Yang Ying, Lin Rijia, Ge Lei, Hou Lei, Bernhardt Paul, Rufford Thomas E, Wang Shaobin, Rudolph Victor, Wang Yaoyu, Zhu Zhonghua
School of Chemical Engineering, The University of Queensland, Brisbane 4072, Australia.
Dalton Trans. 2015 May 7;44(17):8190-7. doi: 10.1039/c4dt03927k.
The incorporation of Lewis base sites and open metal cation sites into metal-organic frameworks (MOFs) is a potential route to improve selective CO2 adsorption from gas mixtures. In this study, three novel amino-functionalized metal-organic frameworks (MOFs): Mg-ABDC [Mg3(ABDC)3(DMF)4], Co-ABDC [Co3(ABDC)3(DMF)4] and Sr-ABDC [Sr(ABDC)(DMF)] (ABDC = 2-aminoterephthalate) were synthesized by solvothermal reactions of 2-aminoterephthalic acid (H2ABDC) with magnesium, cobalt and strontium metal centers, respectively. Single-crystal structure analysis showed that Mg-ABDC and Co-ABDC were isostructural compounds comprising two-dimensional layered structures. The Sr-ABDC contained a three-dimensional motif isostructural to its known Ca analogue. The amino-functionalized MOFs were characterized by powder X-ray diffraction, thermal gravimetric analysis and N2 sorption. The CO2 and N2 equilibrium adsorption capacities were measured at different temperatures (0 and 25 °C). The CO2/N2 selectivities of the MOFs were 396 on Mg-ABDC, 326 on Co-ABDC and 18 on Sr-ABDC. Both Mg-ABDC and Co-ABDC exhibit high heat of CO2 adsorption (>30 kJ mol(-1)). The Sr-ABDC displays good thermal stability but had a low adsorption capacity resulting from narrow pore apertures.
将路易斯碱位点和开放金属阳离子位点引入金属有机框架（MOF）是提高从混合气体中选择性吸附二氧化碳的一条潜在途径。在本研究中，通过2-氨基对苯二甲酸（H2ABDC）分别与镁、钴和锶金属中心的溶剂热反应，合成了三种新型氨基功能化金属有机框架（MOF）：Mg-ABDC [Mg3(ABDC)3(DMF)4]、Co-ABDC [Co3(ABDC)3(DMF)4] 和 Sr-ABDC [Sr(ABDC)(DMF)] （ABDC = 2-氨基对苯二甲酸酯）。单晶结构分析表明，Mg-ABDC 和 Co-ABDC 是具有二维层状结构的同构化合物。Sr-ABDC 包含一种与其已知钙类似物同构的三维结构单元。通过粉末X射线衍射、热重分析和N2吸附对氨基功能化MOF进行了表征。在不同温度（0和25°C）下测量了CO₂和N₂的平衡吸附容量。这些MOF对CO₂/N₂的选择性在Mg-ABDC上为396，在Co-ABDC上为326，在Sr-ABDC上为18。Mg-ABDC和Co-ABDC均表现出较高的CO₂吸附热（>30 kJ mol⁻¹）。Sr-ABDC表现出良好的热稳定性，但由于孔径狭窄导致吸附容量较低。
