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Electroreduction of CO2 to fuels or valuable chemicals is a promising way to mitigate the greenhouse effect. Herein, ultrathin In2Se3 nanosheets are reported as a robust catalyst for CO2-to-CO conversion with a faradaic efficiency of 89% and a stable activity of >24 h. Theoretical investigations show that the exposed electronegative Se atoms stabilize *COOH and, thus, facilitate CO2-to-CO conversion. Keywords: CO2 reduction, Electrocatalysis, Ultrathin In2Se3 nanosheets, CO
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