Abstract
HighlightsThe formation of manganese oxide induces self-assembly of block copolymers to form polymeric vesicles.The polymeric vesicles possessed strong stability and high drug loading capacity.The drug-loaded polymeric vesicles have been demonstrated, especially in in vivo studies, to exhibit a higher efficacy of tumor suppression without known cardiotoxicity.Molecular self-assembly is crucially fundamental to nature. However, the aqueous self-assembly of polymers is still a challenge. To achieve self-assembly of block copolymers [(polyacrylic acid–block–polyethylene glycol–block–polyacrylic acid (PAA68–b–PEG86–b–PAA68)] in an aqueous phase, manganese oxide (MnO2) is first generated to drive phase separation of the PAA block to form the PAA68–b–PEG86–b–PAA68/MnO2 polymeric assembly that exhibits a stable structure in a physiological medium. The polymeric assembly exhibits vesicular morphology with a diameter of approximately 30 nm and high doxorubicin (DOX) loading capacity of approximately 94%. The transformation from MnO2 to Mn2+ caused by endogenous glutathione (GSH) facilitates the disassembly of PAA68–b–PEG86–b–PAA68/MnO2 to enable its drug delivery at the tumor sites. The toxicity of DOX-loaded PAA68–b–PEG86–b–PAA68/MnO2 to tumor cells has been verified in vitro and in vivo. Notably, drug-loaded polymeric vesicles have been demonstrated, especially in in vivo studies, to overcome the cardiotoxicity of DOX. We expect this work to encourage the potential application of polymer self-assembly.
Highlights
In nature, self-assembly is one of the most crucial approaches that enables the building of micro- and nanostructures [1]
The P AA68–b–PEG86–b–PAA68 triblock copolymer was synthesized using a combination of acylation reaction, atomic transfer radical polymerization (ATRP), and hydrolysis reaction (Fig. S1)
A simple and efficient aqueous self-assembly strategy was investigated for the construction of polymeric vesicles
Summary
Self-assembly is one of the most crucial approaches that enables the building of micro- and nanostructures [1]. We describe the use of the self-assembly approach in an aqueous phase in the fabrication of polymeric vesicles with high stability for selective delivery of anticancer agents. Compared to the silica/organosilica cross-linked block copolymer architectures [22], the PAA68–b–PEG86–b–PAA68/ MnO2 vesicles can respond to GSH and weak acidic conditions to unload their cargos These polymeric vesicles were further degraded to hydrophilic linear polymers and M n2+ ions after effectively delivery (Scheme 1). Through the self-assembly of copolymers by the formation of MnO2 in an aqueous phase, polymeric micelles with controlled morphology and stability were fabricated for the selective delivery of anticancer agents, which may be extended to the development of polymeric architectures
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