Sulfur dioxide removal by calcium-modified fibrous KCC-1 mesoporous silica: kinetics, thermodynamics, isotherm and mass transfer mechanism

Abstract

The removal of sulfur dioxide from industrial flue gas through dry flue gas desulfurization method commonly involves the use of adsorption process with porous sorbent. The efficiency of this process is highly dependent on the adsorption capacity and the adsorption rate of SO2 onto the sorbent materials. The use of KCC-1 mesoporous silica modified with calcium metal additives (Ca/KCC-1) in SO2 adsorption is examined in a fixed bed reactor system. The adsorption capacity of Ca/KCC-1 is found to be critically governed by the reaction temperature and inlet SO2 concentration where low values of both parameters are favorable to achieve the highest adsorption capacity of 3241.94 mg SO2/g sorbent. SO2 molecules are adsorbed on the surface of Ca/KCC-1 by both physisorption and chemisorption processes as assumed by the Avrami kinetic model. Thermodynamic study shows that the process is exothermic and spontaneous in nature, and changes from an ordered stage on the surface of KCC-1 towards an increasingly random stage. The process is well explained by Freundlich isotherm model indicating a slightly heterogeneous process and moderate adsorption capacity. The adsorption stage is limited by film diffusion at the initial stage and by intraparticle diffusion during the transfer of SO2 into the network of pores before adsorption takes place on the active sites.