期刊
NATURE CHEMISTRY
卷 10, 期 3, 页码 325-332出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.2915
关键词
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资金
- Division of Chemical Sciences, Office of Basic Energy Sciences, CPIMS Program, US Department of Energy [FG02-10ER16170]
- US Department of Energy [DE-FG02-05ER15730]
- Department of Energy Office of Science [DE-AC02-06CH11357]
- Engineering and Physical Sciences Research Council UK [1352369]
- DOE Office of Science User Facility [DE-AC05-00OR22725]
- US Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0012573]
- embedded Computer Science and Engineering (eCSE) programme of the ARCHER UK National Supercomputing Service [eCSE01-001, eCSE10-8]
- European Research Council under the European Union's Seventh Framework Programme-European Research Council [616121]
- Royal Society
- Engineering and Physical Sciences Research Council [1352369] Funding Source: researchfish
The recent availability of shale gas has led to a renewed interest in C-H bond activation as the first step towards the synthesis of fuels and fine chemicals. Heterogeneous catalysts based on Ni and Pt can perform this chemistry, but deactivate easily due to coke formation. Cu-based catalysts are not practical due to high C-H activation barriers, but their weaker binding to adsorbates offers resilience to coking. Using Pt/Cu single-atom alloys (SAAs), we examine C-H activation in a number of systems including methyl groups, methane and butane using a combination of simulations, surface science and catalysis studies. We find that Pt/Cu SAAs activate C-H bonds more efficiently than Cu, are stable for days under realistic operating conditions, and avoid the problem of coking typically encountered with Pt. Pt/Cu SAAs therefore offer a new approach to coke-resistant C-H activation chemistry, with the added economic benefit that the precious metal is diluted at the atomic limit.
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