Bi, LitingGodwin, BenjaminBaran, MirandaNazir, RashidWulff, Jeremy2024-03-082024-03-082023Bi, L., Godwin, B., Baran, M. J., Nazir, R., & Wulff, J. E. (2023). A cleavable crosslinking strategy for commodity polymer functionalization and generation of reprocessable thermosets. Angewandte Chemie, 135(30). https://doi.org/10.1002/ange.202304708https://doi.org/10.1002/ange.202304708https://hdl.handle.net/1828/16058Covalently crosslinked polymeric materials, known as thermosets, possess enhanced mechanical strength and thermal stability relative to the corresponding uncrosslinked thermoplastics. However, the presence of covalent inter-chain crosslinks that makes thermosets so attractive is precisely what makes them so difficult to reprocess and recycle. Here, we demonstrate the introduction of chemically cleavable groups into a bis-diazirine crosslinker. Application of this cleavable crosslinker reagent to commercial low-functionality polyolefins (or to a small-molecule model) results in the rapid, efficient introduction of molecular crosslinks that can be uncoupled by specific chemical inputs. These proof-of-concept findings provide one potential strategy for circularization of the thermoplastic/thermoset plastics economy, and may allow crosslinked polyolefins to be manufactured, used, reprocessed, and re-used without losing value. As an added benefit, the method allows the ready introduction of functionality into non-functionalized commodity polymers.enAttribution 4.0 InternationalArticleDepartment of Chemistry