Abstract
A polyurethane based thermogelling system comprising poly(ω-pentadecalactone) (PPDL), poly(ethylene glycol) (PEG), and poly(propylene glycol) (PPG), termed as PDEP, was synthesized. The incorporation of PPDL lowers critical micelle concentration (CMC) as well as critical gelation concentration (CGC) of the novel copolymers compared to commercial Pluronic® F127. The thermogels showed excellent thermal stability at high temperature up to 80°C, fast response to temperature change in a time frame of less than second, as well as remarkable self-healing properties after being broken at high strain. In vitro drug release studies using docetaxel (DTX) and cell uptake studies using doxorubicin (DOX) show high potential of the hydrogel as drug reservoir for sustainable release profile of payloads, while the in vivo anti-tumor evaluation using mice model of hepatocellular carcinoma further demonstrated the significant inhibition on the growth of tumor. Together with its excellent biocompatibility in different organs, the novel PDPE thermogelling copolymers reported in this work could potentially be utilized as in situ-forming hydrogels for liver cancer therapy.
Highlights
Thermoresponsive hydrogels, known as thermogels, are an important class of physically crosslinked hydrogels whose aqueous polymer solution undergoes reversible sol-gel transition upon temperature change depending on the delicate balance between hydrophilicity and hydrophobicity (Liow et al, 2016)
A series of random multiblock PDEP copolymers with different amounts of PPDL incorporated were synthesized via co-condensation of the macrodiols of PPDL, poly(ethylene glycol) (PEG), and PPG using an aliphatic diisocyanate HDI as coupling reagent in the presence of catalyst DBT linker
The chemical structure of the ω-pentadecalactone, PPDL-diol and PDEP copolymers were verified by 1H nuclear magnetic resonance (NMR) and 13C NMR spectroscopy
Summary
Thermoresponsive hydrogels, known as thermogels, are an important class of physically crosslinked hydrogels whose aqueous polymer solution undergoes reversible sol-gel transition upon temperature change depending on the delicate balance between hydrophilicity and hydrophobicity (Liow et al, 2016). Temperature ramps were performed between 25 and 37◦C and temperature sweeps were performed from 4 to 80◦C at a heating rate of 5◦C·min−1, both with strain fixed at 1% and frequency fixed at 1 Hz. Self-healing properties of the thermogels were evaluated by amplitude sweep test at two predetermined strain for 10 cycles, 300 s at low strain and 120 s at high strain, with temperature fixed at 37◦C and frequency fixed at 1 Hz. One milligram docetaxel was dissolved in an acetone solution together with 10 mg polymer material, dispersed in a phosphate buffer solution, and self-assembled in water to form micelles. All charts and data processing were processed using origin 8 analysis software, the experimental data were expressed as mean and variance, and the significance analysis was analyzed using GraphPad 5.0
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