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Mechanism of Cations Suppressing Proton Diffusion Kinetics for Electrocatalysis
Xiao-Yu Li1, Tao Wang1, Yu-Chen Cai1
1State Key Laboratory of Physical Chemistry of Solid Surfaces, Tan Kah Kee Innovation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, P. R. China.
Angewandte Chemie (International Ed. in English)
|February 10, 2023
Summary
Cations at electrochemical interfaces significantly slow proton transfer, impacting electrocatalysis. This study reveals cation-induced water structure changes, not electric fields, are key to this kinetic suppression.
Area of Science:
- Electrochemistry
- Physical Chemistry
- Materials Science
Background:
- Proton transfer is vital for electrocatalysis.
- Accumulating cations at interfaces can tune electrocatalytic performance.
- The precise mechanism of cation influence on proton transfer remains unclear.
Purpose of the Study:
- To quantify the effect of cations on proton diffusion rates during electrocatalysis.
- To elucidate the underlying mechanism by which cations alter proton transfer kinetics.
- To explore strategies for tuning electrocatalytic performance through cation-mediated effects.
Main Methods:
- Hydrogen evolution reaction (HER) on microelectrodes to measure proton diffusion.
- Fourier-transform infrared (FTIR) spectroscopy to probe water structure.
- Path integral molecular dynamics (PIMD) simulations to model proton behavior.
Main Results:
- Cation accumulation suppressed proton transfer rates by over 10 times.
- The primary mechanism involves cation-induced alterations in water structure, not electric field modification.
- Protons were observed to diffuse within cation hydration shells, disrupting bulk water networks.
- Disrupted water network connectivity significantly impedes proton hopping.
Conclusions:
- Cation-induced changes in water structure are the dominant factor regulating proton transfer kinetics.
- Altering water structure offers a novel approach to control proton transfer in electrocatalysis.
- Understanding these effects can guide the design of more efficient electrocatalytic systems.
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