苯分子与Si6O18H12和Al6O24H30团簇模型相互作用的理论研究

doi:10.3866/PKU.WHXB201312042

Abstract

Abstract:

Clay minerals are used to remove organics and to remediate soils and groundwater contaminated with petroleum hydrocarbons. Cluster models of Si₆O₁₈H₁₂ and Al₆O₂₄H₃₀ for the tetrahedral (Si―O) and octahedral (Al―O) surfaces of kaolinite were set up to mimic kaolinite surfaces. The interactions of benzene molecule and the kaolinite cluster models were systematically studied at the MP2/6- 31G(d,p)//B3LYP/6-31G(d,p) level. The gas- state adsorption properties of benzene on the kaolinite surfaces, such as the optimized structures, structural parameters, adsorption energies, natural bond orbital charge distributions, vibration frequencies, electrostatic potential maps, electron density characteristics (the ρ and ▽²ρ values of secondary hydrogen-bonds), and electron density difference, were analyzed in this work. The optimized structures indicate that the adsorption of benzene molecule on the kaolinite surfaces may be caused by formation of secondary hydrogen-bonds. The results for the other properties further confirmed the existence of secondary hydrogen-bonds. Benzene molecule is more likely to be adsorbed on the Al―O surface than on the Si―O surface. The adsorption angle between the benzene ring plane and the kaolinite Al―O surface is about 90°.

Key words: Density functional theory, Benzene, Kaolinite, Adsorption, Secondary hydrogen bond

WANG Xing, QIAN Ping, SONG Kai-Hui, ZHANG Chao, SONG Wei. Theoretical Investigation of Interaction of Benzene Molecule and Si₆O₁₈H₁₂ and Al₆O₂₄H₃₀ Cluster Models[J]. Acta Phys. -Chim. Sin. 2014, 30(2), 241-250. doi: 10.3866/PKU.WHXB201312042

References

(1) Roldan, R.; Romero, F. J.; Jimenez, C.; Borau, V.; Marinas, J.M. Appl. Catal. A 2004, 266, 203. doi: 10.1016/j.apcata.2004.02.008
(2) Maliyekkal, S. M.; Rene, E. R.; Philip, L.; Swaminathan, T.J. Hazard. Mater. 2004, 109, 201. doi: 10.1016/j.jhazmat.2004.04.001
(3) Pilidis, G. A.; Karakitsios, S. P.; Kassomenos, P. A.; Kazos, E.A.; Stalikas, C. D. Environ. Monit. Assess. 2009, 150, 285. doi: 10.1007/s10661-008-0230-9
(4) Lesage, S. Anal. Chem. ACS Publications 1993, 65, 647A.
(5) Michalková, A.; Tunega, D.; Nagy, L. T. J. Mol. Struct. - Theochem 2002, 581, 37. doi: 10.1016/S0166-1280(01)00741-2
(6) Hess, A. C.; Saunders, V. R. J. Phys. Chem. 1992, 96, 4367. doi: 10.1021/j100190a047
(7) Shua, H. T.; Lib, D.; Scalaa, A. A.; Mab, Y. H. Purif. Technol.1997, 11, 27. doi: 10.1016/S1383-5866(96)01005-2
(8) Beltrán, A.; Andrés, J.; Calatayud, M.; Martins, J. B. L. Chem. Phys. Lett. 2001, 338, 224. doi: 10.1016/S0009-2614(01)00238-X
(9) Martins, J. B. L.; Sambrano, J. R.; Vasconcellos, L. A. S.;Longo, E.; Taft, C. A. Quim. Nova. 2004, 27, 10. doi: 10.1590/S0100-40422004000100003
(10) Martins, J.; Taft, C.; Lie, S.; Longo, E. J. Mol. Struct. - Theochem 2000, 528, 161. doi: 10.1016/S0166-1280(99)00498-4
(11) Almeida, A.; Martins, J.; Longo, E.; Taft, C.; Murgich, J.;Jalbout, A. F. J. Mol. Struct. -Theochem 2003, 664, 111.
(12) Sambrano, J.; Vasconcellos, L.; Martins, J.; Santos, M.; Longo,E.; Beltran, A. J. Mol. Struct. -Theochem 2003, 629, 307. doi: 10.1016/S0166-1280(03)00200-8
(13) Castro, E. A. S.; Gargano, R.; Martins, J. B. L. Int. J. Quantum Chem. 2012, 112, 2828. doi: 10.1002/qua.v112.16
(14) Castro, E. A. S.; Martins, J. B. L. J. Comput. Aided Mater. Des.2005, 12, 121.
(15) Bickmore, B. R.; Rosso, K. M.; Nagy, K. L.; Cygan, R. T.;Tadanier, C. J. Clays Clay Min. 2003, 51, 359.
(16) Castro, E. A. S.; Martins, J. B. L. Int. J. Quantum Chem. 2005,103, 550.
(17) Balan, E.; Saitta, A. M.; Mauri, F.; Lemaire, C.; Guyot, F. Am. Mineral. 2002, 87, 1286.
(18) Michalková, A.; Szymczak, J. J.; Leszczynski, J. Struct. Chem.2005, 16, 325. doi: 10.1007/s11224-005-4463-8
(19) Pelmenschikov, A.; Leszczynski, J. J. Phys. Chem. B 1999, 103,6886. doi: 10.1021/jp990091q
(20) Gorb, L.; Lutchyn, R.; Zub, Y.; Leszczynska, D.; Leszczynski, J.J. Mol. Struct. -Theochem 2006, 766, 151. doi: 10.1016/j.theochem.2006.04.013
(21) Lee, J. F.; Mortland, M. M.; Chiou, C. T.; Kile, D. E.; Boyd, S.A. Clay Clay Min. 1990, 38, 113.
(22) Wilson, M. A.; Lee, G. S. H.; Taylor, R. C. Clay Clay Min.2002, 50, 348.
(23) Frisch, M. J.; Trucks, G.W.; Schlegel, H. B.; et al. Gaussian 03,Revision A.01; Gaussian Inc.: Pittsburgh, PA, 2003.
(24) Young, R. A.; Hewat, A.W. Clay Clay Min. 1988, 36, 225.
(25) Bish, D. L. Clay Clay Min. 1993, 41, 738.
(26) Karl, K. I.; Russell, D. J.; Raghu, N. K. J. Phys. Chem. A 2005,109, 8430. doi: 10.1021/jp052793n
(27) Koch, U.; Popelier, P. J. Phys. Chem. 1995, 99, 9747. doi: 10.1021/j100024a016
(28) Popelier, P. J. Phys. Chem. A 1998, 102, 1873. doi: 10.1021/jp9805048
(29) Bader, R.W. F. Accounts Chem. Res. 1985, 18, 9.
(30) Flükiger, P.; Lüthi, H.; Portmann, S.;Weber, J. Molekel 4.0;Swiss Center for Scientific Computing: Manno, Switzerlan,2000.
(31) Lu, T.; Chen, F. J. Comput. Chem. 2012, 33, 580. doi: 10.1002/jcc.v33.5
(32) Lu, T. GsGrid: Extracting Data from Gaussian Grid File andGrid File Calculation [EB/OL]. http:∥gsgrid.codeplex.com, in.
(33) Zhang, C.; Song, K. H.;Wang, X.; Yin, H. Z.; Qian, P. J. Mol. Sci. 2013, 29, 134. [张超, 宋开慧, 王幸, 尹洪宗,钱萍. 分子科学学报, 2013, 29, 134.]
(34) Hu, X. L.; Michaelides, A. Surf. Sci. 2008, 602, 960. doi: 10.1016/j.susc.2007.12.032
(35) Neder, R.; Burghammer, M.; Grasl, T.; Schulz, H.; Bram, A.;Fiedler, S. Clay Clay Min. 1999, 47, 487.
(36) Austen, K. F.; White, T. O. H.; Marmier, A.; Parker, S. C.;Artacho, E.; Dove, M. T. J. Phys: Condes. Matter 2008, 20,035215. doi: 10.1088/0953-8984/20/03/035215
(37) Sainz-Díaz, I.; Francisco-Márquez, M.; Vivier-Bunge, A.Environ. Chem. 2011, 8, 429.

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Theoretical Investigation of Interaction of Benzene Molecule and Si₆O₁₈H₁₂ and Al₆O₂₄H₃₀ Cluster Models

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Theoretical Investigation of Interaction of Benzene Molecule and Si6O18H12 and Al6O24H30 Cluster Models

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Theoretical Investigation of Interaction of Benzene Molecule and Si₆O₁₈H₁₂ and Al₆O₂₄H₃₀ Cluster Models