Impact of Mg on Pd-based methane oxidation catalysts for lean-burn natural gas emissions control

Sreshtha Sinha Majumdar; Melanie Moses-DeBusk; Dhruba Jyoti Deka; Michelle K. Kidder; Calvin R. Thomas; Josh A. Pihl

doi:10.1016/j.apcatb.2023.123253

Impact of Mg on Pd-based methane oxidation catalysts for lean-burn natural gas emissions control

Sreshtha Sinha Majumdar, Melanie Moses-DeBusk, Dhruba Jyoti Deka, Michelle K. Kidder, Calvin R. Thomas, Josh A. Pihl

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

5 Scopus citations

Abstract

More efficient lean-burn, natural gas engines are limited by greenhouse gas emissions due to methane oxidation catalysts (MOC) that suffer from water inhibition and high temperature activation. Herein, we report that the addition of Mg to supported 1 wt% Pd MOCs improved hydrothermal stability even after severe hydrothermal aging. The superior methane oxidation activity compared to the corresponding Mg-free catalyst was attributed to (1) influence of Mg during surface roughening and restructuring at 700 °C on metal-support interaction, (2) reducibility of PdOx sites and (3) preferential stabilization of active Pd (1 0 0) facets in the sample as was evidenced by H₂ TPR and CO TPD characterization experiments. Methane conversion under synthetic exhaust conditions relevant to natural gas, lean-burn engines were investigated. BET, TPR, CO pulse chemisorption followed by TPD provided valuable insights into the surface area, pore volume, reducibility, Pd dispersion and Pd particle size of the selected catalyst samples.

Original language	English
Article number	123253
Journal	Applied Catalysis B: Environmental
Volume	341
DOIs	https://doi.org/10.1016/j.apcatb.2023.123253
State	Published - Feb 2024

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 Kevin Stork and Gurpreet Singh at DOE VTO. This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05–00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).

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

Keywords

Alumina
Catalyst
Lean burn
Light-off
MOC
Magnesium
Methane oxidation
Natural gas
Palladium catalyst
Zeolite

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.apcatb.2023.123253

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title = "Impact of Mg on Pd-based methane oxidation catalysts for lean-burn natural gas emissions control",

abstract = "More efficient lean-burn, natural gas engines are limited by greenhouse gas emissions due to methane oxidation catalysts (MOC) that suffer from water inhibition and high temperature activation. Herein, we report that the addition of Mg to supported 1 wt% Pd MOCs improved hydrothermal stability even after severe hydrothermal aging. The superior methane oxidation activity compared to the corresponding Mg-free catalyst was attributed to (1) influence of Mg during surface roughening and restructuring at 700 °C on metal-support interaction, (2) reducibility of PdOx sites and (3) preferential stabilization of active Pd (1 0 0) facets in the sample as was evidenced by H2 TPR and CO TPD characterization experiments. Methane conversion under synthetic exhaust conditions relevant to natural gas, lean-burn engines were investigated. BET, TPR, CO pulse chemisorption followed by TPD provided valuable insights into the surface area, pore volume, reducibility, Pd dispersion and Pd particle size of the selected catalyst samples.",

keywords = "Alumina, Catalyst, Lean burn, Light-off, MOC, Magnesium, Methane oxidation, Natural gas, Palladium catalyst, Zeolite",

author = "{Sinha Majumdar}, Sreshtha and Melanie Moses-DeBusk and Deka, {Dhruba Jyoti} and Kidder, {Michelle K.} and Thomas, {Calvin R.} and Pihl, {Josh A.}",

note = "Publisher Copyright: {\textcopyright} 2023",

year = "2024",

month = feb,

doi = "10.1016/j.apcatb.2023.123253",

language = "English",

volume = "341",

journal = "Applied Catalysis B: Environmental",

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AU - Sinha Majumdar, Sreshtha

AU - Moses-DeBusk, Melanie

AU - Deka, Dhruba Jyoti

AU - Kidder, Michelle K.

AU - Thomas, Calvin R.

AU - Pihl, Josh A.

PY - 2024/2

Y1 - 2024/2

N2 - More efficient lean-burn, natural gas engines are limited by greenhouse gas emissions due to methane oxidation catalysts (MOC) that suffer from water inhibition and high temperature activation. Herein, we report that the addition of Mg to supported 1 wt% Pd MOCs improved hydrothermal stability even after severe hydrothermal aging. The superior methane oxidation activity compared to the corresponding Mg-free catalyst was attributed to (1) influence of Mg during surface roughening and restructuring at 700 °C on metal-support interaction, (2) reducibility of PdOx sites and (3) preferential stabilization of active Pd (1 0 0) facets in the sample as was evidenced by H2 TPR and CO TPD characterization experiments. Methane conversion under synthetic exhaust conditions relevant to natural gas, lean-burn engines were investigated. BET, TPR, CO pulse chemisorption followed by TPD provided valuable insights into the surface area, pore volume, reducibility, Pd dispersion and Pd particle size of the selected catalyst samples.

AB - More efficient lean-burn, natural gas engines are limited by greenhouse gas emissions due to methane oxidation catalysts (MOC) that suffer from water inhibition and high temperature activation. Herein, we report that the addition of Mg to supported 1 wt% Pd MOCs improved hydrothermal stability even after severe hydrothermal aging. The superior methane oxidation activity compared to the corresponding Mg-free catalyst was attributed to (1) influence of Mg during surface roughening and restructuring at 700 °C on metal-support interaction, (2) reducibility of PdOx sites and (3) preferential stabilization of active Pd (1 0 0) facets in the sample as was evidenced by H2 TPR and CO TPD characterization experiments. Methane conversion under synthetic exhaust conditions relevant to natural gas, lean-burn engines were investigated. BET, TPR, CO pulse chemisorption followed by TPD provided valuable insights into the surface area, pore volume, reducibility, Pd dispersion and Pd particle size of the selected catalyst samples.

KW - Alumina

KW - Catalyst

KW - Lean burn

KW - Light-off

KW - MOC

KW - Magnesium

KW - Methane oxidation

KW - Natural gas

KW - Palladium catalyst

KW - Zeolite

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JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

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ER -

Impact of Mg on Pd-based methane oxidation catalysts for lean-burn natural gas emissions control

Abstract

Funding

Keywords

UN SDGs

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