Effect of the oxidation state of manganese in the manganese oxides used in the synthesis of Mn-substituted cordierite on the properties of the product

Abstract

Catalysts based on Mn-substituted cordierite 2MnO · 2Al₂O₃ · 5SiO₂ have been synthesized using different manganese oxides (MnO, Mn₂O₃, and MnO₂) at a calcination temperature of 1100°C. The catalysts differ in their physicochemical properties, namely, phase composition (cordierite content and crystallinity), manganese oxide distribution and dispersion, texture, and activity in high-temperature ammonia oxidation. The synthesis involving MnO yields Mn-substituted cordierite with a defective structure, because greater part of the manganese cations is not incorporated in this structure and is encapsulated and the surface contains a small amount of manganese oxides. This catalyst shows the lowest ammonia oxidation activity. The catalysts prepared using Mn₂O₃ or MnO₂ are well-crystallized Mn-substituted cordierite whose surface contains different amounts of manganese oxides differing in their particle size. They ensure a high nitrogen oxides yield in a wide temperature range. The product yield increases with an increasing surface concentration of Mn³⁺ cations. The highest NO_x yield (about 76% at 800–850°C) is observed for the MnO₂-based catalyst, whose surface contains the largest amount of manganese oxides.