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Hydration-Dependent Dynamical Modes in Xyloglucan from Molecular Dynamics Simulation of C-13 NMR Relaxation Times and Their Distributions
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.ORCID iD: 0000-0002-0231-3970
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.ORCID iD: 0000-0001-5818-2378
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2018 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 19, no 7, p. 2567-2579Article in journal (Refereed) Published
Abstract [en]

Macromolecular dynamics in biological systems, which play a crucial role for biomolecular function and activity at ambient temperature, depend strongly on moisture content. Yet, a generally accepted quantitative model of hydration-dependent phenomena based on local relaxation and diffusive dynamics of both polymer and its adsorbed water is still missing. In this work, atomistic-scale spatial distributions of motional modes are calculated using molecular dynamics simulations of hydrated xyloglucan (XG). These are shown to reproduce experimental hydration-dependent C-13 NMR longitudinal relaxation times (T-1) at room temperature, and relevant features of their broad distributions, which are indicative of locally heterogeneous polymer reorientational dynamics. At low hydration, the self-diffusion behavior of water shows that water molecules are confined to particular locations in the randomly aggregated XG network while the average polymer segmental mobility remains low. Upon increasing water content, the hydration network becomes mobile and fully accessible for individual water molecules, and the motion of hydrated XG segments becomes faster. Yet, the polymer network retains a heterogeneous gel-like structure even at the highest level of hydration. We show that the observed distribution of relaxations times arises from the spatial heterogeneity of chain mobility that in turn is a result of heterogeneous distribution of water-chain and chain chain interactions. Our findings contribute to the picture of hydration-dependent dynamics in other macromolecules such as proteins, DNA, and synthetic polymers, and hold important implications for the mechanical properties of polysaccharide matrixes in plants and plant-based materials.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018. Vol. 19, no 7, p. 2567-2579
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-232788DOI: 10.1021/acs.biomac.8b00191ISI: 000438470800020PubMedID: 29688710Scopus ID: 2-s2.0-85046395682OAI: oai:DiVA.org:kth-232788DiVA, id: diva2:1236586
Funder
Swedish Research CouncilKnut and Alice Wallenberg Foundation
Note

QC 20180803

Available from: 2018-08-03 Created: 2018-08-03 Last updated: 2018-08-03Bibliographically approved

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Terenzi, CamillaFuro, IstvanBerglund, LarsWohlert, Jakob

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