环境科学与技术最新文献

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Hidden Giant of Embedded Plastics in China
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-10 DOI: 10.1021/acs.est.4c04814
Shang Zhang, Jinhui Li, Quanyin Tan
{"title":"Hidden Giant of Embedded Plastics in China","authors":"Shang Zhang, Jinhui Li, Quanyin Tan","doi":"10.1021/acs.est.4c04814","DOIUrl":"https://doi.org/10.1021/acs.est.4c04814","url":null,"abstract":"Combating plastic pollution requires an understanding of the complex intersectoral flows of plastics and related products. In this study, we develop an inventory of 150 categories of products consisting of/containing plastics based on bottom-up analysis and establish a plastics input–output material flow analysis (PIO-MFA) model that reveals intersectoral flows, sectoral consumption, exports, and stocks of embedded plastics. In 2018, consumption-based plastic usage in China reached 140 million tons (Mt), with 123.5 Mt being embedded plastics. Approximately 75.5% of embedded plastics were consumed domestically, and 21.3% were exported. Among the plastics exported, embedded plastics accounted for 68.5%, indicating the importance of the implicit transfer of embedded plastics through global trade. Furthermore, based on ambitious recycling targets, the amount of recycled plastics in China is expected to increase by 27.8 Mt. Plastics embedded in containers and packaging have the highest reduction potential, while joint efforts from the entire supply chain are crucial to reduce the amount of such plastics as industrial sectors consume 32.4% of embedded plastics. Identifying high plastic consumption sectors is critical for balancing economic and social goals with pollution control and ensuring comprehensive plastic treaty compliance. The PIO-MFA method’s foreseeable future expansion to a global level is expected to inform plastic treaty obligations and support the development and implementation of national action plans.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"36 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797282","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
Quantifying and Modeling the Impact of Phase State on the Ice Nucleation Abilities of 2-Methyltetrols as a Key Component of Secondary Organic Aerosol Derived from Isoprene Epoxydiols
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-10 DOI: 10.1021/acs.est.4c06285
Xiaohan Li, Martin Wolf, Xiaoli Shen, Isabelle Steinke, Zhenli Lai, Sining Niu, Swarup China, Manish Shrivastava, Zhenfa Zhang, Avram Gold, Jason D. Surratt, Ian C. Bourg, Daniel J. Cziczo, Susannah M. Burrows, Yue Zhang
{"title":"Quantifying and Modeling the Impact of Phase State on the Ice Nucleation Abilities of 2-Methyltetrols as a Key Component of Secondary Organic Aerosol Derived from Isoprene Epoxydiols","authors":"Xiaohan Li, Martin Wolf, Xiaoli Shen, Isabelle Steinke, Zhenli Lai, Sining Niu, Swarup China, Manish Shrivastava, Zhenfa Zhang, Avram Gold, Jason D. Surratt, Ian C. Bourg, Daniel J. Cziczo, Susannah M. Burrows, Yue Zhang","doi":"10.1021/acs.est.4c06285","DOIUrl":"https://doi.org/10.1021/acs.est.4c06285","url":null,"abstract":"Organic aerosols (OAs) may serve as ice-nucleating particles (INPs), impacting the formation and properties of cirrus clouds when their phase state and viscosity are in the semisolid to glassy range. However, there is a lack of direct parameterization between aerosol viscosity and their ice nucleation capabilities. In this study, we experimentally measured the ice nucleation rate of 2-methyltetrols (2-MT) aerosols, a key component of isoprene-epoxydiol-derived secondary organic aerosols (IEPOX-SOA), at different viscosities. These results demonstrate that the phase state has a significant impact on the ice nucleation abilities of OA under typical cirrus cloud conditions, with the ice nucleation rate increasing by 2 to 3 orders of magnitude when the phase state changes from liquid to semisolid. An innovative parametric model based on classical nucleation theory was developed to directly quantify the impact of viscosity on the heterogeneous nucleation rate. This model accurately represents our laboratory measurement and can be implemented into climate models due to its simple, equation-based form. Based on data collected from the ACRIDICON-CHUVA field campaign, our model predicts that the INP concentration from IEPOX-SOA can reach the magnitude of 1 to tens per liter in the cirrus cloud region impacted by the Amazon rainforest, consistent with recent field observations and estimations. This novel parameterization framework can also be applied in regional and global climate models to further improve representations of cirrus cloud formation and associated climate impacts.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"47 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142804693","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
The Effect of Copper Limitation on the Bioavailability of Cu-Organic Complexes
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-10 DOI: 10.1021/acs.est.4c06790
Meizhen Li, Liangliang Kong, Neil M. Price
{"title":"The Effect of Copper Limitation on the Bioavailability of Cu-Organic Complexes","authors":"Meizhen Li, Liangliang Kong, Neil M. Price","doi":"10.1021/acs.est.4c06790","DOIUrl":"https://doi.org/10.1021/acs.est.4c06790","url":null,"abstract":"We examined the bioavailability of synthetic organic Cu complexes (Cu-L) and inorganic Cu species (Cu′) to <i>Thalassiosira oceanica</i> growing under Cu-limiting and Cu-inhibiting conditions. Copper bioavailability depended on the phytoplankton Cu nutritional state and whether Cu′ diffusion to the cell surface was sufficient to meet the cellular demands for growth. Under Cu-limiting conditions when [Cu′] was less than the diffusion concentration threshold (DCT: 10<sup>–14.13</sup> M), growth rate was a hyperbolic function of [Cu-L]. Increasing [Cu′] above the DCT caused growth rate to increase proportionally, but growth rate also increased with increasing [Cu-L] so that both Cu′ and Cu-L were bioavailable. Short-term photosynthesis assays conducted under Cu-limiting conditions showed a similar response to Cu speciation. In contrast, the growth rate of Cu-inhibited cells at high [Cu′] varied inversely with [Cu<sup>2+</sup>] and was independent of [Cu-L], as previously reported. The change in Cu-L bioavailability correlated with expression levels of genes encoding the reduction-dependent, high-affinity Cu uptake pathway, which was regulated by [Cu′]. Our analysis shows that at [Cu′] typical of the open sea, <i>T. oceanica</i>-like phytoplankton are diffusion limited and must rely on Cu-organic complexes to fulfill their Cu requirements for growth.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"2 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797283","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
Buzzing Beyond Annoyance: Flies as Nature’s Composite Samplers of Terrestrial Fecal Contamination
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-10 DOI: 10.1021/acs.est.4c11869
Drew Capone, Christine J. Picard
{"title":"Buzzing Beyond Annoyance: Flies as Nature’s Composite Samplers of Terrestrial Fecal Contamination","authors":"Drew Capone, Christine J. Picard","doi":"10.1021/acs.est.4c11869","DOIUrl":"https://doi.org/10.1021/acs.est.4c11869","url":null,"abstract":"While eating a meal outside or in your kitchen, the presence of flies incessantly buzzing around is common. Not only annoying, flies pose a public health hazard. (1,2) Some flies–including house flies and blow flies–consume feces as part of their diet. This fecal material contains trillions of microbes, which may include pathogens and antibiotic-resistant organisms. Flies carry pathogens two ways: physically attached to their body as they land on the feces, and inside their alimentary canal. When a fly lands on any surface following a meal (which could include the chicken and rice you are planning to eat for dinner), it may vomit. This fly “speck” may be composed of fecal remnants that contain pathogenic organisms. Flies also defecate, and many pathogens can survive passage through the fly alimentary canal. (1) The consumption of these pathogens by humans can lead to an infection, which is a prerequisite for illnesses such as diarrheal disease. The same behavior that causes flies to pose a public health risk also creates a unique opportunity for environmental monitoring. Certain species of flies–including blow flies and house flies–can be viewed as nature’s composite samplers of fecal material in the terrestrial environment. Environmental samples are typically collected via grab, passive, or composite sampling. (3) Grab samples are discrete samples collected from a single location and time-point. Passive samples require a material that spontaneously absorbs or adsorbs the contaminant of interest from the surrounding environment. Composite samples are mixtures of multiple individual samples which may be pooled geographically or temporally. Combining samples to form a composite sample may provide a more representative understanding of the target of interest in a population but loses information about individual samples. Composite sampling is also used because it can dramatically reduce analytical costs via a reduction in the number of analyses required. Methods for composite sampling are well developed for air, water, and soil monitoring, as well as for clinical testing. (3) Natural fly behavior mimics that of a composite sampler (Figure 1). Flies continuously move from attractant to attractant during daytime hours, feeding on a variety of organic material that includes feces for some species. (1,2) Through ingestion, or attachment to the body surface, flies gather microbes and chemicals present in the terrestrial locations they visit, effectively creating a composite sample. While flies are capable of up to 20 km of flight in a single day, long-distance travel is rare when nearby food is plentiful. (1,2) Instead, flies will often travel less than a few hundred meters in a single day, indicating that they may be used as composite samplers of the localized terrestrial environment. Figure 1. Flies move from attractant to attractant, collecting fecal microbes on their outer body and in their alimentary canal. Fecal material contains a wealth of inform","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"47 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797286","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
Molecular Characterization of Organosulfur and Organonitrogen Compounds in Summer and Winter PM2.5 via UHPLC-Q-Orbitrap MS/MS. 通过超高效液相色谱-Q-轨道阱 MS/MS 对夏季和冬季 PM2.5 中的有机硫和有机氮化合物进行分子表征。
IF 10.8 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-10 Epub Date: 2024-11-27 DOI: 10.1021/acs.est.4c02727
Hui Li, Fengkui Duan, Tao Ma, Yongliang Ma, Yunzhi Xu, Shuxiao Wang, Qinqin Zhang, Jingkun Jiang, Lidan Zhu, Fan Li, Tao Huang, Takashi Kimoto, Kebin He
{"title":"Molecular Characterization of Organosulfur and Organonitrogen Compounds in Summer and Winter PM<sub>2.5</sub> via UHPLC-Q-Orbitrap MS/MS.","authors":"Hui Li, Fengkui Duan, Tao Ma, Yongliang Ma, Yunzhi Xu, Shuxiao Wang, Qinqin Zhang, Jingkun Jiang, Lidan Zhu, Fan Li, Tao Huang, Takashi Kimoto, Kebin He","doi":"10.1021/acs.est.4c02727","DOIUrl":"10.1021/acs.est.4c02727","url":null,"abstract":"<p><p>Organosulfur and organonitrogen compounds (OrgSs and OrgNs) notably influence haze formation, reflecting the intricacies of sulfur and nitrogen chemistry in the atmospheric process. Despite this, a comprehensive understanding of OrgSs and OrgNs remains elusive. Here, we conducted molecular analyses of OrgSs and OrgNs in PM<sub>2.5</sub> concurrently during three haze episodes in winter and summer from 2016 to 2019. OrgSs and OrgNs collectively constituted 68.8-73.8% of identified organics, with CHON (35.8%) being the most prevalent followed by CHONS (13.6%), CHN (11.5%), CHOS (5.6%), CHNS (3.2%), and CHS (0.9%). Nitrogen within CHX (CH + CHN + CHS + CHNS) compounds were predominantly present as nitriles or amines, while sulfur existed as alkaline thioethers (ESI+) or acidic mercaptans and thiophenols (ESI-). Oxygen-containing OrgSs and OrgNs exhibited greater structural complexity. Specifically, most CHON were associated with nitric esters and nitro-compounds (ESI-), or basic amino acids (ESI+). CHONS primarily comprised nitrogen heterocyclic substances containing oxygen and sulfur, with some potentially containing organic sulfates (OSs) and organic nitrates if O ≥ 4S + 3N. CHOS with (O-3S)/C ≥ 0 were identified as sulfonic acids or sulfate esters. This comprehensive spectrum of OrgSs and OrgNs enhances the understanding of the physicochemical properties of aerosols, providing insights for future laboratory and air quality model studies.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"21692-21701"},"PeriodicalIF":10.8,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142737783","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
Form-Specific Prospective Environmental Risk Assessment of Graphene-Based Materials in European Freshwater. 欧洲淡水中石墨烯基材料的特定形式前瞻性环境风险评估。
IF 10.8 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-10 Epub Date: 2024-11-27 DOI: 10.1021/acs.est.4c05153
Hyunjoo Hong, Bernd Nowack
{"title":"Form-Specific Prospective Environmental Risk Assessment of Graphene-Based Materials in European Freshwater.","authors":"Hyunjoo Hong, Bernd Nowack","doi":"10.1021/acs.est.4c05153","DOIUrl":"10.1021/acs.est.4c05153","url":null,"abstract":"<p><p>As graphene-based materials (GBMs) such as pristine graphene, graphene oxide, and reduced graphene oxide show great potential to be integrated in various applications, the need for environmental risk assessments grows, aiming to navigate the environmental fate and potential risk of the different forms of GBM. This study used dynamic probabilistic material flow analysis (DPMFA) to ascertain the prospective production volumes and distribution of GBMs within European freshwaters. The hazard assessment leveraged 113 data sets from peer-reviewed studies, addressing aquatic ecotoxicity across 26 species, by performing probabilistic species sensitivity distributions (SSD). Our findings reveal distinct environmental distribution patterns for GBM forms with predicted environmental concentrations in European freshwaters by 2030 of approximately 0.67 ng/L (SD = 0.24 ng/L) for pristine graphene and 0.33 ng/L (SD = 0.10 ng/L) for both graphene oxide and reduced graphene oxide, suggesting not only similar but notably minimal exposure levels. The risk characterization ratios (RCRs) for all forms of GBM were significantly below 1, indicating a negligible environmental risk within the scenarios assessed. Through detailed analysis considering the forms of the material, this research can inform regulatory decisions, support sustainable material design, and provide a solid foundation for a further investigation considering the environmental fate of GBM.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"21750-21759"},"PeriodicalIF":10.8,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11636196/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142737712","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}
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
环境科学与技术 Pub Date : 2024-12-10 Epub 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
{"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":"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":"21794-21803"},"PeriodicalIF":10.8,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11636241/pdf/","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":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Bridging the Gap between Molecular Simulations and Surface Complexation Modeling for Heterogeneous Surfaces: A Case Study with Uranium and Arsenic Adsorption on Clay Minerals
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-10 DOI: 10.1021/acs.est.4c07338
Pengyuan Gao, Xiandong Liu, Zhijun Guo, Christophe Tournassat
{"title":"Bridging the Gap between Molecular Simulations and Surface Complexation Modeling for Heterogeneous Surfaces: A Case Study with Uranium and Arsenic Adsorption on Clay Minerals","authors":"Pengyuan Gao, Xiandong Liu, Zhijun Guo, Christophe Tournassat","doi":"10.1021/acs.est.4c07338","DOIUrl":"https://doi.org/10.1021/acs.est.4c07338","url":null,"abstract":"Among all natural submicrosized phases, clay minerals are ubiquitous in soils and sedimentary rocks in nature as well as in engineered environments, and while clay minerals’ adsorption properties have been studied extensively, their unique level of surface reactivity heterogeneities necessitates further investigation at the molecular level to understand and predict the influence of these heterogeneities on their macroscopic properties. In this study, we investigated the surface structures and desorption-free energies of U(VI) species (UO<sub>2</sub><sup>2+</sup>) and As(V) species (H<sub>2</sub>AsO<sub>4</sub><sup>–</sup> and HAsO<sub>4</sub><sup>2–</sup>) complexed at different edge surface reactive sites of a cis-vacant montmorillonite layer using first-principles molecular dynamics (FPMD). We show that U(VI) forms bidentate and tridentate complexes on montmorillonite edge surfaces, whereas As(V) monodentate complexes are the most stable. Then, we constrained a state-of-the-art surface complexation model (SCM) with surface acid–base chemistry and surface complexation properties obtained from the molecular-level simulation results. While our results highlighted the complexity of the interfacial chemistry controlling the complexation of inorganic contaminants on clay mineral surfaces, they also evidenced the reliability of an integrated workflow using modern multiscale simulation techniques to address the challenge of predicting heterogeneities in mineral surface reactivity.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"4 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797284","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
环境科学与技术 Pub Date : 2024-12-10 Epub 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
{"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":"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":"21871-21881"},"PeriodicalIF":10.8,"publicationDate":"2024-12-10","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
The Mobility of Mo during Microbially Mediated Ferrihydrite Phase Transformation. 微生物介导的铁酸盐相变过程中钼的流动性。
IF 10.8 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-10 Epub Date: 2024-11-27 DOI: 10.1021/acs.est.4c09144
Jing Zhang, Mengqiang Zhu, Jonathan R Lloyd, Samuel Shaw, Victoria S Coker, Jinxin Xie, Ke Wen, Sungsik Lee, Thomas L Goût, Jingyue Hao, Lin Ma, Yandi Hu, Bo Pan
{"title":"The Mobility of Mo during Microbially Mediated Ferrihydrite Phase Transformation.","authors":"Jing Zhang, Mengqiang Zhu, Jonathan R Lloyd, Samuel Shaw, Victoria S Coker, Jinxin Xie, Ke Wen, Sungsik Lee, Thomas L Goût, Jingyue Hao, Lin Ma, Yandi Hu, Bo Pan","doi":"10.1021/acs.est.4c09144","DOIUrl":"10.1021/acs.est.4c09144","url":null,"abstract":"<p><p>Molybdenum (Mo) is an essential nutrient for almost all organisms. However, at high concentrations, it can be toxic to animals and plants. This study investigated the interactions of Mo(VI) with iron oxyhydroxides during ferrihydrite bioreduction in the presence of Fe(III)-reducing <i>Geobacter sulfurreducens</i>. Here, we showed that Mo concentration controlled ferrihydrite phase transformation, leading to Mo release. With the biotic reduction of ferrihydrite and Fe(II) production, Mo(VI) reduction and Mo(IV)O<sub>2</sub> formation were observed for the first time, which further immobilized Mo after surface adsorption of Mo(VI). At low Mo levels (Mo/Fe molar ratios of 1-2%), sufficient Fe(II) adsorption onto ferrihydrite resulted in its transformation into magnetite nanoparticles (>80%, ∼25 nm), which catalyzed the reduction of Mo(VI) to form Mo(IV)O<sub>2</sub> and immobilized Mo. Contrastingly, at high Mo concentrations (Mo/Fe molar ratios of 5-10%), Mo(VI)O<sub>4</sub><sup>2-</sup> adsorption onto ferrihydrite limited Fe(II) adsorption; subsequently, less magnetite (<8-12%) formed while more goethite (∼30-50%, width and length >15 and 100 nm, respectively) and siderite (∼20-30%, width and length >100 and 200 nm, respectively) with larger particle sizes formed instead, causing Mo(VI) release due to lower Mo adsorption. This study provides a comprehensive understanding of the interaction mechanisms among <i>Geobacter sulfurreducens</i>, Mo(VI), and iron oxyhydroxides, enabling predictions and controls of long-term Mo mobility and Fe mineral transformation under a variety of biogeochemical scenarios.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"21653-21661"},"PeriodicalIF":10.8,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142737787","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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