Abstract
Deep catalytic removal of nitrogen oxides is one of the widespread research topics, mainly limited by the low temperature activity and hydrothermal stability of the first step for NO oxidation. Oxygen vacancies (Ov) and oxygen migration capacity play a crucial role in this challenge. Particularly, tuning the Mn-O coordination environment according to the radius and valence differences of dopant ions can increase Ov, while accelerate oxygen migration by constructing Pt/mullite interfaces. Here, based on the hydrothermal stability of Pt/mullite to NO oxidation, we designed Mg2+- and Ba2+-doped catalysts. And the NO oxidation performance of the Mg2+-doped catalyst was significantly enhanced compared to the undoped catalysts (After hydrothermal aging, turnover frequency = 1.9 s−1 at 150 °C and activation energy = 21 kJ/mol). Meanwhile, all catalysts tested with simulated diesel exhaust and the NO oxidation performance showed essentially no decrease after 16 h of hydrothermal aging at 800 °C. Furthermore, X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) demonstrated the Ov content of doped catalysts increased significantly. In addition, O2 temperature programmed desorption (O2-TPD) and Thermogravimetry (TG) proved that the oxygen migration capacity of doped catalysts was enhanced by several times. Notably, the simple doping method is general for the modification of other mullites and worthy of industrial application.
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