First-principles prediction of high-capacity, thermodynamically reversible hydrogen storage reactions based on (NH4)2B 12H12

Wenhao Q. Sun*, C. Wolverton, A. R. Akbarzadeh, V. Ozolins

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

12 Scopus citations

Abstract

We use a combination of first-principles density functional calculations along with the recently developed grand canonical linear programing method to predict a novel, high-capacity hydrogen storage reaction with thermodynamics suitable for near-ambient reversible storage. Unlike the vast majority of previously proposed complex hydrides, which typically rely on a hydrogen-containing anionic unit, our reaction is based on an ammonium-containing hydride, (NH4)2B12H 12, which contains increased storage capacity due to both anionic and cationic hydrogen-containing complexes. The predicted decomposition of this hydride is a two-step reaction sequence: (NH4)2B 12H12 → 2BN + 1/2B20H16 + 6H2 →2BN + 10B + 10H2, which possesses a theoretical gravimetric capacity of 11.3 wt% H2, a single-crystal volumetric density of 52 g H2/L, and T=300 K reaction enthalpies of 17 and 33 kJ/mol H2, respectively, which are well-suited for near-ambient reversible storage. The combination of these three attributes in a single material makes this decomposition reaction sequence highly promising.

Original languageEnglish (US)
Article number064112
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume83
Issue number6
DOIs
StatePublished - Feb 11 2011

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics

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