First-principles prediction of thermodynamically reversible hydrogen storage reactions in the Li-Mg-Ca-B-H system

V. Ozolins*, E. H. Majzoub, Christopher M Wolverton

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

229 Scopus citations

Abstract

Introduction of economically viable hydrogen cars is hindered by the need to store large amounts of hydrogen. Metal borohydrides [LiBH 4, Mg(BH 4) 2, Ca(BH 4) 2] are attractive candidates for onboard storage because they contain high densities of hydrogen by weight and by volume. Using a set of recently developed theoretical first-principles methods, we predict currently unknown crystal structures and hydrogen storage reactions in the Li-Mg-Ca-B-H system. Hydrogen release from LiBH 4 and Mg(BH 4) 2 is predicted to proceed via intermediate Li 2B 12H 12 and MgB 12H 12 phases, while for Ca borohydride two competing reaction pathways (into CaB 6 and CaH 2, and into CaB 12H 12 and CaH 2) are found to have nearly equal free energies. We predict two new hydrogen storage reactions that are some of the most attractive among the presently known ones. They combine high gravimetric densities (8.4 and 7.7 wt % H 2) with low enthalpies [approximately 25 kJ/(mol H 2)] and are thermodynamically reversible at low pressures due to low vibrational entropies of the product phases containing the [B 12H 12] 2- anion.

Original languageEnglish (US)
Pages (from-to)230-237
Number of pages8
JournalJournal of the American Chemical Society
Volume131
Issue number1
DOIs
StatePublished - Jan 14 2009

ASJC Scopus subject areas

  • Chemistry(all)
  • Catalysis
  • Biochemistry
  • Colloid and Surface Chemistry

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