Understanding the role of cross-link density in the segmental dynamics and elastic properties of cross-linked thermosets

Author:

Zheng Xiangrui1,Guo Yafang1,Douglas Jack F.2ORCID,Xia Wenjie3ORCID

Affiliation:

1. Department of Mechanics, School of Physical Science and Engineering, Beijing Jiaotong University, Beijing 100044, China

2. Materials Science and Engineering Division, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, USA

3. Department of Civil, Construction and Environmental Engineering, North Dakota State University, Fargo, North Dakota 58108, USA

Abstract

Cross-linking is known to play a pivotal role in the relaxation dynamics and mechanical properties of thermoset polymers, which are commonly used in structural applications because of their light weight and inherently strong nature. Here, we employ a coarse-grained (CG) polymer model to systematically explore the effect of cross-link density on basic thermodynamic properties as well as corresponding changes in the segmental dynamics and elastic properties of these network materials upon approaching their glass transition temperatures ( Tg). Increasing the cross-link density unsurprisingly leads to a significant slowing down of the segmental dynamics, and the fragility K of glass formation shifts in lockstep with Tg, as often found in linear polymer melts when the polymer mass is varied. As a consequence, the segmental relaxation time τα becomes almost a universal function of reduced temperature, ( T − Tg)/ Tg, a phenomenon that underlies the applicability of the “universal” Williams–Landel–Ferry (WLF) relation to many polymer materials. We also test a mathematical model of the temperature dependence of the linear elastic moduli based on a simple rigidity percolation theory and quantify the fluctuations in the local stiffness of the network material. The moduli and distribution of the local stiffness likewise exhibit a universal scaling behavior for materials having different cross-link densities but fixed ( T − Tg)/ Tg. Evidently, Tg dominates both τα and the mechanical properties of our model cross-linked polymer materials. Our work provides physical insights into how the cross-link density affects glass formation, aiding in the design of cross-linked thermosets and other structurally complex glass-forming materials.

Funder

National Natural Science Foundation of China

North Dakota State University

Office of Naval Research

Publisher

AIP Publishing

Subject

Physical and Theoretical Chemistry,General Physics and Astronomy

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