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Charge-conversional click polyprodrug nanomedicine for targeted and synergistic cancer therapy.

Polyprodrug nanomedicines hold great potential for combating tumors. However, the functionalization of polyprodrug nanomedicines to improve therapeutic efficacy is restricted by conventional polymerization methods. Herein, we fabricated a charge-conversional click polyprodrug nanomedicine system by metal-free azide-alkyne cycloaddition click polymerization (AACCP) for targeted and synergistic cancer therapy. Specifically, Pt(IV) prodrug-backboned diazide monomer, DMC prodrug-pendent diazide monomer, dialkyne-terminated PEG monomer and azide-modified folate were click polymerized to obtain the target polyprodrug (P1). P1 could self-assemble into nano-micelles (1-NM), where PEG was the hydrophilic shell with folate on the surface, Pt(IV) and DMC prodrugs as the hydrophobic core. Taking advantage of PEGylation and folate-mediated tumor cell targeting, 1-NM achieved prolonged blood circulation time and high tumor accumulation efficiency. Tumor acidic microenvironment-responsive cleavage and cascade activation of pendant DMC prodrug induced surface charge conversion of 1-NM from negative to positive, which promoted tumor penetration and cellular internalization of the remaining 1-NM. After internalization into tumor cells, the reduction-responsive activation of Pt(IV) prodrug to Pt(II) further showed synergetic effect with DMC for enhanced apoptosis. This first designed charge-conversional click polyprodrug nanomedicine exhibited targeted and synergistic efficacy to suppress tumor proliferation in living mice bearing human ovarian tumor model.

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