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Adsorption and separation of carbon dioxide and methane in new zeolites using the Grand Canonical Monte Carlo method

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Abstract

The adsorption and separation behaviors of CO2 and CH4 in new siliceous zeolites (IFO, JSR, OKO, SEW) were simulated using the Grand Canonical Monte Carlo method in the paper. The adsorption isotherms for pure components and binary mixtures of CO2 and CH4 in four siliceous zeolites were obtained. The adsorption thermodynamic properties including Gibb’s free energy change, enthalpy change and entropy change were investigated. The results demonstrate that the adsorbed amount of pure components increases with an increase in pressure, and larger pore volume and surface area are beneficial to improve the adsorption capacity. The adsorption amount of CO2 and CH4 in the JSR zeolite is 7.08 and 2.27 mmol g−1 at 1000 kPa, respectively. In view of the thermodynamic results, the new siliceous zeolites show a higher affinity for CO2. The adsorption capacities of CO2 in all zeolites were five times more than those of CH4 in binary mixtures based on the ratios of equilibrium adsorption capacity. Considering the adsorption uptake and selectivity for CO2/CH4, the JSR zeolite is a good candidate for the separation of CO2/CH4 at low pressure.

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References

  • Ackley, M.W., Rege, S.U., Saxena, H.: Application of natural zeolites in the purification and separation of gases. Microporous Mesoporous Mater. 61(3), 25–42 (2003)

    Article  CAS  Google Scholar 

  • Agnihotri, S., Kim, P., Zheng, Y., Mota, J.P.B., Yang, L.: Regioselective competitive adsorption of water and organic vapor mixtures on pristine single-walled carbon nanotube bundles. Langmuir 24(11), 5746–5754 (2008)

    Article  CAS  Google Scholar 

  • Alonso-Vicario, A., Ochoa-Gómez, J.R., Gil-Río, S., Gómez-Jiménez-Aberasturi, O., Ramírez-López, C.A., Torrecilla-Soria, J., Domínguez, A.: Purification and upgrading of biogas by pressure swing adsorption on synthetic and natural zeolites. Microporous Mesoporous Mater. 134(1), 100–107 (2010)

    Article  CAS  Google Scholar 

  • Babarao, R., Hu, Z., Jiang, J., Chempath, S., Sandler, S.I.: Storage and separation of CO2 and CH4 in silicalite, C168 schwarzite, and IRMOF-1: a comparative study from Monte Carlo simulation. Langmuir 23(3), 659–666 (2007)

    Article  CAS  Google Scholar 

  • Bakhtyari, A., Mofarahi, M.: Pure and binary adsorption equilibria of methane and nitrogen on zeolite 5A. J. Chem. Eng. Data 59(3), 626–639 (2014)

    Article  CAS  Google Scholar 

  • Biswas, M.M., Cagin, T.: Simulation studies on hydrogen sorption and its thermodynamics in covalently linked carbon nanotube scaffold. J. Phys. Chem. B 114(43), 13752–13763 (2010)

    Article  CAS  Google Scholar 

  • Catlow, C.R.A., Smit, B., van Santen, R.: Computer Modelling of Microporous Materials. Academic Press, New York (2004)

    Google Scholar 

  • Colabella, J.M., Stall, R.A., Sorenson, C.T.: The adsorption and subsequent oxidation of AsH3 and PH3 on activated carbon. J. Cryst. Growth 92(1–2), 189–195 (1988)

    Article  CAS  Google Scholar 

  • Connolly, M.L.: Computation of molecular volume. J. Am. Chem. Soc. 107(5), 1118–1124 (1985)

    Article  CAS  Google Scholar 

  • Cosoli, P., Ferrone, M., Pricl, S., Fermeglia, M.: Hydrogen sulfide removal from biogas by zeolite adsorption. Part II. MD aimulations. Chem. Eng. J. 145(1), 93–99 (2008a)

    Article  CAS  Google Scholar 

  • Cosoli, P., Ferrone, M., Pricl, S., Fermeglia, M.: Hydrogen sulphide removal from biogas by zeolite adsorption: Part I. GCMC molecular simulations. Chem. Eng. J. 145(1), 86–92 (2008b)

    Article  CAS  Google Scholar 

  • Dubbeldam, D., Torres-Knoop, A., Walton, K.S.: On the inner workings of Monte Carlo codes. Mol. Simul. 39(14–15), 1253–1292 (2013)

    Article  CAS  Google Scholar 

  • Dunne, L.J., Furgani, A., Jalili, S., Manos, G.: Monte-carlo simulations of methane/carbon dioxide and ethane/carbon dioxide mixture adsorption in zeolites and comparison with matrix treatment of statistical mechanical lattice model. Chem. Phys. 359(1–3), 27–30 (2009)

    Article  CAS  Google Scholar 

  • Ebner, A.D., Ritter, J.A.: State-of-the-art adsorption and membrane separation processes for carbon dioxide production from carbon dioxide emitting industries. Sep. Sci. Technol. 44(6), 1273–1421 (2009)

    Article  CAS  Google Scholar 

  • García-Pérez, E., Parra, J.B., Ania, C.O., García-Sánchez, A., van Baten, J.M., Krishna, R., Dubbeldam, D., Calero, S.: A computational study of CO2, N2, and CH4 adsorption in zeolites. Adsorption 13(5–6), 469–476 (2007)

    Article  Google Scholar 

  • Golden, T.C., Sircar, S.: Gas adsorption on silicalite. J. Colloid Interface Sci. 162(1), 182–188 (1994)

    Article  CAS  Google Scholar 

  • Hill, J.R., Sauer, J.: Molecular mechanics potential for silica and zeolite catalysts based on ab initio calculations. 1. Dense and microporous silica. J. Phys. Chem. 98(4), 1238–1244 (1994)

    Article  CAS  Google Scholar 

  • Karasawa, N., Goddard, W.A.: Acceleration of convergence for lattice sums. J. Phys. Chem. 93(21), 7320–7327 (1989)

    Article  CAS  Google Scholar 

  • Kim, K., Lee, S., Ryu, J.H., Lee, K.S., Lee, W.B.: An improved CO2 adsorption efficiency for the zeolites impregnated with the amino group: a molecular simulation approach. Int. J. Greenhouse Gas Control 19(11), 350–357 (2013)

    Article  CAS  Google Scholar 

  • Krishna, R., van Baten, J.M.: Using molecular simulations for screening of zeolites for separation of CO2/CH4 mixtures. Chem. Eng. J. 133(1–3), 121–131 (2007)

    Article  CAS  Google Scholar 

  • Krishna, R., van Baten, J.M., García-Pérez, E., Calero, S.: Diffusion of CH4 and CO2 in MFI, CHA and DDR zeolites. Chem. Phys. Lett. 429(1), 219–224 (2006)

    Article  CAS  Google Scholar 

  • Krishna, R., van Baten, J.M.: Influence of isotherm inflection on the diffusivities of C5–C8 linear alkanes in MFI zeolite. Chem. Phys. Lett. 407(1), 159–165 (2005)

    Article  CAS  Google Scholar 

  • Liu, B., Wu, Y., Liu, D., Wu, Y., Xi, H., Qian, Y.: Molecular simulation and experimental studies of a mesoporous ZSM-5 type molecular sieve. Phys. Chem. Chem. Phys. 15(8), 2741–2748 (2013)

    Article  CAS  Google Scholar 

  • Liu, J., Keskin, S., Sholl, D.S., Johnson, J.K.: Molecular simulations and theoretical predictions for adsorption and diffusion of CH4/H2 and CO2/CH4 mixtures in ZIFs. J. Phys. Chem. C 115(25), 12560–12566 (2011)

    Article  CAS  Google Scholar 

  • Martinez-Franco, R., Moiner, M., Yun, Y., Sun, J., Wan, W., Zou, X., Corma, A.: Synthesis of an extra-large molecular sieve using proton sponges as organic structure-directing agents. Proc. Natl. Acad. Sci. USA 110(10), 3749–3754 (2013)

    Article  CAS  Google Scholar 

  • Metropolis, N., Rosenbluth, A.W., Rosenbluth, M.N., Teller, A.H., Teller, E.: Equation of state calculations by fast computing machines. J. Chem. Phys. 21(6), 1087–1092 (1953)

    Article  CAS  Google Scholar 

  • Mofarahi, M., Gholipour, F.: Gas adsorption aeparation of CO2/CH4 aystem using zeolite 5A. Microporous Mesoporous Mater. 200, 1–10 (2014)

    Article  CAS  Google Scholar 

  • Nugent, P., Belmabkhout, Y., Burd, S.D., Cairns, A.J., Luebke, R., Forrest, K., Pham, T., Ma, S., Space, B., Wojtas, L., Eddaoudi, M., Zaworotko, M.J.: Porous materials with optimal adsorption thermodynamics and kinetics for CO2 separation. Nature 495, 80–84 (2013)

    Article  CAS  Google Scholar 

  • Olajossy, A., Gawdzik, A., Budner, Z., Dula, J.: Methane separation from coal mine methane gas by vacuum pressure swing adsorption. Chem. Eng. Res. Des. 81(4), 474–482 (2003)

    Article  CAS  Google Scholar 

  • Pham, T.D., Xiong, R., Sandler, S.I., Lobo, R.F.: Experimental and computational studies on the adsorption of CO2 and N2 on pure silica zeolites. Microporous Mesoporous Mater. 185, 157–166 (2014)

    Article  CAS  Google Scholar 

  • Rahmati, M., Modarress, H.: Nitrogen adsorption on nanoporous zeolites studied by grand canonical Monte Carlo simulation. J. Mol. Struct. THEOCHEM 901(1–3), 110–116 (2009)

    Article  CAS  Google Scholar 

  • Rahmati, M., Modarress, H., Gooya, R.: Molecular simulation study of polyurethane membranes. Polymer 53(9), 1939–1950 (2012)

    Article  CAS  Google Scholar 

  • Rahmati, M., Modarress, H.: Selectivity of new siliceous zeolites for separation of methane and carbon dioxide by Monte Carlo simulation. Microporous Mesoporous Mater. 176(8), 168–177 (2013)

    Article  CAS  Google Scholar 

  • Rappe, A.K., Goddard, W.A.: Charge equilibration for molecular dynamics simulations. J. Phys. Chem. 95(8), 3358–3363 (1991)

    Article  CAS  Google Scholar 

  • Rouleau, L., Pirngruber, G., Guillou, F., Barrère-Tricca, C., Omegna, A., Valtchev, V., Pera-Titus, M., Miachon, S., Dalmon, J.A.: Nanocomposite MFI-alumina and FAU-alumina membranes: synthesis, characterization and application to paraffin separation and CO2 capture. Oil Gas Sci. Technol. 64(6), 745–758 (2009)

    Article  CAS  Google Scholar 

  • Ruthven, D.M., Farooq, S., Knaebel, K.S.: Pressure Swing Adsorption. VCH, New York (1994)

    Google Scholar 

  • Scholes, C.A., Stevens, G.W., Kentish, S.E.: Membrane gas separation applications in natural gas processing. Fuel 96(1), 15–28 (2012)

    Article  CAS  Google Scholar 

  • Singh, P., Niederer, J.P.M., Versteeg, G.F.: Structure and activity relationships for amine-based CO2 absorbents-II. Chem. Eng. Res. Des. 87(1), 135–144 (2009)

    Article  CAS  Google Scholar 

  • Smit, B., Maesen, T.L.M.: Molecular simulations of zeolites: adsorption, diffusion, and shape selectivity. Chem. Rev. 108(10), 4125–4184 (2008)

    Article  CAS  Google Scholar 

  • Song, L., Sun, Z.L., Rees, L.V.C.: Experimental and molecular simulation studies of adsorption and diffusion of cyclic hydrocarbons in silicalite-1. Microporous Mesoporous Mater. 55(2), 31–49 (2002)

    Article  CAS  Google Scholar 

  • Sun, H.: Ab initio calculations and force field development for computer simulation of polysilanes. Macromolecules 28(3), 701–712 (1995)

    Article  CAS  Google Scholar 

  • Talu, O., Myers, A.L.: Molecular simulation of adsorption: Gibbs dividing surface and comparison with experiment. AIChE J. 47(5), 1160–1168 (2001)

    Article  CAS  Google Scholar 

  • Verheyen, E., Joos, L., Van Havebergh, K., Breynaert, E., Kasian, N., Gobechiya, E., Houthoofd, K., Martineau, C., Hinterstein, M., Taulelle, F., Van Speybroeck, V., Waroquier, M., Bals, S., Van Tendeloo, G., Kirschhock, C.E.A., Martens, J.A.: Design of zeolite by inverse sigma transofrmation. Nat. Mater. 11(12), 1059–1064 (2012)

    CAS  Google Scholar 

  • Wu, J.Y., Liu, Q.L., Xiong, Y., Zhu, A.M., Chen, Y.: Molecular simulation of water/alcohol mixtures’ adsorption and diffusion in zeolite 4A membranes. J. Phys. Chem. B 113(13), 4267–4274 (2009)

    Article  CAS  Google Scholar 

  • Xie, D., McCusker, L.B., Baerlocher, C.: Structure of the boroslicate zeolite catalyst SSZ-82 solved using 2D-XPD charge flipping. J. Am. Chem. Soc. 133(50), 20604–20610 (2011)

    Article  CAS  Google Scholar 

  • Xu, Y., Li, Y., Han, Y., Song, X., Yu, J.: A gallogermanate zeolite with eleven-membered-ring channels. Angew. Chem. Int. Ed. 52(21), 5501–5503 (2013)

    Article  CAS  Google Scholar 

  • Yang, J., Zhao, Q., Xu, H., Li, L., Dong, J., Li, J.: Adsorption of CO2, CH4, and N2 on gas diameter grade ion-exchange small pore zeolites. J. Chem. Eng. Data 57(12), 3701–3709 (2012)

    Article  CAS  Google Scholar 

  • Yang, J.Z., Chen, Y., Zhu, A.M., Liu, Q.L., Wu, J.Y.: Analyzing diffusion behaviors of methanol/water through MFI membranes by molecular simulation. J. Membr. Sci. 318(1–2), 327–333 (2008)

    Article  CAS  Google Scholar 

  • Zeng, Y., Ju, S., Xing, W., Chen, C.: Computer simulation of benzene adsorbed in all-silica Y and NaY zeolites. Ind. Eng. Chem. Res. 46(1), 242–248 (2007)

    Article  CAS  Google Scholar 

  • Zhang, J., Burke, N., Zhang, S., Liu, K., Pervukhina, M.: Thermodynamic analysis of molecular simulations of CO2 and CH4 adsorption in FAU zeolites. Chem. Eng. Sci. 113(13), 54–61 (2014)

    Article  CAS  Google Scholar 

  • Zhang, K., Lively, R.P., Noel, J.D., Dose, M.E., McCool, B.A., Chance, R.R., Koros, W.J.: Adsorption of water and ethanol in MFI-type zeolites. Langmuir 28(23), 8664–8673 (2012)

    Article  CAS  Google Scholar 

  • Zhao, L., Zhai, D., Liu, B., Liu, Z., Xu, C., Wei, W., Chen, Y., Gao, J.: Grand canonical Monte Carlo simulations for energy gases on PIM-1 polymer and silicalite-1. Chem. Eng. Sci. 68(1), 101–107 (2012)

    Article  CAS  Google Scholar 

  • Zhong, D.L., Daraboina, N., Englezos, P.: Recovery of CH4 from coal mine model gas mixture (CH4/N2) by hydrate crystallization in the presence of cyclopentane. Fuel 106(4), 425–430 (2013)

    Article  CAS  Google Scholar 

  • Zhu, W., Hrabanek, P., Gora, L., Kapteijn, F., Moulijn, J.A.: Role of adsorption in the permeation of CH4 and CO2 through a silicalite-1 membrane. Ind. Eng. Chem. Res. 45(2), 767–776 (2006)

    Article  CAS  Google Scholar 

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Acknowledgments

This project was supported by the National Natural Science Foundation of China (21276101 and 21106051), the Jiangsu Program for Production, Teaching, and Research (BY2015052-01), Jiangsu Qing Lan Project and the Six Projects Sponsoring Talent Summits of Jiangsu Province, the Program for Science and Technology Development of Huai’an (HAC2015028, HAG2013073) and the Foundation of Jiangsu Key Laboratory for Chemistry of Low-Dimensional Materials (JSKC15143).

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Authors and Affiliations

  1. Jiangsu Key Laboratory for Biomass-based Energy and Enzyme Technology, Jiangsu Key Laboratory for Chemistry of Low-Dimensional Materials, Huaiyin Normal University, Huaian, 223300, People’s Republic of China

    Xiao-zhong Chu, Song-song Liu, Shou-yong Zhou & Yi-jiang Zhao

  2. Jiangsu Collaborative Innovation Center of Regional Modern Agriculture & Environmental Protection, Huaiyin Normal University, Huaian, 223300, People’s Republic of China

    Shou-yong Zhou & Yi-jiang Zhao

  3. State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing, 210009, People’s Republic of China

    Wei-hong Xing

  4. Huaian Key Laboratory of Advanced Environment Functional Materials, College of Chemistry and Chemical Engineering, Huaiyin Normal University, No.111 West Changjiang Road, Huai’an, 223300, Jiangsu, People’s Republic of China

    Yi-jiang Zhao

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  1. Xiao-zhong Chu
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Chu, Xz., Liu, Ss., Zhou, Sy. et al. Adsorption and separation of carbon dioxide and methane in new zeolites using the Grand Canonical Monte Carlo method. Adsorption 22, 891–899 (2016). https://doi.org/10.1007/s10450-016-9793-x

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  • DOI: https://doi.org/10.1007/s10450-016-9793-x

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