Elastomeric Vitrimers from Designer Polyhydroxyalkanoates with Recyclability and Biodegradability: Article No. eadi1735

Robin Cywar, Chen Ling, Ryan Clarke, Dong Hyun Kim, Colin Kneucker, Davinia Salvachua, Bennett Addison, Sarah Hesse, Christopher Takacs, Shu Xu, Meltem Demirtas, Sean Woodworth, Nicholas Rorrer, Christopher Johnson, Christopher Tassone, Robert Allen, Eugene Chen, Gregg Beckham

Research output: Contribution to journalArticlepeer-review

3 Scopus Citations

Abstract

Cross-linked elastomers are stretchable materials that typically are not recyclable or biodegradable. Medium-chain-length polyhydroxyalkanoates (mcl-PHAs) are soft and ductile, making these bio-based polymers good candidates for biodegradable elastomers. Elasticity is commonly imparted by a cross-linked network structure, and covalent adaptable networks have emerged as a solution to prepare recyclable thermosets via triggered rearrangement of dynamic covalent bonds. Here, we develop biodegradable and recyclable elastomers by chemically installing the covalent adaptable network within biologically produced mcl-PHAs. Specifically, an engineered strain of Pseudomonas putida was used to produce mcl-PHAs containing pendent terminal alkenes as chemical handles for postfunctionalization. Thiol-ene chemistry was used to incorporate boronic ester (BE) cross-links, resulting in PHA-based vitrimers. mcl-PHAs cross-linked with BE at low density (<6 mole %) affords a soft, elastomeric material that demonstrates thermal reprocessability, biodegradability, and denetworking at end of life. The mechanical properties show potential for applications including adhesives and soft, biodegradable robotics and electronics.
Original languageAmerican English
Number of pages15
JournalScience Advances
Volume9
Issue number47
DOIs
StatePublished - 2023

NREL Publication Number

  • NREL/JA-2A00-87219

Keywords

  • elastomeric vitrimers
  • PHAs
  • polyhydroxyalkanoates
  • recyclable soft elastomer

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