Decomposition of Formic Acid Catalyzed by a Phosphine-Free Ruthenium Complex in a Task-Specific Ionic Liquid

J. D. Scholten, M. H. G. Prechtl, J. Dupont

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

Abstract

The dehydrogenation of formic acid is effectively catalyzed by the Ru complex [{RuCl(2)(p-cymene)}(2)] dissolved in the ionic liquid (IL) 1-(2-(diethylamino)ethyl)-3-methylimidazolium chloride at 80 degrees C without additional bases. This catalytic system gives TOF values of up to 1540 h(-1). Preliminary kinetic insights show formal reaction orders of 0.70(+/-0.15), 0.78(+/-0.03) and 2.00(+/-0.17) for the Ru catalyst, IL 1, and formic acid, respectively. The apparent activation energy of this process is estimated to be (69.1+/-7.6) kJ mol(-1). In addition, dimeric Ru hydride ionic species involved in the reaction, such as [{Ru(p-cymene)}(2){(H)mu-(H)-mu-(HCO(2))}](+) and [{Ru(p-cymene)}(2){(H)mu-(Cl)mu- (HCO(2)))](+), are identified by mass spectrometry. The presence of water in large amounts inhibits higher conversions. Finally, a remarkable catalytic activity is observed during recycles, inclicating this system's potential for hydrogen gas production.
OriginalsprogEngelsk
TidsskriftChemCatChem
Vol/bind2
Udgave nummer10
Sider (fra-til)1265-1270
Antal sider6
ISSN1867-3880
DOI
StatusUdgivet - 2010
Udgivet eksterntJa

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