We develop a simple and efficient route for the fabrication of water-soluble metallosupramolecular polymers. We demonstrate that the introduction of environment-responsive metal-organic complexes within supramolecular polymers endows the resulting self-assembled nano-objects with outstanding antibacterial activity and may significantly improve the efficacy and safety of selective cancer therapy. Herein, we successfully developed a silver-containing supramolecular polymer (Ag-Cy-J) possessing a hydrophilic Jeffamine backbone and highly sensitive pH-responsive cytosine-silver-cytosine (Cy-Ag-Cy) linkages, which spontaneously self-assemble to produce sterically stabilized spherical nanogels in water. The resulting nanogels exhibit several attractive features such as unique fluorescence behavior in water, highly stable self-assembled structures in biological media, significant antihemolytic capability, highly sensitive pH-responsiveness and broad-spectrum antibacterial activity against various bacteria strains. Importantly, in vitro cellular assays clearly demonstrated Ag-Cy-J nanogels highly selectively target and induce cytotoxicity in cancer cells, without affecting normal cells. The selective cytotoxic activity in cancer cells is attributed to rapid dissociation of the Cy-Ag-Cy complexes within the nanogels in the cancer cell microenvironment, followed by the intracellular release of silver ions and induction of rapid, massive apoptosis. Overall, the pH-sensitive Cy-Ag-Cy complexes within this supramolecular nanogel system may provide a route to remarkably improve the efficacy of both antibacterial and cancer drug therapies.

Tumor microenvironment-responsive nanogels loading antitumor drugs can improve the chemotherapy efficiency due to their suitable size, great hydrophilicity, excellent biocompatibility, and sensitivity to specific stimulation. Herein, a simple and effective strategy of one-pot laser-induced emulsion polymerization at 532 nm was developed to prepare carmofur-loaded nanogels based on biocompatible and temperature/pH-sensitive monomers including polyethylene glycol diacrylate (PEGDA), N-vinylcaprolactam (NVCL), and 2-(dimethylamino) ethyl methacrylate (DMAEMA). The nanogels loading carmofur with dual-stimuli responsive drug release properties were rapidly obtained under laser irradiation (beam diameter 2.5 mm, laser power 60 mW) for only 100 s. These nanogels exhibited an average hydrodynamic diameter of 195.9 nm and a low polydispersity index of 0.115. The effect of monomer ratio on the size, morphology, double-bond conversion, and thermo/pH-sensitivity of nanogels was investigated. The cumulative carmofur release from nanogels at pH 5.0 within 48 h was nearly three times that at pH 7.4, while the release amount at 42 °C was twice that at 25 °C, showing the controlled and sustainable release with the change of pH and temperature. The in vitro release kinetics of carmofur was in accord with first-order release model.

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Journal of Nano Research & Applications