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Acylated peptides composed of glucagon-like peptide-1 receptor agonists modified with a fatty acid side chain are an important class of therapeutics for type 2 diabetes and obesity but are susceptible to an unusual physical instability in the presence of hydrophobic surfaces, i.e., spontaneous emulsification, also known as ouzo formation in practice. In this work, light scattering, small-angle X-ray scattering, and circular dichroism measurements are used to characterize the physical properties of the semaglutide colloidal phase, including size distribution, shape, secondary structure, internal structure, and internal composition, as a function of solution physico-chemical conditions. The existence and size of the colloids formed are successfully predicted by a classical Rayleigh model, which identifies the parameters controlling their size and formation. Colloid formation is found to be catalyzed by hydrophobic surfaces, and formation rates are modeled as an autocatalytic reaction, enabling the formation of a master curve for various surfaces that elucidates the mechanism. Surfaces differ due to differences in surface wettability, which can be correlated with Hansen solubility parameters. This work provides insights into this unusual colloidal phenomenon and guides the peptide synthesis process and drug product formulation in the pharmaceutical industry. [ABSTRACT FROM AUTHOR]

A novel shear thickening suspoemulsion is formulated and studied with a new rheo-microscope instrument. The experimental fluid system is comprised of a immiscible blend of Newtonian, low molecular weight poly(dimethylsiloxane) and a shear thickening suspension of colloidal silica in poly(ethylene glycol). The blend is studied as a function of composition where phase inversion is evident at low shear rates and is found to be shear rate dependent. A shear thickening viscosity curve is observed when blends comprised of shear thickening fluid dispersed as droplets are subjected to high shear rates. Dispersing a continuously shear thickening fluid, Øsilica= 0.42, results in continuously shear thickening response from the blend. Dispersing a discontinuously shear thickening fluid, Øsilica= 0.51, results in bulk shear thickening that can also be discontinuous. Shear thickening in the final suspoemulsion is consistently first detected at ØSTF= 0.2, with the magnitude of shear thickening being dependent on the particle concentration in the STF phase. The onset of shear thickening also corresponds with the formation of extended droplet structures in the fluid. The complex properties of these suspoemulsions and the ability to formulate dispersed droplet morphologies in this mixture are shown to result from the underlying shear thickening rheology of the dispersed phase.

Model aluminosilicate (N‐A‐S‐H) gel systems give insight to the complex reaction occurring in alkali‐activated binders, allowing for more precise control over chemical composition and exhibiting simpler kinetics. Small angle neutron scattering, oscillatory rheology, and solid‐state NMR were used to characterize N‐A‐S‐H gel samples and relate structure, chemical composition, and rheology. Aluminum concentration was varied in the gel samples at fixed silica and sodium concentration. Past the percolation point, the gel develops in two regimes distinct in structure and rheological behavior. The first gel regime is characterized by increase in modulus and initial formation of fractal structures following a diffusion‐limited monomer‐cluster aggregation mechanism. The second gel regime at higher aluminum concentrations is characterized by a modulus plateau and structure development via reaction‐limited aggregation of existing clusters. NMR data indicate a saturation of aluminum in the network at the transition between gel regimes, which may be pH driven. Understanding the structure‐property relationships critical to formation of the N‐A‐S‐H gel can give valuable insight to the reaction mechanism in alkali‐activated binders and the influence of chemical composition on resultant structure and mechanical properties. [ABSTRACT FROM AUTHOR]