Scientific Achievement

Discovered that proximal amines in crosslinker design enable rapid PDK depolymerization in acid. Moreover, the spacing between amines and the diketoenamine bond offers the ability to fine-tune PDK depolymerization rates.

Significance and Impact

The enhanced and controlled rates of depolymerization address the broader challenge of closing the loop in the chemical recycling of thermosetting plastics to reusable monomers with high selectivity and high efficiency.

Research Details

  • Advanced multipath transition state theory (MP-TST) to accurately connect simulations of diketoenamine acidolysis with experiments, due to the large conformational freedom and strong noncovalent bonds in diketoenamines
  • Achieved 100-fold increase in acidolysis rate with quantitative yields of monomers as well as selective deconstruction of mixed plastics by tailoring relative rates.

Publication Details

R. .Epstein, J. Demarteau, B..A. Helms, K.A. Persson, J. Am. Chem. Soc. 14, 8082–8089 (2023).

DOI: 10.1021/jacs.3c00772