Catalyst Particle Density Controls Hydrocarbon Product Selectivity in CO2 Electroreduction on CuOx

Abstract

A key challenge of the carbon dioxide electroreduction (CO2RR) on Cu-based nanoparticles is its low faradic selectivity toward higher-value products such as ethylene. Here, we demonstrate a facile method for tuning the hydrocarbon selectivities on CuO_x nanoparticle ensembles by varying the nanoparticle areal density. The sensitive dependence of the experimental ethylene selectivity on catalyst particle areal density is attributed to a diffusional interparticle coupling that controls the de- and re-adsorption of CO and thus the effective coverage of CO_ad intermediates. Thus, higher areal density constitutes dynamically favored conditions for CO re-adsorption and *CO dimerization leading to ethylene formation independent of pH and applied overpotential.

Keywords: areal particle density; carbon dioxide; copper oxide; electroreduction; ethylene.