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Title: Catalytic oxidation of HCN over a 0.5% Pt/Al2O3 catalyst

Abstract

The adsorption of HCN on, its catalytic oxidation with 6% O2 over 0.5% Pt/Al2O3, and the subsequent oxidation of strongly bound chemisorbed species upon heating were investigated. The observed N-containing products were N2O, NO and NO2, and some residual adsorbed N-containing species were oxidized to NO and NO2 during subsequent temperature programmed oxidation. Because N-atom balance could not be obtained after accounting for the quantities of each of these product species, we propose that N2 and was formed. Both the HCN conversion and the selectivity towards different N-containing products depend strongly on the reaction temperature and the composition of the reactant gas mixture. In particular, total HCN conversion reaches 95% above 250 C. Furthermore, the temperature of maximum HCN conversion to N2O is located between 200 and 250 C, while raising the reaction temperature increases the proportion of NOx in the products. The co-feeding of H2O and C3H6 had little, if any effect on the total HCN conversion, but C3H6 addition did increase the conversion to NO and decrease the conversion to NO2, perhaps due to the competing presence of adsorbed fragments of reductive C3H6. Evidence is also presented that introduction of NO and NO2 into the reactant gas mixturemore » resulted in additional reaction pathways between these NOx species and HCN that provide for lean-NOx reduction coincident with HCN oxidation.« less

Authors:
; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
883676
Report Number(s):
PNNL-SA-47073
3589; 6694; VT0401000; TRN: US200701%%360
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Applied Catalysis. B, Environmental, 65(2006):282-290
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; HYDROCYANIC ACID; ADSORPTION; CATALYSTS; OXIDATION; PLATINUM; ALUMINIUM OXIDES; CATALYTIC EFFECTS; NITROUS OXIDE; NITRIC OXIDE; NITROGEN DIOXIDE; ETHANE; HCN; oxidation; desorption; supported Pt catalyst; C3H6; NO; N2O; NO2; NOx; Environmental Molecular Sciences Laboratory

Citation Formats

Zhao, Haibo, Tonkyn, Russell G, Barlow, Stephan E, Koel, Bruce E, and Peden, Charles HF. Catalytic oxidation of HCN over a 0.5% Pt/Al2O3 catalyst. United States: N. p., 2006. Web. doi:10.1016/j.apcatb.2006.02.009.
Zhao, Haibo, Tonkyn, Russell G, Barlow, Stephan E, Koel, Bruce E, & Peden, Charles HF. Catalytic oxidation of HCN over a 0.5% Pt/Al2O3 catalyst. United States. doi:10.1016/j.apcatb.2006.02.009.
Zhao, Haibo, Tonkyn, Russell G, Barlow, Stephan E, Koel, Bruce E, and Peden, Charles HF. Mon . "Catalytic oxidation of HCN over a 0.5% Pt/Al2O3 catalyst". United States. doi:10.1016/j.apcatb.2006.02.009.
@article{osti_883676,
title = {Catalytic oxidation of HCN over a 0.5% Pt/Al2O3 catalyst},
author = {Zhao, Haibo and Tonkyn, Russell G and Barlow, Stephan E and Koel, Bruce E and Peden, Charles HF},
abstractNote = {The adsorption of HCN on, its catalytic oxidation with 6% O2 over 0.5% Pt/Al2O3, and the subsequent oxidation of strongly bound chemisorbed species upon heating were investigated. The observed N-containing products were N2O, NO and NO2, and some residual adsorbed N-containing species were oxidized to NO and NO2 during subsequent temperature programmed oxidation. Because N-atom balance could not be obtained after accounting for the quantities of each of these product species, we propose that N2 and was formed. Both the HCN conversion and the selectivity towards different N-containing products depend strongly on the reaction temperature and the composition of the reactant gas mixture. In particular, total HCN conversion reaches 95% above 250 C. Furthermore, the temperature of maximum HCN conversion to N2O is located between 200 and 250 C, while raising the reaction temperature increases the proportion of NOx in the products. The co-feeding of H2O and C3H6 had little, if any effect on the total HCN conversion, but C3H6 addition did increase the conversion to NO and decrease the conversion to NO2, perhaps due to the competing presence of adsorbed fragments of reductive C3H6. Evidence is also presented that introduction of NO and NO2 into the reactant gas mixture resulted in additional reaction pathways between these NOx species and HCN that provide for lean-NOx reduction coincident with HCN oxidation.},
doi = {10.1016/j.apcatb.2006.02.009},
journal = {Applied Catalysis. B, Environmental, 65(2006):282-290},
number = ,
volume = ,
place = {United States},
year = {Mon Mar 27 00:00:00 EST 2006},
month = {Mon Mar 27 00:00:00 EST 2006}
}