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<p>Alkaline hydrogen evolution reaction (HER) is fundamentally limited by the slow water-dissociation (Volmer) step, which is governed by the electric double-layer (EDL) water structure at the solution/electrode interface. Herein, we report an oxygen-bridged carbon-supported metallic Ni nanosheet array (Ni@O-C) with abundant Ni-O-C interfacial motifs derived from Ni-terephthalate metal-organic frameworks (MOFs) by thermal annealing. Ni@O-C delivers low over-potentials of 15 and 286 mV to reach 10 and 2000 mA cm<sup>−2</sup>, respectively, surpassing the state-of-the-art Pt/C, particularly at industrial-scale current densities (&gt;1000 mA cm<sup>−2</sup>). Fine structural analyses indicate that the rich Ni-O-C linkages tune the electronic states, resulting in elevated Ni oxidation states. Experiment result tests show that these oxygen-bridged sites promote the enriched free water molecules at the solution/electrode interface, dramatically accelerating water dissociation and shifting the HER rate-determining Volmer step to the Heyrovsky step. Theoretical studies verify that Ni-O-C motifs lower the energy barrier for water dissociation and optimize the hydrogen adsorption, ultimately facilitating the overall HER process.</p>

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Oxygen-bridged Ni-O-C interfaces enrich free water for ampere-level current density hydrogen evolution

  • 期刊论文

  • 发表日期：

    2026年3月12日

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  • Fanpeng Cheng,
  • Zhichao Zheng,
  • Yulu Wan,
  • Yue Yu,
  • Dashuai Wang,
  • Huijuan Guo,
  • Yi Huang,
  • Lijuan Shi,
  • Liwei Cheng,
  • Shangqing Chen,
  • Qun Yi

摘要

Alkaline hydrogen evolution reaction (HER) is fundamentally limited by the slow water-dissociation (Volmer) step, which is governed by the electric double-layer (EDL) water structure at the solution/electrode interface. Herein, we report an oxygen-bridged carbon-supported metallic Ni nanosheet array (Ni@O-C) with abundant Ni-O-C interfacial motifs derived from Ni-terephthalate metal-organic frameworks (MOFs) by thermal annealing. Ni@O-C delivers low over-potentials of 15 and 286 mV to reach 10 and 2000 mA cm−2, respectively, surpassing the state-of-the-art Pt/C, particularly at industrial-scale current densities (>1000 mA cm−2). Fine structural analyses indicate that the rich Ni-O-C linkages tune the electronic states, resulting in elevated Ni oxidation states. Experiment result tests show that these oxygen-bridged sites promote the enriched free water molecules at the solution/electrode interface, dramatically accelerating water dissociation and shifting the HER rate-determining Volmer step to the Heyrovsky step. Theoretical studies verify that Ni-O-C motifs lower the energy barrier for water dissociation and optimize the hydrogen adsorption, ultimately facilitating the overall HER process.