用于后期C─H氟烷基化的光电化学铁(III)催化
Photoelectrochemical Iron(III) Catalysis for Late-Stage C─H Fluoroalkylations.
作者信息
Motornov Vladimir, Trienes Sven, Resta Simonetta, Oliveira João C A, Lin Zhipeng, Liu Zhi, von Münchow Tristan, Stückl Claudia, Ackermann Lutz
机构信息
Wöhler Research Institute for Sustainable Chemistry (WISCh), Georg-August-Universität, Tammannstraße 2, 37077, Göttingen, Germany.
German Center for Cardiovascular Research (DZHK), Potsdamer Strasse 58, 10785, Berlin, Germany.
出版信息
Angew Chem Int Ed Engl. 2025 Jun 17;64(25):e202504143. doi: 10.1002/anie.202504143. Epub 2025 May 7.
Chemo- and site-selective functionalization of complex molecules poses a fundamental challenge. Herein, we introduce a resource-economic photoelectrocatalysis strategy to enable versatile direct fluoroalkylations catalyzed by Earth-abundant iron and paired with the hydrogen evolution reaction (HER). Notably, the devised approach proved amenable to versatile late-stage C─H fluoroalkylations of bio-relevant heterocycles, such as xanthines, nucleobases, and nucleosides. Mechanistic studies supported a ligand-to-metal charge transfer-induced formation of the fluoroalkyl radical.
复杂分子的化学和位点选择性功能化是一项根本性挑战。在此，我们引入一种资源经济的光电催化策略，以实现由储量丰富的铁催化并与析氢反应（HER）配对的通用直接氟烷基化反应。值得注意的是，所设计的方法被证明适用于生物相关杂环（如黄嘌呤、核碱基和核苷）的通用后期C─H氟烷基化反应。机理研究支持了配体到金属的电荷转移诱导氟烷基自由基的形成。
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