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Dunkelberger, Adam D.
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article
Plasmonic Aerogels as a Three-Dimensional Nanoscale Platform for Solar Fuel Photocatalysis
Abstract
We use plasmonic Au–TiO2 aerogels as a platform in which to marry synthetically thickened particle–particle junctions in TiO2 aerogel networks to Au∥TiO2 interfaces and then investigate their cooperative influence on photocatalytic hydrogen (H2) generation under both broadband (i.e., UV + visible light) and visible-only excitation. In doing so, we elucidate the dual functions that incorporated Au can play as a water reduction cocatalyst and as a plasmonic sensitizer. We also photodeposit non-plasmonic Pt cocatalyst nanoparticles into our composite aerogels in order to leverage the catalytic water-reducing abilities of Pt. This Au–TiO2/Pt arrangement in three dimensions effectively utilizes conduction−band electrons injected into the TiO2 aerogel network upon exciting the Au SPR at the Au∥TiO2 interface. The extensive nanostructured high surface-area oxide network in the aerogel provides a matrix that spatially separates yet electrochemically connects plasmonic nanoparticle sensitizers and metal nanopartic...