Sr-doping effects on La2O3 catalyst for oxidative coupling of methane

doi:10.1016/S1872-2067(17)62823-7

	Sr-doping effects on La2O3 catalyst for oxidative coupling of methane
	Cong, Linna1,2,3 ; 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:899-907
发表状态	已发表
DOI	10.1016/S1872-2067(17)62823-7
摘要	Densityfunctional theory calculations were carried out to study the strontium (Sr)-doping effect on methane activation over a lanthanum-oxide (La2O3) catalyst for the oxidative coupling of methane (OCM) using the cluster model. Eight Sr-doped La2O3 cluster models were built from pure La2O3 clusters that were used previously to model the La2O3 catalyst. These form two distinct categories, namely, those without a radical character (LaSr)(2)(OH), La2SrO4, La3SrO5(OH), and LasSr)(8)(OH)) and those with a radical character (LaSr)(3), La2SrO4(OH), La3SrO6, and La5SrO9). The potentialenergy surface for CH4 activation to form a CH3 radical at different Sr-O and La-O pair sites on these Srdoped La2O3 clusters was calculated to study the Srdoping effect on the OCM catalytic activity. CH4 physisorption and chemisorption energies, and activation barriers, and CH3 desorption energies were predicted. Compared with the pure La2O3 clusters, in general, the Sr-doped La2O3 clusters are thermodynamically and kinetically more reactive with CH4. For the Sr-doped La2O3 clusters without the radical character, the Sr-O pair site is more reactive with CH4 than the La-O pair site, although a direct release of the CH3 radical is also highly endothermic as in the case of the pure La2O3 clusters. In contrast, for the Srdoped La2O3 clusters with a radical character, the activation of CH4 at the oxygen radical site and the release of the CH3 radical are much easier. Thus, our calculations suggest that the Sr dopant prompts the OCM catalytic activity of the La2O3 catalyst by providing a highly active oxygenradical site and by strengthening the basicity of the M-O pair site, which leads to lower CH4 activation energies and lower CH3 desorption energies. (C) 2017, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
关键词	Methane activation Methyl radical generation Cluster models Density functional theory Strontium doping Lanthanum oxide
收录类别	SCI ; 北大核心 ; EI
语种	英语
资助项目	Shanghai Municipal Science and Technology Commission[14ZR1444600]
WOS研究方向	Chemistry ; Engineering
WOS类目	Chemistry, Applied ; Chemistry, Physical ; Engineering, Chemical
WOS记录号	WOS:000402346400015
出版者	SCIENCE PRESS
EI入藏号	20172203701186
EI主题词	Activation energy ; Alkalinity ; Catalyst activity ; Catalysts ; Chemical activation ; Desorption ; Doping (additives) ; Ionization of gases ; Lanthanum ; Lanthanum oxides ; Methane ; Potential energy ; Quantum chemistry ; Strontium
EI分类号	Rare Earth Metals:547.2 ; Alkaline Earth Metals:549.2 ; Chemistry, General:801.1 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Operations:802.3 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Probability Theory:922.1
WOS关键词	ALKALINE-EARTH ; BASIS-SETS ; GEOMETRY OPTIMIZATION ; TRANSITION-STATES ; C-2 HYDROCARBONS ; CONVERSION ; ETHANE ; ATOMS ; PSEUDOPOTENTIALS ; ACTIVATION
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/1384
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	Cong, Linna,Zhao, Yonghui,Li, Shenggang,et al. Sr-doping effects on La2O3 catalyst for oxidative coupling of methane[J]. 催化学报,2017,38(5):899-907.
APA	Cong, Linna,Zhao, Yonghui,Li, Shenggang,&Sun, Yuhan.(2017).Sr-doping effects on La2O3 catalyst for oxidative coupling of methane.催化学报,38(5),899-907.
MLA	Cong, Linna,et al."Sr-doping effects on La2O3 catalyst for oxidative coupling of methane".催化学报 38.5(2017):899-907.