Effect of sweep gas on hydrogen permeation of supported Pd membranes: Experimental and modeling

Abstract

Membrane reactor processes are being increasingly proposed as an attractive solution for pure hydrogen production due to the possibility to integrate production and separation inside a single reactor vessel. High hydrogen purity can be obtained through dense metallic membranes, especially palladium and its alloys, which are highly selective to hydrogen. The use of thin membranes seems to be a good industrial solution in order to increase the hydrogen flux while reducing the cost of materials. Typically, the diffusion through the membrane layer is the rate-limiting step and the hydrogen permeation through the membrane can be described by the Sieverts’ law but, when the membrane becomes thinner, the diffusion through the membrane bulk becomes less determinant and other mass transfer limitations might limit the permeation rate. Another way to increase the hydrogen flux at a given feed pressure, is to increase the driving force of the process by feeding a sweep gas in the permeate side. This effect can however be significantly reduced if mass transfer limitations in the permeate side exist. The aim of this work is to study the mass transfer limitation that occurs in the permeate side in presence of sweep gas. A complete model for the hydrogen permeation through PdAg membranes has been developed, adding the effects of concentration polarization in retentate and permeate side and the presence of the porous support using the dusty gas model equation, which combines Knudsen diffusion, viscous flow and binary diffusion. By studying the influence of the sweep gas it has been observed that the reduction of the driving force is due to the stagnant sweep gas in the support pores while the concentration polarization in the permeate is negligible.