Cleavable Additives for Deconstructable, Recyclable Polyurethane Thermosets
Name
cleavable-additives-for-deconstructable-recyclable-polyurethane-thermosets.pdf
Description
Published version
Size
3.6 MB
Format
Adobe PDF
Checksum (MD5)
d802483cb4d286d6fb0889bb15e07fc5
Author(s)
Ko, Kwangwook
Lundberg, David J
Lensch, Valerie L
AlFaraj, Yasmeen S
Husted, Keith EL
Brutman, Jacob P
Alsbaiee, Alaaeddin
Hamilton, Patrick N
Nguyen, Suong T
Johnson, Jeremiah A
Date Issued
July 23, 2025
Journal
ACS Central Science
Publisher
American Chemical Society
Citation
Kwangwook Ko, David J. Lundberg, Valerie L. Lensch, Yasmeen S. AlFaraj, Keith E. L. Husted, Jacob P. Brutman, Alaaeddin Alsbaiee, Patrick N. Hamilton, Suong T. Nguyen, Jeremiah A. Johnson; Cleavable Additives for Deconstructable, Recyclable Polyurethane Thermosets. ACS Cent. Sci. 27 August 2025; 11 (8): 1355–1363.
Version
Final published version
Abstract
Polyurethane (PU) thermosets, particularly those derived from aliphatic components, are challenging to chemically deconstruct due to their permanent cross-linking. Current approaches to impart deconstructability typically rely on complete substitution of network precursors with cleavable analogs, limiting practicality. Cleavable additives (CAs) offer a potentially simple and cost-effective alternative, yet their application has been largely confined to chain-growth networks and remains unexplored in end-linked systems such as PUs. Here, we present a generalizable reverse gel-point theory that predicts the minimum CA loading required for deconstruction of end-linked networks. We validate this framework experimentally through the incorporation of two classes of silyl ether-based CAsbifunctional cleavable strands (BCSs) and trifunctional cleavable junctions (TCJs)into PU thermosets. Both additives enable selective PU dissolution at low loadings (5-12 wt %), with TCJs demonstrating enhanced efficiency. The combined use of BCSs and TCJs also allows fine-tuning of material properties. Furthermore, we show that polyol fragments generated from the deconstruction of TCJ-containing PUs can be chemically repolymerized to regenerate PU materials without loss of mechanical performance over multiple cycles. This work establishes CAs as a viable strategy for advancing PU circularity and offers a foundational framework for their broader application in end-linked polymer networks.
Terms of Use
Creative Commons Attribution
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1021/acscentsci.5c00689
