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Faraday Discuss. 2019 May 23;214:387-397. doi: 10.1039/c8fd00150b.

Optimizing hot carrier effects in Pt-decorated plasmonic heterostructures.

Faraday discussions

Jorge U Salmón-Gamboa, Mayela Romero-Gómez, Diane J Roth, Matthew J Barber, Pan Wang, Simon M Fairclough, Mazhar E Nasir, Alexey V Krasavin, Wayne Dickson, Anatoly V Zayats

Affiliations

  1. Department of Physics and London Centre for Nanotechnology, King's College London, Strand, London WC2R 2LS, UK. [email protected].

PMID: 30801594 DOI: 10.1039/c8fd00150b

Abstract

Hot carrier generation by light in various semiconductors and metallic nanostructures is important for many photocatalytic and photochemical processes, including water and hydrogen splitting. Here, we report on investigations of hot electron generation and extraction from Pt decorated SiO2-Au nanoparticles using the degradation of methylene blue dye as a test-bed. Enhanced catalytic activity was found with an increase of Pt loading on the surface of the heterostructures. The small size of the Au nanoparticles (∼12 nm) decorating the silica nanoparticles reduces hot electron collisions and related thermalization processes, since charge carriers have short paths to the surface where reactions take place and where Pt is situated. The heterostructures exhibit a broad plasmonic resonance in the visible wavelength range from 500 to 700 nm and hot carrier generation predominately takes place under resonant excitation. Electron-microscopy characterization and numerical modelling have allowed the optimization of Pt coverage for hot-electron transfer, consisting of a thin Pt shell covering the Au nanoparticle with Pt nanoparticles additionally placed on top. This geometry provides an increased number of active sites for methylene blue degradation and promotes separation of charge carriers generated by plasmonic excitations in Au. Such SiO2-Au-Pt nanoparticles are attractive for hot-electron production due to the tunability of their plasmonic resonance and enhanced catalytic activity.

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