0022-4766/14/5504-0757 © 2014 by Pleiades Publishing, Ltd. 757
Journal of Structural Chemistry. Vol. 55, No. 4, pp. 757-763, 2014.
Original Russian Text © 2014 M. Yu. Smirnov, A. V. Kalinkin, D. A. Nazimov, V. I. Bukhtiyarov, E. I. Vovk, E. Ozensoy.
AN XPS STUDY OF THE INTERACTION OF MODEL Ba/TiO
2
AND Ba/ZrO
2
NSR CATALYSTS WITH NO
2
M. Yu. Smirnov,
1
A. V. Kalinkin,
1
D. A. Nazimov,
1,2
V. I. Bukhtiyarov,
1,2
E. I. Vovk,
1,3
and E. Ozensoy
3
UDC 544.723.54:546.174
X-ray photoelectron spectroscopy is used to study the interaction of model NO
2
storage-reduction catalysts
(NSR catalysts) Ba/TiO
2
and Ba/ZrO
2
with NO
2
. The catalysts are prepared on the surface of ultrathin
Al
2
O
3
film substrates obtained by the FeCrAl alloy oxidation. It is shown that at room temperature the
model catalysts react with NO
2
with the successive formation of surface barium nitrite and nitrate. The NO
2
reduction with the formation of barium nitrite at the initial step of the interaction is assumed to be
accompanied by the oxidation of residual metallic barium and amorphous carbon impurity. It is found that
the formation of barium nitrate proceeds more efficiently on Ba/ZrO
2
rather than on Ba/TiO
2
.
DOI: 10.1134/S002247661404026X
Keywords: model NSR catalysts, reaction with NO
2
, barium nitrite, barium nitrate, X-ray photoelectron
spectroscopy.
INTRODUCTION
The purification of automobile exhaust gases from harmful impurities is an important practical problem for the
solution of which complex catalytic systems are applied. In the composition of these systems the NSR (NO
x
storage-
reduction) catalysts serve to neutralize nitrogen oxides [1]. They perform the following two functions: 1) oxidation of
nitrogen oxides with their fixation in the form of nitrates; 2) reduction of nitrates to molecular nitrogen. Ba-containing
compounds (BaO, Ba(OH)
2
or BaCO
3
) supported on γ-Al
2
O
3
have traditionally been used as the main component absorbing
NO
x
. In order to provide more efficient oxidation of NO to NO
2
and further to barium nitrate under oxidizing conditions and
also the subsequent reduction of nitrate to nitrogen under reducing conditions platinum is introduced into the catalyst
composition. A disadvantage of this type of NSR catalysts is their high susceptibility to poisoning by sulfur oxides (SO
x
) that
form in the exhaust gases as a result of oxidation of S-containing impurities in the fuel composition. It is found that the
interaction of the catalyst with sulfur oxides in the oxidizing medium leads to the formation of stable barium sulfates, as a
result of which the absorption capacity with respect to nitrogen oxides decreases [2, 3]. It was reported that the stability of the
NSR catalyst to poisoning by sulfur compounds could be increased by the replacement of the traditional material of the γ-
Al
2
O
3
substrate by other oxides, e.g. TiO
2
or ZrO
2
, in the presence of which barium sulfate easier decomposes in the reducing
medium [4-6].
Using X-ray photoelectron spectroscopy (XPS), we have previously investigated the interaction of NO
x
and SO
x
1
Boreskov Institute of Catalysis, Siberian Branch, Russian Academy of Sciences, Novosibirsk, Russia;
smirnov@catalysis.ru.
2
Novosibirsk State University, Russia.
3
Bilkent University, Bilkent, Ankara, Turkey. Translated from
Zhurnal Strukturnoi Khimii, Vol. 55, No. 4, pp. 791-797, July-August, 2014. Original article submitted January 22, 2014.