Hydrogen Production by Selective Dehydrogenation of HCOOH Catalyzed by Ru-Biaryl Sulfonated Phosphines in Aqueous Solution

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• 作者：Antonella Guerriero ; Herv茅 Bricout ; Katerina Sordakis ; Maurizio Peruzzini ; Eric Monflier ; Fr茅d茅ric Hapiot ; G谩bor Laurenczy ; Luca Gonsalvi
• 刊名：ACS Catalysis
• 出版年：2014
• 出版时间：September 5, 2014
• 年：2014
• 卷：4
• 期：9
• 页码：3002-3012
• 全文大小：435K
• ISSN：2155-5435

文摘

The selective dehydrogenation of aqueous solutions of HCOOH/HCOONa to H₂ and CO₂ gas mixtures has been investigated using RuCl₃路3H₂O as a homogeneous catalyst precursor in the presence of different monoaryl-biaryl or alkyl-biaryl phosphines and aryl diphosphines bearing sulfonated groups. All catalytic systems were used in water without any additives and proved to be active at 90 掳C, giving high conversions and good TOF values. As an alternative Ru(II) metal precursor, the known dimer [Ru(畏⁶-C₆H₆)Cl₂]₂ was also tested as in situ catalyst with selected phosphines as well as an isolated Ru(II)-catalyst with one of them. By using high-pressure NMR (HPNMR) techniques, indications on the nature of the active species involved in the catalytic cycles were obtained.

Keywords:

aqueous-phase catalysis; formic acid; hydrogen generation; ruthenium; sulfonated phosphines