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Time-resolved spectroscopy uncovers deprotonation-induced reconstruction in oxygen-evolution NiFe-based (oxy)hydroxides

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  • Dan Wu

    (University of Science and Technology of China)

  • Longfei Hu

    (University of Science and Technology of China)

  • Xiaokang Liu

    (University of Science and Technology of China)

  • Tong Liu

    (University of Science and Technology of China)

  • Xiangyu Zhu

    (University of Science and Technology of China
    Anhui University)

  • Qiquan Luo

    (Anhui University)

  • Huijuan Zhang

    (University of Science and Technology of China)

  • Linlin Cao

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Jinlong Yang

    (University of Science and Technology of China)

  • Zheng Jiang

    (University of Science and Technology of China)

  • Tao Yao

    (University of Science and Technology of China
    University of Science and Technology of China
    University of Science and Technology of China)

Abstract

Transition-metal layered double hydroxides are widely utilized as electrocatalysts for the oxygen evolution reaction (OER), undergoing dynamic transformation into active oxyhydroxides during electrochemical operation. Nonetheless, our understanding of the non-equilibrium structural changes that occur during this process remains limited. In this study, utilizing in situ energy-dispersive X-ray absorption spectroscopy and machine learning analysis, we reveal the occurrence of deprotonation and elucidate the role of incorporated iron in facilitating the transition from nickel-iron layered double hydroxide (NiFe LDH) into its active oxyhydroxide. Our findings demonstrate that iron substitution promotes deprotonation process within NiFe LDH, resulting in the preferential removal of protons from the specific bridged hydroxyl group (Ni2+-OH-Fe3+) linked to edge-sharing [NiO6] and [FeO6] octahedron. This deprotonation behavior drives the formation of high-valence Ni3+δ species (0

Suggested Citation

  • Dan Wu & Longfei Hu & Xiaokang Liu & Tong Liu & Xiangyu Zhu & Qiquan Luo & Huijuan Zhang & Linlin Cao & Jinlong Yang & Zheng Jiang & Tao Yao, 2025. "Time-resolved spectroscopy uncovers deprotonation-induced reconstruction in oxygen-evolution NiFe-based (oxy)hydroxides," Nature Communications, Nature, vol. 16(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-56070-y
    DOI: 10.1038/s41467-025-56070-y
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