Self-assembly, structure, and dynamic interconversion of metallosupramolecular architectures generated by Pb(II) binding-induced unfolding of a helical ligand

被引:139
作者
Barboiu, M
Vaughan, G
Graff, R
Lehn, JM
机构
[1] Univ Strasbourg, ISIS, Lab Chim Supramol, F-67083 Strasbourg, France
[2] CNRS, Inst Europeen Membranes, IEM 5635, F-34095 Montpellier, France
[3] European Synchrotron Radiat Facil, ESRF, F-38043 Grenoble, France
[4] RMN, Serv Commun, F-67008 Strasbourg, France
关键词
D O I
10.1021/ja0301929
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The binding of lead(11) cations to the terpyridine-type subunits of the helical ligand 1 leads to the self-assembly of different polynuclear metallosupramolecular architectures of nanometric size. Three different entities are generated and may be interconverted as a function of metal/ligand stoichiometry: a [4 x 4]-Pb-16(11) grid-type array 2, a [4 # 4]Pb-12(11) double-cross species 4, and an intermediate complex 3. The structures of 2 and 4 have been confirmed by X-ray crystallography; that of 3 is based on NMR spectral data. The interconversion of the three species generates dynamic diversity and represents an expression of constitutional dynamic chemistry. In the course of ion binding, the helical molecules of ligand 1 unwrap to yield fully extended strands arranged in perpendicular fashion in the architectures 2-4 generated. This process amounts to molecular motions in two directions which confer to the present systems characteristics of two-dimensional nanomechanical devices, capable of performing 2D-contraction/extension motions. The triple features of self-organization, dynamic interconversion, and potential addressability displayed by the processes described trace a self-fabrication approach to nanoscience and nanotechnology.
引用
收藏
页码:10257 / 10265
页数:9
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