Novel regenerated V- and Ce-mixed oxide modified catalysts for the NH3-SCR of NOx displaying a distinctive broad temperature window
The challenge for selective catalytic reduction (SCR) of NOx with NH3 is to improve de-NOx activity at low temperatures while simultaneously improving the tolerance of catalysts towards SO2 poisoning. Herein, V and Ce oxides were loaded on deactivated SCR catalysts subjected to acid pickling (CAT) v...
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Veröffentlicht in: | Journal of cleaner production 2023-01, Vol.382, p.135384, Article 135384 |
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Sprache: | eng |
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Zusammenfassung: | The challenge for selective catalytic reduction (SCR) of NOx with NH3 is to improve de-NOx activity at low temperatures while simultaneously improving the tolerance of catalysts towards SO2 poisoning. Herein, V and Ce oxides were loaded on deactivated SCR catalysts subjected to acid pickling (CAT) via impregnation to recover de-NOx activity. The resulting V–Ce@CAT catalyst exhibited 85–95% NOx conversions over a wide temperature window of 200–450 °C while conversions of only 40–78% over the same temperature range were observed with CAT (spent catalyst treated with acid). Interestingly, in addition to the high tolerance towards SO2 displayed by V–Ce@CAT, the catalyst exhibited improved reactivity after the introduction of 200 ppm SO2, with the NOx conversion increasing from 80% to 87%. The results indicated that a kinetic equilibrium was reached between the formation and decomposition rates of Ce2(SO4)3 on V–Ce@CAT which prevented the accumulation of surface sulfate species, thereby protecting the main active species V from catalytic inactivation. Furthermore, in situ DRIFTS revealed that the NH3-SCR reaction pathway of V–Ce@CAT follows the L-H mechanism.
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•High-performance NH3-SCR of NOx was obtained with regenerated SCR catalysts modified with V and Ce mixed oxides.•The regenerated catalysts shows broad working temperature windows (150–450 °C).•The SO2 tolerance was attributed to the preferential formation of sulfate upon introduction of Ce species.•The interaction between V and Ce enhanced the ratio of surface chemisorbed labile oxygen (Oα), which promoted oxidation. |
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ISSN: | 0959-6526 1879-1786 |
DOI: | 10.1016/j.jclepro.2022.135384 |