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Four typical coal-fired power plants were employed to explore the performance evolution within the whole life cycle of catalysts. The results revealed that the amount of active ingredients in the catalysts decreased over time. The content of V 2 O 5 and WO 3 in four units had decreased by 3.32%–32.8% and 12.9%–22.9% respectively. However, alkali metals and alkaline earth metals in flue gas were gradually deposited on the catalyst and led to catalyst poisoning, especially in two units due to arsenic poisoning. The specific surface area of catalysts decreased significantly in the first year of operation, accounting for 87.3%, 47.8%, 55.1% and 86.7% of the decline in the lifetime, which may be the main reason for the decline of catalyst activity during this period. The wall thickness of catalysts decreased linearly with the operation time in the lifetime. The relative activity of catalysts at the end of designed service lifetime was between 0.90 and 0.93, whereas the decrease range of SO 2 /SO 3 conversion rate was within 15.4%–35.6%. Influenced by the catalyst design and the variations of practical operation conditions, the difference between the actual and designed service lifetimes of catalysts in the four units was 2.08%, 44.0%, 4.17%, and − 25.0%, respectively. • SCR catalyst of four typical coal-fired power plant was investigated. • Catalyst performance evolution in three consecutive years of operation were analyzed. • A method for checking actual service lifetime of SCR catalyst was proposed. • Difference between the actual and designed catalyst lifetimes was obtained. • K/K 0 at the end of catalyst service lifetime was between 0.91 and 0.93. [ABSTRACT FROM AUTHOR]

Investigation of the low-temperature (LT) selective catalytic reduction (SCR) of NOx has adsorbed extensive efforts, and is now a hot topic in environmental catalysis. In this work, we cautiously explore the mechanism beneath LT-SCR via a combination of chemical-trapping methods, using BaO/Al2O3 as a NOx-intermediate trap, temperature-programmed desorption (TPD) and in situ FTIR spectroscopy over a series of metal-oxide catalysts. Our results show a linear correlation between LT-SCR rates and amounts of nitrites generated from NO oxidative activation and sequentially stored on BaO/Al2O3, implying key roles of nitrites/nitrite-precursors in LT-SCR. [ABSTRACT FROM AUTHOR]

Ceria has absorbed extensive interests in functioning as catalysts for low-temperature (LT) selective catalytic reduction (SCR) of NOx due to its abundant surface oxygen species and salient redox property. The mechanistic interpretations of how such redox property contributes to its LT-SCR activity, however, still remain debated. Here, we use a model tungsten-promoted ceria catalyst (WO 3 /CeO 2), known as preeminent in LT-SCR reactions, and combine steady-state kinetic, structural characteristic and in situ spectroscopic experiments with theoretical treatments to reveal the mechanistic connections between NO oxidative activation and LT-SCR turnovers. We show that, compared with NO oxidation to NO 2 , NO oxidative activation to nitrite intermediates is both kinetically and thermodynamically more favorable; surface nitrate species are not detected in the present case, indicating their more difficult formation than nitrites. All these results thus suggest the prevalence of NO activation to nitrites over NO to nitrates or oxidation to NO 2 and subsequent occurrence of fast SCR in the WO 3 /CeO 2 -catalyzed LT-SCR reaction. These findings progress the understanding of LT-SCR reaction mechanism on CeO 2 -based catalysts and convey a detailed perspective of different reaction intermediates and their consequences for LT-SCR turnovers, which may contribute to the rational design of catalysts towards further improved LT-SCR activity. [ABSTRACT FROM AUTHOR]