期刊
CHEM
卷 8, 期 9, 页码 2380-2392出版社
CELL PRESS
DOI: 10.1016/j.chempr.2022.04.017
关键词
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资金
- National Key R&D Program of China [2017YFA0207302]
- NNSF of China [21890752, 21731005, 21721001]
- Program of Introducing Talents of Discipline to Universities of China [B08027]
- Academy of Finland [292352, 315549, 319208]
- Academy of Finland (AKA) [315549, 315549] Funding Source: Academy of Finland (AKA)
A catalyst containing atomically dispersed Pd sites on N-heterocyclic carbene (NHC)-stabilized Au nanoclusters has been developed for efficient and regioselective hydrogenation of alkenes. The unique molecular structure of the catalyst allows the Pd atom to activate molecular hydrogen and catalyze the hydrogenation reaction effectively. However, the catalyst shows lower activity towards crowded alkenes due to the stringent steric requirements of the NHC ligands.
A catalyst containing atomically dispersed Pd sites on N-heterocyclic carbene (NHC)-stabilized Au nanoclusters, with the precise formula of PdAu9(NHCBn)7X2 (NHCBn is dibenzylbenzimidazolin-2-ylidene, X is Br or Cl), has been developed for the regioselective hydrogenation of alkenes. Each Pd site is encircled by an Au9 ring protected by seven NHC and two halide ligands. Such an encirclement arrangement and open stereochemical framework endow the single Pd atom with the power to activate molecular hydrogen and catalyze the hydrogenation of alkenes efficiently. Interestingly, it otherwise exhibits much lower activity toward the crowded alkenes, owing to the inherent and highly stringent steric requirement of NHC ligands, as also visualized by the theory. As such, these clusters are demonstrated to be a highly efficient (653 h(-1) of turnover frequency) and highly selective (97%) catalyst in the regioselective hydrogenation of linalool, an important synthetic perfume and a key intermediate in the synthesis of vitamin A.
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