JOURNAL ARTICLE

Deactivation\nMechanism of Multipoisons in Cement Furnace\nFlue Gas on Selective Catalytic Reduction Catalysts

Abstract

Increasing numbers of cement furnaces\nhave applied selective catalytic\nreduction (SCR) units for advanced treatment of NO in the flue gas.\nHowever, the SCR catalysts may face various poisons, such as acidic,\nalkaline, and heavy metal species, in the fly ash. In this work, we\nstudied the deactivation mechanisms of multipoisons (Ca, Pb, and S)\non the CeO<sub>2</sub>–WO<sub>3</sub>/TiO<sub>2</sub> catalyst,\nusing the <i>in situ</i> diffuse reflectance infrared Fourier\ntransform spectroscopy method. Calcium promoted the conversion of\nCe­(III) to Ce­(IV) and, thus, (i) suppressed the redox cycle, (ii)\ndecreased the NO adsorption (monodentate NO<sub>3</sub><sup>–</sup> and bridged NO<sub>2</sub><sup>–</sup>), and (iii) enriched\nthe Lewis acid sites. Pb­(IV) blocked Ce<sub>2</sub>(WO<sub>4</sub>)<sub>3</sub>, aggravating the electronegativity of W<sup>6+</sup>, which inhibited (i) the binding stability of tungsten and ammonia\nspecies, (ii) bridged NO<sub>3</sub><sup>–</sup> (bonded to\ntungsten), and (iii) the Brønsted acid sites. The multipoisoning\nprocesses enriched O<sup>2–</sup> by repairing partial surface\noxygen defects, which suppressed O<sub>2</sub><sup>2–</sup> and O<sup>–</sup>. Sulfur occupied the surface base sites\nand formed PbSO<sub>4</sub> after Ce<sub>2</sub>(WO<sub>4</sub>)<sub>3</sub> was saturated.

Keywords:
Catalysis Adsorption Flue gas Metal Redox Cement Lewis acids and bases Infrared spectroscopy Selective catalytic reduction

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