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21.
Vasil'ev YV Kotsiris SG Bashkin IO Antonov VE Moravsky AP Drewello T 《The journal of physical chemistry. B》2005,109(24):11875-11879
The high-pressure treatment of C60 in an H2 atmosphere at high temperatures leads to the efficient formation of a covalently bound dimer and some oligomeric species. The resulting hydrogenated C120 is an example of the bulk production of covalently bound derivatized fullerene cores. Matrix-assisted laser desorption/ionization in conjunction with reflectron time-of-flight mass spectrometry has been applied to the product analysis. The dissociation pattern of selected C120H(2x)+ ions (x > 30) indicates the dimeric structure of (C60H(x))2, as opposed to a giant hydrofullerene species possessing a fused C120 core. However, the results also clearly indicate a much stronger bonding (multiple sigma bonding) between the C60H(x) units than present in cycloaddition products. Evidence of a covalently linked dimer was obtained in labeling experiments, on the basis of which any laser-induced gas-phase aggregation of the C60H(x) monomer during the analysis is discounted. 相似文献
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Streletskii AV Ioffe IN Kotsiris SG Barrow MP Drewello T Strauss SH Boltalina OV 《The journal of physical chemistry. A》2005,109(4):714-719
The mechanism of formation of fluorofullerene (FF) negative ions derived from the compounds C(60)F(18), C(60)F(36), and C(60)F(48) was studied by matrix-assisted laser desorption/ionization (MALDI) time-of-flight (ToF) mass spectrometry (MS). A combined experimental/theoretical approach provides compelling evidence of nondissociative, thermodynamically controlled electron transfer from matrix-derived negative ions to the FF analyte as the main secondary-ionization process. Consistent with this thermochemical model, analyte parent molecular ion yield and degree of fragmentation for a particular MALDI experiment was found to depend on the nature of the matrix material (the five matrices investigated were sulfur, trans-2-[3-{4-tert-butylphenyl}-2-methyl-2-propenylidene]malononitrile, 9-nitroanthracene, 2,6-bis((furan-2-yl)methylene)cyclohexanone, and 2,6-bis((thiophen-2-yl)methylene)cyclohexanone). For mixtures of C(60)F(n) compounds with different n values and therefore different electron affinitites, unwanted electron-transfer reactions, which can lead to the suppression of C(60)F(n)(-) ions with low n values, were successfully blocked for the first time by judicious choice of the matrix. Therefore, reliable qualitative MS analysis of FF mixtures with wide ranges of composition is now possible. 相似文献
24.
Sotirios I. Pantos Ekaterini Tiligada 《International journal of quantum chemistry》2013,113(8):1095-1106
Residual dipolar couplings (RDC) of proteins dissolved in anisotropic media promise to speed up the determination of protein structures. We consider the backbone as a robotic mechanism and formulate inverse kinematics problems using RDC restraints from two media. The φ, ψ of each secondary structure element (SSE) are computed from oriented vectors in consecutive peptide planes. We search for the optimum conformation joining the solutions of two independent backbone halves. The matrix transforming the vector Z of a global frame from one SSE into the other determines their orientation. Three distance constraints between two oriented SSE determine their relative position by solving nine polynomial equations. The benefit of this method is that complete and accurate solutions are obtained overcoming the local minima problems of heuristic procedures. The algorithm is implemented on MAPLE using the least number of experimental data; the runtimes take an order of seconds on a common PC. © 2013 Wiley Periodicals, Inc. 相似文献
25.
Kotsiris SG Vasil'ev YV Streletskii AV Han M Mark LP Boltalina OV Chronakis N Orfanopoulos M Hungerbühler H Drewello T 《European journal of mass spectrometry (Chichester, England)》2006,12(6):397-408
A variety of derivatized fullerenes have been studied by matrix-assisted laser desorption/ionization (MALDI) mass spectrometry. Of particular emphasis has been the evaluation of a recently introduced solvent-free sample/target preparation method. Solvent-free MALDI is particularly valuable in overcoming adverse solvent-related effects, such as insolubility and/or degradation of the sample. The method was applied to fullerene derivatives susceptible to decomposition under insufficiently "soft" MALDI conditions. Analytes included the hydrofullerene: C(60)H(36), fluorofullerenes: C(60)F(x) where x = 18, 36, 46, 48 and C(70)F(x) where x = 54, 56, methano-bridged amphiphilic ligand adducts to C(60) and the [4 + 2] cycloadduct of tetracene to C(60). The new solvent-free sample preparation is established as an exceedingly valuable addition to the repertoire of preparation protocols within MALDI. The MALDI mass spectra were of very high quality throughout, providing a testimony that "soft" MALDI conditions could be achieved. Using the [4 + 2] cycloadduct of tetracene to C(60) as the model analyte for direct comparison with solvent-based MALDI, the solvent-free approach led to less fragmentation and more abundant analyte ions. Applying solvent-free sample preparation, different matrix compounds have been examined for use in the MALDI of derivatized fullerenes, including sulfur, tetracyanoquinodimethane (TCNQ), 9-nitroanthracene (9-NA) and trans-2-[3-(4-tert-butylphenyl)-2-methyl-2- propenylidene]malononitrile (DCTB). DCTB was confirmed as the best performing matrix, reducing unwanted decomposition and suppression effects. 相似文献
26.
Johan F. T. van Lieshout Odette N. Pérez Gutiérrez Wietse Vroom Antoni Planas Willem M. de Vos John van der Oost Sotirios Koutsopoulos 《Applied biochemistry and biotechnology》2012,167(7):2039-2053
An intein-driven protein splicing approach allowed for the covalent linkage between the N- and C-termini of a polypeptide chain to create circular variants of the endo-??-1,3-1,4-glucanase, LicA, from Bacillus licheniformis. Two circular variants, LicA-C1 and LicA-C2, which have connecting loops of 20 and 14 amino acids, respectively, showed catalytic activities that are approximately two and three times higher, respectively, compared to that of the linear LicA (LicA-L1). The thermal stability of the circular variants was significantly increased compared to the linear form. Whereas the linear glucanase lost half of its activity after 3?min at 65?°C, the two circular variants have 6-fold (LicA-C1) and 16-fold (LicA-C2) increased half-life time of inactivation. In agreement with this, fluorescence spectroscopy and differential scanning calorimetry studies revealed that circular enzymes undergo structural changes at higher temperatures compared to that of the linear form. The effect of calcium on the conformational stability and function of the circular LicAs was also investigated, and we observed that the presence of calcium ions results in increased thermal stability. The impact of the length of the designed loops on thermal stability of the circular proteins is discussed, and it is suggested that cyclization may be an efficient strategy for the increased stability of proteins. 相似文献
27.
Swati Agrawal Snigdha Banerjee Sotirios Papachristos 《Applied Mathematical Modelling》2013,37(20-21):8912-8929
In this paper, we consider a two warehouse inventory model, an owned one (OW) and a rented one (RW). Inventory deteriorates in the two warehouses at different constant rates, demand rate is a general ramp-type function of time and shortages are partially backlogged at a constant rate. Existence and uniqueness of the optimal solution is discussed. An algorithm is developed to obtain the overall optimal replenishment policy, which would enable the manager to decide upon the feasibility of renting a warehouse. The dynamics of the model and application of the algorithm are demonstrated through numerical examples. Sensitivity analysis is conducted with respect to model parameters and some important observations are drawn. 相似文献
28.
P. Poulopoulos S. Baskoutas L.F. Kiss L. Bujdosó T. Kemény F. Wilhelm A. Rogalev V. Kapaklis C. Politis M. Angelakeris K. Saksl 《Journal of Non》2008,354(2-9):587-591
The new Fe71.2B24Y4.8 glassy alloy has been prepared in amorphous ribbon form via melt spinning and splat cooling. The high degree of sample homogeneity and structural quality of the ribbon is revealed by the observation of narrow linewidths in the spectra of the field derivatives of the absorbed microwave power in ferromagnetic resonance experiments. Combination of vibrating sample magnetometry and element-specific X-ray magnetic circular dichroism experiments at the L3,2-edges of Y revealed an induced magnetic moment of 0.065 μB/atom for Y antiparallel oriented to an Fe magnetic moment of 1.83 μB/atom. 相似文献
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30.
Consider a (nonnegative) measure with support in the interval such that the respective orthogonal polynomials, above a specific index , satisfy a three-term recurrence relation with constant coefficients. We show that the corresponding Stieltjes polynomials, above the index , have a very simple and useful representation in terms of the orthogonal polynomials. As a result of this, the Gauss-Kronrod quadrature formulae for have all the desirable properties, namely, the interlacing of nodes, their inclusion in the closed interval (under an additional assumption on ), and the positivity of all weights. Furthermore, the interpolatory quadrature formulae based on the zeros of the Stieltjes polynomials have positive weights, and both of these quadrature formulae have elevated degrees of exactness.