Catalysis Surveys from Japan 2 (1998) 99106 99

Optimum catalytic reactor design for methanol synthesis with TEC

MRF-Zr reactor
Kunio Hirotani, Hitoshi Nakamura and Kazuo Shoji
Toyo Engineering Corporation (TEC), 2-8-1 Akanehama, Narashino-shi, Chiba 275-0024, Japan

The concept of Multi-stage indirect cooling and Radial Flow (MRF) is ideal for designing a catalytic reactor in which an exothermic
equilibrium reaction takes place. The reaction is controlled to go on along the path of the maximum reaction rate in the catalyst bed
where synthesis gas flows radially in the catalyst beds from the outer side to an inner center pipe across boiler (cooling) tubes to recover
the reaction heat as qualitative steam. The MRF concept has already been proven in a commercial scale methanol plant and is unique
not only for saving energy but also for considerable scale-up for which the enhanced design, MRF-Zr , provides. MRF-Zr is now
offered for single train 5,000 t/d reactors used in so-called jumbo methanol plants.
Keywords: methanol synthesis catalyst, MRF concept, steam rising reactor, radial flow reactor, bayonet boiler tube

1. Introduction periments with respect to heat transfer and reaction kinetics

Methanol is no doubt an excellent fuel which may re-
place gasoline or fossil oil in the 21st century because:
(1) it can be handled as a liquid at atmospheric pressure
and at ambient temperature; (2) it can be produced from
synthesis gas which can be converted from any carbona-
ceous substances including natural gas and coal; and (3) it
is a convenient and emission-free motor fuel. If fuel use of
methanol is finally accepted for vehicles in large quantities,
how can we build the large-scale methanol plants necessary
to achieve reduction in capital cost per product? This is the
key economic question at present.
Since the first experiment by M. Pier in 1922 in Leuna,
Germany, to synthesize methanol from CO and H2 , using
zinc chromate as a catalyst, methanol had been produced in
reactors operating under high pressure of 2535 MPa and
high temperatures of 320450 C. For the first 45 years
the process required using relatively poison-resistant ZnO
Cr2 O3 catalyst [1]. In 1966, Imperial Chemicals Industries
introduced its low pressure methanol process in Billingham,
England, using a more active (but less poison-resistant)
ZnOCuO catalyst under 510 MPa and 220300 C [2].
ICI overcame the poison problem for the low pressure syn-
thesis catalyst with the development of the combined desul-
phurization technology applying ZnO and CoMo catalysts
which are well-known today. While the invention of the
low pressure process was a considerable breakthrough for
energy saving, further improvements on plant efficiency and
optimization have been made and are still continuing in ad-
dition to efforts to improve the activity and selectivity of
the catalysts.
CH3 OH H = 90.6 kJ/gmol
TEC sought to improve the performance of methanol
CH3 OH + H2 O H = 49.4 kJ/gmol
synthesis reactors by optimizing operating conditions of
CO + H2 O H = 41.2 kJ/gmol
the above low pressure synthesis catalyst and consequently
patented the concept of MRF (Multi-stage indirect cooling
& Radial Flow) for reactors in 1979. After intensive ex-
during 19801981, the MRF concept was demonstrated at a
50 t/d plant with a side stream reactor located in a 1000 t/d
methanol plant in Osaka, Japan, in 19821983 [3]. The
design procedure with the MRF concept was then fully de-
veloped and completed in 1985 and TEC endeavored to
find the first client to install a commercial-scale reactor
employing this concept during 19861988. The first award
of a TEC reactor using the MRF concept was in 1989 for a
project in Trinidad with a capacity of 300 t/d. The concept
was proven there with the fully anticipated performance of
the commercial scale plant in May 1990 [4]. TEC finally
developed the enhanced version of the reactor, MRF-Zr ,
in 1993 based on the operating experience in Trinidad [5].
The first reactor has been running over seven (7) years
without any problem since its 1990 startup. The MRF-Zr
Reactor was ordered for two (2) methanol projects in P.
R. China in 1993 and 1996 respectively and the first one
will be on stream in 1998. TEC is now prepared to of-
fer, with the entirely same design philosophy and criteria,
the MRF-Zr Reactor on a single train for methanol plants
from a small 300 t/d size to the largest 5,000 t/d plant,
which means doubling capacity compared with existing so-
called world scale plants of 2,0002,500 t/d, in order to
meet the required economies of scale [6].
2. Methanol synthesis catalyst
The major reactions occurring in methanol synthesis re-
actor are:
CO + 2 H2
CO2 + 3 H2
CO2 + H2
The main two reactions are exothermic and decrease in vol-
ume, and thus the methanol formation is favored with lower

Baltzer Science Publishers BV

100 K. Hirotani et al. / Optimum catalytic reactor design
Figure 1. Catalyst Activity. A typical curve of deactivation of a methanol
synthesis catalyst available commercially in the market.
temperature and higher pressure. The maximum conversion
is determined by the equilibrium conditions.
ZnOCuO based catalysts have been developed by sev-
eral catalyst manufacturers to achieve reasonably high con-
versions within the range of low temperatures applied for
the low pressure process. Since the ZnOCuO catalyst also
catalyzes the water shift reaction (since low temperature
shift catalyst contains the same components in principle),
the shift reactions have to be considered together. An in-
dividual kinetic model taking into account all three equa-
tions is used to describe performance of the catalyst by
each manufacturer who treats the model as a business se-
cret. The catalyst activity is a function of the operation
time. Figure 1 illustrates a typical curve of deactivation of
a methanol synthesis catalyst.
Control of the reaction temperature is one of the key
issues for daily plant operation. While the catalyst has
high thermal stability over a wide range of temperatures,
the operator has to keep in mind to maintain the temper-
ature of the catalyst bed below a certain limit to avoid
excessive sintering of the catalyst. The reaction tempera-
ture also affects selectivity for methanol since it is possible
for a variety of byproducts to be formed much more out-
side the desired temperature range depending on the sorts
and/or the amounts of reactive impurities contained in the
feed synthesis gas or originated in the catalyst itself.
3. Review of methanol synthesis reactor
In order to understand specific features of the MRF-Zr
Reactor it is worthwhile to review the characteristics of
various types of methanol synthesis reactors. Today six
(6) types of methanol synthesis reactor are commercially in
operation. They are:
(1) Adiabatic Quench Cooling Reactor
(2) Adiabatic External and Indirect Cooling Reactor
(3) Tube Cooling Reactor
(4) Steam Rising Isothermal Tubular Bed Reactor
Figure 2. Reaction Equilibrium and Maximum Reaction Rate for Metha-
nol Synthesis. Methanol synthesis reactions from CO and H2 or CO2 and
H2 are exothermic. The reaction takes place favorably where the tem-
perature is low. The reaction is also controlled by an equilibrium. The
reaction taking place in the area of low temperature progresses slowly
and according to increase of the temperature it progresses more rapidly.
However, in the area near the equilibrium line the reaction rate becomes
slow due to approach to equilibrium. In the area of low methanol concen-
tration the reaction rate is fast while it is slow in the area of high methanol
concentration. Thus, the maximum reaction rate line is existing almost in
parallel to the equilibrium line. R is relative reaction rate defined by a
function of total pressure, gas composition and temperature.
(5) Steam Rising Isothermal Boiler Coil Reactor
(6) Steam Rising Multi-stage Indirect-cooling Boiler Tube
Reactor.
The maximum capacity of a single train reactor is one of the
important characteristics to be discussed. As plant capacity
increases, there is a breakpoint for each type of reactor
where it becomes more economical to construct two parallel
reactors instead of a single reactor. Allowable pressure drop
is a major limit for the capacity of a single train reactor in
addition to the manufacturing limits of currently available
technology for high pressure vessels. Details are discussed
below for each reactor type.
The reaction temperature profile or the reaction path in
a reactor is also important for understanding the basic re-
action characteristics of each type of reactor. Figure 2
illustrates the maximum reaction rate curve on methanol
concentration as a function of temperature at a constant
pressure together with related equilibrium curve.
If the reaction heat is not removed, methanol concen-
tration increases proportionally with temperature rise and
directly approaches the equilibrium limit. Therefore the re-
action heat has to be removed if the methanol yield is to be
increased. Measures used to remove the heat are: (1) using
quench with low temperature synthesis gas, (2) by external
heat exchangers located between the catalyst beds, (3) by
pre-heating the feed gas or (4) by raising steam. Figure 3(a)
to figure 8(a) illustrate the different concepts of the reactor
schemes and figure 3(b) to figure 8(b) trace each operating
line in the same correlation chart as figure 2.
The adiabatic quench cooling reactor (figure 3(a)) is
presently the most popular methanol reactor designed. Af-
 K. Hirotani et al. / Optimum catalytic reactor design
(a)
(b)
Figure 3. Quench Cooling Reactor: (a) Process Configuration and (b)
Temperature Profile. By quenching cold and fresh synthesis gas to exit of
each catalyst bed, the temperature of reaction gas can be lowered, but the
concentration of methanol also decreases.
ter quench fractions are separated, the main flow of the feed
gas is fed to the reactor inlet and each quench fraction is
fed to each intermediate bed respectively. The efficiency
of quench distributors for mixing the hot and cold gases is
most important in this type of reactor. Poor distribution of
the quench gases will cause hot spots in the catalyst bed
and shorten the catalyst life as well as increase byproduct
formation.
In comparison with other types of reactors, the adiabatic
quench cooling reactor does require a relatively large cat-
alyst volume since the temperature profile or the reaction
path is away from the maximum reaction rate curve (fig-
101
(a)
(b)
Figure 4. Adiabatic External Indirect Cooling Reactors; (a) Process Con-
figuration and (b) Temperature Profile. The reactors are installed in series.
Cooling does not cause decrease of concentration of methanol produced
in each bed.
ure 3(b)). This reactor has many variables to control and it
is somewhat complex to optimize those. The largest pos-
sible capacity for this type reactor is estimated as 3,000
3,500 t/d due to manufacturing limitations in building a
high pressure vessel with the necessary diameter and to the
drawback of an increase in pressure drop through the cat-
alyst beds which causes an increase of recirculator power
resulting in penalty for energy consumption.
In the case of the adiabatic external and indirect cooling
reactor (figure 4(a)), all the gas is passed to the first adi-
abatic bed. The exit gas from the first bed enters the first
heat exchanger where steam is usually raised. The total cat-
alyst volume is smaller than in the adiabatic quench cooling
reactor since all the gas passes through all of the catalyst.
However, the reaction path is still away from the maximum
reaction rate curve (figure 4(b)). The major drawback of
this system is the need to have much larger numbers of
high pressure reactors, heat exchangers and interconnect-
ing piping which inhibit cost savings.
The tube cooling reactor (figure 5(a)) uses reaction heat
directly to pre-heat the inlet gas of the reactor. The main
advantage of this reactor is the need of a relatively small
catalyst volume since the reaction curve closely follows the
102 K. Hirotani et al. / Optimum catalytic reactor design

(a)
(a)

(b)
Figure 5. Tube Cooling Reactor: (a) Process Configuration and (b) Tem-
perature Profile. Catalyst is loaded in the shell-side. Sufficient heat trans-
fer area (many tubes) are required to maintain preferable temperature pro-
file.
(b)
Figure 6. Steam Rising Isothermal Tubular Bed Reactor: (a) Process
Configuration and (b) Temperature Profile. Catalyst is loaded in the tube-
side. A large number of tubes, i.e., a large number of heat transfer surface
provided to load sufficient amount of catalyst, leads to almost isothermal
temperature profile which is far from the maximum reaction rate line.

maximum reaction rate curve (figure 5(b)). This type of re-

actor is very easy to control because all the temperatures in
the reactor are set only by the inlet temperature. A special
device is employed to ensure even gas distribution from the
cooling tube to the inlet of the catalyst bed. The limit of
single train capacity is due to the same reason as for the
adiabatic quench cooling reactor, but the capacity could be
up to approximately 2,0002,500 t/d due to restricted usage
of the reactor internal space which is shared by the cooling
tubes.
The most efficient mean to recover the reaction heat of
methanol synthesis is to use the heat directly in generating
steam in the synthesis reactor. The steam rising isothermal Figure 7. Isothermal Boiler Coil Reactor. Process configuration. Catalyst
tubular reactor (figure 6(a)) has such an advantage together is loaded in the shell-side.
with a considerably small catalyst requirement due to good
catalyst stability because of operation at low catalyst peak plant. A drawback with having a catalyst in the tubelar
temperature (figure 6(b)). The low peak temperature also reactor is to require a large number of tubes in order to
ensures a lower level of byproducts formation. The recov- accommodate the catalyst. This requirement is very expen-
ered heat is used to generate qualitative steam to be applied sive and the manufacturing restriction would limit a single
for steam reforming in the upstream unit of the methanol train capacity of this type reactor up to 1,2001,500 t/d.
 K. Hirotani et al. / Optimum catalytic reactor design 103

Similar near isothermal performance is obtained by load-

ing the catalyst in the shellside as a steam rising isother-
mal boiler coil reactor can demonstrate. An example of
commercial scale installation of this reactor type employs
spirally wounded tubes in a multilayer arrangement over
spacers running the length of the unit (figure 7). The ca-
pacity restriction of this type reactor is determined appar-
ently by pressure drop over the catalyst bed although the
authors have no information on this complex structure of
the reactor.
The TEC MRF-Zr Reactor is a steam rising multi-stage
indirect-cooling reactor using bayonet boiler tubes for the (a)
reaction heat removal together with radial flow of synthe-
sis gas across the catalyst bed in the shellside (figure 8(a)
and (c)). In a multi-stage indirect cooling system the reac-
tion conditions can be adequately controled along the path
of the maximum reaction rate curve in order to achieve
maximum conversion per pass and minimum catalyst vol-
ume per unit product (figure 8(b)). In addition, a radial
flow system ensures achievement of a higher heat transfer
coefficient (gas-cross-flow), less pressure drop and larger
catalyst volume within the restricted manufacturing limit
of a high pressure vessel diameter.
Because of these features, a single 5,000 t/d reactor
can be designed with currently available manufacturing
technology. Fabrication, maintenance and catalyst load-
ing/unloading are also much easier than those for the two (b)
steam rising isothermal reactors described above.

4. Features of MRF-Zr reactor

4.1. Steam rising methanol reactor

The heat of the exothermic reaction over the catalyst bed

is removed by means of cooling tubes arranged adequately
in the bed (figure 8(c)). Saturated boiler feed water (BFW)
is charged inside of the tubes as the cooling medium and
steam is risen by absorbing the reaction heat through the
tube wall. Temperature of the catalyst bed is controlled
by the steam pressure. Thus a steam drum is equipped for
steam recovery and pressure control as well as receiving
the boiler water.
A BFW circulation pump is also provided in order to
ensure adequate heat transfer in the steam rising system.
The steam thus risen has a quality level sufficient for the
steam reforming unit usually existing in the front-end of
the methanol plant and can save energy to generate or
import an equivalent amount of steam for the methanol
plant.

4.2. Radial gas flow

Due to the large cross surface area for gas flow in a ra-
dial flow reactor, extremely small pressure drop through the
catalyst bed is expected. Figure 9 illustrates the estimated
data vs. the actual operating data from the 50 t/d demon-
stration plant on the pressure drops of the reactor and the
(c)
Figure 8. TEC MRF-Zr Reactor: (a) Process Configuration, (b) Temper-
ature Profile and (c) Conceptional Drawing. Catalyst is loaded in shell-
side and radial flow is applied for synthesis gas stream over the catalyst.
The ideal temperature profile is accomplished with adequate number and
bayonet tubes.
104 K. Hirotani et al. / Optimum catalytic reactor design

is that scale up of the reactor is achieved without sacrific-

ing pressure drop by vertical extension until the limit of
the catalyst loading. In other words, the radial flow reactor
can load the maximum volume of the catalyst mechani-
cally within the manufacturing limit of the high pressure
vessel diameter on that date. Thus this concept leads to the
possibility of designing a large single train reactor.

4.3. Cross flow

Figure 10 illustrates the heat transfer coefficient ob-

Figure 9. Pressure Drop of MRF-Zr Reactor. Overall and catalyst bed
pressure drops in a 50 t/d demonstration plant (marked) are compared with
calculated values (real lines).
catalyst bed. These are fitted very well and prove that the
pressure drop of the MRF-Zr Reactor is very small.
This extremely small pressure drop through the catalyst
bed allows more pressure drop over the inside of the reactor
which in turn enables the use of the orifice plate for even
distribution of the gas flow to the catalyst bed. This mild
operating environment avoids mal-distribution and ensures
long catalyst life.
The most important advantage of a radial flow reactor
served during the demonstration test together with a line
of the experimental equation used for the design of the
demonstration plant. Fundamental experiments had been
executed to determine the heat transfer coefficient on the
surface of the cooling tubes in the packed bed where gas
flows radially cross over the tubes. Only a few studies had
been reported in this field. The dotted line in figure 10
indicates the heat transfer coefficient for the parallel flow
system.
The observed figures of the heat transfer coefficient are
well fitted with the experimental equation. It is also con-
firmed thereby that the heat transfer coefficient for the cross
flow is twice as large as that of the parallel flow at the same
gas velocity.
4.4. Adequate boiler tube arrangement
In accordance with figure 8(b), the temperature profile
of the reactor follows the maximum reaction rate line by

Figure 10. Heat Transfer Coefficient in the term of Nusselt Number: N u = h0 (d0 /2)/k vs. Peclet Number: P e = (d0 v/2/)(Cp /k) where h0 :
Packed Bed Overall Heat Transfer Coefficient (kcal/m2 /h/ C) d0 : External Tube Diameter (O.D.) (m). k: Gas Thermal Conductivity (kcal/m/h/ C).
: Gas Density (kg/m3 ). v: Gas Velocity (m/h). : Gas Viscosity (kg/m/h) Cp : Gas Specific Heat (kcal/kg/ C).
 K. Hirotani et al. / Optimum catalytic reactor design
Figure 11. A Top Internal View of MRF-Zr Reactor. The photograph was of a reactor designed for Chuandong Chemical Industry Corp., Sichuan
Province, China.
arranging the boiler tubes adequately. TEC has completed
its own design simulator to execute a variety of complicated
case studies in connection with optimum tube arrangement.
Due to this optimization, the reactor can achieve higher
conversion of synthesis gas per pass on the same volume
of catalyst or can require a smaller volume of catalyst for
the same conversion per pass.
4.5. Bayonet boiler tubes
The MRF-Zr Reactor uses bayonet tubes as an opti-
mum device for the boiler tubes. This design permits free
thermal stress together with the advantage of self drainage
by the tubes themselves, and further permits inspection and
maintenance of the tubes without unloading the catalyst.
Figure 11 shows a top view of the bayonet tube. The bayo-
net tube assembly enables the elimination of a tube sheet on
the one side of the reactor and leads to economical design
accordingly. A forced water circulation system is applied
to ensure steady flow pattern. Boiler water is charged from
a water chamber to the inner tubes and a mixture of steam
and boiler water flows downward through annular spaces
after boiling in the tubes. The mixture is then collected in
the mixture chamber.
4.6. Operation benefits
According to the operating experience over 7 years in the
Trinidad plant, a reactor using the MRF concept is remark-
ably stable in operation. The Trinidad operator confirmed
simple, easy, steady and very reliable operation as well as
easy catalyst handling during loading and unloading com-
pared with other types of methanol synthesis reactors which
they have in their plants. In 1993, at the end of the 3 years
expected life of the catalyst, the Trinidad operator replaced
the catalyst for the first batch even though its activity had
not decreased, however for the second batch, it was decided
105
to continue operations with the catalyst until the real life
of the catalyst expired. At present, over 4 years later, it is
still continuing operation.
5. Commercially proven performance of the MRF
concept
In May 1990 a prototype reactor using the MRF con-
cept was linked with the existing synthesis loop of the No.1
methanol plant at Trinidad Tobago Methanol Co., Ltd. im-
mediately upon completion of the catalyst reduction. It was
clearly observed that operating conditions of the existing
plant were improved dramatically because of excellent per-
formance of the new reactor. The improved performances
for the scheme of 300 t/d MRF plus 1,080 t/d quench cool-
ing reactor (having the catalyst volume for 1,200 t/d) are
summarized as follows, compared with the original 1,200
t/d quench cooling reactor:
(1) 34 kPa of pressure drop for the reactor maintained con-
stantly during the catalyst life (more than 4 years),
(2) 14% less pressure drop achieved for the entire synthesis
loop,
(3) 11% higher gas flow rate achieved through the existing
circulator consequentially,
(4) 33% less purge gas rate achieved due to efficient con-
version,
(5) 8.5% higher crude methanol production per unit feed
gas rate,
(6) 14% less steam import to the plant achieved due to
quality steam generated in the new reactor.
After the start-up the reactor is still in continuous op-
eration over 7 years without any trouble and maintaining
excellent performances.
106 K. Hirotani et al. / Optimum catalytic reactor design

Table 1
the case employing a quench cooling reactor. Our evalua-
Comparison of MRF-Zr Reactor and Quench Cooling Reactor. Mechan-
ical design and process performance of the MRF-Zr Reactor is compared
tion has indicated that total capital expenditure of 2,600 t/d
with Quench Cooling Reactor on which the unity is used for each relative methanol plant using the MRF-Zr Reactor is about 56%
factor of the MRF-Zr Reactor. cheaper than that using a quench cooling reactor.
Table 2 shows the relative energy savings of the MRF-
MRF-Zr Quench cooling
reactor reactor Zr Reactor on a basis of 2,600 t/d plant in comparison
with a quench cooling reactor. Energy saving by using the
Reactive catalyst volume 0.68 1.00
MRF-Zr Reactor would be about 78% superior to that of
Number of reactors 1 1
Relative reactor weights 1.25 1.00 a quench cooling reactor.
Relative heat exchanger area 0.91 1.00
Relative total plant cost 0.94 0.95 1.00
Natural gas consumption 0.93 1.00 7. Design of 5,000 t/d MRF-Zr reactor
Natural gas cost and catalyst cost 0.92 1.00
Table 2 indicates the brief design specification of a sin-
Table 2 gle train MRF-Zr Reactor to produce 5,000 t/d of refined
Specification of A 5,000 t/d MRF-Zr Reactor: Inlet and outlet gas com- methanol. The shell internal diameter of the reactor is only
positions, operating conditions and dimensions of the reactor are summa-
5 m and absolutely within current manufacturing restric-
rized.
tions for high pressure vessels. The height of the reactor is
Inlet Outlet
22.4 m including spaces for all internal devices and cham-
Composition (mol%) bers.
H2 83.2 77.3
CO 7.9 2.1
CO2 5.8 4.4
CH4 + N2 2.7 3.2
8. Conclusion
H2 O 0.1 2.8
MeOH 0.3 10.2 The MRF concept, which is ideal for design of a catalytic
reactor with exothermic equilibrium reaction in terms of
100.0 100.0 cost and energy savings, was first applied to a methanol
Pressure (MPa) 10.00 synthesis reactor and its performances have already been
Temperature ( C) 240 260 proven in a commercial scale operation for more than 7
Internal diameter (mm) 5,000 years. The enhanced design of the same concept is now
TT Length (mm) 22,400
available as the TEC MRF-Zr Reactor which can almost
double the capacity of the current maximum single train
6. Economics of MRF-Zr reactor methanol reactor to 5,000 t/d without any change of the
design philosophy for a small plant of 300500 t/d. The
Table 1 shows economics of the MRF-Zr Reactor on MRF-Zr Reactor promises to achieve a reduction in capital
a basis of 2,600 t/d plant in comparison with a quench cost per product by making possible the construction of
cooling reactor. The MRF-Zr Reactor has many tubes to- necessary jumbo methanol plants if fuel use of methanol is
gether with an associated tube sheet, but its weight is not finally accepted in the not so distant future.
so heavy as it restricts transportation and erection. It has
a relatively small volume of catalyst. A major drawback
of a steam rising reactor such as the MRF-Zr Reactor is References
the need to employ a much larger surface area in the in-
terchanger which is installed for heating all the synthesis [1] H. Roos, G. Steigelmann and R. Klause, 1993 World Methanol Con-
gas up to the inlet temperature before entering the reactor ference, Atlanta, Georgia, 1993.
by heat exchange with the reactor exit gas, whilst a quench [2] ICI Catalogue, ICI Low Pressure Methanol Process (1987).
[3] K. Ohsaki, K. Shoji, O. Okuda and Y. Kobayashi, AIChE 1984 Spring
cooling reactor needs to heat only part of the gas. How- National Meeting, Anaheim, California, 1984.
ever, due to less pressure drop of the MRF-Zr Reactor, [4] Y. Kobayashi and A.F. Greene, 1990 World Methanol Conference,
it is possible to reduce the surface area by giving more Marbella, Spain, 1990.
pressure drop in the interchanger to improve the concerned [5] Y. Kobayashi and H. Nakamura, AIChE 1993 Spring National Meet-
heat transfer coefficient within economic allowance which ing, Houston, Texas, 1993.
[6] K. Hirotani, M. Sasaki and N. Mochizuki, 1997 Asian Methanol Con-
is compensated against the power of the circulator. Our
ference, Singapore, 1997.
optimization results in 91% of surface area compared with