Abstract
The exploitation of transitional metal catalysts for high-efficient conversion of NO to NO2 still persists as an imperative issue due to the high cost of currently used Pt–based catalysts. Herein, we report a TEA-modification strategy to anchor Mn single atoms/clusters on Al2O3 (Mn/Al2O3-T) for NO oxidation. Activity tests show that Mn/Al2O3-T (T83 = 275 °C) displays a superior NO-to-NO2 capacity compared with the unmodified Mn nanoparticle on Al2O3 (Mn/Al2O3-B, T66 = 300 °C) and Pt/Al2O3 (T43 = 350 °C) counterparts. Comprehensive characterization and DFT calculations discover that the effective adjustment of TEA can promote the generation of coordination unsaturated Mn sites with elongated Mn-O bonds, which can improve the mobility of surface lattice oxygen and facilitate the activation of molecular oxygen. Additionally, reducing Mn size from nanoparticles to single atoms/clusters favors the formation of labile nitrate species and facile desorption of NO2, thereby regenerating active sites and accelerating overall NO oxidation reaction.
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