This study investigates the reaction kinetics of Fe2O3/Ce-γAl2O3 oxygen carrier for chemical looping hydrogen production (CLHP), aiming to overcome the limited reactivity of Fe-based carriers at moderate temperatures. A comprehensive approach was employed combining temperature-programmed desorption (TPD), kinetic modeling, and experimental validation in a CREC Riser Simulator. TPD results revealed that Fe–CeγAl demonstrated the highest CO2 desorption capacity (1.589 mmol/g), strong CH4 retention at moderate and strong sites, and balanced CO interaction, supporting its superior gas–solid performance. Kinetic modeling of three reaction pathways (CH4 partial and complete oxidation, and CO oxidation) yielded excellent model fitting (R2 = 98.67, AIC = −106.22). The intrinsic rate constants (k1° = 0.024, k2° = 0.013, k3° = 0.019) and activation energies (E1 = 94.30, E2 = 101.59, E3 = 68.72 kJ/mol) confirmed that CH4 partial oxidation is kinetically favored, while CO oxidation proceeds most rapidly for Fe–CeγAl under surface-controlled conditions in the CREC Riser Simulator. The deactivation function parameter (λ = 0.25) indicated moderate oxygen depletion, sufficient to sustain reaction efficiency up to 675 °C. This work bridges a critical gap in current CLHP research by providing a validated kinetic model and mechanistic interpretation for Ce-modified Fe2O3 systems. The results serve as a robust foundation for reactor design, solid circulation optimization, and predictive simulation of CLHP operations, advancing the development of low-emission hydrogen production technologies.
Putra et al. (Thu,) studied this question.