We show that the aerosol water content (AWC) set a pH \"baseline\" as the peak buffer pH, while the <i>R</i>_C/A and particle-phase chemical compositions determine the deviation of pH from this baseline within the buffer ranges. Therefore, contrasting long-term pH trends may emerge when <i>R</i>_C/A increases while the AWC or nitrate fraction decreases, or vice versa. Our results provided a theoretical framework for a quantitative understanding of the response of aerosol pH to variations in SO₂, NO_x versus NH₃, and dust emissions, offering broad applications in studies on aerosol pH and the associated environmental and health effects.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142131161","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}

{"title":"Socioeconomic Inequalities in the External Exposome in European Cohorts: The EXPANSE Project.","authors":"Apolline Saucy, Fabián Coloma, Sergio Olmos, Christofer Åström, Natalia Blay, Jolanda M A Boer, Payam Dadvand, Jeroen de Bont, Rafael de Cid, Kees de Hoogh, Konstantina Dimakopoulou, Ulrike Gehring, Anke Huss, Dorina Ibi, Klea Katsouyanni, Gerard Koppelman, Petter Ljungman, Erik Melén, Mark Nieuwenhuijsen, Federica Nobile, Annette Peters, Regina Pickford, Roel Vermeulen, Danielle Vienneau, Jelle Vlaanderen, Kathrin Wolf, Zhebin Yu, Evangelia Samoli, Massimo Stafoggia, Cathryn Tonne","doi":"10.1021/acs.est.4c01509","DOIUrl":"10.1021/acs.est.4c01509","url":null,"abstract":"<p><p>Socioeconomic inequalities in the exposome have been found to be complex and highly context-specific, but studies have not been conducted in large population-wide cohorts from multiple countries. This study aims to examine the external exposome, encompassing individual and environmental factors influencing health over the life course, and to perform dimension reduction to derive interpretable characterization of the external exposome for multicountry epidemiological studies. Analyzing data from over 25 million individuals across seven European countries including 12 administrative and traditional cohorts, we utilized domain-specific principal component analysis (PCA) to define the external exposome, focusing on air pollution, the built environment, and air temperature. We conducted linear regression to estimate the association between individual- and area-level socioeconomic position and each domain of the external exposome. Consistent exposure patterns were observed within countries, indicating the representativeness of traditional cohorts for air pollution and the built environment. However, cohorts with limited geographical coverage and Southern European countries displayed lower temperature variability, especially in the cold season, compared to Northern European countries and cohorts including a wide range of urban and rural areas. The individual- and area-level socioeconomic determinants (i.e., education, income, and unemployment rate) of the urban exposome exhibited significant variability across the European region, with area-level indicators showing stronger associations than individual variables. While the PCA approach facilitated common interpretations of the external exposome for air pollution and the built environment, it was less effective for air temperature. The diverse socioeconomic determinants suggest regional variations in environmental health inequities, emphasizing the need for targeted interventions across European countries.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11411702/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142138566","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Chemically Resolved Respiratory Deposition of Ultrafine Particles Characterized by Number Concentration in the Urban Atmosphere.","authors":"Jinghao Zhai, Shi Shao, Xin Yang, Yaling Zeng, Tzung-May Fu, Lei Zhu, Huizhong Shen, Jianhuai Ye, Chen Wang, Shu Tao","doi":"10.1021/acs.est.4c03279","DOIUrl":"10.1021/acs.est.4c03279","url":null,"abstract":"<p><p>Ultrafine particles (UFPs) dominate the atmospheric particles in number concentration, impacting human health and climate change. However, existing studies primarily rely on mass-based approaches, leading to a restricted understanding of the number-based and chemically resolved health effects of atmospheric UFPs. In this study, we utilized a high-mass-resolution single-particle aerosol mass spectrometer to investigate the online chemical composition and number size distribution of ultrafine, fine, and coarse particles during the summertime in urban Shenzhen, China. Human respiratory deposition dose assessments of particles with varying chemical compositions were further conducted by a respiratory deposition model. The results showed that during our observation, particles containing elemental carbon (EC) were the dominant components in UFPs (0.05-0.1 μm). Compared to fine and coarse particles, UFPs can deposit more deeply into the respiratory tract with a daily dose of ∼2.08 ± 0.67 billion particles. Among the deposited UFPs, EC-cluster particles constituted ∼85.7% in number fraction, accounting for a daily number dose of ∼1.78 billion particles, which poses a greater impact on human health. Simultaneously, we found discrepancies in the chemically resolved particle depositions among number-, surface area-, and mass-based approaches, emphasizing the importance of an appropriate metric for particle health-risk evaluation.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142118284","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}

{"title":"High-Performance Nanofiltration Membrane with Dual Resistance to Gypsum Scaling and Biofouling for Enhanced Water Purification.","authors":"Fuxin Zheng, Hao Zhang, Chanhee Boo, Mengmeng Wang, Junjun Tan, Shuji Ye, Shihong Lin, Yunkun Wang","doi":"10.1021/acs.est.4c07334","DOIUrl":"10.1021/acs.est.4c07334","url":null,"abstract":"<p><p>Nanofiltration (NF) technology is pivotal for ensuring a sustainable and reliable supply of clean water. To address the critical need for advanced thin-film composite (TFC) polyamide (PA) membranes with exceptional permselectivity and fouling resistance for emerging contaminant purification, we introduce a novel high-performance NF membrane. This membrane features a selective polypiperazine (PIP) layer functionalized with amino-containing quaternary ammonium compounds (QACs) through an <i>in situ</i> interfacial polycondensation reaction. Our investigation demonstrated that precise QAC functionalization enabled the construction of the selective PA layer with increased surface area, enhanced microporosity, stronger electronegativity, and reduced thickness compared to the control PIP membrane. As a result, the QAC NF membrane exhibited an approximately 51% increase in water permeance compared to the control PIP membrane, while achieving superior retention capabilities for divalent salts (>99%) and emerging organic contaminants (>90%). Furthermore, the incorporation of QACs into the PIP selective layer was proved to be effective in mitigating mineral scaling by allowing selective passage of scale-forming cations, while simultaneously exhibiting strong antimicrobial properties to combat biofouling. The <i>in situ</i> QAC incorporation strategy presented in this study provides valuable guidelines for the fit-for-purpose design of the selective PA layer, which is crucial for the development of high-performance NF membranes for efficient water purification.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142118286","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}

{"title":"Toward More Realistic Estimates of Product Displacement in Life Cycle Assessment.","authors":"Jingcheng Yang, Linlin Duan, Shitong Peng, Reinout Heijungs, Xinyi Geng, Peng Wang, Wei-Qiang Chen, Yi Yang","doi":"10.1021/acs.est.4c04006","DOIUrl":"10.1021/acs.est.4c04006","url":null,"abstract":"<p><p>Life-cycle assessment (LCA) is one of the most widely applied methods for sustainability assessment. A main application of LCA is to compare alternative products to identify and promote those that are more environmentally friendly. Such comparative LCA studies often rest on, explicitly or implicitly, an idealized assumption, namely, 1:1 displacement between functionally equivalent products. However, product displacement in the real world is much more complicated, affected by various factors such as the rebound effect and policy schemes. Here, we quantitatively review studies that have considered these aspects to evaluate the magnitude and distribution of realistic displacement estimates across several major product categories (biofuels, electricity, electric vehicles, and recycled products). Results show that displacement ratios concentrate around 40-60%, suggesting considerable overestimation of the benefits of alternative products if the 1:1 displacement assumption was used. Overall, there have been a small number of modeling studies on realistic product displacement and their scopes were limited. Additional research is needed to cover more product categories and geographies and improve the modeling of market and policy complexities. As such research accumulates, their displacement estimates can form a database that can be drawn upon by comparative LCA studies to more accurately determine the environmental impacts of alternative products.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142142987","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}

{"title":"Revisiting the Iron(II)/Cobalt(II)-Based Homogenous Fenton-like Processes from the Standpoint of Diverse Metal-Oxygen Complexes.","authors":"Yingxu Gong, Zhonglin Chen, Yining Wu, Aijie Wang, Shengxin Zhao","doi":"10.1021/acs.est.4c03211","DOIUrl":"10.1021/acs.est.4c03211","url":null,"abstract":"<p><p>The aqueous Fe^IV-oxo complex and Fe^III-peroxy complex (e.g., ligand-assisted or interfacial Fe^III-hydroperoxo intermediates) have been recognized as crucial reactive intermediates for decontamination in iron-based Fenton-like processes. Intermediates with terminal oxo ligands can undergo the oxygen atom exchange process with water molecules, whereas peroxides are unable to induce such exchanges. Therefore, these distinct metal-oxygen complexes can be distinguished based on the above feature. In this study, we identified previously unknown intermediates with a peroxy moiety and cobalt center that were generated during peroxymonosulfate (PMS) activation via aqueous Co^II ions under acidic conditions. Results of theoretical calculations and tip-enhanced Raman spectroscopy revealed that the Co^II ion tended to coordinate with the PMS anion to form a bidentate complex with a tetrahedral structure. These reactive cobalt intermediates were collectively named the Co^II-PMS* complex. Depending on the inherent characteristics of the target contaminants, the Co^II-PMS* complex can directly oxidize organic compounds or trigger PMS disproportionation to release hydroxyl radicals and sulfate radicals for collaborative decontamination. This work provides a comparative study between iron- and cobalt-based Fenton-like processes and proposes novel insights from the standpoint of diverse metal-oxygen complexes.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142138565","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}

{"title":"Life-Cycle Environmental Impacts of Additive-Related Chemicals in Polyvinyl Chloride Plastics and the Mitigation Potential.","authors":"Kai Zhao, Xin Wang, Zhenye Zhang, Yijun Li, Sitong Li, Enlin Tian, Xin Xie, Hang Fu, Shanying Hu","doi":"10.1021/acs.est.4c00449","DOIUrl":"10.1021/acs.est.4c00449","url":null,"abstract":"<p><p>Plastic additive-related chemicals, particularly in polyvinyl chloride (PVC) plastics, have become a key issue in plastic pollution. Although addressing plastic pollution through the life-cycle approach is crucial, the environmental impacts of typical plastic additive-related chemicals in PVC plastics during the cradle-to-gate stage remain unexplored. Consequently, managing the life-cycle environmental impacts of these additives remains challenging. Herein, the environmental impacts of 23 typical plastic additive-related chemicals and six PVC plastic products were evaluated throughout the cradle-to-gate life-cycle stage using a life cycle assessment-material flow analysis (LCA-MFA) coupled model. The results indicate that plastic additives significantly contribute to the environmental impacts of PVC plastic products across various end point indicators, ranging from 8.7 to 40.6%. Additionally, scenario analysis (SA) reveals that conventional strategies for addressing plastic pollution may not be highly effective in mitigating the environmental impacts associated with plastic additives. Specifically, compared to primary polymers, these additives exhibit 4 to 13% lower mitigation potential under the same policy scenarios. However, technical adjustment strategies targeting additives show a mitigation potential of 12 to 39%, suggesting that guiding the plastic additive industry toward green transformation is a key strategy for reducing environmental impacts.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142138564","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}