Ammonia Borane Hydrogen Release in Ionic Liquids
| Autor: | Daniel W. Himmelberger, Laif R. Alden, Martin E. Bluhm, Larry G. Sneddon |
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| Rok vydání: | 2009 |
| Předmět: | |
| Zdroj: | Inorganic Chemistry. 48:9883-9889 |
| ISSN: | 1520-510X 0020-1669 |
| DOI: | 10.1021/ic901560h |
| Popis: | The rate and extent of H(2)-release from ammonia borane (AB), a promising, high-capacity hydrogen storage material, was found to be enhanced in ionic-liquid solutions. For example, AB reactions in 1-butyl-3-methylimidazolium chloride (bmimCl) (50:50-wt %) exhibited no induction period and released 1.0 H(2)-equiv in 67 min and 2.2 H(2)-equiv in 330 min at 85 degrees C, whereas comparable solid-state AB reactions at 85 degrees C had a 180 min induction period and required 360 min to release approximately 0.8 H(2)-equiv, with the release of only another approximately 0.1 H(2)-equiv at longer times. Significant rate enhancements for the ionic-liquid mixtures were obtained with only moderate increases in temperature, with, for example, a 50:50-wt % AB/bmimCl mixture releasing 1.0 H(2)-equiv in 5 min and 2.2 H(2)-equiv in only 20 min at 110 degrees C. Increasing the AB/bmimCl ratio to 80:20 still gave enhanced H(2)-release rates compared to the solid-state, and produced a system that achieved 11.4 materials-weight percent H(2)-release. Solid-state and solution (11)B NMR studies of AB H(2)-release reactions in progress support a mechanistic pathway involving: (1) ionic-liquid promoted conversion of AB into its more reactive ionic diammoniate of diborane (DADB) form, (2) further intermolecular dehydrocoupling reactions between hydridic B-H hydrogens and protonic N-H hydrogens on DADB and/or AB to form neutral polyaminoborane polymers, and (3) polyaminoborane dehydrogenation to unsaturated cross-linked polyborazylene materials. |
| Databáze: | OpenAIRE |
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