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过程工程学报 ›› 2020, Vol. 20 ›› Issue (1): 108-115.DOI: 10.12034/j.issn.1009-606X.219164

• 环境与能源 • 上一篇    下一篇

离子液体自模板合成多孔碳氮材料及其对二氧化碳的吸附

刘佳慧1,2, 刘会婷2, 赵国英2*, 孙振宇1*   

  1. 1. 北京化工大学化学工程学院,有机?无机复合材料国家重点实验室,北京 100029 2. 中国科学院过程工程研究所多相复杂系统国家重点实验室,离子液体清洁过程北京市重点实验室,北京 100190
  • 收稿日期:2019-03-25 修回日期:2019-05-07 出版日期:2020-01-22 发布日期:2020-01-14
  • 通讯作者: 赵国英
  • 基金资助:
    高芳烃高含氮重油催化转化反应基础研究;国家重点基础研究发展基金资助项目;国科学院仪器发展基金资助项目

Ionic liquids self-templating to synthesize nitrogen-doped porous carbon materials for CO2 adsorption

Jiahui LIU1,2, Huiting LIU2, Guoying ZHAO2*, Zhenyu SUN1*   

  1. 1. State Key Laboratory of Organic–Inorganic Composites, School of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China 2. Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
  • Received:2019-03-25 Revised:2019-05-07 Online:2020-01-22 Published:2020-01-14
  • Contact: ZHAO Guo-ying

摘要: 以多种氰基离子液体为前驱体,采用高温碳化法直接制备多孔碳氮材料,系统考察了离子液体前驱体阳离子结构、阴离子种类及合成条件等因素对碳化材料比表面积、氮元素含量及氮种类的影响,并研究其对CO2的吸附性能。结果表明,阴离子在聚合过程中起模板剂的作用。合成材料主要呈介孔结构,比表面积最高达732.6 m2/g,氮含量最高为9.9wt%,在温度25℃、压力1.8 MPa条件下,CO2的吸附量最高达20.9wt%。多孔碳氮材料经180℃真空加热后可完全脱附再生,再生稳定性良好。

关键词: 离子液体, 富氮, 多孔碳材料, 二氧化碳, 吸附

Abstract: With the increase of man-made emissions, CO2 capture after combustion has become a key component of greenhouse gas emission reduction. The search for a better CO2 capture material has caused great attention and nitrogen-doped porous carbon materials are considered as one of the most promising candidates. However, traditional preparation methods of nitrogen-doped porous carbon materials suffer from the shorts of complex process, harsh reaction conditions and low product yield. Using ionic liquids as the raw materials to synthesize nitrogen-doped porous carbon materials through ionothermal cyclotrimerization is a simplified and high-yield manner. In the present works, a series of nitrogen-doped porous carbon materials were synthesized directly by high temperature carbonization using cyano ionic liquids as raw material. By varying the structure and anions of the ionic liquid precursor and synthesis conditions, the pore architecture and surface functional groups of the materials could be controlled. The ionic liquid precursors were characterized by 1H-NMR, CHN element analysis and thermogravimetric analysis (TGA). The nanostructure of the porous carbon materials were observed by Transmission Electron Microscope (TEM) and the types of N-containing groups of the carbon material were investigated by X-ray photoelectron spectroscopy (XPS). The N element content was confirmed by elements analysis. The pore structures were evaluated by Brunauer–Emmett–Teller (BET) nitrogen sorption isotherms measured at 77 K. CO2 adsorption performance of these materials was carried out on a gravimetric microbalance (IGA). Combing the BET results and TGA analysis showed that the anions of ionic liquids acted as the template agent in the process of polymerization. These nitrogen-doped porous carbon materials mainly had mesoporous structure and the highest specific surface area reached to 732.6 m2/g. The highest N content reached to 9.9wt%. Owing to strong interactions between the CO2 molecules and nitrogen-containing basic sites, the highest CO2 adsorption quantity reached to 20.9wt% under 1.8 MPa at 25℃. The materials could be completely regenerated under the vacuum at 180℃, indicating its good stability.

Key words: ionic liquids, nitrogen-enriched, porous carbon materials, CO2, adsorption