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Engineering high-density microcrystalline boundary with V-doped RuO2 for high-performance oxygen evolution in acid
Han Wu1, Zhanzhao Fu2, Jiangwei Chang3
1College of Chemistry and Pingyuan Laboratory, Zhengzhou University, Zhengzhou, 450001, P.R. China.
Nature Communications
|May 14, 2025
Summary
This study introduces V-doped RuO2 with grain boundaries (GB-V-RuO2) as a highly active and stable oxygen evolution catalyst for water electrolyzers. This new catalyst overcomes the typical activity-stability trade-off in acidic environments.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Designing efficient acidic oxygen evolution catalysts for proton exchange membrane water electrolyzers faces challenges due to the activity-stability trade-off.
- Ruthenium dioxide (RuO2) is a promising material, but its performance in acidic conditions is limited.
Purpose of the Study:
- To develop a highly active and acid-resistant oxygen evolution reaction (OER) catalyst by engineering RuO2.
- To investigate the role of grain boundaries and vanadium doping in enhancing catalyst performance.
Main Methods:
- Synthesis of high-density microcrystalline grain boundaries with V-dopant in RuO2 matrix (GB-V-RuO2).
- Electrochemical characterization including overpotential measurements at various current densities in 0.5 M H2SO4.
- Operando techniques such as Electrochemical Impedance Spectroscopy (EIS), Attenuated Total Reflection Surface-Enhanced Infrared Reflection Absorption Spectroscopy (ATR-SEIRAS FTIR), and Differential Electrochemical Mass Spectrometry (DEMS).
- Density Functional Theory (DFT) analyses to understand the electronic structure and reaction mechanisms.
Main Results:
- GB-V-RuO2 demonstrated low overpotentials: 159 mV at 10 mA cm-2, 222 mV at 100 mA cm-2, and 300 mV at 1500 mA cm-2.
- Operando studies revealed that grain boundaries stabilize lattice oxygen, suppressing the lattice oxygen-mediated OER pathway and promoting the adsorbate evolution mechanism pathway, even at high current densities.
- DFT calculations confirmed that grain boundaries stabilize V dopants, synergistically modulating the electronic structure of RuO2 for optimized intermediate adsorption and enhanced stability.
Conclusions:
- The engineered GB-V-RuO2 catalyst effectively overcomes the traditional activity/stability dilemma in acidic OER.
- This rational design strategy offers significant potential for developing high-performance acidic OER catalysts for water electrolyzers.
