Materials Letters 58 (2003) 154 – 158

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A novel ultrasonic transducer backing from porous epoxy resin–titanium–

silane coupling agent and plasticizer composites
Farid El-Tantawy a,*, Yong Kiel Sung b
a
Department of Physics, Faculty of Science, Suez Canal University, Ismailia, Egypt
b
Department of Chemistry, Dongguk University, Seoul 100-715, South Korea
Received 6 January 2003; received in revised form 5 May 2003; accepted 9 May 2003

Abstract

In this paper, a new composite for ultrasonic attenuation backing has been successfully fabricated from porous epoxy resin containing
titanium (Ti), silane coupling agent and plasticizer composites. The effect of Ti particles on the network structure and mechanical properties
of epoxy resin has been analyzed in detail. The ultrasonic parameters in epoxy composites have been measured by a conventional pulse-echo-
overlap technique at a frequency of 1 – 5 MHz. The effect of Ti content and temperature on the longitudinal sound velocity and attenuation of
epoxy resin composites were investigated. Precise in situ observations of the acoustic properties such as attenuation and acoustic impedance
of epoxy composites are expected to be useful for ultrasonic transducer systems for new as well as for backing application with high
attenuation.
D 2003 Elsevier B.V. All rights reserved.

Keywords: Epoxy resin; Titanium; Materials composite; Microstructure; Mechanical properties; Ultrasonic properties; Backing; High attenuation

1. Introduction ized by a hardener to obtain composite materials. This

This study is part of an on-going research project aiming
to develop a high performance composite material for ultra-
sonic transducer backing with high acoustic impedance,
attenuation and toughness. Epoxy resins are commonly
used as polymeric matrices in high-performance composites
due to their good thermal stability, environmental resistance
and good mechanical properties and in the manufacture of
backings because of its low initial viscosity and its high
adhesion [1 –5]. In fact, the need for transducer suitable for
use in attenuation backing under high hydrostatic conditions
is increasing in industry. Typically, backings are composed
of epoxies loaded with metallic filler such as tungsten, iron,
copper, magnesium and aluminum are used to obtain high
acoustic impedance for the backing material, whereas fillers
of wood dust, glass and cork are used for low impedance
backings [4,5]. It is well known that there are two methods
to modify epoxy resin: the first consists of adding rubber
particles in the initial liquid resin, which is then polymer-
* Corresponding author. Fax: +20-81-025-262-6265.
E-mail address: faridtantawy@yahoo.com (F. El-Tantawy).
method allows one to achieve simultaneously a low initial
viscosity, a high attenuation and a high stiffness. The
second uses a reactive liquid rubber, which is initially
soluble in epoxy resin and the phase separation occurs
during the vulcanization of the epoxy. This method does
not increase significantly the mixture viscosity of the
composite [6]. To overcome this shortcoming and to fulfill
the above stated needs, the epoxy resin has been modified
by adding plasticizer, coupling agent and Ti powder. To the
best of the author’s knowledge, porous epoxy filled with Ti
particles, silane coupling agent and plasticizer for ultrasonic
backings are still unavailable in publications. The target of
the study is the fabrication of a novel attenuation backing
based on porous epoxy – Ti – silane coupling agent and
plasticizer composites. The effect of Ti content on the
structure and mechanical properties of the epoxy compo-
sites was interpreted in detail. Also, the temperature depen-
dence of attenuation and sound velocity of epoxy
composites were tested. For ultrasonic transducer backing,
the effect of Ti content and frequency on the attenuation
was investigated. Furthermore, the effect of Ti content on
the acoustic impedance of epoxy composites was also
tested.

0167-577X/$ - see front matter D 2003 Elsevier B.V. All rights reserved.
doi:10.1016/S0167-577X(03)00435-X
 F. El-Tantawy, Y.K. Sung / Materials Letters 58 (2003) 154–158
2. Experimental work
With the above aim in mind, the polymer used in this
investigation was a commercial epoxy resin (type 828) and
hardener (type B002W) supplied by (Yuka shell epoxy
chemical, Tokyo, Japan). A stoichiometric resin/hardening
ratio 100:20 by weight was used according to the manu-
facturer’s data sheets. Titanium powder with particle size 20
Am was used as reinforcing and attenuation scattering agent.
Glycerol (Gly, analytical grade) and g-glycidoxy propyl
trimethoxy silane (A-188) were used as the plasticizer and
coupling agent, respectively. The amount of glycerol was 15
wt.% and silane was 2 wt.% in the composite. Several
batches of epoxy – Ti weight ratios were considered:
99.8:0.2, 99.6:0.4, 99.4:0.6, 99.2:0.8 and 99:1, respectively
and abbreviated as Ti1, Ti2, Ti3, Ti4 and Ti5, respectively.
The green epoxy-hardener with different content of filler
was prepared by centrifuging mixer for 2 min at room
temperature. The bulk samples of composite were obtained
by casting the green composites on alumina mould and
placed in an electrical oven that was preheated to 60 jC for
30 min. Then, the epoxy-filler composites were cured under
hot uniaxial pressure 150 KN/m2 at 100 jC for 2 h.
Morphology study of the epoxy composites was conducted
on Scanning Electron Microscopy (SEM, JSM-5310 LVB,
JEOL). The molar volume of the composites (Vm) was
measured by a pycnometer using a mixture of carbon
tetrachloride and toluene as a medium [2]. Before the
measurements were made, the specimens were cut into
fragments and vacuum dried for 1 day. The mechanical
properties of the epoxy composites were measured using an
Instron materials testing machine. The samples were pre-
pared according to ASTM DIN53557 standard [1]. The
dielectric properties of the composites were measured at
frequency 1 kHz by using RLC Bridge (3541 Y-Hitester,
Hioki, Japan). Silver paste was used to ensure a good
contact of the sample surface with copper electrodes. The
glass transition temperature (Tg) and specific heats (Cp) are
measured by differential scanning calorimeter as described
elsewhere [2]. Viscosity (g) was measured by viscometer
model (VM-A, Japan). Surface tension (ST) was measured
by using a surface tension-meter model (GPYP-A3, Japan).
The ultrasonic measurements were performed using an
ultrasonic flaw detector of type Krautkramer-Branson
USD-10. The adopted technique is the pulse-echo immer-
sion technique [2]. The tested sample was sandwiched
between two piezoelectric ceramics operating at about
8 MHz used as transducer. Sound velocity was determined
with reference to its velocity in distilled water at 20 jC
(1483 m/s). The accuracy of the sound velocity was esti-
mated to be better than 0.3%. The sound velocity in water
(in m/s) was found to vary with the absolute temperature (T)
according to linear relation in the form:
Vw
2:55T þ 2230 ð1Þ
155
3. Results and discussion
3.1. Network structure and mechanical properties of the
composite
Knowledge of the network structure and mechanical
properties of thermosetting resins is essential in order to
be able to choose a proper set of processing parameters and
type of fillers, which give good material properties. The
SEM was used to investigate the morphology of the cured
epoxy – Ti composites. Fig. 1a presents the SEM for sample
Ti5 of epoxy composites. It is shown that the Ti particles are
homogeneously distributed and sink into the porous epoxy
matrix. Closer inspection shows that there is big amount of
epoxy matrix adhered and Ti particles are coated by an
epoxy resin, indicating a strong interface within epoxy
composites. The cross-link density (CLD) = qE NA/Mw,
where qE is the density of epoxy, NA is Avogadro’s number
and Mw is the molecular weight between cross-link’s. The
extent of filler reinforcement (g) is given by: Vr0 /
Vrf = 1
c(f/1-f), where Vrf is the volume fraction of
swollen epoxy in the fully swollen filled sample and f is
the volume fraction of Ti. The dependence of cross-linking
density, extent of filler reinforcement and molar volume
(Vm) on Ti content of epoxy composites is shown in Fig. 1b.
It is observed that the CLD, c and Vm increase linearly and
strongly depend on the Ti content. The reason is considered
to be due to the chemical cross-linking to increase the
entanglement contribution in the network structure of epoxy
composite. It is worthy that the positive value of c refers that
a reinforcing filler has good polymer –filler interaction. This
implies that Ti acts as a reinforcing effect and reacts with
epoxy molecules and increases the interfacial adhesion
within epoxy composites as confirmed by the glass transi-
tion (Tg), viscosity (g), surface tension (ST) and packing
factor PF = qb/qt (where qb and qt are the particle bulk and
true densities, respectively). The results shown in Fig. 1c
relate to the effect of Ti content on the Tg, g, ST and PF of
epoxy composites. It is found that Tg, g and PF increase with
increasing filler content in the epoxy composites. The
increase in Tg is most likely due to the increase of cross-
linking density [8]. The viscosity and packing factors
support this claim; a greater cross-link density tends to
correlate with less free volume into epoxy composites.
Indeed, the surface tension increases remarkably with in-
creasing Ti content due to the increase of the action force
among the epoxy chains and cross-link reaction of the
epoxy. Therefore, the filler and matrix might reach the good
wettability. Considering this observation, it is reasonable to
believe that the adhesive force among filler and matrix
increases, and hence there is a molecular structural change.
However, the mechanical properties of epoxy composites
were examined in order to figure out and understand how
the Ti particles influenced the performances of epoxy
matrix. Fig. 1d presents the plots of the breaking strength
(Eb), Young’s modulus ( Ym), hardness (shore A) and frac-
156 F. El-Tantawy, Y.K. Sung / Materials Letters 58 (2003) 154–158

Fig. 1. (a) SEM photographs for sampleTi5, (b) Cross-linking density, extent of filler reinforcement and molar volume as a function of Ti content of epoxy
composites. (c) The relationship between Tg, g, ST, PF and Ti content of epoxy composites. (d) Breaking strength, Young’s modulus, hardness and fracture
toughness as a function of Ti content for epoxy composites.

ture toughness Tg = 0.0824( P/C1.5) where P is the indenta-
tion load and C is the crack length, as a function of Ti
content for epoxy composites. It is seen that all the me-
chanical property improves as the Ti content increases in the
composite. This indicate that the Ti particles acts as a
reinforcing agent as confirmed by network structure results
before. The breaking strength increases with increasing Ti
particles. This is ascribed to a good ductility of epoxy matrix
and a strong interphase adhesion between Ti and epoxy
matrix. Also, it is seen that Young’s modulus increases with
an increase in a Ti content in the composites. This is
attributed to the integrated interfacial bonding and good
wettability between filler and matrix due to the higher
surface area of the Ti particles. In the author’s opinion,
the fracture toughness in these composites is due to the
generic characteristics of plasticizer and coupling agent
modified epoxy resin: the higher the plastic deformability
and the lower the crack pinning, the greater the fracture
toughness. Thereby, we conclude that the plastic deform-
ability of bulk epoxy adhesive was enhanced with inclusion
of filler, plasticizer and coupling agent. Lastly, the hardness
increased with increasing Ti content. The reasons are that Ti
particles reduced the creep of epoxy matrix and therein led
to enhance the network structure stability within the epoxy
matrix. This result provides another indication that the
dispersed particles within the epoxy matrix are easily dis-
placed under the applied load at low Ti content.
3.2. Temperature dependence of longitudinal wave velocity
and attenuation
The ultrasonic parameters like longitudinal velocity and
attenuation of polymer are strongly affected by their net-
work structure, and thereby the measurement of these
parameters can provide useful information about the mod-
ification of the architecture of molecular structure when the
filler, temperature, pressure or frequency of the simulation
changes. The longitudinal sound velocity (V) and attenua-
tion (a) was calculated by the following equations [7,8]:
2LVw
VE ¼ ð2Þ
ð2L
Vw ðt1
t2 ÞÞ
 
qw Vw q VE 1
expð
2aE LÞ ¼ Rð
2Law Þ þ E þ ð3Þ
4qE VE 4qw Vw 2
 F. El-Tantawy, Y.K. Sung / Materials Letters 58 (2003) 154–158 157

where the subscripts E and w stand for epoxy and water,

respectively, L is the specimen thickness, t1 and t2 are the
times of flight of ultrasonic waves in a round trip with the
specimen removed and immersed, respectively, qw is the
density of water and R is the ratio of the received amplitudes
when the sample removed and immersed.
The variation of ultrasonic velocity and attenuation on
temperature for epoxy composites is presented in Fig. 2a
and b, respectively. It is seen that the ultrasonic velocity
and attenuation value increase with increasing Ti content
in the epoxy composites. This is ascribed to the strong

Fig. 2. (a) The variation of ultrasonic velocity on temperature for epoxy

composites. (b) The variation of attenuation on temperature for epoxy Fig. 3. (a) The attenuation versus frequency for epoxy composites. (b) The
composites. (c) The variation of a, Cp, Ka and Ki as a function of Ti content acoustic impedance, dielectric constant and dissipation factor versus Ti
for epoxy composites. content for the epoxy composites.
158 F. El-Tantawy, Y.K. Sung / Materials Letters 58 (2003) 154–158
adhesion force between neighboring chains and filler
matrix interactions into epoxy matrix. On the other hand,
the ultrasonic velocity and attenuation decrease with
raising temperature. This ascribed to the dilatation effect
due to the increases of the thermal expansion of epoxy
chains at high temperature. The temperature coefficient of
ultrasonic velocity b=(
1/V)(DV/DT), as a function of Ti
content is plotted in Fig. 2c. The adiabatic compressibility
Ka=(qcV2s )
1 and the isothermal compressibility Ki =
Ka + Tqch2/Cp, where Cp is the specific heat of the
composite. The values of Cp as a function of Ti content
are plotted in Fig. 2c. It is seen that the Cp increases with
increasing Ti content. This is another clue confirming that
the inclusion of Ti particles enhances the network struc-
ture and thermal stability of epoxy matrix. However Fig.
2c presents the variation of b, Ka and Ki as a function of
Ti content. In Fig. 2c, it is clearly that b decreases while
Ka and Ki increases with increasing Ti content in the
composite. The decrease of b and increases of Ka and Ki
gives an indication of good interface adhesion between
epoxy and Ti in the composite. As the temperature is
raised, the expansion of epoxy is restricted by the Ti
phase, which has lower b, resulting in a decrease of
overall b in the composites. This suggested again that
the incorporation of Ti particles enhances the thermody-
namic stability and molecular structure of epoxy matrix as
confirmed before.
3.3. Applicability of composites in ultrasonic backing
To test the applicability of epoxy composites for ultra-
sonic backing application, the attenuation and acoustic
impedance was investigated. Fig. 3a represents the atten-
uation versus frequency plot for neat epoxy and epoxy –Ti
composites. It is seen that there is a considerable increase
in attenuation with increasing the frequency. This is
ascribed to the cross-linking density and the contribution
of Ti particles to acoustic scattering and multireflecting
within porous epoxy matrix. Also, the increment in atten-
uation with increasing Ti content can be accounted for by
the interactions involving the epoxy and the Ti phases. The
attenuation values are very high thus making the epoxy –Ti
composites very useful for attenuation backing applications
[4,6]. To obtain more information about the applicability
for backings, the acoustic impedance as a function of Ti
contents were computed. The relationship between the
acoustic impedance Z = Vqc as a function of Ti concentra-
tion is plotted in Fig. 3b. The increase in acoustic
impedance with addition of Ti is due to the increase in
the chain connectivity and interfacial polarization associ-
ated with Ti particles. This fact is also supported by
dielectric properties that has resulted. The variation of
the dielectric constant (e) and dissipation factor (tan d)
with Ti content are shown in the same Fig. 3b. Both the
dielectric constant and dissipation factor increases with
increasing Ti content in the epoxy composites. One pos-
sible reason for increase e and tan d is considered to be the
reduction of average distance between Ti particles. Fur-
thermore, the average interfacial polarization associated
with a cluster of Ti particles is coarser than that of an
individual particle because of the increase in the dimen-
sions of the metallic inclusion within epoxy matrix.
4. Conclusions
(1) The porous epoxy, Titanium, Silane coupling agent and
plasticizer composites has been fabricated for transducer
attenuation backing applications. The macromolecular
network of epoxy resin is modified considerably by the
inclusion of Ti powder, coupling agent and plasticizer as
confirmed by network structure and mechanical ana-
lyzes.
(2) The ultrasonic sound velocity and the attenuation
decrease with raising temperature due to the dilatation
effect of the epoxy matrix.
(3) The attenuation increases with increasing Ti content and
frequency in porous epoxy composites. Also, the
acoustic impedance increases with increasing Ti content.
The high attenuation and acoustic impedance values
reflect that the porous epoxy –Ti composites are useful
for transducer backing applications.
Acknowledgements
This research was supported by Dongguk University,
Department of Chemistry, Seoul, Korea.
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