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21.
Novel alkaline earth metal aryl-substituted silylamides were prepared using alkane (Mg) and salt elimination reactions (Mg, Ca, Sr, and Ba). The salt elimination regime involved the treatment of the alkaline earth metal iodides with 2 equiv of the respective potassium amide KNDiip(SiMe(3)), (Diip = 2,6-i-Pr(2)C(6)H(3)). The organomagnesium source for the alkane elimination was ((n)()Bu/(s)()Bu)(2)Mg. All compounds were characterized using (1)H, (13)C NMR, and IR spectroscopy, in addition to X-ray crystallography (except Mg[NDiip(SiMe(3))](2)THF(2)). Crystal data with Mo Kalpha (lambda = 0.710 73 A) are as follows: Mg[NDiip(SiMe(3))](2), 1, a = 9.4687(6) A, b = 9.6818(6) A, c = 17.9296(1) A, alpha = 96.487(1) degrees, beta = 94.537(1) degrees, gamma = 89.222(1) degrees, V = 1608.8(2) A(3), Z = 2 (two independent molecules), triclinic, space group P(-)1, R1 (all data) = 0.0508; (n)()BuMg[NDiip(SiMe(3))]THF(2), 2, a = 9.5413(1) A, b = 16.493(2) A, c = 9.8218(1) A, beta = 108.149(2) degrees, V = 1468.7(4) A(3), Z = 2, monoclinic, space group P2(1), R1(all data) = 0.1232; Ca[NDiip(SiMe(3))](2)THF(2), 4, a = 9.7074(1) A, b = 20.9466(4) A, c = 21.6242(3) A, alpha = 73.573(1) degrees, beta = 78.632(1) degrees, gamma = 89.621(1) degrees, V = 4129.1(1) A(3), Z = 4 (two independent molecules), triclinic, space group P(-)1, R1 (all data) = 0.0902; Sr[NDiip(SiMe(3))](2)THF(2), 5, a = 20.5874(5) A, b = 9.8785(2) A, c = 20.8522(5) A, beta = 102.035(2) degrees, V = 4147.6(2) A(3), Z = 4 (two independent molecules), monoclinic, space group P2/n, R1 (all data) = 0.0756; Ba[NDiip(SiMe(3))](2)THF(2), 6, a = 20.5476(2) A, b = 10.0353(2) A, c = 20.9020(4) A, beta = 101.657(1) degrees, V = 4221.0(1) A(3), Z = 4 (two independent molecules), monoclinic, space group P2/n, R1 (all data) = 0.0573. 相似文献
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23.
Miguel A. Miranda Francisco Boscaa Franklin Vargas Nieves Canudas 《Photochemistry and photobiology》1994,59(2):171-174
Fenofibric acid, the major metabolite of fenofibrate, was found to be photolabile. Its irradiation in aqueous solution gave rise to two photoproducts, whose formation involves photodecarboxylation of the dissociated acid to an aryloxy-substituted carbanion, which is directly protonated or, alternatively, undergoes a Wittig rearrangement. A comparative in vitro phototoxicity study has been carried out on the anti-hyperlipoproteinemic drug fenofibrate, its metabolites and the photoproducts of fenofibric acid. Fenofibrate, fenofibric acid and its two photoproducts were found to be active when examined by the photohemolysis test and were able to photosensitize peroxidation of linoleic acid, as evidenced by the UV monitoring of dienic hydroperoxides. In summary, the major metabolite of fenofibrate (fenofibric acid), as well as its photoproducts, are phototoxic in vitro . This behavior can be attributed to the fact that the four compounds retain the benzophenone chromophore present in fenofibrate and is indicative of free radicalmediated photosensitization. In agreement with this rationalization, the metabolites with a reduced ketone functionality exhibit no detectable in vitro phototoxicity. 相似文献
24.
In this work the effect of the basis set superposition error (BSSE) is explored with the counterpoise method on the occupied and unoccupied Hartree-Fock (HF) and Kohn-Sham (KS) orbitals. Three different systems linked by hydrogen bonds, H(2)O...FH, H(2)O...H(2)O, and H(2)O...CFH(3), were studied by using the basis set families cc-pVXZ and aug-cc-pVXZ (X = D, T, Q). The basis sets were tested with the HF method and two approximations for the exchange-correlation functional of KS: a generalized gradient approximation and a hybrid approach. In addition to these methods, the second-order M?ller-Plesset perturbation theory, MP2, was considered. It was found that the presence of the "ghost" basis set affects the orbitals in two ways: (1) The occupied KS orbitals are more sensitive to the presence of this "ghost" basis set than the occupied HF orbitals. For this reason the BSSE observed in HF is less than that obtained with KS. (2) The unoccupied HF orbitals are more sensitive to the presence of the "ghost" basis set than their corresponding occupied orbitals. Because the MP2 method uses both, occupied and unoccupied HF orbitals, to compute the total energy, the contribution of the BSSE is bigger than that obtained with HF or KS methodologies. 相似文献
25.
Angelo J. Amoroso Brian F. G. Johnson Jack Lewis Chi-Keung Li Catherine A. Morewood Paul R. Raithby Maria D. Vargas Wing-Tak Wong 《Journal of Cluster Science》1995,6(1):163-173
Reduction of the heptaosmium cluster [Os7(CO)21] With [Et4N][NH4) gives the cluster dianion [Os7(CO)20]2–,1, in high yield. The reaction of the dianion with [AuPR
3Cl] (R=Et or Ph) in the presence of TlPF6 forms [Os7((CO)20(AuPR
3)2] [R=Et (2a);R = Ph(2b)] in 80% yield, while the corresponding reaction with (Os(C6H6)(CH3CN)3]2+ gives [Os8(CO)20 (
6-C6H6)] (3) in reasonable yield (ca. 30%). The dianion,1, and the clusters2 and3 have been fully characterized by bout spectroscopic and crystallographic methods. The crystal structure of the [Ph4P]+ salt of1 shows that the metals in the anion adopt a capped octahedral geometry, with all twenty carbonyl ligands in terminal sites. The metal core geometry in2a is best described as a tricapped octahedron, and is based on the structure of the dianion1 with two adjacent octahedral faces capped by the Au atoms of the two AuPEt3 groups. In a similar fashion, the geometry of3 is related to that of1 with the addition of an Os(C6H6) unit capped to a triangular face, to give a bicapped octahedral framework. 相似文献
26.
José G. Vargas 《Foundations of Physics》1992,22(4):507-526
A connection viewed from the perspective of integration has the Bianchi identities as constraints. It is shown that the removal of these constraints admits a natural solution on manifolds endowed with a metric and teleparallelism. In the process, the equations of structure and the Bianchi identities take standard forms of field equations and conservation laws.The Levi-Civita (part of the) connection ends up as the potential for the gravity sector, where the source is geometric and tensorial and contains an explicit gravitational contribution.Nonlinear field equations for the torsion result. In a low-energy approximation (linearity andlow energy-momentumtransfer), the postulate that only charge and velocities contribute to the source transforms these equations into the Maxwell system. Moreover, the affine geodesics become the equations of motion of special relativity with Lorentz force in the same approximation [J. G. Vargas,Found. Phys.
21, 379 (1991)]. The field equations for the torsion must then be viewed as applying to an electromagnetic/strong interaction.A classical unified theory thus arises where the underlying geometry confers their contrasting characters to Maxwell-Lorentz electrodynamics and to an Einstein's-like theory of gravity. The highly compact field equations must, however, be developed in phase-spacetime, since the connection is velocity-dependent, i.e., Finsler-like.Further opportunities for similarities with present-day physics are discussed: (a) teleparallelism allows for the formulation of the torsion sector of the theory as a flat space theory with concomitant point-dependent transformations; (b) spinors should replace Lorentz frames in their role as the subjects to which the connection refers; (c) the Dirac equation consistent with the frame bundle for a velocity-dependent metric with Lorentz signature generates a weak-like interaction in the torsion sector.Work done at the Department of Mathematics and Physics of the Interamerican University of Puerto Rico, San German, Puerto Rico 00683. 相似文献
27.
28.
M. E. Vargas J. D. Batchelor E. A. Schweikert 《Journal of Radioanalytical and Nuclear Chemistry》1987,119(2):81-86
The determination of lead via 30 MeV4He bombardment to produce the long-lived radioisotope210Po was studied. The validity of the technique was tested by the analysis of a series of NBS glass samples doped with 61 different trace elements at nominal 500 to 1 ppm level concentrations. The measurement sensitivity of alpha counting with surface barrier detectors was evaluated. The detection limit was estimated at 0.1 ppm. The4He-activation technique coupled with -counting features a unique combination of sensitivity and accuracy for the trace determination of lead. 相似文献
29.
R. Rodríguez G. Rojas M. Estevez S. Vargas 《Journal of Sol-Gel Science and Technology》2002,23(2):99-105
The fractal characterization of silica particles prepared by the sol-gel method was obtained; from the beginning of the sol-gel synthesis to the aggregation process of these particles by adding metal ions in solution, the fractal dimension was determined. At the beginning of the sol-gel process, unstable structures were formed due, essentially, to the auto-catalytic nature of the sol-gel condensation reactions; these particles are fractal structures with a fractal exponent corresponding to a reaction limited aggregation regime. As the time proceeds, the reactants are consumed approaching the system to equilibrium, stabilizing the size of the silica particles. The silica sol can be flocculated by adding metal ions in solution. The fractal exponent for the aggregation process was determined, obtaining a value corresponding to a diffusion limited aggregation regime. 相似文献
30.