A Molecular Foaming and Activation Strategy to Porous N-Doped Carbon Foams for Supercapacitors and CO2 Capture

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).

活性泡沫炭用于超级电容器电极材料

以酚醛树脂、煤沥青泡沫炭为原料,经水蒸气活化制得比表面积分别为961和953m2/g的活性泡沫炭。采用扫描电镜、BET吸附仪、恒流充放电法和循环伏安法对两种活性泡沫炭的结构进行了表征并研究其充放电性能。结果表明,酚醛树脂泡沫炭在1.0nm以下的孔较煤沥青泡沫炭丰富。在1.0mA充放电时,两者的充放电容量分别为106.28和105.1F/g,相差不大,当充放电电流增大到50mA时,前者容量为41.94F/g,后者为17.23F/g。可见,微孔的孔径分布对充放电性能具有很大影响,增大微孔的孔径有利于提高活性炭电极的充放电容量和功率。循环伏安法测试表明在100mV/min扫描速率下酚醛树脂泡沫炭粉的电化学窗口大于煤沥青泡沫炭粉。