Machine Learning-Guided Exploration of Ternary Metal Borohydrides

Cheng, Rong; Xue, Xuyan; Wang, C. Z.

doi:10.1021/acs.jpcc.4c00754

Machine Learning-Guided Exploration of Ternary Metal Borohydrides

Journal Article · Thu Apr 25 00:00:00 EDT 2024 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.4c00754· OSTI ID:2349085

^[1]; Xue, Xuyan ^[2]; ^[3]

Qingdao Univ., Shandong (China); Ames Lab., and Iowa State Univ., Ames, IA (United States)
Qingdao Univ., Shandong (China)
Ames Lab., and Iowa State Univ., Ames, IA (United States)

We employ deep machine learning (ML) combined with first-principles calculations to explore energetically favorable ternary metal borohydrides. Using La–B–H as a prototype system, we demonstrate that iteratively trained ML models can efficiently screen hundreds of thousands of hypothetical structures and accurately select a small fraction of promising structures and compositions for further studies by first-principles calculations. Such an ML-guided approach dramatically accelerates the pace of materials discovery. A number of new La–B–H ternary compounds with formation energies within 100 meV/atom above the known ternary convex hull are discovered, including a known stable La(BH₄)₃ phase. Moreover, by replacing La with Group 1, 2, 3, 13, and 14 elements in the four lowest-energy La–B–H structures from our ML-guided predictions, several low-energy X–B-H (X = Mg, Ca, Sr, Ba, Sc, Y, Ac, Al, Ga, In, Si, Ge, Sn, Pb) compounds are predicted.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 2349085

Report Number(s):: IS-J--11,323

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 18 Vol. 128; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (45)

Borohydride as Magnetic Superexchange Pathway in Late Lanthanide Borohydrides Wegner, Wojciech; van Leusen, Jan; Majewski, Jacek European Journal of Inorganic Chemistry, Vol. 2019, Issue 13 https://doi.org/10.1002/ejic.201801488	journal	March 2019
Metal hydrides for concentrating solar thermal power energy storage Sheppard, D. A.; Paskevicius, M.; Humphries, T. D. Applied Physics A, Vol. 122, Issue 4 https://doi.org/10.1007/s00339-016-9825-0	journal	March 2016
Borohydride complexes of rare earths, and their applications in various organic transformations Visseaux, Marc; Bonnet, Fanny Coordination Chemistry Reviews, Vol. 255, Issue 3-4 https://doi.org/10.1016/j.ccr.2010.09.016	journal	February 2011
Rare-earth metal complexes as catalysts for ring-opening polymerization of cyclic esters Lyubov, Dmitry M.; Tolpygin, Aleksey O.; Trifonov, Alexander A. Coordination Chemistry Reviews, Vol. 392 https://doi.org/10.1016/j.ccr.2019.04.013	journal	August 2019
CALYPSO: A method for crystal structure prediction Wang, Yanchao; Lv, Jian; Zhu, Li Computer Physics Communications, Vol. 183, Issue 10 https://doi.org/10.1016/j.cpc.2012.05.008	journal	October 2012
Application of hydrides in hydrogen storage and compression: Achievements, outlook and perspectives Bellosta von Colbe, Jose; Ares, Jose-Ramón; Barale, Jussara International Journal of Hydrogen Energy, Vol. 44, Issue 15 https://doi.org/10.1016/j.ijhydene.2019.01.104	journal	March 2019
Structures of the strontium and barium dodecahydro-closo-dodecaborates Her, Jae-Hyuk; Wu, Hui; Verdal, Nina Journal of Alloys and Compounds, Vol. 514 https://doi.org/10.1016/j.jallcom.2011.10.085	journal	February 2012
Structural and magnetocaloric properties of novel gadolinium borohydrides Schouwink, Pascal; Didelot, Emilie; Lee, Young-Su Journal of Alloys and Compounds, Vol. 664 https://doi.org/10.1016/j.jallcom.2015.12.182	journal	April 2016
New perspectives of functional metal borohydrides Grinderslev, Jakob B.; Amdisen, Mads B.; Skov, Lasse N. Journal of Alloys and Compounds, Vol. 896 https://doi.org/10.1016/j.jallcom.2021.163014	journal	March 2022
Probing the structure, stability and hydrogen storage properties of calcium dodecahydro-closo-dodecaborate Stavila, Vitalie; Her, Jae-Hyuk; Zhou, Wei Journal of Solid State Chemistry, Vol. 183, Issue 5 https://doi.org/10.1016/j.jssc.2010.03.026	journal	May 2010
Complex hydrides for hydrogen storage – new perspectives Ley, Morten B.; Jepsen, Lars H.; Lee, Young-Su Materials Today, Vol. 17, Issue 3 https://doi.org/10.1016/j.mattod.2014.02.013	journal	April 2014
Realizing high-Tc ambient-pressure superconductivity in hole-doped hydride Mg(BH4)2 Liu, Xiaohan; Zhang, Liying; Wang, Muyao Materials Today Physics, Vol. 40 https://doi.org/10.1016/j.mtphys.2023.101299	journal	January 2024
Solid-state electrolytes for beyond lithium-ion batteries: A review Aziam, Hasna; Larhrib, Badre; Hakim, Charifa Renewable and Sustainable Energy Reviews, Vol. 167 https://doi.org/10.1016/j.rser.2022.112694	journal	October 2022
Metal Borohydrides as Electrolytes for Solid-State Li, Na, Mg, and Ca Batteries: A First-Principles Study Lu, Ziheng; Ciucci, Francesco Chemistry of Materials, Vol. 29, Issue 21 https://doi.org/10.1021/acs.chemmater.7b03284	journal	October 2017
One Ion, Many Facets: Efficient, Structurally and Thermally Sensitive Luminescence of Eu²⁺ in Binary and Ternary Strontium Borohydride Chlorides Wylezich, Thomas; Sontakke, Atul D.; Castaing, Victor Chemistry of Materials, Vol. 31, Issue 21 https://doi.org/10.1021/acs.chemmater.9b03048	journal	October 2019
Machine Learning-Guided Discovery of Ternary Compounds Containing La, P, and Group 14 Elements Sun, Huaijun; Zhang, Chao; Xia, Weiyi Inorganic Chemistry, Vol. 61, Issue 42 https://doi.org/10.1021/acs.inorgchem.2c02431	journal	October 2022
From Metal Hydrides to Metal Borohydrides Richter, Bo; Grinderslev, Jakob B.; Møller, Kasper T. Inorganic Chemistry, Vol. 57, Issue 17 https://doi.org/10.1021/acs.inorgchem.8b01398	journal	August 2018
Crystal Structure of Li ₂ B ₁₂ H ₁₂ : a Possible Intermediate Species in the Decomposition of LiBH ₄ Her, Jae-Hyuk; Yousufuddin, Muhammed; Zhou, Wei Inorganic Chemistry, Vol. 47, Issue 21 https://doi.org/10.1021/ic801345h	journal	November 2008
NMR Confirmation for Formation of [B ₁₂ H ₁₂ ] ^2- Complexes during Hydrogen Desorption from Metal Borohydrides Hwang, Son-Jong; Bowman, Robert C.; Reiter, Joseph W. The Journal of Physical Chemistry C, Vol. 112, Issue 9 https://doi.org/10.1021/jp710894t	journal	March 2008
Role of Cation Size on the Structural Behavior of the Alkali-Metal Dodecahydro- closo -Dodecaborates Her, Jae-Hyuk; Zhou, Wei; Stavila, Vitalie The Journal of Physical Chemistry C, Vol. 113, Issue 26 https://doi.org/10.1021/jp904980m	journal	June 2009
Machine learning guided discovery of ternary compounds involving La and immiscible Co and Pb elements Wang, Renhai; Xia, Weiyi; Slade, Tyler J. npj Computational Materials, Vol. 8, Issue 1 https://doi.org/10.1038/s41524-022-00950-0	journal	December 2022
Sodium superionic conduction in Na ₂ B ₁₂ H ₁₂ Udovic, Terrence J.; Matsuo, Motoaki; Unemoto, Atsushi Chem. Commun., Vol. 50, Issue 28 https://doi.org/10.1039/C3CC49805K	journal	January 2014
Unparalleled lithium and sodium superionic conduction in solid electrolytes with large monovalent cage-like anions Tang, Wan Si; Unemoto, Atsushi; Zhou, Wei Energy & Environmental Science, Vol. 8, Issue 12 https://doi.org/10.1039/C5EE02941D	journal	January 2015
First-principles study of closo-dodecaborates M₂B₁₂H₁₂ (M = Li, Na, K) as solid-state electrolyte materials Akrouchi, A.; Benzidi, H.; Al-Shami, A. Physical Chemistry Chemical Physics, Vol. 23, Issue 47 https://doi.org/10.1039/D1CP03215A	journal	January 2021
A high-throughput exploration of magnetic materials by using structure predicting methods Arapan, S.; Nieves, P.; Cuesta-López, S. Journal of Applied Physics, Vol. 123, Issue 8 https://doi.org/10.1063/1.5004979	journal	February 2018
Accelerating the discovery of novel magnetic materials using machine learning–guided adaptive feedback Xia, Weiyi; Sakurai, Masahiro; Balasubramanian, Balamurugan Proceedings of the National Academy of Sciences, Vol. 119, Issue 47 https://doi.org/10.1073/pnas.2204485119	journal	November 2022
From DFT to machine learning: recent approaches to materials science–a review Schleder, Gabriel R.; Padilha, Antonio C. M.; Acosta, Carlos Mera Journal of Physics: Materials, Vol. 2, Issue 3 https://doi.org/10.1088/2515-7639/ab084b	journal	May 2019
High-throughput discovery of high-temperature conventional superconductors Shipley, Alice M.; Hutcheon, Michael J.; Needs, Richard J. Physical Review B, Vol. 104, Issue 5 https://doi.org/10.1103/PhysRevB.104.054501	journal	August 2021
Phonon-mediated high-temperature superconductivity in the ternary borohydride KB 2 H 8 under pressure near 12 GPa Gao, Miao; Yan, Xun-Wang; Lu, Zhong-Yi Physical Review B, Vol. 104, Issue 10 https://doi.org/10.1103/PhysRevB.104.L100504	journal	September 2021
Superconductivity in compressed ternary alkaline boron hydrides Li, Simin; Wang, Haiyan; Sun, Weiguo Physical Review B, Vol. 105, Issue 22 https://doi.org/10.1103/PhysRevB.105.224107	journal	June 2022
Metal borohydrides as ambient-pressure high- Tc superconductors Di Cataldo, Simone; Boeri, Lilia Physical Review B, Vol. 107, Issue 6 https://doi.org/10.1103/PhysRevB.107.L060501	journal	February 2023
Stabilizing a hydrogen-rich superconductor at 1 GPa by charge transfer modulated virtual high-pressure effect Gao, Miao; Guo, Peng-Jie; Yang, Huan-Cheng Physical Review B, Vol. 107, Issue 18 https://doi.org/10.1103/PhysRevB.107.L180501	journal	May 2023
Machine learning guided discovery of superconducting calcium borocarbides Zhang, Chao; Tang, Hui; Pan, Chen Physical Review B, Vol. 108, Issue 2 https://doi.org/10.1103/PhysRevB.108.024512	journal	July 2023
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Multivalent metal tetrahydroborides of Al, Sc, Y, Ti, and Zr Łodziana, Zbigniew Physical Review B, Vol. 81, Issue 14 https://doi.org/10.1103/PhysRevB.81.144108	journal	April 2010
Exploring the Structural Complexity of Intermetallic Compounds by an Adaptive Genetic Algorithm Zhao, X.; Nguyen, M. C.; Zhang, W. Y. Physical Review Letters, Vol. 112, Issue 4 https://doi.org/10.1103/PhysRevLett.112.045502	journal	January 2014
Crystal Graph Convolutional Neural Networks for an Accurate and Interpretable Prediction of Material Properties Xie, Tian; Grossman, Jeffrey C. Physical Review Letters, Vol. 120, Issue 14 https://doi.org/10.1103/PhysRevLett.120.145301	journal	April 2018
Molecular Geometry Optimization with a Genetic Algorithm Deaven, D. M.; Ho, K. M. Physical Review Letters, Vol. 75, Issue 2 https://doi.org/10.1103/PhysRevLett.75.288	journal	July 1995
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Formation Process of [B₁₂H₁₂]²⁻ from [BH₄]⁻ during the Dehydrogenation Reaction of Mg(BH₄)₂ Yan, Yigang; Li, Hai-Wen; Maekawa, Hideki MATERIALS TRANSACTIONS, Vol. 52, Issue 7 https://doi.org/10.2320/matertrans.MA201002	journal	January 2011
Complex Metal Hydrides for Hydrogen, Thermal and Electrochemical Energy Storage Møller, Kasper; Sheppard, Drew; Ravnsbæk, Dorthe Energies, Vol. 10, Issue 10 https://doi.org/10.3390/en10101645	journal	October 2017
Rare Earth Borohydrides—Crystal Structures and Thermal Properties Frommen, Christoph; Sørby, Magnus; Heere, Michael Energies, Vol. 10, Issue 12 https://doi.org/10.3390/en10122115	journal	December 2017
Metal Borohydrides beyond Groups I and II: A Review Suárez-Alcántara, Karina; Tena García, Juan Rogelio Materials, Vol. 14, Issue 10 https://doi.org/10.3390/ma14102561	journal	May 2021

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