Although the vast majority of fuels and hydrocarbon products are presently derived from petroleum, there is much interest in the development of routes for synthesizing these same products by hydrogenating carbon oxygenates. Electrochemical methods for CO2 reduction are attractive because they operate under conditions of ambient pressure and temperature and have high theoretical efficiencies. However, current catalysts suffer from a combination of low selectivities, high overpotentials, and poor stability. Metals in the form of foils are increasingly well-characterized as electrocatalysts for CO2 reduction, but their nanoscale counterparts remain poorly understood.  We present a combination of electrochemical conditions and ligands which afford control over the stability of gold and copper nanoparticles for electrochemical CO2 reduction. Monte Carlo simulations reveal the mechanism by which the nanoparticles assemble into dendrites under polarization conditions and detailed electrochemical studies highlight the role of the ligand in driving dendrite formation. In addition, we have found that the nanoparticles exhibit selectivities for electrochemical carbon dioxide reduction that are distinct from their foil counterparts. Our improved understanding of the activity and stability of gold and copper nanoparticles for electrochemical CO2 reduction is a first step towards their incorporation into membrane electrode assemblies for electrolyzers.

Activity and stability of gold and copper nanoparticles for electrochemical carbon dioxide reduction

248th National Meeting (2014)

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