Role of a nanoparticle on ultrasonic cavitation in nanofluids

Zaiwei Liu1, Chunhui Ji1 ✉, Bing Wang2, Shuangqiu Sun1

1
Key Laboratory of Advanced Ceramics and Machining Technology, Ministry of Education, Tianjin University, Tianjin,
People’s Republic of China
2
George W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, GA 30332-0405, USA
✉ E-mail: [email protected]

Published in Micro & Nano Letters; Received on 12th January 2019; Revised on 21st March 2019; Accepted on 13th May 2019

Ultrasonic cavitation in nanofluids improves material removal rate and surface quality. Ultrasonic cavitation in nanofluids was investigated
using molecular dynamics simulations. The formation and growth of nanobubbles were promoted, by nanoparticles in water systems.
Three distinct impact stages were observed which were caused by the impact of the shock wave, nanojet and nanoparticle. These differed
in the system without a nanoparticle. The material removal rate was primarily caused by the nanoparticle hit, a result of the nanobubble
collapsing during the third impact. A mechanism of material removal in ultrasonic polishing is discussed at a nanometric level.

1. Introduction: Cavitation is the phenomenon in which the 2. Formation of cavitation bubbles in nanofluids: The all-atomic
pressure on a liquid is decreased causing the liquid to rupture and model was used to study the evolution of nanobubbles in a
form bubbles [1]. Ultrasonic polishing involves an ultrasonic vibra- nanofluid. The size of the MD system was 10 × 10 × 10 nm3, and
tion generator to be accelerated away from a solid surface creating a the periodic boundary condition was applied in the x-, y- and
negative pressure which eventually produces a vacuum, resulting in z-directions. The water system contained ∼32,201 water molecules,
the formation of micro and nanobubbles in the abrasive suspension. and the nanoparticle system contained 31,864 water molecules and
When the generator approaches the solid surface, the cavitation one 2 nm diameter SiO2 nanoparticle. The previously described
bubbles collapse instantly resulting in a nanojet, strengthening TIP4P/2005 water model was used to represent interactions
abrasive particle movement, pushing them into cracks or pits on between atoms in a water system [16]. The Tersoff potential [17]
the solid surface, hence improving material removal rate and was used to represent interactions between atoms in SiO2 nano-
surface quality [2–5]. particles. The Lennard–Jones (LJ) potential [18] was used to
Recently, ultrasonic cavitation was used as a finishing technique represent interactions between atoms in H2O and SiO2, and the
improving the surface roughness Ra of Inconel 625 side surfaces parameters were determined using the Lorentz–Berthelot mixing
by ∼45% after a processing time of 30 min [6]. The magnitude rule [19]. The particle–particle particle-mesh solver [20] was used
and distribution of the impact of hydrodynamic pressure generated to compute long-range Coulomb interactions and long-range 1/r 6
from the implosion of cavitation bubbles close to the rigid boundary interactions.
have been investigated, and found that high-velocity micro-jets The LJ potential is described as follows:
(200–700 m/s) were produced when the bubble collapses [7]. ⎡

6 ⎤
12
Shock-induced collapse of nanobubbles in water using molecular s s ⎦
dynamic (MD) simulations [8], damage caused by nanobubble U (rij ) = 41⎣ − (1)
rij rij
collapse in water near the silica surface using billion-atom reactive
MD simulations [9], and the mechanism determining membrane
porosity as a result of nanobubble collapse through performing where ɛ and σ are the energy parameter and length scale, respective-
coarse-grained (CG) MD simulations [10] have all been investi- ly, and rij is the intermolecular distance between atoms i and j.
gated. In addition, Nair et al. [11] enhanced the tribological The LJ parameters calculated using the mixing rule are shown in
properties through encompassing the micro and nanoparticles in Table 1.
sesame oil, and Kalyanasundaram and Molian [12] improved the The Lorentz–Berthelot mixing rule is described in the following
tribological properties through depositing nanodiamond particles equation:
on aluminium alloy A319. Also, Wu et al. [13] found that the 
MD simulations well revealed the notch sensitivity of nano- 1ij = 1ii 1 jj
crystalline Cu. sii + s jj (2)
Despite extensive research reported in the literature investigating sij =
2
ultrasonic cavitation, particularly with respect to bubble collapse,
the cavitation produced by ultrasonic polishing is indistinguishable The MD system was initially equilibrated in the (N, P, T ) ensemble
from the particle effect. The introduction of particles has been (T = 298 K, P = 1 atm) using a Nosé–Hoover thermostat and
reported to alter the motion of cavitation bubbles. The bubbles barostat [21], and the pressure of equilibrated system was then
collapsing accelerate the particles, thereby impacting and eroding changed to −1500 atm. Fig. 1 compares the evaluation of cavitation
the surface layer via ploughing and cutting mechanisms [14, 15]. bubbles in the water system with and without a nanoparticle. Fig. 2
In the ultrasonic polishing process, the effect of the nanoparticles shows the average volume of water molecules at different times.
on the formation and collapse of a nanobubble is unknown. How Under negative pressure, many cavities formed with fluctuating
the nanoparticle is accelerated by the nanobubble collapse and volumes caused by the rapid growth and disappearance of the
how the solid surface is impacted by the shock wave, nanojet holes in the metastable water. Once the cavitation reached critical
and nanoparticle is also unknown. In this study, MD simulations size, the water system became unstable and a nanobubble formed
were used to further understand the nanobubble/nanoparticle which grew rapidly. A nanobubble was formed in the nanofluid
interactions. on the interface of nanoparticle and water system, which is

Micro & Nano Letters, 2019, Vol. 14, Iss. 10, pp. 1041–1045 1041
doi: 10.1049/mnl.2019.0033 & The Institution of Engineering and Technology 2019
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Table 1 LJ parameters of SiO2/Si and H2O

Parameter ɛ (eV) σ (nm)

Si–Si(SiO2/Si) 0.001735 4.0534

O–O(SiO2) 0.009886 2.8598
O–O(H2O) 0.008030 3.1589

Fig. 3 Representation of a water system with a nanoparticle

Fig. 1 Cavitation bubbles in a water system with and without one SiO2
nanoparticle

Fig. 4 Bubble collapse in water with a nanoparticle

Fig. 2 Average volume of water molecules at different times

consistent with the reported results investigating heterogeneous nu-

cleation as a result of a microscopic air pocket on a nanoparticle in
liquid [22].

3. Collapse of the cavitation bubble in nanofluid: To model a

larger MD system, the CG water model was used in which the
four water molecules were modelled as one particle [10]. The Fig. 5 Variation in force impacting the silicon wafer

1042 Micro & Nano Letters, 2019, Vol. 14, Iss. 10, pp. 1041–1045
& The Institution of Engineering and Technology 2019 doi: 10.1049/mnl.2019.0033
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all-atom model was used to model the SiO2 nanoparticle and silicon
wafer. Fig. 3 shows the MD model, 100 × 100 × 120 nm3 in size and
includes 8,002,357 CG water particles. The 1 nm thick silicon
wafer was modelled as a rigid body to reflect the impact of nano-
bubble collapse in the water system. To create the cavitation
bubble, 95% CG water particles with a radius of 30 nm were
deleted after relaxation for 10 ps under (N, P, T ) ensemble
(T = 298 K, P = 1 atm). Then one 20 nm diameter SiO2 nanoparticle
was placed in the bubble in an optimal position, as shown in Fig. 3.
The periodic boundary condition was applied in the x- and
y-directions, and the non-periodic condition was applied in the
z-direction to define the shock wave.
Similar to the above definitions, Tersoff potential was used to
represent interactions between the atoms in the SiO2 nanoparticle
and silicon wafer. In addition, the Morse potential was used to
describe particle–particle interactions in the water model [23],
different to that of the TIP4P/2005 water model. The LJ potential
was used to represent the interactions between the particle in CG
water and the atoms in SiO2 or silicon, and the parameters were
Fig. 6 Stress distribution in the water system, observed in the X–Z plane calculated using the mixing rule. The LJ parameters of the CG
water particles as defined by CG MARTINI force field are
5 kJ/mol (ɛcg) and 0.47 nm (σcg) [24].
The momentum mirror method was used to generate a shock
wave in the z-direction. Therefore, if an atom moves such that it
is outside the wall on a time step by distance, then it returns
inside the face at the same distance, and the velocity relative
to the moving wall is flipped in the z-direction. For example,

Fig. 8 Sketch of slice and centre regions in the water system

Fig. 7 Stress distribution in the water system close to the silicon wafer,
observed in the X–Y plane (shown in Fig. 8) Fig. 9 Velocity distribution of the water system, observed in X–Z plane

Micro & Nano Letters, 2019, Vol. 14, Iss. 10, pp. 1041–1045 1043
doi: 10.1049/mnl.2019.0033 & The Institution of Engineering and Technology 2019
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the piston velocity vp and particle velocity before reflection vz, then Fig. 5 shows the variation in force impacting the silicon wafer.
the particle velocity after reflection is −vzi + 2 × vp [25]. In this It can be observed that the whole impact process can be divided
study, the velocity of the piston was fixed at 1.5 km/s and the into three stages, in which the impact force of the second
moving distance fixed at 15 nm. Therefore, the velocity of the stage was the largest (< 5.4 × 104 nN), and the smallest impact
shock wave generated was ∼3 km/s, but weakened as the wave was produced during the first stage. In order to understand the
propagated. impact process, the distribution of stress in the water system
Fig. 4 shows the collapse process of the nanobubble in a water at the moment of impact is shown in Fig. 6. The first impact
system with a nanoparticle. The propagation of the shock wave was produced by a small part of the nanojet which bypassed
was observed using colours to indicate water particle velocity. the nanoparticle. The second impact was caused by a combination
A shock wave, created using the momentum mirror method, and of water particle movement driven by the nanoparticle movement
cavitation bubble came into contact – the bubble collapsed instantly and the shock wave created by the momentum mirror method.
and energy was released which produced a nanojet. When the The third impact was produced by the direct hit of the nano-
nanojet reached the nanoparticle, most of the nanojet increased particle on the silicon wafer. The three stress waves caused by
the nanoparticle movement and a small amount bypassed the the three impacts on the silicon wafer can be clearly seen in
nanoparticle. Figs. 7 and 8.
Fig. 9 shows the velocity distribution of the water system
observed in the X–Z plane. The stationary nanoparticle was initially
impacted by the nanojet at high energy, and the outer water particles
of the nanojet directly impacted the silicon wafer by bypassing the
nanoparticle. At the same time, the nanoparticle moved and the
water molecules in front of nanoparticle impacted the silicon
wafer until the nanoparticle hit the silicon wafer, with a velocity
of ∼0.85 km/s.
To investigate the effect of the presence or absence of the nano-
particle on bubble collapse, the collapse process of a nanobubble in
water without a nanoparticle was simulated. Fig. 10a shows the
force impacting the silicon wafer. Unlike the water system with a
nanoparticle, two distinct impacts can be observed in water
without nanoparticle, with a maximum force of ∼4.9 × 104 nN,
which is smaller than that observed in water with a nanoparticle.
Furthermore, the impacts were produced earlier due to the
absence of a nanoparticle. Figs. 10b and c show the stress distribu-
tions in the water system at different stages of impact. The two
impact stages induced by the nanojet can be observed, and the
stress distribution was concentrated on the silicon wafer when com-
pared to the system with the nanoparticle.
Fig. 11 compares the variation in force impacting the centre
region (2 × 2 nm2, Fig. 8) of the silicon wafer in a water system
without the nanoparticle and with one 2 nm nanoparticle. It can
be observed that for the system with a nanoparticle, the nanoparticle
hit the silicon wafer during the third stage and the impact on
the centre region was significantly greater compared to the other
stages. The water system without a nanoparticle had the
maximum impact produced by the nanojet, which was significantly
smaller than that in the nanofluid. This indicates that the polishing
effect was enhanced due to the presence of the SiO2 nanoparticle.

Fig. 10 The effect of cavitation on the silicon wafer

a Variation in the force impacting the silicon wafer Fig. 11 Force impacting the centre region of the silicon wafer in water with
b, c Stress distribution of the water system without a nanoparticle one 20 nm diameter nanoparticle

1044 Micro & Nano Letters, 2019, Vol. 14, Iss. 10, pp. 1041–1045
& The Institution of Engineering and Technology 2019 doi: 10.1049/mnl.2019.0033
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51375334) and the Natural Science Foundation of Tianjin City
(grant no. 18JCYBJC19800).

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Micro & Nano Letters, 2019, Vol. 14, Iss. 10, pp. 1041–1045 1045
doi: 10.1049/mnl.2019.0033 & The Institution of Engineering and Technology 2019