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Title: Supported, Alkali-Promoted Cobalt Oxide Catalysts for NOx Removal from Coal Combustion Flue Gases

A series of cobalt oxide catalysts supported on alumina ({gamma}-Al{sub 2}O{sub 3}) were synthesized with varying contents of cobalt and of added alkali metals, including lithium, sodium, potassium, rubidium, and cesium. Unsupported cobalt oxide catalysts and several cobalt oxide catalysts supported ceria (CeO{sub 2}) with varying contents of cobalt with added potassium were also prepared. The catalysts were characterized with UV-visible spectroscopy and were examined for NO{sub x} decomposition activity. The CoO{sub x}/Al{sub 2}O{sub 3} catalysts and particularly the CoO{sub x}/CeO{sub 2} catalysts show N{sub 2}O decomposition activity, but none of the catalysts (unsupported Co{sub 3}O{sub 4} or those supported on ceria or alumina) displayed significant, sustained NO decomposition activity. For the Al{sub 2}O{sub 3}-supported catalysts, N{sub 2}O decomposition activity was observed over a range of reaction temperatures beginning about 723 K, but significant (>50%) conversions of N{sub 2}O were observed only for reaction temperatures >900 K, which are too high for practical commercial use. However, the CeO{sub 2}-supported catalysts display N{sub 2}O decomposition rates similar to the Al{sub 2}O{sub 3}-supported catalysts at much lower reaction temperatures, with activity beginning at {approx}573 K. Conversions of >90% were achieved at 773 K for the best catalysts. Catalytic rates per cobalt atommore » increased with decreasing cobalt content, which corresponds to increasing edge energies obtained from the UV-visible spectra. The decrease in edge energies suggests that the size and dimensionality of the cobalt oxide surface domains increase with increasing cobalt oxide content. The rate data normalized per mass of catalyst that shows the activity of the CeO{sub 2}-supported catalysts increases with increasing cobalt oxide content. The combination of these data suggest that supported cobalt oxide species similar to bulk Co{sub 3}O{sub 4} are inherently more active than more dispersed cobalt oxide species, but this effect was only observed with the CeO{sub 2}-supported catalysts.« less
Authors:
Publication Date:
OSTI Identifier:
913563
DOE Contract Number:
FG26-04NT42181
Resource Type:
Technical Report
Research Org:
University Of Wyoming
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
01 COAL, LIGNITE, AND PEAT; ALKALI METALS; ATOMS; CATALYSTS; CESIUM; COAL; COBALT; COBALT OXIDES; COMBUSTION; GASES; LITHIUM; POTASSIUM; REMOVAL; RUBIDIUM; SODIUM; SPECTRA; SPECTROSCOPY