The electrochemical conversion of carbon dioxide (CO2) into value-added multi-carbon (C2+) products is an attractive route to close the carbon loop. However, the formation of C2+ products with high selectivity remains a major challenge in this field. Modification of gas diffusion electrode (GDE) provides a promising approach for improving the selectivity of C2+ products in CO2 reduction reaction (CO2RR). However, the vital role of interfacial wettability for reaction pathways of ethylene and ethanol remains largely unexplored. This work describes the design and realization of balance between mass transport of CO2 and H2O via modifying alkanethiols to reveal the contribution of interfacial wettability to ethylene and ethanol pathways. The ethanol to ethylene ratio can be continuously tailored in a wide range with remarkable Faradaic efficiencies toward ethanol and C2+ products. Characterization and CFD results unveil that the vibration in intermediate coverage derived from changes in CO2 and H2O mass transport via interfacial wettability governs the pathways of ethylene and ethanol. Interfacial wettability is thus proved as a controlling factor in CO2 reduction pathways and should be considered in the future design of stable modifiers or catalysts for further extending activity and selectivity.

Balanced interfacial wettability to efficiently control CO2 electroreduction to ethanol and ethylene

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