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Reaction mechanism and kinetics of CO oxidation over a CuO/Ce0.75Zr0.25O2-delta catalyst
Kang RN(康润宁); Wei XL(魏小林); Bin F(宾峰); Wang ZB; Hao QL; Dou BJ
2018-09-05
发表期刊APPLIED CATALYSIS A-GENERAL
卷号565页码:46-58
ISSN0926-860X
摘要

The CuO/Ce0.75Zr0.25O2-(delta) and Ce0.75Zr0.25O delta catalysts were prepared by the sol-gel method, and Cu0.07Ce0.75Zr0.25O2-delta was obtained by treatingCuO/Ce0.75Zr0.25O2-(delta) with nitric acid to remove the well-dispersed CuO on the surface. Various characterizations were used to reveal the different active sites, such as surface-dispersed CuO and Cu-Ce-Zr-O-delta solid solutions in CuO/Ce0.75Zr0.25O2-(delta) , Cu-Ce-Zr-O-delta solid solutions in Cu0.07Ce0.75Zr0.25O2-(delta) and Ce-Zr-O-delta solid solutions in CuO/Ce0.75Zr0.25O delta. The Raman and O-2-TPD results showed that the concentration of oxygen vacancies in Cu-Ce-Zr-O-delta solid solutions was higher than that in Ce-Zr-O-delta solid solutions. CO oxidation testing suggested that the catalytic activity decreases in the order of CuO/Ce0.75Zr0.25O2-(delta) > Cu0.07Ce0.75Zr0.25O2-delta > Ce0.75Zr0.25O delta. Combined with the in situ diffuse-reflectance Fourier transform (in situ DRIFT) results, the reaction senitivity followed the order of CO linear chemisorption onto dispersed CuOx species (Mars-van Krevelen mechanism) > carbonate species onto a Cu-Ce-Zr-O-delta solid solution (Langmuir-Hinshelwood mechanism) > carbonate species onto a Ce-Zr-O-delta solid solution (Langmuir-Hinshelwood mechanism). Kinetic studies suggested that the power-law rate expressions and apparent activation energies were r = 6.02 x 10(-)(7)x P(CO)(0.68)x P-O2(0.03) (53 +/- 3 kJ/mol) for CuO/Ce0.75Zr0.25O2-(delta), r = 5.86 x 10(-7) x P(CO)(0.8 )x P-O2(0.07) (105 +/- 5 kJ/mol) for Cu0.07Ce0.75Zr0.25O2-(delta) and r = 5.7 x 10(-7) x P(CO)(0.75 )x P-O2(0.12) (115 +/- 6 kJ/mol) for Ce0.75Zr0.25O delta. The Mars-van Krevelen mechanism should be the crucial reaction pathway over CuO/Ce0.75Zr0.25O2-(delta) in CO interfacial reactions, although the Langmuir-Hinshelwood mechanism cannot be ignored, and the Langmuir-Hinshelwood mechanism mainly occurred over theCu(0)(.)(07)Ce(0)(.)(75)Zr(0)(.)(25)O(2)-(delta) and Ce0.75Zr0.25O delta catalysts, where the contribution from the Mars-van Krevelen mechanism was negligible due to the absence of surface CuOx species.

关键词Co Oxidation Reaction Active Sites Kinetics Reaction Mechanism Cuo/ce0.75zr0.25o2-(Delta)Scatalyst
DOI10.1016/j.apcata.2018.07.026
URL查看原文
收录类别SCI ; EI
语种英语
WOS记录号WOS:000444932800006
关键词[WOS]Self-sustained Combustion ; Hydrogen-rich Gas ; Carbon-monoxide ; Low-temperature ; Cuo-ceo2 Catalysts ; Solid-solutions ; Structural Characteristics ; Preferential Oxidation ; Cuo/ceo2 Catalysts ; Oxygen Vacancies
WOS研究方向Chemistry, Physical ; Environmental Sciences
WOS类目Chemistry ; Environmental Sciences & Ecology
项目资助者National Natural Science Foundation of China [51776216, 51736010]
论文分区一类
力学所作者排名1
引用统计
文献类型期刊论文
条目标识符http://dspace.imech.ac.cn/handle/311007/77853
专题高温气体动力学国家重点实验室
通讯作者Bin F(宾峰); Dou BJ
作者单位1.Chinese Acad Sci, Inst Mech, State Key Lab High Temp Gas Dynam, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Sch Engn Sci, Beijing 100049, Peoples R China
3.North China Univ Sci & Technol, Coll Met & Energy, Tangshan 063210, Peoples R China
4.Tianjin Univ Sci & Technol, Coll Environm Sci, Tianjin 300457, Peoples R China
推荐引用方式
GB/T 7714
Kang RN,Wei XL,Bin F,et al. Reaction mechanism and kinetics of CO oxidation over a CuO/Ce0.75Zr0.25O2-delta catalyst[J]. APPLIED CATALYSIS A-GENERAL,2018,565:46-58.
APA Kang RN,Wei XL,Bin F,Wang ZB,Hao QL,&Dou BJ.(2018).Reaction mechanism and kinetics of CO oxidation over a CuO/Ce0.75Zr0.25O2-delta catalyst.APPLIED CATALYSIS A-GENERAL,565,46-58.
MLA Kang RN,et al."Reaction mechanism and kinetics of CO oxidation over a CuO/Ce0.75Zr0.25O2-delta catalyst".APPLIED CATALYSIS A-GENERAL 565(2018):46-58.
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