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<p>The generation of pure hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) through two-electron oxygen reduction reaction represents a promising avenue for sustainable chemical production. However, a fundamental understanding of inevitable reconstruction of active sites during electrolysis remains elusive, hindering the development of dualable electrocatalysts. Herein, we report a structure-adaptive electrocatalyst featuring self-regulating capabilities under reaction. A series of single-atom Ni catalysts with B/N coordination (NiB<sub>x</sub>N<sub>y</sub>) serves as a model system to explore structure flexibility. Under the applied potential, the structural evolution of Ni<sup>+0.98</sup>-B<sub>2</sub>N<sub>2</sub> into Ni<sup>+0.98</sup>-B<sub>1</sub>N<sub>2</sub> occurs at initial stage. The Ni-B and Ni-N bond length in Ni<sup>+0.98</sup>-B<sub>1</sub>N<sub>2</sub>, as the genuine active site, are self-regulated to redistribute interfacial electrons by B/N coordination and then boost both intrinsic activity and stability of Ni site. When the potential is removed, the catalyst returns to its initial Ni-B<sub>2</sub>N<sub>2</sub> configuration. The H<sub>2</sub>O<sub>2</sub> productivity is up to 9320 mmol g <sub>catalyst</sub><sup>-1</sup> h<sup>-1</sup> with a continuous output of ~5 wt% H<sub>2</sub>O<sub>2</sub> solution under industrial current density for over 300 h. This work elucidates the dynamic reconstruction-activity enhancement for H<sub>2</sub>O<sub>2</sub> electrosynthesis.</p>

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Structure-adaptive single-atom nickel catalysts for pure hydrogen peroxide electrosynthesis at industrial current density

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月26日

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  • Zining Wang,
  • Hongbao Jia,
  • Aiyang Xie,
  • Yanchao Li,
  • Zheng Chen,
  • Xunyu Lu,
  • Hongying Zhao

摘要

The generation of pure hydrogen peroxide (H2O2) through two-electron oxygen reduction reaction represents a promising avenue for sustainable chemical production. However, a fundamental understanding of inevitable reconstruction of active sites during electrolysis remains elusive, hindering the development of dualable electrocatalysts. Herein, we report a structure-adaptive electrocatalyst featuring self-regulating capabilities under reaction. A series of single-atom Ni catalysts with B/N coordination (NiBxNy) serves as a model system to explore structure flexibility. Under the applied potential, the structural evolution of Ni+0.98-B2N2 into Ni+0.98-B1N2 occurs at initial stage. The Ni-B and Ni-N bond length in Ni+0.98-B1N2, as the genuine active site, are self-regulated to redistribute interfacial electrons by B/N coordination and then boost both intrinsic activity and stability of Ni site. When the potential is removed, the catalyst returns to its initial Ni-B2N2 configuration. The H2O2 productivity is up to 9320 mmol g catalyst-1 h-1 with a continuous output of ~5 wt% H2O2 solution under industrial current density for over 300 h. This work elucidates the dynamic reconstruction-activity enhancement for H2O2 electrosynthesis.