物理化学学报 >> 2014, Vol. 30 >> Issue (6): 1169-1174.doi: 10.3866/PKU.WHXB201404223

催化和表面科学 上一篇    下一篇

源自密胺基多孔聚合物的富氮微孔炭及选择性吸附CO2

胡敬秀, 张静, 邹建锋, 肖强, 钟依均, 朱伟东   

  1. 浙江师范大学物理化学研究所, 先进催化材料省部共建教育部重点实验室, 浙江金华321004
  • 收稿日期:2014-02-19 修回日期:2014-04-21 发布日期:2014-05-26
  • 通讯作者: 肖强,钟依均 E-mail:xiaoq@zjnu.cn;jyzhong@zjnu.cn
  • 基金资助:

    国家自然科学基金(21101139,21371152)资助项目

Nitrogen-Rich Microporous Carbon Derived from Melamine-Based Porous Polymer for Selective CO2 Adsorption

HU Jing-Xiu, ZHANG Jing, ZOU Jian-Feng, XIAO Qiang, ZHONG Yi-Jun, ZHU Wei-Dong   

  1. Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, Zhejiang Province, P. R. China
  • Received:2014-02-19 Revised:2014-04-21 Published:2014-05-26
  • Contact: XIAO Qiang, ZHONG Yi-Jun E-mail:xiaoq@zjnu.cn;jyzhong@zjnu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (21101139, 21371152).

摘要:

以间苯二甲醛和三聚氰胺为原料,通过Schiff 碱缩合反应合成了密胺基多孔聚合物(POP),经高温炭化后得到富氮微孔炭(NMC). 利用N2吸脱附和傅里叶变换红外(FTIR)光谱表征了POP和炭化后产物NMC的结构和组成,与POP相比,NMC的官能团数量减少,比表面积和微孔孔容大幅增加. 元素分析表明NMC含氮量高达12.5% (w). 采用体积法测定了CO2、CH4和N2在NMC上的单组分吸附平衡等温线,NMC展示出良好的CO2 吸附性能,298 K、100 kPa 下CO2 平衡吸附量可达2.34 mmol·g-1. 双位Langmuir (DSL)模型和单位Langmuir (SSL)模型分别较好地描述了CO2、CH4和N2在NMC上的吸附平衡数据,在此基础上,应用理想吸附溶液理论(IAST)预测了双组分混合气在NMC上的吸附等温线,结果表明NMC对CO2-N2和CO2-CH4有非常高的CO2吸附选择性,分别为144.9和12.8.

关键词: 微孔炭, CO2吸附, Langmuir模型, 理想吸附溶液理论, 选择性

Abstract:

Nitrogen-rich microporous carbon (NMC) was prepared by the carbonization of a melaminebased porous polymer (POP), which was synthesized via a Schiff base condensation using isophthalaldehyde and melamine as starting materials. N2 adsorption-desorption and Fourier transform infrared (FTIR) spectroscopy were used to characterize the structural properties of POP and the derived NMC. NMC contains less functional groups and has a higher specific surface area and microporous volume compared to POP. NMC has a N content of up to 12.5% (w), as determined by elemental analysis. Single-component adsorption equilibrium isotherms of CO2, CH4, and N2 on NMC were obtained using a volumetric method. NMC has a good CO2 capture property and its CO2 adsorption capacity was 2.34 mmol·g-1 at 298 K and 100 kPa. Dual-site Langmuir (DSL) or single-site Langmuir (SSL) models appropriately describe the adsorption equilibrium behavior of CO2, CH4, and N2 on NMC. Based on the combined fitting parameters, binary adsorption isotherms were predicted by ideal adsorbed solution theory (IAST). Very high adsorption selectivities of CO2 over N2 and CH4 were obtained and the values were 144.9 and 12.8, respectively.

Key words: Microporous carbon, CO2 adsorption, Langmuir model, IAST, Selectivity