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Probing Microscale Structuring-Induced Phase Separation with Fluorescence Recovery Diffusion Dynamics in Poly(ethylene glycol) Solutions
[Image: see text] Apart from biocompatibility, poly(ethylene glycol) (PEG)-based biomedical constructs require mechanical tunability and optimization of microscale transport for regulation of the release kinetics of biomolecules. This study illustrates the role of inhomogeneities due to aggregates a...
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/PMC10536873/ https://www.ncbi.nlm.nih.gov/pubmed/37780024 http://dx.doi.org/10.1021/acsomega.3c04917 |
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author | Bhatt, Shipra Bagchi, Debjani Das, Avik Kumar, Ashwani Sen, Debasis |
author_facet | Bhatt, Shipra Bagchi, Debjani Das, Avik Kumar, Ashwani Sen, Debasis |
author_sort | Bhatt, Shipra |
collection | PubMed |
description | [Image: see text] Apart from biocompatibility, poly(ethylene glycol) (PEG)-based biomedical constructs require mechanical tunability and optimization of microscale transport for regulation of the release kinetics of biomolecules. This study illustrates the role of inhomogeneities due to aggregates and structuring in the PEG matrix in the microscale diffusion of a fluorescent probe. Comparative analysis of fluorescence recovery after photobleaching (FRAP) profiles with the help of diffusion half-time is used to assess the diffusion coefficient (D). The observations support a nontrivial dependence of diffusion dynamics on polymer concentration (volume fraction, φ) and that of fillers carboxymethyl cellulose (CMC) and nanoclay bentonite (B). D values follow the Rouse scaling D ∼ φ(–0.54) in PEG solutions. The diffusion time of the fluorescent probe in the PEG+bentonite matrix reveals the onset of depletion interaction-induced phase separation with an increase in bentonite concentration in the PEG matrix beyond 0.1 wt %. Beyond this concentration, structure factors obtained from prebleach FRAP images show a rapid increase at low Q. The two-phase system (PEG-rich and bentonite-rich) was characterized by the hierarchical structural topology of bentonite aggregates, and aggregate sizes were obtained at different length scales with phase contrast imaging, small-angle neutron scattering, and small-angle X-ray scattering. The microscale transport detection presented captures sensitively the commencement of phase separation in the PEG + bentonite matrix, as opposed to the PEG or PEG + CMC matrix, which are observed to be one-phase systems. This method of diffusion half-time and prebleach image analysis can be used for the fast, high-throughput experimental investigation of microscale mechanical response and its correlation with structuring in the polymer matrix. |
format | Online Article Text |
id | pubmed-10536873 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-105368732023-09-29 Probing Microscale Structuring-Induced Phase Separation with Fluorescence Recovery Diffusion Dynamics in Poly(ethylene glycol) Solutions Bhatt, Shipra Bagchi, Debjani Das, Avik Kumar, Ashwani Sen, Debasis ACS Omega [Image: see text] Apart from biocompatibility, poly(ethylene glycol) (PEG)-based biomedical constructs require mechanical tunability and optimization of microscale transport for regulation of the release kinetics of biomolecules. This study illustrates the role of inhomogeneities due to aggregates and structuring in the PEG matrix in the microscale diffusion of a fluorescent probe. Comparative analysis of fluorescence recovery after photobleaching (FRAP) profiles with the help of diffusion half-time is used to assess the diffusion coefficient (D). The observations support a nontrivial dependence of diffusion dynamics on polymer concentration (volume fraction, φ) and that of fillers carboxymethyl cellulose (CMC) and nanoclay bentonite (B). D values follow the Rouse scaling D ∼ φ(–0.54) in PEG solutions. The diffusion time of the fluorescent probe in the PEG+bentonite matrix reveals the onset of depletion interaction-induced phase separation with an increase in bentonite concentration in the PEG matrix beyond 0.1 wt %. Beyond this concentration, structure factors obtained from prebleach FRAP images show a rapid increase at low Q. The two-phase system (PEG-rich and bentonite-rich) was characterized by the hierarchical structural topology of bentonite aggregates, and aggregate sizes were obtained at different length scales with phase contrast imaging, small-angle neutron scattering, and small-angle X-ray scattering. The microscale transport detection presented captures sensitively the commencement of phase separation in the PEG + bentonite matrix, as opposed to the PEG or PEG + CMC matrix, which are observed to be one-phase systems. This method of diffusion half-time and prebleach image analysis can be used for the fast, high-throughput experimental investigation of microscale mechanical response and its correlation with structuring in the polymer matrix. American Chemical Society 2023-09-14 /pmc/articles/PMC10536873/ /pubmed/37780024 http://dx.doi.org/10.1021/acsomega.3c04917 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by-nc-nd/4.0/Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/). |
spellingShingle | Bhatt, Shipra Bagchi, Debjani Das, Avik Kumar, Ashwani Sen, Debasis Probing Microscale Structuring-Induced Phase Separation with Fluorescence Recovery Diffusion Dynamics in Poly(ethylene glycol) Solutions |
title | Probing Microscale
Structuring-Induced Phase Separation
with Fluorescence Recovery Diffusion Dynamics in Poly(ethylene glycol)
Solutions |
title_full | Probing Microscale
Structuring-Induced Phase Separation
with Fluorescence Recovery Diffusion Dynamics in Poly(ethylene glycol)
Solutions |
title_fullStr | Probing Microscale
Structuring-Induced Phase Separation
with Fluorescence Recovery Diffusion Dynamics in Poly(ethylene glycol)
Solutions |
title_full_unstemmed | Probing Microscale
Structuring-Induced Phase Separation
with Fluorescence Recovery Diffusion Dynamics in Poly(ethylene glycol)
Solutions |
title_short | Probing Microscale
Structuring-Induced Phase Separation
with Fluorescence Recovery Diffusion Dynamics in Poly(ethylene glycol)
Solutions |
title_sort | probing microscale
structuring-induced phase separation
with fluorescence recovery diffusion dynamics in poly(ethylene glycol)
solutions |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10536873/ https://www.ncbi.nlm.nih.gov/pubmed/37780024 http://dx.doi.org/10.1021/acsomega.3c04917 |
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