The development of thermo-responsive hydrogels with therapeutic capability with spatial and temporal control to support tissue engineering applications is of importance. Therefore, this work demonstrates the synthesis of a novel antioxidant, degradable, nontoxic spatially and temporally controlled thermo-responsive injectable hydrogel. The hybrid hydrogels PVCL-graft-meHA-graft-nutraceutical (PVCL-g-meHA-g-NUTR) and PVCL-crosslinked-meHA-crosslinked-nutraceutical (PVCL-c-meHA-c-NUTR) are composed of Poly (N-vinyl caprolactam) (PVCL,) an alternative to PNIPAAM, methacrylated hyaluronic acid (meHA), and with four different functionalized antioxidants, allyl α-tocopherol (AATP), allyl carvacrol (ACARV), allyl curcumin (ACUR), and allyl catechin (ACAT) were synthesized via free radical polymerization. Several techniques were used to characterize hydrogels. Fourier transform infrared spectroscopy (FTIR) data showed that hydrogel is primarily composed of either graft or crosslinked of PNVCL, one of the nutraceuticals and meHA. FTIR microscopic images confirmed the spatial distribution of PVCL-g-meHA-g-NUTR and PVCL-c-meHA-c-NUTR. In the DPPH and FRAP assays, very low antioxidant activity was observed for GATP, GCARV, GCAT, CATP, CCARV, and CCAT.. On the contrary, GCURC, and CCURC inhibited 11.0 %, 9.0 % of the DPPH radical, and 38.3, 35.0 mM ferrous equivalent FRAP radicals respectively. All hydrogels exhibited lower critical solution temperature (LCST) at ~32°C. Scanning electron microscopy (SEM) images showed that the porous microstructure of meHA and PNVCL homopolymer changed to compact architecture after grafting and became denser after crosslinking. Fluorescent measurement confirmed the highest crosslinking in CCAT hydrogel. The spatial distribution of the series of graft and crosslinked hydrogel was determined using unique ChemiMaps values; C-H (2989 cm−1, 2861 cm−1) and C=O (1698 cm−1,1620 cm−1). We have synthesized and characterized a novel trihybrid hydrogel having an LCST at 32 °C with GCURC and CCURC hydrogels exhibiting elevated antioxidant properties. The combination of FTIR imaging and ,spectroscopy, DSC, and SEM confirms a robust nontoxic, degradable hydrogel via crosslinking polymerization.

Synthesis, characterization, and analysis of free radical scavenging thermo-responsive hydrogels with therapeutic capabilities

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ACS Fall 2022

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