Institution: | 1. State Key Laboratory of Chemical Resource Engineering, Laboratory of Electrochemical Process and Technology for Materials, Beijing University of Chemical Technology, Beijing, 100029 China
Beijing Advanced Innovation Center for Soft Matter Science, and Engineering, Beijing University of Chemical Technology, Beijing, 100029 China;2. Harris Science Research Institute, Doshisha University, 1–3 Miyakodani Tatara, Kyotanabe, Kyoto, 611-0394 Japan;3. State Key Laboratory of Chemical Resource Engineering, Laboratory of Electrochemical Process and Technology for Materials, Beijing University of Chemical Technology, Beijing, 100029 China |
Abstract: | An ice/salt-assisted strategy has been developed to achieve the green and efficient synthesis of ultrathin two-dimensional (2D) micro/mesoporous carbon nanosheets (CNS) with the dominant active moieties of Fe?N4 (Fe-N-CNS) as high-performance electrocatalysts for the oxygen reduction reaction (ORR). The strategy involves freeze-drying a mixture of iron porphyrin and KCl salt using ice as template followed by a confined pyrolysis with KCl as an independent sealed nanoreactor to facilitate the formation of 2D carbon nanosheets, N incorporation, and porosity creation. The well-defined assembly of ultrathin 2D carbon nanosheets ensures high utilization of D1 and D3 Fe?N4 active sites, and effectively promotes the mass transport of ORR reactants by virtue of the pronounced mesoporous structure. The resulting Fe-N-CNS electrocatalyst was shown to exhibit superior ORR activity, better electrochemical durability, and methanol tolerance towards ORR in alkaline electrolyte relative to the commercial Pt/C electrocatalyst. |