A multistep mechanism has been elucidated for the reduction of NOx in the presence of ethanol over silver-exchanged zeolite Y (Ag/Y). Ethanol reacts with O-2 and/or NO2 to form acetaldehyde at temperatures as low as 200 degrees C. Surface acetate ions, formed from the oxidation of acetalclehyde, react with NO2 to yield nitromethane, a critical intermediate in Subsequent deNOx chernistry. CN-, NC-, and NCO- are intermediates likely bound to silver ions. Both CN- and NC- are stable toward reaction under experimental conditions. A significant difference exists between the catalytic activities of Ag/Y and Ag/gamma-Al2O3; oxidation of ethanol to acetate at low temperature is significantly faster over Ag/Y than over Ag/gamma-Al2O3, and both NO2 and O-2 are effective oxidants over Ag/Y. With Ag/Y, pretreatment with either O-2 or H-2 does not affect the yield of N-2, which approaches 60% and remains constant for at least 5 h, making this catalyst promising for NOx reduction. (c) 2007 Elsevier Inc. All rights reserved.