Scalable, biologically sourced depolymerizable polydienes with intrinsically weakened carbon–carbon bonds

Hu, Qixuan; Luo, Xuyi; Ogunfowora, Lawal Adewale; Athaley, Abhay; DesVeaux, Jason S.; Klein, Bruno C.; Xu, Shu; Wu, Pengfei; Wei, Zitang; Lin, Chenjian; Haraniya, Tejaswini; Maiorano, Dominick; Boudouris, Bryan; Mei, Jianguo; Urgun-Demirtas, Meltem; Beckham, Gregg T.; Savoie, Brett M.; Dou, Letian

doi:10.1038/s44286-025-00183-0

Scalable, biologically sourced depolymerizable polydienes with intrinsically weakened carbon–carbon bonds

Journal Article · Wed Feb 12 00:00:00 UTC 2025 · Nature Chemical Engineering

DOI:https://doi.org/10.1038/s44286-025-00183-0· OSTI ID:2561256

^[1]; Luo, Xuyi ^[1]; ^[1]; Athaley, Abhay ^[2]; ^[2]; ^[3]; ^[4]; Wu, Pengfei ^[1]; ^[1]; ^[1]; Haraniya, Tejaswini ^[1]; Maiorano, Dominick ^[1]; ^[1]; ^[1]; Urgun-Demirtas, Meltem ^[5]; ^[6]; ^[1]; ^[1]

Purdue University, West Lafayette, IN (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States); BOTTLE Consortium, Golden, CO (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States); USDOE Agile BioFoundry, Emeryville, CA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States); Northwestern University, Evanston, IL (United States). Argonne Institute of Science and Engineering (NAISE)
Argonne National Laboratory (ANL), Argonne, IL (United States)
BOTTLE Consortium, Golden, CO (United States); USDOE Agile BioFoundry, Emeryville, CA (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Currently, there are few examples of circularly recyclable polymers with all-carbon backbones, probably owing to the challenge of using selective C–C bond cleavage to efficiently produce monomers in recycling processes. Furthermore, here we demonstrate a series of biologically sourced polymuconate polymers synthesized via simple free-radical polymerization that exhibit intrinsically weakened C–C bonds and controlled chemical recycling to monomers. Modifying the side chains and copolymerization ratios allows a wide range of mechanical property tuning, achieving performances comparable to those of commercial plastics such as polystyrene, polymethyl methacrylate and polybutadiene. Techno-economic analysis and life cycle assessment for production at a scale of 100 kilotons per year show that the materials are currently slightly more expensive and environmentally intensive compared with conventional rubbers. However, use of recycled materials via depolymerization can greatly decrease the cost and environmental impacts of polymuconate production (for example, down to US$1.59 per kilogram) to outperform its commercial counterparts.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Bioenergy Technologies Office (BETO)

Grant/Contract Number:: AC02-06CH11357; AC36-08GO28308

OSTI ID:: 2561256

Alternate ID(s):: OSTI ID: 2998905

Report Number(s):: NREL/JA--2A00-89471; MainId:90250; UUID:888642cd-8f6a-4292-8487-2b2215be0ca2; MainAdminId:76696; 199780

Journal Information:: Nature Chemical Engineering, Journal Name: Nature Chemical Engineering Journal Issue: 2 Vol. 2; ISSN 2948-1198

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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