期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 1, 页码 2091-2099出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c20211
关键词
amphiphile; breathing vesicle; chirality inversion; supramolecular chirality; photoresponsiveness
资金
- Qilu Young Scholarship Funding of Shandong University
- National Natural Science Foundation of China [21872087, 21901145]
- Natural Science Foundation of Jiangsu Province [BK20190209]
- Youth cross-scientific innovation group of Shandong University [2020QNQT003]
This study demonstrates the fabrication of chiral vesicles with photoresponsive supramolecular chirality and structural transformation property, providing unprecedented rational control over supramolecular chirality using photoresponsiveness in vesicular membranes and offering insights into the understanding of biomembrane functions.
Though phospholipids possess chiral centers, their chiral aggregation within bilayer cell membranes has seldom been referred and recognized. Insight into the chirality at higher levels in artificial molecular bilayer assemblies such as vesicles or liposomes is important to better understand biomembrane functions. In this work, we illustrate the fabrication of chiral vesicles with photoresponsive supramolecular chirality and structural transformation property. Cholesterol was conjugated to azobenzene via different spacers, of which molecular chirality underwent transfer to supramolecular level upon aggregation in water. The resultant building block self-assembled into unilamellar vesicles that could respond to light irradiation by showing reversible extension/contraction behavior. Such breathing behavior was accompanied with supramolecular chirality inversion from M- to P-handedness, confirmed by the solid-state crystal structure and electronic circular dichroism spectra based on density functional theory. The vesicle membrane behaves as a matrix to accommodate guest molecules via aromatic interactions, which significantly elevated the UV light resistance with respect to the structural and supramolecular chirality transformation. This work offers an unprecedented rational control over supramolecular chirality using photoresponsiveness in vesicular membranes.
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