DOE OSTI · 2543100
Cleavable Strand‐Fusing Cross‐Linkers as Additives for Chemically Deconstructable Thermosets with Preserved Thermomechanical Properties
Abstract
Abstract Permanently cross‐linked polymer networks—thermosets—are often difficult to chemically deconstruct. The installation of cleavable bonds into the strands of thermosets using cleavable comonomers as additives can facilitate thermoset deconstruction without replacement of permanent cross‐links, but such monomers can lead to reduced thermomechanical properties and require high loadings to function effectively, motivating the design of new and optimal cleavable 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 as little as one‐fifth of the molar loading needed to achieve deconstruction using traditional cleavable comonomers. SFCs function 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 to prior cleavable comonomer designs. This work motivates the development of increasingly improved cleavable additives to enable thermoset deconstruction without compromising material performance.
Keep this discovery
Explore connections, maps & timelines
Zhang, Shuyi [Department of Chemistry Massachusetts Institute of Technology Cambridge Massachusetts 02139 USA], Xu, Zhenchuang [Beckman Institute for Advanced Science and Technology University of Illinois at Urbana–Champaign Urbana Illinois 61801 USA, Department of Chemistry University of Illinois at Urbana–Champaign Urbana Illinois 61801 USA], Husted, Keith E. L. [Department of Chemistry Massachusetts Institute of Technology Cambridge Massachusetts 02139 USA], Lundberg, David J. [Department of Chemical Engineering Massachusetts Institutes of Technology Cambridge Massachusetts 02139 USA], Brown, Christopher M. [Department of Chemistry Massachusetts Institute of Technology Cambridge Massachusetts 02139 USA], Wang, Yuyan [Department of Chemistry Massachusetts Institute of Technology Cambridge Massachusetts 02139 USA], Shieh, Peyton [Department of Chemistry Massachusetts Institute of Technology Cambridge Massachusetts 02139 USA], Ko, Kwangwook [Department of Chemistry Massachusetts Institute of Technology Cambridge Massachusetts 02139 USA], Moore, Jeffrey S. [Beckman Institute for Advanced Science and Technology University of Illinois at Urbana–Champaign Urbana Illinois 61801 USA, Department of Chemistry University of Illinois at Urbana–Champaign Urbana Illinois 61801 USA], Johnson, Jeremiah A. [Department of Chemistry Massachusetts Institute of Technology Cambridge Massachusetts 02139 USA] (ORCID:0000000191576491). 2025-03-27. Cleavable Strand‐Fusing Cross‐Linkers as Additives for Chemically Deconstructable Thermosets with Preserved Thermomechanical Properties. https://doi.org/10.1002/ange.202500104
Cite the original work for its findings. Save a collection to share your selection of sources.