期刊
ACS CATALYSIS
卷 10, 期 19, 页码 10932-10945出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c02238
关键词
oxidation; bimetallic catalysts; glucose; tartaric acid; lattice distortion; electronic reconfiguration
资金
- National Natural Science Foundation of China [21706290]
- Natural Science Foundation of Shandong Province [ZR2017MB004]
- Innovative Research Funding from Qingdao City, Shandong Province [17-1-1-80-jch]
- Fundamental Research Funds for the Central Universities
- Development Fund of State Key Laboratory of Heavy Oil Processing [17CX02017A, 20CX02204A]
- New Faculty Start-Up Funding from China University of Petroleum [YJ201601059]
Tartaric acid is an important industrial building block in the food and polymer industry. However, green manufacture of tartaric acid remains a grand challenge in this area. To date, chemical synthesis from nitric acid-facilitated glucose oxidation leads to only <10% yield with significant toxics as byproducts. We reported a one-pot aqueous-phase oxidation of glucose and gluconic acid using bimetallic AuPt/TiO2 catalysts in the presence of molecular O-2, with similar to 50% yield toward tartaric acid at 110 degrees C and 2 MPa. Structural characterization and density functional theory (DFT) calculation reveal that the lattice mismatch between fcc Pt and bcc Au induces the formation of twinned boundaries in nanoclusters and Jahn-Teller distortion in an electronic field. Such structural and electronic reconfiguration leads to enhanced s-activation of the C-H bond competing with p-p electronic sharing of the C=O bond on the catalyst surface. As a result, both C-H (oxidation) and C-C (decarboxylation) bond cleavage reactions synergistically occur on the surface of bimetallic AuPt/TiO2 catalysts. Therefore, glucose and gluconic acid can be efficiently transformed into tartaric acid in a base-free medium. Lattice distortion-enhanced reconfiguration of the electronic field in Pt-based bimetallic nanocatalysts can be utilized in many other energy and environmental fields for catalyzing synergistic oxidation reactions.
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