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Mechanism for the promotional formation of NH_(4)^(+) by SO_(2) on different mineral dust surfaces

Particuology 2023年第4期75卷 109-118页

作者： Hao Li Qingxin Ma Biwu Chu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-environmental SciencesChinese Academy of SciencesBeijing100085China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen361021China Institute of Atmospheric Physics Chinese Academy of SciencesBeijing100029China

Ammonium is an important atmospheric particulate component that dictates many environmental *** promotion of the heterogeneous conversion of NH_(3) to NH_(4)^(+) by SO_(2) on different mineral dust surfaces displays remarkable discrepancies,especially on MgO and α-Fe2O3 surfaces,however,the underlying mechanisms are not well ***,using periodic density functional theory(DFT)calculation and Born-Oppenheimer molecular dynamics(BOMD)simulation,we explored the hetero-geneous adsorption of NH_(3) on MgO(110)and α--Fe2O3(001)surfaces in the presence and absence of SO_(2).The results show that on MgO(110)surface,hydrogen-bonding interactions of NH_(3) on both adsorbed hydroxyl or bisulfite/bisulfate sites are observed no matter whether SO_(2) is present or ***,on theα-Fe2O3(001)surface,significant conversion of NH_(3) to NH_(4)^(+)occurs with the coexistence of SO_(2),which is due to the hydrogen transfer reaction from surface HSO4 to N in NH_(3).The fundamental reason may be that the stronger electron affinity of Fe3+than Mg2+results in adsorbed bisulfate and/or bisulfite with greater acidity on α-Fe2O3 surface than MgO *** results give a molecular-level explanation for the heterogeneous conversion of NH_(3) to NH_(4)^(+)on different mineral dust surfaces under complex air pollution *** the fact that ammonium is abundant in secondary particulates,this work would help in understanding the rapid conversion of ammonia to ammonium and in developing classification governance policies for the key precursor pollutants in China.

关键词： Mineral dust Heterogeneous reaction Theoretical calculation Ammonium SO_(2)

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Development and assessment of an onsite large volume solid phase extraction (LV-SPE) device for the determination of pharmaceuticals and personal care products (PPCPs) in water

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Emerging Contaminants 2024年第1期10卷 24-31页

作者： Xue Cheng Ning Fang Yuxi Ge Wenchao Li Yamei Hui Zilong Tang Yu Wan Yuancheng Li State Key Joint Laboratory of Environmental Simulation and Pollution Control(SKLESPC) Beijing Key Laboratory for Emerging Organic Contaminants Control(BKLEOC)Beijing Laboratory for Environmental Frontier Technologies(BLEFT)School of EnvironmentTsinghua UniversityBeijing100084China CSD IDEA(Beijing)Environmental Test and Analysis Co. Ltd.Beijing100192China School of Public Health Shandong First Medical University&Shandong Academy of Medical ScienceShandong Province250117China

It is essential to determine the occurrence of emerging organic contaminants(EOCs),such as pharmaceuticals and personal care products(PPCPs),in the ambient environment to address growing public ***,such analysis is quite challenging due to the low trace level of such contaminants in water,which therefore requires several litres of water *** this study,a large volume solid phase extraction(LV-SPE)device was developed and evaluated for its performance in monitoring PPCPs as an *** good recoveries and reproducibility were obtained under specific operating conditions:a water sample volume of no more than 20 L,a flow rate not exceeding 120 mL/min,and a methanol elution volume of at least 30 *** addition,the results from the onsite enrichment approach using LV-SPE were compared with those from the conventional approach using a standard SPE device in the laboratory for real groundwater *** the eight selected PPCPs(nalidixic acid,carbamazepine,bezafibrate,clofibric acid,sulfadiazine,sulfamethoxypyridazine,sulfamethazine and sulfamonomethoxine),LV-SPE approach detected more target *** the detected concentrations were generally comparable,slightly higher concentrations were observed for carbamazepine,clofibric acid,sulfadiazine and sulfamethazine using the LV-SPE *** developed LV-SPE device provides an alternative approach for trace analysis of PPCPs and may also be applicable for other emerging organic contaminants.

关键词： Large-volume Solid phase extraction Onsite enrichment PPCPs Emerging organic pollutants

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Recent advances,challenges,and perspectives on carbon capture

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Frontiers of environmental Science & Engineering 2024年第6期18卷 75-104页

作者： Shihan Zhang Yao Shen Chenghang Zheng Qianqian Xu Yifang Sun Min Huang Lu Li Xiongwei Yang Hao Zhou Heliang Ma Zhendong Li Yuanhang Zhang Wenqing Liu Xiang Gao Institute of Energy and Sustainable Development Zhejiang University of TechnologyHangzhou 310014China College of Environment Zhejiang University of TechnologyHangzhou 310014China Baima Lake Laboratory Hangzhou 310051China Institute of Carbon Neutrality College of Energy EngineeringZhejiang UniversityHangzhou 310027China State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China Key Laboratory of Environmental Optics and Technology Anhui Institute of Optics and Fine MechanicsHFIPSChinese Academy of SciencesHefei 230031China

Carbon capture,utilization and storage(CCUS)technologies play an essential role in achieving Net Zero Emissions *** the lack of timely reviews on the recent advancements in promising CCUS technologies,it is crucial to provide a prompt review of the CCUS advances to understand the current research gaps pertained to its industrial *** that end,this review first summarized the developmental history of CCUS technologies and the current large-scale ***,based on a visually bibliometric analysis,the carbon capture remains a hotspot in the CCUS *** that the materials applied in the carbon capture process determines its *** a result,the state-of-the-art carbon capture materials and emerging capture technologies were comprehensively summarized and *** between state-of-art carbon capture process and its ideal counterpart are analyzed,and insights into the research needs such as material design,process optimization,environmental impact,and technical and economic assessments are provided.

关键词： Carbon capture,utilization and storage Visualization analysis Research hotspots and trends CO_(2)capture technology

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Mixing regime shapes the community assembly process,microbial interaction and proliferation of cyanobacterial species Planktothrix in a stratified lake

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Journal of environmental Sciences 2022年第5期34卷 103-113页

作者： Junwen Chen Huacong Liu Yaohui Bai Jing Qi Weixiao Qi Huijuan Liu Jianfeng Peng Jiuhui Qu Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution ControlSchool of EnvironmentTsinghua UniversityBeijing 100084China Key Laboratory of Drinking Water Science and Technology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

Lake mixing influences aquatic chemical properties and microbial community composition,and thus,we hypothesized that it would alter microbial community assembly and *** clarify this issue,we explored the community assembly processes and cooccurrence networks in four seasons at two depths(epilimnion and hypolimnion)in a mesotrophic and stratified lake(Chenghai Lake),which formed stratification in the summer and turnover in the *** the stratification period,the epilimnion and hypolimnion went through contrary assembly processes but converged to similar assembly patterns in the mixing *** a highly homogeneous selection environment,species with low niche breadth were filtered,resulting in decreased species *** mixing in the winter homogenized the environment,resulting in a simpler microbial cooccurrence ***,we observed a high abundance of the cyanobacterial genus Planktothrix in the winter,proba-bly due to nutrient redistribution and Planktothrix adaptivity to the winter environment in which mixing played important *** study provides deeper fundamental insights into how environmental factors influence microbial community structure through community assembly processes.

关键词： Stratified lake Water mixing Microbial community assembly Microbial interaction Planktothrix

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Screening legacy and emerging organic pollutants in the contaminated soil of Dhaka,Bangladesh

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Emerging Contaminants 2024年第3期10卷 343-353页

作者： Refayat Nigar Shizhen Zhao Xin Liu Huanfang Huang Lele Tian Yuwei Xiao Ahsan Habib Gan Zhang State Key Laboratory of Organic Geochemistry Guangzhou Institute of GeochemistryChinese Academy of SciencesGuangzhou510640China Guangdong-Hong Kong-Macao Joint Laboratory for Environmental Pollution and Control and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization Guangzhou510640China Anti-Drug Technology Center of Guangdong Province and National Anti-Drug Laboratory Guangdong Regional Center Guangzhou510230China State Environmental Protection Key Laboratory of Water Environmental Simulation and Pollution Control South China Institute of Environmental SciencesMinistry of Ecology and EnvironmentGuangzhou510530China Department of Chemistry University of DhakaDhaka1000Bangladesh University of Chinese Academy of Sciences Beijing100049China

The current understanding of the legacy and emerging organic pollutants in the soil of Bangladesh remains *** disposal practices,particularly in e-waste,landfills,and industrial operations,may lead to the pervasive presence of persistent organic pollutants(POPs)and polycyclic aromatic hydrocarbons(PAHs)in the *** study aimed to systematically investigate the concentrations,sources,and risk assessment of halogenated flame retardants(HFRs),polychlorinated biphenyls(PCBs),polychlorinated naphthalenes(PCNs),organochlorine pesticides(OCPs),chlorinated paraffins(CPs),and PAHs in the contaminated soil of Dhaka's dumpsites,e-waste,and industrial areas collected in *** total concentration of investigated pollutants averaged at 4790±4040 ng g^(-1)dw,with the following order:P44CPs(4110±4140 ng g^(-1)dw)>P16PAHs(422±491 ng g^(-1)dw)>P16HFRs(190±538 ng g^(-1)dw)>P209PCBs(43.5±73.5 ng g^(-1)dw)>P50PCNs(17.7±21.0 ng g^(-1)dw)>P27OCPs(9.41±9.61 ng g^(-1)dw).The e-waste site exhibited the highest total concentration of the target pollutants,reaching 12,700 ng g1 *** were the predominant contributors,accounting for averages of 81.8%,70.5%,and 68.5%to waste landfills,e-waste,and industrial sites,respectively.A comprehensive analysis of 209 PCB congeners revealed their primary origin from Aroclor PCBs,with minor contributions from unintentionally produced *** highest incremental lifetime carcinogenic risk(ILCR)occurred in e-waste sites,contributed by dioxin-like PCBs,with a maximum value of 5.9×10^(-5)for adults,exceeding the limit 1.0×10^(-6)set by the *** non-carcinogenic hazard quotients(HQs)were much lower,suggesting no significant risk from the investigated *** findings highlight the importance of proper waste management and regulated e-waste recycling to mitigate potential hazardous risks to the Bangladeshi population.

关键词： Persistent organic pollutants Polycyclic aromatic hydrocarbons Chlorinated paraffins Polychlorinated biphenyls Risk assessment Contaminated soil Bangladesh

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Peracetic acid catalytic activation using Co_(3)O_(4) nanocluster decorated graphitic carbon nitride for cefapirin degradation in water

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Science China(Technological Sciences) 2024年第10期67卷 3103-3115页

作者： YIN ShiMei GAO YiXuan CHEN Long LI Fan LIU XiaoNa QI Fei LIU Wen Beijing Key Lab for Source Control Technology of Water Pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China Key Laboratory of Water and Sediment Sciences(Ministry of Education) College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China School of Environmental Science and Engineering Taiyuan University of TechnologyTaiyuan 030024China State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems Peking UniversityBeijing 100871China Beijing National Laboratory for Molecular Sciences Peking UniversityBeijing 100871China

This study innovated cobalt-based catalytic nanocomposites(CCNs)for the heterogeneous activation of peracetic acid(PAA),a green and efficient advanced oxidation process for removing antibiotics from *** Co_(3)O_(4) catalysts exhibit limited activity due to stable electronic *** overcome this,CCNs were synthesized using a one-step condensation method,incorporating a size control strategy that anchors Co_(3)O_(4) nanoclusters within 4‒5 nm onto six-fold cavity of g-C3N4,simultaneously modifying the coordination environment of *** alteration significantly enhances the adsorption energy of PAA and catalytic activity compared to commercial Co_(3)O_(4).The improved performance of CCN2,in particular,is attributed to a shift in the cobalt d band center towards the Fermi level,facilitating electron delocalization and transfer,enhancing Co‒O bonding,and accelerating PAA ***2’s superior activity,with a cefapirin(CFP)degradation kinetic rate constant(k1=0.760 min^(−1))~11 times that of PAA direct oxidation(k1=0.070 min^(−1))and~5 times that of commercial Co_(3)O_(4)/PAA system(k1=0.164 min^(−1)),is due to its ability to generate dominant reactive species for antibiotic degradation,including alkoxy radicals(CH3C(=O)OO•),high valence metal(Co^(Ⅳ)(=O)^(2+)),and singlet oxygen(^(1)O_(2)),with the latter two being crucial for the degradation *** degradation of CFP involved three mechanisms,including direct oxidation by PAA,decarboxylation,and open-ring reactions at nitrogen *** research provides insights into developing high-activity catalysts for efficient PAA activation and antibiotic removal,leveraging the strategy of shifting the transition metal d band center.

关键词： peracetic acid Co_(3)O_(4)nanocluster high valence metal singlet oxygen cefapirin

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Trends and drivers of anthropogenic NOx emissions in China since 2020

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environmental Science and Ecotechnology 2024年第5期21卷 287-293页

作者： Hui Li Bo Zheng Yu Lei Didier Hauglustaine Cuihong Chen Xin Lin Yi Zhang Qiang Zhang Kebin He Shenzhen Key Laboratory of Ecological Remediation and Carbon Sequestration Institute of Environment and EcologyTsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing 100084China State Environmental Protection Key Laboratory of Environmental Planning and Policy Simulation and Center of Air Quality Simulation and System Analysis Chinese Academy of Environmental PlanningBeijing 100041China Laboratoire des Sciences du Climat et de l’Environnement LSCE/IPSLCEA-CNRS-UVSQUniversite Paris-SaclayGif-sur-YvetteFrance Center for Satellite Application on Ecology and Environment Ministry of Ecology and Environment of ChinaBeijing 100094China Institute of Future Human Habitats Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China Ministry of Education Key Laboratory for Earth System Modeling Department of Earth System ScienceTsinghua UniversityBeijing 100084China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China

Nitrogen oxides(NOx),significant contributors to air pollution and climate change,form aerosols and ozone in the ***,timely,and transparent information on NOx emissions is essential for decision-making to mitigate both haze and ozone ***,a comprehensive understanding of the trends and drivers behind anthropogenic NOx emissions from Chinadthe world's largest emitterdhas been lacking since 2020 due to delays in emissions *** we show a consistent decline in China's NOx emissions from 2020 to 2022,despite increased fossil fuel consumption,utilizing satellite observations as constraints for NOx emission estimates through atmospheric *** reduction is corroborated by data from two independent spaceborne instruments:the TROPOspheric Monitoring Instrument(TROPOMI)and the Ozone Monitoring Instrument(OMI).Notably,a reduction in transport emissions,largely due to the COVID-19 lockdowns,slightly decreased China's NOx emissions in *** subsequent years,2021 and 2022,reductions in NOx emissions were driven by the industry and transport sectors,influenced by stringent air pollution *** satellite-based inversion system developed in this study represents a significant advancement in the real-time monitoring of regional air pollution emissions from space.

关键词： China's NOx emissions pollution control Socio-economic drivers Atmospheric inversion

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Eutrophication in cold-arid lakes: molecular characteristics and transformation mechanism of DOM under microbial action at the ice-water interface

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Carbon Research 2024年第1期3卷 1-17页

作者： Wang, Tengke Feng, Weiying Liu, Jing Fan, Wenhong Li, Tingting Song, Fanhao Yang, Fang Liao, Haiqing Leppäranta, Matti School of Materials Science and Engineering Beihang University Beijing100191 China Environment Research Institute Shandong University Qingdao266273 China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental Sciences Beijing100012 China State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing100084 China Institute for Atmospheric and Earth System Research University of Helsinki Helsinki00014 Finland

During freezing periods, nutrients (carbon and organic matter, etc.) are enriched in the water and sediment of lakes in cold-arid regions, leading to potential algal bloom outbreaks and other health risks to the ecosystem. Particularly, dissolved organic matter (DOM) is a critical component of the nutrients and plays an important role in the global carbon cycle. However, the mechanisms of DOM transfer between ice and water remain unclear. This study analyzed the influence of microbial community on DOM composition using 16 s RNA, 3DEEM, and FT-ICR MS in Daihai Lake and Wuliangsuhai Lake in the Yellow River Basin, China. According to the spectral analysis, the content of endogenous organic matter, such as humus, accounted for 40% of the total DOM in water, while the content of tryptophan and tyrosine accounted for 80% of the total DOM in ice. The results of mass spectrometry showed that lignin was the main component, and the content of organic matter in the ice was less than that in the water. Molecular structures of seven DOM coexisting in the lake ice and water were elucidated with adapted Kendrick-analogous network visualization, which clearly illustrates that long-chain DOM molecules are derived from small molecules, while other heteroatoms are complexed with the side groups. The positive correlations between CHO, CHNO, CHOS, CHOS and Actinomyces indicate that DOM actively interacted with the microbial community. 44% of CHO compounds have the same molecular formula in water, the content of CHOS in the water of the two lakes was closed to 7% higher than that in the ice. Meanwhile, DOM dynamically migrate between ice and water via interstitial water because of the solubility changes under microbial transformation, which has been proved by the decrease in the contents of the humus and tryptophan-like substances in the ice from the bottom to the surface and lower contents of carbohydrate and unsaturated aromatic hydrocarbon in the water than the ice. This study helps

关键词： Aromatization

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Insight into the effects of C_(3)H_(6)on fresh and hydrothermally aged Cu-SSZ-39 catalysts

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Chinese Chemical Letters 2025年第3期36卷 164-169页

作者： Jinpeng Du Junlin Chen Yulong Shan Tongliang Zhang Yu Sun Zhongqi Liu Xiaoyan Shi Wenpo Shan Yunbo Yu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341119China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China

Hydrocarbons(HCs),as major poisoning substances,have a crucial influence on NH_(3)-SCR *** this work,the effects of C_(3)H_(6)on fresh and hydrothermally aged Cu-SSZ-39 catalysts with different copper contents were *** catalysts suffered a deactivation above 250℃,especially between 300-400℃,which was mainly related to the reaction between NH_(3)and C_(3)H_(6).However,the hydrothermally aged and the high-copper-loaded Cu-SSZ-39 catalysts could achieve a recovery of NH_(3)-SCR performance at high *** activity recovery was attributed to the oxidation of C_(3)H_(6)by CuxOy species,which therefore inhibited the reaction between NH_(3)and C_(3)H_(6).As a result,more NH_(3)could be available for the NH_(3)-SCR reaction and the Cu-SSZ-39 catalysts could maintain a good catalytic *** on these findings,we proposed that high loaded Cu-SSZ-39 catalysts with a little CuOx formed are preferred for application.

关键词： Diesel vehicle emission NO_(x)abatement NH3-SCR Cu-SSZ-39 zeolite C_(3)H_(6)poisoning

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The effect of hydrogen reduction of α-MnO_(2) on formaldehyde oxidation: The roles of oxygen vacancies

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Chinese Chemical Letters 2023年第3期34卷 171-174页

作者： Liping Zhou Chunying Wang Yaobin Li Xiaofeng Liu Hua Deng Wenpo Shan Hong He College of Resources and Environmental Sciences Fujian Agriculture and Forestry UniversityFuzhou 350002China Center for Excellence in Regional Atmospheric Environment Key Laboratory of Urban Pollutant ConversionInstitute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Zhejiang Key Laboratory of Urban Environmental Processes and Pollution Control Ningbo Urban Environment Observation and Research StationInstitute of Urban EnvironmentChinese Academy of SciencesNingbo 315800China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

A series of α-MnO_(2) catalysts with various Mn valence states were treated by hydrogen reduction for different periods of time. Their catalytic capacity for formaldehyde(HCHO) oxidation was evaluated. The results indicated that hydrogen reduction dramatically improves the catalytic performance of α-MnO_(2) in HCHO oxidation. The α-MnO_(2) sample reduced by hydrogen for 2 h possessed superior activity and could completely oxidize 150 ppm HCHO to CO_(2) and H_(2)O at 70℃. Multiple characterization results illustrated that hydrogen reduction contributed to the production of more oxygen vacancies. The oxygen vacancies on the catalyst surface enhanced the adsorption, activation and mobility of O_(2) molecules, and thereby enhanced HCHO catalytic oxidation. This study provides novel insight into the design of outstanding MnO_x catalysts for HCHO oxidation at low temperature.

关键词： Hydrogen reduction α-MnO_(2) Formaldehyde oxidation Oxygen vacancies

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