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Nonlinear properties in coordination copolymers derived from randomly mixed ligands

机译：随机混合配体衍生的配位共聚物的非线性特性

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摘要

Random copolymerization is a core strategy of the polymer industry, enabling broad tuning of materials properties through mixing monomers with similar reactivities. In coordination polymers, analogous results have recently been achieved using combinations of isomorphic linkers copolymerized by appropriate metals; in general, the properties of the resultant coordination copolymers can be described as a linear combination of the properties of the constituent building blocks. Here we demonstrate that this need not be the case: coordination copolymerization is a powerful strategy for directing phase formation. For example, reaction of 1,4-benzenedicarboxylic acid with Zn ~(2+) typically affords phase-impure material in N,N-dimethylformamide whereas using an amino functionalized linker leads to pure high surface area material with the structure of MOF-5. However, mixed-linker copolymers derived from a combination of both linkers display surface areas comparable to that of MOF-5 synthesized in N,N-diethylformamide, indicating that even a minor linker component can direct phase selection. In a second illustration, the pore blockage of the bulky group in 9,10-bis(triisopropylsilyloxy)phenanthrene-2,7- dicarboxylate (TPDC) not only suppresses the framework interpenetration of biphenyl-based IRMOF architectures but also blocks adsorption sites, yielding a low surface area material. However, the random coordination copolymerization of Zn~(2+) with a mixture of TPDC and 3,3′,5,5′-tetramethyl-4, 4′-biphenyldicarboxylate (Me_4BPDC) controls the level of framework interpenetration and the degree of pore blockage, resulting in higher surface area (up to ～3000 m~2/g) copolymers than the noninterpenetrated Zn_4O(TPDC)_3 and interpenetrated Zn _4O(Me_4BPDC)_3 frameworks.
机译：无规共聚是聚合物工业的核心战略，它可以通过混合具有类似反应性的单体来广泛调节材料性能。在配位聚合物中，最近通过使用适当金属共聚的同构连接基的组合​​获得了类似的结果。通常，所得配位共聚物的性质可以描述为组成结构单元的性质的线性组合。在这里，我们证明情况并非必须如此：配位共聚是指导相形成的有效策略。例如，1,4-苯二甲酸与Zn〜（2+）的反应通常在N，N-二甲基甲酰胺中提供不纯相的材料，而使用氨基官能化的连接基可得到具有MOF-5结构的纯高表面积材料。但是，衍生自两个接头的组合的混合接头共聚物的表面积与在N，N-二乙基甲酰胺中合成的MOF-5相当，表明即使是较小的接头组分也可以指导相选择。在第二个插图中，9,10-双（三异丙基甲硅烷氧基）菲-2,7-二羧酸酯（TPDC）中大体积基团的孔堵塞不仅抑制了基于联苯的IRMOF结构的骨架互穿，而且还阻止了吸附位点，低表面积材料。然而，Zn〜（2+）与TPDC和3,3'，5,5'-四甲基-4，4'-联苯二甲酸（Me_4BPDC）的混合物的无规共聚控制了骨架互穿度和孔堵塞，导致比未互穿的Zn_4O（TPDC）_3和互穿的Zn _4O（Me_4BPDC）_3骨架更大的表面积（最多〜3000 m〜2 / g）。

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