Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 15, Issue 22, Pages 8722-8731Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c3cp44519d
Keywords
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Funding
- National Basic Research Program of China (973 program) [2013CB632401]
- National Science foundation of China [11174180]
- Fund for Doctoral Program of National Education [20120131110066]
- Natural Science Foundation of Shandong Province [ZR2011AM009]
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It is fundamental to uncover the real adsorption properties of Ag clusters on an AgCl surface and the energy transfer mechanisms at the interface to understand the highly active photocatalytic performance and the stability of the plasmonic photocatalyst Ag@AgCl. Based on density functional theory calculations we provide valuable insights into the binding nature of Ag clusters on AgCl surface, where the binding between Ag atoms in the cluster and on the surface plays a decisive role in determining the most stable adsorption configurations. Our results demonstrate that there is energy transfer from the plasmonic metals to substrate. The hot holes excited by the decay of surface plasmon resonance on the metals can diffuse into the Cl ions in the outermost two layers of the surface producing highly oxidative Cl atoms. The dipole-dipole interaction between the plasmonic metal clusters and substrate Cl ions can also generate electron-hole pairs in the surface layers. It is deduced that the positively charged nature of adsorbed clusters acting as electron trapping centers and reduction sites plays a crucial role in keeping the stability of the Ag@AgCl system during the photocatalytic process. Finally, the validity of the cluster adsorption model for energy transfer is verified with respect to the nucleation and aggregation process of Ag atoms on the AgCl surface and a detailed description of the formation and evolution of Ag nanoparticles on an AgCl surface is provided. The present study may be helpful for understanding and designing this novel plasmonic photocatalyst and can be useful for investigating other relevant photocatalysts as well.
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