Divergent Aminolysis Approach for Constructing Recyclable Self-Blown Nonisocyanate Polyurethane Foams

We report an approach to fabricate self-blown nonisocyanate polyurethane (NIPU) foams by capitalizing on the divergent chemistries of amines with cyclic carbonates─creating the polymer network─and thiolactone─delivering in situ a thiol that generates the blowing agent (CO₂) by reaction with a cyclic carbonate. Multiple linkages (hydroxyurethanes, thioethers, and amides) are created within the polymer network by this domino process. This one-pot methodology furnishes flexible to rigid foams with open-cell morphology at moderate temperature. The foams are easily repurposed into films or structural composites by thermal treatment, showing the first example of recyclable NIPU foams. Remarkably, both the formation and the recycling of the thermoset foams do not necessarily require the use of a catalyst. This facile and robust process is opening new avenues for designing more sustainable PU foams and offers new end-of-life options by facile material repurposing.