Abstract

This paper reports on the rational design of linear sustainable polyurethanes with on-demand depolymerization capabilities and film-forming properties. In this molecular approach, self-immolative urethane motifs are engineered to not only induce rapid degradation in response to an external stimulus via sequential elimination but also provide sufficient inter-chain interactions to yield nanofibers or free-standing films. Amalgamation with various isocyanate or polyol components results in a range of degradable polyurethanes, while doping with europium complexes or carbon black leads to the formation of free-standing hybrid films with photoluminescent or conductive properties, respectively. These films can be reversibly cast using a facile dissolution process, and the predetermined depolymerization products can then be used to generate upcycled materials such as polyurea or polyacrylate films. We believe that our conceptual design for sustainable polyurethanes can be advanced further when combined with conventional engineering techniques to meet industrial and environmental requirements and create desirable materials for contemporary applications.

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