Pasca Francesco, Gelato Yuri, Andresini Michael, Serbetci Defne, Natho Philipp, Romanazzi Giuseppe, Degennaro Leonardo, Colella Marco, Luisi Renzo
Flow Chemistry and Microreactor Technology FLAME-Lab, Department of Pharmacy-Drug Sciences, University of Bari "A. Moro", Bari 70125, Italy.
DICATECh, Politecnico di Bari, Via E. Orabona 4, Bari 70125, Italy.
JACS Au. 2025 Feb 2;5(2):684-692. doi: 10.1021/jacsau.4c00902. eCollection 2025 Feb 24.
Herein, we report a scalable and mild strategy for the monofluoroalkylation of a wide array of Giese acceptors via visible-light-mediated photoredox catalysis in continuous flow. The use of flow technology significantly enhances productivity and scalability, whereas mildness of conditions and functional group tolerance are ensured by leveraging 4CzIPN, a transition-metal-free organic photocatalyst. Structurally diverse secondary and tertiary monofluoroalkyl radicals can thus be accessed from readily available α-monofluorocarboxylic acids. Given the mild reaction conditions, this protocol is also amenable to the late-stage functionalization of biologically relevant molecules such as menthol, amantadine, bepotastine, and estrone derivatives, rendering it suitable for application to drug discovery programs, for which the introduction of fluorinated fragments is highly sought after. This method was also extended to enable a reductive multicomponent radical-polar crossover transformation to rapidly increase the complexity of the assembled fluorinated architectures in a single synthetic operation.
在此,我们报道了一种通过连续流中可见光介导的光氧化还原催化作用,对多种吉泽受体进行单氟烷基化的可扩展且温和的策略。流动技术的使用显著提高了生产率和可扩展性,而通过利用无过渡金属的有机光催化剂4CzIPN确保了条件的温和性和官能团耐受性。因此,可以从容易获得的α-单氟羧酸获得结构多样的仲和叔单氟烷基自由基。鉴于反应条件温和,该方案也适用于薄荷醇、金刚烷胺、贝波他斯汀和雌酮衍生物等生物相关分子的后期官能团化,使其适用于药物发现计划,在该计划中引入氟化片段是非常受欢迎的。该方法还被扩展以实现还原性多组分自由基-极性交叉转化,从而在单一合成操作中快速增加组装的氟化结构的复杂性。