Journal of Nigerian Society of Chemical Engineers, Vol. 27, No.

1 1-8, 2012

A NOVEL SYNGAS PRODUCTION PROCESS DESIGN FOR

GAS-TO-LIQUID (GTL) TECHNOLOGY

Ntuk, U.U.*, Bassey E.N. and Etuk, B.R.

Department of Chemical and Petroleum Engineering
University of Uyo, Akwa Ibom State, Nigeria

*Corresponding author: e-mail:ubting2001@yahoo.com

ABSTRACT
The Gas-to-Liquid (GTL) technology presents a well proven route for utilising stranded natural
gas and securing the world energy future. In this process natural gas is converted to liquid
transport fuels (naphtha and diesel) in three major stages: Methane reforming (Syngas
production), synthesis of GTL liquids from the Syngas (Fischer Tropsch process), refining of the
GTL liquids to transport fuels (Product up-grade).The Syngas production stage accounts for 60%
of the total cost of the GTL process. This is mainly due to the air separation unit (ASU) which
supplies oxygen for the reforming process. In this work a novel syngas production process is
proposed, using the oxygen ion transport membrane concept. The Oxygen ion transport
membrane is a cutting edge technology that combines air separation and high-temperature
synthesis gas generation processes into a single Oxygenmembrane reactor. This design can
reduce the capital cost of the entire process by 30%. A simulation analysis using Aspen HYSYS
proves the viability of the proposed design.

1.0 INTRODUCTION barrels and daily consumption was about 85

The world crude oil reserve is depleting and million barrels, shifting the estimated oil
there is the need to secure the world’s future depletion year to 2057. Another study has
energy needs. It has been estimated that predicted that the world consumption of oil
world oil supply will have peaked by 2030 will increase to 98.3 million barrels per day
and would be depleted between 2062 and in 2015 and 118 million barrels per day in
2094, assuming total world oil reserves is 2030 (Emmanuel et al, 2010). All these are
between 1.4 and 2 trillion barrels and pointing to a foreseeable energy crisis.
consumption at 80 million barrels per day
Gas-to-Liquid (GTL) technology presents
(Wilsam, 2008). In 2004, total world
one of the most immediate and ready remedy
reserves were estimated to be 1.25 trillion
for the impending energy crisis. GTL is the
chemical process of converting natural gas to reactor for methane reforming by partial
liquid transport fuels like; diesel, naphtha oxidation. This process also involves a pre-
and Liquefied Petroleum Gas (LPG). It reformer where steam reforming occurs prior
involves three major stages; the reforming of to entry to the autothermal reformer. This
natural gas to carbon monoxide and two-step reforming process is adopted to
hydrogen (Syngas production), the chain reduce oxygen demand and energy
reaction of the hydrogen and carbon requirement of steam generation.
monoxide to produce syncrude (Fischer
The steam reforming (SR) process converts
Tropsch process) and the upgrading of the
natural gas (methane) with steam on a nickel
syncrude to the desired transport fuel (hydro-
catalyst at 800-1000oC (1073 -1273 K)and
cracking).It is an established fact that there is
30-40bars (3000-4000kN/m2) to a hydrogen
far more gas than oil, and the world will still
rich synthesis gas (Christopher, 2004).
be heavily dependent on the conventional
Ni
hydrocarbon liquid fuels in the foreseeable CH4 + H2O CO +
future (Tony, 2009). 3H2∆H = + 206 kJ/mole
(1)
Most of the world natural gas reserves are in
remote locations. In these regions, pipelines The typical (H2/CO) ratio is greater than 3:1
are not economical to bring the natural gas to (Chen et.al., 2007). The natural gas must be
the market; hence converting them to liquid de-sulphurized to prevent catalyst
fuels makes it easier for transportation to the deactivation.
markets. Liquefying the gas (LNG) (which
In the partial oxidation process (PO), natural
adds only a little value to the gas) has been
gas reacts with pure oxygen in an open flame
an existing method of bringing stranded gas
at a temperature of 1473-1773 K,
to the market, which again is limited by
(Christopher, 2000).
available reception terminals and high
handling cost. CH4 + 1/2 O2 CO +
2H2∆H = - 36 kJ/mole
1.1 The Conventional Process
(2)
Most of the current world GTL plants make
use of the Haldor Topsoe process for their The process is carried out with the use of

syngas production (Figure 1). This process Nickel catalyst and it produces synthesis gas

involves the cryogenic air separation unit with a H2 to CO ratio (H2/CO) typically less

(Linde Process) to obtain oxygen, and the than 2:1, on a molar bases (Wilsam, 2008).

utilization of the oxygen in the autothermal

Reaction (2) is exothermic; the syngas exits electrons through their lattice. Mixed
the auto thermal reactor at high temperatures Perovskite/Flourite is derived from a mixture
of between 1,100-1500oC (1,373K and of the two to obtain better quality.
1,773K). The partial oxidation reaction is
2.2 Oxygen Membrane Reactor
carried out usually at high pressures of about
40 bar (4,000kN/m2). The Oxygen membrane reactor is made from
non-porous, oxygen transport membrane
materials, which have both electronic and
2.0 OXYGEN ION TRANSPORT oxygen ionic conductivity and does not
MEMBRANE degrade when operated at high temperatures,
typically between 800oC and 900oC.
Oxygen ion transport membrane (ITM) is the
Assuming a constant ionic conductivity that
commercial name for a category of ceramic
is much less than the electronic conductivity,
materials made from ionic and mixed
the oxygen flux through the membrane is
conducting metal oxides that selectively
given by the Nernst Einstein equation;
conduct oxygen ions at elevated
temperatures from bulk air. The material has 𝝈𝝈𝒋𝒋 𝑹𝑹𝑹𝑹 P′O
𝒋𝒋𝒐𝒐𝟐𝟐 = − 𝒍𝒍𝒍𝒍 �P′′O2 �
𝟒𝟒𝑳𝑳𝑳𝑳𝟐𝟐 𝑭𝑭𝟐𝟐 2
the ability of separating oxygen from air at
(3)
far lower cost than the cryogenic air
separation process. It provides a cheap Where ;
source of oxygen for syngas production with 𝒋𝒋𝒐𝒐𝟐𝟐 - the oxygen flux constant through unit
a potential significant reduction in the capital area.
expenditure of the GTL process. L - the membrane thickness (cm); n is
the charge of the charge carrier (2 for
2.1 Chemical Structure
oxygen).
There are three main types of ceramics with R - the ideal gas constant; Tis the
ion transport capabilities: Perovskite, absolute temperature.
Fluorite and mixed Perovskite/Fluorite P’O2 - the oxygen partial pressure at the
(Kirsten 2005). Perovskite ion transport feed surface of the membrane.
ceramics have the chemical structure ABO3. P’’O2 - the oxygen partial pressure at the
There may be a mixture of more elements in permeate surface of the membrane.
the A and/or B site, e.g σj - the ionic conductivity and is the only
Ba0.5Sr0.5Co0.8Fe0.2O3. Fluorite ion transport material property in the equation.
ceramics have the structure AO2, e.g ZrO2 F - Faraday’s constant.
and they can both conduct either oxygen or
The expression in equation (3) identifies the and methane reforming. Oxygen atoms
oxygen partial pressure ratio as the driving present in bulk air are reduced by the oxygen
force for the oxygen flux. reduction catalyst. This permits the charged
oxygen ions to selectively pass through the
2.3 How Oxygen Membrane Reactor
membrane. The Oxygen depleted air stream
Works
leaves the reactor as a by-product.
As shown on Figure 1, the oxygen
membrane reactor combines air separation

Figure1:Schematic of the workability of the Oxygen Membrane Reactor.

Source: Air Products and Chemicals Incorporated (2008).

The permeated oxygen ions immediately The conventional GTL process is capital
react with natural gas (reforming reaction) intensive; hence the plant needs to be large
with the aid of the reforming catalyst. The scaled in order to achieve economic
reaction product is syngas and is collected as operation. Synthesis gas production accounts
the main product of the reactor. As seen in for more than 60% of the total cost of the
equation 3, oxygen partial pressure ratio is plant (Kim et al., 2009). This huge capital
the driving force for oxygen transport. cost is mainly due the cryogenic air
Oxygen partial pressure is always higher on separation unit (ASU) which supplies
the bulk air side of the reactor and lower on oxygen for syngas production. The air
the permeate side due to depletion by separation unit in
reforming reaction. Figure 2 is said to be the single most
expensive unit of a GTL plant and makes up
3.0 STATEMENT OF PROBLEM 20% of the cost of a typical GTL plant
including off sites and utilities (Steynberg, 2007).

P-17
P-19 P-20 P-18 P-20

P-1 P-27
P-2 I-3
V-2
P-5
P-6
P-26
P-66 P-67 P-24
I-2

E-12 I-4

P-16

P-8
E-8

P-7

P-3 E-2 E-3

P-28
E-1
P-44

P-50 P-15
V-6 E-4

P-39
I-10
P-34 P-51 E-7
P-32 P-48
V-1
I-14 P-14
V-5
V-4
I-7 P-56
P-65
P-61
P-58 P-43 P-53 P-9 P-10 P-11 P-12
E-21

I-9 E-9 E-10 E-11

P-55
E-22
P-54

I-8 P-57 E-6

E-16 E-17 I-6 I-11
V-3 I-12 P-13
I-5
E-25
E-19 P-64 E-18 P-49 E-5

P-33
I-13
P-38 P-63 P-46 P-60 P-35 P-41
P-47
P-29
E-24
P-52 P-62
P-37
E-20

Figure 2 :Process Flow Diagram of the Conventional Syngas Production Process

N/B: Reddened area is the ASU which makes up more than 20% of the total cost of a typical GTLprocess (Steynberg,2007)

In this work, the ability of the ‘oxygen generation, making the process a net
membrane reactor’ to combine air separation electricity generator.
and methane reforming is employed, to
modify the conventional ‘HaldoeTopsoe’ 3.1 Proposed Modification of Conventional
syngas process. The objective is to greatly GTL Process
reduce the overall cost of the Gas-to-Liquid Using the Oxygen transport membrane
process, making it more economical and concept, Figure 3 is a proposed flow diagram
enhance its proliferation. To maximise the for the modification of the conventional
energy consumption of the process, the high syngas generation process; combining air
pressure, depleted-air stream is further separation and methane reforming into a
utilized in a turbine for electricity single oxygen membrane reactor with co-
power generation.
3.2 Detailed Process Description 10. The compressed air is heated to between
800oC and 900OC,the operating temperature
The two major feeds to the process are
of the oxygen membrane reactor (E-4). The
natural gas and atmospheric air, while the
heating is done by externally fired heaters
main product is syngas. The processed is
within heat exchanger-fired heater E-1. The
described based on these streams.
heated air stream P-27, is introduced to the
3.2.1 Air Stream cathode side of the oxygen

Atmospheric air P-25 is compressed to a

pressure of 30 to 40 bars by a compressor E-
P-36 Hydrogen purge stream P-15
Pure Syngas 2:1 H2/CO ratio. Feed to Fische Tropsch process

P-5
P-14
Raw Syngas
300c
I-1
P-16
CO2 rich stream Condensate P-35

Flue gas
P-42
Component splitter
E-9 E-8
E-15 CO2 Compressor
Condenser
P-17
P-19
Desulphurizer E-2 Sub-cooled Syngas
P-37
200 C
E-14
P-20
Steam vent Steam turbine
P-39 S-2 P-13
P-4
Natural Gas Feed P-6 300c
P-31
40bar Electricity
HE
P-22 P-21
P-23 I-4 E-16 Cooled Syngas
I-2
I-8 400 C
450-500 C I-5
P-12
P-7 P-24

P-32
P-8 P-19 P-18
E-1 Steam
Boiler feed water
Boiler
Fired Heater

Pre-reformer E-5

P-26 P-27
E-3
Atmospheric air 21% oxygen

P-9 1100-1200C P-10

P-33 P-11
P-40 P-41
Reformed natural gas Hot Syngas
P-25 ITM Oxygen reactor
E-4 1000C
E-10 P-34
Air Compressor P-30

30-40bar
I-7
Depleted air 3-4% oxygen

E-13
Turbine P-28
P-38 S-1
P-29
Electricity

Figure 3 : PFD of the Proposed Modification of the GTL Syngas Process using the Novel
Oxygen Membrane Reactor.

membrane reactor where some of the consumed by the anode-side reactions, the
contained oxygen is transferred to the anode partial oxygen pressure at that side will be
side to react with natural gas. The driving very low and the ratio of partial oxygen
force for oxygen permeation is the ratio of pressures very high, thereby permitting
partial oxygen pressures at the cathode and transport of oxygen.
anode side of the membrane. Since oxygen is
The oxygen permeation within the reactor hydrocarbons, to methane, carbon monoxide
produces an oxygen depleted air stream P-28 and hydrogen.
containing between 3% to 10% oxygen. This
Since the adiabatic pre-reforming is
depleted air stream is first of all heated to a
endothermic, the gas will experience a drop
temperature of about 1200oC and expanded
in temperature across the pre-former, hence
in the turbine unit E-13. The turbine drives
the resultant stream P-9 is heated to the
the compressor unit E-10 and also drives a
membrane operating temperature. The
power generator that produces part of the
methane containing stream P-10 enters the
electrical power requirement by the plant.
anode side of the oxygen membrane reactor
The expanded stream P-29 is then
at a temperature and pressure that permits
discharged through the heat exchanger-fired
the conversion of all the remaining methane
heaterE-1 where it transfers sensible heat to
to syngas (typically about 1000°C and 30-40
entering gases and the contained residual
bar pressure). The anode side of the oxygen
oxygen supports combustion of fuel to the
membrane reactor has a first section which
extent required to raise incoming cold
contains no catalyst. Process gas in the
streams to the desired temperature.
methane containing stream reacts with the
3.2.2 Natural Gas Stream permeated oxygen predominantly in a partial
oxidation reaction because of the absence of
Natural gas feed stream P-6 is heated to an
reforming catalyst. Since the reaction is
intermediate temperature of about 300°C
exothermic, the temperature of the permeate
within the heat exchanger-fired heater E-
and non-permeate side gases increase.
1, then mixed with hydrogen purge stream
Beyond this point, a catalyst is installed
P-36 and desulphurized in the
within a second section of the anode side of
desulphurization unit E-2. The resultant
reactor.
stream, having a super- reduced sulphur
content, is mixed with a stream P-23 made In the catalyst containing section of the
up of steam and recycled CO2 stream to form reactor, permeated oxygen reacts with the
a stream P-7 having the desired steam to process gases in a combined partial
carbon ratio (typically 0.6:1.5) needed to oxidation and steam reforming reaction. The
feed the pre-reformer. Stream P-7 is heated exothermic heat released by the oxidation
to between 450°C and 550°C within the heat reactions balances the endothermic heat
exchanger-fired heater E-1 and the hotter consumed by the steam reforming reactions.
stream P-8 is passed through an adiabatic The reforming reaction is promoted by the
pre-reformer E-3 which converts heavier catalyst which is either contained in the
porous support of the membrane or in a
catalyst bed adjacent to the membrane. To The syngas stream P-14 still contains some
maintain the overall and local heat balances impurities which are predominantly carbon
along the bed at a level which prevents dioxide. This carbon dioxide rich component
excessive temperature rise of the transiting is removed in an acid gas removal unit E-9,
gases, control is exercised by adjusting local which can be a liquid wash system in which
catalyst activity, gas composition, and acid gases are stripped or absorbed by an
oxidant supply. amine wash.The pure stream leaves as the
final syngas product stream P-15 for
The reactions occurring in the Oxygen
delivery to the downstream Fischer Tropsch
membrane reactor are as shown in equations
process.
(1) and (2).

3.2.3 The Syngas Stream

4.0 SIMULATION OF THE
The raw syngas stream P-11 is at a
MODIFIED DESIGN
temperature of about 1000oC and has a
composition that is conducive to dusting of The proposed design was simulated using
metal surfaces. In this design, metal dusting Aspen HYSYS version 2006 and the
is avoided by cooling the process gas in a diagram is as shown in Figure 4.
boiler E-5, using a cold water streamP-18 to
Oxygen membrane reactor is provided for in
produce steam (P-19). The produced steam
the simulation scheme by the use of a
is used to drive the turbine unit E-14, which
combination of two reactors. Stream 28
generates part of the electricity for the plant
carries compressed air to the first reactor
and also drives the CO2 compressor.After
which acts as the cathode. Permeated oxygen
leaving boiler E-5 the water contained in the
is sent to the second reactor (stream 32)
raw syngas stream is condensed in a
while the oxygen depleted air is sent to the
condenser E-16 and removed in a
turbine (stream 2). The reforming reaction
separator E-8 as a process condensate
occurs in reactor 2.
stream P-35.
Figure 4 : Simulation Diagram of the Modified GTL Syngas Process using Aspen HYSYS.
Courtesy: The University of Manchester, United Kingdom.

4.1 Simulation Result that the modified design is viable and can
provide the same capacity as the
The simulation successfully solved at the
conventional process. The results obtained
conditions described above. This confirms
are summarised as shown in Table 1

Table1: Summary of Simulation Result.

Feed Product

Natural gas feed = 183, 333.33m3/h Syngas produced = 27700 m3/h

Steam feed = 109, 999.998 m3/h CO2 produced = 1.803 × 107 kg/h

Plant Steam consumption = 363,100 kg/h Steam Turbine duty = 5.176MW

Gas Turbine duty = 43.1MW

syngas process which are elaborated below.

The most significant of which is the reduced
5.0 DISCUSSION
energy consumption of the proposed process.
The proposed syngas process (Figure 3) has
a lot of advantages over the conventional
5.1 Elimination of Air Separation Unit source of oxygen at over 99% purity at the
desired temperature and pressure of 900oC
The greatest advantage of the proposed
and 30 bar eliminating the need for storage,
design is the elimination of the cryogenic air
excessive compression, cooling water
separation unit, which greatly reduces the
requirement and over 64% electrical energy
capital cost of the entire plant. The proposed
savings on power consuming equipment
design offers a just-in-time and cheaper
alone.

Table 2: Comparison of the Major Electricity Power consuming Equipment

for 3,500mt/day-oxygen production.
Equipment Description Conventional Proposed Process Savings
Process
Refrigeration compressor 2743KW Absent 2743KW
HP BFW pump 7569KW 2523 KW 5046KW
Water cooling pumps 3132KW 2192.4KW 939.6KW
TOTAL 13444KW 4715.4KW 8728.6KW

5.2 Compact Size 5.3 Intergration With Power Production

The integration of oxygen production and The proposed design is a net electricity
methane reforming into a single unit of producer. It integrates syngas production
oxygen membrane reactor greatly reduces with power generation into a single plant as
the size of the entire GTL plant. The reactor shown in the PFD. According to the
supplements the function of the ATR and simulation result, 43.1 MW of electricity can
ASU in the conventional design. According be produced from the proposed design.
to Paul et al. (2007) this route will reduce the This can be used to not only supply the
size of an entire GTL plant by a factor of electricity need of the syngas plant but can
about 20 and the weight in tonnage by a be exported to other parts of the entire GTL
factor of 60. This has a far reaching cost and plant.
logistics advantage especially in locations
5.4 Safety
where space is a limitation like offshore
locations. Due to the elimination of the ASU, the risk
of handling pure oxygen (which is highly
flammable) is eliminated. The oxygen
membrane reactor is designed to consume
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The proposed syngas production process will
offer great cost savings in the Gas-to-Liquid
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APPENDIX A
Equipment Summary for PFD of 15. P-18: Boiler feed water stream
Proposed Process 16. P-19:Boiler produced steam
Main Units: 17. P-20:Steam vent stream
1. E-1: Fired heater 18. P-30:CO2 by-pass stream
2. E-2:Desulphurizer 19. P-21: Steam by-pass stream
3. E-3:Adiabatic pre-reformer 20. P-25: Air compressor feed stream
4. E-4: Oxygenmembrane reactor 21. P-26:Compressed air stream
5. E-5:Boiler/heat exchanger 22. P-28:Depleted air-stream
6. E-16:Heat exchanger 23. P-37:Fired heater flue gas stream
7. E-8:Condenser 24. P-35:Condensate stream
8. E-9:Component splitter 25. P-22:CO2/steam mixed stream
9. E-10:Air compressor 26. P-23:P-22 Split stream 1
10. E-13: Gas turbine 27. P-24: P-22 split stream 2
11. E-14:Steam turbine Equipment Summary for PFD of
12. E-15:Carbon dioxide compressor Conventional Process
Utility Units: Main Units:
1. 1-2:Disulphurizer exit/CO2 recycle 1. E-1:Disulphurizer
mixer 2. E-2: Steam reformer
2. 1-7:Fired heater mixer 3. E-3:Fired Heater
3. 1-5: CO2/steam stream splitter 4. E-4: Autothermal reformer
4. 1-4:CO2/steam stream Mixer 5. E-5:Cryogenic Oxygen tank
Piping/Streams: 6. E-6: Condenser
1. P-6:Natural gas feed stream 7. E-7:CO2 extractor
2. P-5:Heateddesulphurizer feed. 8. E-8: CO2 Compressor
3. P-32:Desulphirized mix stream 9. E-9: Cooler 1
4. P-7:Pre-reformer heated feed. 10. E-10: Cooler 2
5. P-9:Reformed natural gas 11. E-11: Cooler 3
6. P-10: ITM oxygen reactor feed. 12. E-12: Heat Exchanger
7. P-11:Hot syngas stream 13. E-16: Inter-stage cooler
8. P-12:Cooled syngas stream 14. E-17: Stage Compressor
9. P-19:Sub-cooled syngas stream 15. E-18: Final Stage Cooler
10. P-14:Raw syngas stream 16. E-19: Air Feed Compressor
11. P-15: Pure syngas product stream 17. E-20: Linde Lower Column
12. P-36: Hydrogen purge stream. 18. E-21: Linde Upper Column
13. P-16: CO2 rich stream 19. E-22: Condenser-reboiler
14. P-17: Compressed CO2 stream 20. E-24: Reboiler
21. E-25: Heat Exchanger 32. P-11:3rdStage cooled reactor product
33. P-12: CO2/Syngas stream
Major Streams 34. P-13: Condensed Liquid stream
22. P-1: Natural Gas Feed 35. P-14: Purified Syngas to F-T Plant
23. P-2: Pre-heated NG stream 36. P-15: CO2 Compressor feed
24. P-3: Disulphurized NG Stream 37. P-16: Compressed CO2
25. P-4: Air feed 38. P-23: Pure Oxygen
26. P-5: CO2 Mixed NG Stream 39. P-46: Liquid Nitrogen (with traces of
27. P-6: Heated CO2/NG Stream Argon and other air-components)
28. P-7: Pre-reformed NG
29. P-8: Autothermal NG/CO2 feed
30. P-9: 1st Stage cooled reactor product
31. P-10: 2ndStage cooled reactor product
28. P-27: Heated Atmospheric air.