Abstract
Magnetic nanocomposites are a class of smart materials that have attracted recent interest as drug delivery systems or as medical implants. A new approach toward the biocompatible nanocomposites suitable for remote melting is presented. It is shown that magnetite nanoparticles (MNPs) can be embedded into a matrix of biocompatible thermoplastic dextran esters. For that purpose, fatty acid esters of dextran with adjustable melting points in the range of 30–140 °C were synthesized. Esterification of the polysaccharide by activation of the acid as iminium chlorides guaranteed mild reaction conditions leading to high-quality products as confirmed by Fourier-transform infrared (FTIR) and nuclear magnetic resonance (NMR) spectroscopy as well as by gel permeation chromatography (GPC). A method for the preparation of magnetically responsive bionanocomposites (BNCs) was developed consisting of combined dissolution/suspension of the dextran ester and hydrophobized MNPs in an organic solvent followed by homogenization with ultrasonication, casting of the solution, drying and melting of the composite for a defined shaping. This process leads to a uniform distribution of MNPs in BNC as revealed by scanning electron microscope (SEM). Samples of different geometries were exposed to high-frequency alternating magnetic field (AMF). It could be shown that defined remote melting of such biocompatible nanocomposites is possible for the first time. This may lead to a new class of magnetic remote-control systems, which are suitable for controlled release applications or self-healing materials. BNCs containing biocompatible dextran fatty acid ester melting close to human body temperature were prepared and loaded with Rhodamine B (RhB) or green fluorescent protein (GFP) as model drugs to evaluate their potential use as drug delivery system. The release of the model drugs from the magnetic BNC investigated under the influence of a high-frequency AMF (20 kA/m at 400 kHz) showed that on-demand release is realized by applying the external AMF. The BNC possessed a long-term stability (28 d) of the incorporated iron oxide particles after incubation in artificial body fluids. Temperature-dependent mobility investigations of MNP in the molten BNC were carried out by optical microscopy, magnetometry, alternating current (AC) susceptibility, and Mössbauer spectroscopy measurements. Optical microscopy shows a movement of agglomerates and texturing in the micrometer scale, whereas AC susceptometry and Mössbauer spectroscopy investigations reveal that the particles perform diffusive Brownian motion in the liquid polymer melt as separated particles rather than as large agglomerates. Furthermore, a texturing of MNP in the polymer matrix by a static magnetic field gradient was investigated. First results on the preparation of cross-linkable dextran esters are shown. Cross-linking after irradiation of the BNC prevents melting that can be used to influence texturing procedures.
Design of Magnetic Hydrogels for Hyperthermia and Drug Delivery
