Effect of Dithering on post-catalyst exhaust gas composition and on short time regeneration of deactivated PdO/Al2O3 catalysts under real engine conditions 2024-37-0002

Fossil fuels such as natural gas used in engines still play the most important role worldwide despite such measures as the German energy transition which however is also exacerbating climate change as a result of carbon dioxide emissions. One way of reducing carbon dioxide emissions is the choice of energy sources and with it a more favourable chemical composition. Natural gas, for instance, which consist mainly of methane, has the highest hydrogen to carbon ratio of all hydrocarbons, which means that carbon dioxide emissions can be reduced by up to 35% when replacing diesel with natural gas. Although natural gas engines show an overall low CO2 and pollutant emissions level, methane slip due to incomplete combustion occurs, causing methane emissions with a more than 20 higher global warming potential than CO2. Additionally, further tightening of emissions legislation is to be expected bringing methane emissions even more into focus making exhaust gas aftertreatment issues remain relevant. For lean gas applications, (Pd)-based catalysts turned out to convert CH4 most efficiently usually being supported by metal oxides such as aluminium oxide (Al2O3). Water (H2O) contained in the exhaust gas causes strong inhibition on Pd catalysts. In real exhaust gases, not only water vapour but also pollutants and sulphur-containing compounds such as hydrogen sulphide (H2S) or sulphur oxides (SOx) poisoning the catalytic converter. Rich pulses decomposing sulphur species adsorbed on Pd-Pt methane oxidation catalysts, enable efficient regeneration of heavily poisoned catalysts. A strategy similar to operation with rich pulses, but with a different motivation, is the use of high-frequency oscillations between lean and rich exhaust gas, so-called dithering, to improve pollutant conversion. A combination of a stoichiometric pulse while simultaneously dithering shows better results in recovery as well as emissions during regeneration than a pure rich pulse.