Structural Modulation of Covalent Organic Frameworks for Efficient Hydrogen Peroxide Electrocatalysis - Laboratoire catalyse et spectrochimie
Article Dans Une Revue Angewandte Chemie International Edition Année : 2024

Structural Modulation of Covalent Organic Frameworks for Efficient Hydrogen Peroxide Electrocatalysis

Rui Wang
  • Fonction : Auteur
Ziqi Zhang
  • Fonction : Auteur
Haiping Zhou
  • Fonction : Auteur
Mingrui Yu
  • Fonction : Auteur
Yan Wang
  • Fonction : Auteur
Sheng Wang
  • Fonction : Auteur
Haiyan Lu
  • Fonction : Auteur
Shilun Qiu
  • Fonction : Auteur
Qianrong Fang
  • Fonction : Auteur

Résumé

The electrochemical production of hydrogen peroxide (H2O2) using metal-free catalysts has emerged as a viable and sustainable alternative to the conventional anthraquinone process. However, the precise architectural design of these electrocatalysts poses a significant challenge, requiring intricate structural engineering to optimize electron transfer during the oxygen reduction reaction (ORR). Herein, we introduce a novel design of covalent organic frameworks (COFs) that effectively shift the ORR from a four-electron to a more advantageous two-electron pathway. Notably, the JUC-660 COF, with strategically charge-modified benzyl moieties, achieved a continuous high H2O2 yield of over 1200 mmol g-1 h-1 for an impressive duration of over 85 hours in a flow cell setting, marking it as one of the most efficient metal-free and non-pyrolyzed H2O2 electrocatalysts reported to date. Theoretical computations alongside in-situ infrared spectroscopy indicate that JUC-660 markedly diminishes the adsorption of the OOH* intermediate, thereby steering the ORR towards the desired pathway. Furthermore, the versatility of JUC-660 was demonstrated through its application in the electro-Fenton reaction, where it efficiently and rapidly removed aqueous contaminants. This work delineates a pioneering approach to altering the ORR pathway, ultimately paving the way for the development of highly effective metal-free H2O2 electrocatalysts.
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Dates et versions

hal-04650621 , version 1 (16-07-2024)

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Citer

Rui Wang, Ziqi Zhang, Haiping Zhou, Mingrui Yu, Li Liao, et al.. Structural Modulation of Covalent Organic Frameworks for Efficient Hydrogen Peroxide Electrocatalysis. Angewandte Chemie International Edition, 2024, ⟨10.1002/anie.202410417⟩. ⟨hal-04650621⟩
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