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101.
Hughes KJ Griffiths JF Fairweather M Tomlin AS 《Physical chemistry chemical physics : PCCP》2006,8(27):3197-3210
The purpose of this paper is to show the application of global uncertainty analysis to comprehensive and reduced kinetic models as a tool to identify important thermochemical and reaction rate parameters as determinants of the conditions leading to autoignition. Propane oxidation is taken as the test case. The simulation of experimental investigations of the cool flames and two-stage ignitions, via the pressure-temperature ignition diagram, show that existing kinetic models for the low temperature combustion of propane at sub-atmospheric pressures reflect a greater reactivity than seems to be appropriate. That is, the models lead to a prediction of two-stage ignition at pressures somewhat lower and with ignition delays shorter than is found experimentally. The inconsistency between experiment and numerical simulation seems not to be an inherent problem of the qualitative structure of the models, but may derive from uncertainties in the parameters within the mechanism. By use of "brute force", Morris-one-at-a-time and Monte-Carlo simulations, we show that uncertainties in only a small number of parameters, and falling well within the errors that may reasonably be assigned, can shift the response appropriately. Moreover, it appears that in the low temperature combustion regime, thermochemistry is at least as, if not more, important than the reaction rates, yet usually receives less attention within sensitivity studies. In the present case, the main factors controlling the temperature reached in the first stage of two-stage ignition and the time to ignition appear to be connected with the thermochemistry of three specific hydroperoxyalkyl radicals and their derivatives. Other factors, such as heat and mass transport are also addressed, and their effects are mitigated to some extent by evaluation of initial and revised models against experimental data for ignition delay obtained under microgravity. The results highlight more general issues that pertain to the numerical simulation of the combustion of higher hydrocarbons and contribute to the development of the protocol necessary for testing kinetic models before they are ready for use in a predictive capacity. 相似文献
102.
Badger CL Griffiths PT George I Abbatt JP Cox RA 《The journal of physical chemistry. A》2006,110(21):6986-6994
The kinetics of reactive uptake of N2O5 on submicron aerosol particles containing humic acid and ammonium sulfate has been investigated as a function of relative humidity (RH) and aerosol composition using a laminar flow reactor coupled with a differential mobility analyzer (DMA) to characterize the aerosol. For single-component humic acid aerosol the uptake coefficient, gamma, was found to increase from 2 to 9 x 10(-4) over the range 25-75% RH. These values are 1-2 orders of magnitude below those typically observed for single-component sulfate aerosols (Phys. Chem. Chem. Phys. 2003, 5, 3453-3463;(1) Atmos. Environ. 2000, 34, 2131-2159(2)). For the mixed aerosols, gamma was found to decrease with increasing humic acid mass fraction and increase with increasing RH. For aerosols containing only 6% humic acid by dry mass, a decrease in reactivity of more than a factor of 2 was observed compared with the case for single-component ammonium sulfate. The concentration of liquid water in the aerosol droplets was calculated using the aerosol inorganic model (for the ammonium sulfate component) and a new combined FTIR-DMA system (for the humic acid component). Analysis of the uptake coefficients using the water concentration data shows that the change in reactivity cannot be explained by the change in water content alone. We suggest that, due to its surfactant properties, the main effect of the humic acid is to reduce the mass accommodation coefficient for N2O5 at the aerosol particle surface. This has implications for the use of particle hygroscopicity data for predictions of the rate of N2O5 hydrolysis. 相似文献
103.
P.J. Cregg Kieran Murphy Adriele Prina-Mello 《Journal of magnetism and magnetic materials》2010,322(15):2087-2094
The implant assisted magnetic targeted drug delivery system of Avilés, Ebner and Ritter is considered both experimentally (in vitro) and theoretically. The results of a 2D mathematical model are compared with 3D experimental results for a magnetizable wire stent. In this experiment a ferromagnetic, coiled wire stent is implanted to aid collection of particles which consist of single domain magnetic nanoparticles (radius ). In order to model the agglomeration of particles known to occur in this system, the magnetic dipole-dipole and hydrodynamic interactions for multiple particles are included. Simulations based on this mathematical model were performed using open source C++ code. Different initial positions are considered and the system performance is assessed in terms of collection efficiency. The results of this model show closer agreement with the measured in vitro experimental results and with the literature. The implications in nanotechnology and nanomedicine are based on the prediction of the particle efficiency, in conjunction with the magnetizable stent, for targeted drug delivery. 相似文献
104.
We report an experimental study of low-frequency (~10 kHz) self-pulsing of the output intensity in a high-concentration erbium-doped fiber laser. We suggest that the fast intensity fluctuations caused by multimode and polarization instabilities play the role of an external noise source, leading to low-frequency auto-oscillations through a coherence resonance scenario. 相似文献
105.
Current knowledge about the variety and complexity of the processes that allow regulated gene expression in living organisms calls for a new understanding of genes. A 'postgenomic' understanding of genes as entities constituted during genome expression is outlined and illustrated with specific examples that formed part of a survey research instrument developed by two of the authors for an ongoing empirical study of conceptual change in contemporary biology. 相似文献
106.
Martin Griffiths 《International Journal of Mathematical Education in Science & Technology》2013,44(8):1268-1273
In this article, we derive a number of identities involving both Pell numbers and binomial coefficients. We also consider briefly the potential for obtaining Pell identities involving trinomial coefficients and beyond. A key point is the simplicity of the derivations, and indeed this work can lead on to a number of interesting explorations for first-year undergraduates. 相似文献
107.
Ibon Alkorta Mark Z. Griffiths Paul L. A. Popelier 《Journal of Physical Organic Chemistry》2013,26(10):791-796
Linear correlations were established between the calculated bond lengths and the pKa or σI values for a series of 4‐substituted bicyclo[2.2.2]octane‐1‐carboxylic acid and 4‐cubane‐1‐carboxylic acid derivatives. The bond lengths have been calculated at a modest computational level, HF/6‐31G(d), both in the gas phase and with the continuum solvation model, polarisable continuum model (PCM). In general, the best correlations are obtained when the PCM model is taken into account, especially when neutral and charged molecules are considered together. The best models in each case show square correlation coefficients (R2) larger than 0.9 and indicate that they can be used as predictive tools. These results expand previous results that indicate the possibility of a relationship between gas phase bond length and pKa values in aqueous solution and indicate that such relationships are more general than hitherto expected. Copyright © 2013 John Wiley & Sons, Ltd. 相似文献
108.
109.
Jaegler Hugo Pointurier Fabien Onda Yuichi Angulo Jaime F. Griffiths Nina M. Moureau Agnes Faure Anne-Laure Marie Olivier Hubert Amélie Evrard Olivier 《Journal of Radioanalytical and Nuclear Chemistry》2019,322(1):57-66
An aqueous biphasic system has been used for selective extraction of U(VI) ions from Th(IV), Sm(III) and Ce(III). Role of different biomolecules like morin, catechin, hesperidin and 4-hydroxycoumarin have been studied. Morin serves as the best reagent when citrate ions are used as a masking agent. Citrate forms stronger complexes with the other metal ions than morin thereby restricting their extractions. Contrarily, U(VI) forms a stronger complex with morin than citrate and is selectively extracted under the same conditions. It was also observed that morin can act as a spectrophotometric reagent for ratiometric detection and analysis of U(VI) ions.
相似文献110.