Encoding Circularity in Polydiketoenamine Thermoplastics via Oxy-Functionalization

Here, we show that oxy-functionalization at specific sites along polydiketoenamine (PDK) backbones affects depolymerization rates by over three orders of magnitude, due to differences in distortion energies associated with reactive chain conformations in transition states for acidolysis. Site-specific oxy-functionalization, resulting in the fastest rates of acidolysis, opens the door to deconstructing linear PDK chain topologies for the first time, broadening the scope of applications for PDK plastics in a circular manufacturing economy, including chemically recyclable adhesives for a diverse range of surfaces.