Post Elias A J, Fletcher Stephen P
Department of Chemistry, Chemistry Research Laboratory, University of Oxford 12 Mansfield Road Oxford OX1 3TA UK
Chem Sci. 2020 Aug 12;11(35):9434-9442. doi: 10.1039/d0sc02768e.
The bottom-up synthesis of artificial, life-like systems promises to enable the study of emergent properties distinctive to life. Here, we report protocell systems generated from phase-separated building blocks. Vesicle protocells self-reproduce through a phase-transfer mechanism, catalysing their own formation. Dissipative self-assembly by the protocells is achieved when a hydrolysis step to destroy the surfactant is introduced. Competition between micelle and vesicle based replicators for a common feedstock shows that environmental conditions can control what species predominates: under basic conditions vesicles predominate, but in a neutral medium micelles are selected for a mechanism which inhibits vesicle formation. Finally, the protocells enable orthogonal reactivity by catalysing formation of an amphiphilic organocatalyst, which after incorporation into the vesicle bilayer enantioselectively forms a secondary product.
自下而上合成人工的、类似生命的系统有望实现对生命所特有的涌现特性的研究。在此,我们报告了由相分离构建块生成的原始细胞系统。囊泡原始细胞通过相转移机制进行自我复制,催化自身的形成。当引入一个水解步骤以破坏表面活性剂时,原始细胞实现了耗散性自组装。基于胶束和囊泡的复制体对共同原料的竞争表明,环境条件可以控制哪种物种占主导:在碱性条件下囊泡占主导,但在中性介质中,由于一种抑制囊泡形成的机制,胶束被选择。最后,原始细胞通过催化两亲性有机催化剂的形成实现了正交反应性,该有机催化剂在掺入囊泡双层后对映选择性地形成次级产物。