Heterogeneity of network structures and water dynamics in κ-carrageenan gels probed by nanoparticle diffusometry

Daan W. de Kort, Erich Schuster, Freek J.M. Hoeben, Ryan Barnes, Meike Emondts, Henk M. Janssen, Niklas Lorén, Songi Han, Henk van As, John P.M. van Duynhoven

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    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
    Number of pages11
    JournalLangmuir
    Volume34
    Issue number37
    DOIs
    Publication statusPublished - 18 Sep 2018

    Fingerprint

    Carrageenan
    Gels
    gels
    Nanoparticles
    nanoparticles
    Water
    diffusivity
    mesh
    water
    Nuclear magnetic resonance
    Dendrimers
    Photobleaching
    nuclear magnetic resonance
    Biopolymers
    biopolymers
    dendrimers
    solutes
    Fluorescence
    recovery
    Spectroscopy

    Cite this

    de Kort, Daan W. ; Schuster, Erich ; Hoeben, Freek J.M. ; Barnes, Ryan ; Emondts, Meike ; Janssen, Henk M. ; Lorén, Niklas ; Han, Songi ; van As, Henk ; van Duynhoven, John P.M. / Heterogeneity of network structures and water dynamics in κ-carrageenan gels probed by nanoparticle diffusometry. In: Langmuir. 2018 ; Vol. 34, No. 37. pp. 11110-11120.
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    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}, {Daan W.} and Erich Schuster and Hoeben, {Freek J.M.} and Ryan Barnes and Meike Emondts and Janssen, {Henk M.} and Niklas Lor{\'e}n and Songi Han and {van As}, Henk and {van Duynhoven}, {John P.M.}",
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    doi = "10.1021/acs.langmuir.8b01052",
    language = "English",
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    de Kort, DW, Schuster, E, Hoeben, FJM, Barnes, R, Emondts, M, Janssen, HM, Lorén, N, Han, S, van As, H & van Duynhoven, JPM 2018, 'Heterogeneity of network structures and water dynamics in κ-carrageenan gels probed by nanoparticle diffusometry', Langmuir, vol. 34, no. 37, pp. 11110-11120. https://doi.org/10.1021/acs.langmuir.8b01052

    Heterogeneity of network structures and water dynamics in κ-carrageenan gels probed by nanoparticle diffusometry. / de Kort, Daan W.; Schuster, Erich; Hoeben, Freek J.M.; Barnes, Ryan; Emondts, Meike; Janssen, Henk M.; Lorén, Niklas; Han, Songi; van As, Henk; van Duynhoven, John P.M.

    In: Langmuir, Vol. 34, No. 37, 18.09.2018, p. 11110-11120.

    Research output: Contribution to journalArticleAcademicpeer-review

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    AU - Emondts, Meike

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    AU - Lorén, Niklas

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    AU - van As, Henk

    AU - van Duynhoven, John P.M.

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    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.

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