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

Zou, Yingying; Zhang, Yulin; Zhang, Chaoqi; Bao, Tong; Xi, Yamin; Ao, Niqi; Li, Zhijie; Wang, Yunying et al. · Nat Commun · 2025

basic_science · Level V

Where this comes from

Abstract

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@cMOF) heterostructure is designed for industrial-level H<sub>2</sub>O<sub>2</sub> 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 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-cMOF, 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.