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Molecular dynamics (MD) simulation is used to study the microscopic mechanism of CO2 separation from integrated gasification combined cycle(IGCC) syngas (CO2/H2) via the hydrate formation. The stable structures and microscopic properties of CO2 hydrate, H2 hydrate, and CO2/H2 hydrate from one stage separation for IGCC syngas are investigated systematically. The binding energy for loading the hydrate structure with the guest molecules, ΔEn, was analyzed. It was shown that the binding between CO2 and water is more stable than that between H2 and water. That is, CO2 can more easily form the hydrate. Therefore, CO2 in the CO2/H2 gas mixture more easily transfers into the hydrate phase. Based on this, CO2 can be separated from the IGCC syngas. The binding energy for loading the single cavity with the guest molecules, ΔEGH, was analyzed. It was found that the gas mixture can form structure Ⅰ(SⅠ) hydrate, in which CO2 molecules preferably occupy the big cavity and then occupy the small cavity, and H2 molecules only occupy the small cavity. The simulation was carried out at pressure of 85 MPa and temperature of 2737 K for the stable structure of the CO2/H2 hydrate in one stage separation for IGCC syngas. From the ΔEn and ΔEGH of the systems with H2 single and double occupancy in the small cavity, it is concluded that the configurations with the single occupancy is most stable. The stable structure of the hydrate in one stage separation is attained by MD. It provides a theoretical evidence of CO2 separation for formation hydrate in IGCC syngas.
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Keywords:
- separation by forming hydrate /
- molecular dynamics simulation /
- integrated gasification combined cycle syngas /
- CO2 separation
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[37] ］Zhang L, Wang Q, Liu Y 2007 J. Phys. Chem. B 111 4291
[38] ］Babarao R, Jiang J W 2008 Langmuir 24 6270
[39] ］Ota M, Ferdows M 2005 JSME Int. J. 48 802
[40] ］Van Klaveren E P, Michels J P J, Schouten J A 2001 J. Chem. Phys. 115 10500
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[1] ［1］Perinline H W, Luebke D R, Jones K L, Myers C R, Morsi B I, Heintz Y J, Ilconich J B 2008 Fuel. Process. Technol. 89 897
[2] ［2］Aaron D, Tsouris C 2005 Sep. Sci. Technol. 40 321
[3] ［3］Ishida M, Zheng D, Akehata T 1987 Energy 12 147
[4] ［4］Winnick J, Toghiani H, Quattrone P 1982 AICHE J. 28 103
[5] ［5］Linga P, Kumar R, Englezos P 2007 J. Hazard. Mater. 149 625
[6] ［6］Glew D N 1966 U. S. Patent 3231630
[7] ［7］Elliot D G, Chen J J 1977 U. S. Patent 5660603
[8] ［8］Happel J, Hnatow M A, Meyer H 1994 Ann. N. Y. Acad. Sci. 715 412
[9] ［9］Kang S P, Lee H, Lee C S, Sung W M 2001 Fluid Phase Equilib. 185 101
[10] ］Park J, Seo Y T, Lee J W, Lee H 2006 Catal. Today. 115 279
[11] ］Ma C F, Chen G J, Zhang S X, Wang F, Guo T M 2001 J. Chem. Ind. Eng. 52 1113 (in Chinese) ［马昌峰、陈光进、张世喜、王峰、郭天民 2001 化工学报 52 1113］
[12] ］Zhang S X, Chen G J, Guo T M 2004 J. Univ. Petrol. 28 95 (in Chinese) ［张世喜、陈光进、郭天民 2004 石油大学学报 28 95］
[13] ］Li D L, Du J W, Fan S S, Liang D Q, Li X S, Huang N S 2007 J. Chem. Eng. Data 52 1916
[14] ］Li X S, Lu T, Chen Z Y, Yan K F, Li G 2009 Mod. Chem. Ind. 29(10) 37 (in Chinese)［李小森、鲁涛、陈朝阳、颜克凤、李刚 2009 现代化工 29(10) 37］
[15] ］Zhu C Z, Zhang P X, Xu Q M, Liu J H, Ren X Z, Zhang Q L, Hong W L, Li L L 2006 Acta Phys. Sin. 55 4795 (in Chinese) ［朱才镇、张培新、许启明、刘剑洪、任祥忠、张黔玲、洪伟良、李琳琳 2006 55 4795］
[16] ］Geng C Y, Wang C Y, Zhu T 2005 Acta Phys. Sin. 54 1320(in Chinese) ［耿翠玉、王崇愚、朱弢 2005 54 1320］
[17] ］Chen M J, Liang Y C, Li H Z, Li D 2006 Chin. Phys. 15 2087
[18] ］Alavi S, Ripmeester J A, Klug D D 2005 J. Chem. Phys. 123 024507
[19] ］Geng C Y, Wen H, Zhou H 2009 J. Phys. Chem. A 113 5463
[20] ］Chialvo A A, Houssa M, Cummings P T 2002 J. Phys. Chem. B 106 442
[21] ］Mao W L, Mao H K, Goncharov A F, Struzhkin V V, Guo Q Z, Hu J Z, Shu J F, Hemley R J, Somayazulu M, Zhao Y S 2002 Science 297 2247
[22] ］Storr M T, Taylor P C, Monfort J P, Eodger P M 2004 J. Am. Chem. Soc. 126 1569
[23] ］Yan K F, Li X S, Chen Z Y, Li G, Tang L G, Fan S S 2007 Acta Phys. Sin. 56 4994 (in Chinese) ［颜克凤、李小森、陈朝阳、李刚、唐良广、樊栓狮 2007 56 4994］
[24] ］Kirchner M T, Boese R, Billups W E, Norman L R 2004 J. Am. Chem. Soc. 126 9407
[25] ］Smith W, Yong C W, Rodger P M 2002 Mol. Simul. 28 385
[26] ］Berendsen H J C, Postma J P M, van Gunsteren W F, Hermans J 1981 In Intermolecular Forces: Proceedings of the Fourteenth Jerusalem Symposium on Quantum Chemistry and Biochemistry (Dordrecht: D. Reidel Publishing Co.) p331
[27] ］Bernal J D, Fowler R H 1933 J. Chem. Phys. 1 515
[28] ］Dauber O P, Roberts V A, Osguthorpe D J, Wolff J, Genest M, Hagler A T 1988 Proteins: Struct. Funct. Genet. 4 31
[29] ］Ewald P P 1921 Ann. Phys. 64 253
[30] ］Allen M P, Tildeslay D J 1987 Computer Simulation of Liquids (Oxford: Clarendon Press) p156
[31] ］Nose S A 1984 Mol. Phys. 52 255
[32] ］Chen Z L, Xu W R, Tang L D 2007 Practice and Theory of Molecular Simulation (Beijing: Chemical Industry Press) p4 (in Chinese) ［陈正隆、徐为人、汤立达 2007 分子模拟的理论与实践 (北京: 化学工业出版社) 第4页］
[33] ］Cygan R T, Guggenheim S, van Groos A F K 2004 J. Phys. Chem. B 108 15141
[34] ］Greathouse J A, Cygan R T 2008 The 6th International Conference on Gas Hydrates (Vancouver: British Columbia) p5529
[35] ］Udachin K A, Ratcliffc C I, Ripmeester J A 2001 J. Phys. Chem. B 105 4200
[36] ］Zhou Z E, Xue C Y, Yang Q Y, Zhong C L 2009 Acta Chim. Sin. 67 477 (in Chinese) ［周子娥、薛春瑜、阳庆元、仲崇立 2009 化学学报 67 477］
[37] ］Zhang L, Wang Q, Liu Y 2007 J. Phys. Chem. B 111 4291
[38] ］Babarao R, Jiang J W 2008 Langmuir 24 6270
[39] ］Ota M, Ferdows M 2005 JSME Int. J. 48 802
[40] ］Van Klaveren E P, Michels J P J, Schouten J A 2001 J. Chem. Phys. 115 10500
[41] ］Kim D Y, Lee H 2005 J. Am. Chem. Soc. 127 9996
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