Sulfur poisoning and regeneration of Rh-ZSM-5 catalysts for total oxidation of methane

Yu Zhang; Peter Glarborg; Martin Peter Andersson; Keld Johansen; Thomas Klint Torp; Anker Degn Jensen; Jakob Munkholt Christensen

doi:10.1016/j.apcatb.2020.119176

Sulfur poisoning and regeneration of Rh-ZSM-5 catalysts for total oxidation of methane

Yu Zhang, Peter Glarborg, Martin Peter Andersson, Keld Johansen, Thomas Klint Torp, Anker Degn Jensen, Jakob Munkholt Christensen^*

^*Corresponding author for this work

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

31 Scopus citations

Abstract

The activity of Rh/ZSM-5 catalysts for methane oxidation was investigated under conditions simulating the exhaust from lean burning, natural gas fueled engines to evaluate the influence of reaction atmosphere on catalytic activity. The Rh-catalysts yield high methane conversion at conditions achievable in real exhaust systems, despite the inhibiting effects of H₂O and SO₂. The influence of temperature and SO₂ concentration (1−20 ppm) on the activity were studied. The deactivation caused by SO₂ was intensified with decreasing temperature and increasing SO₂ concentration, and the SO₂-poisoning could be modeled as the occupation of active sites following a Temkin adsorption isotherm. At 400 °C essentially full coverage of S-species was reached with 1−2 ppm of SO₂, but at 500 °C the coverage had decreased significantly, and considerable catalytic activity was preserved in the presence of SO₂. Significant activity was regenerated in SO₂-free gas, but the nature of the SO₂-free regeneration atmosphere was unimportant.

Original language	English
Article number	119176
Journal	Applied Catalysis B: Environmental
Volume	277
DOIs	https://doi.org/10.1016/j.apcatb.2020.119176
State	Published - 15 Nov 2020
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2020 Elsevier B.V.

Keywords

Catalyst
Methane
Oxidation
Rhodium
Sulfur tolerance

ASJC Scopus subject areas

Catalysis
General Environmental Science
Process Chemistry and Technology

UN SDGs

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

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10.1016/j.apcatb.2020.119176

Cite this

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title = "Sulfur poisoning and regeneration of Rh-ZSM-5 catalysts for total oxidation of methane",

abstract = "The activity of Rh/ZSM-5 catalysts for methane oxidation was investigated under conditions simulating the exhaust from lean burning, natural gas fueled engines to evaluate the influence of reaction atmosphere on catalytic activity. The Rh-catalysts yield high methane conversion at conditions achievable in real exhaust systems, despite the inhibiting effects of H2O and SO2. The influence of temperature and SO2 concentration (1−20 ppm) on the activity were studied. The deactivation caused by SO2 was intensified with decreasing temperature and increasing SO2 concentration, and the SO2-poisoning could be modeled as the occupation of active sites following a Temkin adsorption isotherm. At 400 °C essentially full coverage of S-species was reached with 1−2 ppm of SO2, but at 500 °C the coverage had decreased significantly, and considerable catalytic activity was preserved in the presence of SO2. Significant activity was regenerated in SO2-free gas, but the nature of the SO2-free regeneration atmosphere was unimportant.",

keywords = "Catalyst, Methane, Oxidation, Rhodium, Sulfur tolerance",

author = "Yu Zhang and Peter Glarborg and Andersson, \{Martin Peter\} and Keld Johansen and Torp, \{Thomas Klint\} and Jensen, \{Anker Degn\} and Christensen, \{Jakob Munkholt\}",

note = "Publisher Copyright: {\textcopyright} 2020 Elsevier B.V.",

year = "2020",

month = nov,

day = "15",

doi = "10.1016/j.apcatb.2020.119176",

language = "English",

volume = "277",

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T1 - Sulfur poisoning and regeneration of Rh-ZSM-5 catalysts for total oxidation of methane

AU - Zhang, Yu

AU - Glarborg, Peter

AU - Andersson, Martin Peter

AU - Johansen, Keld

AU - Torp, Thomas Klint

AU - Jensen, Anker Degn

AU - Christensen, Jakob Munkholt

PY - 2020/11/15

Y1 - 2020/11/15

N2 - The activity of Rh/ZSM-5 catalysts for methane oxidation was investigated under conditions simulating the exhaust from lean burning, natural gas fueled engines to evaluate the influence of reaction atmosphere on catalytic activity. The Rh-catalysts yield high methane conversion at conditions achievable in real exhaust systems, despite the inhibiting effects of H2O and SO2. The influence of temperature and SO2 concentration (1−20 ppm) on the activity were studied. The deactivation caused by SO2 was intensified with decreasing temperature and increasing SO2 concentration, and the SO2-poisoning could be modeled as the occupation of active sites following a Temkin adsorption isotherm. At 400 °C essentially full coverage of S-species was reached with 1−2 ppm of SO2, but at 500 °C the coverage had decreased significantly, and considerable catalytic activity was preserved in the presence of SO2. Significant activity was regenerated in SO2-free gas, but the nature of the SO2-free regeneration atmosphere was unimportant.

AB - The activity of Rh/ZSM-5 catalysts for methane oxidation was investigated under conditions simulating the exhaust from lean burning, natural gas fueled engines to evaluate the influence of reaction atmosphere on catalytic activity. The Rh-catalysts yield high methane conversion at conditions achievable in real exhaust systems, despite the inhibiting effects of H2O and SO2. The influence of temperature and SO2 concentration (1−20 ppm) on the activity were studied. The deactivation caused by SO2 was intensified with decreasing temperature and increasing SO2 concentration, and the SO2-poisoning could be modeled as the occupation of active sites following a Temkin adsorption isotherm. At 400 °C essentially full coverage of S-species was reached with 1−2 ppm of SO2, but at 500 °C the coverage had decreased significantly, and considerable catalytic activity was preserved in the presence of SO2. Significant activity was regenerated in SO2-free gas, but the nature of the SO2-free regeneration atmosphere was unimportant.

KW - Catalyst

KW - Methane

KW - Oxidation

KW - Rhodium

KW - Sulfur tolerance

UR - https://www.scopus.com/pages/publications/85086589939

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DO - 10.1016/j.apcatb.2020.119176

M3 - Article

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SN - 0926-3373

VL - 277

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

M1 - 119176

ER -

Sulfur poisoning and regeneration of Rh-ZSM-5 catalysts for total oxidation of methane

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

UN SDGs

Access to Document

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Cite this