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首页> 外文期刊>Chemistry: A European journal >Self-Assembly of a [2]Pseudorotaxane by an Inchworm-Motion Mechanism
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Self-Assembly of a [2]Pseudorotaxane by an Inchworm-Motion Mechanism

机译：ch运动机制自组装[2]假轮烷。

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摘要

The threading of biomolecules through pores or channels in membranes is important to validate the physiological activities of cells. To aid understanding of the controlling factors required for the translocation in space with confined size and distorted conformation, it is desirable to identify experimental systems with minimized complexity. We demonstrate the mechanism of a linear guest L1 threading into a tris(crown ether) host TC with a combinational distorted cavity to form a triply interlocked [2]pseudorotaxane 3in[L1 subset of TC]. An inchworm-motion mechanism is proposed for the process. For the forward-threading steps that lead to the formation of higher-order interlocked species, guest L1 must adopt a bent conformation to find the next crown ether cavity. Two simplified models are applied to investigate the self-assembly dynamic of 3in-[L1 subset of TC]. Kinetic NMR spectroscopic and molecular dynamics (MD) studies show that formation of the singly penetrated species is fast, whereas formation of the doubly and triply threaded species is several orders of magnitude slower. During threading the freedom of both the guest L1 and host TC gradually decrease due to their interactions. This results in a significant entropy effect for the threading dynamic, which is also observed for the threading of a biomolecular chain through a channel.
机译：生物分子穿过膜中的孔或通道的穿线对于验证细胞的生理活性很重要。为了帮助理解空间受限且构象变形的空间易位所需的控制因素，希望找出具有最小复杂性的实验系统。我们演示了线性客体L1插入具有组合畸变腔的三（冠醚）宿主TC形成三联互锁[2]假轮烷3in [TC L1子集]的机制。提出了一种蠕虫运动机制。对于导致形成更高阶互锁物种的前移步骤，来宾L1必须采用弯曲构型才能找到下一个冠醚腔。应用两个简化模型研究3in- [TC的L1子集]的自组装动力学。动力学NMR光谱和分子动力学（MD）研究表明，单渗透物质的形成速度很快，而双螺纹和三重螺纹物质的形成速度要慢几个数量级。在线程化期间，来宾L1和主机TC的自由度由于它们的交互而逐渐减小。这对穿线动力学产生显着的熵效应，对于通过通道穿入生物分子链也观察到了熵效应。

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