Department of Applied Chemistry, Graduate School of Engineering, Tokyo University of Agriculture and Technology, 2-24-16 Naka-cho, Koganei, Tokyo 184-8588, Japan.
Department of Bioengineering, Graduate School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan.
J Am Chem Soc. 2023 Mar 22;145(11):6210-6220. doi: 10.1021/jacs.2c12348. Epub 2023 Feb 28.
Biological membranes are functionalized by membrane-associated protein machinery. Membrane-associated transport processes, such as endocytosis, represent a fundamental and universal function mediated by membrane-deforming protein machines, by which small biomolecules and even micrometer-size substances can be transported via encapsulation into membrane vesicles. Although synthetic molecules that induce dynamic membrane deformation have been reported, a molecular approach enabling membrane transport in which membrane deformation is coupled with substance binding and transport remains critically lacking. Here, we developed an amphiphilic molecular machine containing a photoresponsive diazocine core (AzoMEx) that localizes in a phospholipid membrane. Upon photoirradiation, AzoMEx expands the liposomal membrane to bias vesicles toward outside-in fission in the membrane deformation process. Cargo components, including micrometer-size M13 bacteriophages that interact with AzoMEx, are efficiently incorporated into the vesicles through the outside-in fission. Encapsulated M13 bacteriophages are transiently protected from the external environment and therefore retain biological activity during distribution throughout the body via the blood following administration. This research developed a molecular approach using synthetic molecular machinery for membrane functionalization to transport micrometer-size substances and objects via vesicle encapsulation. The molecular design demonstrated in this study to expand the membrane for deformation and binding to a cargo component can lead to the development of drug delivery materials and chemical tools for controlling cellular activities.
生物膜通过膜相关蛋白机制实现功能化。膜相关的运输过程,如内吞作用,是由膜变形蛋白机器介导的基本和普遍的功能,通过这种功能,小分子甚至微米大小的物质可以通过包裹进入膜泡进行运输。尽管已经报道了一些诱导动态膜变形的合成分子,但在膜运输中,膜变形与物质结合和运输相偶联的分子方法仍然严重缺乏。在这里,我们开发了一种含有光响应重氮嗪核心(AzoMEx)的两亲性分子机器,该分子机器可以定位于磷脂膜中。光照射后,AzoMEx 会扩展脂质体膜,从而在膜变形过程中使囊泡偏向于从外向内分裂。货物成分,包括与 AzoMEx 相互作用的微米大小的 M13 噬菌体,通过从外向内分裂被有效地纳入囊泡中。封装的 M13 噬菌体在外部环境中得到短暂保护,因此在给药后通过血液在全身分布过程中保持生物活性。这项研究开发了一种使用合成分子机械进行膜功能化的分子方法,通过囊泡包裹来运输微米大小的物质和物体。本研究中展示的用于扩展膜以变形和结合货物成分的分子设计,可以为控制细胞活动的药物输送材料和化学工具的发展提供指导。