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

Haldor Topsoe AS

Research output: Contribution to journal › Journal article › Research › peer-review

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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 SO₂was 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
Number of pages	8
ISSN	0926-3373
DOIs	https://doi.org/10.1016/j.apcatb.2020.119176
Publication status	Published - 2020

Keywords

Methane
Catalyst
Oxidation
Rhodium
Sulfur tolerance

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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 = "Methane, Catalyst, 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}",

year = "2020",

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

language = "English",

volume = "277",

journal = "Applied Catalysis B: Environmental",

issn = "0926-3373",

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TY - JOUR

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

Y1 - 2020

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 - Methane

KW - Catalyst

KW - Oxidation

KW - Rhodium

KW - Sulfur tolerance

U2 - 10.1016/j.apcatb.2020.119176

DO - 10.1016/j.apcatb.2020.119176

M3 - Journal article

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

Keywords

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