Towards Pareto optimal high entropy hydrides <i>via</i> data-driven materials discovery

Witman, Matthew; Ling, Sanliang; Wadge, Matthew D.; Bouzidi, Anis; Pineda-Romero, Nayely; Clulow, Rebecca; Ek, Gustav; Chames, Jeffery M.; Allendorf, Emily; Agarwal, Sapan; Allendorf, Mark D.; Walker, Gavin S.; Grant, David M.; Sahlberg, Martin; Zlotea, Claudia; Stavila, Vitalie

doi:10.1039/d3ta02323k

Cited by 12 publications

(11 citation statements)

References 57 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…, use only the composition to generate the materials descriptors), which employs tree-based regressors and interpretability analysis to both predict hydride thermodynamics and elucidate their physically informed design rules. Ref also provides the open-source repository to access the code and pretrained models for community use. The 0 and 25 atom % Cr samples had already been synthesized and measured at the publishing date of the v0.0.4 database and are therefore in the training data.…”

Section: Resultsmentioning

confidence: 99%

“…ML predictions in this work correspond to metal hydride capacity and thermodynamics models, trained on v0.0.4 of the ML-ready HydPARK database . Details on model development, validation, and demonstrated utility for metal hydride discovery are described in ref ; briefly, we use a compositional ML modeling approach ( i.e. , use only the composition to generate the materials descriptors), which employs tree-based regressors and interpretability analysis to both predict hydride thermodynamics and elucidate their physically informed design rules.…”

Section: Resultsmentioning

confidence: 99%

See 1 more Smart Citation

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

Strozi

Witman

Stavila

et al. 2023

ACS Appl. Mater. Interfaces

Self Cite

View full text Add to dashboard Cite

The hydrogen sorption properties of single-phase bcc (TiVNb)100–x Cr x alloys (x = 0–35) are reported. All alloys absorb hydrogen quickly at 25 °C, forming fcc hydrides with storage capacity depending on the Cr content. A thermodynamic destabilization of the fcc hydride is observed with increasing Cr concentration, which agrees well with previous compositional machine learning models for metal hydride thermodynamics. The steric effect or repulsive interactions between Cr–H might be responsible for this behavior. The cycling performances of the TiVNbCr alloy show an initial decrease in capacity, which cannot be explained by a structural change. Pair distribution function analysis of the total X-ray scattering on the first and last cycled hydrides demonstrated an average random fcc structure without lattice distortion at short-range order. If the as-cast alloy contains a very low density of defects, the first hydrogen absorption introduces dislocations and vacancies that cumulate into small vacancy clusters, as revealed by positron annihilation spectroscopy. Finally, the main reason for the capacity drop seems to be due to dislocations formed during cycling, while the presence of vacancy clusters might be related to the lattice relaxation. Having identified the major contribution to the capacity loss, compositional modifications to the TiVNbCr system can now be explored that minimize defect formation and maximize material cycling performance.

show abstract

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

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

Strozi

Witman

Stavila

et al. 2023

ACS Appl. Mater. Interfaces

Self Cite

View full text Add to dashboard Cite

show abstract

“…This class of materials is especially attractive due to immense opportunities for tuning hydrogen solubility and preferential absorption sites by altering chemical composition and crystal structure. 32–35 While some recently discovered HEAs demonstrate excellent hydrogen resistances, 36,37 others can be used for hydrogen storage applications. 34,38 It was shown that the mechanical properties of HEAs strongly depend on hydrogen concentration and the distribution of hydrogen atoms within a metal matrix.…”

Section: Introductionmentioning

confidence: 99%

“…32–35 While some recently discovered HEAs demonstrate excellent hydrogen resistances, 36,37 others can be used for hydrogen storage applications. 34,38 It was shown that the mechanical properties of HEAs strongly depend on hydrogen concentration and the distribution of hydrogen atoms within a metal matrix. Large combinatorial space of HEAs and intermetallic compounds makes systematic investigations of their composition rather challenging, and the optimal combination of elements in these materials for a chosen hydrogen technology cannot be easily identified.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Simple local environment descriptors for accurate prediction of hydrogen absorption and migration in metal alloys

Korostelev,

Wagner,

Klyukin

2023

J. Mater. Chem. A

View full text Add to dashboard Cite

show abstract

Thermodynamic and Kinetic Regulation for Mg‐Based Hydrogen Storage Materials: Challenges, Strategies, and Perspectives

Wang,

Li,

Wei

et al. 2024

Adv Funct Materials

View full text Add to dashboard Cite

Mg‐based hydrogen storage materials have drawn considerable attention as the solution for hydrogen storage and transportation due to their high hydrogen storage density, low cost, and high safety characteristics. However, their practical applications are hindered by the high dehydrogenation temperatures, low equilibrium pressure, and sluggish hydrogenation and dehydrogenation (de/hydrogenation) rates. These functionalities are typically determined by the thermodynamic and kinetic properties of de/hydrogenation reactions. This review comprehensively discusses how the compositeization, catalysts, alloying, and nanofabrication strategies can improve the thermodynamic and kinetic performances of Mg‐based hydrogen storage materials. Since the introduction of various additives leads the samples being a multiple‐phases and elements system, prediction methods of hydrogen storage properties are simultaneously introduced. In the last part of this review, the advantages and disadvantages of each approach are discussed and a summary of the emergence of new materials and potential strategies for realizing lower‐cost preparation, lower operation temperature, and long‐cycle properties is provided.

show abstract

Towards Pareto optimal high entropy hydrides via data-driven materials discovery

Abstract: Data-driven predictions of metal hydride thermodynamic properties elucidate the Pareto optimal front of high entropy alloy candidates for hydrogen storage.

Cited by 12 publications

References 57 publications

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

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

Simple local environment descriptors for accurate prediction of hydrogen absorption and migration in metal alloys

Thermodynamic and Kinetic Regulation for Mg‐Based Hydrogen Storage Materials: Challenges, Strategies, and Perspectives

Contact Info

Product

Resources

About