A.A. Belyaev, D.V. Krupenya, E.V. Grachova, V.V. Gurzhiy, A.S. Melnikov, P.Yu. Serdobintsev, E.S. Sinitsyna, E.G. Vlakh, T.B. Tennikova, S.P. Tunik
“Supramolecular AuI–CuI Complexes as New Luminescent Labels for Covalent Bioconjugation”
Bioconjugate Chem, 2016, 27, 143-150
Two new supramolecular organometallic complexes, namely, [Au6Cu2(C2C6H4CHO)6(PPh2C6H4PPh2)3](PF6)2 and [Au6Cu2(C2C6H4NCS)6(PPh2C6H4PPh2)3](PF6)2, with highly reactive aldehyde and isothiocyanate groups have been synthesized and characterized using X-ray crystallography, ESI mass spectrometry, and NMR spectroscopy. The compounds obtained demonstrated bright emission in solution with the excited-state lifetime in microsecond domain both under single- and two-photon excitation. The luminescent complexes were found to be suitable for bioconjugation in aqueous media. In particular, they are able to form the covalent conjugates with proteins of different molecular size (soybean trypsin inhibitor, human serum albumin, rabbit anti-HSA antibodies). The conjugates demonstrated a high level of the phosphorescent emission from the covalently bound label, excellent solubility, and high stability in physiological media. The highest quantum yield, storage stability, and luminance were detected for bioconjugates formed by covalent attachment of the aldehyde-bearing supramolecular AuI–CuI complex. The measured biological activity of one of the labeled model proteins clearly showed that introduced label did not prevent the biorecognition and specific protein–protein complex formation that was extremely important for the application of the conjugates in biomolecular detection and imaging.
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Статья пользователей РЦ МРМИ, попавшая на обложку журнала Inorganic Chemistry:
A.A. Penney, V.V. Sizov, E.V. Grachova, D.V. Krupenya, V.V. Gurzhiy, G.L. Starova, S.P. Tunik
“Aurophilicity in Action: Fine-Tuning the Gold(I)–Gold(I) Distance in the Excited State To Modulate the Emission in a Series of Dinuclear Homoleptic Gold(I)–NHC Complexes”
Inorg. Chem., 2016, 55, 4720-4732
The formation of exciplexes between cationic dinuclear Au(I) bis(carbene) complexes and bromide ions was found to decrease the Au−Au distance in the triplet excited state, leading to pronounced changes in emission. The stimuli-responsive nature of the intracationic aurophilic interaction paves the way for fine-tuning the emission energy and opens new possibilities for practical applications.
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Michael Vovk has successfully completed the training course “Advanced NMR Methods”. The course covered the uses of gradients, different options of shimming, set of 1D, 2D and 3D homonuclear and heteronuclear correlation experiments with gradient selection and water suppression, other aspects of modern NMR methods.
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| Tags: Vovk
Within the framework of the Congress of the University of Arctic (12-16.09.2016, St.Petersburg; http://www.uarctic.org/about-uarctic/events/uarctic-congress-2016/) Peter Tolstoy has given a presentation about the Research Park on the example of the Center for Magnetic Resonance. During the presentation a video-conference has been established, where CMR specialists Anton Mazur and Mikhail Vovk answered the questions about the current projects and the overall workload.
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M.S. Mishina, A.Yu. Ivanov, P.S. Lobanov, D.V. Dar’in
“A New Synthesis of 2-Aminoindoles and 6-Aminopyrrolo[3,2-d]pyrimidines from π-Deficient 1,2-Dihaloarenes and Geminal Enediamines”
Synthesis, 2016, 48, 2851-2862
An efficient approach for the synthesis of fused 2-aminopyrroles via geminal enediamines and π-deficient 1,2-dihaloarenes is presented. The two-step methodology includes aromatic nucleophilic substitution of the activated halogen of dihaloarene with enediamine C-nucleophilic center followed by Cu-catalyzed intramolecular N-arylation. This approach allows access to a variety of 2-amino-6-nitroindoles and 6-aminopyrrolo[3,2-d]pyrimidines (including N-mono- and N,N-disubstituted) in moderate and good yields under mild conditions.
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| Tags: Ivanov
E.S. Yandanova, D.M. Ivanov, M.L. Kuznetsov, A.G. Starikov, G.L. Starova, V.Yu. Kukushkin
“Recognition of S···Cl Chalcogen Bonding in Metal-Bound Alkylthiocyanates”
Chem. Commun., 2016, 52, 5565
Reaction of K2[PtCl4] with excess AlkSCN in water gives the alkylthiocyanate complexes trans-[PtCl2(AlkSCN)2] (Alk = Et 1, nPr 2; 80–85%). These species were studied, in particular, by X-ray crystallography. In the solid state, both 1 and 2 exhibit the previously unreported S···Cl chalcogen bonding, which consolidates the complexes into networks and leads to layered structures. Theoretical density functional theory calculations and Bader’s atoms in molecules analysis demonstrated two types of intermolecular interactions in tetramer (1)4, viz. the S···Cl chalcogen and the H···Cl hydrogen bonds. Despite that each particular S···Cl or H···Cl bonding is weak with the estimated energy of 1–2 kcal/mol, altogether they play a crucial role in the stabilization of the S2Cl2 fragment in (1)4, the basis set of superposition error corrected interaction energy being −12.8 kcal/mol per monomer complex molecule. The chalcogen bonding and the rhomboidal structure of the S2Cl2 fragment can be interpreted in terms of electrostatic arguments as a result of the interaction between the belt of negative electrostatic potential around the Cl atoms and the sulfur σ-holes. The natural bond orbital analysis revealed that both LP(S) → LP*(Pt)/σ*(Pt–N)/σ*(Pt–Cl) and LP(Cl) → σ*(S–C) types of hyperconjugative charge transfers are important in the chalcogen bonding.
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Total in August 1059 service applications were carried out.
All together measured:
- 1006 1H spectra
- 192 13C spectra
- 79 DEPT spectra
- 17 COSY spectra
- 9 NOESY spectra
- 2 31P spectra
- 10 19F spectra
129 applications were carried out.
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