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Enhancing Water Tolerance and N 2 Selectivity in NH 3 -SCR Catalysts by Protecting Mn Oxide Nanoparticles in a Silicalite-1 Layer.

Authors :
Komaty S
Andijani M
Wang N
Navarro de Miguel JC
Kumar Veeranmaril S
Hedhili MN
Silva CIQ
Wang Y
Abou-Daher M
Han Y
Ruiz-Martinez J
Source :
Environmental science & technology [Environ Sci Technol] 2024 Jul 31. Date of Electronic Publication: 2024 Jul 31.
Publication Year :
2024
Publisher :
Ahead of Print

Abstract

Mn-based catalysts are promising candidates for eliminating harmful nitrogen oxides (NO <subscript> x </subscript> ) via selective catalytic reduction with ammonia (NH <subscript>3</subscript> -SCR) due to their inherent strong redox abilities. However, poor water tolerance and low N <subscript>2</subscript> selectivity are still the main limitations for practical applications. Herein, we succeeded in preparing an active catalyst for NH <subscript>3</subscript> -SCR with improved water tolerance and N <subscript>2</subscript> selectivity based on protecting MnO <subscript> x </subscript> with a secondary growth of a hydrophobic silicalite-1. This protection suppressed catalyst deactivation by water adsorption. Interestingly, impregnating MnO <subscript> x </subscript> on MesoTS-1 followed by silicalite-1 protection allowed for a higher dispersion of MnO <subscript> x </subscript> species, thus increasing the concentration of acid sites. Consequently, the level of N <subscript>2</subscript> O formation is decreased. These improvements resulted in a broader operating temperature of NO <subscript> x </subscript> conversion and a modification of the NH <subscript>3</subscript> -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.

Details

Language :
English
ISSN :
1520-5851
Database :
MEDLINE
Journal :
Environmental science & technology
Publication Type :
Academic Journal
Accession number :
39083593
Full Text :
https://doi.org/10.1021/acs.est.4c01585