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First Observation of the Hydration Layer around Polymer Chain by Scattering and Its Relationship to Thromboresistance: Dilute Solution Properties of PMEA in THF/Water

Cite this: J. Phys. Chem. B 2021, 125, 26, 7251–7261
Publication Date (Web):June 28, 2021
https://doi.org/10.1021/acs.jpcb.1c01864
Copyright © 2021 American Chemical Society

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    Abstract

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    Poly(2-methoxyethyl acrylate) (PMEA) is known to exhibit excellent thromboresistance, i.e., hardly causing blood-clot formation on its surface. Hence, PMEA and its analogues have been commercially used for blood-contacting materials in medical devices. In this study, we investigated the conformation and solvation state of PMEA in mixtures of tetrahydrofuran (THF) and water with various water volume fractions (ϕwater) by viscosity, sedimentation equilibrium, small-angle X-ray scattering (SAXS), and dielectric relaxation measurements. We also comparatively investigated those of poly[2-(2-methoxyethoxy)ethyl methacrylate] (PMe2MA) and polystyrene (PS). For all of these, THF is a good solvent and water is a nonsolvent or poor solvent. PMe2MA and PMEA show equally good thromboresistance, while PS does not at all. The solution properties of PMe2MA and PMEA were found to be quite different from PS. There are clear attractive interactions (or correlation) between the PMEA chain (or PMe2MA) and the waters in the vicinity of the chain despite their water insolubility. These correlated waters give additional scattering and the angular dependence of SAXS was analyzed in terms of the hydration layer model that has been used in protein solution scattering. The hydration is related to increasing both the chain stiffness and excluded volume. These distinctive properties are likely related to the origin of its good thromboresistance.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpcb.1c01864.

    • Berry plots by SEC-MALS, ν̅ and dndc at different ϕwater, Huggins plots, VH and A2 of PBA, Berry plots of PMe2MA by SAXS, determining ML by SEC-MALS, F(q) of the wormlike chain models with various λ–1 and L values, third mode in the dielectric spectra, DR strength of fourth mode, and symbols (PDF)

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    Cited By

    This article is cited by 2 publications.

    1. André M. Striegel. Absolute molar mass determination in mixed solvents. 2. SEC/MALS/DRI in a mix of two “nearly-isovirial” solvents. Analytica Chimica Acta 2022, 1231 , 340369. https://doi.org/10.1016/j.aca.2022.340369
    2. Kei Nishida, Takahisa Anada, Masaru Tanaka. Roles of interfacial water states on advanced biomedical material design. Advanced Drug Delivery Reviews 2022, 186 , 114310. https://doi.org/10.1016/j.addr.2022.114310

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