Ligand Charge Separation To Build Highly Stable Quasi-Isomer of MOF-74-Zn,Journal of the American Chemical Society

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Ligand Charge Separation To Build Highly Stable Quasi-Isomer of MOF-74-Zn
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2019-06-14 , DOI: 10.1021/jacs.9b04432
Huajun Yang ₁ , Fang Peng ₁ , Candy Dang ₁ , Yong Wang ₂ , Dandan Hu ₂ , Xiang Zhao ₂ , Pingyun Feng ₂ , Xianhui Bu ₁

Affiliation

Built from an unusual high-charge-density ligand 2,5-dioxido-1,4-benzenedicarboxylate (dobdc4-), MOF-74 M (M2dobdc) have unsurpassed gas uptake and separation properties. It is thus intriguing to mimic or replicate such ligand properties in other chemical systems. Here, we show a ligand charge separation (LCS) model that could offer one pathway toward this goal. Two new materials (CPM-74 and -75, corresponding to MOF-74 and IRMOF-74-II, respectively) are presented here to illustrate this concept and its feasibility. Specifically, the dobdc4- ligand in MOF-74 can be conceptually broken down into OH- and obdc3- (H3obdc = 2-hydroxyterephthalic acid), which leads to CPM-74, Zn2(OH)(obdc), that is nearly isomeric with MOF-74-Zn. Different from MOF-74, CPM-74 is made from homohelical rod packing. Moreover, CPM-74 has high hydrothermal and thermal stability uncommon for Zn-MOFs. It contains open Zn sites on 4-coordinated Zn2+ and its isosteric heat of adsorption for CO2 is 22% higher than that of MOF-74-Zn at low pressures.

中文翻译：

配体电荷分离构建高度稳定的 MOF-74-Zn 准异构体

MOF-74 M (M2dobdc) 由不寻常的高电荷密度配体 2,5-二氧化-1,4-苯二甲酸酯 (dobdc4-) 构建而成，具有无与伦比的气体吸收和分离性能。因此，在其他化学系统中模拟或复制此类配体特性是很有趣的。在这里，我们展示了一种配体电荷分离 (LCS) 模型，该模型可以为实现这一目标提供一条途径。这里介绍了两种新材料（CPM-74 和 -75，分别对应于 MOF-74 和 IRMOF-74-II）来说明这一概念及其可行性。具体来说，MOF-74 中的 dobdc4- 配体在概念上可以分解为 OH- 和 obdc3-（H3obdc = 2-羟基对苯二甲酸），这导致 CPM-74，Zn2(OH)(obdc)，它几乎与MOF-74-Zn。与 MOF-74 不同的是，CPM-74 由同螺旋杆填料制成。而且，CPM-74 具有 Zn-MOF 不常见的高水热和热稳定性。它在 4 配位的 Zn2+ 上含有开放的 Zn 位点，在低压下，它对 CO2 的等量吸附热比 MOF-74-Zn 高 22%。

更新日期：2019-06-14

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