Scientific Achievement
- Researchers in the CUP program found that targeted oxy-functionalization increased acidolysis rates and allowed for efficient deconstruction of linear polydiketoenamine (PDK) chains, imparting chemical recyclability on linear PDK thermoplastics and demonstrating the effects of in-chain functionalities on deconstruction rates
Significance and Impact
- The effect of chain conformation on polymer deconstruction rates and how this can be controlled through remote substituents to cleavable bond sites is largely unexplored. The insights from this study broaden the design possibilities for deconstructable PDKs and other condensation polymers
Research Details
- Relative hydrolysis rates of PDKs with differing sites of oxy-functionalization were evaluated through computational modeling
- A series of PDK resins were synthesized and deconstructed under acidic conditions to verify modeling predictions
- The investigation demonstrated that selective oxy-functionalization of triketone and diamine monomers allowed for deconstruction at faster rates and higher monomer purity as compared to controls
- Additionally, oxy-functionalization was demonstrated to improve strength of PDK thermoplastics used as adhesives for a range of substrates
Publication Details
J. Demarteau, A.R. Epstein, L.J. Reed, N.R. Ciccia, J.F. Hartwig, K.A. Persson, B.A. Helms, Scientific Advances (2025).
Work was performed in the Molecular Foundry, NERSC, and computing resources at NREL.
