Trapping probabilities of multiple rings in end-linked gels

K Hagita and T Murashima and M Ebe and T Isono and T Satoh, POLYMER, 245, 124683 (2022).

DOI: 10.1016/j.polymer.2022.124683

To create a tough polymer network material with rings as a movable crosslink, it is important to prepare materials in which multiple linear chains penetrate a ring or a ring complex. The ring size is an important factor in realizing novel mechanical properties. Establishment of close correspondence between simulations and experiments is effective for selecting a target ring polymer for synthesis. The penetration of a ring by a linear chain in a mixed system containing rings and linear chains can be evaluated using the trapping probability of rings in the end- linked gel. By performing coarse-grained molecular dynamics (CGMD) simulations of the Kremer-Grest model corresponding to poly(dimethylsiloxane) (PDMS) chains, we directly clarified the relationship between the penetration and trapping probability of rings in the end-linked gel. In addition, we introduced the concept of the ring-bridge probability, which is the probability that multiple chains penetrate a ring or a ring complex. The dependence of the trapping probability and ring-bridge probability on the ring size were investigated. To establish a correspondence between ring complexes, such as bonded rings and spiro-multicyclic polymers, a mixed system consisting of complexes of bonded three-rings and linear chains was evaluated through the CGMD simulations and confirmed via PDMS experiments. A close correspondence between the experimental and simulation results enables the prediction of the trapping and bridge probabilities of spiro-multicyclic polymers. The findings illustrate that simulation-based prediction can substantially contribute to the development of polymer network materials with ring-linear blends.

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