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Full Paper
Selective Formic Acid Decomposition for High-Pressure Hydrogen Generation: A Mechanistic Study
Article first published online: 19 FEB 2009
DOI: 10.1002/chem.200801824
Copyright © 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Additional Information
How to Cite
Fellay, C., Yan, N., Dyson, P. J. and Laurenczy, G. (2009), Selective Formic Acid Decomposition for High-Pressure Hydrogen Generation: A Mechanistic Study. Chemistry - A European Journal, 15: 3752–3760. doi: 10.1002/chem.200801824
Publication History
- Issue published online: 26 MAR 2009
- Article first published online: 19 FEB 2009
- Manuscript Received: 3 SEP 2008
Funded by
- Swiss National Science Foundation
- EPFL
Keywords:
- formic acid;
- homogeneous catalysis;
- hydrogen storage;
- hydrogen;
- ruthenium
Graphical Abstract
A viable storage system for hydrogen based on selective formic acid decomposition into H2 and CO2 has been developed (see scheme). Continuous generation of H2 of very high purity, over a wide range of pressures and under mild conditions was achieved.
Abstract
A viable storage system for hydrogen based on selective formic acid decomposition into H2 and CO2 has been developed (see scheme). Continuous generation of H2 of very high purity, over a wide range of pressures and under mild conditions was achieved.
A homogenous catalytic system has been developed that efficiently and selectively decomposes formic acid into hydrogen and carbon dioxide. [Ru(H2O)6]2+, [Ru(H2O)6]3+ and RuCl3⋅x H2O are all excellent pre-catalysts in presence of TPPTS (TPPTS=meta-trisulfonated triphenylphosphine), the formic acid decomposition taking place in the aqueous phase, under mild conditions and over a large range of pressures. Optimisation of the reaction conditions is described together with a detailed mechanistic study leading to a tentative catalytic cycle. The performance of the catalytic system for continuous hydrogen generation is presented. Overall, the method proposed overcomes the limitations of other catalysts for the decomposition of formic acid making it a viable hydrogen-storage material.