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Asanbaeva Nargiz B. Rychkov Denis A. Tyapkin Pavel Yu. Arkhipov Sergey G. Uvarov Nikolay F. 《Structural chemistry》2021,32(3):1261-1267
Structural Chemistry - The crystal and molecular structure of tris(tetrabutylammonium) pentanitratoplumbate(II) was determined and characterized by single-crystal and powder X-ray diffraction and... 相似文献
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Nargiz B. Asanbaeva Larisa Yu. Gurskaya Yuliya F. Polienko Tatyana V. Rybalova Maxim S. Kazantsev Alexey A. Dmitriev Nina P. Gritsan Nadia Haro-Mares Torsten Gutmann Gerd Buntkowsky Evgeny V. Tretyakov Elena G. Bagryanskaya 《Molecules (Basel, Switzerland)》2022,27(10)
Spiro-substituted nitroxyl biradicals are widely used as reagents for dynamic nuclear polarization (DNP), which is especially important for biopolymer research. The main criterion for their applicability as polarizing agents is the value of the spin–spin exchange interaction parameter (J), which can vary considerably when different couplers are employed that link the radical moieties. This paper describes a study on biradicals, with a ferrocene-1,1′-diyl-substituted 1,3-diazetidine-2,4-diimine coupler, that have never been used before as DNP agents. We observed a substantial difference in the temperature dependence between Electron Paramagnetic Resonance (EPR) spectra of biradicals carrying either methyl or spirocyclohexane substituents and explain the difference using Density Functional Theory (DFT) calculation results. It was shown that the replacement of methyl groups by spirocycles near the N-O group leads to an increase in the contribution of conformers having J ≈ 0. The DNP gain observed for the biradicals with methyl substituents is three times higher than that for the spiro-substituted nitroxyl biradicals and is inversely proportional to the contribution of biradicals manifesting the negligible exchange interaction. The effects of nucleophiles and substituents in the nitroxide biradicals on the ring-opening reaction of 1,3-diazetidine and the influence of the ring opening on the exchange interaction were also investigated. It was found that in contrast to the methyl-substituted nitroxide biradical (where we observed the ring-opening reaction upon the addition of amines), the ring opening does not occur in the spiro-substituted biradical owing to a steric barrier created by the bulky cyclohexyl substituents. 相似文献
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Rogozhnikova O. Yu. Trukhin D. V. Asanbaeva N. B. Tormyshev V. M. 《Russian Journal of Organic Chemistry》2021,57(6):905-913
Russian Journal of Organic Chemistry - The reaction of tris(8-carboxy-2,2,6,6-tetramethylbenzo[1,2-d;4,5-d′]bis[1,3]dithiol-4-yl)methanol, diamagnetic precursor of Finland trityl radical}... 相似文献
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