Theoretical screening of antifouling polymer repeat units by molecular dynamics simulations

Nagumo, Ryo; Terao, Shohei; Miyake, Takaaki; Furukawa, Haruki; Iwata, Shuichi; Mori, Hideki; Takaba, Hiromitsu

doi:10.1038/pj.2014.45

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Published: 11 June 2014

Polymer Engineering

Theoretical screening of antifouling polymer repeat units by molecular dynamics simulations

Ryo Nagumo¹,
Shohei Terao¹,
Takaaki Miyake¹,
Haruki Furukawa¹,
Shuichi Iwata¹,
Hideki Mori¹ &
…
Hiromitsu Takaba²

Polymer Journal volume 46, pages 736–739 (2014)Cite this article

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Antifouling/biocompatible polymer surfaces and interfaces have attracted considerable attention because of their utility in membrane separation processes for water treatment, marine coatings and biomedical materials. Nonionic hydrophilic polymer surfaces with good antifouling/biocompatible properties have recently been developed.¹ Numerous mechanisms have been proposed to explain the compatibility of such materials. For example, poly(2-methoxyethylacrylate) (PMEA) can suppress platelet adhesion remarkably well compared with poly(2-hydroxyethylmethacrylate) (PHEMA).^{2, 3} To clarify the origin of the excellent blood compatibility of PMEA, a previous study² investigated the adsorption of proteins onto PMEA. The results indicated that the interactions between PMEA and proteins were weaker than those observed between PHEMA and proteins. The structure of water in the vicinity of polymer surfaces has been recognized as a fundamental factor for antifouling properties, as it plays a key role in preventing proteins and blood cells from directly interacting with the polymer interface.

Molecular dynamics (MD) calculations have provided useful information at the atomistic level in various fields,^{4, 5} including protein adsorption.^{6, 7, 8} To elucidate the correlation between antifouling/biocompatible properties and the behavior of water molecules at an interface, detailed physicochemical data are required. In particular, the adsorption free energy of proteins approaching a polymer surface is a key thermodynamic factor for evaluating their adsorption properties.⁹ From an engineering perspective, recent studies^{10, 11, 12} have shown that antifouling/biocompatible properties can be evaluated from the free energy profiles, which are generated from MD simulations in water, of amino acids approaching polymer repeat units. Specifically, the hydrophobic residue phenylalanine (Phe) can be conveniently used as a probe molecule because the profiles of Phe differ significantly depending on the nature of the repeat units.¹⁰ Simple strategies for assessing the interactions between hydrophobic probe molecules and polymer repeat units offer a convenient theoretical approach for initial screening of the antifouling/biocompatible properties of polymers. However, because of the high computational costs, it is generally difficult to acquire sufficient statistical samplings for the free energy calculations.¹³ However, if the free energy profiles of structurally simpler probe molecules, such as benzene, are in qualitative agreement with those of Phe, the computational cost for the initial screening of antifouling polymer repeat units would be reduced. Thus, structural simplification of the probe molecule could enable more sophisticated combinatorial screening. In this study, benzene was examined as a probe molecule for estimating antifouling properties using free energy calculations from MD simulations.

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Acknowledgements

This work was partially supported by the Salt Science Research Foundation (grant no. 1305) and by an A-step feasibility study program (AS242Z01737M) of the Japan Science and Technology Agency (JST).

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Department of Materials Science and Engineering, Nagoya Institute of Technology, Showa-ku, Nagoya, Japan
Ryo Nagumo, Shohei Terao, Takaaki Miyake, Haruki Furukawa, Shuichi Iwata & Hideki Mori
Department of Environmental and Energy Chemistry, Faculty of Engineering, Kogakuin University, Hachioji-shi, Tokyo, Japan
Hiromitsu Takaba

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Ryo Nagumo
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Shohei Terao
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Takaaki Miyake
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Hideki Mori
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Correspondence to Ryo Nagumo.

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Nagumo, R., Terao, S., Miyake, T. et al. Theoretical screening of antifouling polymer repeat units by molecular dynamics simulations. Polym J 46, 736–739 (2014). https://doi.org/10.1038/pj.2014.45

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Received: 06 February 2014
Revised: 17 April 2014
Accepted: 18 April 2014
Published: 11 June 2014
Issue date: October 2014
DOI: https://doi.org/10.1038/pj.2014.45

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Molecular dynamics study of the molecular mobilities and side-chain terminal affinities of 2-methoxyethyl acrylate and 2-hydroxyethyl methacrylate

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