Synergetic effect of ZrO2 on the oxidation–reduction reaction of Fe2O3 during chemical looping combustion

Fe2O3/ZrO2 model oxygen carrier is constructed at atomic-level precision under ultra-high-vacuum conditions. Based on density functional theory calculations and molecular dynamical simulations, structure and energy analysis suggests that the complex Fe2O3/ZrO2 is stable and more chemically active than the pure Fe2O3, ZrO2 promotes the adsorption of CO, which is chemisorption rather than physisorption on the pure Fe2O3 surface. Interface electronic interaction of Fe2O3/ZrO2 makes Fe2O3 positive to accept electron from CO easily and hence promoting the chemisorption of CO and the formation of carbonate species, while such electronic interaction makes it relatively more difficult in oxidizing Fe2O2 supported on ZrO2. However, all reaction barrier energies are small enough for Fe2O2 oxidation to happen under high temperature in the CLC system. Both CO oxidation by Fe2O3/ZrO2 related to the fuel reactor in the chemical looping combustion (CLC) system and Fe2O2/ZrO2 oxidation by O2 related to the air reactor in CLC system illustrate the synergetic effect of ZrO2 on the CO oxidation and Fe2O2 oxidation.