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7417689 
Journal Article 
Regulating vesicle bilayer permeability and selectivity via stimuli-triggered polymersome-to-PICsome transition 
Wang, X; Yao, C; Zhang, G; Liu, S; , 
2020 
1 
Nature Communications
EISSN: 2041-1723 
NATURE PUBLISHING GROUP 
LONDON 
11 
1 
1524 
English 
32251282 
WOS:000522193100008 
Compared to liposomes, polymersomes of block copolymers (BCPs) possess enhanced stability, along with compromised bilayer permeability. Though polyion complex vesicles (PICsomes) from oppositely charged block polyelectrolytes possess semipermeable bilayers, they are unstable towards physiologically relevant ionic strength and temperature; moreover, permselectivity tuning of PICsomes has remained a challenge. Starting from a single component diblock or triblock precursor, we solve this dilemma by stimuli-triggered chemical reactions within pre-organized BCP vesicles, actuating in situ polymersome-to-PICsome transition and achieving molecular size-selective cargo release at tunable rates. UV light and reductive milieu were utilized to trigger carboxyl decaging and generate ion pairs within hydrophobic polymersome bilayers containing tertiary amines. Contrary to conventional PICsomes, in situ generated ones are highly stable towards extreme pH range (pH 2-12), ionic strength (~3 M NaCl), and elevated temperature (70 °C) due to multivalent ion-pair interactions at high local concentration and cooperative hydrogen bonding interactions of pre-organized carbamate linkages. 
copolymer; doxorubicin; drug carrier; fluorouracil; gemcitabine; liposome; nanomaterial; polyelectrolyte; polyion complex vesicle; polymer; polymersome; tertiary amine; unclassified drug; carbamate (ester); electrolyte; molecular analysis; permeability; polymer; Article; bilayer membrane; chemical reaction; controlled study; drug delivery system; drug release; encapsulation; hydrodynamics; hydrogen bond; hydrophobicity; ionic strength; membrane permeability; molecular size; molecular stability; pH; proton transport; ultraviolet radiation 
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