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Tuning interfacial proton transfer for directing oxygen reduction reaction toward hydrogen peroxide
Yu Fan1,2, Hao Chen1, Wangxin Ge2
1Key Laboratory for Ultrafine Materials of Ministry of Education, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China.
National Science Review
|November 13, 2025
Summary
Chelating molecules in electrolytes can tune interfacial proton transfer, enhancing electrochemical reactions. Ethylenediaminetetraacetic acid (EDTA) directs oxygen reduction reactions (ORR) towards hydrogen peroxide (H2O2) electrosynthesis.
Area of Science:
- Electrochemistry
- Surface Science
- Materials Science
Background:
- Proton transfer at electrified interfaces is crucial for proton-coupled electron transfer (PCET) reactions.
- Electrolyte engineering offers a promising avenue for optimizing interfacial proton transfer and electrochemical performance.
- Directing the oxygen reduction reaction (ORR) towards specific products like hydrogen peroxide (H2O2) is vital for electrosynthesis.
Purpose of the Study:
- To investigate the role of chelating molecules as electrolyte additives for controlling interfacial proton transfer.
- To establish chelation strength as a criterion for selecting additives to enhance H2O2 electrosynthesis via ORR.
- To understand how electrolyte additives modify hydrogen-bond networks and influence PCET kinetics.
Main Methods:
- Utilized chelating molecules with varying strengths as alkaline electrolyte additives.
- Investigated the impact of these additives on cation solvation shells and interfacial hydrogen-bond networks.
- Analyzed the effect of modified hydrogen-bond networks on proton transfer dynamics and ORR pathways.
- Quantified H2O2 selectivity and Faradaic efficiency in electrolytes with different additives.
Main Results:
- Chelating molecules disrupt long-range hydrogen-bond networks by forming rigid near-range bonds, slowing proton transfer.
- Ethylenediaminetetraacetic acid (EDTA), with strong chelation, effectively modulates proton availability at the interface.
- EDTA addition decelerates 4e- PCET kinetics, favoring the 2e- pathway for H2O2 production.
- EDTA-containing electrolytes exhibit significantly enhanced H2O2 selectivity and Faradaic efficiency compared to other systems.
Conclusions:
- Chelation strength of additives is a key factor in directing ORR towards H2O2 electrosynthesis.
- Interfacial hydrogen-bond networks play a critical role in regulating electrochemical reaction kinetics.
- This study provides a strategy for designing electrolytes to optimize electrochemical reactions, including H2O2 production.
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