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Enhancing Steric Hindrance via Ligand Design in Dysprosium Complexes: From Induced Slow Relaxation to Zero-Field Single-Molecule Magnet Properties
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2021-08-27 , DOI: 10.1021/acs.inorgchem.1c00973 Christina M Legendre 1 , Regine Herbst-Irmer 1 , Dietmar Stalke 1
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2021-08-27 , DOI: 10.1021/acs.inorgchem.1c00973 Christina M Legendre 1 , Regine Herbst-Irmer 1 , Dietmar Stalke 1
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The synthesis and magnetic characterization of three novel Dy compounds, [Dy{PPh2S(NtBu)2}2(μ-Cl2)Li(THF)2] (1), [Dy{PhS(NtBu)2}2(μ-Cl2)Li(THF)2] (2), and [Dy{MeS(NtBu)3}2(μ-Cl2)Li(THF)2] (3), based on the sulfur–nitrogen ligands RS(NtBu)x– (where R = PPh2, x = 2 for (1); R = Ph, x = 2 for (2); and R = Me, x = 3 for (3)) are reported. They represent rare examples of lanthanide-based complexes containing sulfur–nitrogen ligands, whose suitability to enhance the magnetic anisotropy in 3d metals was only recently established. Changes in the ligand field environment drastically affect the magnetic properties, with compounds 1 and 2 displaying field-induced single-molecule magnet (SMM) behavior, while compound 3 shows slow relaxation at zero field. These trends strongly suggest that ligand engineering strategies toward linear dysprosium complexes, similar to those for dysprosocenium complexes, should enhance the SMM performances of SN-based lanthanide compounds.
中文翻译：
通过镝配合物中的配体设计增强空间位阻：从诱导缓慢弛豫到零场单分子磁体特性
三种新型 Dy 化合物的合成和磁性表征，[Dy{PPh 2 S(N t Bu) 2 } 2 (μ-Cl 2 )Li(THF) 2 ] ( 1 ), [Dy{PhS(N t Bu) 2 } 2 (μ-Cl 2 )Li(THF) 2 ] ( 2 ) 和 [Dy{MeS(N t Bu) 3 } 2 (μ-Cl 2 )Li(THF) 2 ] ( 3 )，基于硫-氮配体 RS(N t Bu) x –（其中 R = PPh 2，x = 2 对于 ( 1 ); R = Ph, x = 2 对于 ( 2 ); 和 R = Me, x = 3 for ( 3 )) 被报道。它们代表了含有硫 - 氮配体的镧系元素络合物的罕见例子，其适用于增强 3d 金属中的磁各向异性直到最近才被确定。配体场环境的变化极大地影响了磁性，化合物1和2显示了场诱导的单分子磁体 (SMM) 行为，而化合物3在零场显示缓慢弛豫。这些趋势强烈表明，线性镝配合物的配体工程策略，类似于镝络合物，应该提高基于 SN 的镧系元素化合物的 SMM 性能。
更新日期：2021-09-20
中文翻译：
通过镝配合物中的配体设计增强空间位阻：从诱导缓慢弛豫到零场单分子磁体特性
三种新型 Dy 化合物的合成和磁性表征，[Dy{PPh 2 S(N t Bu) 2 } 2 (μ-Cl 2 )Li(THF) 2 ] ( 1 ), [Dy{PhS(N t Bu) 2 } 2 (μ-Cl 2 )Li(THF) 2 ] ( 2 ) 和 [Dy{MeS(N t Bu) 3 } 2 (μ-Cl 2 )Li(THF) 2 ] ( 3 )，基于硫-氮配体 RS(N t Bu) x –（其中 R = PPh 2，x = 2 对于 ( 1 ); R = Ph, x = 2 对于 ( 2 ); 和 R = Me, x = 3 for ( 3 )) 被报道。它们代表了含有硫 - 氮配体的镧系元素络合物的罕见例子，其适用于增强 3d 金属中的磁各向异性直到最近才被确定。配体场环境的变化极大地影响了磁性，化合物1和2显示了场诱导的单分子磁体 (SMM) 行为，而化合物3在零场显示缓慢弛豫。这些趋势强烈表明，线性镝配合物的配体工程策略，类似于镝络合物，应该提高基于 SN 的镧系元素化合物的 SMM 性能。
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