Molecular Simulation of Chemically Reacting Flows Inside Micro/Nano-channels
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The main objective of this thesis is to study the fundamental behaviour of multi-component gas mixture flows in micro/nano-channels undergoing catalytic chemical reactions on the walls. This work is primarily focused on nano-scale reacting flows seen in related applications; especially, miniaturized energy sources such as micro-fuel cells and batteries. At these geometries, the order of the characteristic length is close to the mean free path of the flowing gas, making the flow highly rarefied. As a result, non-equilibrium conditions prevail even the bulk flow and therefore, continuum assumptions are not held anymore. Hence, discrete methods should be adopted to simulate molecular movements and interactions described by the Boltzmann equation. The Direct Simulation Monte Carlo (DSMC) method was employed for the present research due to its natural ability for simulating a broad range of rarefied gas flows, and its flexibility to incorporate surface chemical reactions. In the first step, fluid dynamics and the heat transfer of H₂/N₂ and H₂/N₂/CO₂ gas mixture slip flows in a plain micro-channel are simulated. The obtained results are compared to the corresponding data achieved from Navier-Stokes equations with slip/jump boundary conditions. Generally, very good agreements are observed between the two methods. It proves the ability of DSMC in replicating the fluid properties of multi-component gas mixtures even when high mass discrepancies exist among the species. Based on this comparison, the proper parameters are set for the prepared DSMC code, and the appropriate intermolecular collision model is identified. It is also found that stream variables should be calculated more accurately at flow boundaries in order to simulate the intense upstream diffusion emerging at low velocity flows frequently seen in micro/nano-applications. Therefore, in the second step, a novel pressure boundary condition is introduced for gas mixture flows by substituting the commonly used Maxwell velocity distribution with the Chapman-Enskog distribution function. It is shown that this new method yields better results for lower velocity and higher rarefaction level cases. In the last step, a new method is proposed for coupling the flow field simulated by DSMC and surface reactions modelled by the species conservation ODE system derived from the reaction mechanism. First, a lean H₂/air slip flow subjected to oxidation on platinum coated walls in a flat micro-channel 4μm in height is simulated as a verification test case. The results obtained are validated against the solutions of the Navier-Stokes equations with slip/jump boundary conditions and very good conformity is achieved. Next, several cases undergoing the same reaction with Reynolds numbers ranging from 0.2 to 3.6 and Knudsen numbers ranging from 0.025 to 0.375, are simulated using the verified code to investigate the effects of the channel height ranging from 0.5μm to 2μm , the inlet mass flow rate ranging from 5 kg/m².s to 25 kg/m².s, the inlet temperature ranging from 300K to 700K, the wall temperature ranging from 300K to 1000K, and the fuel/air equivalence ratio ranging from 0.28 to 1.5. Some of the findings are as follows: (1) increasing the surface temperature from 600K to 1000K and/or the inlet temperature from 300K to 700K results in negligible enhancement of the conversion rate, (2) the optimum value of the equivalence ratio is on the fuel lean side (around 0.5), (3) the efficiency of the reactor is higher for smaller channel heights, and (4) increasing the inlet mass flux elevates the reaction rate especially for the smaller channels; this effect is not linear and is more magnified for lower mass fluxes.