物理化学学报 >> 2012, Vol. 28 >> Issue (04): 985-992.doi: 10.3866/PKU.WHXB201202071

材料物理化学 上一篇    

有机胺修饰具有较大孔径介孔材料的二氧化碳吸附性能

赵会民, 林丹, 杨刚, 淳远, 须沁华   

  1. 南京大学化学化工学院, 教育部介观重点实验室, 南京 210093
  • 收稿日期:2011-09-01 修回日期:2012-01-09 发布日期:2012-03-21
  • 通讯作者: 淳远 E-mail:ychun@nju.edu.cn
  • 基金资助:

    国家高技术研究发展计划项目(863) (2008AA06Z327), 中央高校基础研究基金(1116020503)及南京大学开放测试基金(0205001330)资助

Adsorption Capacity of Carbon Dioxide on Amine Modified Mesoporous Materials with Larger Pore Sizes

ZHAO Hui-Min, LIN Dan, YANG Gang, CHUN Yuan, XU Qin-Hua   

  1. Key Laboratory of Mesoscopic Chemistry of the Ministry of Education, School of Chemistry & Chemical Engineering, Nanjing University, Nanjing 210093, P. R. China
  • Received:2011-09-01 Revised:2012-01-09 Published:2012-03-21
  • Contact: CHUN Yuan E-mail:ychun@nju.edu.cn
  • Supported by:

    The project was supported by the National High-Tech Research and Development Program of China (863) (2008AA06Z327), Fundamental Research Funds for the Central Universities, China (1116020503), and Testing Fund of Nanjing University, China (0205001330).

摘要: 以非离子表面活性剂P123为模板剂, 正硅酸甲酯为硅源, 通过加入不同的扩孔剂制得具有较大孔径的SBA-15 类介孔材料, 并采用粉末X 射线衍射(XRD)、低温氮气吸附-脱附、扫描电镜(SEM)、傅里叶变换红外(FTIR)光谱等手段对所得样品进行了表征. 加入扩孔剂可以明显增大介孔材料的孔容和孔径, 而异辛烷为扩孔剂的扩孔效果明显优于四氯化碳. 经四乙烯五胺(TEPA)镀饰后, 这些样品均表现出良好的CO2吸附性能. 其中对于除去模板剂后再镀胺的样品, 其CO2吸附能力与介孔材料孔道结构关系不大, 而对于未除模板剂的原粉镀胺样品, CO2吸附能力则随孔道的变大而增强. 此外, 通过吸附等温线和CO2-程序升温脱附(TPD)手段比较了温度和压力对CO2吸附的影响, 发现在较高温度下吸附时CO2的吸附能力随压力的变化存在显著差别, 因而在这类TEPA修饰的介孔材料上可通过变压吸附的途径来实现对环境气流中CO2的吸附和分离.

关键词: 扩孔剂, 介孔材料, CO2, 变压吸附, 模板剂, 四乙烯五胺

Abstract: Mesoporous silica SBA-15-like materials with large pores were synthesized using tri-block copolymer P123 as a structure-directing agent, tetramethoxysilane as the silicon source, and different organic solvents as swelling agents. The resulting materials were characterized by powder X-ray diffraction (XRD), N2 adsorption-desorption, scanning electron microscopy (SEM), and Fourier transform infrared (FTIR) spectroscopy. The results showed that the introduction of swelling agents effectively enlarged the pore diameter and pore volume of the SBA-15 materials, and pore swelling with isooctane was larger than that with CCl4. When modified with tetraethylenepentamine (TEPA), all of these composite materials exhibited excellent adsorption capacities for CO2. The adsorption capacity of CO2 was independent of the pore structure, if the template was removed before modification with TEPA. By contrast, the adsorption capacity increased with the pore diameter when the as-synthesized mesoporous material was modified with TEPA. The effects of temperature and pressure on the CO2 adsorption capacity were investigated using adsorption isotherms and CO2 temperature-programmed desorption (TPD). With CO2 adsorption at higher temperature, the composite materials showed different adsorption capacities with pressure variation. As a result, the adsorption and separation of CO2 on these TEPA modified mesoporous materials in ambient air flow can be realized via pressure swing adsorption.

Key words: Swelling agent, Mesoporous materials, CO2, Pressure swing adsorption, Template, Tetraethylenepentamine

MSC2000: 

  • O647