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Title: Elastomeric vitrimers from designer polyhydroxyalkanoates with recyclability and biodegradability

Journal Article · · Science Advances
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [5]; ORCiD logo [6];  [7]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [5]; ORCiD logo [1]; ORCiD logo [8]; ORCiD logo [9]
  1. National Renewable Energy Laboratory (NREL), Golden, CO (United States); BOTTLE Consortium, Golden, CO (United States)
  2. National Renewable Energy Laboratory (NREL), Golden, CO (United States); USDOE Agile BioFoundry, Golden, CO (United States)
  3. National Renewable Energy Laboratory (NREL), Golden, CO (United States); BOTTLE Consortium, Golden, CO (United States); Colorado State Univ., Fort Collins, CO (United States)
  4. National Renewable Energy Laboratory (NREL), Golden, CO (United States)
  5. BOTTLE Consortium, Golden, CO (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  6. Argonne National Laboratory (ANL), Argonne, IL (United States); Northwestern Argonne Institute of Science and Engineering, Evanston, IL (United States)
  7. Argonne National Laboratory (ANL), Argonne, IL (United States)
  8. Colorado State Univ., Fort Collins, CO (United States)
  9. National Renewable Energy Laboratory (NREL), Golden, CO (United States); BOTTLE Consortium, Golden, CO (United States); USDOE Agile BioFoundry, Golden, CO (United States)

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.

Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States); Argonne National Laboratory (ANL), Argonne, IL (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Bioenergy Technologies Office (BETO); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO)
Grant/Contract Number:
AC36-08GO28308; AC02-06CH11357; AC02-76SF00515
OSTI ID:
2280788
Report Number(s):
NREL/JA-2A00-87219; MainId:87994; UUID:85c12ffa-cbe5-402f-babb-4a18016589a6; MainAdminID:70884
Journal Information:
Science Advances, Vol. 9, Issue 47; ISSN 2375-2548
Publisher:
AAASCopyright Statement
Country of Publication:
United States
Language:
English

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