Excited-State Palladium-Catalyzed Radical Allylic Alkylation: Rapid Access to C2-Allyl Carbohydrates

激发态钯催化自由基烯丙基烷基化反应:快速合成C2-烯丙基碳水化合物

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Abstract

Glycomimetics has emerged as a promising strategy to mimic the biological activities of carbohydrates while enhancing drug-like properties. Yet, their efficient synthesis and modifications remain a major challenge. Herein, we report an excited-state Pd-catalyzed, rapid synthesis of C2-allylated carbohydrates, useful synthons for preparing glycomimetics, from readily available α-bromosugars. The transformation features a high level of atom economy, broad functional group tolerance, and suitability for late-stage modification of complex molecules. Preliminary experimental and computational studies suggest a radical mechanism involving excited Pd species, 1,2-radical migration (RaM), and kinetic-controlled β-H elimination processes. We anticipate that our findings will broaden the reaction profile of excited-state Pd catalysis and enable rapid access to valuable glycomimetics.

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