Zhang Jun, Yang Min, Liu Jin-Biao, He Fu-Sheng, Wu Jie
School of Pharmaceutical and Materials Engineering, Taizhou University, 1139 Shifu Avenue, Taizhou 318000, China.
School of Pharmacy, Gannan Medical University, 1 Yixueyuan Road, Ganzhou 341000, China.
Chem Commun (Camb). 2020 Mar 12;56(21):3225-3228. doi: 10.1039/d0cc00375a.
A copper-catalyzed three-component reaction of O-acyl oximes, DABCO·(SO2)2, and 2H-azirines under mild conditions has been achieved. This protocol provides an efficient route for the construction of various tetrasubstituted β-sulfonyl N-unprotected enamines in moderate to good yields with excellent stereoselectivity and regioselectivity. Notably, this method represents a rare example of 2H-azirines as useful synthons for β-functionalized N-unprotected enamines. Preliminary mechanistic studies indicate that the reaction proceeds through coupling of a sulfonyl radical and α-carbon radical via copper-catalyzed ring-opening C-C bond cleavage of O-acyl oxime and C-N bond cleavage of 2H-azirine with the insertion of sulfur dioxide.
在温和条件下实现了铜催化的O-酰基肟、DABCO·(SO2)2和2H-氮杂环丙烷的三组分反应。该方法为构建各种四取代的β-磺酰基N-未保护烯胺提供了一条有效途径,产率适中至良好,具有出色的立体选择性和区域选择性。值得注意的是,该方法是2H-氮杂环丙烷作为β-官能化N-未保护烯胺有用合成子的罕见例子。初步机理研究表明,反应通过铜催化的O-酰基肟的开环C-C键裂解和2H-氮杂环丙烷的C-N键裂解,伴随二氧化硫插入,使磺酰基自由基和α-碳自由基偶联而进行。