Journal
COMBUSTION AND FLAME
Volume 211, Issue -, Pages 270-280Publisher
ELSEVIER SCIENCE INC
DOI: 10.1016/j.combustflame.2019.09.035
Keywords
Catalytic combustion; Syngas; Palladium catalyst; Surface kinetics; H-2-CO kinetic interactions; Coverage-dependent activation energies
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Funding
- Swiss National Science Foundation EPM fellowship [178619]
- US National Science Foundation [CHE160084]
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Kinetic interactions between H-2 and CO over PdO, a widely used catalyst in combustion systems, were studied experimentally and numerically. Global reaction parameters of H-2 and CO oxidation over PdO were extracted from wire microcalorimetry experiments at atmospheric pressure in the temperature range 380-800K, based on which a full catalytic reaction mechanism was developed. Comparison of ignition temperatures and heat release rates of different H-2/CO blends along with density functional theory (DFT) simulations revealed complex physicochemical coupling of the H-2 and CO catalytic oxidation pathways. The coupling evolves from an inhibiting effect of one fuel component onto the other due to their competition for surface adsorption sites and a direct repelling mechanism between the co-adsorbed H(s) and CO(s), to a promoting effect at sufficiently high temperatures caused by alleviated O(s) surface blocking. Implications of the H-2-CO kinetic coupling to the operation of practical power generation systems are outlined. (C) 2019 The Combustion Institute. Published by Elsevier Inc. All rights reserved.
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