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Ferromagnetic Archimedean polyhedra {Fe24M18} (M = Fe, Ni, and Mn) with tunable electron configurations
Inorganic Chemistry Frontiers ( IF 7 ) Pub Date : 2021-07-21 , DOI: 10.1039/d1qi00593f
Wen Wen 1, 2, 3, 4 , Yin-Shan Meng 1, 2, 3, 4 , Cheng-Qi Jiao 1, 2, 3, 4 , Qiang Liu 1, 2, 3, 4 , Hai-Lang Zhu 1, 2, 3, 4 , Ya-Ming Li 1, 2, 3, 4 , Hiroki Oshio 1, 2, 3, 4 , Tao Liu 1, 2, 3, 4
Affiliation  

Construction of metal–organic polyhedral clusters is promising and challenging in science due to their highly symmetric structures and potential application to molecular devices. In this work, three neutral nanocages of {[Fe(Tp)(CN)3]24[M(H2O)2]6[M(L)(H2O)]12xH2O (1-Fe, 2-Ni, and 3-Mn for M = Fe, Ni, Mn and x = 6, 2, 4, respectively; Tp = hydrotris(pyrazolyl)borate and L = pyridine-4-carboxylate) were prepared through the assembly of [Fe(Tp)(CN)3] with FeII, NiII, or MnII ions and pyridine-4-carboxaldehyde, which was oxidized to pyridine-4-carboxylic acid during the reactions. Single crystal structure analyses revealed that each cage has the same core structure of an Archimedean polyhedra, the pseudo-rhombicuboctahedron. Elemental analyses and magnetic and spectroscopic measurements were performed to determine the oxidation and spin states of the composite metal ions, demonstrating that their electron configurations can be altered by changing the metal ions and deprotonating the auxiliary ligands. In addition, magnetic studies indicated that the metal ions were ferromagnetically coupled within the cage structure. These clusters exhibited magnetocaloric effects (MCEs) with the entropy changes of 11.55 J kg−1 K−1 for 1-Fe, 5.84 J kg−1 K−1 for 2-Ni, and 19.84 J kg−1 K−1 for 3-Mn at 3 K and 8.5 T, and 3-Mn is among the family of high-performance 3d-metal-based magnetic coolants.

中文翻译:

具有可调电子构型的铁磁阿基米德多面体 {Fe24M18}(M = Fe、Ni 和 Mn)

由于其高度对称的结构和在分子器件中的潜在应用,金属-有机多面体簇的构建在科学上具有前景和挑战性。在这项工作中,三个中性纳米笼 {[Fe(Tp)(CN) 3 ] 24 [M(H 2 O) 2 ] 6 [M(L)(H 2 O)] 12x H 2 O ( 1 -Fe2-Ni3-Mn,其中 M = Fe、Ni、Mn 和x = 6、2、4;Tp = 氢三(吡唑基)硼酸盐和 L = 吡啶-4-羧酸盐)是通过以下方法制备的[Fe(Tp)(CN) 3 ] 的组装-含 Fe II , Ni II , 或 Mn II离子和吡啶-4-甲醛,在反应过程中被氧化成吡啶-4-羧酸。单晶结构分析表明,每个笼具有相同的阿基米德多面体核心结构,即伪菱形八面体。进行元素分析和磁性和光谱测量以确定复合金属离子的氧化和自旋状态,证明它们的电子构型可以通过改变金属离子和去质子化辅助配体来改变。此外,磁性研究表明金属离子在笼状结构内铁磁耦合。这些簇表现出与11.55 j的熵变磁效应(的MCE)千克-1 ķ -11 -铁, 2-Ni为5.84 J kg -1 K -13-Mn为19.84 J kg -1 K -1在 3 K 和 8.5 T 下,3-Mn属于高性能 3d-金属-基于磁性冷却剂。
更新日期:2021-08-11
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