Reactivity of net-zero carbon alcohol fuels and their corresponding aldehyde intermediates on PGM-based commercial oxidation catalysts for lean-burn emissions control

Sreshtha Sinha Majumdar; Md Masudur Rahman; Josh A. Pihl

doi:10.1016/j.cej.2024.158490

Reactivity of net-zero carbon alcohol fuels and their corresponding aldehyde intermediates on PGM-based commercial oxidation catalysts for lean-burn emissions control

Sreshtha Sinha Majumdar, Md Masudur Rahman, Josh A. Pihl

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

Abstract

Alcohol net-zero carbon fuels will play a significant role in decarbonization of the hard-to-electrify transportation sectors. However, the combustion process in alcohol-fueled engines generate toxic aldehydes. For commercialization of net-zero carbon fuels on engines, compliance with the stringent U.S. EPA regulations is necessary. This contribution focuses on reactivity of alcohols and aldehydes on commercial diesel oxidation catalysts (DOC) to inform selection of future net-zero carbon fuels. Alcohol (and aldehyde) light-off temperatures were measured on aged DOCs under full synthetic engine-exhaust conditions. Methanol was the most reactive, while ethanol completely oxidized at higher temperatures. Alcohols typically formed less reactive aldehyde intermediates. DRIFTS revealed strongly adsorbing surface formates and acetates during methanol and ethanol oxidation, respectively, resulting in inhibition effects. Preliminary alcohol oxidation mechanisms combining flow reactor and DRIFTS observations are presented. Aldehydes inhibited CO oxidation. Minimal N₂O formation was observed for the alcohols investigated.

Original language	English
Article number	158490
Journal	Chemical Engineering Journal
Volume	503
DOIs	https://doi.org/10.1016/j.cej.2024.158490
State	Published - Jan 1 2025

Funding

This research was supported by the Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy (EERE) and Vehicle Technologies Office (VTO) and used resources at the National Transportation Research Center, a DOE-EERE User Facility at Oak Ridge National Laboratory. The authors gratefully acknowledge guidance and support from Nicholas Hansford, Siddiq Khan, Kevin Stork, and Gurpreet Singh at DOE VTO. The authors also acknowledge the discussions and guidance from Dave Montgomery, Kenth Svennson and Josh Ratts at Caterpillar Inc.

Funders	Funder number
Office of Energy Efficiency and Renewable Energy
Oak Ridge National Laboratory
DOE-EERE
Vehicle Technologies Office
U.S. Department of Energy

Keywords

Alcohol oxidation
Aldehyde oxidation
Diesel oxidation catalysts
Formaldehyde & acetaldehyde
Light off
Methanol & ethanol
Net zero carbon fuels

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10.1016/j.cej.2024.158490

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@article{66135d76df64477b8f326c1b5b291ee8,

title = "Reactivity of net-zero carbon alcohol fuels and their corresponding aldehyde intermediates on PGM-based commercial oxidation catalysts for lean-burn emissions control",

abstract = "Alcohol net-zero carbon fuels will play a significant role in decarbonization of the hard-to-electrify transportation sectors. However, the combustion process in alcohol-fueled engines generate toxic aldehydes. For commercialization of net-zero carbon fuels on engines, compliance with the stringent U.S. EPA regulations is necessary. This contribution focuses on reactivity of alcohols and aldehydes on commercial diesel oxidation catalysts (DOC) to inform selection of future net-zero carbon fuels. Alcohol (and aldehyde) light-off temperatures were measured on aged DOCs under full synthetic engine-exhaust conditions. Methanol was the most reactive, while ethanol completely oxidized at higher temperatures. Alcohols typically formed less reactive aldehyde intermediates. DRIFTS revealed strongly adsorbing surface formates and acetates during methanol and ethanol oxidation, respectively, resulting in inhibition effects. Preliminary alcohol oxidation mechanisms combining flow reactor and DRIFTS observations are presented. Aldehydes inhibited CO oxidation. Minimal N2O formation was observed for the alcohols investigated.",

keywords = "Alcohol oxidation, Aldehyde oxidation, Diesel oxidation catalysts, Formaldehyde & acetaldehyde, Light off, Methanol & ethanol, Net zero carbon fuels",

author = "{Sinha Majumdar}, Sreshtha and Rahman, {Md Masudur} and Pihl, {Josh A.}",

note = "Publisher Copyright: {\textcopyright} 2024",

year = "2025",

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doi = "10.1016/j.cej.2024.158490",

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AU - Sinha Majumdar, Sreshtha

AU - Rahman, Md Masudur

AU - Pihl, Josh A.

PY - 2025/1/1

Y1 - 2025/1/1

N2 - Alcohol net-zero carbon fuels will play a significant role in decarbonization of the hard-to-electrify transportation sectors. However, the combustion process in alcohol-fueled engines generate toxic aldehydes. For commercialization of net-zero carbon fuels on engines, compliance with the stringent U.S. EPA regulations is necessary. This contribution focuses on reactivity of alcohols and aldehydes on commercial diesel oxidation catalysts (DOC) to inform selection of future net-zero carbon fuels. Alcohol (and aldehyde) light-off temperatures were measured on aged DOCs under full synthetic engine-exhaust conditions. Methanol was the most reactive, while ethanol completely oxidized at higher temperatures. Alcohols typically formed less reactive aldehyde intermediates. DRIFTS revealed strongly adsorbing surface formates and acetates during methanol and ethanol oxidation, respectively, resulting in inhibition effects. Preliminary alcohol oxidation mechanisms combining flow reactor and DRIFTS observations are presented. Aldehydes inhibited CO oxidation. Minimal N2O formation was observed for the alcohols investigated.

AB - Alcohol net-zero carbon fuels will play a significant role in decarbonization of the hard-to-electrify transportation sectors. However, the combustion process in alcohol-fueled engines generate toxic aldehydes. For commercialization of net-zero carbon fuels on engines, compliance with the stringent U.S. EPA regulations is necessary. This contribution focuses on reactivity of alcohols and aldehydes on commercial diesel oxidation catalysts (DOC) to inform selection of future net-zero carbon fuels. Alcohol (and aldehyde) light-off temperatures were measured on aged DOCs under full synthetic engine-exhaust conditions. Methanol was the most reactive, while ethanol completely oxidized at higher temperatures. Alcohols typically formed less reactive aldehyde intermediates. DRIFTS revealed strongly adsorbing surface formates and acetates during methanol and ethanol oxidation, respectively, resulting in inhibition effects. Preliminary alcohol oxidation mechanisms combining flow reactor and DRIFTS observations are presented. Aldehydes inhibited CO oxidation. Minimal N2O formation was observed for the alcohols investigated.

KW - Alcohol oxidation

KW - Aldehyde oxidation

KW - Diesel oxidation catalysts

KW - Formaldehyde & acetaldehyde

KW - Light off

KW - Methanol & ethanol

KW - Net zero carbon fuels

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JO - Chemical Engineering Journal

JF - Chemical Engineering Journal

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Reactivity of net-zero carbon alcohol fuels and their corresponding aldehyde intermediates on PGM-based commercial oxidation catalysts for lean-burn emissions control

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