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111.
112.
Electron detachment dissociation (EDD) has recently been shown by Amster and coworkers to constitute a valuable analytical approach for structural characterization of glycosaminoglycans. Here, we extend the application of EDD to neutral and sialylated oligosaccharides. Both branched and linear structures are examined, to determine whether branching has an effect on EDD fragmentation behavior. EDD spectra are compared to collisional activated dissociation (CAD) and infrared multiphoton dissociation (IRMPD) spectra of the doubly and singly deprotonated species. Our results demonstrate that EDD of both neutral and sialylated oligosaccharides provides structural information that is complementary to that obtained from both CAD and IRMPD. In all cases, EDD resulted in additional cross-ring cleavages. In most cases, cross-ring fragmentation obtained by EDD is more extensive than that obtained from IRMPD or CAD. Our results also indicate that branching does not affect EDD fragmentation, contrary to what has been observed for electron capture dissociation (ECD). 相似文献
113.
Measurement Instruction in the Context of Scientific Investigations With Diverse Student Populations
Karen Adamson Walter Secada Jaime Maerten‐Rivera Okhee Lee 《School science and mathematics》2011,111(6):288-299
The purpose of this study was to investigate the impact of a hands‐on science curriculum, which integrates mathematics and supports English language development, on third‐grade students' mathematics achievement—specifically the measurement subscale of the statewide assessment. The data drew from a larger five‐year research and development project consisting of reform‐based science curriculum units and teacher workshops designed to promote effective science instruction while integrating mathematics and supporting English language development. The third‐grade curriculum places a strong emphasis on measurement skills in the context of science inquiry. The third‐grade students' performance on the measurement subscale of the statewide mathematics assessment in the treatment schools was compared with that of comparison schools using a hierarchical linear model. Students at the treatment schools performed significantly higher than students at the comparison schools. The results provide evidence that an integrated approach to mathematics and science instruction can benefit diverse student groups. 相似文献
114.
An efficient homogeneous catalytic system for the visible-light-induced production of hydrogen from water utilizing cyclometalated iridium(III) and tris-2,2'-bipyridyl rhodium(III) complexes is described. Synthetic modification of the photosensitizer Ir(C--N) 2(N--N) (+) and water reduction catalyst Rh(N--N) 3 (3+) creates a family of catalysts with diverse photophysical and electrochemical properties. Parallel screening of the various catalyst combinations and photoreaction conditions allows the rapid development of an optimized photocatalytic system that achieves over 5000 turnovers with quantum yields ( (1)/ 2 H 2 per photon absorbed) greater than 34%. Photophysical and electrochemical characterization of the optimized system reveals that the reductive quenching pathway provides the necessary driving force for the formation of [Rh(N--N) 2] (0), the active catalytic species for the reduction of water to produce hydrogen. Tests for system poisoning with mercury or CS 2 provide strong evidence that the system is a true homogeneous system for photocatalytic hydrogen production. 相似文献
115.
Adamson PE Duan XF Burggraf LW Pak MV Swalina C Hammes-Schiffer S 《The journal of physical chemistry. A》2008,112(6):1346-1351
The nuclear-electronic orbital (NEO) method was modified and extended to positron systems for studying mixed positronic-electronic wavefunctions, replacing the mass of the proton with the mass of the positron. Within the modified NEO framework, the NEO-HF (Hartree-Fock) method provides the energy corresponding to the single-configuration mixed positronic-electronic wavefunction, minimized with respect to the molecular orbitals expressed as linear combinations of Gaussian basis functions. The electron-electron and electron-positron correlation can be treated in the NEO framework with second-order perturbation theory (NEO-MP2) or multiconfigurational methods such as the full configuration interaction (NEO-FCI) and complete active space self-consistent-field (NEO-CASSCF) methods. In addition to implementing these methods for positronic systems, strategies for calculating electron-positron annihilation rates using NEO-HF, NEO-MP2, and NEO-FCI wavefunctions were also developed. To apply the NEO method to the positronium hydride (PsH) system, positronic and electronic basis sets were optimized at the NEO-FCI level and used to compute NEO-MP2 and NEO-FCI energies and annihilation rates. The effects of basis set size on NEO-MP2 and NEO-FCI correlation energies and annihilation rates were compared. Even-tempered electronic and positronic basis sets were also optimized for the e+LiH molecule at the NEO-MP2 level and used to compute the equilibrium bond length and vibrational energy. 相似文献
116.
Prof. Dr. José‐Luis M. Abboud Dr. Balázs Németh Prof. Dr. Jean‐Claude Guillemin Prof. Dr. Peeter Burk Aiko Adamson Eva Roos Nerut 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(13):3981-3991
A Fourier transform ion cyclotron resonance spectrometry (FT‐ICR) study of the gas‐phase protonation of ammonia‐borane and sixteen amine/boranes R1R2R3N? BH3 (including six compounds synthesized for the first time) has shown that, without exception, the protonation of amine/boranes leads to the formation of dihydrogen. The structural effects on the experimental energetic thresholds of this reaction were determined experimentally. The most likely intermediate and the observed final species (besides H2) are R1R2R3N? BH4+ and R1R2R3N? BH2+, respectively. Isotopic substitution allowed the reaction mechanism to be ascertained. Computational analyses ([MP2/6‐311+G(d,p)] level) of the thermodynamic stabilities of the R1R2R3N? BH3 adducts, the acidities of the proton sources required for dihydrogen formation, and the structural effects on these processes were performed. It was further found that the family of R1R2R3N? BH4+ ions is characterized by a three‐center, two‐electron bond between B and a loosely bound H2 molecule. Unexpected features of some R1R2R3N? BH4+ ions were found. This information allowed the properties of amine/boranes most suitable for dihydrogen generation and storage to be determined. 相似文献
117.
The objective was to use multiple paths through the slurry to determine the lowest concentration that provided accurate attenuation measurements and to measure the velocity of sound through an effective long path. Ultrasonic attenuation measurements were obtained for slurries of silica (10 microm diameter) in water for concentrations of 0.1%, 0.25%, 0.5%, 0.75% and 1% silica by weight. Attenuation measurements for concentrations less than 0.1% may prove useful for process control to detect contaminants. A long path is obtained due to multiple reflections occurring within the stainless steel (SS) vessel used; broad-band transducers are affixed on the outside of the thick-walled vessel. The signal in the receive transducer permits the measurement of the attenuation and also the velocity by measuring the time-of-flight. The FFT of the appropriate signal for each echo was obtained and compared with that for water to yield the attenuation as a function of frequency. The attenuation measurements are self-calibrating because they are not affected by changes in the pulser voltage. The data show the feasibility for measuring a concentration of 0.025 wt% silica, which is equivalent to 0.25 g of silica in 1 l of water. Therefore, such measurements can prove useful for detecting contaminants in liquid. The velocity of sound measurements for solutions of hydrogen peroxide in water were obtained and accurate to about 0.3m/s, or 0.02% uncertainty. 相似文献
118.
Peep Adamson 《Optics Communications》2012,285(13-14):3210-3216
The possibilities of determining the optical parameters of uniaxially anisotropic non-absorbing ultrathin films on the basis of ellipsometric parameters are analyzed in the framework of a long-wavelength approximation. It is shown that the special convenience of this analytical approach lies in the fact that it enables to find out the situations where it is possible to decouple the optical constants and the thickness (to provide correlation-free measurements) of an anisotropic ultrathin film. The accuracy of the obtained formulas for determining the parameters of ultrathin films is estimated by computer simulation of the reflection problem on the basis of the exact electromagnetic theory for anisotropic layered systems. 相似文献