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Harvesting resonantly-trapped light for small molecule oxidation reactions at the Au/α-Fe2O3 interface

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Abstract

Plasmonic metal nanoparticles (NPs) extend the overall light absorption of semiconductor materials. However, it is not well understood how coupling metal NPs to semiconductors alters the photo-electrochemical activity of small molecule oxidation (SMO) reactions. Different photo-anode electrodes comprised of Au NPs and α-Fe2O3 are designed to elucidate how the coupling plays not only a role in the water oxidation reaction (WO) but also performs for different SMO reactions. In this regard, Au NPs are inserted at specific regions within and/or on α-Fe2O3 layers created with a sequential electron beam evaporation method and multiple annealing treatments. The SMO and WO reactions are probed with broad-spectrum irradiation experiments with an emphasis on light-driven enhancements above and below the α-Fe2O3 band gap. Thin films of α-Fe2O3 supported on a gold back reflective layer resonantly-traps incident light leading to enhanced SMO/WO conversion efficiencies at high overpotential (η) for above band-gap excitations with no SMO activity observed at low η. In contrast, a substantial increase in the light-driven SMO activity is observed at low η, as well as for below band-gap excitations when sufficiently thin α-Fe2O3 films are decorated with Au NPs at the solution-electrode interface. The enhanced photo-catalytic activity is correlated with increased surface oxygen content (hydroxyl groups) at the Au/α-Fe2O3 interface, as well as simulated volume-integrated near-field enhancements over select regions of the Au/α-Fe2O3 interface providing an important platform for future SMO/WO photo-electrocatalyst development.

Graphical abstract: Harvesting resonantly-trapped light for small molecule oxidation reactions at the Au/α-Fe2O3 interface

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Publication details

The article was received on 14 Feb 2018, accepted on 30 Mar 2018 and first published on 02 Apr 2018


Article type: Paper
DOI: 10.1039/C8NR01330F
Citation: Nanoscale, 2018, Advance Article
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    Harvesting resonantly-trapped light for small molecule oxidation reactions at the Au/α-Fe2O3 interface

    J. P. McClure, K. N. Grew, D. R. Baker, E. Gobrogge, N. Das and D. Chu, Nanoscale, 2018, Advance Article , DOI: 10.1039/C8NR01330F

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