Rationally designing mixed Cu-(mu-O)-M (M = Cu, Ag, Zn, Au) centers over zeolite materials with high catalytic activity towards methane activation

doi:10.1039/c8cp04872j

	Rationally designing mixed Cu-(mu-O)-M (M = Cu, Ag, Zn, Au) centers over zeolite materials with high catalytic activity towards methane activation
	Zheng, Anmin3 ; Zhou, Jian 1; Chen, Wei 2,3; Huang, Ling 3; Wang, Guiru 2,3
刊名	PHYSICAL CHEMISTRY CHEMICAL PHYSICS
	2018-11-07
卷号	20 期号:41 页码:26522-26531
ISSN号	1463-9076
DOI	10.1039/c8cp04872j
英文摘要	The direct conversion of methane to methanol on [Cu(-O)M](2+) (M = Cu, Ag, Zn, Au) bimetal centers in ZSM-5 zeolite is investigated using periodic density functional theory for the first time. Some conclusions are drawn: (1) methane activation on [Cu(-O)M](2+) (M = Cu, Ag, Zn, Au) in the ZSM-5 zeolite proceeds through radical-like transition states, and the ability for CH4 activation decreases in the sequence [Cu(-O)Ag](2+) > [Cu(-O)Au](2+) > [Cu(-O)Cu](2+) > [Cu(-O)Zn](2+). (2) There are two factors that can dramatically enhance C-H bond activation: a greater spin density and a less negative charge of the -O atom. (3) The angles ?CuOM play a minor role in the reactivity difference among [CuOM](2+)-ZSM-5 (M = Cu, Ag, Zn, Au). Our findings will provide insight into methane activation for designing highly effective catalysts applied in industrial processes.
资助项目	National Natural Science Foundation of China[21522310] ; National Natural Science Foundation of China[21473244] ; National Natural Science Foundation of China[91645112] ; National Natural Science Foundation of China[51503222] ; Natural Science Foundation of Hubei Province of China[2018CFA009] ; Key Research Program of Frontier Sciences, CAS[QYZDB-SSW-SLH026] ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase)[U1501501]
WOS关键词	H BOND ACTIVATION ; COMBINED QUANTUM-MECHANICS ; DENSITY-FUNCTIONAL THEORY ; FINDING SADDLE-POINTS ; HYDROGEN-ATOM TRANSFER ; AUGMENTED-WAVE METHOD ; AB-INITIO ; SELECTIVE CONVERSION ; ELECTRONIC-STRUCTURE ; 2-STATE REACTIVITY
WOS研究方向	Chemistry ; Physics
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000448665900050
资助机构	National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase)
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/13139]
专题	中国科学院武汉物理与数学研究所
通讯作者	Zheng, Anmin
作者单位	1.SINOPEC, Shanghai Res Inst Petrochem Technol, Shanghai 201208, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Natl Ctr Magnet Resonance Wuhan, Key Lab Magnet Resonance Biol Syst,Wuhan Inst Phy, Wuhan 430071, Hubei, Peoples R China
推荐引用方式 GB/T 7714	Zheng, Anmin,Zhou, Jian,Chen, Wei,et al. Rationally designing mixed Cu-(mu-O)-M (M = Cu, Ag, Zn, Au) centers over zeolite materials with high catalytic activity towards methane activation[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2018,20(41):26522-26531.
APA	Zheng, Anmin,Zhou, Jian,Chen, Wei,Huang, Ling,&Wang, Guiru.(2018).Rationally designing mixed Cu-(mu-O)-M (M = Cu, Ag, Zn, Au) centers over zeolite materials with high catalytic activity towards methane activation.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,20(41),26522-26531.
MLA	Zheng, Anmin,et al."Rationally designing mixed Cu-(mu-O)-M (M = Cu, Ag, Zn, Au) centers over zeolite materials with high catalytic activity towards methane activation".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 20.41(2018):26522-26531.