Cluster formation and phase separation in mixtures of sodium κ-carrageenan and sodium caseinate

Mixtures of the polysaccharide κ-carrageenan (KC) and caseinate proteins (SC) from milk were investigated at pH 7 in aqueous solution using confocal scanning laser microscopy and light scattering. Phase separation was observed at higher concentrations and the phase diagram was established. In the mixtures SC was observed to form large aggregates mediated by a relatively small amount of KC. At small KC concentrations the aggregates were initially relatively small and could be characterized by light scattering. At higher KC concentrations or on longer storage at 20 °C, dense clusters with a radius of a few microns were formed that slowly precipitated. The fraction of precipitated protein increased linearly with increasing KC concentration, but was independent of the protein concentration. It increased with decreasing pH from about 20% at pH 8 to 100% at pH 5.