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Cobalt-Catalyzed Acceptorless Dehydrogenation of Primary Amines to Nitriles
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2024-04-16 , DOI: 10.1021/jacs.4c00493 Haitao Tian 1 , Cai-Yun Ding 1 , Rong-Zhen Liao 1 , Man Li 1 , Conghui Tang 1, 2
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2024-04-16 , DOI: 10.1021/jacs.4c00493 Haitao Tian 1 , Cai-Yun Ding 1 , Rong-Zhen Liao 1 , Man Li 1 , Conghui Tang 1, 2
Affiliation
The direct double dehydrogenation from primary amines to nitriles without an oxidant or hydrogen acceptor is both intriguing and challenging. In this paper, we describe a non-noble metal catalyst capable of realizing such a transformation with high efficiency. A cobalt-centered N,N-bidentate complex was designed and employed as a metal–ligand cooperative dehydrogenation catalyst. Detailed kinetic studies, control experiments, and DFT calculations revealed the crucial hydride transfer, proton transfer, and hydrogen evolution processes. Finally, a tandem outer-sphere/inner-sphere mechanism was proposed for the dehydrogenation of amines to nitriles through an imine intermediate.
中文翻译:
钴催化伯胺无受体脱氢生成腈
在没有氧化剂或氢受体的情况下,从伯胺到腈的直接双脱氢既有趣又具有挑战性。在本文中,我们描述了一种能够高效实现这种转化的非贵金属催化剂。设计了一种以钴为中心的N , N-二齿配合物,并将其用作金属-配体协同脱氢催化剂。详细的动力学研究、控制实验和 DFT 计算揭示了关键的氢化物转移、质子转移和析氢过程。最后,提出了一种串联的外球/内球机制,用于通过亚胺中间体将胺脱氢为腈。
更新日期:2024-04-17
中文翻译:
钴催化伯胺无受体脱氢生成腈
在没有氧化剂或氢受体的情况下,从伯胺到腈的直接双脱氢既有趣又具有挑战性。在本文中,我们描述了一种能够高效实现这种转化的非贵金属催化剂。设计了一种以钴为中心的N , N-二齿配合物,并将其用作金属-配体协同脱氢催化剂。详细的动力学研究、控制实验和 DFT 计算揭示了关键的氢化物转移、质子转移和析氢过程。最后,提出了一种串联的外球/内球机制,用于通过亚胺中间体将胺脱氢为腈。