A model of transient heat and mass transfer in a heterogeneous medium of cerium dioxide undergoing nonstoichiometric reduction

The redox chemistry of nonstoichiometric metal oxides can be used to produce chemical fuels by harnessing concentrated solar energy to split water and/or carbon dioxide. In such a process, it is desirable to use a porous reactive substrate for increased surface area and improved gas transport. The present study develops a macroscopic-scale model of porous ceria undergoing thermal reduction. The model captures the coupled interactions between the heat and mass transfer and the heterogeneous chemistry using a local thermal non-equilibrium (LTNE) formulation of the volume averaged conservation of mass and energy equations in an axisymmetric cylindrical domain. The results of a representative test case simulation demonstrate strong coupling between gas phase mass transfer and the chemical kinetics as well as the pronounced impact of optical thickness on the temperature distribution and thus global solar-to-chemical energy conversion.