5-Fluorouracil adsorption on graphene oxide-amine modified graphene oxide/hydroxyapatite composite for drug delivery applications: Optimization and release kinetics studies

The present study focused on investigation of graphene oxide/hydroxyapatite (GO/HAp) and amine modified graphene oxide/hydroxyapatite (GO-NH₂/HAp) composites as potential drug carrier agents for 5-Fluorouracil (5-FU). Incorporation of 5-Fluorouracil drug was performed via adsorption through π-π interactions and electrostatic attractions. Modification of graphene oxide was performed for the production of amine modified graphene oxide/hydroxyapatite composite with the intention of enhancing adsorption performance. The X-Ray Diffraction (XRD), Fourier Transform Infrared Spectroscopy (FTIR), Thermogravimetric Analysis (TGA) and zeta potential/particle size analysis were performed for particle characterization while Scanning Electron Microscopy (SEM) and Transmission Electron Microscopy (TEM) analysis were used to analyze detailed morphological properties. Experimental design studies were followed out in order to determine the effect of adsorption parameters including graphene oxide amount, pH and initial drug concentration on 5-Fluorouracil adsorption behavior. Adsorption isotherms of both composites with unmodified and modified GO were best fitted to Freundlich model with R² values of 0.9616 and 0.9682 respectively. The maximum adsorption capacities (q_m) were calculated as 47.3 mg/g and 18.4 for graphene oxide/hydroxyapatite and amine modified graphene oxide/hydroxyapatite composites respectively at pH 2.0. The highest adsorption percentage was obtained for amine modified graphene oxide/hydroxyapatite composite as 40.87 % at pH 2.0 condition. In vitro release kinetic studies revealed that compliance with Higuchi and Korsmeyer-Peppas kinetic models were observed for graphene oxide/hydroxyapatite, whereas zero order and Korsmeyer-Peppas kinetic models pointed out as the well-fitted model for amine modified graphene oxide/hydroxyapatite composite. The release period of 5-FU drug from all composites were continued up to 8-10 h in physiological conditions (pH 7.4, 37 °C) indicating an achieved controlled release. Based on the overall findings, graphene oxide/hydroxyapatite and amine modified graphene oxide/hydroxyapatite composites could be suggested as a potential drug delivery agent for 5-FU in clinical applications.