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Material relationships at low temperatures were determined for concentrated surfactant solutions using a combination of rheological experiments, cross-polarized microscopy, calorimetry, and small angle X-ray scattering. A lamellar structured 70 wt% solution of sodium laureth sulfate in water was used as a model system. At cold temperatures (5 °C and 10 °C), the formation of surfactant crystals resulted in extremely high viscosity. The bulk flow behavior of multi-lamellar vesicles (20 °C) and focal conic defects (90 °C) in the lamellar phase was similar. Shear-induced crystallization at temperatures higher than the equilibrium crystallization temperature range resulted in an unusual complex viscosity peak. The effects of processing-relevant parameters including temperature, cooling time, and applied shear were investigated. Knowledge of key low-temperature structure–property-processing relationships for concentrated feedstocks is essential for the sustainable design and manufacturing of surfactant-based consumer products for applications such as cold-water laundry. 

Current methods to develop surfactant phase diagrams are time-intensive and fail to capture the kinetics of phase evolution. Here, the design and performance of a quantitative swelling technique to study the dynamic phase behavior of surfactants are described. The instrument combines cross-polarized optical and short-wave infrared imaging to enable high-resolution, high-throughput, and in situ identification of phases and water compositions. Data across the entire composition spectrum for the dynamics and phase evolution of a binary aqueous non-ionic surfactant solution at two isotherms are presented. This instrument provides pathways to develop non-equilibrium phase diagrams of surfactant systems—critical to predicting the outcomes of formulation and processing. It can be applied to study time-dependent material relationships across a diverse range of materials and processes, including the dissolution of surfactant droplets and the drying of aqueous polymer films.