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Lithium-Ion Battery Recycling: Bridging Regulation Implementation and Technological Innovations for Better Battery Sustainability
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-02 DOI: 10.1021/acs.est.4c10819
Min Liu, Xuexing Pan, Xin Sun, Hyung Chul Kim, Wei Shen, Daniel De Castro Gomez, Ye Wu, Shaojun Zhang
Lithium-ion batteries (LIBs) are critical in our increasingly electrified world in terms of a carbon-neutral future. For the transportation sector, the rapid expansion of electric vehicles is expected to lead to a 7-fold increase in the demand for LIBs by 2030. (1) This surge raises substantial concerns regarding resource depletion and environmental impacts caused by the coming boom in retired LIBs. Therefore, battery recycling is emerging as a critical component of sustainable battery management, which requires both regulation development and technological advancement. Notably, the European Union (EU) has set regulations requiring at least 6% recycled lithium and nickel and 16% recycled cobalt in new batteries from 2031. (2) China also has introduced policies promoting the collection, repurposing, and recycling of spent LIBs. Existing research has largely focused on the environmental benefits of battery recycling, including technologies such as hydrometallurgical, pyrometallurgical, and direct recycling. (3,4) However, due to the scarcity of data from the battery recycling industry, these studies primarily relied on model simulations (e.g., BatPaC model) or laboratory-derived data. Similarly, the EU battery regulations for the carbon footprint propose a circular footprint formula (CFF) for battery recycling based on the product environmental footprint framework, encompassing material recycling, energy recovery, and waste disposal. Material recycling includes recovering metals from disassembled batteries (e.g., copper and aluminum), recycling printed wiring board (PWB) components, and extracting nickel and cobalt from battery cells through hydrometallurgical or pyrometallurgical processes. The specific calculation method of impacts of using primary and secondary materials is illustrated in eq 1, and that of the impacts and credits of producing secondary materials from battery cell recycling is presented in eq 2. Globally, pyrometallurgical recycling and hydrometallurgical recycling are the two primary industrial methods for cathode recovery, categorized into three typical routes depending on the recycling technology and desired products (Figure 1). Pyrometallurgical recycling involves high-temperature smelting, while hydrometallurgical recycling employs aqueous chemistry, using acid leaching followed by concentration and purification. Hydrometallurgical recycling is the dominant technology in the United States (route 2) and China (routes 2 and 3), largely due to its high recovery efficiency, high material purity, and ability to recover most LIB components. By 2023, the installed capacity of hydrometallurgical recycling has reached 105 000 tons in the United States and 3 300 000 tons in China. In Europe, pyrometallurgical technology is more commonly used (route 1). In 2023, the EU’s total recycling capacity exceeded 160 000 tons, with >50% relying on pyrometallurgical technology. However, the high energy demand and inability to recover some mat
{"title":"Lithium-Ion Battery Recycling: Bridging Regulation Implementation and Technological Innovations for Better Battery Sustainability","authors":"Min Liu, Xuexing Pan, Xin Sun, Hyung Chul Kim, Wei Shen, Daniel De Castro Gomez, Ye Wu, Shaojun Zhang","doi":"10.1021/acs.est.4c10819","DOIUrl":"https://doi.org/10.1021/acs.est.4c10819","url":null,"abstract":"Lithium-ion batteries (LIBs) are critical in our increasingly electrified world in terms of a carbon-neutral future. For the transportation sector, the rapid expansion of electric vehicles is expected to lead to a 7-fold increase in the demand for LIBs by 2030. (1) This surge raises substantial concerns regarding resource depletion and environmental impacts caused by the coming boom in retired LIBs. Therefore, battery recycling is emerging as a critical component of sustainable battery management, which requires both regulation development and technological advancement. Notably, the European Union (EU) has set regulations requiring at least 6% recycled lithium and nickel and 16% recycled cobalt in new batteries from 2031. (2) China also has introduced policies promoting the collection, repurposing, and recycling of spent LIBs. Existing research has largely focused on the environmental benefits of battery recycling, including technologies such as hydrometallurgical, pyrometallurgical, and direct recycling. (3,4) However, due to the scarcity of data from the battery recycling industry, these studies primarily relied on model simulations (e.g., BatPaC model) or laboratory-derived data. Similarly, the EU battery regulations for the carbon footprint propose a circular footprint formula (CFF) for battery recycling based on the product environmental footprint framework, encompassing material recycling, energy recovery, and waste disposal. Material recycling includes recovering metals from disassembled batteries (e.g., copper and aluminum), recycling printed wiring board (PWB) components, and extracting nickel and cobalt from battery cells through hydrometallurgical or pyrometallurgical processes. The specific calculation method of impacts of using primary and secondary materials is illustrated in eq 1, and that of the impacts and credits of producing secondary materials from battery cell recycling is presented in eq 2. Globally, pyrometallurgical recycling and hydrometallurgical recycling are the two primary industrial methods for cathode recovery, categorized into three typical routes depending on the recycling technology and desired products (Figure 1). Pyrometallurgical recycling involves high-temperature smelting, while hydrometallurgical recycling employs aqueous chemistry, using acid leaching followed by concentration and purification. Hydrometallurgical recycling is the dominant technology in the United States (route 2) and China (routes 2 and 3), largely due to its high recovery efficiency, high material purity, and ability to recover most LIB components. By 2023, the installed capacity of hydrometallurgical recycling has reached 105 000 tons in the United States and 3 300 000 tons in China. In Europe, pyrometallurgical technology is more commonly used (route 1). In 2023, the EU’s total recycling capacity exceeded 160 000 tons, with >50% relying on pyrometallurgical technology. However, the high energy demand and inability to recover some mat","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"79 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758229","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
Exploring the Effect of Environmental Conditions on Decay Kinetics of Aerosol Unsaturated Fatty Acids: New Insights Gained from Long-Term Ambient Measurements
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-02 DOI: 10.1021/acs.est.4c09808
Qiongqiong Wang, Shan Wang, Shuhui Zhu, Siyu Meng, Huan Yu, Jian Zhen Yu
Unsaturated fatty acids (uFAs) are important constituents of atmospheric organic aerosols, undergoing rapid degradation in the atmosphere that significantly influences aerosol’s physical and chemical properties. This study quantified the effective pseudo-first order decay rates of three abundant uFAs-oleic, elaidic, and linoleic acids under real atmospheric conditions using continuous bihourly measurement at a suburban site in Hong Kong over a 9-month period from November 2020 to August 2021. The impact of key environmental parameters, including ozone, initial uFA concentration, relative humidity, and temperature, on the decay rates was rigorously examined. Distinct kinetic behaviors were observed across different temperature ranges (TR1: 5–13 °C; TR2: 13–22 °C; TR3: 22–26 °C; TR4: 26–30 °C). Arrhenius plots of the decay rates revealed contrasting effective activation energies under TR2 and TR4, likely due to different phase states of aerosols and reaction mechanisms under varying environmental conditions. This study extends previous laboratory research by incorporating a wider range of ambient conditions, uncovering the complex interactions between environmental factors and the decay kinetics of uFAs. The findings provide critical insights for accurately modeling the fate of ambient organic aerosols and understanding the intricate impacts of atmospheric conditions on aerosol chemistry.
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引用次数: 0
Specifying the Associations between PM2.5 Constituents and Gastrointestinal Cancer Incidence: Findings from a Prospective Cohort Study in Beijing, China
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-12-02 DOI: 10.1021/acs.est.4c10986
Lei Yang, Ning Kang, Ning Wang, Xi Zhang, Shuo Liu, Huichao Li, Lili Cao, Tao Xue, Ziyu Li, Jiafu Ji, Tong Zhu
This study aimed to test the association between PM2.5 and the incidence of gastrointestinal (GI) cancer, and further to detect the primary constituents on this association. A sum of 142,982 participants without GI cancer at baseline were derived from the National Urban Cancer Screening Program in Beijing (2013–2019). The 5 year averaged concentrations of PM2.5 mass and its five constituents, namely, black carbon (BC), ammonium (NH4+), nitrate (NO3), organic matter (OM), and inorganic sulfate (SO42–), were estimated by using a hybrid machine learning model. The Cox proportional hazard model with fixed effects was used to explore the associations between PM2.5 mass and its constituents with the incidence of GI cancer. The double-exposure linear model, the mixture exposure model of quantile-based g-computation, and an explainable machine learning model were utilized to evaluate the importance of different PM2.5 constituents. Long-term exposure to PM2.5 mass and its constituents was linearly associated with GI cancer; the estimated hazard ratio and 95% confidence interval (95% CI) of per standard deviation increment were 1.367 (95% CI: 1.257 to 1.487) for PM2.5 mass, 1.434 (95% CI: 1.307 to 1.574) for BC, 1.255 (95% CI: 1.169 to 1.349) for NH4+, 1.217 (95% CI: 1.139 to 1.301) for NO3, 1.410 (95% CI: 1.287 to 1.546) for OM, and 1.410 (95% CI: 1.288 to 1.542) for SO42–. By using multiple methods, results indicated that SO42– and BC were the most important constituents. Results indicated that long-term exposure to PM2.5 was associated with a high incidence of GI cancer, and BC and SO42– were robustly identified as the primary constituents.
{"title":"Specifying the Associations between PM2.5 Constituents and Gastrointestinal Cancer Incidence: Findings from a Prospective Cohort Study in Beijing, China","authors":"Lei Yang, Ning Kang, Ning Wang, Xi Zhang, Shuo Liu, Huichao Li, Lili Cao, Tao Xue, Ziyu Li, Jiafu Ji, Tong Zhu","doi":"10.1021/acs.est.4c10986","DOIUrl":"https://doi.org/10.1021/acs.est.4c10986","url":null,"abstract":"This study aimed to test the association between PM<sub>2.5</sub> and the incidence of gastrointestinal (GI) cancer, and further to detect the primary constituents on this association. A sum of 142,982 participants without GI cancer at baseline were derived from the National Urban Cancer Screening Program in Beijing (2013–2019). The 5 year averaged concentrations of PM<sub>2.5</sub> mass and its five constituents, namely, black carbon (BC), ammonium (NH<sub>4</sub><sup>+</sup>), nitrate (NO<sub>3</sub><sup>–</sup>), organic matter (OM), and inorganic sulfate (SO<sub>4</sub><sup>2–</sup>), were estimated by using a hybrid machine learning model. The Cox proportional hazard model with fixed effects was used to explore the associations between PM<sub>2.5</sub> mass and its constituents with the incidence of GI cancer. The double-exposure linear model, the mixture exposure model of quantile-based g-computation, and an explainable machine learning model were utilized to evaluate the importance of different PM<sub>2.5</sub> constituents. Long-term exposure to PM<sub>2.5</sub> mass and its constituents was linearly associated with GI cancer; the estimated hazard ratio and 95% confidence interval (95% CI) of per standard deviation increment were 1.367 (95% CI: 1.257 to 1.487) for PM<sub>2.5</sub> mass, 1.434 (95% CI: 1.307 to 1.574) for BC, 1.255 (95% CI: 1.169 to 1.349) for NH<sub>4</sub><sup>+</sup>, 1.217 (95% CI: 1.139 to 1.301) for NO<sub>3</sub><sup>–</sup>, 1.410 (95% CI: 1.287 to 1.546) for OM, and 1.410 (95% CI: 1.288 to 1.542) for SO<sub>4</sub><sup>2–</sup>. By using multiple methods, results indicated that SO<sub>4</sub><sup>2–</sup> and BC were the most important constituents. Results indicated that long-term exposure to PM<sub>2.5</sub> was associated with a high incidence of GI cancer, and BC and SO<sub>4</sub><sup>2–</sup> were robustly identified as the primary constituents.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"259 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758234","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
Refining Metal-Free Carbon Nanoreactors through Electronic and Geometric Comodification for Boosted H2O2 Electrosynthesis toward Efficient Water Decontamination
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-29 DOI: 10.1021/acs.est.4c11612
Yifei Wang, Beibei Li, Guangheng Chen, Yuhan Wu, Meng Tian, Yongzhen Peng, Shixue Dou, Laiquan Li, Jingyu Sun
Hydrogen peroxide (H2O2) electrosynthesis using metal-free carbon materials via the 2e oxygen reduction pathway has sparked considerable research interest. However, the scalable preparation of carbon electrocatalysts to achieve satisfactory H2O2 yield in acidic media remains a grand challenge. Here, we present the design of a carbon nanoreactor series that integrates precise O/N codoping alongside well-regulated geometric structures targeting high-efficiency electrosynthesis of H2O2. Theoretical computations reveal that strategic N/O codoping facilitates partial electron transfer from C sites to O sites, realizing electronic rearrangement that optimizes C-site adsorption of *OOH. Concurrently, the O–O bond in *OOH is strengthened by charge transfer from antibonding to π-orbitals, stabilizing the O–O bond and preventing its dissociation. The carbon nanoreactor with a hollow bowl geometry also facilitates the mass transport of O2 and H2O2, achieving an H2O2 selectivity of 96% in acidic media. Furthermore, a flow cell integrated with the refined nanoreactor catalyst achieves an impressive H2O2 production rate of 2942.4 mg L–1 h–1, coupled with stable operation of nearly 80 h, surpassing the state-of-the-art metal-free analogs. The feasibility of the electro-synthesized H2O2 is further demonstrated to be highly efficient in wastewater remediation.
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引用次数: 0
Investigating Major Sources of Methane Emissions at US Landfills
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-29 DOI: 10.1021/acs.est.4c07572
Tia R. Scarpelli, Daniel H. Cusworth, Riley M. Duren, Jinsol Kim, Joseph Heckler, Gregory P. Asner, Eben Thoma, Max J. Krause, Daniel Heins, Susan Thorneloe
Airborne remote sensing observations were collected at 217 landfills across 17 states in the US in 2023. We used these observations to attribute emissions to major sources, including the landfill work face, where new waste is placed at the landfill and gas-control infrastructure. Methane emissions from the work face appeared to be more prevalent than gas-control infrastructure emissions, with 52 landfills exhibiting work face emissions out of the 115 observed landfills shown to be emitting in 2023. Landfills with work face emissions were often the highest emitters, especially sites with associated renewable natural gas facilities, and the total average site emissions from these landfills accounted for 79% of the observed emissions, indicating inefficient gas capture at these sites. Landfills with work face emissions also displayed the greatest disparity between observed emission rates and hourly emission rates that we estimated using annual emissions reported to the US EPA’s Greenhouse Gas Reporting Program. Work face emissions present a major opportunity for methane mitigation: Observed emissions from work face emitting-landfills in this study were equivalent to 15% of US methane emissions from municipal solid waste landfills in 2022, as reported in the 2024 Greenhouse Gas Inventory, though these landfills accounted for only 4% of open sites in the US. As the 217 landfills in this study cover only 17% of open landfills in the US, the total mitigation potential is likely greater. Using remote sensing, we find that the largest contributor to observed methane emissions at US landfills is the landfill work face, an area of the landfill often left out of the required monitoring and traditional emissions accounting methods.
{"title":"Investigating Major Sources of Methane Emissions at US Landfills","authors":"Tia R. Scarpelli, Daniel H. Cusworth, Riley M. Duren, Jinsol Kim, Joseph Heckler, Gregory P. Asner, Eben Thoma, Max J. Krause, Daniel Heins, Susan Thorneloe","doi":"10.1021/acs.est.4c07572","DOIUrl":"https://doi.org/10.1021/acs.est.4c07572","url":null,"abstract":"Airborne remote sensing observations were collected at 217 landfills across 17 states in the US in 2023. We used these observations to attribute emissions to major sources, including the landfill work face, where new waste is placed at the landfill and gas-control infrastructure. Methane emissions from the work face appeared to be more prevalent than gas-control infrastructure emissions, with 52 landfills exhibiting work face emissions out of the 115 observed landfills shown to be emitting in 2023. Landfills with work face emissions were often the highest emitters, especially sites with associated renewable natural gas facilities, and the total average site emissions from these landfills accounted for 79% of the observed emissions, indicating inefficient gas capture at these sites. Landfills with work face emissions also displayed the greatest disparity between observed emission rates and hourly emission rates that we estimated using annual emissions reported to the US EPA’s Greenhouse Gas Reporting Program. Work face emissions present a major opportunity for methane mitigation: Observed emissions from work face emitting-landfills in this study were equivalent to 15% of US methane emissions from municipal solid waste landfills in 2022, as reported in the 2024 Greenhouse Gas Inventory, though these landfills accounted for only 4% of open sites in the US. As the 217 landfills in this study cover only 17% of open landfills in the US, the total mitigation potential is likely greater. Using remote sensing, we find that the largest contributor to observed methane emissions at US landfills is the landfill work face, an area of the landfill often left out of the required monitoring and traditional emissions accounting methods.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"81 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142742494","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
A Micro Total Analysis System (μTAS) for the In Situ, Real-Time Tracking of Produced Water Discharges through Detection of PAHs and Other Aromatic Compounds. 用于通过检测多环芳烃和其他芳香族化合物对生产水排放进行现场实时跟踪的微型总体分析系统 (μTAS)。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-28 DOI: 10.1021/acs.est.4c08392
Espen Eek, Christian Totland, Stephen Hayes, Bent Frode Buraas, Axel Walta, Ivar-Kristian Waarum, Erlend Leirset, Harald Lura, Rolf Christian Sundt, Arne Pettersen, Gerard Cornelissen

Here, we present a novel micro Total Analysis System (μTAS) for the measurement of poly cyclic aromatic hydrocarbon (PAH) and other aromatic hydrocarbons (AHs) in water at ng/L levels in situ and in real time (IMiRO). The μTAS is based on in-line membrane extraction followed by detection of extracted aromatic substances with fluorescence. An offshore field demonstration of the method was conducted close to produced water (PW) discharged in the North Sea. PW was monitored with the IMiRO μTAS and compared to results from a simultaneously conducted independent tracer release experiment, where fluorescein was added to the PW as a tracer. The μTAS monitoring and fluorescein tracer experiment showed similar ability to track the dispersion of the PW plume in space, depth, and time. Moreover, the method detected the sum of phenanthrenes and the sum of heavier PAHs with limits of detection down to 6 ng/L, with a response time of 6 min. The novel μTAS system opens up for in situ real-time discharge monitoring of both permitted and accidental oil or PW releases from oil platforms as well as other sources. Such monitoring can also be used to test and verify dispersion models used for environmental risk assessment.

在此,我们介绍一种新型微量总分析系统(μTAS),用于原位和实时(IMiRO)测量水中的多环芳烃(PAH)和其他芳烃(AHs)的纳克/升水平。μTAS 基于在线膜萃取,然后用荧光检测萃取的芳烃物质。该方法在北海产水(PW)排放附近进行了近海现场演示。使用 IMiRO μTAS 对生产水进行监测,并与同时进行的独立示踪剂释放实验结果进行比较。μTAS监测和荧光素示踪实验在空间、深度和时间上跟踪污泥羽流扩散的能力相似。此外,该方法还能检测到菲类总和以及较重的多环芳烃总和,检测限低至 6 纳克/升,响应时间为 6 分钟。新型 μTAS 系统为原位实时监测石油平台和其他来源的允许和意外石油或污染物排放开辟了道路。这种监测还可用于测试和验证用于环境风险评估的扩散模型。
{"title":"A Micro Total Analysis System (μTAS) for the <i>In Situ</i>, Real-Time Tracking of Produced Water Discharges through Detection of PAHs and Other Aromatic Compounds.","authors":"Espen Eek, Christian Totland, Stephen Hayes, Bent Frode Buraas, Axel Walta, Ivar-Kristian Waarum, Erlend Leirset, Harald Lura, Rolf Christian Sundt, Arne Pettersen, Gerard Cornelissen","doi":"10.1021/acs.est.4c08392","DOIUrl":"https://doi.org/10.1021/acs.est.4c08392","url":null,"abstract":"<p><p>Here, we present a novel micro Total Analysis System (μTAS) for the measurement of poly cyclic aromatic hydrocarbon (PAH) and other aromatic hydrocarbons (AHs) in water at ng/L levels <i>in situ</i> and in real time (IMiRO). The μTAS is based on in-line membrane extraction followed by detection of extracted aromatic substances with fluorescence. An offshore field demonstration of the method was conducted close to produced water (PW) discharged in the North Sea. PW was monitored with the IMiRO μTAS and compared to results from a simultaneously conducted independent tracer release experiment, where fluorescein was added to the PW as a tracer. The μTAS monitoring and fluorescein tracer experiment showed similar ability to track the dispersion of the PW plume in space, depth, and time. Moreover, the method detected the sum of phenanthrenes and the sum of heavier PAHs with limits of detection down to 6 ng/L, with a response time of 6 min. The novel μTAS system opens up for <i>in situ</i> real-time discharge monitoring of both permitted and accidental oil or PW releases from oil platforms as well as other sources. Such monitoring can also be used to test and verify dispersion models used for environmental risk assessment.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":10.8,"publicationDate":"2024-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142737696","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
Activation of PAA at the Fe-Nx Sites by Boron Nitride Quantum Dots Enhanced Charge Transfer Generates High-Valent Metal-Oxo Species for Antibiotics Degradation. 氮化硼量子点增强电荷转移在 Fe-Nx 位激活 PAA,产生高价金属氧化物用于抗生素降解。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-28 DOI: 10.1021/acs.est.4c08224
Shuo Li, Yalun Yang, Junfeng Niu, Heshan Zheng, Wen Zhang, Yoong Kit Leong, Jo-Shu Chang, Bo Lai

Advanced oxidation processes (AOPs) based on peracetic acid (PAA) offer a promising strategy to address antibiotic wastewater pollution. In this study, Fe-doped graphitic carbon nitride (g-C3N4) nanomaterials were used to construct Fe-Nx sites, and the electronic structure was tuned by boron nitride quantum dots (BNQDs), thereby optimizing PAA activation for the degradation of antibiotics. The BNQDs-modified Fe-doped g-C3N4 catalyst (BNQDs-FCN) achieved an excellent reaction rate constant of 0.0843 min-1, marking a 21.6-fold improvement over the carbon nitride (CN)-based PAA system. DFT calculations further corroborate the superior adsorption capacity of the Fe-Nx sites for PAA, facilitating its activation. Charge transfer mechanisms, with PAA serving as an electron acceptor, were identified as the source of high-valent iron-oxo species. Moreover, the BNQDs-FCN system preferentially targets oxygen-containing functional groups in antibiotic structures, elucidating the selective attack patterns of these highly electrophilic species. This research not only elucidates the pivotal role of high-valent iron-oxo species in pollutant degradation within the PAA-AOPs framework but also pioneers a wastewater treatment system characterized by excellent degradation efficiency coupled with low ecological risk, thereby laying the groundwork for applications in wastewater management and beyond.

基于过乙酸(PAA)的高级氧化工艺(AOPs)为解决抗生素废水污染问题提供了一种前景广阔的策略。本研究利用掺杂铁的氮化石墨碳(g-C3N4)纳米材料构建铁-氮基点,并通过氮化硼量子点(BNQDs)调整其电子结构,从而优化了 PAA 对抗生素降解的活化作用。氮化硼量子点修饰的掺杂铁的 g-C3N4 催化剂(BNQDs-FCN)达到了 0.0843 min-1 的优异反应速率常数,比基于氮化碳(CN)的 PAA 系统提高了 21.6 倍。DFT 计算进一步证实,Fe-Nx 位点对 PAA 具有卓越的吸附能力,从而促进了 PAA 的活化。以 PAA 作为电子受体的电荷转移机制被确定为高价铁-氧物种的来源。此外,BNQDs-FCN 系统优先针对抗生素结构中的含氧官能团,阐明了这些高亲电性物种的选择性攻击模式。这项研究不仅在 PAA-AOPs 框架内阐明了高价铁氧物种在污染物降解中的关键作用,还开创了一种降解效率高、生态风险低的废水处理系统,从而为废水管理及其他领域的应用奠定了基础。
{"title":"Activation of PAA at the Fe-N<sub><i>x</i></sub> Sites by Boron Nitride Quantum Dots Enhanced Charge Transfer Generates High-Valent Metal-Oxo Species for Antibiotics Degradation.","authors":"Shuo Li, Yalun Yang, Junfeng Niu, Heshan Zheng, Wen Zhang, Yoong Kit Leong, Jo-Shu Chang, Bo Lai","doi":"10.1021/acs.est.4c08224","DOIUrl":"https://doi.org/10.1021/acs.est.4c08224","url":null,"abstract":"<p><p>Advanced oxidation processes (AOPs) based on peracetic acid (PAA) offer a promising strategy to address antibiotic wastewater pollution. In this study, Fe-doped graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) nanomaterials were used to construct Fe-N<sub><i>x</i></sub> sites, and the electronic structure was tuned by boron nitride quantum dots (BNQDs), thereby optimizing PAA activation for the degradation of antibiotics. The BNQDs-modified Fe-doped g-C<sub>3</sub>N<sub>4</sub> catalyst (BNQDs-FCN) achieved an excellent reaction rate constant of 0.0843 min<sup>-1</sup>, marking a 21.6-fold improvement over the carbon nitride (CN)-based PAA system. DFT calculations further corroborate the superior adsorption capacity of the Fe-N<sub><i>x</i></sub> sites for PAA, facilitating its activation. Charge transfer mechanisms, with PAA serving as an electron acceptor, were identified as the source of high-valent iron-oxo species. Moreover, the BNQDs-FCN system preferentially targets oxygen-containing functional groups in antibiotic structures, elucidating the selective attack patterns of these highly electrophilic species. This research not only elucidates the pivotal role of high-valent iron-oxo species in pollutant degradation within the PAA-AOPs framework but also pioneers a wastewater treatment system characterized by excellent degradation efficiency coupled with low ecological risk, thereby laying the groundwork for applications in wastewater management and beyond.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":10.8,"publicationDate":"2024-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142737706","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
High Viscosity and Two Phases Observed over a Range of Relative Humidities in Biomass Burning Organic Aerosol from Canadian Wildfires. 加拿大野火中生物质燃烧产生的有机气溶胶在一定相对湿度范围内观察到的高粘度和两相现象。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-28 DOI: 10.1021/acs.est.4c09148
Nealan G A Gerrebos, Julia Zaks, Florence K A Gregson, Max Walton-Raaby, Harrison Meeres, Ieva Zigg, Wesley F Zandberg, Allan K Bertram

Biomass burning organic aerosol (BBOA) is a major contributor to organic aerosol in the atmosphere. The impacts of BBOA on climate and health depend strongly upon their physicochemical properties, including viscosity and phase behavior (number and types of phases); these properties are not yet fully characterized. We collected BBOA field samples during the 2021 British Columbia wildfire season to constrain the viscosity and phase behavior at a range of relative humidities and compared them to previous studies on BBOA. Particles from all samples exhibited two-phased behavior with a polar hydrophilic phase and a nonpolar hydrophobic phase. We used the poke-flow viscosity technique to estimate the viscosity of the particles. Both phases of the BBOA had viscosities of >108 Pa s at relative humidities up to 50%. Such high viscosities correspond to mixing times within 200 nm BBOA particles of >5 h. Two phases and high viscosity have implications for how BBOA should be treated in atmospheric models.

生物质燃烧有机气溶胶(BBOA)是大气中有机气溶胶的主要来源。生物质燃烧有机气溶胶对气候和健康的影响在很大程度上取决于其物理化学特性,包括粘度和相态(相的数量和类型);这些特性尚未得到充分表征。我们在 2021 年不列颠哥伦比亚省野火季节期间采集了 BBOA 实地样本,以确定其在一系列相对湿度条件下的粘度和相行为,并将其与之前的 BBOA 研究进行比较。所有样本中的颗粒都表现出两相行为,即极性亲水相和非极性疏水相。我们使用戳流粘度技术来估算颗粒的粘度。当相对湿度达到 50%时,BBOA 的两相粘度都大于 108 Pa s。两相和高粘度对大气模型中如何处理 BBOA 产生了影响。
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引用次数: 0
Formation of Aromatic Halogenated Disinfection Byproducts in Swimming Pool Water during Chlorination: Organic Precursors and Mechanisms.
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-28 DOI: 10.1021/acs.est.4c08239
Junjie Wang, Hongyu Wu, Tao Ma, Haoran Chen, Chuze Chen, Yuting Wang, Qiming Xian, Tingting Gong

Disinfection byproducts (DBPs) in swimming pool water are a significant public health concern. The formation of aromatic halogenated DBPs in swimming pool water has not been clarified previously. In this study, the occurrence of aromatic halogenated DBPs in swimming pool water was examined, and it was found that halohydroxybenzoic acids (HBAs) and halobenzoquinones (HBQs) were the most dominant aromatic halogenated DBPs in swimming pool water that were continuously formed. Thus, the formation of HBAs and HBQs in swimming pool water from different organic precursors, including natural organic matter (NOM), pharmaceuticals and personal care products (PPCPs), during chlorination was examined. The results demonstrate that the formation of HBAs and HBQs from the PPCPs was relatively high compared with that from NOM, suggesting that the PPCPs from human inputs might be important organic precursors of aromatic halogenated DBPs in swimming pool water. The formation mechanisms of HBAs and HBQs from three typical PPCPs (benzophenone-3 (BP-3), methyl p-hydroxybenzoate (MeP) and carbamazepine) were further explored. The results show that the PPCPs containing phenolic groups with higher degradation rates (BP-3 and MeP) possessed higher formation of HBAs and HBQs. The three organic precursors underwent a series of substitution, hydrolysis, oxidation, rearrangement, and intramolecular cyclization reactions to form HBAs and HBQs, while the phenolic groups and ring structures may significantly affect the reactions. The chlorine dose, bromide/iodide concentration, and temperature significantly affected the formation of HBAs and HBQs from MeP during chlorination.

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引用次数: 0
Unraveling Potential Causative Components for the Deleterious Effect of Atmospheric Fine Particulate Matter on Red Blood Cells 揭示大气细颗粒物对红细胞产生有害影响的潜在致因成分
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-27 DOI: 10.1021/acs.est.4c06657
Yuzhu Zhang, Laijin Zhong, Jing Zhan, Zhipeng Yin, Yao Pei, Dong Cao, Qian S. Liu, Qunfang Zhou, Qian Liu, Guibin Jiang
Atmospheric fine particulate matter (PM2.5) poses threats to the cardiovascular system. Red blood cells (RBCs) are the most abundant cells in blood, which are actively involved in multiple hematological diseases, such as blood clot formation and thrombosis. Exploring how PM2.5 with spatiotemporal heterogeneity influences the hematological system by targeting RBCs would help gain insights into the deleterious effects of PM2.5 and provide clues for finding the causative components therein. Herein, the PM2.5 samples collected from 3 urban sites in Beijing (i.e., Chaoyang, Shunyi, and Yanqing districts) during 4 seasons of 2022 were studied for their toxicities to mouse RBCs, and the main contributing components were further explored through chemical analysis and correlation measure. The results showed that exposure to PM2.5 samples decreased adenosine triphosphate (ATP) levels and increased phosphatidylserine (PS) externalization of RBCs, causing cell morphological deformity. The Pearson correlation analysis showed that the aromaticity of the dissolved organic matter (DOM) in PM2.5 samples was positively correlated with PS exposure of RBCs, showing that the lignin-like compounds were the potential contributors. The negative correlation of zeta potentials of PM2.5 samples with PS exposure of RBCs showed the particle-derived bioactivities of this airborne pollutant. The simulative test based on artificial nanomaterials of carbon black (CB) and oxidized CB (OCB) confirmed the crucial role of particulate carbon in PM2.5-induced effects on RBCs, and soot with a certain oxidation degree was, thus, recognized as another contributor, given its ubiquitous existence in PM2.5 samples. This study, for the first time, revealed PM2.5-induced PS exposure of RBCs, and the causative components of DOM and soot were unraveled. Considering the inevitable contact of airborne PM2.5 with RBCs in the blood circulatory system, the findings obtained herein would help bridge the gap between PM2.5 exposure and the risk of cardiovascular diseases, like thrombogenesis.
大气中的细颗粒物(PM2.5)对心血管系统构成威胁。红细胞(RBC)是血液中含量最高的细胞,积极参与多种血液病的发生,如血凝块的形成和血栓的形成。探索具有时空异质性的 PM2.5 如何通过靶向红细胞影响血液系统,将有助于深入了解 PM2.5 的有害影响,并为找到其中的致病成分提供线索。本文研究了2022年4个季节在北京3个城市(朝阳区、顺义区和延庆区)采集的PM2.5样本对小鼠红细胞的毒性,并通过化学分析和相关测量进一步探讨了主要致病成分。结果表明,暴露于PM2.5样品会降低小鼠红细胞的三磷酸腺苷(ATP)水平,增加磷脂酰丝氨酸(PS)外化,导致细胞形态畸变。皮尔逊相关分析表明,PM2.5 样品中溶解有机物(DOM)的芳香度与 RBC 的 PS 暴露呈正相关,表明木质素类化合物是潜在的致病因素。PM2.5 样品的 zeta 电位与 RBC 的 PS 暴露呈负相关,这表明这种空气污染物的生物活性来源于颗粒。基于炭黑(CB)和氧化炭黑(OCB)人工纳米材料的模拟测试证实了颗粒碳在 PM2.5 诱导的对红细胞的影响中的关键作用,而具有一定氧化程度的烟尘由于在 PM2.5 样品中无处不在,因此被认为是另一个贡献者。这项研究首次揭示了 PM2.5 诱导的红细胞 PS 暴露,并揭示了 DOM 和烟尘的致病成分。考虑到空气中的PM2.5与血液循环系统中的红细胞不可避免地发生接触,本研究的发现将有助于弥合PM2.5暴露与心血管疾病(如血栓形成)风险之间的差距。
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引用次数: 0
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