Modelling and Simulation of Heterogeneous Reactions with Statistical Particle Methods

TL;DR

This paper develops and evaluates a kinetic Monte Carlo model integrated with particle flow simulations to accurately estimate heat loads on re-entry vehicles by modeling catalytic reactions on surfaces, matching experimental data.

Contribution

It introduces a kinetic Monte Carlo approach for catalytic gas-surface interactions within particle simulations, improving heat load estimation accuracy without experimental parameter fitting.

Findings

Kinetic Monte Carlo model accurately predicts heat fluxes.

Model matches experimental recombination coefficients.

Simulation demonstrates effectiveness for SiO2 surfaces.

Abstract

Estimating the heat loads on re-entry vehicles is a crucial part of preparing for atmospheric re-entry manoeuvres. Re-entry flows at high altitudes are in the rarefied regime and are governed by high enthalpies and thermodynamic non-equilibrium. Additionally, catalytic gas-surface reactions change the gas flow composition and can have a major influence on the heat transfer. Our goal is to estimate the heat loads without a priori fitting of simulation parameters to experiments. We use the tool PICLas for simulations of such rarefied gas flows. It combines different particle methods, including the Direct Simulation Monte Carlo method, for modelling of gases. Recently it has been extended to include different catalysis models to treat reactions on surfaces. We evaluate a kinetic Monte Carlo approach to model catalytic gas-surface interactions in combination with flow simulations using particle methods. Here, the adsorbate distribution is modelled by reproducing a surface system using a kinetic Monte Carlo approach and estimating the necessary parameters using model assumptions. This catalytic model is compared to a simple recombination model. We present simulations that show the capability of the implemented models for a $\mathrm{SiO_2}$ surface in an Oxygen flow. Furthermore, simulation results are compared to heat fluxes and recombination coefficient obtained from the respective experiment. The results show that simulations using the kinetic Monte Carlo approach match the experimentally obtained values. Thus, the approach can be used to estimate the reactivity of oxygen flows over $\mathrm{SiO_2}$ surfaces.