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The Role of Polymeric Ligand Shells in the Diffusive Behavior of Nanoparticles in Hydrogels

Moncure, Paige Josephine (2023) The Role of Polymeric Ligand Shells in the Diffusive Behavior of Nanoparticles in Hydrogels. Doctoral Dissertation, University of Pittsburgh. (Unpublished)

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Understanding nanoparticle (NP) diffusion in a hydrogel matrix is important to the development of NP biological technologies.
Hydrogels have a complex network structure that resembles important biological media, like mucus.
NP diffusion in hydrogels can be used to isolate and model transport of NPs in these biological materials.
To improve the understanding of hydrogel nanocomposites, a fundamental knowledge on how parameters of the NP affect their diffusion in hydrogels is necessary.
In this dissertation, I studied how the ligand shell impacts NP diffusion.
Using bulk diffusion measurements, I studied the impact of ligand shell molecular weight, ligand shell density, and ligand shell charge.
For fully functionalized NPs, regardless of core diameter, I found that the diffusion
coefficient was well-predicted by the confinement ratio calculated from the diameter of the
particle and the gel mesh size, as described by the Rubinstein hopping model.
For NPs with low density of high molecular weight capping ligands, the ligand chains on the surface are more dynamic, effectively making the particles smaller than their hydrodynamic diameters.
Finally, when NPs were functionalized with charged ligands, I found that the diffusion coefficients were slower compared to NPs with neutral ligands.
Overall, these studies revealed that the ligand shell plays a significant role in the diffusion of NPs in hydrogels.
Properties of the NP, including surface functionalization, shape, size, and composition, should all be considered when developing models for NPs diffusing under confinement.
This work will inform models for predicting NP diffusion in polymer networks that can be used to better understand NP behavior in complex biological environments.


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Item Type: University of Pittsburgh ETD
Status: Unpublished
CreatorsEmailPitt UsernameORCID
Moncure, Paige Josephinepam126@pitt.edupam1260000-0001-5465-645X
ETD Committee:
TitleMemberEmail AddressPitt UsernameORCID
Committee CoChairLaaser,
Committee CoChairMillstone,
Committee MemberSean,
Committee MemberRussel,
Date: 11 May 2023
Date Type: Publication
Defense Date: 31 March 2023
Approval Date: 11 May 2023
Submission Date: 6 April 2023
Access Restriction: 2 year -- Restrict access to University of Pittsburgh for a period of 2 years.
Number of Pages: 152
Institution: University of Pittsburgh
Schools and Programs: Dietrich School of Arts and Sciences > Chemistry
Degree: PhD - Doctor of Philosophy
Thesis Type: Doctoral Dissertation
Refereed: Yes
Uncontrolled Keywords: Diffusion, Nanoparticles, Hydrogels, Hopping Model, Ligand Shell
Date Deposited: 11 May 2023 19:48
Last Modified: 11 May 2023 19:48


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