Heterogeneity of Network Structures and Water Dynamics in κ‑Carrageenan Gels Probed by Nanoparticle Diffusometry

D.W. de Kort, Erich Schuster, F.J.M. Hoeben, R. Barnes, Meike Emondts, Henk M. Janssen, Niklas Lorén, Songi Han, H. Van As, J.P.M. van Duynhoven

Research output: Contribution to journalArticleAcademicpeer-review

1 Citation (Scopus)

Abstract

A set of functionalized nanoparticles (PEGylated dendrimers, d = 2.8−11 nm) was used to probe the structural heterogeneity in Na+/K+ induced κ-carrageenan gels. The self-diffusion behavior of these nanoparticles as observed by 1H pulsed-field gradient NMR, fluorescence recovery after photobleaching, and raster image correlation spectroscopy revealed a fast and a slow component, pointing toward microstructural heterogeneity in the gel network. The self-diffusion behavior of the faster nanoparticles could be modeled with obstruction by a coarse network (average mesh size <100 nm), while the slower-diffusing nanoparticles are trapped in a dense network (lower mesh size limit of 4.6 nm). Overhauser dynamic nuclear polarization-enhanced NMR relaxometry revealed a reduced local solvent water diffusivity near 2,2,6,6-tetramethylpiperidin-1-oxyl (TEMPO)-labeled nanoparticles trapped in the dense network, showing that heterogeneity in the physical network is also reflected in heterogeneous self-diffusivity of water. The observed heterogeneity in mesh sizes and in water self-diffusivity is of interest for understanding and modeling of transport through and release of solutes from heterogeneous biopolymer gels.
Original languageEnglish
Pages (from-to)11110-11120
JournalLangmuir
Volume34
DOIs
Publication statusPublished - 22 Aug 2018

Fingerprint

Carrageenan
Gels
gels
Nanoparticles
nanoparticles
Water
diffusivity
water
mesh
Nuclear magnetic resonance
Dendrimers
Photobleaching
nuclear magnetic resonance
Biopolymers
biopolymers
dendrimers
solutes
Polarization
gradients
polarization

Cite this

de Kort, D.W. ; Schuster, Erich ; Hoeben, F.J.M. ; Barnes, R. ; Emondts, Meike ; Janssen, Henk M. ; Lorén, Niklas ; Han, Songi ; Van As, H. ; van Duynhoven, J.P.M. / Heterogeneity of Network Structures and Water Dynamics in κ‑Carrageenan Gels Probed by Nanoparticle Diffusometry. In: Langmuir. 2018 ; Vol. 34. pp. 11110-11120.
@article{6297ca360a3e4f5f8164a1aab57fb719,
title = "Heterogeneity of Network Structures and Water Dynamics in κ‑Carrageenan Gels Probed by Nanoparticle Diffusometry",
abstract = "A set of functionalized nanoparticles (PEGylated dendrimers, d = 2.8−11 nm) was used to probe the structural heterogeneity in Na+/K+ induced κ-carrageenan gels. The self-diffusion behavior of these nanoparticles as observed by 1H pulsed-field gradient NMR, fluorescence recovery after photobleaching, and raster image correlation spectroscopy revealed a fast and a slow component, pointing toward microstructural heterogeneity in the gel network. The self-diffusion behavior of the faster nanoparticles could be modeled with obstruction by a coarse network (average mesh size <100 nm), while the slower-diffusing nanoparticles are trapped in a dense network (lower mesh size limit of 4.6 nm). Overhauser dynamic nuclear polarization-enhanced NMR relaxometry revealed a reduced local solvent water diffusivity near 2,2,6,6-tetramethylpiperidin-1-oxyl (TEMPO)-labeled nanoparticles trapped in the dense network, showing that heterogeneity in the physical network is also reflected in heterogeneous self-diffusivity of water. The observed heterogeneity in mesh sizes and in water self-diffusivity is of interest for understanding and modeling of transport through and release of solutes from heterogeneous biopolymer gels.",
author = "{de Kort}, D.W. and Erich Schuster and F.J.M. Hoeben and R. Barnes and Meike Emondts and Janssen, {Henk M.} and Niklas Lor{\'e}n and Songi Han and {Van As}, H. and {van Duynhoven}, J.P.M.",
year = "2018",
month = "8",
day = "22",
doi = "10.1021/acs.langmuir.8b01052",
language = "English",
volume = "34",
pages = "11110--11120",
journal = "Langmuir",
issn = "0743-7463",
publisher = "American Chemical Society",

}

Heterogeneity of Network Structures and Water Dynamics in κ‑Carrageenan Gels Probed by Nanoparticle Diffusometry. / de Kort, D.W.; Schuster, Erich; Hoeben, F.J.M.; Barnes, R.; Emondts, Meike; Janssen, Henk M.; Lorén, Niklas; Han, Songi; Van As, H.; van Duynhoven, J.P.M.

In: Langmuir, Vol. 34, 22.08.2018, p. 11110-11120.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Heterogeneity of Network Structures and Water Dynamics in κ‑Carrageenan Gels Probed by Nanoparticle Diffusometry

AU - de Kort, D.W.

AU - Schuster, Erich

AU - Hoeben, F.J.M.

AU - Barnes, R.

AU - Emondts, Meike

AU - Janssen, Henk M.

AU - Lorén, Niklas

AU - Han, Songi

AU - Van As, H.

AU - van Duynhoven, J.P.M.

PY - 2018/8/22

Y1 - 2018/8/22

N2 - A set of functionalized nanoparticles (PEGylated dendrimers, d = 2.8−11 nm) was used to probe the structural heterogeneity in Na+/K+ induced κ-carrageenan gels. The self-diffusion behavior of these nanoparticles as observed by 1H pulsed-field gradient NMR, fluorescence recovery after photobleaching, and raster image correlation spectroscopy revealed a fast and a slow component, pointing toward microstructural heterogeneity in the gel network. The self-diffusion behavior of the faster nanoparticles could be modeled with obstruction by a coarse network (average mesh size <100 nm), while the slower-diffusing nanoparticles are trapped in a dense network (lower mesh size limit of 4.6 nm). Overhauser dynamic nuclear polarization-enhanced NMR relaxometry revealed a reduced local solvent water diffusivity near 2,2,6,6-tetramethylpiperidin-1-oxyl (TEMPO)-labeled nanoparticles trapped in the dense network, showing that heterogeneity in the physical network is also reflected in heterogeneous self-diffusivity of water. The observed heterogeneity in mesh sizes and in water self-diffusivity is of interest for understanding and modeling of transport through and release of solutes from heterogeneous biopolymer gels.

AB - A set of functionalized nanoparticles (PEGylated dendrimers, d = 2.8−11 nm) was used to probe the structural heterogeneity in Na+/K+ induced κ-carrageenan gels. The self-diffusion behavior of these nanoparticles as observed by 1H pulsed-field gradient NMR, fluorescence recovery after photobleaching, and raster image correlation spectroscopy revealed a fast and a slow component, pointing toward microstructural heterogeneity in the gel network. The self-diffusion behavior of the faster nanoparticles could be modeled with obstruction by a coarse network (average mesh size <100 nm), while the slower-diffusing nanoparticles are trapped in a dense network (lower mesh size limit of 4.6 nm). Overhauser dynamic nuclear polarization-enhanced NMR relaxometry revealed a reduced local solvent water diffusivity near 2,2,6,6-tetramethylpiperidin-1-oxyl (TEMPO)-labeled nanoparticles trapped in the dense network, showing that heterogeneity in the physical network is also reflected in heterogeneous self-diffusivity of water. The observed heterogeneity in mesh sizes and in water self-diffusivity is of interest for understanding and modeling of transport through and release of solutes from heterogeneous biopolymer gels.

U2 - 10.1021/acs.langmuir.8b01052

DO - 10.1021/acs.langmuir.8b01052

M3 - Article

VL - 34

SP - 11110

EP - 11120

JO - Langmuir

JF - Langmuir

SN - 0743-7463

ER -