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151.
152.
Tyler T. Clikeman Dr. Igor V. Kuvychko Dr. Natalia B. Shustova Dr. Yu‐Sheng Chen Dr. Alexey A. Popov Dr. Olga V. Boltalina Prof. Steven H. Strauss 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(16):5070-5080
The sequential addition of CN? or CH3? and electrophiles to three perfluoroalkylfullerenes (PFAFs), Cs‐C70(CF3)8, C1‐C70(CF3)10, and Cs‐p‐C60(CF3)2, was carried out to determine the most reactive individual fullerene C atoms (as opposed to the most reactive C?C bonds, which has previously been studied). Each PFAF reacted with CH3? or CN? to generate metastable PFAF(CN)? or PFAF(CH3)22? species with high regioselectivity (i.e., one or two predominant isomers). They were treated with electrophiles E+ to generate PFAF(CN)(E) or PFAF(CH3)2(E)2 derivatives, also with high regioselectivity (E+=CN+, CH3+, or H+). All of the predominant products, characterized by mass spectrometry and 19F NMR spectroscopy, are new compounds. Some could be purified by HPLC to give single isomers. Two of them, C70(CF3)8(CN)2 and C70(CF3)10(CH3)2(CN)2, were characterized by single‐crystal X‐ray diffraction. DFT calculations were used to propose whether a particular reaction is under kinetic or thermodynamic control. 相似文献
153.
Dr. Samir Safi Dr. Gaëlle Creff Dr. Aurélie Jeanson Lei Qi Christian Basset Dr. Jérome Roques Dr. Pier Lorenzo Solari Prof. Eric Simoni Dr. Claude Vidaud Prof. Christophe Den Auwer 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(34):11261-11269
Herein, we describe the structural investigation of one possible uranyl binding site inside a nonstructured protein. This approach couples spectroscopy, thermodynamics, and theoretical calculations (DFT) and studies the interaction of uranyl ions with a phosphopeptide, thus mimicking a possible osteopontin (OPN) hydroxyapatite growth‐inhibition site. Although thermodynamical aspects were investigated by using time‐resolved laser fluorescence spectroscopy (TRLFS) and isothermal titration calorimetry (ITC), structural characterization was performed by extended X‐ray absorption fine structure (EXAFS) at the U LIII‐edge combined with attenuated total reflection Fourier transform infrared (ATR‐FTIR) spectroscopy. From the vibrational and fluorescence spectra, several structural models of a UO22+/peptide complex were developed and subsequently refined by using theoretical calculations to fit the experimental EXAFS obtained. The structural effect of the pH value was also considered under acidic to moderately acidic conditions (pH 1.5–5.5). Most importantly, the uranyl/peptide coordination environment was similar to that of the native protein. 相似文献
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156.
A novel approach utilizing automated Raman microspectroscopic mapping for gunshot residue (GSR) detection was investigated. A well-established technique for GSR recovery (tape lifting) was utilized for GSR particle collection. Uncontaminated samples of the substrate (tape), organic GSR (OGSR), and inorganic GSR (IGSR) particles were characterized to generate three respective Raman spectroscopic training sets. Automated Raman mapping was used to rapidly collect spectra over areas of the tape substrate populated with GSR particles. Raman spectra collected from the maps were classified against the training sets via partial least squares discriminant analysis (PLS-DA) to determine if GSR was present. We report the application of Raman chemical mapping as a proof of concept for the positive detection of GSR particles of varying morphologies. The estimated size of GSR particles, which could be readily detected by this method, is about 3.4 μm. The efficiency of the classification was quantitated with rates of true positives and negatives. Validation studies scrutinizing the practicality of this approach as a viable tool for potential forensics investigations are currently in progress. Figure
The figure illustrates a novel approach for the recovery and identification of gunshot residue on adhesive tape. The emerging approach combines tape lifting and a rapid, non-destructive Raman spectroscopic scanning over the tape, which was used for collecting GSR from a surface of interest. Detection of GSR is achieved through multivariate classification of mapping spectra against a known training set. 相似文献
157.
Yury Kostyukevich Alexey Kononikhin Alexander Zherebker Igor Popov Irina Perminova Eugene Nikolaev 《Analytical and bioanalytical chemistry》2014,406(26):6655-6664
We report a simple approach for enumeration of non-labile oxygen atoms in individual molecules of dissolved organic matter (DOM), using acid-catalyzed 16O/18O exchange and ultrahigh-resolution Fourier-transform ion-cyclotron-resonance mass spectrometry (FTICR-MS). We found that by dissolving DOM in H2 18O at 95 °C for 20 days it is possible to replace all oxygen atoms of DOM molecules (excluding oxygen from ether groups) with 18O. The number of exchanges in each molecule can be determined using high-resolution FTICR. Using the proposed method we identified the number of non-labile oxygen atoms in 231 molecules composing DOM. Also, using a previously developed hydrogen–deuterium (H/D)-exchange approach we identified the number of labile hydrogen atoms in 450 individual molecular formulas. In addition, we observed that several backbone hydrogen atoms can be exchanged for deuterium under acidic conditions. The method can be used for structural and chemical characterization of individual DOM molecules, comparing different DOM samples, and investigation of biological pathways of DOM in the environment. 相似文献
158.
Igor Dobovšek 《PAMM》2015,15(1):383-384
We consider a class of non-dissipative materials whose constitutive equations are derived from a suitably constructed thermodynamic potential function. The Gibbs energy relation is introduced as a function of stress, strain, magnetic field, magnetization, and temperature. By minimization with respect to the chosen subset of independent variables we derive the corresponding set of constitutive equations. The chosen form of the free energy function leads to the linear elastic and nonlinear ferromagnetic coupling where non-linearity emerges in terms associated with the strength of magnetization. (© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献
159.
The paper deals with a methodology of shaping the vibro-isolation properties of suspensions applied in automotive systems. The developed optimisation procedure allows to find the Pareto-optimal system configuration for the conflicted vibro-isolating criteria. The correctness of proposed methodology is evaluated using the semi active and active systems with optimal controller settings. (© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献
160.
Igor Vigdorovich 《PAMM》2015,15(1):499-500
A consistent asymptotic theory describing hydrodynamic and thermal turbulent boundary layers on a flat plate in zero pressure gradient is developed. The fact that the flow depends on a limited number of governing parameters allows us to formulate algebraic closure conditions that relate the turbulent shear stress and turbulent heat flux to mean velocity and temperature gradients. As a result of an exact asymptotic solution of the boundary-layer equations, the known laws of the wall for the velocity and temperature and the velocity and temperature defect laws as well as the expressions for the skin-friction coefficient, Stanton number, and Reynolds-analogy factor are obtained. The latter implies two new formulations for the temperature defect law one of which is completely similar to the velocity defect law and does not contain the Stanton number and the turbulent Prandtl number, and the other does not contain the skin-friction coefficient. A heat-transfer law is obtained that relates only thermal quantities. The theoretical conclusions agree well with experimental data. (© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献