Journal
SCIENCE
Volume 333, Issue 6050, Pages 1733-1736Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1206613
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Funding
- Mecklenburg-Vorpommern, Bundesministerium fur Bildung, Wissenschaft, Forschung und Technologie
- Deutsche Forschungsgemeinschaft
- Fonds der Chemischen Industrie (FCI)
- Ecole Polytechnique Federale de Lausanne
- Swiss National Science Foundation
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Hydrogen is one of the essential reactants in the chemical industry, though its generation from renewable sources and storage in a safe and reversible manner remain challenging. Formic acid (HCO(2)H or FA) is a promising source and storage material in this respect. Here, we present a highly active iron catalyst system for the liberation of H(2) from FA. Applying 0.005 mole percent of Fe(BF(4))(2)center dot 6H(2)O and tris[(2-diphenylphosphino)ethyl]phosphine [P(CH(2)CH(2)PPh(2))(3), PP(3)] to a solution of FA in environmentally benign propylene carbonate, with no further additives or base, affords turnover frequencies up to 9425 per hour and a turnover number of more than 92,000 at 80 degrees C. We used in situ nuclear magnetic resonance spectroscopy, kinetic studies, and density functional theory calculations to explain possible reaction mechanisms.
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