First Principles Modeling of the Temperature Dependent Ternary Phase Diagram for the Cu-Pd-S System

TL;DR

This paper uses first principles calculations combined with thermodynamics to predict the temperature-dependent phase diagram of the Cu-Pd-S system, aiding hydrogen membrane development without empirical parameters.

Contribution

It introduces a parameter-free modeling approach for phase diagrams, integrating electronic structure calculations with thermodynamic models for the Cu-Pd-S system.

Findings

Predicted solubility ranges in crystalline phases.

Explained phase stability via electronic densities of states.

Calculated sulfidization thresholds and activities.

Abstract

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.