Engineering high-density microcrystalline boundary with V-doped RuO2 for high-performance oxygen evolution in acid

Abstract Designing efficient acidic oxygen evolution catalysts for proton exchange membrane water electrolyzers is challenging due to a trade-off between activity and stability. In this work, we construct high-density microcrystalline grain boundaries (GBs) with V-dopant in RuO2 matrix (GB-V-RuO2)....

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Main Authors: Han Wu, Zhanzhao Fu, Jiangwei Chang, Zhiang Hu, Jian Li, Siyang Wang, Jingkun Yu, Xue Yong, Geoffrey I. N. Waterhouse, Zhiyong Tang, Junbiao Chang, Siyu Lu
Format: Article
Language:English
Published: Nature Portfolio 2025-05-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-59472-0
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Summary:Abstract Designing efficient acidic oxygen evolution catalysts for proton exchange membrane water electrolyzers is challenging due to a trade-off between activity and stability. In this work, we construct high-density microcrystalline grain boundaries (GBs) with V-dopant in RuO2 matrix (GB-V-RuO2). Our theoretical and experimental results indicate this is a highly active and acid-resistant OER catalyst. Specifically, the GB-V-RuO2 requires low overpotentials of 159, 222, and 300 mV to reach 10, 100, and 1500 mA cm-2 geo in 0.5 M H2SO4, respectively. Operando EIS, ATR-SEIRAS FTIR and DEMS measurements reveal the importance of GBs in stabilizing lattice oxygen and thus inhibiting the lattice oxygen mediated OER pathway. As a result, the adsorbate evolution mechanism pathway becomes dominant, even at high current densities. Density functional theory analyses confirm that GBs can stabilize V dopant and that the synergy between them modulates the electronic structure of RuO2, thus optimizing the adsorption of OER intermediate species and enhancing electrocatalyst stability. Our work demonstrates a rational strategy for overcoming the traditional activity/stability dilemma, offering good prospects of developing high-performance acidic OER catalysts.
ISSN:2041-1723