Jun Xu , Ying Luo , Qiaoqi Guo , Wenzheng Sun , Shanshan Chen , Zheng Wang , Hong He
{"title":"掺镁 SrTaO2N 作为可见光驱动的 H2 演变光催化剂,用于加速 Z 型整体水分离","authors":"Jun Xu , Ying Luo , Qiaoqi Guo , Wenzheng Sun , Shanshan Chen , Zheng Wang , Hong He","doi":"10.1016/S1872-2067(24)60082-3","DOIUrl":null,"url":null,"abstract":"<div><div>Perovskite SrTaO<sub>2</sub>N is one of the most promising narrow-bandgap photocatalysts for Z-scheme overall water splitting. However, the formation of defect states during thermal nitridation severely hinders the separation of charges, resulting in poor photocatalytic activity. In the present study, we successfully synthesize SrTaO<sub>2</sub>N photocatalyst with low density of defect states, uniform morphology and particle size by flux-assisted one-pot nitridation combined with Mg doping. Some important parameters, such as the size of unit cell, the content of nitrogen, and microstructure, prove the successful doping of Mg. The defect-related carrier recombination has been significantly reduced by Mg doping, which effectively promotes the charge separation. Moreover, Mg doping induces a change of the band edge, which makes proton reduction have a stronger driving force. After modifying with the core/shell-structured Pt/Cr<sub>2</sub>O<sub>3</sub> cocatalyst, the H<sub>2</sub> evolution activity of the optimized SrTaO<sub>2</sub>N:Mg is 10 times that of the undoped SrTaO<sub>2</sub>N, with an impressive apparent quantum yield of 1.51% at 420 nm. By coupling with Au-FeCoO<sub><em>x</em></sub> modified BiVO<sub>4</sub> as an O<sub>2</sub>-evolution photocatalyst and [Fe(CN)<sub>6</sub>]<sup>3−</sup>/[Fe(CN)<sub>6</sub>]<sup>4−</sup> as the redox couple, a redox-based Z-scheme overall water splitting system is successfully constructed with an apparent quantum yield of 1.36% at 420 nm. This work provides an alternative way to prepare oxynitride semiconductors with reduced defects to promote the conversion of solar energy.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"65 ","pages":"Pages 70-78"},"PeriodicalIF":15.7000,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Mg-doped SrTaO2N as a visible-light-driven H2-evolution photocatalyst for accelerated Z-scheme overall water splitting\",\"authors\":\"Jun Xu , Ying Luo , Qiaoqi Guo , Wenzheng Sun , Shanshan Chen , Zheng Wang , Hong He\",\"doi\":\"10.1016/S1872-2067(24)60082-3\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Perovskite SrTaO<sub>2</sub>N is one of the most promising narrow-bandgap photocatalysts for Z-scheme overall water splitting. However, the formation of defect states during thermal nitridation severely hinders the separation of charges, resulting in poor photocatalytic activity. In the present study, we successfully synthesize SrTaO<sub>2</sub>N photocatalyst with low density of defect states, uniform morphology and particle size by flux-assisted one-pot nitridation combined with Mg doping. Some important parameters, such as the size of unit cell, the content of nitrogen, and microstructure, prove the successful doping of Mg. The defect-related carrier recombination has been significantly reduced by Mg doping, which effectively promotes the charge separation. Moreover, Mg doping induces a change of the band edge, which makes proton reduction have a stronger driving force. After modifying with the core/shell-structured Pt/Cr<sub>2</sub>O<sub>3</sub> cocatalyst, the H<sub>2</sub> evolution activity of the optimized SrTaO<sub>2</sub>N:Mg is 10 times that of the undoped SrTaO<sub>2</sub>N, with an impressive apparent quantum yield of 1.51% at 420 nm. By coupling with Au-FeCoO<sub><em>x</em></sub> modified BiVO<sub>4</sub> as an O<sub>2</sub>-evolution photocatalyst and [Fe(CN)<sub>6</sub>]<sup>3−</sup>/[Fe(CN)<sub>6</sub>]<sup>4−</sup> as the redox couple, a redox-based Z-scheme overall water splitting system is successfully constructed with an apparent quantum yield of 1.36% at 420 nm. This work provides an alternative way to prepare oxynitride semiconductors with reduced defects to promote the conversion of solar energy.</div></div>\",\"PeriodicalId\":9832,\"journal\":{\"name\":\"Chinese Journal of Catalysis\",\"volume\":\"65 \",\"pages\":\"Pages 70-78\"},\"PeriodicalIF\":15.7000,\"publicationDate\":\"2024-10-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chinese Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1872206724600823\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chinese Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1872206724600823","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
Mg-doped SrTaO2N as a visible-light-driven H2-evolution photocatalyst for accelerated Z-scheme overall water splitting
Perovskite SrTaO2N is one of the most promising narrow-bandgap photocatalysts for Z-scheme overall water splitting. However, the formation of defect states during thermal nitridation severely hinders the separation of charges, resulting in poor photocatalytic activity. In the present study, we successfully synthesize SrTaO2N photocatalyst with low density of defect states, uniform morphology and particle size by flux-assisted one-pot nitridation combined with Mg doping. Some important parameters, such as the size of unit cell, the content of nitrogen, and microstructure, prove the successful doping of Mg. The defect-related carrier recombination has been significantly reduced by Mg doping, which effectively promotes the charge separation. Moreover, Mg doping induces a change of the band edge, which makes proton reduction have a stronger driving force. After modifying with the core/shell-structured Pt/Cr2O3 cocatalyst, the H2 evolution activity of the optimized SrTaO2N:Mg is 10 times that of the undoped SrTaO2N, with an impressive apparent quantum yield of 1.51% at 420 nm. By coupling with Au-FeCoOx modified BiVO4 as an O2-evolution photocatalyst and [Fe(CN)6]3−/[Fe(CN)6]4− as the redox couple, a redox-based Z-scheme overall water splitting system is successfully constructed with an apparent quantum yield of 1.36% at 420 nm. This work provides an alternative way to prepare oxynitride semiconductors with reduced defects to promote the conversion of solar energy.
期刊介绍:
The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.