Coupling of carbon monoxide molecules over oxygen-defected UO2(111) single crystal and thin film surfaces

S D Senanayake, G I N Waterhouse, Hicham Idriss

Research output: Contribution to journalArticle

16 Citations (Scopus)

Abstract

While coupling reactions of carbon-containing compounds are numerous in organometallic chemistry, they are very rare on well-defined solid surfaces. In this work we show that the reductive coupling of two molecules of carbon monoxide to C-2 compounds (acetylene and ethylene) could be achieved on oxygen-defected UO2(111) single crystal and thin film surfaces. This result allows in situ electron spectroscopic investigation of a typical organometallic reaction such as carbon coupling and extends it to heterogeneous catalysis and solids. By using high-resolution photoelectron spectroscopy (HRYPS) it was possible to track the changes in surface states of the U and 0 atoms as well as identify the intermediate of the reaction. Upon CO adsorption U cations in low oxidation states are oxidized to U4+ ions; this was accompanied by an increase of the O-to-U surface ratios. The HRYPS C 1s lines show the presence of adsorbed species assigned to diolate species (-OCH=CHO-) that are most likely the reaction intermediate in the coupling of two CO molecules to acetylene and ethylene.

Original languageEnglish
Pages (from-to)11141-11145
Number of pages5
JournalLangmuir
Volume21
Issue number24
DOIs
Publication statusPublished - 22 Nov 2005

Keywords

  • McMurry reaction
  • uranium oxides
  • CO
  • hydrogenation
  • formaldehyde
  • actinides
  • oxidation
  • catalysts
  • mechanism
  • pathways

Cite this

Coupling of carbon monoxide molecules over oxygen-defected UO2(111) single crystal and thin film surfaces. / Senanayake, S D ; Waterhouse, G I N ; Idriss, Hicham.

In: Langmuir, Vol. 21, No. 24, 22.11.2005, p. 11141-11145.

Research output: Contribution to journalArticle

Senanayake, S D ; Waterhouse, G I N ; Idriss, Hicham. / Coupling of carbon monoxide molecules over oxygen-defected UO2(111) single crystal and thin film surfaces. In: Langmuir. 2005 ; Vol. 21, No. 24. pp. 11141-11145.
@article{3a53ef078e3840c785e604b106796f72,
title = "Coupling of carbon monoxide molecules over oxygen-defected UO2(111) single crystal and thin film surfaces",
abstract = "While coupling reactions of carbon-containing compounds are numerous in organometallic chemistry, they are very rare on well-defined solid surfaces. In this work we show that the reductive coupling of two molecules of carbon monoxide to C-2 compounds (acetylene and ethylene) could be achieved on oxygen-defected UO2(111) single crystal and thin film surfaces. This result allows in situ electron spectroscopic investigation of a typical organometallic reaction such as carbon coupling and extends it to heterogeneous catalysis and solids. By using high-resolution photoelectron spectroscopy (HRYPS) it was possible to track the changes in surface states of the U and 0 atoms as well as identify the intermediate of the reaction. Upon CO adsorption U cations in low oxidation states are oxidized to U4+ ions; this was accompanied by an increase of the O-to-U surface ratios. The HRYPS C 1s lines show the presence of adsorbed species assigned to diolate species (-OCH=CHO-) that are most likely the reaction intermediate in the coupling of two CO molecules to acetylene and ethylene.",
keywords = "McMurry reaction, uranium oxides, CO, hydrogenation, formaldehyde, actinides, oxidation, catalysts, mechanism, pathways",
author = "Senanayake, {S D} and Waterhouse, {G I N} and Hicham Idriss",
year = "2005",
month = "11",
day = "22",
doi = "10.1021/la0519103",
language = "English",
volume = "21",
pages = "11141--11145",
journal = "Langmuir",
issn = "0743-7463",
publisher = "AMER CHEMICAL SOC",
number = "24",

}

TY - JOUR

T1 - Coupling of carbon monoxide molecules over oxygen-defected UO2(111) single crystal and thin film surfaces

AU - Senanayake, S D

AU - Waterhouse, G I N

AU - Idriss, Hicham

PY - 2005/11/22

Y1 - 2005/11/22

N2 - While coupling reactions of carbon-containing compounds are numerous in organometallic chemistry, they are very rare on well-defined solid surfaces. In this work we show that the reductive coupling of two molecules of carbon monoxide to C-2 compounds (acetylene and ethylene) could be achieved on oxygen-defected UO2(111) single crystal and thin film surfaces. This result allows in situ electron spectroscopic investigation of a typical organometallic reaction such as carbon coupling and extends it to heterogeneous catalysis and solids. By using high-resolution photoelectron spectroscopy (HRYPS) it was possible to track the changes in surface states of the U and 0 atoms as well as identify the intermediate of the reaction. Upon CO adsorption U cations in low oxidation states are oxidized to U4+ ions; this was accompanied by an increase of the O-to-U surface ratios. The HRYPS C 1s lines show the presence of adsorbed species assigned to diolate species (-OCH=CHO-) that are most likely the reaction intermediate in the coupling of two CO molecules to acetylene and ethylene.

AB - While coupling reactions of carbon-containing compounds are numerous in organometallic chemistry, they are very rare on well-defined solid surfaces. In this work we show that the reductive coupling of two molecules of carbon monoxide to C-2 compounds (acetylene and ethylene) could be achieved on oxygen-defected UO2(111) single crystal and thin film surfaces. This result allows in situ electron spectroscopic investigation of a typical organometallic reaction such as carbon coupling and extends it to heterogeneous catalysis and solids. By using high-resolution photoelectron spectroscopy (HRYPS) it was possible to track the changes in surface states of the U and 0 atoms as well as identify the intermediate of the reaction. Upon CO adsorption U cations in low oxidation states are oxidized to U4+ ions; this was accompanied by an increase of the O-to-U surface ratios. The HRYPS C 1s lines show the presence of adsorbed species assigned to diolate species (-OCH=CHO-) that are most likely the reaction intermediate in the coupling of two CO molecules to acetylene and ethylene.

KW - McMurry reaction

KW - uranium oxides

KW - CO

KW - hydrogenation

KW - formaldehyde

KW - actinides

KW - oxidation

KW - catalysts

KW - mechanism

KW - pathways

U2 - 10.1021/la0519103

DO - 10.1021/la0519103

M3 - Article

VL - 21

SP - 11141

EP - 11145

JO - Langmuir

JF - Langmuir

SN - 0743-7463

IS - 24

ER -