Slow magnetic relaxation in CoII-LnIII heterodinuclear complexes achieved through a functionalized nitronyl nitroxide biradical.,Dalton Transactions

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Slow magnetic relaxation in CoII-LnIII heterodinuclear complexes achieved through a functionalized nitronyl nitroxide biradical.
Dalton Transactions ( IF 3.5 ) Pub Date : 2019-12-24 , DOI: 10.1039/c9dt04036f
Lu Xi ₁ , Juan Sun ₁ , Kang Wang ₁ , Jiao Lu ₁ , Pei Jing ₁ , Licun Li ₁

Affiliation

A new nitronyl nitroxide biradical ligand NITPh-PyPzbis (5-(3-(2-pyridinyl)-1H-pyrazol-1-yl)-1,3-bis(1'-oxyl-3'-oxido-4',4',5',5'-tetramethyl-4,5-hydro-1H-imidazol-2-yl)benzene) has been successfully applied for constructing a 3d-4f CoII-LnIII system, giving rise to a family of novel hetero-tri-spin complexes, namely, [LnCo(hfac)5(NITPh-PyPzbis)]·CH2Cl2 (LnCo = YCo 1, GdCo 2, TbCo 3, DyCo 4, and HoCo 5; hfac = hexafluoroacetylacetonate). In these hetero-tri-spin complexes, the NITPh-PyPzbis biradical chelates one LnIII and one CoII simultaneously by means of its adjacent aminoxyl moieties and two N donors from the 3-(2-pyridinyl)-1H-pyrazol-1-yl unit, respectively, realizing the unique biradical-Co-Ln heterodinuclear structure. Direct-current magnetic susceptibility investigations show that antiferromagnetic coupling is predominant in the YCo derivative, while the leading magnetic interaction in the GdCo analogue is ferromagnetic. Alternating-current data for the DyCo complex display visible temperature/frequency-dependent χ'' peaks, indicating the SMM behavior. In the fluorescence spectra, four characteristic emission bands of the TbIII ion have been detected for the TbCo analogue.

中文翻译：

CoII-LnIII异双核配合物中的慢磁弛豫是通过功能化的硝酰基硝基氧双自由基实现的。

新的硝酰基硝基氧双自由基配体NITPh-PyPzbis（5-（3-（2-pyridinyl）-1H-pyrazol-1-yl）-1,3-bis（1'-oxyl-3'-oxido-4'，4 '，5'，5'-四甲基-4,5-氢-1H-咪唑-2-基）苯已成功用于构建3d-4f CoII-LnIII系统，从而产生了一系列新型的杂原子三自旋配合物，即[LnCo（hfac）5（NITPh-PyPzbis）]·CH2Cl2（LnCo = YCo 1，GdCo 2，TbCo 3，DyCo 4和HoCo 5； hfac =六氟乙酰丙酮酸酯）。在这些杂三-自旋复合物中，NITPh-PyPzbis双自由基螯合一个LnIII和一个CoII，同时通过其相邻的氨氧基部分和来自3-（2-吡啶基）-1H-吡唑-1-基单元的两个N供体分别实现了独特的双自由基-Co-Ln异双核结构。直流磁化率研究表明，YCo衍生物中反铁磁耦合是主要的，而GdCo类似物中主要的磁相互作用是铁磁的。DyCo配合物的交流数据显示可见的温度/频率相关的χ''峰，表明SMM行为。在荧光光谱中，已为TbCo类似物检测到TbIII离子的四个特征发射带。

更新日期：2020-01-06

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