Periodic modeling of zeolite Ti-LTA

• Published in: The Journal of chemical physics Vol. 147; no. 7; pp. 074701 - 74711
• Main Authors: Hernandez-Tamargo, Carlos E., Roldan, Alberto, Ngoepe, Phuti E., de Leeuw, Nora H.
• Format: Journal Article
• Language: English
• Published: United States 21.08.2017
• ISSN: 0021-9606; 1089-7690
• DOI: 10.1063/1.4998296

We have proposed a combination of density functional theory calculations and interatomic potential-based simulations to study the structural, electronic, and mechanical properties of pure-silica zeolite Linde Type A (LTA), as well as two titanium-doped compositions. The energetics of the titanium distribution within the zeolite framework suggest that the inclusion of a second titanium atom with configurations T i – ( S i ) 0 – T i , T i – ( S i ) 1 – T i , and T i – ( S i ) 2 – T i is more energetically favorable than the mono-substitution. Infra-red spectra have been simulated for the pure-silica LTA, the single titanium substitution, and the configurations T i – ( S i ) 0 – T i and T i – ( S i ) 2 – T i , comparing against experimental benchmarks where available. The energetics of the direct dissociation of water on these Lewis acid sites indicate that this process is only favored when two titanium atoms form a two-membered ring (2MR) sharing two hydroxy groups, T i – ( O H ) 2 – T i , which suggests that the presence of water may tune the distribution of titanium atoms within the framework of zeolite LTA. The electronic analysis indicates charge transfer from H 2 O to the Lewis acid site and hybridization of their electronic states.