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Alkali-Resistant Catalytic Reduction of NOx via Naturally Coupling Active and Poisoning Sites.

Releasing the poisoning effect of alkali metals over catalysts is still an intractable issue for selective catalytic reduction (SCR) of NOx with ammonia. The presence of K in fly ash always dramatically suppressed catalytic activity by impairing acidity and redox properties, leading to severe reduction of lifetime for SCR catalysts. Herein, alkali-resistant NOx reduction over TiO2-supported Fe2(SO4)3 catalysts was originally demonstrated via naturally coupling active and poisoning sites. Notably, TiO2-supported Fe2(SO4)3 catalysts expressed admirable NOx conversion and K resistance within a quite broad temperature window of 200-500 °C. The catalysts with more conserved sulfate species revealed that sulfate groups preferred to migrate from the bulk phase to surface, thus effectively binding with K poisons to release the damage on iron active sites. Because of protection effects of migrated sulfates and closely coupling effects with Fe active sites, NH3 and NO adsorption amounts and rates were well maintained. In this way, Fe metal sites and sulfate species closely coupled together on a self-preserved TiO2-supported Fe2(SO4)3 catalyst played essential roles as highly active sites and unique poisoning sites. This work paves a new way to design SCR catalysts with superior alkali resistance that are more reliable in practical deNOx application.