Fuel electrooxidation reactions catalyzed by noble metal electrodes are often complex multistep processes, plagued by incomplete reaction to partially oxidized byproducts and catalyst poisoning. Electrodes featuring noble metal nanoparticles with surface plasmon resonances present the opportunity to combine catalytic activity with light-harvesting capability as a means to enhance catalytic performance.<br/><br/>In this work, photoelectrodes composed of large area Pd, Au, and Au-Pd alloy nanoparticle films with strong surface plasmon resonances in the visible spectrum were fabricated and evaluated in terms of photoenhancement of the electrooxidation of small molecules and other reactions. In addition to the pure metal and alloy films, where the catalyst and light absorber are one and the same, bimetallic Au-Pd photoelectrodes were also produced so as to benchmark the performance of other design strategies; for example, a chromophore-catalyst configuration of plasmonic Au with non-plasmonic Pd. Photoenhancement was evaluated by voltammetry, spectroelectrochemistry, and gas-chromatography, and rationalized in terms of mechanistic insight gleaned from experiments and literature on the dark chemistry.

Plasmonic Pd, Au, and Au-Pd nanoparticle photoelectrocatalysts for small molecule oxidation

2019 Fall National Meeting

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