Physical autocatalysis driven by a bond-forming thiol-ene reaction
Physical autocatalysis driven by a bond-forming thiol-ene reaction
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DOI：
10.1038/ncomms5607
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发表时间：
2014-09-01
影响因子：
16.6
通讯作者：
Fletcher, Stephen P.
中科院分区：
文献类型：
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作者：
Bissette, Andrew J.;Odell, Barbara;Fletcher, Stephen P.
自催化作用被广泛研究，因为它是生命系统繁殖的中心。像活细胞一样自我繁殖的化学系统将提供对生物学及其从无生命物质中产生的潜在原理的洞察。原细胞模型以表面活性剂边界为特征，以胶束或囊泡的形式提供隔间，任何细胞生命出现的模型都必须考虑到这种边界的出现和演化。在这里，我们描述了一个自催化系统，其中两个相对简单的组分结合在一起形成了更复杂的产品。反应产物聚集成胶束，催化分子自我复制。对反应动力学和聚集行为的研究表明，这是一种胶束介导的物理自催化机制，并导致了第二代体系的合理设计。这些反应是由不可逆键形成驱动的，并为两个简单分子组分的耦合自催化形成原细胞提供了一个工作模型。
Autocatalysis has been extensively studied because it is central to the propagation of living systems. Chemical systems which self-reproduce like living cells would offer insight into principles underlying biology and its emergence from inanimate matter. Protocellular models feature a surfactant boundary, providing compartmentalization in the form of a micelle or vesicle and any model of the emergence of cellular life must account for the appearance, and evolution of, such boundaries. Here, we describe an autocatalytic system where two relatively simple components combine to form a more complex product. The reaction products aggregate into micelles that catalyse molecular self-reproduction. Study of the reaction kinetics and aggregation behaviour suggests a mechanism involving micelle-mediated physical autocatalysis and led to the rational design of a second-generation system. These reactions are driven by irreversible bond formation and provide a working model for the autocatalytic formation of protocells from the coupling of two simple molecular components.