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Mechanism of Fast Selective Catalytic Reduction of NO with NH 3 over MnO X -CeO 2 Catalysts
H
Z
K
王
S
Z
Z
杨
DOI:10.1039/D5CY01103E.png)
Abstract
En 中文
MnOₓ-CeO₂ composites are promising candidates as low-temperature active catalysts for selective catalytic reduction (SCR) of NO with NH3; which is a leading technology for controlling NO emissions from non-electric flue gases. In this study; we systematically investigate the Fast-SCR mechanism over MnOₓ-CeO₂ through both experimental and theoretical approaches.Our results reveal that Fast-SCR is coupled with the Standard-SCR through three coupled redox cycles: Mn-redox; Ce-redox; and O₂-Ov (surface oxygen vacancy in CeO₂) cycles occurring at distinct active site. Even under O₂-rich reaction conditions; the Fast-SCR reaction route still needs to overcome a higher energy barrier of 1.56 eV in the rate-determining step; compared to the energy barrier of 1.44 eV in the Standard-SCR route. Intriguingly; Fast-SCR significantly enhances the SO₂ resistance and N₂ selectivity by reducing the residence time of NH₃ adsorbed on Mn³⁺ ions in the center of MnOX clusters; thereby suppressing its reaction with SOₓ and minimizing its deep oxidation to induce N2O emission.
Journal
IF:
4.2
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8.6K
Citations:
3.1W
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