Ceria-zirconia modified MnOx catalysts for gaseous elemental mercury oxidation and adsorption

Abstract

A series of MnOx/CeO2 (Mn/Ce), MnOx/ZrO2 (Mn/Zr), and MnOx/Ce0.75Zr0.25O2 (Mn/CZ) catalysts prepared by an impregnation method were tested for their ability to catalyse the oxidation of Hg0 at relatively low temperature (423 K). Various characterization techniques, namely, Brunauer-Emmett-Teller (BET) surface area analysis, X-ray diffraction (XRD), Raman spectroscopy (RS), X-ray photoelectron spectroscopy (XPS), and H2-temperature programmed reduction (H2-TPR) were employed to understand the structural, surface, and redox properties of the prepared catalysts. Specific aspects of the catalysis of Hg0 oxidation that were investigated included the influence of MnOx loading (5, 15, and 25%) and the influence of HCl and O2. Among the catalysts tested, the 15Mn/CZ catalyst achieved the best Hg0 oxidation performance (~83% conversion of Hg0 to Hg2+) in the presence of HCl and O2. The higher activity of the 15Mn/CZ catalyst was most likely due to the presence of more oxygen vacancies, enhanced Mn4+/Mn4+ + Mn3+ + Mn2+ ratio and more surface adsorbed oxygen, which were proved by XRD, BET, Raman, and XPS. H2-TPR results also show that the strong interaction between the Ce0.75Zr0.25O2 support and MnOx improved the redox properties significantly as compared to pure CeO2 and ZrO2 supported MnOx catalysts.