4.8 Article

Engineering the Metal/Dielectric Interface to Unlock the Potential of Scattered Light for Boosted Photoredox Catalysis

Journal

ACS NANO
Volume 17, Issue 16, Pages 15666-15677

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.3c02766

Keywords

absorption enhancement; scattered light; dualmetal; dielectric interfaces; photocatalysis; palladiumnanoparticles

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In this study, dual metal/high-refractive-index dielectric interfaces were constructed within the SiO2 core@TiO2 shell-Pd satellite@TiO2 shell, effectively enhancing the scattering efficiency and electric field confinement. This strategy improved the absorption of Pd towards scattered light and the separation of interfacial charge carriers, leading to enhanced photoactivity. The engineering of metal/dielectric interfaces presents a promising avenue to upgrade the optical response of metals and the photocatalytic performance.
Therecycling of scattered light by metals has been emergingasa promising light-manipulation-capture strategy, but how to bringits potential into better play remains to be explored. Herein, wepresent that constructing dual metal/high-refractive-index dielectricinterfaces within the SiO2 core@TiO2 shell-Pdsatellite@TiO2 shell effectively strengthens both the scatteringefficiency of the dielectric SiO2 support and electricfield confinement. Consequently, the absorption of Pd toward near-fieldscattered light and the interfacial charge carrier separation areboth enhanced. The synergy of these effects leads to boosted photoactivitytoward the aerobic oxidation of cyclohexanol to cyclohexanone andthe anaerobic reduction of proton for hydrogen evolution under visible-lightirradiation as compared to the counterparts with a single metal/dielectricinterface and dual metal/dielectric interfaces consisting of low-refractive-indexdielectric component. Notably, the similar enhancements in both opticalabsorption and photoactivity can be achieved through the present dualmetal/high-refractive-index dielectric interfaces engineering strategyfor other metals, such as Pt nanoparticles. This work presents aninstructive avenue to upgrade the optical response of metals and thusthe photocatalytic performance by engineering metal/dielectric interfaces.

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