{"title":"通过锚定 Pt 位点的 2D/2D 异质结构催化剂促进可见光驱动的氢气进化:Cd-TCPP(Pt)@CdS","authors":"Guo-Wei Guan, Yi-Tao Li, Li-Ping Zhang, Su-Tao Zheng, Si-Chao Liu, Hao-Ling Lan, Qing-Yuan Yang","doi":"10.1016/j.gce.2024.03.002","DOIUrl":null,"url":null,"abstract":"<div><div>Solar-powered water splitting is an up-and-coming method for hydrogen production. Still, it faces several challenges, including improving light responsiveness, maximizing utilization of photocatalyst active sites, and effectively utilizing photo-induced carriers to prevent low hydrogen production. In this research, we propose an approach for designing a 2D/2D heterostructure catalyst, the Cd-TCPP(Pt)@CdS, which consists of 2D CdS nanosheets (NSs) and a 2D metal-organic framework (MOF) with Pt active sites (Cd-TCPP(Pt)), aiming to achieve highly efficient visible-light-driven hydrogen evolution. Firstly, CdS NSs exhibit excellent responsiveness to visible light, ensuring robust generation of photo-induced carriers. Secondly, the 2D MOF provides abundant Pt active sites, enhancing electron utilization and reducing the energy barrier for proton reduction. Compared to pure CdS NSs (which demonstrate a hydrogen production activity of 1220 μmol/g/h), the newly designed 2D/2D composite catalyst Cd-TCPP(Pt)@CdS exhibits an activity of 13,434 μmol/g/h, representing an 11-fold increase. Impressively, Cd-TCPP(Pt)@CdS maintains a high activity of 3062 μmol/g/h even under sunlight. Density functional theory (DFT) calculations were employed to investigate the principle of proton reduction. The suitable bandgap of CdS and energy gap of 2D Cd-TCPP(Pt) contribute to their strong interaction and consequently higher efficiency in hydrogen evolution. The Pt-single atom (Pt-SA) also provides sites with low free energy for proton reduction, contributing to improved activity. The photocatalytic performance of Cd-TCPP(Pt)@CdS NSs composites demonstrates a synergistic effect between the 2D inorganic semiconductor and the 2D MOF containing the Pt-site, resulting in enhanced utilization of photo-induced carriers and atoms.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"6 1","pages":"Pages 68-75"},"PeriodicalIF":9.1000,"publicationDate":"2024-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Boosting visible-light-driven hydrogen evolution through Pt site anchored 2D/2D heterostructure catalyst: Cd-TCPP(Pt)@CdS\",\"authors\":\"Guo-Wei Guan, Yi-Tao Li, Li-Ping Zhang, Su-Tao Zheng, Si-Chao Liu, Hao-Ling Lan, Qing-Yuan Yang\",\"doi\":\"10.1016/j.gce.2024.03.002\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Solar-powered water splitting is an up-and-coming method for hydrogen production. Still, it faces several challenges, including improving light responsiveness, maximizing utilization of photocatalyst active sites, and effectively utilizing photo-induced carriers to prevent low hydrogen production. In this research, we propose an approach for designing a 2D/2D heterostructure catalyst, the Cd-TCPP(Pt)@CdS, which consists of 2D CdS nanosheets (NSs) and a 2D metal-organic framework (MOF) with Pt active sites (Cd-TCPP(Pt)), aiming to achieve highly efficient visible-light-driven hydrogen evolution. Firstly, CdS NSs exhibit excellent responsiveness to visible light, ensuring robust generation of photo-induced carriers. Secondly, the 2D MOF provides abundant Pt active sites, enhancing electron utilization and reducing the energy barrier for proton reduction. Compared to pure CdS NSs (which demonstrate a hydrogen production activity of 1220 μmol/g/h), the newly designed 2D/2D composite catalyst Cd-TCPP(Pt)@CdS exhibits an activity of 13,434 μmol/g/h, representing an 11-fold increase. Impressively, Cd-TCPP(Pt)@CdS maintains a high activity of 3062 μmol/g/h even under sunlight. Density functional theory (DFT) calculations were employed to investigate the principle of proton reduction. The suitable bandgap of CdS and energy gap of 2D Cd-TCPP(Pt) contribute to their strong interaction and consequently higher efficiency in hydrogen evolution. The Pt-single atom (Pt-SA) also provides sites with low free energy for proton reduction, contributing to improved activity. The photocatalytic performance of Cd-TCPP(Pt)@CdS NSs composites demonstrates a synergistic effect between the 2D inorganic semiconductor and the 2D MOF containing the Pt-site, resulting in enhanced utilization of photo-induced carriers and atoms.</div></div>\",\"PeriodicalId\":66474,\"journal\":{\"name\":\"Green Chemical Engineering\",\"volume\":\"6 1\",\"pages\":\"Pages 68-75\"},\"PeriodicalIF\":9.1000,\"publicationDate\":\"2024-03-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Green Chemical Engineering\",\"FirstCategoryId\":\"1089\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2666952824000165\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Green Chemical Engineering","FirstCategoryId":"1089","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2666952824000165","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Boosting visible-light-driven hydrogen evolution through Pt site anchored 2D/2D heterostructure catalyst: Cd-TCPP(Pt)@CdS
Solar-powered water splitting is an up-and-coming method for hydrogen production. Still, it faces several challenges, including improving light responsiveness, maximizing utilization of photocatalyst active sites, and effectively utilizing photo-induced carriers to prevent low hydrogen production. In this research, we propose an approach for designing a 2D/2D heterostructure catalyst, the Cd-TCPP(Pt)@CdS, which consists of 2D CdS nanosheets (NSs) and a 2D metal-organic framework (MOF) with Pt active sites (Cd-TCPP(Pt)), aiming to achieve highly efficient visible-light-driven hydrogen evolution. Firstly, CdS NSs exhibit excellent responsiveness to visible light, ensuring robust generation of photo-induced carriers. Secondly, the 2D MOF provides abundant Pt active sites, enhancing electron utilization and reducing the energy barrier for proton reduction. Compared to pure CdS NSs (which demonstrate a hydrogen production activity of 1220 μmol/g/h), the newly designed 2D/2D composite catalyst Cd-TCPP(Pt)@CdS exhibits an activity of 13,434 μmol/g/h, representing an 11-fold increase. Impressively, Cd-TCPP(Pt)@CdS maintains a high activity of 3062 μmol/g/h even under sunlight. Density functional theory (DFT) calculations were employed to investigate the principle of proton reduction. The suitable bandgap of CdS and energy gap of 2D Cd-TCPP(Pt) contribute to their strong interaction and consequently higher efficiency in hydrogen evolution. The Pt-single atom (Pt-SA) also provides sites with low free energy for proton reduction, contributing to improved activity. The photocatalytic performance of Cd-TCPP(Pt)@CdS NSs composites demonstrates a synergistic effect between the 2D inorganic semiconductor and the 2D MOF containing the Pt-site, resulting in enhanced utilization of photo-induced carriers and atoms.