Cr dopant mediates hydroxyl spillover on RuO2 for high-efficiency proton exchange membrane electrolysis

IF 14.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Nature Communications Pub Date : 2024-09-09 DOI:10.1038/s41467-024-51871-z

Yu Shen, Xiao-Long Zhang, Ming-Rong Qu, Jie Ma, Sheng Zhu, Yu-Lin Min, Min-Rui Gao, Shu-Hong Yu

{"title":"Cr dopant mediates hydroxyl spillover on RuO2 for high-efficiency proton exchange membrane electrolysis","authors":"Yu Shen, Xiao-Long Zhang, Ming-Rong Qu, Jie Ma, Sheng Zhu, Yu-Lin Min, Min-Rui Gao, Shu-Hong Yu","doi":"10.1038/s41467-024-51871-z","DOIUrl":null,"url":null,"abstract":"Simultaneously improving the activity and stability of catalysts for anodic oxygen evolution reaction (OER) in proton exchange membrane water electrolysis (PEMWE) remains a notable challenge. Here, we report a chromium-doped ruthenium dioxide with oxygen vacancies, termed Cr0.2Ru0.8O2-x, that drives OER with an overpotential of 170 mV at 10 mA cm−2 and operates stably over 2000 h in acidic media. Experimental and theoretical studies show that the synergy of Cr dopant and oxygen vacancy induces an unconventional dopant-mediated hydroxyl spillover mechanism. Such dynamic hydroxyl spillover from Cr dopant to Ru active site changes the rate-determining step from OOH* formation to O2 formation and thus greatly improves the OER performance. Moreover, the Cr dopant and oxygen vacancy also play a crucial role in stabilizing surface Ru and lattice oxygen in the Ru-O-Cr structural motif. When assembled into the anode of a practical PEMWE device, Cr0.2Ru0.8O2-x enables long-term durability of over 200 h at an ampere-level current density and 60 degrees centigrade.","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":null,"pages":null},"PeriodicalIF":14.7000,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-024-51871-z","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}

引用次数: 0

Abstract

Simultaneously improving the activity and stability of catalysts for anodic oxygen evolution reaction (OER) in proton exchange membrane water electrolysis (PEMWE) remains a notable challenge. Here, we report a chromium-doped ruthenium dioxide with oxygen vacancies, termed Cr_0.2Ru_0.8O_2-x, that drives OER with an overpotential of 170 mV at 10 mA cm⁻² and operates stably over 2000 h in acidic media. Experimental and theoretical studies show that the synergy of Cr dopant and oxygen vacancy induces an unconventional dopant-mediated hydroxyl spillover mechanism. Such dynamic hydroxyl spillover from Cr dopant to Ru active site changes the rate-determining step from OOH* formation to O₂ formation and thus greatly improves the OER performance. Moreover, the Cr dopant and oxygen vacancy also play a crucial role in stabilizing surface Ru and lattice oxygen in the Ru-O-Cr structural motif. When assembled into the anode of a practical PEMWE device, Cr_0.2Ru_0.8O_2-x enables long-term durability of over 200 h at an ampere-level current density and 60 degrees centigrade.

Abstract Image

查看原文

微信好友朋友圈 QQ好友复制链接

本刊更多论文

铬掺杂剂介导 RuO2 上的羟基溢出，实现高效质子交换膜电解

同时提高质子交换膜电解水（PEMWE）中阳极氧进化反应（OER）催化剂的活性和稳定性仍然是一个显著的挑战。在此，我们报告了一种掺杂铬的二氧化钌（称为 Cr0.2Ru0.8O2-x），它具有氧空位，在 10 mA cm-2 的过电位为 170 mV 时可驱动 OER，并可在酸性介质中稳定运行 2000 小时。实验和理论研究表明，铬掺杂剂和氧空位的协同作用诱导了一种非传统的掺杂剂介导的羟基溢出机制。这种从掺杂铬到 Ru 活性位点的动态羟基溢出将速率决定步骤从 OOH* 的形成改变为 O2 的形成，从而大大提高了 OER 的性能。此外，Cr 掺杂剂和氧空位在稳定 Ru-O-Cr 结构图案中的表面 Ru 和晶格氧方面也起着至关重要的作用。当把 Cr0.2Ru0.8O2-x 装入实用 PEMWE 器件的阳极时，它能在安培电流密度和 60 摄氏度条件下长期保持 200 小时以上的耐用性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文去求助

来源期刊

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

期刊介绍： Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.