Influence of water vapor on hydrogen permeation through 2.5 μm Pd–Ag membranes

Abstract

Hydrogen permeation experiments were performed to evaluate the influence of water vapor on hydrogen permeability in 80–20% by weight Pd–Ag membranes of 2.5 μm thickness. In particular, hydrogen flux was measured in pure hydrogen permeation tests as well as in experiments with binary mixtures containing also nitrogen or water vapor, that were performed at temperatures ranging from 473 to 723 K and at a transmembrane pressure differences up to about 3 bar. The membranes, supplied by NGK Insulator Ltd., Japan, showed a very high hydrogen permeance and lifetime, as well as virtually infinite selectivity (exceeding 10000 for H 2–N 2 mixtures). The experiments in hydrogen–nitrogen mixtures were carried out at different temperatures, hydrogen concentrations and feed flow rates and confirmed the existence of a non-negligible concentration polarization phenomenon in the experimental module. The gas phase mass transport and the module fluid dynamics were thus analyzed and the dimensionless numbers characterizing these processes were evaluated at the different operative conditions; a linear correlation was found to hold between Sherwood and Péclet numbers. Interestingly, the hydrogen permeate fluxes measured with feeds containing H 2–H 2O mixtures resulted always lower than those obtained for the nitrogen–hydrogen mixtures performed at the same hydrogen mole fraction and operative conditions: in particular, the hydrogen flux depletion increased with decreasing temperature and/or increasing the concentration of water vapor. All the experimental evidences suggest a clear interaction between water vapor and metallic layer, causing a lower hydrogen adsorption capacity of the membrane surface. That phenomenon is reversible, since the original permeance of the membrane was restored once the water vapor was removed from the feed, and is apparently due to a competitive H 2–H 2O adsorption on the Pd–Ag surface. The hydrogen flux depletion was then modeled by considering the simultaneous effects of gas phase resistance and competitive adsorption on the surface, obtaining a rather good agreement between experimental data and calculated results.