期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 56, 期 43, 页码 13406-13410出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201706009
关键词
ab initio calculations; C-H bond activation; cluster compounds; gold; vibrational spectroscopy
资金
- Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO)
- LASERLAB-EUROPE (European Union's Horizon research and innovation program) [654148]
- ESF Baden Wugrttemberg
- Air Force Office of Scientific Research [FA9550-15-1-0519]
- Office of Basic Energy Sciences of the US Department of Energy [FG05-86ER45234]
Methane represents the major constituent of natural gas. It is primarily used only as a source of energy by means of combustion, but could also serve as an abundant hydrocarbon feedstock for high quality chemicals. One of the major challenges in catalysis research nowadays is therefore the development of materials that selectively cleave one of the four C-H bonds of methane and thus make it amenable for further chemical conversion into valuable compounds. By employing infrared spectroscopy and first-principles calculations it is uncovered herein that the interaction of methane with small gold cluster cations leads to selective C-H bond dissociation and the formation of hydrido methyl complexes, H-Au-x(+)-CH3. The distinctive selectivity offered by these gold clusters originates from a fine interplay between the closed-shell nature of the dstates and relativistic effects in gold. Such fine balance in fundamental interactions could prove to be a tunable feature in the rational design of a catalyst.
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