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Materials 2015, 8(6), 3155-3167; doi:10.3390/ma8063155

A New Homogeneous Catalyst for the Dehydrogenation of Dimethylamine Borane Starting with Ruthenium(III) Acetylacetonate

Department of Chemistry, Middle East Technical University, 06800 Ankara, Turkey
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Author to whom correspondence should be addressed.
Academic Editor: Christof Schneider
Received: 21 April 2015 / Revised: 11 May 2015 / Accepted: 15 May 2015 / Published: 2 June 2015
(This article belongs to the Section Energy Materials)
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Abstract

The catalytic activity of ruthenium(III) acetylacetonate was investigated for the first time in the dehydrogenation of dimethylamine borane. During catalytic reaction, a new ruthenium(II) species is formed in situ from the reduction of ruthenium(III) and characterized using UV-Visible, Fourier transform infrared (FTIR), 1H NMR, and mass spectroscopy. The most likely structure suggested for the ruthenium(II) species is mer-[Ru(N2Me4)3(acac)H]. Mercury poisoning experiment indicates that the catalytic dehydrogenation of dimethylamine-borane is homogeneous catalysis. The kinetics of the catalytic dehydrogenation of dimethylamine borane starting with Ru(acac)3 were studied depending on the catalyst concentration, substrate concentration and temperature. The hydrogen generation was found to be first-order with respect to catalyst concentration and zero-order regarding the substrate concentration. Evaluation of the kinetic data provides the activation parameters for the dehydrogenation reaction: the activation energy Ea = 85 ± 2 kJ·mol−1, the enthalpy of activation ∆H# = 82 ± 2 kJ·mol−1 and the entropy of activation; ∆S# = −85 ± 5 J·mol−1·K−1. The ruthenium(II) catalyst formed from the reduction of ruthenium(III) acetylacetonate provides 1700 turnovers over 100 hours in hydrogen generation from the dehydrogenation of dimethylamine borane before deactivation at 60 °C. View Full-Text
Keywords: ruthenium; acetylacetonate; hydrogen generation; dimethylamine borane; dehydrogenation; homogeneous catalysis ruthenium; acetylacetonate; hydrogen generation; dimethylamine borane; dehydrogenation; homogeneous catalysis
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. (CC BY 4.0).

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MDPI and ACS Style

Barın, E.Ü.; Masjedi, M.; Özkar, S. A New Homogeneous Catalyst for the Dehydrogenation of Dimethylamine Borane Starting with Ruthenium(III) Acetylacetonate. Materials 2015, 8, 3155-3167.

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