Abstract
The thermal reaction of diatomic gold boride cation AuB+ with methane has been studied by using state-of-the-art mass spectrometry in conjunction with density functional theory calculations. The AuB+ ion can activate a methane molecule to produce exclusively the free hydrogen atom, an important intermediate in hydrocarbon transformation. This result is different from the reactivity of AuC+ and CuB+ counterparts with methane in previous studies. The AuC+ cation mainly transforms methane into ethylene. The CuB+ reaction system principally generates the free hydrogen atoms, but it also gives rise a portion of ethylene-like product H2B−CH2. The B atom of AuB+ is the active site to activate methane. The strong relativistic effect on gold plays an important role for the product selectivity. The mechanistic insights obtained from this study provide guidance for rational design of active sites with high product selectivity toward methane activation.
Funding source: National Natural Science Foundation of China
Award Identifier / Grant number: 91645203
Award Identifier / Grant number: 21773253
Funding source: China Postdoctoral Science Foundation
Award Identifier / Grant number: 2017M611002
Funding source: Beijing Natural Science Foundation
Award Identifier / Grant number: 2182092
Funding source: Chinese Academy of Sciences
Award Identifier / Grant number: 2018041
Funding statement: This work was supported by the National Natural Science Foundation of China (Funder Id: http://dx.doi.org/10.13039/501100001809, Nos. 91645203 and 21773253), the China Postdoctoral Science Foundation (Funder Id: http://dx.doi.org/10.13039/501100002858, No. 2017M611002), and the Beijing Natural Science Foundation (No. 2182092). Y.-X. Zhao thanks the grant from the Youth Innovation Promotion Association, Chinese Academy of Sciences (No. 2018041).
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