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Boosting Hydrogen Peroxide Electrosynthesis via Modulating the Interfacial Hydrogen‐Bond Environment

Yushuang Fang, Fan Yu, Kunchi Xie, Wangxin Ge, Yihua Zhu, Zhiwen Qi, Zhen Song, Hongliang Jiang, Chunzhong Li

2023Angewandte Chemie International Edition99 citationsDOIOpen Access PDF

Abstract

Abstract Designing highly efficient and stable electrode‐electrolyte interface for hydrogen peroxide (H 2 O 2 ) electrosynthesis remains challenging. Inhibiting the competitive side reaction, 4 e − oxygen reduction to H 2 O, is essential for highly selective H 2 O 2 electrosynthesis. Instead of hindering excessive hydrogenation of H 2 O 2 via catalyst modification, we discover that adding a hydrogen‐bond acceptor, dimethyl sulfoxide (DMSO), to the KOH electrolyte enables simultaneous improvement of the selectivity and activity of H 2 O 2 electrosynthesis. Spectral characterization and molecular simulation confirm that the formation of hydrogen bonds between DMSO and water molecules at the electrode‐electrolyte interface can reduce the activity of water dissociation into active H* species. The suitable H* supply environment hinders excessive hydrogenation of the oxygen reduction reaction (ORR), thus improving the selectivity of 2 e − ORR and achieving over 90 % selectivity of H 2 O 2 . This work highlights the importance of regulating the interfacial hydrogen‐bond environment by organic molecules as a means of boosting electrochemical performance in aqueous electrosynthesis and beyond.

Topics & Concepts

ElectrosynthesisHydrogen peroxideHydrogen bondChemistryBoosting (machine learning)PhotochemistryCombinatorial chemistryOrganic chemistryElectrochemistryMoleculeComputer sciencePhysical chemistryElectrodeMachine learningCO2 Reduction Techniques and CatalystsAdvanced battery technologies researchElectrocatalysts for Energy Conversion