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Strong Interaction of CoOx with POx for Enhanced N2 Selectivity in Selective Catalytic Oxidation of Ammonia
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DOI:10.1021/acs.est.5c18708.png)
Abstract
En 中文
Selective catalytic oxidation of ammonia (NH3–SCO) over transition metal oxide catalysts with high NH3 conversion and N2 selectivity at low temperatures is important but remains a significant challenge. Herein, we propose a novel strategy for depositing phosphate (POx) onto CeO2 nanorods, and POx acts as a host for CoOx (CoOx-P0.05/CeO2). The CoOx-P0.05/CeO2 enables an NH3 conversion of 84% and a N2 selectivity of 86% at a low temperature of 200 °C, obviously outperforming CoOx/CeO2 (N2 selectivity of 40%) and P0.05/CeO2 (NH3 conversion of 7% even at 250 °C). The strong interaction of CoOx with POx strengthens the Co–O bond and generates medium-strong acid sites, which are found to play an important role in improving N2 selectivity. Density functional theory (DFT) calculations and in situ diffuse reflectance infrared Fourier transform spectra (in situ DRIFTS) reveal that the introduction of POx enhances the binding energy with NH3 and significantly alters the bidentate nitrate of CoOx/CeO2 to monodentate nitrate of CoOx-P0.05/CeO2, thereby substantially suppressing the formation of byproducts N2O and NO and enhancing N2 selectivity.
Keywords:
strong interaction
CoOx
POx
N2 selectivity
selective catalytic oxidation of NH3
Journal
E
IF:
11.3
Papers:
1.9K
Citations:
1
