{"title":"Suppressing lattice oxygen oxidation in ruthenium oxide via equivalent substitution for sustainable oxygen evolution reaction in PEMWEs","authors":"Xiaojie Chen, Rongpeng Ma, Wenqi Jia, Xuejie Cao, Jinyang Zhang, Fangyi Cheng, Lifang Jiao","doi":"10.1016/j.checat.2025.101335","DOIUrl":null,"url":null,"abstract":"Developing cost-effective Ru-based electrocatalysts for the acidic oxygen evolution reaction (OER) is crucial for proton-exchange membrane water electrolyzers (PEMWEs). However, the prominent lattice-oxygen-mediated mechanism (LOM) at high oxidative potential leads to crystal destruction and poor operational stability for RuO<sub>2</sub>. Here, we report that introducing equivalent Ti<sup>4+</sup> into RuO<sub>2</sub> can significantly suppress the oxidation of lattice oxygen. Spectroscopic and theoretical results demonstrate that Ti<sup>4+</sup> incorporation not only decreases the LOM ratio by weakening Ru–O bond covalency but also suppresses the dynamic activation of lattice oxygen at high oxidative bias by inhibiting Ru–O bond contraction. Potential-resolved differential electrochemical mass spectrometry (DEMS) verified the decreased LOM ratio (from 53.45% to 5% at 1.8 V) after Ti<sup>4+</sup> incorporation. The equivalent-Ti<sup>4+</sup>-substituted RuO<sub>2</sub> not only exhibits an extended operation time of over 500 h at 100 mA cm<sup>−2</sup> but also withstands fluctuating voltage input (1.5–1.8 V) for 120 h in PEMWEs.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"73 1","pages":""},"PeriodicalIF":11.5000,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chem Catalysis","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1016/j.checat.2025.101335","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Developing cost-effective Ru-based electrocatalysts for the acidic oxygen evolution reaction (OER) is crucial for proton-exchange membrane water electrolyzers (PEMWEs). However, the prominent lattice-oxygen-mediated mechanism (LOM) at high oxidative potential leads to crystal destruction and poor operational stability for RuO2. Here, we report that introducing equivalent Ti4+ into RuO2 can significantly suppress the oxidation of lattice oxygen. Spectroscopic and theoretical results demonstrate that Ti4+ incorporation not only decreases the LOM ratio by weakening Ru–O bond covalency but also suppresses the dynamic activation of lattice oxygen at high oxidative bias by inhibiting Ru–O bond contraction. Potential-resolved differential electrochemical mass spectrometry (DEMS) verified the decreased LOM ratio (from 53.45% to 5% at 1.8 V) after Ti4+ incorporation. The equivalent-Ti4+-substituted RuO2 not only exhibits an extended operation time of over 500 h at 100 mA cm−2 but also withstands fluctuating voltage input (1.5–1.8 V) for 120 h in PEMWEs.
期刊介绍:
Chem Catalysis is a monthly journal that publishes innovative research on fundamental and applied catalysis, providing a platform for researchers across chemistry, chemical engineering, and related fields. It serves as a premier resource for scientists and engineers in academia and industry, covering heterogeneous, homogeneous, and biocatalysis. Emphasizing transformative methods and technologies, the journal aims to advance understanding, introduce novel catalysts, and connect fundamental insights to real-world applications for societal benefit.