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21.
The dissociation kinetics of proton-bound dimers of betaine with molecules of comparable gas-phase basicity were investigated using blackbody infrared radiative dissociation (BIRD). Threshold dissociation energies were obtained from these data using master equation modeling. For bases that have comparable or higher gas-phase basicity, the binding energy of the protonated base.betaine complex is ~1.4 eV. For molecules that are ~2 kcal/mol or more less basic, the dissociation energy of the complexes is ~1.2 eV. The higher binding energy of the former is attributed to an ion-zwitterion structure which has a much larger ion-dipole interaction. The lower binding energy for molecules that are ~2 kcal/mol or more less basic indicates that an ion-molecule structure is more favored. Semiempirical calculations at both the AM1 and PM3 levels indicate the most stable ion-molecule structure is one in which the base interacts with the charged quaternary ammonium end of betaine. These results indicate that the measurement of binding energies of neutral molecules to biological ions could provide a useful probe for the presence of zwitterions and salt bridges in the gas phase. From the BIRD data, the gas-phase basicity of betaine obtained from the kinetic method is found to be 239.2 +/- 1.0 kcal/mol. This value is in excellent agreement with the value of 239.3 kcal/mol (298 K) from ab initio calculations at the MP2/6-31+g** level. The measured value is slightly higher than those reported previously. This difference is attributed to entropy effects. The lower ion internal energy and longer time frame of BIRD experiments should provide values closer to those at standard temperature. 相似文献
22.
Price PJ 《Physical review. B, Condensed matter》1992,45(16):9042-9045
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B. M. K. Nefkens S. D. Adrian D. B. Barlow P. DiBernardo A. D. Eichon R. S. Kessler J. N. Labrenz C. Pillai J. W. Price J. A. Wightman W. J. Briscoe L. H. Kramer M. F. Taragin D. F. Ottewell 《Few-Body Systems》1992,12(2-4):133-140
First results on –
d are reported. The measurements were made using 8 specially designed neutron counters, which were carefully calibratedin situ. The differential cross sections atT
=142, 180, 217, and 254 MeV were obtained at four angles between 0° and 90°, they are compared to +
d pp data measured at the same energies and angles with the same setup. At every beam energy, the shape of the angular distributions of –
d nn and +
d pp is the same to ±2%. The absolute cross sections differ by 1 to 10%. The error in this comparison is ±4% implying a small violation of charge symmetry.Dedicated to Prof. I. laus on the occasion of his 60th birthdayDeceased 相似文献
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Becker-Szendy R Bratton CB Cady R Casper D Dye ST Gajewski W Goldhaber M Haines TJ Halverson PG Jones TW Kielczewska D Kropp WR Learned JG LoSecco JM Matsuno S McGrew C Mudan MS Price L Reines F Schultz J Sobel HW Stone JL Sulak LR Svoboda R Wittel F 《Physical review D: Particles and fields》1991,43(4):1413-1415
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Fission-track and K-Ar dating of basaltic glass from the Mid-Atlantic Ridge gives results which are consistent with the proposal of ocean-floor spreading. Correlation exists between the magnetic anomaly patterns over the Crest Mountains at 45°N and the age of the outcropping basalts. The observed sequences of ages progressing outward from the Median Valley 11,000, 230,000, 310,000, 750.000, 8,000,000, and 16,000,000 years constitute strong, direct support for the idea of ocean-bottom spreading. 相似文献
28.
Yankeelov TE Lepage M Chakravarthy A Broome EE Niermann KJ Kelley MC Meszoely I Mayer IA Herman CR McManus K Price RR Gore JC 《Magnetic resonance imaging》2007,25(1):1-13
PURPOSE: The objective of this study was to assess changes in the water apparent diffusion coefficient (ADC) and in pharmacokinetic parameters obtained from the fast-exchange regime (FXR) modeling of dynamic contrast-enhanced magnetic resonance imaging (DCE-MRI) during neoadjuvant chemotherapy in breast cancer. MATERIALS AND METHODS: Eleven patients with locally advanced breast cancer underwent MRI examination prior to and after chemotherapy but prior to surgery. A 1.5-T scanner was used to obtain T1, ADC and DCE-MRI data. DCE-MRI data were analyzed by the FXR model returning estimates of K(trans) (volume transfer constant), v(e) (extravascular extracellular volume fraction) and tau(i) (average intracellular water lifetime). Histogram and correlation analyses assessed parameter changes post-treatment. RESULTS: Significant (P < .05) changes or trends towards significance (P < .10) were seen in all parameters except tau(i), although there was qualitative reduction in tau(i) values post-treatment. In particular, there was reduction (P < .035) in voxels with K(trans) values in the range 0.2-0.5 min(-1) and a decrease (P < .05) in voxels with ADC values in the range 0.99 x 10(-3) to 1.35 x 10(-3) mm2/s. ADC and v(e) were negatively correlated (r = -.60, P < .02). Parameters sensitive to water distribution and geometry (T(1), v(e), tau(i) and ADC) correlated with a multivariable linear regression model. CONCLUSION: The analysis presented here is sensitive to longitudinal changes in breast tumor status; K(trans) and ADC are most sensitive to these changes. Relationships between parameters provide information on water distribution and geometry in the tumor environment. 相似文献
29.
Perturbation of Spin Crossover Behavior by Covalent Post‐Synthetic Modification of a Porous Metal–Organic Framework 下载免费PDF全文
John E. Clements Dr. Jason R. Price Dr. Suzanne M. Neville Prof. Cameron J. Kepert 《Angewandte Chemie (International ed. in English)》2014,53(38):10164-10168
Covalent post‐synthetic modification is a versatile method for gaining high‐level synthetic control over functionality within porous metal–organic frameworks and for generating new materials not accessible through one‐step framework syntheses. Here we apply this topotactic synthetic approach to a porous spin crossover framework and show through detailed comparison of the structures and properties of the as‐synthesised and covalently modified phases that the modification reaction proceeds quantitatively by a thermally activated single‐crystal‐to‐single‐crystal transformation to yield a material with lowered spin‐switching temperature, decreased lattice cooperativity, and altered color. Structure–function relationships to emerge from this comparison show that the approach provides a new route for tuning spin crossover through control over both outer‐sphere and steric interactions. 相似文献
30.
An investigation is being undertaken into the influence of flame retardant type on the pyrolytic degradation of cotton (cellulose) fabrics in air over the temperature range 300–100°C. Thermal analysis techniques (TGA and DSC), detailed evolved gas analysis and extent of char formation measurements have all been utilised. The information obtained is used to develop a detailed model for the pyrolytic degradation of cellulose in air and the influence of flame retardants thereon. This paper reports the use of differential scanning calorimetry to further investigate the proposed CELLULOSE → CELLULOSE* transition. 相似文献