Calcination of calcium-based sorbents at pressure in a broad range of CO2 concentrations

The calcination reaction of two limestones and a dolomite with different porous structures was studied by thermogravimetric analysis. The effects of calcination temperature (1048-1173 K), particle size (0.4-2.0 mm), CO2 concentration (0-80%) and total pressure (0.11.5 MPa) were investigated. SEM analysis indicated the existence of two different particle calcination models depending on the sorbent type: a shrinking core model with a sharp limit between the uncalcined and calcined parts of the particle and a grain model with changing calcination conversion at the particle radial position. The appropriate reaction model was used to determine the calcination kinetic parameters of each sorbent. Chemical reaction and mass transport in the particle porous system were the main limiting factors of the calcination reaction at the experimental conditions. A Langmuir-Hinshelwood-type kinetic model using the Freundlich isotherm was proposed to account for the effect of the CO2 during sorbent calcination. This allowed us to predict the calcination conversion of very different sorbents in a broad range of CO2 partial pressures. Total pressure also inhibited the sorbent calcination. This fact was accounted for by an additional decrease in the molecular diffusion coefficient with increasing total pressure with respect to that indicated by Fuller's equation. (C) 2002 Published by Elsevier Science Ltd.