Upgrading of Low Rank Coal as Coal Water Slurry and Its

Utilization

Ryo Moriyama, Shohei Takeda, and Yukuo Katayama

In this paper, a new brown coal utilization process, combining the techniques of coal/water
slurry (CWS) production and CWS in-line vaporization, was proposed. In the process, brown
coal was converted to CWS with high-pressure kneader under mechanical shear stress and
moderate heating. Water in obtained CWS was vaporized with special designed pre-heater,
termed in-line vaporizer, processing about 2.0 t/day (dry coal base). Indonesian brown coal
containing 22% water and Australian brown coal containing 59% water were successfully
converted to the CWS. CWS of Australian brown coal was pre-heated with the in-line
vaporizer. The CWS was converted to coal/steam mixture and directly burned in a combustion
furnace.
Keywords

Brown coal; Low rank coal; Coal water slurry; CWS; CWM

INTRODUCTION
It is known that Australian brown coals, such as Loy Yang and Yallourn, have very high
moisture content from 60 to 70%. When these brown coals are utilized for coal combustion or
a coal gasification process, the thermal efficiency of the process significantly decreases as a
result of the water evaporation. More CO2 is emitted and lager volume of a combustion
chamber is required based on the heating value of the brown coals. The brown coals must be
used at a power plant adjacent to an open cut mine since the high moisture raises
calorie-based cost of transport. Furthermore, the spontaneous combustibility of the brown
coals also restricts their transport. Inexpensive and safe drying technologies are required for
utilization of the brown coals.
Several coal-dewatering technologies have been developed for effective utilization of the
brown coals [1-8]. Hydrothermal Dewatering (HTD) process is one of the coal-dewatering
technologies [1-6]. In the process, brown coal containing 62% moisture is mixed with water
and is converted to coal/water slurry (CWS) of 75% moisture. The CWS is heated to around
570 K under a sufficient pressure to prevent evaporation of water. After the cooling and

Address correspondence to Ryo Moriyama, The Institute of Applied Energy, Shinbashi SY

BLDG. 14-2, Nishishinbashi 1-chome, Minato-ku, Tokyo, 105-0003, Japan. E-mail:
moriyama@iae.or.jp

Upgrading of Low Rank Coal

depressurizing processes, excess liquid water is separated from the CWS. The product is
pumpable CWS containing 50% moisture and can be fired in a conventional boiler. During
the dewatering process, the latent heat of water evaporation is not expended since the water is
removed as a liquid. Water-soluble inorganic compounds are also removed with the water.
Mechanical Thermal Expression (MTE) process is being developed [1,7,8]. In the process,
water is expressed from the brown coal by means of mechanical pressure (4 to 6 MPa) and
moderate heating (450 to 475 K) with comparatively low energy consumption. The
mechanical energy required to remove the water from the brown coal is less than 1% of the
thermal energy required for an equivalent drying by evaporation. However, wastewater
treatment raises processing costs for HTD and MTE processes. Furthermore, products
obtained with HTD and MTE processes still contain 50% and below 25% moisture,
respectively.
KEM Corporation developed a new process, which converts the brown coals to CWS. In
this process, the brown coal is subjected to moderate heating (< 525 K) and high shear stress.
By removing a part of water during the process, the heating value of the CWS will be
equivalent to that of conventional CWS from bituminous coal.
From an energy point of view, coal gasification or combustion process using CWS as feed
has a disadvantage in the heat required for the processing. Considerable amount of coal burns
in order to compensate the latent heat of water evaporation, and this results in the generation
of more CO2. For many years, increasing the thermal efficiency of the coal gasification or
combustion with the pre-heating of CWS has been challenged.
Miyatani [9] proposed heat recovery system of a coal gasifier. Heat recovered from the
system can be applied to the heat for evaporation of water in CWS. Roffe et al. [10] tried to
evaporate water in CWS with pre-heating and found line plugging in a pre-heater using CWS
of 40-60 wt.%-coal as feed. Usui at al. [11] also found that CWS of 65 wt.% coal caused line
plugging in a pre-heater at a temperature range of 423 to 433 K due to increase in the
viscosity of the CWS. They concluded that the combined effect of the swelling of coal and
the change of surface condition of coal was mainly responsible for the increase in the
viscosity. Novack et al. [12] reported CWS vaporizer development with useful experimental
observations and conclusions. However, there is no commercialized process of the CWS
vaporizer, and direct injection of CWS without vaporization is commonly used.
The authors designed the CWS pre-heater, termed CWS in-line vaporizer, which
accommodates CWS pressure and flow change as well as phase change in the same transfer
line leading the feed from a CWS tank to a gasifier [13]. In the present paper, the authors
propose a brown coal utilization process combining the CWS production process licensed by
KEM Corporation and the CWS in-line vaporizer.
EXPERIMENTAL

Upgrading of Low Rank Coal

Sample
Indonesian (ID) and Australian (AU) brown coals were used as samples, whose properties
are shown in Table 1. Commonly, commercialized CWS contains moisture over 30%. This
content is greater than the moisture of ID coal while less than that of AU coal. Considering
CWS produced from the brown coals, a known amount of water should be added into ID coal
and be removed from AU coal. Diameter of AU coal was greater than that of ID coal. Mass
mean diameter of AU coal was 0.46 mm.
CWS production process
Three kneaders of different performance and one autoclave were used for CWS production
experiment. Their names and performances were listed in Table 2.
The experimental kneader processing 2.5 kg was used for CWS production. The kneader
was equipped with a jacket filled with hot oil around the pressure vessel, of which the design
pressure was 1.0 MPa-G. The kneader had two sigma-shaped blades that gave mechanical
shear stress of < 0.2 MPa to the sample.
2.5 kg of the sample was heated in the closed vessel with kneading. During the heating, the
pressure in the vessel went up due to the increase in the vapor pressure of water. When the
temperature of the sample reached 457 K, the pressure reached 0.98 MPa-G. After
maintaining the pressure for 1 or 5 hours, the vessel was cooled down to an ambient
temperature, and product slurry was collected. The obtained slurries from ID coal and AU
coal were termed ID slurry and AU slurry, respectively.
In order to investigate the effect of shear stress on the CWS production, AU coal was
processed with the autoclave and the high-shear kneader. The autoclave equipped with a
stirrer, which gave little shear stress to the sample. AU coal introduced into the autoclave was
heated to 457 K, and the temperature was maintained for 1 h. Sample collected after the
cooling process was termed AU-Test. The high-shear kneader had a specific shaft [14] with a
special designed stir wing screws and blades to give shear stress of < 1.0 MPa to the sample.
Photograph of high-shear kneader is shown in Figure 1.
The large-scale kneader with the capacity of about 200 kg was used to produce a large
amount of AU slurry for experiment using CWS in-line vaporizer. The kneader also had a
specific shaft and gave shear stress of < 1.0 MPa to the sample without an external heater and
a pressurization system. 180 kg of AU coal was introduced into the kneader and was kneaded
for 4.5 h.
Characterization of original coals and obtained slurries
Original coals and obtained slurries were subjected to several instrumental analyses. The

Upgrading of Low Rank Coal

viscosities of the obtained slurries were measured with a rotary viscometer (shear rate:
6.71008 s-1) at room temperature. Distributions of types of water for AU coal, AU slurry and
AU-Test were measured with a 1H-NMR spectrometer (JEOL: Mu-25) on the basis of
freezing properties of water [15]. About 1 g of sample was inserted to 8 mm I.D. NMR
sample tube. One pulse method was used to obtain the entire free induction decays (FID). The
FID was measured at temperatures of 296, 268, and 223 K. The signal at each temperature
was recorded under temperature equilibration.
Pore size distribution of dried AU coal and dried AU slurry were measured by argon gas
adsorption and desorption at 78 K. AU coal and AU slurry were dried at 333 K under the
vacuum condition for 1 day and subjected to the measurement.
CWS in-line vaporizer
The CWS in-line vaporizer processing about 2.0 t/day (dry coal base) [13] with a
combustion furnace is schematically shown in Figure 2. This apparatus was mainly composed
of a CWS tank, a high-pressure pump and three heaters. Temperature of heating oil and flow
rate of slurry were 570585 K and 100140 L/h, respectively. AU slurry was heated through a
feed tube soaked in heating oil in the three heaters, termed 1st, 2nd or 3rd heater. Diameters
and lengths of the feed tube were determined in such a manner to steadily heat up the feed
slurry and to completely vaporize the water in the slurry. The coal/steam mixture was directly
introduced into a combustion furnace and burned. Prior to the CWS feed, the temperature in
the furnace was maintained with a fuel burner. An exhaust line was prepared for start-up with
vaporization of water, monitoring exhaust of coal/steam mixture, and sampling of dried coal
particles.
The inner diameters of the feed tubes were 6 mm at the 1st heater, 2 to 8 mm at the 2nd
heater, and 10 mm at the 3rd heater. At the 1st heater, CWS was preheated to the temperature
about 10 K below that of the heating oil under high pressure in order to maintain slurry phase
without vaporization. The length of the feed tube in the 1st heater was about 70 m, that is, the
residence time of the CWS in the heater was calculated to be 80 sec. At the 2nd heater, a part
of water in CWM evaporated. The inner diameters of tubes discreetly increased so as to
maintain the velocity in a range to cause atomizing and preventing the tubes from erosion.
Finally, the rest of water was evaporated and was super heated in the 3rd heater. Total length
of tubes in the 2nd and the 3rd heaters is 47.9 m, that is, the residence time of the CWS in the
heaters was calculated to be less than 10 sec.
The temperatures and the pressures at the outlet of each heater were measured in order to
estimate the state of the fluid and analyze them from fluid dynamics point of view.
RESULTS

Upgrading of Low Rank Coal

Production of the slurries from brown coals

ID slurry was produced with the experimental kneader. 1.1 kg of water was added to 2.0
kg of ID coal and then total moisture of the mixture became about 50%. Figure 3a shows
photographs of the CWS production for ID coal at the start and the end of the operation. The
pumpable ID slurry with low viscosity was obtained by this operation.
AU coal was also kneaded with the experimental kneader. In this case, no water was added
since AU coal had high moisture content. The slurry was obtained as shown in Figure 3b.
In both cases, any surfactant was not added. Therefore, stability of the slurry was observed
by a precipitation test. The slurry was left at rest in a vessel. Precipitation was not found 2 or
more days after the experiment for both slurries. This characteristic might be attributed to the
hydrophilic property of the brown coals and/or the effect of organic acid dissolved in the
liquid phase.
The AU slurry was also produced with the large-scale kneader. About 180 kg of sample
was introduced into the kneader and was kneaded. Despite low temperature and atmospheric
pressure, viscous AU slurry was obtained by this operation.
Properties of the slurries obtained from brown coals
The viscosities of obtained slurries were measured with a rotary viscometer at room
temperature. AU-Test obtained with the autoclave was too hard to measure the viscosity. It
seemed to be a kind of gel. Plots of flow curves for slurries are shown in Figure 4. In the
figure, shear stress linearly increases with increasing shear rate in a range of small shear rate
while the slope lowers with increasing shear rate. This behavior is typical characteristic of the
pseudo-plastic fluid, which is one of the non-Newtonian fluids. Apparent viscosity of AU
slurry was relatively higher than that of ID slurry. This difference might be caused by the
difference in the particle size of coal particles in the slurry.
Apparent viscosity of AU slurry processed with experimental kneader for 1 h is an order of
magnitude higher than that for 5 h. This result implies that processing time is one of the key
factors for producing slurry with low viscosity. Flow curve of AU slurry processed with
high-shear kneader for 1 h is similar to that processed with experimental kneader for 5 h. This
result suggests that increase of shear stress shorten experimental period. Furthermore, effect
of particle size was investigated. Coarse particles with size larger than 0.84 mm were
removed from AU slurry. Apparent viscosity of the slurry was considerably decreased by
means of removal of coarse particles.
Distributions of types of water for AU coal and AU slurry were measured using 1H-NMR
spectroscope on the basis of freezing properties of water. 1H-NMR relaxation measurement
was performed at 296, 268, and 223 K. In Figure 5, FID intensities for AU coal at 296, 268,
and 223 K are plotted versus decay times. FID intensity at decay time zero corresponds to the

Upgrading of Low Rank Coal

total amount of 1H in the sample while slope of the intensity corresponds to molecular
mobility of 1H. Slope of FID intensity seems to be composed of two or more components. The
slowly decaying component appeared after 30 s for each temperature is described by an
exponential function and it corresponds to 1H in water. If a part of water freezes, the intensity
of this component decreases. Therefore, the authors defined FID intensity at decay time 40 s
to be relative amount of water in the sample. From above analysis, water was classified on the
basis of freezing properties of water [15].
Figure 6 shows the distributions for AU coal, AU slurry and AU-Test. AU slurry and
AU-Test were obtained with experimental kneader operated for 1 h and with autoclave,
respectively. Free water is identical to bulk water that freezes at around 273 K, bound water is
defined as pore condensed water that freezes at a temperature range of 273 to 223 K, and
non-freezable water does not freeze even at 223 K. The comparison demonstrates that the
CWS production process decreases amount of non-freezable water and increases amount of
free water. Fluidity of AU coal increases with increasing free water content. From the above
results, both heat and shear stress are found to be important factors for producing pumpable
slurry with low viscosity.
Figure 7 shows pore size distributions for dried AU coal and dried AU slurry. The pore
volume with 5-20 nm of pore radii was decreased and that with smaller than 5 nm was
increased by the CWS production process. Destruction of coal pores might cause restriction of
removed water from recovery.
Preheating and combustion of CWS obtained from AU coal
The CWS in-line vaporizer shown in Figure 2 was used for pre-heating of AU slurry. The
slurry produced by the large-scale kneader contained about 10% of particles with diameter of
>0.5 mm. Water was added and large coal particles were removed from the slurry by
precipitation before the experiment since the minimum inner diameter of the feed tube was 2
mm. The water content of the slurry was about 75% and apparent viscosity of the slurry was
less than 1000 mPas.
The AU slurry was pre-heated and exhausted into atmosphere for several minutes in order
to monitor the condition of the exhaust and to measure the water content of exhausted coal
particles. The temperature of heating oil and the flow rate of sample were 573 K and 120 L/h,
respectively. Figure 8 shows the exhaust of steam and steam/coal mixture. The moisture in
obtained coal particles was 5-6 wt.%. Water in the slurry was completely evaporated with this
vaporizer.
The AU slurry was pre-heated and directly introduced into the combustion furnace. At the
experiment, the temperature of heating oil and the flow rate of sample were 583 K and 120
L/h, respectively. The log data at the experiment is shown in Figure 9. The AU slurry was
steadily fed into the combustion furnace for 90 min without plugging of the feed tube. The

Upgrading of Low Rank Coal

experiment was terminated because 200 L of sample in the CWS tank was completely fed.
From read out the log data, followings were found:
1. Fluid was in a solid/liquid (slurry) phase at the outlet of the 1st heater since the pressure
and the temperature at the outlet of the heater were 8.5 MPa and 558 K, respectively.
(vapor pressure of water is 8.5 MPa, at 573 K)
2. Fluid was in a solid/liquid/gas phase at the outlet of the 2nd heater since the temperature
at the outlet of the heater was 473 K and pressure of the outlet was close to the vapor
pressure of water.
3. Fluid was in a solid/gas phase at the outlet of the 3rd heater since the pressure and the
temperature at the outlet of the heater were 0.8 MPa and > 473 K, respectively. (vapor
pressure of water is 0.8 MPa, at 449 K)
The temperature in the combustion furnace increased from 803 to 873 K and the
consumption of the fuel oil decreased with feeding the AU slurry. This means that the AU
slurry steadily burned in the furnace.
SUMMARY
From the above results, AU coal was converted to slurry using their own moisture and
without any surfactant. Obtained slurry was pumpable. Water in the slurry was completely
evaporated with the in-line vaporizer, and coal in the slurry burned in the combustion furnace
during 1.5 h of experimental period.
ACKNOWLEDGMENTS
The research and development of CWS vaporizer are a part of technological project,
termed Production of Methanol from Coal, Natural Gas and Carbon Dioxide using Solar
Energy, funded by Ministry of Economy, Trade and Industry (METI) in Japan. Production
and test of preheating of CWS were carried out in collaboration with Hokkaido Center of
International Institute of Advanced Industrial Science & Technology in Japan. The
experiment of large-scale kneader was performed with Japan Systematization Laboratory and
KEM Corporation. Preheating and combustion of CWS were carried out with the cooperation
of Tokai-Pulp & Paper Co., Ltd.
REFERENCES
1. D. J. Allardice and B. C. Young, Utilisation of low rank coals, 18th Annual International
Pittsburgh Coal Conference (2001).
2. G. Favas and W. R. Jackson, Hydrothermal dewatering of lower rank coals. 1. Effects of
process, Fuel, vol. 82, pp. 5357 (2003).

Upgrading of Low Rank Coal

3.

4.

5.

6.

7.
8.
9.
10.
11.
12.
13.

14.
15.

G. Favas and W. R. Jackson, Hydrothermal dewatering of lower rank coals. 2. Effects of

coal characteristics for a range of Australian and international coals, Fuel, vol. 82, pp.
5969 (2003).
G. Favas, W. R. Jackson and M. Marshall, Hydrothermal dewatering of lower rank coals.
3. High-concentration slurries from hydrothermally treated lower rank coals, Fuel, vol.
82, pp. 7179 (2003).
L. Racovails L, M. D. Hobday and S. Hodges, Effect of processing conditions on
organics in wastewater from hydrothermal dewatering of low-rank coal, Fuel, vol. 81, pp.
13691378 (2002).
D. J. Allardice, L. M. Clemow, G. Favas, W. R. Jackson, M. Marshall and R. Sakurovs,
The characterization of different forms of water in low rank coals and some
hydrothermally dried products, Fuel, vol. 82, pp. 661667 (2003).
C. Bergins, C. Kinetics and mechanism during mechanical thermal dewatering of lignite,
Fuel, vol. 82, pp. 355364 (2003).
C. Bergins, Mechanical/thermal dewatering of lignite. Part 2: A rheological model for
consolidation and creep process, Fuel, vol. 83, pp. 267276 (2004).
K. Miyatani, Heat recovery technique on entrained gasifier, J. Fuel Soc. Japan, vol. 62,
pp. 874-881 (1983).
G. Roffe and G. Miller, Thermal preconditioning of coal/water mixtures for gas turbine
applications, ASME Paper, 85-GT (1985).
H. Usui, Y. Yamasaki and Y. Sano, Heat transfer of coal-water mixtures in a round tube
flow, J. Chem. Eng. Japan, vol. 20, pp. 6570 (1987).
M. Novack, G. Roffe and G. Miller, Combustion of coal/water mixtures with thermal
preconditioning, ASME Paper, 87-GT (1987).
R. Moriyama, K. Aiuchi, S. Takeda, S. Kitada, M. Onozaki and Y. Katayama, Preheating
feed of coal-water mixture in green fuel production, 12th International Conference on
Coal Science (2003).
T. Inoue, Japanese patent No. P2000-169274A, 2000.
K. Norinaga, Ji. Hayashi, N. Kudo and T. Chiba, Evaluation of effect of predrying on the
porous structure of water-swollen coal based on the freezing property of pore condensed
water, Energy Fuels, vol. 13, pp. 10581066 (1999).

TABLE 1

Properties of raw materials

Moist.

Particle size

(wt.%)*

(mm)

Ash

22.2

< 0.25

6.34

66.03

5.19

20.59

1.37

0.39

59.0

< 2.0

0.90

67.28

4.97

25.34

0.60

0.28

wt.% (dry basis)

Indonesian
(ID) Coal
Australian
(AU) Coal

* as received

TABLE 2

Performance of facilities

Sample amount

Pressure

Temperature

Shear Stress

(kg/batch)

(MPa-G)

(K)

(MPa)

Autoclave

0.33

10.0

570

Experimental kneader

2.5

1.0

460

< 0.2

Large-scale kneader

200

0.0

< 1.0

High-shear kneader

20

3.0

500

< 1.0

FIGURE 1. Photograph of high-shear kneader.

10
8

Dry Coal
+ Steam

CWS+
Steam

7
11

CWS

1.
2.
3.
4.
5.
6.

CWS tank
Pump
Water pump
High-pressure pump
1st heater
2nd heater

7.
8.
9.
10.
11.

3rd heater
Let down valve
Combustion furnace
Exhaust line
Oil heater

FIGURE 2. Schematic diagram of CWS in-line vaporizer.

(a) Indonesian (ID) coal

Start

End

(b) Australian (AU) coal

Start

End

FIGURE 3. Photographs of CWS production process.

(a) ID coal; (b) AU coal .

1200

1000

Shear stress [Pa]

800
Coal/Period/Apparatus
AU/1h/exp.
AU/5h/exp.
ID/5h/exp.
AU/1h/high
AU/1h/high/mod.

600

400

200

200

400

600

800

1000

-1

Shear rate [s ]

FIGURE 4. Flow curves for obtained slurries.

Intensity [A.U.]

296 K
268 K
223 K

0.1

50

100

150

200

Decay time [s]

FIGURE 5. Free induction decay (FID) curves for AU coal

obtained at 296, 268 and 223 K.

Free water
Bound water
Non-freezable water

AU slurry

AU-Test

AU coal

0.0

0.5

1.0

1.5

Water content [g-water/g-dry coal]

FIGURE 6. Distribution of types of water in AU coal

and its derivatives.

3.0
AU coal
AU slurry

2.0

-3

Pore volume [10 cm /g]

2.5

1.5

1.0

0.5

0.0
0.1

10

100

Pore radius [nm]

FIGURE 7. Pore size distributions for dried AU coal

and AU slurry

Steam exhaust

Steam/coal exhaust

FIGURE 8. Exhaust of steam/coal mixture.

600

Temperature [K]

550

500

450
Outlet of 1st
Outlet of 2nd
Outlet of 3rd

400
Picked up
Operation period

350
12

Pressure [MPa-G]

10

8
Outlet of 1st
Outlet of 2nd
Outlet of 3rd
Inlet of burner

20

40

60

80

100

120

25

30

35

40

Time [min]

FIGURE 9. Log data of in-line vaporizer during feeding

of AU slurry for 100 min.