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141.
Adam W Bargon RM Bosio SG Schenk WA Stalke D 《The Journal of organic chemistry》2002,67(20):7037-7041
The direct molybdenum-catalyzed sulfuration of a variety of isonitriles with elemental sulfur or propene sulfide as sulfur donors affords the corresponding isothiocyanates in good yields and under mild reaction conditions. A catalytic cycle is suggested, in which the molybdenum oxo disulfur complex operates as the active sulfur-transferring species. A novel adduct between the isonitrile and the molybdenum complex has been characterized by X-ray analysis and its association constant determined by UV-vis spectroscopy, but this adduct appears not to be involved in the sulfur-transfer process. 相似文献
142.
de Peralta Menendez RG Murray MM Andino SL 《IEEE transactions on bio-medical engineering》2004,51(9):1680-1683
This paper proposes a new strategy for improving the localization capabilities of linear inverse solutions, based on the relationship between the real solution and the estimated solution as described by the resolution matrix equation. Specifically, we present two alternatives based on either the partial or total inversion of the resolution matrix and applied them to the minimum norm solution, which is known for its poor performance in three-dimensional (3-D) localization problems. The minimum norm transformed inverse showed a clear improvement in 3-D localization. The strong dependence of localization errors with the eccentricity of the sources, characteristic of this solution, disappears after the proposed transformation. A similar effect is illustrated, using a realistic example where multiple generators at striate areas are active. While the original minimum norm incorrectly places the generators at extrastriate cortex, the transformed minimum norm localizes, for the example considered, the sources at their correct eccentricity with very low spatial blurring. 相似文献
143.
Stringer JA Bronnimann CE Mullen CG Zhou DH Stellfox SA Li Y Williams EH Rienstra CM 《Journal of magnetic resonance (San Diego, Calif. : 1997)》2005,173(1):40-48
Heating due to high power 1H decoupling limits the experimental lifetime of protein samples for solid-state NMR (SSNMR). Sample deterioration can be minimized by lowering the experimental salt concentration, temperature or decoupling fields; however, these approaches may compromise biological relevance and/or spectroscopic resolution and sensitivity. The desire to apply sophisticated multiple pulse experiments to proteins therefore motivates the development of probes that utilize the RF power more efficiently to generate a high ratio of magnetic to electric field in the sample. Here a novel scroll coil resonator structure is presented and compared to a traditional solenoid. The scroll coil is demonstrated to be more tolerant of high sample salt concentrations and cause less RF-induced sample heating. With it, the viable experimental lifetime of a microcrystalline ubiquitin sample has been extended by more than an order of magnitude. The higher B1 homogeneity and permissible decoupling fields enhance polarization transfer efficiency in 15N-13C correlation experiments employed for protein chemical shift assignments and structure determination. 相似文献
144.
Piras A Colussi S Trovarelli A Sergo V Llorca J Psaro R Sordelli L 《The journal of physical chemistry. B》2005,109(22):11110-11118
A series of CeO(2)/Al(2)O(3) samples with different ceria loadings in the range 0-25 wt % (0, 2, 5, 7.5, 15, and 25%) were prepared by incipient wetness and studied using several complementary techniques such as Brunauer-Emmett-Teller (BET), X-ray diffraction (XRD), temperature-programmed reduction (TPR), Raman, high-resolution transmission electron microscopy (HRTEM), and extended X-ray absorption fine structure (EXAFS). The aim of the investigation was to understand the behavior of ceria when deposited on alumina and treated under oxidizing and reducing conditions at high temperature (T >/= 1273 K). It is shown that ceria can partially stabilize alumina toward the formation of low-surface-area phases up to 1373 K under oxidizing conditions, while enhanced stabilization is observed under reducing conditions, being effective up to 1473 K. A detailed quantitative temperature-programmed reduction (TPR) analysis made at different loadings and calcination temperatures allowed us to identify three characteristic regions where the reduction of small and large ceria crystallites occurs with the formation of CeAlO(3) crystallites at high temperature. These are likely responsible for surface-area stabilization. For dispersed ceria samples, reduction takes place almost exclusively at low temperature (<700 K), while a shift to higher temperatures is observed upon increasing the ceria particle size. A fraction of Ce, in samples at low loadings, is stable in the lower oxidation state, even if subjected to strongly oxidizing conditions. 相似文献
145.
Farrell D Cheng Y McCallum RW Sachan M Majetich SA 《The journal of physical chemistry. B》2005,109(28):13409-13419
The magnetic properties of monodisperse Fe nanoparticles with over 4 orders of magnitude difference in concentration are studied by a combination of ordinary and remanent hysteresis loops, zero field cooled magnetization as a function of temperature, and magnetic relaxation rates. We compare the behavior of dilute dispersions with different concentrations, dispersions, and arrays made from the same particles, and nanoparticle arrays with different particle sizes and separations. The results are related to theoretical predictions and are used to create a unified picture of magnetostatic interactions within the assemblies. 相似文献
146.
Causo MS Ciccotti G Montemayor D Bonella S Coker DF 《The journal of physical chemistry. B》2005,109(14):6855-6865
We generalize the linearized path integral approach to evaluate quantum time correlation functions for systems best described by a set of nuclear and electronic degrees of freedom, restricting ourselves to the adiabatic approximation. If the operators in the correlation function are nondiagonal in the electronic states, then this adiabatic linearized path integral approximation for the thermal averaged quantum dynamics presents interesting and distinctive features, which we derive and explore in this paper. The capability of these approximations to accurately reproduce the behavior of physical systems is demonstrated by calculating the diffusion constant for an excess electron in a metal-molten salt solution. 相似文献
147.
Basurto S Torroba T Comes M Martínez-Máñez R Sancenón F Villaescusa L Amorós P 《Organic letters》2005,7(24):5469-5472
[structure: see text] A new sensory MCM-41-based material for the colorimetric sensing and discrimination of amines has been developed. 相似文献
148.
Objective: We have shown that High-Intensity Focused Ultrasound (HIFU) can effectively control bleeding from injuries to solid organs such as liver, spleen, and lung. Achievement of hemostasis was augmented when a homogenate of tissue and blood was formed. The objective of this study was to investigate quantitatively the effect of homogenate production on HIFU application time for hemostasis. Possible mechanisms involved in homogenate production were also studied.Methods: Ten anesthetized rabbits had laparotomy and liver exposure. Liver incisions, 15-25 mm long and 3-4 mm deep, were made followed immediately by HIFU application. Two electrical powers of 80 and 100 W corresponding to focal acoustic intensities of 2264 and 2829 W/cm2, respectively were used. Tissue and homogenate temperatures were measured. Smear and histological tissue sample analysis using light microscopy were performed.Results: In treatments with homogenate formation, hemostasis was achieved in 76 ± 1.3 s (Mean ± Standard Error Mean: SEM) at 80 W. In treatments without homogenate formation (at 80 W), hemostasis was achieved in 106 ± 0.87 s. At 100 W, hemostasis was achieved in 46 ± 0.3 s. The time required for homogenate formation, at 80 and 100 W were 60 ± 2.5 and 23 ± 0.3 s, respectively. The homogenate temperature was 83 °C (SEM 0.6 °C), and the non-homogenate tissue temperature at the treatment site was 60 °C (SEM 0.4 °C). The smear and histological analysis showed significant blood components and cellular debris in the homogenate, with some intact cells.Conclusion: The HIFU-induced homogenate of blood and tissue resulted in a statistically significant shorter HIFU application time for hemostasis. The incisions with homogenate had higher temperatures as compared to incisions without homogenate. Further studies of the correlation between homogenate formation and temperature must be done, as well as studies on the long-term effects of homogenate in achieving hemostasis. 相似文献
149.
We study the dynamics of excitable integrate-and-fire neurons in a small-world network. At low densities p of directed random connections, a localized transient stimulus results either in self-sustained persistent activity or in a brief transient followed by failure. Averages over the quenched ensemble reveal that the probability of failure changes from 0 to 1 over a narrow range in p; this failure transition can be described analytically through an extension of an existing mean-field result. Exceedingly long transients emerge at higher densities p; their activity patterns are disordered, in contrast to the mostly periodic persistent patterns observed at low p. The times at which such patterns die out follow a stretched-exponential distribution, which depends sensitively on the propagation velocity of the excitation. 相似文献