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

TL;DR

This study combines experimental and ab-initio methods to model the thermodynamics of FeTi hydrogenation, providing data crucial for designing new hydrogen storage materials and understanding phase behavior.

Contribution

It integrates experimental PCI data with DFT calculations to develop thermodynamic models for FeTi hydrides, advancing the understanding of their hydrogenation thermodynamics.

Findings

Thermodynamic properties like dissociation pressure and formation enthalpy were accurately predicted.

Phase diagrams aligned well with experimental and literature data.

The models enable future design of FeTi-based hydrides for hydrogen storage.

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)$_{1-x}$H$_{x}$ (0 $\leq x \leq$ 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 \emph{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.