Conventional polymer networks cannot be recycled into high-value products because of permanent, covalent cross-links. Rubber tires illustrate well the issues ranging from economic loss to environmental problems that arise with spent, cross-linked polymers. Here, we developed a one-step strategy using nitroxide-mediated polymerization to synthesize recyclable cross-linked polymers from any monomers or polymers which contain carbon-carbon double bonds that are amenable to radical polymerization. Through this strategy, we designed a network polymer using polybutadiene and styrene as a model for recyclable tires, showing full property recovery after multiple melt-reprocessing recycles; we also produced polymer networks from monomers with good reprocessability and relative uniformity. With dynamic alkoxyamine covalent bond serving as thermally reversible cross-links and simple functionalization of monomers, this one-step strategy provides for both robust, sustainable recyclability of cross-linked polymers and design of networks for advanced technologies.

Recyclable cross-linked polymer networks via one-step controlled radical polymerization

254th National Meeting (2017)

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