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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author 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
author_facet 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
author_sort Han Wu
collection DOAJ
description 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.
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spelling doaj-art-22a0d164b7ea4ddf97fc122c6aabd31e2025-08-20T01:51:28ZengNature PortfolioNature Communications2041-17232025-05-0116111210.1038/s41467-025-59472-0Engineering high-density microcrystalline boundary with V-doped RuO2 for high-performance oxygen evolution in acidHan Wu0Zhanzhao Fu1Jiangwei Chang2Zhiang Hu3Jian Li4Siyang Wang5Jingkun Yu6Xue Yong7Geoffrey I. N. Waterhouse8Zhiyong Tang9Junbiao Chang10Siyu Lu11College of Chemistry and Pingyuan Laboratory, Zhengzhou UniversityState Key Laboratory for Clean Energy Utilization, Institute for Thermal Power Engineering, Zhejiang UniversityCollege of Chemistry and Pingyuan Laboratory, Zhengzhou UniversityCollege of Chemistry and Pingyuan Laboratory, Zhengzhou UniversityCollege of Chemistry and Pingyuan Laboratory, Zhengzhou UniversityCollege of Chemistry and Pingyuan Laboratory, Zhengzhou UniversityCollege of Chemistry and Pingyuan Laboratory, Zhengzhou UniversityDepartment of Electrical Engineering and Electronics, University of LiverpoolSchool of Chemical Sciences, The University of AucklandCAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and TechnologyCollege of Chemistry and Pingyuan Laboratory, Zhengzhou UniversityCollege of Chemistry and Pingyuan Laboratory, Zhengzhou UniversityAbstract 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.https://doi.org/10.1038/s41467-025-59472-0
spellingShingle 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
Engineering high-density microcrystalline boundary with V-doped RuO2 for high-performance oxygen evolution in acid
Nature Communications
title Engineering high-density microcrystalline boundary with V-doped RuO2 for high-performance oxygen evolution in acid
title_full Engineering high-density microcrystalline boundary with V-doped RuO2 for high-performance oxygen evolution in acid
title_fullStr Engineering high-density microcrystalline boundary with V-doped RuO2 for high-performance oxygen evolution in acid
title_full_unstemmed Engineering high-density microcrystalline boundary with V-doped RuO2 for high-performance oxygen evolution in acid
title_short Engineering high-density microcrystalline boundary with V-doped RuO2 for high-performance oxygen evolution in acid
title_sort engineering high density microcrystalline boundary with v doped ruo2 for high performance oxygen evolution in acid
url https://doi.org/10.1038/s41467-025-59472-0
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