期刊
NANO LETTERS
卷 17, 期 6, 页码 3710-3717出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.7b00992
关键词
Localized surface plasmons; electromagnetic field enhancement; antenna reactor; photocatalysis; size dependence; light-limited
类别
资金
- Air Force Office of Scientific Research MURI Grant [FA9550-15-10022]
- University of California, Riverside, Center for Catalysis
- Army Research Office [W911NF-15-1-0533]
- Welch Foundation [C-1220, C-1222]
Efficient photocatalysis requires multifunctional materials that absorb photons and generate energetic charge carriers at catalytic active sites to facilitate a desired chemical reaction. Antenna reactor complexes are an emerging multifunctional photocatalytic structure where the strong, localized near field of the plasmonic metal nanoparticle (e.g., Ag) is coupled to the catalytic properties of the nonplasmonic metal nanoparticle (e.g., Pt) to enable chemical transformations. With an eye toward sustainable solar driven photo catalysis, we investigate how the structure of antenna reactor complexes governs their photocatalytic activity in the light-limited regime, where all photons need to be effectively utilized. By synthesizing core@shell/satellite (Ag@SiO2/Pt) antenna reactor complexes with varying Ag nanoparticle diameters and performing photocatalytic CO oxidation, we observed plasmon-enhanced photocatalysis only for antenna reactor complexes. with antenna components of intermediate sizes (25 and 50 nm). Optimal photocatalytic performance was shown to be determined by a balance between maximized local field enhancements at the catalyticallyactive Pt surface,-minimized collective scattering of photons out of the catalyst bed by the complexes, and minimal light;absorption in the Ag nanoparticle antenna. These results elucidate the critical aspects of local field enhancement, light scattering, and absorption in plasmonic photocatalyst design, especially under light-limited illumination conditions.
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