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

  1. Jackson D. Scholten,
  2. Dr. Martin H. G. Prechtl,
  3. Prof. Dr. Jairton Dupont

Article first published online: 2 AUG 2010

DOI: 10.1002/cctc.201000119

Issue

ChemCatChem

ChemCatChem

Volume 2, Issue 10, pages 1265–1270, October 11, 2010

Additional Information

How to Cite

Scholten, J. D., Prechtl, M. H. G. and Dupont, J. (2010), Decomposition of Formic Acid Catalyzed by a Phosphine-Free Ruthenium Complex in a Task-Specific Ionic Liquid. ChemCatChem, 2: 1265–1270. doi: 10.1002/cctc.201000119

Author Information

  1. INCT-Catal., Laboratory of Molecular Catalysis, Institute of Chemistry, Universidade Federal do Rio Grande do Sul (UFRGS), Av. Bento Gonçalves 9500, Porto Alegre, RS, Brazil, CEP 90710-501 (Brazil), Fax: (+55) 51-3308-7304

Publication History

  1. Issue published online: 2 AUG 2010
  2. Article first published online: 2 AUG 2010
  3. Manuscript Revised: 12 MAY 2010
  4. Manuscript Received: 14 APR 2010

Funded by

  • CNPq
  • CAPES
  • Petrobras
  • Alexander-von-Humboldt Foundation

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Keywords:

  • dehydrogenation;
  • formic acid;
  • homogeneous catalysis;
  • ionic liquid;
  • ruthenium

Abstract

The dehydrogenation of formic acid is effectively catalyzed by the Ru complex [{RuCl2(p-cymene)}2] dissolved in the ionic liquid (IL) 1-(2-(diethylamino)ethyl)-3-methylimidazolium chloride at 80 °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)μ-(H)-μ-(HCO2)}]+ and [{Ru(p-cymene)}2{(H)μ-(Cl)μ-(HCO2)}]+, are identified by mass spectrometry. The presence of water in large amounts inhibits higher conversions. Finally, a remarkable catalytic activity is observed during recycles, indicating this system’s potential for hydrogen gas production.

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