Electroreduction of carbon dioxide into higher-energy liquid fuels and chemicals is a promising but challenging renewable energy conversion technology. Among the electrocatalysts screened so far for carbon dioxide reduction, which includes metals, alloys, organometallics, layered materials and carbon nanostructures, only copper exhibits selectivity towards formation of hydrocarbons and multi-carbon oxygenates at fairly high efficiencies, whereas most others favour production of carbon monoxide or formate. Here we report that nanometre-size N-doped graphene quantum dots (NGQDs) catalyse the electrochemical reduction of carbon dioxide into multi-carbon hydrocarbons and oxygenates at high Faradaic efficiencies, high current densities and low overpotentials. The NGQDs show a high total Faradaic efficiency of carbon dioxide reduction of up to 90%, with selectivity for ethylene and ethanol conversions reaching 45%. The C2 and C3 product distribution and production rate for NGQD-catalysed carbon dioxide reduction is comparable to those obtained with copper nanoparticle-based electrocatalysts.

Graphene has initiated intensive research efforts on 2D crystalline materials due to its extraordinary set of properties and the resulting host of possible applications. Here the authors report on the controllable large-scale synthesis of C N, a 2D crystalline, hole-free extension of graphene, its structural characterization, and some of its unique properties. C N is fabricated by polymerization of 2,3-diaminophenazine. It consists of a 2D honeycomb lattice with a homogeneous distribution of nitrogen atoms, where both N and C atoms show a D -symmetry. C N is a semiconductor with an indirect bandgap of 0.39 eV that can be tuned to cover the entire visible range by fabrication of quantum dots with different diameters. Back-gated field-effect transistors made of single-layer C N display an on-off current ratio reaching 5.5 × 10 . Surprisingly, C N exhibits a ferromagnetic order at low temperatures (<96 K) when doped with hydrogen. This new member of the graphene family opens the door for both fundamental basic research and possible future applications.

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