Volume 214, 2019

Plasmonic photocatalysis applied to solar fuels

Abstract

The induction of chemical processes by plasmonic systems is a rapidly growing field with potentially many strategic applications. One of them is the transformation of solar energy into chemical fuel by the association of plasmonic metal nanoparticles (M NPs) and a semi-conductor (SC). When the localized surface plasmon resonance (LSPR) and the SC absorption do not match, one limitation of these systems is the efficiency of hot electron transfer from M NPs to SC through the Schottky barrier formed at the M NP/SC interfaces. Here we show that high surface area 1 wt% Au/TiO2-UV100, prepared by adsorption of a NaBH4-protected 3 nm gold sol, readily catalyzes the photoreduction of carbon dioxide with water into methane under both solar and visible-only irradiation with a CH4vs. H2 selectivity of 63%. Tuning Au NP size and titania surface area, in particular via thermal treatments, highlights the key role of the metal dispersion and of the accessible Au–TiO2 perimeter interface on the direct SC-based solar process. The impact of Au NP density in turn provides evidence for the dual role of gold as co-catalyst and recombination sites for charge carriers. It is shown that the plasmon-induced process contributes up to 20% of the solar activity. The plasmon-based contribution is enhanced by a large Au NP size and a high degree of crystallinity of the SC support. By minimizing surface hydroxylation while retaining a relatively high surface area of 120 m2 g−1, pre-calcining TiO2-UV100 at 450 °C leads to an optimum monometallic system in terms of activity and selectivity under both solar and visible irradiation. A state-of-the-art methane selectivity of 100% is achieved in the hot electron process.

Graphical abstract: Plasmonic photocatalysis applied to solar fuels

Associated articles

Article information

Article type
Paper
Submitted
02 Oct 2018
Accepted
16 Nov 2018
First published
16 Nov 2018

Faraday Discuss., 2019,214, 417-439

Plasmonic photocatalysis applied to solar fuels

S. Bardey, A. Bonduelle-Skrzypczak, A. Fécant, Z. Cui, C. Colbeau-Justin, V. Caps and V. Keller, Faraday Discuss., 2019, 214, 417 DOI: 10.1039/C8FD00144H

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