(2hu) Amine-Functionalized Carbon Nanodot Electrocatalysts Converting Carbon Dioxide to Methane
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2022
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The electrochemical conversion of carbon dioxide (CO2) to methane (CH4), which can be used not only as fuel but also as a hydrogen carrier, has drawn great attention for use in supporting carbon capture and utilization. The design of active and selective electrocatalysts with exceptional CO2-to-CH4 conversion efficiency is highly desirable; however, it remains a challenge. Here a molecular tuning strategyâin situ amine functionalization of nitrogen-doped graphene quantum dots (GQDs) for highly efficient CO2-to-CH4 conversion is presented. Amine functionalized nitrogen-doped GQDs achieve a CH4 Faradic efficiency (FE) of 63% and 46%, respectively, at CH4 partial current densities of 170 and 258 mA cmâ2, approximating to or even outperforming state-of-the-art Cu-based electrocatalysts. These GQDs also convert CO2 to C2 products mainly including C2H4 and C2H5OH with a maximum FE of â10%. A systematic analysis reveals that the CH4 yield varies linearly with amine group content, whereas the C2 production rate is positively dependent on pyridinic N dopant content. This work provides insight into the rational design of carbon catalysts with CO2-to-CH4 conversion efficiency at the industrially relevant level.
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