摘要
Porous carbon nitride(CN)spheres with partially crystalline frameworks have been successfully synthesized via a nanocasting approach by using spherical mesoporous cellular silica foams(MCFs)as a hard template,and ethylenediamine and carbon tetrachloride as precursors.The resulting spherical CN materials have uniform diameters of ca.4μm,hierarchical three-dimensional(3-D)mesostructures with small and large mesopores with pore diameters centered at ca.4.0 and 43 nm,respectively,a relatively high BET surface area of~550 m^(2)/g,and a pore volume of 0.90 cm^(3)/g.High-resolution transmission electron microscope(HRTEM)images,wide-angle X-ray diffraction(XRD)patterns,and Raman spectra demonstrate that the porous CN material has a partly graphitized structure.In addition,elemental analyses,X-ray photoelectron spectra(XPS),Fourier transform infrared spectra(FT-IR),and CO_(2) temperature-programmed desorption(CO_(2)-TPD)show that the material has a high nitrogen content(17.8 wt%)with nitrogen-containing groups and abundant basic sites.The hierarchical porous CN spheres have excellent CO_(2) capture properties with a capacity of 2.90 mmol/g at 25℃and 0.97 mmol/g at 75℃,superior to those of the pure carbon materials with analogous mesostructures.This can be mainly attributed to the abundant nitrogen-containing basic groups,hierarchical mesostructure,relatively high BET surface area and stable framework.Furthermore,the presence of a large number of micropores and small mesopores also enhance the CO_(2) capture performance,owing to the capillary condensation effect.
基金
This work was supported by the National Natural Science Foundation of China(NSFC)(Nos.2089012,20721063,20821140537,20871030)
State Key Basic Research Program of PRC(Nos.2006CB932302 and 2009AA033701)
Shanghai Leading Academic Discipline Project(No.B108)
Science&Technology Com-mission of Shanghai Municipality(No.08DZ2270500)
C.S.Ha also thanks the National Research Foundation(NRF)of Korea for support through the Korea-China Joint Research Center Program on Mesoporous Thin Films(No.K20803001459-10B1200-00310)
the Acceleration Research Program(No.2010-0000790).
