高等学校化学学报2026，Vol.47Issue(2)：7-17,11.DOI:10.7503/cjcu20250225
新型三维单核Zn(Ⅱ)配合物多位点协同催化单和双取代喹唑啉酮的绿色合成
Green Synthesis of Mono-and Disubstituted Quinazolinones by Multi-site Synergistic Catalysis of Novel Three-dimensional Single-nuclear Zn(Ⅱ)Complexes
摘要
Abstract
Two zinc-based complexes,[Zn(4,4′-bipy)(H2O)4]·(4-ABS)2(1,CCDC:2171834)and[Zn(4,4′-bipy)(H2O)4]·(4-MBS)₂(2,CCDC:2225758),were obtained through solvothermal synthesis with Zn(II)salts using p-aminobenzenesulfonate(4-ABS-)and p-methylbenzenesulfonate(4-MBS-)as the main ligands and 4,4′-bipyridine(4,4′-bipy)as the auxiliary ligand.The complexes were characterized by single-crystal X-ray diffraction(SXRD),infrared spectroscopy(IR),thermogravimetric analysis(TGA),powder X-ray diffraction(PXRD),nitrogen adsorption-desorption test and field-emission scanning electron microscopy(SEM).The performance of complexes 1 and 2 in catalyzing the synthesis of 2,3-diphenyl-2,3-dihydroquinazoline-4(1H)-one was investigated,and complex 1 with better catalytic effect was chosen for substrates universality experiments.The experimental results showed that high-yield products could be obtained using a small amount of catalyst in short time under solvent-free conditions.This green process was applicable to a variety of raw materials amines/ammonium compounds and aromatic aldehydes with different substituents.In addition,density functional theory(DFT)was used to optimize the structures of complex 1 and the three reactants.Through computational analysis of the frontier molecular orbitals(FMO),the reac-tion sequence and the core active sites of complex 1 for the three reactants were inferred.The active sites of complex 1 and the reaction sites of the reaction substrates were further predicted in detail by analyzing the electrostatic potential(ESP)of the molecular surface,the average local ionization energy(ALIE)and the Mulliken charges.Finally,the reaction mechanism of multi-site synergistic catalysis of the complexes was explained in combination with DFT.关键词
锌基配合物/晶体结构/2,3-二氢喹唑啉-4(1H)-酮/催化机理/密度泛函理论Key words
Zinc-based complex/Crystal structure/2,3-Dihydroquinazolin-4(1H)-one/Catalytic mechanism/Density functional theory分类
化学化工引用本文复制引用
徐一铭,史燚威,王鑫,朱志慧,宋志国,王敏..新型三维单核Zn(Ⅱ)配合物多位点协同催化单和双取代喹唑啉酮的绿色合成[J].高等学校化学学报,2026,47(2):7-17,11.基金项目
教育部产学合作协同育人项目(批准号:231105940171618,230805940290824)资助. Supported by the Ministry of Education's Industry-university Collaborative Education Project,China(Nos.231105940171618,230805940290824). （批准号:231105940171618,230805940290824）
