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动态化学装置:通过耦合离子结合/ pH变化诱导的结构转换来调节收缩/伸展分子运动。

Dynamic chemical devices: modulation of contraction/extension molecular motion by coupled-ion binding/pH change-induced structural switching.

作者信息

Barboiu Mihail, Lehn Jean-Marie

机构信息

Institut de Science et d'Ingénierie Supramoléculaires, Université Louis Pasteur, Centre National de la Recherche Scientifique/Unité Mixte de Recherche 7006, 4 Rue Blaise Pascal, 67000 Strasbourg, France.

出版信息

Proc Natl Acad Sci U S A. 2002 Apr 16;99(8):5201-6. doi: 10.1073/pnas.082099199. Epub 2002 Apr 9.

DOI:10.1073/pnas.082099199
PMID:11943865
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC122746/
Abstract

Dynamic chemical devices involve morphological or constitutional modifications in molecular or supramolecular systems, induced by internal or external physical or chemical triggers. Reversible changes in shape result in molecular motions and define motional dynamic devices presenting mechanical-like actions of various types. Suitably designed polyheterocyclic strands such as compounds 1-5 wrap into helical conformations. The binding of lead(II) ions to the coordination subunits contained in the strand leads to complete uncoiling and yields a polymetallic complex presenting a fully extended shape. The addition of a cryptand complexing agent that strongly binds lead(II) ions and releases them under protonation allows a reversible pH-modulation of lead(II) levels in the medium, which in turn induces coiling/uncoiling of the molecular strand. This system thus represents a motional dynamic device which performs a mechano-chemical process, realizing alternating extension/contraction motions triggered by ion binding. It achieves a linear motor-type of action of very large stroke amplitude fueled by ionic processes.

摘要

动态化学装置涉及分子或超分子系统中的形态或结构修饰,这些修饰由内部或外部的物理或化学触发因素诱导。形状的可逆变化会导致分子运动,并定义出呈现各种类型类似机械作用的运动动态装置。经过适当设计的多杂环链,如化合物1 - 5,会缠绕成螺旋构象。铅(II)离子与链中所含配位亚基的结合会导致完全解旋,并产生呈现完全伸展形状的多金属配合物。添加一种能强烈结合铅(II)离子并在质子化时释放它们的穴状配体络合剂,可实现介质中铅(II)水平的可逆pH调节,这进而会诱导分子链的卷曲/解旋。因此,该系统代表了一种执行机械化学过程的运动动态装置,实现了由离子结合触发的交替伸展/收缩运动。它通过离子过程实现了非常大行程幅度的线性电机式作用。