CO2 Reduction for C2+ in Seawater Using a Graphitic Frustrated Lewis Pair Catalyst

Abstract Ocean acidification due to the absorption of 40% of the world’s anthropogenic CO2 emissions severely affects the faltering marine ecosystem and the economy. However, there are few reports on reducing CO2 dissolved in seawater. Herein, we introduce an electrochemical CO2 reduction battery system for use in seawater with a graphitic frustrated Lewis pair catalytic cathode doped with boron and nitrogen (BN-GFLP). BN-GFLP converts CO2 dissolved in seawater to multi-carbon (C2+) products during the discharge process, thus increasing the pH of intentionally acidified seawater from 6.4 to 8.0 with more than 87% Faradaic efficiency. In computational chemistry and spectroscopy, BN-GFLP binds CO2 in a unique manner that enables exothermic C–C coupling pathway to deliver 95% selectivity for valuable C2+ products. Based on our results, we suggest a molecular design strategy for next-generation CO2 reduction catalysts for both green oceans and the atmosphere.