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Rare CH3O/CH3CH2O-bridged nine-coordinated binuclear DyIII single-molecule magnets (SMMs) significantly regulate and enhance the effective energy barriers

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Abstract

Based on a multidentate Schiff-base ligand, N,N′-bis(2-hydroxy-5-methyl-3-formylbenzyl)-N,N′-bis-(pyridin-2-ylmethyl)ethylenediamine (H2L), two binuclear DyIII compounds, with formulas [Dy2(L)(NO3)3(CH3O)] (1) and [Dy2(L)(NO3)3(CH3CH2O)] (2), have been synthesized under different solvent systems. The DyIII ions in 1 and 2 adopt monocapped square antiprism coordination geometries, while different structural distortions can be observed. The two DyIII ions in 1 and 2 are bridged by two phenoxide atoms of one L2− ligand and one bridged CH3O/CH3CH2O oxygen node, leading to an approximate fusiform Dy2O3 core. The different DyIII–Obridged node distances, DyIII–Obridged node–DyIII angles and DyIII⋯DyIII distances can be observed. Magnetic studies reveal that 1 and 2 display slow magnetic relaxation behaviours under a zero direct-current field with the effective energy barriers (Ueff) of 114.17 K and 171.23 K, respectively. Furthermore, compound 2 possesses the highest Ueff in nine-coordinated Dy2 compounds. The M versus H data exhibit weak butterfly-shaped hysteresis loops at 2 K for 2. The rare CH3O/CH3CH2O-bridged nine-coordinated binuclear DyIII single-molecule magnets (SMMs) significantly regulate and enhance the Ueff of compounds 1 and 2. To deeply understand their different magnetic behaviours, the magnetic anisotropies and magnetic interactions of 1 and 2 were studied by ab initio calculations. These findings demonstrate an efficient approach for regulating and enhancing the magnetic anisotropy barriers using a bridged CH3O anion or CH3CH2O anion.

Graphical abstract: Rare CH3O−/CH3CH2O−-bridged nine-coordinated binuclear DyIII single-molecule magnets (SMMs) significantly regulate and enhance the effective energy barriers

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Supplementary files

Article information


Submitted
19 Dec 2019
Accepted
28 Jan 2020
First published
29 Jan 2020

CrystEngComm, 2020, Advance Article
Article type
Paper

Rare CH3O/CH3CH2O-bridged nine-coordinated binuclear DyIII single-molecule magnets (SMMs) significantly regulate and enhance the effective energy barriers

S. Zhang, N. Shen, S. Liu, R. Ma, Y. Zhang, D. Hu, X. Liu, J. Zhang and D. Yang, CrystEngComm, 2020, Advance Article , DOI: 10.1039/C9CE02000D

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