Trapping probabilities of multiple rings in end-linked gels

• Published in: Polymer (Guilford) 2022-04, Vol.245, p.124683, Article 124683
• Main Authors: Hagita, Katsumi, Murashima, Takahiro, Ebe, Minami, Isono, Takuya, Satoh, Toshifumi
• Format: Article
• Language: English
• Subjects: Chemical synthesis; Coarse-grained molecular dynamics simulation; End-linked polymer network; Gels; Mechanical properties; Molecular dynamics; Penetration; Polydimethylsiloxane; Polymer blends; Polymers; Probability; Ring polymer; Simulation; Trapping; Trapping probability
• ISSN: 0032-3861; 1873-2291
• 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. [Display omitted] •End-linked gels penetrating rings and ring complexes were considered.•Trapping probability was evaluated through MD simulations and confirmed via PDMS experiments.•The dependence of the trapping probability on the ring size were investigated.•Ring–bridge probability that multiple chains penetrate a ring or a ring complex was also investigated.•The good correspondence between the experimental and simulation enables further predictions of the probabilities.