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抗磁性锌（II）离子对一系列三核锌镝和四核锌镝（Ln = 镝、铽、钆）配合物单分子磁体性质的影响：实验与理论相结合的研究

Effect of diamagnetic Zn(II) ions on the SMM properties of a series of trinuclear ZnDy and tetranuclear ZnDy (Ln = Dy, Tb, Gd) complexes: combined experimental and theoretical studies.

作者信息

Shukla Pooja, Tarannum Ibtesham, Roy Soumalya, Rajput Amit, Lama Prem, Singh Saurabh Kumar, Kłak Julia, Lee Junseong, Das Sourav

机构信息

Department of Basic Sciences, Chemistry Discipline, Institute of Infrastructure Technology Research and Management, Near Khokhra Circle, Maninagar East, Ahmedabad-380026, Gujarat, India.

Department of Chemistry, Johannes Gutenberg University, Duesbergweg 10-14, 55128 Mainz, Germany.

出版信息

Dalton Trans. 2024 Apr 23;53(16):7053-7066. doi: 10.1039/d4dt00417e.

DOI:10.1039/d4dt00417e
PMID:38564260
Abstract

To study the effect of diamagnetic ions on magnetic interactions, utilizing a compartmental ligand ()-2-(hydroxymethyl)-4-methyl-6-((quinolin-8-ylimino)methyl)phenol (LH), two different series of Zn-Ln complexes, namely the trinuclear series of [DyZn(L)(μ-OAc)(CHOH)]·NO·MeOH (1), [TbZn(L)(μ-OAc)(CHOH)]·NO·5MeOH·HO (2), and [GdZn(L)(μ-OAc)(CHOH)]·NO·MeOH·CHCl (3) and the tetranuclear series of [DyZn(LH)(NO)(μOAc)]·NO·MeOH·HO (4), [TbZn(LH)(NO)(μ-OAc)]·NO·MeOH·2HO (5), and [GdZn(LH)(NO)(μ-OAc)]·NO·MeOH·2HO (6), were synthesized. Trinuclear Zn-Ln complexes 1-3 consist of one Ln ion sandwiched between two peripheral Zn ions forming a bent type Zn-Dy-Zn array with an angle of 110.64°. Tetranuclear Zn-Ln complexes 4-6 are basically a combination of two dinuclear moieties of [LnZn(LH)(NO)] connected by one bidentate bridging acetate ion in μ-OAc coordination mode. The detailed magnetic analysis reveals that complexes 1 and 4 are single molecule magnets having energy barriers of 34.98 K and 46.71 K with relaxation times () of 5.05 × 10 s and 5.24 × 10 s, respectively. calculations were employed to analyze the magnetic anisotropy and magnetic exchange interaction between the Zn and Ln centers with the aim of gaining better insights into the magnetic dynamics of complexes 1-6.

摘要

为了研究抗磁性离子对磁相互作用的影响，利用一种隔室配体（）-2-（羟甲基）-4-甲基-6-（（喹啉-8-基亚氨基）甲基）苯酚（LH），合成了两个不同系列的锌-镧系元素配合物，即三核系列的[DyZn（L）（μ-OAc）（CHOH）]·NO·MeOH（1）、[TbZn（L）（μ-OAc）（CHOH）]·NO·5MeOH·HO（2）和[GdZn（L）（μ-OAc）（CHOH）]·NO·MeOH·CHCl（3）以及四核系列的[DyZn（LH）（NO）（μOAc）]·NO·MeOH·HO（4）、[TbZn（LH）（NO）（μ-OAc）]·NO·MeOH·2HO（5）和[GdZn（LH）（NO）（μ-OAc）]·NO·MeOH·2HO（6）。三核锌-镧系元素配合物1-3由一个镧系离子夹在两个外围锌离子之间组成，形成一个角度为110.64°的弯曲型Zn-Dy-Zn阵列。四核锌-镧系元素配合物4-6基本上是两个[LnZn（LH）（NO）]双核部分通过一个以μ-OAc配位模式的双齿桥连醋酸根离子连接而成的组合。详细的磁性分析表明，配合物1和4是单分子磁体，能垒分别为34.98 K和46.71 K，弛豫时间（）分别为5.05×10 s和5.24×10 s。采用计算方法分析锌和镧系中心之间的磁各向异性和磁交换相互作用，旨在更好地了解配合物1-6的磁动力学。

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