4.8 Article

Hybrid monomer design for unifying conflicting polymerizability, recyclability, and performance properties

Journal

CHEM
Volume 7, Issue 3, Pages 670-685

Publisher

CELL PRESS
DOI: 10.1016/j.chempr.2021.02.003

Keywords

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Funding

  1. Colorado State University (CSU)
  2. U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office (AMO)
  3. Bioenergy Technologies Office (BETO)
  4. National Renewable Energy Laboratory [DE-AC36-08GO28308]

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The article introduces a new hybrid monomer design strategy that combines high ceiling temperature (HCT) and low ceiling temperature (LCT) sub-structures within the same monomer to achieve high polymerizability and depolymerizability. This innovative approach resulted in a polymer with high performance properties, demonstrating that the HCT/LCT hybrid monomer strategy is a powerful method for designing circular polymers with conflicting properties.
Intrinsically recyclable polymers represent a circular economy approach to address plastics problems. However, the design of such circular polymers is challenged by unyielding trade-offs between the monomer's polymerizability and the polymer's depoly-merizability and performance properties. Here, we introduce a hybrid monomer design strategy that synergistically couples a high ceiling temperature (HCT) sub-structure for high polymerizability and performance properties with a low ceiling temperature (LCT) sub-structure for high depolymerizability and recyclability within the same monomer structure. Thus, structural hybridization between HCT e-caprolactone and LCT g-butyrolactone led to an offspring [3.2.1]bicyclic lactone, which exhibits both high polymerizability and depolymerizability, otherwise conflicting properties in a typical monomer. The resulting polymer becomes a high-performance material, and thermal transition temperatures are similar to 200 degrees C higher and tensile modulus 103 higher than its parent polymers. These results demonstrate that the HCT/LCT hybrid monomer strategy is a powerful approach for designing circular polymers where conflicting properties must be exploited and unified.

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