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A Porous Coordination Polymer with Accessible Metal Sites and its Complementary Coordination Action

机译：具有可及金属位点的多孔配位聚合物及其互补配位作用

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摘要

Porous coordination polymers (PCPs) have attracted much attention in recent years,[1] and progress has been achieved in the aspects of controlling stability, porosity, and pore shape/size and with regards to their applications, such as storage,[2] separation,[3] catalysis,[4] and molecular array.[5] To achieve further functionalization of PCPs, much effort has recently been directed at introducing various functional groups to the pore surface of PCPs to which guest molecules can have access, by modification of building blocks, using the approaches of predesign[6] and, recently, postsynthesis.[7] Among these, the immobilization of coordinatively unsaturated metal centers (UMCs) into porous frameworks is very attractive.[8] This is because a combination of PCP characteristics (regularity, high surface area, micropore filling, and shape/size selectivity) and UMC characteristics (Lewis acidity,[ 9] catalytic activity,[10] chromic property,[11] and enhanced sorption property,[12] etc.) can be used to create desirable and sophisticated functionalities. To derive the suggested functions from metal sites on the pore surface, permanent guest-accessibility to the metal sites is essential. However, the unsaturated state of metal ions is highly reactive and often unstable, owing to a lack of the electronic requirements,[13] resulting in a loss of integrity or permanent porosity of the framework, and then guest molecules cannot get access to the metal sites.[2a] A small number of PCPs are precluded from these problems by using rigid Cu paddlewheel cores.[12a, 14] Thus, it should be beneficial to devise alternative methods for retaining both permanent porosity and accessibility/functionality of the metal sites simultaneously. One promising method would be to stabilize the active metal,through complementary coordination-bond cleavage and formation between the framework atoms.
机译：近年来，多孔配位聚合物（PCP）引起了广泛关注，[1]在控制稳定性，孔隙率和孔形状/尺寸以及在其应用（例如储存）方面已经取得了进展，[2]分离，[3]催化，[4]和分子阵列。[5]为了实现PCP的进一步功能化，最近人们进行了很多努力，目的是通过使用预先设计的方法，通过修饰构件，将各种官能团引入客体分子可以进入的PCP的孔表面[6]。后合成。[7]其中，将不饱和配位金属中心（UMC）固定在多孔骨架中是非常有吸引力的。[8]这是因为PCP特性（规则性，高表面积，微孔填充和形状/尺寸选择性）和UMC特性（刘易斯酸度，[9]催化活性，[10]铬性，[11]）和增强的吸附性相结合，[12]等）可用于创建理想且复杂的功能。为了从孔表面的金属位点获得建议的功能，永久性的客人对金属位点的可及性至关重要。但是，由于缺乏电子要求，金属离子的不饱和状态具有很高的反应性，并且常常不稳定，[13]导致骨架完整性或永久孔隙率的损失，然后客体分子无法接近金属[2a]通过使用刚性Cu桨叶铁心，可以避免少量PCP出现这些问题。[12a，14]因此，设计出替代方法来保持金属部位的永久孔隙率和可及性/功能性应该是有益的同时。一种有希望的方法是通过互补的配位键断裂和骨架原子之间的形成来稳定活性金属。

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