Toward Efficient Entropic Recycling by Mastering Ring–Chain Kinetics Article Swipe
Jeffrey C. Foster
,
Isaiah T. Dishner
,
Joshua T. Damron
,
Vilmos Kertész
,
Ilja Popovs
,
Tomonori Saito
·
YOU?
·
· 2025
· Open Access
·
· DOI: https://doi.org/10.1021/acs.macromol.4c03090
YOU?
·
· 2025
· Open Access
·
· DOI: https://doi.org/10.1021/acs.macromol.4c03090
Traditional chemical recycling approaches for condensation polymers suffer compounding energy losses and CO2 emissions across multiple polymerization and depolymerization cycles. Entropic recycling can address these energy losses by entrapping free energy within the deconstruction products. Entropic recycling involves depolymerization to macrocyclic monomers, but such processes have not been feasible due to the high dilutions typically required to generate macrocyclic compounds. Here, we leverage selective catalysis to allow entropic recycling at concentrations 20–2000× higher than typical for macrocyclization reactions. We find that Ru-based olefin metathesis catalysts containing bulky iodine ligands significantly bias the ring–chain kinetic product distribution during ring-closing metathesis (RCM) toward the formation of oligomeric cycloalkenes. Further improvements in reaction concentration and macrocycle yield are obtained by using high catalyst loadings and by predisposing the alkene substrates to undergo favorable macrocyclization. These RCM optimizations translate effectively to cyclodepolymerization (CDP) of an olefin-containing polymer, with RCM and CDP affording similar macrocycle product distributions under identical reaction conditions. Macrocycle polymerization by entropy-driven ring-opening metathesis provides much higher molecular weight polymers than condensation polymerization of linear analogues, reducing the time to achieve high molecular weight from hours to minutes and enabling polymerization at room temperature. Finally, our findings re-emphasize the importance of energy consumption during a polymer’s lifecycle and provide a framework for the design of efficient entropic recycling systems.
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Metadata
- Type
- article
- Language
- en
- Landing Page
- https://doi.org/10.1021/acs.macromol.4c03090
- OA Status
- green
- Cited By
- 3
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All OpenAlex metadata
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https://openalex.org/W4407729677Canonical identifier for this work in OpenAlex
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https://doi.org/10.1021/acs.macromol.4c03090Digital Object Identifier
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Toward Efficient Entropic Recycling by Mastering Ring–Chain KineticsWork title
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articleOpenAlex work type
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enPrimary language
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2025Year of publication
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2025-02-19Full publication date if available
- Authors
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Jeffrey C. Foster, Isaiah T. Dishner, Joshua T. Damron, Vilmos Kertész, Ilja Popovs, Tomonori SaitoList of authors in order
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https://doi.org/10.1021/acs.macromol.4c03090Publisher landing page
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YesWhether a free full text is available
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greenOpen access status per OpenAlex
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https://www.osti.gov/servlets/purl/2538032Direct OA link when available
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Kinetics, Chain (unit), Ring (chemistry), Chemistry, Materials science, Thermodynamics, Polymer science, Polymer chemistry, Physics, Organic chemistry, Astronomy, Quantum mechanicsTop concepts (fields/topics) attached by OpenAlex
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3Total citation count in OpenAlex
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| referenced_works | https://openalex.org/W4362657618, https://openalex.org/W3017199550, https://openalex.org/W4400183597, https://openalex.org/W3123866115, https://openalex.org/W2163795898, https://openalex.org/W1896534329, https://openalex.org/W2954217568, https://openalex.org/W2122156490, https://openalex.org/W2100428375, https://openalex.org/W2913584997, https://openalex.org/W2564016101, https://openalex.org/W3138683322, https://openalex.org/W2859861982, https://openalex.org/W2914224351, https://openalex.org/W2497820219, https://openalex.org/W1970776762, https://openalex.org/W4361289851, https://openalex.org/W2783425955, https://openalex.org/W2913335019, https://openalex.org/W3208221000, https://openalex.org/W2117833047, https://openalex.org/W2046777428, https://openalex.org/W4390580438, https://openalex.org/W1967874625, https://openalex.org/W4382794642, https://openalex.org/W4389687611, https://openalex.org/W1855919732, https://openalex.org/W2994651187, https://openalex.org/W1968619057, https://openalex.org/W3152076460, https://openalex.org/W2814239323, https://openalex.org/W302314459, https://openalex.org/W2093800803 |
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