Hostname: page-component-848d4c4894-mwx4w Total loading time: 0 Render date: 2024-06-26T21:31:30.460Z Has data issue: false hasContentIssue false
  • English
  • Français

Molecular Dynamics Simulation of Alkylammonium-Intercalated Vermiculites

Published online by Cambridge University Press:  01 January 2024

Cheng Chen ,
Xiandong Liu ,
Yingchun Zhang ,
Chi Zhang  and
Xiancai Lu
Cheng Chen
Affiliation:
State Key Lab for Mineral Deposits Research, School of Earth Sciences and Engineering, Nanjing University, 210046, Nanjing, P. R. China
Xiandong Liu*
Affiliation:
State Key Lab for Mineral Deposits Research, School of Earth Sciences and Engineering, Nanjing University, 210046, Nanjing, P. R. China
Yingchun Zhang
Affiliation:
State Key Lab for Mineral Deposits Research, School of Earth Sciences and Engineering, Nanjing University, 210046, Nanjing, P. R. China
Chi Zhang
Affiliation:
State Key Lab for Mineral Deposits Research, School of Earth Sciences and Engineering, Nanjing University, 210046, Nanjing, P. R. China
Xiancai Lu
Affiliation:
State Key Lab for Mineral Deposits Research, School of Earth Sciences and Engineering, Nanjing University, 210046, Nanjing, P. R. China
*
*E-mail address of corresponding author: [email protected]
Get access Rights & Permissions [Opens in a new window]

Abstract

In order to understand the microscopic properties of alkylammonium-intercalated vermiculites, molecular dynamics simulations employing the clayff-CVFF force field were performed to obtain the interlayer structures and dynamics. The layering behavior of alkyl chains was uncovered. With the model used in the present study (1.2 e per unit cell), the alkyl chains formed monolayers with carbon-chain lengths of C6, bilayers from C7 to C10, and pseudo-trimolecular layers from C15 to C18. Intermediate states also existed between bilayer and pseudo-trimolecular layer states from C11 to C14. The ammonium groups had two locations: most ammonium groups were located over the six-member rings (~90%), and the rest above the substitution sites (~10%). The ammonium groups interacted with the vermiculite surface through H bonds between ammonium H atoms and surface O atoms. The ammonium groups were fixed firmly on surfaces and, therefore, had very low mobility. The alkyl chains were slightly more mobile. The similarities and differences between alkylammonium-intercalated vermiculites and smectites were revealed. The layering behaviors of alkyl chains were similar in alkylammonium-intercalated vermiculites and smectites: the alkyl chain behavior was controlled by both the amount of layer charge and the carbon chain length. The distributions of ammonium groups, however, were different, caused by the layer-charge distribution in vermiculites being different from that in smectites. The atomic-level results derived in the present study will be useful for future research into and the applications of organo-vermiculites.

Keywords

AlkylammoniumIntercalationInterlayer StructuresMobilityMolecular DynamicsVermiculites
Type
Article
Information
Clays and Clay Minerals , Volume 65 , Issue 6 , December 2017 , pp. 378 - 386
Copyright
Copyright © Clay Minerals Society 2017

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

Allen, M.P. and Tildesley, D.J. (1987) Computer Simulation of Liquids. Clarendon Press, Oxford, UK.Google Scholar
Al-Samhan, M. Samuel, J. Al-Attar, F. and Abraham, G., 2017 Comparative effects of MMT clay modified with two different cationic surfactants on the thermal and rheological properties of polypropylene nanocomposites International Journal of Polymer Science 2 1–8.CrossRefGoogle Scholar
Bardziński, P.J., 2014 On the impact of intermolecular interactions between the quaternary ammonium ions on interlayer spacing of quat-intercalated montmorillonite: A molecular mechanics and ab-initio study Applied Clay Science 95 323–339.CrossRefGoogle Scholar
Brigatti, M.F. Galán, E. Theng, B.K.G., Bergaya, F. and Lagaly, G., 2013 Structure and mineralogy of clay minerals Handbook of Clay Science 2 Amsterdam Elsevier 21–81.CrossRefGoogle Scholar
Carrizosa, M.J. Rice, P.J. Koskinen, W.C. Carrizosa, I. and Hermosín, M.D., 2004 Sorption of isoxaflutole and DKN on organoclays Clays and Clay Minerals 52 341–349.CrossRefGoogle Scholar
Chang, F-RC Skipper, N.T. and Sposito, G., 1997 Monte Carlo and molecular dynamics simulations of interfacial structure in lithium-montmorillonite hydrates Langmuir 13 2074–2082.CrossRefGoogle Scholar
Cygan, R.T., 2001 Molecular modeling in mineralogy and geochemistry Molecular Modeling Theory: Applications in the Geosciences 42 1–35.Google Scholar
Cygan, R.T. Liang, J.-J. and Kalinichev, A.G., 2004 Molecular models of hydroxide, oxyhydroxide, and clay phases and the development of a general force field Journal of Physical Chemistry B 108 1255–1266.CrossRefGoogle Scholar
Dauber-Osguthorpe, P. Roberts, V.A. Osguthorpe, D.J. Wolff, J. Genest, M. and Hagler, A.T., 1988 Structure and energetics of ligand binding to proteins: E. coli dihydrofolate reductasetrimethoprim, a drug-receptor system Proteins: Structure, Function and Genetics 4 31–47.CrossRefGoogle ScholarPubMed
Escamilla-Roa, E. Nieto, F. and Sainz-Díaz, C.I., 2016 Stability of hydronium cation in the structure of illite Clays and Clay Minerals 64 413–424.CrossRefGoogle Scholar
Ferrage, E., 2016 Investigation of the interlayer organization of water and ions in smectite from the combined use of diffraction experiments and molecular simulations. A review of methodology, applications, and perspectives Clays and Clay Minerals 348–373.CrossRefGoogle Scholar
Greenwell, H.C. Harvey, M.J. Boulet, P. Bowden, A.A. Coveney, P.V. and Whiting, A., 2005 Interlayer structure and bonding in nonswelling primary amine intercalated clays Macromolecules 38 6189–6200.CrossRefGoogle Scholar
Gruner, J.W., 1934 The structures of vermiculites and their collapse by dehydration American Mineralogist 19 557–575.Google Scholar
Harvey, C.C. Lagaly, G., Bergaya, F. and Lagaly, G., 2013 Industrial applications Handbook of Clay Science 2 Amsterdam Elsevier 451–490.CrossRefGoogle Scholar
He, H.P. Galy, J. and Gerard, J.F., 2005 Molecular simulation of the interlayer structure and the mobility of alkyl chains in HDTMA(+)/montmorillonite hybrids Journal of Physical Chemistry B 109 13301–13306.CrossRefGoogle ScholarPubMed
Heinz, H. Koerner, H. Anderson, K.L. Vaia, R.A. and Farmer, B.L., 2005 Force field for mica-type silicates and dynamics of octadecylammonium chains grafted to montmorillonite Chemistry of Materials 17 5658–5669.CrossRefGoogle Scholar
Janek, M. and Smrcok, L., 1999 Application of an internal standard technique by transmission X-ray diffraction to assess layer charge of a montmorillonite by using the alkylammonium method Clays and Clay Minerals 47 113–118.CrossRefGoogle Scholar
Jankovič, L. Kronek, J. Madejová, J. and Hronský, V., 2015 (9, 10-Dihydroxyoctadecyl)ammonium: A structurally unique class of clay intercalable surfactants European Journal of Inorganic Chemistry 17 2841–2850.CrossRefGoogle Scholar
Kalinichev, A.G. Liu, X.D. and Cygan, R.T., 2016 Introduction to a special issue on molecular computer simulations of clays and clay-water interfaces: Recent progress, challenges, and opportunities Clays and Clay Minerals 64 335–336.CrossRefGoogle Scholar
Lagaly, G., 1981 Characterization of clays by organic compounds Clay Minerals 16 1–21.CrossRefGoogle Scholar
Lagaly, G., 1982 Layer charge heterogeneity in vermiculites Clays and Clay Minerals 30 215–222.CrossRefGoogle Scholar
Lagaly, G. Ogawa, M. Dekany, I., Bergaya, F. and Lagaly, G., 2013 Clay mineralorganic interactions Handbook of Clay Science 2 Amsterdam Elsevier 435–505.CrossRefGoogle Scholar
Laird, D.A. Scott, A.D. and Fenton, T.E., 1989 Evaluation of the alkylammonium method of determining layer charge Clays and Clay Minerals 37 41–46.CrossRefGoogle Scholar
Lee, J.F. Mortland, M.M. Chiou, C.T. and Boyd, S.A., 1989 Shape-selective adsorption of aromatic molecules from water by tetramethylammonium-smectite Journal of the Chemical Society 85 2953–2962.Google Scholar
Li, Z.H. Jiang, W.T. and Hong, H.L., 2008 An FTIR investigation of hexadecyltrimethylammonium intercalation into rectorite Spectrochimica Acta Part A 71 1525–1534.CrossRefGoogle ScholarPubMed
Liu, X.D. Lu, X.C. Wang, R.C. Zhou, H.Q. and Xu, S.J., 2007 Interlayer structure and dynamics of alkylammonium- intercalated smectites with and without water: A molecular dynamics study Clays and Clay Minerals 55 554–564.CrossRefGoogle Scholar
Liu, X.D. Lu, X.C. Wang, R.C. Zhou, H.Q. and Xu, S.J., 2009 Molecular dynamics insight into the cointercalation of hexadecyltrimethyl-ammonium and acetate ions into smectites American Mineralogist 94 143–150.CrossRefGoogle Scholar
Loewenstein, W., 1954 The distribution of aluminum in the tetrahedra of silicates and aluminates American Mineralogist 39 92–96.Google Scholar
Madejová, J. Sekeráková, L. Bizovská, V. Slaný, M. and Jankovič, L., 2016 Near-infrared spectroscopy as an effective tool for monitoring the conformation of alkylammonium surfactants in montmorillonite interlayers Vibrational Spectroscopy 84 44–52.CrossRefGoogle Scholar
Mykola, S. Olga, N. and Dmitry, M., 2016 The influence of alkylammonium modified clays on the fungal resistance and biodeterioration of epoxy-clay nanocomposites International Biodeterioration & Biodegradation 110 136–140.CrossRefGoogle Scholar
Nguemtchouin, Marie Goletti Mbouga Ngassoum, Martin Benoît Kamga, Richard Deabate, Stéfano Lagerge, Serge Gastaldi, Emmanuelle Chalier, Pascale and Cretin, Marc, 2015 Characterization of inorganic and organic clay modified materials: An approach for adsorption of an insecticidal terpenic compound Applied Clay Science 104 110–118.CrossRefGoogle Scholar
Osman, MA S G UW, 2000 Twodimensional melting of alkane monolayers ionically bonded to mica Journal of Physical Chemistry B 104 4433–4439.CrossRefGoogle Scholar
Osman, M.A. Ernst, M. Meier, B.H. and Suter, U.W., 2002 Structure and molecular dynamics of alkane monolayers self-assembled on mica platelets Journal of Physical Chemistry B 106 653–662.CrossRefGoogle Scholar
Osman, M.A. Ploetze, M. and Skrabal, P., 2004 Structure and properties of alkylammonium monolayers self-assembled on montmorillonite platelets Journal of Physical Chemistry B 108 2580–2588.CrossRefGoogle Scholar
Pazos, M.C. Cota, A. Osuna, F.J. Pavon, E. and Alba, M.D., 2015 Self-assembling of tetradecylammonium chain on swelling high charge micas (Na-Mica-3 and Na-Mica-2): Effect of alkylammonium concentration and mica layer charge Langmuir 31 4394–4401.CrossRefGoogle ScholarPubMed
Perry, T.D. Cygan, R.T. and Mitchell, R., 2006 Molecular models of alginic acid: Interactions with calcium ions and calcite surfaces Geochimica et Cosmochimica Acta 70 3508–3532.CrossRefGoogle Scholar
Sarkar, M. Dana, K. and Ghatak, S., 2011 Evolution of molecular structure and conformation of n-alkylammonium intercalated iron rich bentonites Journal of Molecular Structure 1005 161–166.Google Scholar
Scholtzová, E. Madejová, J. Jankovič, L. and Tunega, D., 2016 Structural and spectroscopic characterization of montmorillonite intercalated with n-butylammonium cations (N=1-4)-modeling and experimental study Clays and Clay Minerals 64 401–412.CrossRefGoogle Scholar
Smith, W. and Forester, T.R., 1996 DL_POLY_2.0: A general-purpose parallel molecular dynamics simulation package Journal of Molecular Graphics 14 136–141.CrossRefGoogle ScholarPubMed
Szczerba, M. Kuligiewicz, A. Derkowski, A. Gionis, V. Chryssikos, G.D. and Kalinichev, A.G., 2016 Structure and dynamics of water-smectite interfaces: Hydrogen bonding and the origin of the sharp O-Dw/O-Hw infrared band from molecular simulations Clays and Clay Minerals 64 452–471.CrossRefGoogle Scholar
Tambach, T.J. Boek, E.S. and Smit, B., 2006 Molecular order and disorder of surfactants in clay nanocomposites Physical Chemistry Chemical Physics 8 2700–2702.CrossRefGoogle ScholarPubMed
Vaia, R.A. Teukolsky, R.K. and Giannelis, E.P., 1994 Interlayer structure and molecular environment of alkylammonium layered silicates Chemistry of Materials 6 1017–1022.CrossRefGoogle Scholar
Wang, L.Q. Liu, J. Exarhos, G.J. Flanigan, K.Y. and Bordia, R., 2000 Conformation heterogeneity and mobility of surfactant molecules in intercalated clay minerals studied by solid-state NMR Journal of Physical Chemistry B 104 2810–2816.CrossRefGoogle Scholar
Weiss, A., 1963 Organic derivatives of mica-type layer silicates Angewandte Chemie International Edition 2 134–144.CrossRefGoogle Scholar
Wen, X.Y. He, H.P. Zhu, J.X. Jun, Y. Ye, C.H. and Deng, F., 2006 Arrangement, conformation, and mobility of surfactant molecules intercalated in montmorillonite prepared at different pillaring reagent concentrations as studied by solid-state NMR spectroscopy Journal of Colloid and Interface Science 299 754–760.CrossRefGoogle ScholarPubMed
Zeng, Q.H. Yu, A.B. Lu, G.Q. and Standish, R.K., 2003 Molecular dynamics simulation of organic-inorganic nanocomposites: the layering behavior and interlayer structure of organoclays Chemistry of Materials 15 4732–4738.CrossRefGoogle Scholar
Zeng, Q.H. Yu, A.B. Lu, G.Q. and Standish, R.K., 2004 Molecular dynamics simulation of the structural and dynamic properties of organoclay Journal of Physical Chemistry B 108 10025–10033.CrossRefGoogle Scholar
Zhao, Q. and Burns, S.E., 2012 Molecular dynamics simulation of secondary sorption behavior of montmorillonite modified by single chain quaternary ammonium cations Environmental Science & Technology 46 3999–4007.CrossRefGoogle ScholarPubMed
Zhu, J.X. He, H.P. Zhu, L.Z. Wen, X.Y. and Deng, F., 2005 Characterization of organic phases in the interlayer of montmorillonite using FTIR and C-13 NMR Journal of Colloid and Interface Science 286 239–244.CrossRefGoogle Scholar