摘要
In this work,nitrogen-doped porous carbons(NACs)were fabricated as an adsorbent by urea modification and KOH activation.The CO_(2) adsorption mechanism for the NACs was then explored.The NACs are found to present a large specific surface area(1920.72-3078.99 m2·g^(-1))and high micropore percentage(61.60%-76.23%).Under a pressure of 1 bar,sample NAC-650-650 shows the highest CO_(2) adsorption capacity up to 5.96 and 3.92 mmol·g^(-1) at 0 and 25℃,respectively.In addition,the CO_(2)/N_(2) selectivity of NAC-650-650 is 79.93,much higher than the value of 49.77 obtained for the nonnitrogen-doped carbon AC-650-650.The CO_(2) adsorption capacity of the NAC-650-650 sample maintains over 97% after ten cycles.Analysis of the results show that the CO_(2) capacity of the NACs has a linear correlation(R^(2)=0.9633)with the cumulative pore volume for a pore size less than 1.02 nm.The presence of nitrogen and oxygen enhances the CO_(2)/N_(2) selectivity,and pyrrole-N and hydroxy groups contribute more to the CO_(2) adsorption.In situ Fourier transform infrared spectra analysis indicates that CO_(2) is adsorbed onto the NACs as a gas.Furthermore,the physical adsorption mechanism is confirmed by adsorption kinetic models and the isosteric heat,and it is found to be controlled by CO_(2) diffusion.The CO_(2) adsorption kinetics for NACs at room temperature and in pure CO_(2) is in accordance with the pseudo-first-order model and Avramís fractional-order kinetic model.
基金
funded by the National Key Research and Development Program of China(Grant No.2018YFB0605401)
the National Natural Science Foundation of China(Grant No.21868025)
the National First-rate Discipline Construction Project of Ningxia(No.NXYLXK2017A04)
the Key Research and Development Program of Ningxia Province,China(No.2018BCE01002)
Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(Grant No.2020-KF-39).
