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基于联苯四甲酸构筑的镁(Ⅱ)金属有机框架的合成及其CO2吸附和催化转化性能

Mg(Ⅱ) metal-organic frameworks based on biphenyltetracarboxylic acid:Synthesis and CO2 adsorption and catalytic conversion performance

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【作者】 时文娟; 卢瑜珂; 李秀媛; 侯磊; 王尧宇;

【Author】 SHI Wenjuan;LU Yuke;LI Xiuyuan;HOU Lei;WANG Yaoyu;Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education,College of Chemistry & Materials Science,Northwest University;School of Materials and Chemical Engineering,Xi′an Technological University;

【通讯作者】 侯磊;

【机构】 西北大学化学与材料科学学院,合成与天然功能分子教育部重点实验室; 西安工业大学材料与化工学院;

【摘要】 在溶剂热合成条件下,利用含有胺基基团的有机羧酸配体4,4’-二胺基-[1,1’-联苯]-3,3’,5,5’-四甲酸(H4L)与Mg2+离子反应,制备了一例三维金属有机框架{[Mg2(L)(DMA)(H2O)2]·2DMA·H2O}n(Mg-MOF,DMA=N,N-二甲基乙酰胺)。通过X射线单晶衍射、元素分析、热重分析等确定了Mg-MOF的结构和稳定性,并深入探究了其CO2吸附和催化转化性能。结果表明:Mg-MOF属于单斜晶系,P21/n空间群,a=1.399 88(15) nm,b=1.400 49(15) nm,c=1.768 57(19) nm,β=94.307(2)°。Mg-MOF具有4-连接的(42·84)-ant拓扑网,含有胺基基团修饰的一维孔道,而且在298 K和100 kPa条件下表现出优异的CO2/CH4、CO2/CO吸附选择性(分别为18.7~19.9、8.9~9.5),以及高效催化转化CO2与环氧化合物生成环状碳酸酯的性能。

【Abstract】 Under solvothermal synthetic conditions,this study employed the organic carboxylic acid ligand containing amino groups,4,4’-diamino-[1,1’-biphenyl]-3,3’,5,5 ’-tetracarboxylic acid(H4L),to react with Mg2+ions,resulting in the preparation of a novel three-dimensional metal-organic framework:{[Mg2(L)(DMA)(H2O)2]·2DMA·H2O}n(Mg-MOF,DMA=N,N-dimethyl acetamide).The structure and stability of Mg-MOF were determined by singlecrystal X-ray diffraction,elemental analysis,thermogravimetric analysis,and so on,and the CO2 adsorption and catalytic conversion properties were also deeply investigated.The results indicate that Mg-MOF crystallizes in the monoclinic system with space group P21/n,unit cell parameters a=1.399 88(15) nm,b=1.400 49(15) nm,c=1.768 57(19)nm,β=94.307(2)°.Mg-MOF shows a 4-connected(42·84)-ant topological net,possessing one-dimensional channels decorated with amino groups.It reveals excellent adsorption selectivity for CO2 over CH4 and CO(18.7-19.9 and 8.9-9.5,respectively),as well as highly efficient catalytic performance for the conversion of CO2 and epoxides into cyclic carbonates at the condition of 298 K and 100 kPa.CCDC:2468229.

【基金】 国家自然科学基金(No.22371226);陕西省杰出青年科学基金(No.2024JC-JCQN-18);陕西省(化学、生物)基础研究院科研计划基金(No.23JHZ004)资助
  • 【文献出处】 无机化学学报 ,Chinese Journal of Inorganic Chemistry , 编辑部邮箱 ,2025年12期
  • 【分类号】X701;TQ225.52;O647.3;O643.36
  • 【下载频次】116
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