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Heterogeneity of Network Structures and Water Dynamics in ?-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 ?-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.

SUBMITTER: de Kort DW 

PROVIDER: S-EPMC6146320 | biostudies-literature | 2018 Sep

REPOSITORIES: biostudies-literature

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

de Kort Daan W DW   Schuster Erich E   Hoeben Freek J M FJM   Barnes Ryan R   Emondts Meike M   Janssen Henk M HM   Lorén Niklas N   Han Songi S   Van As Henk H   van Duynhoven John P M JPM  

Langmuir : the ACS journal of surfaces and colloids 20180906 37


A set of functionalized nanoparticles (PEGylated dendrimers, d = 2.8-11 nm) was used to probe the structural heterogeneity in Na<sup>+</sup>/K<sup>+</sup> induced κ-carrageenan gels. The self-diffusion behavior of these nanoparticles as observed by <sup>1</sup>H 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 b  ...[more]

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