Metal-organic frameworks and self-assembled supramolecular coordination complexes: comparing and contrasting the design, synthesis, and functionality of metal-organic materials.
Metal-organic frameworks and self-assembled supramolecular coordination complexes: comparing and contrasting the design, synthesis, and functionality of metal-organic materials.
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DOI：
10.1021/cr3002824
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发表时间：
2013-01-09
期刊：
影响因子：
62.1
通讯作者：
Stang, Peter J.
中科院分区：
文献类型：
--
作者：
Cook, Timothy R.;Zheng, Yao-Rong;Stang, Peter J.
1893年，阿尔弗雷德·维尔纳描述了八面体过渡金属配合物的结构，并为分配当时称为复盐的配位数和氧化态提供了基础。[1]这一术语源于这样的观察：过渡金属离子似乎不仅与中和其电荷的阴离子配体形成键，而且与其他物质形成键，这似乎是不必要的，因为已经达到了中性。这项工作是现代配位化学的起源，极大地拓展了无机化学的领域。通过了解金属离子的优选配位几何形状，现在可以合理地合成方法来安装特定的配体。在过去的119年里，配位化学取得了巨大的发展，使我们对新型配合物和材料的合成、结构和反应性的理解取得了进步，从简单的金属配体配合物到有机金属催化剂和扩展的无机聚合物。近几十年来，出现了两个新的配位化学分支，金属有机框架（MOFs）和超分子配位络合物（SCC）。前者由金属中心或无机簇的无限网络组成，这些网络通过金属-配体配位键由简单的有机连接体桥接。后者包括离散系统，其中精心选择的金属中心与含有多个结合位点的配体进行自组装，这些结合位点以特定的角度取向，以产生有限的超分子复合物。在最基本的层面上，SCC和MOF都共享由有机配体连接的金属节点的设计，这样的结构可以广泛地定义为金属有机材料（MOM）。1.1.超分子配位驱动的自组装基于金属配位的超分子多边形和多面体的出现部分是由于Pedersen及其同事在20世纪60年代的研究，该研究表明互补小分子可以通过非共价相互作用表现出分子间识别。2早期的分子识别系统很简单：可以合成冠醚并选择性地容纳简单的客体离子。新的主体/客体系统迅速跟进，导致更复杂的合奏，如穴状和球状主体与小分子客体，由Lehn 3和Cram开创。[4]控制主体/客体形成的非共价相互作用随后被应用于从分子组分构建大实体。这些结构通过分子内氢键、π-π相互作用、货车范德华力和
In 1893, Alfred Werner described the structure of octahedral transition metal complexes and provided the basis for assigning coordination number and oxidation state to what were then known as double salts. 1 This term arose from the observation that transition metal ions appeared to form bonds not only to anionic ligands with which to neutralize their charge, but also to additional species, which seemed unnecessary since neutrality was already achieved. This work was the origin of modern coordination chemistry and greatly expanded the field of inorganic chemistry. By understanding the preferred coordination geometry about a metal ion, rational synthetic methodologies to install specific ligands was now possible. The past 119 years have witnessed a tremendous growth in coordination chemistry, leading to advances in our understanding of the synthesis, structure, and reactivity of novel complexes and materials from simple metal− ligand complexes to organometallic catalysts and extended inorganic polymers. In recent decades, two new branches of coordination chemistry have emerged, metal− organic frameworks (MOFs) and supramolecular coordination complexes (SCCs). The former are comprised of infinite networks of metal centers or inorganic clusters bridged by simple organic linkers through metal− ligand coordination bonds. The latter encompass discrete systems in which carefully selected metal centers undergo self-assembly with ligands containing multiple binding sites oriented with specific angularity to generate a finite supramolecular complex. On the most basic level, both SCCs and MOFs share the design of metal nodes linked by organic ligands and such constructs can be broadly defined as metal− organic materials (MOMs). 1.1. Supramolecular Coordination-Driven Self-AssemblySupramolecular polygons and polyhedra based on metal− ligand coordination emerged in part as a result of studies in the 1960s by Pedersen and co-workers, which demonstrated that complementary small molecules could exhibit intermolecular recognition via noncovalent interactions. 2 Early molecularrecognition systems were simple: crown ethers could be synthesized and selectively accommodate simple guest ions. New host/guest systems quickly followed, leading to more complex ensembles such as cryptand and spherand hosts with small molecule guests, pioneered by Lehn 3 and Cram. 4 The noncovalent interactions governing host/guest formation were then applied to construct large entities from molecular components. These constructs, held together by intramolecular hydrogen bonding, π− π interactions, van der Waals forces, and
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