A Series of Metal鈥揙rganic Frameworks Built of Triazolate-Trinuclear and Paddlewheel Units: Solid-Solution Framework Approach for Optimizing CO2 Adsorption and Separation

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• 作者：Mingli Deng ; Feilong Yang ; Pan Yang ; Zhouxun Li ; Jinyu Sun ; Yongtai Yang ; Zhenxia Chen ; Linhong Weng ; Yun Ling ; Yaming Zhou
• 刊名：Crystal Growth & Design
• 出版年：2015
• 出版时间：December 2, 2015
• 年：2015
• 卷：15
• 期：12
• 页码：5794-5801
• 全文大小：687K
• ISSN：1528-7505

文摘

Metal鈥搊rganic frameworks with tunable functional groups like solid-solution have received considerable interest. In this paper, a crs-type structure built of [Zn₃(OH)(dmtrz)₃] triazolate-trinuclear and [Zn₂(COO)₄] paddlewheel units, linked by 3,5-dimethyl-1,2,4-triazolate (dmtrz) and isophthalate (ipa) ligands (named as MAC-4-A), has been used as a prototype framework. Four types of functional groups (B: 5-hydroxyisophthalate, C: 5-aminoisophthalate, D: 5-ethoxyisophthalate, and E: 5-acetamidoisophthalate) have been integrated into the framework, giving isostructures of MAC-4-B to E, respectively. Then, by the solid-solution framework approach, four group samples are prepared, which are MAC-4-AB-x, MAC-4-AC-x, MAC-4-AD-x, and MAC-4-AE-x (x denoted as the ratio of functional ligands in the framework, x = 0.3, 0.5, 0.7), and their CO₂ and N₂ adsorptions have been studied. Our results revealed that the CO₂ capacity is enhanced with the increase of functional groups and then decreases, showing a maximum uptake amount on MAC-4-AB-0.5, MAC-4-AC-0.5, MAC-4-AD-0.7, and MAC-4-AE-0.5 at 298 K and 1 bar, respectively. On the other hand, the calculated selectivity of CO₂ over N₂ gradually increases, giving the highest selectivity after the pore surface is completely functionalized.