The electrochemical reduction of CO2 (CO2RR) to obtain high-value products such as hydrocarbons or liquid fuels can effectively alleviate energy and environmental problems. However, the production of C2+ products with high selectivity remains a major challenge of CO2RR. Limited mass transport is one of the important reasons that hinder the deep reduction of CO2 to C2+ products. The catalyst design should be combined with the reactor design and optimization to further break through the mass transport limitation and improve the performance of CO2RR. The superior CO2 mass transport in gas diffusion electrode (GDE)-based systems originates from shorter diffusional lengths than that in conventional H-type cells. Gas diffusion in the catalyst layer becomes the mass transport limiting step in the cathode, which is due to the hydrophilicity of metallic nature. Herein, 1-dodecanethiol was used to modify the GDE interface, which effectively promoted gas mass transport and ensured proper H2O transport. The alkylthiol-modified electrode exhibits a remarkable Faradaic efficiency for C2+ products. This work provides deep insight of the influence of local environment on CO2RR pathways, which also contributes new ideas for the highly selective preparation of C2+ products.

Interfacial modification for effective CO2 electroreduction

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