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

Pineda Romero, Nayely; Witman, Matthew David; Harvey, Kimberlyann Rose; Stavila, Vitalie; Nassif, Vivian; Elkaïm, Erik; Zlotea, Claudia

doi:10.1021/acsaem.3c02696

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

Journal Article · 12 December 2023 · ACS Applied Energy Materials

DOI: https://doi.org/10.1021/acsaem.3c02696 · OSTI ID:2311277

Pineda Romero, Nayely ^[1];

^[2]; Harvey, Kimberlyann Rose ^[2];

^[2]; Nassif, Vivian ^[3]; Elkaïm, Erik ^[4];

^[1]

Paris-East Créteil University (France); Centre National de la Recherche Scientifique (CNRS) (France)
Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Univ. of Grenoble Alpes, Grenoble (France); Centre National de la Recherche Scientifique (CNRS) (France)
Synchrotron SOLEIL, Gif-sur-Yvette (France)

High-entropy alloys (HEAs) represent an interesting alloying strategy that can yield exceptional performance properties needed across a variety of technology applications, including hydrogen storage. Examples include ultrahigh volumetric capacity materials (BCC alloys → FCC dihydrides) with improved thermodynamics relative to conventional high-capacity metal hydrides (like MgH₂), but still further destabilization is needed to reduce operating temperature and increase system-level capacity. Here, in this work, we demonstrate efficient hydride destabilization strategies by synthesizing two new Al_0.05(TiVNb)_0.95–xMo_x (x = 0.05, 0.10) compositions. We specifically evaluate the effect of molybdenum (Mo) addition on the phase structure, microstructure, hydrogen absorption, and desorption properties. Both alloys crystallize in a bcc structure with decreasing lattice parameters as the Mo content increases. The alloys can rapidly absorb hydrogen at 25 °C with capacities of 1.78 H/M (2.79 wt %) and 1.79 H/M (2.75 wt %) with increasing Mo content. Pressure-composition isotherms suggest a two-step reaction for hydrogen absorption to a final fcc dihydride phase. The experiments demonstrate that increasing Mo content results in a significant hydride destabilization, which is consistent with predictions from a gradient boosting tree data-driven model for metal hydride thermodynamics. Furthermore, improved desorption properties with increasing Mo content and reversibility were observed by in situ synchrotron X-ray diffraction, in situ neutron diffraction, and thermal desorption spectroscopy.

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

Sponsoring Organization:: 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); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: NA0003525

OSTI ID:: 2311277

Report Number(s):: SAND--2024-00013J

Journal Information:: ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 24 Vol. 6; ISSN 2574-0962

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
high-entropy alloys
hydrogen absorption/desorption
in situ synchrotron X-ray diffraction
in situ neutron diffraction
thermodynamics

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

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