三种基于2,4,6-三(3-吡啶基)-1,3,5-苯配体的Ni(Ⅱ)基配位聚合物的合成、结构及催化性能 |
Syntheses, structures, and catalytic properties of three Ni(Ⅱ)-based coordination polymers from 2,4,6-tris(3-pyridyl)-1,3,5-benzene ligand |
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摘要: 通过调变溶剂热的反应条件,我们合成了3种Ni(Ⅱ)基的配位聚合物(CPs)[Ni (CH3-BDC)(3-TBT)(H2O)2]·EtOH·2H2O (CP1)、[Ni3(CH3-BDC)3(3-TBT)2(H2O)5]·2DMF·2H2O (CP2)和[Ni3(CH3-BDC)3(3-TBT)2(H2O)6]·2DMF·4H2O (CP3),其中CH3-H2BDC=5-methyl isophthalic acid,3-TBT=2,4,6-tris (3-pyridyl)-1,3,5-benzene。X射线单晶衍射分析表明,3个CPs都是由相似的Ni2(CH3-BDC)2的双核单元构建的,并分别呈现出从零维(0D)、2D到3D结构的网络骨架。反应条件的微小调变,导致了不同结构的配位聚合物。同时,催化实验表明,3在无溶剂的温和反应条件下,CP3对苄醇及其衍生物与苯胺的氧化-偶联反应表现出极好的催化活性和循环稳定性。 |
关键词: 配位聚合物 溶剂热反应 C3对称性配体 催化活性 |
基金项目: 上海市自然科学基金(No.18090503600)和上海市教委高校实验技术人才队伍建设项目(No.10110N210018-A07-2021)资助。 |
Abstract: By tuning the solvothermal reaction conditions, we prepared three Ni(Ⅱ)-based coordination polymers (CPs), namely[Ni(CH3-BDC)(3-TBT)(H2O)2]·EtOH·2H2O (CP1),[Ni3(CH3-BDC)3(3-TBT)2(H2O)5]·2DMF·2H2O (CP2), and[Ni3(CH3-BDC)3(3-TBT)2(H2O)6]·2DMF·4H2O (CP3), where CH3-H2BDC=5-methyl isophthalic acid, 3-TBT=2,4,6-tris(3-pyridyl)-1,3,5-benzene. X-ray single crystal diffraction analyses reveal that three CPs are constructed from similar Ni2(CH3-BDC)2 binuclear units and exhibited different zero-dimensional (0D), 2D, and 3D networks, respectively. Meanwhile, the catalytic experiments show that CP3 exhibits the best catalytic activities and cycle stability for the oxidative coupling reaction of benzyl alcohol and its derivatives with aniline under solvent-free conditions. CCDC:2168727, CP1; 2168728, CP2, 2222864, CP3. |
Keywords: coordination polymers solvothermal reaction C3-symmetric ligands catalytic activity |
投稿时间:2022-11-29 修订日期:2023-04-23 |
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包玉梅,陈彦合,邢媛媛,张建勇,邓维.三种基于2,4,6-三(3-吡啶基)-1,3,5-苯配体的Ni(Ⅱ)基配位聚合物的合成、结构及催化性能[J].无机化学学报,2023,39(6):993-1004. |
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