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Role of Ligand Shell Density in the Diffusive Behavior of Nanoparticles in Hydrogels
[Image: see text] The diffusion coefficients of poly(ethylene glycol) methyl ether thiol (PEGSH)-functionalized gold nanoparticles (NPs) with different effective grafting densities were measured in polyacrylamide hydrogels. The NP core size was held constant, and the NPs were functionalized with mix...
Autores principales: | , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10626584/ https://www.ncbi.nlm.nih.gov/pubmed/37857360 http://dx.doi.org/10.1021/acs.jpcb.3c03249 |
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author | Moncure, Paige J. Millstone, Jill E. Laaser, Jennifer E. |
author_facet | Moncure, Paige J. Millstone, Jill E. Laaser, Jennifer E. |
author_sort | Moncure, Paige J. |
collection | PubMed |
description | [Image: see text] The diffusion coefficients of poly(ethylene glycol) methyl ether thiol (PEGSH)-functionalized gold nanoparticles (NPs) with different effective grafting densities were measured in polyacrylamide hydrogels. The NP core size was held constant, and the NPs were functionalized with mixtures of short oligomeric ligands (254 Da PEGSH) and longer (either 1 or 2 kDa PEGSH) ligands. The ratio of short and long ligands was varied such that the grafting density of the high-molecular-weight (MW) ligand ranged from approximately 1 to 100 high-MW ligands/NP. The diffusion coefficients of the NPs were then measured in gels with varying average mesh sizes. The measured diffusion coefficients decreased with higher MW ligand density. Interestingly, the diffusion coefficients for NPs with high effective grafting densities were well-predicted by their hydrodynamic diameters, but the diffusion coefficients for NPs with low effective grafting densities were higher than expected from their hydrodynamic diameters. These results suggest that crowding in the NP ligand shell influences the mechanism of diffusion, with lower grafting densities allowing ligand chain relaxations that facilitate movement through the gel. This work brings new insights into the factors that dictate how NPs move through hydrogels and will inform the development of models for applications such as drug delivery in complex viscoelastic biological materials. |
format | Online Article Text |
id | pubmed-10626584 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-106265842023-11-07 Role of Ligand Shell Density in the Diffusive Behavior of Nanoparticles in Hydrogels Moncure, Paige J. Millstone, Jill E. Laaser, Jennifer E. J Phys Chem B [Image: see text] The diffusion coefficients of poly(ethylene glycol) methyl ether thiol (PEGSH)-functionalized gold nanoparticles (NPs) with different effective grafting densities were measured in polyacrylamide hydrogels. The NP core size was held constant, and the NPs were functionalized with mixtures of short oligomeric ligands (254 Da PEGSH) and longer (either 1 or 2 kDa PEGSH) ligands. The ratio of short and long ligands was varied such that the grafting density of the high-molecular-weight (MW) ligand ranged from approximately 1 to 100 high-MW ligands/NP. The diffusion coefficients of the NPs were then measured in gels with varying average mesh sizes. The measured diffusion coefficients decreased with higher MW ligand density. Interestingly, the diffusion coefficients for NPs with high effective grafting densities were well-predicted by their hydrodynamic diameters, but the diffusion coefficients for NPs with low effective grafting densities were higher than expected from their hydrodynamic diameters. These results suggest that crowding in the NP ligand shell influences the mechanism of diffusion, with lower grafting densities allowing ligand chain relaxations that facilitate movement through the gel. This work brings new insights into the factors that dictate how NPs move through hydrogels and will inform the development of models for applications such as drug delivery in complex viscoelastic biological materials. American Chemical Society 2023-10-19 /pmc/articles/PMC10626584/ /pubmed/37857360 http://dx.doi.org/10.1021/acs.jpcb.3c03249 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Moncure, Paige J. Millstone, Jill E. Laaser, Jennifer E. Role of Ligand Shell Density in the Diffusive Behavior of Nanoparticles in Hydrogels |
title | Role of Ligand
Shell Density in the Diffusive Behavior
of Nanoparticles in Hydrogels |
title_full | Role of Ligand
Shell Density in the Diffusive Behavior
of Nanoparticles in Hydrogels |
title_fullStr | Role of Ligand
Shell Density in the Diffusive Behavior
of Nanoparticles in Hydrogels |
title_full_unstemmed | Role of Ligand
Shell Density in the Diffusive Behavior
of Nanoparticles in Hydrogels |
title_short | Role of Ligand
Shell Density in the Diffusive Behavior
of Nanoparticles in Hydrogels |
title_sort | role of ligand
shell density in the diffusive behavior
of nanoparticles in hydrogels |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10626584/ https://www.ncbi.nlm.nih.gov/pubmed/37857360 http://dx.doi.org/10.1021/acs.jpcb.3c03249 |
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