化工学报

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氨气改性的NH3@MIL-53(Cr)吸附CO2和CH4的性能

杨琰1, 王莎1, 张志娟2, 夏启斌1, 李忠1   

  1. 1 华南理工大学化学与化工学院, 广东 广州 510640;
    2 暨南大学大气环境安全与污染控制研究所, 广东 广州 510632
  • 收稿日期:2014-02-17 修回日期:2014-03-26 出版日期:2014-05-05 发布日期:2014-05-05
  • 通讯作者: 夏启斌
  • 基金资助:

    国家重点基础研究发展计划项目(2013CB733506);国家自然科学基金项目(21176085)。

CO2 and CH4 adsorption performance of modified MIL-53(Cr) via ammonia vapor

YANG Yan1, WANG Sha1, ZHANG Zhijuan2, XIAQibin1, LI Zhong1   

  1. 1 School of Chemical Engineering, South China University of Technology, Guangzhou 510640, Guangdong, China;
    2 Institute of Atmospheric Environment Safety and Pollution Control, Jinan University, Guangzhou 510632, Guangdong, China
  • Received:2014-02-17 Revised:2014-03-26 Online:2014-05-05 Published:2014-05-05
  • Supported by:

    supported by the National Basic Research Program of China (2013CB733506) and the National Natural Science Foundation of China (21176085).

摘要: 采取水热法成功合成MIL-53(Cr)晶体,分别应用0.1、1、3 mol·L-1的氨气对MIL-53(Cr)进行改性,制得系列的NH3@MIL-53(Cr)-1#,NH3@MIL-53(Cr)-2#,NH3@MIL-53(Cr)-3#。实验结果表明:与原始的MIL-53(Cr)晶体相比,尽管制得NH3@MIL-53(Cr)系列材料的比表面积依次减少,但其单位比表面积的CO2吸附容量大小依次为:NH3@MIL-53(Cr)-3#>NH3@MIL-53(Cr)-2#>NH3@MIL-53(Cr)-1#。表明氨气改性会使得材料表面的碱性增强,从而增强了其对酸性气体CO2的吸附。此外,改性后的NH3@MIL-53(Cr)对水蒸气的吸附量明显减少,表明其憎水性能得到改善。较高浓度氨气改性会导致材料的比表面积大幅下降,会引起单位质量吸附剂的吸附容量下降。用1 mol·L-1浓度的氨气改性得到的NH3@MIL-53(Cr)-2#,不仅对CO2的吸附容量最大,而且对CH4的吸附容量明显下降,这将有助于进一步提高改性材料NH3@MIL-53(Cr)-2# 对CO2/CH4的吸附选择性。

关键词: MIL-53(Cr), 二氧化碳, 甲烷, 水蒸气, 吸附, 氨气

Abstract: MIL-53(Cr)crystals were synthesized by the hydrothermal synthesis method, and then modified by ammonia vapor of different concentrations to obtain the modified materials NH3@MIL-53(Cr). The CO2 and water vapor isotherms on the NH3@MIL-53(Cr)were determined by means of the gravity method. Although the specific surface area of the modified materials NH3@MIL-53(Cr)became smaller compared to original MIL-53(Cr), their CO2 adsorption capacities per unit surface area of adsorbent became significantly higher, following the order: NH3@MIL-53(Cr)-3#>NH3@MIL-53(Cr)-2#>NH3@MIL-53(Cr)-1#. In addition, Isotherms of water vapor on the modified samples NH3@MIL-53(Cr) were lower than those on the MIL-53(Cr), suggesting significant improvement of hydrophobicity of the modified samples. The CO2 adsorption capacity of the NH3@MIL-53(Cr)-2# modified by using ammonia vapor of 1 mol·L-1 was the highest among the modified samples. More interestingly, the CO2 adsorption performance of the modified sample NH3@MIL-53 (Cr)-2# was significantly improved, while its CH4 adsorption performance was weakened, which would be helpful to enhance its selectivity for CO2/CH4 adsorption.

Key words: MIL-53(Cr), CO2, CH4, water vapor, adsorption, ammonia vapor

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