N-heterocyclic olefin (mNHO) was introduced as a metal-free catalyst for the reductive functionalization of CO2 leading to consecutive double N-methylation of primary amines in the presence of 9-borabicyclo[3.3.1]nonane (9-BBN). A wide range of secondary amines and primary amines were successfully methylated under mild conditions. The catalyst sustained over six successive cycles of N-methylation of secondary
引入介离子 N-杂环烯烃 (mNHO) 作为无
金属催化剂,用于 CO 2的还原官能化,导致
伯胺在
9-硼双环[3.3.1]壬烷存在下连续双N-甲基化 (9- BBN)。多种仲胺和
伯胺在温和条件下成功甲基化。该催化剂能够持续六个连续的仲胺N-甲基化循环,而不会影响其活性,这鼓励我们检查其对
伯胺双N-甲基化的功效。此外,该方法还用于合成两种市售药物分子。通过执行一系列控制反应以及通过单晶 X 射线研究或与 DFT 计算相关的 NMR 光谱研究成功表征活性催化中间体,提出了详细的机械循环。