Dual-Responsive Lipid Nanotubes: Two-Way Morphology Control by pH and Redox Effects

Lipid nanotubes are the preferred structures for many applications, especially biological ones, and thus have attracted much interest recently. However, there is still a significant need for developing more lipid nanotubes that are reversibly controllable to improve their functionality and usability. Here, we presented a two-way reversible morphology control of the nanotubes formed by the recently designed molecule AQUA (C25H29NO4). Because of its special design, the AQUA has both pH-sensitive and redox-active characters provided by the carboxylic acid and anthraquinone groups. Upon chemical reduction, the nanotubes turned into thinner ribbons, and this structural transformation was significantly reversible. The reduction of the AQUA nanotubes also switched the nanotubes from electrically conductive to insulative. Nanotube morphology can additionally be altered by decreasing the pH below the pKa value of the AQUA, at ∼4.9. Decreasing the pH caused the gradual unfolding of the nanotubes, and the interlayer distance in the nanotube's walls increased. This morphological change was fast and reversible at a wide pH range, including the physiological pH. Thus, the molecular design of the AQUA allowed for an unprecedented two-way and reversible morphology control with both redox and pH effects. These unique features make AQUA a very promising candidate for many applications, ranging from electronics to controlled drug delivery.