Synthesis and study of CuII complex with nitroxide, a jumping crystal analog View Full Text


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Article Info

DATE

2017-02

AUTHORS

R. Z. Sagdeev, S. E. Tolstikov, S. V. Fokin, I. V. Obsharova, S. V. Tumanov, S. L. Veber, G. V. Romanenko, A. S. Bogomyakov, M. V. Fedin, E. V. Tretyakov, M. Halcrow, V. I. Ovcharenko

ABSTRACT

We synthesized 1-ethylimidazolyl-substituted nitronyl nitroxides, i.e., 2-(1-ethylimidazol-4-yl)- (L4Et) and 2-(1-ethylimidazol-5-yl)-4,4,5,5-tetramethyl-4,5-dihydro-1H-imidazole 3-oxide-1-oxyl (L5Et). The stable radical L5Et is an ethyl analog of 2-(1-methylimidazol-5-yl)-4,4,5,5-tetramethyl-4,5-dihydro-1H-imidazole 3-oxide-1-oxyl (L5Me) described earlier, the reaction of which with Cu(hfac)2 (hfac is 1,1,1,5,5,5-hexafluoropentane-2,4-dionate) leads to the formation of the [Cu(hfac)2(L5Me)2] jumping crystals. The reaction of Cu(hfac)2 with L5Et with reagent ratios 1: 2 and 1: 1 yields heterospin complexes [Cu(hfac)2(L5Et)2] and [Cu(hfac)2L5Et]2, respectively. X-ray diffraction study of the mononuclear complex [Cu(hfac)2(L5Et)2] determined that the compound has a packing similar to that of jumping crystals studied earlier, with the only difference being that the O...O contacts between neigh- boring nitroxide groups were found to be 0.3—0.5 Å longer than in [Cu(hfac)2(L5Me)2]. As a result of the lengthening of these contacts, [Cu(hfac)2(L5Et)2] crystals lack chemomechanical activi- ty. We found that when cooling crystals of binuclear complex [Cu(hfac)2L5Et]2 below 50 K, the antiferromagnetic exchange between unpaired electrons of the >N—•O groups of neighboring molecules leads to the full spin-pairing of the nitroxides, with only the Cu2+ ions contributing to the residual paramagnetism of the compound. More... »

PAGES

222-230

Identifiers

URI

http://scigraph.springernature.com/pub.10.1007/s11172-017-1722-y

DOI

http://dx.doi.org/10.1007/s11172-017-1722-y

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1090363498


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    "description": "We synthesized 1-ethylimidazolyl-substituted nitronyl nitroxides, i.e., 2-(1-ethylimidazol-4-yl)- (L4Et) and 2-(1-ethylimidazol-5-yl)-4,4,5,5-tetramethyl-4,5-dihydro-1H-imidazole 3-oxide-1-oxyl (L5Et). The stable radical L5Et is an ethyl analog of 2-(1-methylimidazol-5-yl)-4,4,5,5-tetramethyl-4,5-dihydro-1H-imidazole 3-oxide-1-oxyl (L5Me) described earlier, the reaction of which with Cu(hfac)2 (hfac is 1,1,1,5,5,5-hexafluoropentane-2,4-dionate) leads to the formation of the [Cu(hfac)2(L5Me)2] jumping crystals. The reaction of Cu(hfac)2 with L5Et with reagent ratios 1: 2 and 1: 1 yields heterospin complexes [Cu(hfac)2(L5Et)2] and [Cu(hfac)2L5Et]2, respectively. X-ray diffraction study of the mononuclear complex [Cu(hfac)2(L5Et)2] determined that the compound has a packing similar to that of jumping crystals studied earlier, with the only difference being that the O...O contacts between neigh- boring nitroxide groups were found to be 0.3\u20140.5 \u00c5 longer than in [Cu(hfac)2(L5Me)2]. As a result of the lengthening of these contacts, [Cu(hfac)2(L5Et)2] crystals lack chemomechanical activi- ty. We found that when cooling crystals of binuclear complex [Cu(hfac)2L5Et]2 below 50 K, the antiferromagnetic exchange between unpaired electrons of the >N\u2014\u2022O groups of neighboring molecules leads to the full spin-pairing of the nitroxides, with only the Cu2+ ions contributing to the residual paramagnetism of the compound.", 
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