Cleavable Strand‐Fusing Cross‐Linkers as Additives for Chemically Deconstructable Thermosets with Preserved Thermomechanical Properties
Name
Angew Chem Int Ed - 2025 - Zhang - Cleavable Strand‐Fusing Cross‐Linkers as Additives for Chemically Deconstructable.pdf
Size
2.39 MB
Format
Adobe PDF
Checksum (MD5)
faf9075a30e1937988bceb410cdff210
Author(s)
Zhang, Shuyi
Xu, Zhenchuang
Husted, Keith E. L.
Lundberg, David J.
Brown, Christopher M.
Wang, Yuyan
Shieh, Peyton
Ko, Kwangwook
Moore, Jeffrey S.
Johnson, Jeremiah A.
Date Issued
March 27, 2025
Journal
Angewandte Chemie International Edition
Publisher
Wiley
Citation
S. Zhang, Z. Xu, K. E. L. Husted, D. J. Lundberg, C. M. Brown, Y. Wang, P. Shieh, K. Ko, J. S. Moore, J. A. Johnson, Angew. Chem. Int. Ed. 2025, 64 e202500104.
Version
Final published version
Abstract
Permanently cross-linked polymer networks—thermosets—are often difficult to chemically deconstruct. Theinstallation of cleavable bonds into the strands of thermosets using cleavable comonomers as additives can facilitatethermoset deconstruction without replacement of permanent cross-links, but such monomers can lead to reducedthermomechanical properties and require high loadings to function effectively, motivating the design of new and optimalcleavable additives. Here, we introduce “strand-fusing cross-linkers” (SFCs), which fuse two network strands via a four-way cleavable cross-link. SFCs enable deconstruction of model polydicyclopentadiene (pDCPD) thermosets with aslittle as one-fifth of the molar loading needed to achieve deconstruction using traditional cleavable comonomers. SFCsfunction under traditional oven curing as well as low-energy frontal ring-opening metathesis polymerization (FROMP)conditions and lead to improved thermomechanical properties, for example, glass transition temperatures, compared toprior cleavable comonomer designs. This work motivates the development of increasingly improved cleavable additives toenable thermoset deconstruction without compromising material performance.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Massachusetts Institute of Technology. Department of Chemical Engineering
Terms of Use
Creative Commons Attribution-Noncommercial
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1002/anie.202500104
