IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-10-21 DOI: 10.1021/acs.est.4c06351

Fukun Bi, Jiafeng Wei, Bin Gao, Shuting Ma, Ning Liu, Jingcheng Xu, Baolin Liu, Yuandong Huang, Xiaodong Zhang

{"title":"How the Most Neglected Residual Species in MOF-Based Catalysts Involved in Catalytic Reactions to Form Toxic Byproducts","authors":"Fukun Bi, Jiafeng Wei, Bin Gao, Shuting Ma, Ning Liu, Jingcheng Xu, Baolin Liu, Yuandong Huang, Xiaodong Zhang","doi":"10.1021/acs.est.4c06351","DOIUrl":"https://doi.org/10.1021/acs.est.4c06351","url":null,"abstract":"In recent years, multifarious new materials have been developed for environmental governance. Thereinto, metal organic framework (MOF)-based catalysts have been widely employed for heterogeneous catalysis because of their high porosity to confine noble metal particles faraway from aggregation. However, the potential reactions between residual species from the material synthesis process and target pollutants, which could form highly toxic byproducts, are often neglected. Herein, we took the widely used Zr-MOF, UiO-66, with highly thermal stability supported Pd catalysts as the example to investigate how the residual species in catalysts are involved in aromatic volatile organic compounds (VOCs) degradation reaction. The results showed that residual Cl species originated from the ZrCl4 metal precursor participated in the VOC degradation reaction, leading to the production of various chlorine-containing byproducts, even the hypertoxicity dioxin precursor, dichlorobenzene. Meanwhile, the chlorination mechanism for the formation of chlorine-containing byproducts was revealed by density functional theory calculation. Furthermore, the highly efficient residual Cl removal approaches are proposed. Importantly, the migration and transformation of residual Cl during the degradation of five benzene series VOCs are comprehensively studied and elucidated. We anticipate that these findings will raise alarm about the neglected issue of residual species in MOF-based catalysts for heterogeneous catalysis, especially environmentally friendly catalysis.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452141","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

Enhanced Rock Weathering as a Source of Metals to Promote Methanogenesis and Counteract CO2 Sequestration 强化岩石风化作为促进甲烷生成和抵消二氧化碳封存的金属来源

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-10-21 DOI: 10.1021/acs.est.4c04751

Donglei Zhang, Qiang Zeng, Hongyu Chen, Dongyi Guo, Gaoyuan Li, Hailiang Dong

引用次数: 0

Eutrophication and Dissolved Organic Matter Exacerbate the Diel Discrepancy of CO2 Emissions in China’s Largest Urban Lake 富营养化和溶解有机物加剧了中国最大城市湖泊二氧化碳排放量的昼夜差异

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-10-21 DOI: 10.1021/acs.est.4c06244

Yang Wang, Bingjie Ma, Y. Jun Xu, Shuai Shen, Xi Huang, Yan Wang, Songlin Ye, Xiaokang Tian, Yifei Zhang, Tong Wang, Siyue Li

{"title":"Eutrophication and Dissolved Organic Matter Exacerbate the Diel Discrepancy of CO2 Emissions in China’s Largest Urban Lake","authors":"Yang Wang, Bingjie Ma, Y. Jun Xu, Shuai Shen, Xi Huang, Yan Wang, Songlin Ye, Xiaokang Tian, Yifei Zhang, Tong Wang, Siyue Li","doi":"10.1021/acs.est.4c06244","DOIUrl":"https://doi.org/10.1021/acs.est.4c06244","url":null,"abstract":"The large variability in the emissions of carbon dioxide (CO2) from urban lakes remains a challenge for partitioning these sources at meaningful spatial and temporal scales. Dissolved organic matter (DOM) governs the spatial and temporal variations in CO2, yet relationships of the CO2 concentration (cCO2) and emission flux (FCO2) with DOM in urban lakes have rarely been reported. In this study, we monitored levels of cCO2, FCO2, and the composition of DOM over a 24 h period at three sites during the dry and wet seasons in China’s largest urban lake, Tangxun Lake. Our study found the ratio of day/night FCO2 (millimoles per square meter per day) decreased from the dry season (0.79; 7.68/9.68) to the wet season (0.25; 6.05/24.16), averaging 0.42 (6.77/15.97), implying that accounting for nighttime CO2 emissions can increase regional estimates by 70%. This study revealed that eutrophication affected diurnal CO2 emissions with greater algal growth enhancing daytime CO2 uptake and subsequently increasing nighttime CO2 emissions via DOM degradation (larger protein-like DOM fraction). We anticipate that the relative magnitude of FCO2 between day and night from lakes is likely to increase due to urbanization and climate change, underscoring the importance of treating urban lakes as a distinct group and integrating DOM dynamics into carbon cycling in future research.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452154","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

Coupling Effect of Elemental Carbon and Organic Carbon on the Changes of Optical Properties and Oxidative Potential of Soot Particles under Visible Light 元素碳和有机碳对可见光下烟尘颗粒光学特性和氧化电位变化的耦合效应

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-10-21 DOI: 10.1021/acs.est.4c09217

Rui Tang, Jiong Cao, Jing Shang, Yu Kuang, Hong Geng, Xinghua Qiu

{"title":"Coupling Effect of Elemental Carbon and Organic Carbon on the Changes of Optical Properties and Oxidative Potential of Soot Particles under Visible Light","authors":"Rui Tang, Jiong Cao, Jing Shang, Yu Kuang, Hong Geng, Xinghua Qiu","doi":"10.1021/acs.est.4c09217","DOIUrl":"https://doi.org/10.1021/acs.est.4c09217","url":null,"abstract":"Soot particles, coming from the incomplete combustion of fossil or biomass fuels, feature a core–shell structure with inner elemental carbon (EC) and outer organic carbon (OC). Both EC and OC are known to be photoactive under solar radiation. However, research on their coupling effect during photochemical aging remains limited. This study examines how the optical properties and oxidative potential (OP) of wood, coal, and diesel soot particles with varying EC and OC levels are affected by exposure to visible light. Wood soot, which has the highest OC content, showed the most significant changes in both optical properties and OP, indicating its highest sensitivity to visible light aging. Molecular composition analysis revealed that the reduction of polycyclic aromatic hydrocarbons (PAHs) and methyl-PAHs primarily affects the optical properties, while oxygenated PAHs play a major role in OP. Combined with the results from reactive oxygen species detection, it is suggested that EC initiates photoreactions by generating superoxide anions, while OC undergoes compositional changes that result in subsequent atmospheric effects. These findings enhance our understanding of the photochemical aging process of soot particles and their implications for climate and health.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452155","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

Mitigating Grand Challenges in Life Cycle Inventory Modeling through the Applications of Large Language Models 通过应用大型语言模型缓解生命周期库存建模的巨大挑战

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-10-21 DOI: 10.1021/acs.est.4c07634

Qingshi Tu, Jing Guo, Nan Li, Jianchuan Qi, Ming Xu

{"title":"Mitigating Grand Challenges in Life Cycle Inventory Modeling through the Applications of Large Language Models","authors":"Qingshi Tu, Jing Guo, Nan Li, Jianchuan Qi, Ming Xu","doi":"10.1021/acs.est.4c07634","DOIUrl":"https://doi.org/10.1021/acs.est.4c07634","url":null,"abstract":"The accuracy of life cycle assessment (LCA) studies is often questioned due to the two grand challenges of life cycle inventory (LCI) modeling: (1) missing foreground flow data and (2) inconsistency in background data matching. Traditional mechanistic methods (e.g., process simulation) and existing machine learning (ML) methods (e.g., similarity-based selection methods) are inadequate due to their limitations in scalability and generalizability. The large language models (LLMs) are well-positioned to address these challenges, given the massive and diverse knowledge learned through the pretraining step. Incorporating LLMs into LCI modeling can lead to the automation of inventory data curation from diverse data sources and to the implementation of a multimodal analytical capacity. In this article, we delineated the mechanisms and advantages of LLMs to addressing these two grand challenges. We also discussed the future research to enhance the use of LLMs for LCI modeling, which includes the key areas such as improving retrieval augmented generation (RAG), integration with knowledge graphs, developing prompt engineering strategies, and fine-tuning pretrained LLMs for LCI-specific tasks. The findings from our study serve as a foundation for future research on scalable and automated LCI modeling methods that can provide more appropriate data for LCA calculations.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142451950","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

Chemical Fingerprinting of PM2.5 via Sequential Speciation Analysis Using Electrochemical Mass Spectrometry 利用电化学质谱法进行序贯标样分析，对 PM2.5 进行化学指纹识别

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-10-21 DOI: 10.1021/acs.est.4c01682

Lili Song, Luyao Zhong, Ting Li, Yufei Chen, Xinglei Zhang, Konstantin Chingin, Ni Zhang, Hui Li, Liyun Hu, Dongfa Guo, Huanwen Chen, Rui Su, Jiaquan Xu

{"title":"Chemical Fingerprinting of PM2.5 via Sequential Speciation Analysis Using Electrochemical Mass Spectrometry","authors":"Lili Song, Luyao Zhong, Ting Li, Yufei Chen, Xinglei Zhang, Konstantin Chingin, Ni Zhang, Hui Li, Liyun Hu, Dongfa Guo, Huanwen Chen, Rui Su, Jiaquan Xu","doi":"10.1021/acs.est.4c01682","DOIUrl":"https://doi.org/10.1021/acs.est.4c01682","url":null,"abstract":"Chemical fingerprinting to characterize the occurrence state and abundance of organic and inorganic constituents within fine particulate matter (PM2.5) is useful in evaluating the associated health risks and tracing pollution sources. Herein, an analytical strategy for the rapid analysis of metal and organic constituents in PM2.5 was developed employing a combination of sequential chemical extraction coupled with mass spectrometry detection. H2O, CH3OH, EDTA-2Na, electrochemical oxidation, and electrochemical reduction were sequentially utilized to extract the chemical constituents in PM2.5 samples on a homemade device employing simultaneous online detection using two linear trap quadrupole mass spectrometers (LTQ-MS) with electrospray ionization (ESI) in positive and negative modes. After a single analytical procedure, dozens of metals (e.g., Pb, Cr, and Cu), organic compounds (e.g., amines, polycyclic aromatic hydrocarbons, and aliphatic acids), and negative ions (e.g., NO3–, NO2–, and Cl–) were comprehensively detected in the water-soluble, liposoluble, insoluble, oxidizable, and reducible fractions of PM2.5 samples, and their physical and chemical relationships were established.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142451949","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

Effect, Fate and Remediation of Pharmaceuticals and Personal Care Products (PPCPs) during Anaerobic Sludge Treatment: A Review 厌氧污泥处理过程中药物和个人护理产品 (PPCPs) 的影响、归宿和补救：综述

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-10-20 DOI: 10.1021/acs.est.4c06760

Xiaomin Wang, Yufen Wang, Zixin Zhang, Lixin Tian, Tingting Zhu, Yingxin Zhao, Yindong Tong, Yongkui Yang, Peizhe Sun, Yiwen Liu

{"title":"Effect, Fate and Remediation of Pharmaceuticals and Personal Care Products (PPCPs) during Anaerobic Sludge Treatment: A Review","authors":"Xiaomin Wang, Yufen Wang, Zixin Zhang, Lixin Tian, Tingting Zhu, Yingxin Zhao, Yindong Tong, Yongkui Yang, Peizhe Sun, Yiwen Liu","doi":"10.1021/acs.est.4c06760","DOIUrl":"https://doi.org/10.1021/acs.est.4c06760","url":null,"abstract":"Biomass energy recovery from sewage sludge through anaerobic treatment is vital for environmental sustainability and a circular economy. However, large amounts of pharmaceutical and personal care products (PPCPs) remain in sludge, and their interactions with microbes and enzymes would affect resource recovery. This article reviews the effects and mechanisms of PPCPs on anaerobic sludge treatment. Most PPCPs posed adverse impacts on methane production, while certain low-toxicity PPCPs could stimulate volatile fatty acids and biohydrogen accumulation. Changes in the microbial community structure and functional enzyme bioactivities were also summarized with PPCPs exposure. Notably, PPCPs such as carbamazepine could bind with the active sites of the enzyme and induce microbial stress responses. The fate of various PPCPs during anaerobic sludge treatment indicated that PPCPs featuring electron-donating groups (e.g., ·–NH2 and ·–OH), hydrophilicity, and low molecular weight were more susceptible to microbial utilization. Key biodegrading enzymes (e.g., cytochrome P450 and amidase) were crucial for PPCP degradation, although several PPCPs remain refractory to biotransformation. Therefore, remediation technologies including physical pretreatment, chemicals, bioaugmentation, and their combinations for enhancing PPCPs degradation were outlined. Among these strategies, advanced oxidation processes and combined strategies effectively removed complex and refractory PPCPs mainly by generating free radicals, providing recommendations for improving sludge detoxification.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142451679","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

Water Uptake of Airborne Cells of P. syringae Measured with a Hygroscopicity Tandem Differential Mobility Analyzer 利用吸湿性串联差分迁移率分析仪测量空气中 P. syringae 细胞的吸水率

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-10-19 DOI: 10.1021/acs.est.4c01817

Lærke Sloth Nielsen, Tina Šantl-Temkiv, María Palomeque Sánchez, Andreas Massling, Josephine Caroline Ward, Pia Bomholt Jensen, Thomas Boesen, Markus Petters, Kai Finster, Merete Bilde, Bernadette Rosati

{"title":"Water Uptake of Airborne Cells of P. syringae Measured with a Hygroscopicity Tandem Differential Mobility Analyzer","authors":"Lærke Sloth Nielsen, Tina Šantl-Temkiv, María Palomeque Sánchez, Andreas Massling, Josephine Caroline Ward, Pia Bomholt Jensen, Thomas Boesen, Markus Petters, Kai Finster, Merete Bilde, Bernadette Rosati","doi":"10.1021/acs.est.4c01817","DOIUrl":"https://doi.org/10.1021/acs.est.4c01817","url":null,"abstract":"Airborne microorganisms impact cloud formation and are involved in disease spreading. The ability of airborne cells to survive and express genes may be limited by reduced water availability in the atmosphere and depend on the ability of the cells to attract water vapor at subsaturated conditions, i.e., their hygroscopicity. We assessed hygroscopic properties of the plant pathogen Pseudomonas syringae, known to participate in cloud formation. We used a hygroscopicity tandem differential mobility analyzer to examine both hydration and dehydration behavior in the relative humidity (RH) range 5–90%. The cells were aerosolized either from Milli-Q water or from a 35 g L–1 NaCl solution, resulting in pure cells or cells associated with NaCl. Pure cells exhibited no deliquescence/efflorescence and a small gradual water uptake reaching a maximum growth factor (GF) of 1.09 ± 0.01 at 90% RH. For cells associated with NaCl, we observed deliquescence and a much larger maximum GF of 1.74 ± 0.03 at 90% RH. Deliquescence RH was comparable to that of pure NaCl, highlighting the major role of the salt associated with the cells. It remains to be investigated how the observed hygroscopic properties relate to survival, metabolic, and ice-nucleation activities of airborne P. syringae.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142449724","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

Regulating the Electronic Structure of Cu Single-Atom Catalysts toward Enhanced Electro-Fenton Degradation of Organic Contaminants via 1O2 and •OH 通过 1O2 和 -OH 调节铜单原子催化剂的电子结构以增强电-芬顿降解有机污染物的能力

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-10-19 DOI: 10.1021/acs.est.4c08704

Genwang Zhu, Xinfei Fan, Yueling Yu, Yanming Liu, Xie Quan

{"title":"Regulating the Electronic Structure of Cu Single-Atom Catalysts toward Enhanced Electro-Fenton Degradation of Organic Contaminants via 1O2 and •OH","authors":"Genwang Zhu, Xinfei Fan, Yueling Yu, Yanming Liu, Xie Quan","doi":"10.1021/acs.est.4c08704","DOIUrl":"https://doi.org/10.1021/acs.est.4c08704","url":null,"abstract":"Heterogeneous electro-Fenton degradation with 1O2 and •OH generated from O2 reduction is cost-effective for the removal of refractory organic pollutants from wastewater. As 1O2 is more tolerant to background constituents such as salt ions and a high pH value than •OH, tuning the production of 1O2 and •OH is important for efficient electro-Fenton degradation. However, it remains a great challenge to selectively produce 1O2 and improve the species yield. Herein, the electronic structure of atomically dispersed Cu–N4 sites was regulated by doping electron-deficient B into porous hollow carbon microspheres (CuBN-HCMs), which improved *O2 adsorption and significantly enhanced 1O2 selectivity in electro-Fenton degradation. Its 1O2 yield was 2.3 times higher than that of a Cu single-atom catalyst without B doping. Meanwhile, •OH was simultaneously generated as a minor species. The CuBN-HCMs were efficient for the electro-Fenton degradation of phenol, sulfamethoxazole, and bisphenol A with a high mineralization efficiency. Its kinetic constants showed insignificant changes under various anions and a wide pH range of 1–9. More importantly, it was energy-efficient for treating actual coking wastewater with a low energy consumption of 19.0 kWh kgCOD–1. The superior performance of the CuBN-HCMs was contributed from 1O2 and •OH and its high 1O2 selectivity.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142449935","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

Free Chlorine Can Inhibit Lead Solder Corrosion via Electrochemical Reversal 游离氯能通过电化学逆转抑制铅焊料腐蚀

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-10-18 DOI: 10.1021/acs.est.4c07375

Frank A. Mazzola, Kathryn G. Lopez, Marc Edwards

引用次数: 0

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