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作 者:Zhiwei Zhou Qianqian Li Guijin Su Jiaxin Pang Bohua Sun Jing Meng Bin Shi
机构地区:[1]Henan Institute of Advanced Technology,Zhengzhou University,Zhengzhou 450052,China [2]Key Laboratory of Environmental Nanotechnology and Health Effects,State Key Laboratory of Environmental Chemistry and Ecotoxicology,Research Center for Eco-Environmental Sciences,Chinese Academy of Sciences,Beijing 100085,China [3]University of Chinese Academy of Sciences,Beijing 100049,China
出 处:《Journal of Environmental Sciences》2024年第4期326-338,共13页环境科学学报(英文版)
基 金:supported by the National Key R&D Program of China(No.2020YFC1910100);the National Natural Science Foundation of China(Nos.22006156 and 21876193);the Chengdu Science and Technology Bureau(No.2018-ZM01-00019-SN);the Youth Innovation Promotion Association CAS。
摘 要:Developing industrially moldable catalysts with harmonized redox performance and acidity is of great significance for the efficient disposal of chlorinated volatile organic compounds(CVOCs)in actual exhaust gasses.Here,commercial TiO_(2),typically used for molding catalysts,was chosen as the carrier to fabricate a series of Ce_(0.02)Mn_(0-0.24)TiO_(x) materials with different Mn doping ratios and employed for chlorobenzene(CB)destruction.The introduction of Mn remarkedly facilitated the synergistic effect of each element via the electron transfer processes:Ce^(3+)+Mn^(4+/3+)■Ce^(4+)+Mn^(3+/2+)and Mn^(4+/3+)+Ti^(4+)■Mn^(3+/2+)+Ti^(3+).These synergistic interactions in Ce_(0.02)Mn_(0.04-0.24)TiO_(x),especially Ce_(0.02)Mn_(0.16)TiO_(x),significantly elevated the active oxygen species,oxygen vacancies and redox properties,endowing the superior catalytic oxidation of CB.When the Mn doping amount increased to 0.24,a separate Mn_(3)O_(4) phase appeared,which in turn might weaken the synergistic effect.Furthermore,the acidity of Ce_(0.02)Mn_(0.04-0.24)TiO_(x) was decreased with the Mn doping,regulating the balance of redox property and acidity.Notably,Ce_(0.02)Mn_(0.16)TiO_(x) featured relatively abundant B-acid sites.Its coordinating redox ability and moderate acidity promoted the deep oxidation of CB and RCOOH-intermediates,as well as the rapid desorption of Cl species,thus obtaining sustainable reactivity.In comparison,CeTiO_(x) owned the strongest acidity,however,its poor redox property was not sufficient for the timely oxidative decomposition of the easier adsorbed CB,resulting in its rapid deactivation.This finding provides a promising strategy for the construction of efficient commercial molding catalysts to decompose the industrial-scale CVOCs.
关 键 词:CHLOROBENZENE Ce_(0.02)Mn_(0-0.2)4tiox materials Redox ability ACIDITY Synergistic interaction
分 类 号:X701[环境科学与工程—环境工程] TQ426[化学工程]
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