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<p>Metal–organic frameworks (MOFs) emerge as promising materials for catalyzing the oxygen evolution reaction (OER), a fundamental process in water splitting. This study describes the development of an optimized CoFe-based MOF, demonstrating significant enhancement in its catalytic activity for the OER. The catalytic activity of zeolitic imidazolate framework-67 (ZIF-67) is markedly improved via a facile post-synthetic modification. This process involved partially substituting cobalt ions at specific sites via metal-ion exchange/etching under mild reaction conditions. A remarkable 100&#xa0;mV reduction in the overpotential is observed at 10&#xa0;mA&#xa0;cm<sup>−2</sup> with ZIF-67/Fe-1 compared with pristine ZIF-67, reaching only 287&#xa0;mV. Incorporating Fe into Co‐based MOFs improves the efficiency of reaction kinetics and charge transfer, resulting in optimal OER activity. This enhancement is attributed to the synergistic effect between Fe and Co within the MOFs. A combination of experimental characterization and theoretical simulation demonstrated the modulation of the electronic structure of Co sites and intermediate binding affinity. The developed synthetic strategy exhibits broad applicability, enabling the facile synthesis of other MOFs, such as ZIF-67/Cu-1, ZIF-67/Mn-1, and ZIF-67/Ni-1, for efficient OER catalysis. The proposed strategy can be easily extended to other MOF-based OER electrocatalysts.</p> Graphical Abstract <p></p>

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Ion exchange regulation of electronic structure in zeolitic imidazolate framework-67 for boosting electrocatalytic water oxidation

  • 期刊论文

  • 发表日期：

    2026年5月3日

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  • Qi-Ling Li,
  • Ying-Zhe Zhao,
  • Jia Yu,
  • Jia-Jia Wen,
  • Wang-Qiong Xu,
  • Juan Li,
  • Jian-Jun Liu,
  • Jia Huo,
  • Fei-Xiang Cheng,
  • Shu-Biao Xia

摘要

Metal–organic frameworks (MOFs) emerge as promising materials for catalyzing the oxygen evolution reaction (OER), a fundamental process in water splitting. This study describes the development of an optimized CoFe-based MOF, demonstrating significant enhancement in its catalytic activity for the OER. The catalytic activity of zeolitic imidazolate framework-67 (ZIF-67) is markedly improved via a facile post-synthetic modification. This process involved partially substituting cobalt ions at specific sites via metal-ion exchange/etching under mild reaction conditions. A remarkable 100 mV reduction in the overpotential is observed at 10 mA cm−2 with ZIF-67/Fe-1 compared with pristine ZIF-67, reaching only 287 mV. Incorporating Fe into Co‐based MOFs improves the efficiency of reaction kinetics and charge transfer, resulting in optimal OER activity. This enhancement is attributed to the synergistic effect between Fe and Co within the MOFs. A combination of experimental characterization and theoretical simulation demonstrated the modulation of the electronic structure of Co sites and intermediate binding affinity. The developed synthetic strategy exhibits broad applicability, enabling the facile synthesis of other MOFs, such as ZIF-67/Cu-1, ZIF-67/Mn-1, and ZIF-67/Ni-1, for efficient OER catalysis. The proposed strategy can be easily extended to other MOF-based OER electrocatalysts.

Graphical Abstract