Abstract
Kinetics of formaldehyde oxidation over Pt-based catalytic converters at oxygen-rich conditions related to the exhaust of lean-burn natural gas engines is investigated experimentally and numerically. The numerical model proposed in this work is based on a thermodynamically consistent detailed surface reaction mechanism consisting of 30 elementary-like-steps among six gas-phase and ten surface species. The surface mechanism is evaluated by comparison of the results of the numerical simulation with the experimental measurements. The experimental data are derived from isothermal end-of-pipe tests over a powdered Pt–TiO2–SiO2 catalyst as well as spatially resolved concentration measurements conducted with a catalytic monolith sample over a wide range of temperature. The measurements were performed in a gas mixture of 80 ppm HCHO, 10 vol% O2, 12 vol% H2O and 6 vol% CO2 balanced with N2, containing a formaldehyde concentration typical in the exhaust of lean-burn gas engines. The simulations are based on a one-dimensional approach for the description of a packed-bed reactor and a two-dimensional model for the calculation of flow field and chemical reactions inside a single channel of a monolith.
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Acknowledgements
We very much appreciate fruitful discussions with Maria Casapu (KIT). We also gratefully thank the German Research Association for Combustion Engines e.V. (FVV) for funding the project “Formaldehyde” (Project-No. 1187) chaired by Heinrich Baas. The authors also thank Steinbeis GmbH & Co. KG für Technologietransfer (STZ 240 Reaktive Strömungen) for a cost free license of DETCHEM™.
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Torkashvand, B., Maier, L., Lott, P. et al. Formaldehyde Oxidation Over Platinum: On the Kinetics Relevant to Exhaust Conditions of Lean-Burn Natural Gas Engines. Top Catal 62, 206–213 (2019). https://doi.org/10.1007/s11244-018-1087-y
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DOI: https://doi.org/10.1007/s11244-018-1087-y