{"title":"Periodic Macroporous K<sub>2</sub>Ta<sub>2</sub>O<sub>6</sub> Fabricated for Photocatalytic Hydrogen Production from Pure Water Splitting.","authors":"Shaoqiang You, Yuan Liu, Ling Zhou, Ping Niu, Junchao Wei, Rongbin Zhang, Xuewen Wang","doi":"10.1021/acs.inorgchem.4c05279","DOIUrl":null,"url":null,"abstract":"<p><p>Periodic macroporous materials are extensively utilized in photocatalytic hydrogen production from water splitting owing to their smooth mass transfer and abundant active sites. Therefore, it is essential to develop highly stable materials featuring interconnected channels and appropriate surface states to enhance the photocatalytic capability. Periodic macroporous K<sub>2</sub>Ta<sub>2</sub>O<sub>6</sub> (PM-K<sub>2</sub>Ta<sub>2</sub>O<sub>6</sub>) with a pyrochlore structure emerges as the ideal candidate to fulfill these requirements. Adding oxygen vacancies to PM-K<sub>2</sub>Ta<sub>2</sub>O<sub>6</sub> also makes it easier for localized energy levels to develop inside the bandgap, which improves light absorption and maximizes surface active sites. In comparison to nonporous K<sub>2</sub>Ta<sub>2</sub>O<sub>6</sub>, PM-K<sub>2</sub>Ta<sub>2</sub>O<sub>6</sub> exhibits a broad light absorption band, rapid carrier transfer rates, prolonged photogenerated carrier lifetimes, high surface area, and abundant active sites, thus enabling stable photocatalytic hydrogen production from pure water. During surface photochemical reactions, the photogenerated electrons and holes in PM-K<sub>2</sub>Ta<sub>2</sub>O<sub>6</sub> are more readily trapped and subsequently participate in pure water splitting. The H<sub>2</sub> produced by PM-K<sub>2</sub>Ta<sub>2</sub>O<sub>6</sub> is 1285.91 μmol g<sup>-1</sup> in the 5 h H<sub>2</sub> production test. Herein, we propose a strategy for developing periodic macropore catalysts capable of efficiently decomposing pure water to produce H<sub>2</sub> without necessitating cocatalysts.</p>","PeriodicalId":40,"journal":{"name":"Inorganic Chemistry","volume":" ","pages":""},"PeriodicalIF":4.3000,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Inorganic Chemistry","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.inorgchem.4c05279","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
引用次数: 0
Abstract
Periodic macroporous materials are extensively utilized in photocatalytic hydrogen production from water splitting owing to their smooth mass transfer and abundant active sites. Therefore, it is essential to develop highly stable materials featuring interconnected channels and appropriate surface states to enhance the photocatalytic capability. Periodic macroporous K2Ta2O6 (PM-K2Ta2O6) with a pyrochlore structure emerges as the ideal candidate to fulfill these requirements. Adding oxygen vacancies to PM-K2Ta2O6 also makes it easier for localized energy levels to develop inside the bandgap, which improves light absorption and maximizes surface active sites. In comparison to nonporous K2Ta2O6, PM-K2Ta2O6 exhibits a broad light absorption band, rapid carrier transfer rates, prolonged photogenerated carrier lifetimes, high surface area, and abundant active sites, thus enabling stable photocatalytic hydrogen production from pure water. During surface photochemical reactions, the photogenerated electrons and holes in PM-K2Ta2O6 are more readily trapped and subsequently participate in pure water splitting. The H2 produced by PM-K2Ta2O6 is 1285.91 μmol g-1 in the 5 h H2 production test. Herein, we propose a strategy for developing periodic macropore catalysts capable of efficiently decomposing pure water to produce H2 without necessitating cocatalysts.
期刊介绍:
Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.