The overall mechanical performance
of ionic elastomers, such as
carboxylated nitrile rubber (XNBR), is largely governed by ionic clusters
formed during the cross-linking of the elastomers with zinc oxide.
These ionic aggregates promote microphase separation and show additional
high-temperature relaxation behavior in dynamic mechanical analysis.
In this study, the nature of these ionic aggregates is explored for
the first time. We find that some zinc-containing compounds, such
as zinc–aluminum-layered double hydroxide and zinc chloride,
do not exhibit any extra high-temperature dynamic mechanical relaxation
processes, although ionic cross-linking reactions with XNBR occur
with all of these zinc compounds. Detailed analysis by Fourier-transform
infrared spectroscopy and dynamic mechanical analysis revealed that
this high-temperature relaxation behavior does not originate from
ionic cross-linking but is associated with the formation of an additional
zinc-enriched polymer phase that arises due to reactions between carboxylic
groups and zinc oxide. Infrared spectroscopic investigation indicates
further that a tetrahedrally coordinated complex facilitates the formation
of a zinc–carboxylic polymeric network. Clear microphase separation
of the ionic polymer in the elastomer could be directly visualized
by transmission electron microscopy for the first time.
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