Mechanisms for delivering hydrogen from ammonia-borane via protons, hydrides, and a dative bond
Abstract/Contents
- Abstract
- The hydrogen economy is a hypothetical replacement for the world's reliance on fossil fuels. Concerns over carbon dioxide and global warming have driven research into creating reliable systems to utilize hydrogen as a vehicular fuel. Because molecular hydrogen is a gas, storage at practical densities is a major problem for its utilization. One highly promising material for hydrogen storage is ammonia-borane (AB), or NH3BH3. AB has a high weight percent hydrogen (~20%) and its protic (N-H) and hydridic (B-H) hydrogens appear ripe for dehydrogenation. However, reversible release of H2 from AB requires fine control over dehydrogenation mechanisms. Using ab initio simulations, we elucidate the fundamental mechanisms involved in removing hydrogen from AB. Herein, we investigate mechanisms for the dehydrogenation of AB by homogeneous catalysis and thermolysis. We show that unexpected active catalysts and experimentally unobservable intermediates are key aspects of this chemistry. Furthermore, the effects of solvent and dynamics are vital to understanding product distributions. Finally, two-hydrogen transfer is highlighted as a fascinating chemistry involving the simultaneous transfer of protic and hydridic hydrogen.
Description
| Type of resource | text |
|---|---|
| Form | electronic; electronic resource; remote |
| Extent | 1 online resource. |
| Publication date | 2010 |
| Issuance | monographic |
| Language | English |
Creators/Contributors
| Associated with | Zimmerman, Paul Martin |
|---|---|
| Associated with | Stanford University, Department of Chemical Engineering |
| Primary advisor | Jaramillo, Thomas Francisco |
| Primary advisor | Musgrave, Charles |
| Thesis advisor | Jaramillo, Thomas Francisco |
| Thesis advisor | Musgrave, Charles |
| Thesis advisor | Waymouth, Robert M |
| Advisor | Waymouth, Robert M |
Subjects
| Genre | Theses |
|---|
Bibliographic information
| Statement of responsibility | Paul Martin Zimmerman. |
|---|---|
| Note | Submitted to the Department of Chemical Engineering. |
| Thesis | Thesis (Ph. D.)--Stanford University, 2010. |
| Location | electronic resource |
Access conditions
- Copyright
- © 2010 by Paul Martin Zimmerman
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