Abstract

Efficient electroreduction of carbon dioxide has been a widely pursued goal as a sustainable method to produce value-added chemicals while mitigating greenhouse gas emissions. Processes have been demonstrated for the electroreduction of CO2 to CO at nearly 100 % faradaic efficiency, and as a consequence, there has been growing interest in the further electroreduction of carbon monoxide. Oxide-derived copper catalysts have promising performance for the reduction of CO to hydrocarbons but have still been unable to achieve high selectivity to individual products. A pulsed-bias technique is one strategy for tuning electrochemical selectivity without changing the catalyst. Herein a pulsed-bias electroreduction of CO was investigated on oxide-derived copper catalyst. Increased selectivity for single-carbon products (i.e., formate and methane) was achieved for higher pulse frequencies (<1 s pulse times), as well as an increase in the fraction of charge directed to CO reduction rather than hydrogen evolution.

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