Intermolecular C-H silylations of arenes and heteroarenes with mono-, bis-, and tris(trimethylsiloxy)hydrosilanes: control of silane redistribution under operationally diverse approaches

利用单(三甲基硅氧基)氢硅烷、双(三甲基硅氧基)氢硅烷和三(三甲基硅氧基)氢硅烷对芳烃和杂芳烃进行分子间CH硅烷化反应:在多种操作方法下控制硅烷的重新分布

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Abstract

Efficient catalytic protocols for C-H silylations of arenes and heteroarenes with sterically and electronically different hydrosiloxysilanes are disclosed. The silylations are catalyzed by a well-defined Rh-complex (1 mol%), derived from [Rh(1,5-hexadiene)Cl](2) and a bulky BINAP type ligand. This catalyst not only promotes C-Si bond formation affording the desired products in up to 95% isolated yield, but also can suppress the silane redistribution side reactions of HSiMe(2)(OTMS). The protocol can also be applied for the C-H silylations of more reactive HSiMe(OTMS)(2) with a much lower catalyst loading (0.25 mol%) and even with sterically demanding HSi(OTMS)(3). The steric bulk of the arene substituent and hydrosiloxysilane is a major factor in determining the regioselectivity and electronic effect as secondary. The current method can be performed under operationally diverse conditions: with/without a hydrogen scavenger or solvent.

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