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Dynamic Imine Bond-Based Shape Memory Polymers with Permanent Shape Reconfigurability for 4D Printing.

Jia-Tao Miao1, Meiying Ge1, Shuqiang Peng1,2

  • 1CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Key Laboratory of Nanomaterials , Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences , Fuzhou 350002 , People's Republic of China.

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This study introduces novel dynamic imine bond (meth)acrylate systems for 4D printing, enhancing material toughness and enabling permanent shape reconfiguration for advanced applications.

Keywords:
(meth)acrylate4D printingdynamic covalent bondreconfigurationshape memory

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Area of Science:

  • Polymer Science
  • Materials Science
  • Additive Manufacturing

Background:

  • Shape memory polymers (SMPs) combined with 3D printing create active materials.
  • Current SMP 4D printing materials, often based on (meth)acrylates, have fixed covalent bonds limiting permanent shape changes.
  • There is a need for SMP materials that allow for permanent shape modification after printing.

Purpose of the Study:

  • To develop novel (meth)acrylate-based SMP systems for 4D printing with dynamic imine bonds.
  • To enhance material toughness and shape memory properties.
  • To enable permanent shape reconfiguration of 4D printed structures.

Main Methods:

  • Synthesis of a novel (meth)acrylate monomer with an aldehyde group (MEFB).
  • Development of a hyperbranched cross-linker (HPASi) to create (meth)acrylate systems (IEMSis) with dynamic imine bonds.
  • Characterization of mechanical properties, shape memory performance, and stress relaxation behavior.

Main Results:

  • IEMSis exhibited significantly enhanced toughness (33-97-fold higher than IEM).
  • High shape fixity (97.5-97.6%) and shape recovery (91.4-93.7%) were achieved.
  • IEMSis demonstrated permanent shape reconfiguration via dynamic imine bond exchange, with IEMSi3 showing an 84.3% shape retention ratio.

Conclusions:

  • The novel IEMSis offer superior toughness and shape memory properties compared to traditional systems.
  • The dynamic imine bonds allow for catalyst-free, mild condition stress relaxation and permanent shape reconfiguration.
  • These reconfigurable 4D printing materials hold potential for applications in aerospace, robotics, electronics, and intelligent packaging.