Abstract
Cost competitive electroreduction of CO2 to CO requires electrochemical systems that exhibit partial current density (jCO) exceeding 150 mA cm–2 at cell overpotentials (|ηcell|) less than 1 V. However, achieving such benchmarks remains difficult. Here, we report the electroreduction of CO2 on a supported gold catalyst in an alkaline flow electrolyzer with performance levels close to the economic viability criteria. Onset of CO production occurred at cell and cathode overpotentials of just −0.25 and −0.02 V, respectively. High jCO (∼99, 158 mA cm–2) was obtained at low |ηcell| (∼0.70, 0.94 V) and high CO energetic efficiency (∼63.8, 49.4%). The performance was stable for at least 8 h. Additionally, the onset cathode potentials, kinetic isotope effect, and Tafel slopes indicate the low overpotential production of CO in alkaline media to be the result of a pH-independent rate-determining step (i.e., electron transfer) in contrast to a pH-dependent overall process.
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