New Undisputed Evidence and Strategy for Enhanced Lattice‐Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation
Abstract Oxygen evolution reaction (OER) is a key half‐reaction in many electrochemical transformations, and efficient electrocatalysts are critical to improve its kinetics which is typically sluggish due to its multielectron‐transfer nature. Perovskite oxides are a popular category of OER catalysts...
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| Format: | Article |
| Language: | English |
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Wiley
2022-05-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202200530 |
| _version_ | 1818206723584819200 |
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| author | Xiaomin Xu Yangli Pan Yijun Zhong Chenliang Shi Daqin Guan Lei Ge Zhiwei Hu Yi‐Ying Chin Hong‐Ji Lin Chien‐Te Chen Hao Wang San Ping Jiang Zongping Shao |
| author_facet | Xiaomin Xu Yangli Pan Yijun Zhong Chenliang Shi Daqin Guan Lei Ge Zhiwei Hu Yi‐Ying Chin Hong‐Ji Lin Chien‐Te Chen Hao Wang San Ping Jiang Zongping Shao |
| author_sort | Xiaomin Xu |
| collection | DOAJ |
| description | Abstract Oxygen evolution reaction (OER) is a key half‐reaction in many electrochemical transformations, and efficient electrocatalysts are critical to improve its kinetics which is typically sluggish due to its multielectron‐transfer nature. Perovskite oxides are a popular category of OER catalysts, while their activity remains insufficient under the conventional adsorbate evolution reaction scheme where scaling relations limit activity enhancement. The lattice oxygen‐mediated mechanism (LOM) has been recently reported to overcome such scaling relations and boost the OER catalysis over several doped perovskite catalysts. However, direct evidence supporting the LOM participation is still very little because the doping strategy applied would introduce additional active sites that may mask the real reaction mechanism. Herein, a dopant‐free, cation deficiency manipulation strategy to tailor the bulk diffusion properties of perovskites without affecting their surface properties is reported, providing a perfect platform for studying the contribution of LOM to OER catalysis. Further optimizing the A‐site deficiency achieves a perovskite candidate with excellent intrinsic OER activity, which also demonstrates outstanding performance in rechargeable Zn–air batteries and water electrolyzers. These findings not only corroborate the key role of LOM in OER electrocatalysis, but also provide an effective way for the rational design of better catalyst materials for clean energy technologies. |
| first_indexed | 2024-12-12T04:17:34Z |
| format | Article |
| id | doaj.art-d7bc230ccb404cdeb188f0c4733d082b |
| institution | Directory Open Access Journal |
| issn | 2198-3844 |
| language | English |
| last_indexed | 2024-12-12T04:17:34Z |
| publishDate | 2022-05-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj.art-d7bc230ccb404cdeb188f0c4733d082b2022-12-22T00:38:24ZengWileyAdvanced Science2198-38442022-05-01914n/an/a10.1002/advs.202200530New Undisputed Evidence and Strategy for Enhanced Lattice‐Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency ManipulationXiaomin Xu0Yangli Pan1Yijun Zhong2Chenliang Shi3Daqin Guan4Lei Ge5Zhiwei Hu6Yi‐Ying Chin7Hong‐Ji Lin8Chien‐Te Chen9Hao Wang10San Ping Jiang11Zongping Shao12WA School of Mines: Minerals, Energy and Chemical Engineering (WASM‐MECE) Curtin University Perth WA 6102 AustraliaCentre for Future Materials University of Southern Queensland Springfield Central QLD 4300 AustraliaWA School of Mines: Minerals, Energy and Chemical Engineering (WASM‐MECE) Curtin University Perth WA 6102 AustraliaState Key Laboratory of Materials‐Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University Nanjing 211800 ChinaDepartment of Building and Real Estate Research Institute for Sustainable Urban Development (RISUD) and Research Institute for Smart Energy (RISE) The Hong Kong Polytechnic University Hung Hom Kowloon Hong Kong 999077 ChinaCentre for Future Materials University of Southern Queensland Springfield Central QLD 4300 AustraliaMax Planck Institute for Chemical Physics of Solids Nöthnitzer Str. 40 Dresden 01187 GermanyDepartment of Physics National Chung Cheng University Min‐Hsiung Chiayi 62102 TaiwanNational Synchrotron Radiation Research Center Hsinchu 30076 TaiwanNational Synchrotron Radiation Research Center Hsinchu 30076 TaiwanCentre for Future Materials University of Southern Queensland Springfield Central QLD 4300 AustraliaWA School of Mines: Minerals, Energy and Chemical Engineering (WASM‐MECE) Curtin University Perth WA 6102 AustraliaWA School of Mines: Minerals, Energy and Chemical Engineering (WASM‐MECE) Curtin University Perth WA 6102 AustraliaAbstract Oxygen evolution reaction (OER) is a key half‐reaction in many electrochemical transformations, and efficient electrocatalysts are critical to improve its kinetics which is typically sluggish due to its multielectron‐transfer nature. Perovskite oxides are a popular category of OER catalysts, while their activity remains insufficient under the conventional adsorbate evolution reaction scheme where scaling relations limit activity enhancement. The lattice oxygen‐mediated mechanism (LOM) has been recently reported to overcome such scaling relations and boost the OER catalysis over several doped perovskite catalysts. However, direct evidence supporting the LOM participation is still very little because the doping strategy applied would introduce additional active sites that may mask the real reaction mechanism. Herein, a dopant‐free, cation deficiency manipulation strategy to tailor the bulk diffusion properties of perovskites without affecting their surface properties is reported, providing a perfect platform for studying the contribution of LOM to OER catalysis. Further optimizing the A‐site deficiency achieves a perovskite candidate with excellent intrinsic OER activity, which also demonstrates outstanding performance in rechargeable Zn–air batteries and water electrolyzers. These findings not only corroborate the key role of LOM in OER electrocatalysis, but also provide an effective way for the rational design of better catalyst materials for clean energy technologies.https://doi.org/10.1002/advs.202200530cation deficiencylattice‐oxygen participationoxygen evolution reactionperovskiteswater splittingZn–air batteries |
| spellingShingle | Xiaomin Xu Yangli Pan Yijun Zhong Chenliang Shi Daqin Guan Lei Ge Zhiwei Hu Yi‐Ying Chin Hong‐Ji Lin Chien‐Te Chen Hao Wang San Ping Jiang Zongping Shao New Undisputed Evidence and Strategy for Enhanced Lattice‐Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation Advanced Science cation deficiency lattice‐oxygen participation oxygen evolution reaction perovskites water splitting Zn–air batteries |
| title | New Undisputed Evidence and Strategy for Enhanced Lattice‐Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation |
| title_full | New Undisputed Evidence and Strategy for Enhanced Lattice‐Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation |
| title_fullStr | New Undisputed Evidence and Strategy for Enhanced Lattice‐Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation |
| title_full_unstemmed | New Undisputed Evidence and Strategy for Enhanced Lattice‐Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation |
| title_short | New Undisputed Evidence and Strategy for Enhanced Lattice‐Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation |
| title_sort | new undisputed evidence and strategy for enhanced lattice oxygen participation of perovskite electrocatalyst through cation deficiency manipulation |
| topic | cation deficiency lattice‐oxygen participation oxygen evolution reaction perovskites water splitting Zn–air batteries |
| url | https://doi.org/10.1002/advs.202200530 |
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