化学
脱羧
组合化学
羧酸
基质(水族馆)
催化作用
功能群
有机化学
硼酸
芳基
双重角色
化学合成
劈理(地质)
有机合成
小学(天文学)
羧酸盐
前药
亚砜
反应机理
化学生物学
氢原子
立体化学
作者
Yongchen Wang,Jess C Tang,Gang Wu,Julian G. West
标识
DOI:10.1038/s41467-026-69851-w
摘要
Bicyclo[1.1.1]pentane (BCP) boronic esters are crucial intermediates for accessing BCP-containing drugs with improved pharmacokinetic profiles, yet their synthesis typically relies on pre-formed redox-active esters derived from carboxylic acids. Here we report a general, single-step method for the direct conversion of carboxylic acids into BCP boronic esters. Upon irradiation of carboxylic acids with [1.1.1]propellane and bis(pinacolato)diboron (B2pin2) in dimethyl sulfoxide (DMSO), BCP boronates are obtained in good yields, which are further enhanced by the addition of an iron catalyst. Mechanistic studies suggest that photolytic cleavage of a B2pin2-DMSO complex initiates decarboxylation via hydrogen atom transfer (HAT), while iron catalysis enables a parallel ligand-to-metal charge transfer (LMCT) pathway. This synergistic HAT/LMCT process displays broad substrate scope and remarkable functional group tolerance. Additionally, BCP analogs of two approved drugs, butenafine and buclizine, have been readily synthesized, underscoring the potential of this dual HAT/LMCT paradigm to reshape strategies in synthetic chemistry and drug discovery.
科研通智能强力驱动
Strongly Powered by AbleSci AI