In situ observation of a surface catalysed chemical reaction by fast X-ray photoelectron spectroscopy

A.F. Lee, K. Wilson, R.M. Lambert

Research output: Contribution to journalArticle

Abstract

The first application of time-resolved fast X-ray photoelectron spectroscopy as a chemically specific, quantitative probe for surface catalysed organic synthesis is described. The trimerisation of ethyne to benzene over a catalytically active Pd(111) surface has been followed in situ by C 1s core-level XPS. Ethyne reacts to form flat-lying (η) benzene above ∼150 K with a low activation barrier of ∼5 ± 1 kJ mol. At 280 K a tilted (η) benzene moeity is formed on the surface, some of which desorbs, the remainder interconverting to flat-lying benzene above 330 K. Unreacted ethyne is not present above 330 K. Flat-lying benzene begins desorbing ∼500 K, in competition with C-H bond cleavage to form a tilted (η or η) phenyl species. The latter may disproportionate yielding gaseous benzene and carbon.
Original languageEnglish
Pages (from-to)3095-3100
Number of pages6
JournalStudies in surface science and catalysis
Volume130
DOIs
Publication statusPublished - 2000

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Benzene
Chemical reactions
chemical reactions
X ray photoelectron spectroscopy
benzene
photoelectron spectroscopy
Acetylene
x rays
Core levels
cleavage
Carbon
Chemical activation
activation
probes
carbon
synthesis

Cite this

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title = "In situ observation of a surface catalysed chemical reaction by fast X-ray photoelectron spectroscopy",
abstract = "The first application of time-resolved fast X-ray photoelectron spectroscopy as a chemically specific, quantitative probe for surface catalysed organic synthesis is described. The trimerisation of ethyne to benzene over a catalytically active Pd(111) surface has been followed in situ by C 1s core-level XPS. Ethyne reacts to form flat-lying (η) benzene above ∼150 K with a low activation barrier of ∼5 ± 1 kJ mol. At 280 K a tilted (η) benzene moeity is formed on the surface, some of which desorbs, the remainder interconverting to flat-lying benzene above 330 K. Unreacted ethyne is not present above 330 K. Flat-lying benzene begins desorbing ∼500 K, in competition with C-H bond cleavage to form a tilted (η or η) phenyl species. The latter may disproportionate yielding gaseous benzene and carbon.",
author = "A.F. Lee and K. Wilson and R.M. Lambert",
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In situ observation of a surface catalysed chemical reaction by fast X-ray photoelectron spectroscopy. / Lee, A.F.; Wilson, K.; Lambert, R.M.

In: Studies in surface science and catalysis, Vol. 130 , 2000, p. 3095-3100.

Research output: Contribution to journalArticle

TY - JOUR

T1 - In situ observation of a surface catalysed chemical reaction by fast X-ray photoelectron spectroscopy

AU - Lee, A.F.

AU - Wilson, K.

AU - Lambert, R.M.

PY - 2000

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N2 - The first application of time-resolved fast X-ray photoelectron spectroscopy as a chemically specific, quantitative probe for surface catalysed organic synthesis is described. The trimerisation of ethyne to benzene over a catalytically active Pd(111) surface has been followed in situ by C 1s core-level XPS. Ethyne reacts to form flat-lying (η) benzene above ∼150 K with a low activation barrier of ∼5 ± 1 kJ mol. At 280 K a tilted (η) benzene moeity is formed on the surface, some of which desorbs, the remainder interconverting to flat-lying benzene above 330 K. Unreacted ethyne is not present above 330 K. Flat-lying benzene begins desorbing ∼500 K, in competition with C-H bond cleavage to form a tilted (η or η) phenyl species. The latter may disproportionate yielding gaseous benzene and carbon.

AB - The first application of time-resolved fast X-ray photoelectron spectroscopy as a chemically specific, quantitative probe for surface catalysed organic synthesis is described. The trimerisation of ethyne to benzene over a catalytically active Pd(111) surface has been followed in situ by C 1s core-level XPS. Ethyne reacts to form flat-lying (η) benzene above ∼150 K with a low activation barrier of ∼5 ± 1 kJ mol. At 280 K a tilted (η) benzene moeity is formed on the surface, some of which desorbs, the remainder interconverting to flat-lying benzene above 330 K. Unreacted ethyne is not present above 330 K. Flat-lying benzene begins desorbing ∼500 K, in competition with C-H bond cleavage to form a tilted (η or η) phenyl species. The latter may disproportionate yielding gaseous benzene and carbon.

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