Lawrence Berkeley National Laboratory

Electrochemical carbon dioxide reduction represents a promising path to utilize CO2 as a feedstock for generating valuable products such as fuels and chemicals. Faradaic efficiencies near 100% have been achieved for certain CO2 reduction products such as CO, but the electrolyzer outlet streams usually contain large fractions of unreacted CO2, dropping the product concentrations below 1% in many cases. The system disclosed here recycles the unreacted CO2 together with the products and flows them back into the CO2 reduction reactor, enabling much higher CO2 conversion rates without dropping the gas flow rate. However, simple recirculation is shown to accumulate significant amounts of hydrogen, impeding effective CO2 reduction. In this looped system, an electrochemical H2 pump is placed in series with the CO2 reactor, which effectively removes all the H2 from the recycled gas stream, increasing the concentrations of carbon-containing products. The system was initially tested with a CO-generating catalyst and CO concentrations above 70% were achieved in the recycled gas stream, compared to a maximum CO concentration of 8% in single-pass configuration. Results with a CO2 reactor targeting ethylene as the main product show that ethylene concentrations of at least 10% can be achieved, which is roughly 20 times higher compared to a single-pass system.