Single-Atom Iron Catalyst as an Advanced Redox Mediator for Anodic Oxidation of Organic Electrosynthesis

Xin-Yu Wang, Yong-Zhou Pan, Jiarui Yang, Wen-Hao Li*, Tao Gan, Ying-Ming Pan, Hai-Tao Tang*, Dingsheng Wang*

*Corresponding author for this work

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

41 Citations (Scopus)

Abstract

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. Moreover, Fe-SA@NC demonstrated a great potential in exploring new synthetic method for organic electrosynthesis. We employed 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. © 2024 Wiley-VCH GmbH.
Original languageEnglish
Article numbere202404295
JournalAngewandte Chemie - International Edition
Volume63
Issue number27
Online published22 Apr 2024
DOIs
Publication statusPublished - 1 Jul 2024
Externally publishedYes

Research Keywords

  • Indirect oxidation
  • Organic electrosynthesis
  • Redox mediator
  • Single-atom catalysts
  • Single-electron transfer

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