Proceedings of the International Heat Transfer Conference
IHTC14
August 8-13, 2010, Washington, DC, USA

IHTC14-22742
EXPERIMENTAL STUDY ON A COMPACT METHANOL-FUELED REFORMERWITH HEAT REGENERATION USING CERAMIC HONEYCOMB
Yasuhiro RAI
Dept. of Mech. Eng. & Sci., Kyoto Univ.
Kyoto, JAPANKazuya TATSUMI
Dept. of Mech. Eng. & Sci., Kyoto Univ.
Kyoto, JAPANABSTRACTOn the way to a new era of our society which will be basedon hydrogen energy, it is needed to develop on-site hydrogenproduction systems to cover current insufficient infrastructuresof hydrogen supply network systems. For this, a highly efficientcompact reformer can be one of the most suitable solutions foron-site production of hydrogen which is supplied to distributed
electric power-generation systems. But, the local and overall
energy balance in the reformer should be precisely controlled
since the reforming reaction processes of hydrocarbon fuels arevery sensitive to reaction temperature in the reformer. For
smaller reformers, in particular, the amount of heat loss throughthe outer surfaces is large enough to dominate the reactions. An
appropriate way for thermal energy management, therefore, isnecessary to accomplish highly efficient reformers. For thesebackgrounds, a compact tubular-typed fuel reformer was
fabricated in this study, and was applied to produce hydrogenfrom methanol, focusing on the partial oxidation reaction(POR). The reformer was composed of a stainless steel pipe as
the reactor exterior and ceramic honeycomb blocks inserted in
two locations of the reactor. The honeycomb blocks are
expected to assist the reforming reactions and transfer thethermal energy of the exhaust gas to the reaction region, acting
as a heat regenerator. The upstream-side honeycomb block wasaimed to perform an effective heat exchange from the reactor
wall to the reactant gas. By inserting the block, the reforming
reaction became stable at right after the block. The maximum
hydrogen production was achieved in the condition ofequivalence ratio, around 3.5. The other honeycomb block wasinserted in the downstream of the reaction zone to convert thethermal energy of exhaust gas to radiation energy which can be

Kazuyoshi NAKABE
Dept. of Mech. Eng. & Sci., Kyoto Univ.
Kyoto, JAPANtransferred to the upstream reaction region. Comparing to thecase without the downstream-side block, the temperature of thereaction region became higher. Gas temperatures in thedownstream region, on the other hand, became lower. Methanol
conversion ratio and hydrogen production ratio enhanced due tothe higher temperature at the reaction region. These results
indicate that the thermal energy possessed by the exhaust gas
was regenerated in the reaction region by the downstream-side
honeycomb block and contributes to enhance the efficiency of
the fuel reformer.
1. INTRODUCTION
Hydrogen, which is called one of the most promisingenergy sources, can be used for highly efficient energy systems
such as fuel cells and hydrogen engines. Although large-scaleindustrial process of hydrogen production has been establishedin chemical plants, time is required until the infrastructures ofhydrogen distributions and storages are developed in civil life.
Meanwhile, on-site hydrogen production will be cruciallyrequired for future distributed power supplying systems.
Therefore, it is essential to develop a compact fuel reformer
which is able to apply for variety of fuels and wide range of fuelpurity. It is reported that the thermal condition of the reformer
greatly affects the reforming performance in either case: withand without catalyst [1, 2]. Therefore, temperature control of
the reformer will help improving the reformer effectiveness,start-up characteristic, response and the reduction of undesired
exhausts such as soot or CO [3-6].
By considering the social and technical trend, bio-fuels
may be one of the options of hydrogen carriers. Also, in the
future, low purified fuel may be used as a reforming fuel due to1

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2. EXPERIMENTAL SETUP
Figure 1 illustrates the schematic and cross-sectional viewsof the reformer. As shown in the figure, the reformer wascomposed of two parts, i.e., the evaporator and reactor.
The evaporator was made of a galvanized steel pipe with
inner diameter and length of 28mm and 200mm, respectively. A
fuel injection port was located at the side surface, on which an
injector with electric valve was mounted. An electrical
rectangular signal was sent from a function generator(Yokogawa; WE500, WE7281) to this injector to control thevalve opening. Flow rate of the fuel jet was, therefore,
controlled by adjusting the frequency and duty ratio of theelectrical signal to a certain value. An air supply port was set atthe upstream end of the evaporator. Air supplied to this port wasprovided from a compressor, and the flow rate was controlled
by rotameter with needle valve (Kofloc; RK1250). In the
upstream and downstream areas adjacent to the fuel supply port,
electric band heaters (Sakaguchi E.H. Voc.; BH3430) werewrapped around the evaporator pipe. This heater was poweredby a voltage slider (Yamabishi; V-130-3) and heated theevaporator wall up to a specified temperature. Thus, the fuelinjected from the fuel supply port impinged on the inner wall of
the evaporator, and was vaporized there. The vaporized fuel

④ Ceramic honeycomb blocks② Fuel injection port
⑤ Thermocouples③ Baffle plate① Air supply port

⑥ Electric heaters
15
100

115

60

50

D=36.7rx

Heat insulator(thickness: 35mm)

Fig. 1: Schematic view of the reformer (evaporator & reactor).
8

6 -φ 2 0 .
φ55 .

φ 16

15

φ42

0.25

φ 34

energy resource depletion. For such a low energy density fuel, it
is more important to design fuel reformer considering heat
energy management. When it comes to relatively small-sizedcompact fuel reformer, this consideration is more important,since heat release to the out of the system will be dominant due
to its large surface area to volume ratio.
Okuyama et al. [7] reported that by applying heat
regeneration by porous media which works as a radiantconverter, it is possible to stabilize super-fuel-rich flame. Thisporous radiant converter efficiently converts the enthalpy of
exhaust gas penetrating through the porous media and realizes
energy regeneration to the upstream region of the reactor.
In the authors’ previous studies [8, 9], partial oxidation
reaction (POR) of methanol was studied in terms of temperature
control, and it was reported that temperature greatly affects theefficiency of the reformer. In this paper, results of a prototype
tubular-typed reformer using heat regeneration by ceramichoneycomb are reported. Methanol was used as fuel in the bothprevious and present experiments. Alcoholic fuel is relatively
easy to transport and store since it is chemically stable and is inliquid phase under atmospheric temperature and pressure. It is,therefore, considered to be suitable to compact energy supply
systems with an output of several kilo watts [10]. No catalyst
was mounted on the reformer in the studies. As the initial stepof evaluating the reformer, the experiment was conductedwithout inserting the catalyst to separate the effects of thecatalyst characteristics from those of temperature control.
Reforming gas temperatures and exhaust gas components weremonitored in the reformer. The effects of equivalence ratio andreactant flow rate on the reforming characteristics are discussed,
mainly focusing on POR.

1.50(a) Baffle plate(b) Ceramic honeycomb
Fig. 2: Elements of the reformer.
Table 1: Flow rate conditions (Qfuel = 0.092cm3/s).
3.0
3.5
4.0
4.5

Qair [L/min]
7.65
6.56
5.74
5.10
joining the air flowing from the upstream air supply port wasthen supplied to the reactor through a baffle plate.
As shown in Fig. 1, this baffle plate was located between
the evaporator and reactor. Multiple holes were drilled in the
12mm-thick stainless steel disk. The configuration of the holes
is shown in Fig. 2(a), i.e., a 5.5mm hole was located at thecenter of the disk and six holes with 2mm diameter surrounded
the center one. This multi-hole baffle plate was expected toenhance the mixing between the vaporized fuel and air, and toprevent backfire from the reactor to the evaporator.
The reactor was made of a stainless steel pipe D = 36.7mm
in inner diameter and 300mm in length. Ceramic honeycomb
blocks shown in Fig. 2(b) were inserted in several locations in
the reactor upstream region, which were expected to enhanceheat transfer to the reactant gas and also to use heat
regeneration from the exhaust gas by using radiative heattransfer. This 34-mm-in-diameter honeycomb was made ofcordierite ceramic, and has mesh of cell number 300. Eachblock was 8mm-in-thickness, so that several blocks were put
together by fireproof cement for desired thickness. Band heater(Watlow; MB01E1AB3005) was attached to the pipe sidewall
at the location of 3.1 ≤ x/D ≤ 4.3. This heater was powered by a
voltage slider in the same way as those in the evaporator, andthe pipe wall was preheated before the experiment started, so

2

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that POR starts smoothly after reactants were supplied to thereactor.
Several loading ports were applied to the sidewalls of theevaporator and reactor at the locations shown in Fig. 1. These
multiple ports can be used to insert measurement probes andpossible multiple reactant supplying nozzles. Probes fortemperature measurement made of K-type thermocouples wereinserted into the pipe through these ports to measure the gas
temperature at the axial center, Tin. To protect the exposed partsof the thermocouples from the flame and reactive gas, and also
to prevent any catalysis effects, the thermocouples were coatedby silica-particles. Thermocouples were also attached to thereactor exterior in order to measure the wall surface
temperature, Tex. Signals from the thermocouples were recorded
by a personal computer through a digital multi-thermometer(Keyence; NR-1000). The sampling rate and accuracy of thetemperature measurement was 1s-1 and ±1°C, respectively.
Gas sampling for gas component analysis was conductedby inserting a sampling probe into one of the loading ports. The
probe was made of stainless steel tube, 3mm in outer diameter,
to which a 0.3mm hole was applied at the end in order to freeze
the gaseous reaction. The position of the tip end was set at thereactor centerline, and the gas was collected by connecting thetube to a vacuum-collecting chamber. The collected gas wasthen supplied to a gas chromatograph (Shimadzu; GC-8A)
through a filtering chamber packed with silica gel, by whichwater and unburned methanol were removed from the gas. A
component detector on the basis of TCD (Thermal Conductivity
Detector) method was applied to the gas chromatography. The
column (Shinwa chem.; Shincarbon ST) mounted in thechromatograph oven was calibrated for H2, N2, O2, CO, andCO2 gases. Argon gas was used as the carrier gas.
3. EXPERIMENTAL CONDITIONSIn this study, we investigate how ceramic honeycomb
blocks affect reforming reactions.
First, we inserted one honeycomb block with thickness of
40mm at the region of the reactor, 1.8 ≤ x/D ≤ 2.9 andinvestigated basic reforming characteristic of this fuel reformer
without using heat regeneration. In this case, the honeycomb
block will be expected to improve reforming efficiency and also
maintain stable reaction under high equivalence ratio byincreasing the heat transfer to the reactant gas; POR did not
happen at all if honeycomb block was not inserted.
Secondly, another honeycomb block (40mm in length) was
inserted downstream of the first block. The secondary block
will be expected to play the role of heat regeneration, i.e.,
enthalpy of exhaust gas was absorbed by the secondary
honeycomb when the exhaust gas penetrates through thehoneycomb, and a portion of the enthalpy was regenerated tothe upstream reaction region by radiative and conductive heattransfer. By using energy regeneration from the exhaust gas, thereforming efficiency can be increased. The secondary
honeycomb block was inserted downstream of the first blockwith streamwise space of 58mm, which works as a reaction

region of POR. It was confirmed that enough space for reaction
was needed to stabilize POR in this reformer. This is because
the reaction speed of POR is very slow compare to the complete
combustion reaction because of its fuel rich condition.
As described in the previous section, experiments werecarried out with regard to POR of methanol. Table 1 shows theflow rate conditions of reactants. Fuel and air were bothsupplied to the reactor from the evaporator through the baffle
plate. Qair and Qfuel are the volume flow rates of the air and fuelfed to the evaporator, respectively. Note that Qfuel represents thevolume flow rate of the fuel in liquid form.  is the equivalence
ratio based on the complete oxidative reaction. The
stoichiometric equivalence ratio of the POR, therefore, is = 3.
As shown in Table 1, Qfuel was fixed to one condition in thepresent experiments, and Qair was varied in the range ofequivalence ratios, 3.0 ≤ ≤ 4.5.
The procedure applied in the reaction experiment is
described as follows. The evaporator and reactor pipes werefirst heated by the electric band heaters so that the temperatures
measured at the locations of x/D = −3.9, upstream of the baffle
plate rear surface, and x/D = 3.0 reached 200°C and 550°C,
respectively. Then, the heaters attached to the reactor wereturned off and the fuel and air were supplied to the reformer.
Note that the heaters of the evaporator continued to be powered
during the experiment and the temperature inside the evaporator
was kept at about 150°C.
4. RESULTS AND DISCUSSION
4.1 Parameters for evaluation of reformer performance
In the present study, the quantity of the consumed methanol
cannot be measured directly due to the silica gel chamber, whichcollects water and unreacted methanol. Therefore, these quantities
were estimated from the concentrations of the other gases
included in the exhaust gas. Since the summation of the analyzed
concentrations of H2, N2, O2, CO and CO2 in the exhaust gas was
100±2%, the major components of the gas was expected to bethese five species plus water and unreacted methanol that werecollected by the silica gel chamber. When paying attention to thecarbon atoms, the components possessing carbon atoms among
the products are CO, CO2 and unreacted methanol. Therefore, thequantity of the consumed methanol can be calculated using theconcentrations of CO and CO2 in the exhaust gas. Therefore, themethanol conversion ratio, , is defined as follows:

M CH3OH, consumed M CO  M CO2

M CH3OH, supplied M CH3OH, supplied(1)

YCO  YCO2
M N2

YN2
M CH3OH, supplied

where MX is the molar flow rate of the X component in theexhaust gas, and YX is the X’s concentration.
To evaluate the production efficiency of each component, theproduction rate of component X against 1mol of methanol
supplied, X, is defined as follows:3

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1000

(2)
800
o

Temperature [ C]

(Y / Y ) MX  X N2 N2
M CH3OH, supplied M CH3OH, suppliedMX

In calculating the production rate of H2O, H2O, it is assumed that
all hydrogen atoms originated from the reacted methanol are usedin producing H2 and H2O. Thus, H2O can be obtained by thefollowing equation:

400
200

(3)

0

As a ratio of POR to complete combustion of methanol, we
define H2 production efficiency,  , as follows:

M H2
M CH3OH,consumed

 2

M H2
M H2  M H2O

= 4.0

3

4
x/D

5

6

7

8

80

Concentration [%]

H2
N2
CO2

60

O2
CO

40

20

(5)
0
3.0

As an index of exhaust gas performance of the reformer, we
introduce CO selectivity, , defined as the following equation:
M CO
M CO  M CO2

= 4.0

= 3.0(4)

parameters defined above is as follows:2

 = 3.0

Tex

Fig. 3: Temperature distributions (Case-1).

 indicates how large amount of H2 was produced against 1molof consumed methanol. Therefore, the relation between  and  H2


1

Tin

3.5
4.0
Equivalence ratio 

4.5

Fig. 4: Gas components concentration (Case-1).
1.0

(6)

0.9

4.2 Reforming experiments without heat regeneration(First honeycomb block only; Case-1)
Figure 3 shows the streamwise temperature distributions in
the cases without heat regeneration, i.e., honeycomb block isinserted in the reactor only at the upstream region. The ordinate
indicates the temperature measured, and the abscissa indicates thedimensionless streamwise position x/D from the downstream
surface of the baffle plate. Hatched region in the graph indicatesthe location of honeycomb block. The present fuel reformer was
possible to operate under as wide conditions as of equivalence
ratio between 3.0 and 4.5. In Fig. 3, temperature distributions
show similar trend regardless of equivalence ratio. Distributionsof Tin take its maximum value at x/D = 4.4 and temperature
decreases as moves to downstream. These temperature
distributions infer that the reforming reaction started near at theoutlet of the first honeycomb block, and that the main exothermic
reaction took place at the region of 3.0 ≤ x/D ≤ 5.7. At x/D > 5.7,
temperature decreases as x/D increases, so that the exothermic
reaction did not take place at the downstream region. The wall
surface temperature, Tex, which is plotted using an open symbol
and a broken line, does not experience a sudden temperature
increase as seen in Tin but corresponds moderately to the gas
temperature, Tin. The most upstream surface temperature, Texmonitored at x/D = 1.6, is a bit higher than the corresponding



0.8
0.7
0.6
0.5
3.0

3.5
4.0
Equivalence ratio 

4.5

Fig. 5: Methanol conversion ratio,  (Case-1).
2.0

1.0
CO

H2,H2O

1.6

0.8

1.2

0.6

H2

CO,CO2

 H2O  2   H2

600

0.8

0.4
H2O

0.4

0.2

CO2
0.0

0.0
3.0

3.5
4.0
Equivalence ratio 

4.5

Fig. 6: Production ratio, X, for each species (Case-1).

4

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gas temperature, which will be caused by heat conduction
through the surface wall from the downstream side of thereactor. However, Tex shows its maximum value at x/D = 4.4
which is the same trend as Tin.
Comparing the temperature distributions in Fig. 3 with regard
to equivalence ratio, maximum temperature level was obtained in
the case of = 3.0. The temperature level decreases as 
increases. This is due to the fact that when  becomes small, theoxygen supply rate to methanol increases, which results inpromoting the exothermic reaction of oxidation and increasing thetemperature of the reforming gas.
Figure 4 shows the relation between the concentrations ofcomponents in the exhaust gas and equivalence ratio, . The
concentration of O2 is less than 0.5% in all cases indicating thatthe supplied O2 was totally consumed in the reaction. The
concentration of H2 slightly increases as  increases in the regionof < 4.0. In terms of concentration, the best operating conditionof this fuel reformer was seemed to be near the equivalence ratio,
= 4.0. However, since water and unreacted methanol were
removed by the silica gel column when analyzing the exhaust gas
components, the results of concentration does not show theaccurate evaluation of the efficiency of the fuel reformer. For
these reasons, we introduce the above-defined parameters;
methanol conversion ratio, , and production ratio X.
Figure 5 shows the relation between methanol conversion
ratio, , and equivalence ratio, .  takes its maximum value at
= 3.5 and decreases as  increases. This is due to the fact thatlarger equivalence ratio represents fuel-rich condition, whichmeans oxidation reaction lacks oxygen supply relative tosmaller equivalence ratio conditions, which cause smaller
methanol conversion ratio compared to smaller  conditions.
The production ratio, X, is shown in Fig. 6. H2 takes its
maximum value at , and decreases in the region of > 3.5.
This trend is similar to the methanol conversion ratio,  (cf. Fig.
5). This result indicates that the production efficiency of hydrogenis greatly affected by the methanol conversion ratio. Therefore, it
is assumed that if it is possible to increase  somehow, it may
result in larger hydrogen production.

1000

o

Temperature [ C]

800
600
400
200
0

1

2

3

Tin

 = 3.0

= 4.0Tex

= 3.0

= 4.0

4
x/D

5

6

7

8

Fig. 7: Temperature distributions (Case-2).
1.0
0.9



0.8
0.7
Case-1Case-2

0.6
0.5
3.0

3.5
4.0
Equivalence ratio 

4.5

Fig. 8: Methanol conversion ratio,  (Cases-1&2).
1.2
1.1

H2

1.0
0.9
Case-1Case-2

0.8
0.7
3.0

3.5
4.0
Equivalence ratio 

4.5

Fig. 9: Hydrogen production ratio,  (Cases-1&2).
4.3 Reforming experiments with heat regeneration (Twohoneycomb blocks inserted; Case-2)
Figure 7 shows the temperature distributions of Case-2,
which is the case applying heat regeneration by the secondary
honeycomb block insertion. By comparison with Case-1 (cf.
Fig. 3), temperature rise between two honeycomb blocks (3.0 ≤x/D ≤ 4.4) and temperature drop downstream of the secondary
honeycomb block (x/D ≥ 5.7) were observed for all theequivalence ratio conditions. The temperature drop at thedownstream of the secondary block was caused by absorptionof exhaust gas enthalpy by the honeycomb. Thus, it wasconsidered that a portion of the enthalpy was regenerated to theregion between the two honeycomb blocks. The wall surface
temperatures plotted with open symbols and broken lines follow
the gas temperatures with a similar trend to Case 1. From these

1.3
1.2



1.1
1.0
Case-1Case-2

0.9
0.8
3.0

3.5
4.0
Equivalence ratio 

4.5

Fig. 10: Hydrogen production efficiency,  (Cases-1&2).

5

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5. CONCLUSIONSIn the present article, the methanol fuel reformer using heat
regeneration by ceramic honeycomb was experimentally
evaluated on the basis of the thermal and reaction characteristics.
The major conclusions obtained are listed in the following.
1. An alcoholic-fuel reformer consisting of evaporator andreactor was fabricated and operated under the conditions ofvarying the equivalence ratio, , in the range of 3.0    4.5.
Hydrogen production and a suitable temperature level forpractical use were obtained by the reformer.
2. A better performance was obtained under the conditions of
= 3.5, which is fuel-rich condition compare to thestoichiometric value of POR, = 3.
3. Production ratio of hydrogen is greatly affected by themethanol conversion ratio. Therefore, it is assumed that if it ispossible to increase , it results in larger hydrogen production.
4. In the case with the secondary ceramic honeycomb (Case-2),
higher conversion ratio was obtained for all cases. This
result suggests that ceramic honeycomb works as a heat
regenerator in this reformer.

1.0
0.9
0.8



results of temperature distributions, the secondary honeycomb
block was proved to work as a heat regenerator by absorbing
the enthalpy of the exhaust gas.
Figures 8 and 9 show the comparison between Cases-1&2of methanol conversion ratio, , and hydrogen production ratio,
H2 plotted with regard to equivalence ratio, . Methanol
conversion ratio, , was improved in all the conditions of  byinserting the secondary honeycomb block. As the best case, =3.0,  was observed about 10% enhancement by inserting thesecondary honeycomb block. It is assumed that the
improvement in  was caused by the temperature rise between
the honeycomb blocks. Higher temperature is believed toenhance methanol decomposition reaction and resulted inhigher conversion ratio.
Hydrogen production ratio, H2, had a similar trend to  asshown in Fig. 9. H2 was improved in all the conditions of ,and at most 8% improvement was observed for the case of =
3.0. This improvement was mainly caused by the enhancementof  which is an effect of heat regeneration by the secondary
honeycomb block.
Figure 10 shows the hydrogen production efficiency, , ofboth Cases-1&2. Both cases show the similar trend;  increases
with . This trend is due to the fact that smaller  results inhigher temperature in the reformer as shown in Figs. 3&7,
which accelerated the oxidation of hydrogen and produced
more water rather hydrogen. From the view point of , higher 
results in much better performance, however, the total amountof hydrogen production is small, since higher  leads smaller .
Figure 11 shows the CO selectivity, , for both cases. From
this graph,  is not affected by  and does not have significant
difference between Cases-1&2. Therefore, it is difficult by thepresent fuel reformer to reduce the amount of CO; CO
reduction device or CO selective oxidation catalyst are needed
for practical use.

0.7
Case-1Case-2

0.6
0.5
3.0

3.5
4.0
Equivalence ratio 

4.5

Fig. 11: CO selectivity (Cases-1&2).
ACKNOWLEDGMENTS
This research was partially supported by Kyocera
Corporation and Toyota Central R&D Labs., Inc. The authors
also would like to acknowledge the great advice and help by thefollowing colleagues: Mr. Keisuke Kuwabara, Mr. Daisuke
Yamashita, and Mr. Masashi Kawabe.
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