Advances in Chemical Engineering and Science, 2011, 1, 169-175
doi:10.4236/aces.2011.14025 Published Online October 2011 (http://www.SciRP.org/journal/aces)
Copyright © 2011 SciRes. ACES
Structured Perovskite-Based Oxides: Use in the Combined
Methane Reforming
Adriana García
1
, Norymar Becerra
1
, Luis García
1
, Ini Ojeda
1
, Estefanía López
1
,
Carmen M. López
2
, Mireya R. Goldwasser
2
1
Facultad de Ingeniería, Universidad Central de Venezuela, Caracas, Venezuela
2
Facultad de Ciencias, Universidad Central de Venezuela, Caracas, Venezuela
E-mail: adriana.ucv@gmail.com
Recieved July 16, 2011; revised August 10, 2011; accepted August 30, 2011
Abstract
The behavior of metallic structured perovskite-based catalysts was evaluated in the combined methane re-
forming reaction with CO
2
-O
2
. The reaction conditions were established by varying the reaction temperature
and reactor input composition in the range of 650 to 850˚C and CH
4
/CO
2
ratio 1 to 5, respectively. The re-
sults of the catalytic tests at 750˚C showed a positive effect of the metallic structure, producing higher con-
versions and H
2
/CO ratios in the products compare to that obtained with the powder catalyst.
Keywords: Methane Reforming, Perovskites, Syngas Production, Structured Catalysts
1. Introduction
Catalytic steam methane reforming (SMR) is the princi-
pal commercial technology for syngas production [1-3].
This process has the advantage of using natural gas as
feedstock, which is an abundant material available at low
cost, in addition to producing a high H
2
/CO ratio, ac-
cording Equation (1):
4 2 2 r
CH HO CO 3H (H 206 kJ/mol) (1)
Since this reaction (Equation (1)) is highly endother-
mic, it is necessary to use high temperature and pressures.
These severe reaction conditions cause catalyst deactiva-
tion due to carbon deposits on the catalyst surface. The
possibility of combining exothermic oxidation of meth-
ane (Equations (2) and (3)) with the SMR has emerged
as an alternative to overcome this disadvantage. The pur-
pose is to provide the heat required by the endothermic
reactions, from the heat released by the exothermic reac-
tions [4-6]. In the same way, methane reforming with
carbon dioxide, known as dry methane reforming (DMR),
to produce syngas with a H
2
/CO ratio equal to unity
(Equation (4)), is one of the methods that utilize one the
major greenhouse contributor. There are abundant re-
serves of natural gas with significant proportions of CO
2
,
which can serve as raw material to the process of dry
methane reforming. The combination of DMR and dry
methane oxidation (Equations (2) and (3)) is known as
combined methane reforming. Recently this subject has
been a matter of increasing interest as observed by the
large number of publications [7-10].
4 2 2 r
1
CH O CO 2H ( H 36 kJ/mol)
2
(2)
4 2 2 2 r
CH 2O CO 2H O( H 802 kJ/mol) (3)
4 2 2 r
CH CO 2CO 2H ( H 264 kJ/mol) (4)
Combination of exothermic and endothermic reactions
is a very important accomplishment to obtain tempera-
ture compensation of the process. A new approach pre-
sented by several authors is based in the use of structured
metal carriers instead of random ceramic supports. The
new carriers with open structures allow achievement of
higher heat transfer coefficients and lower pressures drop
[11-13].
Oxygen addition to DMR reduces carbon deposition
on the catalyst surface and increases methane conversion.
Similarly, the type of catalyst used could also inhibit
coke formation. In this sense, the use of perovskite type
oxides emerge as an alternative since after reduction it is
possible to produce highly disperse metallic particles,
diminishing deactivation of the catalyst by suppressing
the coke forming reactions [14-18]. However, the re-
fractory character of heat conduction in perovskite ox-
ides could be disadvantageous to the combined processes.
The use of metallic structures as carriers of catalysts has