期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 57, 期 4, 页码 909-913出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201708092
关键词
atomic layer deposition (ALD); heterogeneous catalysis; metal-organic frameworks (MOFs); platinum; sinter-resistance
资金
- Inorganometallic Catalysis Design Center, an Energy Frontier Research Center - U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences [DE-SC0012702]
- DOE Office of Science [DE-AC02-06CH11357]
installed on the zirconia nodes of a metal-organic framework (MOF) NU-1000 via targeted vapor-phase synthesis. The catalytic Pt clusters, site-isolated by organic linkers, are shown to exhibit high catalytic activity for ethylene hydrogenation while exhibiting resistance to sintering up to 200 degrees C. In situ IR spectroscopy reveals the presence of both single atoms and few-atom clusters that depend upon synthesis conditions. Operando X-ray absorption spectroscopy and Xray pair distribution analyses reveal unique changes in chemical bonding environment and cluster size stability while on stream. Density functional theory calculations elucidate a favorable reaction pathway for ethylene hydrogenation with the novel catalyst. These results provide evidence that atomic layer deposition (ALD) in MOFs is a versatile approach to the rational synthesis of size-selected clusters, including noble metals, on a high surface area support.
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