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Alkali and Heavy Metal Copoisoning Resistant Catalytic Reduction of NO x via Liberating Lewis Acid Sites.

Authors :
Shen Z
Liu X
Impeng S
Zhang C
Yan T
Wang P
Zhang D
Source :
Environmental science & technology [Environ Sci Technol] 2022 Apr 19; Vol. 56 (8), pp. 5141-5149. Date of Electronic Publication: 2022 Apr 03.
Publication Year :
2022

Abstract

The catalyst deactivation caused by the coexistence of alkali and heavy metals remains an obstacle for selective catalytic reduction of NO <subscript>x</subscript> with NH <subscript>3</subscript> . Moreover, the copoisoning mechanism of alkali and heavy metals is still unclear. Herein, the copoisoning mechanism of K and Cd was revealed from the adsorption and variation of reaction intermediates at a molecular level through time-resolved in situ spectroscopy combined with theoretical calculations. The alkali metal K mainly decreased the adsorption of NH <subscript>3</subscript> on Lewis acid sites and altered the reaction more depending on the formation of the NH <subscript>4</subscript> NO <subscript>3</subscript> intermediate, which is highly related to NO <subscript> x </subscript> adsorption and activation. However, Cd further inhibited the generation of active nitrate intermediates and thus decreased the NO <subscript> x </subscript> abatement about 60% on potassium-poisoned CeTiO <subscript> x </subscript> catalysts. Physically mixing with acid additives for CeTiO <subscript> x </subscript> catalysts could significantly liberate the active Lewis acid sites from the occupation of alkali metals and relieve the high dependence on NO <subscript> x </subscript> adsorption and activation, thus recovering the NO <subscript> x </subscript> removal rate to the initial state. This work revealed the copoisoning mechanism of K and Cd on Ce-based de-NO <subscript> x </subscript> catalysts and developed a facile anti-poisoning strategy, which paves a way for the development of durable catalysts among alkali and heavy metal copoisoning resistant catalytic reduction of NO <subscript> x </subscript> .

Details

Language :
English
ISSN :
1520-5851
Volume :
56
Issue :
8
Database :
MEDLINE
Journal :
Environmental science & technology
Publication Type :
Academic Journal
Accession number :
35369691
Full Text :
https://doi.org/10.1021/acs.est.1c08096