Economical Way to Synthesize SSZ-13 with Abundant Ion-Exchanged Cu+ for an Extraordinary Performance in Selective Catalytic Reduction (SCR) of NOx by Ammonia
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Abstract
In this study, an economical way for SSZ-13 preparation with the essentially cheap choline chloride as template has been attempted. The as-synthesized SSZ-13 zeolite after ion exchange by copper nitrate solution exhibited a superior SCR performance (over 95% NOx conversion across a broad range from 150 to 400 °C) to the traditional zeolite-based catalysts of Cu-Beta and Cu-ZSM-5. Furthermore, the opportune size of pore opening (∼3.8 Å) made Cu-SSZ-13 exhibiting the best selectivity to N2 as well as satisfactory tolerance toward SO2 and C3H6 poisonings. The characterization (XRD, XPS, XRF, and H2-TPR) of samples confirmed that Cu-SSZ-13 possessed the most abundant Cu cations among three investigated Cu-zeolites; furthermore, either on the surface or in the bulk the ratio of Cu(+)/Cu(2+) ions for Cu-SSZ-13 is also the highest. New finding was announced that CHA-type topology is in favor of the formation of copper cations, especially generating much more Cu(+) ions than the others, rather than CuO. The activity test of Cu(CuCl)-ZSM-5 (prepared by a solid-state ion-exchange method) clearly indicated that Cu(+) ions could make a major contribution to the low-temperature deNOx activity. The activity of protonic zeolites (H-SSZ-13, H-Beta, H-ZSM-5) revealed the topology effect on SCR performances.
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