You are on page 1of 10

See discussions, stats, and author profiles for this publication at: https://www.researchgate.

net/publication/269762373

Recent development in converting coal to clean fuels in China

Article  in  Fuel · July 2015


DOI: 10.1016/j.fuel.2014.11.059

CITATIONS READS

53 2,633

3 authors, including:

Jian Xu Yong-Wang Li
Synfuels China Ltd. Chinese Academy of Sciences
64 PUBLICATIONS   1,238 CITATIONS    608 PUBLICATIONS   12,852 CITATIONS   

SEE PROFILE SEE PROFILE

Some of the authors of this publication are also working on these related projects:

Applied-fundamental research on iron based Fischer Tropsch synthesis catalsysts View project

We are working on commisioning of a large scale FTS plant using the slurry Fischer-Tropsch process developed by us. I am summarizing literature in Fischer-Tropsch in
my spare time, and review papers, reports and design schemes for new projects. View project

All content following this page was uploaded by Jian Xu on 14 March 2018.

The user has requested enhancement of the downloaded file.


Fuel 152 (2015) 122–130

Contents lists available at ScienceDirect

Fuel
journal homepage: www.elsevier.com/locate/fuel

Review article

Recent development in converting coal to clean fuels in China


Jian Xu, Yong Yang ⇑, Yong-Wang Li ⇑
National Engineering Laboratory for Indirect Coal Liquefaction, Chinese Academy of Science, Leyuan South Street, No. 1, Yanqi Economic Development Section C, Huairou
District, Beijing 101407, China
State-Key Laboratory of Coal Conversion, Chinese Academy of Science, P.O. Box 165, Taoyuan Nan Road 27, Taiyuan 030001, China
Synfuels China Technology Co., Ltd., Chinese Academy of Science, Leyuan South Street, No. 1, Yanqi Economic Development Section C, Huairou District, Beijing 101407, China
Institute of Coal Chemistry, Chinese Academy of Science, P.O. Box 165, Taoyuan Nan Road 27, Taiyuan 030001, China

h i g h l i g h t s

 CTL/SNG projects in China are integrated to improve the energy efficiency and process economics.
 Dry feed entrained flow gasification are major choice for large scale gasification.
 It is proposed to combine the SNG and FTS processes by using moving bed gasification.
 New syngas conversion technologies are emphasized for efficient conversion catalyst.

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

Article history: To achieve energy security in an environmentally benign way, China has to convert a significant fraction
Received 12 June 2014 of its abundant coal resource to clean fuels (liquid fuels or synthetic natural gas, SNG) to meet the fast
Received in revised form 13 November 2014 increasing demand on transportation fuel and municipal gas. Following the successful operation of the
Accepted 17 November 2014
4000 bbl/d Yitai and Luan coal-to-liquids plants using the medium temperature Fischer Tropsch synthesis
Available online 9 December 2014
(MTFT) process technology from Synfuels China, tremendous progresses have been made in upscaling the
Fischer–Tropsch synthesis (FTS) process in China. Past experiences gained from the efforts in this field
Keywords:
have shown that further exploration in the coal conversion field requires significant technological
Coal to liquids
Synthetic natural gas
improvement on gasification, synthesis, and utilities related to integrating more efficient and environ-
Fischer Tropsch synthesis mentally friendly processes on the basis of current status of applications.
Gasification Ó 2014 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 123
2. Syngas production and gasification technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 123
2.1. Syngas production from coal . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 123
2.2. Lurgi moving bed gasification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 124
2.3. Entrained flow gasification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 125
3. Gasification-based coal conversion processes development . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 127
3.1. CTL and SNG projects in China . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 127
3.2. Syngas conversion technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 127
4. Perspectives . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 129
5. Conclusions. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 129
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 130
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 130

⇑ Corresponding authors at: National Engineering Laboratory for Indirect Coal Liquefaction, Chinese Academy of Science, Leyuan South Street, No. 1, Yanqi Economic
Development Section C, Huairou District, Beijing 101407, China. Tel.: +86 10 69667788; fax: +86 10 69667800.
E-mail addresses: yyong@sxicc.ac.cn (Y. Yang), ywl@sxicc.ac.cn (Y.-W. Li).

http://dx.doi.org/10.1016/j.fuel.2014.11.059
0016-2361/Ó 2014 Elsevier Ltd. All rights reserved.
J. Xu et al. / Fuel 152 (2015) 122–130 123

1. Introduction converter (WGS) and gas purification (Rectisol and sulfur recovery)
(Fig. 1), which is a sophisticated plant and costly investment.
Global energy structure transformation has been taking place in Depending on the regional difference in coal feedstock across
industries, especially in areas with limited conventional oil and gas China, the gasification technology selection criteria has to take
resources. These changes along with the fast increasing demands the following parameters into consideration for evaluating the per-
for motor fuels and town gas have greatly impacted on the energy formance of any industrial gasification process: (1) the energy con-
sector inside China [1]. Due to lack of sufficient gas or oil reserves, version efficiency; (2) carbon efficiency; (3) thermal efficiency; (4)
coal accounts for about 92.6% of the gross reserves of exploitable cold gas efficiency. Additionally, performance parameters such as
fossil energy resources in China [2]. The dramatic increase in raw gas composition, capacity, operation pressure, coal and oxygen
energy demand has decreased the current oil self-sufficiency level consumption should also be compared. Details on gasification
to about 41.9% by the end of 2013. Within the next ten to fifteen chemistry, gasifier concepts, applications and research trends can
years, the Chinese oil demands and supply capacity is predicated be referred to excellent reviews by Gräbner and Meyer [7] Higman
to approach a level of 750–800 million tons annually. The domestic and Tam [8,9], Bell et al. [10] and Tang [11].
production of the crude will hardly exceed 200 million tons per During the past twenty years, international as well as local gas-
year, leaving the gap of about 550–600 million tons to be imported, ifier vendors are competing for licensing their technology in China
which is equivalent to an alarming oil self-sufficiency level of only market, while local vendors have been investing heavily on invent-
25–28%. This is in agreement with an IEA forecast which points to ing and improving their technology to suit the specific requirement
China’s primary oil demand of 15.3 million barrels per day (about of gasifying a variety of coal. As shown in Table 1, major vendors of
700 million tons/a equivalent), and import dependency of 77% gasification technologies imported into China are Shell [3,12,13],
[3]. Traditionally, energy products are supplied by processing Siemens GSP [14–16], General Electric Energy (formerly
crude oil and natural gas. However, domestic production of oil GE-Texaco) [17] and Lurgi [11,18]. Along the progress of coal
and natural gas is very limited because of a lack of reserves, and gasifier installation and commissioning in chemical, metallurgical
in the past years, an ‘‘energy diplomatic politics’’ has been formed and town gas production industry and based on the knowledge
for China during its economy boosting era. However, eventually it and operation experiences learned, several indigenous gasifier
is the trade balance as a decisive factor pushing China to convert concepts have been conceived and scaled up to commercial scales.
coal into energy products such as clean liquid fuels (CTL) and syn- A summary of the performance comparison is given in Table 1,
thetic natural gas (SNG), which can partially reduce the ever which lists operation performances of Chinese gasification technol-
increasing cost in importing these resources [4,5]. ogies including East China University of Science and Technology’s
Coal to liquid has been a long story for China since the war time Opposed multi-nozzle (ECUST-OMB) [19,20] and the Hangtian
in 1940s, which has been a debating topic for every stage formulat- Gasifier (HT-L) [20,21].
ing the country’s energy strategy [1,6]. Progresses from early For coal and other solid fuel as feed, coal gasification process
efforts were limited mainly resulting from the upheavals in operating typically at the temperature range from 900 °C to
economics along with crude oil price fluctuations. The high oil 1600 °C can be selected according to the properties of the feed.
price since the end of 1990s has prompted the latest efforts in coal Currently, there are several types of coal gasification technologies
to liquid development in the country: the route via gasification that can be selected using solid fuel as a feedstock. Lurgi gasifica-
and Fischer–Tropsch synthesis has been technically well developed tion has been used to gasify tens of millions tons of high ash coal
and many related processes have been tested. This article will annually in the world largest CTL facilities of Sasol, a well-known
conduct a general review of these developments in this direction South Africa company running CTL business since 1950s [22].
and the future developments of these fields will be discussed on Recently, three CTL plants have been established based on the
the basis of the technological as well as industrial demands for MTFT (Medium Temperature Slurry Fischer–Tropsch Process) tech-
the future. nology developed by Synfuels China [1,6]. The CTL plants have used
different types of gasification technologies, i.e., multi-slurry gasifi-
2. Syngas production and gasification technologies cation in Inner Mongolia Yitai plant, pressurized fixed bed gasifica-
tion in Shanxi Luan plant, and Shell dry powder gasification in
2.1. Syngas production from coal Inner Mongolia Shenhua plant.
The major concerns of syngas production units for the
Syngas production is the key to high plant availability and successful industrial Fischer–Tropsch processes are:
economic success for CTL/SNG projects. The gasification complex
for syngas production, gas conditioning and cleaning usually costs (1) Maximized conversion efficiency in terms of specific fuel
about two thirds of the total direct capital investment of a CTL feeds by taking care of the syngas production units
plant. The gasification complex typically consists of units like coal themselves and considering the integration of the whole
preparation, air separation (ASU), gasification, water gas shift plant from the preparation of the feed to the final products.

Fuel
Preparation CO2 S
Fuels Raw Shifted
Syngas Syngas
Air Separation O2 Gasifier or WGS Rectisol
Unit Converters Converter Process
Steam
Ash slag Purified
Syngas to
FT/SNG

Fig. 1. Typical syngas production complex.


124 J. Xu et al. / Fuel 152 (2015) 122–130

Table 1
Performance of major coal gasification technology in China [8,9,11–16,18–20,22,23].

Parameter/item Vendors/licensors
Shell SCGP Siemens/GSP Lurgi (Mark V) ECUST OMB HT-L GE-energy
Raw syngas (dry) (km3 (std)/h) 187–206 132–142 159–185 119–131
Raw syngas composition
CO (vol%) 60–65 65–75 16–28 61.6 61.9 39/45
H2 (vol%) 23.84; 18–23; 30 20–28 38–40 30.24; 37.6 26.3 38; 36.63
CO2 (vol%) 3.84; 2–3; 1.6 4–5 27–32 16.5; 4.51 8.2 21; 17.69
H2O (vol%) 0.1
CH4 (vol%) 100–200 ppm 0.05–0.1 7–12; 16–18 756 ppm 0.09
H2S (vol%) 0.3
Dry coal input (t/h) 2000–2850 2000–2300 1800 2500–3000 1800 2000
Operation pressure (MPa) 2.0–4.0 2.5–4.2 3.0–5.0 3.0–6.5 3.7–4.0 4.0–6.5; 8.7
Maximum gasification temperature (°C) 1400–1600 1350–1750 1300–1400 1400–1750 1300–1400
CO + H2 (vol%) 90–94 92–95 65 77; 81–83.4 86–92 78–81
Coal consumption (kg/kN m3) (H2 + CO) 635 653 693 640
Oxygen consumption (N m3/kN m3) (H2 + CO) 320; 330–360 331 160–270 432 322 380–430
Cold gas efficiency (%) 80–85 78–85 65–75 70–76 75–84 70–76
Carbon efficiency (%) >99 98–99 88–95 98.6–99.1 98–99.5 96–98
Thermal efficiency (%) 98 90 95–96 90–95

(2) Syngas process must be designed for maximizing the opera- 2.2. Lurgi moving bed gasification
tion reliability.
(3) For typical CTL/SNG plant, 70–80% of the total water con- The Lurgi moving bed gasification was introduced into China for
sumption and emission of the entire plant are due to the ammonia and town gas production from coal in late 1970s. The fol-
syngas production unit. Therefore, water saving and envi- lowing diagram shows schematic flow sheet of around Lurgi-type
ronment protection must be seriously considered in the syn- gasifiers [11].
gas production process. The original moving bed gasifier was designed for operation at
(4) The success of the gasification technology for solid fuel feeds about 28–30 bar using granular coal with size between 8 mm
has been proven to rely heavily on the properties of the feed, and 50 mm, for example in SASOL CTL plants and in early China’s
and the wrong selection of the gasification technology ammonia and town gas plants. The experiences from those plants
always leads to the failure of the whole project. show that although mechanic maintenance efforts are demanded
(5) Upgrading the fuel feed to higher energy density should be due to these moving parts in the gasifier the overall availability
encouraged for the conversion of the low energy density could be high when many units operate in parallel [8].
raw feed. In China, many lessons have been learned from the operation of
the moving bed gasifiers. The coal selection must be carefully
Syngas produced must be well conditioned and purified for considered in order to have successful operation. Normally, the
down-stream FTS. Generally, raw syngas from gasification unit non-sticky coal with properly high mechanic strength and higher
cannot meet the down-stream FTS requirement because of (1) melting point of ash (>1200 °C) can be easily handled in this type
improper H2/CO ratio, (2) contents of sulfur and other poisoning of gasifier. The biggest problem is the heavy cost of the treatment
components, and (3) contents of significant amount of CO2 unde- of large volume of waste-water (gas water) condensed from the
sired for the FTS loop. The ash or carbon dust contained in the hot gas cooling system as shown in Fig. 2. Eventually, the gasifier
raw syngas is generally removed by wet scrubbing. For most coal needs large volume of steam to be fed with oxygen to keep the
derived syngas, H2/CO ratio needs to be increased by using sul- temperature in the combustion zone lower than the melting point
fur-resistance water–gas shift (WGS) unit, where the dust-free of ash, which increases coal contaminated water after the gas cool-
syngas passes through the water–gas shift reactor, converting CO ing system. This not only causes high water consumption but also
into H2 through the water–gas shift reaction. creates challenges for down-stream waste water treatment.
After the H2/CO ratio conditioning unit, the shifted syngas mix- Recent demands for synthetic natural gas (SNG) in China have
ture is introduced into the purification unit to remove sulfur, CO2, greatly promoted the mass application of Lurgi-type gasification
and any other harmful components. The most effective technology because of the advantage with high content of methane from coal
for this purpose is the Rectisol type of process, which uses metha- pyrolysis being maintained only from Lurgi-type gasifier. From
nol as solvent for adsorbing these impurities and operates at cryo- these SNG projects, even much more lessons have been added:
genic conditions. The Rectisol process outputs clean syngas to (1) corrosion problems arising from the coal with high salt (Na,
typically sulfur content below 0.1 ppm and CO2 content less than K) contents (close to 10% in ash); (2) corrosion problems probably
0.5 vol%, and the sulfur captured by the solvent can then be pro- resulting from higher pressure up to 45 bars; (3) much waste water
cessed to produce pure sulfur or sulfuric acid as by-product. After- produced from high moisture coal feed and higher added steam
wards the syngas passes through a guard-bed filled with solid and from coal with lower melting temperature (1100 °C). These
adsorbents for further sulfur capture, leading to the final syngas lessons have shown that a systematic research and development
suitable for the CTL/SNG with a few ppb of sulfur. The sulfur con- is still required for further improvement of this old version of gas-
tent must strictly be suppressed during the syngas preparation ification technology.
step. In the cases of FTS with the iron catalyst in the fixed bed, It is also worth mentioning a moving bed slagging gasifier orig-
the sulfur content below 0.1 ppm is safe, while the sulfur content inally developed by British gas and Lurgi, called BGL gasifier, which
below 0.05 ppm is normally required for the iron catalyst in the is an extension of original Lurgi moving bed gasifier with the ash
slurry bed. The sulfur content below 0.005 ppm is necessary for discharge oriented for slagging conditions. Because the gasifier
the cobalt catalyst in the slurry bed. can be operated at higher combustion temperature, the capacity
J. Xu et al. / Fuel 152 (2015) 122–130 125

Coal

LP steam
Lock gas
Coal BFW
BFW
lock Dewater gas
Raw gas
300-520oC

BFW BFW

Gasifer

Gas water Gas water Gas water


Steam
Water jacket
Oxygen
Steam
Recycling
Ash
water
lock

Ash

Fig. 2. Typical scheme for moving bed gasifers.

Gas water

Oxygen

Washing
tower Dust free
Gasificaon wet raw gas
chamber

Coal Quench water


Wet raw gas
with dust
Exit Black water recycle
Coal Slurry

Mill
Dust lean water
Coal Slurry

Waste water

Ash
lock
Slurry tank Slurry pump

Black water recycle


Dust rich water
Ash/slagg

Fig. 3. Entrained flow gasification with coal–water slurry.

is higher and the steam consumption is significantly reduced, quenched with water at the top of the down pipe, where both
therefore largely reducing the problematic waste water [8]. High gas and ash are cooled quickly. The quenched gas and ash pass
oxygen consumption and lower methane content in the gas stream down to the down pipe into a water bath at the bottom of the gas-
is the major pay-off from Lurgi upgraded to BGL. ifier vessel. The gas is then washed in the bath and flows up
through the baffles between the outer wall of the down pipe and
2.3. Entrained flow gasification the gasifier vessel and exits the vessel. The ash is removed from
the bottom of the gasifier vessel through a slag lock. The gas is fur-
The entrained flow gasification with coal–water slurry as feed ther washed in a washing tower to remove the carried dust.
first invented by Texaco was introduced into China for ammonia This type of the gasification produces good quality syngas with
projects in 1980 [24]. The gasification uses coal–water slurry as H2/CO ratio of 0.7–0.85 and a low methane content, which is suit-
feed at the top of the gasifier vessel, which reacts with oxygen at able for F–T synthesis. In addition, a fraction of polluted water can
temperature between 1300 and 1400 °C, ensuring the ash in the be consumed by water slurry benefiting the environmental protec-
melting state in the gasification chamber (Fig. 3). The hot gas and tion efforts. However, the high oxygen consumption and lower
melting ash flowing down through the refractory wall are energy efficiency due to the low energy density in the water
126 J. Xu et al. / Fuel 152 (2015) 122–130

Oxygen
Gas water

Washing
tower
Gasificaon
chamber Dust free
Pulverized wet raw gas
Coal stack
Quench water
Exit
Wet raw gas
with dust

Black water recycle


Coal

Coal powder

Dust lean water


lock

Mill

Ash
Hot flue gas lock

Coal powder
Feeding tank
Black water recycle
Dust rich water
Carrying gas
Ash/slagg
CO2

Fig. 4. HTL gasification system developed in China.

diluted feed is the major disadvantage of this gasification system The major gasification technologies used in China in the past fif-
although much experiences have been accumulated in the large teen years are listed in Table 1 with some important performance
scale operation. parameters. The experiences in the application of gasification tech-
The original Texaco gasifier uses single jet (at the top of the nologies in China can be summarized here:
gasification vessel). The latest development for coal–water slurry
gasifier is expanded to multiple jets around the upper part of the (1) The long and stable operation has been achieved for water-
gasifier with the top jet, which leads to better flow field in the com- slurry, Shell, HTL, GSP gasification system;
bustion chamber and therefore higher conversion of carbon in (2) Coal property control for a specific gasification technology is
flowing ash. With multiple jets, the gasifier can be easily scaled very critical for reach good performance;
up to a capacity of processing 3000–4000 t coal per day [19]. (3) The higher throughput of single train gasifiers can signifi-
The HTL gasification system developed in China is designed to cantly reduce the cost;
use dry pulverized coal. The cooling screen around the gasification (4) Moving bed gasification system is safe for some hard coal
chamber is used to protect the pressurized vessel from the high with sufficient mechanic strength and higher ash melting
gasification temperature (1350–1600 °C). More than thirty HTL point;
gasifiers have been constructed for ammonia and methanol pro- (5) For most of the water-slurry gasification, the oxygen con-
jects in the past ten years in China. After the gasification chamber, sumption is high, and the energy efficient is low due to
the major design is quite similar to that in coal–water slurry gasifi- diluted energy density of coal feed by water;
ers (Fig. 4). A similar gasification system but with different struc- (6) For most of the dry feed entrained flow gasification technol-
ture in the gasifier is GSP gasification (now owned by Siemens). ogies, high power consumption of feeding system counter-
Five GSP gasifiers have been used in methanol to propylene acts part of the efficiency gained from higher energy
(MTP) project in Ningxia. From the initial operation tests of these density in dry feed;
dry feed gasification system, major issue is that flying ash carrying (7) For HTL and GSP gasifiers, it is more difficult to form slag
high carbon content causes down-stream problems and low carbon film on the cool screen than for Shell gasifiers due to differ-
conversion (93–95%). After major modification in gas washing sys- ent flow field in the combustion chamber;
tem, long term operation can be achieved, especially for GSP gasi- (8) HTL and GSP gasification technologies have lower carbon
fication system [8]. conversion due to the high flowing ash with high carbon
Shell gasification is another type of system applied in ammonia, content;
direct coal liquefaction, and recently indirect coal liquefaction pro- (9) Single jet entrained flow gasifier is difficult to scale up to the
jects [12]. Empowered by lessons learned from previous projects, capacity 3000–4000 t/d.
this type of gasification system is approaching long term operation (10) Moving bed gasification has not reached to success in recent
with high carbon conversion. A dry gas cleaning system consisted large scale project due to coal properties and the very low
of filtration units is used in capturing flying ash from the gas capacity of this type of gasifier;
stream at about 300 °C downstream the gasification and boiler (11) High steam demands and large waste water production are
train. Because less water is consumed in the Shell gasifier, the syn- major issues existing in the Lurgi type moving bed gasifier
gas thus generated has very low moisture, which requires addi- with solid ash removal.
tional steam from the hot gas driven boiler in the WGS unit.
Major issue in selecting Shell gasifier is its high capital cost result- Recent efforts in China will greatly promote the improvement of
ing from the boiler and filtration system and the WGS system [11]. all kinds of involved gasification technologies. The important
J. Xu et al. / Fuel 152 (2015) 122–130 127

aspects will focus on scaling up to the capacity of 4000 ton coal per Coal Steam
day for entrained flow gasification, realizing a pump for pressuriz- Water Power Station Power Air Separation Air
ing pulverized coal to replace the power demanding feeding sys-
Steam & Power
tem for dry feed entrained flow systems, and improving the dry to all units
Oxygen
feed gasifiers and its syngas composition in terms of WGS cost,
waste water generation and the heat removal from hot gas after Coal Raw
gasification chamber. Additional efforts is a completely new Gasification WGS Purification
Syngas
scheme for black water from gasification and gas water from syn- Clean Syngas
gas condensates for all type, especially Lurgi-type, of gasification
technologies. Syngas Syncrude Product Fuel
Conversion upgrading Products
3. Gasification-based coal conversion processes development Fig. 5. Schematic process diagram of a typical coal conversion plant.

3.1. CTL and SNG projects in China


In contrast, the indirect coal liquefaction (ICTL) technology for
CTL and SNG have been paid great attention recently in China, producing mainly ultra clean diesel fuel is well established in the
with mega projects approved by the central government as an engineering field and is steadily pushing forward even under strict
important strategic development of the national energy system government control. The latest development is the government
(see Table 2) [5,25,26]. Both CTL and SNG share the same kind of approved commercial scale four million ton per year Shenhua–
syngas generation and cleaning units and utilities prior to the syn- Ningmei project. The construction work was started in 2013 and
gas conversion unit, where FT synthesis and methanation taking is scheduled to commission in 2017. In addition, the Shanxi Luan
place respectively. The synthetic products are upgraded to either High Sulphur Coal Co-production project also started construction
liquid fuels or synthetic natural gas as final outputs as schemati- in 2013. The technology for these two projects is both licensed by
cally shown in Fig. 5. Synfuels China, which provided licensors to three 160 kt/a
The striving to meet challenges in energy independence and demonstration projects in 2009. At the same time, Yankuang
environmental concerns has led to the recent booming in research Shaanxi Yulin 1 million ton per year ICTL project is under construc-
and project activities in coal to liquid fuels (CTL) and coal to syn- tion, targeting to be commissioned in 2015. Yankuang energy
thetic natural gas (SNG). A summary of government approved carried 4500 t/a pilot scale test in 2004. More projects are pro-
CTL/SNG projects are listed in Table 2. For detailed history and posed at the feasibility stage in remote provinces such as Xinjiang
research progresses in CTL technology, please refer to reviews by and Inner Mongolia, with technology mainly from Synfuels China.
Maitlis and de Clerk [6], Liu [27], Tang [28] and Yang [29]. Here, According to the latest information, the total ICTL capacity will
an updated summary on the technology development and the reach 10–16 million ton/a in 2018.
engineering experience learned from these projects will be given
for further enhancing energy efficiency and economics from whole
3.2. Syngas conversion technologies
plant integration and optimization.
In terms of project experience, Shenhua Energy is the only
Syngas produced in the coal gasification stage can be converted
entity conducting research and commercialization of direct coal
to different hydrocarbon products:
liquefaction (DCTL) technology. A pilot plant of 1800 ton per year
To methane via methanation reaction
was built in Shanghai to collect process design package data in
2003. Afterwards, the first government approved Shenhua DCTL CO þ 3H2 ¼ CH4 þ H2 O DH ¼ 206 kJ ð1Þ
1.08 million ton/year demonstration project started construction
work in April, 2005, which was commissioned in December 30, To widely distributed hydrocarbons from C1 to C100+ via
2008. After more than three years hard work and steady improve- Fischer–Tropsch synthesis
ment in the process, the plant was reported to be running
CO þ 2H2 ¼ —CH2 — ðhydrocarbonsÞ þ H2 O DH ¼ 160 kJ ð2Þ
smoothly. However, no operation process data and further expan-
sion plan was reported elsewhere, especially in the open literature The above synthesis reactions are the bases of the processes for
[28,30]. the coal to clean fuels via gasification.

Table 2
A summary of major CTL/SNG research and development projects in China.

CTL/SNG project Capacity Commission timing Location Gasifier licensor Synthesis technology licensor
ICC slurry bed reactor pilot test 750–1000 t/a 2000–2002 Taiyuan ICC MFT
Yankuang industrial test plant 4500 t/a 2003–2004 Lunan ECUST-OMB Yankuang Fe-LTFT
Yitai ICTL Demonstration 160 kt/a 2009–2011 Dalu Texaco Synfuels China MTFT
Luan ICTL Demonstration 160 kt/a 2009 Tunliu Lurgi Synfuels China MTFT
Shenhua ICTL Demonstration 180 kt/a 2009–2010 Majiata Shell Synfuels China MTFT
Shenhua-Ningmei ICTL 4 Mt/a 2016 Yinchuan, Ningxia Siemens-GSP Synfuels China MTFT
Shanxi Luan High Sulphur Coal Co-production 1 Mt/a 2015 Changzhi Lurgi Synfuels China MTFT
Yankuang Shaanxi Yulin ICTL 1 Mt/a 2015 Yulin ECUST Yankuang ICTL
Yitai Xinjiang ICTL 2 Mt/a Xinjiang Synfuels China MTFT
Yitai Yili ICTL 1 Mt/a Yili Synfuels China MTFT
Datang International Power Keqi SNG 4 bn N m3/a 2012 Hexigten Lurgi Lurgi
Datang International Power Fuxin SNG 4 bn N m3/a Fuxin, Liaoning Province Lurgi
Huineng Coal Power Erdos SNG 1.6 bn N m3/a Erdos, Inner Mongolia
Qinghua Yili SNG 1.4 bn N m3/a Ili, Xinjiang Haldor Topsoe TREMP™
Sinopec Zhundong SNG Demonstration 30 bn N m3/a Zhundong, Xinjiang
128 J. Xu et al. / Fuel 152 (2015) 122–130

SNG cooler

Synthesis
water Reacted gas
SNG dryer

Diluted syngas
BFW
Reacted gas

Heat exchanger

Reactor I Reactor II
Fresh syngas
600-700 oC 500 oC SNG product

Reactor III
350 oC

MP steam

Recycling gas
BFW MP steam Raw SNG
BFW
LP steam

BFW

Fig. 6. An optional flow sheet for the methanation process.

As shown in Fig. 5, the syngas production complex for SNG pro- of an efficient Fischer–Tropsch synthesis loop is much more com-
cess is identical to that of the CTL. However, for SNG the preferred plicated than SNG processes due to the Fischer–Tropsch catalysts
gasification technology is Lurgi-type process, mainly for its high and the reactor unit are of much more complex in operation than
methane generation in gasifiers. The crude syngas can contain up those for methanation. Fig. 7 shows a typical F–T loop for the MTFT
to 16–18% methane which significantly reduces the methanation process developed by Synfuels China.
unit load downstream. Past experiences has shown that the new generation of high
For synthetic natural gas processes, the reaction (1) is typically temperature (270–290 °C) slurry phase FTS catalyst and process
conducted in fixed bed reactors with supported Ni catalysts at (or internationally referred to as MTFT process) can greatly
350–700 °C and 15–30 bar. The reaction process is highly exother- increase the hydrocarbon productivity. In contrast to the conven-
mic and an integrated process needs to manage the temperature tional low temperature slurry bed process, MTFT process boosts
control for the synthesis reactors and the efficient reaction heat the hydrocarbon productivity from 0.25–0.3 to 0.8–1.2 g C3+/
recovery. Fig. 6 shows an optional flow sheet for the methanation g cat/h, while decreasing the methane selectivity from 5–10 wt%
process with reaction and heat recovery management. to 2.5–4 wt%. Moreover, the operating temperature of the MTFT
The major methanation processes currently introduced into process is increased to approximately 275 °C by using the specially
China are mainly from Haldor Topsoe (TREMP), Davy (CRG) and designed iron-based catalyst. The major advantages of Synfuels
Lurgi technologies. Application of these SNG technologies have China’s MTFT over conventional low temperature slurry processes
shown that methanation processes are rather stable for operation are: (i) lower (about 1/3) solid catalyst charge in the slurry bed
and care must be taken for the productivity margins for the cata- reactor due to the ultra-active F–T synthesis catalyst used, (ii) effi-
lytic process in order to keep the sufficient conversion level of syn- cient recovery of F–T synthesis reaction heat from the slurry bed
gas and to achieve the high methane content (higher than 95%) reactor as steam up to 30 bars, resulting in an improved energy
required for pipeline gas in China, namely the catalyst charge efficiency, (iv) production of high quality F–T synthesis syncrudes
should be sufficient for long term operation with required syngas with very low oxygenates, especially acids (about 1/3), and (v) easy
conversion capability. retrofit to both CTL and GTL processes.
For producing liquid hydrocarbons, the Fischer–Tropsch reac- The experiences gained from the early demonstration projects
tion in reaction (2) plays major role in syngas conversion. Practi- for CTL (5000 b/d) and SNG (1300 Mm3/a) have shown that CTL
cally, this reaction is typically catalyzed by either cobalt or iron projects are economically competitive with the current high oil
based catalysts at 190–360 °C and 15–50 bars, leading to low tem- price, while SNG projects are economically not attractive, espe-
perature (190–240 °C, cobalt and iron as catalysts), medium tem- cially for the projects with all the methane produced from syngas
perature (260–300 °C, iron as catalysts), and high temperature methanation in the case of using other gasification technologies
(320–360 °C, iron as catalysts) Fischer–Tropsch synthesis pro- than the Lurgi-type moving bed due mainly to the natural gas
cesses named as LTFT, MTFT and HTFT processes. Currently, LTFT prices is much lower compared to motor fuels in the China market.
has mainly been applied with cobalt catalyst by Shell and SASOL In other words, for SNG projects, it is true that the Lurgi-type gas-
in gas to liquids projects, MTFT with iron catalysts by Synfules ification has to be chosen for high methane production through
China in Coal to liquids projects, and HTFT with iron catalysts by pyrolysis of coal in the gasifier rather than synthesis from CO
SASOL for coal to liquids projects [6]. and H2. Comparing the liquid and methane production from
Obviously, Fischer–Tropsch synthesis reaction is also very synthesis is useful to understand the economical status of the
exothermic although less than methanation, and the integration SNG and CTL projects as shown in the chemical balances of the
J. Xu et al. / Fuel 152 (2015) 122–130 129

Heat exchanger
Air cooler

Separator
MP Separator
steam
Heavy Light F-T
condensates condensates water

Recycling gas Recycling


Wax compressor
Filtraon unit
back flushing gas

CO2
BFW
De-CO 2 gas

Benfield
Adsorbor
MTFT slurry reactor

Fresh syngas

Fig. 7. A typical F–T loop for the MTFT process developed by Synfuels China.

Table 3 technologies, advanced synthesis technologies, and improved


Typical balance data from 1000 N m3 syngas CO + H2 to fuels. waste management technologies.
Processes Syngas Products Notes Large scale gasification technologies are mainly focused on the
conversion (%) yields (kg) dry feed entrained flow gasification. The latest effort is to demon-
SNG 98 175 CH4 as product
strate a 4000 t/d dry feed entrained flow gasifier with partial
CTL 96 188 LPG + liquid selectivity 94% quenching by water and steam (to 900–950 °C), where the water
gas shift is significant, leading to an increase of H2/CO ratio from
0.3 to about 0.8. This gasification technology may significantly
two processes. The typical performance parameters are summa- reduce the cost of gasification and the downstream water–gas shift
rized in Table 3. in a CTX project. Another major improvement for gasification is to
The current cost from CTX plant of the above products in China demonstrate the polluted water recycling within the gasification
are 2800 RMB/ton for pipe line natural gas (methane basis) and process for both moving bed gasification as well as the new partial
7000 RMB for the average CTL liquid products. It is obvious that quench gasification. This type of effort may significantly reduce the
the SNG from syngas is hardly economical competitive while CTL waste water treatment load and save the fresh water feed.
can be very competitive although the capital cost is 1.5 times to The development of new syngas conversion technologies are
an equivalent SNG projects with the same thermal capacity. How- also emphasized especially for highly efficient conversion catalyst.
ever, if the methane can be produced in the gasification stage like The next generation F–T catalyst is in the stage of pilot plant devel-
in Lurgi-type moving bed gasification, the directly produced meth- opment, aiming at much higher productivity to the level of
ane can be very economically competitive due to higher efficiency 2000 ton oil/t catalyst (currently 1000 t/t catalyst). The gasoline
and lower conversion cost. process via MTFT processes is under demonstration stage, aiming
The recent effort from Synfuels China is to combine the SNG and at the supper clean gasoline supply for large cities.
FTS processes together by using moving bed gasification, in which The integration of the CTL/SNG processes has arisen many new
the methane from gasification and in Fischer–Tropsch tail gas is requirements for utilities in terms of the stringent regulations.
separated as natural gas products (SNG or LNG) and the syngas Water saving investment with closed cycling has been used in sev-
after separation of methane is fed into Fischer–Tropsch loop to pro- eral CTL projects, significantly reducing the water consumption
duce liquids. The combined scheme shows high energy efficiency from the standard of 8 t/t oil to 3–4 t/t oil. Several projects have
up to 60% comparing to the single CTL plant of 45%, and the undergone the CO2 emission control by large investment in plant-
economics becomes much better than single CTL projects, showing ing trees in the rural land around the project site.
strong growing potentials with the frame of the clean coal
development policy in the country. 5. Conclusions

4. Perspectives (1) China has to convert its abundant coal to clean fuels for envi-
ronmental and economic reasons. Numerous large CTL/SNG
The increasing demand for clean energy products is one of the projects are under construction with processes integrating
major driving forces for the development of coal conversion a variety of advanced international as well as domestic gas-
processes on the basis of the gasification in China. The recent CTL ification technologies, aiming to improve the energy effi-
and SNG projects approved by the central government have experi- ciency and process economics.
enced hardest stages for scaling up clean coal processes. These pro- (2) From data obtained from CTL (5000 b/d) and SNG
cesses have provided unique platforms for demonstrating new (1300 Mm3/a) projects, it can be concluded that CTL projects
technologies covering improved or newly developed gasification are economically competitive with the current oil price,
130 J. Xu et al. / Fuel 152 (2015) 122–130

while projects for SNG produced from syngas methanation [9] Higman C, Tam S. Advances in coal gasification, hydrogenation, and gas treating
for the production of chemicals and fuels. Chem Rev 2013;114:1673–708.
are not, especially under the current relatively low natural
[10] Bell DA, Towler BF, Fan M. Coal gasification and its applications. Oxford: William
gas price in China. Therefore, one option is to combine the Andrew; 2011.
SNG and FTS processes together by using moving bed gasifi- [11] Tang H. Coal gasification technology development trend. Chem Eng Des
cation to improve energy efficiency and economics. Commun 2013;39:1–11. in Chinese.
[12] Gong J. Shell coal gasification technology and its engineering applications.
(3) The integrated SNG/FTS process scheme recently developed Chem Fertil Des 2007;45:8–18. in Chinese.
by Synfuels China can achieve an energy efficiency up to [13] Zheng Z. Features of shell coal gasification technology. Coal Chem Ind
60% and great economics potentials in clean coal conversion. 2003;31:7–11. in Chinese.
[14] Zhao R, Li L, Zhang F, Hu Y. GSP gasification technology of the future energy
company. Coal Chem Ind 2005;33:19–22. in Chinese.
[15] Huang W, Ma Y. Process analysis on syngas production with GSP coal
gasification technology. Mod Chem Ind 2013;33:93–6. in Chinese.
Acknowledgments [16] Tang H. GSP process technology. Medium-sized Nitrogen Fertil Prog
2005:14–8.
We thank the National Natural Science Foundation of China [17] Ma L, Jiao H, Ren S. Application analysis on Texaco and GSP coal gasification
technologies adopted by the Shenhua Ningxia coal group. Coal Chem Ind
(20703054), the National Basic Research program of China (973 2013;41:51–4. in Chinese.
Program, 2011CB201401) and the National High Technology [18] Cai D, Wang L, Xu J, Wang Z. Present status and analysis on coal gasification
Research and Development Program of China (863 program, technology for SNG. Clean Coal Technol 2011;17:44–7. in Chinese.
[19] Dai Z, Gong X, Guo X, Liu H, Wang F, Yu Z. Pilot-trial and modeling of a new
2011AA05A205). This work is also supported by Synfuels China type of pressurized entrained-flow pulverized coal gasification technology.
Co., Ltd. Fuel 2008;87:2304–13.
[20] Guo X, Dai Z, Gong X, Chen X, Liu H, Wang F, et al. Performance of an
entrained-flow gasification technology of pulverized coal in pilot-scale plant.
References Fuel Process Technol 2007;88:451–9.
[21] Li Y. Analysis of entrained-bed coal gasification technology. Technol Dev Chem
[1] Vertes AA, Qureshi N, Blaschek HP, Yukawa H. Biomass to biofuels: strategies Ind 2013;42:26–8. in Chinese.
for global industries. Chichester: John Wiley & Sons, Ltd.; 2010. [22] van Dyk JC, Keyser MJ, Coertzen M. Syngas production form South African coal
[2] Xie K, Sun Q, editors. Coal indirect liquefaction. Beijing: Chemical Industry sources using Sasol-Lurgi gasifiers. Int J Coal Geol 2006;65:243–53.
Press; 2012. [23] Guo X, Tong W. Advantages of HT-L gasification technology in industry. Chem
[3] Zhao L, Gallagher KS. Research, development, demonstration, and early Eng Des Commun 2012;38:64–9. in Chinese.
deployment policies for advanced-coal technology in China. Energy Policy [24] He Y, editor. Handbook of modern coal chemical engineering
2007;35:6467–77. technology. Beijing: Chemical Industry Press; 2003.
[4] Jin E, Zhang Y, He L, Gordon Harris H, Teng B, Fan M. Indirect coal to liquid [25] Lin H, Li K, Zhao L. Status and development of coal to SNG. Shanghai Chem Ind
technologies. Appl Catal A: Gen 2014;476:158–74. 2010;35:25–8. in Chinese.
[5] Ding Y, Han W, Chai Q, Yang S, Shen W. Coal-based synthetic gas (SNG): a [26] Guo D. Study on China coal SNG development status. Guangzhou Chem Ind
solution to China’s energy security and CO2 reduction. Energy Policy 2013;41:26–7.
2013;55:445–53. [27] Liu Z, Shi S, Li Y-w. Coal liquefaction technologies-development in China and
[6] Maitlis PM, de Klerk A, editors. Greener Fischer–Tropsch processes for fuels challenges in chemical reaction engineering. Chem Eng Sci 2010;65:12–7.
and feedstocks. Weinheim, Germany: Wiley-VCH Verlag GmbH & Co. KGaA; [28] Tang H. Six turns of enthusiasm waves in coal chemical industry development.
2013. Chem Eng Des Commun 2011;37:1–9. in Chinese.
[7] Grabner M, Meyer B. Performance and exergy analysis of the current [29] Yang C. Developing modern coal chemical industry to reduce dependence on
developments in coal gasification technology. Fuel 2014;116:910–20. foreign petroleum. Sino-Glob Energy 2013;18:1–5. in Chinese.
[8] Higman C, van der Burgt M. Gasification. Oxford: Gulf Professional Publishing; [30] Zhang H. Shenhua Group’s practice and endeavors in coal liquefaction and
2008. chemical industry fields. China Petrol Chem Stand Qual 2012;33:51.

View publication stats

You might also like