Compensation or Aggravation: Pb and SO₂ Copoisoning Effects over Ceria-Based Catalysts for NO_x Reduction

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Abstract

Severe catalyst deactivation caused by multiple poisons, including heavy metals and SO₂, remains an obstinate issue for the selective catalytic reduction (SCR) of NO_x by NH₃. The copoisoning effects of heavy metals and SO₂ are still unclear and irreconcilable. Herein, the unanticipated differential compensated or aggravated Pb and SO₂ copoisoning effects over ceria-based catalysts for NO_x reduction was originally unraveled. It was demonstrated that Pb and SO₂ exhibited a compensated copoisoning effect over the CeO₂/TiO₂ (CT) catalyst with sole active CeO₂ sites but an aggravated copoisoning effect over the CeO₂-WO₃/TiO₂ (CWT) catalyst with dual active CeO₂ sites and acidic WO₃ sites. Furthermore, it was uniquely revealed that Pb preferred bonding with CeO₂ among CT while further being combined with SO₂ to form PbSO₄ after copoisoning, which released the poisoned active CeO₂ sites and rendered the copoisoned CT catalyst a recovered reactivity. In comparison, Pb and SO₂ would poison acidic WO₃ sites and active CeO₂ sites, respectively, resulting in a seriously degraded reactivity of the copoisoned CWT catalyst. Therefore, this work thoroughly illustrates the internal mechanism of differential compensated or aggravated deactivation effects for Pb and SO₂ copoisoning over CT and CWT catalysts and provides effective solutions to design ceria-based SCR catalysts with remarkable copoisoning resistance for the coexistence of heavy metals and SO₂.

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