First principles investigations of complex hydrides AMH4 and A3MH6 (A=Li, Na, K, M=B, Al, Ga) as hydrogen storage systems

Dompablo, M. E. Arroyo y de; Ceder, Gerbrand

doi:10.1016/s0925-8388(03)00522-x

Cited by 91 publications

(62 citation statements)

References 20 publications

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“…In particular, we consider the series of simple metal hydrides LiH, NaH, MgH 2 , AlH 3 , and the binary metal hydrides Li 3 AlH 6 , Na 3 AlH 6 , LiAlH 4 , NaAlH 4 , and Mg͑AlH 4 ͒ 2 . 6,8,[23][24][25][26][27][28][29] The trends in the optical spectra and electronic structure are discussed and interpreted in terms of the structure and bonding of the materials. This paper is organized as follows.…”

Section: Introductionmentioning

confidence: 99%

Electronic structure and optical properties of lightweight metal hydrides

et al. 2007

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, using first-principles densityfunctional theory and GW calculations. All compounds are large gap insulators with GW single-particle band gaps varying from 3.5 eV in AlH 3 to 6.6 eV in LiAlH 4 . Despite considerable differences between the band structures and the band gaps of the various compounds, their optical responses are qualitatively similar. In most of the spectra the optical absorption rises sharply above 6 eV and has a strong peak around 8 eV. The quantitative differences in the optical spectra are interpreted in terms of the structure and the electronic structure of the compounds. In the simple hydrides the valence bands are dominated by the hydrogen atoms, whereas the conduction bands have mixed contributions from the hydrogens and the metal cations. The electronic structure of the aluminium compounds is determined mainly by aluminium hydride complexes and their mutual interactions.

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Section: Introductionmentioning

confidence: 99%

Electronic structure and optical properties of lightweight metal hydrides

et al. 2007

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“…[3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19] Typically, in these studies some flavor of density functional theory (DFT) 20-22 is used to calculate properties of the bulk solid or of the surface of the solid material. A wide range of DFT methodologies and implementations are currently in regular use for these predictive studies, with little attention being paid to any strengths or weaknesses of particular methods.…”

Section: Introductionmentioning

confidence: 99%

The Crystal Structure and Surface Energy of NaAlH₄: A Comparison of DFT Methodologies

Frankcombe

Løvvik

2005

J. Phys. Chem. B

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This paper presents a comparison of the bulk structure, cleavage energies, and local densities of states of solid NaAlH 4 calculated using several different density functional theory methodologies. Good agreement is obtained for the bulk crystal structure. Larger differences become apparent for the calculated surface energies and local densities of states. The (001) NaAlH 4 surface is clearly identified as the most stable surface, followed by the (112) and (101) surfaces, with the (100) surface being the least stable. We present an analysis of the local density of states of atoms in the exposed NaAlH 4 surface.

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“…14,18,23,24,25,26,27,28,29,30,31,32,33,34,35,36,37,38,39,40,41,42,43,44,45,46,47,48,49,50,51,52,53 In these calculations, the a priori knowledge of a compound's crystal structure is typically obtained from experiments where the system has already been structurally well characterized. By contrast, for the DFT calculations in this work, the crystal structure information is currently not available.…”

Section: Methodsmentioning

confidence: 99%

Prediction of a Ca(BH4)(NH2) quaternary hydrogen storage compound from first-principles calculations

2011

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We use a combination of density functional theory (DFT) calculations, and a Monte Carlo based crystal structure prediction tool, the Prototype Electrostatic Ground State (PEGS) method, to search for new hydrogen storage compounds in the Ca based mixed amide-borohydride quaternary system. We predict the existence of a new ordered quaternary compound, CaBNH 6 , whose stoichiometry comes from a 1:1 mixture of Ca(BH 4 ) 2 and Ca(NH 2 ) 2 . Our DFT calculations show that CaBNH 6 is ~12.5 kJ/mol Ca (at T = 0 K) lower in energy than the mixture of 1/2[Ca(BH 4 ) 2 + Ca(NH 2 ) 2 ]. DFT phonon calculations of vibrational thermodynamics show that this stability of CaBNH 6 [with respect to Ca(BH 4 ) 2 and Ca(NH 2 ) 2 ] persists to finite temperatures. The predicted crystal structure contains two formula units of CaBNH 6 . We have also performed a thermodynamic analysis of hydrogen decomposition of our predicted compound using the Grand Canonical Linear Programming (GCLP) method combined with a large database of DFT energies and vibrational thermodynamics. We find that the thermodynamically preferred decomposition reaction for CaBNH 6 involves formation of BN with a low decomposition enthalpy. Though the decomposition enthalpy is low, the kinetic behavior of CaBNH 6 decomposition is not yet known. We assert that further experimental investigation of this system is warranted to verify the existence of predicted quaternary compounds in this Ca-B-N-H system, as well as to elucidate their hydrogen release reaction pathways.3

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First principles investigations of complex hydrides AMH4 and A3MH6 (A=Li, Na, K, M=B, Al, Ga) as hydrogen storage systems

Cited by 91 publications

References 20 publications

Electronic structure and optical properties of lightweight metal hydrides

Electronic structure and optical properties of lightweight metal hydrides

The Crystal Structure and Surface Energy of NaAlH₄: A Comparison of DFT Methodologies

Prediction of a Ca(BH4)(NH2) quaternary hydrogen storage compound from first-principles calculations

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First principles investigations of complex hydrides AMH4 and A3MH6 (A=Li, Na, K, M=B, Al, Ga) as hydrogen storage systems

Cited by 91 publications

References 20 publications

Electronic structure and optical properties of lightweight metal hydrides

Electronic structure and optical properties of lightweight metal hydrides

The Crystal Structure and Surface Energy of NaAlH4: A Comparison of DFT Methodologies

Prediction of a Ca(BH4)(NH2) quaternary hydrogen storage compound from first-principles calculations

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The Crystal Structure and Surface Energy of NaAlH₄: A Comparison of DFT Methodologies