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Title: Selective C−H Bond Cleavage in Methane by Small Gold Clusters

Journal Article · · Angewandte Chemie
ORCiD logo [1];  [1];  [2]; ORCiD logo [2];  [3]; ORCiD logo [3]
  1. Institute of Surface Chemistry and Catalysis University of Ulm Albert-Einstein-Allee 47 89069 Ulm Germany
  2. Institute for Molecules and Materials FELIX Laboratory Radboud University 6525 ED Nijmegen The Netherlands
  3. School of Physics Georgia Institute of Technology Atlanta GA 30332-0430 USA

Abstract 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 + ‐CH 3 . The distinctive selectivity offered by these gold clusters originates from a fine interplay between the closed‐shell nature of the d states 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.

Sponsoring Organization:
USDOE
Grant/Contract Number:
FG05-86ER45234
OSTI ID:
1394003
Journal Information:
Angewandte Chemie, Journal Name: Angewandte Chemie Vol. 129 Journal Issue: 43; ISSN 0044-8249
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

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