Classical Polarizable Force Field to Study Dry Charged Clays and Zeolites

Stéphane Tesson (1) , Wilfried Louisfrema (2) , Mathieu Salanne (1) , Anne Boutin (2) , Benjamin Rotenberg (1) , Virginie Marry (1)

1 PHENIX - PHysicochimie des Electrolytes et Nanosystèmes InterfaciauX
2 PASTEUR - Processus d'Activation Sélective par Transfert d'Energie Uni-électronique ou Radiatif (UMR 8640)

We extend the classical Polarizable Ion Model (PIM) to charged clays. We focus on Na-, Ca-, Sr- and Cs-montmorillonite with two types of structures for the octahedral sheet : trans- and cis-vacant. The full set of parameters of the force field is determined by density functional theory calculations, using maximally localized Wannier functions with a force- and dipole-optimization procedure. Simulation results for our polarizable force field are compared to the state-of-the-art non-polarizable flexible force field named Clay Force Field (ClayFF), in order to assess the importance of taking polarization effects into account for the prediction of structural properties. This force field is validated by comparison with experimental data. We also demonstrate the transferability of this force field to other aluminosilicates by considering faujasite-type zeolites and comparing the cation distribution for anhydrous Na, Ca, and Sr Y (and X) faujasites predicted by the PIM model and with experimental data.

Mots clés: Cis-vacant montmorillonite; Montmorillonite; Trans-vacant montmorillonite; Molecular Dynamics; Density Functional Theory; Polarizability; Crystal Structure; Charged Clay; Zeolite faujasite

Domaines: Chimie théorique et/ou physique; Modélisation et simulation

Stéphane Tesson, Wilfried Louisfrema, Mathieu Salanne, Anne Boutin, Benjamin Rotenberg, et al.. Classical Polarizable Force Field to Study Dry Charged Clays and Zeolites. Journal of Physical Chemistry C, 2017, ⟨10.1021/acs.jpcc.7b00270⟩. ⟨hal-01515667⟩