不同管径碳纳米管中CO2/CH4分离的分子模拟

doi:10.3969/j.issn.0438-1157.2014.05.025

化工学报

不同管径碳纳米管中CO₂/CH₄分离的分子模拟

曹伟¹, 吕玲红¹, 黄亮亮², 王珊珊¹, 朱育丹¹

1 南京工业大学材料化学工程国家重点实验室, 江苏南京 210009;
2 Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, NC 27695-7905, USA

收稿日期:2014-01-02 修回日期:2014-03-17 出版日期:2014-05-05 发布日期:2014-05-05
通讯作者: 吕玲红
基金资助:
国家重点基础研究发展计划项目（2013CB733501）；国家自然科学基金项目（ 21176113，21136004，21206070，91334202）；江苏高校优势学科建设工程项目。

Molecular simulations on diameter effect of carbon nanotube for separation of CO₂/CH₄

CAO Wei¹, LÜ Linghong¹, HUANG Liangliang², WANG Shanshan¹, ZHU Yudan¹

1 State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, Jiangsu, China;
2 Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, NC 27695-7905, USA

Received:2014-01-02 Revised:2014-03-17 Online:2014-05-05 Published:2014-05-05
Supported by:
supported by the National Basic Research Program of China (2013CB733501), the National Natural Science Foundation of China(21176113, 21136004, 21206070, 91334202) and the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).

摘要/Abstract

摘要： 生物甲烷路线在CO₂减排和节能方面有很大的应用前景。而对生物沼气的分离是此路线的一个关键问题，特别是在60℃和0.1 MPa下。巨正则Monte Carlo（GCMC）和平衡分子动力学（EMD）的分子模拟方法研究CO₂和CH₄在不同管径的碳纳米管（CNT）中的吸附和扩散，可以从分子层面研究生物沼气的分离机理。分别计算了CO₂/CH₄二元混合物吸附量、吸附选择性、自扩散系数和渗透选择性等参数。模拟结果表明：由于碳管的受限空间和CO₂与碳纳米管壁面分子之间强相互作用，导致二元等物质的量的混合物CO₂/CH₄的吸附量和扩散系数的差异。CO₂的吸附量和自扩散系数都比CH₄的大。渗透选择性在碳管管径达到最接近1 nm时达到最大值，此时混合物的分离过程是吸附控制，而非扩散控制。

关键词: 分子模拟, 碳纳米管, 生物沼气, 分离, 自扩散, 选择性

Abstract: Biomethane route has large potential in emission reduction and energy saving. One of the key issues is separation of biogas in operating conditions of 333 K and 0.1 MPa. Grand canonical Monte Carlo (GCMC) and equilibrium molecular dynamics simulations (EMD) were used to compute adsorption loadings and self-diffusivities of CH₄/CO₂ at various diameters of carbon nanotube (CNT) bundles. Single component and equimolar gases were simulated. CO₂ always had larger adsorption loading and diffusion coefficient than CH₄ as the result of relatively strong interaction between CO₂ molecules and tube walls, due to the confined capacity. The permselectivity reached a maximum in closely 1 nm, and under such conditions the separation process was controlled by adsorption rather than diffusion.

Key words: molecular simulation, carbon nanotube, biogas, separation, self-diffusion, selectivity

中图分类号:

TQ015.9

曹伟, 吕玲红, 黄亮亮, 王珊珊, 朱育丹. 不同管径碳纳米管中CO₂/CH₄分离的分子模拟[J]. 化工学报, DOI: 10.3969/j.issn.0438-1157.2014.05.025.

CAO Wei, LÜ Linghong, HUANG Liangliang, WANG Shanshan, ZHU Yudan. Molecular simulations on diameter effect of carbon nanotube for separation of CO₂/CH₄[J]. CIESC Journal, DOI: 10.3969/j.issn.0438-1157.2014.05.025.

参考文献 27

[1]	Liu Chang(刘畅), Lu Xiaohua(陆小华). Carbon reduction pattern in China:comparison of CCS and biomethane route [J]. CIESC Journal(化工学报), 2013, 64(1): 7-10
[2]	Luo G, Angelidaki I. Co-digestion of manure and whey for in situ biogas upgrading by the addition of H2: process performance and microbial insights [J]. Applied Microbiology and Biotechnology, 2013, 97: 1373-1381
[3]	Weiland P. Biogas production: current state and perspectives [J]. Applied Microbiology and Biotechnology, 2010, 85: 849-860
[4]	Yang H, Xu Z, Fan M, Gupta R, Slimane R B, Bland A E, Wright I. Progress in carbon dioxide separation and capture: a review [J]. Journal of Environmental Sciences, 2008, 20: 14-27
[5]	Freeman B D. Basis of permeability/selectivity tradeoff relations in polymeric gas separation membranes [J]. Macromolecules, 1999, 32: 375-380
[6]	Iijima S. Helical microtubules of graphitic carbon [J]. Nature, 1991, 354: 56-58
[7]	Krishna R, van Baten J M. Using molecular simulations for screening of zeolites for separation of CO2/CH4 mixtures [J]. Chemical Engineering Journal, 2007, 133: 121-131
[8]	Babarao R, Hu Z, Jiang J, Chempath S, Sandler S I. Storage and separation of CO2 and CH4 in silicalite, C168 schwarzite, and IRMOF(Ⅰ): A comparative study from Monte Carlo simulation [J]. Langmuir, 2007, 23: 659-666
[9]	Chen H, Sholl D S. Rapid diffusion of CH4/H2 mixtures in single-walled carbon nanotubes [J]. Journal of the American Chemical Society, 2004, 126: 7778-7779
[10]	Hicks J M, Desgranges C, Delhommelle J. Characterization and comparison of the performance of IRMOF-1, IRMOF-8, and IRMOF-10 for CO2 adsorption in the subcritical and supercritical regimes [J]. The Journal of Physical Chemistry C, 2012, 116: 22938-22946
[11]	Huang L, Zhang L, Shao Q, Lu L, Lu X, Jiang S, Shen W. Simulations of binary mixture adsorption of carbon dioxide and methane in carbon nanotubes: temperature, pressure, and pore size effects [J]. The Journal of Physical Chemistry C, 2007, 111: 11912-11920
[12]	Lu L, Wang S, Müller E A, Cao W, Zhu Y, Lu X, Jackson G. Adsorption and separation of CO2/CH4 mixtures using nanoporous adsorbents by molecular simulation [J]. Fluid Phase Equilibria, 2014, 362: 227-234
[13]	Holt J K, Park H G, Wang Y, Stadermann M, Artyukhin A B, Grigoropoulos C P, Noy A, Bakajin O. Fast mass transport through sub 2 nanometer carbon nanotubes [J]. Science, 2006, 312: 1034-1037
[14]	Ban S, Huang C. Molecular simulation of CO2/N2 separation using vertically-aligned carbon nanotube membranes [J]. Journal of Membrane Science, 2012, 417: 113-118
[15]	Wang J, Zhu Y, Zhou J, Lu X H. Diameter and helicity effects on static properties of water molecules confined in carbon nanotubes [J]. Physical Chemistry Chemical Physics, 2004, 6: 829-835
[16]	Huang L, Zhang L, Shao Q, Wang J, Lu L, Lu X, Jiang S, Shen W. Molecular dynamics simulation study of the structural characteristics of water molecules confined in functionalized carbon nanotubes [J]. The Journal of Physical Chemistry B, 2006, 110: 25761-25768
[17]	Zhou J, Lu X, Wang Y, Shi J. Molecular dynamics study on ionic hydration [J]. Fluid Phase Equilibria, 2002, 194: 257-270
[18]	Shao Q, Zhou J, Lu L, Lu X, Zhu Y, Jiang S. Anomalous hydration shell order of Na+ and K+ inside carbon nanotubes [J]. Nano Letters, 2009, 9: 989-994
[19]	Huang L L, Shao Q, Lu L H, Lu X H, Zhang L Z, Wang J, Jiang S Y. Helicity and temperature effects on static properties of water molecules confined in modified carbon nanotubes [J]. Physical Chemistry Chemical Physics, 2006, 8: 3836-3844
[20]	Journet C, Maser W, Bernier P, Loiseau A, De La Chapelle M L, Lefrant D L S, Deniard P, Lee R, Fischer J. Large-scale production of single-walled carbon nanotubes by the electric-arc technique [J]. Nature, 1997, 388: 756-758
[21]	Thess A, Lee R, Nikolaev P, Dai H, Petit P, Robert J, Xu C, Lee Y H, Kim S G, Rinzler A G. Crystalline ropes of metallic carbon nanotubes [J]. Science-AAAS-Weekly Paper Edition, 1996, 273: 483-487
[22]	Jiang J, Sandler S I. Monte Carlo simulation for the adsorption and separation of linear and branched alkanes in IRMOF-1 [J]. Langmuir, 2006, 22: 5702-5707
[23]	Do D, Do H, Wongkoblap A, Nicholson D. Henry constant and isosteric heat at zero-loading for gas adsorption in carbon nanotubes [J]. Physical Chemistry Chemical Physics, 2008, 10: 7293-7303
[24]	Plimpton S. Fast parallel algorithms for short-range molecular dynamics [J]. Journal of Computational Physics, 1995, 117: 1-19
[25]	Ryckaert J-P, Ciccotti G, Berendsen H J. Numerical integration of the Cartesian equations of motion of a system with constraints: molecular dynamics of n-alkanes [J]. Journal of Computational Physics, 1977, 23: 327-341
[26]	Harris J G, Yung K H. Carbon dioxide's liquid-vapor coexistence curve and critical properties as predicted by a simple molecular model [J]. The Journal of Physical Chemistry, 1995, 99: 12021-12024
[27]	Keskin S. Adsorption, diffusion, and separation of CH4/H2 mixtures in covalent organic frameworks: molecular simulations and theoretical predictions [J]. The Journal of Physical Chemistry C, 2012, 116: 1772-1779

不同管径碳纳米管中CO₂/CH₄分离的分子模拟

Molecular simulations on diameter effect of carbon nanotube for separation of CO₂/CH₄

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