The role of geometrical micro-barriers on the conversion efficiency of reactive flows in narrow three-dimensional channels of millimetric size is investigated. Using a Lattice-Boltzmann-Lax-Wendroff code, we show that micro-barriers have an appreciable effect on the effective reaction efficiency of the device. If extrapolated to macroscopic scales, these effects can result in a sizeable increase of the overall reaction efficiency.
We investigate the effects of geometrical micro-irregularities on the conversion efficiency of reactive flows in narrow channels of millimetric size. Three-dimensional simulations, based upon a Lattice-Boltzmann-Lax-Wendroff code, indicate that periodic micro-barriers may have an appreciable effect on the effective reaction efficiency of the device. Once extrapolated to macroscopic scales, these effects can result in a sizeable increase of the overall reaction efficiency.
Finite-difference Lattice Boltzmann (LB) models are proposed for simulating gas flows in devices with microscale geometries. The models employ the roots of half-range Gauss-Hermite polynomials as discrete velocities. Unlike the standard LB velocity-space discretizations based on the roots of full-range Hermite polynomials, using the nodes of a quadrature defined in the half-space permits a consistent treatment of kinetic boundary conditions. The possibilities of the proposed LB models are illustrated by studying the one-dimensional Couette flow and the two-dimensional driven cavity flow. Numer…
A non-perturbative analysis of the Bhatnagar-Gross-Krook (BGK) model kinetic equation for finite values of the Knudsen number is presented. This analysis indicates why discrete kinetic versions of the BGK equation, and notably the Lattice Boltzmann method, can provide semi-quantitative results also in the non-hydrodynamic, finite-Knudsen regime, up to $Kn\sim {\cal O}(1)$. This may help the interpretation of recent Lattice Boltzmann simulations of microflows, which show satisfactory agreement with continuum kinetic theory in the moderate-Knudsen regime.
A new lattice Boltzmann model (LBM) for chemically reactive mixtures is presented. The approach capitalizes on the recently introduced thermodynamically consistent LBM for multicomponent mixtures of ideal gases. Similar to the non-reactive case, the present LBM features Stefan--Maxwell diffusion of chemical species and a fully on-lattice mean-field realization of the momentum and energy of the flow. Besides introducing the reaction mechanism into the kinetic equations for the species, the proposed LBM also features a new realization of the compressible flow by using a concept of extended equil…
A new lattice Boltzmann model for reactive ideal gas mixtures is presented. The model is an extension to reactive flows of the recently proposed multi-component lattice Boltzmann model for compressible ideal gas mixtures with Stefan-Maxwell diffusion for species interaction. First, the kinetic model for the Stefan--Maxwell diffusion is enhanced to accommodate a source term accounting the change of the mixture composition due to chemical reaction. Second, by including the heat of formation in the energy equation, the thermodynamic consistency of the underlying compressible lattice Boltzmann mod…
We propose a multi-component discrete Boltzmann model (DBM) for premixed, nonpremixed, or partially premixed nonequilibrium reactive flows. This model is suitable for both subsonic and supersonic flows with or without chemical reaction and/or external force. A two-dimensional sixteen-velocity model is constructed for the DBM. In the hydrodynamic limit, the DBM recovers the modified Navier-Stokes equations for reacting species in a force field. Compared to standard lattice Boltzmann models, the DBM presents not only more accurate hydrodynamic quantities, but also detailed nonequilibrium effects…
High-resolution porous structures of catalyst layer (CL) with multicomponent in proton exchange membrane fuel cells are reconstructed using a reconstruction method called quartet structure generation set. Characterization analyses of nanoscale structures are implemented including pore size distribution, specific area and phase connectivity. Pore-scale simulation methods based on the lattice Boltzmann method are developed and used to predict the macroscopic transport properties including effective diffusivity and proton conductivity. Nonuniform distributions of ionomer in CL generates more tort…
The Lattice Boltzmann method has been gaining acceptance for hydrodynamic problems involving complex boundaries, non-equilibrium dynamics and interfacial phenomena in multiphase or multicomponent systems. lb2d.pm is a Perl module offering a clear framework for simple Lattice Boltzmann simulations in 2D. The syntax and some basic applications are presented. Mainly, the new version 0.1 enables solute transport and accounts for reactive boundaries leading to surface growth.
Many catalyst devices employ flow through porous structures, which leads to a complex macroscopic mass and heat transport. To unravel the detailed dynamics of the reactive gas flow, we present an all-encompassing model, consisting of thermal lattice Boltzmann model by Kang et al., used to solve the heat and mass transport in the gas domain, coupled to a finite differences solver for the heat equation in the solid via thermal reactive boundary conditions for a consistent treatment of the reaction enthalpy. The chemical surface reactions are incorporated in a flexible fashion through flux bounda…
The Washburn law has always played a critical role for ceramics. In the microscale, surface forces take over volume forces and the phenomenon of spontaneous infiltration in narrow interstices becomes of particular relevance. The Lattice Boltzmann method is applied in order to ascertain the role of surface reaction and subsequent deformation of a single capillary in 2D for the linear Washburn behavior. The proposed investigation is motivated by the problem of reactive infiltration of molten silicon into carbon preforms. This is a complex phenomenon arising from the interplay between fluid flow,…
We derive the second-order hydrodynamic equation for reactive multi-component systems from the relativistic Boltzmann equation. In the reactive system, particles can change their species under the restriction of the imposed conservation laws during the collision process. Our derivation is based on the renormalization group (RG) method, in which the Boltzmann equation is solved in an organized perturbation method as faithfully as possible and possible secular terms are resummed away by a suitable setting of the initial value of the distribution function. The microscopic formulae of the relaxati…
It is widely recognized that the structure of porous media is of relevance for a variety of mechanical and physical phenomena. The focus of the present work is on capillarity, a pore-scale process occurring at the micron scale. We attempt to characterize the influence of pore shape for capillary infiltration by means of Lattice Boltzmann simulations in 2D with reactive boundaries leading to surface growth and ultimately to pore closure. The systems under investigation consist of single channels with different simplified morphologies: namely, periodic profiles with sinusoidal, step-shaped and z…
How to accurately probe chemically reactive flows with essential thermodynamic nonequilibrium effects is an open issue. Via the Chapman-Enskog analysis, the local nonequilibrium particle velocity distribution function is derived from the gas kinetic theory. It is demonstrated theoretically and numerically that the distribution function depends on the physical quantities and derivatives, and is independent of the chemical reactions directly. Based on the simulation results of the discrete Boltzmann model, the departure between equilibrium and nonequilibrium distribution functions is obtained an…
The development of high-efficiency porous catalyst membranes critically depends on our understanding of where the majority of the chemical conversions occur within the porous structure. This requires mapping of chemical reactions and mass transport inside the complex nano-scale architecture of porous catalyst membranes which is a multiscale problem in both the temporal and spatial domain. To address this problem, we developed a multi-scale mass transport computational framework based on the Lattice Boltzmann Method (LBM) that allows us to account for catalytic reactions at the gas-solid interf…
Reactive Rayleigh-Taylor systems are characterized by the competition between the growth of the instability and the rate of reaction between cold (heavy) and hot (light) phases. We present results from state-of-the-art numerical simulations performed at high resolution in 2d by means of a self-consistent lattice Boltzmann method which evolves the coupled momentum and thermal equations and includes a reactive term. We tune the parameters affecting flame properties, in order to address the competition between turbulent mixing and reaction, ranging from slow to fast-reaction rates. We also study …
Effects of heterogeneity of mineral distribution and reaction rate on the rock dissolution process are investigated using a pore-scale reactive transport model based on the lattice Boltzmann method. Coupled fluid flow, species transport, chemical reaction and solid structure alternation due to dissolution are simulated. Effects of mineral distributions and chemical heterogeneity on the dissolution behaviors and evolutions of hydrologic properties are studied under different reactive transport conditions. Simulation results show that the coupling between advection, diffusion and reaction as wel…
A hybrid lattice Boltzmann/finite-difference solver for low Mach thermo-compressible flows developed in earlier works is extended to more realistic and challenging configurations involving turbulence and complex geometries in the present article. The major novelty here as compared to previous contributions is the application of a more robust collision operator, considerably extending the stability of the original single relaxation time model and facilitating larger Reynolds number flow simulations. Additionally, a subgrid model and the thickened flame approach have also been added allowing for…
Gas-generating reactive flows in bicontinuous catalyst support structures
Helmholtz Institute Erlangen-Nürnberg für Erneuerbare Energien（埃尔朗根-纽伦堡亥姆霍兹可再生能源研究所）；Friedrich-Alexander-Universität Erlangen-Nürnberg（埃尔朗根-纽伦堡弗里德里希·亚历山大大学）
In this work we want to simulate with the Lattice-Boltzmann method in 2D the capillary infiltration into porous structures obtained from the packing of particles. The experimental problem motivating our work is the densification of carbon preforms by reactive melt infiltration. The aim is to determine optimization principles for the manufacturing of high-performance ceramics. Simulations are performed for packings with varying structural properties. Our analysis suggests that the observed slow infiltrations can be ascribed to interface dynamics. Pinning represents the primary factor retarding …
The process of liquid silicon infiltration is investigated for channels with radii from $0.25$ to $0.75$ [mm] drilled in compact carbon preforms. The advantage of this setup is that the study of the phenomenon results to be simplified. For comparison purposes, attempts are made in order to work out a framework for evaluating the accuracy of simulations. The approach relies on dimensionless numbers involving the properties of the surface reaction. It turns out that complex hydrodynamic behavior derived from second Newton law can be made consistent with Lattice-Boltzmann simulations. The experim…
