A new class of ionomers is described wherein ion-pairs bear reactive functionality, thereby facilitating further chemical modification. Halide displacement from brominated poly(isobutylene-co-isoprene) by 1-vinylimidazole is used to prepare ionomer derivatives that can be crosslinked by radical oligiomerization of pendant vinyl groups. The resulting thermosets contain a labile network of imidazolium bromide ion-pair aggregates as well as a stable covalent network. As a result of their hybrid ionic/covalent composition, these thermoset elastomers provide a unique combination of rheological, tensile and stress relaxation properties that cannot be achieved from conventional covalent or ionic networks. © 2013 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2013, 51, 2438–2444
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