Porous Lanthanide-Organic Frameworks: Control over Interpenetration, Gas Adsorption, and Catalyst Properties
Porous Lanthanide-Organic Frameworks: Control over Interpenetration, Gas Adsorption, and Catalyst Properties
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多孔镧系元素有机骨架：互穿、气体吸附和催化剂性能的控制
DOI：
10.1021/cg400531j
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发表时间：
2013-07-01
影响因子：
3.8
通讯作者：
Sun, Daofeng
中科院分区：
文献类型：
--
作者：
He, Haiyan;Ma, Huiqing;Sun, Daofeng
以1，4-苯二甲酸(H_2BDC)为原料，合成了两种类晶稀土有机骨架Ln(BDC)(1.5)(DMF)-(H2O)(Ln=Er(1)，Tm(2))。由于二次互穿，两个互穿网络部分堵塞了孔道，没有明显的气体吸附作用。通过使用带有阻碍基团的有机配体或用螯合配体取代配位的溶剂分子来控制互穿，合成了三个与1和2具有相同拓扑结构的非互穿稀土有机骨架：Er-2(Bdc)(3)(Phen)(2)中心点3H(2)O(3)，TM-(Tbdc)(1.5)(DMF)(H2O)中心点2H(2)O(4)，Er-2(Tbdc)(3)(Phen)(2)中心点4DMF中心点2H(2)O(5)。进一步改变反应条件，构建了另外三种不同结构的多孔稀土有机骨架：Tm(BDC)(1.5)(H2O)中心点0.5DMF中心点C2H5OH中心点2H(2)O(6)，Tm-4(BDC)(6)(H2O)(2)(DMF)(C2H5OH)中心点2DMF中心点2H(2)O(7)和Sm(Tbdc)(1.5)(Phen)-(H2O)中心点DMF中心点H2O(8)。对5、6、7和8进行了气体吸附测试，结果表明这些材料具有永久孔隙率。对络合物6的催化性能进行了研究。
Two isomorphous lanthanide-organic frameworks, Ln(BDC)(1.5)(DMF)-(H2O) (Ln = Er (1), Tm (2)) have been synthesized based on 1,4-benzenedicarboxylic acid (H2BDC). Because of the 2-fold interpenetration, the pores are partly blocked and there are no significant gas adsorptions for these two interpenetrating nets. Through control over interpenetration by applying an organic ligand with hindrance groups or replacing coordinated solvent molecules with a chelating ligand, three non-interpenetrating lanthanide-organic frameworks, Er-2(BDC)(3)(phen)(2)center dot 3H(2)O (3), Tm-(TBDC)(1.5)(DMF)(H2O)center dot 2H(2)O (4), Er-2(TBDC)(3)(phen)(2)center dot 4DMF center dot 2H(2)O (5), possessing the same topology with 1 and 2, have been synthesized and characterized. Further changing reaction conditions, three other porous lanthanide-organic frameworks with different structures with 1-5, Tm(BDC)(1.5)(H2O)center dot 0.5DMF center dot C2H5OH center dot 2H(2)O (6), Tm-4(BDC)(6)(H2O)(2)(DMF)(C2H5OH)center dot 2DMF center dot 2H(2)O (7), and Sm(TBDC)(1.5)(phen)-(H2O)center dot DMF center dot H2O (8), have been constructed. Gas sorption measurements for 5, 6, 7, and 8 have been carried out and revealed that these materials possess permanent porosity. The catalytic property for complex 6 has also been studied.