Hydrogen-bonded multilayer thin films and capsules based on poly(2-n-propyl-2-oxazoline) and tannic acid : investigation on intermolecular forces, stability, and permeability

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 degrees C, as a hydrogen bonding acceptor are advantageous over other conventional hydrogen-bonded systems because of their high stability in physiological pH range, biocomparibility, 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

Tannic acid-stabilized self-degrading temperature-sensitive poly(2-n-propyl-2-oxazoline)/gellan gum capsules for lipase delivery

In recent years, stable hydrogen-bonded stimuli-responsive polymer capsules have been receiving great interest for the encapsulation and release of sensitive molecules such as lipase enzymes. Compartmental capsules having a liquid gel core stabilized with temperature-responsive hydrogen-bonded multilayers are advantageous over other conventional systems because of their ability to maintain hydrophilic lipase and other hydrophobic compounds in compatible protected molecular vehide environments and prolong their native properties, e.g., in the body. In this work, we report a methodology to stabilize an aqueous liquid gellan gum (GG) core in a capsule using neutral and nontoxic building blocks, namely, poly(2-n-propyl-2-oxazoline) (PnPrOx) and tannic acid (TA), to fabricate temperature-responsive capsules, comprising both lipase and hydrophobic oil droplets. The capsules were fabricated by adding GG droplets to a PnPrOx suspension at a temperature (T) higher than its cloud point temperature (T-CP). Notably, the formed capsules were not stable in water without TA stabilization via hydrogen bonding. Scanning electron microscopy (SEM) investigations of the GG/building block interphase revealed that the collapsed PnPrOx globules that are present above the T-CP stabilized the GG interphase as a Pickering emulsion, while undergoing a configurational transformation into its linear form by interacting with TA in the next step of capsule formation resulting in a smooth PnPrOx/TA capsule wall. The encapsulation efficiencies of the capsules for model fluorescent molecules were found to be 52, 54, and 24% for FITC-dextran, rhodamine, and Nile red, respectively. The stability experiments exhibited swelling and shell thinning at certain locations followed by complete rupture of the capsules at 37 degrees C, while the capsules were stable for several weeks at temperatures below the T-CP of PnPrOx. The capsules were found to be stable in stimulated gastric fluid (SGF) for several hours at 37 degrees C while successfully releasing the encapsulated lipase and Nile red (model hydrophobic compound) in stimulated intestinal fluid (SIF). The released lipase was found to retain almost 100% of its activity. The reported capsules have high potential for use as carriers for encapsulation and release of a variety of payloads ranging from proteins and vitamin supplements to enzymes and probiotics through the oral route of administration

Hydrogen bonded capsules by layer-by-layer assembly of tannic acid and poly(2-n-propyl-2-oxazoline) for encapsulation and release of macromolecules

We report hydrogen bonded capsules with the built-in ability to release loaded bioactive molecules at a physiological temperature of 37 degrees C. The use of neutral and non-toxic building blocks such as tannic acid (TA) and poly(2-n-propyl-2-oxazoline)s (PnPropOx) as hydrogen bonding donor and acceptor results in stable hollow capsules. The temperature induced morphological changes of the shell were investigated using a scanning electron microscope and an optical microscope and revealed pore formation in the shell when the temperature (T) increases beyond the cloud point temperature (T-CP) of PnPropOx. Furthermore, confocal laser scanning microscopic investigation of the hollow capsules loaded with different probes of varying hydrodynamic diameters revealed that the open and closed state of the capsules could be effectively manipulated by varying the incubation time and hydrodynamic radius of the probes. Such hydrogen bonded capsules have high potential for use in temperature responsive sustained drug delivery applications

Laser receptive polyelectrolyte thin films doped with biosynthesized silver nanoparticles for antibacterial coatings and drug delivery applications

We report a simple method to fabricate multifunctional polyelectrolyte thin films to load and deliver the therapeutic drugs. The multilayer thin films were assembled by the electrostatic adsorption of poly (allylamine hydrochloride) (PAH) and dextran sulfate (DS). The silver nanoparticles (Ag NPs) biosynthesized from novel Hybanthus enneaspermus leaf extract as the reducing agent were successfully incorporated into the film. The biosynthesized Ag NPs showed excellent antimicrobial activity against the range of enteropathogens, which could be significantly enhanced when used with commercial antibiotics. The assembled silver nano composite multilayer films showed rupture and deformation when they are exposed to laser. The Ag NPs act as an energy absorption center, locally heat up the film and rupture it under laser treatment. The antibacterial drug, moxifloxacin hydrochloride (MH) was successfully loaded into the multilayer films. The total amount of MH release observed was about 63% which increased to 85% when subjected to laser light exposure. Thus, the polyelectrolyte thin film reported in our study has significant potential in the field of remote activated drug delivery, antibacterial coatings and wound dressings. (C) 2013 Elsevier B.V. All rights reserved

Lysozyme microspheres incorporated with anisotropic gold nanorods for ultrasound activated drug delivery

We report on the fabrication of lysozyme microspheres (LyMs) incorporated with gold nanorods (NRs) as a distinctive approach for the encapsulation and release of an anticancer drug, 5-Fluorouracil (5-FU). LyMs with an average size of 4.0 & PLUSMN; 1.0 mu m were prepared by a sonochemical method and characterized using scanning electron microscopy (SEM), transmission electron microscopy (TEM) and Fourier-transform infrared spectroscopy (FTIR). The LyMs were examined using hydrophobic (nile red) as well as hydrophilic (trypan blue) dyes under confocal laser scanning microscopy (CLSM) to obtain information about the preferential distribution of fluorescent molecules. Notably, the fluorescent molecules were accumulated in the inner lining of LyMs as the core was occupied with air. The encapsulation efficiency of 5-FU for LyMs-NR was found to be-64%. The drug release from control LyMs as well as LyMs incorporated with NRs was investigated under the influence of ultrasound (US) at 200 kHz. The total release for control LyMs and LyMs incorporated with gold NRs was found to be-70 and 95% after 1 h, respectively. The density difference caused by NR incorporation on the shell played a key role in rupturing the LyMs-NR under US irradiation. Furthermore, 5-FU loaded LyMs-NR exhibited excellent anticancer activity against the THP-1 cell line (-90% cell death) when irradiated with US of 200 kHz. The enhanced anti-cancer activity of LyMs-NR was caused by the transfer of released 5-FU molecules from bulk to the interior of the cell via temporary pores formed on the surface of cancer cells, i.e., sonoporation. Thus, LyMs-NR demonstrated here has a high potential for use as carriers in the field of drug delivery, bio-imaging and therapy