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Anion-Dependent Assembly of 3d-4f Heterometallic Clusters Ln5Cr2 and Ln8Cr4.
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-01-17 , DOI: 10.1021/acs.inorgchem.9b03308
Jia-Jia Yin 1 , Cheng Chen 1 , Gui-Lin Zhuang 2 , Jun Zheng 1 , Xiu-Ying Zheng 1, 3 , Xiang-Jian Kong 3
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A series of heterometallic Ln-Cr clusters with the formulas [Ln5Cr2(H2L)2(OAc)6(μ3-OH)6(H2O)15](ClO4)7·xH2O (Ln = Gd and x = 33 for 1 and Ln = Dy and x = 21 for 2) and [Ln8Cr4(H2L)4(OAc)8(μ3-OH)16(μ4-O)1(H2O)8](Cl)(ClO4)5·10H2O (Ln = Gd for 3 and Ln = Dy for 4) was obtained through the reaction of the acetate ligands 2,2-dimethylolpropionic acid (H3L) and Ln(ClO4)3 in the presence of chromium salts with different anions under the same high pH conditions. X-ray analysis revealed that compound 1 contained a metal unit [Gd3Cr2] displaying the pentagonal bipyramid configuration and that compound 3 was templated by Cl- and ClO4- as a mixed anion template featuring a quadrangular structure. In compound 3, the 12 metal atoms were arranged in a wheel-shaped metal skeleton [Gd8Cr4], which was produced by 4 tetrahedral metal units [Gd3Cr] sharing vertices. The introduction of the mixed anion template increased the number of metal atoms in the Ln-Cr clusters. Magnetic calculations indicated that there was weak antiferromagnetic Gd···Cr coupling and weak ferromagnetic Gd···Gd coupling in 1, whereas both Gd···Cr and Gd···Gd in 3 exhibited weak antiferromagnetic interactions. Magnetothermal studies showed that compounds 1 and 3 displayed magnetic entropy changes of 25.2 J kg-1 K-1 at 5 K and 7 T and 33.8 J kg-1 K-1 at 2 K and 7 T, respectively.

中文翻译:

3d-4f杂金属簇Ln5Cr2和Ln8Cr4的阴离子依赖性组装。

一系列具有[Ln5Cr2(H2L)2(OAc)6(μ3-OH)6(H2O)15](ClO4)7·xH2O的式子的Ln-Cr簇(Ln = Gd,x = 33表示1和Ln = Dy,对于2)x = 21)和[Ln8Cr4(H2L)4(OAc)8(μ3-OH)16(μ4-O)1(H2O)8](Cl)(ClO4)5·10H2O(Ln = Gd在相同的高pH条件下,在具有不同阴离子的铬盐存在下,通过乙酸盐配体2,2-二羟甲基丙酸(H3L)和Ln(ClO4)3的反应获得了3的Ln(4的Ln = Dy)。X射线分析表明,化合物1含有表现出五边形双锥体构型的金属单元[Gd3Cr2],并且化合物3由Cl-和ClO4-作为具有四边形结构的混合阴离子模板而模板化。在化合物3中,这12个金属原子排列在轮状金属骨架[Gd8Cr4]中,该骨架由4个共享顶点的四面体金属单元[Gd3Cr]产生。混合阴离子模板的引入增加了Ln-Cr簇中金属原子的数量。磁性计算表明,在1中存在弱的反铁磁Gd···Cr耦合和弱的铁磁Gd···Gd耦合,而在3个中的Gd··Cr和Gd···Gd都表现出弱的反铁磁相互作用。磁热研究表明,化合物1和3在5 K和7 T时的磁熵变分别为25.2 J kg-1 K-1和2 K和7 T时的磁熵变分别为33.8 J kg-1 K-1。
更新日期:2020-01-17
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