We demonstrate the preparation and unique properties of composite vitrimer-like materials containing silica nanoparticles (SNPs). The matrix is composed of polyacrylate-based polymers crosslinked via a pyridine–bromo quaternization reaction, where the quaternized pyridine at the crosslinking point exchanges the bond pair via trans-N-alkylation at high temperatures. Homogeneous composite samples without a large aggregation of SNPs were prepared within the silica volume fraction range (ϕP) from 0.06 to 0.36. The formation of the bound rubber phase and the strong adhesion between the SNP and matrix are admitted in the data from structural, thermal, and mechanical investigations. The crosslinked composites exhibit great stress relaxation at high temperatures because of bond exchange, wherein unique bimodal relaxation behaviors are observed for the samples with high ϕP because of the bound rubber phase. In the final section, some useful functions, such as reprocessability and recyclability, derived from the bond exchange nature are exhibited.
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The authors thank Dr Y. Sakurai for her assistance with the SEM observation. The SAXS measurements were performed in beamline BL-6A at the Photon Factory (PF) of the High Energy Accelerator Research Organization in Tsukuba, Japan (KEK). This work was supported by the TOYOAKI Scholarship Foundation (MH). The SEM observation, DMA measurements, and stress-relaxation tests were supported by the Equipment Sharing Division, Organization for Co-Creation Research and Social Contributions, Nagoya Institute of Technology.
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Kimura, T., Hayashi, M. Exploring the effects of bound rubber phase on the physical properties of nano-silica composites with a vitrimer-like bond exchangeable matrix. Polym J (2022). https://doi.org/10.1038/s41428-022-00654-8