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Selective catalytic reduction of NO{sub x} by olefins

Abstract

The removal of nitrogen oxides from the exhaust of lean-burn gasoline fuelled and diesel-fuelled engines, operating under net oxidizing conditions, has recently attracted considerable attention. In this work, three different catalytic systems (Al{sub 2}O{sub 3}, Cu/Al{sub 2}O{sub 3} and Cu/ZSM-5) are investigated for their suitability as catalysts for the selective reduction of nitrogen oxides by hydrocarbons in excess oxygen. Special emphasis is given to the formation of potentially harmful byproducts such as hydrogen cyanide (HCN), cyanic acid (HNCO), ammonia (NH{sub 3}) and nitrous oxide (N{sub 2}O). The effect of reaction temperature, nitrogen oxide (NO, NO{sub 2}), hydrocarbon (ethene, propene) and water on activity and the formation of byproducts is investigated. In situ FTIR spectroscopy and temperature-programmed surface reactions (TPSR) of absorbed species in different atmospheres were used to investigate the nature and reactivity of adsorbates formed under reaction conditions. The catalytic activity was strongly influenced by the presence of water in the feed. The effects of the other parameters were suppressed and the performance generally decreased, except when propene was used for the reduction of NO{sub x} over Cu/ZSM-5. Over Cu/ZSM-5 clearly higher conversion was obtained, when ethene was used as reducing agent, while there was no significant difference when  More>>
Authors:
Publication Date:
Dec 31, 1996
Product Type:
Miscellaneous
Reference Number:
SCA: 330701; PA: CH-97:0E0251; EDB-97:097584; SN: 97001817423
Resource Relation:
Other Information: DN: Diss. ETH Nr. 11792; TH: Diss. (Dr.sc.techn.); PBD: 1996
Subject:
33 ADVANCED PROPULSION SYSTEMS; GASOLINE; COMBUSTION; DIESEL FUELS; NITROGEN OXIDES; REDUCTION; ALUMINIUM OXIDES; COPPER OXIDES; HYDROCYANIC ACID; NITROUS OXIDE; AMMONIA; INFRARED SPECTRA; EXPERIMENTAL DATA
OSTI ID:
495613
Research Organizations:
Eidgenoessische Technische Hochschule, Zurich (Switzerland)
Country of Origin:
Switzerland
Language:
English
Other Identifying Numbers:
TRN: CH97E0251
Availability:
Available from ETH-Bibliothek, Raemistr. 101, CH-8092 Zuerich, Switzerland
Submitting Site:
CH
Size:
143 p.
Announcement Date:
Aug 01, 1997

Citation Formats

Radtke, F. Selective catalytic reduction of NO{sub x} by olefins. Switzerland: N. p., 1996. Web.
Radtke, F. Selective catalytic reduction of NO{sub x} by olefins. Switzerland.
Radtke, F. 1996. "Selective catalytic reduction of NO{sub x} by olefins." Switzerland.
@misc{etde_495613,
title = {Selective catalytic reduction of NO{sub x} by olefins}
author = {Radtke, F}
abstractNote = {The removal of nitrogen oxides from the exhaust of lean-burn gasoline fuelled and diesel-fuelled engines, operating under net oxidizing conditions, has recently attracted considerable attention. In this work, three different catalytic systems (Al{sub 2}O{sub 3}, Cu/Al{sub 2}O{sub 3} and Cu/ZSM-5) are investigated for their suitability as catalysts for the selective reduction of nitrogen oxides by hydrocarbons in excess oxygen. Special emphasis is given to the formation of potentially harmful byproducts such as hydrogen cyanide (HCN), cyanic acid (HNCO), ammonia (NH{sub 3}) and nitrous oxide (N{sub 2}O). The effect of reaction temperature, nitrogen oxide (NO, NO{sub 2}), hydrocarbon (ethene, propene) and water on activity and the formation of byproducts is investigated. In situ FTIR spectroscopy and temperature-programmed surface reactions (TPSR) of absorbed species in different atmospheres were used to investigate the nature and reactivity of adsorbates formed under reaction conditions. The catalytic activity was strongly influenced by the presence of water in the feed. The effects of the other parameters were suppressed and the performance generally decreased, except when propene was used for the reduction of NO{sub x} over Cu/ZSM-5. Over Cu/ZSM-5 clearly higher conversion was obtained, when ethene was used as reducing agent, while there was no significant difference when starting from NO or NO{sub 2}. In contrast, with {gamma}-Al{sub 2}O{sub 3} NO{sub 2} was reduced more efficiently than NO with both reductants. The impregnation of {gamma}-Al{sub 2}O{sub 3} with copper led to an extensive loss of this performance. For dry feeds and with increasing CuO loading, the catalysts reached maximum activity at lower temperature and the maximum yield of nitrogen slightly decreased. (author) figs., tabs., refs.}
place = {Switzerland}
year = {1996}
month = {Dec}
}