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Type-I CdS/ZnS Core/Shell Quantum Dot-Gold Heterostructural Nanocrystals for Enhanced Photocatalytic Hydrogen Generation.
Jin, Na; Sun, Yonglei; Shi, Wenwu; Wang, Ping; Nagaoka, Yasutaka; Cai, Tong; Wu, Rongzhen; Dube, Lacie; Nyiera, Hawi N; Liu, Yuzi; Mani, Tomoyasu; Wang, Xinzhong; Zhao, Jing; Chen, Ou.
Afiliación
  • Jin N; Department of Chemistry, Brown University, Providence, Rhode Island 02912, United States.
  • Sun Y; Institute of Materials Science, University of Connecticut, Storrs Mansfield, Connecticut 06269, United States.
  • Shi W; School of Physical Science and Technology, Southwest University, Chongqing 400715, People's Republic of China.
  • Wang P; Institute of Information Technology, Shenzhen Institute of Information Technology, Shenzhen 518172, China.
  • Nagaoka Y; Key Laboratory of Preparation and Applications of Environmental Friendly Materials of the Ministry of Education, College of Chemistry, Jilin Normal University, Changchun 130103, China.
  • Cai T; Department of Chemistry, Brown University, Providence, Rhode Island 02912, United States.
  • Wu R; Department of Chemistry, Brown University, Providence, Rhode Island 02912, United States.
  • Dube L; Department of Chemistry, Brown University, Providence, Rhode Island 02912, United States.
  • Nyiera HN; Department of Chemistry, Brown University, Providence, Rhode Island 02912, United States.
  • Liu Y; Department of Chemistry, University of Connecticut, Storrs Mansfield, Connecticut 06269, United States.
  • Mani T; Center for Nanoscale Materials, Argonne National Laboratory, Argonne, Illinois 60439, United States.
  • Wang X; Department of Chemistry, University of Connecticut, Storrs Mansfield, Connecticut 06269, United States.
  • Zhao J; Institute of Information Technology, Shenzhen Institute of Information Technology, Shenzhen 518172, China.
  • Chen O; Institute of Materials Science, University of Connecticut, Storrs Mansfield, Connecticut 06269, United States.
J Am Chem Soc ; 145(40): 21886-21896, 2023 Oct 11.
Article en En | MEDLINE | ID: mdl-37768875
Developing Type-I core/shell quantum dots is of great importance toward fabricating stable and sustainable photocatalysts. However, the application of Type-I systems has been limited due to the strongly confined photogenerated charges by the energy barrier originating from the wide-bandgap shell material. In this project, we found that through the decoration of Au satellite-type domains on the surface of Type-I CdS/ZnS core/shell quantum dots, such an energy barrier can be effectively overcome and an over 400-fold enhancement of photocatalytic H2 evolution rate was achieved compared to bare CdS/ZnS quantum dots. Transient absorption spectroscopic studies indicated that the charges can be effectively extracted and subsequently transferred to surrounding molecular substrates in a subpicosecond time scale in such hybrid nanocrystals. Based on density functional theory calculations, the ultrafast charge separation rates were ascribed to the formation of intermediate Au2S layer at the semiconductor-metal interface, which can successfully offset the energy confinement introduced by the ZnS shell. Our findings not only provide insightful understandings on charge carrier dynamics in semiconductor-metal heterostructural materials but also pave the way for the future design of quantum dot-based hybrid photocatalytic systems.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos
Texto completo
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos