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Mechanically Robust and Chemically Recyclable Polyhydroxyurethanes from CO2-Derived Six-Membered Cyclic Carbonates.

Pengcheng Miao1, Ziyue Jiao1, Jie Liu1

  • 1State Key Laboratory of Fine Chemicals, Department of Polymer Science and Engineering, Liaoning Key Laboratory of Polymer Science and Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian116024, China.

ACS Applied Materials & Interfaces
|December 23, 2022
PubMed
Summary

This study introduces novel shape memory polyhydroxyurethanes (PHUs) synthesized via a green, isocyanate-free route using CO2. These PHUs exhibit exceptional mechanical strength, shape recovery, and chemical recyclability, advancing sustainable polymer development.

Keywords:
chemically recyclablemechanically robustpolyhydroxyurethanessix-membered cyclic carbonatesvitrimer

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Area of Science:

  • Polymer Chemistry
  • Sustainable Materials Science
  • Green Chemistry

Background:

  • Growing demand for sustainable materials and regulations favor isocyanate-free polyurethane alternatives.
  • Aminolysis of cyclic carbonates offers a promising pathway to polyhydroxyurethanes (PHUs).

Purpose of the Study:

  • To develop a novel shape memory polyhydroxyurethane (PHU) vitrimer with enhanced mechanical properties and chemical recyclability.
  • To demonstrate a green, carbon-neutral synthetic strategy for PHUs using CO2.

Main Methods:

  • Synthesis of bis(six-membered cyclic carbonate) of 4,4'-biphenol (BCC-BP) from bi(1,3-diol) precursors and CO2.
  • Aminolysis of BCC-BP to form PHU vitrimers.
  • Characterization of thermal, mechanical, and dynamic properties.
  • Evaluation of shape memory behavior and chemical recyclability via alcoholysis.

Main Results:

  • Achieved maximum breaking strength of 65 MPa and elongation at break of 452%.
  • Demonstrated significant shape recovery, lifting a load 4700 times its own weight.
  • Successfully regenerated bi(1,3-diol) precursors through alcoholysis, confirming chemical recyclability.

Conclusions:

  • The developed PHU vitrimers possess outstanding combined mechanical performance and shape memory effects.
  • The isocyanate-free, CO2-based synthetic route is environmentally friendly and supports carbon neutrality.
  • This work validates a green approach for designing high-performance, recyclable PHU materials.