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<p>Electrochemical two-electron oxygen reduction reaction (2e<sup>–</sup> ORR) in neutral environments holds remarkable promise for sustainable hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production. However, its practical application is largely hindered due to the scarcity of electrocatalysts with high selectivity and durability under ampere-level current densities. Herein, a hydrogen-bonded organic framework@conductive metal-organic framework (HOF@<i>c</i>MOF) heterostructure is designed for industrial-level H<sub>2</sub>O<sub>2</sub> electrosynthesis. Through integrating DAT-HOF (DAT=diaminotriazole) and Co-<i>c</i>MOF, Co-N bonds formed at the heterointerface modulates the electronic structure of Co sites, optimizing the adsorption strength of oxygen intermediates with improved activity and selectivity. Besides, the formation of built-in electric field drives the proton migration from DAT-HOF to Co-<i>c</i>MOF, facilitating the O<sub>2</sub> protonation to H<sub>2</sub>O<sub>2</sub> at Co sites. In further combination with the high proton donation capability of DAT-HOF and high conductivity of Co-<i>c</i>MOF, efficient H<sub>2</sub>O<sub>2</sub> production is achieved with a H<sub>2</sub>O<sub>2</sub> Faradic efficiency of 97.1 ± 0.4%, a H<sub>2</sub>O<sub>2</sub> yield of 738.9 mg h⁻<sup>1</sup> cm⁻<sup>2</sup> and a long-term durability over 100 h at 1200 mA cm⁻<sup>2</sup>. This work offers a high-performance electrocatalyst for promoting the industrial implementation of H<sub>2</sub>O<sub>2</sub> electrosynthesis.</p>

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Hydrogen-bonded organic framework@conductive metal-organic framework heterostructures for ampere-level hydrogen peroxide production

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月4日

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  • Yingying Zou,
  • Yulin Zhang,
  • Chaoqi Zhang,
  • Tong Bao,
  • Yamin Xi,
  • Niqi Ao,
  • Zhijie Li,
  • Yunying Wang,
  • Chao Liu,
  • Chengzhong Yu

摘要

Electrochemical two-electron oxygen reduction reaction (2e– ORR) in neutral environments holds remarkable promise for sustainable hydrogen peroxide (H2O2) production. However, its practical application is largely hindered due to the scarcity of electrocatalysts with high selectivity and durability under ampere-level current densities. Herein, a hydrogen-bonded organic framework@conductive metal-organic framework (HOF@cMOF) heterostructure is designed for industrial-level H2O2 electrosynthesis. Through integrating DAT-HOF (DAT=diaminotriazole) and Co-cMOF, Co-N bonds formed at the heterointerface modulates the electronic structure of Co sites, optimizing the adsorption strength of oxygen intermediates with improved activity and selectivity. Besides, the formation of built-in electric field drives the proton migration from DAT-HOF to Co-cMOF, facilitating the O2 protonation to H2O2 at Co sites. In further combination with the high proton donation capability of DAT-HOF and high conductivity of Co-cMOF, efficient H2O2 production is achieved with a H2O2 Faradic efficiency of 97.1 ± 0.4%, a H2O2 yield of 738.9 mg h⁻1 cm⁻2 and a long-term durability over 100 h at 1200 mA cm⁻2. This work offers a high-performance electrocatalyst for promoting the industrial implementation of H2O2 electrosynthesis.