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首页> 外文期刊>Inorganic Chemistry: A Research Journal that Includes Bioinorganic, Catalytic, Organometallic, Solid-State, and Synthetic Chemistry and Reaction Dynamics >Trapping of a Pseudotetrahedral (CoO4)-O-II Core in Mixed-Valence Mixed-Geometry [Co-5] Coordination Aggregates: Synthetic Marvel, Structures, and Magnetism
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Trapping of a Pseudotetrahedral (CoO4)-O-II Core in Mixed-Valence Mixed-Geometry [Co-5] Coordination Aggregates: Synthetic Marvel, Structures, and Magnetism

机译：在混合价混合 - 几何形状[CO-5]协调聚集体中捕获假氮（COO4）-O-II核：合成辐射，结构和磁力

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A systematic one-step one-pot multicomponent reaction of Co(ClO4)(2)center dot 6H(2)O, H3L (2,6-bis((2-(2-hydroxyethylamino)ethylimino)methyl)-4-methylphenol), and readily available carboxylate salts (RCO2Na; R = CH3, C2H5) resulted in the two structurally novel coordination aggregates [(CoCo4L2)-Co-II-L-III(mu(1,3)-O2CCH3)(2)(mu-OH)(2)](ClO4)(4)(center dot) 4H(2)O(1) and [Co(II)co(4)(III)L(2)(mu(1,3)-O2CC2H5)(2)(mu-OH)(mu-OMe)](ClO4)(4)center dot 5H(2)O (2). At room temperature, reactions of H3L in MeOH with cobalt(II) perchlorate salts led to coassembly of initially formed ligand-bound {Co-2(II)} fragments following aerial oxidation of metal centers and bridging by in situ generated hydroxido/alkoxido groups and added carboxylate anions. Available alkoxido arms of the initially formed {L(mu(1,3)-O2CCH3)(mu-OH/OMe)Co-2}(+) fragments were utilized to trap a central Co-II ion during the formation of [Co-5] aggregates. In the solid state, both complexes have been characterized by X-ray crystallography, variable-temperature magnetic measurements, and theoretical studies. Both 1 and 2 show field-induced slow magnetic relaxation that arises from the single pseudo-T-d Co-II ion present. The structural distortion leads to an easy-axis magnetic anisotropy (D = -31.31 cm(-1) for 1 and -21.88 cm(-)1 for 2) and a small but non-negligible transverse component (E/D = 0.11 for 1 and 0.08 for 2). The theoretical studies also reveal how the O-Co-O bond angles and the interplanar angles control D and E values in 1 and 2. The presence of two diamagnetic {Co-2(mu-L)} hosts controls the distortion of the central {CoO4} unit, highlighting a strategy to control single-ion magnetic anisotropy by trapping single ions within a diamagnetic coordination environment.
机译：CO（CLO4）（2）中心点6H（2）O，H3L（2,6-双（（2-羟基乙基氨基）乙基氨基）甲基）-4-甲基苯酚（2）o，H3L（2,6-双（（2-（2-羟乙基氨基）乙基苯酚的系统的一步式一步式反应），并且易于使用的羧酸盐（RCO2NA; R = CH 3，C 2 H 5）产生两种结构新颖的配位聚集体[（Coco4L2）-CO-II-L-III（MU（1,3）-O2CCH 3）（2）（ mu-OH）（2）]（CLO 4）（4）（中心点）4H（2）O（1）和[CO（II）CO（4）（III）L（2）（mu（1,3） -O2CC2H5）（2）（MU-OH）（MU-OME）]（CLO 4）（4）中心点5H（2）O（2）。在室温下，H3L在MeOH中的反应与钴（II）的钴（II）高氯酸盐盐导致最初形成的配体结合的{CO-2（II）}片段后金属中心的空中氧化和原位产生的羟基/烷氧基氧酰胺基团并添加羧酸盐阴离子。最初形成的{L（1,3）-O2CCH 3）（Mu-OH / OME）CO-2}（+）片段的可用烷氧基臂用于在形成期间捕获中心CO-II离子[CO -5]聚集体。在固态中，两种复合物的特征在于X射线晶体学，可变温度磁测量和理论研究。图1和2均显示出从单一假型T-D Co-II离子的源自诱导的慢磁性弛豫。结构变形导致易轴磁各向异性（D = -31.31cm（-1）1和-21.88cm（ - ）1，横向但不可忽略的横向组件（E / D = 0.11 2）1和0.08）。理论研究还揭示了O-Co-O键角和平面角度控制D和e值在1和2中的存在。两个二极管{CO-2（MU-L）}主机控制中央的失真{COO4}单元，突出策略来控制单离子磁各向异性，通过捕获抗磁的配位环境中的单离子。

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