TY - GEN
T1 - Computational search for dehydrogenation pathways and destabilization schemes in complex metal hydrides
AU - Siegel, Donald J.
AU - Wolverton, Chris
AU - Ozolins, Vidvuds
PY - 2007
Y1 - 2007
N2 - First-principles modeling is rapidly emerging as a valuable tool in the search for new, high-density hydrides for use in mobile energy storage systems. These methods can be used to supplement experimental characterization techniques, and as a means to rapidly screen for new materials in order to guide subsequent experimental testing. We discuss how these characterization and materials-discovery capabilities have been used to explore the properties of two candidate hydrogen storage materials, Li4BN3H10 and LiBH4. For Li4BN3H10, calorimetry experiments have been unable to definitively determine the thermodynamics of hydrogen release, as the dehydrogenation reaction occurs simultaneously with one or more additional reactions. By screening ∼20 candidate reactions, we have identified the likely dehydrogenation pathways, evaluated their thermodynamics, and assessed the potential for reversibility. Recent experiments have shown that H2 desorption in LiBH4 can be facilitated by thermodynamic destabilization via mixing with MgH2. We explore whether further destabilization is possible by evaluating desorption free energies for several other LiBH4/metal-hydride combinations.
AB - First-principles modeling is rapidly emerging as a valuable tool in the search for new, high-density hydrides for use in mobile energy storage systems. These methods can be used to supplement experimental characterization techniques, and as a means to rapidly screen for new materials in order to guide subsequent experimental testing. We discuss how these characterization and materials-discovery capabilities have been used to explore the properties of two candidate hydrogen storage materials, Li4BN3H10 and LiBH4. For Li4BN3H10, calorimetry experiments have been unable to definitively determine the thermodynamics of hydrogen release, as the dehydrogenation reaction occurs simultaneously with one or more additional reactions. By screening ∼20 candidate reactions, we have identified the likely dehydrogenation pathways, evaluated their thermodynamics, and assessed the potential for reversibility. Recent experiments have shown that H2 desorption in LiBH4 can be facilitated by thermodynamic destabilization via mixing with MgH2. We explore whether further destabilization is possible by evaluating desorption free energies for several other LiBH4/metal-hydride combinations.
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M3 - Conference contribution
AN - SCOPUS:37349041041
SN - 084127438X
SN - 9780841274389
T3 - ACS National Meeting Book of Abstracts
BT - 233rd ACS National Meeting, Abstracts of Scientific Papers
T2 - 233rd ACS National Meeting
Y2 - 25 March 2007 through 29 March 2007
ER -