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题名: Self-Assembly of a [2]Pseudorotaxane by an Inchworm-Motion Mechanism
作者: Meng, Zheng1, 2; Wang, Bo-Yang3; Xiang, Jun-Feng3; Shi, Qiang3; Chen, Chuan-Feng1
关键词: inchworm motion ; rotaxanes ; self-assembly ; threading mechanism ; triptycene
刊名: CHEMISTRY-A EUROPEAN JOURNAL
发表日期: 2016-10-01
卷: 22, 期:42, 页:15075-15084
收录类别: SCI
英文摘要: 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.
语种: 英语
内容类型: 期刊论文
URI标识: http://ir.iccas.ac.cn/handle/121111/35637
Appears in Collections:分子识别与功能实验室_期刊论文

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作者单位: 1.Chinese Acad Sci, Inst Chem, CAS Key Lab Mol Recognit & Funct, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Chinese Acad Sci, Inst Chem, Beijing 100190, Peoples R China
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