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Journal of Chemical Physics / Volume 131 / Issue 10 / ARTICLES / Condensed Phase Dynamics, Structure, and Thermodynamics: Spectroscopy, Reactions, and Relaxation

J. Chem. Phys. 131, 104506 (2009); doi:10.1063/1.3230973 (7 pages)

Thermal decomposition of ammonia borane at high pressures

Johanna Nylén, Toyoto Sato, Emmanuel Soignard, Jeffery L. Yarger, Emil Stoyanov, and Ulrich Häussermann

Department of Chemistry and Biochemistry, Arizona State University, P.O. Box 871604, Tempe, Arizona 85287-1604, USA

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(Received 20 May 2009; accepted 26 August 2009; published online 11 September 2009)

The effects of high pressure (up to 9 GPa) on the thermal decomposition of ammonia borane, BH3NH3, were studied in situ by Raman spectroscopy in a diamond anvil cell. In contrast with the three-step decomposition at ambient pressure, thermolysis under pressure releases almost the entire hydrogen content of the molecule in two distinct steps. The residual of the first decomposition is polymeric aminoborane, (BH2NH2)x, which is also observed at ambient pressure. The residual after the second decomposition is unique to high pressure. Presumably it corresponds to a precursor to hexagonal BN where macromolecular fragments of planar hexagon layers formed by B and N atoms are terminated by H atoms. Increasing pressure increases the temperature of both decomposition steps. Due to the increased first decomposition temperature it becomes possible to observe a new high pressure, high temperature phase of BH3NH3 which may represent melting.

© 2009 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. EXPERIMENTAL METHODS
  3. RESULTS AND DISCUSSION
    1. Raman spectrum of 1 at room temperature and its pressure dependency
    2. Temperature dependent study of 1 at 1 GPa
    3. Temperature dependent study of 1 at 5.5 GPa
    4. Temperature induced phase transition of 1 to 1′ at high pressure
    5. Ex situ analysis of residuals 2 and 3 from the thermal decomposition of 1 at 5.5 GPa
  4. CONCLUSIONS

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KEYWORDS and PACS

Keywords

high-pressure effects, hydrogen storage, organic compounds, pyrolysis, Raman spectra, spectrochemical analysis

PACS

  • 82.30.Lp

    Decomposition reactions (pyrolysis, dissociation, and fragmentation)

  • 82.40.Fp

    Shock wave initiated reactions, high-pressure chemistry

  • 62.50.-p

    High-pressure effects in solids and liquids

  • 84.60.-h

    Direct energy conversion and storage

  • 78.30.Jw

    Organic compounds, polymers

ARTICLE DATA

Permalink
http://link.aip.org/link/doi/10.1063/1.3230973

PUBLICATION DATA

ISSN:

0021-9606 (print)  
1089-7690 (online)

Publisher:

$abstract.society.value is a Member of CrossRef American Institute of Physics

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