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<p>Photoelectrochemical (PEC) synthesis offers a sustainable route for fine chemicals production, yet comprehending and modulating the reaction processes at the atomic level remains a challenge. Herein, we develop a single-atom Ir decorated Ti-doped <i>α</i>-Fe<sub>2</sub>O<sub>3</sub> photoanode for selective PEC synthesis of adipic acid from cyclohexanone using water as the oxygen source. The PEC system achieves 6.0 μmol cm<sup>–2</sup> h<sup>–1</sup> adipic acid production with ~60% Faradaic efficiency and ~88% selectivity. The single-atom Ir promotes the photogenerated carrier separation and transfer, while regulating the electronic structure of Ti-doped <i>α</i>-Fe<sub>2</sub>O<sub>3</sub> photoanode to optimize its adsorption strength of OH<sup>–</sup> and cyclohexanone. Mechanistic studies reveal a non-free-radical reaction pathway at the atomic level, driven by photogenerated holes through an adsorbed hydroxyl transfer. Notably, integrating the photoanode and an amorphous silicon-based photocathode leads to a bias-free PEC device that enables stable adipic acid production for over 80 hours, underscoring the potential for sustainable light-driven synthesis.</p>

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Selective photoelectrochemical synthesis of adipic acid using single-atom Ir decorated α-Fe2O3 photoanode

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年6月2日

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  • Shenghe Si,
  • Yuyin Mao,
  • Ying-Ao Liu,
  • Jun Ma,
  • Weiyi Jiang,
  • En-Dian Zhao,
  • Kepeng Song,
  • Hefeng Cheng,
  • Baibiao Huang,
  • Dong Liu,
  • Yujie Xiong

摘要

Photoelectrochemical (PEC) synthesis offers a sustainable route for fine chemicals production, yet comprehending and modulating the reaction processes at the atomic level remains a challenge. Herein, we develop a single-atom Ir decorated Ti-doped α-Fe2O3 photoanode for selective PEC synthesis of adipic acid from cyclohexanone using water as the oxygen source. The PEC system achieves 6.0 μmol cm–2 h–1 adipic acid production with ~60% Faradaic efficiency and ~88% selectivity. The single-atom Ir promotes the photogenerated carrier separation and transfer, while regulating the electronic structure of Ti-doped α-Fe2O3 photoanode to optimize its adsorption strength of OH– and cyclohexanone. Mechanistic studies reveal a non-free-radical reaction pathway at the atomic level, driven by photogenerated holes through an adsorbed hydroxyl transfer. Notably, integrating the photoanode and an amorphous silicon-based photocathode leads to a bias-free PEC device that enables stable adipic acid production for over 80 hours, underscoring the potential for sustainable light-driven synthesis.