TY - JOUR
T1 - A study of the mechanism for NOx reduction with ethanol on γ-alumina supported silver
AU - Yeom, Young Hoon
AU - Li, Meijun
AU - Sachtler, Wolfgang M.H.
AU - Weitz, Eric
N1 - Funding Information:
This work was partially supported by the Donors of the American Chemical Society Petroleum Research Fund (grant 41855-AC5) and the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy (grant DE-FG02-03ER15457).
PY - 2006/2/15
Y1 - 2006/2/15
N2 - A multistep mechanism has been elucidated for the reduction of NO x in the presence of added ethanol over Ag/γ-Al 2O3 at 320°C. Under these conditions, ethanol principally reacts with oxygen to form acetaldehyde. Surface acetate ions, which are formed from adsorbed acetaldehyde, react with NO2 to yield nitromethane. Evidence is presented indicating that the aci-anion of nitromethane is an intermediate. In contrast, NOx reduction with ethanol over Ag/γ-Al2O3 at 200°C is inefficient, because surface acetate ions are much less reactive at 200°C than at 320°C. At 200°C, the dominant pathway for ethanol oxidation is reaction with NO2, producing ethyl nitrite, which decomposes into a number of products, including N2O, which is stable under reaction conditions. On the basis of these mechanistic data, conditions can be defined under which NOx reduction with ethanol may be viable.
AB - A multistep mechanism has been elucidated for the reduction of NO x in the presence of added ethanol over Ag/γ-Al 2O3 at 320°C. Under these conditions, ethanol principally reacts with oxygen to form acetaldehyde. Surface acetate ions, which are formed from adsorbed acetaldehyde, react with NO2 to yield nitromethane. Evidence is presented indicating that the aci-anion of nitromethane is an intermediate. In contrast, NOx reduction with ethanol over Ag/γ-Al2O3 at 200°C is inefficient, because surface acetate ions are much less reactive at 200°C than at 320°C. At 200°C, the dominant pathway for ethanol oxidation is reaction with NO2, producing ethyl nitrite, which decomposes into a number of products, including N2O, which is stable under reaction conditions. On the basis of these mechanistic data, conditions can be defined under which NOx reduction with ethanol may be viable.
KW - Acetaldehyde
KW - Aci-anion of nitromethane
KW - Ethanol
KW - Ethyl nitrite
KW - FTIR
KW - NO reduction
KW - Nitromethane
KW - Reactivity of surface acetate
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U2 - 10.1016/j.jcat.2005.11.036
DO - 10.1016/j.jcat.2005.11.036
M3 - Article
AN - SCOPUS:30944459416
SN - 0021-9517
VL - 238
SP - 100
EP - 110
JO - Journal of Catalysis
JF - Journal of Catalysis
IS - 1
ER -