【作者】 张月；

【导师】 韩正波；

【作者基本信息】 辽宁大学 ， 无机化学， 2018， 硕士

【摘要】 金属有机骨架材料（MOFs）作为一种新兴的多孔材料,不但具有极高的表面积、可调节的孔尺寸、可循环性和大量的活性位点,而且还可以通过预功能化和后合成修饰的方法向金属有机骨架材料中引入多种活性位点,所以近年来在催化领域发展迅速,被广泛的应用于光催化,电催化和许多非均相催化方面。串联反应和多组分反应,都可以减少化学品的使用,减少污染物的产生和缩短反应时间,是经济,有效和环境友好型的化学方法,吸引了越来越多研究者的兴趣。本文主要介绍通过溶剂热的方法合成了两种新型的金属有机骨架材料,并对他们的结构、功能和催化性能进行了研究。全文一共分为四章:第一章中,我们首先介绍了MOFs材料的研究背景和现阶段的发展情况,接着介绍了MOFs材料在催化领域的研究进展,主要是催化串联反应和多组分反应方面的进展。第二章中,我们利用配体2-氨基对苯二甲酸（NH₂-H₂BDC）和稀土离子（Ln=Yb,Dy,Sm）通过溶剂热的方法合成了一系列含六核稀土簇的阴离子型MOFs材料:[（CH3）2NH2]2[Yb6（μ3-OH）8（BDC-NH2）6（H2O）6]?（solv）x（1）[（CH3）2NH2]2[Dy6（μ3-OH）8（BDC-NH2）6（H2O）6]?（solv）x（2）[（CH₃）₂NH₂]₂[Sm₆（μ₃-OH）₈（BDC-NH₂）₆（H₂O）₆]?（solv）_x（3）这些配合物展示了十二连接的,fcu拓扑构型的三维骨架结构。这些配合物不仅展示了很高的化学稳定性和热稳定性,而且还具有很好的二氧化碳吸附能力。由于同时具有Lewis酸性和Br?nsted碱性位点,所以这些材料可以作为Deacetalization-Knoevenagel缩合反应的催化剂。第三章中,我们利用配体4,4’,4’’-s-三嗪-2,4,6-三苯甲酸（H₃TATB）和铟离子通过溶剂热的方法合成了一个具有二重穿插结构的配位聚合物:[In（TATB）₂（HCOO）₃（DMF）₃]·2DMF·H₂O（4）,并介绍了该配合物催化三组分Biginelli反应的催化性能。第四章中,我们对所合成的配合物和所进行的多组分反应和串联反应的工作进行了总结,为金属有机骨架材料应用于多组分反应和串联反应方面提供了依据。更多还原

【Abstract】 Metal-Organic Frameworks（MOFs）,as a new porous material,not only possess extremely high surface areas,tunable pore size and recoverability,as well as a wide range of accessible catalytic sites,but also could be introduced into many active sites by means of pre-functionalization and post-synthetic modification.So,metal-organic frameworks developed rapidly in catalytic field in the recent years,which is applied to photocatalysis,electrocatalysis and many heterogeneous catalysts.Tandem reactions and multicomponent reaction are in one pot,which could reduce the use of chemicals,mitigate the generation of pollutants,and shorten reaction time.They are economical,efficient and environment-friendly chemical methods,and have been attracting widespread research interests.In this paper,two new kinds of metal-organic frameworks were synthesized by solvothermal reactions,and their structure,function and catalytic performance were studied.The full paper is divided into four chapters:In the first chapter,we first introduced the research background of MOFs materials and the development of the current situation,and then introduced the MOFs materials research progress in the field of catalysis,series mainly catalytic reaction progress.In the second chapter,a series of 12-connected hexanuclear Ln（Ln=Yb,Dy and Sm）clusters-based MOFs incorporating[Ln₆（?₃-OH）₈（COO-）₁₂]and an amino-functionalized ligand（2-amino-benzenedicarboxylate,BDC-NH₂）have been synthesizedbysolvothermalreactionswiththeformula[（CH₃）₂NH₂]₂[Ln₆（?₃-OH）₈（BDC-NH₂）₆（H₂O）₆]?（solv）_x（Ln=Yb（1）,Dy（2）and Sm（3））.These compounds show high chemical stability and generic thermal stability in common organic solvents and water with pH values ranging from 2-12.Due to the existence of-NH2 groups,they show high adsorption capacity of CO2.More strikingly,the Ln clusters afford Lewis acid sites and ligands offer Br?nsted base sites,making them as highly efficient bifunctional catalysts for one-pot tandem deacetalization-Knoevenagel condensation reaction.In the third chapter,we used ligand 4,4’,4’’-s-triazine-2,4,6-tribenzoic acid（H₃TATB）and indium ions through solvothermal reactions to synthesize a coordination polymer with the formula[In（TATB）₂（HCOO）₃（DMF）₃]·2DMF·H₂O（4）with double interpenetrating structure,and then introduced its catalytic performance of Biginelli reaction.In the fourth chapter,we summarize the work of the synthesized compounds,tandem reactions and multicomponent reactions,which provides the basis for the application of the metal-organic frameworks materials in tandem reactions and multicomponent reactions.更多还原