First-principles study of point defects under varied chemical potentials in Li<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mrow /><mml:mn>4</mml:mn></mml:msub></mml:math>BN<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mrow /><mml:mn>3</mml:mn></mml:msub></mml:math>H<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mrow /><mml:mn>10</mml:mn></mml:msub></mml:math>

Farrell, D. E.; Wolverton, Chris

doi:10.1103/physrevb.85.174102

Cited by 10 publications

(14 citation statements)

References 63 publications

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“…H − i , on the other hand, is found situated in a void surrounded by (Li) + units. Like H + i , H 0 i also forms an NH 3 unit, which is in agreement with the configuration reported by Farrell and Wolverton, 18 and is lower in energy than that reported previously by us where the neutral H atom loosely bonds to a (BH 4 ) − unit. 17 However, even with this low-energy configuration, H 0 i is never the most stable charge state of hydrogen interstitials.…”

Section: Resultssupporting

confidence: 91%

“…For comparison, Farrell and Wolverton reported µ int e ∼2.5−3.2 eV under different sets of the atomic chemical potentials. 18 It emerges from our results that some native defects in Li 4 BN 3 H 10 can have very low formation energies. With our choice of the atomic chemical potentials, V 0 NH (a complex of V + NH2 and H − i ) and V 0 BH3 (a complex of V + BH4 and H − i ) even have a zero formation energy.…”

Section: Discussionmentioning

confidence: 66%

“…Farrell and Wolverton, on the other hand, took into account only the "potential alignment" term, reported to be of ∼0.2−0.9 eV depending specific defects. 18 The chemical potentials µ i are variables and can be chosen to represent experimental situations. For defect calculations in Li 4 BN 3 H 10 , from Eq.…”

Section: Methodsmentioning

confidence: 99%

See 2 more Smart Citations

The role of native defects in the transport of charge and mass and the decomposition of Li$_{4}$BN$_{3}$H$_{10}$

Hoang,

Janotti,

Van de Walle

2014

Preprint

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Section: Resultssupporting

confidence: 91%

Section: Discussionmentioning

confidence: 66%

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The role of native defects in the transport of charge and mass and the decomposition of Li$_{4}$BN$_{3}$H$_{10}$

Hoang,

Janotti,

Van de Walle

2014

Preprint

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“…A number of computational studies have also shown that vacancy defects are relatively abundant under dehydrogenation conditions and may thus mediate mass transport in the bulk of the hydrides. The important role of hydrogen vacancies for dehydrogenation in hydrides was confirmed in studies on AlH 3 , Li amide (LiNH 2 ), Li imide (Li 2 NH), LiBH 4 and Li 4 BN 3 H 10 [10,11,12,13,14]. It was also shown that transition metal additives in MgH 2 lower the formation energy of native defects and increase their concentration resulting in higher hydrogen desorption rates [15,16,17,18].…”

Section: Introductionmentioning

confidence: 78%

Point-defect kinetics in α- and γ-MgH2

Sander

Ismer

Walle

2016

International Journal of Hydrogen Energy

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The kinetics of hydrogen desorption from storage materials in principle depend on the crystalline phase of the material. In MgH 2 , desorption rates may be higher in the crystalline γ phase compared to the equilibrium bulk α phase. It has been suggested [R. A. Varin, T. Czujko, Z. Wronski, Nanotechnol., 17 (15) (2006) 3856-3865] that this effect is responsible for enhanced desorption from ball-milled MgH 2 , since smaller particles contain a higher proportion of the metastable γ phase. We investigate hydrogen transport kinetics in these phases of MgH 2 by using first-principles calculations based on density functional theory. Imposing charge neutrality, we find that the formation energy of hydrogen vacancies in γ-MgH 2 is smaller by 0.032 eV compared to α-MgH 2. Our calculations of migration barriers show that the only relevant point defect for mass transport in both crystal structures is the positively charged hydrogen vacancy, and that its lowest migration barrier in γ-MgH 2 is 0.02 eV lower than in α-MgH 2. We conclude that hydrogen vacancies exist in higher concentrations and are also more mobile in the γ phase than in the α phase, thus explaining the faster dehydrogenation kinetics of γ-MgH 2 .

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“…GCLP is a physical model for determining the thermodynamically preferred behavior of a system with very complicated chemistry without relying on chemical intuition or inefficient brute force methods 52. Subsequently this method has been used for identifying reactions and generating ground state phase diagrams51, 53–58 Here we use GCLP in conjunction with DFT to explore the phase diagrams of transition metal stannides, phosphides and silicides. We found 291 known compounds from the ICSD, from which there are 24,388,710 possible conversion reactions, but the vast majority of these reactions are thermodynamically unstable.…”

Section: Introductionmentioning

confidence: 99%

High‐Throughput Computational Screening of New Li‐Ion Battery Anode Materials

Kirklin

Meredig

Wolverton

2012

Advanced Energy Materials

182

141

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We use density functional theory (DFT) in conjunction with grand canonical linear programming (GCLP), a powerful automated tool for analyzing ground state thermodynamics, to exhaustively enumerate the 515 thermodynamically stable lithiation reactions of transition metal silicides, stannides and phosphides, and compute cell potential, volume expansion, and capacity for each. These reactions comprise an exhaustive list of all possible thermodynamically stable ternary conversion reactions for these transition metal compounds. The reactions are calculated based on a library DFT energies of 291 compounds, including all transition metal silicides, phosphides and stannides found in the Inorganic Crystal Structure Database (ICSD). We screen our computational database for the most appealing anode properties based on gravimetric capacity, volumetric capacity, cell potential, and volume expansion when compared with graphitic carbon anodes. This high‐throughput computational approach points towards several promising anode compositions with properties significantly superior to graphitic carbon, including CoSi2, TiP and NiSi2.

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First-principles study of point defects under varied chemical potentials in Li4BN3H10

Cited by 10 publications

References 63 publications

The role of native defects in the transport of charge and mass and the decomposition of Li$_{4}$BN$_{3}$H$_{10}$

The role of native defects in the transport of charge and mass and the decomposition of Li$_{4}$BN$_{3}$H$_{10}$

Point-defect kinetics in α- and γ-MgH2

High‐Throughput Computational Screening of New Li‐Ion Battery Anode Materials

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