Work

Learning chemical kinetics through data assimilation: Theory and application to ammonia oxidation

Year: 2025

Type: article

Abstract: Chemical kinetics plays a crucial role in understanding and predicting combustion processes, yet accurately estimating rate parameters remains challenging due to complex reaction dynamics and intrinsic uncertainties. This study examines the potential of the Augmented Ensemble Kalman Filter (AEnKF) for assimilating experimental data into chemical kinetic models. By employing an ensemble of stochastic simulations, AEnKF facilitates robust estimation of a consolidated state that consists of state variables and model parameters while incorporating observational data to enhance predictions. The developed framework simultaneously estimates key kinetic parameters governing reaction dynamics, simultaneously improving state predictions and parameter representation. As a representative case study, the model is applied to ammonia oxidation kinetics using species time-histories from shock tube experiments. By selecting a subset of key reaction rates, we demonstrate that the methodology handles the inherent nonlinearities of chemical kinetics while retaining physical consistency throughout the parameter estimation process. By performing systematic parameter studies to assess the effects of sample size and assimilation frequency, we show that the algorithm operates efficiently across a broad range of conditions and learns different kinetic parameters effectively. Results illustrate the potential of AEnKF as a reliable tool for state- and parameter estimation in the development of advanced combustion kinetic models. • Augmented Ensemble Kalman Filter was applied to data-driven estimation of kinetic rate parameters. • Four rate-equation parameters for ammonia oxidation recovered from shock tube data. • Estimated parameters improved model accuracy in varied conditions vs baseline. • The methodology improved model accuracy while providing chemical reaction insights. • Data assimilation revealed intrinsic temperature dependence of reaction parameters.

Source: Chemical Engineering Journal

DOI: 10.1016/j.cej.2025.168863

Authors: Timoteo Dinelli, Alessandro Stagni, Matthias Ihme

Institutions: Politecnico di Milano, Stanford University, SLAC National Accelerator Laboratory

Language: English

Topic: Advanced Combustion Engine Technologies

Subfield: Fluid Flow and Transfer Processes

Field: Chemical Engineering

Domain: Physical Sciences

Open Access status: hybrid

Estimated APC paid: $4,830