石墨烯/纳米管复合结构吸附分离CO2/CH4混合物的分子模拟

doi:10.3866/PKU.WHXB201501291

物理化学学报 >> 2015, Vol. 31 >> Issue (4): 660-666.doi: 10.3866/PKU.WHXB201501291

石墨烯/纳米管复合结构吸附分离CO₂/CH₄混合物的分子模拟

雷广平, 刘朝, 解辉

重庆大学低品位能源利用技术及系统教育部重点实验室, 重庆400030

收稿日期:2014-09-24 修回日期:2015-01-28 发布日期:2015-04-03
通讯作者: 刘朝 E-mail:liuchao@cqu.edu.cn
基金资助:
国家自然科学基金(51206195)资助项目

Molecular Simulation of Adsorption and Separation Performances for CO₂/CH₄ Mixtures in Graphene/Nanotube Hybrid Structures

LEI Guang-Ping, LIU Chao, XIE Hui

Key Laboratory of Low-Grade Energy Utilization Technologies and Systems of Ministry of Education, Chongqing University, Chongqing 400030, P. R. China

Received:2014-09-24 Revised:2015-01-28 Published:2015-04-03
Contact: LIU Chao E-mail:liuchao@cqu.edu.cn
Supported by:
The project was supported by the National Natural Science Foundation of China (51206195).

摘要/Abstract

摘要：

采用巨正则蒙特卡洛(GCMC)及分子动力学(MD)方法探讨了石墨烯/碳纳米管三维骨架结构(GNHS)对等摩尔CO₂/CH₄二元混合物的吸附分离性能. 模拟结果表明CO₂比CH₄更易吸附于GNHS中, GNHS与(6, 6)SWCNT (单壁碳纳米管)相比具有更高的分离性能. 随着温度升高, CO₂的吸附量快速降低, 而CH₄的吸附量则呈现出先升高后降低的趋势. 最后采用分子动力学方法计算了CO₂与CH₄的自扩散系数及停留时间等动力学相关参数, 发现CO₂在GNHS内扩散的阻力更大. 而各组分在吸附剂外部吸附层内的扩散过程对混合物的分离也存在一定影响.

关键词: 石墨烯/碳纳米管三维骨架结构, 吸附等温线, 停留时间, 吸附选择性, 吸附系数

Abstract:

The adsorption and separation behaviors of CO₂ and CH₄ binary mixture in graphene/nanotube hybrid structures (GNHSs) are investigated by grand canonical Monte Carlo (GCMC) combined with molecular dynamics (MD) simulations. CO₂ is preferentially adsorbed in the adsorbents. Compared with a (6, 6) SWCNT (single walled carbon nanotube), GNHSs show improved separation performance. As the temperature rises, the loading of CO₂ reduces rapidly while the loading of CH₄ first increases before being reduced. Finally, the kinetic parameters of CO₂ and CH₄, such as self-diffusivity and residence time, are calculated by MD simulation. The CO₂ molecules diffusing in the GNHS need to overcome a higher barrier relative to that for CH₄. The diffusion of the two components in the adsorption layer outside of adsorbent also influences the separation of the mixture.

Key words: Graphene/nanotube hybrid structure, Adsorption isotherm, Residence time, Adsorption selectivity, Adsorption coefficient

雷广平, 刘朝, 解辉. 石墨烯/纳米管复合结构吸附分离CO₂/CH₄混合物的分子模拟[J]. 物理化学学报, 2015, 31(4): 660-666.

LEI Guang-Ping, LIU Chao, XIE Hui. Molecular Simulation of Adsorption and Separation Performances for CO₂/CH₄ Mixtures in Graphene/Nanotube Hybrid Structures[J]. Acta Phys. -Chim. Sin., 2015, 31(4): 660-666.

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201501291

https://www.whxb.pku.edu.cn/CN/Y2015/V31/I4/660

参考文献

(1) Peng, X.; Cao, D. P. AIChE Journal 2013, 59, 2928. doi: 10.1002/aic.v59.8
(2) Zhang, J. H.; Shen, B. X.; Sun, H.; Liu, J. C. Petroleum Science and Technology 2011, 29, 48. doi: 10.1080/10916460903330221
(3) Krischan, J.; Makaruk, A.; Harasek, M. Journal of Hazardous Materials 2012, 215 -216, 49.
(4) Ma, Y. H.; Zhao, H. L.; Tang, S. J.; Hu, J.; Liu, H. L. Acta Phys. -Chim. Sin. 2011, 27, 689. [马燕辉, 赵会玲, 唐圣杰, 胡军, 刘洪来. 物理化学学报, 2011, 27, 689.] doi: 10.3866/PKU.WHXB20110335
(5) Cosoli, P.; Ferrone, M.; Pricl, S.; Fermeglia, M. Chemical Engineering Journal 2008, 145, 93. doi: 10.1016/j.cej.2008.08.013
(6) Chen, S. J.; Dai, W.; Luo, J. S.; Tang, Y. J.; Wang, C. Y.; Sun, W. G. Acta Phys. -Chim. Sin. 2009, 25, 285. [陈善俊, 戴伟, 罗江山, 唐永建, 王朝阳, 孙卫国. 物理化学学报, 2009, 25, 285.] doi: 10.3866/PKU.WHXB2009021
(7) Wu, X. J.; Zheng, J.; Li, J.; Cai, W. Q. Acta Phys. -Chim. Sin. 2013, 29, 2207. [吴选军, 郑佶, 李江, 蔡卫权. 物理化学学报, 2013, 29, 2207.] doi: 10.3866/PKU.WHXB201307191
(8) An, X. H, ; Liu, D. H.; Zhong, C. L. Acta Phys. -Chim. Sin. 2011, 27, 553. [安晓辉, 刘大欢, 仲崇立. 物理化学学报, 2011, 27, 553.] doi: 10.3866/PKU.WHXB20110319
(9) Feng, W.; Kwon, S.; Borguet, E.; Vidic, R. Environmental Science Technology 2005, 39, 9744. doi: 10.1021/es0507158
10) Arab, M.; Picaud, F.; Devel, M.; Ramseyer, C.; Girardet, C. Physical Review B 2004, 69, 165401. doi: 10.1103/PhysRevB.69.165401
(11) Huang, L.; Zhang, L.; Shao, Q.; Lu, L.; Lu, X.; Jiang, S.; Shen, W. The Journal of Physical Chemistry C 2007, 111, 11912. doi: 10.1021/jp067226u
(12) Jiang, J.; Sandler, S. I. Physical Review B 2003, 68, 245412. doi: 10.1103/PhysRevB.68.245412
(13) Liu, L.; Bhatia, S. K. The Journal of Physical Chemistry C 2013, 117, 13479. doi: 10.1021/jp403477y
(14) Razavi, S. S.; Hashemianzadeh, S. M.; Karimi, H. J. Mol. Model. 2011, 17, 1163. doi: 10.1007/s00894-010-0810-9
(15) Liu, X. Q.; Tian, Z. Y.; Chu, W.; Xue, Y. Acta Phys. -Chim. Sin. 2014, 30, 251. [刘晓强, 田之悦, 储伟, 薛英. 物理化学学报, 2014, 30, 251.] doi: 10.3866/PKU.WHXB201312243
(16) Ye, Q.; Zhang, Y.; Li, M.; Shi, Y. Acta Phys. -Chim. Sin. 2012, 28, 1223. [叶青, 张瑜, 李茗, 施耀. 物理化学学报, 2012, 28, 1223.] doi: 10.3866/PKU.WHXB201202234
(17) Lei, G. P.; Liu, C.; Xie, H. Journal of Engineering Thermophysics 2014, 35, 428. [雷广平, 刘朝, 解辉. 工程热物理学报, 2014, 35, 428.]
(18) Bittolo, B.; Valentini, L.; Kenny, J. M. Physica Status Solidi (a) 2010, 207, 2461. doi: 10.1002/pssa.v207:11
(19) Cai, D.; Song, M.; Xu, C. Advanced Materials 2008, 20, 1706.
(20) Zhu, X.; Ning, G.; Fan, Z. Carbon 2012, 50, 2764. doi: 10.1016/j.carbon.2012.02.037
(21) Xu, L.; Wei, N.; Zheng, Y. Journal of Materials Chemistry 2012, 22, 1435. doi: 10.1039/c1jm13799a
(22) Novaes, F. D.; Rurali, R.; Ordejon, P. ACS Nano 2010, 4, 7596. doi: 10.1021/nn102206n
(23) Dimitrakakis, G. K.; Tylianakis, E.; Froudakis, G. E. Nano Letters 2008, 8, 3166. doi: 10.1021/nl801417w
(24) Wu, C.; Fang, T.; Lo, J. International Journal of Hydrogen Energy 2012, 37, 14211. doi: 10.1016/j.ijhydene.2012.07.040
(25) Weso?owski, R. P.; Terzyk, A. P. Physical Chemistry Chemical Physics 2011, 13, 17027. doi: 10.1039/c1cp21590f
(26) Liu, L.; Nicholson, D.; Bhatia, S. K. Chemical Engineering Science 2015, 121, 268. doi: 10.1016/j.ces.2014.07.041
(27) Gupta, A.; Chempath, S.; Sanborn, M. J.; Clark, L. A.; Snurr, R. Q. Molecular Simulation 2003, 29, 29. doi: 10.1080/0892702031000065719
(28) Frenkel, S. Understanding Molecular Mimulation —from Algorithms to Applications; Chemical Industry Press: Beijing, 2002; pp 112-113; translated byWang, W. C. [Frenkel, S. 分子模拟—从算法到应用. 汪文川译. 北京: 化学工业出版社, 2002: 112-113.]
(29) Skarmoutsos, I.; Tamiolakis, G.; Froudakis, G. E. The Journal of Physical Chemistry C 2013, 117, 19373.
(30) Simon, J. M.; Bellat, J. P.; Salazar, J. M. Molecular Simulation 2014, 40, 52. doi: 10.1080/08927022.2013.845332

[1]	邢建东,敬方梨,储伟,孙红丽,喻磊,张欢,罗仕忠. CeO₂对CuCl/活性炭吸附剂C₂H₄/C₂H₆吸附分离性能促进作用[J]. 物理化学学报, 2015, 31(11): 2158 -2164 .
[2]	王朝阳, 李钢, 孙志国. 磺酸功能化金属-有机骨架吸附脱氮性能[J]. 物理化学学报, 2013, 29(11): 2422 -2428 .
[3]	彭璇, 张勤学, 成璇, 曹达鹏. 二氧化碳/甲烷/氮气二元混合物在有序介孔碳材料CMK-3 中的吸附和分离[J]. 物理化学学报, 2011, 27(09): 2065 -2071 .
[4]	高萌, 姚新秋, 佘振苏, 刘志荣, 朱怀球. 蛋白折叠中的暂态结构与表面水分子慢尺度动力学[J]. 物理化学学报, 2010, 26(07): 1998 -2006 .
[5]	张翔, 马聪聪, 张学军, 邵晓红, 曹达鹏. 空气中微量1,1,1,2-四氟乙烷吸附分离的分子模拟[J]. 物理化学学报, 2010, 26(06): 1637 -1642 .
[6]	吴健, 王瑜, 黄峰, 杨阳, 孟长功. ZSM-5晶体内SnO₂团簇的热扩散法合成及表征[J]. 物理化学学报, 2010, 26(06): 1705 -1710 .
[7]	陈善俊;戴伟;罗江山;唐永建;王朝阳;孙卫国. 甲烷在AFS型分子筛中的吸附模拟[J]. 物理化学学报, 2009, 25(02): 285 -290 .
[8]	岳巧红;邵晓红;曹达鹏. 高比表面活性碳微球分离H₂中少量CO₂[J]. 物理化学学报, 2007, 23(07): 1080 -1084 .
[9]	关莉莉;段连运;谢有畅. Li^＋交换的几种分子筛的氮氩分离性能[J]. 物理化学学报, 2004, 20(07): 684 -689 .
[10]	关莉莉;段连运;谢有畅. Ca^2＋交换的几种分子筛的氮氩分离性能[J]. 物理化学学报, 2002, 18(11): 998 -1004 .
[11]	戴闽光,缪蕊平. 二组分气体在固体上吸附的研究(IV)[J]. 物理化学学报, 1995, 11(07): 596 -600 .
[12]	刘朝纲. 气相色谱法测定气固表面的吸附停留时间[J]. 物理化学学报, 1993, 9(04): 489 -494 .
[13]	欧锦如;郁蕴璐;林炳承;林炳昌. 非线性色谱保留时间与进样量关系的实验分析[J]. 物理化学学报, 1993, 9(01): 111 -116 .

石墨烯/纳米管复合结构吸附分离CO₂/CH₄混合物的分子模拟

Molecular Simulation of Adsorption and Separation Performances for CO₂/CH₄ Mixtures in Graphene/Nanotube Hybrid Structures

PDF

赞

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 13

Metrics

推荐阅读 0