Kinetics of hydrogen sulfide removal from coke oven gas over faujasite zeolite: Experimental and modeling studies

Abstract

The removal of H₂S from coke oven gas (COG) is an important issue for the further utilization of COG. Zeolites could be used for industrial desulfurization owing to their high thermal stability and regenerability. However, further analysis on the kinetics of deep desulfurization using zeolites is necessary to provide relevant information for industrial design. In this study, the desulfurization breakthrough curves of faujasite (FAU) zeolite in COG were measured using a fixed bed reactor. The adsorption isotherm was investigated using the Langmuir, Freundlich, Temkin, Dubinin-Radushkevich models. The adsorption saturated capacity of H₂S was inversely related to the temperature. The results show that the Langmuir model best fits the adsorption isotherm with a lower value of root-mean-square-error (RMSE) and Chi-Square (χ²), and the calculated activation energy is 14.62 kJ·mol⁻¹. The adsorption kinetics were investigated using pseudo-first-order (PFO), pseudo-second-order (PSO), Bangham and Weber-Morris models. The Bangham model fitted the kinetic data well, indicating that pore diffusion is an influential factor in the adsorption process. The Weber-Morris model suggests that the adsorption rate was not solely determined by the pore diffusion, but was also influenced by the active site on the FAU zeolite. The adsorption breakthrough curves under different gas flow rates were fitted using the bed depth service time (BDST) model, and it provides an accurate prediction of the breakthrough time with a small relative error. The results of thermodynamic analysis demonstrated the feasibility and spontaneity (ΔG<0) and exothermic (ΔH<0) nature of the adsorption process of the FAU zeolite for H₂S under COG.