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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Modulating the magnetization dynamics in Ln-Cu-Rad hetero-tri-spin complexes through cis/trans coordination of nitronyl nitroxide radicals around the metal center
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Modulating the magnetization dynamics in Ln-Cu-Rad hetero-tri-spin complexes through cis/trans coordination of nitronyl nitroxide radicals around the metal center

机译：通过在金属中心周围的氮氮氮氧化物基团的顺式/反式协调调节LN-Cu-rad杂环三旋络合物中的磁化动力学

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摘要

Self-assembling the novel nitronyl nitroxide radical NIT-3Py-5-Ph (2-(5-phenyl-3-pyridyl)-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide) with Ln(hfac)(3)center dot 2H(2)O and Cu(hfac)(2) (hfac = hexafluoroacetylacetonate) resulted in two heterometallic complexes with formula [LnCu(hfac)(5)(NIT-3Py-5-Ph)(2)] (Ln = Gd 1, Dy 2), in which two NIT-3Py-5-Ph radicals are coordinated with the Ln(III) ion via their nitroxide units in the cis-arrangement manner and the Cu-II ion is ligated by the pyridyl N donors of the radicals. Interestingly, when the phenyl group of NIT-3Py-5-Ph was replaced with a p-pyridyl group, a new family of 2D networks, namely, {[Ln(hfac)(3)][Cu(hfac)(2)](2)(NIT-3Py-5-4Py)(2)}(n) (Ln = Gd 3, Tb 4, Dy 5; NIT-3Py-5-4Py = 2-(5-(4-pyridyl)-3-pyridyl)-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide) was obtained. In the 2D sheet, each NIT-3Py-5-4Py ligand serves as a mu(3)-bridge to bind one Ln(III) center by the aminoxyl moiety and two Cu-II ions through two pyridine groups to form a 2D structure. The Ln(III) ion is coordinated by two NO units of two radicals in a trans configuration. DC magnetic measurements indicate that ferromagnetic Ln(III)-NO exchange occurs in 1-5. AC studies reveal that 2 displays slow relaxation of the magnetization while no such magnetic relaxation is found in complex 5. The observed different magnetic relaxation behaviors of two Dy analogues could be attributed to the different coordination modes of NO groups of the radicals, and the coordination geometry of the Dy center is from C-2v in 2 to D-2d in 5.
机译：新型亚硝基氮氧自由基NIT-3Py-5-Ph（2-（5-苯基-3-吡啶基）-4,4,5,5-四甲基咪唑啉-1-氧基-3-氧化物）与Ln（hfac）（3）中心点2H（2）O和Cu（hfac）（2）（hfac=六氟乙酰丙酮）自组装形成了两种具有式[LnCu（hfac）（5）（NIT-3Py-5-Ph）（2）]（Ln=Gd 1，Dy 2）的杂金属配合物，其中，两个NIT-3Py-5-Ph自由基以顺式排列方式通过氮氧化物单元与Ln（III）离子配位，CuⅡ离子由自由基的吡啶氮供体连接。有趣的是，当NIT-3Py-5-Ph的苯基被一个对吡啶基取代时，一个新的二维网络家族，即，{[Ln（hfac）（3）][Cu（hfac）（2）]（NIT-3Py-5-4Py）（2）}（n）（Ln=Gd 3，Tb 4，Dy 5；NIT-3Py-5-4Py=2-（5-（4-吡啶基）-3-吡啶基）-4,4,5,5-四甲基咪唑啉-1-氧基-3-氧化物）被获得。在2D薄片中，每个NIT-3Py-5-4Py配体作为一个mu（3）-桥，通过氨基部分和两个Cu II离子通过两个吡啶基团结合一个Ln（III）中心，形成2D结构。Ln（III）离子由两个反式构型的自由基的两个NO单元配位。直流磁场测量表明，铁磁性Ln（III）-在1-5中没有发生交换。交流研究表明，配合物2表现出缓慢的磁化弛豫，而在配合物5中未发现这种磁弛豫。观察到的两种Dy类似物的不同磁弛豫行为可归因于自由基中NO基团的不同配位模式，Dy中心的配位几何结构从2的C-2v到5的D-2d。

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    Lu Jiao; Jing Pei; Jin Chaoyi; Xie Junfang; Li Licun;

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    Nankai Univ Coll Chem Dept Chem Key Lab Adv Energy Mat Chem Tianjin 300071 Peoples R China;

    Nankai Univ Coll Chem Dept Chem Key Lab Adv Energy Mat Chem Tianjin 300071 Peoples R China;

    Nankai Univ Coll Chem Dept Chem Key Lab Adv Energy Mat Chem Tianjin 300071 Peoples R China;

    Nankai Univ Coll Chem Dept Chem Key Lab Adv Energy Mat Chem Tianjin 300071 Peoples R China;

    Nankai Univ Coll Chem Dept Chem Key Lab Adv Energy Mat Chem Tianjin 300071 Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;无机化学;
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