Desilylative allylation of 3,3-borylsilylpropene under metallaphotoredox catalysis.

Liu, Longfei; Li, Haojie; Zhang, Minglong; Diao, Renyi; Tian, Lifang; Zhang, Chi; Zhang, Yu; Shen, Zhi-Liang et al. · Nat Commun · 2026

basic_science · Level V

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Abstract

Chemoselective functionalization of hetero-gem-dimetalloid represents an attractive strategy in terms of diversity-oriented synthesis. In particular, desilylative functionalization of gem-silylboronate esters remains a challenging task and existing solutions heavily relied on ionic reactions. Herein, we report a desilylative functionalization of allylic gem-silylboronate esters with aldehydes under synergistic photoredox and chromium(II) catalysis. With different substrates, both α- and γ-functionalization are realized with exclusive regioselectivity and diastereoselectivity, which is dictated by the chair-like transition state of predominant isomer of Cr<sup>III</sup> allyl intermediate. Moreover, γ-functionalization products bearing CF<sub>2</sub> unit are acquired when gem-difluoroalkene-containing substrates are employed. In the presence of chiral ligand, enantioselective allylation of aldehydes is successfully accomplished, affording alkenylated 1,2-diols after oxidative workup with excellent regio-, diastereo- and enantioselectivity. The current protocol displays wide substrate generality and broad functional group compatibility. In addition, diverse post-transformations converted obtained products into a variety of valuable structures.