Wei, Baiyin; Chen, Junjun; Liu, Xiaofang; Hua, Kaimin; Li, Lin; Zhang, Shunan; Luo, Hu; Wang, Hui; Sun, Yuhan

CELL REPORTS PHYSICAL SCIENCE

2022, 3,

Wei, Baiyin; Chen, Junjun; Liu, Xiaofang; Hua, Kaimin; Li, Lin; Zhang, Shunan; Luo, Hu; Wang, Hui; Sun, Yuhan

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.