Surface Science 459 (2000) 149–160
www.elsevier.nl/locate/susc
Reaction of CH
2
with adsorbed O on Ru ( 001 ) surface
A. Kis, J. Kiss, F. Solymosi *
Institute of Solid State and Radiochemistry, University of Szeged,
and Reaction Kinetics Research Group of the Hungarian Academy of Sciences1, P.O. Box 168, H-6701 Szeged, Hungary
Received 15 January 2000; accepted for publication 30 March 2000
Abstract
The reaction pathways of CH
2
in the presence of coadsorbed oxygen atoms on Ru(001) surface were investigated
by means of temperature-programmed desorption ( TPD), photoelectron spectroscopy ( XPS and UPS ) and work
function measurements. CH
2
species were produced by thermal and photoinduced dissociation of CH
2
I
2
. Preadsorbed
oxygen atoms markedly stabilized CMI bonds, shifted the desorption of CH
2
I
2
to higher temperatures and reacted
with CH
2
formed to give formaldehyde above 200 K. Adsorbed formate was also detected in the temperature range
of 300–450 K. The oxidation of surface species (CH
2
O, HCOO, C
x
H
y
) proceeded above 450 K, to produce CO, CO
2
,
and H
2
O. Illumination of the (CH
2
I
2
+O) coadsorbed layer initiated the dissociation of CH
2
I
2
, and induced the
reaction of CH
2
with O slightly above 110 K. © 2000 Elsevier Science B.V. All rights reserved.
Keywords: Aldehydes; Oxygen; Photochemistry; Ruthenium; Thermal desorption spectroscopy; Ultraviolet photoelectron spectro-
scopy; Work function measurements; X-ray photoelectron spectroscopy
1. Introduction In this case adsorbed O did not alter the dominant
pathways of the reaction of CH
2
formed above
200 K, e.g., the coupling of CH
2
into C
2
H
4
. The coupling and reactions of hydrocarbon
Formaldehyde formation was observed only when fragments (CH
2
, CH
3
,C
2
H
5
, etc.) with adsorbed
CH
2
was produced at 100 K by illumination of oxygen atoms represent important elementary
CH
2
I
2
+O/Cu(100) system.
steps in the selective and total oxidation of hydro-
In a previous paper we gave an account on the
carbons and also in the reforming of methane to
chemistry of CH
2
I
2
on the Ru(001) surface [10].
produce synthesis gas [1]. Previous works showed
The aim of the present work is to elaborate the
that CH
2
produced by the thermal and photodisso-
primary interaction of adsorbed CH
2
with atomi-
ciation of adsorbed CH
2
I
2
on Pt(111) [2], Rh(111)
cally adsorbed O on Ru(001) surface and to
[3–7] and Pd(100) [8] surfaces is readily combined
determine the routes of subsequent reactions in
with adsorbed oxygen atoms to give CH
2
O which
the coadsorbed layer. Unlike other platinum
is released in the gas phase after its formation.
metals, Ru is an excellent catalyst for the synthesis
Di erent results were obtained for Cu(100) [9].
of higher hydrocarbons, but it is markedly less
active and selective in the production of
* Corresponding author. Fax: +36 62 322 378.
oxygenated hydrocarbons. Therefore, it was inter-
E-mail address: fsolym@chem.u-szeged.hu ( F. Solymosi)
esting to see its e ect on the coupling of CH
2
1 This laboratory is a part of the Center for Catalysis, Surface
and Materials Science at the University of Szeged. with O.
0039-6028/00/$ - see front matter © 2000 Elsevier Science B.V. All rights reserved.
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