Experimental and Computational Prediction of the Hydrogen Transport Properties of Pd4S

Abstract

Computational and experimental methods were used to quantify the apparent influence of a Pd4S corrosion product resulting from flux testing of 100-micron thick pure palladium membranes in a 0.1%H2S−10%He−H2 retentate gas mixture. The permeability of Pd4S was estimated to be approximately 20 times less than that of pure palladium from the results obtained through sulfide growth kinetics using gravimetric methods and the observed H2 flux decay during permeability characterization from 623 to 908 K. To complement experimental analysis, density functional theory was used to predict the hydrogen permeability of Pd4S by examining diffusivity and solubility of H in bulk Pd4S. Results are in good agreement between the experimental and computational prediction of the activation energy of permeation, while only in moderate agreement when comparing the hydrogen permeability of Pd4S. The permeability values obtained through experimentation were approximately 7 times greater than the computational predictions.