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A catalyst system with dedicated selectivity toward a single hydrocarbon or oxygenate product is essential to enable the industrial application of electrochemical conversion of CO 2  to high-value chemicals. Cu is the only known metal catalyst that can convert CO 2  to high-order hydrocarbons and oxygenates. However, the Cu-based catalysts suffer from diverse selectivity. Here, we report that the functionalized graphene quantum dots can direct CO 2  to CH 4  conversion with simultaneous high selectivity and production rate. The electron-donating groups facilitate the yield of CH 4  from CO 2  electro-reduction while electron-withdrawing groups suppress CO 2  electro-reduction. The yield of CH 4  on electron-donating group functionalized graphene quantum dots is positively correlated to the electron-donating ability and content of electron-donating group. The graphene quantum dots functionalized by either –OH or –NH 2  functional group could achieve Faradaic efficiency of 70.0% for CH 4  at −200 mA cm −2  partial current density of CH 4 . The superior yield of CH 4  on electron-donating group- over the electron-withdrawing group-functionalized graphene quantum dots possibly originates from the maintenance of higher charge density of potential active sites (neighboring C or N) and the interaction between the electron-donating group and key intermediates. This work provides insight into the design of active carbon catalysts at the molecular scale for the CO 2  electro-reduction.

Regulation of functional groups on graphene quantum dots directs selective CO2 to CH4 conversion