摘要
Hierarchically porous carbon materials are promising for energy storage,separation and catalysis.It is desirable but fairly challenging to simultaneously create ultrahigh surface areas,large pore volumes and high N contents in these materials.Herein,we demonstrate a facile acid-base enabled in situ molecular foaming and activation strategy for the synthesis of hierarchically macro-/meso-/microporous N-doped carbon foams(HPNCFs).The key design for the synthesis is the selection of histidine(His)and potassium bicarbonate(PBC)to allow the formation of 3D foam structures by in situ foaming,the PBC/His acid-base reaction to enable a molecular mixing and subsequent a uniform chemical activation,and the stable imidazole moiety in His to sustain high N contents after carbonization.The formation mechanism of the HPNCFs is studied in detail.The prepared HPNCFs possess 3D macroporous frameworks with thin well-graphitized carbon walls,ultrahigh surface areas(up to 3200 m^2 g^-1),large pore volumes(up to 2.0 cm^3 g^-1),high micropore volumes(up to 0.67 cm^3 g^-1),narrowly distributed micropores and mesopores and high N contents(up to 14.6 wt%)with pyrrolic N as the predominant N site.The HPNCFs are promising for supercapacitors with high specific capacitances(185-240 F g^-1),good rate capability and excellent stability.They are also excellent for CO2 capture with a high adsorption capacity(~4.13 mmol g^-1),a large isosteric heat of adsorption(26.5 kJ mol^-1)and an excellent CO2/N2 selectivity(~24).
基金
the National Natural Science Foundation of China(Nos.21875153,21501125)
the Natural Science Foundation of Jiangsu Province(BK20150312)
the Jiangsu Shuangchuang Team Program is appreciated.