Lu Heng, Fan Zhoulong, Zou Yike, Zhang Ao
Shanghai Frontiers Science Center of Drug Target Identification and Delivery, School of Pharmaceutical Sciences, Shanghai Jiao Tong University, Shanghai, 200240, China.
National Key Laboratory of Innovative Immunotherapy, Shanghai Jiao Tong University, Shanghai, 200240, China.
Adv Sci (Weinh). 2025 Feb;12(6):e2408781. doi: 10.1002/advs.202408781. Epub 2024 Dec 24.
Given the widespread presence of fluoroalkyl functionalities in bioactive molecules, the development of fluoroalkylation reactions with bench-stable and easy-to-use fluoroalkylating reagents is highly desirable. In addition, realization of mono-, di-, tri-, or polyfluoroalkyation usually requires distinct types of fluoroalkylating reagents under different or even harsh reaction conditions, and a universal method to accomplish different hydrofluoroalkylation of alkenes is lacking. Herein, the use of quaternary fluoroalkyl alcohols is reported as the universal fluoroalkylating reagents to readily facilitate mono-, di-, tri-, or polyfluoroalkylation of a wide range of alkene substrates in high yields. Moreover, a cascade reaction of hydrofluoroalkylation followed by intramolecular fluoroalkylation facilitates the construction of a variety of high-value complex heterocycles bearing diverse fluoroalkyl functionalities from alkenes. Mechanistic studies suggest that a proton-coupled electron transfer (PCET) process may be involved through a radical-generating pathway. The utility of this method is showcased by the late-stage fluoroalkylation of various high-value complex molecules derived from either natural products or drug-like compounds. Of note is that a continuous-flow system is amenable to this homogeneous photoredox conditions, thereby opening up a possibility of using this protocol to realize large-scale manufacturing of fluoroalkyl products with industrial interests.
鉴于含氟烷基官能团在生物活性分子中广泛存在,开发使用易于操作且稳定的含氟烷基化试剂进行氟烷基化反应是非常必要的。此外,实现单氟烷基化、二氟烷基化、三氟烷基化或多氟烷基化通常需要在不同甚至苛刻的反应条件下使用不同类型的含氟烷基化试剂,目前缺乏一种通用方法来实现烯烃的不同氢氟烷基化反应。在此,我们报道了使用季铵盐型氟代烷基醇作为通用的氟烷基化试剂,能够以高产率轻松实现多种烯烃底物的单氟烷基化、二氟烷基化、三氟烷基化或多氟烷基化反应。此外,氢氟烷基化反应与分子内氟烷基化反应的串联反应有助于从烯烃构建多种带有不同氟烷基官能团的高价值复杂杂环化合物。机理研究表明,质子耦合电子转移(PCET)过程可能通过自由基生成途径参与反应。该方法的实用性通过对各种源自天然产物或类药物化合物的高价值复杂分子进行后期氟烷基化反应得到了展示。值得注意的是,连续流系统适用于这种均相光氧化还原条件,从而为利用该方案实现具有工业应用价值的氟烷基化产物的大规模生产提供了可能性。