Applied Catalysis B: Environmental, Vol.182, 550-561, 2016
Studies on the influence of H2S and SO2 on the activity of a PdO/Al2O3 catalyst for removal of oxygen by total oxidation of (bio-)methane at very low O-2:CH4 ratios
This work focuses on the deactivation and in-situ regeneration effects of a commercial PdO/Al2O3 catalyst for removal of oxygen by oxidation of CH4 at low O-2:CH4 ratios when hydrogen sulfide and sulfur dioxide are applied to the gas stream. The experimental work is carried out at an operating temperature range of 200 degrees C< T <300 degrees C, atmospheric pressure and H2S/SO2 contents of <100 ppmv. SO2 and H2S show a different behavior in the examined range of operating conditions. Due to the low operating temperatures and low oxygen contents applied in this work, it was possible to identify an intermediate species, presumably PdSO3, with an increased activity for the oxidation of methane. This stands in contrast to the literature, where SO2 is typically seen to cause catalyst deactivation. Based on the experimental results, a reaction scheme was derived and kinetic measurements for each of the participating reactions were carried out separately. Furthermore, a deactivation model was derived and validated by experimental data with low contents of H2S, showing that residual activities, as observed by some authors, are a result of rate-equality of deactivation and in-situ regeneration process on the surface of the catalyst. (C) 2015 Elsevier B.V. All rights reserved.
Keywords:Catalytic combustion;PdO/Al2O3 catalyst;Sulfur contaminants;Deactivation;In-situ regeneration