The reactions of ethanol over M/CeO2 catalysts

Evidence of carbon-carbon bond dissociation at low temperatures over Rh/CeO2

A Yee, S J Morrison, Hicham Idriss

Research output: Contribution to journalArticle

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Abstract

The reactions of ethanol over Rh/CeO2 have been investigated using the techniques of temperature programmed desorption (TPD) and FT-IR spectroscopy, in addition to steady state catalytic tests. A comparison with previous studies of ethanol adsorption over Pd/CeO2 [J. Catal. 186 (1999) 279] and Pt/CeO2 [J. Catal. 191 (2000) 30] catalysts is presented. The apparent activation energy for the reaction was 49, 40, and 43 kJ mol(-1) for Rh/CeO2, Pd/CeO2 and Pt/CeO2. respectively, while the turnover number (TON) at 400 K was 5.9, 8.6 and 2.6, respectively. Surface compositions of catalysts were characterised by XPS. A decrease of the atomic O(ls)/Ce(3d) ratio of the CeO2 support indicates its partial reduction upon addition of the noble metal. The extent of reduction per metal atom was in the following order: Pt > Pd > Ph. FT-IR and TPD studies have shown that dehydrogenation of ethanol to acetaldehyde occurred over Pd/CeO2, Pt/CeO2 and Rh/CeO2. Moreover, Rh/CeO2 readily dissociated the C-C bond of ethanol at room temperature to form adsorbed CO (IR bands at 1904-2091 cm(-1)). This was corroborated by the low desorption temperature of CH4 over Rh/CeO2 (450 K) when compared to that of Pd/CeO2 (550 K) or Pt/CeO2 (585 K). (C) 2000 Elsevier Science B.V. All rights reserved.

Original languageEnglish
Pages (from-to)327-335
Number of pages9
JournalCatalysis Today
Volume63
Issue number2-4
DOIs
Publication statusPublished - 25 Dec 2000

Keywords

  • ethanol dehydrogenation
  • TPD-ethanol
  • Rh/CeO2-ethanol
  • ethanol-IR
  • C-C bond
  • SITU FT-IR
  • 3-WAY CATALYSTS
  • OXYGEN STORAGE
  • FORMIC-ACID
  • CERIA
  • ACETALDEHYDE
  • ADSORPTION
  • SURFACES
  • COPPER
  • CO
  • C-C bond

Cite this

The reactions of ethanol over M/CeO2 catalysts : Evidence of carbon-carbon bond dissociation at low temperatures over Rh/CeO2. / Yee, A ; Morrison, S J ; Idriss, Hicham.

In: Catalysis Today, Vol. 63, No. 2-4, 25.12.2000, p. 327-335.

Research output: Contribution to journalArticle

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N2 - The reactions of ethanol over Rh/CeO2 have been investigated using the techniques of temperature programmed desorption (TPD) and FT-IR spectroscopy, in addition to steady state catalytic tests. A comparison with previous studies of ethanol adsorption over Pd/CeO2 [J. Catal. 186 (1999) 279] and Pt/CeO2 [J. Catal. 191 (2000) 30] catalysts is presented. The apparent activation energy for the reaction was 49, 40, and 43 kJ mol(-1) for Rh/CeO2, Pd/CeO2 and Pt/CeO2. respectively, while the turnover number (TON) at 400 K was 5.9, 8.6 and 2.6, respectively. Surface compositions of catalysts were characterised by XPS. A decrease of the atomic O(ls)/Ce(3d) ratio of the CeO2 support indicates its partial reduction upon addition of the noble metal. The extent of reduction per metal atom was in the following order: Pt > Pd > Ph. FT-IR and TPD studies have shown that dehydrogenation of ethanol to acetaldehyde occurred over Pd/CeO2, Pt/CeO2 and Rh/CeO2. Moreover, Rh/CeO2 readily dissociated the C-C bond of ethanol at room temperature to form adsorbed CO (IR bands at 1904-2091 cm(-1)). This was corroborated by the low desorption temperature of CH4 over Rh/CeO2 (450 K) when compared to that of Pd/CeO2 (550 K) or Pt/CeO2 (585 K). (C) 2000 Elsevier Science B.V. All rights reserved.

AB - The reactions of ethanol over Rh/CeO2 have been investigated using the techniques of temperature programmed desorption (TPD) and FT-IR spectroscopy, in addition to steady state catalytic tests. A comparison with previous studies of ethanol adsorption over Pd/CeO2 [J. Catal. 186 (1999) 279] and Pt/CeO2 [J. Catal. 191 (2000) 30] catalysts is presented. The apparent activation energy for the reaction was 49, 40, and 43 kJ mol(-1) for Rh/CeO2, Pd/CeO2 and Pt/CeO2. respectively, while the turnover number (TON) at 400 K was 5.9, 8.6 and 2.6, respectively. Surface compositions of catalysts were characterised by XPS. A decrease of the atomic O(ls)/Ce(3d) ratio of the CeO2 support indicates its partial reduction upon addition of the noble metal. The extent of reduction per metal atom was in the following order: Pt > Pd > Ph. FT-IR and TPD studies have shown that dehydrogenation of ethanol to acetaldehyde occurred over Pd/CeO2, Pt/CeO2 and Rh/CeO2. Moreover, Rh/CeO2 readily dissociated the C-C bond of ethanol at room temperature to form adsorbed CO (IR bands at 1904-2091 cm(-1)). This was corroborated by the low desorption temperature of CH4 over Rh/CeO2 (450 K) when compared to that of Pd/CeO2 (550 K) or Pt/CeO2 (585 K). (C) 2000 Elsevier Science B.V. All rights reserved.

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KW - OXYGEN STORAGE

KW - FORMIC-ACID

KW - CERIA

KW - ACETALDEHYDE

KW - ADSORPTION

KW - SURFACES

KW - COPPER

KW - CO

KW - C-C bond

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DO - 10.1016/S0920-5861(00)00476-4

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EP - 335

JO - Catalysis Today

JF - Catalysis Today

SN - 0920-5861

IS - 2-4

ER -