Fuel Vol. 77, No. 11, DD. 1203-1208.

1998
0 1998 Elsevier Science Lid All rights reserved
Printed in Great Britain
0016.2361/98 $19.00+0.00

PII: SOO16-2361(98)00019-2

Effect of coal properties and porous

structure on tensile strength of
metallurgical coke
Hiroshi Satoa, John W. Patrickb and Alan Walkerb8*
aNippon Steel Chemical Co., Ltd, Kimitsu Works, Kimitsu, Chiba 299- 11, Japan
bCarbon Research Group, Chemical Engineering
Department,
Loughborough
University,
Loughborough,
Leicestershire
LE7 1 3TlJ, UK
(Received 30 May 1997; revised 14 August 1997)

The tensile strength of coke was studied to obtain a better understanding of coke strength and its relation to coal
properties. The tensile strength was examined by considering coke as a porous material with two influential
factors, namely, the matrix strength and the porous structure, which were estimated from the measured tensile
strength and porosity. The coke carbon matrix was evaluated in the light of the structure of the coke carbon
estimated using X-ray diffraction on the basis of the concept of graphitic and non-graphitic carbon. It was found
that the coke matrix strength becomes stronger as the coke carbon structure approaches that of non-graphitic
carbon. The porous structure was governed by the coking properties, in this case, the maximum fluidity and the
swelling number. As regards the factors governing the coke porous structure, determined by means of image
analysis and optical microscopy, it was demonstrated that a poor porous structure was associated with a wide pore
size distribution caused mainly by a high proportion of the pores of length < 20 pm, and a rough surface of the
pore periphery, which provides potential stress concentration points. The strength anisotropy, which is considered
to affect the route of a crack path in lump coke, was also related to pore orientation and the quality of the porous
structure. 0 1998 Elsevier Science Ltd. All rights reserved
(Keywords: coke; tensile strength; coal properties)

INTRODUCTION
For metallurgical coke, strength is a most important quality,
since it governs coke degradation in the blast furnace and
consequently
influences the permeability
in the bed and
operation efficiency. Industrial coke strength has been
evaluated mainly by means of drum indices and although
these are useful assessments of coke quality for the blast
furnace operation, the breakage mechanism in the drum is
complicated and it is therefore difficult to understand the
precise meaning of the indices and to interpret them in terms
of mechanical properties.
To improve the understanding of the strength indices and
to facilitate accurate and cost effective coal blend formulation for the production of coke of the required quality, it is
important to understand further the coke strength indices as
a mechanical property. Moreover improved understanding
of the relationships between the drum test indices and the
mechanical properties, and between the mechanical properties and coal properties and carbonisation
conditions is
desirable.
Since coke is a brittle material, the tensile strength of
coke has been studied mainly to evaluate the mechanical
strength of coke as a porous materiallm3. To evaluate and
discuss the nature of the strength of a porous material, it is
* Corresponding

author.

necessary to take into consideration

the effect of the
porosity-and to separate the effects of the matrix strength
and the porous structure. It was previously reported that a
qualitative evaluation
of the coke matrix strength was
possible by using an empirical equation which explained the
tensile strength in terms of the matrix strength and porosity4.
Amongst the various equations used, that based on the
results of Ryshkewitch5 and examined by Knudsen6 has
been widely applied to many studies of the strength of
porous materials since the equation separates the effect of
porous structure from the tensile strength as well as the
effects of matrix strength and porosity.
Some studies have used the equation to obtain a better
understanding of the strength of coke on the basis of coke
being a porous material. The porous structure of coke has
been determined to establish a relation between the porous
structure coefficient in the equation and the porous structure
as observed by optical microscopy and image analysis7. By
assuming an identical porous structure, attempts were made
to evaluate the coke matrix strength in relation to the coke
carbon texture* and to model the coke tensile strength by
estimating the matrix strength in relation to the microstrength index. The effects of the coking properties of the
coal and the carbonisation
conditions
on the porous
structure were discussed by assuming identical matrix
strength for a metallurgical
coke. However, no study

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Tensile strength of metallurgical coke: H. Sato et al.

Table 1

Properties of coal
VM

VM
wt% dmmf

Ash
wt% db

Fixed C
wt% db

Sw. no.

wt% db

Maximum fluidity
log ddpm

Gray-King
coke type

20.0

21.1

5.0

75.0

8.0

2.93

G9

26.6

28.4

6.3

67.1

8.0

4.09

G9

29.4

38.7

21.2

49.4

2.5

1.54

35.9

37.2

5.0

59.1

7.5

2.78

G5

38.9

41.6

5.3

55.8

4.5

3.11

G6

appears to have been made to evaluate both the porous

structure and the matrix strength simultaneously for
cokes made from coals covering a wide range of coking
properties.
Furthermore, it is recognised that coke has a strength
anisotropy due to the anisotropy of the porous structure.
Since this strength anisotropy could influence crack
propagation and the direction of the crack path, and these
cracks affect the coke strength index and mean size of coke,
it is important to assess this effect in relation to the porous
structure.
In this study, cokes made from coals with a wide range of
properties were examined. The effects of the porous
structure and the coke matrix strength on the tensile strength
were evaluated separately using the empirical equation
which relates strength and porosity and the effects of the
coal properties were also assessed. The porous structure was
observed by means of optical microscopy and image
analysis and coke matrix strength was evaluated in the
light of the carbon structure estimated by X-ray diffraction.
The strength anisotropy is discussed with regard to the
porous structure by relating the tensile strength and crack
path angle, i.e. the angle between the crack path and average
pore orientation measured in the image analysis.
EXPERIMENTAL

sliced off these cores and about 30 suitable disc specimens

for each sample were selected for the strength test.
Coke carbon structure analysis

Crystallite stack height, Lc, and width, La, of the coke

carbon matrix were estimated by means of X-ray diffraction13 to evaluate the difference in coke carbon structure for
each coke sample. Samples for the measurement were
obtained by crushing fragments of the fractured coke
specimens from the tensile strength measurement. To
represent the nature of the coke carbon matrix, the following
parameter was defined;
carbon structure factor = L.u/Lc

(1)

The carbon structure factors for the cokes made from each
coal were determined using the crystallite size of cokes
prepared at the three final temperatures of 600, 800 and
1000C. This factor is defined on the basis of the concept
of graphitic and non-graphitic carbon introduced by
Franklin14. Although coke samples discussed in this study
were carbonised at a relatively low temperature for the division into graphitic and non-graphitic carbon, it was assumed
that the carbon structure factor can represent the nature of
the coke carbon. According to the definition, as the carbon
structure factor increases, the nature of carbon approaches
that of non-graphitic carbon and tends to have a cross-linked
carbon structure.

Laboratory scale coke oven

To produce coke samples carbonised under carbonisation

conditions similar to those of a commercial coke oven but
small enough to prevent significant property variations in
the coke lump, a coal charge was carbonised in a laboratory
scale oven heated from the two side walls. Air-dried coal,
sized less than 3 mm, was packed in a charge box, 160 mm
long, 100 mm wide and 100 mm tall, to a charge density of
800 kg/m3. Cokes were carbonised at 3Wmin to final
temperatures of 600,800 and 1000C measured at the centre
of the half oven width. The final temperature was
determined on the basis of the heating conditions of a
previous stu$ on the strength development during
carbonisation . To assess the effect of coal properties on
the tensile strength, a wide range of coals with regard to
coking properties and coal rank were used. The properties of
the five coals used are listed in Table I.
Tensile strength

Tensile strength of the coke samples was determined

using the diametral compression test . Specimens of each
sample for the test were obtained by drilling cylindrical
cores using a lo-mm diameter diamond-tipped core drill. TO
evaluate the tensile strength in relation to fissure direction,
coke cylinders were prepared in the direction normal to the
heat flow from the centre of the half oven width, where the
thermocouple was placed. Discs about 7 mm thick were

1204

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Porous structure analysis

The porous structure of the coke was observed by means

of image analysis using incident light microscopy. Samples
for the image analysis were obtained by mounting the
fractured coke samples from the tensile strength test in a
block of resin and prepared as polished sections. The porous
structure of each sample was determined by examining
more than 300 fields, 1.2 X 1.26 mm, from approximately
20 specimens for each sample. Since the larger pores were of
most interest, a low power objective lens, magnification X
4, was used to give a pixel size 3.3 X 2.9 pm and very small
pores under 12 pm were eliminated by image processing
(erosion followed by a dilation).
The image analysis system was programmed to give
measurements of the number, length, breadth, circularity
and orientation of pores. To evaluate the effect of the porous
structure on the strength, the following parameters were
introduced by using the measured data from the image
analysis.
Pore size distribution factor: the gradient of the linear
relation obtained by regression analysis when the pore
size and the cumulative number of pores are plotted in
a log-log plot. As the factor becomes larger, the pore size
distribution range becomes narrower.
Pore rugosity factor: this parameter was defined to

Tensile strength of metallurgical coke: H. Sato et al.

Crack path angle

Figure 1

Schematic diagram of the crack path angle definition

04

evaluate the degree of smoothness of the pores, since a

sharp pore shape can be a stress concentration point and
affect the strength15. The rugosity was calculated from
the pore circularity defined as
pore circularity = 4n(pore area)/(pore perimeter)

Relationship between carbon structure factor Lu/ti

strength of coke matrix

(2)

(3)

Since pore perimeter is strongly affected by the pore size

because of its strong dependence on resolution, the
parameter was calculated for pore length in the range
between 200 and 300 pm. When a pore has a rough surface, the perimeter is longer than that of an ideal ellipse of
the same aspect ratio and the pore circularity is smaller.
Therefore, when the pore rugosity factor becomes smaller, the pore shape has a rough surface and deviates from
an ideal elliptical shape.
. Crack path angle: the angle between crack path and average pore orientation. It is measured as a pore orientation
in the image analysis procedure by setting a crack path in
the fractured specimen along the Y-axis in the measuring
field as shown in Figure I.

Coke matrix strength and carbon structure

In considering the effect of the coke carbon structure on
the coke matrix strength, a relationship between the carbon
structure factor, which represents a nature of carbon in
relation to graphitic or non-graphitic carbon, and the
estimated strength of the coke matrix at 1000C was
examined. Figure 2 shows the relationship for coals A, B, D
and E. In this figure, coal C was excluded since it contained
a considerable amount of mineral matter and this could not
be taken into consideration in the carbon structure factor,
which is defined only by the X-ray diffraction of the coke
carbon. The large amount of mineral matter content and an
associated poor coking quality caused a weak porous
structure and led to a large estimated coke matrix strength.
Although the estimated matrix strength for coal C could be
taken as a qualitative value in relation to the other coals, it is

RESULTS AND DISCUSSION

Evaluation of the coke matrix strength and the porous
structure
To evaluate the porous structure and the matrix strength
separately, and to exclude the effect of porosity, the
empirical formula for porous materials, which relates
strength and porosity5,6, was used
(4)

where [Tand uo are the tensile strength of the porous material

and the matrix material, respectively, P is the volume porosity and c is a coefficient which represents the porous
structure of the material. Although this is an empirical
equation and has no strict physical meaning, the equation

Table 2

and

has been used widely to evaluate the strength of porous

materials in relation to porosity and hence the effect of
the porous stmcture6. Therefore, it was considered that
this equation is capable of qualitatively estimating the
matrix strength and effect of the porous structure4.
The coefficient c was determined by the statistical
regression technique using approximately 90 values for
the coke samples made from the same coal by assuming that
the porous structure was identical for each coke. This was
assumed because the samples were prepared under the same
heating conditions, apart from the final temperature, and
therefore the heating conditions during the plastic stage
which, in conjunction with coking properties, governs the
porous structure, was considered to be identical in all
cases thereby leading to the same porous structure. The
strength of the coke matrix for each final temperature was
also determined by this procedure. A summary of the results
obtained for the cokes carbonised to 1000C is given in
Table 2.

pore rugosity factor = (pore circulanty)

0 = a0 exp( - cP)

Figure 2

The circularity of the pores compared with that of an

equivalent ellipse, i.e. with the same aspect ratio, then
gives a measure of the pore rugosity.

/(pore circularity of equivalent ellipse)

4
3
Carbon structure factor [-]

Summary of coke strength and structural data

Apparent density (kg/m)

True density (kg/m3)
Fractional volume porosity
Tensile strength (MPa)
standard deviation (MPa)
Strength of matrix (MPa)
Porous structure coefficient

911
1981
0.54
4.31
0.93
55.6
4.77

910
2044
0.56
5.36
1.21
58.9
4.37

801
2060
0.61
4.70
0.96
385.0
7.25

863
1949
0.56
4.96
0.99
97.5
5.38

829
2017
0.59
4.60
1.22
122.5
5.64

Fuel 1998 Volume

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Tensile strength

coke: H. Sato et al.

of metallurgical

-8m

&!_a

E7

2.5

.$
E
$6
0
F
$5

Sw.No.
2.0
4.0
6.0
8.0

2
j
.4
CF,t..........
24
15

20

:
40

VcEile

Figure 3
factor

ma?&

:
45

Relationship between coal rank and carbon structure

Fuel 1998 Volume

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11

1.5

2.5

Maximum

[dmrTwt%]

difficult to discuss this difference in relation to the carbon

structure factor defined in this study.
The coke matrix strength increases with an increase in the
carbon structure factor. In other words, the coke carbon
matrix becomes stronger when the carbon becomes a more
non-graphitic carbon like structure. This can be explained
on the basis of the carbon structure model which describes
the non-graphitic carbon as a cross-linked structure4. It was
reported that the non-graphitic carbon has a strong system of
cross-linking
in the carbon structure and it binds the
crystallites in a rigid mass, so that the resulting carbons
are termed hard carbon13.14. Furthermore,
the measured
high Knoop hardness of coke is concluded to be attributable
to the three-dimensional
network structure7. Since the
hardness of materials has a correlation with their tensile
strength, the strength of coke was expected to be higher
when the coke carbon has a cross-linked structure. Therefore, it is possible to conclude that the estimated matrix
strength is able to represent the coke carbon matrix strength,
at least qualitatively.
Figure 3 shows the relationship between the volatile
matter (dmrnf) and the carbon structure factor. Since a lower
rank coal tends to have a smaller LX, crystallite stack height,
the carbon structure factor derived from eqn (1) becomes
larger. This tendency suggests that the carbon from the
lower rank coal approaches that of a non-graphitic carbon
and is in good agreement with previous studies about
graphitisation
of carbon and carbonisationlg,
where nongraphitic properties were associated with low-rank coal.
Hence, it is concluded that the carbon structure factor
defined in this study is capable of representing the nature of
the coke carbon.
However, from the results shown in Figure 1 and
Figure 2, it appears that the coke carbon matrix is stronger
for the coke made from lower rank coal in the range of coal
rank used in this study. This is different to the general
understanding, which associates a strong coke matrix to the
coke made from medium rank coal, i.e. with a maximum
reflectance of vitrinite around 1 .O- 1.2% or higher rank coal
(in a coal rank range around VM 20-40 dmmf wt%)7320.
Apart from the study which measured the coke matrix
strength as the Knoop hardness number17, the coke matrix
strengths were estimated using tensile strength data on
the basis of an identical porous structure for various
coke samples, and using mercury pressure porosimetry
and modelling of the coke porous structure as an ideal
and identical porous structure for every coke sample*.

1206

Figure 4
coefficient

3.5

4.5

fluidity [log ddpm]

Effect of coking properties on porous structure

Accordingly,
these results are considered to contain an
effect of the porous structure, which is strongly influenced
by coking properties, and therefore they differ from the real
coke carbon matrix strength. Even the data based on the
Knoop hardness number varied and it is difficult to
determine at which point the maxima in strength occurred
being from 85 to 90 wt% (d.a.f.) of the coal carbon
content17 . Since, the high Knoop number was attributed to a
three dimensional
network structure of carbon, the coke
which has a cross-linked carbon structure, namely, close to
that of the non-graphitic carbon can be considered to have a
strong matrix strength. Consequently,
it is concluded that
the coke matrix strength is stronger when the coke carbon
has a cross-linked structure and this feature tends to be
associated with a coke made from a lower rank of coal.
Effect of coking properties on the porous structure of coke
As a porous material, the coke strength is governed by
the matrix strength and the porous structure. In this
study, the effect of porous structure on the tensile
strength was represented by the coefficient c in eqn (4).
A larger coefficient means a weaker porous structure
because
of the reduction
in strength when porosity
increases.
The relationship between the porous structure coefficient
and the coking properties, maximum
fluidity and the
swelling number, is shown in Figure 4. The lines shown
in the figure were derived from the relationship between the
porous structure coefficient and the coking qualities, the
maximum
fluidity and swelling number, by statistical
regression. The porous structure coefficient decreases, in
other words, the porous structure improves as the maximum
fluidity and the swelling number increase. Since differences
between the coefficient appear to be well explained by these
two coking properties it is possible to explain the quality of
porous structure on the basis of the relation of an adhesive
and a force to put particles together. In this case the
maximum fluidity indicates the quality of adhesive and the
swelling number indicates the force for adhesion. Therefore,
it is necessary to have a good quality in both coking
parameters to obtain a better porous structure. On the basis
of this concept, the porous structure is considered to be
improved by a high heating rate and high charge density
which improve the fluidity and state of adhesion between
particles, respectively lo. Although these considerations
apply in this instance, it is recognised
that there is
likely to be optimum values of these parameters. Such

Tensile strength of metallurgical coke: H. Sato et al.

4
0.5

0.55

0.6

0.65

Pore size dist. factor [-]

0.45

Pore diameter 200-300 pm

0.65

0.6
0.55
0.5
Pore smoothness factor [-]

Figure 5 Relationship between pore size distribution factor and

porous structure coefficient

Figure 6 Relationship between pore rugosity factor and porous

structure coefficient

considerations
was used.

As shown in Figure 5 and Figure 6, the measured coke

pore structure clearly indicates that the adhesion of the coal
particles is vital for a good porous structure and hence a
strong coke. To obtain a good porous structure, enough
adhesive and force to fuse particles together are necessary to
fill the space between particles and to prevent sharp edges in
pores at which stress concentration could take place.

may be applicable

if a wider range of coals

Relationship between measured porous structure and

estimated coefSlcient
Measurements
of coke porous structure by optical
microscopy
have been used in attempts to find an
explanation for coke strength differences. However, there
has been little in the way of quantitative evaluation of the
porous structure and its relationship
with the porous
structure coefficient in eqn (4)7S21. Therefore, an attempt
was made to quantify the porous structure using optical
microscopy and image analysis with the aim of establishing
a parameter which has a strong correlation with the porous
structure coefficient.
Figure 5 shows the relationship between the pore size
distribution
factor defined previously
and the porous
structure coefficient. There is a good correlation between
two parameters, with a poor pore structure being associated
with a wide pore size distribution. This difference in the
pore size distribution factor was mainly attributable to the
proportion of the smallest pores-pore
length less than
20 pm-in
the pore size distribution.
A low pore size
distribution factor was caused by a large proportion of the
small pores in the pore size distribution. On the basis of
the relationship between the porous structure coefficient and
the coking properties, it is deduced that the large proportion
of small pores in the coke porous structure is attributable to
poor coking properties and represents a consequent inferior
adhesion between coal particles, which might lead to
unfilled gaps between particles.
The poor coking properties were used to explain the poor
coke strength in relation to pore shape, where a rough pore
shape caused by lack of fluidity was associated with poor
strength whilst a smooth pore shape was associated with
high strength because of the possible stress concentration at
sharp edges in a pore22. However, no qualitative evaluation
for such a concept has been made. It is to represent this
smoothness of the pores in the coke that the pore rugosity
factor was introduced.
The effect of the pore smoothness on the porous structure
factor is shown in Figure 6. In the figure, an effect of pore
aspect ratio was neglected since all average aspect ratios of
each sample were within 0.61-0.64 and the effect of this
variation was considered to be small. The figure shows that
as the pore shape becomes smoother, the porous structure
becomes better.

EfSect of pore orientation on tensile strength

It is well known that coke has a porous structure
anisotropy due to the coking pressure generated during
carbonisation.
Pores tend to distort through the semicoke
being compressed towards the hot walls by the coal swelling
pressure during carbonisation2 and consequently the coke
strength differs in the directions normal to and parallel to the
oven wall. It was reported that the compressive strength of
coke specimens compressed at right angle to the long axis to
the coke lump, that is in the direction parallel to the heat
flow, was 1.36 times greater than that measured in the
direction normal to the heat flow.
The effect of the anisotropy of the porous structure on the
tensile strength was discussed on the basis of the relationship between a crack path angle and the tensile strength. By
the definition, a crack path angle of 90 represents the
strength for the propagation of fissures normal to the oven
wall and when it is 0 for fissures parallel to the oven wall.
Although the strength anisotropy
is considered
to be
influenced by the extent of the pore distortion, the aspect
ratio of the pores, this effect was neglected in this study
since the pore aspect ratio obtained was similar for all the
coke samples.
To evaluate the effect of the crack path angle on the
tensile strength and the effect of quality of the porous
structure on the strength anisotropy, the tensile strength,
normalised to an identical porosity of 0.55, was examined
for specimens with good (coal B), medium (coal D) and
poor (coal C) porous structure factors. The results inevitably
showed variability since many factors affect the tensile
strength, but they suggest that the tensile strength improves
when the crack path angle increases. This leads to the
conclusion
that the coke is more resistant
to the
penetration
of a longitudinal
fissure, which is normal
to the oven wall, than a transverse fissure, which is
parallel to the oven wall. There are indications that this
strength dependency
on the crack path angle becomes
less marked when the coke porous structure becomes
poor, but further study is necessary to confirm this idea

Fuel 1998 Volume

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Tensile strength

of metallurgical

coke: H. Sato

et al.

that the difference in coke strength anisotropy in

relation to the porous structure quality affects the
mechanism of the fissure formation in coke lumps.

student with the Carbon Research Group, Loughborough

University.

CONCLUSION

REFERENCES

The effect of coal properties on the tensile strength of coke

has been discussed by separating the tensile strength into the
matrix strength factor and the porous structure factor.
The matrix strength of coke carbon was evaluated on the
basis of the carbon structure in relation to graphitic and nongraphitic carbon structures. It appears that the coke with a
larger carbon structure factor, i.e. a carbon structure closer
to that of non-graphitic carbon, tends to have a stronger
matrix strength, due to the cross-linking of the carbon
structure. The carbon structure factor depends on the rank of
coal and for the range of coal rank used in this study, the
coke made from lower rank coal tended to have a larger
carbon structure factor. Thus, the coke matrix strength
tended to be stronger for lower rank coal over the limited
range of coal rank studied.
It was clearly demonstrated that the porous structure was
governed by the coking properties. For the range of coal
used, the porous structure improved as the maximum
fluidity and the swelling number of the coal used increased.
The quality of the porous structure can be evaluated on the
basis of the pore size distribution and the smoothness of the
pores as defined in this study. Both parameters were
considered to represent the state of adhesion between coal
particles.
The strength of coke differs depending on the orientation
of the pores and it is considered that this strength anisotropy
affects the fracture phenomena, such as the direction of the
crack path. This strength anisotropy seems to be influenced
by the quality of the porous structure and the effect of
porous structure anisotropy is more apparent when the
porous structure, represented by the defined porous structure
factor, is better.
ACKNOWLEDGEMENTS
H.S. would like to thank Nippon Steel Chemical Co., Ltd.
for financial support to undertake this study as a research

1208

Fuel 1998 Volume

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