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

Abstract: X-ray microtomography and ImageJ 1.39u is used as a tool to quantify volume percentage of

B4C as fillers in thermoplastic-natural rubber blend composites. The use of percentage of area occupied

by fillers as obtain from ImageJ from the microtomography sliced images enables the proposed technique

to easily obtain the amount volume percentage of B4C in the composite non-destructively. Comparison

with other technique such as density measurement and chemical analysis proves the proposed technique

as one of the promising approach.

Keywords: Non-destructive testing, X-ray Microtomography, Thermoplastic-natural rubber blend, Boron

Carbide, Composites

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/cm3

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

Correlation 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 B4C 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.% B 4C 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.