Bronsted/Lewis acid sites synergistically promote the initial C-C bond formation in the MTO reaction

doi:10.1039/c8sc02302f

	Bronsted/Lewis acid sites synergistically promote the initial C-C bond formation in the MTO reaction
	Chu, Yueying; Yi, Xianfeng; Li, Chengbin; Sun, Xianyong; Zheng, Anmin
刊名	CHEMICAL SCIENCE
	2018-08-21
卷号	9 期号:31
ISSN号	2041-6520
DOI	10.1039/c8sc02302f
文献子类	Article
英文摘要	The methanol-to-olefin (MTO) reaction is an active field of research due to conflicting mechanistic proposals for the initial carbon-carbon (C-C) bond formation. Herein, a new methane-formaldehyde pathway, a Lewis acid site combined with a BrOnsted acid site in zeolite catalysts can readily activate dimethyl ether (DME) to form ethene, is identified theoretically. The mechanism involves a hydride transfer from Al-OCH3 on the Lewis acid site to the methyl group of the protonated methanol molecule on the adjacent BrOnsted acid site leading to synchronous formation of methane and Al-COH2+ (which can be considered as formaldehyde (HCHO) adsorbed on the Al3+ Lewis acid sites). The strong electrophilic character of the Al-COH2+ intermediate can strongly accelerate the C-C bond formation with CH4, as indicated by the significant decrease of activation barriers in the rate-determining-step of the catalytic processes. These results highlight a synergy of extra-framework aluminum (EFAl) Lewis and BrOnsted sites in zeolite catalysts that facilitates initial C-C bond formation in the initiation step of the MTO reaction via the Al-COH2+ intermediate.
WOS关键词	CARBON-CARBON BOND ; METHANOL-TO-HYDROCARBONS ; SOLID-STATE NMR ; OLEFINS CONVERSION ; CATALYTIC CYCLE ; EXTRAFRAMEWORK ALUMINUM ; HYDROGEN-TRANSFER ; ZEOLITE CATALYST ; DIMETHYL ETHER ; H-ZSM-5
WOS研究方向	Chemistry
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000442262400002
资助机构	National Natural Science Foundation of China(21403290 ; National Natural Science Foundation of China(21403290 ; Natural Science Foundation of Hubei Province of China(2018CFA009) ; Natural Science Foundation of Hubei Province of China(2018CFA009) ; Key Research Program of Frontier Sciences, CAS(QYZDB-SSW-SLH026) ; 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) ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase)(U1501501) ; 21522310 ; 21522310 ; 21473244 ; 21473244 ; 91645112 ; 91645112 ; 21773296) ; 21773296) ; National Natural Science Foundation of China(21403290 ; National Natural Science Foundation of China(21403290 ; Natural Science Foundation of Hubei Province of China(2018CFA009) ; Natural Science Foundation of Hubei Province of China(2018CFA009) ; Key Research Program of Frontier Sciences, CAS(QYZDB-SSW-SLH026) ; 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) ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase)(U1501501) ; 21522310 ; 21522310 ; 21473244 ; 21473244 ; 91645112 ; 91645112 ; 21773296) ; 21773296) ; National Natural Science Foundation of China(21403290 ; National Natural Science Foundation of China(21403290 ; Natural Science Foundation of Hubei Province of China(2018CFA009) ; Natural Science Foundation of Hubei Province of China(2018CFA009) ; Key Research Program of Frontier Sciences, CAS(QYZDB-SSW-SLH026) ; 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) ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase)(U1501501) ; 21522310 ; 21522310 ; 21473244 ; 21473244 ; 91645112 ; 91645112 ; 21773296) ; 21773296) ; National Natural Science Foundation of China(21403290 ; National Natural Science Foundation of China(21403290 ; Natural Science Foundation of Hubei Province of China(2018CFA009) ; Natural Science Foundation of Hubei Province of China(2018CFA009) ; Key Research Program of Frontier Sciences, CAS(QYZDB-SSW-SLH026) ; 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) ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase)(U1501501) ; 21522310 ; 21522310 ; 21473244 ; 21473244 ; 91645112 ; 91645112 ; 21773296) ; 21773296)
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/13052]
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	Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Key Lab Magnet Resonance Biol Syst, Natl Ctr Magnet Resonance Wuhan,Wuhan Inst Phys &, Wuhan 430071, Hubei, Peoples R China
推荐引用方式 GB/T 7714	Chu, Yueying,Yi, Xianfeng,Li, Chengbin,et al. Bronsted/Lewis acid sites synergistically promote the initial C-C bond formation in the MTO reaction[J]. CHEMICAL SCIENCE,2018,9(31).
APA	Chu, Yueying,Yi, Xianfeng,Li, Chengbin,Sun, Xianyong,&Zheng, Anmin.(2018).Bronsted/Lewis acid sites synergistically promote the initial C-C bond formation in the MTO reaction.CHEMICAL SCIENCE,9(31).
MLA	Chu, Yueying,et al."Bronsted/Lewis acid sites synergistically promote the initial C-C bond formation in the MTO reaction".CHEMICAL SCIENCE 9.31(2018).