期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 21, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202116059
关键词
Coordination Effects; Hydroxyl Acid; Polyols; Selective Oxidation; Single-Atom Catalysts
资金
- National Natural Science Foundation of China [22108305, 21978325, 22108307]
- Independent Innovation Research Projects [20CX06072A, 20CX06095A, 20CX06096A]
- Natural Science Foundation of Shandong Province [ZR2021QB076, ZR2020KB00, ZR2020YQ17]
- China Postdoctoral international exchange program [2020072]
- Qingdao Postdoctoral Funded Project [qdyy20200069, qdyy20200073]
Efficient catalytic conversion in aqueous solution with excellent resistance against leaching remains a challenge. The design of a single-atom Pt-1/hydroxyapatite (HAP) catalyst results in remarkable catalytic selectivity and stability for the oxidation of C-2-C-4 polyols to hydroxy acids. The Pt-(O-P) linkages with PO43- serve as active sites for activation of C-H bonds and destabilization of the transition state, increasing the selectivity of hydroxy acids. The strong PO43--coordination effect provides electrostatic stabilization and ensures superior leaching resistance for Pt-1/HAP catalyst.
Achieving efficient catalytic conversion over a heterogeneous catalyst with excellent resistance against leaching is still a grand challenge for sustainable chemical synthesis in aqueous solution. Herein, we devised a single-atom Pt-1/hydroxyapatite (HAP) catalyst via a simple hydrothermal strategy. Gratifyingly, this robust Pt-1/HAP catalyst exhibits remarkable catalytic selectivity and catalyst stability for the selective oxidation of C-2-C-4 polyols to corresponding primary hydroxy acids. It is found that the Pt-(O-P) linkages with strong electron-withdrawing function of PO43- (Pt-1-OPO43- pair active site) not only realize the activation of the C-H bond, but also destabilize the transition state from adsorbed hydroxy acids toward the C-C cleavage, resulting in the sharply increased selectivity of hydroxy acids. Moreover, the strong PO43--coordination effect provides electrostatic stabilization for single-atom Pt, ensuring the highly efficient catalysis of Pt-1/HAP for over 160 hours with superior leaching resistance.
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