{"title":"过渡金属卤化物上的单原子电子泵促进光催化作用","authors":"Jia-Qi Chen, Yu-Shan Cai, Xian Yan, Qiao-Ling Mo, Jiao-Nan Yuan, Chu-Hao Liu, Yue Wu, Fang-Xing Xiao","doi":"10.1002/smll.202405228","DOIUrl":null,"url":null,"abstract":"Cocatalyst is of paramount significance to provide fruitful active sites for suppressing the spatial charge recombination toward boosted photocatalysis. Up to date, exploration of robust and stable cocatalysts is remained challenging. Inspired by the intrinsic merits of single-atom catalysts (SACs), such as distinctive electronic structure and high atomic utilization efficiency, single-atom/transition metal chalcogenides (TMCs) is utilized as a model to synthesize CdS-Pd single-atom catalyst (CdS-PdSA) heterostructures. This demonstrates the precise anchoring of isolated metal single-atom catalysts (SACs) onto TMCs through a simple yet effective wet-chemical strategy. The resulting heterostructures exhibit significantly enhanced and stable photocatalytic activity for selective anaerobic organic transformations and hydrogen production under visible light. This enhancement is primarily inferred due to the role of Pd SACs as electron pumps, which directionally trap the electrons photoexcited over CdS, accelerating the spatial charge separation and prolonging the carrier lifespan. The charge transport route and photocatalytic mechanism are elucidated. This work underscores the potential of SACs as cocatalysts in heterogeneous photocatalysis, offering valuable insights for the rational design of atomic-level cocatalysts for solar-to-chemical energy conversion and beyond.","PeriodicalId":228,"journal":{"name":"Small","volume":null,"pages":null},"PeriodicalIF":13.0000,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Single-Atom Electron Pumps Over Transition Metal Chalcogenides Boosting Photocatalysis\",\"authors\":\"Jia-Qi Chen, Yu-Shan Cai, Xian Yan, Qiao-Ling Mo, Jiao-Nan Yuan, Chu-Hao Liu, Yue Wu, Fang-Xing Xiao\",\"doi\":\"10.1002/smll.202405228\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Cocatalyst is of paramount significance to provide fruitful active sites for suppressing the spatial charge recombination toward boosted photocatalysis. Up to date, exploration of robust and stable cocatalysts is remained challenging. Inspired by the intrinsic merits of single-atom catalysts (SACs), such as distinctive electronic structure and high atomic utilization efficiency, single-atom/transition metal chalcogenides (TMCs) is utilized as a model to synthesize CdS-Pd single-atom catalyst (CdS-PdSA) heterostructures. This demonstrates the precise anchoring of isolated metal single-atom catalysts (SACs) onto TMCs through a simple yet effective wet-chemical strategy. The resulting heterostructures exhibit significantly enhanced and stable photocatalytic activity for selective anaerobic organic transformations and hydrogen production under visible light. This enhancement is primarily inferred due to the role of Pd SACs as electron pumps, which directionally trap the electrons photoexcited over CdS, accelerating the spatial charge separation and prolonging the carrier lifespan. The charge transport route and photocatalytic mechanism are elucidated. This work underscores the potential of SACs as cocatalysts in heterogeneous photocatalysis, offering valuable insights for the rational design of atomic-level cocatalysts for solar-to-chemical energy conversion and beyond.\",\"PeriodicalId\":228,\"journal\":{\"name\":\"Small\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":13.0000,\"publicationDate\":\"2024-10-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Small\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1002/smll.202405228\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Small","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/smll.202405228","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Single-Atom Electron Pumps Over Transition Metal Chalcogenides Boosting Photocatalysis
Cocatalyst is of paramount significance to provide fruitful active sites for suppressing the spatial charge recombination toward boosted photocatalysis. Up to date, exploration of robust and stable cocatalysts is remained challenging. Inspired by the intrinsic merits of single-atom catalysts (SACs), such as distinctive electronic structure and high atomic utilization efficiency, single-atom/transition metal chalcogenides (TMCs) is utilized as a model to synthesize CdS-Pd single-atom catalyst (CdS-PdSA) heterostructures. This demonstrates the precise anchoring of isolated metal single-atom catalysts (SACs) onto TMCs through a simple yet effective wet-chemical strategy. The resulting heterostructures exhibit significantly enhanced and stable photocatalytic activity for selective anaerobic organic transformations and hydrogen production under visible light. This enhancement is primarily inferred due to the role of Pd SACs as electron pumps, which directionally trap the electrons photoexcited over CdS, accelerating the spatial charge separation and prolonging the carrier lifespan. The charge transport route and photocatalytic mechanism are elucidated. This work underscores the potential of SACs as cocatalysts in heterogeneous photocatalysis, offering valuable insights for the rational design of atomic-level cocatalysts for solar-to-chemical energy conversion and beyond.
期刊介绍:
Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments.
With a remarkable 2022 Journal Impact Factor of 13.3 (Journal Citation Reports from Clarivate Analytics, 2023), Small remains among the top multidisciplinary journals, covering a wide range of topics at the interface of materials science, chemistry, physics, engineering, medicine, and biology.
Small's readership includes biochemists, biologists, biomedical scientists, chemists, engineers, information technologists, materials scientists, physicists, and theoreticians alike.