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首页> 外文期刊>Crystal growth & design >Modeling PCN-61 and PCN-66: Isostructural rht-Metal?Organic Frameworks with Distinct CO_2 Sorption Mechanisms
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Modeling PCN-61 and PCN-66: Isostructural rht-Metal?Organic Frameworks with Distinct CO_2 Sorption Mechanisms

机译：对PCN-61和PCN-66进行建模：具有明显CO_2吸附机制的同构rht-金属有机框架

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Simulations of CO2 sorption were performed in two members of the highly tunable rht-metal?organic framework (MOF) platform: PCN-61 and PCN-66. These MOFs differ only in the triisophthalate ligand used to synthesize the respective MOFs. In PCN-61, the center of the ligand contains a benzene ring; this ring is substituted with a triphenylamine group in PCN-66. There are two chemically distinct Cu~(2+) ions that comprise the copper paddlewheels, [Cu_2(O_2CR)_4], in all rht-MOFs. One type of Cu~(2+) ion, denoted Cu1, projects into the truncated tetrahedral (T?T_d) and truncated octahedral (T?O_h) cages, while the other Cu~(2+) ion, denoted Cu2, projects into the cuboctahedral (cub?Oh) cages. Electronic structure calculations revealed that, in PCN-61, the Cu2 ions have a significantly higher partial positive charge than the Cu1 ions, whereas the opposite was observed in PCN-66. The simulations revealed that the CO_2 molecules sorb initially onto the Cu~(2+) ions that have the higher partial positive charge, i.e., the Cu2 ions in PCN-61 and the Cu1 ions in PCN-66. This was demonstrated by examining the radial distribution function, g(r), about both Cu~(2+) ions and the modeled structure at low loading for both MOFs. This study provided insights into how differences in the charge distributions about the copper paddlewheels between two isostructural MOFs, arising from the choice of functionality on the ligand, can lead to different CO_2 binding sites at low loading and suggests a more general conceptual framework for controlling sorption through the tuning of MOF electronics.
机译：在高度可调的rh-金属-有机框架（MOF）平台的两个成员中进行了CO2吸附的模拟：PCN-61和PCN-66。这些MOF仅在用于合成各个MOF的三间苯二甲酸配体上有所不同。在PCN-61中，配体的中心含有一个苯环。该环被PCN-66中的三苯胺基取代。在所有rht-​​MOF中，有两个化学上不同的Cu〜（2+）离子组成铜桨轮[Cu_2（O_2CR）_4]。一种表示为Cu1的Cu〜（2+）离子伸入截断的四面体（T？T_d）和截断的八面体（T？O_h）笼中，另一种表示为Cu2（2+）的离子伸入立方八面体（cub？Oh）笼子。电子结构计算表明，在PCN-61中，Cu2离子具有比Cu1离子更高的部分正电荷，而在PCN-66中观察到相反的电荷。模拟结果表明，CO_2分子最初吸附在部分正电荷较高的Cu〜（2+）离子上，即PCN-61中的Cu2离子和PCN-66中的Cu1离子。通过检查两个MOF在低负荷下关于Cu〜（2+）离子的径向分布函数g（r）可以证明这一点。这项研究提供了关于两个同构MOF之间的铜桨轮电荷分布差异的见解，这些电荷是由于配体上官能团的选择而引起的，从而可以在低负载下导致不同的CO_2结合位点，并提出了一个更一般的概念框架来控制吸附通过调整MOF电子设备。

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