Destabilizing high-capacity high entropy hydrides via earth abundant substitutions: From predictions to experimental validation

Agafonov, Andrei; Pineda-Romero, Nayely; Witman, Matthew; Nassif, Vivian; Vaughan, Gavin B.M.; Lei, Lei; Ling, Sanliang; Grant, David M.; Dornheim, Martin; Allendorf, Mark; Stavila, Vitalie; Zlotea, Claudia

doi:10.1016/j.actamat.2024.120086

Destabilizing high-capacity high entropy hydrides via earth abundant substitutions: From predictions to experimental validation

Journal Article · Fri Jun 07 00:00:00 EDT 2024 · Acta Materialia

DOI:https://doi.org/10.1016/j.actamat.2024.120086· OSTI ID:2512450

Agafonov, Andrei ^[1]; Pineda-Romero, Nayely ^[1]; Witman, Matthew ^[2]; Nassif, Vivian ^[3]; Vaughan, Gavin B.M. ^[4]; Lei, Lei ^[5]; Ling, Sanliang ^[5]; Grant, David M. ^[5]; Dornheim, Martin ^[5]; Allendorf, Mark ^[2]; Stavila, Vitalie ^[2]; Zlotea, Claudia ^[1]

Université Paris-Est Créteil, Thiais (France); Centre National de la Recherche Scientifique (CNRS), Thiais (France). Institut de Chimie et des Matériaux Paris-Est (ICMPE)
Sandia National Laboratories (SNL-CA), Livermore, CA (United States)
Centre National de la Recherche Scientifique (CNRS), Grenoble (France); Univ. of Grenoble Alpes, Grenoble (France). Institut Néel
European Synchrotron Radiation Facility (ESRF), Grenoble (France)
Univ. of Nottingham (United Kingdom)

The vast chemical space of high entropy alloys (HEAs) makes trial-and-error experimental approaches for materials discovery intractable and often necessitates data-driven and/or first principles computational insights to successfully target materials with desired properties. In the context of materials discovery for hydrogen storage applications, a theoretical prediction-experimental validation approach can vastly accelerate the search for substitution strategies to destabilize high-capacity hydrides based on benchmark HEAs, e.g. TiVNbCr alloys. Here, in this study, machine learning predictions, corroborated by density functional theory calculations, predict substantial hydride destabilization with increasing substitution of earth-abundant Fe content in the (TiVNb)₇₅Cr_25-xFe_x system. The as-prepared alloys crystallize in a single-phase bcc lattice for limited Fe content x < 7, while larger Fe content favors the formation of a secondary C14 Laves phase intermetallic. Short range order for alloys with x < 7 can be well described by a random distribution of atoms within the bcc lattice without lattice distortion. Hydrogen absorption experiments performed on selected alloys validate the predicted thermodynamic destabilization of the corresponding fcc hydrides and demonstrate promising lifecycle performance through reversible absorption/desorption. This demonstrates the potential of computationally expedited hydride discovery and points to further opportunities for optimizing bcc alloy ↔ fcc hydrides for practical hydrogen storage applications.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-CA), Livermore, CA (United States)

Sponsoring Organization:: Engineering and Physical Sciences Research Council (EPSRC); Leverhulme Trust; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO)

Grant/Contract Number:: NA0003525

OSTI ID:: 2512450

Report Number(s):: SAND--2024-07515J

Journal Information:: Acta Materialia, Journal Name: Acta Materialia Vol. 276; ISSN 1359-6454

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (39)

Chemical and Physical Solutions for Hydrogen Storage Eberle, Ulrich; Felderhoff, Michael; Schüth, Ferdi Angewandte Chemie International Edition, Vol. 48, Issue 36 https://doi.org/10.1002/anie.200806293	journal	August 2009
The absorption of hydrogen by binary vanadium-chromium alloys Lynch, J. F.; Reilly, J. J.; Millot, F. Journal of Physics and Chemistry of Solids, Vol. 39, Issue 8 https://doi.org/10.1016/0022-3697(78)90150-6	journal	January 1978
Ab-initio structure determination of LiSbWO6 by X-ray powder diffraction Le Bail, A.; Duroy, H.; Fourquet, J. L. Materials Research Bulletin, Vol. 23, Issue 3 https://doi.org/10.1016/0025-5408(88)90019-0	journal	March 1988
Recent advances in magnetic structure determination by neutron powder diffraction Rodríguez-Carvajal, Juan Physica B: Condensed Matter, Vol. 192, Issue 1-2 https://doi.org/10.1016/0921-4526(93)90108-I	journal	October 1993
A critical review of high entropy alloys and related concepts Miracle, D. B.; Senkov, O. N. Acta Materialia, Vol. 122 https://doi.org/10.1016/j.actamat.2016.08.081	journal	January 2017
Counting electrons - A new approach to tailor the hydrogen sorption properties of high-entropy alloys Nygård, Magnus Moe; Ek, Gustav; Karlsson, Dennis Acta Materialia, Vol. 175 https://doi.org/10.1016/j.actamat.2019.06.002	journal	August 2019
Local order in high-entropy alloys and associated deuterides – a total scattering and Reverse Monte Carlo study Nygård, Magnus M.; Sławiński, Wojciech A.; Ek, Gustav Acta Materialia, Vol. 199 https://doi.org/10.1016/j.actamat.2020.08.045	journal	October 2020
The average and local structure of TiVCrNbD x ( x = 0 , 2.2 , 8 ) from total scattering and neutron spectroscopy Nygård, Magnus M.; Fjellvåg, Øystein S.; Sørby, Magnus H. Acta Materialia, Vol. 205 https://doi.org/10.1016/j.actamat.2020.116496	journal	February 2021
Machine learning assisted design of BCC high entropy alloys for room temperature hydrogen storage Halpren, Ethan; Yao, Xue; Chen, Zhi Wen Acta Materialia, Vol. 270 https://doi.org/10.1016/j.actamat.2024.119841	journal	May 2024
Hydrogen storage behaviours of high entropy alloys: A Review Somo, Thabang R.; Lototskyy, Mykhaylo V.; Yartys, Volodymyr A. Journal of Energy Storage, Vol. 73 https://doi.org/10.1016/j.est.2023.108969	journal	December 2023
Development of AB2-type TiZrCrMnFeCoV intermetallic high-entropy alloy for reversible room-temperature hydrogen storage Zhu, Yongyang; Yang, Xu-Sheng; Xu, Zheng-Long Journal of Energy Storage, Vol. 75 https://doi.org/10.1016/j.est.2023.109553	journal	January 2024
Hydrogen storage in high-entropy alloys with varying degree of local lattice strain Nygård, Magnus Moe; Ek, Gustav; Karlsson, Dennis International Journal of Hydrogen Energy, Vol. 44, Issue 55 https://doi.org/10.1016/j.ijhydene.2019.03.223	journal	November 2019
Notable hydrogen storage in Ti–Zr–V–Cr–Ni high entropy alloy Kumar, Abhishek; Yadav, Thakur Prasad; Mukhopadhyay, Nilay Krishna International Journal of Hydrogen Energy, Vol. 47, Issue 54 https://doi.org/10.1016/j.ijhydene.2022.05.107	journal	June 2022
The effect of 10 at.% Al addition on the hydrogen storage properties of the Ti0.33V0.33Nb0.33 multi-principal element alloy Pineda-Romero, Nayely; Witman, Matthew; Stavila, Vitalie Intermetallics, Vol. 146 https://doi.org/10.1016/j.intermet.2022.107590	journal	July 2022
Tuning the hydride stability of the TiVNb-based alloys by equimolar Cr/Al addition Ferreira, Tales; Pineda-Romero, Nayely; Botta, Walter José Intermetallics, Vol. 161 https://doi.org/10.1016/j.intermet.2023.107992	journal	October 2023
Materials for hydrogen-based energy storage – past, recent progress and future outlook Hirscher, Michael; Yartys, Volodymyr A.; Baricco, Marcello Journal of Alloys and Compounds, Vol. 827 https://doi.org/10.1016/j.jallcom.2019.153548	journal	June 2020
Hydrogen storage properties of the refractory Ti–V–Zr–Nb–Ta multi-principal element alloy Montero, Jorge; Ek, Gustav; Laversenne, Laetitia Journal of Alloys and Compounds, Vol. 835 https://doi.org/10.1016/j.jallcom.2020.155376	journal	September 2020
Tuning the hydrogen storage properties of Ti-V-Nb-Cr alloys by controlling the Cr/(TiVNb) ratio Strozi, R. B.; Silva, B. H.; Leiva, D. R. Journal of Alloys and Compounds, Vol. 932 https://doi.org/10.1016/j.jallcom.2022.167609	journal	January 2023
Reversible room temperature hydrogen storage in high-entropy alloy TiZrCrMnFeNi Edalati, Parisa; Floriano, Ricardo; Mohammadi, Abbas Scripta Materialia, Vol. 178 https://doi.org/10.1016/j.scriptamat.2019.12.009	journal	March 2020
Data-Driven Discovery and Synthesis of High Entropy Alloy Hydrides with Targeted Thermodynamic Stability Witman, Matthew; Ek, Gustav; Ling, Sanliang Chemistry of Materials, Vol. 33, Issue 11 https://doi.org/10.1021/acs.chemmater.1c00647	journal	April 2021
Structure and Hydrogenation Properties of a HfNbTiVZr High-Entropy Alloy Karlsson, Dennis; Ek, Gustav; Cedervall, Johan Inorganic Chemistry, Vol. 57, Issue 4 https://doi.org/10.1021/acs.inorgchem.7b03004	journal	February 2018
Phase Diagrams of Alloys and Their Hydrides via On-Lattice Graph Neural Networks and Limited Training Data Witman, Matthew D.; Bartelt, Norman C.; Ling, Sanliang The Journal of Physical Chemistry Letters, Vol. 15, Issue 5 https://doi.org/10.1021/acs.jpclett.3c03369	journal	February 2024
Extracting an Empirical Intermetallic Hydride Design Principle from Limited Data via Interpretable Machine Learning Witman, Matthew; Ling, Sanliang; Grant, David M. The Journal of Physical Chemistry Letters, Vol. 11, Issue 1 https://doi.org/10.1021/acs.jpclett.9b02971	journal	December 2019
Large Destabilization of (TiVNb)-Based Hydrides via (Al, Mo) Addition: Insights from Experiments and Data-Driven Models Pineda Romero, Nayely; Witman, Matthew; Harvey, Kim ACS Applied Energy Materials, Vol. 6, Issue 24 https://doi.org/10.1021/acsaem.3c02696	journal	December 2023
Elucidating Primary Degradation Mechanisms in High-Cycling-Capacity, Compositionally Tunable High-Entropy Hydrides Strozi, Renato Belli; Witman, Matthew; Stavila, Vitalie ACS Applied Materials & Interfaces, Vol. 15, Issue 32 https://doi.org/10.1021/acsami.3c05206	journal	August 2023
A general-purpose machine learning framework for predicting properties of inorganic materials Ward, Logan; Agrawal, Ankit; Choudhary, Alok npj Computational Materials, Vol. 2, Issue 1 https://doi.org/10.1038/npjcompumats.2016.28	journal	August 2016
Challenges to developing materials for the transport and storage of hydrogen Allendorf, Mark D.; Stavila, Vitalie; Snider, Jonathan L. Nature Chemistry, Vol. 14, Issue 11 https://doi.org/10.1038/s41557-022-01056-2	journal	October 2022
Review and outlook on high-entropy alloys for hydrogen storage Marques, Felipe; Balcerzak, Mateusz; Winkelmann, Frederik Energy & Environmental Science, Vol. 14, Issue 10 https://doi.org/10.1039/D1EE01543E	journal	January 2021
Towards Pareto optimal high entropy hydrides via data-driven materials discovery Witman, Matthew D.; Ling, Sanliang; Wadge, Matthew Journal of Materials Chemistry A, Vol. 11, Issue 29 https://doi.org/10.1039/D3TA02323K	journal	January 2023
Synthesis of small metallic Mg-based nanoparticles confined in porous carbon materials for hydrogen sorption Zlotea, Claudia; Chevalier-César, Clotaire; Léonel, Eric Faraday Discussions, Vol. 151 https://doi.org/10.1039/c0fd00016g	journal	January 2011
Inelastic neutron scattering evidence for anomalous H–H distances in metal hydrides Borgschulte, Andreas; Terreni, Jasmin; Billeter, Emanuel Proceedings of the National Academy of Sciences, Vol. 117, Issue 8 https://doi.org/10.1073/pnas.1912900117	journal	February 2020
PDFfit2 and PDFgui: computer programs for studying nanostructure in crystals Farrow, C. L.; Juhas, P.; Liu, J. W. Journal of Physics: Condensed Matter, Vol. 19, Issue 33 https://doi.org/10.1088/0953-8984/19/33/335219	journal	July 2007
PDFgetX3 : a rapid and highly automatable program for processing powder diffraction data into total scattering pair distribution functions Juhás, P.; Davis, T.; Farrow, C. L. Journal of Applied Crystallography, Vol. 46, Issue 2 https://doi.org/10.1107/S0021889813005190	journal	March 2013
The fast azimuthal integration Python library: pyFAI Ashiotis, Giannis; Deschildre, Aurore; Nawaz, Zubair Journal of Applied Crystallography, Vol. 48, Issue 2 https://doi.org/10.1107/S1600576715004306	journal	March 2015
ID15A at the ESRF – a beamline for high speed operando X-ray diffraction, diffraction tomography and total scattering Vaughan, Gavin B. M.; Baker, Robert; Barret, Raymond Journal of Synchrotron Radiation, Vol. 27, Issue 2 https://doi.org/10.1107/S1600577519016813	journal	January 2020
Band Structure Calculations for Metal Hydrogen Systems* Switendick, A. C. Zeitschrift für Physikalische Chemie, Vol. 117, Issue 117 https://doi.org/10.1524/zpch.1979.117.117.089	journal	January 1979
Compositional effects on the hydrogen storage properties in a series of refractory high entropy alloys Zlotea, Claudia; Bouzidi, Anis; Montero, Jorge Frontiers in Energy Research, Vol. 10 https://doi.org/10.3389/fenrg.2022.991447	journal	October 2022
Effect of Cr/Mn Addition in TiVNb on Hydrogen Sorption Properties: Thermodynamics and Phase Transition Study Bouzidi, Anis; Elkaim, Erik; Nassif, Vivian Hydrogen, Vol. 5, Issue 1 https://doi.org/10.3390/hydrogen5010008	journal	February 2024
Uncovering the Effect of Al Addition on the Hydrogen Storage Properties of the Ternary TiVNb Alloy Pineda-Romero, Nayely; Zlotea, Claudia Materials, Vol. 15, Issue 22 https://doi.org/10.3390/ma15227974	journal	November 2022

Similar Records

Large Destabilization of (TiVNb)-Based Hydrides via (Al, Mo) Addition: Insights from Experiments and Data-Driven Models

Journal Article · Tue Dec 12 19:00:00 EST 2023 · ACS Applied Energy Materials · OSTI ID:2311277

Elucidating Primary Degradation Mechanisms in High-Cycling-Capacity, Compositionally Tunable High-Entropy Hydrides

Journal Article · Thu Aug 03 20:00:00 EDT 2023 · ACS Applied Materials and Interfaces · OSTI ID:2311510

Revisit the VEC rule in high entropy alloys (HEAs) with high-throughput CALPHAD approach and its applications for material design-A case study with Al–Co–Cr–Fe–Ni system

Journal Article · Fri Apr 10 20:00:00 EDT 2020 · Acta Materialia · OSTI ID:1669890

Related Subjects

36 MATERIALS SCIENCE
Density functional theory
High entropy alloys
Hydrogen storage
Machine learning
Neutron diffraction
Pair distribution function
Synchrotron X-ray diffraction

Destabilizing high-capacity high entropy hydrides via earth abundant substitutions: From predictions to experimental validation

Citation Formats

References (39)

Similar Records

Related Subjects