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Catalysts 2017, 7(11), 348; doi:10.3390/catal7110348

Dehydrogenation of Formic Acid over a Homogeneous Ru-TPPTS Catalyst: Unwanted CO Production and Its Successful Removal by PROX

1
Laboratory of Organometallic and Medical Chemistry, Group of Catalysis for Energy and Environment, École Polytechnique Fédérale de Lausanne, EPFL, CH-1015 Lausanne, Switzerland
2
Molecular Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, 5612 AZ Eindhoven, The Netherlands
3
GRT Operations SA, CH-1350 Orbe, Switzerland
*
Author to whom correspondence should be addressed.
Received: 26 October 2017 / Revised: 13 November 2017 / Accepted: 13 November 2017 / Published: 20 November 2017
(This article belongs to the Special Issue Homogeneous Catalysis and Mechanisms in Water and Biphasic Media)
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Abstract

Formic acid (FA) is considered as a potential durable energy carrier. It contains ~4.4 wt % of hydrogen (or 53 g/L) which can be catalytically released and converted to electricity using a proton exchange membrane (PEM) fuel cell. Although various catalysts have been reported to be very selective towards FA dehydrogenation (resulting in H2 and CO2), a side-production of CO and H2O (FA dehydration) should also be considered, because most PEM hydrogen fuel cells are poisoned by CO. In this research, a highly active aqueous catalytic system containing Ru(III) chloride and meta-trisulfonated triphenylphosphine (mTPPTS) as a ligand was applied for FA dehydrogenation in a continuous mode. CO concentration (8–70 ppm) in the resulting H2 + CO2 gas stream was measured using a wide range of reactor operating conditions. The CO concentration was found to be independent on the reactor temperature but increased with increasing FA feed. It was concluded that unwanted CO concentration in the H2 + CO2 gas stream was dependent on the current FA concentration in the reactor which was in turn dependent on the reaction design. Next, preferential oxidation (PROX) on a Pt/Al2O3 catalyst was applied to remove CO traces from the H2 + CO2 stream. It was demonstrated that CO concentration in the stream could be reduced to a level tolerable for PEM fuel cells (~3 ppm). View Full-Text
Keywords: formic acid; dehydrogenation; dehydration; ruthenium; carbon monoxide; preferential oxidation; PROX formic acid; dehydrogenation; dehydration; ruthenium; carbon monoxide; preferential oxidation; PROX
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. (CC BY 4.0).

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Henricks, V.; Yuranov, I.; Autissier, N.; Laurenczy, G. Dehydrogenation of Formic Acid over a Homogeneous Ru-TPPTS Catalyst: Unwanted CO Production and Its Successful Removal by PROX. Catalysts 2017, 7, 348.

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