ISIJ International, Vol. 54 (2014), No. 11, pp.

2454–2460

Effect of Woody Biomass Addition on Coke Properties

Yasuaki UEKI,1)* Yoko NUNOME,1) Ryo YOSHIIE,2) Ichiro NARUSE,1) Yuko NISHIBATA3) and
Sadayoshi AIZAWA4)

1) EcoTopia Science Institute, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Aichi, 464-8603 Japan. 2) Graduate School
of Engineering, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Aichi, 464-8603 Japan. 3) Research and Development
Center, Kansai Coke and Chemicals Co., Ltd., 2-30 Ohama-cho, Amagasaki Hyogo, 660-0095 Japan. 4) Process
Research Laboratories, Nippon Steel & Sumitomo Metal Corporation, 20-1 Shintomi Futtsu, Chiba, 293-8511 Japan.
(Received on March 24, 2014; accepted on July 8, 2014)

The price of caking coal, which is used in the production of metallurgical coke, has risen in recent years.
Also of concern is the amount of CO2 emitted from steel industries, comprising approximately 15% of
total CO2 emissions in Japan. Therefore, CO2 emissions from the ironmaking process should be reduced
to avoid global warming. In this work, fundamental research is conducted on the effect of adding woody
biomass to the properties of coke, with the aim of possibly using woody biomass, which is carbon neu-
tral, as a raw material in coke-making. Experimental results showed that the connectivity between coal
particles in the coke sample during carbonization and coke strength drastically decrease by adding woody
biomass to caking coal. However, the coke properties of the coke sample with added woody biomass
could be improved by removing the partly volatile matter of woody biomass before mixing with caking
coal, and as a result, the possibility of using woody biomass as a raw material for coke-making with prior
carbonization at temperatures of more than 500°C was found.

KEY WORDS: coke; coal; woody biomass; connectivity; coke strength.

research.8–15) Diez et al.11) found that eucalyptus sawdust

1. Introduction
In recent years, the price of caking coal used in the pro-
duction of metallurgical coke soars, and the price in 2012
was approximately twice that in 2005.1) It is expected that
the prices will continue to increase in future. In addition,
emissions of CO2 gas from the steel industry make up for
approximately 15% of total emissions in Japan.2) Especially,
CO2 emissions from the ironmaking process account for
about 70% of all those from the steel industry, because large
amounts of fossil fuels are used as both a heat source and a
reducing agent in the process.3) Therefore, in relation to the
need to ameliorate global warming, it is considered critical
to reduce CO2 emissions from the ironmaking process, and
to reduce coal consumption and find alternative sources.
From this perspective, the recycling of the waste plastics in
the coke-making process has been researched.4–6)
On the other hand, the use of woody biomass has also
attracted attention as an alternative energy resource because
it is carbon neutral. Woody chips, as byproducts of sawmills
and the construction industry, are currently being used as
fuel for power generation and so on. However, it is neces-
sary to consider the utilization of forest remaining wood
discarded from forest management processes such as tree
thinning, as this forest remaining wood producing approxi-
mately 8 million tons each year are hardly used.7) Therefore,
the utilization of woody biomass including high amounts of
oxygen in the coke-making process has been the subject of
* Corresponding author: E-mail: ueki@mech.nagoya-u.ac.jp
DOI: http://dx.doi.org/10.2355/isijinternational.54.2454
and its carbonization products obtained at 415°C (tars and
charcoal) inhibited the fluidity of coking coals to varying
degrees. MacPhee et al.12) mainly studied the influence of
charcoal particle size on the quality of the coke produced
using charcoal additions. Coke made with a fine charcoal
addition (–150 μ m) was found to be considerably weaker
than those made from a base blend, but an increase in the
particle size of charcoal had a dramatic improvement on the
quality of the coke produced. Additionally, the effect of bio-
mass addition on the thermoplastic properties of coal has
also been investigate,13–15) and it has been found that the flu-
idity of a coking blend is usually reduced by the addition of
biomass, and that fluidity increased with an increase in the
heating rate.
In this work, we conducted fundamental research on the
possibility of using woody biomass as a raw material for the
coke-making. Connectivity between coal particles in the
coke with added woody biomass was evaluated quantitative-
ly by observing the coke structure, and the strength was
measured using an I-type tumbler tester for a single particle
in order to investigate the effect of woody biomass addition
on coke properties. Furthermore, a method for improving
the influence of woody biomass addition on coke properties
was found.
2. Experiment
2.1. Experimental Samples
Caking coal (Goonyella coal: G), non-slightly-caking

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Table 1. Properties of coal and woody biomass.

Proximate analysis (wt%) Ultimate analysis (wt%)

1)
Sample a.r dry basis d.a.f. 2)

Moisture VM FC Ash C H N S O 3)
Goonyella (G) 1.4 24.1 67.3 8.6 87.40 5.20 1.90 0.60 4.90
White haven (W) 0.8 36.8 56.4 6.8 82.30 5.39 1.94 0.46 9.90
Woody biomass (B) 3.8 86.1 11.8 2.1 47.56 5.66 0.27 – 46.51
1) a.r: as received, 2) d.a.f.: dry ash free, 3) O: by diffrence

Table 2. Properties of woody biomass char.

Proximate analysis (wt%) Ultimate analysis (wt%)

Carbonization
Sample Temperature a.r 1) dry basis d.a.f. 2)
(°C)
Moisture VM FC Ash C H N O 3)
BC(300) 300 1.1 60.3 37.3 2.4 69.07 4.63 0.15 26.15
BC(400) 400 1.9 32.0 66.1 1.9 74.69 3.86 0.16 21.29
BC(500) 500 2.0 24.7 72.4 2.9 82.21 3.43 0.16 14.19
BC(1000) 1 000 2.2 18.3 77.2 4.5 74.54 2.61 0.12 22.72
1) a.r: as received, 2) d.a.f.: dry ash free, 3) O: by diffrence
BC: Woody biomass char

Table 4. Mixing ratio of coal and woody biomass char.

Fixed carbon basis (wt%) Sample weight basis (wt%)

BC BC BC BC BC BC BC BC
Sample G G
(300) (400) (500) (1000) (300) (400) (500) (1000)
G95–BC(300)5 95 5 – – – 91.3 8.7 – – –
G95–BC(400)5 95 – 5 – – 94.9 – 5.1 – –
G95–BC(500)5 95 – – 5 – 95.3 – – 4.7 –
G95–BC(1000)5 95 – – – 5 95.6 – – – 4.4
G: Goonyella, BC: Woody biomass char

coal (White haven coal: W) and woody biomass (sawdust of Table 3. Mixing ratio of coal and woody biomass.
Japanese cedar: B) were used in this study. Table 1 shows Fixed carbon basis (wt%) Sample weight basis (wt%)
the properties of samples of coal and woody biomass. In
addition, chars carbonized the sawdust of Japanese cedar at Sample G W B G W B
each temperatures (300, 400, 500 and 1 000°C) in N2 gas G100 100 – – 100.0 – –
atmosphere were also used as woody biomass char G90–W10 90 10 – 88.7 11.3 –
(BC(300), BC(400), BC(500) and BC(1000)). Table 2
G80–W20 80 20 – 77.7 22.3 –
shows the properties of those woody biomass char samples.
Coals had a particle diameter of –1 mm, and woody biomass G99.8–B0.2 99.8 – 0.2 99.0 – 1.0
and chars had a particle diameter of –150 μ m. G95–B5 95 – 5 76.9 – 23.1
G90–B10 90 – 10 61.2 – 38.8
2.2. Carbonization Method
G: Goonyella, W: White haven, B: Woody biomass
Caking coal (G) and non-slightly-caking coal (W), woody
biomass (B), or woody biomass char (BC(300), BC(400),
BC(500) and BC(1000)) were mixed as shown in Tables 3
and 4. Samples were prepared using the designated mixing
ratio based on the fixed carbon weight. The mixed sample
was put into a ceramic crucible (test tube type with 11 mm
inner diameter) so that the weight of fixed carbon in the
mixed sample equaled approximately 0.4 g. A stainless steel
rod (φ 10 mm × L90 mm) was then inserted into the ceramic
crucible to apply a pressure of about 6 kPa on the mixed
sample. The ceramic crucible was put in a stainless steel
sample holder as shown in Fig. 1. The sample holder was
heated to 1 000°C at a rate of 3°C/min in N2 gas atmosphere Fig. 1. Schematic diagram of sample holder.

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 ISIJ International, Vol. 54 (2014), No. 11
Fig. 2. Example of the macrostructure image binarized.
using a muffle furnace. The temperature was then retained
at 1 000°C for 60 min, and cooled to 200°C in the furnace.
The coke sample obtained (carbonized sample) was buried
in a resin, cut horizontally and then polished. Finally, a cross
section of the polished coke sample was observed using an
optical microscope.
2.3. Method of Evaluation Used to Analyze Connectiv-
ity between Coal Particles in Coke Sample
Connectivity between coal particles in the coke sample
was evaluated by analyzing a macrostructure image of the
cross section of a coke sample. Three macrostructure images
were observed, and approximately 25% of the cross-sectional
area of the coke sample was analyzed. There was hardly any
variation in the porosity obtained from the image analysis,
and the results of the image analysis were reliable. The coke
structure derived from coal was distinguished from the other
parts (the pore and coke structure derived from woody bio-
mass), and the macrostructure image was binarized using
image analysis software. Figure 2 shows an example of the
macrostructure image binarized. From this, the area and
number of coal particles connected within the coke structure
derived from coal were determined (the white area in Fig.
2(b)). In this way, the connectivity between coal particles in
the coke sample, how coal particles were connected during
carbonization, was quantitatively evaluated.
2.4. Coke Strength Measurement
In order to quantitatively evaluate the influence of wood
biomass addition on coke strength, the coke strength of sin-
gle particles was measured using the I-type tumbler tester16)
showed in Fig. 3. This tester is comprised of a stainless steel
tubular vessel with 40 mm inner diameter and a length of
350 mm length, a rotation speed-setting device, and a motor.
A single particle from a coke sample was used in the
strength measurement, and the procedure was repeated
twice. The rotation speed was set to 30 rpm. The stainless
steel tubular vessel was turned at the rotation speed of 30
rpm for 25 min. The sample in the tubular vessel was
extracted every five minutes, and samples with particle sizes
of more than 1 mm were weighed. After that, all sample par-
ticles were put in the tubular vessel and it was turned again.
The tumbler strength index was defined to indicate the coke
strength quantitatively, as described in Eq. (1).
© 2014 ISIJ
Fig. 3. Schematic diagram of the I-type tumbler tester.
W+1 mm
TI +1 mm = × 100 ....................... (1)
W0
where TI+1 mm is the tumbler strength index (%); and W+1 mm
and W0 are the weight of sample with a particle size more
than 1 mm (g) and the initial coke sample (g), respectively.
The standard deviation of the tumbler strength index was
3.04%.
3. Results and Discussion
3.1. Effect of Woody Biomass Addition on Connectivity
between Coal Particles in Coke Sample
Figure 4 shows macrostructure images of G100, G90–
W10 and G80–W20. The bright-gray part, dark-gray part,
and black part are the coke structure derived from coal, res-
in, and pore, respectively. When White haven coal (non-
slightly-caking coal) was added to Goonyella coal (caking
coal), it was possible to observe coal particles, such as those
of a raw coal, that did not soften and melt during carboniza-
tion. The number of these coal particles increased with an
increase in the mixing ratio of non-slightly-caking coal.
Figure 5 shows macrostructure images of G99.8–B0.2,
G95–B5 and G90–B10. The dark-gray part is resin and
woody biomass, and the other parts are the same as those in
Fig. 4. In the case of G95–B5 and G90–B10, the caking coal
particles exist as a single particle without connection to oth-
er particles; however the particles soften, melt, and swell
during carbonization. Moreover, with an increase in the
mixing ratio of woody biomass, there is an increase in the
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Fig. 4. Macrostructure images of G100, G90–W10 and G80–W20.

Fig. 5. Macrostructure images of G99.8–B0.2, G95–B5 and G90–B10.

distance between coal particles, as a substantial amount of
carbonaceous matter derived from woody biomass exists
between the coal particles. In the case of G99.8–B0.2, where
the mixing ratio of woody biomass is very small, the coke
structure that was similar to that of G100 in Fig. 4 was
observed.
The area fraction of coal particles obtained by image
analysis is shown in Fig. 6. The term “Others” in Fig. 6 indi-
cates the pore and the coke structure derived from woody
biomass. In comparison with G100, the area fraction of the
particle (lump) with an area less than 0.5 mm2 increased,
and that with an area greater than 0.5 mm2 decreased when
non-slightly-caking coal was added to caking coal. Accord-
ingly, the connectivity between coal particles in the coke
sample decreased with addition of non-slightly-caking coal
to caking coal. On the other hand, when woody biomass was

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 ISIJ International, Vol. 54 (2014), No. 11
Fig. 6. Effect of the addition of non-slightly-caking coal and
woody biomass on the area fraction of coal particles.
Fig. 7. Weight change curve of woody biomass heated at a rate of
3°C/min in N2 gas atmosphere.
added to caking coal (G95–B5 and G90–B10), there were no
particles with areas larger than 0.5 mm2, and the area frac-
tion of particles with areas less than 0.5 mm2 increased con-
siderably. This result suggests that connectivity between
coal particles in the coke sample drastically decreases when
woody biomass is added to caking coal.
Figure 7 shows the weight change curve of the woody
biomass, heated at a rate of 3°C/min in N2 gas atmosphere,
obtained using thermogravimetric analysis. Drastic weight
loss occurred at temperature between 250 and 350°C due to
the release of volatile matter from the woody biomass, and
it is supposed that the wood biomass shrinks with release of
volatile matter. In the case of woody biomass addition, a
large number of woody biomass particles exist between the
coal particles, so the density of woody biomass is much
smaller than that of coal. Therefore, voids are formed
between coal particles during carbonization because woody
biomass begins to release volatile matter and shrink at a
lower temperature (250–350°C) than a softening and melt-
ing temperature (410–490°C)17) of Goonyella coal (caking
coal). After that, when caking coal swells at a softening and
melting temperature, it cannot fill the void between coal par-
ticles. This is because there are many voids between the coal
particles. Even if the void between coal particles can be
filled, the swelling of Goonyella coal is in a state of free
expansion, and the consolidation effect becomes small.
Moreover, in the case of plastic addition to coal, the coal
caking property is inhibited by a stabilization of a radical
derived from plastic.5) In addition, heteroatoms like oxygen
© 2014 ISIJ
Fig. 8. Microstructure image of G95–B5.
have a deleterious effect on the thermoplastic properties of
coal.18) From these, volatile matter released from woody
biomass (including high amounts of oxygen) may inhibit the
thermoplastic properties of coal. That is why the adhesion
between coal particles, and between coal particle and woody
biomass particle, is insufficient, as shown in Fig. 8. Where
there is a small mixing ratio of woody biomass (G99.8–
B0.2), the area fraction distribution of G99.8–B0.2 is similar
to that of G100, as it is difficult to inhibit the adhesion
between coal particles. Although the area fraction of the par-
ticle with an area greater than 0.5 mm2 decreases slightly,
that reason is that the woody biomass particles control the
further growth of the coke structure that is connected by
coal particles.
3.2. Reduction in Inhibition of Connectivity between
Coal Particles
As mentioned above, the release of volatile matter from
woody biomass at low temperatures during carbonization is
one of the factors that inhibits connectivity between coal
particles. Accordingly, woody biomass was heated at each
temperature (300, 400, 500 and 1 000°C) in a N2 gas atmo-
sphere for 60 min, and woody biomass char with partly
removed volatile matter was prepared. The effect of remov-
ing the volatile matter from the woody biomass and the car-
bonization temperature on the connectivity between coal
particles in the coke sample was investigated. Macrostruc-
ture images of G95–BC(300)5, G95–BC(400)5, G95–
BC(500)5 and G95–BC(1000)5 are shown in Fig. 9. The
rugged dark-gray part is the woody biomass char, and the
other parts are the same as those shown in Fig. 5. Unlike the
coke structure in the coke sample with added woody bio-
mass shown in Fig. 5 (G95–B5, G90–B10), coal particles
were seen to be connected when woody biomass char was
added to caking coal.
The area fraction of coal particles obtained from macro-
structure images in Fig. 9 is shown in Fig. 10, with results
of G100 and G95–B5. For the samples with woody biomass
char addition, in comparison to the sample with woody bio-
mass addition (G95–B5), there is a small decrease in the
area fraction of particles with areas less than 0.5 mm2, and
particles with areas larger than 0.5 mm2 are in existence.
Moreover, the area fraction of particles with areas greater
than 0.5 mm2 increases with an increase in the carbonization
temperature of woody biomass char. Figure 11 shows
microstructure image of G95–BC(1000)5. When woody
biomass char with partly removed volatile matter is added,
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Fig. 9. Macrostructure images of G95–BC(300)5, G95–BC(400)5, G95–BC(500)5 and G95–BC(1000)5.

Fig. 11. Microstructure image of G95–BC(1000)5.

Fig. 10. Effect of woody biomass or woody biomass char addition

on the area fraction of coal particles.

woody biomass char adheres to the coal particles that soft-

ened and melted, and exists in the coke structure (carbona-
ceous matters) derived from coal, unlike in the microstructure
of G95–B5, as shown in Fig. 7. These results indicate that
the inhibition of connectivity between coal particles during
carbonization, due to the release of volatile matter from
woody biomass, can be reduced by partly removing the vol-
atile matter in advance. Furthermore, the effect is larger with
an increase in the carbonization temperature of woody bio- Fig. 12. Changes in TI+1 mm with time of G100, G90–W10, G80–
W20, G99.8–B0.2, G95–B5, and G90–B10.
mass char.

3.3. Effect of Woody Biomass Addition on Coke
Strength
Figure 12 shows changes in TI+1 mm of G100, G90–W10,
G80–W20, G99.8–B0.2, G95–B5, and G90–B10 with time.
TI+1 mm of G100 was 92.0%, and TI+1 mm of G90–W10 and
G80–W20 (with addition of non-slightly-caking coal) were
89.3% and 87.5%, respectively. The coke strength of the
coke sample deteriorates with an increase in the mixing ratio
of non-slightly-caking coal. In the case of woody biomass
addition, on the other hand, TI+1 mm of G95–B5 and G90–B10
decreased substantially to 6.2% and 3.3%, respectively, in
comparison with TI+1 mm of G100. These results indicate that
the addition of woody biomass causes a remarkable deterio-
ration in the strength of coke. The reason is that connectivity

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 ISIJ International, Vol. 54 (2014), No. 11
Fig. 13. Changes in TI+1 mm with time of G95–BC(300)5, G95–
BC(400)5, G95–BC(500)5, and G95–BC(1000)5.
between the coal particles during carbonization is inhibited
by the release of volatile matter from woody biomass, as
mentioned in Sec. 3.1. However, TI+1 mm (96.3%) of G99.8–
B0.2 was roughly equivalent to TI+1 mm of G100. Therefore,
the addition of a small amount of woody biomass weighing
0.2 wt% on the basis of the fixed carbon weight (1 wt% on
the basis of the sample weight) does not affect coke
strength.
Figure 13 shows changes in TI+1 mm of G95–BC(300)5,
G95–BC(400)5, G95–BC(500)5, and G95–BC(1000)5 with
time. TI+1 mm (7.4%) of G95–BC(300)5 was about the same
as TI+1 mm of G95–B5. There was a remarkable increase in
TI+1 mm of G95–BC(400)5 to 73.7%, and TI+1 mm of G95–
BC(500)5 and G95–BC(1000)5 reached 85.2% and 82.6%,
respectively. Values of TI+1 mm increase with an increase in
the carbonization temperature of woody biomass char.
TI+1 mm of G95–BC(500)5 had almost the same value as that
of G95–BC(1000)5. This indicates that the shrinkage of
wood biomass after resolidification of the caking coal (at
500°C and above) has very little influence on the strength
of coke. From these results, it is suggested that the carbon-
ization of woody biomass at temperatures of more than
500°C reduces the inhibition of connectivity between coal
particles during carbonization due to the release of volatile
matter from woody biomass, and improves coke strength to
the same degree as that of the coke sample made from cak-
ing coal.
4. Conclusions
Connectivity between coal particles and the coke strength
of a coke sample to which non-slightly-caking coal, woody
biomass, and woody biomass char were added to caking
coal, were evaluated quantitatively by observing the coke
structure and using an I-type tumbler tester for single parti-
cles, in order to investigate the possibility of using woody
biomass as a raw material in coke-making. The following
results were obtained.
(1) Connectivity between coal particles during carbon-
© 2014 ISIJ
ization was inhibited by the addition of non-slightly-caking
coal to caking coal. This inhibition of connectivity between
coal particles caused a decrease in coke strength.
(2) When woody biomass was added to caking coal,
connectivity between coal particles during carbonization,
and the coke strength, drastically decreased, although the
addition of a small amount of woody biomass (0.2 wt% on
the basis of the fixed carbon weight) hardly affected either
the connectivity between the coal particles or the coke
strength.
(3) The inhibition of connectivity between coal parti-
cles in the coke sample with added woody biomass can be
reduced by partly-removing the volatile matter of woody
biomass in advance. The effect of this was larger with an
increase in the carbonization temperature of woody biomass
char.
(4) The carbonization of woody biomass at tempera-
tures of more than 500°C improved the coke strength of the
coke sample with added woody biomass char to the same
degree as that of the coke sample made from caking coal.
Acknowledgments
This work has performed in a Research Group for Prog-
ress in Cokemaking Technology for Low-quality Coals and
Unused Carbon Resources, in The Iron and Steel Institute of
Japan (the chief examiner is Prof. H. Aoki, from Tohoku
Univ.). The authors would like to acknowledge the contri-
bution of all research group members.
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