Bian Kang-Jie, Lu Yen-Chu, Nemoto David, Kao Shih-Chieh, Chen Xiaowei, West Julian G
Department of Chemistry, Rice University, Houston, TX, USA.
Nat Chem. 2023 Dec;15(12):1683-1692. doi: 10.1038/s41557-023-01365-0. Epub 2023 Nov 13.
Incorporation of fluoroalkyl motifs in pharmaceuticals can enhance the therapeutic profiles of the parent molecules. The hydrofluoroalkylation of alkenes has emerged as a promising route to diverse fluoroalkylated compounds; however, current methods require superstoichiometric oxidants, expensive/oxidative fluoroalkylating reagents and precious metals, and often exhibit limited scope, making a universal protocol that addresses these limitations highly desirable. Here we report the hydrofluoroalkylation of alkenes with cheap, abundant and available fluoroalkyl carboxylic acids as the sole reagents. Hydrotrifluoro-, difluoro-, monofluoro- and perfluoroalkylation are all demonstrated, with broad scope, mild conditions (redox neutral) and potential for late-stage modification of bioactive molecules. Critical to success is overcoming the exceedingly high redox potential of feedstock fluoroalkyl carboxylic acids such as trifluoroacetic acid by leveraging cooperative earth-abundant, inexpensive iron and redox-active thiol catalysis, enabling these reagents to be directly used as hydroperfluoroalkylation donors without pre-activation. Preliminary mechanistic studies support the radical nature of this cooperative process.
在药物中引入氟烷基基团可以增强母体分子的治疗特性。烯烃的氢氟烷基化已成为合成多种氟烷基化化合物的一条有前景的途径;然而,目前的方法需要使用超化学计量的氧化剂、昂贵的/氧化性氟烷基化试剂和贵金属,并且通常适用范围有限,因此非常需要一种能够解决这些局限性的通用方法。在此,我们报道了以廉价、丰富且易得的氟烷基羧酸作为唯一试剂实现烯烃的氢氟烷基化反应。氢三氟烷基化、二氟烷基化、单氟烷基化和全氟烷基化均已得到证实,该反应具有广泛的适用范围、温和的条件(氧化还原中性)以及对生物活性分子进行后期修饰的潜力。成功的关键在于利用储量丰富、价格低廉的铁和具有氧化还原活性的硫醇协同催化,克服原料氟烷基羧酸(如三氟乙酸)极高的氧化还原电位,使这些试剂无需预活化即可直接用作全氟烷基化氢供体。初步的机理研究支持了这一协同过程的自由基性质。