A New Approach Toward Metal‐Free Self‐Healing Ionomers Based on Phosphate and Methacrylate Containing Copolymers

Abstract In order to accelerate the progress of the development of new self‐healing ionomers, a new pathway toward fully organic ionomers containing methacrylic acid and phosphate‐based functional groups, respectively, as well as butyl methacrylate as comonomer is presented in the current study. The well‐defined copolymer structures are synthesized using the reversible addition‐fragmentation chain transfer polymerization and further characterized by NMR, size exclusion chromatography as well as titration. Two different metal‐free ionomers as well as one reference K + based ionomer are created and tested. The results of the detailed investigation by NMR, thermal analysis, and rheology are correlated with the scratch‐healing performance in order to identify trends and dependencies leading to preconditions for further improvements.