Japanese Journal of Applied Physics 51 (2012) 07GB11 BRIEF NOTE

DOI: 10.1143/JJAP.51.07GB11

Effect of Focused Ultrasound on Residual Particle Size Distribution in Water

Jungsoon Kim, Moojoon Kim1
, Misun Jo1 , and Mincheol Chu2
Media Engineering, Tongmyong University, Busan 608-711, Korea
1
Department of Physics, Pukyong National University, Busan 608-737, Korea
2
Korea Research Institute of Standard and Science, Daejeon 305-340, Korea
Received November 17, 2011; accepted January 23, 2012; published online July 20, 2012

The residual particle distribution in pure water could be a problem in the nanoscience fields because nanoparticles are usually suspended in pure
water such as deionized or distilled water. The effect of ultrasound on the residual particle distribution in pure water should be analyzed because
the nano particles used in nanoscience are usually dispersed using ultrasound power. In this study, using a cylindrical piezoelectric vibrator, a
noncontact-type focusing ultrasound system was fabricated to keep the purity of the water. The residual particle distribution in pure water was
investigated. The number of residual particles increased as the ultrasound exposure time increased.
# 2012 The Japan Society of Applied Physics

Residual nanosize particles have been reported even in pure

water such as distilled water. Even though many studies
about these particles are being carried out, the reasons for
their existence and their treatments have not been clarified
yet.1,2) In the application fields of synthesized nanoparticles,
the residual particle distribution in water contributes to
problems in evaluating the dispersion state of nanoparticles.
It is hypothesized by LaFranchi et al.3) that water pH and
the storage container of water affect the residual particle
distribution. However, the basis of this hypothesis has been
undefined. On the other hand, the change in water pH
associated with the collapse of ultrasonic cavitation has been
noted in many reports.4–6) As reported in the literature, water
pH can be reduced to 4.0 by ultrasonic cavitation. Therefore,
in this study, to change water pH without adding acid to
maintain the purity of water, a focused ultrasound was
irradiated into pure water, and the effect of water pH on
residual particle distribution was investigated.
The primary mechanism underlying the synthesis of nitric
acid induced by ultrasound is as follows.7) Pure water
involves the H and OH radicals. Atomic nitrogen and
oxygen can be produced at high temperatures and pressures
caused by ultrasonic cavitation, and nitrogen fixation can
occur in cavities, as shown in the following reactions.
N2 ! 2N; O2 ! 2O; N þ O ! NO:
Nitric oxide can be converted to nitrous acid with the OH
radical from water.
OH þ NO ! HNO2 :
HNO2 is the major acid component formed during ultrasonic
cavitation. On the other hand, very small amounts of nitric
oxide could be readily converted to NO2 by its reaction with
atomic oxygen produced during the ultrasonic cavitation.
NO þ O ! NO2 :
NO2 can be converted to nitric acid in a reaction similar to
that shown in eq. (3).
OH þ NO2 ! HNO3 :
From these processes, even pure water can have acid.
To produce a focused ultrasound field, an experimental
system was fabricated using a cylindrical piezoelectric
transducer, as shown in Fig. 1. A glass tube at the center


E-mail address: kimmj@pknu.ac.kr
Fig. 1. (Color online) Schematic of ultrasonic cavitation-generating
system.
of the cylindrical transducer was used because the ultrasonic
field can be focused in a noncontact manner. The cylindrical
vibrator has an inner radius of 38.5 mm, an outer radius of
46.5 mm, and a height of 19.2 mm. The vibration mode of
the vibrator is approximately the mode of thickness between
the inner surface and the outer surface because the
polarization is in the radial direction. A tungsten tube filled
with cooling water was inserted between the transducer
and the glass tube because the ultrasonic field from the
ð1Þ
transducer can be transferred to the glass tube by the cooling
water. To prevent the piezoelectric transducer from heating
up, the cooling water was circulated by a water pump. The
thicknesses of the glass tube and tungsten tube were 0.3 and
ð2Þ
0.5 mm, respectively. They were chosen to be thin enough to
be effective for the ultrasound. Deionized water (DI water)
and distilled water were circulated through a plastic tube
connecting the glass tube to a water pump. The piezoelectric
transducer has a resonant frequency of 480 kHz, and it was
driven at this frequency. DI water was generated with a
ð3Þ
Barnstead Nanopure system (Model D1794).
Purified water and cooling water were circulated at flow
rates of 3.0 and 1.5 mL/s, respectively. The piezoelectric
transducer was driven by a power amplifier at 120 W. The
ð4Þ
ultrasound wave from the transducer was focused on the
center of the glass tube filled with purified water. The size
distribution of residual particles in water was measured
using the particle counter CPC 5.403 (GRIMM Aerosol
Technik) with an aerosol generator and a disperser (TSI).
The measurements were performed five times for each
sample. To obtain precise data, the first and last measure-
07GB11-1 # 2012 The Japan Society of Applied Physics
Jpn. J. Appl. Phys. 51 (2012) 07GB11
8.0
7.5
7.0
6.5
pH
6.0
5.5
5.0
4.5
4.0
0 5 10 15
Time [min]
Fig. 2. Changes in pH in distilled water with ultrasound exposure time.
Distilled water
6000
5000
Particles (dN [/cm ])
3
4000
3000
2000
1000
0 before the ultrasonic irradiation. Similarly to the results for
10
Particle size [nm]
Fig. 3. Changes in particle distribution with ultrasonic exposure time in
distilled water.
ments were abandoned. Prior to the experiment, all the
containers and equipment such as the water pump, plastic
tubes, glass tube, and beakers were rinsed carefully. We
confirmed that their impurity did not have any significant
effects on the distribution of the residual particles in the
waters.
To confirm the ultrasonic effect on the pH of pure water,
the pH was measured for different ultrasound exposure
times, as shown in Fig. 2. In this figure, the pH of distilled
water decreased with ultrasound exposure time. In a given
range, the pH was 5.0 at 30 min of insonation. This
decreasing tendency is in agreement with a previous study.5)
The pH of the ideal distilled water should be 7. However,
practically, the pH of distilled water was slightly lower than
pH 7 because the interaction of distilled water with the
atmosphere dissolves carbon dioxide into water, forming
carbonic acid. It is the reason why the initial pH was 6.5 in
this study.
To investigate the effect of ultrasound, the particle size
distribution in distilled water was measured using different
ultrasound exposure times, as shown in Fig. 3. In this figure,
the y-axis denotes the number of particles per unit volume.
Each distribution was measured three times on average. The
results shown in Fig. 3 reveal that the residual nanoparticles
are distributed even in distilled water. In this figure, the solid
line shows the particle distribution of distilled water without
ultrasound, and the peak was observed to be in the range of
10–20 nm. This distribution is in agreement with those
reported in the literature.1,2) When the focused ultrasound
was irradiated, the peak moved to be in the range of 20–
30 nm. The particle number of each distribution increased
J. Kim et al.
DI water
6000
5000 0 min
Particles (dN [/cm ])
3
10 min
4000 20 min
60 min
3000
2000
1000
0
10 100
Particle size [nm]
20 25 30
Fig. 4. Changes in particle distribution with ultrasonic exposure time in
DI water.
with ultrasound exposure time. It can be confirmed that
particle increment due to the ultrasound is the maximum at
0 min
40 nm approximately when the exposure time is shorter than
10 min 30 min from this result. However, in the case of 60 min
20 min
60 min
exposure, the maximum of the particle increment is at a
particle size of 25 nm. The results for DI water are shown in
Fig. 4. The residual particles in DI water are distributed in
the particle size range smaller than that in distilled water
100
distilled water, the peak of particle number moved to a
particle size of approximately 20 nm, and particle number
increased over the whole range after the focused ultrasound
irradiation. The increment in particle number due to the
ultrasound is considered that the ultrasound irradiation
generated nitric acid, and which changed water pH.5) From
the literature,3) adding nitric acid to distilled water increases
the number of residual particles in water, which is in
agreement with the results of this study. Leaching of the
residual particles from the container walls owing to the
acidity of water has been considered the reason for this
increase.3) From the results shown in Figs. 3 and 4, it is
noted that the distribution shapes are similar for each
exposure time in each result even though the value and the
peaks are changed by the ultrasound. It is considered that the
distribution change caused by the ultrasound depends on the
original distribution of the residual particles.
The effects of a focused ultrasound field on the residual
particle distribution in the DI/distilled water were investi-
gated. The particle size distribution was measured at various
ultrasound exposure times. The number of residual particles
increased because of the change in water pH ultrasound
exposure time increased. This study will be useful for the
analysis of the distribution of suspended nanoparticles used
in industrial fields.
Acknowledgment This work was supported by the Pukyong National
University Research Abroad Fund in 2011 (PS-2011-006).
1) J. Krames, H. Buttner, and F. Ebert: J. Aerosol Sci. 22 (1991) s15.
2) J. Ho, B. Kournikakis, and A. Gunning: J. Aerosol Sci. 19 (1988) 1425.
3) B. LaFranchi, M. Knight, and G. Petrucci: J. Aerosol Sci. 34 (2003) 1589.
4) F. Young: J. Acoust. Soc. Am. 60 (1976) 100.
5) S. Koda, K. Endo, Y. Kojima, and H. Nomura: Kagaku Kogaku Ronbunshu
25 (1999) 290 [in Japanese].
6) T. Uchida, T. Kikuchi, T. Aoki, N. Kawashima, and S. Takeuchi: Jpn. J.
Appl. Phys. 48 (2009) 07GH03.
7) E. Mead, R. Sutherland, and R. Verrall: Can. J. Chem. 54 (1976) 1114.
07GB11-2 # 2012 The Japan Society of Applied Physics