A study of the mechanism for NOx reduction with ethanol on γ-alumina supported silver

Young Hoon Yeom; Meijun Li; Wolfgang M.H. Sachtler; Eric Weitz

doi:10.1016/j.jcat.2005.11.036

A study of the mechanism for NO_x reduction with ethanol on γ-alumina supported silver

Young Hoon Yeom, Meijun Li, Wolfgang M.H. Sachtler, Eric Weitz

Research output: Contribution to journal › Article › peer-review

63 Scopus citations

Abstract

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, NO_x 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 NO_x reduction with ethanol may be viable.

Original language	English
Pages (from-to)	100-110
Number of pages	11
Journal	Journal of Catalysis
Volume	238
Issue number	1
DOIs	https://doi.org/10.1016/j.jcat.2005.11.036
State	Published - Feb 15 2006
Externally published	Yes

Funding

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).

Funders	Funder number
Office of Basic Energy Sciences
U.S. Department of Energy	DE-FG02-03ER15457
Office of Science
American Chemical Society Petroleum Research Fund	41855-AC5
Chemical Sciences, Geosciences, and Biosciences Division

Keywords

Acetaldehyde
Aci-anion of nitromethane
Ethanol
Ethyl nitrite
FTIR
NO reduction
Nitromethane
Reactivity of surface acetate

Access to Document

10.1016/j.jcat.2005.11.036

Cite this

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title = "A study of the mechanism for NOx reduction with ethanol on γ-alumina supported silver",

abstract = "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.",

keywords = "Acetaldehyde, Aci-anion of nitromethane, Ethanol, Ethyl nitrite, FTIR, NO reduction, Nitromethane, Reactivity of surface acetate",

author = "Yeom, {Young Hoon} and Meijun Li and Sachtler, {Wolfgang M.H.} and Eric Weitz",

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AU - Yeom, Young Hoon

AU - Li, Meijun

AU - Sachtler, Wolfgang M.H.

AU - Weitz, Eric

PY - 2006/2/15

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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.

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