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We report the influence of surface morphology and charge of alginate/chitosan (ACA) microcapsules on both the amount of adsorbed protein and its secondary structural changes during adsorption. Variations in surface morphology and charge were controlled by varying alginate molecular weight and chitosan concentration. Plasma fibrinogen (Fgn) was chosen to model this adsorption to foreign surfaces. The surface of ACA microcapsules exhibited a granular structure after incubating calcium alginate beads with chitosan solution to form membranes. The surface roughness of ACA microcapsule membranes decreased with decreasing alginate molecular weight and chitosan concentration. Zeta potential measurements showed that there was a net negative charge on the surface of ACA microcapsules which decreased with decreasing alginate molecular weight and chitosan concentration. The increase in both surface roughness and zeta potential resulted in an increase in the amount of Fgn adsorbed. Moreover, the higher the zeta potential was, the stronger the protein-surface interaction between fibrinogen and ACA microcapsules was. More protein molecules adsorbed spread and had a greater conformational change on rougher surfaces for more surfaces being available for protein to attach.

The chemical modification of the alginate/chitosan/alginate (ACA) hydrogel microcapsule with methoxy poly(ethylene glycol) (MPEG) was investigated to reduce nonspecific protein adsorption and improve biocompatibility in vivo. The graft copolymer chitosan-g-MPEG (CS-g-MPEG) was synthesized, and then alginate/chitosan/alginate/CS-g-MPEG (ACAC(PEG)) multilayer hydrogel microcapsules were fabricated by the layer-by-layer (LBL) polyelectrolyte self-assembly method. A quantitative study of the modification was carried out by the gel permeation chromatography (GPC) technique, and protein adsorption on the modified microcapsules was also investigated. The results showed that the apparent graft density of the MPEG side chain on the microcapsules decreased with increases in the degree of substitution (DS) and the MPEG chain length. During the binding process, the apparent graft density of CS-g-MPEG showed rapid growth-plateau-rapid growth behavior. CS-g-MPEG was not only bound to the surface but also penetrated a certain depth into the microcapsule membranes. The copolymers that penetrated the microcapsules made a smaller contribution to protein repulsion than did the copolymers on the surfaces of the microcapsules. The protein repulsion ability decreased with the increase in DS from 7 to 29% with the same chain length of MPEG 2K. CS-g-MPEG with MPEG 2K was more effective at protein repulsion than CS-g-MPEG with MPEG 550, having a similar DS below 20%. In this study, the microcapsules modified with CS-g-MPEG2K-DS7% had the lowest IgG adsorption of 3.0 ± 0.6 μg/cm(2), a reduction of 61% compared to that on the chitosan surface.