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Multiscale modeling of thermomechanical properties of stereoregular polymers

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Abstract

Multiscale coarse-grained (CG) models are expected to play the critical roles in molecular simulations of complex polymers. However, this poses a great challenge for accurately simulating their thermomechanical properties, for which excellent representability and transferability are required for the CG potentials. In this work, virtual sites and elastic network bonds are introduced to improve the structural and volumetric property–based CG models including explicit electrostatic interactions, which is exemplarily applied to the iso- and syndio-tactic poly(methyl methacrylate). A variety of thermomechanical properties of the two stereoregular polymer bulks are reasonably reproduced by the extensive molecular dynamics simulations with the so-parameterized CG potentials. In particular, the attractive nature of electrostatic interactions and tacticity effects on glass transition temperatures (Tg) are well captured. Furthermore, stronger electrostatic interactions lead to higher mass density and bulk modulus, and their effects on Young’s modulus, Poisson’s ratio, and shear modulus depend upon the chain tacticity. It is also demonstrated that all these elastic constants can be effectively modulated by imposing external electric field. The proposed multiscale scheme can be very valuable to molecular designs of polar polymer materials.

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Acknowledgments

The author is indebted to the Molecular Simulation Center of Hunan Province (situated at Hunan University), which provides the commercial software (Materials Studio-4.0) to build the initial structural models and to perform the empirical calculations. The MD simulations were carried out at Shanxi Supercomputing Center (SXSC) in China.

Funding

This work is financially supported by the Natural Science Foundation of Hunan Province (2022JJ30311), and Double First-Class Discipline Construction Program of Hunan Province, and the Innovative Research Team in Higher Educational Institute of Hunan Province, and the Talent Support Plan of Hunan University of Humanities Science & Technology (HUHST).

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  1. Hunan Provincial Key Laboratory of Fine Ceramics and Powder Materials, School of Materials and Environmental Engineering, Hunan University of Humanities, Science and Technology, Loudi, Hunan, 417000, People’s Republic of China

    Chaofu Wu

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Wu C. is the only author who carried out all works underlying this manuscript.

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Correspondence to Chaofu Wu.

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Wu, C. Multiscale modeling of thermomechanical properties of stereoregular polymers. J Mol Model 28, 214 (2022). https://doi.org/10.1007/s00894-022-05214-8

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