Hydrogen-Bonded Multilayer Thin Films and Capsules Based on Poly(2-n-propyl-2-oxazoline) and Tannic Acid:...

In recent years, hydrogen-bonded multilayer thin films and capsules based on neutral and nontoxic building blocks have been receiving interest for the design of stimuli-responsive drug delivery systems and for the preparation of thin-film coatings. Capsule systems made of tannic acid (TA), a natural polyphenol, as a hydrogen bonding donor and poly(2-n-propyl-2-oxazoline) (PnPropOx), a polymer with lower critical solution temperature around 25 °C, as a hydrogen bonding acceptor are advantageous over other conventional hydrogen-bonded systems because of their high stability in physiological pH range, biocompatibility, good renal clearance, stealth behavior, and stimuli responsiveness for temperature and pH. In this work, investigations on the interactive forces in TA/PnPropOx capsule formation, film thickness, stability, and permeability are reported. The multilayer thin films were assembled on quartz substrates, and the layer-by-layer film growth was investigated by UV-vis spectroscopy, atomic force microscopy, and profilometry. Hollow capsules were fabricated by sequential coating of TA and PnPropOx onto CaCO₃ colloidal particles, followed by template dissolution with a 0.2 M ethylenediaminetetraacetic acid solution. The obtained capsules and multilayer thin films were found to be stable over a wide pH range of 2-9. It is found that both hydrogen bonding and hydrophobic interactions are responsible for the enhanced stability of the capsules at higher pH range. Swelling followed by dissolution of the capsules was observed at a pH value lower than 2, while the capsules undergo shrinking at a pH value higher than 8 and finally transform into a particle-like morphology before dissolution. The TA/PnPropOx capsules reported here could be used as a temperature-responsive drug delivery system in controlled drug delivery applications.