具有缺陷孔结构的炭膜分离CO2/CH4混合气的分子模拟

doi:10.11949/j.issn.0438-1157.20161790

化工学报 ›› 2017, Vol. 68 ›› Issue (8): 3100-3108.DOI: 10.11949/j.issn.0438-1157.20161790

具有缺陷孔结构的炭膜分离CO₂/CH₄混合气的分子模拟

何流¹, 赵昊瀚², 李花¹, 周子瑞¹, 王同华¹, 潘艳秋¹

1 大连理工大学化工学院, 辽宁大连 116024;
2 沈阳铝镁设计研究院有限公司, 辽宁沈阳 110001

收稿日期:2016-12-22 修回日期:2017-03-28 出版日期:2017-08-05 发布日期:2017-08-05
通讯作者: 潘艳秋
基金资助:
国家自然科学基金面上与重点项目（21176036，21376037）；国家高技术研究发展计划项目（Z2012AA03A611）。

Molecular simulation on separation of CO₂/CH₄ gas mixture in carbon membranes with defect pore structure

HE Liu¹, ZHAO Haohan², LI Hua¹, ZHOU Zirui¹, WANG Tonghua¹, PAN Yanqiu¹

1 School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China;
2 Shenyang Aluminum and Magnesium Engineering and Research Institute Company Limited, Shenyang 110001, Liaoning, China

Received:2016-12-22 Revised:2017-03-28 Online:2017-08-05 Published:2017-08-05
Supported by:
supported by the National Natural Science Foundation of China (21176036, 21376037) and the National High Technology Research and Development Program of China (Z2012AA03A611).

摘要/Abstract

摘要：

基于炭膜无缺陷Z字形孔模型研究结果，建立随机缺陷、均匀缺陷与局部缺陷3种不同缺陷方式的炭膜微孔模型，研究等摩尔CO₂/CH₄混合气在缺陷膜孔中的吸附和扩散过程，探讨缺陷对炭膜气体分离的影响。结果表明，在273~348 K的温度范围内，CO₂与CH₄在缺陷炭膜孔模型内的平衡吸附量与扩散系数均低于无缺陷炭膜孔模型；与无缺陷、均匀缺陷和随机缺陷孔模型相比，局部缺陷孔模型的CO₂/CH₄总分离系数最低；温度低于298 K时，随机缺陷和均匀缺陷孔模型的总分离系数均大于无缺陷孔模型；随机缺陷孔模型的总分离系数大于均匀缺陷孔模型，说明随机删除碳原子的方式比均匀删除和局部删除更加合理。研究结果可为炭膜气体渗透机理的深入研究提供依据。

关键词: 分子模拟, 二氧化碳, 甲烷, 炭膜, 缺陷孔模型

Abstract:

Three kinds of defect micropore models, i.e., random defect, averaged defect and partial defect models, were established based on the defect-free zigzag pore model in carbon membrane. Adsorption and diffusion behaviors of equimolar CO₂/CH₄ gas mixture within pores of carbon membrane were investigated in an effort to discuss the influences of pore defect in carbon membranes on gas separation. Results showed that under the operating temperatures ranging from 273 to 348 K, both equilibrium adsorption capacities and diffusion coefficients of CO₂ and CH₄ in the defect pore models were smaller than those of the defect-free pore model. Total CO₂/CH₄ separation coefficient of the partial defect pore model was relatively low compared with the defect-free pore model and the other two defect pore models. When the temperature was less than 298 K, total separation coefficients of the random defect and averaged defect pore models were greater than the defect-free pore model, and the total separation coefficients of random defect pore model are beneficial to the averaged defect pore model. Random carbon atom deletion approach is more reasonable than average deletion and partial deletion. The results could provide a basis for the further study of gas permeation mechanism in carbon membranes.

Key words: molecular simulation, carbon dioxide, methane, carbon membranes, defect pore model

中图分类号:

TQ028.1

何流, 赵昊瀚, 李花, 周子瑞, 王同华, 潘艳秋. 具有缺陷孔结构的炭膜分离CO₂/CH₄混合气的分子模拟[J]. 化工学报, 2017, 68(8): 3100-3108.

HE Liu, ZHAO Haohan, LI Hua, ZHOU Zirui, WANG Tonghua, PAN Yanqiu. Molecular simulation on separation of CO₂/CH₄ gas mixture in carbon membranes with defect pore structure[J]. CIESC Journal, 2017, 68(8): 3100-3108.

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具有缺陷孔结构的炭膜分离CO₂/CH₄混合气的分子模拟

Molecular simulation on separation of CO₂/CH₄ gas mixture in carbon membranes with defect pore structure

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