ArticlePolymers2026
Mobility-Driven Design of PDMS-Modified Glassy Polymer Networks for Thermally Activated Shape Memory in Vat Photopolymerization.
Article in Polymers, 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
Glass-transition-driven shape memory polymers are promising materials for 4D printing because their thermally activated transition enables programmed deformation and recovery without relying on melting or crystallization-driven switching. In this study, PDMS-MMA-modified photocurable networks were designed for vat photopolymerization-based 4D printing by varying PDMS-MMA content and switching monomer structure while maintaining a fixed TMPTMA crosslinker content. The resin formulations were prepared using tert-butyl acrylate (tBA) or isobornyl acrylate (IBOA) as switching monomers, PDMS-MMA as a flexible mobility-regulating segment, and TMPTMA as a multifunctional crosslinker. The effects of formulation composition on printability, network formation, thermal stability, thermomechanical transition, mechanical properties, and shape memory behavior were systematically investigated. FT-IR analysis confirmed effective photocuring of the acrylate/methacrylate networks, while rheological evaluation showed that resin viscosity depended on monomer structure and PDMS-MMA content. DMA results revealed thermomechanical transition, although some formulations exhibited broad tan δ responses due to network heterogeneity and distributed segmental relaxation. Based on resin printability, printed-part resolution, and relatively well-defined tan δ transitions, T-15 and I-15 were selected as representative formulations for quantitative shape memory evaluation. Shape memory testing was conducted under force-control mode because stable strain-controlled programming was not achievable for the printed specimens. Both T-15 and I-15 exhibited high shape fixity over two programming-recovery cycles. I-15 showed stable recovery behavior with recovery ratios of 91.51% and 95.87%, whereas T-15 showed apparent over-recovery with recovery ratios exceeding 100%, likely due to residual stress release during reheating. Overall, these results demonstrate that thermally activated shape-memory performance is governed not only by the nominal transition temperature but also by the coupled effects of PDMS-mediated segmental mobility, switching monomer structure, mechanical integrity, and elastic energy storage within a fixed crosslinked network framework.
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