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Visible-Light-Driven Four-Component Radical Relay Aminocarbonylation of Unactivated Alkenes

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Chinese Journal of Chemistry 2024年第9期42卷 990-996页

作者： Bin Lu Feng-Shuo Bao Zi-Wei He Wen-Jing Xiao Jia-Rong Chen engineering research center of photoenergy utilization for pollution control and carbon reduction College of ChemistryCentralChina Normal University152 Luoyu RoadWuhanHubei 430079China Wuhan Institute of Photochemistry and Technology 7North Bingang RoadWuhanHubei 430083China Key Laboratory of Organo-Pharmaceutical Chemistry of Jiangxi Province Gannan Normal UniversityGanzhouJiangxi 341000China

Catalytic four-component radical carbonylation of unactivated alkenes has recently been recognized as a robust protocol for rapid construction of various structurally diverse carbonyl *** the significance of fluorine-containing groups,this reaction class has been extensively applied to assembly of a variety of perfluoroalkyl carboxylic acid derivatives by transition metal ***,we report a visible-light-driven radical relay 1,2-perfluoroalkylation aminocarbonylation of unactivated alkenes using CO gas as carbonyl source and 4CzIPN as organic photocatalyst.A wide range of alkenes and amines were well tolerated,providing the valuableβ-perfluoroalkylated amides with generally good yields and high chemoselectivity.

关键词： Visible light Photoredox catalysis Radical aminocarbonylation Multicomponent reaction carbon monoxide Unactivated alkenes AmidesIReactionmechanisms

Unveiling the geometric site dependent activity of spinel Co_(3)O_(4)for electrocatalytic chlorine evolution reaction

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Journal of Energy Chemistry 2024年第5期92卷 95-103页

作者： Linke Cai Yao Liu Jingfang Zhang Qiqi Jia Jiacheng Guan Hongwei Sun Yu Yu Yi Huang Key Laboratory of Pesticide&Chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of EducationCollege of ChemistryCentral China Normal UniversityWuhan 430079HubeiChina Key Laboratory of Green Chemical engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Key Laboratory of Novel Reactor and Green Chemical TechnologySchool of Chemical Engineering&PharmacyWuhan Institute of TechnologyWuhan 430205HubeiChina College of Materials Science and engineering Fuzhou UniversityFuzhou 350108FujianChina School of Chemistry and Chemical engineering Anhui UniversityHefei 230601AnhuiChina

Spinel cobalt oxide(Co_(3)O_(4)),consisting of tetrahedral Co^(2+)(CoTd)and octahedral Co^(3+)(CoOh),is considered as promising earth-abundant electrocatalyst for chlorine evolution reaction(CER).Identifying the catalytic contribution of geometric Co site in the electrocatalytic CER plays a pivotal role to precisely modulate electronic configuration of active Co sites to boost ***,combining density functional theory calculations and experiment results assisted with operando analysis,we found that the Co_(Oh) site acts as the main active site for CER in spinel Co_(3)O_(4),which shows better Cl^(-)adsorption and more moderate intermediate adsorption toward CER than CoTd site,and does not undergo redox transition under CER condition at applied *** by above findings,the oxygen vacancies were further introduced into the Co_(3)O_(4) to precisely manipulate the electronic configuration of Co_(Oh) to boost Cl^(-)adsorption and optimize the reaction path of CER and thus to enhance the intrinsic CER activity *** work figures out the importance of geometric configuration dependent CER activity,shedding light on the rational design of advanced electrocatalysts from geometric configuration optimization at the atomic level.

关键词： Chlorine evolution reaction Geometry effects Active chlorine Electronic configuration optimization Spinel oxides

Dynamic steric confinement effect expands the frontier of Cu-catalyzed asymmetric propargylic aminations

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Science China Chemistry 2024年

作者： Peng Chen Mao-Mao Zhang Wen-Jing Xiao Liang-Qiu Lu engineering research center of photoenergy utilization for pollution control and carbon reduction Ministry of Education College of Chemistry Central China Normal University Wuhan Institute of Photochemistry and Technology State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics (LICP) Chinese Academy of Sciences School of Chemistry and Chemical engineering Henan Normal University

Chiral α-tertiary amines and related azacycles are commonly found in many natural products, pharmaceuticals and agrochemicals [1]. Copper-catalyzed asymmetric propargylic amination(APA) reactions have been established as a reliable method to access enantio-enriched propargylic amines,largely due to the seminal contribution of Nishibayashi et al.[2] and van Maarseveen et al. [3] in 2008.

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Effect of oxide interactions on chromium speciation transformation during simulated municipal solid waste incineration

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Journal of Environmental Sciences 2024年第8期142卷 11-20页

作者： Guodong Zhao Chong Tian Peidong Wu Xuguang Zhang Zhikang Wang Xiaoxiang Chen Zhuo Xiong Yongchun Zhao Junying Zhang State Key Laboratory of Coal Combustion School of Energy and Power EngineeringHuazhong University of Science and TechnologyWuhan 430074China School of Power and Mechanical engineering Wuhan UniversityWuhan 430072China National Environmental Protection engineering Technology center for Trace Elements pollution control and Low carbon utilization of Coal Huazhong University of Science and TechnologyWuhan 430074China School of Environmental engineering Wuhan Textile UniversityWuhan 430200China

Chromium released during municipal solid waste incineration(MSWI)is toxic and *** removal of chromium from simulated MSWI flue gas by four sorbents(CaO,bamboo charcoal(BC),powdered activated carbon(PAC),and Al_(2)O_(3))and the effects of four oxides(SiO_(2),Al_(2)O_(3),Fe_(2)O_(3),and CaO)on chromium speciation transformationwere *** results showed that the removal rates of total Cr by the four sorbents were Al_(2)O_(3)reduction of Na_(2)CrO_(4)and K_(2)CrO_(4)above 1000℃due to its strong acidity,and the addition of CaO significantly inhibited the reduction of Cr(Ⅵ).MgCrO_(4)decomposed above 700℃to form MgCr_(2)O_(4),and the reaction between MgCrO_(4)and oxides also existed in the form of a more stable trivalent ***,when investigating the effect of oxides on the oxidation of Cr(Ⅲ)in CrC_(l3),it was discovered that CaO promoted the conversion of Cr(Ⅲ)to Cr(Ⅵ),while the presence of chlorine caused chromium to exist in the form of Cr(V),and increasing the content of CaO and extending the heating time facilitated the oxidation of Cr(Ⅲ).In addition,silicate,aluminate,and ferrite were generated after the addition of SiO_(2),Al_(2)O_(3),and Fe_(2)O_(3),which reduced the alkalinity of CaO and had an important role in inhibiting the oxidation of Cr(Ⅲ).The acidic oxides can not only promote the reduction of Cr(Ⅵ)but also have an inhibitory effect on the oxidation of Cr(Ⅲ)ascribed to alkali metals/alkaline earth metals,and the proportion of acidic oxides can be increased moderately to reduce the generation of harmful substances in the hazardous solid waste heat treatment.

关键词： Cr(Ⅵ)reduction Cr(Ⅲ)oxidation Alkali oxides Acidic oxides Municipal solid waste incineration

Electrostatic removal of ultrafine carbon black with square-grooved collecting plates:Insights for capturing black carbon emitted from ships

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Journal of Environmental Sciences 2024年第2期136卷 559-569页

作者： Zhicheng Wu YifanWang Lingyu Shao Hao Zhang Haobo Dai Haidong Fan Chenghang Zheng Xiang Gao State Key Lab of Clean Energy utilization State Environmental Protection Engineering Center for Coal-Fired Air Pollution ControlZhejiang UniversityHangzhou 310027China Department of Earth and Environmental Sciences University of ManchesterOxford RoadUnited Kingdom Zhejiang Tiandi Environmental Protection engineering Co. Ltd.Hangzhou 310012China Baima Lake Laboratory(Zhejiang Provincial Laboratory of Energy and carbon Neutrality) Hangzhou 310000China

Ships and other mobile pollution sources emitted massive ultrafine and low-resistivity particles containing black carbon(BC),which were harmful to human health and were difficult to capture by conventional electrostatic precipitators(ESPs).In this study,nanoscale carbon black was adopted as simulated particles(SP)with similar physicochemical properties for black carbon emitted from ships(SP-BC)to investigate the feasibility of using an ESP with square-grooved collecting plates for the removal of SP-BC at low *** increased applied voltage significantly improved the total collection of SP-BC whereas may also promote the conversion of relatively larger particle size SP-BC into nano-size below *** outlet number concentration of SP-BC under 27 kV at 130℃was three times that of the *** the reduction of the flow rate could strengthen the capture of SP-BC below20 nm,and under the combined action of low flow rate and maximum applied voltage,the collection efficiency of 20-100 nm SP-BC could exceed 90%.In addition,the escape and capture characteristics of SP-BC under long-term rapping were *** square-grooved collecting plate could effectively restrain the re-entrainment of collected SP-BC generated by rapping,and the nanoscale SP-BC was trapped in the grooves after *** results could provide insights into the profound removal of massive nanoscale black carbon emissions from mobile sources.

关键词： Simulated ship black carbon Electrostatic removal Square-grooved collecting plate Long-term rapping

Application of UiO-66 and its composites for remediation and resource recovery of typical environmental contaminants:a review

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Rare Metals 2024年第6期43卷 2498-2526页

作者： Hui-Min Zhang Yun-Long Wang Xin-Feng Zhu Zhen-Zhen Huang Dan-Dan Pang Kai Wang Chao-Hai Wang Zhong-Xian Song Shi-Qiang Yin Lin-Lin Chang Jin-Hui Zhang School Infirmary Henan University of Urban ConstructionPingdingshan 467036China Faculty of Environmental and Municipal engineering Henan Key Laboratory of Water Pollution Control and Rehabilitation TechnologyKey Laboratory of Carbon Emission Reduction and Combined Air Pollution Control TechnologyHenan University of Urban ConstructionPingdingshan 467036China School of Resources&Environment Collaborative Innovation Center of Coalbed Methane and Shale Gas for Central Plains Economic RegionHenan Polytechnic UniversityJiaozuo 454003China The Key Lab of pollution control and Ecosystem Restoration in Industry Clusters Ministry of EducationGuangzhou Higher Education Mega CentreSouth China University of TechnologyGuangzhou 510006China

UiO-66 series metal-organic framework materials(MOFs)are typical porous materials assembled by Zr^(4+) with a large mass-to-nucleus ratio and terephthalic acid ligands,which form tetrahedral and octahedral cages arranged in a periodic triangular window *** to the strong interaction between Zr and O,UiO-66 series MOFs exhibit high thermal stability,structural stability,and chemical *** article mainly reviews the applications of UiO-66 and its composites in adsorption,photocatalysis,and resource utilization,while exploring the harm of pollutants to human health and the *** the first part,the differences in adsorption and removal mechanisms of liquid organic pollutants,heavy metals,and volatile organic compounds(VOCs)are *** results show that organic pollutants are mainly removed by physical adsorption,electrostatic interactions,hydrogen bonding,andπ-πinteractions,while heavy metals are mainly removed by chemical adsorption,electrostatic interactions,reduction,and *** are mainly removed by the pore volume and pore size structure of the *** catalysis can achieve non-toxic treatment of pollutants,and this study mainly focuses on UiO-based composite materials constructed by strategies such as semiconductor composites,ion doping,and metal/dye *** the second part,the synergistic effect between the components of UiO-based composite materials promotes the oriented and rapid separation and transfer of earriers at the material interface,thereby promoting the generation of active species such as h^(+),·O_(2)^(-) and·OH,and achieving rapid degradation of pollutants and detoxification of heavy *** the third part,heterojunctions can realize the resource utilization of pollutants in water and air,producing energy-type substances such as hydrogen and methanol while solving environmental *** addition,this article also summarizes the harm of common typical pollutants to the environment

关键词： UiO Adsorption Photocatalysis Environmental pollution Resource recovery

Metallaphotoredox-Catalyzed Three-Component Couplings for Practical Synthesis of Ureas and Carbamates

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Chinese Journal of Chemistry 2024年第3期42卷 264-270页

作者： Ernest Koranteng Zhen-Cao Shu Yi-Yin Liu Qian Yang Bin Shi Qiang-Xian Wu Fen Tan Liang-Qiu Lu Wen-Jing Xiao engineering research center of photoenergy utilization for pollution control and carbon reduction Ministry of EducationCollege of ChemistryCentral China Normal University152 Luoyu RoadWuhanHubei430079 China Wuhan Youji Industries Co. LtdNo.1 2nd Chemical Rd.WuhanHubei430082 China Hubei Key Laboratory of Purification and Application of Plant Anti-cancer Active Ingredients School of Chemistry and Life SciencesHubei University of EducationWuhanHubei430205 China State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhouGansu730000 China School of Chemistry and Chemical engineering Henan Normal UniversityXinxiangHenan453007 China Wuhan Institute of Photochemistry and Technology WuhanHubei430082 China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai200032 China

Ureas are widely used in drugs,materials and catalysts because of their diamide structure,which can form strong hydrogen ***,it is of great scientific significance to develop efficient and green methods for the synthesis of urea compounds,especially unsymmetrical ***,we have disclosed novel and highly efficient three-component coupling reactions of organic halides,sodium cyanate and amines enabled by nickel/photoredox dual catalysis for the preparation of unsymmetrical *** reaction features simple and safe operations,broad substrate scopes,and product *** allows the facile synthesis of N-aryl/vinyl ureas from readily available,user-friendly feedstocks under mild conditions(27 examples,36%—98%yields).In addition,this method is further derived to alcohols as nucleophiles to synthesize a series of carbamates(15 examples,40%—95%yields).The mechanism experiment shows that the isocyanate produced by the coupling of halide and sodium cyanate may be the key intermediate in this reaction.

关键词： Cross-coupling Nickel Photoredox catalysis Three-component reaction Ureas Carbamates

Molecular behavior and interactions with microbes during anaerobic degradation of bio-derived DOM in waste leachate

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Journal of Environmental Sciences 2023年第4期126卷 174-183页

作者： Junjie Qiu Tianqi Li Fan Lü Yulong Huang Chao Li Hua Zhang Liming Shao Pinjing He Institute of Waste Treatment and Reclamation Tongji UniversityShanghai 200092China Shanghai Institute of pollution control and Ecological Security Shanghai 200092China Shanghai engineering research center of Multi-source Solid Wastes Co-Processing and Energy utilization Shanghai 200092China

It is the key to control bio-derived dissolved organic matters (DOM) in order to reduce the effluent concentration of wastewater treatment, especially for waste leachate with high organic contaminants. In the present study, the anaerobic degradation of aerobically stabilized DOM was investigated with DOM substrate isolated through electrodialysis. The degradation of bio-derived DOM was confirmed by reduction of 15%of total organic carbon in 100 *** characterized the molecular behavior of bio-derived DOM by coupling molecular and biological information analysis. Venn based Sankey diagram of mass features showed the transformation of bio-derived DOM mass features. Occurrence frequency analysis divided mass features into six categories so as to distinguish the fates of intermediate metabolites and persistent compounds. Reactivity continuum model and machine learning technologies realized the semi-quantitative determination on the kinetics of DOM mass features in the form of pseudo-first order, and confirmed the reduction of inert mass features. Furthermore, network analysis statistically establish relationship between DOM mass features and microbes to identify the active microbes that are able to utilize bio-derived DOM. This work confirmed the biological technology is still effective in controlling recalcitrant bio-derived DOM during wastewater treatment.

关键词： Soluble microbial products Data mining Machine learning Solid waste Orbitrap

A highly porous animal bone-derived char with a superiority of promoting nZVI for Cr(Ⅵ)sequestration in agricultural soils

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Journal of Environmental Sciences 2021年第6期33卷 27-39页

作者： Kai Liu Fangbai Li Qingwen Tian Chengrong Nie Yibing Ma Zhenlong Zhu Liping Fang Yuanying Huang Siwen Liu Guangdong Key Laboratory of Integrated Agro-environmental pollution control and Management Institute of Eco-environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China National-Regional Joint engineering research center for Soil pollution control and Remediation in South China Guangzhou 510650China School of Food Science and engineering Foshan universityFoshan 528225China Macao Environmental research Institute Macao University of Science and TechnologyTaipaMacaoChina National research center for Geoanalysis Beijing 100037China Key Laboratory of Ministry of Natural Resources for Eco-geochemistry Beijing 100037China

Paddy soil and irrigation water are commonly contaminated with hexavalent chromium[Cr(Ⅵ)]near urban industrial areas,thereby threatening the safety of agricultural products and human *** this study,we develop a porous and high specific area bone char(BC)to support nanoscale zero-valent iron(n ZVI)and apply it to remediate Cr(Ⅵ)pollution in water and paddy soil under anaerobic *** batch experiments reveal that BC/n ZVI exhibits a higher removal capacity of 516.7 mg/(g·n ZVI)for Cr(Ⅵ)than n ZVI when normalized to the actual n ZVI content,which is 2.8 times that of n ZVI;moreover,the highest n ZVI utilization is the n ZVI loading of 15%(BC/n ZVI15).The Cr(Ⅵ)removal efficiency of BC/n ZVI15 decreases with increasing p H(4–10).Coexisting ions(phosphate and carbonate)and humic acid can inhibit the removal of Cr(Ⅵ)with BC/n ***,BC exhibits a strong advantage in promoting Cr(Ⅵ)removal by n ZVI compared to the widely used biochar and activated *** results demonstrate that reduction and coprecipitation are the dominant Cr(Ⅵ)removal ***,BC/n ZVI15 shows a significantly higher reduction and removal efficiency as well as a strong anti-interference ability for Cr(Ⅵ)in paddy soil,as compared to n *** findings provide a new effective material for remediating Cr(Ⅵ)pollution from water and soil.

关键词： Bone char Nano zero-valent iron Adsorption Chromium reduction