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51.
D Kruk A Korpała J Kowalewski EA Rössler J Moscicki 《The Journal of chemical physics》2012,137(4):044512
(1)H relaxation dispersion of decalin and glycerol solutions of nitroxide radicals, 4-oxo-TEMPO-d(16)-(15)N and 4-oxo-TEMPO-d(16)-(14)N was measured in the frequency range of 10 kHz-20 MHz (for (1)H) using STELAR Field Cycling spectrometer. The purpose of the studies is to reveal how the spin dynamics of the free electron of the nitroxide radical affects the proton spin relaxation of the solvent molecules, depending on dynamical properties of the solvent. Combining the results for both solvents, the range of translational diffusion coefficients, 10(-9)-10(-11) m(2)∕s, was covered (these values refer to the relative diffusion of the solvent and solute molecules). The data were analyzed in terms of relaxation formulas including the isotropic part of the electron spin - nitrogen spin hyperfine coupling (for the case of (14)N and (15)N) and therefore valid for an arbitrary magnetic field. The influence of the hyperfine coupling on (1)H relaxation of solvent molecules depending on frequency and time-scale of the translational dynamics was discussed in detail. Special attention was given to the effect of isotope substitution ((14)N∕(15)N). In parallel, the influence of rotational dynamics on the inter-molecular (radical - solvent) electron spin - proton spin dipole-dipole coupling (which is the relaxation mechanism of solvent protons) was investigated. The rotational dynamics is of importance as the interacting spins are not placed in the molecular centers. It was demonstrated that the role of the isotropic hyperfine coupling increases for slower dynamics, but it is of importance already in the fast motion range (10(-9)m(2)∕s). The isotope effects is small, however clearly visible; the (1)H relaxation rate for the case of (15)N is larger (in the range of lower frequencies) than for (14)N. It was shown that when the diffusion coefficient decreases below 5 × 10(-11) m(2)∕s electron spin relaxation becomes of importance and its role becomes progressively more significant when the dynamics slows done. As far as the influence of the rotational dynamics is concerned, it was show that this process is of importance not only in the range of higher frequencies (like for diamagnetic solutions) but also at low and intermediate frequencies. 相似文献
52.
Coastal erosion, accelerated by sea level rise, and subsidence are major Louisiana issues. With current sea-level-rise projections, coupled with the state's eroding barrier islands and coastal wetlands, the region's estuarine environments are in jeopardy of being lost, redefined, or permanently altered. As the coast erodes, Louisiana is endangered of losing valuable wetland's habitat. In addition, if the barrier islands disappear, the region's wetland-oriented oil and gas wells and associated infrastructure will be at risk to open Gulf conditions. If this should occur, each well, pipeline, and storage battery represents a potential environmental catastrophe. 相似文献
53.
CHEN Hong-jie LI Sheng LI Zhi-wei WU Zhi-shen ZHANG Ping-yu ZHANG Zhi-jun 《高等学校化学研究》2005,21(6):646-649
IntroductionMetal or alloy nanoparticles,because of their con-spicuous physicochemical properties,have been widelyapplied to various fields such as electronics,catalysis,magnetism,and corrosion-resistant materialsfields[1—4].It has been estimated that the particle sizeand the properties of nanoparticles depend strongly onthe specific method of fabrication and the applied ex-periment conditions,which makes the controlled syn-thesis of nanomaterials become an increasingly activeand important ar… 相似文献
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Chaotic modes of nonlinear deformation of thin cylindrical shells partially filled with a fluid are studied 相似文献
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A method is proposed for the calculation of free oscillations of circular cylindrical shells taking into account the non-linear interaction of their bending deformations. Cases are studied in which a shell is characterized by eigenfrequencies, which are in close proximity or multiple frequencies. Based on analysis of the averaged equations, a number of solutions have been constructed. These solutions are used to investigate the particular qualities of the energy exchange and interaction of the modes of the shell. Phase patterns corresponding to interaction of conjugate forms (2-D model) and forms of various wave-forming parameters (4-D model) are studied. The impact of initial conditions on deformation shapes of free multi-mode-oscillating shells is considered. 相似文献
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Queueing Systems - We provide two examples of strictly subcritical multiclass queueing networks which are unstable under the shortest remaining processing time (SRPT) service protocol. Both of them... 相似文献
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Matos JR Kruk M Mercuri LP Jaroniec M Zhao L Kamiyama T Terasaki O Pinnavaia TJ Liu Y 《Journal of the American Chemical Society》2003,125(3):821-829
FDU-1 silicas with large cage-like pores (diameter about 10 nm) were synthesized under acidic conditions from tetraethyl orthosilicate in the presence of a poly(ethylene oxide)-poly(butylene oxide)-poly(ethylene oxide) triblock copolymer template B50-6600 (EO(39)BO(47)EO(39)). High-resolution transmission electron microscopy and small-angle X-ray scattering provided strong evidence that FDU-1 silica synthesized under typical conditions is a face-centered cubic Fm3m structure with 3-dimensional hexagonal intergrowth and is not a body-centered cubic Im3m structure, as originally reported. Samples synthesized in a wide range of conditions (initial temperatures from 298 to 353 K; hydrothermal treatment at 333-393 K) exhibited similar XRD patterns and their nitrogen adsorption isotherms indicated a good-quality cage-like pore structure. The examination of low-pressure nitrogen adsorption isotherms for FDU-1 samples, whose pore entrance diameters were evaluated using an independent method, allowed us to conclude that low-pressure adsorption was appreciably stronger for samples with smaller pore entrance sizes. This prompted us to examine low-pressure adsorption isotherms for a wide range of samples and led us to a conclusion that the FDU-1 pore entrance size can be systematically enlarged from about 1.3 nm (perhaps even lower) to at least 2.4 nm without an appreciable loss of uniformity by increasing the temperature of the hydrothermal treatment or the initial synthesis. Further enlargement of pore entrance size was achieved for sufficiently long hydrothermal treatment times at temperatures of 373 K or higher, as seen from the shape of nitrogen desorption isotherms. This allowed us to obtain samples with uniform pore sizes, high adsorption capacity, and with pore entrances enlarged so much that their size was similar to the size of the pore itself, resulting in a highly open porous structure. However, in the latter case, there was evidence that the pore entrance size distribution was quite broad. 相似文献