Tailoring the electron redistribution of RuO2 by constructing a Ru-O-La asymmetric configuration for efficient acidic oxygen evolution
Stabilizing the highly active RuO2 electrocatalyst for the oxygen evolution reaction (OER) is critical for the application of proton exchange membrane water electrolysis, but this remains challenging due to the inevitable over-oxidation of Ru in harsh oxidative environments. Herein, we describe cons...
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KeAi Communications Co. Ltd.
2025-01-01
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| Series: | eScience |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2667141724001009 |
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| author | Cong-Hui Li Cheng-Zong Yuan Xiaolei Huang Hongrui Zhao Fuling Wu Lei Xin Xiaomeng Zhang Shufeng Ye Yunfa Chen |
| author_facet | Cong-Hui Li Cheng-Zong Yuan Xiaolei Huang Hongrui Zhao Fuling Wu Lei Xin Xiaomeng Zhang Shufeng Ye Yunfa Chen |
| author_sort | Cong-Hui Li |
| collection | DOAJ |
| description | Stabilizing the highly active RuO2 electrocatalyst for the oxygen evolution reaction (OER) is critical for the application of proton exchange membrane water electrolysis, but this remains challenging due to the inevitable over-oxidation of Ru in harsh oxidative environments. Herein, we describe constructing Ru-O-La asymmetric configurations into RuO2 via a facile sol-gel method to tailor electron redistribution and thereby eliminate the over-oxidation of Ru centers. Specifically, the as-prepared optimal La0.1Ru0.9O2 shows a low overpotential of 188 mV at 10 mA cm−2, a high mass activity of 251 A gRu−1 at 1.6 V vs. reversible hydrogen electrode (RHE), and a long-lasting durability of 63 h, far superior to the 8 h achieved by standard RuO2. Experiments and density functional theory calculations jointly reveal that the Ru-O-La asymmetric configuration could trigger electron redistribution in RuO2. More importantly, electron transfer from La to Ru via the Ru-O-La configuration could lead to increased electron density around Ru, thus preventing the over-oxidation of Ru. In addition, electron redistribution tunes the Ru 4d band center’s energy level, which optimizes the adsorption and desorption of oxygen intermediates. This work offers an effective strategy for regulating electronic structure to synergistically boost the activity and stability of RuO2-based acidic OER electrocatalysts. |
| format | Article |
| id | doaj-art-310bd4da80cb4626a7f4d9364bebcc62 |
| institution | Kabale University |
| issn | 2667-1417 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | KeAi Communications Co. Ltd. |
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| series | eScience |
| spelling | doaj-art-310bd4da80cb4626a7f4d9364bebcc622025-01-04T04:57:22ZengKeAi Communications Co. Ltd.eScience2667-14172025-01-0151100307Tailoring the electron redistribution of RuO2 by constructing a Ru-O-La asymmetric configuration for efficient acidic oxygen evolutionCong-Hui Li0Cheng-Zong Yuan1Xiaolei Huang2Hongrui Zhao3Fuling Wu4Lei Xin5Xiaomeng Zhang6Shufeng Ye7Yunfa Chen8School of Rare Earths, University of Science and Technology of China, Hefei 230026, China; Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganjiang 341119, ChinaSchool of Rare Earths, University of Science and Technology of China, Hefei 230026, China; Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganjiang 341119, China; Corresponding authors.School of Rare Earths, University of Science and Technology of China, Hefei 230026, China; Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganjiang 341119, ChinaSchool of Rare Earths, University of Science and Technology of China, Hefei 230026, China; Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganjiang 341119, ChinaSchool of Rare Earths, University of Science and Technology of China, Hefei 230026, China; Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganjiang 341119, ChinaSchool of Rare Earths, University of Science and Technology of China, Hefei 230026, China; Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganjiang 341119, ChinaSchool of Rare Earths, University of Science and Technology of China, Hefei 230026, China; Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganjiang 341119, China; State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China; Corresponding authors.State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, ChinaState Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, ChinaStabilizing the highly active RuO2 electrocatalyst for the oxygen evolution reaction (OER) is critical for the application of proton exchange membrane water electrolysis, but this remains challenging due to the inevitable over-oxidation of Ru in harsh oxidative environments. Herein, we describe constructing Ru-O-La asymmetric configurations into RuO2 via a facile sol-gel method to tailor electron redistribution and thereby eliminate the over-oxidation of Ru centers. Specifically, the as-prepared optimal La0.1Ru0.9O2 shows a low overpotential of 188 mV at 10 mA cm−2, a high mass activity of 251 A gRu−1 at 1.6 V vs. reversible hydrogen electrode (RHE), and a long-lasting durability of 63 h, far superior to the 8 h achieved by standard RuO2. Experiments and density functional theory calculations jointly reveal that the Ru-O-La asymmetric configuration could trigger electron redistribution in RuO2. More importantly, electron transfer from La to Ru via the Ru-O-La configuration could lead to increased electron density around Ru, thus preventing the over-oxidation of Ru. In addition, electron redistribution tunes the Ru 4d band center’s energy level, which optimizes the adsorption and desorption of oxygen intermediates. This work offers an effective strategy for regulating electronic structure to synergistically boost the activity and stability of RuO2-based acidic OER electrocatalysts.http://www.sciencedirect.com/science/article/pii/S2667141724001009Ru-O-La asymmetric configurationElectron redistributiond-band centerEnhanced stabilityAcidic oxygen evolution |
| spellingShingle | Cong-Hui Li Cheng-Zong Yuan Xiaolei Huang Hongrui Zhao Fuling Wu Lei Xin Xiaomeng Zhang Shufeng Ye Yunfa Chen Tailoring the electron redistribution of RuO2 by constructing a Ru-O-La asymmetric configuration for efficient acidic oxygen evolution eScience Ru-O-La asymmetric configuration Electron redistribution d-band center Enhanced stability Acidic oxygen evolution |
| title | Tailoring the electron redistribution of RuO2 by constructing a Ru-O-La asymmetric configuration for efficient acidic oxygen evolution |
| title_full | Tailoring the electron redistribution of RuO2 by constructing a Ru-O-La asymmetric configuration for efficient acidic oxygen evolution |
| title_fullStr | Tailoring the electron redistribution of RuO2 by constructing a Ru-O-La asymmetric configuration for efficient acidic oxygen evolution |
| title_full_unstemmed | Tailoring the electron redistribution of RuO2 by constructing a Ru-O-La asymmetric configuration for efficient acidic oxygen evolution |
| title_short | Tailoring the electron redistribution of RuO2 by constructing a Ru-O-La asymmetric configuration for efficient acidic oxygen evolution |
| title_sort | tailoring the electron redistribution of ruo2 by constructing a ru o la asymmetric configuration for efficient acidic oxygen evolution |
| topic | Ru-O-La asymmetric configuration Electron redistribution d-band center Enhanced stability Acidic oxygen evolution |
| url | http://www.sciencedirect.com/science/article/pii/S2667141724001009 |
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