Chemical-Looping Combustion Process: Kinetics and Mathematical Modeling

Chemical Looping Combustion technology involves circulating a metal oxide between a fuel zone where methane reacts under anaerobic conditions to produce a concentrated stream of CO, and water and an oxygen rich environment where the metal is reoxidized. Although the needs for electrical power generation drive the process to high temperatures, lower temperatures (600-800 degrees C) are sufficient for industrial processes such as refineries. In this paper, we investigate the transient kinetics of NiO carriers in the temperature range of 600 to 900 degrees C in both a fixed bed microreactor (WNW = 2-4 g CH4/h/g oxygen carrier) and a fluid bed reactor (WHSV = 0.014-0.14 g CH4/h per g oxygen carrier). Complete methane conversion is achieved in the fluid bed for several minutes. In the microreactor, the methane conversion reaches a maximum after an initial induction period of less than 10 s. Both CO2 and H2O yields are highest during this induction period. As the oxygen is consumed, methane conversion drops and both CO and H-2 yields increase, whereas the CO2 and H2O concentrations decrease. The kinetics parameter of the gas solids reactions (reduction of NiO with CH4, H-2, and CO) together with catalytic reactions (methane reforming, methanation, shift, and gasification) were estimated using experimental data obtained on the fixed bed microreactor. Then, the kinetic expressions were combined with a detailed hydrodynamic model to successfully simulate the comportment of the fluidized bed reactor. (C) 2010 American Institute of Chemical Engineers AIChE J, 56: 1063-1079, 2010