Key role of NO + C3H8 reaction for the elimination of NO in automobile exhaust by three-way catalyst.

Abstract

Pd-only three-way catalysts with improved catalytic activity for NO elimination were prepared. In order to explore the catalytic reaction rules of NO reduction under a three-way catalytic system, a series of single reactions related to NO reduction were evaluated. It was found that the reaction temperatures of NO + H2 or NO + CO or NO + C3H6 reactions were below 250°C, while that of NO + C3H8 was up to 350°C. Thus, the reaction NO + C3H8 served as the key reaction in determining the purification efficiency of NO at the high-temperature stage. By in situ FTIR, we proposed that three possible steps were involved in NO + C3H8 reaction. The first step was the oxidation of C3H8 and NO to acetone and nitrate species by active oxygen species, respectively (C3H8 + O* → C3H6O, NO + O* → NO3-). XPS results revealed that the amount of active oxygen species in Pd/CeO2-ZrO2-Al2O3 (Pd/CZA, 73.7%) was much higher than that in Pd/CexZr1-xO2+Al2O3 (Pd/CZ+A, 64.1%). This was in line with the higher reaction efficiency of the first step over Pd/CZA. Then the NO + C3H8 reaction was accelerated by the first step, which consequently contributed to the higher NO elimination efficiency of Pd/CZA.