分子模拟研究微孔材料对光气吸附扩散性能的影响及材料筛选

doi:10.7503/cjcu20180575

高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (2): 317.doi: 10.7503/cjcu20180575

分子模拟研究微孔材料对光气吸附扩散性能的影响及材料筛选

陈晓锋¹, 宁贺佳¹, 杨犁¹(), 彭昌军², 孙炜¹

1. 武汉工程大学绿色化工过程教育部重点实验室和湖北省新型反应器与绿色化学工艺重点实验室, 化工与制药学院, 武汉 430205
2. 华东理工大学化学与分子工程学院, 上海 200237

收稿日期:2018-08-16 出版日期:2019-02-10 发布日期:2018-11-05
作者简介:
联系人简介: 杨犁, 男, 博士, 副教授, 主要从事分子热力学模型开发、分子模拟和统计力学方面的研究. E-mail: liyang@wit.edu.cn
基金资助:
国家自然科学基金(批准号: 21406172)和湖北省自然科学基金(批准号: 2016CFB388)资助

Molecular Simulation Study on Influence and Screening of Micro-porous Materials for Phosgene Adsorption and Diffusion^†

CHEN Xiaofeng¹, NING Hejia¹, YANG Li^1,^*(), PENG Changjun², SUN Wei¹

1. Key Laboratory of Green Chemical Process of Ministry of Education, Key Laboratory of Novel Reactor and Green Chemical Technology of Hubei Province, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430205, China
2. School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China

Received:2018-08-16 Online:2019-02-10 Published:2018-11-05
Contact: YANG Li E-mail:liyang@wit.edu.cn
Supported by:
† Supported by the National Natural Science Foundation of China(No.21406172) and the Natural Science Foundation of Hubei Province, China(No.2016CFB388)

摘要/Abstract

摘要：

利用分子模拟的方法研究了微量光气(COCl₂)在微孔材料中的吸附和扩散性能, 并分析了材料结构的影响. 结果表明, 光气在金属有机框架材料(MOF)和共价有机框架材料(COF)中的吸附等温线主要表现为第Ⅰ类型和第Ⅴ类型吸附. 当光气压力较低时, COF材料和含有开放金属位点的材料对其吸附性能较好. 通过对不同压力下吸附量的比较发现, 吸附达到饱和前, 随着压力和孔隙率(VF)的升高, 材料对光气的吸附量增大. 通过分子动力学模拟研究光气在微孔材料中的扩散性能发现, 较强吸附位点的存在不利于光气在孔道中的扩散. 通过气体分子在材料中的径向函数分布图及模拟轨迹分析发现, 分子协同效应和空间位阻效应相互竞争决定了扩散速率的快慢. 综合评价材料的吸附和扩散性能发现, COF-102, COF-300, ZnMOF-74, Zn-DOBDC和PCN-60是理想的吸附材料, 这些材料可以应用于环境中光气泄漏的防治.

关键词: 光气, 微孔材料, 分子模拟, 吸附性能, 扩散系数

Abstract:

The adsorption and diffusion of phosgene(COCl₂) were calculated using molecular simulation in micro-porous materials. The influence of geometry of materials was still analyzed. The results show that the adsorption isotherms mainly are type Ⅰ and type Ⅴ in the researches. At low pressure the good performance of adsorption is covalent organic framework(COF) series and metal-organic framework(MOF) containing open-metal sites. Through the comparison of adsorption in different pressures, the adsorption capacity was determined by void fraction(VF) of materials with pressure increasing before reaching saturated adsorption. The strong adsorption site could obstruct the diffusivity of phosgene in micro-porous materials from molecular dynamic simulation. The diffusivity of phosgene is affected by competition between molecular synergy effects and steric effects through the analysis of radial distribution function(RDF) and molecular trajectory. It was found that COF-102, COF-300, ZnMOF-74, Zn-DOBDC and PCN-60 are good candidates for phosgene adsorption, which would be implemented in environment governance for capture of phosgene.

Key words: Phosgene, Micro-porous material, Molecular simulation, Adsorption ability, Coefficient of diffusion

中图分类号:

O647
O552

TrendMD:

陈晓锋, 宁贺佳, 杨犁, 彭昌军, 孙炜. 分子模拟研究微孔材料对光气吸附扩散性能的影响及材料筛选. 高等学校化学学报, 2019, 40(2): 317.

CHEN Xiaofeng,NING Hejia,YANG Li,PENG Changjun,SUN Wei. Molecular Simulation Study on Influence and Screening of Micro-porous Materials for Phosgene Adsorption and Diffusion^†. Chem. J. Chinese Universities, 2019, 40(2): 317.

图/表 6

Fig.1 Adsorption isotherms COCl2 of in COFs and MOFs at 298 K(solid line), 320 K(dash line) and 350 K(dash point line)

Fig.2 Diffusion of COCl2 in COFs and MOFs with concentration changes

Fig.3 Atom distance as a function of time for COCl2 in IRMOF-16(A, B) and RDF curve(C)(A) Low concentration; (B) high concentration.

Fig.4 Atom distance as a function of time for COCl2 in COF-103(A, B) and RDF curve(C)(A) Low concentration; (B) high concentration.

Fig.5 Adsorption density diagrams(A—C) and snapshot of MD simulation(D—F) for COCl2 in IRMOF-16(A)—(C) From high density to low density; (D)—(F) from low concentration to high concentration.

Fig.6 Adsorption density diagrams(A—C) and snapshot of MD simulation(D—F) for COCl2 in COF-103(A)—(C) From high density to low density; (D)—(F) from low concentration to high concentration.

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分子模拟研究微孔材料对光气吸附扩散性能的影响及材料筛选

Molecular Simulation Study on Influence and Screening of Micro-porous Materials for Phosgene Adsorption and Diffusion^†

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分子模拟研究微孔材料对光气吸附扩散性能的影响及材料筛选

Molecular Simulation Study on Influence and Screening of Micro-porous Materials for Phosgene Adsorption and Diffusion†

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Molecular Simulation Study on Influence and Screening of Micro-porous Materials for Phosgene Adsorption and Diffusion^†