Silver-Exchanged Mordenite for Capture of Water Vapor in Off-Gas Streams: A Study of Adsorption Kinetics

Abstract

Reduced silver-exchanged mordenite (Ag0Z) has been recognized as the benchmark adsorbent for radioactive iodine removal from the nuclear fuel reprocessing off-gases. It has also been shown to have a considerable adsorption capacity for water vapor, which is a major component (tritiated water) in the off-gases of spent nuclear fuel reprocessing facilities. Therefore, understanding the kinetics of water vapor adsorption on Ag0Z is necessary for a better design of off-gas treatment systems. The adsorption kinetics were studied through adsorption experiments of water vapor on Ag0Z pellets and analyses of the kinetic data with adsorption models that describe processes of mass transfer and inter/intracrystalline diffusion. Uptake curves of water vapor on Ag0Z pellets were obtained with a continuous-flow adsorption system at temperatures of 25, 40, 60, 100, 150, and 200 °C and dew points from −53.6 °C to 12.1 °C. The diffusion-controlling factors were determined experimentally and analytically. It was found that the diffusion process of water vapor in Ag0Z pellets was controlled by macropore diffusion. Gas film mass-transfer resistance also contributed to the adsorption process of the 0.9 mm Ag0Z pellets, but it could be minimized with a high gas velocity and small pellet radius. Kinetic models including macropore diffusion (MD), linear driving force (LDF) and shrinking core (SC) were used to fit the uptake curves. The macropore diffusivity for water vapor adsorption on Ag0Z pellets was determined using the three models. It was found that the LDF and SC models could well describe the kinetic process, while the fitting with the MD model was not quite as good due to the existence of external mass-transfer resistance for the 0.9 mm Ag0Z pellets.