Abstract
A microfluidic device was utilized to measure the viscosity gradients formed in carbohydrate solutions of biological significance during desiccation and skin formation. A complementary numerical model employed the free volume theory to predict the concentration-dependent diffusion coefficients and viscosity gradients in concentrated solutions. It was established that the glassy skin formation at the gas-liquid interface played a key role in water entrapment and the formation and persistence of very steep concentration and viscosity gradients in the desiccating solutions. The results of this study highlighted an important phenomenon that should be accounted for during isothermal drying of glass-forming solutions: solutions with high glass transition temperatures, inevitably, dry heterogeneously. In the final product, there are significant spatial variations in water and solute content affecting the storage stability.
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