期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 2, 页码 504-509出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201805820
关键词
alkyne semi-hydrogenation; gold; molecular recognition; N-doped carbon; single-atom catalysis
资金
- Swiss National Science Foundation [200021-169679]
- ETH Research Grant [ETH-40 17-1]
- Spanish MINECO [CTQ2015-68770-R]
- MINECO La Caixa-Severo Ochoa through Severo Ochoa Excellence Accreditation 2014-2018 [SEV-2013-0319]
Single-atom heterogeneous catalysts with well-defined architectures are promising for deriving structure-performance relationships, but the challenge lies in finely tuning the structural and electronic properties of the metal. To tackle this point, a new approach based on the surface diffusion of gold atoms on different cavities of N-doped carbon is presented. By controlling the activation temperature, the coordination neighbors (Cl, O, N) and the oxidation state of the metal can be tailored. Semi-hydrogenation of various alkynes on the single-atom gold catalysts displays substrate-dependent catalytic responses; structure insensitive for alkynols with gamma-OH and unfunctionalized alkynes, and sensitive for alkynols with alpha-OH. Density functional theory links the sensitivity for alkynols to the strong interaction between the substrate and specific gold-cavity ensembles, mimicking a molecular recognition pattern that allows to identify the cavity site and to enhance the catalytic activity.
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