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DOE OSTI · 2573910

Re-directing mixed-feed deconstruction products to hybrid polyesters: Tolerance windows for commodity plastics reconstruction

Clarke, Ryan W. [National Renewable Energy Laboratory (NREL), Golden, CO (United States); BOTTLE Consortium, Golden, CO (United States)]·Carswell, Briona J. [Florida State Univ., Tallahassee, FL (United States); Florida A & M University, Tallahassee, FL (United States)] (ORCID:0009000799345568)·DesVeaux, Jason S. [BOTTLE Consortium, Golden, CO (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)] (ORCID:0000000179266327)·Hamernik, Levi J. [National Renewable Energy Laboratory (NREL), Golden, CO (United States); BOTTLE Consortium, Golden, CO (United States)]·Lincoln, Clarissa [National Renewable Energy Laboratory (NREL), Golden, CO (United States); BOTTLE Consortium, Golden, CO (United States)]·Konaganti, Vinod K. [Amazon Corporation, Seattle, WA (United States)] (ORCID:0000000220180809)·Alamo, Rufina G. [Florida State Univ., Tallahassee, FL (United States); Florida A & M University, Tallahassee, FL (United States)] (ORCID:000000023061499X)·Knauer, Katrina M. [National Renewable Energy Laboratory (NREL), Golden, CO (United States); BOTTLE Consortium, Golden, CO (United States)] (ORCID:0000000201257532)
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Abstract

Solvolysis is a promising strategy for mixed-feed polyester recycling, but little attention has been given to downstream product separations or the impact of using imperfectly separated monomer mixtures in recycled polymer reconstruction. Here, we challenge the traditional need for high-purity monomers in polycondensation synthesis of engineering thermoplastics. Monomer mixtures are derived from catalyzed methanolysis of polyethylene terephthalate (PET), polybutylene terephthalate (PBT), and polybutylene adipate-co-terephthalate (PBAT), with separation scenarios ranging from high (99:1) to low (90:10) purity. We focus on challenging-to-separate products like ethylene glycol and 1,4-butanediol and evaluate tolerance for comonomer incorporation in recycled hybrid polyesters: polybutylene-co-ethylene terephthalate (PBET) and polybutylene ethylene adipate-co-terephthalate (PBEAT). Evaluations are made between “contaminant” monomer incorporation, and the resulting materials’ thermal properties, crystalline structure, tensile toughness, and rheology. Ultimately, we highlight that despite incorporation of contaminant monomer, high-performance hybrid polyesters of PET, PBT, and PBAT are obtained while reducing the strain of high-throughput separations.

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36 MATERIALS SCIENCEchemical recyclingmonomer separationsplasticspolycondensationpolyesters

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Clarke, Ryan W. [National Renewable Energy Laboratory (NREL), Golden, CO (United States); BOTTLE Consortium, Golden, CO (United States)], Carswell, Briona J. [Florida State Univ., Tallahassee, FL (United States); Florida A & M University, Tallahassee, FL (United States)] (ORCID:0009000799345568), DesVeaux, Jason S. [BOTTLE Consortium, Golden, CO (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)] (ORCID:0000000179266327), Hamernik, Levi J. [National Renewable Energy Laboratory (NREL), Golden, CO (United States); BOTTLE Consortium, Golden, CO (United States)], Lincoln, Clarissa [National Renewable Energy Laboratory (NREL), Golden, CO (United States); BOTTLE Consortium, Golden, CO (United States)], Konaganti, Vinod K. [Amazon Corporation, Seattle, WA (United States)] (ORCID:0000000220180809), Alamo, Rufina G. [Florida State Univ., Tallahassee, FL (United States); Florida A & M University, Tallahassee, FL (United States)] (ORCID:000000023061499X), Knauer, Katrina M. [National Renewable Energy Laboratory (NREL), Golden, CO (United States); BOTTLE Consortium, Golden, CO (United States)] (ORCID:0000000201257532). 2025-06-10. Re-directing mixed-feed deconstruction products to hybrid polyesters: Tolerance windows for commodity plastics reconstruction. https://doi.org/10.1016/j.resconrec.2025.108439

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The transition to a flexible and reliable energy infrastructure, using electro-thermal energy generation technologies such as geothermal, concentrated solar power, and nuclear, usually demands simultaneous advancement of thermal energy storage (TES) to support on-demand electricity generation and industrial applications while mitigating the inherent intermittency of renewable energy sources and power outages from direct energy generation. Among TES technologies, thermochemical energy storage (TCES) based on calcium looping emerges as a compelling high-power energy storage candidate due to its high reaction enthalpy, compatibility with elevated operating temperatures, and abundance of low-cost materials. However, the long-term durability of calcium-based sorbents for TCES is hindered by surface sintering and particle aggregation, leading to performance degradation over repeated thermal cycles. This study explores a moisture hydration-based strategy to regenerate a degraded calcium sorbent and mitigate performance degradation for long duration TCES. The addition of moisture transforms calcium oxide into calcium hydroxide and produces intercalation water layers, associated with a regenerated surface area and reduced calcium oxide crystallite size. Both these effects are beneficial in restoring the sorbents' reactivity for carbonization. Additionally, an optimized hydration-assisted reactivation protocol balances the recovered energy storage capacity with heating penalty required for moisture removal from hydrated samples, resulting in an enhanced energy storage capacity up to 176% compared to benchmark sorbents that undergo cycling without reactivation after 60 cycles. In conclusion, these results highlight the potential of hydration-assisted reactivation to enhance the long-term performance of TCES, providing an effective pathway to advancing electro-thermal storage technologies.

36 MATERIALS SCIENCE↗