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NO reduction with CO over a highly dispersed Mn/TiO2catalyst at low temperature: a combined experimental and
Lilei Zhang1, Botan Li1, Chunyan Liu1
1College of Chemistry and Chemical Engineering, Luoyang Normal University, Luoyang 471934, People's Republic of China.
Abstract:
A highly dispersed Mn/TiO2catalyst, which has high efficiency for NO conversion with CO and almost completed N2selectivity at a low-temperature range (350-550 K), was investigated using experimental and DFT theoretical calculation. The characterization results illustrated that the catalyst assembled with nanoparticles and the Mn doping into the TiO2surface lattice led to the formation of Mn-O-Ti configuration, which enhanced the dispersion of Mn on the body of TiO2. The DFT study mapped out the complete catalytic cycle, including reactants adsorption, oxygen vacancy generation, N2O intermediates formation, N2formation in Eley-Rideal (ER), Langmuir-Hinshelwood, and termolecular Eley-Rideal mechanisms. With thermodynamic and kinetic analysis combined with experimental results, the ER reaction process was considered to be the fundamental mechanism over the highly dispersed Mn/TiO2catalyst. The calculation results indicated that N2O was a significant intermediate. However, the rapid N2O reduction process led to high N2selectivity. The rate-limiting step was the deoxygenation step of NO-MnOv/TiO2from N-O bond scission. The active site Mn-Ovpair embedded in Mn/TiO2was responsible not only for the formation of N-Mn/TiO2in the ER-1 step but also for the N2O deoxygenation process to make the final product N2in the ER-2 step. The synergetic effect between Mn 3d electron and the oxygen vacancy of TiO2were responsible for the catalytic activity of Mn/TiO2.
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