Modeling the thermodynamics of the FeTi hydrogenation under para-equilibrium: An ab-initio and experimental study

Alvares, Ebert; Jerabek, Paul; Shang, Yuanyuan; Santhosh, Archa; Pistidda, Claudio; Heo, Tae Wook; Sundman, Bo; Dornheim, Martin

Abstract

FeTi-based hydrides have recently re-attracted attention as stationary hydrogen storage materials due to favorable reversibility, good sorption kinetics and relatively low costs compared to alternative intermetallic hydrides. Employing the OpenCalphad software, the thermodynamics of the (FeTi)1−xHx (0 ≤x≤ 1) system were assessed as a key basis for modeling hydrogenation of FeTi-based alloys. New thermodynamic data were acquired from our experimental pressure-composition-isotherm (PCI) curves, as well as first-principles calculations utilizing density functional theory (DFT). The thermodynamic phase models were carefully selected based on critical analysis of literature information and ab-initio investigations. Key thermodynamic properties such as dissociation pressure, formation enthalpies and phase diagrams were calculated in good agreement to our performed experiments and literature-reported data. This work provides an initial perspective, which can be extended to account for higher-order thermodynamic assessments and subsequently enables the design of novel FeTi-based hydrides. In addition, the assessed thermodynamic data can serve as key inputs for kinetic models and hydride microstructure simulations.

Citation

Alvares, E., Jerabek, P., Shang, Y., Santhosh, A., Pistidda, C., Heo, T. W., Sundman, B., & Dornheim, M. (2022). Modeling the thermodynamics of the FeTi hydrogenation under para-equilibrium: An ab-initio and experimental study. Calphad, 77, Article 102426. https://doi.org/10.1016/J.CALPHAD.2022.102426

• Journal Article Type: Article
• Acceptance Date: Apr 12, 2022
• Online Publication Date: May 21, 2022
• Publication Date: Jun 1, 2022
• Deposit Date: Aug 5, 2024
• Journal: Calphad: Computer Coupling of Phase Diagrams and Thermochemistry
• Print ISSN: 0364-5916
• Publisher: Elsevier
• Peer Reviewed: Peer Reviewed
• Volume: 77
• Article Number: 102426
• DOI: https://doi.org/10.1016/J.CALPHAD.2022.102426
• Keywords: Hydrogen storage, Metal Hydrides, FeTi, DFT, Pressure-composition isotherms
• Public URL: https://nottingham-repository.worktribe.com/output/34872340
• Publisher URL: https://www.sciencedirect.com/science/article/pii/S0364591622000347?via%3Dihub
• Additional Information: This article is maintained by: Elsevier; Article Title: Modeling the thermodynamics of the FeTi hydrogenation under para-equilibrium: An ab-initio and experimental study; Journal Title: Calphad; CrossRef DOI link to publisher maintained version: https://doi.org/10.1016/j.calphad.2022.102426; Content Type: article; Copyright: © 2022 Elsevier Ltd. All rights reserved.