| 双吡啶基配体和间苯二甲酸构筑的金属有机骨架的结构及性质 | |
| Synthesis, structures, and properties of metal-organic frameworks based on bipyridyl ligands and isophthalic acid | |
| 摘要: 合成了2种双吡啶基配体：(2E，6E)-4-甲基-2，6-双(吡啶-3-基亚甲基)环己-1-酮(L1)和4-甲基-2，6-双[(E)-4-(吡啶-4-基)亚苄基]环己-1-酮(L2)，并在溶剂热条件下，以其与间苯二甲酸(H2IP)和过渡金属反应，制备了4种金属有机骨架(MOFs)材料：[Zn(IP)(L1)]n (1)、{[Cd(IP)(L1)]·H2O}n (2)、{[Co(IP)(L1)]·H2O}n (3)、[Zn(IP)(L2)(H2O)]n (4)。通过单晶 X 射线衍射、粉末 X 射线衍射、热重和元素分析对其进行了表征。单晶X射线衍射分析表明，MOF 1属于单斜晶系P21/n空间群，MOF 2~4都属于三斜晶系P$overline{1}$空间群。1~3 具有二维结构，其中 2 和 3 具有相似结构，4 为一维链状结构。光催化降解有机染料性能研究结果表明，1~3 对罗丹明 B(RhB)和盐酸副玫瑰苯胺(PH)有一定降解活性。以 4作为催化剂用于苯甲醛衍生物和丙二腈的 Knoevenagel缩合反应，催化结果表明，4可在3 h内催化生成产物，可循环利用3次并保持其活性。初步探究了4催化Knoevenagel缩合反应的机理。 | |
| 关键词: 双吡啶基配体 金属有机骨架 光催化降解 Knoevenagel缩合反应 | |
| 基金项目: 国家自然科学基金(No.21771088)资助。 | |
| Abstract: (2E,6E)-4-methyl-2,6-bis(pyridin-3-ylmethylene)cyclohexan-1-one (L1) and 4-methyl-2,6-bis[(E)-4-(pyridin-4-yl)benzylidene]cyclohexan-1-one (L2) were synthesized and combined with isophthalic acid (H2IP), then under solvothermal conditions, to react with transition metals achieving four novel metal organic frameworks (MOFs): [Zn(IP)(L1)]n (1), {[Cd(IP)(L1)]·H2O}n (2), {[Co(IP)(L1)]·H2O}n (3), and [Zn(IP)(L2)(H2O)]n (4). MOFs 1-4 have been characterized by single-crystal X-ray diffraction, powder X-ray diffraction, thermogravimetry, and elemental analysis. Single-crystal X-ray diffraction shows that MOF 1 crystallizes in the monoclinic crystal system with space group P2 1/n, and MOFs 2-4 belong to the triclinic system with the P$overline{1}$ space group. 1-3 are 2D sheet structures, 2 and 3 have similar structural characters, whereas 4 is a 1D chain structure. Furthermore, 1-3 exhibited certain photocatalytic capability in the degradation of rhodamine B (RhB) and pararosaniline hydrochloride (PH). 4 could be used as a heterogeneous catalyst for the Knoevenagel reaction starting with benzaldehyde derivative and malononitrile. 4 could promote the reaction to achieve corresponding products in moderate yields within 3 h. Moreover, the catalyst exhibited recyclability for up to three cycles without significantly dropping its activity. A mechanism for MOF 4 cat-alyzed Knoevenagel condensation reaction of aromatic aldehyde and malononitrile has been initially proposed. | |
| Keywords: bipyridyl ligands metal-organic frameworks photocatalytic degradation Knoevenagel condensation | |
| 投稿时间：2024-09-25 修订日期：2024-12-03 | |
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| 侯纪敏,李梦洋,宫春华,张少壮,詹才宏,徐昊,谢景力.双吡啶基配体和间苯二甲酸构筑的金属有机骨架的结构及性质[J].无机化学学报,2025,41(3):549-560. | |
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