DEVELOPMENT OF IMPROVED CATALYSTS FOR THE SELECTIVE CATALYTIC REDUCTION OF NITROGEN OXIDES WITH HYDROCARBONS

Akyurtlu, Ates ; Akyurtlu, Jale F.

Hampton University (United States)

关键词: Copper;    Hydrocarbons;    02 Petroleum;    Flow Rate;    Reaction Kinetics;   

DOI  :  10.2172/823017
RP-ID  :  NONE
RP-ID  :  FG26-99FT40617
RP-ID  :  823017

美国|英语

来源: UNT Digital Library

【 摘 要 】

Significant work has been done by the investigators on the cerium oxide-copper oxide based sorbent/catalysts for the combined removal of sulfur and nitrogen oxides from the flue gases of stationary sources. Evaluation of these sorbents as catalysts for the selective reduction of NO{sub x} gave promising results with methane. Since the replacement of ammonia by methane is commercially very attractive, in this project, the effect of promoters on the activity and selectivity of copper oxide/cerium oxide-based catalysts and the reaction mechanism for the SCR with methane was investigated. Unpromoted and promoted catalysts were investigated for their SCR activity with methane in a microreactor setup and also, by the temperature-programmed desorption (TPD) technique. The results from the SCR experiments indicated that manganese is a more effective promoter than the other metals (Rh, Li, K, Na, Zn, and Sn) for the supported copper oxide-ceria catalysts under study. The effectiveness of the promoter increased with the increase in Ce/Cu ratio. Among the catalysts tested, the Cu1Ce3 catalyst promoted with 1 weight % Mn was found to be the best catalyst for the SCR of NO with methane. This catalyst was subjected to long-term testing at the facilities of our industrial partner TDA Research. TDA report indicated that the performance of this catalyst did not deteriorate during 100 hours of operation and the activity and selectivity of the catalyst was not affected by the presence of SO{sub 2}. The conversions obtained by TDA were significantly lower than those obtained at Hampton University due to the transport limitations on the reaction rate in the TDA reactor, in which 1/8th inch pellets were used while the Hampton University reactor contained 250-425-{micro}m catalyst particles. The selected catalyst was also tested at the TDA facilities with high-sulfur heavy oil as the reducing agent. Depending on the heavy oil flow rate, up to 100% NO conversions were obtained. The temperature programmed desorption studies a strong interaction between manganese and cerium. Presence of manganese not only enhanced the reduction rate of NO by methane, but also significantly improved the N{sub 2} selectivity. To increase the activity of the Mn-promoted catalyst, the manganese content of the catalyst need to be optimized and different methods of catalyst preparation and different reactor types need to be investigated to lower the transport limitations in the reactor.