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<p>Understanding the structural dynamics of ligands and their interaction with catalytic centres under reaction conditions remains a fundamental challenge, yet it is essential for catalyst design. Here we reveal an in situ transformation of Ni–Fe hydroxide into a stable superoxo-hydroxide phase, which is accompanied by the formation of lattice O–O (O<sub>latt</sub>–O<sub>latt</sub>) ligands, as demonstrated using operando <sup>18</sup>O-labelling spectroelectrochemistry and machine-learning-assisted global optimization. By correlating the intrinsic activity of Fe with the O<sub>latt</sub>–O<sub>latt</sub> concentration across a series of Fe-incorporated transition-metal hydroxides and oxides, we demonstrate that O<sub>latt</sub>–O<sub>latt</sub> triggers Fe activation for oxygen evolution electrocatalysis—a finding further supported by first-principles calculations. Oxygen production proceeds via an adsorbate evolution mechanism, and the enhanced reaction kinetics stem from the lowered activation energy at surface Fe sites in the newly formed superoxo-hydroxide structure. This work offers a strategic framework for designing high-performance Fe-incorporated electrocatalysts and underscores the pivotal role of ligand dynamics in activating catalytic centres.</p><p></p>

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Lattice O–O ligands in Fe-incorporated hydroxides enhance water oxidation electrocatalysis

  • 期刊论文

  • 发表日期：

    2025年8月18日

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  • Guoshuai Shi,
  • Jili Li,
  • Tingyu Lu,
  • Chunlei Yang,
  • Qinshang Xu,
  • Huoliang Gu,
  • Haonan Tong,
  • Siwen Zhao,
  • Chenyuan Zhu,
  • Yuluo Shen,
  • Jing Wu,
  • Xianzhuo Lao,
  • Peng-Cheng Chen,
  • Jiong Li,
  • Shuo Zhang,
  • Jueli Shi,
  • Kelvin H. L. Zhang,
  • Ye-Fei Li,
  • Zhi-Pan Liu,
  • Liming Zhang

摘要

Understanding the structural dynamics of ligands and their interaction with catalytic centres under reaction conditions remains a fundamental challenge, yet it is essential for catalyst design. Here we reveal an in situ transformation of Ni–Fe hydroxide into a stable superoxo-hydroxide phase, which is accompanied by the formation of lattice O–O (Olatt–Olatt) ligands, as demonstrated using operando 18O-labelling spectroelectrochemistry and machine-learning-assisted global optimization. By correlating the intrinsic activity of Fe with the Olatt–Olatt concentration across a series of Fe-incorporated transition-metal hydroxides and oxides, we demonstrate that Olatt–Olatt triggers Fe activation for oxygen evolution electrocatalysis—a finding further supported by first-principles calculations. Oxygen production proceeds via an adsorbate evolution mechanism, and the enhanced reaction kinetics stem from the lowered activation energy at surface Fe sites in the newly formed superoxo-hydroxide structure. This work offers a strategic framework for designing high-performance Fe-incorporated electrocatalysts and underscores the pivotal role of ligand dynamics in activating catalytic centres.