Unlocking Circularity Through the Chemical Recycling and Upcycling of Lignin-Derivable Polymethacrylates
| Author(s) | Christoff-Tempesta, Ty | |
| Author(s) | O’Dea, Robert M. | |
| Author(s) | Epps, Thomas H. III | |
| Date Accessioned | 2024-02-09T20:46:35Z | |
| Date Available | 2024-02-09T20:46:35Z | |
| Publication Date | 2023-11-22 | |
| Description | This article was originally published in Macromolecules. The version of record is available at: https://doi.org/10.1021/acs.macromol.3c01985. Copyright © 2023 The Authors. Published by American Chemical Society. | |
| Abstract | The synthesis of polymers from lignin-derivable compounds can replace petrochemical building blocks with a renewable feedstock. However, the end-of-life management of bioderivable, nonbiodegradable polymers remains an outstanding challenge. Herein, the chemical recycling and upcycling of two higher-glass-transition temperature (>100 °C), lignin-derivable polymethacrylates, poly(syringyl methacrylate) (PSM) and poly(guaiacyl methacrylate) (PGM), is reported. Neat PSM and PGM were thermally depolymerized to quantitative conversions, producing their constituent monomers at high yields and purity. The deconstruction atmosphere influenced the depolymerization reaction order, and depolymerization was thermodynamically favored in air over N2. Further, monomer bulkiness and volatility impacted depolymerization activation energies. Notably, bulk depolymerization of PSM and PGM was performed without solvent or catalyst to high polymer conversions (89–90 wt %) and monomer yields (86–90 mol %) without byproduct formation. The resultant monomers were then upcycled to narrow-dispersity polymers and phase-separated block polymers. The findings herein offer a pathway to material circularity for higher-performance, lignin-derivable polymethacrylates. | |
| Sponsor | T.C.-T. and T.H.E., III are grateful for the financial support from the Army Research Office under Cooperative Agreement Number W911NF-22-2-0257. R.M.O and T.H.E., III thank the National Science Foundation (NSF) Growing Convergence Research program (NSF GCR CMMI 1934887) in Materials Life Cycle Management for supporting the initial experiments. R.M.O. and T.H.E., III thank the Center for Plastics Innovation, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award DE-SC0021166, for support during the writing of this manuscript. The views and conclusions herein are those of the authors and should not be interpreted as representing the official policies, either expressed or implied, of the Army Research Office, the Department of Energy, the National Science Foundation, or the U.S. Government. | |
| Citation | Christoff-Tempesta, Ty, Robert M. O’Dea, and Thomas H. Epps. “Unlocking Circularity Through the Chemical Recycling and Upcycling of Lignin-Derivable Polymethacrylates.” Macromolecules 56, no. 23 (December 12, 2023): 9796–9803. https://doi.org/10.1021/acs.macromol.3c01985. | |
| ISSN | 1520-5835 | |
| URL | https://udspace.udel.edu/handle/19716/33969 | |
| Language | en_US | |
| Publisher | Macromolecules | |
| dc.rights | Attribution-NonCommercial-NoDerivatives 4.0 International | en |
| dc.rights.uri | http://creativecommons.org/licenses/by-nc-nd/4.0/ | |
| Title | Unlocking Circularity Through the Chemical Recycling and Upcycling of Lignin-Derivable Polymethacrylates | |
| Type | Article |
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