Accelerated deactivation studies of the natural-gas oxidation catalyst - Verifying the role of sulfur and elevated temperature in catalyst aging

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Accelerated deactivation studies of the natural-gas oxidation catalyst - Verifying the role of sulfur and elevated temperature in catalyst aging. / Honkanen, Mari; Kärkkäinen, Marja; Kolli, Tanja; Heikkinen, Olli; Viitanen, Ville; Zeng, Lunjie; Jiang, Hua; Kallinen, Kauko; Huuhtanen, Mika; Keiski, Riitta L.; Lahtinen, Jouko; Olsson, Eva; Vippola, Minnamari.

In: APPLIED CATALYSIS B-ENVIRONMENTAL, Vol. 182, 01.03.2016, p. 439-448.

Research output: Contribution to journalArticleScientificpeer-review

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Honkanen, M, Kärkkäinen, M, Kolli, T, Heikkinen, O, Viitanen, V, Zeng, L, Jiang, H, Kallinen, K, Huuhtanen, M, Keiski, RL, Lahtinen, J, Olsson, E & Vippola, M 2016, 'Accelerated deactivation studies of the natural-gas oxidation catalyst - Verifying the role of sulfur and elevated temperature in catalyst aging' APPLIED CATALYSIS B-ENVIRONMENTAL, vol. 182, pp. 439-448. https://doi.org/10.1016/j.apcatb.2015.09.054

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Honkanen, Mari ; Kärkkäinen, Marja ; Kolli, Tanja ; Heikkinen, Olli ; Viitanen, Ville ; Zeng, Lunjie ; Jiang, Hua ; Kallinen, Kauko ; Huuhtanen, Mika ; Keiski, Riitta L. ; Lahtinen, Jouko ; Olsson, Eva ; Vippola, Minnamari. / Accelerated deactivation studies of the natural-gas oxidation catalyst - Verifying the role of sulfur and elevated temperature in catalyst aging. In: APPLIED CATALYSIS B-ENVIRONMENTAL. 2016 ; Vol. 182. pp. 439-448.

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@article{37b653536c1b4099854dafb02df50fb7,
title = "Accelerated deactivation studies of the natural-gas oxidation catalyst - Verifying the role of sulfur and elevated temperature in catalyst aging",
abstract = "Accelerated deactivation, caused by thermal aging (TA) and/or sulfur + water poisoning (SW), of the PtPd/γ-Al2O3 natural-gas oxidation catalyst was studied. Thermal aging and poisoning treatments were performed separately and with varied combinations and comprehensive characterization of the catalyst was carried out after each step. The fresh catalyst has small, oxidized PtPd particles (<5 nm) uniformly distributed in the γ-alumina washcoat. After the SW-treatment, a small amount of bulk aluminum sulfate was observed near the slightly grown noble metal particles. During the thermal aging, γ-alumina changed to δ-/θ- and α-alumina. In addition, total decomposition of oxidized Pt and partly decomposition of oxidized Pd occurred resulting in the formation of the grown noble metal particles with a bimetallic PtPd core and a polycrystalline PdO shell. Also few, small (∼5 nm) bimetallic PtPd particles were still detected. In the TA + SW-treated catalyst with grown noble metal particles, a small amount of bulk aluminum sulfate was detected and it was randomly distributed over the noble metal particles and washcoat. The activity in the terms of methane conversion over the TA-, SW-, and SW + TA-treated catalysts was similar but it was decreased compared to the fresh catalyst. The activity of the TA + SW-treated catalyst was drastically decreased compared to the fresh catalyst due to significant morphological changes and aluminum sulfate formation.",
keywords = "Deactivation, Palladium, Platinum, Sulfur poisoning, Thermal aging",
author = "Mari Honkanen and Marja K{\"a}rkk{\"a}inen and Tanja Kolli and Olli Heikkinen and Ville Viitanen and Lunjie Zeng and Hua Jiang and Kauko Kallinen and Mika Huuhtanen and Keiski, {Riitta L.} and Jouko Lahtinen and Eva Olsson and Minnamari Vippola",
year = "2016",
month = "3",
day = "1",
doi = "10.1016/j.apcatb.2015.09.054",
language = "English",
volume = "182",
pages = "439--448",
journal = "APPLIED CATALYSIS B-ENVIRONMENTAL",
issn = "0926-3373",
publisher = "Elsevier BV",

}

RIS - Download

TY - JOUR

T1 - Accelerated deactivation studies of the natural-gas oxidation catalyst - Verifying the role of sulfur and elevated temperature in catalyst aging

AU - Honkanen, Mari

AU - Kärkkäinen, Marja

AU - Kolli, Tanja

AU - Heikkinen, Olli

AU - Viitanen, Ville

AU - Zeng, Lunjie

AU - Jiang, Hua

AU - Kallinen, Kauko

AU - Huuhtanen, Mika

AU - Keiski, Riitta L.

AU - Lahtinen, Jouko

AU - Olsson, Eva

AU - Vippola, Minnamari

PY - 2016/3/1

Y1 - 2016/3/1

N2 - Accelerated deactivation, caused by thermal aging (TA) and/or sulfur + water poisoning (SW), of the PtPd/γ-Al2O3 natural-gas oxidation catalyst was studied. Thermal aging and poisoning treatments were performed separately and with varied combinations and comprehensive characterization of the catalyst was carried out after each step. The fresh catalyst has small, oxidized PtPd particles (<5 nm) uniformly distributed in the γ-alumina washcoat. After the SW-treatment, a small amount of bulk aluminum sulfate was observed near the slightly grown noble metal particles. During the thermal aging, γ-alumina changed to δ-/θ- and α-alumina. In addition, total decomposition of oxidized Pt and partly decomposition of oxidized Pd occurred resulting in the formation of the grown noble metal particles with a bimetallic PtPd core and a polycrystalline PdO shell. Also few, small (∼5 nm) bimetallic PtPd particles were still detected. In the TA + SW-treated catalyst with grown noble metal particles, a small amount of bulk aluminum sulfate was detected and it was randomly distributed over the noble metal particles and washcoat. The activity in the terms of methane conversion over the TA-, SW-, and SW + TA-treated catalysts was similar but it was decreased compared to the fresh catalyst. The activity of the TA + SW-treated catalyst was drastically decreased compared to the fresh catalyst due to significant morphological changes and aluminum sulfate formation.

AB - Accelerated deactivation, caused by thermal aging (TA) and/or sulfur + water poisoning (SW), of the PtPd/γ-Al2O3 natural-gas oxidation catalyst was studied. Thermal aging and poisoning treatments were performed separately and with varied combinations and comprehensive characterization of the catalyst was carried out after each step. The fresh catalyst has small, oxidized PtPd particles (<5 nm) uniformly distributed in the γ-alumina washcoat. After the SW-treatment, a small amount of bulk aluminum sulfate was observed near the slightly grown noble metal particles. During the thermal aging, γ-alumina changed to δ-/θ- and α-alumina. In addition, total decomposition of oxidized Pt and partly decomposition of oxidized Pd occurred resulting in the formation of the grown noble metal particles with a bimetallic PtPd core and a polycrystalline PdO shell. Also few, small (∼5 nm) bimetallic PtPd particles were still detected. In the TA + SW-treated catalyst with grown noble metal particles, a small amount of bulk aluminum sulfate was detected and it was randomly distributed over the noble metal particles and washcoat. The activity in the terms of methane conversion over the TA-, SW-, and SW + TA-treated catalysts was similar but it was decreased compared to the fresh catalyst. The activity of the TA + SW-treated catalyst was drastically decreased compared to the fresh catalyst due to significant morphological changes and aluminum sulfate formation.

KW - Deactivation

KW - Palladium

KW - Platinum

KW - Sulfur poisoning

KW - Thermal aging

UR - http://www.scopus.com/inward/record.url?scp=84943638016&partnerID=8YFLogxK

U2 - 10.1016/j.apcatb.2015.09.054

DO - 10.1016/j.apcatb.2015.09.054

M3 - Article

VL - 182

SP - 439

EP - 448

JO - APPLIED CATALYSIS B-ENVIRONMENTAL

JF - APPLIED CATALYSIS B-ENVIRONMENTAL

SN - 0926-3373

ER -

ID: 1499432