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31.
Karen J. Ardila‐Fierro Stipe Lukin Martin Etter Krunoslav Uarevi Ivan Halasz Carsten Bolm Jos G. Hernndez 《Angewandte Chemie (International ed. in English)》2020,59(32):13458-13462
Recent progress in the field of mechanochemistry has expanded the discovery of mechanically induced chemical transformations to several areas of science. However, a general fundamental understanding of how mechanochemical reactions by ball milling occur has remained unreached. For this, we have now implemented in situ monitoring of a mechanochemically induced molecular rearrangement by synchrotron X‐ray powder diffraction, Raman spectroscopy, and real‐time temperature sensing. The results of this study demonstrate that molecular rearrangements can be accomplished in the solid state by ball milling and how in situ monitoring techniques enable the visualization of changes occurring at the exact instant of a molecular migration. The mechanochemical benzil–benzilic acid rearrangement is the focal point of the study. 相似文献
32.
Bidyut B. Sarma Jonglack Kim Jonas Amsler Giovanni Agostini Claudia Weidenthaler Norbert Pfnder Raul Arenal Patricia Concepcin Philipp Plessow Felix Studt Gonzalo Prieto 《Angewandte Chemie (International ed. in English)》2020,59(14):5806-5815
Realizing the full potential of oxide‐supported single‐atom metal catalysts (SACs) is key to successfully bridge the gap between the fields of homogeneous and heterogeneous catalysis. Here we show that the one‐pot combination of Ru1/CeO2 and Rh1/CeO2 SACs enables a highly selective olefin isomerization‐hydrosilylation tandem process, hitherto restricted to molecular catalysts in solution. Individually, monoatomic Ru and Rh sites show a remarkable reaction specificity for olefin double‐bond migration and anti‐Markovnikov α‐olefin hydrosilylation, respectively. First‐principles DFT calculations ascribe such selectivity to differences in the binding strength of the olefin substrate to the monoatomic metal centers. The single‐pot cooperation of the two SACs allows the production of terminal organosilane compounds with high regio‐selectivity (>95 %) even from industrially‐relevant complex mixtures of terminal and internal olefins, alongside a straightforward catalyst recycling and reuse. These results demonstrate the significance of oxide‐supported single‐atom metal catalysts in tandem catalytic reactions, which are central for the intensification of chemical processes. 相似文献
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L. Raul W. Abramo 《International Journal of Theoretical Physics》2004,43(3):563-573
We investigate tachyon dynamics with an inverse power-law potential V ()
–. We find global attractors of the dynamics leading to a dust behavior for > 2 and to an accellerating universe for 0 < 2. We study linear cosmological perturbations and we show that metric fluctuations are constant on large scales in both cases. In the presence of an additional perfect fluid, the tachyon with this potential behaves as dust or dark energy. 相似文献
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Uncertainty evaluation of the spectral UV irradiance evaluated by using the UVSPEC radiative transfer model 总被引:1,自引:0,他引:1
The radiative transfer models allow calculating the spectral UV irradiance from some set of measured input quantities linked with the surface reflectivity, the solar zenith angle, the ozone column and the characteristics of clouds and aerosols. The spectral irradiance yielded by a model is influenced by errors in the measurement of the input quantities. In this paper, the influences of these errors are characterized and compared with other systematic effects through an uncertainty analysis. We evaluated the uncertainty of the spectral UV irradiance rendered by the UVSPEC model, under cloudless sky conditions. In order to express the uncertainty of the output quantities (the global, direct and diffuse irradiances) in terms of the standard uncertainties of the input quantities, we used a Monte Carlo-based uncertainty propagation technique. We found that the uncertainty of the irradiance in the UV-B part of the spectrum was strongly influenced by the uncertainty attributed to the ozone column datum. Moreover, the uncertainities associated with the aerosol parameters accounted for most of the UV-A global irradiance uncertainty; the latter increased from about 4% under low aerosol conditions, up to about 14% in case of polluted air. We conclude that the UV irradiance evaluation through radiative transfer models requires paying special attention to the assessment of the aerosols properties. 相似文献
38.
Churruca F SanMartin R Carril M Urtiaga MK Solans X Tellitu I Domínguez E 《The Journal of organic chemistry》2005,70(8):3178-3187
Novel dibenzo[a,c]phenanthridines are prepared regioselectively by the application of a straightforward synthetic pathway, starting from new 3,4-diaryl- and 3,4-dihydro-3,4-diarylisoquinolines prepared via Ritter-type heterocyclization and the more classical two-step reductive amination/Bischler-Napieralski cyclization of triarylethanones, respectively. A comparative study of nonphenolic oxidative coupling methodologies provides a highly efficient procedure, based on the hypervalent iodine reagent phenyliodine(III) bis(trifluoroacetate) (PIFA), to accomplish the final coupling step. 相似文献
39.
Set-Valued and Variational Analysis - For solving monotone inclusion problems, we propose an inertial under-relaxed version of the relative-error hybrid proximal extragradient method. We study the... 相似文献
40.
The time evolution of silica nanoparticles in solutions of tetrapropylammonium (TPA) has been studied using a combination of small-angle scattering, conductivity, and pH measurements to provide the first comprehensive analysis of nanoparticle structural and compositional changes at elevated temperatures. We have found that silica-TPA nanoparticles subjected to hydrothermal treatment (70-90 degrees C) grow via an Ostwald ripening mechanism with growth rates that depend on both pH and temperature. Small-angle X-ray (SAXS) and neutron (SANS) scattering confirm that the core-shell structure of the particles, initially present at room temperature, is maintained during heating, but an evolution toward sphericity is evidenced especially at high values of pH. SAXS absolute intensity calculations were utilized to calculate the changes in nanoparticle composition and concentration over time. These changes along with the conductivity and pH measurements and SANS contrast matching studies indicate that, upon heating, TPA becomes embedded in the core of nanoparticles giving rise to more zeolitic-looking nanomaterials. 相似文献