First principles screening of destabilized metal hydrides for high capacity H2 storage using scandium

Alapati, Sudhakar V.; Johnson, J. Karl; Sholl, David S.

doi:10.1016/j.jallcom.2006.10.166

Cited by 38 publications

(65 citation statements)

References 23 publications

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“…Among all of the conditions that a candidate hydrogen storage material should satisfy, one of the most difficult to achieve is reversible hydrogen storage at an appropriate temperature [4]. A hydrogen storage candidate should be able to reversibly store and release H 2 at 323-423 K at a pressure of 1-100 bars [5][6][7][8][9].…”

Section: Introductionmentioning

confidence: 99%

Prediction of thermodynamically reversible hydrogen storage reactions utilizing Ca–M(M = Li, Na, K)–B–H systems: a first-principles study

Guo

Ren

et al. 2013

J Mol Model

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Calcium borohydride is a potential candidate for onboard hydrogen storage because it has a high gravimetric capacity (11.5 wt.%) and a high volumetric hydrogen content (∼130 kg m(-3)). Unfortunately, calcium borohydride suffers from the drawback of having very strongly bound hydrogen. In this study, Ca(BH₄)₂ was predicted to form a destabilized system when it was mixed with LiBH₄, NaBH₄, or KBH₄. The release of hydrogen from Ca(BH₄)₂ was predicted to proceed via two competing reaction pathways (leading to CaB₆ and CaH₂ or CaB₁₂H₁₂ and CaH₂) that were found to have almost equal free energies. Using a set of recently developed theoretical methods derived from first principles, we predicted five new hydrogen storage reactions that are among the most attractive of those presently known. These combine high gravimetric densities (>6.0 wt.% H₂) with have low enthalpies [approximately 35 kJ/(mol(-1) H₂)] and are thermodynamically reversible at low pressure within the target window for onboard storage that is actively being considered for hydrogen storage applications. Thus, the first-principles theoretical design of new materials for energy storage in future research appears to be possible.

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Section: Introductionmentioning

confidence: 99%

Prediction of thermodynamically reversible hydrogen storage reactions utilizing Ca–M(M = Li, Na, K)–B–H systems: a first-principles study

Guo

Ren

et al. 2013

J Mol Model

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“…First-principles calculations have been shown to yield reaction free energies that are accurate within AE10 kJ mol À1 H 2 -a level that is adequate for screening large numbers of potentially interesting reactions. [17][18][19] Several earlier efforts have been made to categorize metal hydride mixtures using thermodynamic calculations based on density functional theory (DFT) calculations and a database of crystal compounds. [20][21][22][23][24][25] The methodological basis of these calculations is the grand canonical linear programming method introduced by Ozolins and co-workers.…”

Section: Introductionmentioning

confidence: 99%

Large-scale screening of metal hydrides for hydrogen storage from first-principles calculations based on equilibrium reaction thermodynamics

Kim

Kulkarni

Johnson

et al. 2011

Phys. Chem. Chem. Phys.

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Systematic thermodynamics calculations based on density functional theory-calculated energies for crystalline solids have been a useful complement to experimental studies of hydrogen storage in metal hydrides. We report the most comprehensive set of thermodynamics calculations for mixtures of light metal hydrides to date by performing grand canonical linear programming screening on a database of 359 compounds, including 147 compounds not previously examined by us. This database is used to categorize the reaction thermodynamics of all mixtures containing any four non-H elements among Al, B, C, Ca, K, Li, Mg, N, Na, Sc, Si, Ti, and V. Reactions are categorized according to the amount of H(2) that is released and the reaction's enthalpy. This approach identifies 74 distinct single step reactions having that a storage capacity >6 wt.% and zero temperature heats of reaction 15 ≤ΔU(0)≤ 75 kJ mol(-1) H(2). Many of these reactions, however, are likely to be problematic experimentally because of the role of refractory compounds, B(12)H(12)-containing compounds, or carbon. The single most promising reaction identified in this way involves LiNH(2)/LiH/KBH(4), storing 7.48 wt.% H(2) and having ΔU(0) = 43.6 kJ mol(-1) H(2). We also examined the complete range of reaction mixtures to identify multi-step reactions with useful properties; this yielded 23 multi-step reactions of potential interest.

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“…It is worth pointing out that the individual compounds are not destabilized but rather the overall reaction is destabilized by decomposing to a more stable alloy thus requiring less energy for decomposition. During the MHCoE, many new destabilized hydride material systems were explored both computationally [46,47,[55][56][57][58][59] Vajo et al [16,67] demonstrated a remarkable "destabilized" material system in LiBH 4 /Mg 2 NiH 4 . The reaction revealed many new features contradictory to the individual complex compounds such as full reversibility, low enthalpy and entropy and reaction through a unique low-temperature kinetic pathway.…”

Section: Destabilized Hydridesmentioning

confidence: 99%

“…First-principles methods such as Prototype Electrostatic Ground State [74], were developed and used to predict new crystalline materials and their thermodynamic properties, as well as provide validation of experimental results. It is estimated that computational methods allowed such rapid screening that over twenty million reactions were assessed for favorable hydrogen release properties over the duration of the Center [23,25,46,47,[55][56][57]59,[74][75][76]. For example, during the course of the Center interest had turned to Ca(BH 4 ) 2 as a potential high capacity material; however the true structure of the complex hydride was unknown.…”

Section: Computational Guidance Of Metal Hydride Developmentmentioning

confidence: 99%

Moderate Temperature Dense Phase Hydrogen Storage Materials within the US Department of Energy (DOE) H2 Storage Program: Trends toward Future Development

McWhorter

O’Malley

Adams³

et al. 2012

Crystals

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Hydrogen has many positive attributes that make it a viable choice to augment the current portfolio of combustion-based fuels, especially when considering reducing pollution and greenhouse gas (GHG) emissions. However, conventional methods of storing H 2 via high-pressure or liquid H 2 do not provide long-term economic solutions for many applications, especially emerging applications such as man-portable or stationary power. Hydrogen storage in materials has the potential to meet the performance and cost demands, however, further developments are needed to address the thermodynamics and kinetics of H 2 uptake and release. Therefore, the US Department of Energy (DOE) initiated three Centers of Excellence focused on developing H 2 storage materials that could meet the stringent performance requirements for on-board vehicular applications. In this review, we have summarized the developments that occurred as a result of the efforts of the Metal

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First principles screening of destabilized metal hydrides for high capacity H2 storage using scandium

Cited by 38 publications

References 23 publications

Prediction of thermodynamically reversible hydrogen storage reactions utilizing Ca–M(M = Li, Na, K)–B–H systems: a first-principles study

Prediction of thermodynamically reversible hydrogen storage reactions utilizing Ca–M(M = Li, Na, K)–B–H systems: a first-principles study

Large-scale screening of metal hydrides for hydrogen storage from first-principles calculations based on equilibrium reaction thermodynamics

Moderate Temperature Dense Phase Hydrogen Storage Materials within the US Department of Energy (DOE) H2 Storage Program: Trends toward Future Development

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