Cai Chen-Yan, Zheng Yun-Tao, Li Jing-Fu, Xu Hai-Chao
State Key Laboratory of Physical Chemistry of Solid Surfaces, Key Laboratory of Chemical Biology of Fujian Province, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, People's Republic of China.
J Am Chem Soc. 2022 Jul 13;144(27):11980-11985. doi: 10.1021/jacs.2c05126. Epub 2022 Jun 30.
The 1,2-diamine motif is prevalent in natural products, small-molecule pharmaceuticals, and catalysts for asymmetric synthesis. Transition metal catalyzed alkene diazidation has evolved to be an attractive strategy to access vicinal primary diamines but remains challenging, especially for practical applications, due to the restriction to a certain type of olefins, the frequent use of chemical oxidants, and the requirement for high loadings of metal catalysts (1 mol % or above). Herein we report a scalable Cu-electrocatalytic alkene diazidation reaction with 0.02 mol % (200 ppm) of copper(II) acetylacetonate as the precatalyst without exogenous ligands. In addition to its use of low catalyst loading, the electrocatalytic method is scalable, compatible with a broad range of functional groups, and applicable to the diazidation of α,β-unsaturated carbonyl compounds and mono-, di-, tri-, and tetrasubstituted unactivated alkenes.
1,2 - 二胺基序在天然产物、小分子药物以及不对称合成催化剂中普遍存在。过渡金属催化的烯烃重氮化反应已发展成为一种制备邻位伯二胺的有吸引力的策略,但由于对特定类型烯烃的限制、化学氧化剂的频繁使用以及对高负载金属催化剂(1 mol%或更高)的要求,该反应仍然具有挑战性,尤其是在实际应用中。在此,我们报道了一种可扩展的铜电催化烯烃重氮化反应,该反应以0.02 mol%(200 ppm)的乙酰丙酮铜(II)作为预催化剂,无需外加配体。除了使用低催化剂负载量外,该电催化方法具有可扩展性,与广泛的官能团兼容,适用于α,β - 不饱和羰基化合物以及单取代、二取代、三取代和四取代未活化烯烃的重氮化反应。