Abstract

AbstractUsing sunlight to produce valuable chemicals and fuels from carbon dioxide (CO2), i.e., artificial photosynthesis (AP) is a promising strategy to achieve solar energy storage and a negative carbon cycle. However, selective synthesis of C2compounds with a high CO2conversion rate remains challenging for current AP technologies. We performed CO2photoelectroreduction over a graphene/silicon carbide (SiC) catalyst under simulated solar irradiation with ethanol (C2H5OH) selectivity of>99 % and a CO2conversion rate of up to 17.1 mmol gcat−1 h−1with sustained performance. Experimental and theoretical investigations indicated an optimal interfacial layer to facilitate the transfer of photogenerated electrons from the SiC substrate to the few‐layer graphene overlayer, which also favored an efficient CO2to C2H5OH conversion pathway.

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