Competing effects of surface catalysis and ablation in hypersonic reentry aerothermodynamic environment

Under hypersonic flow conditions, the complicated gas-graphene interactions including surface catalysis and surface ablation would occur concurrently and intervene together with the thermodynamic response induced by spacecraft reentry. In this work, the competing effects of surface heterogeneous catalytic recombination and ablation characteristics at elevated temperatures are investigated using the Reactive Molecular Dynamics (RMD) simulation method. A Gas-Surface Interaction (GSI) model is established to simulate the collisions of hyper-enthalpy atomic oxygen on graphene films in the temperature range of 500–2500 K. A critical temperature T_c around 900 K is identified to distinguish the graphene responses into two parts: at T < T_c, the heterogeneous surface catalysis dominates, while the surface ablation plays a leading role at T > T_c. Contradicting to the traditional Arrhenius expression that the recombination coefficient increases with the increase of surface temperature, the value is found to be relatively uniform at T < T_c but declines sharply as the surface temperature increases further due to the competing ablation effect. The occurrence of surface ablation decreases the amounts of active sites on the graphene surface for oxygen adsorption, leading to reduced recombination coefficient from both Langmuir-Hinshelwood (L-H) and Eley-Rideal (E-R) mechanisms. It suggests that the traditional Computational Fluid Dynamics (CFD) simulation method, which relies on the Arrhenius-type catalysis model, would result in large discrepancies in predicting aerodynamic heat for carbon-based materials during reentry into strong aerodynamic thermal environment.