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Anion-Driven Conformational Polymorphism in Homochiral Helical Coordination Polymers
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2009-08-05 , DOI: 10.1021/ja901154p
Guozan Yuan 1 , Chengfeng Zhu 1 , Yan Liu 1 , Weimin Xuan 1 , Yong Cui 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2009-08-05 , DOI: 10.1021/ja901154p
Guozan Yuan 1 , Chengfeng Zhu 1 , Yan Liu 1 , Weimin Xuan 1 , Yong Cui 1
Affiliation
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Three homochiral 3D frameworks are assembled based on periodically ordered arrays of helices built from axial chiral 3,3'-bipyridine-5,5',6,6'-tetramethyl-2,2'-dimethoxy-1,1'-biphenyl ligands and linearly coordinated Ag(I) ions. The aggregation behavior of silver salts and the ditopic ligand in solutions was investigated by a variety of techniques, including (1)H NMR, UV-vis, CD, GPC and MALDI-TOF. The cationic polymer skeleton exhibits an unprecedented conformational polymorphism in the solid-state, folding into two-, three- and four-fold helices with NO(3)(-), PF(6)(-) and ClO(4)(-) as the counteranion, respectively. The two-fold helices cross-link via argentophilic Ag-Ag interactions to form sextuple helices, which lead to a three-dimensional (3D) chiral framework. The three-fold or four-fold helices, on the other hand, self-associates in pairs to form three-dimensional tubular architectures. This anion-dependent self-assembly behavior can be rationalized by considering the sizes, geometries and binding abilities of the counteranions and subsequent chain conformation to minimize steric repulsions and maximize secondary interactions.
中文翻译：
同手性螺旋配位聚合物中阴离子驱动的构象多态性
基于由轴向手性 3,3'-bipyridine-5,5',6,6'-四甲基-2,2'-二甲氧基-1,1'-联苯配体构建的周期性有序螺旋阵列组装了三个同手性 3D 框架和线性配位的 Ag(I) 离子。溶液中银盐和双位配体的聚集行为通过多种技术进行研究，包括 (1) H NMR、UV-vis、CD、GPC 和 MALDI-TOF。阳离子聚合物骨架在固态中表现出前所未有的构象多态性，折叠成具有 NO(3)(-)、PF(6)(-) 和 ClO(4)(- ) 分别作为抗衡阴离子。双重螺旋通过亲银 Ag-Ag 相互作用交联形成六重螺旋，从而形成三维 (3D) 手性框架。另一方面，三重或四重螺旋，自结合成对形成三维管状结构。这种依赖于阴离子的自组装行为可以通过考虑抗衡阴离子的大小、几何形状和结合能力以及随后的链构象来合理化，以最大限度地减少空间排斥并最大限度地提高二次相互作用。
更新日期：2009-08-05
中文翻译：
同手性螺旋配位聚合物中阴离子驱动的构象多态性
基于由轴向手性 3,3'-bipyridine-5,5',6,6'-四甲基-2,2'-二甲氧基-1,1'-联苯配体构建的周期性有序螺旋阵列组装了三个同手性 3D 框架和线性配位的 Ag(I) 离子。溶液中银盐和双位配体的聚集行为通过多种技术进行研究，包括 (1) H NMR、UV-vis、CD、GPC 和 MALDI-TOF。阳离子聚合物骨架在固态中表现出前所未有的构象多态性，折叠成具有 NO(3)(-)、PF(6)(-) 和 ClO(4)(- ) 分别作为抗衡阴离子。双重螺旋通过亲银 Ag-Ag 相互作用交联形成六重螺旋，从而形成三维 (3D) 手性框架。另一方面，三重或四重螺旋，自结合成对形成三维管状结构。这种依赖于阴离子的自组装行为可以通过考虑抗衡阴离子的大小、几何形状和结合能力以及随后的链构象来合理化，以最大限度地减少空间排斥并最大限度地提高二次相互作用。
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