The facile preparation, modular design, and multi‐responsiveness are extremely critical for developing pervasive nanoplatforms to meet heterogeneous applications. Here, cationic nanogels (NGs) are modularly engineered with tunable responsiveness, versatility, and biodegradation. Cationic PVCL‐based NGs with core/shell structure are fabricated by facile one‐step synthesis. The formed PVCL‐NH2 NGs exhibit uniform size, thermal/pH dual‐responsive behaviors, and redox‐triggered degradation. Moreover, the NGs can be employed to modify or/and load with various functional agents to construct multipurpose nanoplatforms in a modular manner. Notably, the novel hybrid structure with copper sulfide (CuS) NPs loaded in the NGs shell is prepared, which leads to higher photothermal conversion efficiency (31.1%) than other CuS randomly loaded NGs reported. By personalized tailoring, these functionalized NGs display fluorescent property, r1 relaxivity, strong near‐infrared (NIR) absorption, good biocompatibility, and targeting specificity. The superior photothermal effect of hybrid NGs (CuS@NGs‐LA) is presented under NIR II over NIR I. Importantly, hybrid NGs encapsulated doxorubicin (CuS@NGs‐LA/DOX) show endogenous pH/redox and exogenous NIR multi‐triggered drug release for efficient photothermal‐chemotherapy, which can completely eliminate advanced tumors and effectively inhibit recurrence. Overall, the pervasive nanoplatforms based on intelligent cationic NGs with tunable responsiveness, versatility, and biodegradation are developed by engineered modular strategy for precision medicine applications.
Nanomedicine has revolutionized disease theranostics by the accurate diagnosis and efficient therapy. Here, the PAMAM dendrimer decorated PVCL-GMA nanogels (NGs) were developed for favorable biodistribution in vivo and enhanced antitumor efficacy of ovarian carcinoma. By an ingenious design, the NGs with a unique structure that GMA-rich domains were localized on the surface were synthesized via precipitation polymerization. After G2 dendrimer decoration, the overall charge is changed from neutral to positive, and the NGs-G2 display the whole charge nature of positively charged corona and neutral core. Importantly, the unique architecture and charge conversion of NGs-G2 have a profound impact on the biodistribution and drug delivery in vivo . As a consequence of this alteration, the NGs-G2 as nanocarriers emerge the highly sought biodistribution of reduced liver accumulation, enhanced tumor uptake, and promoted drug release, resulting in the significantly augmented antitumor efficacy with low side effects. Remarkably, this finding is contrary to some reported work that the nanocarriers with positive charge have preferential liver uptake. Moreover, the NGs-G2 also displayed thermal/pH dual-responsive behaviors, excellent biocompatibility, improved cellular uptake, and stimuli-responsive drug release. Encouragingly, this work demonstrates a novel insight into the strategy for optimizing design, improving biodistribution and enhancing theranostic efficacy of nanocarriers.
Herein we report the synthesis of new reactive stimuli-responsive polymers by RAFT copolymerization of glycidyl methacrylate and three cyclic N-vinyllactam derivatives. The copolymerization process was thoroughly investigated and the influence of the steric hindrance originating from the monomer structure of cyclic N-vinyllactams on the polymerization process and the properties of obtained copolymers were studied. A series of water-soluble copolymers with variable chemical composition, controlled molecular weight and narrow dispersity (Đ) were synthesized and their properties are systematically investigated. Experimentally determined cloud points for different copolymers in aqueous solutions indicate shift of lower critical solution temperature (LCST) to lower values with the increase of GMA content in copolymers and increase of the lactam ring size. The obtained reactive stimuli-responsive copolymers can be efficiently used for encapsulation of cellulase in water-in-oil emulsions forming biohybrid nanogels. The enzymes entrapped in nanogels demonstrated significantly improved resistance against harsh store conditions, chaotropic agents, and organic solvents.
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