Highly dispersed supported ruthenium oxide as an aerobic catalyst for acetic acid synthesis

Anders Bo Laursen, Yury Gorbanev, Filippo Cavalca, Paolo Malacrida, Alan Kleiman-Shwarsctein, Søren Kegnæs, Anders Riisager, Ib Chorkendorff, Søren Dahl

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

The increasing need for shifting to renewable feedstocks in the chemical industry has driven research toward using green aerobic, selective oxidation reactions to produce bulk chemicals. Here, we report the use of a ruthenium mixed oxide/hydroxide (RuOx) on different support materials for the selective aerobic oxidation of ethanol to acetic acid. The RuOx was deposited onto different oxide supports using a new gas-phase reaction, which in all cases resulted in homogeneous nanoparticulate films. The RuOx particle size ranged from 0.3 to 1.5nm. The catalytic activity was evaluated on TiO2, Mg6Al2(CO3)(OH)16·4(H2O), MgAl2O4, Na2Ti6O13 nanotubes, ZnO, γ-Al2O3, WO3, CeO2, and Ce0.5Zr0.5O2 supports. The CeO2 supported RuOx had the highest activity, and selectivity toward acetic acid, of all the materials when normalized with respect to Ru-loading. This high activity was independent of the surface area of the support and the loading of RuOx under the tested conditions. This was attributed to the highly uniform size of the RuOx deposits, demonstrating that the deposition is suitable for producing small nanoparticles at high loadings. To elucidate the reason for the promotional effect of CeO2, Ce0.5Zr0.5O2 was investigated as a high oxygen storage capacity support, however, this did not result in higher catalytic activity. The high activity of CeO2 supports compared to the low activity ZnO appear correlated to the presence of high valence Ru(VI) species analogous to that observed in literature.
Original languageEnglish
JournalApplied Catalysis A: General
Volume433-434
Pages (from-to)243-250
ISSN0926-860X
DOIs
Publication statusPublished - 2012

Keywords

  • Heterogeneous catalysis
  • Ruthenium oxide
  • Aerobic ethanol oxidation
  • RuO4
  • Support effects
  • High-loading catalysts
  • Ru(VI) oxide

Cite this

Laursen, A. B., Gorbanev, Y., Cavalca, F., Malacrida, P., Kleiman-Shwarsctein, A., Kegnæs, S., ... Dahl, S. (2012). Highly dispersed supported ruthenium oxide as an aerobic catalyst for acetic acid synthesis. Applied Catalysis A: General, 433-434, 243-250. https://doi.org/10.1016/j.apcata.2012.05.025
Laursen, Anders Bo ; Gorbanev, Yury ; Cavalca, Filippo ; Malacrida, Paolo ; Kleiman-Shwarsctein, Alan ; Kegnæs, Søren ; Riisager, Anders ; Chorkendorff, Ib ; Dahl, Søren. / Highly dispersed supported ruthenium oxide as an aerobic catalyst for acetic acid synthesis. In: Applied Catalysis A: General. 2012 ; Vol. 433-434. pp. 243-250.
@article{fe04b1c5b8604f8bba9bc8a24e8edf42,
title = "Highly dispersed supported ruthenium oxide as an aerobic catalyst for acetic acid synthesis",
abstract = "The increasing need for shifting to renewable feedstocks in the chemical industry has driven research toward using green aerobic, selective oxidation reactions to produce bulk chemicals. Here, we report the use of a ruthenium mixed oxide/hydroxide (RuOx) on different support materials for the selective aerobic oxidation of ethanol to acetic acid. The RuOx was deposited onto different oxide supports using a new gas-phase reaction, which in all cases resulted in homogeneous nanoparticulate films. The RuOx particle size ranged from 0.3 to 1.5nm. The catalytic activity was evaluated on TiO2, Mg6Al2(CO3)(OH)16·4(H2O), MgAl2O4, Na2Ti6O13 nanotubes, ZnO, γ-Al2O3, WO3, CeO2, and Ce0.5Zr0.5O2 supports. The CeO2 supported RuOx had the highest activity, and selectivity toward acetic acid, of all the materials when normalized with respect to Ru-loading. This high activity was independent of the surface area of the support and the loading of RuOx under the tested conditions. This was attributed to the highly uniform size of the RuOx deposits, demonstrating that the deposition is suitable for producing small nanoparticles at high loadings. To elucidate the reason for the promotional effect of CeO2, Ce0.5Zr0.5O2 was investigated as a high oxygen storage capacity support, however, this did not result in higher catalytic activity. The high activity of CeO2 supports compared to the low activity ZnO appear correlated to the presence of high valence Ru(VI) species analogous to that observed in literature.",
keywords = "Heterogeneous catalysis, Ruthenium oxide, Aerobic ethanol oxidation, RuO4, Support effects, High-loading catalysts, Ru(VI) oxide",
author = "Laursen, {Anders Bo} and Yury Gorbanev and Filippo Cavalca and Paolo Malacrida and Alan Kleiman-Shwarsctein and S{\o}ren Kegn{\ae}s and Anders Riisager and Ib Chorkendorff and S{\o}ren Dahl",
year = "2012",
doi = "10.1016/j.apcata.2012.05.025",
language = "English",
volume = "433-434",
pages = "243--250",
journal = "Applied Catalysis A: General",
issn = "0926-860X",
publisher = "Elsevier",

}

Highly dispersed supported ruthenium oxide as an aerobic catalyst for acetic acid synthesis. / Laursen, Anders Bo; Gorbanev, Yury; Cavalca, Filippo; Malacrida, Paolo; Kleiman-Shwarsctein, Alan; Kegnæs, Søren; Riisager, Anders; Chorkendorff, Ib; Dahl, Søren.

In: Applied Catalysis A: General, Vol. 433-434, 2012, p. 243-250.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Highly dispersed supported ruthenium oxide as an aerobic catalyst for acetic acid synthesis

AU - Laursen, Anders Bo

AU - Gorbanev, Yury

AU - Cavalca, Filippo

AU - Malacrida, Paolo

AU - Kleiman-Shwarsctein, Alan

AU - Kegnæs, Søren

AU - Riisager, Anders

AU - Chorkendorff, Ib

AU - Dahl, Søren

PY - 2012

Y1 - 2012

N2 - The increasing need for shifting to renewable feedstocks in the chemical industry has driven research toward using green aerobic, selective oxidation reactions to produce bulk chemicals. Here, we report the use of a ruthenium mixed oxide/hydroxide (RuOx) on different support materials for the selective aerobic oxidation of ethanol to acetic acid. The RuOx was deposited onto different oxide supports using a new gas-phase reaction, which in all cases resulted in homogeneous nanoparticulate films. The RuOx particle size ranged from 0.3 to 1.5nm. The catalytic activity was evaluated on TiO2, Mg6Al2(CO3)(OH)16·4(H2O), MgAl2O4, Na2Ti6O13 nanotubes, ZnO, γ-Al2O3, WO3, CeO2, and Ce0.5Zr0.5O2 supports. The CeO2 supported RuOx had the highest activity, and selectivity toward acetic acid, of all the materials when normalized with respect to Ru-loading. This high activity was independent of the surface area of the support and the loading of RuOx under the tested conditions. This was attributed to the highly uniform size of the RuOx deposits, demonstrating that the deposition is suitable for producing small nanoparticles at high loadings. To elucidate the reason for the promotional effect of CeO2, Ce0.5Zr0.5O2 was investigated as a high oxygen storage capacity support, however, this did not result in higher catalytic activity. The high activity of CeO2 supports compared to the low activity ZnO appear correlated to the presence of high valence Ru(VI) species analogous to that observed in literature.

AB - The increasing need for shifting to renewable feedstocks in the chemical industry has driven research toward using green aerobic, selective oxidation reactions to produce bulk chemicals. Here, we report the use of a ruthenium mixed oxide/hydroxide (RuOx) on different support materials for the selective aerobic oxidation of ethanol to acetic acid. The RuOx was deposited onto different oxide supports using a new gas-phase reaction, which in all cases resulted in homogeneous nanoparticulate films. The RuOx particle size ranged from 0.3 to 1.5nm. The catalytic activity was evaluated on TiO2, Mg6Al2(CO3)(OH)16·4(H2O), MgAl2O4, Na2Ti6O13 nanotubes, ZnO, γ-Al2O3, WO3, CeO2, and Ce0.5Zr0.5O2 supports. The CeO2 supported RuOx had the highest activity, and selectivity toward acetic acid, of all the materials when normalized with respect to Ru-loading. This high activity was independent of the surface area of the support and the loading of RuOx under the tested conditions. This was attributed to the highly uniform size of the RuOx deposits, demonstrating that the deposition is suitable for producing small nanoparticles at high loadings. To elucidate the reason for the promotional effect of CeO2, Ce0.5Zr0.5O2 was investigated as a high oxygen storage capacity support, however, this did not result in higher catalytic activity. The high activity of CeO2 supports compared to the low activity ZnO appear correlated to the presence of high valence Ru(VI) species analogous to that observed in literature.

KW - Heterogeneous catalysis

KW - Ruthenium oxide

KW - Aerobic ethanol oxidation

KW - RuO4

KW - Support effects

KW - High-loading catalysts

KW - Ru(VI) oxide

U2 - 10.1016/j.apcata.2012.05.025

DO - 10.1016/j.apcata.2012.05.025

M3 - Journal article

VL - 433-434

SP - 243

EP - 250

JO - Applied Catalysis A: General

JF - Applied Catalysis A: General

SN - 0926-860X

ER -