Elucidating the Roles of Local and Nonlocal Rate Enhancement Mechanisms in Plasmonic Catalysis

Elias, Rachel C.; Linic, Suljo

doi:10.1021/jacs.2c08561

Elucidating the Roles of Local and Nonlocal Rate Enhancement Mechanisms in Plasmonic Catalysis

Journal Article · Mon Oct 24 00:00:00 EDT 2022 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.2c08561· OSTI ID:2338166

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Univ. of Michigan, Ann Arbor, MI (United States); University of Michigan - Ann Arbor, MI (United States). Department of Chemical Engineering
Univ. of Michigan, Ann Arbor, MI (United States)

Plasmonic metal nanoparticles (e.g., Ag, Au, and Cu) constitute a class of materials that interact with light via the excitation of localized surface plasmon resonance (LSPR). Numerous studies have reported substantial enhancements in the rates of chemical reactions on illuminated plasmonic nanoparticle catalysts compared to corresponding systems in the absence of illumination. There are two mechanisms that have been proposed to explain the LSPR-induced chemical reactivity. One mechanism assumes a local plasmon-induced hot charge-carrier-mediated activation of the reactants, while the other assumes an LSPR-induced equilibrium heating of the catalyst, which leads to energy transfer to and chemical reaction of the adsorbed reactants. Here, in this contribution, we developed a setup amenable to accurate in situ catalyst temperature and kinetic reaction rate measurements. We employed this setup to study the LSPR-induced rate enhancement in a case study of the CO oxidation reaction on plasmonic, monometallic Ag nanoparticle catalysts supported on α-Al₂O₃. We explored various Ag loadings and clustering levels. Our data show that the equilibrium heating of the catalyst cannot fully explain the illumination-induced plasmonic rate enhancements. This is the case even for high loading and clustering of Ag nanoparticles, where the equilibrium heating significantly increases. Based on the analysis, we propose that local effects, related to the plasmon-induced activation of adsorbates (reactants) via electronic excitation of the reactant or photothermal heating of the reactants that is highly localized to the individual nanoparticles, play a critical role in driving LSPR-induced chemical reactions.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Michigan, Ann Arbor, MI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0021008; SC0021362

OSTI ID:: 2338166

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 43 Vol. 144; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Elucidating the Roles of Local and Nonlocal Rate Enhancement Mechanisms in Plasmonic Catalysis

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