Journal
CATALYSIS TODAY
Volume 360, Issue -, Pages 294-304Publisher
ELSEVIER
DOI: 10.1016/j.cattod.2020.02.022
Keywords
Natural gas; Three-way catalyst (TWC); Methane oxidation; CH4-NO cross-over point; Oxygen dosage; Lean/rich dithering
Funding
- U.S. Department of Energy [DE-AC05-00OR22725]
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The study evaluated the effects of oscillations in gas composition on the performance of a commercial Pd-based three-way catalyst for stoichiometric natural gas engines. The relationship between CH4 conversion and lambda change was explored, with the findings indicating that dynamic CH4 conversion is related to catalyst oxidation state. O-2 dosage was proposed as an effective descriptor of TWC dithering performance, and maps of dithering amplitude and O-2 dosage provide insights into optimal operation strategies for high CH4 and NO conversions.
The effects of oscillations in gas composition, known as lean/rich dithering, on the performance of a commercial Pd-based three-way catalyst (TWC) for stoichiometric natural gas (NG) engines were evaluated using synthetic exhaust flow reactor experiments. Under simulated NG exhaust conditions, NO conversion was intimately correlated to CH4 conversion at slightly fuel-rich operating conditions. CH4 conversion significantly varied with lambda (or O-2 concentration) and depended on the direction of the lambda change. The dynamic CH4 conversion is likely related to the change of catalyst oxidation state and structures of Pd active sites. The CH4-NO cross-over point was found at a rich-biased lambda rather than stoichiometry. Compared to static operation, catalyst performance was much higher under a realistic dithering condition. The impacts of dithering parameters including amplitude and frequency on CH4 and NO conversions were explored. O-2 dosage is proposed as an effective descriptor of the TWC dithering performance. In the O-2-dosage space, the performance of distinct dithering parameters collapse, helping to elucidate the fundamental influence of dithering parameters on TWC performance. With the help of O-2 dosage, an optimal operating window leading to high CH4 and NO conversions was identified. A higher dithering amplitude is required to keep the catalyst in a reduced state for higher CH4 and NO conversions, while an appropriate O-2 dosage that does not exceed the breakthrough OSC is necessary to avoid excess O-2 that results in NO slip. The dithering amplitude and O-2-dosage-metric maps provide a new method for studying dynamic TWC performance and identifying optimum operation strategies.
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