Journal of Alloys and Compounds 732 (2018) 748e758

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Journal of Alloys and Compounds

journal homepage: http://www.elsevier.com/locate/jalcom

Microstructure and mechanical properties of graphene nanoplates

reinforced pure Al matrix composites prepared by pressure infiltration
method
Wenshu Yang a, *, Qiqi Zhao a, Ling Xin a, b, Jing Qiao a, **, Junyu Zou a, Puzhen Shao a,
Zhenhe Yu a, Qiang Zhang a, Gaohui Wu a, ***
a
Department of Material Science and Engineering, Harbin Institute of Technology, Harbin, 150001, China
b
Beijing Institute of Electronic System Engineering, Beijing, 100854, China

a r t i c l e i n f o a b s t r a c t

Article history: In the present work, microstructure and mechanical behavior of the graphene nanoplates (GNPs) rein-
Received 15 September 2017 forced pure Al (GNPs/Al) composites prepared by the pressure infiltration method was investigated. No
Received in revised form Al4C3 phase was detected in the composites, while GNPs have been well bonded with the Al matrix. It is
29 October 2017
suggested that the reaction between pure Al matrix and graphene could also be inhibited by using
Accepted 30 October 2017
Available online 31 October 2017
graphene with fewer defects. It has been found that the mechanical properties of the composites could
be significantly improved by the addition of graphene. After addition of 0.54 wt% GNPs, the improvement
of the yield and tensile strength before the extrusion was 116% and 45%, respectively. However, after the
Keywords:
Metal matrix composites
extrusion treatment, the corresponding increment of the yield and tensile strength was increased to
Al matrix composites 228% and 93%, respectively. Moreover, the fracture surface of the GNPs/Al composites before and after
Graphene the extrusion treatment was mainly characterized by the lamellar structure with bridging of GNPs and
Interfacial reaction the fine equiaxed structure with the pulling-out of the GNPs, respectively. Based on the modified shear-
Strengthening mechanism lag model, the strengthening mechanism of the GNPs/Al composites has been discussed, and the effect of
Extrusion GNPs and the extrusion treatment on the yield strength of the composites have been analyzed.
© 2017 Elsevier B.V. All rights reserved.

1. Introduction Recently, the preparation, microstructure and mechanical

Because of the outstanding mechanical, thermal and electrical
properties, graphene has been considered as an ideal reinforce-
ment in composites [1], which is an important practical application
field for graphene. It has been found that the addition of graphene
nanoplates (GNPs) could significantly improve the mechanical
properties of polymer [2,3] and ceramics [4,5].
* Corresponding author. P. O. 3023, Science park, No. 2 Yikuang Street, School of
Materials Science and Engineering, Harbin Institute of Technology, Harbin, 150080,
China.
** Corresponding author. P. O. 3023, Science park, No. 2 Yikuang Street, School of
Materials Science and Engineering, Harbin Institute of Technology, Harbin, 150080,
China.
*** Corresponding author. P. O. 3023, Science park, No. 2 Yikuang Street, School of
Materials Science and Engineering, Harbin Institute of Technology, Harbin, 150080,
China.
E-mail addresses: yws001003@163.com (W. Yang), jingqiao@hit.edu.cn (J. Qiao),
wugh@hit.edu.cn (G. Wu).
properties of graphene reinforced Al matrix composites has been
widely explored. Table 1 listed the main development and
improvement of graphene/Al composites reported in literatures. As
summarized in Table 1, the main techniques reported to prepare
graphene/Al composites are solid methods, such as powder met-
allurgy (PM) and corresponding the extrusion method. Wang et al.
[7] found that the tensile strength of the composites could be
significantly improved (62%) after the addition of 0.3 wt% graphene.
Meanwhile, Shin et al. [13,14] firstly revealed that the higher
strengthening efficiency of few-layer graphene than multi-walled
carbon nanotube could be mainly attributed to their larger spe-
cific surface, which could be described by the modified Rule of
Mixture after introducing the geometry factor, interfacial bonding
factor, and alignment factor. Moreover, Kwon et al. [21] achieved
113% and 300% increments in tensile and flexural strength after
addition of 1 vol% graphene into AlMg5 matrix, respectively.
Furthermore, Li et al. [31] employed reduced graphene oxide (RGO)
and carbon nanotube (CNT) hybrid reinforcement in Al matrix

https://doi.org/10.1016/j.jallcom.2017.10.283
0925-8388/© 2017 Elsevier B.V. All rights reserved.
 W. Yang et al. / Journal of Alloys and Compounds 732 (2018) 748e758 749

Table 1
The main development of graphene/Al composites reported in literatures.

Published year Optimized amount Matrix alloy Preparation methods Results Ref.

2011 0.1 wt% Pure Al PM and extrusion Hardness was decreased due to the formation of Al4C3. [6]
2012 0.3 wt% Pure Al PM and extrusion 62% increment in tensile strength [7]
2012 5 wt% Pure Al PM 30% increment in hardness and compressive strength [8]
2014 1.0 wt% 6061Al PM 47% increment in bending strength [9]
2014 1.0 wt% Pure Al PM 138% increment in micro-hardness [10]
2014 0.3 wt% Pure Al PM and hot extrusion 11% increment in yield and tensile strength [11]
2014 0.5 wt% Al-Mg-Cu PM and extrusion 25% increment in yield and tensile strength [12]
2015 0.7 vol% Pure Al PM and hot-rolling 71.7% increment in yield strength [13,14]
2015 0.5 wt% Pure Al PM 10% increment in hardness [15]
2016 0.3 wt% Pure Al PM 30% increment in tensile strength [16]
2016 1.0 wt% 5083Al PM and hot extrusion 50% increment in tensile strength [17]
2016 0.15 wt% Pure Al PM 43% increment in hardness [18]
2017 0.25 wt% Pure Al PM 38% increment in yield strength [19]
2017 1 wt% Pure Al PM 54% increment in compressive yield strength [20]
2017 1 vol% Pure Al PM 113% increment in tensile strength [21]
2017 0.7 wt% 6061Al PM 75% increment in yield strength [22]
2014 0.5 wt% Pure Al High-pressure torsion 18% increment in tensile strength [23]
2015 1.0 wt% Pure Al Clad forming 77.5% increment in tensile strength [24]
2015 1 wt% Al-0.5Si Cryomilling and hot extrusion 60% increment in tensile strength [25]
2016 2 wt% Pure Al In-situ reaction in liquid Al 50% increment in tensile strength [26]
2016 5 wt% 7075 Al Electrocharging assisted process 50% increment in tensile strength [27]
2017 3 vol% 5052Al Friction stir 100% increment in yield strength [28]
2017 3 wt% Al-Mg SPS 47% increment in compressive strength [29]
2017 1.8 wt% Al-20Si Pressure infiltration method 130% in tensile strength [30]

nanolaminated composites, which demonstrated higher strength
and strengthening efficiency.
Compared with the solid methods, liquid methods, which have
been widely used to prepare Al matrix composite [32], have been
less investigated in the preparation of graphene/Al composites
(Table 1). Yolshina et al. [26] achieved 50% increment in tensile
strength by in-situ graphene in liquid Al. Meanwhile, Iftekhar Jaim
et al. [27] prepared crystalline graphene nanoribbons by the elec-
trocharging assisted process, and obtained 50% increment in tensile
strength. Moreover, Khodabakhshi et al. [28] obtained 100% in yield
strength in Al-2.2Mg by friction stir process. In our previous work
[30], graphene nanoflakes reinforced Al-20Si matrix composites
were prepared by the pressure infiltration method, and more than
130% increment in tensile strength and 230% in bending strength
has been achieved, respectively. The above investigations indicate
that the liquid methods could also be the feasible and successful
way to prepare graphene/Al composites. Regardless of the prepa-
ration methods, inhibition of Al4C3 phase is one of the main chal-
lenges for preparation of high performance graphene/Al
composites. In our previous work, Al alloy with high Si content
(20 wt%) was chosen with the aim to inhibit the formation of Al4C3,
and the microstructure observation verified the effectiveness of the
alloying treatment in the pressure infiltration process [30]. How-
ever, applicability of the pressure infiltration method in other
graphene/Al composites has not been investigated.
In the present work, graphene nanoplates (GNPs) reinforced
pure Al (GNPs/Al) composites were prepared by the pressure
infiltration method, and the effect of the GNFs on the microstruc-
ture and the mechanical properties of the GNPs/Al composites have
been discussed. It has been found that the pressure infiltration
method could also be used for the preparation of graphene/pure Al
composites without formation of Al4C3 and with good mechanical
properties.
2. Material and methods
GNPs (Fig. 1a, c) and pure Al powders (7 mm, Fig. 1b) were
supplied by Qingdao Huagao Graphene Technology Corp. Ltd. China
and Northeast Light Alloy Corp. Ltd. China, respectively. In order to
inhibit the reaction between graphene and Al matrix, GNPs pre-
pared by micromechanical exfoliation method was used in the
present work. Raman Spectra of as received multilayer GNPs
dispersed on SiO2 substrate with the significant D band (disorder
related) at 1355 cm
1, strong G band (graphite related) at
1565 cm
1 and a broad second order 2D band at 2719 cm
1.
Representative transmission electron microscopy (TEM) image of
GNPs has been shown in Fig. 1c. Wrinkles and folds were very
evident on the surface of GNPs. As shown in Fig. 1d, The intensity
ratio D Band to G band (ID/IG) indicated that the defects content in
the received GNPs was relatively low, and the intensity ratio 2D
Band to G band (I2D/IG) indicated that the GNPs was multilayer
(about 10 layers).
The schematic preparation process of the GNPs/Al composites is
given in Fig. 2. The GNPs were firstly mixed with pure Al powder
using a planetary mill at a rotation speed of 100 rpm for 1 h. The
weight ratios of the GNPs in the mixed powders were 0.1, 0.2, 0.4
and 0.9 wt%, respectively. The mixture was then put into a steel
mold and further pressed to the set height to prepare the preforms,
and the volume content of the milled particles in the mold was
about 60 vol% to 70 vol%. In order to inhibit the reaction and to
overcome the poor wettability between graphene and Al matrix,
the infiltration of molten Al was carried out at lower temperature
with higher pressure. The preheating temperatures for the preform
and pressure infiltration dies were 500 and 730  C, respectively.
During the infiltration process, a pressure of 15 MPa was applied
and maintained for 5 min, followed by the solidification of the
composites in air, and then GNPs/Al composites with different
GNPs contents have been obtained. After measuring the height of
composites, which represented the actual volume contents of the
milled particles, the accurate amounts of the GNPs in the GNPs/Al
composites have been calculated to be 0.06, 0.14, 0.21 and 0.54 wt%,
respectively. For comparison, a pure Al specimen was also prepared
by the same process. Afterward, in order to investigate the effect of
the extrusion treatment, parts of samples were extruded at 450  C
with the extrusion ratio of 11:1. Before microstructure observation
and properties testing, all samples were annealed at 400  C for 2 h.
Morphologies of the GNPs/Al composites were observed by the
Olympus PMG3 optical microscope. Microstructure and electron
750 W. Yang et al. / Journal of Alloys and Compounds 732 (2018) 748e758

Fig. 1. Microstructure of the GNPs and pure Al powders used in the present work. (a) SEM microstructure of GNPs, (b) SEM microstructure of pure Al powder, (c) TEM observation of
GNPs, (d) Raman spectra of GNPs.

Fig. 2. The schematic preparation process of the GNPs/Al composites.

backscatter diffraction (EBSD) of the GNPs/Al composites speci- spectrometer (EDS). TEM observation was performed on JEM-2010F
mens composite were characterized by FEI Quanta 200FEG scan- transmission electron microscopy. Raman measurement is per-
ning electron microscope (SEM) equipped with energy dispersive formed on a JY-HR800 laser Raman spectrometer using a 532 nm
 W. Yang et al. / Journal of Alloys and Compounds 732 (2018) 748e758
solid-state laser as excitation source. Tensile tests were performed
on Instron 5569 universal electrical tensile testing machine with a
cross-head speed of 0.5 mm/min. All the tests have been performed
on at least five samples to improve statistical significance of the
results. The fracture surface of GNPs/Al composites was observed
by FEI Sirion Quanta 200 SEM.
3. Results and discussion
Microstructure of the milled Al particles with GNPs (Al-0.9 wt%
GNPs) has been shown in Fig. 3. Due to the impacting effect of the
Al2O3 milling balls, the morphology of the Al particles has been to
be flaky-like (Fig. 3a), which is beneficial for the absorption of the
GNPs onto the surface of the Al particles [7,33]. Higher magnifica-
tion image (Fig. 3b) shows that several GNPs have been attached on
the surface of the Al particles. However, due to the damage caused
by the ball-milling process, the raw GNPs have been broken to be
small pieces, which is unfavorable for the mechanical performance.
The morphologies of the 0.54 wt% GNPs/Al composite before and
after the extrusion treatment have been show in Fig. 4. No signif-
icant pores were found in the composites before and after the
extrusion treatment. Moreover, large Al grains could be observed in
the as-casted GNPs/Al composites (Fig. 4a), and the average grain
size of the Al matrix was about 6.8 mm before the extrusion treat-
ment (Fig. 4b), However, after the extrusion treatment, the grain
size of the Al matrix has been greatly refined to be about 2.1 mm
(Fig. 4d and e). It has been widely reported in the Al matrix com-
posites that the extrusion treatment has the effect of grain-
refinement, densification, improving the interfacial bonding and
directional arrangement of the reinforcements [34e36], which are
beneficial for the improvement of the composites. Moreover, no
significant orientation of the Al grains was found in the as-casted
GNPs/Al composites (Fig. 4c). It has been reported that the 〈001〉
direction is the preferred growth direction of the solidification of
pure Al [37]. However, the Al matrix in the preform could be so-
lidified in all the direction while the milled Al particles with GNPs
could be act as the nucleation particles. Therefore, no significant
texture has been observed (Fig. 4c) in the as-casted GNPs/Al com-
posites. However, more Al grains along [101] directions have been
detected after the extrusion treatment (Fig. 4f) and no significant
effect of the GNPs phases has been found, which indicating the
formation of the cubic texture, which was mainly formed due to the
deformation of the Al grains along the (111) planes [38]. The back
scattering SEM microstructure of the 0.54 wt% GNPs/Al composite
has been shown in Fig. 5. The presence of the GNPs could not be
easily observed in the Fig. 5a due to the small dimension and low
Fig. 3. Microstructure of the Al particles with GNPs (Al-0.9 wt%GNPs) after ball-milling. (a) SEM observation of the powders, (b) High magnification of the selected area in (a) to
illuminate the presence of the GNPs.
751
content of GNPs. EDS analysis results (Fig. 5b and c) revealed the
distribution of Al and C elements, implying the relative uniform
distribution of GNPs in the composite.
XRD analysis result of the GNPs/Al composites with various
GNPs content before the extrusion treatment has been shown in
Fig. 6. Regardless of the GNPs content, the distinct peaks detected in
the GNPs/Al composites were at the 2q angles of 38.29 , 44.54 ,
64.89 , 78.05 and 82.17, which is corresponded to the peaks of Al
(38.47, 44.71, 65.10 , 78.23 and 82.44 according to PDF#85-
1372), respectively. It should be noted that the XRD curves of the
GNPs/Al composites was deviated 0.2 to left due to the systematic
error. It has been reported by Zhang et al. [17] and Li et al. [19] that
the peaks of Al4C3 (the 2q angles at 31.13 , 31.77, 35.89 , 40.12 and
55.05 according to PDF#35-0799) have been detected in the gra-
phene/Al composites. However, only one peak at the 2q angles of
32.67, which should be at about 32.87 after calibrated with the
systematic error, was found in the high magnification image of the
0.54 wt% GNPs/Al composite at the top left corner in Fig. 6.
Although the phase has not been determined yet, the peaks at the
2q angles of 32.67 should not be the diffraction peak of the Al4C3
phase. Moreover, the microstructure of the 0.54 wt% GNPs/Al
composite before the extrusion treatment has been observed by
TEM, as shown in Fig. 7. Al4C3 phase, which has been widely re-
ported to be needle-like [17,21], has not been found (Fig. 7a).
Moreover, the distribution of Al ad C elements (Fig. 7c) indicated
that the GNPs have been well uniformly embedded in the Al matrix,
while the GNPs and Al matrix has been well bonded.
Although Zhang et al. [17] found that the Al4C3 phase could act
as the strengthening precipitate in the GNFs/5083Al composites, it
is generally reported that the presence of Al4C3 phase would
deteriorate the mechanical and corrosion resistance properties of
the Al matrix composites reinforced with carbonaceous phases
[39]. Bartolucci et al. [6] used high energy ball-milling and 550  C/
4 h hot isostatic pressing (HIP) to prepared educed graphene ox-
ides/pure Al composites, and found that the formation of Al4C3
deteriorate the mechanical properties of the composites. Pe
rez-
Bustamante et al. [10] used GNPs with high defects to prepare
GNPs/Al composites. Although relative low sintering temperature
was used (500  C/2 h), Al4C3 phase was still detected by XRD
analysis. Li et al. [19] also observed the formation of Al4C3 phase in
the composites reinforced with graphene nanosheets (GNSs)
fabricated by high energy ball milling and HIP (610  C/4 h). How-
ever, Yolshina et al. [26] utilized the reaction between the carbon
containing components and the molten Al in molten alkali halide
media to form in-situ graphene. Based on the electrochemical
analysis in NaCl solution, they further proved that no Al4C3 phase
752 W. Yang et al. / Journal of Alloys and Compounds 732 (2018) 748e758

Fig. 4. The morphologies of the 0.54 wt% GNPs/Al composite (a) (b) (c) before (perpendicular to the Al infiltration direction) and (d) (e) (f) after the extrusion treatment
(perpendicular to the extrusion direction). (a) (d) Morphologies observed by optical microscopes, (b) (e) EBSD morphologies, (c) (f) Inverse pole figures of (b) and (e), respectively.

Fig. 5. Backscattered SEM observation of 0.54 wt% GNPs/Al composite before the extrusion treatment. (a) Morphology and corresponding distribution of (b) Al and (c) C elements in
Fig.5a, respectively.

was formed [26]. It implies that the graphene with fewer defects
might not be prone to react with Al matrix, which agrees well with
the conclusion suggested by Bartolucci et al. [6] that the defective
nature of graphene is likely responsible for promoting aluminum
carbide formation. Our previous research indicated that high Si
element in the Al matrix could inhabit the formation of the Al4C3
phase although the preparation temperature of the composite was
beyond the melting point of Al (770  C). It should be noted that
addition of alloying elements is a common method to control the
interfacial reaction between Al matrix and carbonaceous phases,
such as carbon fibre [40,41] and diamond particles [42,43]. Usually,
the chemical reaction could be controlled from the reaction ther-
modynamics and kinetics fields. From the aspect of reaction ther-
modynamics, the formation of Al4C3 could be inhibited by
 W. Yang et al. / Journal of Alloys and Compounds 732 (2018) 748e758
Fig. 6. XRD analysis result of the GNPs/Al composites with various GNPs content
before the extrusion treatment.
decreasing the reactivity of the Al-C systems, such as using carbo-
naceous phases with fewer defects [44] and addition of alloying
elements to change Gibbs free energy of the reactions [40].
Meanwhile, from the aspect of reaction kinetics, the formation of
Al4C3 could be inhibited by controlling the reaction rate, such as
sintering at lower temperature/short time [45] and separating the
Al and carbonaceous phases by coating treatment [46]. Our
Fig. 7. TEM observation of 0.54 wt% GNPs/Al composites before the extrusion treatment. (a) Low magnification image, (b) High magnification image, (c) Distribution of Al (displayed
as red color) and C (displayed as green color) elements of (b). (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this
article.)
753
previous work verified the effectiveness of the alloying treatment
(addition of Si) in the inhibition of the Al4C3 phase [30]. Combining
the present results and the experimental results reported by Yol-
shina et al. [26], it is suggested that the reaction between pure Al
matrix and graphene could also be inhibited by using graphene
with fewer defects.
The representative tensile curves of the GNPs/Al composites
before and after the extrusion treatment have been shown in Fig. 8a
and b, respectively. The tensile strength of GNPs/Al composites
have been significantly improved with the trade-off of decreased
ductility. The variations of yield and tensile strength with the
amount of GNPs have been shown in Fig. 9a and b, respectively.
Regardless of the extrusion treatment, it is obvious that yield and
tensile strength of GNPs/Al composites were increased with the
amount of GNPs. After addition of 0.54 wt% GNPs, the yield strength
of composites has been increased 116% and 228% before and after
the extrusion, while the tensile strength of composites has been
increased 45% and 93% before and after the extrusion, respectively.
The fracture surfaces of the GNPs/Al composites before and after
the extrusion treatment have been shown in Fig. 10 and Fig. 11,
respectively. No significant difference was observed in the fracture
surface of the GNPs/Al composites with different GNPs amount.
Moreover, dimples and tearing ridges could be observed in the
GNPs/Al composites before and after the extrusion treatment.
However, the amount of dimples and tearing ridges were higher in
the composites after the extrusion treatment. Furthermore, the
fracture surface of the GNPs/Al composites before the extrusion
treatment was mainly characterized by the lamellar structure
(Fig. 10cei), which is very similar to the fracture surfaces reported
754 W. Yang et al. / Journal of Alloys and Compounds 732 (2018) 748e758
Fig. 8. Representative tensile stress-strain curves of pure Al and GNPs/Al composites (a) Before and (b) After the extrusion treatment.
Fig. 9. Variation of tensile properties of GNPs/Al composites with the amount of GNPs before and after the extrusion treatment. (a) Yield strength, (b) Tensile strength.
by the Bastwros et al. [9], Yan et al. [12] and Zhao et al. [47], while
the fracture surface of the GNPs/Al composites after the extrusion
treatment were mainly characterized by the fine equiaxed structure
(Fig. 11). The difference in the fracture morphologies might be
related to the grain-refinement effect after the extrusion treatment
(Fig. 4) and the relative improved interfacial bonding between
GNPs and Al matrix [48]. Moreover, the bridging (Fig. 12a) and the
pulling-out (Fig. 12b) of the GNPs were mainly found in the GNPs/Al
composites before and after the extrusion treatment, respectively.
It implies that the strengthening effect of GNPs has been utilized
more fully after the extrusion treatment.
Jiang et al. [49] introduced the strengthening efficiency R
(defined as (sc‒sm)/(sm$Vr), where sc and sm are the yield strengths
of the composite and matrix, Vr is the volume concentration of
reinforcement) to evaluate the strengthening effect. To convert
wt.% amount of GNPs in the composite samples to vol% for com-
parison, a density for the GNPs of 2.2 g/cm3 was assumed in the
present work [50,51]. Usually, the strengthening efficiencies of
graphene in Al matrix composites prepared by PM methods are
from 20 to 120, mainly depending on the interfacial bonding and
characteristic of GNPs. The calculated strengthening efficiencies of
GNPs/Al in the present work were more than 200 before and after
the extrusion treatment, which is significant higher than the
literature results [31], implying that the liquid metallurgy (pressure
infiltration method in the present work) is beneficial for improving
the interfacial bonding between GNPs and Al, which might be
attributed to the improved wettability at higher temperature and
pressure. Based on shear-lag model, Shin et al. [14] proposed the
following equation to describe the strengthening behavior of
graphene, as expressed as:
sc ¼ sm Vm þ ckgssr Vr (1)
where the Vm is the volume content of matrix, c is empirical con-
stant, k, g, s are the interfacial bonding factor, the geometry factor
and the alignment factor, respectively.
From Eq. (1), it is clear that the yield strength of GNPs/Al com-
posites is increased with the amount of GNPs, which agree well
with the experimental results. The extrusion treatment would
improve the properties from at least three aspects. The grain size of
Al matrix has been greatly refined after the extrusion treatment
(Fig. 4), which improve the yield strength of matrix according to
HallePetch relationship [12]. Moreover, the extrusion treatment
would decrease the porosity slightly [35] and improve the inter-
facial bonding between GNPs and Al [48], which would increase the
value of k. Furthermore, although it has not been directly observed
in the present work, the GNPs would tend to align along the
extrusion direction due to the shear stress during processing [48].
The unidirectional arrangement is beneficial for utilizing the
strengthening effect of graphene, and it is expected that alignment
factor s would be increased.
4. Conclusions
In the present work, graphene nanoplates (GNPs) reinforced
pure Al (GNPs/Al) composites were prepared by the pressure
infiltration method. The GNPs have been distributed uniformly in
the composites, while the grain size of the Al matrix could be
 W. Yang et al. / Journal of Alloys and Compounds 732 (2018) 748e758 755

Fig. 10. Fracture surface of the GNPs/Al composites with various GNPs contents before the extrusion treatment. (a) Pure Al, (c) þ0.06 wt% GNPs, (e) þ0.14 wt% GNPs, (g) þ0.21 wt%
GNPs and (i) þ0.54 wt% GNPs. (b) (d) (f) (h) (j) are the high magnification image of the selected areas in (a) (c) (e) (g) (j), respectively.

significantly refined by the extrusion treatment. No Al4C3 phase indicated that the GNPs have been well uniformly embedded in the
was detected in the composites by the XRD analysis and further Al matrix, while the GNPs and Al matrix has been well bonded. It is
TEM observation. Moreover, the distribution of Al ad C elements suggested that the reaction between pure Al matrix and graphene
756 W. Yang et al. / Journal of Alloys and Compounds 732 (2018) 748e758

Fig. 11. Fracture surface of the GNPs/Al composites with various GNPs contents after the extrusion treatment. (a) Pure Al, (c) þ0.06 wt% GNPs, (e) þ0.14 wt% GNPs, (g) þ0.21 wt%
GNPs and (i) þ0.54 wt% GNPs. (b) (d) (f) (h) (j) are the high magnification image of the selected areas in (a) (c) (e) (g) (j), respectively.

could also be inhibited by using graphene with fewer defects. GNPs. After addition of 0.54 wt% GNPs, the yield strength of com-
Regardless of the extrusion treatment, the yield and tensile posites has been increased 116% and 228% before and after the
strength of GNPs/Al composites were increased with the amount of extrusion, while the tensile strength of composites has been
 W. Yang et al. / Journal of Alloys and Compounds 732 (2018) 748e758
Fig. 12. Bridging and pulling-out of the GNPs in the GNPs/Al composites before and after the extrusion treatment, respectively. (a) Bridging of the GNPs, (b) Pulling-out of the GNPs.
increased 45% and 93% before and after the extrusion, respectively.
The fracture surface of the GNPs/Al composites before the extrusion
treatment was mainly characterized by the lamellar structure,
while the fracture surface of the GNPs/Al composites after the
extrusion treatment were mainly characterized by the fine equi-
axed structure. Moreover, the bridging and the pulling-out of the
GNPs were mainly found in the GNPs/Al composites before and
after the extrusion treatment, respectively, implying that the
strengthening effect of GNPs has been utilized more fully after the
extrusion treatment. Based on the modified shear-lag model, the
strengthening mechanism of the GNPs/Al composites has been
discussed, and the effect of GNPs and the extrusion treatment on
the yield strength of the composites have been analyzed.
Acknowledgments
This work was supported by the National Natural Science
Foundation of China (grant numbers 51501047, 51771063 and
51571069), China Postdoctoral Science Foundation (grant number
2016M590280 and 2017T100240), Hei Long Jiang Postdoctoral
Foundation (grant number LBH-Z16075) and the Fundamental
Research Funds for the Central Universities (grant numbers
HIT.NSRIF.20161 and HIT. MKSTISP. 201615).
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