Here we report a seminal triple catalysis strategy with the assistance of catalytic ionic liquid. DFT calculations reveal the detailed effect of ionic liquid in this triple catalysis mediated C(sp³)-H functionalizations and a very different mechanism has been established in contrast to all previous dual catalysis research. Based on it, direct coupling between acyl chlorides and very strong or polar C(sp³)-H bonds has been realized in high yields as well as unexpected methylation of acyl chlorides first using just 1.2 equivalent tetramethylsilane as methyl source via successive C(sp³)-H and C(sp³)-Si cleavage. One pot methylation strategy has been developed in this research. This is the first report of that ionic liquid is used for very strong C(sp³)-H bonds functionalization and the first report of that tetramethylsilane is used as methyl source.

在这里，我们报告了一种借助催化离子液体的开创性三重催化策略。DFT 计算揭示了离子液体在这种三重催化介导的 C(sp ³ )-H 官能化中的详细影响，并且已经建立了与之前所有双催化研究相比非常不同的机制。基于此，酰氯与非常强或极性的 C(sp ³ )-H 键之间的直接偶联已经以高产率实现，并且酰氯的意外甲基化首先使用仅 1.2 当量的四甲基硅烷作为甲基源通过连续的 C(sp ³ )-H 和 C(sp ³)-Si 解理。本研究开发了一种罐甲基化策略。这是离子液体用于非常强的C(sp ³ )-H 键官能化的首次报道，也是四甲基硅烷用作甲基源的首次报道。