Enhancing Water Tolerance and N2 Selectivity in NH3–SCR Catalysts by Protecting Mn Oxide Nanoparticles in a Silicalite-1 Layer

Mn-based catalysts are promising candidates for eliminating harmful nitrogen oxides (NOx) via selective catalytic reduction with ammonia (NH3–SCR) due to their inherent strong redox abilities. However, poor water tolerance and low N2 selectivity are still the main limitations for practical applicati...

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Bibliographic Details
Published in:Environmental science & technology 2024-07, Vol.58 (34), p.15279
Main Authors: Komaty, Sarah, Andijani, Marram, Wang, Ning, de Miguel, Juan Carlos Navarro, Veeranmaril, Sudheesh Kumar, Hedhili, Mohamed Nejib, Silva, Cristina I Q, Wang, Yan, Abou-Daher, Mohamad, Han, Yu, Ruiz-Martinez, Javier
Format: Article
Language:English
Subjects:
Adsorbed water
Ammonia
Catalysts
Chemical reduction
Fourier analysis
Fourier transforms
Hydrophobicity
Infrared analysis
Infrared spectroscopy
Nanoparticles
Nitrogen oxides
Nitrous oxide
Operating temperature
Photochemicals
Selective catalytic reduction
Selectivity
Silicalite
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Summary:Mn-based catalysts are promising candidates for eliminating harmful nitrogen oxides (NOx) via selective catalytic reduction with ammonia (NH3–SCR) due to their inherent strong redox abilities. However, poor water tolerance and low N2 selectivity are still the main limitations for practical applications. Herein, we succeeded in preparing an active catalyst for NH3–SCR with improved water tolerance and N2 selectivity based on protecting MnOx with a secondary growth of a hydrophobic silicalite-1. This protection suppressed catalyst deactivation by water adsorption. Interestingly, impregnating MnOx on MesoTS-1 followed by silicalite-1 protection allowed for a higher dispersion of MnOx species, thus increasing the concentration of acid sites. Consequently, the level of N2O formation is decreased. These improvements resulted in a broader operating temperature of NOx conversion and a modification of the NH3–SCR mechanism. Diffuse reflectance infrared Fourier transform spectroscopy analysis revealed that unprotected Mn/MesoTS-1 mainly followed the Eley–Rideal mechanism, while Mn/MesoTS-1@S1 followed both Langmuir–Hinshelwood and Eley–Rideal mechanisms.
ISSN:0013-936X
1520-5851
1520-5851
DOI:10.1021/acs.est.4c01585