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.Her...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.展开更多
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)+1 种基金the Chengdu Science and Technology Bureau(No.2018-ZM01-00019-SN)the Youth Innovation Promotion Association CAS。
文摘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.
