Mixing in a fluid flowing through a packed bed

Thesis (M.S.)--Massachusetts Institute of Technology, Dept. of Chemical Engineering, 1948.Includes bibliographical references (leaf 68).by P.V. Danckwerts, A.C. Sugden.M.S

Moving walls accelerate mixing

Mixing in viscous fluids is challenging, but chaotic advection in principle allows efficient mixing. In the best possible scenario,the decay rate of the concentration profile of a passive scalar should be exponential in time. In practice, several authors have found that the no-slip boundary condition at the walls of a vessel can slow down mixing considerably, turning an exponential decay into a power law. This slowdown affects the whole mixing region, and not just the vicinity of the wall. The reason is that when the chaotic mixing region extends to the wall, a separatrix connects to it. The approach to the wall along that separatrix is polynomial in time and dominates the long-time decay. However, if the walls are moved or rotated, closed orbits appear, separated from the central mixing region by a hyperbolic fixed point with a homoclinic orbit. The long-time approach to the fixed point is exponential, so an overall exponential decay is recovered, albeit with a thin unmixed region near the wall.Comment: 17 pages, 13 figures. PDFLaTeX with RevTeX 4-1 styl

Rigorous Multicomponent Reactive Separations Modelling : Complete Consideration of Reaction-Diffusion Phenomena

This paper gives the first step of the development of a rigorous multicomponent reactive separation model. Such a model is highly essential to further the optimization of acid gases removal plants (CO2 capture, gas treating, etc.) in terms of size and energy consumption, since chemical solvents are conventionally used.Firstly, two main modelling approaches are presented: the equilibrium-based and the rate-based approaches. Secondly, an extended rate-based model with rigorous modelling methodology for diffusion-reaction phenomena is proposed. The film theory and the generalized Maxwell-Stefan equations are used in order to characterize multicomponent interactions. The complete chain of chemical reactions is taken into account. The reactions can be kinetically controlled or at chemical equilibrium, and they are considered for both liquid film and liquid bulk. Thirdly, the method of numerical resolution is described. Coupling the generalized Maxwell-Stefan equations with chemical equilibrium equations leads to a highly non-linear Differential-Algebraic Equations system known as DAE index 3. The set of equations is discretized with finite-differences as its integration by Gear method is complex. The resulting algebraic system is resolved by the Newton- Raphson method. Finally, the present model and the associated methods of numerical resolution are validated for the example of esterification of methanol. This archetype non-electrolytic system permits an interesting analysis of reaction impact on mass transfer, especially near the phase interface. The numerical resolution of the model by Newton-Raphson method gives good results in terms of calculation time and convergence. The simulations show that the impact of reactions at chemical equilibrium and that of kinetically controlled reactions with high kinetics on mass transfer is relatively similar. Moreover, the Fick’s law is less adapted for multicomponent mixtures where some abnormalities such as counter-diffusion take place

Robust plasmon waveguides in strongly-interacting nanowire arrays

Arrays of parallel metallic nanowires are shown to provide a tunable, robust, and versatile platform for plasmon interconnects, including high-curvature turns with minimum signal loss. The proposed guiding mechanism relies on gap plasmons existing in the region between adjacent nanowires of dimers and multi-wire arrays. We focus on square and circular silver nanowires in silica, for which excellent agreement between both boundary element method and multiple multipolar expansion calculations is obtained. Our work provides the tools for designing plasmon-based interconnects and achieving high degree of integration with minimum cross talk between adjacent plasmon guides.Comment: 4 pages, 5 figure

Quantification of the performance of chaotic micromixers on the basis of finite time Lyapunov exponents

Chaotic micromixers such as the staggered herringbone mixer developed by Stroock et al. allow efficient mixing of fluids even at low Reynolds number by repeated stretching and folding of the fluid interfaces. The ability of the fluid to mix well depends on the rate at which "chaotic advection" occurs in the mixer. An optimization of mixer geometries is a non trivial task which is often performed by time consuming and expensive trial and error experiments. In this paper an algorithm is presented that applies the concept of finite-time Lyapunov exponents to obtain a quantitative measure of the chaotic advection of the flow and hence the performance of micromixers. By performing lattice Boltzmann simulations of the flow inside a mixer geometry, introducing massless and non-interacting tracer particles and following their trajectories the finite time Lyapunov exponents can be calculated. The applicability of the method is demonstrated by a comparison of the improved geometrical structure of the staggered herringbone mixer with available literature data.Comment: 9 pages, 8 figure

Unstationary film model for the determination of absolute gas-liquid kinetic rate constants: ozonation of Acid Red 27, Acid Orange 7, and Acid Blue 129

A method for the determination of absolute kinetic rate constants is proposed using an unstationary film model. This methodology avoids the experimental determination of parameters like the enhancement factor or the Hatta number which are usually model-dependent. The mathematical model is general for gas-liquid systems with irreversible second order reactions. An optimization procedure based on artificial neural networks is used to estimate the initial guess of the parameters and the subsequent application of Gauss-Newton algorithm for the final nonlinear parameter estimation. The model is tested with the ozonation reaction of Acid Red 27, Acid Orange 7 and Acid Blue 129. The second-order kinetic rate constants for the direct reaction with O3 are 1615±93, 609±83, and 49±2M−1s−1, respectivelyJF acknowledges the support of the doctoral fellowship from the Universitat Politecnica de Valencia (UPV-PAID-FPI-2010-04).Ferre Aracil, J.; Cardona Navarrete, SC.; López Pérez, MF.; Abad Sempere, A.; Navarro-Laboulais, J. (2013). Unstationary film model for the determination of absolute gas-liquid kinetic rate constants: ozonation of Acid Red 27, Acid Orange 7, and Acid Blue 129. Ozone: Science and Engineering. 35(6):423-437. https://doi.org/10.1080/01919512.2013.815104S423437356Biń, A. K. (2006). Ozone Solubility in Liquids. Ozone: Science & Engineering, 28(2), 67-75. doi:10.1080/01919510600558635Cardona, S. C., López, F., Abad, A., & Navarro-Laboulais, J. (2010). On bubble column reactor design for the determination of kinetic rate constants in gas-liquid systems. The Canadian Journal of Chemical Engineering, 88(4), 491-502. doi:10.1002/cjce.20327Chang, C. S., & Rochelle, G. T. (1982). Mass transfer enhanced by equilibrium reactions. Industrial & Engineering Chemistry Fundamentals, 21(4), 379-385. doi:10.1021/i100008a011Dachipally, P., & Jonnalagadda, S. B. (2011). Kinetics of ozone-initiated oxidation of textile dye, Amaranth in aqueous systems. Journal of Environmental Science and Health, Part A, 46(8), 887-897. doi:10.1080/10934529.2011.580201Danckwerts, P. V., & Lannus, A. (1970). Gas-Liquid Reactions. Journal of The Electrochemical Society, 117(10), 369C. doi:10.1149/1.2407312Das, A. K., & Das, P. K. (2009). Bubble Evolution through a Submerged Orifice Using Smoothed Particle Hydrodynamics: Effect of Different Thermophysical Properties. Industrial & Engineering Chemistry Research, 48(18), 8726-8735. doi:10.1021/ie900350hFerrell, R. T., & Himmelblau, D. M. (1967). Diffusion coefficients of nitrogen and oxygen in water. Journal of Chemical & Engineering Data, 12(1), 111-115. doi:10.1021/je60032a036Gerlach, D., Alleborn, N., Buwa, V., & Durst, F. (2007). Numerical simulation of periodic bubble formation at a submerged orifice with constant gas flow rate. Chemical Engineering Science, 62(7), 2109-2125. doi:10.1016/j.ces.2006.12.061Glasscock, D. A., & Rochelle, G. T. (1989). Numerical simulation of theories for gas absorption with chemical reaction. AIChE Journal, 35(8), 1271-1281. doi:10.1002/aic.690350806Gomes, A. C., Nunes, J. C., & Simões, R. M. S. (2010). Determination of fast ozone oxidation rate for textile dyes by using a continuous quench-flow system. Journal of Hazardous Materials, 178(1-3), 57-65. doi:10.1016/j.jhazmat.2010.01.043Gupta, P., Al-Dahhan, M. H., Duduković, M. P., & Mills, P. L. (2000). A novel signal filtering methodology for obtaining liquid phase tracer responses from conductivity probes. Flow Measurement and Instrumentation, 11(2), 123-131. doi:10.1016/s0955-5986(99)00025-4Hoigné, J., & Bader, H. (1983). Rate constants of reactions of ozone with organic and inorganic compounds in water—I. Water Research, 17(2), 173-183. doi:10.1016/0043-1354(83)90098-2Jamialahmadi, M., Zehtaban, M. R., Müller-Steinhagen, H., Sarrafi, A., & Smith, J. M. (2001). Study of Bubble Formation Under Constant Flow Conditions. Chemical Engineering Research and Design, 79(5), 523-532. doi:10.1205/02638760152424299Johnson, P. N., & Davis, R. A. (1996). Diffusivity of Ozone in Water. Journal of Chemical & Engineering Data, 41(6), 1485-1487. doi:10.1021/je9602125King, C. J. (1966). Turbulent Liquid Phase Mass Transfer at Free Gas-Liquid Interface. Industrial & Engineering Chemistry Fundamentals, 5(1), 1-8. doi:10.1021/i160017a001Ledakowicz, S., Maciejewska, R., Perkowski, J., & Bin, A. (2001). Ozonation of Reactive Blue 81 in the bubble column. Water Science and Technology, 44(5), 47-52. doi:10.2166/wst.2001.0248Lewis, W. K., & Whitman, W. G. (1924). Principles of Gas Absorption. Industrial & Engineering Chemistry, 16(12), 1215-1220. doi:10.1021/ie50180a002Lopez, A., Benbelkacem, H., Pic, J. ‐S., & Debellefontaine, H. (2004). Oxidation pathways for ozonation of azo dyes in a semi‐batch reactor: A kinetic parameters approach. Environmental Technology, 25(3), 311-321. doi:10.1080/09593330409355465Meldon, J. H., Olawoyin, O. O., & Bonanno, D. (2007). Analysis of Mass Transfer with Reversible Chemical Reaction†. Industrial & Engineering Chemistry Research, 46(19), 6140-6146. doi:10.1021/ie0705397Navarro-Laboulais, J., Cardona, S. C., Torregrosa, J. I., Abad, A., & López, F. (2006). Structural identifiability analysis of the dynamic gas–liquid film model. AIChE Journal, 52(8), 2851-2863. doi:10.1002/aic.10901Navarro-Laboulais, J., Cardona, S. C., Torregrosa, J. I., Abad, A., & López, F. (2008). Practical identifiability analysis in dynamic gas–liquid reactors. Computers & Chemical Engineering, 32(10), 2382-2394. doi:10.1016/j.compchemeng.2007.12.004Rapp, T., & Wiesmann, U. (2007). Ozonation of C.I. Reactive Black 5 and Indigo. Ozone: Science & Engineering, 29(6), 493-502. doi:10.1080/01919510701617959Tanaka, M., Girard, G., Davis, R., Peuto, A., & Bignell, N. (2001). Recommended table for the density of water between 0  C and 40  C based on recent experimental reports. Metrologia, 38(4), 301-309. doi:10.1088/0026-1394/38/4/3Tizaoui, C., & Grima, N. (2011). Kinetics of the ozone oxidation of Reactive Orange 16 azo-dye in aqueous solution. Chemical Engineering Journal, 173(2), 463-473. doi:10.1016/j.cej.2011.08.014Von Gunten, U. (2003). Ozonation of drinking water: Part I. Oxidation kinetics and product formation. Water Research, 37(7), 1443-1467. doi:10.1016/s0043-1354(02)00457-

Anyons in a weakly interacting system

We describe a theoretical proposal for a system whose excitations are anyons with the exchange phase pi/4 and charge -e/2, but, remarkably, can be built by filling a set of single-particle states of essentially noninteracting electrons. The system consists of an artificially structured type-II superconducting film adjacent to a 2D electron gas in the integer quantum Hall regime with unit filling fraction. The proposal rests on the observation that a vacancy in an otherwise periodic vortex lattice in the superconductor creates a bound state in the 2DEG with total charge -e/2. A composite of this fractionally charged hole and the missing flux due to the vacancy behaves as an anyon. The proposed setup allows for manipulation of these anyons and could prove useful in various schemes for fault-tolerant topological quantum computation.Comment: 7 pages with 3 figures. For related work and info visit http://www.physics.ubc.ca/~fran

Atomic-scale confinement of optical fields

In the presence of matter there is no fundamental limit preventing confinement of visible light even down to atomic scales. Achieving such confinement and the corresponding intensity enhancement inevitably requires simultaneous control over atomic-scale details of material structures and over the optical modes that such structures support. By means of self-assembly we have obtained side-by-side aligned gold nanorod dimers with robust atomically-defined gaps reaching below 0.5 nm. The existence of atomically-confined light fields in these gaps is demonstrated by observing extreme Coulomb splitting of corresponding symmetric and anti-symmetric dimer eigenmodes of more than 800 meV in white-light scattering experiments. Our results open new perspectives for atomically-resolved spectroscopic imaging, deeply nonlinear optics, ultra-sensing, cavity optomechanics as well as for the realization of novel quantum-optical devices