Multilayered assembly of poly(vinylidene fluoride) and poly(methyl methacrylate) for achieving multi-shape memory effects

Xiaoying Ji, Dayong Chen, Yu Zheng, Jiabin Shen, Shaoyun Guo, Eileen Harkin-Jones

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The alternately-organized poly(vinylidene fluoride) (PVDF)/poly(methyl methacrylate) (PMMA) multilayer materials were prepared through layer-multiplying coextrusion. With the multiplication of layers, the thickness of each layer was reduced in proportion and the layer interfaces were enriched generating a broader and more continuous thermal transition temperature (Ttrans) from PVDF to PMMA layers as mapped by in-situ thermal analysis. The low-Ttrans side originated from the glass transition of PMMA, whereas the high-Ttrans side was dominated by the melting of PVDF crystals based on the heating curves of DMA and DSC. The dielectric spectroscopy and 2D-SAXS were performed and demonstrated that the compositional diffusion not only broadened the relaxation distribution of amorphous chains, but also strengthened the interaction between amorphous and crystalline domains. Therefore, a unique multilayer network, where the crystals in PVDF layers acting as physical networks connected the neighboring amorphous layers, was fabricated and its potential application in obtaining multi-shape memory effect (MSME) was disclosed for the first time. The results exhibited that the 1024-layer specimen owned a better triple- and quadruple-shape memory capacity than conventional blend which possessed the same compositions and a similar Ttrans range. The latter one even failed to successively memorize more than
two temporary shapes. A possible mechanism was proposed through polarized IR and creeping-recovery measurements. Higher phase continuity which benefited for the stress transfer was revealed to play a significant role in strengthening the shape-fixing and -recovering ability during each shape memory progress. Accordingly, a new physically-compounding strategy was addressed to achieve outstanding MSME for meeting complex demands in smart applications.
Original languageEnglish
Pages (from-to)190-198
Number of pages9
JournalChemical Engineering Journal
Early online date6 Jan 2019
Publication statusPublished (in print/issue) - 15 Apr 2019


  • Multi-shape memory effect
  • Multilayer structure
  • Phase continuity
  • Interfacial diffusion


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