Department of Chemistry, University of Cambridge , Lensfield Road, Cambridge CB2 1EW, United Kingdom.
Department of Chemistry, University of Sheffield , Sheffield S3 7HF, United Kingdom.
J Am Chem Soc. 2017 May 10;139(18):6461-6466. doi: 10.1021/jacs.7b02345. Epub 2017 May 2.
Membrane signaling proteins transduce information across lipid bilayer membranes in response to extra-cellular binding of chemical messengers. The design of chemical systems that initiate transmembrane signal transduction through molecular binding events is a critical step toward preparing responsive synthetic vesicles. Here we report a vesicle-based signaling system controlled by a metal cation binding event. Competition between binding of copper ions to a membrane-embedded synthetic transducer and to an extra-vesicle messenger (EDTA) is used to control translocation of the transducer across the lipid bilayer. The translocation process is coupled to activation of a catalyst that turns over encapsulated substrates on the inside of the vesicle to generate an amplified fluorescence output signal. External EDTA and copper ions can be used to reversibly switch catalysis inside the vesicles on and off in a controlled manner.
膜信号蛋白在响应细胞外化学信使的结合时，在脂双层膜中传递信息。设计通过分子结合事件引发跨膜信号转导的化学系统是制备响应性合成囊泡的关键步骤。在这里，我们报告了一种基于囊泡的信号系统，该系统受金属阳离子结合事件的控制。铜离子与嵌入膜中的合成转导器和囊外信使（EDTA）的结合竞争用于控制转导器穿过脂质双层的易位。易位过程与一种催化剂的激活偶联，该催化剂使囊泡内部包裹的底物周转，产生放大的荧光输出信号。外部 EDTA 和铜离子可用于以可控的方式在囊泡内可逆地打开和关闭催化作用。
