Use of molecular interactions and mesoscopic scale transitions to modulate protein-polysaccharide structures.

Mixed protein-polysaccharide structures have found widespread applications in various fields, such as in foods, pharmaceuticals or personal care products. A better understanding and a more precise control over the molecular interactions between the two types of macromolecules leading to an engineering of nanoscale and colloidal building blocks have fueled the design of novel structures with improved functional properties. However, these building blocks often do not constitute the final matrix. Rather, further process operations are used to transform the initially formed structural entities into bulk matrices. Systematic knowledge on the relation between molecular structure design and subsequent mesoscopic scale transitions induced by processing is scarce. This article aims at establishing a connection between these two approaches. Therefore, it reviews not only studies on the underlying molecular interaction phenomena leading to either a segregative or associative phase behavior and nanoscale or colloidal structures, but also looks at the less systematically studied approach of using macroscopic processing operations such as shearing, heating, crosslinking, and concentrating/drying to transform the initially generated structures into bulk matrices. Thereby, a more comprehensive look is taken at the relationship between different influencing factors, namely solvent conditions (i.e. pH, ionic strength), biopolymer characteristics (i.e. type, charge density, mixing ratio, biopolymer concentration), and processing parameters (i.e. temperature, mechanical stresses, pressure) to generate bulk protein-polysaccharide matrices with different morphological features. The need for a combinatorial approach is then demonstrated by reviewing in detail current mixed protein-polysaccharide applications that increasingly make use of this. In the process, open scientific questions that will need to be addressed in the future are highlighted.