期刊
ACS CATALYSIS
卷 7, 期 7, 页码 4497-4503出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b00729
关键词
CO2 hydrogenation; graphene quantum dots; N doping; methane
资金
- SABIC
- U.S. Department of Energy [DE-AC02-05CH11231]
- South Carolina Center of Economic Excellence for Strategic Approaches to the Generation of Electricity
The hydrogenation of CO2 into useful chemicals provides an industrial-scale pathway for CO2 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 CO2 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 CO2 reduction and also higher CO2 conversion and selectivity toward CH4 over CO.
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