Isothermal desulfation of pre-sulfated Pt-BaO/γ-Al2O3 lean NOx trap catalysts with H2: The effect of H2 concentration and the roles of CO2 and H2O

The desulfation mechanisms of pre-sulfated Pt-BaO/γ-Al2O3 lean NOx trap catalysts were investigated under isothermal conditions (600 °C) using H2 as the reductant. Sulfates were found to be reduced first with H2 to produce SO2, followed by a reaction between SO2 and H2 to produce H2S. Gas analysis during the rich pulse reveals that the sulfur removal efficiency is initially proportional to the H2 concentration. At constant H2 concentration the overall desulfation efficiency decreases in the order of H2/CO2/H2O > H2/CO2 > H2/H2O > H2, as confirmed by XPS analysis of residual sulfur in the desulfated samples. H2O limits the evolution of SO2 at an early stage of the rich pulse and enhances the production of H2S in later stages of reduction. CO2 is involved in both the formation of COS and the production of H2O (via the reverse water–gas shift reaction), therefore, resulting in an increased overall efficiency.

Graphical abstractFigure optionsDownload full-size imageDownload as PowerPoint slideHighlights► Sulfates were found to be reduced with H2 to produce SO2, followed by the formation of H2S. ► The sulfur removal efficiency is initially proportional to the H2 concentration, then leveled off. ► At constant H2 concentration the overall desulfation efficiency decreases in the order of H2/CO2/H2O > H2/CO2 > H2/H2O > H2. ► H2O enhances the production of H2S in later stages of reduction. ► CO2 is involved in both the formation of COS and the production of H2O.