Title:
Development of accurate computational methods for simulations of adsorption and diffusion in zeolites

dc.contributor.author Awati, Rohan Vivek
dc.contributor.committeeMember Sholl, David S.
dc.contributor.committeeMember Koros, William J.
dc.contributor.committeeMember Nair, Sankar
dc.contributor.committeeMember Walton, Krista S.
dc.contributor.committeeMember Jang, Seung Soon
dc.contributor.department Chemical and Biomolecular Engineering
dc.date.accessioned 2016-05-27T13:11:57Z
dc.date.available 2016-05-27T13:11:57Z
dc.date.created 2016-05
dc.date.issued 2016-01-15
dc.date.submitted May 2016
dc.date.updated 2016-05-27T13:11:57Z
dc.description.abstract The overall objective of this thesis has been to develop accurate computational methods for the diffusion and adsorption of small gases in zeolites. Firstly, the effect of the zeolite framework flexiblity on the single component and binary diffusion of various gases were discussed. Results indicate that for tight fitting molecules the rigid framework approximation can produce order(s) of magnitude difference in diffusivities as compared to the simulations performed with a fully flexible framework. We proposed two simple methods in which the flexible structure of a zeolite is approximated as a set of discrete rigid snapshots. Both methods are orders of magnitude more efficient than the simulations with the fully flexible structure. Secondly, we use a combined classical and quantum chemistry based approach to systematically develop the force fields based on DFT calculations for interactions of simple molecules like CH4, N2, linear alkanes, and linear alkenes in zeolites. We used a higher level of theory known as the DFT/CC method to correct DFT energies that were used in the periodic DFT calculations to develop force fields. Our results show that DFT-derived force fields give good predictions of macroscopic properties like adsorption isotherms in zeolites. The force fields are transferrable across zeolites and hence can be further used to screen materials for different storage and separation applications.
dc.description.degree Ph.D.
dc.format.mimetype application/pdf
dc.identifier.uri http://hdl.handle.net/1853/54945
dc.language.iso en_US
dc.publisher Georgia Institute of Technology
dc.subject Molecular simulations
dc.subject Force field
dc.subject Flexible framework
dc.title Development of accurate computational methods for simulations of adsorption and diffusion in zeolites
dc.type Text
dc.type.genre Dissertation
dspace.entity.type Publication
local.contributor.corporatename School of Chemical and Biomolecular Engineering
local.contributor.corporatename College of Engineering
relation.isOrgUnitOfPublication 6cfa2dc6-c5bf-4f6b-99a2-57105d8f7a6f
relation.isOrgUnitOfPublication 7c022d60-21d5-497c-b552-95e489a06569
thesis.degree.level Doctoral
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