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首页> 外文期刊>Acta Crystallographica, Section B. Structural Science >TEMPO radicals showing magnetic interactions. II. 4-(benzylideneamino)-TEMPO and related compounds
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TEMPO radicals showing magnetic interactions. II. 4-(benzylideneamino)-TEMPO and related compounds

机译：TEMPO自由基显示出磁性相互作用。二。 4-（亚苄基氨基）-TEMPO及相关化合物

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摘要

X-ray crystal structure analyses were performed on 4-(Ar-methyleneamino)-TEMPO radicals at room temperature (TEMPO = 2,2,6,6-tetramethylpiperidyl-1-oxyl): Ar = Ph [4-(benzylideneamino)-2,2,6,6-tetra-methylpiperidyl-1-oxyl], 4-MeS-Ph [2,2,6,6-tetramethyl-4-(4-methylthiobenzylideneamino)piperidyl-1-oxyl], 4-Me-Ph [4-(4-methylbenzylideneamino)-2,2,6,6-tetramethylpiperidyl-1-oxyl], 4-PhO-Ph [2,2,6,6-tetramethyl-4-(4-phenoxybenzylideneamino)piperidyl-1-oxyl], 4-MeSO2-Ph [2,2,6,6-tetramethyl-4-(4-methylsulfonylbenzylideneamino)piperidyl-1-oxyl] , 3-Py [2,2,6,6-tetramethyl-4-(3-pyridylmethylideneamino)piperidyl-1-oxyl] and 2-Naph [2,2,6,6-tetramethyl-4-(2-naphthylideneamino)piperidyl-1-oxyl]. Structures of Ph and 4-Me-Ph derivatives were also determined at 100 K. Some of these crystals have been revealed to show intermolecular ferromagnetic interactions at an extremely low temperature. Structural features of crystals of Ph, 4-MeS-Ph and 3-Py derivatives, which show ferromagnetic interactions, are very similar to each other. In these crystals, O atoms are arranged to form a sheet. The ferromagnetic interactions are considered to be transferred through O ... H van der Waals' interactions of the B-H atoms of the neighboring TEMPO rings within the sheet. Between O ... O sheets, the aryl groups are arranged in a herringbone manner. The crystal structure of the 4-Me-Ph derivative, which shows an antiferromagnetic interaction, is also pseudo-isostructural with those of Ph, 4-MeS-Ph and 3-Py derivatives, while the arrangement of the aryl groups is different. The packing mode of the crystals of the 4-MeSO2-Ph derivative, of which the Weiss constant theta is nearly zero, is very different from those of the other derivatives showing magnetic interactions. The fact that the crystal structure of the paramagnetic 4-MeSO2-Ph derivative does not show the O ... O sheet structure accompanying the O ...beta-H interactions indicates that the intermolecular ferromagnetic interactions through B-H atoms within the O ... O sheet are important for these TEMPO radical crystals. [References: 20]
机译：在室温下对4-（Ar-亚甲基氨基）-TEMPO基团进行X射线晶体结构分析（TEMPO = 2,2,6,6-四甲基哌啶-1-氧基）：Ar = Ph [4-（苄叉基氨基）- 2,2,6,6-四甲基哌啶基-1-氧基]，4-MeS-Ph [2,2,6,6-四甲基-4-（4-甲基硫代亚苄基氨基）哌啶基-1-氧基]，4-Me -Ph [4-（4-甲基苄叉基氨基）-2,2,6,6-四甲基哌啶-1-氧基]，4-PhO-Ph [2,2,6,6-四甲基-4-（4-苯氧基苄叉基氨基）哌啶基-1-氧基]，4-MeSO2-Ph [2,2,6,6-四甲基-4-（4-甲基磺酰基亚苄基氨基）哌啶基-1-氧基]，3-Py [2,2,6,6-四甲基- 4-（3-吡啶基甲叉基氨基）哌啶基-1-氧基]和2-萘酚[2,2,6,6-四甲基-4-（2-萘叉基氨基）哌啶基-1-氧基]。还可以在100 K下测定Ph和4-Me-Ph衍生物的结构。这些晶体中的某些已显示在极低的温度下显示出分子间铁磁相互作用。显示铁磁相互作用的Ph，4-MeS-Ph和3-Py衍生物的晶体结构特征非常相似。在这些晶体中，O原子排列成片。铁磁相互作用被认为是通过板内相邻TEMPO环的B-H原子的O ... H van der Waals相互作用传递的。在O ... O片之间，芳基以人字形方式排列。显示出反铁磁相互作用的4-Me-Ph衍生物的晶体结构与Ph，4-MeS-Ph和3-Py衍生物的晶体结构也是伪同构，而芳基的排列不同。 Weiss常数theta几乎为零的4-MeSO2-Ph衍生物的晶体堆积模式与其他表现出磁性相互作用的衍生物的堆积模式非常不同。顺磁性4-MeSO2-Ph衍生物的晶体结构未显示伴随O.beta-H相互作用的O.O片层结构，这一事实表明通过O.内的BH原子进行了分子间铁磁相互作用。 O片对于这些TEMPO自由基晶体很重要。 [参考：20]

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