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

摘要

Catalysts based on Mn-substituted cordierite 2MnO center dot 2Al(2)O(3) center dot 5SiO(2) have been synthesized using different manganese oxides (MnO, Mn2O3, and MnO2) at a calcination temperature of 1100A degrees 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 800-850A degrees C) is observed for the MnO2-based catalyst, whose surface contains the largest amount of manganese oxides.