Yimeng Cao , Fang Chen , Yongshuai Chen , Mengdie Cai , Jiawei Xue , Yuxue Wei , Jia-qi Bai , Lisheng Guo , Song Sun
{"title":"二价金属阳离子双位点共掺杂策略在SrTiO3上增强光催化水分解","authors":"Yimeng Cao , Fang Chen , Yongshuai Chen , Mengdie Cai , Jiawei Xue , Yuxue Wei , Jia-qi Bai , Lisheng Guo , Song Sun","doi":"10.1016/j.ijhydene.2025.150070","DOIUrl":null,"url":null,"abstract":"<div><div>Dual-site co-doping with low-valence metal cations is a novel strategy to effectively reduce Ti<sup>3+</sup> defects in SrTiO<sub>3</sub>(STO) for efficient hydrogen generation. In this study, the K<sup>+</sup> and Al<sup>3+</sup> were successfully used to achieve co-doping at both the Sr and Ti sites of the STO perovskite structure. Notably, the optimized 0.5K, 1Al-STO sample exhibited water splitting performance of 523.73 μmol h<sup>−1</sup> for H<sub>2</sub> and 256.00 μmol h<sup>−1</sup> for O<sub>2</sub>, respectively, representing a 17.54-fold improvement compared to pure STO. This significant enhancement is attributed to binary low-valence metal dopants, which balance the electron-rich states caused by oxygen vacancies in STO and promote the re-oxidation of Ti<sup>3+</sup> to Ti<sup>4+</sup>. Furthermore, advanced characterization techniques and density functional theory (DFT) calculations indicate that K<sup>+</sup> doping facilitates the incorporation of Al<sup>3+</sup>, while their synergistic effect enhances adsorption of water molecule and lowers the activation barrier for the water splitting reaction. Therefore, the low-valence co-doping strategy provides valuable insights into the potential mechanisms of surface interactions and the improvement of catalytic performance.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"149 ","pages":"Article 150070"},"PeriodicalIF":8.3000,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A dual-site co-doping strategy with binary low-valence metal cations for enhanced photocatalytic water splitting over SrTiO3\",\"authors\":\"Yimeng Cao , Fang Chen , Yongshuai Chen , Mengdie Cai , Jiawei Xue , Yuxue Wei , Jia-qi Bai , Lisheng Guo , Song Sun\",\"doi\":\"10.1016/j.ijhydene.2025.150070\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Dual-site co-doping with low-valence metal cations is a novel strategy to effectively reduce Ti<sup>3+</sup> defects in SrTiO<sub>3</sub>(STO) for efficient hydrogen generation. In this study, the K<sup>+</sup> and Al<sup>3+</sup> were successfully used to achieve co-doping at both the Sr and Ti sites of the STO perovskite structure. Notably, the optimized 0.5K, 1Al-STO sample exhibited water splitting performance of 523.73 μmol h<sup>−1</sup> for H<sub>2</sub> and 256.00 μmol h<sup>−1</sup> for O<sub>2</sub>, respectively, representing a 17.54-fold improvement compared to pure STO. This significant enhancement is attributed to binary low-valence metal dopants, which balance the electron-rich states caused by oxygen vacancies in STO and promote the re-oxidation of Ti<sup>3+</sup> to Ti<sup>4+</sup>. Furthermore, advanced characterization techniques and density functional theory (DFT) calculations indicate that K<sup>+</sup> doping facilitates the incorporation of Al<sup>3+</sup>, while their synergistic effect enhances adsorption of water molecule and lowers the activation barrier for the water splitting reaction. Therefore, the low-valence co-doping strategy provides valuable insights into the potential mechanisms of surface interactions and the improvement of catalytic performance.</div></div>\",\"PeriodicalId\":337,\"journal\":{\"name\":\"International Journal of Hydrogen Energy\",\"volume\":\"149 \",\"pages\":\"Article 150070\"},\"PeriodicalIF\":8.3000,\"publicationDate\":\"2025-06-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"International Journal of Hydrogen Energy\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0360319925030599\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"International Journal of Hydrogen Energy","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0360319925030599","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
A dual-site co-doping strategy with binary low-valence metal cations for enhanced photocatalytic water splitting over SrTiO3
Dual-site co-doping with low-valence metal cations is a novel strategy to effectively reduce Ti3+ defects in SrTiO3(STO) for efficient hydrogen generation. In this study, the K+ and Al3+ were successfully used to achieve co-doping at both the Sr and Ti sites of the STO perovskite structure. Notably, the optimized 0.5K, 1Al-STO sample exhibited water splitting performance of 523.73 μmol h−1 for H2 and 256.00 μmol h−1 for O2, respectively, representing a 17.54-fold improvement compared to pure STO. This significant enhancement is attributed to binary low-valence metal dopants, which balance the electron-rich states caused by oxygen vacancies in STO and promote the re-oxidation of Ti3+ to Ti4+. Furthermore, advanced characterization techniques and density functional theory (DFT) calculations indicate that K+ doping facilitates the incorporation of Al3+, while their synergistic effect enhances adsorption of water molecule and lowers the activation barrier for the water splitting reaction. Therefore, the low-valence co-doping strategy provides valuable insights into the potential mechanisms of surface interactions and the improvement of catalytic performance.
期刊介绍:
The objective of the International Journal of Hydrogen Energy is to facilitate the exchange of new ideas, technological advancements, and research findings in the field of Hydrogen Energy among scientists and engineers worldwide. This journal showcases original research, both analytical and experimental, covering various aspects of Hydrogen Energy. These include production, storage, transmission, utilization, enabling technologies, environmental impact, economic considerations, and global perspectives on hydrogen and its carriers such as NH3, CH4, alcohols, etc.
The utilization aspect encompasses various methods such as thermochemical (combustion), photochemical, electrochemical (fuel cells), and nuclear conversion of hydrogen, hydrogen isotopes, and hydrogen carriers into thermal, mechanical, and electrical energies. The applications of these energies can be found in transportation (including aerospace), industrial, commercial, and residential sectors.