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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Single molecule magnet behaviors of Zn(4)Ln(2) (Ln = Dy-III, Tb-III) complexes with multidentate organic ligands formed by absorption of CO2 in air through in situ reactions
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Single molecule magnet behaviors of Zn(4)Ln(2) (Ln = Dy-III, Tb-III) complexes with multidentate organic ligands formed by absorption of CO2 in air through in situ reactions

机译：Zn（4）LN（2）（LN = DY-III，TB-III）配合物的单分子磁体行为，其具有通过在空气中吸收的二氧化碳通过原位反应形成的多型有机配体

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摘要

In this work, we report the syntheses, crystal structures and magnetic properties of three novel Zn-Ln mixed metal complexes, namely [Zn4Dy2(L-1)(2)(L-2)(2)(N-3)(2)]Cl(2)2H(2)O (1), [Zn4Tb2(L-1)(2)(L-2)(2)(Cl)(2)][ZnN3Cl3]2H(2)O (2), and [Zn4Gd2(L-1)(2)(L-2)(2)(Cl)(2)][ZnN3Cl3]2H(2)O (3), in which L-1(2-) and L-2(3-) were formed from the ligand L [L = N1,N3-bis(3-methoxysalicylidene)diethylenetriamine] through in situ reactions. Interestingly, carbon dioxide in air was absorbed in the process of forming carbamate ligand L-2(3-); this can be ascribed to the insertion of CO2 into M-N amide bonds. Moreover, 1 and 2 represent the first series of 3d-4f SMMs containing carbamate ligands by fixation of CO2 in air. Single-crystal X-ray diffraction analyses reveal that the crystal structures of 1 and 2 are anion-dependent, i.e., the apical positions of the two Zn-II ions in 1 and 2 are occupied by an N atom of N-3(-) and by Cl-, respectively. However, the topologies of 2 and 3 are similar. Two Zn-II ions and one Ln(III) (Ln = Dy (1), Tb (2) and Gd (3)) form nearly linear trinuclear [Zn(2)Ln] units which are double-bridged by two L-2(3-) ligands. Magnetic studies reveal that two complexes show single molecule magnet behavior under a direct current (dc) field, with effective energy barriers (U-eff) of 30.66(5) K for 1 and 8.87(3) K for 2. Ab initio calculations reveal that the Dy-III ions in 1 and the Tb-III ions in 2 are axial in nature; however, a difference in the tunnel splitting of 1 and 2 leads to variation in the magnetization blockades of the two complexes. Theoretical calculations also indicate that the directions of the main magnetic axes severely deviate from the coordination atoms of the first spheres of Dy-III and Tb-III in 1 and 2; thus further results in poor SMM behavior of the two complexes.
机译：在这项工作中，我们报告了三种新型Zn-LN混合金属配合物的合成，晶体结构和磁性，即[Zn4Dy2（L-1）（2）（2）（L-2）（2）（N-3）（2 ）] Cl（2）2H（2）O（1），[Zn4TB2（L-1）（2）（2）（2）（2）（Cl）（2）] [ZnN 3 Cl 3] 2H（2）O（2 ）和[Zn4GD2（L-1）（2）（2）（2）（2）（Cl）（2）] [ZnN 3 Cl 3] 2H（2）O（3），其中L-1（2-）和通过原位反应，由配体L [L = N1，N3-双（3-甲氧基丙烯）二亚乙基三胺]由配体L1，N3-双（3-甲氧基丙烯）二亚乙基三胺形成L-2（3-）。有趣的是，空气中的二氧化碳在形成氨基甲酸酯配体L-2（3-）的过程中被吸收;这可以归因于将CO2插入M-N酰胺键。此外，1和2代表通过在空气中固定CO 2的CO 2来表示含有氨基甲酸酯配体的第一系列3D-4F SMM。单晶X射线衍射分析表明，1和2的晶体结构是阴离子依赖性的，即1和2中的两个Zn-II离子的顶端位置被N-3的n原子占据（ - 分别通过cl-。但是，2和3的拓扑是相似的。两种Zn-II离子和一个LN（III）（LN = Dy（1），Tb（2）和Gd（3））形成几乎线性的三核[Zn（2）LN]单元，其双桥接两个L- 2（3-）配体。磁性研究表明，两种复合物在直流（DC）场下显示单个分子磁体行为，有效的能量屏障（U-EFF）为30.66（5）k，对于2.ab Initio计算显示1中的Dy-III离子和2中的TB-III离子在自然界中是轴向的;然而，隧道分裂的差异为1和2导致两个配合物的磁化块的变化。理论计算还表明主磁轴的方向严重地偏离了1和2中Dy-III和TB-III的第一球体的配位原子;因此进一步导致两种复合物的SMM行为差。

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    Yin Cheng-Ling; Hu Zhao-Bo; Long Qiao-Qiao; Wang Hui-Sheng; Li Jing; Song You; Zhang Zai-Chao; Zhang Yi-Quan; Pan Zhi-Quan;

  • 作者单位

    Wuhan Inst Technol Key Lab Green Chem Proc Sch Chem &

    Environm Engn Minist Educ Wuhan 430074 Hubei Peoples R China;

    Nanjing Univ State Key Lab Coordinat Chem Sch Chem &

    Chem Engn Collaborat Innovat Ctr Adv Microstruct Nanjing 210046 Jiangsu Peoples R China;

    Wuhan Inst Technol Key Lab Green Chem Proc Sch Chem &

    Environm Engn Minist Educ Wuhan 430074 Hubei Peoples R China;

    Wuhan Inst Technol Key Lab Green Chem Proc Sch Chem &

    Environm Engn Minist Educ Wuhan 430074 Hubei Peoples R China;

    Nanjing Univ State Key Lab Coordinat Chem Sch Chem &

    Chem Engn Collaborat Innovat Ctr Adv Microstruct Nanjing 210046 Jiangsu Peoples R China;

    Nanjing Univ State Key Lab Coordinat Chem Sch Chem &

    Chem Engn Collaborat Innovat Ctr Adv Microstruct Nanjing 210046 Jiangsu Peoples R China;

    Huaiyin Normal Univ Sch Chem &

    Chem Engn Jiangsu Key Lab Chem Low Dimens Mat Huaian Jiangsu Peoples R China;

    Nanjing Normal Univ Jiangsu Key Lab NSLSCS Sch Phys Sci &

    Technol Nanjing 210023 Jiangsu Peoples R China;

    Wuhan Inst Technol Key Lab Green Chem Proc Sch Chem &

    Environm Engn Minist Educ Wuhan 430074 Hubei Peoples R China;

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  • 中图分类 化学;无机化学;
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