TPR and FT-IR studies on carbonyl cluster derived Co-Ru/SiO2 catalysts

Jari Kiviaho (Corresponding Author), Marita Niemelä, Matti Reinikainen, Tapani Pakkanen

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Abstract

The decomposition of the Co4-nRunHn(CO)xSiO2 (where n = 0–4 and x = 12 or 13) and (CO4(CO)12 + Ru4H4(CO)12)/SiO2 catalysts was studied by temperature-programmed reduction (TPR) and in-situ diffuse reflectance FT-IR techniques. The FT-IR studies suggested that Ru4H4(CO)12, CoRu3H3(CO)12 and Co3RuH(CO)12 clusters on silica were more stable in room temperature than Co4(CO)12, Co2Ru2H2(CO)12 and Co2Ru2(CO)13 clusters. The FT-IR measurements also indicated that all precursors decomposed during thermal treatment, but the distinct temperature of decarbonylation was not necessarily noticeable. On the other hand, in TPR, the CO desorption peak maxima for the precursors were 123°C for (Co4(CO)12 + Ru4H4(CO)12), 127°C for CoRu3H3(CO)12, 133°C for Co2Ru2(CO)13, 137°C for Co4(CO)12, 144°C for Co2Ru2H2(CO)12, 148°C for Co3RuH(CO)12 and 185°C for Ru4H4(CO)12. Thus, the catalysts with 1:1 atomic ratio of Co:Ru decarbonylated at different temperatures. The temperature of decarbonylation was lower for Co2Ru2(CO)13/SiO2 than for Co2Ru2H2(CO)12/SiO2, i.e., cobalt influenced the decarbonylation more in the first case. In accordance, the CO hydrogenation activity and selectivity results for the decarbonylated catalysts suggested that Co2Ru2(CO)13/SiO2 exhibited the characteristics of cobalt more than Co2Ru2H2(CO)12/SiO2 did.
Original languageEnglish
Pages (from-to)353 - 372
Number of pages20
JournalApplied Catalysis A: General
Volume149
Issue number2
DOIs
Publication statusPublished - 1997
MoE publication typeA1 Journal article-refereed

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Catalysts
Cobalt
Temperature
Catalyst selectivity
Silicon Dioxide
Hydrogenation
Catalyst activity
Desorption
Heat treatment
Silica
Decomposition

Cite this

Kiviaho, Jari ; Niemelä, Marita ; Reinikainen, Matti ; Pakkanen, Tapani. / TPR and FT-IR studies on carbonyl cluster derived Co-Ru/SiO2 catalysts. In: Applied Catalysis A: General. 1997 ; Vol. 149, No. 2. pp. 353 - 372.
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title = "TPR and FT-IR studies on carbonyl cluster derived Co-Ru/SiO2 catalysts",
abstract = "The decomposition of the Co4-nRunHn(CO)xSiO2 (where n = 0–4 and x = 12 or 13) and (CO4(CO)12 + Ru4H4(CO)12)/SiO2 catalysts was studied by temperature-programmed reduction (TPR) and in-situ diffuse reflectance FT-IR techniques. The FT-IR studies suggested that Ru4H4(CO)12, CoRu3H3(CO)12 and Co3RuH(CO)12 clusters on silica were more stable in room temperature than Co4(CO)12, Co2Ru2H2(CO)12 and Co2Ru2(CO)13 clusters. The FT-IR measurements also indicated that all precursors decomposed during thermal treatment, but the distinct temperature of decarbonylation was not necessarily noticeable. On the other hand, in TPR, the CO desorption peak maxima for the precursors were 123°C for (Co4(CO)12 + Ru4H4(CO)12), 127°C for CoRu3H3(CO)12, 133°C for Co2Ru2(CO)13, 137°C for Co4(CO)12, 144°C for Co2Ru2H2(CO)12, 148°C for Co3RuH(CO)12 and 185°C for Ru4H4(CO)12. Thus, the catalysts with 1:1 atomic ratio of Co:Ru decarbonylated at different temperatures. The temperature of decarbonylation was lower for Co2Ru2(CO)13/SiO2 than for Co2Ru2H2(CO)12/SiO2, i.e., cobalt influenced the decarbonylation more in the first case. In accordance, the CO hydrogenation activity and selectivity results for the decarbonylated catalysts suggested that Co2Ru2(CO)13/SiO2 exhibited the characteristics of cobalt more than Co2Ru2H2(CO)12/SiO2 did.",
author = "Jari Kiviaho and Marita Niemel{\"a} and Matti Reinikainen and Tapani Pakkanen",
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journal = "Applied Catalysis A: General",
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TPR and FT-IR studies on carbonyl cluster derived Co-Ru/SiO2 catalysts. / Kiviaho, Jari (Corresponding Author); Niemelä, Marita; Reinikainen, Matti; Pakkanen, Tapani.

In: Applied Catalysis A: General, Vol. 149, No. 2, 1997, p. 353 - 372.

Research output: Contribution to journalArticleScientificpeer-review

TY - JOUR

T1 - TPR and FT-IR studies on carbonyl cluster derived Co-Ru/SiO2 catalysts

AU - Kiviaho, Jari

AU - Niemelä, Marita

AU - Reinikainen, Matti

AU - Pakkanen, Tapani

PY - 1997

Y1 - 1997

N2 - The decomposition of the Co4-nRunHn(CO)xSiO2 (where n = 0–4 and x = 12 or 13) and (CO4(CO)12 + Ru4H4(CO)12)/SiO2 catalysts was studied by temperature-programmed reduction (TPR) and in-situ diffuse reflectance FT-IR techniques. The FT-IR studies suggested that Ru4H4(CO)12, CoRu3H3(CO)12 and Co3RuH(CO)12 clusters on silica were more stable in room temperature than Co4(CO)12, Co2Ru2H2(CO)12 and Co2Ru2(CO)13 clusters. The FT-IR measurements also indicated that all precursors decomposed during thermal treatment, but the distinct temperature of decarbonylation was not necessarily noticeable. On the other hand, in TPR, the CO desorption peak maxima for the precursors were 123°C for (Co4(CO)12 + Ru4H4(CO)12), 127°C for CoRu3H3(CO)12, 133°C for Co2Ru2(CO)13, 137°C for Co4(CO)12, 144°C for Co2Ru2H2(CO)12, 148°C for Co3RuH(CO)12 and 185°C for Ru4H4(CO)12. Thus, the catalysts with 1:1 atomic ratio of Co:Ru decarbonylated at different temperatures. The temperature of decarbonylation was lower for Co2Ru2(CO)13/SiO2 than for Co2Ru2H2(CO)12/SiO2, i.e., cobalt influenced the decarbonylation more in the first case. In accordance, the CO hydrogenation activity and selectivity results for the decarbonylated catalysts suggested that Co2Ru2(CO)13/SiO2 exhibited the characteristics of cobalt more than Co2Ru2H2(CO)12/SiO2 did.

AB - The decomposition of the Co4-nRunHn(CO)xSiO2 (where n = 0–4 and x = 12 or 13) and (CO4(CO)12 + Ru4H4(CO)12)/SiO2 catalysts was studied by temperature-programmed reduction (TPR) and in-situ diffuse reflectance FT-IR techniques. The FT-IR studies suggested that Ru4H4(CO)12, CoRu3H3(CO)12 and Co3RuH(CO)12 clusters on silica were more stable in room temperature than Co4(CO)12, Co2Ru2H2(CO)12 and Co2Ru2(CO)13 clusters. The FT-IR measurements also indicated that all precursors decomposed during thermal treatment, but the distinct temperature of decarbonylation was not necessarily noticeable. On the other hand, in TPR, the CO desorption peak maxima for the precursors were 123°C for (Co4(CO)12 + Ru4H4(CO)12), 127°C for CoRu3H3(CO)12, 133°C for Co2Ru2(CO)13, 137°C for Co4(CO)12, 144°C for Co2Ru2H2(CO)12, 148°C for Co3RuH(CO)12 and 185°C for Ru4H4(CO)12. Thus, the catalysts with 1:1 atomic ratio of Co:Ru decarbonylated at different temperatures. The temperature of decarbonylation was lower for Co2Ru2(CO)13/SiO2 than for Co2Ru2H2(CO)12/SiO2, i.e., cobalt influenced the decarbonylation more in the first case. In accordance, the CO hydrogenation activity and selectivity results for the decarbonylated catalysts suggested that Co2Ru2(CO)13/SiO2 exhibited the characteristics of cobalt more than Co2Ru2H2(CO)12/SiO2 did.

U2 - 10.1016/S0926-860X(96)00279-7

DO - 10.1016/S0926-860X(96)00279-7

M3 - Article

VL - 149

SP - 353

EP - 372

JO - Applied Catalysis A: General

JF - Applied Catalysis A: General

SN - 0926-860X

IS - 2

ER -