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151.
Andrey A. Fokin Prof. Dr. Boryslav A. Tkachenko Dr. Natalie A. Fokina Dr. Heike Hausmann Dr. Michael Serafin Dr. Jeremy E. P. Dahl Dr. Robert M. K. Carlson Dr. Peter R. Schreiner Prof. Dr. 《Chemistry (Weinheim an der Bergstrasse, Germany)》2009,15(15):3851-3862
Functionalized nanodiamonds : Various functional groups have been incorporated into the structures of the naturally occurring diamondoids [1(2)3]tetramantane and [12312]hexamantane (cyclohexamantane), which represent hydrogen‐terminated prism‐shaped nanodiamonds (see picture). The attachment points define the use of these diamond‐like molecules as geometric building blocks for a variety of applications.
152.
A. S. Sklyarova V. N. Rodionov A. A. Fokin 《Russian Journal of Organic Chemistry》2009,45(11):1633-1636
By reaction of pentacyclo[5.3.0.02,5.03,9.04,8]decane-6,10-dione 6-ethyleneketal with lithium aluminum hydride the corresponding hydroxyketal was obtained whose hydroxy
group was replaced by chlorine at boiling in CCl4 in the presence of a 15% molar excess of triphenylphosphine. 6-Ethyleneketal of pentacyclo-[5.3.0.02,5.03,9.04,8]decan-6-one obtained by dechlorination of the chloroketal in a system lithium-t-BuOH in THF was hydrolyzed to ketone by heating in 10% sulfuric acid in the presence of THF. The obtained ketone was reduced
along Wolf-Kishner reaction to pentacyclo[5.3.0.02,5.03,9.04,8]decane. 相似文献
153.
E. V. Tretyakov S. V. Fokin G. V. Romanenko V. N. Ikorskii A. V. Podoplelov V. I. Ovcharenko 《Russian Chemical Bulletin》2006,55(1):66-73
An efficient procedure was developed for the synthesis of alkyltetrazolyl-substituted nitronyl nitroxides (L
1 and L
2). These compounds were used to prepare the first alkyltetrazolyl-substituted imino nitroxides (L
3 and L
4). The molecular structures of L
3 and L
4 were confirmed by X-ray diffraction. Investigation of the products prepared by the reaction of copper(II) bis(hexafluoroacetylacetonate), Cu(hfac)2, with nitroxides made it possible to divide ligands L
1—L
4 into two groups. The reactions of spin-labeled tetrazoles L
1—L
3 with Cu(hfac)2 afford the heterospin complexes Cu(hfac)2L2, whereas L
4 serves as a bidentate ligand in the Cu(hfac)2
L
4 complex. In the solid Cu(hfac)2L2 complexes, antiferromagnetic exchange interactions between the unpaired electrons of the nitroxide fragments of the adjacent
molecules prevail, due to which μeff decreases with decreasing temperature, and the spins of nitroxides are completely compensated at 5–10 K. The Cu(hfac)2
L
4 complex displays strong intramolecular ferromagnetic coupling, due to which μeff at room temperature is close to 2.9 μB.
Published in Russian in Izvestiya Akademii Nauk. Seriya Khimicheskaya, No. 1, pp. 64–70, January, 2006. 相似文献
154.
V. I. Ovcharenko S. V. Fokin G. V. Romanenko V. N. Ikorskii R. Z. Sagdeev D. S. Yachevskii D. L. Chizhov V. N. Charushin 《Russian Chemical Bulletin》2006,55(11):1904-1908
Heterospin complexes of bis(μ2-1,1,2,2,8,8,9,9-octafluorononane-3,5,7-trionato)dicopper(II) ([Cu2L2]) with nitronyl nitroxides 2-(1-methyl-1H-pyrazol-4-yl)-4,4,5,5-tetramethyl-4,5-dihydro-1H-imidazole-1-oxyl 3-oxide (2) and 4,4,5,5-tetramethyl-2-(3-pyridinyl)-4,5-dihydro-1H-imidazole-1-oxyl 3-oxide (1) were synthesized and structurally characterized. Crystals of the complexes are formed by the discrete bis[1-methyl-4-(4,4,5,5-tetramethyl-3-oxide-1-oxyl-4,5-dihydro-1H-imidazol-2-yl)-1H-pyrazole]-bis (μ2-1,1,2,2,8,8,9,9-octafluorononane-3,5,7-trionato)dicopper(II) etherate (3) and bis[3-(4,4,5,5-tetramethyl-3-oxide-1-oxyl-4,5-dihydro-1H-imidazol-2-yl)pyridine]-bis (μ2-1,1,2,2,8,8,9,9-octafluorononane-3,5,7-trionato)dicopper(II) (4) molecules. Each Cu atom of the dinuclear chelate fragment coordinates one paramagnetic ligand through the N atom of the
pyrazole or pyridine fragment, respectively. In complex 3, the paramagnetic ligands are located on one side of the plane of the chelate fragment, whereas the ligands in complex 4 are located above and below the plane of the chelate fragment. The magnetic properties of complexes 3 and 4 are determined by dominant antiferromagnetic exchange interactions between the unpaired electrons of the CuII atoms in the dinuclear Cu2L2 moiety.
Dedicated to Academician O. M. Nefedov on the occasion of his 75th birthday.
Published in Russian in Izvestiya Akademii Nauk. Seriya Khimicheskaya, No. 11, pp. 1836–1840, November, 2006. 相似文献
155.
E. A. Brui A. V. Shchelokova A. V. Sokolov A. P. Slobozhanyuk A. E. Andreychenko V. A. Fokin P. A. Belov I. V. Melchakova 《JETP Letters》2018,108(6):423-427
A hybrid metasurface realized by a double array of brass wires inserted into two high-permittivity dielectric slabs at both sides was used to perform a magnetic resonance spectroscopy experiment at a 1.5 T clinical magnetic resonance scanner. The metasurface coupled inductively to a transceive birdcage body coil located within the scanner’s bore. The metasurface demonstrated an enhancement of the signal-to-noise ratio of the magnetic resonance spectroscopy experiment in vitro. Up to a signal-to-noise ratio gain of 7.4 for choline and creatine spectral lines was observed in the presence of the metasurface compared to the body coil alone. 相似文献
156.
Grimster NP Stump B Fotsing JR Weide T Talley TT Yamauchi JG Nemecz Á Kim C Ho KY Sharpless KB Taylor P Fokin VV 《Journal of the American Chemical Society》2012,134(15):6732-6740
Nicotinic acetylcholine receptors (nAChRs), which are responsible for mediating key physiological functions, are ubiquitous in the central and peripheral nervous systems. As members of the Cys loop ligand-gated ion channel family, neuronal nAChRs are pentameric, composed of various permutations of α (α2 to α10) and β (β2 to β4) subunits forming functional heteromeric or homomeric receptors. Diversity in nAChR subunit composition complicates the development of selective ligands for specific subtypes, since the five binding sites reside at the subunit interfaces. The acetylcholine binding protein (AChBP), a soluble extracellular domain homologue secreted by mollusks, serves as a general structural surrogate for the nAChRs. In this work, homomeric AChBPs from Lymnaea and Aplysia snails were used as in situ templates for the generation of novel and potent ligands that selectively bind to these proteins. The cycloaddition reaction between building-block azides and alkynes to form stable 1,2,3-triazoles was used to generate the leads. The extent of triazole formation on the AChBP template correlated with the affinity of the triazole product for the nicotinic ligand binding site. Instead of the in situ protein-templated azide-alkyne cycloaddition reaction occurring at a localized, sequestered enzyme active center as previously shown, we demonstrate that the in situ reaction can take place at the subunit interfaces of an oligomeric protein and can thus be used as a tool for identifying novel candidate nAChR ligands. The crystal structure of one of the in situ-formed triazole-AChBP complexes shows binding poses and molecular determinants of interactions predicted from structures of known agonists and antagonists. Hence, the click chemistry approach with an in situ template of a receptor provides a novel synthetic avenue for generating candidate agonists and antagonists for ligand-gated ion channels. 相似文献
157.
V. A. Vazhenin A. P. Potapov A. V. Fokin M. Yu. Artyomov 《Physics of the Solid State》2012,54(12):2450-2455
In the EPR spectra of iron-doped lead germanate single crystals, triclinic Fe3+ paramagnetic centers have been found in addition to trigonal centers. Their contribution increases upon annealing in a chlorine-containing atmosphere. The parameters of the spin Hamiltonian of three triclinic centers assigned to Fe3+-Cl? dimeric complexes have been determined. The localization of iron and chlorine ions in Pb5Ge3O11 has been discussed. 相似文献
158.
J Jiaranaikulwanitch P Govitrapong VV Fokin O Vajragupta 《Molecules (Basel, Switzerland)》2012,17(7):8312-8333
Efforts to discover new drugs for Alzheimer's disease emphasizing multiple targets was conducted seeking to inhibit amyloid oligomer formation and to prevent radical formation. The tryptoline and tryptamine cores of BACE1 inhibitors previously identified by virtual screening were modified in silico for additional modes of action. These core structures were readily linked to different side chains using 1,2,3-triazole rings as bridges by copper catalyzed azide-alkyne cycloaddition reactions. Three compounds among the sixteen designed compounds exerted multifunctional activities including β-secretase inhibitory action, anti-amyloid aggregation, metal chelating and antioxidant effects at micromolar levels. The neuroprotective effects of the multifunctional compounds 6h, 12c and 12h on Aβ???? induced neuronal cell death at 1 μM were significantly greater than those of the potent single target compound, BACE1 inhibitor IV and were comparable to curcumin. The observed synergistic effect resulting from the reduction of the Aβ???? neurotoxicity cascade substantiates the validity of our multifunctional strategy in drug discovery for Alzheimer's disease. 相似文献
159.
A A Fokin O Lauenstein P A Gunchenko P R Schreiner 《Journal of the American Chemical Society》2001,123(9):1842-1847
The first highly selective C-H chlorination, bromination, and iodination of cubane (1) utilizing polyhalomethanes as halogen sources under phase-transfer (PT) conditions is described. Isomeric dihalocubanes with all possible combinations of chlorine, bromine, and iodine in ortho, meta, and para positions were also prepared by this method; m-dihalo products form preferentially. Ab initio and density functional theory (DFT) computations were used to rationalize the pronounced differences in the reactions of 1 with halogen (Hal(*)) vs carbon-centered trihalomethyl (Hal(3)C(*)) radicals (Hal = Cl, Br). For Hal(3)C radicals the C-H abstraction pathway is less unfavorable (DeltaG(double dagger)(298) = 21.6 kcal/mol for Cl(3)C(*) and 19.4 kcal/mol for Br(3)C(*) at B3LYP/6-311+G//B3LYP/6-31G) than the fragmentation of the cubane skeleton via S(H)2-attack on one of the carbon atoms of 1 (DeltaG(double dagger)(298) = 33.8 and 35.1 kcal/mol, respectively). In stark contrast, the reaction of 1 with halogen atoms preferentially follows the fragmentation pathway (DeltaG(double dagger)(298) = 2.1 and 7.5 kcal/mol) and C-H abstraction is more unfavorable (DeltaG(double dagger)(298) = 4.6 and 12.0 kcal/mol). Our computational results nicely agree with the behavior of 1 under PT halogenation conditions (where Hal(3)C(*) is involved in the activation step) and under free-radical photohalogenation with Hal(2) (Della, E. W., et al. J. Am. Chem. Soc. 1992, 114, 10730). The incorporation of a second halogen atom preferentially in the meta position of halocubanes demonstrates the control of the regioselectivity by molecular orbital symmetry. 相似文献
160.
Potapov A. P. Vazhenin V. A. Petrosyan A. G. Fokin A. V. 《Physics of the Solid State》2018,60(12):2559-2564
Physics of the Solid State - Electron paramagnetic resonance of rhombic Eu2+ centers in single crystals of Lu3Al5O12 doped with europium ions with the natural isotope abundance was studied.... 相似文献