Date of Original Version
This is the author’s version of a work that was accepted for publication. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version is available at http://dx.doi.org/10.1016/j.commatsci.2014.05.065
Abstract or Description
As an aid to the development of hydrogen separation membranes, we predict the temperature dependent phase diagrams using first principles calculations combined with thermodynamic principles. Our method models the phase diagram without empirical fitting parameters. By applying thermodynamic principles and solid solution models, temperature-dependent features of the Cu–Pd–S system can be explained, specifically solubility ranges for substitutions in select crystalline phases. Electronic densities of states calculations explain the relative favorability of certain chemical substitutions. In addition, we calculate sulfidization thresholds for the Pd–S2 system and activities for the Cu–Pd binary in temperature regimes where the phase diagram contains multiple solid phases.
Computational Materials Science, 92, 377-386.