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91.
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Dr. Carmine D'Agostino Dr. Tatyana Kotionova Dr. Jonathan Mitchell Dr. Peter J. Miedziak Prof. David W. Knight Dr. Stuart H. Taylor Prof. Graham J. Hutchings Prof. Lynn F. Gladden Dr. Mick D. Mantle 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(35):11725-11732
In recent work, it was reported that changes in solvent composition, precisely the addition of water, significantly inhibits the catalytic activity of Au/TiO2 catalyst in the aerobic oxidation of 1,4‐butanediol in methanol due to changes in diffusion and adsorption properties of the reactant. In order to understand whether the inhibition mechanism of water on diol oxidation in methanol is generally valid, the solvent effect on the aerobic catalytic oxidation of 1,3‐propanediol and its two methyl‐substituted homologues, 2‐methyl‐1,3‐propanediol and 2,2‐dimethyl‐1,3‐propanediol, over a Au/TiO2 catalyst has been studied here using conventional catalytic reaction monitoring in combination with pulsed‐field gradient nuclear magnetic resonance (PFG‐NMR) diffusion and NMR relaxation time measurements. Diol conversion is significantly lower when water is present in the initial diol/methanol mixture. A reactivity trend within the group of diols was also observed. Combined NMR diffusion and relaxation time measurements suggest that molecular diffusion and, in particular, the relative strength of diol adsorption, are important factors in determining the conversion. These results highlight NMR diffusion and relaxation techniques as novel, non‐invasive characterisation tools for catalytic materials, which complement conventional reaction data. 相似文献
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95.
Oxidative Addition of Haloheteroarenes to Palladium(0): Concerted versus SNAr‐Type Mechanism 下载免费PDF全文
Prof. Bert U. W. Maes Dr. Stefan Verbeeck Dr. Tom Verhelst Audrey Ekomié Niklas von Wolff Dr. Guillaume Lefèvre Dr. Emily A. Mitchell Prof. Anny Jutand 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(21):7858-7865
The kinetics of the oxidative additions of haloheteroarenes HetX (X=I, Br, Cl) to [Pd0(PPh3)2] (generated from [Pd0(PPh3)4]) have been investigated in THF and DMF and the rate constants have been determined. In contrast to the generally accepted concerted mechanism, Hammett plots obtained for substituted 2‐halopyridines and solvent effects reveal a reaction mechanism dependent on the halide X of HetX: an unprecedented SNAr‐type mechanism for X=Br or Cl and a classical concerted mechanism for X=I. These results are supported by DFT studies. 相似文献
96.
Journal of Nonlinear Science - We compare one-dimensional representations for the isotopy stable dynamics of homeomorphisms in two dimensions. We consider the skeleton graph representative, which... 相似文献
97.
S.L. Mitchell 《Applied Mathematical Modelling》2012,36(1):127-138
In this paper the combined integral method is applied to a simple one-dimensional ablation problem. One of the drawbacks of heat balance integral methods is how to choose the approximating function. It is common to use a polynomial form but even then it is not clear what the power of the highest order term should be. Previous studies have determined exponents either from exact solutions or from expansions valid over short time scales; neither approach is satisfactory nor very accurate for larger times. We combine the heat balance and refined integral methods to determine this exponent as part of the solution process, and conclude that it is in fact time-dependent in the ablation stage. From comparing the approximate solutions with numerical and exact analytical solutions whenever possible, we show that this new method greatly improves the accuracy on standard methods, without overcomplicating the method. 相似文献
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Abstract The family Anacardiaceae consists of 76 genera and about 600 species. A comparison of the species of Anacardiaceae is discussed with special emphasis on the importance of the exudates, the so-called sap, for their importance as lacquer to produce lacquer ware. Many exudates are poisonous. The individual chemical compounds which constitute the active ingredients of the oleoresin part of the sap and their function are described based on space-filling molecular models. Emphasis is also given to the organic components of lacquer trees of the South East Asian region, which is compared to other species of the Anacardiaceae family. 相似文献
100.
Robert G. Gilbert Alex C. Wu Mitchell A. Sullivan Gonzalo E. Sumarriva Natascha Ersch Jovin Hasjim 《Analytical and bioanalytical chemistry》2013,405(28):8969-8980
Two highly branched glucose polymers with similar structures—starch and glycogen—have important relations to human health. Slowly digestible and resistant starches have desirable health benefits, including the prevention and alleviation of metabolic diseases and prevention of colon cancer. Glycogen is important in regulating the use of glucose in the body, and diabetic subjects have an anomaly in their glycogen structure compared with that in healthy subjects. This paper reviews the biosynthesis–structure–property relations of these polymers, showing that polymer characterization produces knowledge which can be useful in producing healthier foods and new drug targets aimed at improving glucose storage in diabetic patients. Examples include mathematical modeling to design starch with better nutritional values, the effects of amylose fine structures on starch digestibility, the structure of slowly digested starch collected from in vitro and in vivo digestion, and the mechanism of the formation of glycogen α particles from β particles in healthy subjects. A new method to overcome a current problem in the structural characterization of these polymers using field-flow fractionation is also given, through a technique to calibrate evaporative light scattering detection with starch. Figure
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