Application of ImageJ and X-ray Microtomography technique to quantify filler distribution in

Thermoplastic-natural rubber blend composites

Sahrim Ahmad a, A. Aziz Mohamed b, Jaafar Abdullah b, Hafizal Yazid a, *, M. Dahlan b, Rozaidi Rasid a,
W. Saffiey W. Abdullah b, Mahathir Mohamad b, Rafhayudi Jamro b, M. Hamzah Harun b, Mouad A. T. a
a
Faculty of Applied Science and Technology, Universiti Kebangsaan Malaysia (UKM), Bandar Baru
Bangi, 43000 Kajang, Malaysia.
b
Malaysian Nuclear Agency, Bangi, 43000 Kajang, Malaysia.
* Corresponding Author: Hafizal Yazid, Faculty of Applied Science and Technology, Universiti
Kebangsaan Malaysia (UKM), Bandar Baru Bangi, 43000 Kajang, Malaysia.
E-mail: hafizal@mint.gov.my Fax: 6-03-89250907 Tel: 6-03-89250510 extn: 1194

1. Introduction
Filler distribution in composite is one of the critical issues once the composite is fabricated. The
information is very important since the resulted properties of the composite are affected by the spatial
distribution of the filler or particles [1-3]. This is true especially in the case of particulate composite.
Therefore a systematic approach is used to characterize the filler distribution in polymer matrix
composite. The approach is to detect the present of the filler or particles and to quantify the particle
distribution through the use of X-ray microtomography and other techniques. Similar approach has been
developed and used to quantify the particle distribution in metal matrix composite with promising results
[4]. Another approach to characterize the filler distribution in thermoplastic is through the use of X-ray
phase contrast imaging, which also gives a promising result [5].
Stringent requirement of product specification leads to the improvement in product quality
control and testing. Thus brings the proposed technique as an attractive method as it is non-destructive in
nature. The non-intrusive nature of the measurement makes it possible for repetition and as a volume is
mapped there is no need for statistical approximation to the final population size or distribution. It is
apparent that tomography is useful in many fields and much work has been done and reported in materials
applications [6-10].
Conventional method in obtaining some quantitative information on the particle distribution in
composites is achieved through micrograph. The micrographs are captured using microscope coupled
with image analysis software. The captured micrographs are taken from slices of prepared sample. The
obtained information is only in 2D and extended to 3D by extrapolation and assumption. One typical
assumption is to treat the particle as point form or having a circular particle shape. These assumptions
may lead to inaccuracy or totally wrong information. Furthermore, sample preparation to turn it into
sliced form is necessary and this may damage the sample. The damage is possibly brought by torn-out
particle or smeared boundaries that result in misrepresentation of size or population [4]. Therefore the
non-intrusive method is required as the obtained data is more accurate and reliable.
X-ray microtomography is a non-destructive technique that produces accurate images of 3D
volumes by reconstruction from multiple X-ray projections, allowing the direct characterization of the 3D
microstructure of samples [11]. The X-ray images are taken around a single axis of rotation and currently
able to resolve details as small as few microns in size, even when imaging objects are made of high
density materials. As long as the density different between reinforcement and the matrix is comparatively
significant, the resulted image would yield a good image contrast. This is the common criterion that has to
be met in the use of any X-ray imaging technique.
The purpose of the development of thermoplastic-natural rubber (TPNR) composites is to
produce a boronated thermoplastic-rubber used as neutron shielding material in nuclear research reactor.
The excellent “ in between property ” of elastic and rigid of thermoplastic natural rubber make it an
attractive materials to be used as the matrix [12] and it could provide wide area coverage that require
radiation shielding. High thermal neutron cross-section material such as B4C is used as filler in order to
provide shielding effect against thermal neutrons [13-15]. The aim of the current work is ultimately to
quantify the distribution of boron carbide in the thermoplastic-natural rubber with the use of X-ray
microtomography and other techniques such as density measurement and thermogravimetry analysis. All
the techniques are compared and used to acquire information pertaining to the filler distribution and
concentration within the sample.
2. Methodology
Thermoplastic-natural rubber used in this study was incorporated with various percentage of
boron carbide with average size of 13.5μm. Boron carbide with natural rubber, thermoplastic and other
additives were compounded in Haake twin blade internal mixer for a predetermined optimum time and
mixing scheme. Finally the composite compound was heated press to form a slab sample with 1mm in
thickness. The sample is depicted in Fig. 1 as observed from the top view of the slab.

Figure 1: Sample in the form of slab as observed from top view

Slab with different formulation is given in Table 1.
Table 1: Slab samples with different formulation
Slab Percentage by weight of
B4C as filler in TPNR
1 A 0
2 B 10
3 C 20
4 D 30
5 E 40
6 F 50

For each slab, five samples or volume of interest are cut. They are denoted as volume of interest 1 or VOI
1, VOI 2, VOI 3, VOI 4 and VOI 5. The size of each VOI is 5mm in diameter and 1mm in thickness. The
location of VOI on the slab are shown in Figure 1 and numbered accordingly. Each of the VOI is the test
sample and subjected to testing and analysis.
A systematic approach is used to obtain information on reinforcement within the sample. The
samples were subjected to density measurement, X-ray microtomography scanning and chemical analysis.
Archimedes principle is used to obtain the density of each small cut section that contain VOI from which
the volume content of B4C could be calculated, as the value of standard blank sample is known. VOI
samples were subjected to Thermogravimetry analysis (TGA) to quantitatively obtain the weight percent
of boron carbide in the test samples. X-ray microtomography measurements were carried out on VOI
using a Sky Scan 1172 desktop x-ray microscanning. Data were collected at 60kV and 167A. The image
was detected on a high resolution (1280 x 1024 pixels) CCD camera as the sample was rotated and the
output from the CCD was fed through a reconstruction algorithm [9]. Beam hardening was also
computationally corrected, to produce a binary grey-scale bitmap image of the sample. The datasets
collected for the tomography were 360 angular range with a step size of 0.7 between images. The sliced
binary images are thresholded to obtain the areas occupied by B 4C. These values are used with results
from chemical analysis to establish a parameter named correlation factor of B 4C in the composites.
3. Results and discussions
Chemical analysis gives an accurate value of percentage of filler within the tested volume of
interest. In this case, TGA is used to obtain the amount of filler in the composite sample. The drawback of
this technique is that it is destructive in nature. This technique gives the overall vol% of B 4C but the
location of the particle within the VOI is not obtained. Result of TGA is given in Figure 2.
Figure 2: Average mass % of B4C in VOI’s for each of the slab
TGA thermograms reveal the actual concentration of B 4C in the slabs. The amount of B4C was
found slightly lower than the target composition as the filler lost is common during mixing process. This
is due to the filler adhesion at the surface of hopper or feeding system. From Figure 2, as expected slab A
was absent of filler. This is followed by slab B to F with a gradual increment of filler or B 4C. However,
this technique does not provide any information on the filler distribution in the sample and exhibit only
information on filler concentration. Therefore this technique is coupled with the X-ray microtomography
to utilise both the information on the particle distribution and the actual filler concentration.
X-ray microtomography reveals the 3D volume microstructure of the sample. The density
difference between the filler and the matrix enable the filler to appear darker than the matrix. Therefore
particle distribution could be observed within the slices of VOI. Typical image reconstruction of 3D
volume microstructure of the sample is shown in Figure 3.

Figure 3: Typical 3D volume microstructure of VOI with 10%wt filler

Typical horizontal X-ray microtomography slices of VOI’s before and after thresholded is shown in
Figures 4 – 10. The image is thresholded in order to show B 4C.
Figure 4: Typical slice of matrix without filler.

(a) (b)
Figure 5: (a) Typical slice of matrix + 10%wt filler, (b) thresholded of image (a) and typically yield
2.515% bright areas.

(a) (b)
Figure 6: (a) Typical slice of matrix + 20%wt filler, (b) thresholded of image (a) and typically yield
5.331% bright areas.
(a) (b) Figure 7: (a)
Typical slice of matrix + 30%wt filler, (b) thresholded of image (a) and typically yield 8.297% bright
areas.

(a) (b)

Figure 8: (a) Typical slice of matrix + 40%wt filler, (b) thresholded of image (a) and typically yield
10.640% bright areas.
(a) (b)

Figure 9: (a) Typical slice of matrix + 50%wt filler, (b) thresholded of image (a) and typically yield
13.402% bright areas.

The microtomography slices (Figures 5b-9b) in the thresholded images show a variation in the
percentage of bright areas. The bright areas indicate the present or occupancy of filler. This is possible
since the density difference between the matrix and the filler is high. The matrix density is 0.920g/cm 3
and the filler is 2.520g/cm3. Thus, this has eased in the thresholding process to obtain the areas that reflect
the present of B4C. It was found that 8.514%wt by chemical analysis corresponds to 2.515% bright areas
in the thresholded image as typically shown in Figure 5b. Other thresholded images give 5.331%,
8.297%, 10.640%, 13.402% bright areas and correspond to 18.4941%wt, 27.8368%wt, 37.6574%wt,
43.224%wt respectively by chemical analysis.
A correlation factor is established to enable the filler in the sliced image being interpreted
quantitatively. This is achieved by having an average value of area occupied by the filler in the sliced
image. In this work, the sliced image is analysed from top to bottom of the VOI with the condition of in
between 2 analysed image, there would be 9 sliced images that are abandoned from analysis to avoid
misleading interpretation. The misleading is from the filler that appeared in more than 1 slice. Thus, the
percentage of area occupied by the filler is compared against the result of chemical analysis. Both results
are correlated by:
A var age vol. percentage of fillers by chemical analysis
Correlatio n factor  (1)
A var age area percentage of fillers in the sliced image
The existence of the correlation factor is clearly observed from the graph of average volume percentage of
fillers from chemical analysis against average area percentage of fillers in the sliced image. This is shown
in Figure 10.
 Figure 10: Volume percentage of fillers from chemical analysis against average area percentage of fillers
in the sliced image
Based on Figure 10, the correlation factor is significantly the slope of the resulted graph. Based on the
graph, the correlation factor was found to be approximately 1.3155. Thus, equation (1) reduced to:
Vol. % of fillers  A var age area percentage of fillers  1.3155 (2)
Equation (2) could be used to estimate the volume percentage of B 4C for any given sample that was
subjected to X-ray microtomography inspection providing any further work done using the same type of
system.
Density measurements lead to the determination of amount of B4C in the sample as the density
of each of the ingredient is known. Average densities of small size cut sections that contain VOI are
obtained for each slab and these results are compared between the slabs. This comparison is shown in
Figure 11.

Figure 11: Avarage density measurement for each slab

From Figure 11, slab A shows the lowest value of density with 0.920g/cm3 due to the absent of filler. As
the filler content is increased from slab B to F, the density also increased accordingly. The maximum
achievable density is for slab F with the value of 1.354 g/cm3.
Results of chemical analysis, corrected X-ray microtomography, Archimedes method and X-ray
microtomography are plotted in Figure 12.
Figure 12: Comparison of volume of B4C for each slab by 4 different methods.
Overall volume percentage of B4C is given by 2 sets of values from chemical analysis and Archimedes
method. Chemical analysis gives an accurate amount vol.% B4C but Archimedes method suffer
discrepancies if samples contain porosity or inclusions. This is shown in Figure 12 for slab C, D and E
where the vol.% B4C value obtained from density result is significantly lower than that obtained from
chemical analysis. This is due to changes in density not only being affected by fillers but also by porosity
or inclusions. The presence of porosity in VOI is typically shown in Figure 13 as detected by
microtomography in the case of slab E.

Porosity

Figure 13: Present of porosity in VOI from slab E.

Although chemical analysis or specifically TGA is good in term of result accuracy and not affected by
porosity, it is still considered as a time consuming analysis and destructive method. However, this
technique could be used as a reference with the microtomography result in order for us to establish the
correlation factor. This is true providing the relationship between the vol.% B4C by chemical analysis and
area% B4C by microtomography is valid. As observed from Figure 12, microtomography results itself
does not show the actual filler concentration. Therefore, the introduction of correlation factor is a must
and in this work, the value was found 1.315. Once this value multiplied by area% of fillers obtained by
microtomography, this new value or known as corrected x-ray microtomography is found close or almost
identical to the actual filler concentration by chemical analysis as shown in Figure 12. Thus,
quantification of B4C in TPNR composite is possible by the use of correlation factor or corrected X-ray
microtomography method. This method provide a simple mean to find the volume percent of fillers
present providing the result of area% of fillers by microtomography is available and the work done using
the same type of system.
4. Conclusions
The work could be considered as an evidence of the applicability of the X-ray microtomography
to quantitatively obtain the concentration of B4C in the TPNR composites. Results of X-ray
microtomography were successfully calibrated using thermogravimetry analysis or TGA. In this work, the
correlation factor was found to be 1.315. This value once multiplied with the area percentage of fillers in
the sliced image would yield the concentration of fillers or B 4C in the sample. This technique enables the
X-ray microtomography results to reveal the composition of B 4C in the sample in a quantitative manner
with the existing capability exhibited the location or distribution of the B 4C. Further research will be
focused on to establish a correlation factor for different types of filler that are typically used in the
polymer composites and to obtain a set of correlation factor data for use in X-ray microtomography
analysis.
Acknowledgements
The authors wish to thank Hishamuddin Husain for proofreading the paper. The excellent support from
MINT and UKM throughout the research is highly appreciated.
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Biography
Hafizal Yazid
Hafizal received his first degree in Materials Engineering from University of Malaya, Kuala Lumpur,
Malaysia. He starts his work as a metallurgical engineer and currently working in Industrial Technology
Division, Malaysian Nuclear Agency, Bangi, Kajang Malaysia. His work relates to the application of
Radiography technique in the industry and carry out research pertaining to radiography image
enhancement. His work also covers development and characterization of materials used as radiation
shielding in nuclear research reactor. His major publication include:
1. Yazid H et al, Circular discontinuities detection in welded joints using Circular Hough
Transform, NDT&E Int. (2007), article in press, doi:10.1016/j.ndteint.2007.05.004
Sahrim Ahmad
Sahrim Ahmad received his doctorate degree from Loughborugh University of Technology, UK in the
area of Materials Engineering in 1988. He is currently a Profesor in Universiti Kebangsaan Malaysia and
involves in the field of polymer development and characterization.
Abdul Aziz Mohamed
Abdul Aziz Mohamed gained his master degree from Surrey University, United Kingdom in 1980. He
then received his doctorate degree from Cranfield University in the area of advanced materials on
application of non-destructive technique in creep problem. He is now a senior research officer in
Malaysian Nuclear Agency.
Jaafar Abdullah
Jaafar Abdullah is currently a senior research officer in Malaysian Nuclear Agency. His work involves in
research and application of tomography in oil and gas industries.
M. Dahlan
M. Dahlan is currently a manager and senior research officer in Malaysian Nuclear Agency. His work
involves in research and application of polymer composites.
Rozaidi Rasid
Rozaidi Rasid is currently a senior lecturer in Universiti Kebangsaan Malaysia. His work involves in
processing and rheological studies of polymer blend.
W. Saffiey W. Abdullah
W. Saffiey W. Abdullah is currently a senior research officer in Malaysian Nuclear Agency. His work
involves in research and development of non-destructive testing.
Mahathir Mohamad
Mahathir Mohamad is a research officer in Malaysian Nuclear Agency. His work involves in research and
development of polymer composites.
Rafhayudi Jamro
Rafhayudi Jamro is a research officer in Malaysian Nuclear Agency. His work involves in research and
development of radiation shielding materials.
M. Hamzah Harun
M. Hamzah Harun is a research officer in Malaysian Nuclear Agency. His work involves in research and
development of polymer blend.
Mouad A. T.
Mouad A. T. is currently a graduate student in Universiti Kebangsaan Malaysia. His work involves in
research and development of polymer nanocomposites.
Eda Rosnita
Ida Rosnita is currently a graduate student in Universiti Kebangsaan Malaysia. Her work involves in
research and development of liquid natural rubber.