Shear-induced orientation of clay nanoplatelets within a physically cross-linked hydrogel based on ionenes, positively charged polyelectrolytes, is studied here. Small angle X-ray scattering measurements (SAXS) are performed under shear within a Couette cell cylinder (rheo-SAXS). As the SAXS signal is dominated by that of the clay component, we follow the evolution of the orientational distribution of the clay nanoplatelets within the hydrogel as a function of shear. We investigate the effect of the clay volume fraction, polyelectrolyte concentration, clay charge location and clay charge density by screening three different types of clay: Wyoming and Arizona montmorillonites and Idaho beidellite. The orientational field of clay nanoplatelets in the gel is shown to strongly depend on the clay charge location and shear rate, whereas it is independent of the clay volume fraction. Approaching the critical gelation concentration of the polyelectrolyte system, these features change drastically.
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