chemical engineering research and design 8 7 ( 2 0 0 9 ) 91–96

Contents lists available at ScienceDirect

Chemical Engineering Research and Design

journal homepage: www.elsevier.com/locate/cherd

Total combustion of propane in a catalytic

microchannel combustor

Y. Men ∗ , G. Kolb, R. Zapf, H. Pennemann, V. Hessel

Institut für Mikrotechnik Mainz GmbH (IMM), Carl Zeiss Street 18-20, D-55129, Germany

a b s t r a c t

The combustion of propane was studied on wash-coated noble metal supported catalysts in a catalytic microchannel
combustor under different reaction conditions in the temperature range 250–750 ◦ C. Pt-based catalyst was found to be
more active than Pd and Rh for the same metal loading on identical support. Pt-based catalyst showed deterioration in
conversion in excess of air owing to inhibition effects of the surplus oxygen. Additionally, minor undesired selectivity
towards carbon monoxide was found under stoichiometric feed ratio over Pt/Al2 O3 catalyst. Palladium and rhodium
catalysts were less active but exclusively selective towards carbon dioxide at stoichiometric oxygen to propane ratio
and deactivation was found in a short time. Catalytic activity of Pt/Al2 O3 catalyst was observed to be significantly
enhanced by the transition metal oxide additives, namely tungsten and molybdenum, and the promoting role of
metal oxides is tentatively discussed. At 325 ◦ C reaction temperature and at a space velocity of 300 NL/(h gcat) full
propane conversion could be achieved over Pt/MoOx /Al2 O3 catalyst in the slight excess of oxygen. Platinum catalyst
promoted by MoOx and WOx proved to be stable for over 1000 h without any detectable degradation in performance
for low and high temperature applications, respectively.
© 2008 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

Keywords: Microchannel reactor; Propane combustion; Heterogeneous catalysis; Oxidation; Noble metals

1. Introduction Future energy generation for stationary, distributed and

Catalytic combustion of hydrocarbons represents one of the
least polluting and economical means of heat and energy
generation (Zwinkels et al., 1993). The application of this tech-
nology is increasing in commercial areas such as domestic
heating appliances, catalytic burners and catalytic cleaners for
exhaust gas and volatile organic compounds. Besides appli-
cations of the large-scale, small-scale applications utilizing
other fuels than natural gas will be of great importance in
the near future, since combined heat and power systems will
be widely introduced for a distributed power generation. For
remote areas where natural gas is not readily available, lique-
fied petroleum gas (LPG) is an attractive alternative due to its
high energy density, and its relatively easy storage through
an established infrastructure. The need for distributed and
portable power generation that relies on modularity and small
scale may render catalytic combustion an appealing technol-
ogy.
mobile applications will be based to a significant extent
upon fuel cell technology (Hoogers, 2002). Hydrogen pow-
ered fuel cells are expected to become important energy
carriers for sustainable energy generation with reduced
impact on the environment. As a result, attention has
been focused on the conversion of more readily available
fuels to hydrogen, either on board of a vehicle (Trimm
and Önsan, 2001) or at a service station. The conversion
of hydrocarbons and alcohols may be achieved by various
routes, such as catalytic steam reforming, partial oxidation
and autothermal reforming (Joensen and Rostrup-Nielsen,
2002). Among these, steam reforming followed by water–gas
shift (WGS) is currently the most economically viable
route:
Cn H2n+2 + nH2 O = nCO + (2n + 1)H2
CO + H2 O = CO2 + H2 (1)

∗
Corresponding author.
E-mail address: men@imm-mainz.de (Y. Men).
Received 17 December 2007; Accepted 11 July 2008
0263-8762/$ – see front matter © 2008 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
doi:10.1016/j.cherd.2008.07.010
92 chemical engineering research and design 8 7 ( 2 0 0 9 ) 91–96
Nomenclature
NL normal litres under standard condition
Si product selectivity (%)
WHSV weight hourly space velocity (NL/(h gcat ))
X propane conversion (%)
Since steam reforming is endothermic, thermal energy needs
to be supplied and a possible energy source is the heteroge-
neously catalytic combustion of hydrocarbons:
3n+1
Cn H2n+2 + 2 O2 = nCO2 + (n + 1)H2 O (2)
Microstructured components have attracted considerable
interest in chemical processing, broadly from lab-scale to
pilot- and production-scale application (Charpentier, 2005;
Hessel et al., 2004, 2005a,b; Jähnisch et al., 2004; Kolb and
Hessel, 2004a; Markowz et al., 2005) due to their superior
advantages in mass and heat transfer, smaller size, energy and
cost saving (Krtschil et al., 2006). A lot of attention is devoted
to hydrogen production in microdevices for portable appli-
cation (Gavriilidis et al., 2002; Hessel et al., 2005b). To date,
numerous microreactors for on-site production of H2 from sev-
eral alcohols and a few hydrocarbons have been developed to
exploit advantages of performing catalytic steam reforming at
the microscale (Conant et al., 2007; Men et al., 2008; Michael
Mitchell and Kenis, 2006; Park et al., 2005; Schuessler et al.,
2003; Terazaki et al., 2005). Combustion converts the chem-
ical energy of fuels into thermal energy, which can then be
harnessed as electricity via various routes, for instance in an
integrated microdevice for hydrogen generation for fuel cell
via reforming (Holladay et al., 2002). Apart from supplying the
steam reformer with energy, total oxidation may be applied for
feeding integrated microevaporators with energy. Integrated
microsystems for H2 production consisting of burner, evapo-
rator, and reformer units have been developed from stainless
steel for steam reforming of methanol (Palo et al., 2002; Reuse
et al., 2004; Yoshida et al., 2006).
Propane combustion has been investigated for decades
by fundamental and experimental studies, however previous
studies were mainly focused on the conventional fixed-bed
reactor, which generally suffer from excessive pressure drops
across the catalyst bed and result in high parastic losses by
the excessive power demand. The present investigation was
undertaken so as to study in detail the total combustion of
propane over different noble-metal catalysts at different pro-
cess conditions within an isothermal microchannel reactor.
The influence of promoters on the catalytic activity has also
been studied.
2. Methods and materials
2.1. Catalyst preparation
Two preparation methods were applied to coat the cata-
lysts (self-developed or commercial) onto the stainless steel
microchannel surface. Reactors used stainless steel sheet pat-
terned microchannel by a wet chemical etching. The square
microchannels (600 ␮m width, 250 ␮m depth) are separated by
50 ␮m fins with the total length of 50 mm.
The self-developed catalyst coatings presented in this
paper were exclusively based upon alumina carriers. Cata-
lysts were prepared by firstly washcoating alumina onto the
microchannels followed by the subsequent impregnation of
the active component. To coat a commercial catalyst, a direct
wash-coating protocol with a commercial catalyst suspen-
sion was applied followed by an appropriate temperature
treatment. The procedure applied for wash-coating of the
combustion catalyst was performed manually by filling the
microchannels with alumina carrier suspension and remov-
ing the excess suspension and calcinations at a temperature of
800 ◦ C in air to avoid the release of unknown species in the sub-
sequent treatment. The alumina carrier coating (∼50 ␮m) was
then impregnated with noble metal salt solutions and calcined
in air at for 2 h. Details of this wash-coating procedure were
described in our previous studies (Kolb et al., 2004b; Zapf et al.,
2003). The deposited washcoats showed very good adhesion
not only for fresh samples but also after application-oriented
tests (Zapf et al., 2006).
The specific surface area was determined by nitrogen
sorption using a Sorptomatic 1990 (Carlo Erba Instruments)
automatic apparatus and calculated by the BET method.
2.2. Experimental set-up
The experimental apparatus consists of the feeding system,
the microchannel reactor and the on-line gas chromatograph,
which has been described in detail elsewhere (Kolb et al.,
2005). Required gas mixtures were regulated by the respective
mass flow controllers (BRONKHORST HI-TEC). Propane com-
bustion was carried out in a plug flow-type apparatus with a
microchannel reactor at atmospheric pressure and a temper-
ature range from 250 to 750 ◦ C. The microreactor sandwiched
in a heating compartment was powered by a heating cartridge
regulated by a PID temperature controller with a K-type ther-
mocouple inserted into the wall of the reactor. The test reactor
has a sandwich design with two microstructured platelets
being attached face to face. The platelets carry 14 channels
each 25 mm long, 500 ␮m wide and 250 ␮m deep. Details of
the reactors has been described elsewhere (Kolb et al., 2005).
The reaction was initiated by introducing a gaseous mix-
ture of propane and air with a total flow rate of 100 mL/min
without any pre-treatment prior to the catalytic test. The high
heat transfer of the microstructured reactor avoids the forma-
tion of hot-spots and enables the investigation of gas phase
reactions under isothermal condition. The composition of the
reactor effluents were analyzed by an on-line ThermoFinnigan
Trace gas chromatograph equipped with two thermal conduc-
tivity detectors. The analytical procedure allows for analysis
of all species present in the reaction effluents including steam
and propylene (C3 H6 ).
The conversion of propane was calculated by the following
equation:
nin − nout
X(C3 H8 ) [%] = × 100%
nin
where nin and nout are the inlet and outlet propane molar
flows, respectively.
All selectivities reported were based on carbon atoms
except for H2 , which was based on hydrogen atoms,
i ni
Si =  × 100%
vn
all product species i i
where  is the number of carbon atoms in the carbon con-
taining species and ni is the molar flow of the species in
the product stream. The same formula is used to calculate
 chemical engineering research and design 8 7 ( 2 0 0 9 ) 91–96 93

Table 1 – Summary of the tested catalysts

Catalyst Metal loading Carrier Surface
[wt.%] area [m2 /g]

Rh 5 ␥-Al2 O3 117
Pd 5 ␥-Al2 O3 127
Pt 5 ␥-Al2 O3 265
Pt/WOx 5/10 ␥-Al2 O3 215
Pt/MoOx 5/10 ␥-Al2 O3 150

Monometallic catalysts are commercial catalysts and Pt promoted

by Mo and W are both self-developed catalysts.

H2 selectivity but  is the number of hydrogen atoms in the

species.

3. Results and discussion

It is well known that catalytic propane combustion proceeds

effectively over various noble metals such as platinum and Fig. 1 – Performance durability test over monometallic
palladium (Choudhary et al., 2002), transition metal oxides noble metal catalysts. Experimental conditions:
(Yuranov et al., 2002), transitional metal containing spinels oxygen/propane = 5/1, flow rate: 100 mL/min,
and perovskites (Song et al., 2001). Although the metal oxide- WHSV = 300 NL/(h gcat ), reaction temperature: 450 ◦ C.
based catalysts are cheaper, thermally stable and also have
greater resistance to sulfur poisoning, supported metals are
usually more active for the complete combustion of hydrocar- but minor carbon monoxide was detected as a by-product at
bons. Hence, the catalysts used in this study were all based on the elevated temperatures of 400 and 450 ◦ C. Propane conver-
noble metals mainly to reduce the reactor size. All the tested sion increase with increasing temperature, meanwhile carbon
catalysts including metal loading and BET surface area are monoxide selectivity increased to 0.8% at 450 ◦ C reaction
summarized in Table 1. temperature. The enhanced selectivity to CO at higher temper-
Propane combustion was firstly investigated over Pd, Rh, atures may also be caused by the initiation of homogeneous
and Pt-based catalysts at stoichiometric oxygen/propane gas phase reactions except catalytic combustion. This result
(O2 /C3 H8 ) ratio of 5/1. The results are presented in Table 2, is consistent with the previous result that platinum catalyst
in which the conversion of propane and selectivity towards is more active than palladium catalyst for the combustion of
carbon dioxide and carbon monoxide are shown as a func- hydrocarbons containing more than one carbon atom (Burch
tion of temperature. In descending order, the following et al., 1998).
sequence could be generally established for the activity: Short-term stability tests were performed. The rhodium
Pt/Al2 O3 > Pd/Al2 O3 > Rh/Al2 O3 . The rhodium catalyst showed catalyst showed significant deactivation at all reaction tem-
the lowest activity at all reaction temperatures and the pal- peratures within 1.5 h of test duration. The Pd/Al2 O3 catalyst
ladium catalyst was slightly more active. Pd and Rh-based was rather robust against deactivation except for the high-
catalyst were found to be exclusively selective towards carbon est reaction temperature and this catalyst was observed to
dioxide. Under atmospheric pressure, Pt/Al2 O3 catalyst clearly rapidly loose its initial activity at 450 ◦ C (see Fig. 1). No deac-
appeared as the most active catalyst in propane combustion, tivation was found in the short term over Pt/Al2 O3 catalyst at
all reaction temperatures.
In order to investigate an influence of the oxygen con-
Table 2 – Propane conversion and selectivity over centration on the catalytic activity, propane combustion
monometallic noble metal catalysts
was carried out over the Pt and Pd-supported catalyst in
Catalyst Temperature [◦ C] stoichiometric oxygen (oxygen/propane = 5/1) and in excess
350 400 450 of oxygen (oxygen/propane = 7/1). As shown in Fig. 2, propane
conversion on Pt-based catalyst was suppressed in the
Rh
excessive oxygen. Contrarily, catalytic activity of Pd-based
X(C3 H8 ) [%] 16.6 42.6 74.3
catalyst was markedly enhanced with the addition of oxygen,
S(CO2 ) [%] 100 100 100
S(CO) [%] 0 0 0 nevertheless, the Pd-based catalyst was less active than Pt-
based catalyst under the experimental conditions employed.
Pd
The observed different response to the excess of oxygen
X(C3 H8 ) [%] 17.7 57.1 84.5
S(CO2 ) [%] 100 100 100
is likely related to the different reaction mechanisms. It is
S(CO) [%] 0 0 0 generally agreed that oxidized palladium or PdO formed over
supported Pd particles is active in hydrocarbon combustion
Pt
(Gelin and Primet, 2002). Pd2+ O2− ion pairs at the PdO surface
X(C3 H8 ) [%] 94.9 95.6 99.6
S(CO2 ) [%] 100 99.9 99.2 activate the C H bonds via heterolytic mechanism, similar
S(CO) [%] 0 0.1 0.8 to that proposed on metal oxide catalysts. Pd and PdO are
in dynamic equilibrium depending on the various reaction
Experimental conditions: oxygen/propane = 5/1, flow rate: 100 mixture compositions. By contrast to Pd-based catalyst, it was
mL/min, WHSV = 300 NL/(h gcat ), catalyst mass 20 mg. Conversion
proposed that Pt activates the C H bond though a homolytic
and selectivity values are those at 450 ◦ C after 90 min.
mechanism via dissociative adsorption of the hydrocarbon
94 chemical engineering research and design 8 7 ( 2 0 0 9 ) 91–96

Table 3 – Propane conversion and selectivity over

unpromoted and promoted Pt-based catalysts
Catalyst Temperature [◦ C]

350 400 450

Pt
X(C3 H8 ) [%] 94.9 95.6 99.6
S(CO2 ) [%] 100 99.9 99.2
S(CO) [%] 0 0.1 0.8

Pt/MoOx
X(C3 H8 ) [%] 98.8 98.8 99.7
S(CO2 ) [%] 100 99.9 99.9
S(CO) [%] 0 0.1 0.1

Pt/WOx
X(C3 H8 ) [%] 98.9 99.9 100
S(CO2 ) [%] 100 99.9 99.8
S(CO) [%] 0 0.1 0.2
Fig. 2 – Comparison test of propane combustion over Pt and
Experimental conditions: oxygen/propane = 5/1, flow rate:
Pd-based catalysts. Experimental conditions: 100 mL/min, WHSV = 300 NL/(h gcat ).
oxygen/propane = 5/1 or 7/1, flow rate: 100 mL/min,
WHSV = 300 NL/(h gcat ).

on the surface metal sites. Oxygen species act as an inhibitor

for the reaction at full coverage (Choudhary et al., 2002).
A possible explanation is that oxidation of active Pt phase
during propane combustion in excess of oxygen leads to cat-
alyst oxidation. Under steady-state reaction conditions, the
oxidation–reduction equilibrium on the catalyst surface con-
trols the amounts of active sites for propane combustion and
hence the catalyst performance.
In agreement with previous studies which revealed that
Pt is the most active noble metal catalyst for combustion
of higher hydrocarbons other than methane, Pt-based cata-
lyst has been found to be the most active catalyst among
tested noble metal catalysts. The catalytic activity of sup-
ported noble metal catalysts can be modified with support
materials and additives (Bond, 1982). An attempt was made to Fig. 3 – Impact of temperature cycle on catalytic
further optimize the Pt-based catalyst formulation by adding performance. Experimental conditions:
a second metal, e.g. W and Mo (Yoshida et al., 2003). As shown oxygen/propane = 5.5/1, flow rate: 100 mL/min,
in Table 3, the results obtained from Pt/MOx /Al2 O3 clearly WHSV = 300 NL/(h gcat ).
show that the addition of MoOx and WOx onto Pt/Al2 O3 cata-
lyst leads to a dramatic enhancement in the catalytic activity be achieved in the excess of oxygen over Pt/WOx /Al2 O3 cata-
for propane combustion, especially in the low temperature lyst at 450 ◦ C, indicating that the inhibition effect of oxygen
range. The higher catalytic activity of the Pt/MoOx /Al2 O3 and of Pt/WOx /Al2 O3 catalyst is much smaller than that of unpro-
Pt/WOx /Al2 O3 catalysts is related to a greater mobility of lattice moted Pt/Al2 O3 catalyst in excess of oxygen. When oxygen is
oxygen in metal oxide in the presence of metal oxide additives. in excess, carbon dioxide and water are the only detectable
MOx -promoted Pt/Al2 O3 catalysts give a similar selectivity products on Pt-based catalysts, regardless of the kind of addi-
pattern of unpromoted Pt/Al2 O3 catalyst at stoichiometric tives.
oxygen/propane ratio of 5/1, producing a small amount of car- Catalytic performance of Pt/MoOx /Al2 O3 catalyst was fur-
bon monoxide at temperature higher than 400 ◦ C (Table 3). ther investigated in a mixture containing a small excess
The influence of oxygen on the propane combustion per- of oxygen (oxygen/propane = 5.5/1) in the lower temperature
formance of WOx -promoted Pt/Al2 O3 catalyst was evaluated in range. The catalyst underwent several temperature cycles
excess of oxygen (oxygen/propane = 7/1). The result is listed in without any pre-treatment. As shown in Fig. 3, full propane
Table 4 to compare with those obtained from Pt/Al2 O3 catalyst. conversion has been achieved at 325 ◦ C, which is about 100 ◦ C
The results demonstrate that the full propane conversion can lower than that obtained from fix-bed reactor (Yazawa et al.,

Table 4 – Influence of oxygen to propane ratio on catalytic activity over Pt and Pt/WOx catalysts
Catalyst O2 /C3 H8 Temperature [◦ C] Conversion [%] S(CO2 ) [%] S(CO) [%]

5 450 99.6 99.2 0.8

Pt
7 450 99.0 100 0

5 450 100 99.8 0.2

Pt/WOx
7 450 100 100 0
 chemical engineering research and design 8 7 ( 2 0 0 9 ) 91–96
Fig. 4 – Time on stream of propane combustion at 350 ◦ C
over Pt/MoOx /Al2 O3 catalyst. Experimental conditions: flow
rate: 100 mL/min, WHSV = 300 NL/(h gcat ).
2002). This result is also quite similar to our previous study
obtained from Pt-based catalyst prepared with inverse opal
method (Guan et al., 2007). It was also noticed that repeated
temperature cycling significantly improved catalytic activ-
ity. Initially, the propane conversion was only 82% at 275 ◦ C
whereas it reached 86% and 98% after the second and third
cycles at 275 ◦ C. This was explained by a self-activation of the
catalyst under reaction conditions. The number of available
active sites on the catalyst depends on the time on stream.
This catalyst has undergone a long-term stability test at 350 ◦ C
under different oxygen to propane ratios (Fig. 4). The propane
conversion is nearly complete even in the large excess of oxy-
gen. No deactivation was observed up to a time on stream of
1000 h.
Fig. 5 shows the results of a time on stream test at 750 ◦ C.
A 1000 h test with Pt/WOx /Al2 O3 catalyst was performed with-
out any noticeable degradation of activity and selectivity. Full
conversion was observed for the entire run with carbon diox-
ide and water as the only products, regardless of the oxygen
to propane ratio.
In the view of available data and information, catalytic
propane combustion may be considered to proceed via the
initial C H bond breaking, typically the slowest or rate deter-
mining step followed by presumably subsequent faster and
further oxidation reactions. It is postulated that the observed
activity enhancement is related to the contribution of MOx
species in close proximity to the Pt particles. It is proposed
that perimeter sites at the Pt/MOx interface may be impor-
Fig. 5 – Time on stream of propane combustion at 750 ◦ C
over Pt/WOx /Al2 O3 catalyst. Experimental conditions:
oxygen/propane = 5.5/1 or 7.5/1, flow rate: 100 mL/min,
WHSV = 300 NL/(h gcat ).
95
Fig. 6 – Proposed interface model to interpret the
promoting effect of metal oxide additives on the propane
combustion on Pt/MOx /Al2 O3 catalyst.
tant in the activation of the first C H bond in propane, in a
similar manner to Lee et al. (1999), and a simplified scheme
account for this promotion is outlined in Fig. 6. A catalytic
site consisting of adjacent metallic Pt and metal oxide would
facilitate the initial (heterolytic) C H bond activation at the
metal oxide surface. The activity of the catalyst for deep oxida-
tion is known to depend on the oxygen mobility, which results
from so-called “weak” metal–oxygen bonds. A high number of
surface oxygen with low binding energies of to the catalyst sur-
face have been reported to be required for the catalysts active
in total combustion (Sokolovskii, 1990). Oxygen species on the
metal particle diffuse rapidly to the metal–support interface
and result in the formation of the new active sites which is
far more active for the combustion reaction, preserving the
catalyst surface from over-oxidation, which is also in accor-
dance with the proposal that Mo and W additives lead to an
oxidation-resistant Pt, resulting in a higher catalytic activity
(Yazawa et al., 2002). Thus, the addition of Mo and W into the
Pt likely facilitates the dissociative chemisorption of propane
onto interfacial Pt/MOx active sites and subsequent promotes
oxidation of propane via a bifunctional mechanism. Inasmuch
as the proposed mechanism is related to the previous studies
and available data and appears plausible, more data might be
necessary for this validation.
4. Conclusions
Catalytically active phases (Pt, Pd, Rh, WO3 , and MoO3 ) were
deposited on the coated alumina support and the catalysts
were tested for propane total combustion within a catalytic
microchannel reactor. The propane conversion of the unpro-
moted noble metal catalysts decreases in the order Pt > Pd > Rh
at a stoichiometric oxygen ratio. It was found that Pd and
Rh catalysts are exclusively selective towards carbon dioxide
whereas carbon monoxide selectivity increases at the ele-
vated temperatures, possibly partially due to homogeneous
gas phase reaction. The results show that Pd and Rh catalysts
underwent a rapid deactivation while Pt catalyst exhibited rel-
atively robust stability against deactivation. Catalytic activity
of Pt/Al2 O3 catalyst was observed to be significantly enhanced
by the tungsten and molybdenum oxide additives, and the
promoting role of metal oxides is ascribed to the active sites
created by the metal–support interaction, which facilitates
chemisorption and initial C H bond breaking of the propane
molecule. However, a further study needs to be performed on
these catalysts to elucidate the exact nature of the interac-
tion. Pt/MoOx /Al2 O3 and Pt/WOx /Al2 O3 catalysts demonstrate
excellent stability after 1000 h of continuous operation at 350
and 750 ◦ C, respectively. Sulfur tolerance of these catalysts
will be important in any practical application. A long-term
stability test is currently under investigation and this issue
will be addressed in the future. In conclusion, these catalytic
microchannel combustors show promise for the efficient total
combustion of propane for small or medium-scale applica-
tions under practical conditions.
96 chemical engineering research and design 8 7 ( 2 0 0 9 ) 91–96

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