调节从双核镝簇到九核簇的弛豫动力学结构转变。
Modulating the relaxation dynamics structural transition from a dinuclear dysprosium cluster to a nonanuclear cluster.
作者信息
Hu Peng, Cao Ling-Hui, Liu Ao-Gang, Zhang Yi-Quan, Zhang Tian-le, Li Bao
机构信息
Hubei Key Laboratory of Radiation Chemistry and Functional Materials, Non-power Nuclear Technology Collaborative Innovation Center, Hubei University of Science and Technology, Xianning 437100, People's Republic of China.
Key laboratory of Material Chemistry for Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, People's Republic of China.
出版信息
Dalton Trans. 2021 Sep 28;50(37):12814-12820. doi: 10.1039/d1dt02380b.
A dinuclear dysprosium cluster [Dy(NO)(HO)(L)]·2CHCN was successfully prepared by employing HL (HL = 2,6-dimethoxyphenol) and Dy(NO)·6HO in a mixture of CHOH and CHCN. The conversion of this Dy compound by reaction with additional deprotonated ligand generated a Dy cluster Dy(μ-OH)(μ-OH)(μ-OCH)(NO)(HO)(L)·2HO with the well-known "diabolo" topology. Magnetic investigation revealed that both of the clusters exhibit typical SMM characteristics, and variable magnetic relaxation with the energy barrier changing from 217.87 K to 9.24 K along with the transition from a dinuclear dysprosium cluster to a nonanuclear one. calculations further confirm the corresponding structure-activity relationships that originate the different magnetic behaviours. This design may afford a feasible strategy for modulating the magnetic relaxation dynamics of polynuclear systems.
通过在甲醇和乙腈的混合物中使用HL（HL = 2,6 - 二甲氧基苯酚）和Dy(NO₃)₃·6H₂O成功制备了双核镝簇合物[Dy(NO₃)(H₂O)(L)]·2CH₃CN。该Dy化合物与额外的去质子化配体反应进行转化，生成了具有著名的“双锥体”拓扑结构的Dy簇合物Dy(μ - OH)(μ - OH)(μ - OCH₃)(NO₃)(H₂O)(L)·2H₂O。磁性研究表明，这两种簇合物均表现出典型的单分子磁体（SMM）特性，并且随着从双核镝簇到九核簇的转变，可变磁弛豫的能垒从217.87 K变化到9.24 K。计算进一步证实了产生不同磁行为的相应结构 - 活性关系。这种设计可能为调节多核体系的磁弛豫动力学提供一种可行的策略。
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