Interactions of NaCl with cellulose Iβ crystal surfaces and the effect on cellulose hydration: a molecular dynamics study

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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä

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en

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15

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Cellulose, Volume 31, issue 7, pp. 4115-4129

Abstract

Crystalline nanocellulose is widely used for example, in the paper-making and food industries, as support matrix material or reinforcement of polymer materials, but also in drug carrier and nanomedicine applications. Interestingly, aqueous solutions of cellulose are extremely sensitive to small amounts of added salt yet mere considerations of charge screening leave open questions regarding the mechanisms, especially for unmodified cellulose in aqueous solutions. Here, we map NaCl ion distributions and the effect of added NaCl salt on the hydration of Iβ cellulose nanocrystal (CNC) surfaces by atomistic detail molecular dynamics simulations with explicit water solvent. The simulations reveal the dependency of the hydration layers of the six surfaces of CNCs on the ions, as well as NaCl ion binding sites, and preferences in terms of binding free energy for the ions near CNC surfaces at different NaCl concentrations. We discuss the modelling results against our prior rheology characterization of cellulose solutions. Together, the results indicate that the high sensitivity of cellulose aqueous solutions to added salt rises from the ions near the surface changing locally the ordering and structure of the hydration layers of the CNC surfaces. The revealed mechanism of salt-induced viscosity changes in cellulose aqueous solutions allows advanced design of gelling CNC systems for various end uses and may also guide tuning cellulose interactions by different solvent environments.

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Publisher Copyright: © The Author(s) 2024.

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Kou, Z, Tolmachev, D, Vuorte, M & Sammalkorpi, M 2024, 'Interactions of NaCl with cellulose Iβ crystal surfaces and the effect on cellulose hydration: a molecular dynamics study', Cellulose, vol. 31, no. 7, pp. 4115-4129. https://doi.org/10.1007/s10570-024-05831-x