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Diffusion of macromolecules in a polymer hydrogel: from microscopic to macroscopic scales

Diffusion of macromolecules in a polymer hydrogel: from microscopic to macroscopic scales
Diffusion of macromolecules in a polymer hydrogel: from microscopic to macroscopic scales
To gain insight into the fundamental processes determining the motion of macromolecules in polymeric matrices{,} the dynamical hindrance of polymeric dextran molecules diffusing as probe through a polyacrylamide hydrogel is systematically explored. Three complementary experimental methods combined with Brownian dynamics simulations are used to study a broad range of dextran molecular weights and salt concentrations. While multi-parameter fluorescence image spectroscopy (MFIS) is applied to investigate the local diffusion of single molecules on a microscopic length scale inside the hydrogel{,} a macroscopic transmission imaging (MTI) fluorescence technique and nuclear magnetic resonance (NMR) are used to study the collective motion of dextrans on the macroscopic scale. These fundamentally different experimental methods{,} probing different length scales of the system{,} yield long-time diffusion coefficients for the dextran molecules which agree quantitatively. The measured diffusion coefficients decay markedly with increasing molecular weight of the dextran and fall onto a master curve. The observed trends of the hindrance factors are consistent with Brownian dynamics simulations. The simulations also allow us to estimate the mean pore size for the herein investigated experimental conditions. In addition to the diffusing molecules{,} MFIS detects temporarily trapped molecules inside the matrix with diffusion times above 10 ms{,} which is also confirmed by anisotropy analysis. The fraction of bound molecules depends on the ionic strength of the solution and the charge of the dye. Using fluorescence intensity analysis{,} also MTI confirms the observation of the interaction of dextrans with the hydrogel. Moreover{,} pixelwise analysis permits to show significant heterogeneity of the gel on the microscopic scale.
1463-9076
12860-12876
Sandrin, D.
3a86ac1a-a253-4a26-8be4-848bce86fa3f
Wagner, D.
32871656-a18a-4cb7-bbde-9ea33e7f0ade
Sitta, C.E.
4d50eed8-f55e-43ed-8288-1eecab0f16ef
Thoma, R.
47e8df8d-52f8-40c1-a5b9-4c8248e96ad7
Felekyan, S.
47d2b7c7-27a7-4352-8226-2292ae68c903
Hermes, H.E.
152bedb6-dc3d-44c4-8b5b-f46c077bad65
Janiak, C.
a38d26b1-6a26-43c2-b8f8-d1cd4ceab87a
Amadeu, N. de Sousa
61e3375b-62bc-43e2-bca7-cdd8b9f2ea6d
Kühnemuth, R.
61eaf944-b4b5-4475-962b-6b2cbc6a07e7
Löwen, H.
a8e9d3f7-90bb-4f96-86da-c8617ffb6ed9
Egelhaaf, S.U.
ba6612e2-8d74-405f-b7ee-dca99c1d8b2a
Seidel, C.A.M.
a0337fd5-613a-48e5-a9c9-6d33e24aab08
Sandrin, D.
3a86ac1a-a253-4a26-8be4-848bce86fa3f
Wagner, D.
32871656-a18a-4cb7-bbde-9ea33e7f0ade
Sitta, C.E.
4d50eed8-f55e-43ed-8288-1eecab0f16ef
Thoma, R.
47e8df8d-52f8-40c1-a5b9-4c8248e96ad7
Felekyan, S.
47d2b7c7-27a7-4352-8226-2292ae68c903
Hermes, H.E.
152bedb6-dc3d-44c4-8b5b-f46c077bad65
Janiak, C.
a38d26b1-6a26-43c2-b8f8-d1cd4ceab87a
Amadeu, N. de Sousa
61e3375b-62bc-43e2-bca7-cdd8b9f2ea6d
Kühnemuth, R.
61eaf944-b4b5-4475-962b-6b2cbc6a07e7
Löwen, H.
a8e9d3f7-90bb-4f96-86da-c8617ffb6ed9
Egelhaaf, S.U.
ba6612e2-8d74-405f-b7ee-dca99c1d8b2a
Seidel, C.A.M.
a0337fd5-613a-48e5-a9c9-6d33e24aab08

Sandrin, D., Wagner, D., Sitta, C.E., Thoma, R., Felekyan, S., Hermes, H.E., Janiak, C., Amadeu, N. de Sousa, Kühnemuth, R., Löwen, H., Egelhaaf, S.U. and Seidel, C.A.M. (2016) Diffusion of macromolecules in a polymer hydrogel: from microscopic to macroscopic scales. Physical Chemistry Chemical Physics, 18 (18), 12860-12876. (doi:10.1039/C5CP07781H).

Record type: Article

Abstract

To gain insight into the fundamental processes determining the motion of macromolecules in polymeric matrices{,} the dynamical hindrance of polymeric dextran molecules diffusing as probe through a polyacrylamide hydrogel is systematically explored. Three complementary experimental methods combined with Brownian dynamics simulations are used to study a broad range of dextran molecular weights and salt concentrations. While multi-parameter fluorescence image spectroscopy (MFIS) is applied to investigate the local diffusion of single molecules on a microscopic length scale inside the hydrogel{,} a macroscopic transmission imaging (MTI) fluorescence technique and nuclear magnetic resonance (NMR) are used to study the collective motion of dextrans on the macroscopic scale. These fundamentally different experimental methods{,} probing different length scales of the system{,} yield long-time diffusion coefficients for the dextran molecules which agree quantitatively. The measured diffusion coefficients decay markedly with increasing molecular weight of the dextran and fall onto a master curve. The observed trends of the hindrance factors are consistent with Brownian dynamics simulations. The simulations also allow us to estimate the mean pore size for the herein investigated experimental conditions. In addition to the diffusing molecules{,} MFIS detects temporarily trapped molecules inside the matrix with diffusion times above 10 ms{,} which is also confirmed by anisotropy analysis. The fraction of bound molecules depends on the ionic strength of the solution and the charge of the dye. Using fluorescence intensity analysis{,} also MTI confirms the observation of the interaction of dextrans with the hydrogel. Moreover{,} pixelwise analysis permits to show significant heterogeneity of the gel on the microscopic scale.

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More information

Accepted/In Press date: 17 March 2016
Published date: 18 March 2016

Identifiers

Local EPrints ID: 435194
URI: http://eprints.soton.ac.uk/id/eprint/435194
ISSN: 1463-9076
PURE UUID: 4a3f88ac-b972-4302-a347-68b5d1201e9b

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Date deposited: 25 Oct 2019 16:30
Last modified: 25 Nov 2021 18:30

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Contributors

Author: D. Sandrin
Author: D. Wagner
Author: C.E. Sitta
Author: R. Thoma
Author: S. Felekyan
Author: H.E. Hermes
Author: C. Janiak
Author: N. de Sousa Amadeu
Author: R. Kühnemuth
Author: H. Löwen
Author: S.U. Egelhaaf
Author: C.A.M. Seidel

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