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Related Experiment Video

Updated: May 10, 2025

Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics

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Published on: April 12, 2019

Proton-coupled electron transfer controls peroxide activation initiated by a solid-water interface.

Jian-Hua Chen¹, Wan-Ting Li^1,2, Kun-Yu Cai¹

¹Interdisciplinary Research Centre for Agriculture Green Development in Yangtze River Basin, Department of Environmental Sciences and Engineering, College of Resources and Environment, Southwest University, Chongqing, 400716, China.

Nature Communications

|April 22, 2025

Summary

This study reveals that protons and electrons are coupled in heterogeneous advanced oxidation processes. This proton-coupled electron transfer mechanism is key for developing more efficient peroxide (O-O) activation technologies.

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Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics

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Published on: August 7, 2018

Area of Science:

Environmental Science
Chemistry

Background:

Decentralized water treatment offers cost and energy advantages over centralized systems.
Heterogeneous advanced oxidation processes using peroxide (O-O) are promising for chemical water treatment.
Existing models predominantly focus on electron transfer in Fenton-like reactions.

Purpose of the Study:

To challenge the universally accepted view of electron transfer dominance in heterogeneous oxidation.
To investigate the role of protons in the redox mechanism at the solid-liquid interface.
To provide experimental evidence for proton-electron coupling in O-O activation.

Main Methods:

In situ quantitative titration to measure proton-electron coupling ratio.
Thermodynamic analyses to understand the redox cycle.
Experimental investigation of heterogeneous advanced oxidation processes.

Main Results:

Protons are thermodynamically coupled to electrons at the solid-liquid interface.
Direct experimental evidence shows a near 1:1 coupling ratio of protons to transferred electrons.
A net proton-coupled electron transfer mechanism occurs, involving both protons and electrons in the redox cycle.

Conclusions:

The study demonstrates a novel proton-coupled electron transfer mechanism in O-O activation.
Findings challenge the prevailing electron transfer-dominated model for heterogeneous oxidation.
This understanding can guide the development of more efficient redox activities in O-O activation technologies.