Accepted Manuscript

Microstructural evolution in ultrafine grained Al-Graphite composite synthesized via

combined use of ultrasonic treatment and friction stir processing

R. Rajeshkumar, V. Udhayabanu, A. Srinivasan, K.R. Ravi

PII: S0925-8388(17)32665-8
DOI: 10.1016/j.jallcom.2017.07.280
Reference: JALCOM 42696

To appear in: Journal of Alloys and Compounds

Received Date: 26 December 2016

Revised Date: 6 June 2017
Accepted Date: 27 July 2017

Please cite this article as: R. Rajeshkumar, V. Udhayabanu, A. Srinivasan, K.R. Ravi, Microstructural
evolution in ultrafine grained Al-Graphite composite synthesized via combined use of ultrasonic
treatment and friction stir processing, Journal of Alloys and Compounds (2017), doi: 10.1016/
j.jallcom.2017.07.280.

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Microstructural Evolution in Ultrafine Grained Al-Graphite Composite Synthesized via

Combined Use of Ultrasonic Treatment and Friction stir processing

R. Rajeshkumar1, V.Udhayabanu2, A. Srinivasan3 and, K.R.Ravi1,

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PSG Institute of Advanced Studies, Coimbatore, India

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2
Viswesvaraya National Institute of Technology, Nagpur, India
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National Institute for Interdisciplinary Science and Technology, Trivandrum, India

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Corresponding author: krr@psgias.ac.in

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Abstract
An attempt was made to develop ultrafine grained Al-Graphite composites through friction stir

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processing (FSP). Al-Graphite composite was initially prepared using stir casting technique and
it subsequently subjected to ultrasonic treatment prior to solidification. The results showed that
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the ultrasonic treatment during the composite preparation reduced the porosity, graphite
particles’ agglomeration and the graphite particles’ size in the composite. The ultrasonic treated
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Al-Graphite composite was subjected to a single pass FSP at a constant tool rotational speed of
1600 rpm with three different feed rates, of 20 mm/min, 40 mm/min and 60 mm/min. The
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microstructure of FSPed composites within the stir zone exhibited a fine recrystallized grain
structure due to the combined effect of severe plastic deformation and frictional heat generation
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during FSP. After the single pass of FSP, the grain size of the composite was reduced from 150
µm to 14 µm, 6 µm and 0.5-1 µm for the tool transverse speeds of 20 mm/min, 40 mm/min and
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60 mm/min, respectively. Distribution of graphite particles in Al matrix was significantly

improved after FSP process due to the strong stirring action of the rotating tool. Most
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importantly, microstructural analysis suggested that a substantial reduction in graphite particles’

size could be achieved with the aid of FSP process. FSPed Al-Graphite samples exhibited
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superior hardness as compared to the unprocessed composites due to the uniform dispersion of
fine graphite particles in ultra-fine grain structure. In a nutshell, ultrafine grained Al-Graphite
composites with uniform dispersion of Graphite nano particles were produced using a single pass
FSP process.

Keywords: Ultrasonic treatment; FSP; Severe plastic deformation; Hardness; Recrystallization.

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1. Introduction
Metal Matrix Composites (MMC) are one of the noteworthy novel class of materials which
exhibit superior mechanical properties such as higher stiffness and hardness, good wear and
erosion resistance [1]. Aluminum based MMCs are widely used in automobile and aircraft
applications in virtue of its high strength to weight ratio, greater stiffness, improved heat

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resistance and good tribological characteristics [2]. Presence of hard reinforcements such as SiC
in the aluminum matrix decreases the machinability and ductility of composites to a large extent

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which restricts its applications [3]. Graphite is a well-known high strength and low dense
material which can be easily deformed due to its soft nature. Hence, incorporation of graphite in

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aluminum matrix is expected to improve the ductility and toughness of the Al based MMCs
thereby their range of applications can be extended. Furthermore, the soft nature of graphite

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particles can offer an antifriction property to Al based MMCs which is essential for automobile
parts such as bearings and pistons.
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Currently, liquid metallurgy route is a preferred method for the production of Al MMCs because
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of its simplicity and lower cost. Moreover, it has the potential to scale up the technology for
large scale applications. Agglomeration of reinforcement particles is one of the main drawbacks
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associated with Al based MMCs which is hard to avoid during solidification processing of the
composites. Studies on Al MMCs suggest that the inhomogeneous distribution of reinforcement
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particles affects the mechanical properties such as strength [4-7] ductility [8, 9], fatigue [10, 11]
and fracture behavior [12, 13]. In recent times, ultrasonic treatment is reported as one of the
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effective methods to break the agglomerates of reinforcement particles and for the reduction of
porosities of MMCs [14-16]. Recently, Christy et al. [16] have reported that the ultrasonic
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treatment of Al-2vol. % graphite composites has significantly reduced the agglomerates,

porosities and the graphite particles’ size.
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Severe plastic deformation (SPD) is a promising technique to produce an ultra-fine grain

structure in materials [17-19]. An investigation on high pressure torsion (HPT) processed Al–7
wt% Si alloy reveals that the ultra -fine grain structure has been obtained with an applied
pressure of 8 GPa for 10 revolutions at room temperature [20]. It is reported that, Al-6061- 10
vol.% Al2O3 composites processing through high pressure torsion (HPT) has shown significant

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grain size reduction from ∼35 µm to ∼170 nm [21]. Ultra-fine grains with an average grain size
of 230 nm have been achieved in Al-Al2O3/B4C hybrid composites by using an accumulative roll
bonding (ARB) technique [22]. Roohollah Jamaati et al. have found that, an ARB technique on
Al/ 15 vol. % Al2O3 composites has generated nano-grains with an average size of less than 100
nm [23]. Interesting finding such that, aluminum/copper multilayered composite which was

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fabricated via ARB process exhibits Cu and Al layers with an average grain size of 50 nm and
200 nm respectively [24]. The microstructural evaluation study of Al–7Si–Mg alloy by ECAP

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process has shown ultra fine structure grains after four passes [25]. Saravanan et al. [26] have
fabricated ultra-fine grained Al-Graphite composite using equal channel angular processing

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(ECAP). Their research work on multipass (4 passes) ECAP of Al-Graphite composites has
resulted grain refinement in submicron level (300 nm). FSP is an alternate route which can be

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used to fabricate ultrafine grained material successfully [27-29]. In the past few years, numerous
aluminium alloys and their composites have been developed with ultrafine grain microstructure
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using friction stir processing [30-32]. A study of FSP on A6082 /Al2O3 composites after four
passes exhibits more uniform distribution of nano sized Al2O3 particles in ultra-fine grains of
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aluminium matrix [33]. Dolatkhah et al. have found that FSPed Al5052/SiC is attained an
ultrafine grained structure with an average grain size of 0.9 µm from an initial average grain size
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of 243 µm [34]. Previous investigations suggest that the mechanical performance of the
composites processed via FSP can be influenced by reinforced particle size, morphology and its
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distribution as well as grain size of matrix [35-36]. Thus, it is imperative to study the detailed
microstructural analysis of FSPed composites. However, the studies on FSP of Al-Graphite
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composite are rather very limited [37-39]. Moreover, the information regarding microstructural
evolution during FSP of Al-Graphite composites has not been reported in detail in the existing
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literature. Hence, the aim of the present research work is to develop an ultra-fine grained Al-
Graphite composite with uniform distribution of graphite particles through the combined use of
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ultrasonic treatment and FSP. The microstructural evolution during ultrasonic treatment and FSP
of Al-Graphite composite is also investigated.

2. Experimental Details:
Pure aluminum (99.8%, EC Grade Aluminum) and graphite powders with average particle size
of 21±4 µm were used to synthesize Al-5 vol.% graphite composite by stir casting technique.

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After adequate stirring of the melt, the preheated ultrasonic probe was dipped into the melt and
sonicated for 5 minutes. A high power ultrasonic probe (Hangzhou Success, China), made of Ti-
6Al-4V, was used to generate a 20 kHz and 2.5 kW power input for ultrasonic treatment process.
After ultrasonic treatment, the composite melt was poured into a cast iron mold having the
dimensions of 100×100×400 mm3. For comparison purpose, the composite sample without

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ultrasonic treatment was also cast.

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Samples of Al- 5 vol.% graphite composites with the dimensions of 100×100×6 mm3, were
electrode discharge machined (EDM) from the ultrasonicated sample and subjected to single FSP

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process at room temperature. FSP processing was carried with a tool made of high carbon high
chromium D3 type steel with shoulder diameter, pin diameter and pin length of 18 mm, 6 mm

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and 3 mm, respectively. A schematic diagram of FSP tool consisting of cylindrical shoulder and
a straight cylindrical pin is shown in Fig.1. A single pass FSP was carried out at a constant tool
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rotational speed of 1600 rpm with different feed rates of 20 mm/min, 40 mm/min and 60
mm/min. Microstructure of ultrasonic treated and FSPed composites were analyzed using
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polarized light optical microscope (Carl Zeiss Axio Scope A1). The size and distribution of
graphite particles in the Aluminium matrix were analyzed using Field Emission Gun Scanning
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Electron Microscopy (FESEM, Carl Zeiss, Sigma, UK) operated under Back Scattered Electron
(BSE) mode. Grain structure and size of the graphite particles in the FSP processed samples were
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analyzed using JEOL JEM 2100 Transmission Electron Microscopy (TEM) operating at 200 kV.
Samples for TEM analysis were prepared by standard methods involving mechanical grinding,
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polishing and dimpling followed by ion milling. Daksh HV100DT microhardness tester was used
for hardness analysis in the FSPed samples. A load of 200 g and a dwell time of 10 sec were
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used for measuring the hardness of the material. Minimum of 15 measurements were carried out
at every region (HAZ, Transition and Stir Zone) and the average value was reported.
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3. Results:
Fig. 2 (a) and 2(b) compare the FESEM micrographs of stir-cast and ultrasonic treated Al-
graphite composite. Microstructure of stir-cast composite shows a significant amount of porosity
along with the agglomeration of graphite particles [Fig. 2(a)]. For the processing of Al MMCs
using stir-cast technique, the molten aluminum is mechanically stirred to create a vortex, which

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draws the reinforcements together with the ambient gases into the liquid medium. Since, the
interface energy for particle/gas interface is lower than the particle/metal interface, entrapped
gases prefer to attach with reinforcement particles. This could be the possible reason for the
presence of agglomerated graphite particles in the vicinity of porosity. In the case of ultrasonic
treated composite, a uniform dispersion of graphite particles with significant reduction in

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porosity is observed [Fig. 2 (b)]. It is also noticed that (Fig. 2 b) the most of the graphite particles
in the ultrasonic treated sample are distributed at grain boundaries rather than the grain interior.

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After ultrasonic treatment, the porosities are significantly reduced and the particle clusters have
been broken considerably. In order to ensure the microstructural observation of a porosity

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reduction in ultrasonic treated composites, density measurements are made using Archimede's
principle. The density of as cast composite material increases significantly after ultrasonic
treatment from 2.61 to 2.67 g/cm3.The density measured after ultrasonic treatment is very close

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to the theoretical density of Al-5 vol.% graphite composite, 2.68 g/cm3.
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The optical micrographs of FSPed Al-Graphite composite shown in Fig.3 displays three distinct
regions namely stir, transition and heat affected zone (HAZ). It is impressive to note that, the
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width of the processed zone is varied with different transverse speeds. It can be seen that, the
width of the processed zone increases with decreasing tool transverse speeds. Among the three
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transverse speeds, the enlarged processed zone width is found with 20 mm/min. It is reported
that, the temperature distribution around the stir zone decreases with increasing tool transverse
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speeds [40]. This indicates that, at 20 mm/min, the higher temperature is generated around the
stir zone region that leads to expand the thermo mechanical affected zone and HAZ areas;
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subsequently the processed zone becomes wider. In another way, due to the increased
temperature, the stirring material is softened, hence it offers less resistance to tool movement and
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the mixing of materials is more effective, hence the extension of processed region is occurred.
Coarse strain free grains are noticed in the HAZ zone. At the same time, marginally finer and
elongated grains are observed in the transition zone. Significantly fine equi-axed grains are
observed in the stir zone. Furthermore, the extent of grain size reduction is found to be increased
with increase in the tool transverse speed. Fig. 4 displays the grain size of the Al-Graphite
composites prepared through without ultrasonic treatment and with ultrasonic treatment. The

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results revealed that, without ultrasonic vibration, the average grain size of the sample was 400
µm. Interestingly, the application of ultrasonic vibration, reduced the average grain size and it
was about 150 µm. Fig. 4 also depict the effect of tool transverse speed on grain size of FSPed
Al-Graphite composite. Under a tool transverse speed of 20 mm/min, 40 mm/min and 60
mm/min the grain size of the samples was 14 µm, 6 µm and 1 µm respectively. Since it was hard

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to distinguish the individual grains in the samples processed at 60 mm/min using optical
microscopy, the microstructural analysis of this sample was done using TEM analysis. The TEM

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results are presented in later section. The optical micrographs showing the distribution,
morphology and size of the reinforced graphite particles in different regions are presented in Fig.

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5. The particles are well fragmented and distributed homogeneously in the Al matrix in stir zone
whereas in the transition zone graphite particles are randomly distributed. The particles in the

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heat affected regions are largely segregated in the grain boundary region which is similar to the
particle distribution noticed in the ultrasonic treated material. During FSP process, rotating tool
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offers a combination of heavy extrusion and crushing effect on the processing material. Thus,
severe plastic strain is introduced in the composite material which breaks the cluster of graphite
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particles. The effect of tool transverse speed on particle size of FSPed Al-Graphite composite is
shown in Fig. 6. The increment in tool transverse speed decreased the size of the graphite
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particles respectively. The size of the graphite particles was 2.5 µm, 2 µm and 1 µm with respect
to tool transverse speed of 20 mm/min, 40 mm/min and 60 mm/min.
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In order to understand the grain structure evolution in the deformed materials TEM is a widely
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used tool. Accordingly, it was utilized to study the grain structure and reinforcement particles
size and distribution. Figure 7 shows the development of grain structure as a function of tool
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transverse speed. According to TEM analysis (Fig. 7 a and c), the materials in the processed zone
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exhibit the coarse grains with grain size greater than 1µm for the tool transverse speeds of
20mm/min and 40mm/min. The spot selected Area Diffraction (SAD) pattern supports the
formation of strain free coarse grains. Significant amount of dislocations and subgrains are
noticed (Fig. 7 b, d and e) within each grain for all the three tool transverse speeds used.

The dislocations are generated due to the difference between the coefficients of thermal
expansion of the matrix and the reinforcement particles and the strong shear force generated

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during FSP process. In the case of 60 mm/min sample, the TEM image illustrates that the
microstructure contains predominantly ultra-fine grains with high angle grain boundaries as
shown in Figure 7 (e-f). The SAD pattern obtained from the TEM analysis indicates a large
number of randomly oriented grains in Figure 7 (e-f). This can be implied that the greater shear
stress and a larger plastic deformation associated with 60mm/min can supply the sufficient

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plastic deformation that can be used to refine the grains. Another salient feature observed in the
TEM examination was the formation of grain boundary fringes in FSPed alloy. The thickness of

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the grain boundary fringes increases with the increasing tool transverse speed (Fig. 7 b,d,g).

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Bright field TEM images of FSPed samples shown in Fig.8 illustrate the influence of tool
transverse speed on the size and shape of graphite particles. It was found that the size of the

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graphite particle is greater than 1µm when FSP is performed with tool transverse speed of 20
mm/min and 40 mm/min. Conversely, in the case of sample FSPed with tool transverse speed of
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60mm/min, extremely fine graphite particles (<0.1µm) are noticed along with bigger size
particles of 1µm. Moreover, fine spherical shaped second phase particles is also present in the
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microstructure of the sample FSPed at the tool transverse speed of 60mm/min.

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Fig. 9 displays the hardness profiles of the experimental Al-Graphite composite samples. The Al-
Graphite sample prepared without ultrasonic treatment and with ultrasonic treatment showed
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average hardness value of 32 HV and 44 HV respectively. The significant reduction in both grain
size and porosities could be the possible reason for the improvement in hardness of ultrasonic
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treated composite than the other. The FSPed sample within the stir zone exhibits hardness values
in the range of 52-58 HV. These results suggest that a significant improvement in the hardness of
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Al- Graphite composites can be achieved with the aid of FSP. The micro hardness profile clearly
shows that the stir zone exhibit a highest hardness value among three zones exiting in the FSPed
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sample., it is also seen that as the distance is away from the nugget center, the micro hardness is
reduced and after a certain distance when it reaches the base metal it shows the hardness of the
base material. Among the three zones, the hardness value in HAZ zone is noticed to be lesser.
Moreover, it can be seen that the hardness of the FSPed composite correspondingly increases
with increase in the tool transverse speed.

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In the experimental details it is already mentioned that the length of the FSP tool as 3 mm
whereas the sample thickness is 6 mm. During the FSP process, the shoulder applies a pressure
to the material to constrain the plasticized material around the pin and generates heat through
friction and plastic deformation in a relatively thin layer under the shoulder surface. Hence, the
grain size and microhardness can vary across the section thickness. This implies that the uniform

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distribution of reinforcement particles, grain refinement and microhardness reported in this work
restricted to the surface i.e. up to 3 mm, not on the bulk.

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4. Discussion

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4.1. Microstrutural evolution during ultrasonic treatment of Al-5 vol. % Grp composites
Microstructural analysis of ultrasonic treated Al-Graphite composite has shown significant

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improvement in the dispersion of reinforcement of particles along with the substantial decrease
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in porosity. The mechanism responsible for the aforementioned findings can be explained as
follows. While fabricating the composite using stir-cast technique, due to the high cohesive
energy of particles and lack of the applied shear stress, graphite particles tend to agglomerate in
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the Al melt. These agglomerations can be effectively broken during the ultrasonic treatment to
ensure uniform distribution of particles. In general, when ultrasound is passed through the liquid
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melt, it imparts significant energy to the molecules in the melt [41-43]. The ultrasound comprises
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of (i) compression phase which exerts a positive pressure for pulling the molecule together and
(ii) rarefaction phase which applies negative pressure for pushing the molecules away from each
other. During rarefaction phase, small vapor filled voids called cavitation bubbles are formed
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[44]. The formed cavity grows in a few cycles of sound waves and reaches an unstable state
causing the bubbles to collapse. These cavitation effects are found in diverse applications in
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material and chemical synthesis [42-43,16]. For such a cavitation aided implosion to occur in
light metals, minimum ultrasonic intensity should lie within 80 – 100 W cm-2 [41 - 43]. The
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intensity of the radiating surface in the aluminium melt is calculated as 89.13 W cm-2 [16]. It
suggests that the occurrences of cavitation related effects are reasonable. During stir casting of
the composites, more number of cavitation sites is introduced into the melt. Particles that are
improperly wetted or associated with gas pockets can readily act as cavitation sites during
ultrasonic treatment [45]. The explosion of cavitation bubbles attached to the particle surfaces
can cause the breakage of particles’ agglomeration and successive occurrence of such cavitation

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events which can significantly promote the dispersion of the particles [44]. Thus, the
agglomerations were significantly reduced after ultrasonic treatment of Al - Graphite composite.

4.2. Microstructural evolutions during FSP of Al-graphite composites

Microstructural analysis of FSPed reveals that the coarse micron size grains are formed during

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low (20 and 40 mm/min) tool transverse speed. In contrary, submicron grains together with
enriched dislocations are noticed in the high (60 mm/min) tool transverse speed sample. The

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microstructural evolution during FSP process consisting of significant plastic deformation,
graphite particles’ breakage along with the dynamic recrystallization and it is a relatively

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complex phenomenon because of the effects of the gradient of strain, strain rate, and temperature
in FSP. The mechanism associated with the microstructural evolution during FSP is discussed in

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the following section. AN
According to Xiaocong et al. [40], equivalent plastic strain about 10 can be imparted in Al alloys
when FSP is conducted with the tool rotational of speed of 1000 RPM. Experimental evidences
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on SPD processing of pure Al suggests that plastic strain about 10 can produce materials with
grain size of 1-2 µm [46-47]. Similarly, ECAP processing of Al-Graphite composites has shown
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that plastic strain equivalent to ~ 4 can produce Al-graphite composites with 0.2 - 0.5 µm grain
size [26]. However, among the three tool transverse speeds used in the present study, ultra -fine
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grain structure with 0.5 - 1 um size grains were observed only when FSP was done with 60
mm/min. In contrast, coarse grains were observed in the samples FSPed using 20 and 40
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mm/min tool transverse speed. This indirectly implies that the decrease in tool transverse speed
(20mm/min and 40mm/min) increases the generation of heat which coarsens the grains via
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dynamic recrystallization process.

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Frigard et al. [48] have made detailed investigation on the role of tool transverse speed on the
temperature generated during FSP process. According to their finding, at constant tool rotational
speed of 1500 RPM and constant force of 7000 N, the peak temperature generated in the friction
stir zone is well above 500oC for all the tool transverse speeds i.e. 300, 480 and 720 mm/min.
They also found that the peak temperature decreases with increase in tool transverse speed.
Since, FSP conducted in the study is at much lower tool transverse speed of 20 40 and 60

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mm/min, similar trend (increase in heat generation with decrease in tool transverse speed) and
much higher peak temperature is expected in the stir zone. If this is true, then all the three FSPed
samples should have coarse strain free grains. However, samples FSPed using 60 mm/min tool
transverse speed has shown the ultra-fine grains (0.5 - 1 µm) in TEM micrograph. In addition to
that, significant amount of dislocations are also observed within the grains. This suggests that the

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presence of graphite reinforcement plays an important role in the microstructural evolution of
FSPed Al-Gr composites and it is discussed in the following section.

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According to Hatch et al [49], second phase or reinforcement particles can inhibit

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recrystallization when the particle size is less than 0.1 µm and the interparticle spacing is less
than 1.5 µm. This is because the dislocation cell structures in the deformed metal get anchored

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and stabilized by the particles. Therefore, there is enough space for the matrix of the composite
to recrystallize. In the current study, during FSP process with the tool transverse speed of 20 and
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40 mm/min, the size of the graphite particles becomes well above the optimum size of 0.1 µm .
Hence, it is reasonable to expect that the existence of coarse graphite particles have not inhibited
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the dynamic recrystallization process which leads to grain coarsening. In the meantime, it seems
that the samples FSPed using 60 mm/min tool transverse speed also consist of graphite particles
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of more than 0.1 µm. In spite of that, ultra-fine grains are observed in sample FSPed using 60
mm/min tool transverse speed. Closer examination of TEM micrograph of this sample shows
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extremely fine (< 0.1 um) graphite particles in few regions (Fig.10 (a)). Interestingly, coarse
strain free grains can be seen in the region where this fine graphite particles are not present
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(Fig.10 (b)). Hence, it can be considered as one of the possible reasons to restrict the growth of
grains during dynamic recrystallization process. Apart from graphite particles, fine spherical
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second phase particles are also seen in the microstructure of sample FSPed using 60 mm/min
tool transverse speed (Fig.10 (c)). This also can be considered as an alternate source to impede
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the grain coarsening while dynamic recrystallization. These second phase particles might have
grown more than 0.1 µm due to high peak temperature generation associated with the low tool
transverse speed (20 and 40 mm/min) FSP process. Thus, it is expected to provide limited role in
controlling the grain growth when the tool transverse speed is low.

4.3. Mechanical behavior of FSPed Al-graphite composites

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Grain size, reinforcement size and dislocation density are important factors influencing the
hardness value of FSPed samples. During FSP, most of the mechanical work is dissipated in the
form of heat and a small fraction of deformation energy is internally retained as stored energy.
When FSP tool comes in contact with base material, shear deformation introduces large number
of dislocations in the material. Large fraction of dislocation formed within the coarse grain, thus

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forms the subgrains and increases the dislocation density. As the material undergoes further
deformation, additional dislocations are introduced into subgrain boundaries, converting them

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into high angle boundaries. Thus, dynamically recrystallized grains are formed. Based on the
above mentioned process, fine recrystallized grains with large amount of dislocations are formed

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during FSP process. In the meantime, rapid tool rotation associated with the FSP process breaks
and distributes the graphite particles uniformly in the Al matrix. The combined influence of

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increase in dislocation density, grain and particle refinement, uniform distribution of
reinforcement particles has significantly improved the hardness of FSPed Al-Graphite
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composite. Since FSP was done at constant rotational speed, the change in tool transverse speed
is not expected to have significant impact on the refinement of graphite particles. On the other
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hand, significant increase in the thermal cycle time associated with the decrease in tool
transverse speed possibly leads to the coarsening of grain size due to the concurrent non-
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isothermal grain growth. This could be the reason for the increase in hardness with increase in
the tool transverse speed.
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5. Conclusions:
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1. The cavitation bubbles formed during the ultrasonic treatment decreased the porosity
of Al-Graphite composites and also broken the graphite particles’ agglomeration
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thereby promoted the graphite particles’ distribution in Al matrix.

2. The graphite particles segregated along the grain boundaries during ultrasonic
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treatment of Al-Graphite were fragmented into very fine particles and uniformly
spread throughout the matrix in stir zone due to the strong stirring action imparted
during FSP process.
3. The strong frictional shear force generated during the FSP process refined the size of
graphite particles down to submicron and nano levels.

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4. FSP of Al-Graphite composite remarkably reduced the grain size of Al matrix to 14

um, 6 µm and 0.5-1 µm for the tool transverse speeds of 20 mm/min, 40 mm/min and
60 mm/min, respectively. The coarsening of grains attributed to high peak
temperature generation during low tool transverse speed.
5. Extremely fine graphite and second phase particles formed during high tool

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transverse speed in FSP process has restricted grain growth of matrix by Zener
pinning process.

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6. FSP has increased the hardness of Al-Graphite samples due to the combined influence
of fine grain structure, high dislocation density and uniform dispersion of fine

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graphite particles

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References:
1. M.E. Smagorinski, P.G. Tsantrizos, S. Grenier. J. Min. Met. Mater. 1996; 48: 56–59.
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2. Miracle DB. Compos Sci.Technol. 2005; 65: 2526–40.
3. C.S. Ramesh, R. Noor Ahmed, M.A. Mujeebu, M.Z. Abdullah. Mater Des. 2009; 30:
M

1957–1965.
4. V.V. Bhanu Prasad, B.V.R. Bhat, Y.R. Mahajan, P. Ramakrishnan. Mater.Sci. Eng. A
D

2002; 337: 179–186.

5. J.E. Spowart, B. Maruyama, D.B. Miracle, Mater. Sci. Eng. A 2001; 307: 51–66.
TE

6. S.J. Hong, H.M. Kim, D. Huh, B.S. Chun, C. Suryanarayana, Mater. Sci.Eng. A 2003;
347 (1–2): 198–204.
EP

7. K.T. Conlon, D.S.Wilkinson, Mater. Sci. Eng.A 2001; 317 (1–2): 108–114.
8. J.E. Spowart, Z.Y. Ma, R.S. Mishra, K.V. Jata, M. Mahoney, R.S.Mishra. Friction Stir
C

Welding and Processing II, TMS, Warrendale, PA. 2003; 243–252.

9. A.M. Murphy, S.J. Howard, T.W. Clyne. Mater. Sci. Tech. 1998; 14: 959–968.
AC

10. A.R. Vaida, J.J. Lewandowski. Mater. Sci. Eng. A 1996; 220: 85–92.
11. J. Llorca, Prog. Mater. Sci. 2002; 47 (3): 283–353.
12. J.J. Lewandowski, C. Liu. Mater. Sci. Eng. A 1989; 107: 241–255.
13. S. Tao, J.D. Boyd, Proceedings of the ASM 1993 Materials Congress, ASM
International, Materials Park, OH, Pittsburgh, PA.1993; 29–40.
14. Yong Yang and Xiaochun Li, Trans. ASME Ser. B, 2007; 129:p 497–501

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15. X. Li, Y. Yang, and D. Weiss, Metall. Sci. Technol., 2008; 26: p 2
16. P. Christy Roshini, B. Nagasivamuni, Baldev Raj, and K.R. Ravi, JMEPEG DOI:
10.1007/s11665-015-1491-4.
17. C.I. Chang, X.H. Du, J.C. Huang, Scripta Mater. 2007; 57: 209–212.
18. N. Fakhar , F. Fereshteh-Saniee, R.Mahmudi Mater Des. 2015; 85:342–348

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19. M.Yu. Murashkin, I. Sabirov, A.E. Medvedev, N.A. Enikeev, W. Lefebvre, R.Z. Valiev,
X. Sauvage Mater Des. 2016; 90: 433–442.

RI
20. Mohamed Ibrahim Abd El Aal ,HyoungSeop Kim Mater Des.2014;53: 373–382.
21. Saleh N. Alhajeri, Khaled J. Al-Fadhalah, Abdulla I. Almazrouee, Terence G. Langdon,

SC
Materials Characterization 2016; 118: 270–278.
22. HosseinAkbaribeni, MortezaAlizadeh, Mohammad Ghaffari, RasoolAmini Composites:

U
Part B 2014; 58: 438–442.
23. RoohollahJamaati, Mohammad Reza Toroghinejad, Jan Dutkiewicz , Jerzy A.
AN
SzpunarMater Des.2012; 35: 37–42.
24. Mohammad Reza Toroghinejad, RoohollahJamaati, Jan Dutkiewicz, Jerzy A.
M

SzpunarMater Des.2013;51: 274–279.

25. Brij Kumar Dhindaw Nguyen Van Thuong, HussainZuhailawati ,Anasyida Abu Seman,
D

Tran DucHuy , Mater Des.2015;67: 448–456.

26. M. Saravanan, R.M. Pillai , K.R. Ravi, B.C. Pai, M. Brahmakumar Compos Sci.Technol.
TE

2007; 67: 1275–1279.

27. Su JQ, Nelson TW, Sterling CJ. J Mater Res 2003; 18: 1757.
EP

28. Z. Chen, J. Li , A. Borbely, G. Ji , S.Y. Zhong , Y.Wu, M.L. Wang, H.W. Wang, Mater
Des. 2015;88: 999–1007.
C

29. P. Xue, B.L. Xiao, Z.Y. Ma Mater Des. 2014; 56 : 848–851.

30. Z.Y. Ma, F.C. Liu a, R.S. Mishra Acta Mater. 2010; 58: 4693–4704.
AC

31. F.C. Liu and Z.Y. Ma Scripta Mater. 2010; 62 : 125–128

32. Jian-Qing Su , Tracy W. Nelson, Colin J. Sterling Scripta Mater. 2005;52: 135–140.
33. A. Shafiei-Zarghani, S.F. Kashani-Bozorg, A. Zarei-HanzakiMater. Sci. Eng. A
2009;500: 84–91.
34. A. Dolatkhah, P. Golbabaei, M.K. BesharatiGivi, F. MolaiekiyaMater Des.2012; 37:
458–464.

13
 ACCEPTED MANUSCRIPT

35. J. Sun, X. Zhang, Y. Zhang, N. Ma, H. Wang, Micron 70 (2015) 21–25.

36. S.M. Ma, P. Zhang, G. Ji, Z. Chen, G.A. Sun, S.Y. Zhong, V. Ji, H.W. Wang, J. Alloys
Compd. 616 (2014) 128–136.
37. T. Prakash ,S. Sivasankaran, P. SasikumarArab J Sci Eng.2015; 40: 559–569.
38. DevarajuAruri, Kumar Adepu, KumaraswamyAdepu, KotiveerachariBazavada,

PT
jmater.res.technol. 2013; 2(4): 362–369.
39. A. Devaraju, A. Kumar, B. KotiveerachariMater Des. 2013; 45: 576–585.

RI
40. Xiaocong He, FengshouGu , Andrew Ball. Progress in Materials Science. 2014; 65:1–66.
41. Yong Yang, JieLan, Xiaochun Li. Mater. Sci. Eng. A 2004; 380: 378–383.

SC
42. Xiaochun Li, Yong Yang, David Weiss. Metall. Sci. Technol. 2008; 26: 2 - Ed.
43. G. Cao, J. Kobliska, H. Konishi,X. Li. Metall. Mater. Trans. A 39, p 880-886.

U
44. K. S. Suslick, Y. Didenko, M. M. Fang, T. Hyeon, K. J. Kolbeck, W. B. McNamara, M.
M. Mdleleni, M. Wong. Phil. Trans. R. Soc. Lond. A 1999; 357: 335-353.
AN
45. G.I. Eskin. Ultrason. Sonochem. 1995; 2(2): 137–141.
46. Megumi Kawasaki, ZenjiHorita, Terence G. LangdonMater. Sci. Eng. A 2009; 524: 143–
M

15.
47. Ehab A. El-DanafMater. Sci. Eng. A 2008;487: 189–200.
D

48. O. Frigaard, O. Grong, O.T. Midling. Metall. Mater. Trans. A 2001;32:1189

49. Hatch JE. Aluminum properties and physical metallurgy. Metals Park, Ohio: American
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Society for Metals; 1984; 121.

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Figure Captions
Fig. 1 shows the dimensions of the FSP tool.
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Fig. 2 FESEM images of (a) stir-cast and (b) ultrasonic treated Al – 5 vol. % Grp composite.
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Fig.3 (a-c) Optical images of processed samples under constant 1600rpm with varying transverse
speeds (a) 20mm/min (b) 40mm/min (c) 60mm/min shows the grains in three distinct regions.

Fig. 4 Comparison on grain size of Al-Graphite composite without UT, with UT and FSPed at
different tool transverse speed

Fig.5 (a-c) Optical images of processed samples under constant 1600rpm with varying transverse
speeds (a) 20mm/min (b) 40mm/min (c) 60mm/min shows the particles distribution in three
distinct regions.

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Fig.6 Effect of tool transverse speed on particle size of FSPed Al-Graphite composite.

Fig . 7 TEM micrograph shows grain structure evaluation at different feed rates (a-b) 20 mm/min
(c-d) 40 mm/min and (e-g) 60 mm/min

Fig . 8 TEM micrograph shows particle size at different feed rates (a) 20 mm/min (b) 40 mm/min
and (c) 60 mm/min

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Fig.9 Microhardness profiles measured along cross-sectional planes of the sample.

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Fig . 10 TEM images at 60 mm/min shows (a) nano sized graphite particles (b) nano sized second
phase particles which inhibit grain growth (c) Coarse grains

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Highlights:

• Ultrasonic treatment reduces porosities and particles agglomeration.

• FSP reduces the particles size to submicron and nano levels

• FSP distributes the particles uniformly throughout the matrix.

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• Ultrafine grained Al-Graphite composites developed via FSP.
• FSPed composites exhibit superior hardness compared to as cast composites.

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