沸石类咪唑骨架材料吸附分离天然气的分子模拟

郭海超; 施帆; 马正飞; 周之雯; 周怡然

doi:10.7498/aps.62.176802

摘要

采用巨正则蒙特卡洛方法研究C2H6, CO2和CH4三种气体在两种沸石类咪唑骨架材料 (ZIF)-ZIF-2和ZIF-71中的吸附与分离性能. 考察了C2H6, CO2和CH4三种气体在ZIF-2和ZIF-71中的单组分吸附等温线、吸附热; C2H6-CH4, CO2-CH4 与C2H6-CO2等摩尔二元混合物的分离; 以及C2H6-CO2-CH4三元体系的分离性能. 研究结果表明: 低压下不同气体的吸附量大小与其吸附热关系紧密; 而高压下因有限的孔空间, 尺寸较小的气体分子吸附量增长趋向更快; 多组分吸附分离中, 低压下能量效应通常占据主导, ZIF优先吸附作用力较强的组分; 高压下堆积效应影响显著, ZIF会优先吸附尺寸较小的组分. ZIF-2和ZIF-71对这3种二元体系的分离性能良好. 对于三元混合物吸附分离, 在常温下3000-4000kPa范围内, ZIF-2具有良好的天然气净化性能, 可有效地分离出天然气中的C2H6和CO2.

关键词:

Abstract

Grand canonical Monte Carlo simulations were employed to investigate the adsorption and separation of C2H6, CO2 and CH4 on two zeolitic imidazolate frameworks (ZIF-2 and ZIF-71). The adsorption isotherm and isosteric heat of pure gas, the separation performance of C2H6-CH4, CO2-CH4 and C2H6-CO2 binary mixtures and C2H6-CO2-CH4 ternary mixtures on two ZIFs were simulated and discussed. For single component gas adsorption at a low pressure, the adsorption amount depended on isosteric heat; at a high pressure, due to the limited pore volume, ZIFs preferably adsorbed smaller size gas molecules. For gas mixture separation, energetic effect dominated at low pressure, therefore, ZIFs selectively adsorbed gas component with strong interactions; packing effect usually played an important role at high pressures, consequently, smaller size component would be more entropically favorable. Results demonstrated that both ZIF-2 and ZIF-71 were of good separation performance for these three binary mixtures. For the ternary mixture separation, it was found that ZIF-2 cowld effectively separate C2H6 and CO2 from CH4 at 3000-4000 kPa and room temperature.

Keywords:

作者及机构信息

1.
南京工业大学化学化工学院, 材料化学工程国家重点实验室, 南京 210009;

2.
URS Corporation, PO Box 618, South Park, PA, USA.;

3.
National Energy Technology Laboratory, U.S. D.O.E., 626 Cochrans Mill Road, Pittsburgh, PA, USA.;

4.
Navi Health and Environment Technology, Pittsburgh, PA, USA.

Authors and contacts

1.
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemistry and Chemical Engineering, Nanjing University of Technology, Nanjing 210009, China;

2.
URS Corporation, PO Box 618, South Park, PA, USA.;

3.
National Energy Technology Laboratory, U.S. D.O.E., 626 Cochrans Mill Road, Pittsburgh, PA, USA.;

4.
Navi Health and Environment Technology, Pittsburgh, PA, USA.

参考文献

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[48]	Pires J, Bestilleiro M, Pinto M, Gil A 2008 Sep. Purif. Technol. 61 161

施引文献

[1]	U.S. Energy Policy Act of 1992 (EPAct)
[2]	Xiao J T 1997 Chem. Eng. Oil Gas 2 94 (in Chinese) [肖锦堂 1997 石油与天然气化工 2 94]
[3]	Burchell T, Rogers M 2000 SAE Tech. Pa. Ser. 2000-01-2205
[4]	Banerjee R, Phan A, Wang B, Knobler C, Furukawa H, O’Keeffe M, Yaghi O M 2008 Science 319 939
[5]	Wang B, Cote A P, Furukawa H, O’Keeffe M, Yaghi O M 2008 Nature 453 207
[6]	Park K S, Ni Z, Cote A P, Choi J Y, Huang R D, Uribe-Romo F J, Chae H K, O’Keeffe M, Yaghi O M 2006 Proc. Nat. Acad. Sci. U.S.A. 103 10186
[7]	Phan A, Doonan C J, Uribe-Romo F J, Knobler C B, O’Keeffe M, Yaghi O M 2010 Acc. Chem. Res. 43 58
[8]	Liu X Y, Li X F, Zhang L Y, Fan Z Q, Ma X K 2012 Acta Phys. Sin. 61 146802-1 (in Chinese) [刘秀英, 李晓凤, 张丽英, 樊志琴, 马兴科 2012 61 146802-1]
[9]	Liu X Y, Wang C Y, Tang Y J, Sun W G, Wu W D, Zhang H Q, Liu M, Yuan L, Xu J J 2009 Acta Phys. Sin. 58 1126 (in Chinese) [刘秀英, 王朝阳, 唐永建, 孙卫国, 吴卫东, 张厚琼, 刘淼, 袁磊, 徐嘉靖 2009 58 1126]
[10]	Li W L, Zhang J P, Guo H C, Gahungu G 2011 J. Phys. Chem. C 115 4935
[11]	Dai W, Luo J S, Tang Y J, Wang C Y, Chen S J, Sun W G 2009 Acta Phys. Sin. 58 1890 (in Chinese) [戴伟, 罗江山, 唐永建, 王朝阳, 陈善俊, 孙卫国 2009 58 1890]
[12]	Dai W, Xiao M, Li Z H, Tang Y J 2012 Acta Phys. Sin. 61 016801 (in Chinese) [戴伟, 肖明, 李志浩, 唐永建 2012 61 016801]
[13]	Keskin S 2011 J. Phys. Chem. C 115 800
[14]	Liu B, Smit B 2010 J. Phys. Chem. C 114 8515
[15]	Battisti A, Taioli S, Garberoglio G 2011 Micropor. Mesopor. Mater. 143 46
[16]	Yang Q Y, Zhong C L 2006 J. Phys. Chem. B 110 17776
[17]	Jiang J W, Sandler S I 2006 Langmuir 22 5702
[18]	Babarao R, Tong Y H, Jiang J W 2009 J. Phys. Chem. B 113 9129
[19]	Martin M G, Siepmann J I 1998 J. Phys. Chem. B 102 2569
[20]	Potoff J J, Siepmann J I 2001 AIChE J. 47 1676
[21]	Rappe A K, Casewit C J, Colwell K S, Goddard W A, Skiff W M 1992 J. Am. Chem. Soc. 114 10024
[22]	Atci E, Keskin S 2012 Ind. Eng. Chem. Res. 51 3091
[23]	Guo H C, Shi F, Ma Z F, Liu X Q 2010 J. Phys. Chem. C 114 12158
[24]	Liu D H, Zheng C C, Yang Q Y, Zhong C L 2009 J. Phys. Chem. C 113 5004
[25]	Sirjoosingh A, Alavi S, Woo T K 2010 J. Phys. Chem. C 114 2171
[26]	Gupta A, Chempath S, Sanborn M J, Clark L A, Snurr R Q 2003 Mol. Simul. 29 29
[27]	Lee C, Yang W, Parr R G 1988 Phys. Rev. B 37 785
[28]	Dill J D, Pople J A 1975 J. Chem. Phys. 62 2921
[29]	Francl M M, Pietro W J, Hehre W J, Binkley J S, Gordon M S, DeFrees D J, Pople J A 1982 J. Chem. Phys. 77 3654
[30]	Hay P J, Wadt W R 1982 J. Chem. Phys. 82 299
[31]	Hay P J, Wadt W R 1982 J. Chem. Phys. 82 270
[32]	Wadt W R, Hay P J 1982 J. Chem. Phys. 82 284
[33]	Breneman C M, Wiberg K B 1990 J. Comput. Chem. 11 361
[34]	Snurr R Q, Bell A T, Theodorou D N 1993 J. Phys. Chem. 97 13742
[35]	Duren T, Millange F, Ferey G, Walton K S, Snurr R Q 2007 J. Phys. Chem. C 111 15350
[36]	Morris W, Leung B, Furukawa H, Yaghi O K, He N, Hayashi H, Houndonougbo Y, Asta M, Laird B B, Yaghi O M 2010 J. Am. Chem. Soc. 132 11006
[37]	Frost H, Duren T, Snurr R Q 2006 J. Phys. Chem. B 110 9565
[38]	Gallo M, Glossman-Mitnik D 2009 J. Phys. Chem. C 113 6634
[39]	Keffer D, Davis H T, McCormick A V 1996 J. Phys. Chem. 100 638
[40]	He Y, Zhang Z, Xiang S, Wu H, Fronczek F R, Zhou W, Krishna R, O’Keeffe M, Chen B 2012 Chem. Eur. J. 18 1901
[41]	Pereira P R, Pires J, de Carvalho M B 2001 Sep. Purif. Technol. 21 237
[42]	Magnowski N B K, Avila A M, Lin C C H, Shi M, Kuznicki S M 2011 Chem. Eng. Sci. 66 1697
[43]	Martin-Calvo A, Garcia-Perez E, Castillo J M, Calero S 2008 Phys. Chem. Chem. Phys. 10 7085
[44]	Yang Q Y, Zhong C L 2006 Chem. Phys. Chem. 7 1417
[45]	Bastin L, Barcia P S, Hurtado E J, Silva J A C, Rodrigues A E, Chen B L 2008 J. Phys. Chem. C 112 1575
[46]	Babarao R, Jiang J W 2009 Energy Environ. Sci. 2 1088
[47]	Bae Y S, Farha O K, Spokoyny A M, Mirkin C A, Hupp J T, Snurr R Q 2008 Chem. Commun. 4135
[48]	Pires J, Bestilleiro M, Pinto M, Gil A 2008 Sep. Purif. Technol. 61 161

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