Bottlebrush Amphiphilic Polymer Co-Networks

We report the synthesis of novel poly­(ethylene glycol) and poly­(dimethyl siloxane) (PEG and PDMS, respectively) bottlebrush amphiphilic polymer co-networks (B-APCNs) with high gel fractions by a grafting-through ring-opening metathesis polymerization. By varying the volume fraction of PEG (ϕ_PEG), we alter the crystallinity of the networks, achieving complete suppression of PEG crystallinity at ϕ_PEG = 0.35. Furthermore, we show that the crystallinity of these networks can be tuned to alter their moduli. Through dynamic mechanical analysis, we show that the storage and loss moduli of networks with completely suppressed crystallinity (ϕ_PEG = 0.35) behave similarly to a PDMS homopolymer bottlebrush network. These bottlebrush networks represent an unexplored architecture for the field of amphiphilic polymer co-networks.