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Multifunctional nanoplatforms developed from natural polymers and graphene oxide (GO) with enhanced biological/physicochemical features have recently attracted attention in the biomedical field. Herein, a new multifunctional near-infrared (NIR) light-, pH- and magnetic field-sensitive hybrid nanoplatform (mGO@AL-g-PHPM@ICG/EP) is developed by combining iron oxide decorated graphene oxide nanosheets (mGO) and poly(2-hydroxypropylmethacrylamide) grafted alginate (AL-g-PHPM) copolymer loaded with indocyanine green (ICG) and etoposide (EP) for chemo/phototherapy. The functional groups, specific crystal structure, size, morphology, and thermal stability of the nanoplatform were fully characterized by XRD, UV, FTIR, AFM/TEM/FE-SEM, VSM, DSC/TG, and BET analyses. In this platform, the mGO and ICG, as phototherapeutic agents, demonstrate excellent thermal effects and singlet oxygen production under NIR-light (808 nm) irradiation. The XRD and DSC analysis confirmed the amorphous state of the ICG/EP in the nanoparticles. In vitro photothermal tests proved that the mGO@AL-g-PHPM@ICG/EP nanoparticles had outstanding light stability and photothermal conversion ability. The in vitro release profiles presented NIR light-, pH- and magnetic field-controlled EP/ICG release behaviors. In vitro experiments demonstrated the excellent antitumor activity of the mGO@AL-g-PHPM@ICG/EP against H1299 tumor cells under NIR laser. Benefiting from its low-cost, facile preparation, and good dual-modal therapy, the mGO@AL-g-PHPM@ICG/EP nanoplatform holds great promise in multi-stimuli-sensitive drug delivery and chemo/phototherapy.

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Recently, pH-responsive nanogels are playing progressively important roles in cancer treatment. The present study focuses on designing and developing pH-responsive alginate-based nanogels to achieve a controlled release of etoposide (Et) while enhancing its hydrophilicity. Alginate (ALG) is grafted with 2-hydroxypropyl methacrylamide (HPMA) through a microwave-supported method, and the chemical structure of the graft copolymer (ALG-g-PHPMA) was verified by 1H/13C NMR and FTIR techniques. The ALG-g-PHPMA and anticancer drug-loaded ALG-g-PHPMA@Et nanogels were obtained using an emulsion method, and their structures were characterized through FTIR, TG/DSC, AFM/TEM, BET, and DLS analyses. The ALG-g-PHPMA nanogels demonstrated a good drug encapsulation efficiency (79.60 %), displaying a pH-dependent release profile and an in vitro accelerated release of Et compared to the ALG nanogels. Thermal and BET analyses revealed enhanced stability, surface area, and porosity volume of the alginate nanogels. The grafting of PHPMA chains onto alginate altered the surface topology of the ALG nanogels, resulting in lower surface roughness. Furthermore, cytotoxicity tests showed the high biocompatibility of the ALG-g-PHPMA copolymer and its nanogels. The ALG-g-PHPMA@Et nanogels exhibited a higher anticancer effect on lung cancer (H1299) cells than free etoposide. These results suggest that the ALG-g-PHPMA nanogels can be applied as a pH-dependent nanoplatform for delivering anticancer drugs.

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In the last decade, interest in the development of new graft copolymers based on natural polysaccharides has grown remarkably due to their potential applications in the wastewater treatment, biomedical, nanomedicine, and pharmaceutical fields. Herein, a novel graft copolymer of κ-carrageenan with poly(2-hydroxypropylmethacrylamide) (κ-Crg-g-PHPMA) was synthesized using a 'microwave induced' technique. The synthesized novel graft copolymer has been well characterized in terms of FTIR, 13C NMR, molecular weight determination, TG, DSC, XRD, SEM, and elemental analyses, taking κ-carrageenan as a reference. The graft copolymers' swelling characteristics were investigated at pH 1.2 and 7.4. The results of swelling studies displayed that the incorporation of PHPMA groups on κ-Crg provides increasing hydrophilicity. The effect of PHPMA percentage in the graft copolymers and pH of the medium on the swelling percentage was studied and the findings exhibited that swelling ability increased with the increment in PHPMA percentage and pH of the medium. The best swelling percentage was attained at pH = 7.4 and a grafting percentage of 81 % reaching 1007 % at the end of 240 min. Moreover, cytotoxicity of the synthesized κ-Crg-g-PHPMA copolymer was assessed on the L929 fibroblast cell line and obtained to be non-toxic.

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In the last two decades, the utilization of magnetic nanospheres in intelligent polymeric structures have received increased attention of researchers in numerous biomedical applications. Here, hybrid nanostructured triple-responsive magnetic nanospheres (κ-Car-g-P(AA/DMA)@Fe3O4) containing inorganic iron oxide core (Fe3O4) and organic graft copolymeric shell based on κ-carrageenan (κ-Car) and poly(acrylic acid/dimethylaminoethyl methacrylate) (P(AA/DMA)) were synthesized by microwave induced co-precipitation technique. The structure, size, surface morphology, magnetic property and stability of synthesized κ-Car-g-P(AA/DMA)@Fe3O4 magnetic nanospheres were characterized using FTIR, UV, XRD, TEM, Zeta-sizer, and VSM. κ-Car-g-P(AA/DMA)@Fe3O4 nanospheres were loaded with 5-Fluorouracil (5-FU) as an antineoplastic drug, and their 5-FU release behavior was explored in diverse graft yields, pH values, temperatures and in the existence of an alternating magnetic field. The κ-Car-g-P(AA/DMA)@Fe3O4 nanospheres demonstrated pH-, thermo-, and magnetic field-responsive 5-FU release with good biocompatibility and excellent anticancer activity. In addition, 5-FU release under 50 mT magnetic field reached to 100% within 4 h. This work exhibits that hybrid nanospheres have a triple stimuli-responsive influence, which is of principal importance for the future design and application of multi-functional responsive platforms to develop externally stimulated release of active agents and their healthcare capability.

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A binary graft copolymerization of dimethylaminoethyl methacrylate (DMAEMA) and acrylic acid (AA) onto κ-carrageenan (CG) was performed by using microwave irradiation in the presence of 4,4'-Azobis(4-cyanovaleric acid) (ACVA). The structure of the CG-g-P(DMAEMA/AA) copolymers was confirmed using 13C NMR, FTIR, DSC/TGA and XRD. The effects of the DMAEMA/AA ratio, the microwave power and irradiation duration, and the concentrations of CG and ACVA on grafting yield and grafting efficiency were all investigated, and the best values of them were found to be 150% and 85%, respectively. The lower critical solution temperatures (LCST) for CG-g-P(DMAEMA/AA) copolymers at various pH conditions were determined, and when the pH value of the medium was increased from 1.2 to 10, the LCST of the copolymer decreased from 53 °C to 39 °C. Moreover, swelling performance of the copolymers under various pH conditions was examined, and it was observed that the swelling ratio of the copolymer increased with a decrease in the pH value of the medium.

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