Abstract
The activated coke is a promising support for catalysts, and it is important to study the performance of the activated coke catalyst on the removal of NOx. In the current research, a series of the activated coke-supported Mn–Cu catalysts are prepared by the incipient wetness impregnation method. The effects of the molar ration of Mn/Cu, the content of Mn–Cu, the calcination temperature, and reaction space velocity on NO conversion are investigated, and it was found that the 8 wt.% Mn0.7Cu0.3/AC had the best catalytic activity when the calcination temperature was 200 °C. The existence of SO2 caused the catalyst to deactivate, but the activity of the poisoning catalyst could be recovered by different regeneration methods. To uncover the underlying mechanism, BET, XPS, XRD, SEM and FTIR characterizations were performed. These results suggested that the specific surface area and total pore volume of the poisoning catalyst are recovered and the sulfite and sulfate on the surface of the poisoning catalysts are removed after water washing regeneration. More importantly, the water washing regeneration returns the value of Mn3+/Mn4+, Cu2+/Cu+, and Oα/Oβ, related to the activity, basically back to the level of the fresh catalyst. Thus, the effect of water washing regeneration is better than thermal regeneration. These results could provide some helpful information for the design and development of the SCR catalysts.
Highlights
Nitrogen oxides (NOX) are the main pollutants in the atmosphere, and these pollutants can cause chemical smog and acid rain, which further result in significant damage to the ecological environment and human health [1,2]
The optimum temperature ranges for the use of the vanadium–tungsten–titanium catalysts are 300~400 ◦C, which does not match with the low-temperature selective catalytic reduction process
The addition of water vapor during the thermal regeneration process could further improve the catalytic activity, and the NO conversion is 45.21% at same conditions. These results suggested that the addition of water vapor has positive effects on the regeneration of the poisoning catalyst; the addition of water vapor is applied in the subsequent thermal regeneration experiments
Summary
Nitrogen oxides (NOX) are the main pollutants in the atmosphere, and these pollutants can cause chemical smog and acid rain, which further result in significant damage to the ecological environment and human health [1,2]. The selective catalytic reduction (SCR) of NOX with NH3 (NH3-SCR) technology has long been a mature and extensively used method for controlling NOX emissions [3,4]. The optimum temperature ranges for the use of the vanadium–tungsten–titanium catalysts are 300~400 ◦C, which does not match with the low-temperature selective catalytic reduction process. Though the physical adsorption performance, chemical adsorption performance and catalytic activity are slightly lower in activated coke than in activated carbon, but the former has a lower price, high mechanical strength, and strong adsorption properties. Activated coke is highly suitable as a carrier for catalysts, and it has very important significance in studying the performance of the activated coke catalyst on the removal of NOx
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