Achieving rhodium-like activity for olefin hydroformylation by electronic metal-support interaction of single atomic cobalt catalyst
Achieving rhodium-like activity for olefin hydroformylation by electronic metal-support interaction of single atomic cobalt catalyst
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通过单原子钴催化剂的电子金属-载体相互作用实现烯烃加氢甲酰化的类铑活性
DOI：
10.1016/j.xcrp.2022.101016
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发表时间：
2022-08
影响因子：
8.9
通讯作者：
Yuhan Sun
中科院分区：
文献类型：
--
作者：
Baiyin Wei;Junjun Chen;Xiaofang Liu;Kaimin Hua;Lin Li;Shunan Zhang;Hu Luo;Hui Wang;Yuhan Sun
烯烃与氢气和一氧化碳的氢甲酰化反应是制醛的重要工业过程，开发具有高催化活性和稳定性的地球富集型催化剂仍是一项具有挑战性的工作。在这里，我们合成了一种在β-Mo2C催化剂上进行烯烃氢甲酰化反应的高效率的单原子钴催化剂。在丙烯氢甲酰化反应中，单原子钴催化剂的转化率为3,834，转化率为749h−1，超过了已报道的所有多相钴基催化剂，接近了Rh催化剂的性能。此外，催化剂可重复使用5次，活性没有明显下降，证实了β-Mo2 C负载的单原子Co具有良好的稳定性。这种EMSI效应在优化电荷密度、降低反应势垒、稳定活性中心等方面起着至关重要的作用。·单原子钴催化剂被开发用于氢甲酰化·Co1-MoxCy基元在碳化物表面形成·电子-金属-载体相互作用起着关键作用。报道了一种用于烯烃氢甲酰化反应的单原子钴催化剂，它的活性是通过电子金属-载体相互作用(EMSI)来调节的，可以与Rh相媲美。EMSI能有效地优化电子结构，降低反应势垒，稳定单原子Co。
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 β-Mo 2 C toward olefin hydroformylation. 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 reported 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 β-Mo 2 C. We demonstrate that a Co 1 -Mo x C y 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. • Single-atom cobalt catalyst is developed for hydroformylation • Co 1 -Mo x C y motif forms on the carbide surface • Electronic metal-support interaction plays a pivotal role Wei et al. report a single-atom cobalt catalyst for olefin hydroformylation, whose activity is tailored by electronic metal-support interaction (EMSI) and is comparable with rhodium. EMSI can effectively optimize the electronic structure, reduce the reaction barrier, and stabilize the single atomic Co.
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影响因子：
12.9
作者：
Seungyeon Lee;Abhirup Patra;P. Christopher;D. Vlachos;S. Caratzoulas
通讯作者：
Seungyeon Lee;Abhirup Patra;P. Christopher;D. Vlachos;S. Caratzoulas
影响因子：
2.8
作者：
Insoo Ro;Mingjie Xu;G. Graham;Xiaoqing Pan;P. Christopher
通讯作者：
Insoo Ro;Mingjie Xu;G. Graham;Xiaoqing Pan;P. Christopher
DOI：
10.1007/3418_016
发表时间：
2006-01-01
期刊：
CATALYTIC CARBONYLATION REACTIONS
影响因子：
--
作者：
Claver, Carmen;Dieguez, Montserrat;Castillon, Sergio
通讯作者：
Castillon, Sergio
影响因子：
22.1
作者：
Xiaohao Liu;Baoshan Hu;K. Fujimoto;M. Haruta;M. Tokunaga
通讯作者：
Xiaohao Liu;Baoshan Hu;K. Fujimoto;M. Haruta;M. Tokunaga
影响因子：
12.9
作者：
Baiyin Wei;Xiaofang Liu;Yuchao Deng;Kaimin Hua;Junjun Chen;Hui Wang;Yuhan Sun
通讯作者：
Baiyin Wei;Xiaofang Liu;Yuchao Deng;Kaimin Hua;Junjun Chen;Hui Wang;Yuhan Sun