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Hydrogen absorption in intermetallic compounds from first principles

Olivier Nadeau1,2,3, Romuald Béjaud1,2, Lucas Baguet1,2, Grégory Geneste1,2, François Bottin1,2, and Gabriel Antonius3

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Phys. Rev. B 113, 094104 – Published 3 March, 2026

DOI: https://doi.org/10.1103/fzwm-cctt

Abstract

Intermetallic compounds such as A2B7 alloys are promising candidates for mobile hydrogen storage applications due to their high and reversible hydrogen absorption capacity. We compute the absorption isotherm of Nd3MgNi14 from first principles using a multiscale modeling approach. Absorption sites are identified through a systematic geometrical analysis, and are characterized with density functional theory (DFT) calculations. The absorption site properties are used in room-temperature grand canonical Monte Carlo simulations to predict hydrogen uptake as a function of pressure, leading to a full absorption isotherm in good agreement with experimental data. We show that both hybrid exchange-correlation functionals and zero-point energy corrections are necessary to obtain accurate absorption properties. The analysis of the fully hydrogenated structure with DFT shows considerable volume expansion, which stabilizes the structure at large hydrogen content.

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Phys. Rev. B 113, 094104– Published 3 March, 2026
  • Received 5 September 2025
  • Accepted 6 February 2026
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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