Properties and Applications of Reversible Bottlebrush Polymers with a Dithiolane Backbone*

1. Bottlebrush polymers have a unique architecture which leads to a variety of interesting and useful properties. but the scalable synthesis of bottlebrush polymers remains challenging and has focused on limited backbone chemistries. Here, we report the preparation and characterization of bottlebrush polymers containing dithiolane backbones. Using a combination of ATRP and photo-initiated ring opening polymerization, we can produce multi-gram quantities of degradable polydithiolane bottlebrushes with control over side-chain chemistry. We characterize the rheological properties of the resulting bottlebrushes and explore new bottlebrush-based materials. In particular, we develop liquid-crystal bottlebrush elastomer networks which combine the soft elasticity of liquid crystal networks and inherent softness of bottlebrush elastomers. We show that the combination of liquid crystal ordering and bottlebrush architecture results in super-soft elastomeric materials useful for adhesie applications. The stimuli-responsive binding and degradation enables control over adhesive properties. This work demonstrates the unique properties of degradable bottlebrush polymers and reports a new approach to the salable synthesis of bottlebrush polymers and networks.