Molecular level simulations of combustion processes using the DSMC method

Chemical reactions significantly influence aerodynamic performance during spacecraft entry into the Martian atmosphere. Several chemical reaction models have been proposed in the direct simulation Monte Carlo simulation. The quantum-kinetics (Q-K) model has been applied in the case of diatomic molecules. Given that the Martian atmosphere consists primarily of CO2, it is crucial to find ways of implementing the Q-K model for polyatomic molecules. Although the chemical reaction rates involving CO2 have been investigated using the Q-K model, the problem of achieving detailed balance remains. Multiple vibrational modes exist for polyatomic molecules. Under the Q-K distribution, the average vibrational level of each mode is higher than that under the equilibrium distribution, and the total energy may be insufficient. Hence, its applicability to polyatomic molecules needs to be revealed. In this study, a comparison is made of the respective results obtained using the Larsen-Borgnakke (L-B) and Q-K distribution methods for the energy distribution of the reaction CO2+O⇋CO+O2, and detailed balance is achieved with the Q-K method but not the L-B method. Under the conditions assumed in this study, the vibrational energy distribution of CO consumed by the reverse reaction is not in good agreement with that generated by the forward reaction, leading to the failure of the L-B method. Finally, the results indicate that detailed balance is reached only when the collision temperature, based on the translational and vibrational energy, is employed to adjust the activation energy rather than the translational temperature generally adopted in the literature.

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Quantum-kinetic chemistry model with an anharmonic oscillator model: Model derivation and limitations

Civrais,

White,

Steijl

2024

Physics of Fluids

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This work presents a new formulation of the quantum-kinetic (QK) chemistry models, in which the vibrational excitation is modeled with an anharmonic oscillator model. The new formulations are applied to some of the most representative dissociation reactions occurring during an Earth re-entry. The newly derived analytical expressions are implemented in a direct simulation Monte Carlo (DSMC) solver. The DSMC reaction rates demonstrate excellent agreement with the newly derived analytical expressions, verifying the successful implementation in the DSMC solver. The new models suggest that dissociation reactions are more likely to occur than with the original QK models. Furthermore, the new formulations are compared against experimental measurements, high-fidelity calculations, and well-established chemistry models for both thermal equilibrium and non-equilibrium conditions, presenting reasonable agreement with the baseline database. Additionally, the limitations of the new formulations are assessed for thermal non-equilibrium conditions where an excessive utilization of the relative translational energy and insufficient utilization of the pre-collision vibrational energy to promote dissociation reactions is found.

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Molecular level simulations of combustion processes using the DSMC method

Cited by 6 publications

References 18 publications

Molecular level simulations of hydrogen-air flame at high pressures

Molecular level simulations of hydrogen-air flame at high pressures

Post-reaction internal energy distributions of quantum-kinetics model for simulating chemical reactions of polyatomic molecules

Quantum-kinetic chemistry model with an anharmonic oscillator model: Model derivation and limitations

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