Complex redox chemistry on the RuO2(110) surface: experiment and theory

S Wendt, A P Seitsonen, Y D Kim, M Knapp, Hicham Idriss, H Over

Research output: Contribution to journalArticle

50 Citations (Scopus)

Abstract

Employing temperature-programmed reaction and desorption, we studied the reduction of RuO2(110) by CO exposure under various conditions. RuO2(110) is mildly and heavily reduced by CO exposure when the reaction temperature is below 400 K and above 500 K, respectively. The restoration of the reduced RuO2(110) surface was investigated by low energy electron diffraction and Auger electron spectroscopy. CO molecules adsorb over the under-coordinated Ru atoms and recombine with the under-coordinated lattice O atoms on the RuO2(110) surface. The initial conversion probability for this process is as high as 80%. The mildly reduced RuO2(110) surface is characterized by the removal of bridging O atoms. A mildly reduced surface, where all bridging O atoms are consumed, is inactive in oxidizing CO below 450 K. However, temperature treatment (greater than or equal to550 K) or oxygen exposure at room temperature is able to reactivate the mildly reduced surface. Heavy reduction of RuO2(110) leads to a roughening of the surface, which is partly restored by annealing at 700-800 K. The activation barriers of various reaction pathways, motivated by the present experiments, are determined by state-of-the-art density function theory calculations and compared with experiments. (C) 2002 Elsevier Science B.V. All rights reserved.

Original languageEnglish
Pages (from-to)137-152
Number of pages16
JournalSurface Science Reports
Volume505
Issue number1-3
Publication statusPublished - 1 May 2002

Keywords

  • thermal desorption
  • surface chemical reaction
  • ruthenium
  • carbon monoxide
  • low energy electron diffraction (LEED)
  • Auger electron spectroscopy
  • CARBON-MONOXIDE OXIDATION
  • CO OXIDATION
  • SINGLE-CRYSTAL
  • OXYGEN
  • REACTIVITY
  • RU(0001)
  • KINETICS
  • PT(111)
  • RUO2

Cite this

Wendt, S., Seitsonen, A. P., Kim, Y. D., Knapp, M., Idriss, H., & Over, H. (2002). Complex redox chemistry on the RuO2(110) surface: experiment and theory. Surface Science Reports, 505(1-3), 137-152.

Complex redox chemistry on the RuO2(110) surface: experiment and theory. / Wendt, S ; Seitsonen, A P ; Kim, Y D ; Knapp, M ; Idriss, Hicham; Over, H .

In: Surface Science Reports, Vol. 505, No. 1-3, 01.05.2002, p. 137-152.

Research output: Contribution to journalArticle

Wendt, S, Seitsonen, AP, Kim, YD, Knapp, M, Idriss, H & Over, H 2002, 'Complex redox chemistry on the RuO2(110) surface: experiment and theory', Surface Science Reports, vol. 505, no. 1-3, pp. 137-152.
Wendt S, Seitsonen AP, Kim YD, Knapp M, Idriss H, Over H. Complex redox chemistry on the RuO2(110) surface: experiment and theory. Surface Science Reports. 2002 May 1;505(1-3):137-152.
Wendt, S ; Seitsonen, A P ; Kim, Y D ; Knapp, M ; Idriss, Hicham ; Over, H . / Complex redox chemistry on the RuO2(110) surface: experiment and theory. In: Surface Science Reports. 2002 ; Vol. 505, No. 1-3. pp. 137-152.
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N2 - Employing temperature-programmed reaction and desorption, we studied the reduction of RuO2(110) by CO exposure under various conditions. RuO2(110) is mildly and heavily reduced by CO exposure when the reaction temperature is below 400 K and above 500 K, respectively. The restoration of the reduced RuO2(110) surface was investigated by low energy electron diffraction and Auger electron spectroscopy. CO molecules adsorb over the under-coordinated Ru atoms and recombine with the under-coordinated lattice O atoms on the RuO2(110) surface. The initial conversion probability for this process is as high as 80%. The mildly reduced RuO2(110) surface is characterized by the removal of bridging O atoms. A mildly reduced surface, where all bridging O atoms are consumed, is inactive in oxidizing CO below 450 K. However, temperature treatment (greater than or equal to550 K) or oxygen exposure at room temperature is able to reactivate the mildly reduced surface. Heavy reduction of RuO2(110) leads to a roughening of the surface, which is partly restored by annealing at 700-800 K. The activation barriers of various reaction pathways, motivated by the present experiments, are determined by state-of-the-art density function theory calculations and compared with experiments. (C) 2002 Elsevier Science B.V. All rights reserved.

AB - Employing temperature-programmed reaction and desorption, we studied the reduction of RuO2(110) by CO exposure under various conditions. RuO2(110) is mildly and heavily reduced by CO exposure when the reaction temperature is below 400 K and above 500 K, respectively. The restoration of the reduced RuO2(110) surface was investigated by low energy electron diffraction and Auger electron spectroscopy. CO molecules adsorb over the under-coordinated Ru atoms and recombine with the under-coordinated lattice O atoms on the RuO2(110) surface. The initial conversion probability for this process is as high as 80%. The mildly reduced RuO2(110) surface is characterized by the removal of bridging O atoms. A mildly reduced surface, where all bridging O atoms are consumed, is inactive in oxidizing CO below 450 K. However, temperature treatment (greater than or equal to550 K) or oxygen exposure at room temperature is able to reactivate the mildly reduced surface. Heavy reduction of RuO2(110) leads to a roughening of the surface, which is partly restored by annealing at 700-800 K. The activation barriers of various reaction pathways, motivated by the present experiments, are determined by state-of-the-art density function theory calculations and compared with experiments. (C) 2002 Elsevier Science B.V. All rights reserved.

KW - thermal desorption

KW - surface chemical reaction

KW - ruthenium

KW - carbon monoxide

KW - low energy electron diffraction (LEED)

KW - Auger electron spectroscopy

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KW - SINGLE-CRYSTAL

KW - OXYGEN

KW - REACTIVITY

KW - RU(0001)

KW - KINETICS

KW - PT(111)

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