Rationally designing mixed Cu–(μ-O)–M (M = Cu, Ag, Zn, Au) centers over zeolite materials with high catalytic activity towards methane activation
文献情報
Ling Huang, Jian Zhou, Anmin Zheng
The direct conversion of methane to methanol on [Cu(μ-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(μ-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(μ-O)Ag]2+ > [Cu(μ-O)Au]2+ > [Cu(μ-O)Cu]2+ > [Cu(μ-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 μ-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.
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![(3R,4aR,7aS,9aR,10S,11R,13aR,13bS,15aS,15bR)-3,11-Dihydroxy-10-(hydroxymethyl)-4,4,7a,10,13a,15b-hexamethyl-1,2,3,4,4a,7,7a,8,9,9a,10,11,12,13,13a,13b,14,15,15a,15b-icosahydro-5H-naphtho[2',1':4,5]cyc
lohepta[1,2-a]naphthalen-5-one structure (3R,4aR,7aS,9aR,10S,11R,13aR,13bS,15aS,15bR)-3,11-Dihydroxy-10-(hydroxymethyl)-4,4,7a,10,13a,15b-hexamethyl-1,2,3,4,4a,7,7a,8,9,9a,10,11,12,13,13a,13b,14,15,15a,15b-icosahydro-5H-naphtho[2',1':4,5]cyc
lohepta[1,2-a]naphthalen-5-one structure](https://static.chemtradehub.com/structs/538/53800-21-8-9f18.webp)
