Rational Design of Efficient Palladium Catalysts for\nElectroreduction of Carbon Dioxide to Formate

Abstract

The electrochemical\nreduction of CO₂ into renewable\nchemical products such as formic acid is an important and challenging\ngoal. Traditional Pd catalysts suffer from CO poisoning, which leads\nto current density decay and short operating lifetimes. Here we explored\nthe ability to control Pd nanoparticle surface morphology to amplify\ncatalytic activity and increase stability in the electroreduction\nof CO₂ to formate. Through computational studies we have\nelucidated trends in intermediate binding which govern the selectivity\nand catalytic activity. We then rationally synthesized Pd nanoparticles\nhaving an abundance of high-index surfaces to maximize electrocatalytic\nperformance. This catalyst displays a record current density of 22\nmA/cm² at a low overpotential of −0.2 V with a Faradaic\nefficiency of 97%, outperforming all previous Pd catalysts in formate\nelectrosynthesis. The findings presented in this work provide rational\ndesign principles which highlight morphological control of high-index\nsurfaces for the effective and stable catalytic electroreduction of\nCO₂ to liquid fuels.