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Development of structured delivery systems using nanolaminated biopolymer layers

Young-Hee Cho, University of Massachusetts Amherst


The objectives of this study were to carry out research to better understand of the formation, stability and properties of multilayer emulsions containing nano-laminated biopolymer coatings, and to utilize this information to develop food-grade delivery systems. The effect of various preparation parameters on the formation and stability of multilayer emulsions was investigated: droplet concentration; mean droplet diameter; droplet charge; biopolymer concentration. β-lactoglobulin (β-Lg) stabilized emulsions (0.5–10 wt% oil) containing different pectin concentrations (0 to 0.5 wt%) were prepared at pH 7 (where lipid droplets and pectin molecules were both anionic) and pH 3.5 (where lipid droplets were cationic and pectin molecules anionic) and "stability maps" were constructed. At pH 3.5, pectin adsorbed to the droplet surfaces, and the emulsions were unstable to bridging flocculation at intermediate pectin concentrations and unstable to depletion flocculation at high pectin concentrations. At certain droplet and pectin concentrations stable multilayer emulsions could be formed consisting of protein-coated lipid droplets surrounded by a pectin layer. An in situ electro-acoustic (EA) technique was introduced to monitor the adsorption of charged polysaccharides onto oppositely charged protein-coated lipid droplets. The possibility of controlling interfacial and functional characteristics of multilayer emulsions by using mixed polysaccharides (pectin/carrageenan or pectin/gum arabic) was then examined. Emulsions containing different types of polysaccharides had different interfacial characteristics and aggregation stabilities: carrageenan had the highest charge density and affinity for the protein-coated lipid droplets, but gave the poorest emulsion stability. The possibility of assembling protein-rich coatings around lipid droplets was examined using the electrostatic deposition method, with the aim of producing emulsions with novel functionality. Protein-rich biopolymer coatings consisting of β-Lg and pectin were formed around lipid droplets using the electrostatic deposition method. The composite particles formed had relatively small diameters (d < 500 nm) and were stable to gravitational separation. They also remained stable after they were heated above the thermal denaturation temperature of the globular protein and had better stability to aggregation at high salt concentrations (50–200 mM NaCl) than conventional emulsions stabilized by only protein. The effect of a polysaccharide coating on the displacement of adsorbed globular proteins by non-ionic surfactants from lipid droplet surfaces was examined to simulate situations where competitive adsorption occurs. Oil-in-water emulsions stabilized by β-Lg were prepared containing either no pectin (1° emulsions) or different amounts of pectin (2° emulsions). At pH 3.5, where pectin forms a coating around the β-Lg stabilized lipid droplets, the amount of desorbed protein was much less for the 2° emulsion (3%) than for the 1° emulsion (39%), which indicated that the pectin coating inhibited protein desorption by surface active agents. Knowledge gained from this research will provide guidelines for rationally designing emulsion-based delivery systems that are resistant to environmental stresses or with controlled release properties. These delivery systems could be used to encapsulate, protect and release functional components in various industrial products, such as foods, pharmaceuticals, cosmetics, and personal care products.

Subject Area

Agronomy|Physical chemistry|Polymer chemistry

Recommended Citation

Cho, Young-Hee, "Development of structured delivery systems using nanolaminated biopolymer layers" (2009). Doctoral Dissertations Available from Proquest. AAI3379948.