AbstractThe influence of chemical structure on mechanical properties of polyurethane ionomers (PU ionomers) has been examined. NCO‐terminated prepolymers prepared from primarily 4,4‐methylene bis(phenyl isocyanate) (MDI) and poly(oxytetramethylene) glycol (PTMO) were chain extended with tertiary amine‐containing diols and the ionomers obtained by quaternization of the prepolymers. TheN‐methyldiethanolamine chain extender gave the best physical properties. The mechanical properties of the PU ionomers were improved with decreasing chain length of PTMO and with increasing concentration of quaternary ammonium centers (or NCO/OH ratio of PU prepolymers). A lower degree of quaternization resulted in a decrease in the mechanical properties of the resulting PU ionomers, but their properties could be improved by post‐quaternization. The adhesion of the PU ionomers to aluminum and the glass transition temperature increased with increasing concentration of quaternizin
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