Fine-tuning the release of molecular guests from mesoporous silicas by controlling the orientation and mobility of surface phenyl substituents
dc.contributor.author | Manzano, J. Sebastián | |
dc.contributor.author | Singappuli-Arachchige, Dilini | |
dc.contributor.author | Parikh, Bosky L. | |
dc.contributor.author | Slowing, Igor | |
dc.contributor.department | Chemistry | |
dc.contributor.department | Ames National Laboratory | |
dc.date.accessioned | 2022-04-15T19:31:34Z | |
dc.date.available | 2022-04-15T19:31:34Z | |
dc.date.issued | 2018-05-15 | |
dc.description.abstract | Phenyl-functionalized mesoporous silica materials were used to explore the effect of non-covalent interactions on the release of Ibuprofen into simulated body fluid. Variations in orientation and conformational mobility of the surface phenyl groups were introduced by selecting different structural precursors: 1) a rigid upright orientation was obtained using phenyl groups directly bound to surface Si atoms (Ph-MSN), 2) mobile groups were produced by using ethylene linkers to connect phenyl groups to the surface (PhEt-MSN), and 3) groups co-planar to the surface were obtained by synthesizing a phenylene-bridged periodic mesoporous organosilica (Ph-PMO). The Ibuprofen release profiles from these materials and non-functionalized mesoporous silica nanoparticles (MSN) were analyzed using an adsorption-diffusion model. The model provided kinetic and thermodynamic parameters that evidenced fundamental differences in drug-surface interactions between the materials. All phenyl-bearing materials show lower Ibuprofen initial release rates than bare MSN. The conformationally locked Ph-MSN and Ph-PMO have stronger interactions with the drug (negative ΔG of adsorption) than the flexible PhEt-MSN and bare MSN (positive ΔG of adsorption). These differences in strength of adsorption are consistent with differences between interaction geometries obtained from DFT calculations. B3LYP-D3-optimized models show that π-π interactions contribute more to drug adsorption than H-bonding with silanol groups. The results suggest that the type and geometry of interactions control the kinetics and extent of drug release, and should therefore serve as a guide to design new drug delivery systems with precise release behaviors customized to any desired target. | |
dc.description.comments | This is a manuscript of an article published as Manzano, J. Sebastián, Dilini Singappuli-Arachchige, Bosky L. Parikh, and Igor I. Slowing. "Fine-tuning the release of molecular guests from mesoporous silicas by controlling the orientation and mobility of surface phenyl substituents." Chemical Engineering Journal 340 (2018): 73-80. DOI: 10.1016/j.cej.2017.12.015. Copyright 2017 Elsevier B.V. Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0). Posted with permission. | |
dc.identifier.uri | https://dr.lib.iastate.edu/handle/20.500.12876/NveoJL3z | |
dc.language.iso | en | |
dc.publisher | Elsevier | |
dc.source.uri | https://doi.org/10.1016/j.cej.2017.12.015 | * |
dc.subject.keywords | Drug delivery systems | |
dc.subject.keywords | Mesoporous silica nanoparticles | |
dc.subject.keywords | Controlled release | |
dc.subject.keywords | Interface | |
dc.subject.keywords | Polarity | |
dc.subject.keywords | Ibuprofen | |
dc.title | Fine-tuning the release of molecular guests from mesoporous silicas by controlling the orientation and mobility of surface phenyl substituents | |
dc.type | Article | |
dspace.entity.type | Publication | |
relation.isAuthorOfPublication | 15e8ccb1-3931-4bf0-bd09-3586ad3c87a9 | |
relation.isOrgUnitOfPublication | 42864f6e-7a3d-4be3-8b5a-0ae3c3830a11 | |
relation.isOrgUnitOfPublication | 25913818-6714-4be5-89a6-f70c8facdf7e |
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