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    Carbon Dioxide Hydrogenation over a Metal-Free Carbon-Based Catalyst

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    The hydrogenation of CO<sub>2</sub> into useful chemicals provides an industrial-scale pathway for CO<sub>2</sub> recycling. The lack of effective thermochemical catalysts currently precludes this process, since it is challenging to identify structures that can simultaneously exhibit high activity and selectivity for this reaction. Here, we report, for the first time, the use of nitrogen-doped graphene quantum dots (NGQDs) as metal-free catalysts for CO<sub>2</sub> hydrogenation. The nitrogen dopants, located at the edge sites, play a key role in inducing thermocatalytic activity in carbon nanostructures. Furthermore, the thermocatalytic activity and selectivity of NGQDs are governed by the doped N configurations and their corresponding defect density. The increase of pydinic N concentration at the edge site of NGQDs leads to lower initial reaction temperature for CO<sub>2</sub> reduction and also higher CO<sub>2</sub> conversion and selectivity toward CH<sub>4</sub> over CO
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