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

Li, Kun and Hogan, Nathaniel J. and Kale, Matthew and Halas, Naomi J. and Nordlander, Peter and Christopher, Phillip (2017) Balancing near-field enhancement, absorption, and scattering for effective antenna-reactor plasmonic photocatalysis. Nano Letters, 17 (6). pp. 3710-3717. ISSN 1530-6984.

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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.

Item Type:Article
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URLURL TypeDescription Information
Li, Kun0000-0001-9399-9498
Halas, Naomi J.0000-0002-8461-8494
Nordlander, Peter0000-0002-1633-2937
Christopher, Phillip0000-0002-4898-5510
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.
Funding AgencyGrant Number
Air Force Office of Scientific Research (AFOSR)FA9550-15-10022
University of California, RiversideUNSPECIFIED
Army Research Office (ARO)W911NF-15-1-0533
Robert A. Welch FoundationC-1220
Robert A. Welch FoundationC-1222
Subject Keywords:Localized surface plasmons, electromagnetic field enhancement, antenna−reactor, photocatalysis, size dependence, light-limited
Issue or Number:6
Record Number:CaltechAUTHORS:20170509-082246071
Persistent URL:
Official Citation:Balancing Near-Field Enhancement, Absorption, and Scattering for Effective Antenna–Reactor Plasmonic Photocatalysis Kun Li, Nathaniel J. Hogan, Matthew J. Kale, Naomi J. Halas, Peter Nordlander, and Phillip Christopher Nano Letters 2017 17 (6), 3710-3717 DOI: 10.1021/acs.nanolett.7b00992
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:77288
Deposited By: Tony Diaz
Deposited On:12 May 2017 20:00
Last Modified:03 Oct 2019 17:55

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