CIESC Journal ›› 2021, Vol. 72 ›› Issue (5): 2688-2696.DOI: 10.11949/0438-1157.20201277

• Separation engineering • Previous Articles     Next Articles

Computational screening study of radioactive gas Rn from zirconium-based metal organic frameworks materials

WANG Ying1(),ZHENG Baishu1(),WANG Liusheng1,WANG Guanyu1,ZENG Wenjiang1,WANG Zhaoxu1,YANG Qingyuan2()   

  1. 1.Key Laboratory of Controllable Preparation and Functional Application of Fine Polymers, Key Laboratory of Theoretical Organic Chemistry and Functional Molecules, School of Chemistry and Chemical Engineering, Hunan University of Science and Technology, Xiangtan 411201, Hunan, China
    2.State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
  • Received:2020-09-07 Revised:2020-12-29 Online:2021-05-05 Published:2021-05-05
  • Contact: ZHENG Baishu,YANG Qingyuan

锆基金属-有机骨架材料分离放射性气体Rn的计算筛选研究

王莹1(),郑柏树1(),王刘盛1,汪冠宇1,曾文江1,汪朝旭1,阳庆元2()   

  1. 1.湖南科技大学化学化工学院,精细聚合物可控制备及功能化应用重点实验室,理论有机化学与功能分子重点实验室,湖南 湘潭 411201
    2.北京化工大学有机无机复合材料国家重点实验室,北京 100029
  • 通讯作者: 郑柏树,阳庆元
  • 作者简介:王莹(1998—),女,硕士研究生,785676085@qq.com
  • 基金资助:
    国家自然科学基金项目(21973029);湖南省自然科学基金项目(2020JJ4290);湖南省教育厅项目(19A178);湖南省研究生科研创新项目(CX20201002)

Abstract:

Radon (Rn) which exists in building materials has become an important radioactive gas that can pollute indoor air and can cause serious harm to human health. Therefore, it is urgent to develop new porous materials with high-performance to selectively adsorb Rn. Based on the grand canonical ensemble Monte Carlo simulation method (GCMC), the adsorption and separation performance of 163 zirconium-based metal organic frameworks (Zr-MOF) for Rn/N2 and Rn/O2 mixtures under room temperature and pressure were systematically studied. The results showed that Zr-MOF materials exhibited excellent adsorption and separation performance of Rn, when their pore size is in the range of 5.6—8 ? and accessible surface area is in the range of 140—870 m2/g. In addition, it was also found that the introduction of strong polar functional groups, such as —COOH and —SO3H on the framework could dramatically enhance the separation performance of materials for Rn/N2 and Rn/O2 mixtures. These results can provide a theoretical reference for the future rational design and controllable synthesis of high-performance MOF separation materials.

Key words: metal organic frameworks, high-throughput screening, molecular simulation, radon, adsorption, separation

摘要:

存在于建筑材料中的氡(Rn)已成为污染室内空气的一种重要放射性气体,对人体的健康可造成严重的危害,因此开发对其具有高效分离性能的新型多孔材料具有重要的意义。基于巨正则系综的Monte Carlo模拟方法,系统地研究了163种锆基金属-有机骨架材料(Zr-MOF)在常温常压下对Rn/N2和Rn/O2混合气体的吸附分离性能。研究结果表明材料的孔径在5.6~8 ?(1 ? =0.1 nm)、可接触比表面积在140 ~870 m2/g范围内,材料对Rn的分离效果最佳,并发现在材料骨架上引入强极性功能基团如羧基(—COOH)和硫磺基(—SO3H)等,有利于强化材料对Rn的分离性能。研究结果可为今后理性设计与可控合成相关高性能MOF分离材料提供理论参考。

关键词: 金属有机骨架材料, 高通量筛选, 分子模拟, 氡, 吸附, 分离

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