Publication | Peer reviewed papers | Sonstige

The effect of the reaction equilibrium on the kinetics of gas-solid reactions — A non-parametric modeling study.

Birkelbach F, Deutsch M, Werner A.

Published 2020

Citation: Birkelbach F, Deutsch M, Werner A. The effect of the reaction equilibrium on the kinetics of gas-solid reactions — A non-parametric modeling study. Renewable Energy 2020.152:300-307.

Abstract

The viability of thermochemical energy storage for a given application is often determined by the reaction kinetics under process conditions. For high exergetic efficiency the process needs to operate in close proximity to the reaction equilibrium. Thus, accurate kinetic models that include the effect of the reaction equilibrium are required.

In the present work, different parametrization methods for the equilibrium term in the General Kinetic Equation are evaluated by modeling the kinetics of two reaction systems relevant for thermochemical energy storage (CaC2O4 and CuO) from experimental data. A non-parametric modeling method based on tensor decompositions is used that allows for a purely data driven assessment of different parametrization methods.

Our analysis shows that including a suitable equilibrium term is crucial. Omitting the equilibrium term when modeling formation reactions can lead to seemingly negative activation energies. Our tests also show that for formation reactions, the reaction rate decreases much faster towards the equilibrium than theory predicts. We present an empirical modeling approach that can predict the reaction rate of gas-solid reactions, regardless of the shortcomings of theory. In this way, non-parametric modeling offers a powerful tool for applied research and may contribute to the advancement of the thermochemical energy storage technology.

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