Alkali and Heavy Metal Copoisoning Resistant Catalytic Reduction of NO_x via Liberating Lewis Acid Sites

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Abstract

The catalyst deactivation caused by the coexistence of alkali and heavy metals remains an obstacle for selective catalytic reduction of NO_x with NH₃. 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 NH₃ on Lewis acid sites and altered the reaction more depending on the formation of the NH₄NO₃ 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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