Electrochemical CO2 reduction reaction (CO2RR) is an attractive solution to close the anthropogenic carbon cycle and store intermittent renewable energy in value-added chemicals and fuels. While Fe nanoparticles (NPs) are typically employed as catalysts for hydrogen evolution reaction (HER, a competing reaction against CO2RR), herein efficient CO2 electroreduction is achieved through tuning their chemical microenvironment. Porous carbon layers were deposited on those Fe NPs, which creates a hydrophobic environment to enrich local CO2 concentration, suppress water penetration and thus HER in the micropores. This strategy successfully turns Fe NPs into an excellent CO2RR catalyst with over 90% CO Faradaic efficiency (FE). Due to the unique local chemical environment created above, the high CO selectivity could be maintained even in acidic electrolytes, which provides a promising approach to addressing the notorious issue of carbonate precipitation in widely used alkaline solutions for CO2 electrolyzers.

Iron nanoparticles tuned to catalyze CO2 electroreduction in acidic solutions through chemical microenvironment engineering

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