Suppression of Oxygen Vacancies in Rutile Ruo2 via In Situ Exsolution for Enhanced Water Electrocatalysis

Abstract Elemental vacancies are proposed as an effective approach to tuning the electronic structure of catalysts that are critical for energy conversion. However, for reactions such as the sluggish oxygen evolution reaction, the excess of oxygen vacancies (VO) is inevitable and detrimental to cata...

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Main Authors: Yudi Zhang, Yan Wang, Wen Sun, Dandan Ma, Jinfu Ma, Jiancun Rao, Qiunan Xu, Juntao Huo, Jian Liu, Guowei Li
Format: Article
Language:English
Published: Wiley-VCH 2023-06-01
Series:Advanced Materials Interfaces
Subjects:
Online Access:https://doi.org/10.1002/admi.202300279
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author Yudi Zhang
Yan Wang
Wen Sun
Dandan Ma
Jinfu Ma
Jiancun Rao
Qiunan Xu
Juntao Huo
Jian Liu
Guowei Li
author_facet Yudi Zhang
Yan Wang
Wen Sun
Dandan Ma
Jinfu Ma
Jiancun Rao
Qiunan Xu
Juntao Huo
Jian Liu
Guowei Li
author_sort Yudi Zhang
collection DOAJ
description Abstract Elemental vacancies are proposed as an effective approach to tuning the electronic structure of catalysts that are critical for energy conversion. However, for reactions such as the sluggish oxygen evolution reaction, the excess of oxygen vacancies (VO) is inevitable and detrimental to catalysts’ electrochemical stability and activities, e.g., in the most active RuO2. While significant work is carried out to hinder the formation of VO, the development of a fast and efficient strategy is limited. Herein, a protection SrO layer produced successfully at the surface of RuO2 with the in situ exsolution method with perovskite SrRuO3 as the precatalyst, which could significantly hinder the generation of VO. Benefited from the suppression of VO, the surface‐modified RuO2 requires a low overpotential of 290 mV at 100 mA cm−2, accompanied by remarkably high electrochemical stability (100 h) and Faraday efficiency (≈100%). Theoretical investigation reveals that the formation energy of VO in RuO2 is almost doubled in the exsolved RuO2 phase as a result of the weakened RuO bond covalency. This work not only provides insight into the structural evolution of perovskite oxide catalysts but also demonstrates the feasibility of controlling vacancy formation via in situ exsolution.
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spelling doaj.art-f3ec494dd5644e2c8d068038b9e938082023-09-21T03:12:59ZengWiley-VCHAdvanced Materials Interfaces2196-73502023-06-011017n/an/a10.1002/admi.202300279Suppression of Oxygen Vacancies in Rutile Ruo2 via In Situ Exsolution for Enhanced Water ElectrocatalysisYudi Zhang0Yan Wang1Wen Sun2Dandan Ma3Jinfu Ma4Jiancun Rao5Qiunan Xu6Juntao Huo7Jian Liu8Guowei Li9CAS Key Laboratory of Magnetic Materials and Devices/Zhejiang Province Key Laboratory of Magnetic Materials and Application Technology Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Ningbo 315201 ChinaQingdao Institute for Theoretical and Computational Sciences Shandong University Qingdao 266237 ChinaCAS Key Laboratory of Magnetic Materials and Devices/Zhejiang Province Key Laboratory of Magnetic Materials and Application Technology Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Ningbo 315201 ChinaSchool of Materials Science and Engineering North Minzu University Yinchuan 750021 ChinaSchool of Materials Science and Engineering North Minzu University Yinchuan 750021 ChinaAIM Lab Maryland NanoCenter University of Maryland MD 20742 USAQingdao Institute for Theoretical and Computational Sciences Shandong University Qingdao 266237 ChinaCAS Key Laboratory of Magnetic Materials and Devices/Zhejiang Province Key Laboratory of Magnetic Materials and Application Technology Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Ningbo 315201 ChinaCenter for Advanced Solidification Technology School of Materials Science and Engineering Shanghai University Shanghai 200444 ChinaCAS Key Laboratory of Magnetic Materials and Devices/Zhejiang Province Key Laboratory of Magnetic Materials and Application Technology Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Ningbo 315201 ChinaAbstract Elemental vacancies are proposed as an effective approach to tuning the electronic structure of catalysts that are critical for energy conversion. However, for reactions such as the sluggish oxygen evolution reaction, the excess of oxygen vacancies (VO) is inevitable and detrimental to catalysts’ electrochemical stability and activities, e.g., in the most active RuO2. While significant work is carried out to hinder the formation of VO, the development of a fast and efficient strategy is limited. Herein, a protection SrO layer produced successfully at the surface of RuO2 with the in situ exsolution method with perovskite SrRuO3 as the precatalyst, which could significantly hinder the generation of VO. Benefited from the suppression of VO, the surface‐modified RuO2 requires a low overpotential of 290 mV at 100 mA cm−2, accompanied by remarkably high electrochemical stability (100 h) and Faraday efficiency (≈100%). Theoretical investigation reveals that the formation energy of VO in RuO2 is almost doubled in the exsolved RuO2 phase as a result of the weakened RuO bond covalency. This work not only provides insight into the structural evolution of perovskite oxide catalysts but also demonstrates the feasibility of controlling vacancy formation via in situ exsolution.https://doi.org/10.1002/admi.202300279exsolutionoxygen evolution reactionoxygen vacanciesRuO 2
spellingShingle Yudi Zhang
Yan Wang
Wen Sun
Dandan Ma
Jinfu Ma
Jiancun Rao
Qiunan Xu
Juntao Huo
Jian Liu
Guowei Li
Suppression of Oxygen Vacancies in Rutile Ruo2 via In Situ Exsolution for Enhanced Water Electrocatalysis
Advanced Materials Interfaces
exsolution
oxygen evolution reaction
oxygen vacancies
RuO 2
title Suppression of Oxygen Vacancies in Rutile Ruo2 via In Situ Exsolution for Enhanced Water Electrocatalysis
title_full Suppression of Oxygen Vacancies in Rutile Ruo2 via In Situ Exsolution for Enhanced Water Electrocatalysis
title_fullStr Suppression of Oxygen Vacancies in Rutile Ruo2 via In Situ Exsolution for Enhanced Water Electrocatalysis
title_full_unstemmed Suppression of Oxygen Vacancies in Rutile Ruo2 via In Situ Exsolution for Enhanced Water Electrocatalysis
title_short Suppression of Oxygen Vacancies in Rutile Ruo2 via In Situ Exsolution for Enhanced Water Electrocatalysis
title_sort suppression of oxygen vacancies in rutile ruo2 via in situ exsolution for enhanced water electrocatalysis
topic exsolution
oxygen evolution reaction
oxygen vacancies
RuO 2
url https://doi.org/10.1002/admi.202300279
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