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

Zhi ShenXiangyu LiuSarawoot ImpengChengbiao ZhangTingting YanPenglu WangDengsong Zhang
Published in: Environmental science & technology (2022)
The catalyst deactivation caused by the coexistence of alkali and heavy metals remains an obstacle for selective catalytic reduction of NO x with NH 3 . 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 3 on Lewis acid sites and altered the reaction more depending on the formation of the NH 4 NO 3 intermediate, which is highly related to NO x adsorption and activation. However, Cd further inhibited the generation of active nitrate intermediates and thus decreased the NO x abatement about 60% on potassium-poisoned CeTiO x catalysts. Physically mixing with acid additives for CeTiO x catalysts could significantly liberate the active Lewis acid sites from the occupation of alkali metals and relieve the high dependence on NO x adsorption and activation, thus recovering the NO x removal rate to the initial state. This work revealed the copoisoning mechanism of K and Cd on Ce-based de-NO x 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 x .
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