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

作     者：YIN ShiMei GAO YiXuan CHEN Long LI Fan LIU XiaoNa QI Fei LIU Wen 

作者机构：Beijing Key Lab for Source Control Technology of Water PollutionCollege 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 EngineeringTaiyuan University of TechnologyTaiyuan 030024China State Environmental Protection Key Laboratory of All Material Fluxes in River EcosystemsPeking UniversityBeijing 100871China Beijing National Laboratory for Molecular SciencesPeking UniversityBeijing 100871China 

出 版 物：《Science China(Technological Sciences)》 (中国科学（技术科学英文版）)

年 卷 期：2024年第67卷第10期

页      面：3103-3115页

核心收录：

学科分类：083002[工学-环境工程] 0830[工学-环境科学与工程（可授工学、理学、农学学位）] 081705[工学-工业催化] 07[理学] 070205[理学-凝聚态物理] 08[工学] 0817[工学-化学工程与技术] 080501[工学-材料物理与化学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0702[理学-物理学] 

基　　金：supported by the National Key Research and Development Program of China (Grant Nos. 2021YFE010080, 2021YFA1202500, and 2023YFC3209600) the National Natural Science Foundation of China (NSFC) (Grant Nos. 52200083 and 52270053) Beijing Natural Science Foundation (Grant No. 8232035) Beijing Nova Program (Grant No. 20220484215) Beijing National Laboratory for Molecular Sciences (Grant No. BNLMS2023011) the Emerging Engineering Interdisciplinary-Young Scholars Project (Peking University) Horizontal Scientific Research Funds of Taiyuan University of Technology (Grant No. RH2300002821) the Science and Technology Projects of Shanxi Transportation Holdings Group Co., Ltd. (Grant No. 2022-JKKJ-8) the Fundamental Research Funds for the Central Universities supported by the High-Performance Computing Platform of Peking University 

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

摘      要：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.