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<p>Although significant progress has been made in doped catalyst development, the intrinsic role of dopants beyond the conventional understanding remains intriguing and unresolved. Herein, we reveal the missed heteroatom doping effect, taking a graphene-supported Co-doped FeS<sub>2</sub> catalyst for example, in the oxygen evolution reaction. Rather than the conventional electronic effect from the dopants, the comprehensive characterization and <i>in situ</i> Raman spectroscopy reveal that Co incorporation disrupts S–S bond symmetry and orbital matching within FeS<sub>2</sub>, generating S<sup>2−</sup> species that accelerate surface reconstruction into active FeOOH under electrochemical conditions. After reconstruction, Co atoms remain integrated within the FeOOH lattice, upshifting its d-band center and optimizing oxygen intermediate adsorption, as confirmed by theoretical calculations. This study reveals the dual functionality of Co dopants, facilitating rapid reconstruction in the pre-catalyst and modulating the electronic structure of the active phase, providing novel mechanistic insights into dopant-induced dynamic reconstruction for electrocatalysis.</p>

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Unraveling the missed heteroatom-doping effect in pyrite FeS2 for oxygen evolution reaction

  • 期刊论文

  • 发表日期：

    2026年2月10日

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  • Luhong Fu,
  • Runze He,
  • Shuli Wang,
  • Anantharaj Sengeni,
  • Weiwei Cai,
  • Ligang Feng

摘要

Although significant progress has been made in doped catalyst development, the intrinsic role of dopants beyond the conventional understanding remains intriguing and unresolved. Herein, we reveal the missed heteroatom doping effect, taking a graphene-supported Co-doped FeS2 catalyst for example, in the oxygen evolution reaction. Rather than the conventional electronic effect from the dopants, the comprehensive characterization and in situ Raman spectroscopy reveal that Co incorporation disrupts S–S bond symmetry and orbital matching within FeS2, generating S2− species that accelerate surface reconstruction into active FeOOH under electrochemical conditions. After reconstruction, Co atoms remain integrated within the FeOOH lattice, upshifting its d-band center and optimizing oxygen intermediate adsorption, as confirmed by theoretical calculations. This study reveals the dual functionality of Co dopants, facilitating rapid reconstruction in the pre-catalyst and modulating the electronic structure of the active phase, providing novel mechanistic insights into dopant-induced dynamic reconstruction for electrocatalysis.