Supporting data for Recyclable crosslinked polyethylene from self-condensing functionalized telechelic polyethylene combining olefin metathesis, hydrogenation, and transesterification

These files contain primary data along with associated output from instrumentation supporting all results reported in Kuenen et al. Recyclable crosslinked polyethylene from self-condensing functionalized telechelic polyethylene combining olefin metathesis, hydrogenation, and transesterification. In Kuenen et al. we found: Crosslinked polyethylene (PEX) is a high-performance thermoset with improved thermomechanical properties compared to its parent linear polymer, polyethylene (PE). The covalent bonds linking PEX, however, prevent efficient recycling or reprocessing, which represents a critical liability with respect to addressing the current global plastic waste crisis. Current strategies to impart recyclability into PEX rely largely on radical chemistries which are difficult to control and lead to side reactions. Here, leveraging the versatility of ruthenium-based catalysis, we prepare self-condensing PE with both telechelic and pendent functional groups (hydroxyls and esters, respectively). Self-condensation of these polymers gives ester-crosslinked PEX which returns to the original linear polymer upon alcoholysis. In addition to chemical recyclability, these materials exhibit stress relaxation at elevated temperatures and we demonstrate their vitrimeric behavior in a simple reprocessing experiment. Together, this study provides a design strategy for recyclable PEX and will inform the design of other self-crosslinkable polymers.