Fuel 80 (2001) 899905

www.elsevier.com/locate/fuel

Reforming of CH4 by partial oxidation: thermodynamic and

kinetic analyses
J. Zhu a, D. Zhang a,*, K.D. King b
a

School of Chemical Engineering, Curtin University of Technology, G.P.O. Box U1987, Perth, WA 6845, Australia
b
Department of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia
Received 7 September 2000; accepted 2 October 2000

Abstract
The traditional technology for synthetic-gas (H2 and CO) production from natural gas is steam reforming. A major drawback of this
technology is the intensive energy requirement due to the high endothermicity of the reforming reactions. A possible alternative is methane
partial oxidation, or in a combination with steam or CO2, which could offer an advantage of vastly reduced energy requirement of the
reforming process. This paper reports on a feasibility study of CH4 partial oxidation into H2 and CO by means of thermodynamic and kinetic
analyses. The thermodynamic analysis has been performed using the Gibbs free energy minimisation method, and the kinetic modelling has
employed the CHEMKIN package incorporating the GRI 1.2 mechanisms of CH4 oxidation. The effects of initial O2/CH4 ratio, temperature
and pressure are examined. The thermodynamic analysis indicates that the synthetic-gas yields are strongly dependent on the initial O2/CH4
ratio with maxima occurring at an optimal initial O2/CH4 ratio varying with temperature. The optimal O2/CH4 ratio decreases with increasing
temperature and approaches 0.5 at temperatures greater than 1073 K. The synthetic-gas yields also increase with increasing temperature but
with decreasing pressure, yet high temperature can suppress the pressure effect. The GRI mechanisms are found to be adequate for the
CHEMKIN simulations of CH4 partial oxidation at temperatures greater than ca. 1273 K and O2/CH4 ratio greater than 0.5. The CHEMKIN
simulations suggest that two distinct stages exist during the partial oxidation. The rst stage is a rapid `oxidation' zone where H2O and CO2
are the main reaction products. The second stage is a slow `conversion' zone where steam and CO2 reforming, water gas shift reaction as well
as C2H2 coupling and C2H2 steam reforming takes place with H2 and CO being the main products. Both thermodynamic and kinetic
predictions of H2 and CO yields compare well at high temperatures. The optimum operating conditions for CH4 partial oxidation reforming
are recommended at 0.5 O2/CH4 ratio, 1473 K and 1 atm. q 2001 Elsevier Science Ltd. All rights reserved.
Keywords: Methane; Partial oxidation; Thermodynamic and kinetic analyses

1. Introduction
Conventional crude oil deposits are dwindling; crude oil
is a non-renewable resource and can not be relied on indenitely as the feedstock or energy for future sustainable
industrial processes. On the contrary, new natural gas
deposits are being continually discovered at a signicant
rate around the globe. In addition, new sources of natural
gas such as coal-bed methane, natural hydrates, and biomass
emissions are now being tapped. The main constituent of
natural gas is methane (CH4), which is valuable by virtue of
its heating value. However, the use of CH4 as a chemical
feedstock has been limited because of its inherently high
chemical stability [1]. Nevertheless, with suitable chemical
processes, CH4 can be reformed to synthetic-gas, consisting
* Corresponding author. Tel.: 161-8-9266-7581; fax: 161-8-9266-3554.
E-mail address: dkzhang@che.curtin.edu.au (D. Zhang).

mainly of hydrogen (H2) and carbon monoxide (CO), which

are suitable for many chemical production processes.
The traditional technology to produce synthetic-gas is
steam reforming. This process has dominated syntheticgas production for 70 years [2]. Although steam reforming
is continuously enhanced by improving the catalysts, operation conditions and heat transfer to achieve better performance, an unavoidable drawback of this process is its
intensive energy requirement. Furthermore, the product
ratio of H2/CO of 3 from steam reforming (Eq. (1)) is
usually too high for many downstream treatments, like
FischerTropsch process, prohibiting its wide application.
CH4 1 H2 Og CO 1 3H2

O
21
DH298
K 205:9 kJ mol

1
CO2 reforming (Eq. (2)), one of the alternatives to steam
reforming of CH4, has received considerable attention
recently for several potential advantages, including a

0016-2361/01/$ - see front matter q 2001 Elsevier Science Ltd. All rights reserved.
PII: S 0016-236 1(00)00165-4

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J. Zhu et al. / Fuel 80 (2001) 899905

Fig. 1. Thermodynamic equilibrium results: normalised equilibrium product yield as a function of initial O2/CH4 ratio at various temperatures (in CH4/air
mixture at 1 atm).

lower H2/CO ratio of 1, reuse of CO2, and a possible means

of energy storage/transmission [3]. The major problems
encountered in CO2 reforming is rapid deactivation of the
catalysts, mainly due to carbon deposition [4].
CH4 1 CO2 2CO 1 2H2

O
DH298
K

247:1 kJ mol

21

2
Unlike the above two endothermic reactions, CH4 partial
oxidation (Eq. (3)) is a mild exothermic process and theoretically yields a synthetic-gas with a H2/CO ratio of 2,
which is desirable for downstream treatments, such as
FischerTropsch process. Several investigators [5] have
offered economic analyses of CH4 reforming by catalytic
partial oxidation for methanol production, and indicated
that the energy required is 1015% less and the capital
investment could be reduced by 2530%. Besides, this
process can also be combined with steam or CO2 reforming
to achieve an exactly desired product H2/CO ratio. Therefore, CH4 partial oxidation is attracting increased attention
from both academia and industry.
CH4 1 0:5O2 CO 1 2H2

O
21
DH298
K 235:9 kJ mol
3

The current contribution reports a thermodynamic and

kinetic study of partial oxidation of CH4 for synthetic-gas
production. The effects of initial O2/CH4 ratio, operating
temperature and pressure on the product yields and composition are examined by means of Gibbs free energy minimisation [6]. A one-dimensional (1D) laminar-ow reaction
stream is simulated using the CHEMKIN package incorporating the GRI 1.2 mechanisms [7]. Good agreements

between the thermodynamic and kinetic analyses are

obtained.
2. Thermodynamic analysis
The thermodynamic equilibrium analysis is performed by
means of Gibbs free energy minimisation method [6]. The
possible species that might be formed in the nal product
gas are assumed to be CH4, O2, CO2, CO, H2O, H2, C, C2H2,
C2H4, C2H6, CH3OH, HCHO and HCOOH [8]. The product
yields are normalised on the basis of initial unit mole of CH4
throughout this paper.
2.1. Effect of initial O2/CH4 ratio and temperature
Fig. 1 shows the equilibrium product composition as a
function of initial O2/CH4 ratio at several different temperatures. As expected, when the O2/CH4 is greater than 2.0,
complete CH4 oxidation (Eq. (4)) occurs, resulting in CO2
and H2O. No CO and H2 are produced. As the O2/CH4 ratio
is reduced from 2.0 to 0.5 (for temperatures above 1073 K),
partial oxidation (Eq. (3)) and full combustion (Eq. (4)) coexist, producing a mixture of H2, CO, H2O, and CO2.
Oxygen is completely consumed. For O2/CH4 ratios less
than 0.5, the equilibrium products involve H2, CO and
excess CH4.
CH4 1 2O2 CO2 1 2H2 O
O
21
DH298
K 2802:6 kJ mol

Temperature has a signicant effect on H2 and CO yields.

At low temperatures, CH4 may not be completely converted,

J. Zhu et al. / Fuel 80 (2001) 899905

901

effect discussed above, and the fact that temperatures below

673 K have no practical meaning, if a high-pressure operation is desirable, a high operating temperature is also
required.
Thermodynamic calculations also suggest that dilution of
the reactants by an inert gas can increase the product yields.
This is supported by high CH4 conversion and H2, CO selectivity found in many laboratory studies in the literature
where the reactants were diluted by an inert gas (N2 or
He) [913].
2.3. Yields of other hydrocarbons
Fig. 2. Effect of the total pressure on H2 yield, as a function of temperature,
at an initial O2/CH4 ratio of 0.5.

even though the O2/CH4 ratio is greater than 0.5, resulting in

lower H2 and CO yields. However, at high temperatures, the
partial oxidation reaction (Eq. (3)) dominates, and H2 and
CO yields increase. Calculations suggest that meaningful
application of partial oxidation reforming requires the operating temperature to be greater than 1073 K.
2.2. Effect of pressure and inert dilution
The pressure effect on the equilibrium composition is that
a high-pressure does not favour synthetic-gas production
since the total product mole number is larger than that of
reactants. Fig. 2 shows the effect of pressure on the normalised H2 yield as a function of temperature from the thermodynamic equilibrium calculations. It also indicates that high
temperatures can suppress the effect of pressure on the nal
product yields. When the temperature is below 673 K or
higher than 1473 K, pressure effect on the production of
synthetic-gas is almost negligible. As seen in Fig. 2, only
within the temperature range of 6731473 K, the pressure
effect is signicantly adverse. Considering the temperature

Fig. 3. Comparison of thermodynamic (lines) and kinetic simulation

(symbols) results: normalised product yield versus initial O2/CH4 ratio
with 70% N2 dilution at 1773 K and 1 atm. For the kinetic calculations,
the reactor length is 10 m, the reactant mass ow-rate is 0.04 g cm 22 s 21.

Formation of other hydrocarbons such as C2H6, C2H4,

C2H2, CH3OH, HCHO, and HCOOH can also be found
during partial oxidation of CH4, although in extremely
small quantities. The yields of these products vary with
the temperature, but usually less than 10 27. Under extraordinary fuel-rich conditions and at high temperatures, C2H4
and C2H2 can reach noticeable levels. This is consistent with
the literature report on methane combustion under `ultrarich' conditions, where C2H4 and C2H2 are detected at
temperatures between 13731673 K [14].
3. Kinetic simulations
The thermodynamic analysis can suggest the potential
product compositions of the reaction but can not offer any
insights into the reaction process. To further understand the
kinetic behaviour of CH4 partial oxidation, a kinetic analysis
is performed using the CHEMKIN package [15,16] incorporating the GRI 1.2 mechanisms with 177 elementary reactions and 32 species [7]. The physical model considered is a
1D pre-mixed laminar-ow reaction system in an exaggerated long reactor of 10 m and with a small ow-rate (mass
ux) of 0.04 g cm 22 s 21 (or 0.35 m s 21 at 298 K). As a preliminary study, energy equation is excluded in the simulations. Instead, a temperature prole along the reactor length
is assumed to be 298 K between 0.000.05 m, followed by a
linear ramp to a desired temperature at 0.2 m, and remains
constant till the exit of the reactor. Simulations were
performed over a temperature range of 8732073 K with
a 100 K interval. In the gas feed, CH4 is varied between
1528% and O2, between 152%, diluted by 70% N2.
Fig. 3 shows that the CHEMKIN predictions and the
thermodynamic calculation results at 1773 K compare
extremely well. Simulations indicate that the higher the
temperature, the better the agreement between the two. As
can be seen from Fig. 3, all product yields from the kinetic
calculations almost exactly match those from the thermodynamic equilibrium results at 1773 K. Only when the
initial O2/CH4 ratio is close to 0.5, the kinetic results become
slightly lower than the equilibrium results. It is expected
that if the reactor length is increased or the ow-rate of
reactant gas reduced, the agreement can be improved.
These results tend to suggest that the GRI 1.2 mechanisms

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J. Zhu et al. / Fuel 80 (2001) 899905

isms may not apply under fuel-rich conditions. Nevertheless, the GRI 1.2 mechanisms seem to serve reasonably well
at high temperatures and high O2/CH4 ratios.
4. Discussion
4.1. Maximum synthetic-gas yield

Fig. 4. Comparison of thermodynamic (lines) and kinetic simulation

(symbols) results: normalised product yield versus initial O2/CH4 ratio
with 70% N2 dilution at 1473 K and 1 atm For the kinetic calculations,
the reactor length is 10 m, the reactant mass ow-rate is 0.0004 g cm 22 s 21.

are adequate for CH4 partial oxidation reforming, particularly at high temperatures and high O2/CH4 ratios.
At lower temperatures between 1273 and 1673 K,
CHEMKIN under-predicts the product yields as compared
with the thermodynamic calculations. This is because the
residence time chosen for the kinetic simulation is not long
enough. To prove this hypothesis an extremely small inlet
mass ow-rate 0.0004 g cm 22 s 21 (,3.5 mm s 21 at 298 K)
was examined. Fig. 4 shows typical results at 1473 K. It can
be seen that with this extremely small feed rate (long residence time), the outlet product yields become very close to
the equilibrium state. However, under fuel-rich conditions
(low O2/CH4 ratios), H2 yield predicted exceeded the equilibrium results. This over-prediction becomes more severe
at lower temperatures, suggesting that the GRI 1.2 mechan-

Fig. 5. Comparison of thermodynamic equilibrium results (lines) with

experimental data (symbols) from the literature on catalytic partial oxidation of CH4: hydrogen selectivity as a function of temperature at 1 atm. 1,
O2/CH4/Inert 1/2/0 [10]; A, O2/CH4/Inert 21/42/79 [9]; K, O2/CH4/
Inert 2/4/11 [11]; W, O2/CH4/Inert 1/2/NA [11]; p , O2/CH4/
Inert 5/10/85 [12]; , O2/CH4/Inert 1/2/13 [13]; dash line for O2/
CH4 ratio of 1/2 without inert dilution and solid line for O2/CH4/N2 of
1/2/17.

It is interesting to note from Fig. 1 that the maximum H2

and CO yields do not always occur at the O2/CH4 ratio of 0.5
as one would have thought. The O2/CH4 ratio for the maximum H2 and CO yields move from a higher value towards
0.5 as temperature increases. At temperatures greater than
1073 K, this optimal O2/CH4 ratio remains at 0.5. This behaviour is also observed in the kinetic simulations. Despite
this, however, most experimental studies reported in the
literature were carried out at 0.5 O2/CH4 ratio while
temperatures were less than 1073 K [914]. At temperatures above 1473 K and for the reactor length of 10 m
considered, there is essentially no difference between the
current thermodynamic and kinetic calculations. This
tends to suggest that the optimal operating conditions should
be 0.5 initial O2/CH4 ratio, 1473 K and 1 atm.
4.2. Comparison with literature data
Fig. 5 compares the H2 selectivity estimated from the
thermodynamic calculations, as a function of temperature,
with experimental data found in the literature [914]. The
thermodynamic calculations considered two initial reactant
gas O2/CH4/N2 ratios, 1/2/0 (dashed line) and 1/2/17 (solid
line), respectively. As can be seen, the dilution of the reactant gases increases the H2 selectivity at temperatures below
1200 K, showing a similar effect to that of pressure. In the
experiments, various catalysts were used and the O2/CH4
ratio was 0.5 in a mixture diluted by an inert gas of varying
quantity. It is clear from Fig. 5 that most experimental
results fall below the equilibrium lines. Only a few data
appear above the equilibrium lines, most likely due to
experimental error, such as inaccurate temperature measurements. This comparison is quite satisfactory and validates
the theoretical results of the present study, at least in part. In
addition, a general observation can be made from both thermodynamic and experimental results in Fig. 5 that dilution
of the reactants by an inert can improve the product yields.
Comparing with the thermodynamic analysis, the kinetic
analysis suggests a higher operating temperature (1473 K).
Similar trends for CH4 conversion and CO selectivity are
obtained.
4.3. Two reaction zones
Fig. 6 shows typical proles of major product yields, for
different temperatures and initial O2/CH4 ratios, along the
reactor determined from the kinetic simulations. Note that
the x-axis is log(100x) (or 2 1 log x), where x is the reactor

J. Zhu et al. / Fuel 80 (2001) 899905

903

Fig. 6. Typical kinetic simulation results: normalised product yield versus the logarithm of reactor length, log 100x at various temperature and initial O2/CH4
ratio in 70% N2 at 1 atm. The initial O2/CH4/N2 ratios are a 5/25/70, b 10/20/70, c 15/15/70.

length in metres. It is clear that CH4 conversion and H2 and

CO yields increase with increasing temperature at any particular initial O2/CH4 ratio. At the lower temperatures (1173,
1273, and 1373 K) displayed, the H2 and CO yields increase
with the initial O2/CH4 ratio, but the trend is reversed for H2
yields at the higher temperatures (1473 and 1573 K). Note
that C2H2 formation becomes noticeable at temperatures
greater than 1273 K and is very signicant at 1573 K and
increases with a decrease in the initial O2/CH4 ratio. Further
more, at the high O2/CH4 ratio, H2 yield is lower than CO
yield at lower temperatures (1173 and 1273 K) but increases
with temperature at a much faster rate than CO yield. The H2
yield exceeds CO yield at .1373 K. A lower initial O2/CH4

ratio favours H2 formation, offering a possible means to

control the product H2/CO ratio.
An inspection of the species proles along the reactor
length (Fig. 6) suggests that there are two distinct zones
of reaction at high temperatures. The rst is a rapid oxidation zone where both full combustion and partial oxidation
of CH4 occur simultaneously; and the second a slow reforming or conversion zone where the full combustion products
further convert residual CH4 into the synthetic-gases. This
two-zone concept is different from the two-stage partial
oxidation process reported in the literature, where complete
oxidation takes place rst followed by steam and CO2
reforming. A further inspection of Fig. 6 indicates that the

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J. Zhu et al. / Fuel 80 (2001) 899905

length of the rapid oxidation zone decreases with increasing

temperature and the initial O2/CH4 ratio.
Within the rapid oxidation zone, the main products are
H2, H2O, CO and CO2. Therefore, the overall reaction could
be expressed as

high H2 yields at high temperatures and low O2/CH4 ratios

shown in Fig. 6 support this theory.

CH4 1 aO2 bH2 1 cH2 O 1 dCO 1 eCO2

CH4 1 CH4 C2 H2 1 3H2

where a, b, c, d and e are reaction stoichiometric coefcients. Their values depend on the temperature and reactant
concentrations. The lower the temperature and the higher
the initial O2/CH4 ratio, the more H2O and CO2 formed. Heat
of oxidation is expected to be released rapidly in this zone,
which is consistent with the observation of `hot spots'
reported in the literature [10] where a temperature jump,
exceeding 200 K, occurred at the inlet of a catalytic reactor.
Most researchers [11,1722] believe that CH4 reforming
by partial oxidation occurs via two stages. In the rst stage
CH4 is converted to CO2 and H2O until O2 is completely
consumed. In the second stage synthetic-gas is produced via
CO2 and steam reforming reactions. However, the present
kinetic calculations show that H2 and CO are also rapidly
formed in the rst stage together with the full combustion
products H2O and CO2. The calculated H2O/CO2 ratio is
always far greater than the stoichiometry of 2, thus supporting that both full combustion and partial oxidation take
place simultaneously.
Steghuis et al [11] claimed that with some catalysts direct
partial oxidation could occur. They suggested the following
overall partial oxidation reaction:
CH4 1 O2 CO 1 H2 1 H2 O
O
21
DH298
K 2276:0 kJ mol

Note that this reaction also contains the full combustion

product of H2O. Besides, CO2 has also been detected as
one of the main species in their experiment [11]. In
addition, since most experiments found in the literature
were carried out at relatively low temperatures
(,1273 K), the high H2O and CO2 formation in the
rst stage was reported. The concern of whether the
full combustion or partial oxidation occurs rst is not
only of academic interest, but also very important from
the practical point of view, since it will guide the strategy of practical reformer design.
After the rapid oxidation zone, whose length depends on
the temperature, the slow reforming reactions follow in the
conversion zone. For temperatures ,1173 K, all product
yields are almost invariant at the reactor outlet. Above
1273 K the levels of H2O and CO2 as well as residual CH4
decrease, while H2 and CO yields increase, indicating that
steam reforming of CH4 (Eq. (1)) is occurring. Water gas
shift reaction (Eq. (7)) is also expected to play an important
role. With a further increase in temperature (.1373 K),
C2H2 is formed and rises with increasing temperature,
symbolising a new reaction, methane coupling reaction
(Eq. (8)), which is rarely mentioned in the literature. The

CO 1 H2 O CO2 1 H2

O
21
DH298
K 241:2 kJ mol
7
O
21
DH298
K 376:6 kJ mol
8

Since this reaction (Eq. (8)) is highly endothermic and takes

place at high temperatures beyond most experiment conditions in the literature, direct verication of its role is
not available at present. Further increase in temperature
(.1473 K) leads to water gas shift reaction approaching
its equilibrium as evidenced by the constant nal CO2 yields
and relatively low CO. At even higher temperatures
(.1573 K), steam reforming of C2H2 (Eq. (9)) occurs and
results in increased CO and H2 yields while C2H2 and H2O
yields decrease.
C2 H2 1 2H2 Og 2CO 1 3H2
O
21
DH298
K 35:2 kJ mol

This slow conversion zone will require a large volume in an

actual reactor thus accounting for a major component of the
capital investment. Therefore, the key issue for the successful design of the CH4 partial oxidation reforming process is
to accelerate the reactions in this zone. Possible solutions
are to search for more effective catalysts, employ high operating temperatures and make a good use of the heat released
in the rapid oxidation zone.

5. Conclusions
CH4 reforming by partial oxidation for synthetic-gas
production has been studied by the means of thermodynamic analyses and kinetic simulations. Thermodynamic
analyses suggest the optimal operating conditions of the
initial O2/CH4 ratio of 0.5 and temperatures .1073 K.
Low pressure reforming is favourable, however, high
temperatures can suppress the pressure effect. Kinetic simulations using CHEMKIN package incorporating the GRI 1.2
mechanisms predict the synthetic-gas yields comparable to
those from the thermodynamic analyses at high temperatures. Both H2 and CO yields increase with temperature
with H2 yield increasing at a higher rate due to the water
gas shift reaction and methane coupling reaction at higher
temperatures. The H2 and CO yields also strongly depend on
the initial O2/CH4 ratio with maxima occurring at an optimal
ratio decreasing towards 0.5 with increasing temperature.
There exist two distinct reaction zones in the partial oxidation process, namely, a rapid oxidation zone and a slow
conversion zone. Both full combustion and partial oxidation
co-exist in the rapid oxidation zone, and steam reforming,
water gas shift reaction, CH4 coupling and C2H2 steam

J. Zhu et al. / Fuel 80 (2001) 899905

reforming reactions dominate in the slow conversion zone.

The length of the rapid oxidation zone decreases with
increasing temperature and the initial O2/CH4 ratio. The optimum operating conditions for CH4 partial oxidation reforming
are recommended at 0.5 O2/CH4 ratio, 1473 K and 1 atm.
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