Welcome to the new version of CaltechAUTHORS. Login is currently restricted to library staff. If you notice any issues, please email coda@library.caltech.edu
Published June 14, 2017 | Supplemental Material
Journal Article Open

Balancing near-field enhancement, absorption, and scattering for effective antenna-reactor plasmonic photocatalysis

Abstract

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 photocatalysis, 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@SiO_2/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 catalytically active 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.

Additional Information

© 2017 American Chemical Society. Received: March 8, 2017; Revised: April 30, 2017; Published: May 8, 2017. P.C., N.J.H., and P.N. acknowledge funding from the Air Force Office of Scientific Research MURI Grant FA9550-15-10022. Partial funding for this work was also provided by the University of California, Riverside, Center for Catalysis (P.C.), Army Research Office grant W911NF-15-1-0533 (P.C.), and the Welch Foundation grants C-1220 (N.J.H.) and C-1222 (P.N.). TEM was carried out at UCR Central Facility for Advanced Microscopy and Microanalysis (CFAMM). The authors declare no competing financial interest.

Attached Files

Supplemental Material - nl7b00992_si_001.pdf

Files

nl7b00992_si_001.pdf
Files (4.2 MB)
Name Size Download all
md5:92c8e5fa030c38a7c84adb30ef995997
4.2 MB Preview Download

Additional details

Created:
August 19, 2023
Modified:
October 25, 2023