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<p>Amorphization engineering of metal-organic frameworks (MOFs) has recently emerged as a promising approach, yielding a semi-crystalline state rich in defect sites that improves the oxygen evolution reaction (OER) efficiency in the anion exchange membrane water electrolysis (AEMWE). While reversible electrochemical reconstruction of MOFs is conducive to sustaining long-term OER durability, relevant studies remain scarce. Herein, we report the targeted design of reversible and reconfigurable amorphous metal-organic framework (aMOF) electrocatalysts via a mild semi-sacrificial template approach. The resulting materials, denoted as (αFe)FeNi-aMOF/INF, exhibited abundant defect sites and ultrathin nanosheet morphology. The (1.2Fe)FeNi-aMOF/INF catalyst demonstrated markedly enhanced OER behavior, needing only 249 mV to provide a current density equal to 100&#xa0;mA cm<sup>− 2</sup>, thus displaying superior performance compared to numerous other advanced electrocatalysts. Notably, the reversible surface reconstruction of aMOF into the catalytically active <i>γ</i>-NiFeOOH phase was validated through multi-cycle experimental evaluations. The transformation in the electronic configuration of Fe sites, identified as in the genuine active centers on the surface of defect <i>γ</i>-NiFeOOH/aMOF, was corroborated by <i>operando</i> Raman spectroscopy, <i>operando</i> FT-IR spectroscopy, in situ Bode analysis, and X-ray absorption spectra, complemented by density functional theory (DFT) calculations. In addition, the constructed AEMWE device reached 1000&#xa0;mA cm<sup>− 2</sup> at 80&#xa0;°C while maintaining a low cell voltage equal to 1.90&#xa0;V. These findings offer new conceptual viewpoints on preparing aMOFs and on the mechanistic basis of OER catalysis, guiding the deliberate development of efficient OER materials for AEMWE applications.</p> Graphical abstract <p></p>

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Amorphous MOFs with electrochemically tailored reversible reconstruction to boost industrial-scale oxygen evolution reactions

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月4日

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  • Tianle Cao,
  • Fei Ni,
  • Guangli Yu,
  • Zhiqi Zhu,
  • Shulin Li,
  • Xuming Qin,
  • Haochen Peng,
  • Kangjun Wang

摘要

Amorphization engineering of metal-organic frameworks (MOFs) has recently emerged as a promising approach, yielding a semi-crystalline state rich in defect sites that improves the oxygen evolution reaction (OER) efficiency in the anion exchange membrane water electrolysis (AEMWE). While reversible electrochemical reconstruction of MOFs is conducive to sustaining long-term OER durability, relevant studies remain scarce. Herein, we report the targeted design of reversible and reconfigurable amorphous metal-organic framework (aMOF) electrocatalysts via a mild semi-sacrificial template approach. The resulting materials, denoted as (αFe)FeNi-aMOF/INF, exhibited abundant defect sites and ultrathin nanosheet morphology. The (1.2Fe)FeNi-aMOF/INF catalyst demonstrated markedly enhanced OER behavior, needing only 249 mV to provide a current density equal to 100 mA cm− 2, thus displaying superior performance compared to numerous other advanced electrocatalysts. Notably, the reversible surface reconstruction of aMOF into the catalytically active γ-NiFeOOH phase was validated through multi-cycle experimental evaluations. The transformation in the electronic configuration of Fe sites, identified as in the genuine active centers on the surface of defect γ-NiFeOOH/aMOF, was corroborated by operando Raman spectroscopy, operando FT-IR spectroscopy, in situ Bode analysis, and X-ray absorption spectra, complemented by density functional theory (DFT) calculations. In addition, the constructed AEMWE device reached 1000 mA cm− 2 at 80 °C while maintaining a low cell voltage equal to 1.90 V. These findings offer new conceptual viewpoints on preparing aMOFs and on the mechanistic basis of OER catalysis, guiding the deliberate development of efficient OER materials for AEMWE applications.

Graphical abstract