Computational design of novel MAX phase alloys as potential hydrogen storage media combining first principles and cluster expansion methods

Das, Pritam; Thekkepat, Krishnamohan; Lee, Young-Su; Lee, Seung Cheol; Bhattacharjee, Satadeep

doi:10.1039/d2cp05587b

Cited by 8 publications

(4 citation statements)

References 34 publications

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“…H 2 molecules also primarily interact with tungsten atoms, with average adsorption energies of about -0.57 and -0.54 eV for the B-(010) and W-(101) surfaces, Figure 2. This number for W-(101) surface is very similar to the one for the Ti 2 AC (A = Al, Ti, Cr, Mn, Fe, Co, Ni, Cu, and Zn) 40 where it is equal to -0.40 eV.…”

Section: Resultssupporting

confidence: 65%

Theoretical Study of Adsorption Properties and CO Oxidation Reaction on Surfaces of Higher Tungsten Boride

Radina,

Baidyshev,

Chepkasov

et al. 2024

Preprint

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Most of the modern catalysts are based on precious metals and rear-earth elements making some reactions of organic synthesis economically insolvent. Density functional theory calculations here are used to describe several differently oriented surfaces of higher tungsten boride WB5-x, along with their catalytic activity for CO oxidation reaction. Based on our findings, WB5-x appears as efficient alternative catalyst for CO oxidation. Computed surface energies enable the use of Wulff construction to determine the equilibrium shape of WB5-x particles. It is found that (010) and (101) facets terminated by boron and tungsten, respectively, are the mainly exposed surfaces for which the various gas agents (СО, СO2, H2, N2, O2, NO, NO2, H2O, NH3, SO2) adsorption is evaluated, to reveal promising prospects of applications. CO oxidation on B-rich (010) and W-rich (101) surfaces is further explored in more detail by analyzing the charge redistribution during the adsorption of CO and O2 molecules. It is found that CO oxidation displays relatively low energy barriers. Implications of the present results, the WB5-x effects on the CO oxidation, and potential use in automotive, chemical, mining industries are discussed.

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Section: Resultssupporting

confidence: 65%

Theoretical Study of Adsorption Properties and CO Oxidation Reaction on Surfaces of Higher Tungsten Boride

Radina,

Baidyshev,

Chepkasov

et al. 2024

Preprint

View full text Add to dashboard Cite

show abstract

“…2 . The number for the W-(101) surface is comparable to that for the Ti 2 AC (A = Al, Ti, Cr, Mn, Fe, Co, Ni, Cu, and Zn) 54 where it is equal to −0.40 eV. Dissociation of the molecule can only occur at sites on the B-B bond.…”

Section: Resultsmentioning

confidence: 87%

Theoretical study of adsorption properties and CO oxidation reaction on surfaces of higher tungsten boride

Radina,

Baidyshev,

Chepkasov

et al. 2024

Sci Rep

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Most modern catalysts are based on precious metals and rear-earth elements, making some of organic synthesis reactions economically insolvent. Density functional theory calculations are used here to describe several differently oriented surfaces of the higher tungsten boride WB5-x, together with their catalytic activity for the CO oxidation reaction. Based on our findings, WB5-x appears to be an efficient alternative catalyst for CO oxidation. Calculated surface energies allow the use of the Wulff construction to determine the equilibrium shape of WB5-x particles. It is found that the (010) and (101) facets terminated by boron and tungsten, respectively, are the most exposed surfaces for which the adsorption of different gaseous agents (CO, CO2, H2, N2, O2, NO, NO2, H2O, NH3, SO2) is evaluated to reveal promising prospects for applications. CO oxidation on B-rich (010) and W-rich (101) surfaces is further investigated by analyzing the charge redistribution during the adsorption of CO and O2 molecules. It is found that CO oxidation has relatively low energy barriers. The implications of the present results, the effects of WB5-x on CO oxidation and potential application in the automotive, chemical, and mining industries are discussed.

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“…Its widespread popularity mainly stems from its ability to accurately predict complex energy landscapes in materials exhibiting significant configurational degrees of freedom while requiring only a relatively small (or at least tractable) number of expensive first-principles electronic structure calculations. The cluster expansion formalism has enabled first-principles accuracy calculations of temperature-composition phase diagrams, 15 activation barriers, 16,17 and even electronic excitations 18 across diverse materials applications, ranging from hydrogen storage 19 to battery 20 to electronic device materials. 21 Furthermore, along with the recent explosion of machine learning (ML) to accelerate various tasks in materials science, ML improvements on the original cluster expansion formalism have been proposed to ameliorate some of its shortcomings.…”

Section: Introductionmentioning

confidence: 99%

Phase diagrams of alloys and their hydrides via on-lattice graph neural networks and limited training data

Witman,

Bartelt,

Ling

et al. 2023

Preprint

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Efficient prediction of sampling-intensive thermodynamic properties in both closed and open systems is needed to evaluate material performance and permit high-throughput materials discovery for a diverse array of technology applications, from rational design of low-density high entropy alloys, to optimizing battery cathodes, to modulating hydrogen absorption equilibria in complex metals. To alleviate the prohibitive computational expense of high-throughput configurational sampling with density functional theory (DFT), surrogate modeling strategies like cluster expansion are many orders of magnitude more efficient, but can be difficult to construct in systems with high compositional complexity. We therefore employ minimal-complexity graph neural network models that accurately predict, and can even extrapolate to out-of-train-distribution, formation energies of DFT-relaxed structures from an ideal (unrelaxed) crystallographic representation. This enables the large-scale sampling necessary for various thermodynamic property predictions that may otherwise be intractable and can be achieved with small training datasets. Two exemplars, optimizing thermodynamic stability of low-density high entropy alloys and the modulating the plateau pressure of hydrogen in metal alloys, demonstrate the power of this approach, which will be extendable to a variety of materials discovery and modeling problems.

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Computational design of novel MAX phase alloys as potential hydrogen storage media combining first principles and cluster expansion methods

Abstract: Finding a suitable material for hydrogen storage at ambient atmospheric conditions is challenging for material scientists and chemists. In this work, using a first principles based cluster expansion approach, the...

Cited by 8 publications

References 34 publications

Theoretical Study of Adsorption Properties and CO Oxidation Reaction on Surfaces of Higher Tungsten Boride

Theoretical Study of Adsorption Properties and CO Oxidation Reaction on Surfaces of Higher Tungsten Boride

Theoretical study of adsorption properties and CO oxidation reaction on surfaces of higher tungsten boride

Phase diagrams of alloys and their hydrides via on-lattice graph neural networks and limited training data

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