Selective C−H Bond Cleavage in Methane by Small Gold Clusters
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‐Aux+‐CH3. 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.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Sep 22, 2017
- Source ID
- 10.1002/anie.201706009
Entities
People
- Joost M Bakker
- Robert N Barnett
- Sandra M Lang
- Thorsten M. Bernhardt
- Uzi Landman
- Valeriy Chernyy
Organizations
- Air Force Office of Scientific Research
- Dutch Research Council
- Georgia Tech
- Horizon 2020
- Radboud University Nijmegen
- Ulm University
- United States Department of Energy