Homogeneous electrocatalysts can indirect oxidate the high overpotential substrates through single‐electron transfer on the electrode surface, enabling efficient operation of organic electrosynthesis catalytic cycles. However, the problems of this chemistry still exist such as high dosage, difficult recovery, and low catalytic efficiency. Single‐atom catalysts (SACs) exhibit high atom utilization and excellent catalytic activity, hold great promise in addressing the limitations of homogeneous catalysts. In view of this, we have employed Fe‐SA@NC as an advanced redox mediator to try to change this situation. Fe‐SA@NC was synthesized using an encapsulation‐pyrolysis method, and it demonstrated remarkable performance as a redox mediator in a range of reported organic electrosynthesis reactions, and enabling the construction of various C‐C/C‐X bonds. What's more, Fe‐SA@NC demonstrated a great potential in exploring new synthetic method for organic electrosynthesis. We em‐ployed it to develop a new electro‐oxidative ring‐opening transformation of cyclopropyl amides. In this new reaction system, Fe‐SA@NC showed good tolerance to drug molecules with complex structures, as well as enabling flow electrochemical syntheses and gram‐scale transformations. This work highlights the great potential of SACs in organic electrosynthesis, thereby opening a new avenue in synthetic chemistry.

中文翻译：

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单原子铁催化剂作为有机电合成阳极氧化的高级氧化还原介体

均相电催化剂可以通过电极表面的单电子转移间接氧化高过电势底物，从而实现有机电合成催化循环的高效运行。但该化学仍存在用量高、回收困难、催化效率低等问题。单原子催化剂（SAC）表现出高原子利用率和优异的催化活性，在解决均相催化剂的局限性方面具有广阔的前景。鉴于此，我们采用Fe-SA@NC作为先进的氧化还原介体来尝试改变这种情况。 Fe-SA@NC 采用封装热解方法合成，在一系列已报道的有机电合成反应中表现出作为氧化还原介体的卓越性能，并能够构建各种 C-C/C-X 键。更重要的是，Fe-SA@NC在探索有机电合成新合成方法方面表现出巨大的潜力。我们利用它开发了一种新的环丙基酰胺电氧化开环转化。在这个新的反应体系中，Fe-SA@NC对复杂结构的药物分子表现出良好的耐受性，并且能够实现流动电化学合成和克级转化。这项工作凸显了 SAC 在有机电合成中的巨大潜力，从而为合成化学开辟了一条新途径。