1Suzhou Key Laboratory of Green Chemical Engineering, School of Chemical and Environmental Engineering, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, Jiangsu, China
2Department of Chemistry and Laboratory of Advanced Materials, Fudan University, Shanghai, China
3Department of Chemical Engineering, Monash University, Clayton, VIC, Australia
Adv. Funct. Mater.2016,26, 6649–6661
A general solvent-free assembly approach via directly heating amino acid and mesoporous silica mixtures is developed for the synthesis of a family of highly nitrogen-doped mesoporous carbons. Amino acids have been used as the sole precursors for templating synthesis of a series of ordered mesoporous carbons. During heating, amino acids are melted and strongly interact with silica, leading to effective loading and improved carbon yields (up to ≈25 wt%), thus to successful structure replication and nitrogen-doping. Unique solvent-free structure assembly mechanisms are proposed and elucidated semi-quantitatively by using two affinity scales. Significantly high nitrogen-doping levels are achieved, up to 9.4 (16.0) wt% via carbonization at 900 (700) °C. The diverse types of amino acids, their variable interactions with silica and different pyrolytic behaviors lead to nitrogen-doped mesoporous carbons with tunable surface areas (700–1400 m2g−1), pore volumes (0.9–2.5 cm3g−1), pore sizes (4.3–10 nm), and particle sizes from a single template. As demonstrations, the typical nitrogen-doped carbons show good performance in CO2capture with high CO2/N2selectivities up to ≈48. Moreover, they show attractive performance for oxygen reduction reaction, with an onset and a half-wave potential of ≈−0.06 and−0.14 V (vs Ag/AgCl).
链接:http://onlinelibrary.wiley.com/doi/10.1002/adfm.201601640/abstract