Abstract:
Chemical Looping Combustion (CLC) is recognized as an efficient carbon capture technology, achieving high CO
2 capture and separation during fossil fuel combustion by utilizing the redox properties of oxygen carriers in redox cycles. The redox cycles of iron-based oxygen carriers in Coal Direct Chemical Looping (CDCL) combustion were thermodynamically simulated using Cantera software. The loss characteristics of the oxygen carriers and the effects of cycle performance on reaction products were systematically studied. Under the defined simulation conditions, the maximum number of cycles reached 388. In the first 120 cycles, the oxygen carriers are primarily composed of Fe
3O
4 and FeO, exhibiting strong oxidation capabilities and reacting with the fuel to produce gas-phase products dominated by CO
2 and H
2O. As the number of cycles increases to 270, the oxygen carriers are gradually reduced to a lower oxidation state (Fe), leading to a decrease in oxidation capacity, with reduction reactions dominating and generating more CO and H
2, resulting in staged changes in product distribution. In subsequent cycles, the oxidation capacity of the oxygen carriers significantly declines, and solid loss stabilizes. Additionally, a dynamic loss mechanism based on energy regulation is introduced, showing that energy utilization efficiency significantly impacts the number of cycles and reaction equilibrium, with a positive correlation observed between energy difference and solid loss. The simulation results indicate that in the fuel reactor, the energy difference initially reaches up to 3.35×10
5 kJ/ mol, then gradually decreases and approaches equilibrium as the reaction progresses. In the air reactor, the energy difference initially peaks at 3.72×10
5 kJ/ mol, with high oxidation reaction efficiency at the beginning, which then gradually decreases and approaches a steady state. By analyzing the energy differences over multiple cycles along with the distribution of solid and gas-phase products, insights are provided for the lifespan assessment and optimization design of iron-based oxygen carriers in CDCL combustion technology.