Jacqueline Hidalgo-Jiménez, Taner Akbay, Xavier Sauvage, Lambert van Eijck, Motonori Watanabe, Jacques Huot, Tatsumi Ishihara, Kaveh Edalati
{"title":"混合 d0 和 d10 电子构型促进了高熵氧化物在二氧化碳转化和水分离方面的光催化活性","authors":"Jacqueline Hidalgo-Jiménez, Taner Akbay, Xavier Sauvage, Lambert van Eijck, Motonori Watanabe, Jacques Huot, Tatsumi Ishihara, Kaveh Edalati","doi":"10.1039/d4ta04689g","DOIUrl":null,"url":null,"abstract":"Photocatalysis offers a sustainable solution for essential reactions such as CO2 conversion and water splitting, but constraints in catalyst properties like bandgap and active site availability often limit its efficiency. High-entropy oxides (HEOs), which incorporate five or more different cations, present significant potential for this application due to their elemental diversity. This study explores active HEO development for photocatalytic applications by integrating cations with d0 and d10 electronic configurations. A single-phase HEO with a monoclinic structure was successfully synthesized, comprising elements with d0 (titanium, zirconium, niobium, and tantalum) and d10 (zinc) electronic configurations. Comprehensive analyses of its microstructure, chemical composition, optical properties, and photocatalytic activity were conducted. The resulting TiZrNbTaZnO10 exhibited superior UV and visible light absorption, a low bandgap of 2.5 eV, minimal radiative electron-hole recombination, and high stability under photocatalytic conditions. Remarkably, TiZrNbTaZnO10 outperformed TiZrHfNbTaO11 photocatalyst which contains solely d0 electronic configurations. This enhanced performance is attributed to the mixed electronic configurations fostering heterogeneous chemical environments, which facilitate efficient charge carrier separation and transfer.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":10.7000,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Hybrid d0 and d10 electronic configurations promote photocatalytic activity of high-entropy oxides for CO2 conversion and water splitting\",\"authors\":\"Jacqueline Hidalgo-Jiménez, Taner Akbay, Xavier Sauvage, Lambert van Eijck, Motonori Watanabe, Jacques Huot, Tatsumi Ishihara, Kaveh Edalati\",\"doi\":\"10.1039/d4ta04689g\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Photocatalysis offers a sustainable solution for essential reactions such as CO2 conversion and water splitting, but constraints in catalyst properties like bandgap and active site availability often limit its efficiency. High-entropy oxides (HEOs), which incorporate five or more different cations, present significant potential for this application due to their elemental diversity. This study explores active HEO development for photocatalytic applications by integrating cations with d0 and d10 electronic configurations. A single-phase HEO with a monoclinic structure was successfully synthesized, comprising elements with d0 (titanium, zirconium, niobium, and tantalum) and d10 (zinc) electronic configurations. Comprehensive analyses of its microstructure, chemical composition, optical properties, and photocatalytic activity were conducted. The resulting TiZrNbTaZnO10 exhibited superior UV and visible light absorption, a low bandgap of 2.5 eV, minimal radiative electron-hole recombination, and high stability under photocatalytic conditions. Remarkably, TiZrNbTaZnO10 outperformed TiZrHfNbTaO11 photocatalyst which contains solely d0 electronic configurations. This enhanced performance is attributed to the mixed electronic configurations fostering heterogeneous chemical environments, which facilitate efficient charge carrier separation and transfer.\",\"PeriodicalId\":82,\"journal\":{\"name\":\"Journal of Materials Chemistry A\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":10.7000,\"publicationDate\":\"2024-10-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Materials Chemistry A\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1039/d4ta04689g\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Chemistry A","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d4ta04689g","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Hybrid d0 and d10 electronic configurations promote photocatalytic activity of high-entropy oxides for CO2 conversion and water splitting
Photocatalysis offers a sustainable solution for essential reactions such as CO2 conversion and water splitting, but constraints in catalyst properties like bandgap and active site availability often limit its efficiency. High-entropy oxides (HEOs), which incorporate five or more different cations, present significant potential for this application due to their elemental diversity. This study explores active HEO development for photocatalytic applications by integrating cations with d0 and d10 electronic configurations. A single-phase HEO with a monoclinic structure was successfully synthesized, comprising elements with d0 (titanium, zirconium, niobium, and tantalum) and d10 (zinc) electronic configurations. Comprehensive analyses of its microstructure, chemical composition, optical properties, and photocatalytic activity were conducted. The resulting TiZrNbTaZnO10 exhibited superior UV and visible light absorption, a low bandgap of 2.5 eV, minimal radiative electron-hole recombination, and high stability under photocatalytic conditions. Remarkably, TiZrNbTaZnO10 outperformed TiZrHfNbTaO11 photocatalyst which contains solely d0 electronic configurations. This enhanced performance is attributed to the mixed electronic configurations fostering heterogeneous chemical environments, which facilitate efficient charge carrier separation and transfer.
期刊介绍:
The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.