Effect of Pd doping on CH4 reactivity over Co3O4 catalysts from density-functional theory calculations

doi:10.1016/S1872-2067(17)62817-1

	Effect of Pd doping on CH4 reactivity over Co3O4 catalysts from density-functional theory calculations
	Zhao, Chengcheng1,2,3 ; Zhao, Yonghui 1; Li, Shenggang1,3 ; Sun, Yuhan1,3
	2017-05
发表期刊	催化学报 (IF:15.7[JCR-2023],11.5[5-Year])
ISSN	0253-9837
卷号	38 期号:5 页码:813-820
发表状态	已发表
DOI	10.1016/S1872-2067(17)62817-1
摘要	Palladium oxide (PdOx) and cobalt oxide (Co3O4) are efficient catalysts for methane (CH4) combustion, and Pd-doped Co3O4 catalysts have been found to exhibit better catalytic activities, which suggest synergism between the two components. We carried out first-principles calculations at the PBE+U level to investigate the Pd-doping effect on CH4 reactivity over the Co3O4 catalyst. Because of the structural complexity of the Pd-doped Co3O4 catalyst, we built Pd-doped catalyst models using Co3O4(001) slabs with two different terminations and examined CH4 reactivity over the possible Pd-O active sites. A low energy barrier of 0.68 eV was predicted for CH4 dissociation over the more reactive Pd-doped Co3O4(001) surface, which was much lower than the 0.98 and 0.89 eV that was predicted previously over the more reactive pure Co3O4(001) and (011) surfaces, respectively. Using a simple model, we predicted CH4 reaction rates over the pure Co3O4(001) and (011) surfaces, and Co3O4(001) surfaces with different amounts of Pd dopant. Our theoretical results agree well with the available experimental data, which suggests a strong synergy between the Pd dopant and the Co3O4 catalyst, and leads to a significant increase in CH4 reaction rate. (C) 2017, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
关键词	Spinel cobalt oxide Palladium dopant Methane combustion Density function theory calculation Reaction rate Collision theory
收录类别	SCI ; 北大核心 ; EI
语种	英语
资助项目	National Natural Science Foundation of China[21473233] ; National Natural Science Foundation of China[21403277]
WOS研究方向	Chemistry ; Engineering
WOS类目	Chemistry, Applied ; Chemistry, Physical ; Engineering, Chemical
WOS记录号	WOS:000402346400006
出版者	SCIENCE PRESS
EI入藏号	20172103686219
EI主题词	Calculations ; Catalysts ; Cobalt ; Cobalt compounds ; Combustion ; Density functional theory ; Doping (additives) ; Methane ; Probability density function ; Reaction rates
EI分类号	Nonferrous Metals and Alloys excluding Alkali and Alkaline Earth Metals:549.3 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Mathematics:921 ; Probability Theory:922.1
WOS关键词	CHEMICAL-VAPOR-DEPOSITION ; TOTAL-ENERGY CALCULATIONS ; AUGMENTED-WAVE METHOD ; ELASTIC BAND METHOD ; H BOND ACTIVATION ; OXIDE THIN-FILMS ; METHANE COMBUSTION ; ELECTRONIC-STRUCTURE ; SADDLE-POINTS ; BASIS-SET
原始文献类型	Article
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/1385
专题	物质科学与技术学院物质科学与技术学院_特聘教授组_孙予罕组物质科学与技术学院_特聘教授组_李圣刚组物质科学与技术学院_硕士生
通讯作者	Li, Shenggang
作者单位	1.Chinese Acad Sci, Shanghai Adv Res Inst, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai 201210, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
第一作者单位	物质科学与技术学院
通讯作者单位	物质科学与技术学院
推荐引用方式 GB/T 7714	Zhao, Chengcheng,Zhao, Yonghui,Li, Shenggang,et al. Effect of Pd doping on CH4 reactivity over Co3O4 catalysts from density-functional theory calculations[J]. 催化学报,2017,38(5):813-820.
APA	Zhao, Chengcheng,Zhao, Yonghui,Li, Shenggang,&Sun, Yuhan.(2017).Effect of Pd doping on CH4 reactivity over Co3O4 catalysts from density-functional theory calculations.催化学报,38(5),813-820.
MLA	Zhao, Chengcheng,et al."Effect of Pd doping on CH4 reactivity over Co3O4 catalysts from density-functional theory calculations".催化学报 38.5(2017):813-820.