New insights and reaction mechanisms in the design of catalysts for the synergistic removal of NOx and VOCs from coke oven flue gas: Dual regulation of oxidative properties and acidic sites.

ABSTRACT

The acid and redox sites of the MnCo catalysts are simultaneously fine-tuned by the addition of V. A dual-function catalyst, designated as V0.5Mn5Co5, has been constructed for the synergistic removal of NOx and volatile organic compounds under coke-oven flue gas conditions, which exhibits > 95 % NOx conversion and > 80 % N2 selectivity at 180-300 °C. Meanwhile, it removes 70 % of ethylene at 240 °C. Besides it has excellent sulfur and water resistance. The characterization results indicate that this acid-redox dual sites modulation strategy appropriately weakens the oxidation capacity of the catalysts while increasing the surface acidity of the catalysts. The catalyst mainly performs SCR reaction through the E-R mechanism, and N2O is generated through the transition dehydrogenation of NH3 and NSCR reaction. Ethylene is first adsorbed on the catalyst surface then oxidized to form carbonate species, and finally decomposed to CO2. Ethylene oxidation follows the MvK mechanism. There is a competitive adsorption between NH3 and C2H4, and a mutual inhibition between the SCR reaction and the ethylene oxidation reaction. V0.5Mn5Co5 exhibits excellent synergistic removal of NOx and VOCs in coke oven flue gas compared with commercial VWTi catalysts, which indicates great promise for industrial application.