
DEVELOPMENT OF MULTI-TASK CATALYSTS FOR REMOVAL OF NOx AND TOXIC ORGANIC COMPOUNDS DURING COAL COMBUSTION
Author(s) -
Panagiotis G. Smirniotis,
Robert G. Jenkins
Publication year - 2002
Language(s) - English
Resource type - Reports
DOI - 10.2172/800982
Subject(s) - catalysis , selective catalytic reduction , valence (chemistry) , vanadium , nox , selectivity , inorganic chemistry , vanadium oxide , ammonia , oxide , chemistry , materials science , combustion , organic chemistry
The work performed during this project focused on the identification of materials capable of providing high activity and selectivity for the selective catalytic reduction of nitric oxide with ammonia. The material surface characteristics were correlated with the catalytic behavior of our catalysts to increase our understanding and to help improve the DeNO{sub x} efficiency. The catalysts employed in this study include mixed oxide composite powders (TiO{sub 2}-Cr{sub 2}O{sub 3}, TiO{sub 2}-ZrO{sub 2}, TiO{sub 2}-WO{sub 3}, TiO{sub 2}-SiO{sub 2}, and TiO{sub 2}-Al{sub 2}O{sub 3}) loaded with varying amounts of V{sub 2}O{sub 5}, along with 5 different commercial sources of TiO{sub 2}. V{sub 2}O{sub 5} was added to the commercial sources of TiO{sub 2} to achieve monolayer coverage. Since the valence state of vanadium in the precursor solution during the impregnation step significantly impacted catalytic performance, catalysts were synthesized from both V{sup +4} and V{sup +5} solutions explain this phenomenon. Specifically, the synthesis of catalysts from V{sup 5+} precursor solutions yields lower-performance catalysts compared to the case of V{sup 4+} under identical conditions. Aging the vanadium precursor solution, which is associated with the reduction of V{sup 5+} to V{sup 4+} (VO{sub 2}{sup +} {yields} VO{sup 2+}), prior to impregnation results in catalysts with excellent catalytic behavior under identical activation and operating conditions. This work also added vanadia to TiO{sub 2}-based supports with low crystallinity. These supports, which have traditionally performed poorly, are now able to function as effective SCR catalysts. Increasing the acidity of the support by incorporating oxides such as WO{sub 3} and Al{sub 2}O{sub 3} significantly improves the SCR activity and nitrogen selectivity. It was also found that the supports should be synthesized with the simultaneous precipitation of the corresponding precursors. The mixed oxide catalysts possess Broensted and Lewis acid sites of comparable strength over a wide range of temperatures. Catalysts prepared from aged vanadium precursor solutions also demonstrated a wider temperature window for optimum operation