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Oxygen vacancy mediated La1-xCexFeO3-delta perovskite oxides as efficient catalysts for CWAO of acrylic acid by A-site Ce doping

文献类型：期刊论文

作者Sun, Wenjing1,3; Wei, Huangzhao3; An, Lu Yang2; Jin, Chengyu1,3; Wu, Huiling1,3; Xiong, Zi-ang4; Pu, Chunying5; Sun, Chenglin3
刊名APPLIED CATALYSIS B-ENVIRONMENTAL
出版日期2019-05-15
卷号245页码:20-28
关键词Catalytic wet air oxidation La1-xCexFeO3-delta Synergistic mechanism Generalized kinetic model First-principles calculations
ISSN号0926-3373
DOI10.1016/j.apcatb.2018.12.024
通讯作者Pu, Chunying(puchunying@126.com) ; Sun, Chenglin(clsun@dicp.ac.cn)
英文摘要The influence of Ce amount on catalytic behaviour of perovskite catalysts La1-xCexFeO3-delta, prepared by coprecipitation was examined in catalytic wet air oxidation (CWAO) of high concentrated acrylic acid pollutant. The catalysts with the molar ratio of Ce/(La + Ce) upper than 0.4 exhibit high catalytic activity, and outstanding stability. Because Ce doping into the skeleton of LaFeO3 could cause the change of iron valence state as well as the change of the reactive oxygen species and oxygen vacancies of the catalyst. Three ways of O-2 involved in this reaction were considered, a synergistic mechanism of oxygen vacancies, the reversible electronic transition Fe3+ <-> Fe2+, and direct oxidization of acrylic acid. First-principles calculations revealed that the oxygen vacancy is more easily to form in the case of Ce content increasing in La1-xCexFeO3-delta, and oxygen would adsorb on oxygen vacancy to form reactive oxygen species. Consequently, the reactive oxygen species (O*) could oxidize acrylic acid. In this process, Fe ions of higher valence sate which would attack organic compounds and itself was reduced to Fe2+ to achieve catalytic cycles. Finally, the reaction was verified as first order, which was well explained by a proposed generalized kinetic model, in good accordance with our experimental data.
WOS关键词WET AIR OXIDATION ; TOTAL-ENERGY CALCULATIONS ; AEROBIC OXIDATION ; AQUEOUS-SOLUTIONS ; LAFEO3 CATALYST ; LABO3 B ; PERFORMANCE ; CU ; DEGRADATION ; REMOVAL
资助项目DICP[DICP ZZBS201614] ; Chinese Academy of Sciences[ZDRW-ZS-2016-5] ; National Natural Science Foundation of China[51878643]
WOS研究方向Chemistry ; Engineering
语种英语
WOS记录号WOS:000467661700003
出版者ELSEVIER SCIENCE BV
资助机构DICP ; DICP ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; DICP ; DICP ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; DICP ; DICP ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; DICP ; DICP ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China
源URL[http://cas-ir.dicp.ac.cn/handle/321008/171913]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者Pu, Chunying; Sun, Chenglin
作者单位1.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
2.Sinosteel Anshan Res Inst Thermoenergy Co Ltd, Natl Engn Res Ctr Coking Technol, Anshan 114044, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
4.Dalian Univ Technol, Dalian 116024, Peoples R China
5.Nanyang Normal Univ, Coll Phys & Elect Engn, Nanyang 473061, Henan, Peoples R China
推荐引用方式
GB/T 7714		 Sun, Wenjing,Wei, Huangzhao,An, Lu Yang,et al. Oxygen vacancy mediated La1-xCexFeO3-delta perovskite oxides as efficient catalysts for CWAO of acrylic acid by A-site Ce doping[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2019,245:20-28.
APA Sun, Wenjing.,Wei, Huangzhao.,An, Lu Yang.,Jin, Chengyu.,Wu, Huiling.,...&Sun, Chenglin.(2019).Oxygen vacancy mediated La1-xCexFeO3-delta perovskite oxides as efficient catalysts for CWAO of acrylic acid by A-site Ce doping.APPLIED CATALYSIS B-ENVIRONMENTAL,245,20-28.
MLA Sun, Wenjing,et al."Oxygen vacancy mediated La1-xCexFeO3-delta perovskite oxides as efficient catalysts for CWAO of acrylic acid by A-site Ce doping".APPLIED CATALYSIS B-ENVIRONMENTAL 245(2019):20-28.

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来源：大连化学物理研究所

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