This study aimed to investigate the pH-induced complexation of silk fibroin (SF) and hyaluronic acid (HA). SF-HA complex coacervation was investigated by monitoring turbidity of the SF-HA system under slow acidification. Gravimetric analysis was performed to determine the yield of complex coacervation and viscosity of the system was measured to study the formation of the complexes at different pH values. The influences of total biopolymer concentration and biopolymer weight ratio on complex coacervation were examined during the analyses. Formation of the complexes was evidenced by the minimum viscosity and the maximum turbidity observed in the system. SF-HA complexes were formed within the pH-window of 2.5-3.5 regardless of the total biopolymer concentration or biopolymer ratio. Complex coacervation of SF-HA showed a reversible behavior and coacervation could be handled even in excess amounts of the biopolymers, which pointed out a non-stoichiometric complexation.

The aim of this study was to explore potential use of the silk fibroin (SF) as an aqueous coating material for theophylline tablets. We have examined the film forming and coating properties of heat-treated fibroin, SF solution having different amounts of polyethylene glycol (PEG) and 1-ethyl-3-(3-dimethyl aminopropyl)carbodiimide (EDC) cross-linked SF. Heat-treated SF material possessed a brittle structure, which resulted in poor film forming and coating properties. The optimum PEG amount in SF solution was determined as 17% (by weight) for an acceptable film forming and zero order release profile. EDC cross-linked SF has shown a very good film forming and coating property with a potential for sustaining the drug release from coated theophylline tablets. Dissolution data for coated theophylline tablets were analyzed using Ritger and Peppas equation to describe the mechanism of drug release. Drug release from the EDC coated tablets followed zero-order kinetics. Release rate constants were found to be 0.26, 0.19, 0.16% min K1 for single-coated, double coated, and triple coated tablets, respectively. These results clearly demonstrated that silk fibroin has high utility as a novel aqueous coating material for controlled release products. q

This study aimed the characterization of the films casted from the aqueous mixtures of the pH induced complexes between silk fibroin (SF) and hyaluronic acid (HA). The insoluble and transparent films were subjected to scanning electron microscopy (SEM) analyses to show the morphological changes. Thermal analysis of complex films was determined by a differential scanning calorimeter (DSC). The changes in the crystalline state were monitored by X-ray diffractometer (XRD) and Fourier transform infrared spectroscopy (FTIR). It was shown that the complexation between HA and SF was dominantly induced by pH. It was shown that the complex films comprised mixtures of crystalline and non-crystalline regions.

a b s t r a c t pH-responsiveness of recently developed silk fibroin (SF) and hyaluronic acid (HA) polyelectrolyte complex (PEC) membranes and their potential use in electro-responsive drug release systems were investigated. PEC membranes were prepared within a narrow pH window (3.0-3.5) for a SF-HA weight ratio of 20 and they were characterized by Atomic Force Microscopy in addition to characterization studies previously reported by our group. Swelling kinetics of the membranes was studied for a pH window of 2.5-7.4 and cyclic swelling test was performed to determine the pH-responsiveness of the membranes. It was shown that membranes swelled more in alkaline conditions and responded to variations in pH of the medium. Electric-stimuli assisted drug permeation and release studies were performed with a custom-made diffusion cell under both passive condition and electric field applied in pulsatile fashion. The instantaneous flux raised as the current was applied and then declined when the current application was terminated, and this process was repeated on subsequent applications. SF-HA complex membranes were found promising for the electric-stimuli-sensitive release of a high molecular weight and charged model drug for a membrane-permeation controlled formulation.

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