期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 57, 期 24, 页码 7071-7075出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201802231
关键词
active sites; biomass conversion; nickel; single-atom catalysts; XANES simulation
资金
- National Natural Science Foundation of China [21690080, 21690084, 21673228, 21721004, 21590792, 91645203, 11435012]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17020100]
- National Key Projects for Fundamental Research and Development of China [2016YFA0202801]
- Fundamental Research Funds for the Central Universities [15CX06037A]
Hydrothermally stable, acid-resistant nickel catalysts are highly desired in hydrogenation reactions, but such a catalyst remains absent owing to the inherent vulnerability of nickel under acidic conditions. An ultra-durable Ni-N-C single-atom catalyst (SAC) has now been developed that possesses a remarkable Ni content (7.5wt%) required for practical usage. This SAC shows not only high activities for hydrogenation of various unsaturated substrates but also unprecedented durability for the one-pot conversion of cellulose under very harsh conditions (245 degrees C, 60bar H-2, presence of tungstic acid in hot water). Using integrated spectroscopy characterization and computational modeling, the active site structure is identified as (Ni-N4)N, where significantly distorted octahedral coordination and pyridinic N constitute a frustrated Lewis pair for the heterolytic dissociation of dihydrogen, and the robust covalent chemical bonding between Ni and N atoms accounts for its ultrastability.
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