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DOE OSTI · 3364914

Alkylidene functionalization produces highly recyclable and scalable polyhydroxyalkanoates

Zhou, Li [Colorado State Univ., Fort Collins, CO (United States)] (ORCID:0000000196073877)·May, James H. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enableing Sciences Center] (ORCID:0000000264519106)·Gowda, Ravikumar R. [Colorado State Univ., Fort Collins, CO (United States)] (ORCID:000000016154224X)·Hamernik, Levi J. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enableing Sciences Center] (ORCID:0009000694763130)·Kenny, Jacob K. [BOTTLE Consortium. Golden, CO (United States); National Laboratory of the Rockies (NLR), Golden, CO (United States). Catalytic Carbon Transformation and Scale-Up Center] (ORCID:0000000158832043)·Wang, Lili [Colorado State Univ., Fort Collins, CO (United States)] (ORCID:0009000734343596)·Stubbs, Christopher D. [Colorado State Univ., Fort Collins, CO (United States)] (ORCID:0000000301273417)·Quinn, Ethan C. [Colorado State Univ., Fort Collins, CO (United States)] (ORCID:000000029609806X)·DesVeaux, Jason S. [BOTTLE Consortium. Golden, CO (United States); National Laboratory of the Rockies (NLR), Golden, CO (United States). Catalytic Carbon Transformation and Scale-Up Center] (ORCID:0000000179266327)·Knauer, Katrina M. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enableing Sciences Center] (ORCID:0000000201257532)·Beckham, Gregg T. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enableing Sciences Center] (ORCID:000000023480212X)·Chen, Eugene Y.-X. [Colorado State Univ., Fort Collins, CO (United States)] (ORCID:0000000175123484)
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Abstract

Recyclable polymers that can be produced at scale and readily tuned within the same polymer framework for specific properties are important to achieving a circular materials economy. To this end, synthetic poly(3-hydroxyalkanoate)s (PHAs) have emerged as high-performance, chemically recyclable variants of biological PHAs, but their difficult monomer syntheses and suboptimal recycling efficiencies pose challenges for large-scale deployment. In this study, we investigated a β-isopropylidene PHA, i-PHA, for which the lactone monomer can be synthesized by existing industrial methods from biomass-derived isobutyric acid. The alkylidene substituent prevents decarboxylative degradation typically observed during PHA depolymerization, enabling near-quantitative chemical recycling to monomer. Controlled hydrogenation of the β-isopropylidene side group produces PHAs with diverse performance metrics that are competitive with a range of commodity polymers, spanning strong fibers to ductile thermoplastics to superglue epoxy resins.

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36 MATERIALS SCIENCE54 ENVIRONMENTAL SCIENCESPHAsbeta-isopropylidene PHAlactonespoly(3-hydroxyalkanoate)recyclable polymers

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Zhou, Li [Colorado State Univ., Fort Collins, CO (United States)] (ORCID:0000000196073877), May, James H. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enableing Sciences Center] (ORCID:0000000264519106), Gowda, Ravikumar R. [Colorado State Univ., Fort Collins, CO (United States)] (ORCID:000000016154224X), Hamernik, Levi J. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enableing Sciences Center] (ORCID:0009000694763130), Kenny, Jacob K. [BOTTLE Consortium. Golden, CO (United States); National Laboratory of the Rockies (NLR), Golden, CO (United States). Catalytic Carbon Transformation and Scale-Up Center] (ORCID:0000000158832043), Wang, Lili [Colorado State Univ., Fort Collins, CO (United States)] (ORCID:0009000734343596), Stubbs, Christopher D. [Colorado State Univ., Fort Collins, CO (United States)] (ORCID:0000000301273417), Quinn, Ethan C. [Colorado State Univ., Fort Collins, CO (United States)] (ORCID:000000029609806X), DesVeaux, Jason S. [BOTTLE Consortium. Golden, CO (United States); National Laboratory of the Rockies (NLR), Golden, CO (United States). Catalytic Carbon Transformation and Scale-Up Center] (ORCID:0000000179266327), Knauer, Katrina M. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enableing Sciences Center] (ORCID:0000000201257532), Beckham, Gregg T. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enableing Sciences Center] (ORCID:000000023480212X), Chen, Eugene Y.-X. [Colorado State Univ., Fort Collins, CO (United States)] (ORCID:0000000175123484). 2026-05-07. Alkylidene functionalization produces highly recyclable and scalable polyhydroxyalkanoates. https://doi.org/10.1126/science.aed3914

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