Energy 51 (2013) 267e272

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Energy
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Experiment of catalyst activity distribution effect on methanol steam

reforming performance in the packed bed plate-type reactor
Guoqiang Wang a, b, Feng Wang a, *, Longjian Li b, Guofu Zhang b
a
Key Laboratory of Low-grade Energy Utilization Technologies and Systems, Chongqing University, Ministry of Education, Chongqing 400044, PR China
b
College of Power Engineering, Chongqing University, Chongqing 400030, PR China

a r t i c l e i n f o a b s t r a c t

Article history: Methanol reforming is considered as a promising candidate for hydrogen production because of its
Received 21 August 2012 advantages in many ways. Conventional reformers of packed-bed catalyst suffer from severe limitations
Received in revised form of mass and heat transfer. These disadvantages result in a low catalyst effectiveness factor in the
23 November 2012
conventional pellet catalyst. In this work, a plate-type reactor has been developed to investigate the
Accepted 22 December 2012
Available online 20 January 2013
influence of catalyst activity distribution on methanol steam reforming. Cold spot temperature differ-
ences are observed in the temperature profile along the reactor axis. It has been experimentally verified
that reducing cold spot temperature differences contributes to the improvement of the catalytic
Keywords:
Uniform distribution
hydrogen production. The minimal cold spot temperature difference is obtained on the optimal catalyst
Gradient distribution distribution. It is found that the optimal catalyst distribution shows superiority in the methanol
Packed bed conversion and H2 production rate in comparison to that of the other ones.
Cold spot temperature difference Ó 2013 Elsevier Ltd. All rights reserved.
Plate-type reactor

1. Introduction Packed beds are widely used to produce hydrogen in industry.

Large-scale application of petroleum poses a great threat to our
environment. Considerable efforts have been made to find cleaner
fuels. It is well accepted that hydrogen has long been considered as
a power source for the future due to its low emission of pollutants.
Recently, the development of hydrogen technologies has become
a hot topic area because of the prominent advantages of hydrogen
[1]. Methanol has a high H/C ratio (4:1) and a low boiling point
(338 K) at a normal atmosphere. Based on the idealized conversion
of all carbon to CO2 and all hydrogen to H2, the values of CO2
content are less than the other fuels, such as ethanol and gasoline
[2]. That contributes to reducing CO2 emissions. What’s more,
methanol does not contain sulfur which is poisonous to the fuel cell
[3]. In addition, methanol can be reformed at a relatively low
temperature and small amount of CO could be obtained in the
products. This advantage does not translate to other hydrocarbon
fuels [4]. Therefore, methanol has drawn a great deal of attention as
a hydrogen carrier for fuel cell applications [5e7]. As compared to
other methanol conversion methods, the (methanol steam
reforming) MSR approach could obtain lower CO production in the
products.
* Corresponding author. Tel.: þ86 013618203569.
E-mail addresses: wangfeng@cqu.edu.cn, wangguoqiang-1987@163.com
(F. Wang).
Unfortunately, the slow heat and mass transfer encountered in the
catalyst bed brings problems such as the occurrence of cold spots.
Due to the severe limitations of heat and mass transfer, conven-
tional steam reformers are limited to an effectiveness factor of
catalyst which is typically less than 5% [8,9]. Extensive work has
been done to tackle such a daunting challenge. Microreactors were
firstly considered to deal with this issue, because the whole system
could become more integrated and compact by using microreactor
technology [10,11]. These research works are reported in some lit-
erature. Deqing Mei and Wei Zhou enhanced the performance of
hydrogen production through a microreactor [12,13]. BH Howard
achieved a 90% conversion by integrating a microchannel heat
exchanger to control and optimize temperature profile [14]. How-
ever, several difficulties and challenges persist. For instance,
although high surface-to-volume ratio and short conduction paths
of microreactors are able to offer high heat transfer rate, these
characteristics lead to a big amount of heat loss from the reactor to
the ambient at the same time [9,15,16]. What’s more, the cold spots
were not removed. Ayman Karim investigated the effect of reactor
diameter on the cold spot temperature difference, and he found
that MSR in a packed-bed reactor of only 1 mm in diameter suffered
from a cold spot temperature difference of up to 22 K due to heat
transfer limitation [17,18]. Moreover, it was indicated that the
temperature difference or cold spot could be removed only when
the equivalent diameter was as small as 300 mm. Unfortunately,

0360-5442/$ e see front matter Ó 2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.energy.2012.12.027
268 G. Wang et al. / Energy 51 (2013) 267e272
such microscale reactors are impractical for a real industrial
application. Therefore, a catalyst coating was proposed to intensify
the process due to its advantages of a lower pressure drop and
superior geometry [19e22]. However, in order to investigate wall
coating behavior of catalyst slurries, Conant T found that the low pH
value of the catalyst slurry caused dissolution and reprecipitation
during the drying step, thus leading to the decrease of the catalyst
activity [23]. Actually, MSR is a complex catalytic process consisting
of multicomponent flow and diffusion. The catalyst activity and
heat load at local position play a crucial role in catalytic production
of hydrogen. Factors that affect the catalyst activity and local heat
load could have an impact on the hydrogen production. These en-
deavors were also reported. Theo Vergunst reduced the inter-
particle temperature differences by adjusting the heat [24]. Benn
Eilers enhanced the hydrogen production by optimizing the tem-
perature profile along the axis of the reactor [25]. All of these are
attributed to a superior thermal management in local areas.
In this paper, we have designed three different distributions of
catalyst bed. MSR has been carried out in these three catalyst beds
with a plate-type reactor. Catalyst distributions have been designed
to optimize the temperature profile and then the catalytic pro-
duction of hydrogen could be improved. We have compared the
methanol conversion and hydrogen production rate in these cases.
An optimal distribution of the catalyst has been proposed for a su-
perior temperature profile for MSR. A higher hydrogen production
rate has been achieved on the catalyst bed of optimal distribution
than the other two cases.
2. Experiment
2.1. Reactor and catalyst distribution design
A plate-type stainless steel microreactor was designed and
fabricated, as shown in Fig. 1. MSR was carried out within a reaction
chamber of 6 mm  6 mm  125 mm. Another chamber of
6 mm  6 mm  60 mm was used to superheat the steam of
Fig. 1. Images of the reactor and catalyst distribution (a) reactor diagram (b) catalyst distribution.
methanol and water before they entered into the reaction chamber.
A couple of holes with 1.5 mm in diameter, designed to measure the
temperature, were placed on the cover plate of reaction chamber.
The temperature distributions along the axis of reaction chamber
were measured by T-type thermocouples. A schematic diagram of
the reactor was shown in Fig. 1.
Catalysts used in all the experiments were commercial CuO/
ZnO/Al2O3 catalyst (CB-7) from Chuanhua Co. Ltd. Three types of
catalyst distributions (uniform, distribution A and distribution B)
were designed. And 3.5 g catalyst was adopted in each distribution.
For uniform distribution, 3.5 g catalyst (with a particle size of
0.5 mm in diameter) was mixed with 1.6 g quartz particles (0.5 mm
in diameter) homogeneously, and then the mixture was uniformly
distributed along the reactor. The quartz showed no catalysis for
this reaction. For the other two distributions, the catalyst (0.5 mm in
diameter) was divided into five segments, marked by ①, ②, ③, ④,
⑤, representing 0.3 g, 0.5 g, 0.7 g, 0.9 g, 1.1 g respectively. And each
segment was diluted with quartz. From ① to ⑤ in sequence, the
mass of quartz particles (0.5 mm in diameter) was 0.7 g, 0.5 g, 0.3 g,
0.1 g and 0.0 g respectively [26]. The distribution A was formed by
packing the mixture into the reaction chamber in order of ①, ②, ③,
④, ⑤ while the distribution B was formed by packing the mixture
into the reaction chamber in the order of ⑤, ④, ③, ②, ①. Therefore
three types of catalyst activity distributions were prepared and each
of them consisted of 3.5 g catalyst pellets. For gradient catalyst
distribution A, the catalyst activity was lower at the inlet and it
gradually increased along the reactor channel. For the gradient
catalyst distribution B, the activity of catalyst was higher at the inlet
and it gradually decreased along the reactor channel. Fig. 1 also
presents a schematic diagram of the catalyst distribution.
2.2. Experimental procedures and analysis
High purity (purity is above 99.5%) methanol was used. Clau-
sen LR has demonstrated that the mixture of water and methanol
with molar ratio of 1.1e1.4 is appropriate for the copper-based
 G. Wang et al. / Energy 51 (2013) 267e272
Fig. 2. A schematic diagram of the reaction system.
catalysts [27]. So the water/methanol mixture with molar ratio of
1.3:1 was adopted in all experiments. Before the experiments, the
catalyst reduction has been carried out. And all experiments were
carried out under atmospheric pressure [28,29]. The effluent stream
was cooled and condensed by the condenser and ice trap. Unreacted
water and methanol were collected before the gas product reached
a soap foam flow meter which was used to measure the total dry
product gas. The effluent composition of the reactor is analyzed by
a gas chromatograph (GC-3000) equipped with a Porapak Q column
and a TCD (thermal conductivity detector) detector. Helium was
used as the carrier gas for the gas chromatograph. Mole fraction of
each component was obtained through material balance calculation
[30]. Multiple parallel samples were measured under each condi-
tion. Fig. 2 is a schematic diagram of the reaction system.
Errors in the experiments include of instrument conditions,
observation, calibration, reading and test planning. Table 1 presents
the calibrated range, accuracy and relative error of the equipment.
Error analysis has been done through the method of average value
and polynomial regression [31,32]. The standard errors of max-
imum values in methanol conversion, hydrogen production rate,
temperature and catalyst mass are 1.98%, 1.24%, 0.98%, 1.05%
respectively. In summary, the total uncertainty of all the values
presented in this paper is less than 5% considering all the uncer-
tainty sources and their values.
3. Results and discussions
3.1. MSR on uniform distributed catalyst bed
A mixture of 1.3:1 M water/methanol has been used as the
reactant. Five components (CH3OH, H2O, CO2, CO, H2) have been
Table 1
Technical parameter of instrument.
Measurement Equipment Calibrated range Accuracy
Catalyst mass FA1104 0.1e110 g 0.1 mg
Dry product EL-102B 1e1000 mL/min 0.1 mL/min
gas
Temperature T-type 73e623 K 0.1 K
(D: Ø 0.3)
Inlet flow DSP-2 0.1e50 mL/min 0.05 mL/min
269
Fig. 3. Methanol conversion as a function of space velocity on uniform distributed
catalyst.
detected in reformate. Results are presented in Fig. 3 which pres-
ents that the growth of space velocity causes the decrease of
methanol conversion. A higher space velocity could lead to
a smaller residence time, thus resulting in a lower catalyst utiliza-
tion. With an increase of space velocity, the methanol conversion
decreases. Therefore, the methanol conversion of MSR decreased
from 82.1% to 38.2% with an inlet temperature of 543 K when the
space velocity increased from 0.96 h1 to 2.44 h1. Since MSR is
highly endothermic, it is very thermodynamically favorable at high
temperatures. Therefore, rising temperature promotes the growth
of methanol conversion, as shown in Fig. 3. This agrees with the
research performed by Naohiro Shimoda [33].
The temperature profile with an inlet temperature of 543 K and
a space velocity of 1.42 h1 is shown in Fig. 4. It could be observed
from this figure that the reaction temperature is not always
maintained at 543 K from the inlet to the outlet. The temperature
decreases firstly and then increases again. And a cold spot tem-
perature difference of 6 K is detected at the position of 22 mm away
from the inlet. This temperature difference could be explained by
the limitations of heat and mass transfer. On the one hand, a high
thermal contact resistance and low thermal conductivity could
easily result in heat transfer limitation. Therefore, the supplied heat
cannot always meet the absorbed heat in the endothermic reaction
per unit time. On the other hand, the reactant diffusion rate may be
lower than the reactant chemical reaction rate, which would lead to
a mass transfer limitation. A dominant amount of reactant mole-
cules could be converted to the reformate before they diffuse to the
surface of the catalyst which is located near the outlet. Therefore,
Relative
error (%)
0.01
0.5
0.5
0.25
Fig. 4. Temperature profile along the reactor on uniform distributed catalyst.
270
Fig. 5. Temperature profile along the reactor under variable inlet condition on uniform
distributed catalyst.
the reactant concentration has a maximum value at the inlet of the
catalyst bed while it will gradually reduce along the axis of the
reactor due to the mass transfer limitations. Since the high reactant
concentration could accelerate the reaction, the required heat by
the reaction could reach the largest at the inlet of the reaction
chamber and thus the “cold spot” occurs there. This cold spot
temperature difference makes MSR performs at a temperature
lower than optimal catalyst operation temperature. Activity of the
catalyst cannot perform sufficiently because this temperature dif-
ference cuts down the catalyst activity and leads to the dropping of
the hydrogen production. Cold spot temperature differences were
reduced as the inlet space velocity increased and the temperature
lowered, as shown in Fig. 5. However, the performance of hydrogen
production got weakened at a higher inlet space velocity and lower
temperature.
3.2. MSR on gradient distributed catalyst bed
In order to reduce the cold spot temperature difference, we have
designed the catalyst distributions A and B to adjust the amount of
catalyst activity at local areas along the reactor. MSR experiments
on these two kinds of catalyst distributions have been carried out.
The longitudinal temperature profiles are presented in Fig. 6 when
the inlet temperature is 543 K and the space velocity is 1.42 h1. It
can be found that the cold spot temperature difference of uniform
plate is 6 K and that of distribution A plate is only 3 K. However, the
cold spot temperature difference of distribution B plate is up to
10 K. As shown in Figs. 7 and 8, the comparisons of the catalytic
hydrogen production among these three different distributions are
presented under the inlet temperature of 543 K. Three distributions
consist of the same catalyst load. However, great difference is
observed. Comparing the performance of distribution A with that of
distribution B, one could easily find that the overall performance of
Fig. 6. Axial temperature distribution on three kinds of catalyst distributions.
G. Wang et al. / Energy 51 (2013) 267e272
Fig. 7. Comparison of methanol conversion on different catalyst activity
distributions.
distribution A is much better distribution A exhibits the best per-
formance with the minimal cold spot temperature difference. For
distribution B, the methanol conversion and hydrogen production
rate drop to the minimal because of the highest cold spot tem-
perature difference. The methanol conversion is 83.4% when space
velocity is about 0.82 h1 on the uniform catalyst distribution plate,
while it increases to 93.1% in the case of distribution A, as shown in
Fig. 7. On the contrary, the methanol conversion drops to 73.6% in
the case of B. The highest hydrogen production rate of 161.3 L/h is
achieved in distribution A. It is 19.1 L/h and 37.9 L/h larger than that
of the other two, as shown in Fig. 8. In the case of distribution A, the
amount of catalyst activity is small at the reactor inlet and gradually
goes up along with the reactor flow channel. Catalytic reaction has
been weakened due to the diminishing of the catalyst amount at
the reactor inlet. This leads to the decrease of the heat absorption
by the reaction in the local areas. Thus, the cold spot temperature
difference can be reduced by adjusting the catalyst amount in local
areas. More catalyst could be used when the isothermal condition
of working temperature is reached. Therefore, the catalytic
reforming performance is improved due to the improvement of the
catalyst utilization. On the contrary, in the case of distribution B, the
amount of catalyst gradually decreases along with the flow channel
of the reactor. At the inlet area, the catalytic reaction has been
strengthened since more catalyst is adopted. The enlarged cold spot
Fig. 8. Comparison of hydrogen production rate on different catalyst activity
distribution.
 G. Wang et al. / Energy 51 (2013) 267e272
Fig. 9. Variation of methanol conversion with temperature.
temperature difference led to the decrease of the efficiency of
catalyst utilization. Due to severe heat and mass transfer limita-
tions, the catalyst effectiveness factor is less than 5% in the con-
ventional pellet catalyst bed [4]. So, a higher activity of catalyst bed
is required in order to improve the catalytic hydrogen production.
Although noble catalysts exhibit much higher catalyst activity, they
are not used widely in industry due to their high cost. To improve
the catalyst activity of the catalyst bed through adjusting the cat-
alyst distribution rather than changing the catalyst species presents
a great advantage. This presents a great challenge. The gradient
distribution of catalyst activity can reduce the cold spot tempera-
ture difference so as to enhance the efficiency of catalyst utilization,
therefore, the hydrogen productivity could be improved. This is
a significant advantage since it is able to improve the productivity
at the same quantity of catalyst or reduce the catalyst cost at the
same productivity.
The methanol conversion and hydrogen production rate are
plotted as a function of temperature in Figs. 9 and 10 respectively. It
has been demonstrated that methanol conversion and hydrogen
production rate of distribution A are superior to the other two
under different inlet temperatures. In addition, temperature pro-
motes the hydrogen production for all these three cases. However,
to maintain a high temperature, extra thermal energy needs to be
supplied and CO concentration could increase. But CO is poisonous
to the downstream fuel cell. So methanol conversion and CO
Fig. 10. Variation of hydrogen production rate with temperature.
271
Fig. 11. CO content as a function of space velocity on gradient catalyst distribution A.
concentration should both be taken into consideration to achieve
a desired temperature level for the reforming reaction in actual
hydrogen production. It is shown in Fig. 11 that the CO concentra-
tion increases as the temperature rises, but decreases as the space
velocity increases. That is because methanol decomposition was
promoted at a higher temperature, but, higher space velocity
means more water is fed into the reformer, which leads to the
consumption of more CO by the water gas shift reaction [34]. In this
work, the optimal methanol conversion of 93.1% is obtained at inlet
temperature of 543 K with the gradient distribution A. The largest
hydrogen production rate is 161.3 L/h at the conversion of 93.1%. It
is 15.1 L/h lower than the theoretic value. That is because the
temperature distribution is still not very uniform on one hand. On
the other hand, flow field is affected for packing catalyst pellets.
Although thermal management in local areas has been improved,
the heat and mass transfer limitation persists in catalyst packed
bed.
Stability is a key factor for catalyst performance. In order to test
the catalyst stability, distribution A was adopted to carry out the
methanol steam reforming reaction. During the reaction, the
methanol conversion scarcely decreased, the H2 concentration and
CO concentration kept at an almost constant level, about 72.4% and
0.61% respectively, as can be seen in Fig. 12. No noticeable catalyst
deactivation has been observed. As a result, distribution A with
CuO/ZnO/Al2O3 catalyst performs a good and stable catalysis for
methanol steam reforming.
Fig. 12. Stability of gradient catalyst distribution A with CuO/ZnO/Al2O3 catalyst.
272 G. Wang et al. / Energy 51 (2013) 267e272
4. Conclusion
Comparative experiments of MSR have been carried out in
a plate-type reactor with catalyst of three different catalyst distri-
butions. Cold spot temperature differences have been observed at
the inlet of the reactor. It is found that the decrease of cold spot
temperature difference can improve the catalytic hydrogen pro-
duction. The minimal cold spot temperature difference of 3 K has
been obtained with catalyst of distribution A. The methanol con-
version and hydrogen production rate have been comprehensively
compared among these three different distributions at different
operation conditions. The hydrogen production of distribution A is
superior to that of the other two catalyst activity distributions. The
optimal methanol conversion of 93.1% and hydrogen production
rate of 161.3 L/h are obtained by using the gradient distribution A at
inlet temperature of 543 K and they are 9.7% and 19.1 L/h higher
than those of the uniform distribution. A conclusion could be
drawn that the optimal activity distribution is the case that the
activity is lower at the reactor inlet and gradually goes up along the
flow channel of the reactor.
Acknowledgments
The authors acknowledge the support of National Natural
Science Foundation of China (50906104).
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