Particle scale modeling of CuFeAlO4 during reduction with CO in chemical looping applications

Particle scale models that couple reaction phenomena to changes in the solid-state chemistry of an oxygen carrier system are critical to the advancement of the chemical looping concept by allowing for a means to assess process scale up. This work presents an analysis of the reduction for a CuFeAlO4 oxygen carrier with Carbon Monoxide (CO). The analysis was utilized to aid in the application of particle scale model representation of the carrier system. An experimentally driven study was conducted to provide an array of operational/parametric data sets for the analysis and their impact accessed. Quantification of the cubic spinel oxide phase and changes due to lattice oxygen depletion from reduction were explored to link the solid-state chemistry changes to the reaction progression. Reduction occurred in a multistep process as oxygen was depleted from the structure. Oxygen bound to Cu cations were the first to react with CO. As oxygen was depleted further phase re-orientation occurred resulting in an iron based aluminate (FeAl2O4) with discrete metallic copper present. FeAl2O4 was further depleted of oxygen to metallic Fe and alumina. The multistep process was emulated through the use of a multi-interface Grainy pellet model. To add to the utility of the model, the effects of product gas, CO2, on the reaction progression were incorporated into the description. In addition, the catalytic effects of the Boudouard reaction were examined and incorporated into the representation adding to the novelty of the work.