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Expanding the Group of Porous Interpenetrated Zr-Organic Frameworks (PIZOFs) with Linkers of Different Lengths
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2016-12-29 00:00:00 , DOI: 10.1021/acs.inorgchem.6b01814
Jann Lippke 1 , Birte Brosent 2 , Tobias von Zons 2 , Erika Virmani 3 , Sebastian Lilienthal 1 , Thomas Preuße 2 , Miriam Hülsmann 2 , Andreas M. Schneider 1 , Stefan Wuttke 3 , Peter Behrens 1 , Adelheid Godt 2
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2016-12-29 00:00:00 , DOI: 10.1021/acs.inorgchem.6b01814
Jann Lippke 1 , Birte Brosent 2 , Tobias von Zons 2 , Erika Virmani 3 , Sebastian Lilienthal 1 , Thomas Preuße 2 , Miriam Hülsmann 2 , Andreas M. Schneider 1 , Stefan Wuttke 3 , Peter Behrens 1 , Adelheid Godt 2
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A Zr-based MOF of the PIZOF type, which consists of two independent and mutually interpenetrating UiO-type frameworks with [Zr6O4(OH)4(O2C)12] nodes, does not only form with a PEPEP dicarboxylic acid (P = phenylene, E = ethynylene). Also dicarboxylic acids with the shorter PPPP and PEPP spacers were found to give PIZOFs, denoted PPPP-PIZOF and PEPP-PIZOF, respectively. Reducing the spacer length even further to a PEEP segment caused a switchover to the formation of a UiO framework. The hysteresis in the Ar sorption curve of PEPP-PIZOF-1 and the slightly too large amount of combustion residue from PPPP-PIZOF-1 suggest structural defects. These hint at a mismatch between the requirement of the optimal linker length for PIZOF formation and the lengths of the PEPP and PPPP dicarboxylates. Nevertheless, these dicarboxylates prefer the formation of a PIZOF over the formation of a UiO structure. PEPEP-PIZOF-2, PPPP-PIZOF-1, and PEPP-PIZOF-1 are stable in air up to 325, 350, and 300 °C, respectively, and have BET surface areas of 2350, 2020, and 1650 m2 g–1, respectively. PEPEP-PIZOFs, even those with very hydrophilic oligo(ethylene glycol) side chains on the linkers, are very stable in water and also during drying from a water-wetted state. On the contrary, PEPP-PIZOF-1 and PPPP-PIZOF-1 that had been exposed to water required exchange of water for ethanol before drying to mostly preserve the framework. The results emphasize the importance of differentiating between framework damage caused through hydrolysis in water and through drying from a water-wetted state. The sensitivity of PEPP-PIZOF-1 and PPPP-PIZOF-1 against drying from a water-wetted state may be the consequence of defects. The drying stability of water-wetted PEPEP-PIZOFs lets us suggest that reversible bending of the linkers contributes to the stability of the PEPEP-PIZOFs.
中文翻译：
使用不同长度的连接子扩展多孔互穿Zr有机框架（PIZOF）的组
PIZOF类型的基于Zr的MOF，该MOF由具有[Zr 6 O 4（OH）4（O 2 C）12的两个独立且互穿的UiO型框架组成。节点，不仅与PEPEP二元羧酸形成（P =亚苯基，E =亚乙炔基）。还发现具有较短PPPP和PEPP间隔基的二元羧酸生成PIZOF，分别表示为PPPP-PIZOF和PEPP-PIZOF。将间隔物的长度进一步减小至PEEP片段，导致转换为UiO框架的形成。PEPP-PIZOF-1的Ar吸附曲线的滞后现象和PPPP-PIZOF-1的燃烧残渣量过大表明存在结构缺陷。这些暗示在PIZOF形成的最佳接头长度的要求与PEPP和PPPP二羧酸酯的长度之间不匹配。然而，这些二羧酸盐优选PIZOF的形成而不是UiO结构的形成。PEPEP-PIZOF-2，PPPP-PIZOF-1和PEPP-PIZOF-1在高达325、350和300°C的空气中稳定，分别为2 g –1。PEPEP-PIZOF，即使在连接基上具有非常亲水的寡（乙二醇）侧链的那些，在水中和从水润湿状态的干燥过程中也非常稳定。相反，已经暴露于水的PEPP-PIZOF-1和PPPP-PIZOF-1需要在干燥前用水交换乙醇，以主要保留框架。结果强调区分因水中水解和从水润湿状态干燥而造成的骨架损伤的重要性。PEPP-PIZOF-1和PPPP-PIZOF-1对从水润湿状态干燥的敏感性可能是缺陷的结果。水润湿的PEPEP-PIZOF的干燥稳定性使我们建议，接头的可逆弯曲有助于PEPEP-PIZOF的稳定性。
更新日期：2016-12-29
中文翻译：
使用不同长度的连接子扩展多孔互穿Zr有机框架（PIZOF）的组
PIZOF类型的基于Zr的MOF，该MOF由具有[Zr 6 O 4（OH）4（O 2 C）12的两个独立且互穿的UiO型框架组成。节点，不仅与PEPEP二元羧酸形成（P =亚苯基，E =亚乙炔基）。还发现具有较短PPPP和PEPP间隔基的二元羧酸生成PIZOF，分别表示为PPPP-PIZOF和PEPP-PIZOF。将间隔物的长度进一步减小至PEEP片段，导致转换为UiO框架的形成。PEPP-PIZOF-1的Ar吸附曲线的滞后现象和PPPP-PIZOF-1的燃烧残渣量过大表明存在结构缺陷。这些暗示在PIZOF形成的最佳接头长度的要求与PEPP和PPPP二羧酸酯的长度之间不匹配。然而，这些二羧酸盐优选PIZOF的形成而不是UiO结构的形成。PEPEP-PIZOF-2，PPPP-PIZOF-1和PEPP-PIZOF-1在高达325、350和300°C的空气中稳定，分别为2 g –1。PEPEP-PIZOF，即使在连接基上具有非常亲水的寡（乙二醇）侧链的那些，在水中和从水润湿状态的干燥过程中也非常稳定。相反，已经暴露于水的PEPP-PIZOF-1和PPPP-PIZOF-1需要在干燥前用水交换乙醇，以主要保留框架。结果强调区分因水中水解和从水润湿状态干燥而造成的骨架损伤的重要性。PEPP-PIZOF-1和PPPP-PIZOF-1对从水润湿状态干燥的敏感性可能是缺陷的结果。水润湿的PEPEP-PIZOF的干燥稳定性使我们建议，接头的可逆弯曲有助于PEPEP-PIZOF的稳定性。
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