Dilute alloy electrocatalysts enable asymmetric C–C coupling for ethylene production from a CO2 post-capture liquid
摘要
Direct air capture of CO2 often uses alkali hydroxides to form carbonate; however, releasing CO2 and regenerating alkali hydroxides requires an energy-intensive thermal cycle at ~900 °C. Reactive capture systems instead seek to integrate CO2 release with its chemical reduction in the pathway to fuels and chemicals. Here we focus on a purely electrosynthetic route, beginning by examining why previous attempts at electrified ethylene synthesis from carbonate post-capture liquids have suffered from low overall energy efficiencies. We find that a hydrophilic environment and limited rate of CO2 generation in situ lead to low CO2 availability and consequently low *CO coverage on the catalyst surface, and that this hinders C–C coupling. We identify dilute alloy catalysts that implement asymmetric CO–CHO coupling, a lower-barrier route to C–C coupling compared with the conventional symmetric pathway. We report a 51% ± 2% ethylene Faradaic efficiency, a 66 wt% ± 2% concentrated ethylene stream and a 20% end-to-end energy efficiency at 200 mA cm−2. The energy efficiency is a twofold improvement over the most efficient prior report of ethylene production via electrified reactive capture.