Afsaneh Dorri Moghadam

Composites Part B 77 (2015) 402e420
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Composites Part B
journal homepage: www.elsevier.com/locate/compositesb
Mechanical and tribological properties of self-lubricating metal matrix

nanocomposites reinforced by carbon nanotubes (CNTs)
and graphene e A review
Afsaneh Dorri Moghadam 1, Emad Omrani*, 1, Pradeep L. Menezes, Pradeep K. Rohatgi
Department of Materials Science and Engineering, College of Engineering & Applied Science, University of Wisconsin, Milwaukee, WI 53211, USA
a r t i c l e i n f o a b s t r a c t
Article history: Rapid innovation in nanotechnology in recent years enabled development of advanced metal matrix
Received 5 November 2014 nanocomposites for structural engineering and functional devices. Carbonous materials, such as graphite,
Received in revised form carbon nanotubes (CNT's), and graphene possess unique electrical, mechanical, and thermal properties.
20 February 2015
Owe to their lubricious nature, these carbonous materials have attracted researchers to synthesize
Accepted 3 March 2015
lightweight self-lubricating metal matrix nanocomposites with superior mechanical and tribological
Available online 11 March 2015
properties for several applications in automotive and aerospace industries. This review focuses on the
recent development in mechanical and tribological behavior of self-lubricating metallic nanocomposites
Keywords:
A. Metal-matrix composites (MMCs)
reinforced by carbonous nanomaterials such as CNT and graphene. The review includes development of
B. Wear self-lubricating nanocomposites, related issues in their processing, their characterization, and investi-
B. Mechanical properties gation of their tribological behavior. The results reveal that adding CNT and graphene to metals decreases
E. Powder processing both coefficient of friction and wear rate as well as increases the tensile strength. The mechanisms
E. Self-lubricating involved for the improved mechanical and tribological behavior is discussed.
© 2015 Elsevier Ltd. All rights reserved.
1. Introduction due to their outstanding properties, such as lightweight, high

strength, high specific modulus, low thermal expansion coefficient,
Composite materials are engineered or naturally occurring and good wear resistance [5]. Depending on final desired properties
materials which contain two or more distinct constituents with of composites, different reinforcements are used as reinforcement
significantly different chemical, physical and mechanical proper- in aluminum matrix composites. Al2O3, SiC, B4C is among the very
ties. The metal matrix composites (MMCs) reinforced by ceramic common particles which are used as reinforcement in aluminum
particles or fibers generally have superior properties, such as high matrix composites.
specific strength and modulus compared to unreinforced alloys. In There are different methods to synthesize particle reinforced
general, composites have the combination of properties of con- MMCs. Generally, these methods are classified into: (1) Solid state
stituents, such as they inherit ductility and toughness of the matrix processing; (2) Liquid state processing; and (3) Vapor deposition.
and high modulus and strength of the reinforcements [1]. In this Two common methods which are applied to fabricate aluminum
regard, the applications of MMCs have been extended to use as matrix composites reinforced by particulate reinforcements in
structural materials in aerospace, automotive, marine and defense large scales are powder metallurgy method (solid state) and casting
industries [2]. (liquid state). In literature, a considerable amount of work has been
In MMCs, different metals or alloys of aluminum, magnesium, devoted to producing aluminum matrix composites by using
copper, or nickel are generally used as matrix materials. Among powder metallurgy and to study their mechanical properties
these matrix materials, aluminum alloys are the most widely used [6e10]. The basic route in the powder metallurgy (P/M) technique,
materials, both in research and industrial viewpoints [3,4]. This is in which all materials remain in the solid state, is mixing the
powders, compacting, and sintering of the compacted part to
achieve the least possible porosities and the highest possible den-
sity. In liquid state methods, the matrix is in the state of a liquid.
* Corresponding author.
E-mail address: [email protected] (E. Omrani). There are different methods of liquid state processing to produce
1
These authors contributed equally to this work. metal matrix composites. These methods include stir casting [11],
http://dx.doi.org/10.1016/j.compositesb.2015.03.014
1359-8368/© 2015 Elsevier Ltd. All rights reserved.
A. Dorri Moghadam et al. / Composites Part B 77 (2015) 402e420 403
pressure infiltration [12], pressureless infiltration [13] and squeeze monolithic alloys, which can be caused by possible nanoparticles
casting [14]. Ünlü et al. [15] investigated and compared the me- agglomeration, in capability of solidification front in capturing
chanical properties of aluminum matrix composites reinforced by nanoparticles (pushing off by growing dendrites), and porosity.
Al2O3 and SiC which are produced both by powder metallurgy Therefore, before these materials can be introduced as an
method and casting. The results show that the mechanical and excellent candidate for conventional metals and alloys, these
tribological properties of composite which are produced by casting challenges in synthesis and processing need to overcome. Gravity
are higher than P/M method. In addition, casting is also a more casting techniques are prone to porosity, which could be one
industrial compatible technique to produce composites in large cause for low yield strength in nanocomposites. However, tech-
scales. niques such as Squeeze Casting can eliminate porosity. Another
Among various reinforcements, recent emerging material, car- factor is the degree to which the particles agglomerate and fail to
bonous materials, is found to have many favorable attributes such achieve uniform dispersion. As far as ultrasonic dispersion is
as high thermal conductivity, low coefficient of thermal expansion, concerned, de-agglomeration depends on how much power can
high damping capacity and good self-lubricant property [4]. The be transmitted to the melt. Therefore, processing technique is
considerable amount of research has been made to study the in- one of the factors which need to be considered in pursuing ad-
fluences of embedding graphite particles into the metal matrix on vances in MMNC's [4].
the tribological properties of aluminum alloys [16e18]. Metal ma- Recently, research has been focused on nano-sized carbonous
trix composites embedded by graphite or carbon fibers have self- materials, such as carbon nanotubes (CNTs) and nano-graphite or
lubricating behavior since graphite act as a solid lubricant [19]. In graphene [1] in order to attain enhanced mechanical, electrical, and
this regard, solid lubricant as reinforcement tends to decrease the tribological properties. For instance, carbon nanotubes have been
friction coefficient of MMCs and improve tribological properties of demonstrated to exhibit ultrahigh strength and modulus, and also
self-lubricating composite compared to composites reinforced by have anisotropic electrical conductivity; when included in a matrix,
ceramic particles. The graphite size, which is commonly used in they could pass on significant property improvements to the
MMCs fabrication and obtaining desired mechanical and self- resulting nanocomposites. Thus, the application of nanotechnology
lubricating properties are in the micron range [1,4,20e25]. to materials science and engineering opens up new opportunity
Generally, size of reinforcement influences the mechanical and research direction for the development of novel smart metal
properties such as strength, ductility and fracture of self- matrix nanocomposites. Carbon nanotubes and graphene possess
lubricating MMCs. By increasing the reinforcement size, tensile exceptional mechanical strength as well as excellent electrical and
strength and ductility decrease simultaneously. MMCs reinforced thermal conductivities, and their incorporation in metallic matrices
by larger particles are susceptible to formation of defects such as leads to composites with higher mechanical, electrical, and mag-
cracking during mechanical testing which results in a premature netic properties. This has been led to an increasing interest in
failure of the composites. Therefore, it is expected to have superior incorporating carbon nanotubes and graphene in MMCs to be the
properties when the reinforcement size is in the nano range. It is most effective reinforcing fillers in synthesizing self-lubricating
expected that by reducing the particle size in MMC's to the range composites for structural engineering and functional devices
of nanosize, some of the limitations such as poor ductility and [28e30]. Table 1 summarizes a list of research on MMCs containing
elongation, poor machinability, and reduced fracture toughness of carbon nanotubes and graphene. Carbon nanotubes and graphene
MMCs can be solved. The reason for significantly improved me- in aluminum and copper alloys based composites enhanced their
chanical properties is due to the combined effect of Orowan strength and tribological properties. The carbon nanotubes and
strengthening and grain refining mechanisms and high tempera- graphene were observed to reduce the grain size in aluminum al-
ture creep resistance properties could make metal matrix nano- loys, resulting in an additional higher strength. The incorporation of
composites (MMNCs) very attractive, especially when lightweight carbon nanotubes and graphene also increases the effectiveness of
metals such as Al or Mg are used as the matrix material. The pure aluminum.
strengthening mechanisms which are involved in enhancing me- Extensive researches have been done on polymer matrix com-
chanical and tribological properties of nano particle reinforced posites reinforced by graphene in the last two decades. Almost all of
metal matrix composites have been discussed carefully elsewhere these researches have shown that by adding graphene as rein-
[4,26]. To briefly discuss, there are a few common different forcement to a polymer matrix, the properties of polymer matrix
mechanisms that have been suggested to enable increased composites tremendously improved [37e42]. Tang et al. [37] have
strength in metal composites; (1) Orowan strengthening from shown that by adding 1 wt% graphene as reinforcement to poly-
dislocation bowing by reinforced particles, (2) HallePetch vinyl alcohol, the tensile strength and tensile modulus increased by
strengthening from grain refinement, (3) Forest strengthening 178% and 139%, respectively. Additionally, only a very low volume
resulting from the Coefficient of Thermal Expansion (CTE) fraction of graphene platelets (GPLs) increases the dielectric con-
mismatch between matrix and particles, and (4) Taylor strength- stant of polymer matrix composite. It has been also reported that by
ening by modulus mismatch between matrix and particles. combining GPLs and BaTiO3 and incorporating them into polymer
MMNCs will benefit from the Orowan mechanism only if a matrix, the highest dielectric constant was reached without scari-
dispersed second phase of nanometer size could be attained. fying the low dissipation factor [38]. Graphene based materials
HallePetch strengthening will in general one of the mostly active provide high thermal conductivity enhancement as well as the
mechanisms which improve strength of MMNCs by incorporation advantage of improving barrier properties in comparison with
of nanoparticles. Usually, the addition of nanoparticles refines polymer matrix composites reinforced by CNTs [39,43]. Although,
grains or confines grain growth. CTE and modulus mismatch are numerous polymer matrix nanocomposites reinforced by graphene
considered to be negligible when compared with Orowan and nano-platelets and CNTs have been studied, still the challenge of
grain refinement in many recent observations [4,23,26,27]. adding nanocarbonous materials into a metallic matrix and syn-
Theoretically, it has been shown that the nanosized particles thesize a fully uniform and dispersed structure is remained open to
can result in dramatic improvements in light of the very low researchers [41,44e47]. At the same time, another important pro-
proportion to the quantities they are added. However, the cessing issue in metal composite fabrication is the low interfacial
strength achieved in most solidification processed and powder strength between the CNTs and the matrix. In CNT/polymer
metallurgy nanocomposites are still below the conventional nanocomposites, CNTs and polymer interact a molecular level
404 A. Dorri Moghadam et al. / Composites Part B 77 (2015) 402e420
Table 1
Research reported in literature on metal matrix/nanocarbonous (including carbon nanotube and graphene) composites.
Matrix Reinforcement Process Properties Ref.
Aluminum Graphene Powder metallurgy technique Increasing the tensile properties by embedding [31]
0.3 wt% graphene while graphene particles were
pulled out from the fracture surface
Aluminum Graphene Mixing AA2124 powder and graphene Increasing the hardness and decreasing [32]
platelets and then cold compaction the relative density. On the other hand,
at 525 MPa pressure there is an optimum point that wear
rate is minimized.
Copper nanographite Powder metallurgy technique where Copper/nano-graphite exhibit better tribological [30]
nanographite were dispersed in ethanol properties than copper/micro-graphite.
and then copper introduced to solution, Also increasing the volume fraction of reinforcement
after that drying the powder and using tends to improve tribological properties
450 MPa pressure to make composite
Aluminum CNT Synthesizing by hot press and hot No nanotubes damaged. No reaction products at the [33]
extrusion. interface between the matrix and carbon nanotubes.
No significant effect of annealing on the strength,
while the strength of the pure aluminum matrix
decreases with annealing time.
Aluminum CNT Sintering the mixture of aluminum No change in elongation while there is a significant [34]
and CNTs powders in a carbon mold improvement in tensile strength.
under 50 MPa pressure
Aluminum MWCNT High energy ball milling, cold compaction Wear resistance and hardness of composite [35]
and hot extrusion were employed significantly increased while COF decreased.
to synthesizing composite.
Chromium MWCNT Cr/MWNT coatings were electrodeposited Wear rate of composite decreased in compared [36]
from electrolytes with unreinforced chromium
while in the case of CNT/metal these types of bonding are not 2. Properties of carbonaceous nanomaterials
available.
It is expected that by adding graphene nano-platelets to a metal 2.1. Carbon nanotubes (CNT)
matrix, the mechanical and tribological properties would be
enhanced. In literature, only limited researches on metal matrix If a sheet of carbon atoms is rolled, the carbon nanotubes will
composites reinforced by graphene are available [10,31,32,48e53]. forms with a diameter of 1e2 nm which is called single-walled
To the authors' knowledge, so far, aluminum matrix composite carbon nanotubes (SWCNT). Other types of carbon nanotubes are
reinforced by graphene has successfully produced only by powder double- and multi-walled nanotubes with diameters ranging from
metallurgy method [31,48]. Recently, Wang et al. [31] have shown 4 to 20 nm which are formed by rolling 2 or more carbon sheets as
that by adding 0.3 wt% Graphene nano-sheets to the aluminum they are schematically shown in Fig. 1. CNT has unique mechanical
matrix, the tensile strength of composite increased by about 62%. and physical properties as well as lubricant nature. Owe to these
However, Bartolucci et al. [48] have shown that the tensile strength characteristics, it would be a promising candidate as reinforcement
and strain at failure of aluminum matrix composites reinforced by in a metallic matrix to enhance the properties of materials such as
0.1 wt% graphene platelets are less than its pure aluminum matrix. inherent stability at high temperature, high strength and stiffness,
In addition to these two researches, Chen et al. [49] have produced superior electrical and thermal conductivity and improved perfor-
magnesium matrix composite reinforced by graphene nano- mance of metals in industrials components.
platelets. They employed a novel method combining liquid state The results of the Brenner potential in predicting the modulus
ultrasonic processing and solid state stirring to fabricate the com- value of CNTs reveal that the modulus value of CNT is 1060 GPa that
posites. By using this novel method, they reported that the gra- it is very close to in-plane graphing [58]. A study was employed
phene nano-platelets (GNPs) could be dispersed uniformly into using Molecular Dynamic (MD) simulation with a universal force
magnesium matrix. The results showed that the micro hardness of field to measure the stiffness value of SWNTs and this turns into a
magnesium matrix composite reinforced by GNPs has been 1 TPa stiffness value for SWNTs [59]. Researchers have developed
increased by 78% compared to that of pure Mg prepared under the several methods to measure elastic modulus and strength of CNTs
same processing condition. They have also shown that the GNPs and one of the key techniques is measuring the amplitudes of
show an excellent strengthening effect on the magnesium matrix thermal vibration of nanotubes. This method measured an average
composite [49,50,54e57]. value of 1.8 TPa for elastic modulus with a large scatter in the re-
Although the emerging research interest in smart materials such sults ranging from 0.4 to 4 TPa. Using a similar technique, the
as self-lubricating composites inspires both academia and industry modulus of 1.25 TPa for MWNTs grown by laser ablation was ach-
that the combination of these carbonous materials and metallic ieved [60].
matrices could potentially create composites that have high ther- Although SWNTs have superior mechanical properties, but yet
mal and mechanical properties as well as exceptional wear resis- they are not employed extensively as a reinforcement because they
tance, there is still a need of understanding the nature, processing, are costly to be produced and purified. On the other hand, MWNTs
and tailoring of these composites. This review initially covers a brief are easier to produce. MWCNTs are composed of number of
introduction of various nano-reinforcements potentially are used in centered layers. One of the drawbacks of using MWNTs is the
self-lubricating nanocomposites. Then, it addresses the current susceptibility of the inner tubes to be pulled-out of the outer tube
progress of research in self-lubricating nanocomposites followed by tensile stresses. This phenomenon is usually referred as “tele-
by discussing the effect of these reinforcements on tribological scoping effect” or “telescopic extension of multiwall carbon nano-
properties. tubes”. In-situ TEM measurements on nanotubes demonstrated
Fig. 1. Single-, double-, and multi-walled CNTs.
that this phenomenon occurs at ultra-low-friction state which 5e100 nm are very common in the fabrication of metal matrix
revealed no wear or fatigue on the atomic scale. Telescoping failure composites. Since, graphene in its single layer form cannot be easily
and the higher probability of defects in MWNTs make them less be stable in the free State, usually GNPs are used as reinforcement
favorable compared to SWNTs. However, still the strength and then the sheets are exfoliated to achieve a single layer
measured in MWNTS is much higher than that of high strength dispersed graphene in a matrix. This inexpensive material pos-
metals such as steel [61,62]. sesses good thermal conductivity, electrical conductivity, me-
chanical strength and more surface area than the expensive carbon
nanotubes (CNTs).
2.2. Graphene
Graphene is two-dimensional single atomic carbon sheet of sp2- 3. Self-lubricating nanocomposites

bounded in which atoms densely packed in a honeycomb lattice.
Graphite, the most common form of carbon, is stack of several During relative motion of two surfaces, different types of wear
graphene sheets along the c-axis with an interlayer spacing of mechanisms, including adhesive wear, abrasive wear, delimitation
0.34 nm. The bonding between carbon atoms is very strong while wear, erosive wear, fretting wear, fatigue wear, and corrosive/
there are weak van der Waals interactions among the layers. In oxidative wear may occur. The nature of wear mechanisms can be
terms of thermodynamics, it was thought that exfoliation of layered understood by studying the worn surfaces of materials. At low
graphite to freestanding atomic layer would not be possible [52]. loads and sliding speeds, abrasion is the dominant wear mecha-
However, to date different approaches have been developed for nism while at higher loads, the wear mechanism changes to
synthesizing graphene in large quantities, including thermal delamination. Presence of grooves on the worn surfaces of the
evaporation of silicon carbide [63,64], chemical vapor deposition composites in the sliding direction at low normal loads shows that
(CVD) of graphene on metal carbides or metal surfaces [65,66], and the abrasion wear mechanism becomes dominant.
wet chemical synthesis of graphene oxides followed by reduction Graphite is well-known reinforcement for metal matrix com-
[67,68]. posites which acts as solid lubricant and makes the composite as
The yield strength predicted for a single graphite layer using MD self-lubricating composites [1,4,22,30,75,76]. When graphite is
simulation has reached an extreme value of 0.912 TPa [69]. Another embedded into a metal matrix, the friction and wear behavior of
study employed quantum mechanical approach revealed that the metal/graphite composite significantly improves compared to un-
elastic modulus for armchair graphene and zigzag graphene are reinforced metal which lead to their increased industrial applica-
1.086 and 1.05 TPa, respectively [70]. The Young's modulus and tions where tribological properties are dominant. Damage
intrinsic tensile strength of graphene monolayer were experi- accumulation will be reduced in the presence of graphite particles
mentally tested by using nano-indentation of the atomic force and hence decrease the wear rate of metal matrix insignificant
microscope (AFM). The Young's modulus and intrinsic tensile extent. MMCs reinforced by graphite particles or fibers are potential
strength obtained using these techniques are 1.1.02 TPa and structural materials for aerospace and automotive owe to their
130 GPa, respectively [71]. By using the same method, mechanical excellent tribological properties.
properties of graphene bilayer and trilayer have been determined Among many alloys, aluminum based composites are exten-
where Young's modulus is 1.04 and 0.98 TPa and intrinsic tensile sively used in various industries because of high strength to weight
strength is 126 and 101 GPa, respectively [72]. These supreme ratio, superior tribological properties, and good corrosion re-
mechanical properties of graphene along with extreme thermal sistivity. The explanation for the superior tribological properties of
conductivity (5000 W m1 K1) [73], and super charge-carrier aluminum/graphite composites can be explained by the wear
mobility (200,000 cm2 V1 s1) [74] makes them an attractive mechanisms which occur in these systems. Aluminum alloys have
material for researchers in the last decade to employ them as low yield stress and deforms extensively during sliding contact
reinforcement into a metal matrix. The graphene has a plate shape; while graphite particles in aluminum/graphite composite improve
dispersion in any kind of matrices is easier in comparison with the deformation and fragmentation of the surface and sub-surface
CNTs. Hence, the graphene too is a good substitution for CNTs as by providing a continuous film of graphite on the contact surfaces
reinforcement for metal matrix composites [31]. Although gra- after short running-in period. The graphite film hinders direct
phene is defined as graphite single layers, graphene nanoplatelets metal to metal contact and hence prevents seizure. Despite of good
(GNPs) or graphene nanosheets (GNSs) which are short stacks of tribological behavior of metal/graphite composite, poor mechanical
platelet-shaped graphene sheets with an average thickness of the properties is the disadvantage in the graphite reinforced MMCs.
Fig. 2. Comparison between aluminum matrix macro and nanocomposites reinforced by 15 vol% Al2O3 [80].
These composites sometimes have lower mechanical properties matrix micro-composites, as it is also experimentally confirmed
than unreinforced alloy [1,77]. In addition, graphite has a reverse and the results are presented in Fig. 2 [1,79,80]. More specifically,
effect on electrical conductivity when copper alloys are reinforced the composite reinforced by nanoparticles (graphene) has lower
by micron sized graphite due to be hindering effect of particles in COF than the composite reinforced by micro particles (graphite).
the continuous copper matrix network, though it has a moderate Also, the hardness of composites reinforced by graphene is found to
electrical conductivity. Another feature that causes to reduce be higher than the composite reinforced by CNTs [4]. Worn surface
electrical conductivity of copperegraphite composite is the poor observation suggested that the dominant wear mechanism for non-
interface bonding between copper and graphite particles which reinforced pure Al specimen has been delaminating wear accom-
leads to more electron scattering [30]. Due to these shortcomings in panied by some adhesive wear mechanism. However, worn sur-
using graphite as reinforcement in metals, incorporation of nano- faces of the nano-particle reinforced composites were smoother
sized carbonous materials sought to be promising. and the total depth of deformations were smaller, grooves were
In general, it is desirable in terms of mechanical properties to finer than the unreinforced aluminum alloy matrix specimens
have matrix grain size in the range of nanometer to achieve [81,82].
enhanced hardness, yield strength, and tribological properties such There is a great challenge in introducing carbonous materials to
as wear resistance and friction coefficient [78]. Using nanosize metal matrices. Generally, molten aluminum is not able to wet
particles as reinforcement also enhances both Young's modulus and carbonous materials, such as carbon fibers (CFs), graphite particles,
tensile strength of composites as well as improving tribological carbon nanotubes (CNTs) and graphene where the contact angle of
performance. Due to the fact that nanocarbonous materials have molten aluminum with graphite is between 140 and 160 [83]. The
superior physical and mechanical properties, they have recently reason for high contact angle between carbonous materials and
employed as a novel reinforcement for self-lubricating metal ma- molten aluminum is due to the high surface tension of aluminum in
trix nanocomposite. Superior properties of MMNCs reinforced by liquid state. The surface tension of molten aluminum and carbon
carbon nanomaterials is due to metallurgical factors, such as nanotubes are 955 mN/m and 45.3 mN/m, respectively [84]. The
HallePetch effect by grain size refinement, Orowan looping and very high value of the surface tension of molten aluminum
dislocation generation resulting from thermal mismatch between compared to carbon nanotubes makes synthesis of aluminum
the matrix and reinforcements [52]. Previous studies revealed that matrix composite reinforced with carbonaceous materials a chal-
the MMCs with smaller size reinforcements exhibit lower coeffi- lenging task. One of typical way to improve wetting behavior of
cient of friction and wear rate, thus, it was concluded that the molten aluminum on carbonous materials is by forming metallic
MMNCs have excellent tribological properties rather than metal coatings, such as copper and nickel on reinforcements to reduce its
Fig. 3. a)Optical image after sessile drop of aluminum droplet on graphite substrate showing non-wetting behavior b) Wetting of molten aluminum on copper-coated graphite
substrate after the wetting angle reaches a nearly steady state [83].
contact angle, as shown in Fig. 3 [85,86]. The formation of Al3Ni, through using these techniques is usually weak, which causes the
Al3Ni2 and CuAl2 as an intermetallic compound plays a key role in load transfer ineffectiveness.
achieving good wettability between aluminum with copper and The potential energies of interaction between two parallel
nickel [28,87]. In the following sections, self-lubricating metal/CNT infinitely long carbon nanotubes of the same diameter can be
and Metal/Graphene (single layer or nanoplatelets) nano- simplified greatly by assuming only van der Waals interactions in
composites have been introduced and their mechanical properties graphitic systems. For a pair of parallel carbon nanotubes at a dis-
are discussed. tance of about 0.315 nm the cohesion energy has been calculated to
be about 37 kT nm1. So, an agglomerated CNT bundle needs about
120 kT nm1 since three tubeetube contacts have to be broken to
3.1. Metal-CNTs nanocomposites
separate a tube from a bundle. On the other hand, carbonecarbon
bond energies lie about 190 kT. From this standpoint, it can be
The shear lag models, used in the case of conventional fiber
concluded that the strong cohesion and very small difference be-
reinforced composites, have also been applied to CNT composites.
tween carbonecarbon covalent bond energy, and CNTeCNT van der
The stress is transferred to the fiber (sf) through the interface and is
Waals energy, dispersing nanotubes is a difficult task which needs
related to the shear stress (tmf) between the fiber and matrix given
careful considerations. In polymer matrix composites, generally,
by:
ultrasonication aqueous media combined with an appropriate
lf sf surfactant is a technique to de-agglomerate CNTs. However, the
¼ (1) task becomes more sophisticated in metals processing. Although
Df 2tmf
high intensity ultrasonication during liquid metal processing has
been employed in synthesizing nanocomposites, but still no
where lf and Df are the length and diameter of the CNT, respectively.
experimental or simulation data is available in CNT reinforced
Carbon nanotubes with a larger aspect ratio assist larger load
nanocomposites confirming the complete and successful disper-
transfer and hence efficient utilization of reinforcement. For a
sion of these reinforcements in a metallic matrix [93e96].
critical length lc, the value of sf becomes equal to the fracture
In late 1990s, Kuzumaki et al. [33] fabricated aluminum/5 vol%
strength of CNTs. For nanotube lengths l < lc, the fracture strength
CNT and aluminum/10 vol% CNT composites by mixing aluminum
of the composite is given as:
powders and carbon nanotubes in ethanol followed by hot pressing
and extrusion. However, no improvement in tensile strength of
l
sFrac
C ¼ Vf sFrac
f þ Vm sFrac
m (2) aluminum/5 vol% CNT and aluminum/10 vol% CNT was reported in
2lc
comparison to pure aluminum due to the poor dispersion of
Dislocation generation by thermal expansion mismatch be- nanotubes in aluminum matrix. Different factors, such as type of
tween matrix and CNTs and also Orowan looping mechanism play nanotubes, functionalization of nanotubes, nanotube contents,
an important role in strengthening of aluminum/CNTs composites matrix materials, and milling times can significantly affect the
[88]. To achieve the theoretical value of strength prediction, uni- dispersion of CNTs in a metallic matrix. Generally, to achieve a
form dispersion of CNTs in the matrix during synthesizing is a great uniform dispersion of CNTs in the final composite, a homogenous
challenge [89]. Many attempts have been done in synthesizing distribution of CNTs in the powder mixture at the starting stage is
CNTs reinforced metal matrix composites using traditional liquid an important factor [52]. Uniform dispersion of CNTs in matrix
casting or powder metallurgy processes which have not shown tends to increase the hardness of composites compared to unre-
promising results [90e92]. In case of liquid mixing due to the poor inforced pure aluminum. If only a small amount of CNT is
wetting properties of CNTs and graphene with liquid aluminum embedded into a metal matrices, the hardness of the composite
and the difference in their densities, CNTs and graphene immedi- increases due to the fact that the micro voids of metal matrix will be
ately float to the surface without being mixed. In P/M route and hot filled by CNTs. Beyond a specific CNT volume percentage, the excess
pressed sintered aluminum CNT composites, CNTs cause a CNTs which were not able to fill the micro voids will be agglom-
tremendous amount of residual stress in aluminum matrix which erated with the aluminum particles. This agglomeration interrupts
cause a lower the tensile strength in the non-annealed composites the complete sintering and leads to the formation of defects which
than that of pure aluminum. Additionally, the bonding obtained ultimately results in gradual reduction in hardness [97,98].
Fig. 4. Variation of (a) relative density and hardness, and (b) tensile strength and elongation with carbon nanotube content for AA2024/MWNT nanocomposites [29].
Deng et al. [29] have investigated the physical and mechanical electrochemical deposition, metal evaporation, and hydrogen
properties of aluminum AA2024/MWNT nanocomposites synthe- reduction of metallic salts-graphite composite [103e105]. Howev-
sized by cold isostatic press followed by hot extrusion. During er, so far fully exfoliated graphite flakes have not been obtained.
synthesis, AA2024 powders and MWNTs were first mixed in Additionally, the difficulty in large-scale synthesis of these com-
ethanol using ultrasonic mixing. Then, ethanol evaporated and the posites becomes an obstacle in their production.
dried mixture ball milled and finally cold isostatic pressing and hot The powder metallurgy (P/M) route which is recently widely
extrusion at 450 C were performed. Fig. 4a shows the changes in developed for the fabrication of aluminum/CNT composites can be
relative density and Vickers hardness with CNTs content. By considered as an applicable pathway to fabricate aluminum/GNS
increasing the weight percentage of CNTs up to 1 wt% of MWNT, the composites. Graphene oxide (GO) nanosheets have hydroxyl and
relative density and hardness of the nanocomposites increase. It epoxy groups on its surface which helps to have better dispersion in
can be clearly seen that the relative density of nanocomposite solvents and form more stable solutions than graphene. That makes
containing 2 wt% MWNT sharply dropped which could be due to the GO nanosheets a more favorable reinforcement rather than
the formation of nanotubes clusters. As shown in Fig. 4b, tensile GNSs [106]. Fig. 5 shows the main difference between graphene and
strength and elongation of aluminum/CNT composites depict the GO. Wang et al. [31] reported a route in synthesizing aluminum/GO
same trend as the relative density. The AA2024/1 wt% MWNT composites using powder metallurgy in which four steps are
exhibit maximum elongation and tensile strength and there is a involved:
drop in mechanical properties at high amount of reinforcements.
Noguchi et al. [99] developed a two-step method in which (1) Exfoliating GO into several-layered or single-layered nano-
initially CNTs were uniformly dispersed in an elastomer matrix; sheets by sonicating GO aqueous dispersion in deionized
and in the second step, the elastomer matrix was displaced by Al. water.
Low-energy ball milling in a Turbula mixer followed by hot (2) Aluminum flakes surface modification through ball milling
compaction, sintering and HIPing was another route which was followed by introducing a hydrophilic membrane on the
used to homogenize the mixture Al/CNTs and eliminate CNT clus- surface of the aluminum flakes such as PVA.
tering. Esawi et al. [100], showed the effect of mixing time and (3) Adsorption and reduction of GO nanosheets by adding the
mixing speed on CNT cluster size using dry mixing in a Turbula powder slurry of modified aluminum flakes in deionized
mixer. He et al. [101] were also developed an in-situ route to syn- water to the GO aqueous dispersion. The mixed slurry color
thesize CNTs inside the aluminum matrix by using a three-step changes from brown to transparent during stirring. Heating
process including deposition-precipitation, reduction, and chemi- the aluminum/GO composite powders decompose the hy-
cally vapor deposition route. They have reported that the first step drophilic membrane and reduce the GO nanosheets to GNSs,
involves producing a Ni(OH)2eAl precursor through a deposi- until finally aluminum/GNS composite powders is obtained.
tioneprecipitation route. In their method, Ni nanoparticles were (4) Compacting and consolidation of aluminum/GNS composite
used as catalyst on which the CNTs will grow. Therefore, by uniform powders. Consolidation can be achieved by sintering in an
distribution of Ni nanoparticles on the surface of Al powders, a argon atmosphere followed by hot extrusion.
uniform distribution of CNTs could be guaranteed. Cha et al. [89]
used another technique to mix CNTs and matrix material in a so- Bastwros et al. [10] used graphite and exfoliated it to graphene
lution. In their fabrication process which basically involves in nitric acid and sodium chlorate solution. The intercalated
molecular-level mixing of CNTs and the matrix material, a sus- graphite was achieved through sedimentation and finally the
pension of reinforcements, and dissolved metal ions in ethanol or intercalated graphite was exfoliated to monolayer or few-layer
water is prepared. Then the suspension was dried and oxidized
metal powders forms. Finally, the metal oxides are reduced under
control atmosphere to achieve a dispersed CNT reinforced metal
matrix composite.
3.2. Metal-graphene nanocomposites
Similar to aluminum/CNT composites, in order to achieve the

full potential of graphene nanosheets (GNSs) as reinforcement, a
homogenous distribution of GNSs in the aluminum matrix along
with maintaining the structural integrity of the GNSs is essential.
Aggregated graphene behaves no differently than particulate
graphite platelets. The ultrahigh surface area that can be obtained
in a 2D graphene sheet is lost when these sheets are clustered
[53,102]. In this regard, the main challenge in fabricating metal/
graphene nanocomposites is to find an approach to fully disperse
these sheets or exfoliate the single sheets of GNS to graphene
monolayer. Although, exfoliation of GNSs in polymeric matrices has
been studied extensively and successful results have been achieved,
but yet in a metallic matrix it has been remain as the key challenge.
The main obstacle in achieving a highly exfoliated structure in
metal-graphene nanocomposites is the high difference between
carbon and metals surface energies. This high surface energy dif-
ference does not let metal to easily wet the graphene sheets and fall
them apart. Several investigations have been carried out to find the
best route to synthesize a fully dispersed and homogenous gra-
phene reinforced metal matrix composite including Fig. 5. Surface structure of the graphene and GO.
graphene oxide using ultrasonication. Then, they employed ball extrusion [31]. The normalized tensile strength and ductility of Al/
mill to mix Al6061 powder and graphene at different milling times. GNS composites in comparison with unreinforced pure matrix is
The composites were then synthesized by hot compaction in the shown in Fig. 7a. The tensile strength of aluminum/GNS nano-
semi-solid regime of the Al6061. Ghazaly et al. [32] have synthe- composite is 249 MPa. The nanocomposite showed a significant
sized the aluminum graphene at different weight percentage (0.5, 3 improvement (about 62%) in tensile strength compared to that of
and 5 wt%) by employing powder metallurgy technique. Aluminum unreinforced aluminum matrix (154 MPa). Higher tensile strength
powder with the graphene nanosheets were mixed in a high energy of nanocomposite compared to unreinforced aluminum demon-
ball mill which resulted in the formation of nonuniform particles of strate that GNSs have a dominant role for increasing mechanical
aluminum covered by graphene layer and disappearance of the properties and reveal that the GNSs have a good potential to be
graphene nanosheets. A combination of cold compaction and hot used as reinforcement in aluminum matrix composites to improve
extrusion at ~0.45Tm (305 C) were employed to synthesize the mechanical properties. Generally, GNSs could contribute to the
aluminum/graphene self-lubricating nanocomposite. The results strength improvement by grain size refinement, dislocation
show a decrease in density of nanocomposites by increasing the strengthening and stress transfer. GNSs hinder grain growth and
amount of graphene as shown in Fig. 6. Also, the variation of hence result in having grain refinement and also provide resistance
hardness with increasing the amount of graphene is presented in to the dislocation movement during thermal processing and plastic
Fig. 6. As there was an expectation that addition of graphene up to
3 wt%, the hardness of nanocomposites reinforced by graphene
increase when compared to unreinforced alloy. The 3 wt% graphene
reinforced composite produced a 47.5% increase in hardness over
the base AA2124 alloy. By further increasing the amount of gra-
phene (more than 3 wt%) nanocomposite, the hardness reduces but
the hardness values are more than the unreinforced alloy and less
than the composite with reinforcements between 0.5 and 3 wt%. By
comparing Figs. 4 and 6, it is obvious that aluminum/graphene has
superior mechanical properties than aluminum/CNT.
To achieve individual graphene sheet, according to many avail-
able literatures, another method is attaching molecules or poly-
mers to graphene sheets to decrease aggregation [51,107]. Xu et al.
[53] suggested a combined technique in which a solvent, graphene
oxide, and an inorganic nano particle was incorporated to obtain
graphene as individual sheets inside a metal matrix. The inorganic
nanoparticles sits in between graphene sheets and prevent re-
agglomeration of them. . After the solvent is dried, dispersion of
isolated graphene sheets can be obtained having graphitic stacks
with inorganic nanoparticles in the interlayer spacing.
Aluminum/0.3 wt% graphene nanocomposite was also synthe-
sized by using a slurry based process followed by sintering and hot
Fig. 6. Relative density and hardness variations as a function of graphene addition to Fig. 7. a) Tensile properties of 0.3 wt% GNS/Al composite and the corresponding flaky
AA2124 nanocomposite [32]. Al specimen b) Fracture surface of 0.3 wt% GNS/Al composite [31].
deformation, therefore, the tensile strength of aluminum matrix

increase in presence of GNSs. Another important reason of high
tensile strength in presence of GNSs is the load bearing ability
where the graphene tolerate a substantial part of load during
plastic deformation. The fracture surface is shown in Fig. 7b. Inas-
much as the fracture strength of a perfect single layer graphene is
125 GPa, the theoretical strength of the aluminum/graphene is
500 MPa by using the rule of mixtures for aluminum/0.3 wt% GNSs.
The experimental result shows that strength of aluminum/0.3 wt%
GNSs is 250 MPa. The less strength in experimental than theoretical
study is due several parameters, such as to different alignment of
GNSs along the tensile direction, processing parameters, micro-
structure, and weak interfacial bonding of the aluminum/GNSs
[48].
Latief et al. [108] have synthesized aluminum/graphene com-
posites using different percentages of exfoliated graphite nano-
platelets particles by employing powder metallurgy method in
order to study the physical and mechanical properties of nano-
composites. As observed in Fig. 8, the results revealed that the
Vickers hardness (Fig. 8a) and compression strength (Fig. 8c) in-
creases with increasing graphene content up to 5 wt% in the pure
aluminum matrix while the density (Fig. 8b) decreases with
increasing graphene content. This can be expressed by following
equation [109]:
4ð1 f Þr
l¼ (3)
3f
where l, f and r are respectively the distance between the rein-

forcement particles, particles volume fraction, and the particle
radius (particle is assumed spherical). The shear stress for all tested
alloys can also be calculated according to the following equation:
Gb
t0 ¼ (4)
l
where, t0, G and b is the shear stress, the shear module, and the
Burger's vector, respectively [110]. According to Equation (3), it can
be concluded that the distance between the graphene particles
decreases by increasing their amount in the composite. Based on
Equation (4), the shear stress that is required to move dislocations
between the graphene particles will increase when the distance
between the reinforcement particles decreases which results in an
increased yield stress of materials [3,111]. In addition, the re-
inforcements are an obstacle that causes to lock dislocation
movement extremely in metal matrix through dispersion
strengthening mechanism. This mechanism can increase the me-
chanical properties of aluminum matrix composites reinforced by
graphene [109].
Bartolucci et al. [48] have compared the mechanical properties
of aluminum/MWNT and aluminum/GNP composites. Fig. 9 depicts
the hardness of self-lubricating aluminum nanocomposites at
different samples after hot isostatic pressing and extrusion. It is
obvious from the results of hardness that the aluminum reinforced
with 1.0 wt% MWNT exhibits the highest hardness than aluminum/
0.1 wt% graphene and pure aluminum. Fig. 10 shows a compression
between the tensile strengths of composite reinforced by MWCNT
and graphene and also effect of fabrication method including
extruded and pressed composites. The metal matrix composite
reinforced by nanotubes show the higher strength than reinforced
by graphene. For extruded composites, the tensile strength of
Fig. 8. Variation of (a) Vickers hardness, (b) Density, and (c) Compressive strength of
aluminum/nanotubes was about 12 percent greater than the pure aluminum alloys with exfoliated graphite nanoplatelets particles contents for GNP/Al
aluminum while the aluminum/graphene showed about 18 percent composites at different sintering temperature [108].
lower tensile strength as compared to the pure aluminum. In
addition, Fig. 10 shows the average strain-to-failure of the samples
Archad [113] expressed a formula for wear of materials that de-

scribes the volume of wear loss (V) of materials due to adhesive
wear:
PL
V ¼c (5)
H
where c, P, L and H are wear coefficient, applied load, sliding dis-

tance, and hardness of the softest contacting surfaces, respectively.
Usually to avoid friction and consequently deterioration of
material under wear, liquid or solid lubricants are employed.
However, in cases such as high vacuum environment, high-speed
conditions, high applied loads, and very low or high tempera-
tures, liquid and grease type lubricants are undesirable. In such a
tribological systems the common liquid and grease type lubricants
do not show desired performance or durability [52]. Another
approach is replacing the liquid and grease type lubricants with
solid lubricant coatings that they are used to decrease coefficient of
friction and wear rate. The coatings are applied on the surface of
materials by depositing via chemical or physical vapor deposition
Fig. 9. Vickers hardness data for the various materials and conditions [48].
techniques to form a coating layer [114,115]. The disadvantages of
solid lubricant coating are limited lifetime, difficulty in replenish-
where the results revealed samples reinforced by nanotubes and ment, oxidation and aging-related degradation, and poor adhesion.
graphene displayed the lowest ductility. Therefore, to avoid the drawbacks of both the liquid and grease type
lubricants and the solid lubricant coatings, embedding carbonous
materials in the metal matrix seems promising.
4. Tribological behavior of self-lubricating nanocomposites
Generally, metal matrix composites have lower coefficient of
friction (COF) compared to unreinforced matrix [1,4,35,116e118].
Tribology is an investigation on wear and friction performance
Furthermore, adding ceramic particles to the metal matrices lead to
of materials. It is the science of interacting surfaces in relative
an increase in wear resistance of the matrices [1,4,118e121]. The
motion [112]. When under an external load, two materials are in
main reason for increasing of wear resistance of metal matrix
contact with each other, the asperities of two surfaces come into
composite is attributed to low friction coefficient of metal matrix
close contact and during movement, deterioration of the surfaces
composite compared to the unreinforced metals. For conventional
occurs which is known as wear. During the sliding process of softer
metal matrix composites, the reinforcements act as load bearing
materials against harder materials, atoms will be taken off from the
components at contact surface which tend to protect the surface
softer one and these atoms tend to locate themselves in the as-
from ploughing during sliding. Generally, the hardness of rein-
perities of harder surface. As results, a cold welding occurs in
forcement greatly affects the wear loss and hence, the wear volume
contact surface and interatomic junctions across the interface
of MMCs. The wear loss of MMCs depend on several intrinsic
forms. By continuing the sliding process, fracture can take place at
properties such as the reinforcements dispersion state, distribution
the junctions and causes the detachment of the fragments from
of reinforcement, size of reinforcing particles, and interfacial bond
adhering asperities. Friction force causes shear at interatomic
between matrix and particles [52]. When bonding between matrix
junctions during movement of two surfaces under an applied force.
and reinforcement is poor, the hard ceramic particles are easily
pulled out from MMCs and then they will be trapped between the
sliding surfaces and act as third body abrasives and help to increase
worn surface damage and wear rate. Among the composites,
composites reinforced by carbonous materials show better tribo-
logical properties compared to composites reinforced by ceramic
reinforcements, such as SiC and Al2O3 due to the lubricative nature
of carbonous materials that make them a potential reinforcement
for self-lubricating composite. The conventional self-lubricating
composites are embedded by graphite particles or carbon fibers [1].
The main reason for significant decrease in COF and wear rate is
due to formation of a lubricant film between the contact surfaces
because of presence of carbon-based solid lubricant in the MMCs.
Thus, the lubricant film prevents direct contact between sliding
surfaces and reducing wear [77]. In addition, due to the presence of
lubricant film which prevents direct contact, the transfer of atoms
from the asperities of softer surface to the asperities of harder
surface will be reduced that hence, it leads to decrease in cold
welding of atoms of softer materials with atoms of harder materials
during sliding and then subsequent fracture of atomic junctions
[30]. As noted before, although the graphite particles in the metal
matrix improve the tribological performance, it tends to reduce the
Fig. 10. Ultimate tensile strengths and strain-to-failure of pure Al, Ale1 wt% MWNT, mechanical properties of the composites. Hence, recently, the nano
and Ale0.1 wt% graphene [48]. solid lubricants are used as the dominant reinforcement for the
metal matrices in self-lubricating composites. This is because the reasonable cost. Thus, there have been many investigations to
metal matrix composite reinforced by nano solid lubricant have develop MMNCs reinforced with MWCNTs using various fabrication
excellent self-lubricating behavior with low coefficient of friction routes [1]. Previous investigations exhibit superior tribological
and wear rate as well as high mechanical properties [122]. properties of metal/CNTs composites as a result of the reduction in
wear rate and the coefficient of friction (COF) due to the lubricating
nature of CNTs. CNTs form a lubricant film between contact surfaces
4.1. Effect of CNT
during sliding.
It has been reported that when there is a strong bonding be-
Carbon nanotubes (CNTs) are one of the important solid lubri-
tween functionalized MWNTs and an epoxy matrix the outer shells
cants that is increasingly employed in novel self-lubricating
of the tube remain embedded in the matrix following pull-out
nanocomposite materials because of the superior properties of
[123,124]. However, in case of metal matrix, the MWCNTs are
CNT including electrical, optical, and mechanical properties and
attached by a very week van der Waals forces, there is no direct
have a key role in enhancement of wear resistance and reduction in
observation that support the telescopic extension of multiwall
COF of metal matrix composite reinforced by CNTs. Metal matrix
carbon nanotubes occurs. The week bonding between CNT-metal
nanocomposites reinforced by CNT is an excellent candidate for
led to easily slide or roll between the contact surfaces and mini-
industrial applications because of its excellent mechanical proper-
mize a direct contact between the surfaces, thus results in decrease
ties, lightweight and superior tribological properties. It is expected
in friction coefficient of the composite. The improvement in wear
that the utilization of Multi-Wall Carbon Nano Tubes (MWCNTs) in
resistance is attributed to the role of CNTs as spacers that prevent
the composites will increase the industrial applications due to their
Fig. 11. Variations of a) Brinell hardness (HB) b) wear rate and coefficient of friction
with MWNTs content for melt-infiltrated MWNT/AleMg composites under an applied Fig. 12. Effect of volume fraction of CNT on friction coefficient and wear loss of Al/CNT
load of 30 N and a sliding velocity of 1.57 m/s [13]. nano composite at normal load 30 N and sliding speed 0.12 m/s [122].
Fig. 13. SEM images of wear tracks for (a) pure aluminum with a grain size of ~150 nm and composites containing MWCNTs of (b) 1.5 vol%, (c) 3.0 vol%, (d) 4.5 vol%, and (e) 6.0 vol%,
respectively [122].
direct contact between rough surfaces [28]. Generally, several as shown in Fig. 11a. The effect of volume fraction of CNTs on the
material parameters, such as amount of reinforcements, size of friction coefficient and wear rate of the composite is shown in
reinforcement, and spatial distribution have direct effect on tribo- Fig. 11b. It can be seen that although hardness has an optimum
logical properties of self-lubricating metal/CNTs composites [1,125]. value with increasing volume fraction of CNTs in the composite, yet
Zhou et al. [13] fabricated AleMg/MWCNT composite by using a the coefficient of friction decreases even at high CNT content. At
preform with MWCNT and then using pressureless infiltration high amount of CNTs the direct contact between the metal surfaces
method to infiltrate molten metal into the MWCNT preform. is hindered which ultimately results in better tribological proper-
Embedding the MWCNT into AleMg alloy increases the hardness of ties. The favorable effects of CNTs on tribological behavior of
the composites compared to unreinforced aluminum alloy. composites depend on their excellent mechanical properties, well
Furthermore, by increasing the MWCNTs volume percentage, the dispersity in the composite and the efficiency of CNTs as rein-
hardness of composite initially increases. Then, further increase in forcement. X-ray diffraction (XRD) analysis of contact surface re-
MWCNTs content has an adverse effect and decreases the hardness veals that the wear particles are mainly aluminum oxide. During
Fig. 14. Variations of COF of 4.5 vol% MWNT/Al composite with (a) applied load at sliding speed 0.12 m/s and (b) sliding speed at applied load 30 N. Variations of wear loss of 4.5 vol
% MWNT/Al composite with (c) applied load at sliding speed 0.12 m/s and (d) sliding speed at applied load 30 N [122].
delamination. As shown in Fig. 13(a) and (b), grooves and material

delamination were observed on the worn surfaces for pure
aluminum and aluminum reinforced by 1.5 vol% MWCNT. This
would confirm that micro-ploughing and delamination are the two
main dominant wear mechanisms of pure aluminum and
aluminum/1.5 vol% MWCNTs. By increasing the volume percentage
of MWCNTs to 3 and 4.5 vol%, less deep grooves can be observed
and the surface is much smoother compared to the one it was
observed in Fig. 13(c) and (d). The surface of aluminum reinforced
by MWCNTs of 6.0 vol% demonstrates rougher worn surface than
aluminum/4.5 vol% MWCNTs. At this amount of CNT the debris are
able to easily separate out from the surface which can be justified
by presence of pores as shown in Fig. 13(e). This can be the main
reason for increasing of wear loss and COF at high volume per-
centage of MWCNTs. Furthermore, They confirmed that the coef-
ficient friction of aluminum composite significantly decreased by
adding CNTs where COF is 0.35 and 0.06 for pure aluminum and
aluminum/4.5 vol% MWNT, respectively, under an applied load of
30 N and a sliding speed of 0.12 m/s. In addition, there is a variation
between COF and volume content of CNT where COF decrease by
Fig. 15. Wear rate and weight loss variation as a function of graphene content in
AA2124 matrices [32].
increasing the amount of CNTs. The effect of applied load and
sliding velocity on coefficient of friction and wear loss was also
investigated and it is shown in Fig. 14. The investigations have
wear process, laminated oxide films formed at contact surfaces that shown that the COF and wear loss increases with increasing normal
they subsequently broke up and flaked off due to low adhesion load for aluminum/5 vol% MWNT composite at sliding speed of
between the oxide films and aluminum matrix. While the oxide 0.12 m/s. However, the coefficient of friction was still lower than 0.1.
particles which form at contact surface are harder than the At higher load, severe wear is the dominant mechanism which
aluminum matrix and are able to increase abrasive wear. As the results in increasing friction coefficient and wear loss and subse-
aluminum matrix gradually wear out during sliding process, the quently severe surface damage. On the other hand, the coefficient
CNTs which was initially embedded in the matrix now are pulled of friction and wear loss slightly decreases with increasing sliding
out and exposed on the contact surface and form a lubricant film on speed at an applied load of 30 N as shown in Fig. 14.
worn surface. Those solid lubricating films significantly reduce the
adhesive wear cause by oxide particles compared to unreinforced 4.2. Effect of graphene
aluminum.
Choi et al. [122] have shown that the wear loss and coefficient of High strength, lightweight and lubricating nature of graphene
friction decrease with increasing the CNTs content. However, made it suitable as reinforcement for self-lubricating ultrahigh
beyond a critical amount, 4.5 vol% CNTs in their investigation, the strength metal matrix nanocomposites. As this is fairly a novel
wear rate and friction coefficient increase as shown in Fig. 12. The material and it is difficult to uniformly disperse in metals as well as
deteriorated wear properties in the composites at high volume of its complex microstructure, there are only a few studies which
MWCNTs may be associated with the presence of voids and cracks investigated the tribological properties of graphene in a metallic
due to the very high amount of CNTs which could act as a source of matrix. Ghazaly et al. [32] who have investigated the effect of
Fig. 16. SEM micrographs of worn surfaces of AA2124 a) unreinforced, b) 0.5, c) 3 and d) 5 wt% graphene nanocomposite [32].
tribological properties under dry wear test compared to unrein-

forced and other amount of graphene reinforcements as shown in
Fig. 15. SEM micrographs of worn surfaces of unreinforced
aluminum alloy and Al/graphene nanocomposites are shown in
Fig. 16, which clearly demonstrate the presence of longitudinal
grooves in all samples. In addition, by comparing the worn surfaces,
it is obvious that the scratches, craters, and delamination of
AA2124/3wt% graphene composite is less than that of unreinforced
alloy. Thus, unreinforced alloy and AA2124/3wt%graphe-
necompositeare in the severe and mild wear regime, respectively.
Shallow parallel grooves and ridges formed on the worn surface of
AA2124/0.5 and 5 wt% graphene nanocomposite due to micro-
ploughing. Thus, the dominant wear mechanism is severe plastic
deformation of the matrix that results in high wear rate. Entrapped
debris between delaminated surfaces was observed at high
magnification on worn surfaces of unreinforced AA2124 alloy while
there is no wear debris on the worn surfaces of nanocomposite as
illustrated in Fig. 17. Alumina fragmented films or strain hardened
Fig. 17. SEM micrographs for the worn surfaces of AA2124-a) 0, b) 3 and c) 5 wt%
graphene nanocomposite [32].
weight percentage of graphene on mechanical properties, also

studied its effect on wear rate of self-lubricating AA2124 aluminum
alloy matrix nanocomposites. The results showed that self-
lubricating composite reinforced by 3 wt% graphene has better
Table 2
Comparison of physical and mechanical properties between micro graphite particles
and nanographite particle [30].
Composite Relative density Hardness Electrical conductivity

(%) (HV) (%IACS)
Cu-15% Gr 92.3 ± 0.13 72 ± 1.6 65 ± 1.5

Cu-5% NG 95.82 ± 0.14 94 ± 1.9 79.8 ± 1.9
Cu-10% NG 96.41 ± 0.13 90 ± 1.0 72.4 ± 1.0
Cu-15% NG 96.92 ± 0.12 81.5 ± 1.6 70 ± 1.3
Fig. 18. Variation of a) Coefficient of friction with normal load at sliding speed 0.77 m/s
Cu-20% NG 88.42 ± 0.15 56 ± 2 38.7 ± 2.5
b) Variation of coefficient of friction with sliding speed at 36 N [30].
Inasmuch as copper has good electrical and thermal conduc-

tivities and graphite has lubricious nature, copper/graphite com-
posites have variety of application in industries. Conversely, the
mechanical properties of copper composites decrease in the pres-
ence of graphite reinforcement. To solve the impact of micro sized
graphite particles, Rajkumar et al. [30] employed powder mixing,
compaction and microwave sintering methods to synthesize cop-
per nanocomposite reinforced by nano-graphite (NG) particles
with an average particle size of 35 nm to form copper/5e20 vol%
NG nanocomposites. The graphite particles were coated with cop-
per using electrodeless plating method. The nanographite particles
have not been exfoliated in this investigation and cannot be
considered as single or “few layer” graphene sheets. Table 2 com-
pares the physical properties, such as relative density and electrical
conductivity and also mechanical properties, such as hardness of
sintered copper/graphite composite and copper/nano-graphite
composites. As comparison shows, the nanocomposites had bet-
ter hardness and electrical conductivity compared to micro-
composites. As stated earlier, the volume percentage of nano-
particles has an effect on physical and mechanical properties of
Fig. 19. Variation of wear rate of composites with normal load at sliding speed 0.77 m/
self-lubricating composites. The amount of nano-particles is also
s [30].
influence the relative density as shown in Table 2. The relative
density increases with increasing the volume percentage up to
particles are the two main sources of debris. This debris is from the 15 vol% of nano-graphite due to ability of nanoparticles to fill up the
heavily milled consolidated powders which were detached under porosity cavities. When the nano-graphite amount is increased
the load during the wear test. By comparing the worn surfaces at over 15% volume fraction, the relative density and hardness
high magnifications, it is obvious that the surface of nanocomposite reduced due to the reduction in the distance between particles,
containing 3% graphene is smoother than that of unreinforced alloy which consequently facilitate nanoparticles agglomeration.
and the composite reinforced with 5wt%graphene. Furthermore, Fig. 18 illustrates the variation of normal load and sliding speed
the surface of AA2124/3 wt% graphene composite was covered by with coefficient of friction at different volume percentage of
lubricant films that results in reducing friction and wear due to the graphite particles. Fig. 19 shows the variation of wear rate with
soft nature of the lubricant film. Conversely, deep grooves and se- normal load for copper based composites reinforced by micro and
vere damage exist on the worn surfaces of AA2124/5 wt% graphene nanographite particles. Results revealed that, at constant volume
composites which delaminated in the direction of sliding that ex- fraction, embedding nano-particles decreases the coefficient of
plains the significant increase in wear rates and weight loss. friction and wear rate compared to the composite reinforced by
Fig. 20. SEM image of worn surface of coppere15% nanographite composites at different sliding speeds at 36 N a) 0.77 m/s, b) 1.77 m/s and c) 2.77 m/s [30].
micro sized graphite particles. Higher hardness, lower porosity and to incomplete spreading of graphite at the contact zone, and hence,
finer microstructure are the reason for the improved wear resis- increases the wear rate. Increasing of COF at high volume fraction of
tance of nano-graphite reinforced composites. Further, the nano- nano-graphite is a result of increasing the deformation and fracture
graphite particles reinforced composites are more effective on the at the contact surface of copper matrix and increasing the amount
degree of self-lubrication compared to micron-size graphite parti- of copper debris at contact surfaces.
cles reinforced composites. The amount of nano-graphite particles It can be seen from Figs. 18 and 19 that the wear rate and co-
also influences the tribological properties of self-lubricating copper efficient of friction both increase with increasing applied load while
composites. The increase in volume percentage of nano-graphite up the coefficient of friction decrease with increasing the sliding
to 15 vol% tends to decrease the wear rate and COF because of the speed. Increasing normal load also increases the amount of copper
formation of a uniform and continuous layer of solid lubricant film. wear debris at the contact zone and hence influences the rate of
This lubricant film reduces the rate of deformation of the matrix increase in the coefficient of friction with normal load. In these
and improves the tribological behavior. When the amount of figures, it can be seen that the coefficient of friction of self-
reinforcement increases, the decrease in the COF is associated with lubricating composite significantly decreases with increasing the
increase in the availability and uniformity of lubricant layer. The sliding speed up to 1.77 m/s because of formation of uniform
lubricant layer causes to minimize the metal to metal contacts lubricant film. By increasing the sliding speeds beyond 1.77 m/s, the
between the copper matrix composite and steel counter surface. In coefficient of friction slightly increase or become constant for 5 and
contrast, when the volume fraction of nano-graphite is more than 10e15 vol%, respectively. This is due to peel off of the self-
15 vol%, a large amount of agglomeration was observed that tends lubricating film on the contact surface at high sliding speed.
Fig. 21. a) Distribution of nanographite in matrix, b) distribution of graphite in matrix, c) contact profile nanographite composite, d) contact profile of graphite composite, e) and
f) conceptual wear generation model for nanographite and graphite reinforced composite respectively, g) and h) typical wear debris at 48 N and 0.77 m/s for copperenanographite
and copperegraphite respectively [30].
Furthermore, sliding speed does not affect the coefficient of friction and reinforcements, and also Orowan looping mechanism. Further,
of copper/nano-graphite with high amount of nano-graphite con- a few research papers are available on tribological behavior of self-
tent due to the contact surface that is uniformly covered with the lubricating nanocomposites reinforced by graphene and CNTs.
highly adherent graphite layer. As shown in SEM micrograph of A significant reduction in wear rate and coefficient of friction can be
worn surface at different sliding speed, at constant normal load, in achieved in presence of CNTs and graphene up to a critical volume
Fig. 20, the lubricant film on copper/15 vol% nano-graphite is not fraction. The reinforcements prevent a direct contact between two
continuous at lower sliding speed. While increasing the sliding surfaces by forming a lubricant film between the contact surfaces.
speed, a lubricant layer uniformly form on the surface of composite Beyond a critical volume fraction of CNTs and graphene, the wear
that decreases COF as a direct result of a decrease in direct surface rate and COF increases. At higher amount of reinforcement, the
to surface contact. However, a gradual increase in COF was mechanical properties also decrease due to agglomeration that
observed for 20 vol% of nano-graphite composite by increasing the leads to the formation of some defects which ultimately decrease
sliding speed that it leads to lower mechanical properties such as the tribological performance of the nanocomposites. Several ma-
hardness due to increase in temperature at the interface. Further, it terial parameters, such as amount of reinforcements, size of rein-
tends to more grain fracture during sliding. This phenomenon is forcement, and spatial distribution have an effect on mechanical
more intensive at higher sliding speeds. and tribological properties. There is an optimum amount of rein-
The mechanism of wear under normal loads suggested by forcement in the composites to have excellent mechanical and
Huang et al. [126]. Fine graphite particles form an adherent layer at tribological properties.
the contact zone and under high normal loads; these nano-graphite
from composite is squeezed out to the contact zone. Owe to their
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Composites Part B 77 (2015) 402e420

Contents lists available at ScienceDirect

Mechanical and tribological properties of self-lubricating metal matrix

1. Introduction due to their outstanding properties, such as lightweight, high

Matrix Reinforcement Process Properties Ref.

Fig. 1. Single-, double-, and multi-walled CNTs.

Graphene is two-dimensional single atomic carbon sheet of sp2- 3. Self-lubricating nanocomposites

3.2. Metal-graphene nanocomposites

Similar to aluminum/CNT composites, in order to achieve the

deformation, therefore, the tensile strength of aluminum matrix

where l, f and r are respectively the distance between the rein-

Archad [113] expressed a formula for wear of materials that de-

where c, P, L and H are wear coefﬁcient, applied load, sliding dis-

delamination. As shown in Fig. 13(a) and (b), grooves and material

tribological properties under dry wear test compared to unrein-

weight percentage of graphene on mechanical properties, also

Composite Relative density Hardness Electrical conductivity

Cu-15% Gr 92.3 ± 0.13 72 ± 1.6 65 ± 1.5

Inasmuch as copper has good electrical and thermal conduc-

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