期刊
CELL REPORTS PHYSICAL SCIENCE
卷 3, 期 9, 页码 -出版社
CELL PRESS
DOI: 10.1016/j.xcrp.2022.101016
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资金
- National Natural Science Foundation of China [21776296, 21905291, 22108289]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDA21090201]
- Shanghai Sailing Program [19YF1453000]
- Shanghai Institute of Cleantech Innovation [CR190904, CR190905]
In this study, a rhodium-like single-atom cobalt catalyst was successfully developed to enhance the catalytic activity of olefin hydroformylation, surpassing heterogeneous cobalt-based catalysts and approaching the performance of rhodium catalysts. The catalyst showed excellent stability and retained high activity even after five repeated uses. The study revealed that electronic metal-support interaction played a pivotal role in improving the catalyst's performance.
Hydroformylation of olefins with H-2 and CO is an important industrial process for aldehyde production, and developing Earth -abundant catalysts with high catalytic activity and stability remains challenging. Here, we synthesize a rhodium-like high-efficiency single-atom cobalt catalyst over beta-Mo2C toward olefin hydroformy-lation. During the hydroformylation of propene, the single atomic cobalt catalyst achieves a turnover number of 3,834 and a turnover frequency of 749 h(-1), which to our knowledge surpasses all the re-ported heterogeneous cobalt-based catalysts and approaches the performance of rhodium catalysts. Moreover, the catalyst can be reused five times without an obvious activity decline, confirming the excellent stability of single-atom Co supported on beta-Mo2C. We demonstrate that a Co-1-MoxCy motif forms on the carbide surface with electronic metal-support interaction (EMSI). Such an EMSI effect plays a pivotal role in optimizing the charge density, reducing the reaction barrier, and stabilizing the active site.
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