Predicting Partial Atomic Charges in Siliceous Zeolites
Document Type
Article
Publication Date
10-27-2018
Publication Title
Microporous and Mesoporous Materials
Volume
277
First page number:
184
Last page number:
196
Abstract
Partial atomic charge, which determines the magnitude of the Coulombic non-bonding interaction, represents a critical parameter in molecular mechanics simulations. Partial charges may also be used as a measure of physical properties of the system, ie. covalency, acidic/catalytic sites, etc. A range of methods, both empirical and ab initio, exist for calculating partial charges in a given solid, and several of them are compared here for siliceous (pure silica) zeolites. The relationships between structure and the predicted partial charge are examined. The predicted partial charges from different methods are also compared with related experimental observations, showing that a few of the methods offer some guidance towards identifying the T-sites most likely to undergo substitution or for proton localization in acidic framework forms. Finally, we show that assigning unique calculated charges to crystallographically unique framework atoms makes an appreciable difference in simulating predicting N2 and O2 adsorption with common dispersion-repulsion parameterizations.
Keywords
Zeolite; Partial charge; Molecular mechanics; DFTT-atom substitution; Acid catalysis
Disciplines
Materials Chemistry
Language
English
Repository Citation
Wolffis, J. J.,
Vanpoucke, D. E.,
Sharma, A.,
Lawler, K. V.,
Forster, P. M.
(2018).
Predicting Partial Atomic Charges in Siliceous Zeolites.
Microporous and Mesoporous Materials, 277
184-196.
http://dx.doi.org/10.1016/j.micromeso.2018.10.028