Selective catalytic reduction of nitrogen oxides by ammonia over Fe{sup 3+}-exchanged TiO{sub 2}-pillared clay catalysts
- Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering
Fe-exchanged TiO{sub 2}-pillared clay (PILC) catalysts were prepared and used for selective catalytic reduction (SCR) of NO{sub x} by ammonia. They were also characterized for surface area, pore size distribution, and by XRD, H{sub 2}-TPR, and FT-IR methods. The Fe-TiO{sub 2}-PILC catalysts showed high activities in the reduction of NO{sub x} by NH{sub 3} in the presence of excess oxygen. SO{sub 2} further increased the catalytic activities at above 350 C, whereas H{sub 2}O decreased the activity slightly. The catalysts were about twice as active as commercial-type V{sub 2}O{sub 5}-WO{sub 3}/TiO{sub 2} catalyst in the presence of H{sub 2}O and SO{sub 2}. Moreover, compared to the commercial catalyst, the Fe-TiO{sub 2}-PILC catalysts had higher N{sub 2}/N{sub 2}O product selectivities (e.g., 0--1% vs 9% N{sub 2}O at 400 C) and substantially lower activities (by 74--88%) for SO{sub 2} oxidation to SO{sub 3} under the same reaction conditions. The activity was further increased to over three times that of the vanadia-based catalyst when Ce was added. The high activity and low N{sub 2}O selectivity for the Fe-TiO{sub 2}-PILC catalysts were attributed to their low activity in the oxidation of ammonia, as compared with vanadia catalysts. XRD patterns of Fe-TiO{sub 2}-PILC were similar to those of TiO{sub 2}-PILC, showing no peaks due to iron oxide, even when the iron content reached 20.1%. The TPR results indicated that iron in the Fe-TiO{sub 2}-PILC catalysts with lower iron contents existed in the form of isolated Fe{sup 3+} ions. The activities of Fe-TiO{sub 2}-PILC catalysts were consistent with their surface acidities, which were identified by FT-IR of the NH{sub 3}-adsorbed samples. The enhancement of activities by H{sub 2}O + SO{sub 2} was attributed to the increase of surface acidity resulting from the formation of surface sulfate species of iron.
- OSTI ID:
- 687738
- Journal Information:
- Journal of Catalysis, Vol. 186, Issue 2; Other Information: PBD: 10 Sep 1999
- Country of Publication:
- United States
- Language:
- English
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