Manganese-Catalyzed Dehydrogenative Silylation of Alkenes Following Two Parallel Inner-Sphere Pathways
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https://figshare.com/articles/dataset/Manganese-Catalyzed_Dehydrogenative_Silylation_of_Alkenes_Following_Two_Parallel_Inner-Sphere_Pathways/16806699
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资源简介：
We report on an additive-free
Mn(I)-catalyzed dehydrogenative silylation
of terminal alkenes. The most active precatalyst is the bench-stable
alkyl bisphosphine Mn(I) complex fac-[Mn(dippe)(CO)3(CH2CH2CH3)]. The catalytic
process is initiated by migratory insertion of a CO ligand into the
Mn–alkyl bond to yield an acyl intermediate which undergoes
rapid Si–H bond cleavage of the silane HSiR3 forming
the active 16e– Mn(I) silyl catalyst [Mn(dippe)(CO)2(SiR3)] together with liberated butanal. A broad
variety of aromatic and aliphatic alkenes was efficiently and selectively
converted into E-vinylsilanes and allylsilanes, respectively,
at room temperature. Mechanistic insights are provided based on experimental
data and DFT calculations revealing that two parallel reaction pathways
are operative: an acceptorless reaction pathway involving dihydrogen
release and a pathway requiring an alkene as sacrificial hydrogen
acceptor.
创建时间：
2021-10-13
