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| Content Provider | World Health Organization (WHO)-Global Index Medicus |
|---|---|
| Author | Djukic, Jean-pierre Boulho, Cédric |
| Description | Author Affiliation: Boulho C ( Institut de Chimie UMR 7177 CNRS, 4 rue Blaise Pascal, 67070, Strasbourg Cedex, France.) |
| Abstract | The reactivity of ruthenacyclic compounds towards ammonia –borane's dehydrogenation was investigated by considering both hydrolytic and anhydrous conditions. The study shows that the highly soluble μ-chlorido dicarbonylruthenium( II) dimeric complex derived from 4- tert-butyl,2-( p-tolyl)pyridine promotes, with an activation energy E $_{a}$ of 22.8 kcal $mol^{−1},$ the complete hydrolytic dehydrogenation of $NH_{3}BH_{3}$ within minutes at ca. 40 °C. The release of 3 eq. of $H_{2}$ entails the formation of boric acid derivatives and the partly reversible protonolysis of the catalyst , which produces free 2-arylpyridine ligand and a series of isomers of “ Ru(CO) $_{2}(H)(Cl)$ ”. Under anhydrous conditions, hydrogen gas release was found to be slower and the dehydrogenation of $NH_{3}BH_{3}$ results in the formation of conventional amino – borane derivatives with concomitant protonolysis of the catalyst and release of isomers of “ Ru(CO) $_{2}(H)(Cl)$ ”. The mechanism of the protonolysis of the ruthenacycle was investigated with state-of-the-art DFT-D methods. It was found to proceed by the concerted direct attack of the catalyst by $NH_{3}BH_{3}$ leading either to the formation of a coordinatively unsaturated “ Ru(CO) $_{2}(H)(Cl)$ ” species. The key role of “ Ru(CO) $_{2}(H)(Cl)”$ species in the dehydrogenation of ammonia – borane was established by trapping and quenching experiments and inferred from a comparison of the catalytic activity of a series of dicarbonylruthenium( II) complexes. |
| ISSN | 14779226 |
| Issue Number | 38 |
| Journal | Dalton Trans. |
| Volume Number | 39 |
| e-ISSN | 13645447 |
| Language | English |
| Publisher | Royal Society of Chemistry |
| Publisher Date | 2010-10-14 |
| Publisher Place | Great Britain (UK) |
| Access Restriction | Subscribed |
| Subject Keyword | Chemistry |
| Content Type | Text |
| Resource Type | Article |
| Subject | Inorganic Chemistry |
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