CARBON x x x ( 2 0 1 1 ) x x x –x x x

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Suppression of wear in graphene polymer composites

Sashi S. Kandanur a, Mohammad A. Rafiee a, Fazel Yavari a, Michael Schrameyer a,

Zhong-Zhen Yu c, Thierry A. Blanchet a,*, Nikhil Koratkar a,b,*
a
Department of Mechanical, Aerospace and Nuclear Engineering, Rensselaer Polytechnic Institute, 110 8th Street, Troy, NY 12180-3590, USA
b
Department of Materials Science and Engineering, Rensselaer Polytechnic Institute, 110 8th Street, Troy, NY 12180-3590, USA
c
State Key Laboratory of Organic-Inorganic Composites, College of Materials Science and Engineering, Beijing University of Chemical
Technology, Beijing 100029, China

A R T I C L E I N F O A B S T R A C T

Article history: Polytetrafluoroethylene (PTFE) is one of the most widely used solid lubricants but suffers
Received 30 August 2011 from a high wear rate which limits its applications. Here we report four orders of magnitude
Accepted 21 October 2011 reduction in the steady state wear rate of PTFE due to graphene additives. The wear rate of
3
Available online xxxx unfilled PTFE was measured to be 0.4 · 10 mm3/N m which is reduced to 10 7
mm3/N m
by the incorporation of 10 wt% of graphene platelets. We also performed a head-to-head
comparison of wear rate with graphene and micro-graphite fillers at the same weight frac-
tions. In general, we find that graphene fillers gave 10–30 times lower wear rates than micro-
graphite at the same loading fraction. Scanning electron microscopy analysis indicated
noticeably smaller wear debris size in the case of graphene/PTFE composites indicating that
graphene additives are highly effective in regulating debris formation in PTFE leading to
reduced wear.
 2011 Elsevier Ltd. All rights reserved.

1. Introduction
Development of low-friction, wear-resistant surfaces is an
important problem in tribology and surface engineering.
While fluid film (hydrodynamic) lubrication is known to pro-
vide the lowest friction coefficients, there are many practical
situations where fluid lubrication is not feasible. For example,
low temperatures can cause conventional liquid lubricants to
freeze, while high temperatures may cause them to degrade,
or evaporate. When fluid lubrication is not practical, solid
lubricants are often used. One of the most common solid
lubricants being utilized by industry is polytetrafluoroethyl-
ene (PTFE) popularly called ‘‘Teflon’’ (its DuPont brand name).
PTFE is a thermoplastic material with wide ranging applica-
tions in the aerospace, chemical-processing, medical, auto-
motive and electronic industries. PTFE, while being capable
of providing low friction in dry sliding conditions, also suffers
from an extremely high wear rate that limits its use. While
the wear rate in PTFE at sufficiently slow sliding speeds is
quite low, Tanaka et al. [1] have shown that at each test tem-
perature a critical sliding speed existed beyond which the
PTFE wear rate sharply transitioned upward by at least an or-
der of magnitude. For example, when it is slid against stain-
less steel at room temperature at speeds beyond 8 mm/s,
PTFE begins wearing at a rate as high as 10 3 mm3/N m [2],
with large plate-like wear debris hundreds of micrometers
in in-plane dimensions and a few micrometers thick.
Microparticle-filled PTFE has proven to be successful in
reducing the wear rates of PTFE by two to three orders of mag-
nitude [3–5]. The hypothesized roles of micro-scale fillers in the
wear reduction mechanism of PTFE composites, though many
and varied, can be broadly classified into two categories – one
in which the micro-fillers reduce wear by limiting the rates of
initial removal and transfer of material from the PTFE slider

* Corresponding authors at: Department of Materials Science and Engineering, Rensselaer Polytechnic Institute, 110 8th Street, Troy, NY
12180-3590, USA (N. Koratkar).
E-mail addresses: blanct@rpi.edu (T.A. Blanchet), koratn@rpi.edu (N. Koratkar).
0008-6223/$ - see front matter  2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.carbon.2011.10.038

Please cite this article in press as: Kandanur SS et al. Suppression of wear in graphene polymer composites. Carbon (2011), doi:10.1016/
j.carbon.2011.10.038
2 CARBON x x x ( 2 0 1 1 ) x x x –x x x
to the counter-surface [2,4–7], and the other in which micro-
fillers reduce wear by limiting the rates of detachment of the
transferred material from the counter-surface [8,9]. The
hypothesized mechanisms [2,6,7] that seem to capture most
experimental observations belong to first category and claim
that micro-fillers reduce wear by regulating the debris size.
Several of these mechanisms in turn suggest that smaller
sub-micrometer and nano-scale fillers, would lack the size
scale necessary to interfere with the crack propagation step
associated with the debris generation process in PTFE, and
would therefore be ineffective in reducing wear. However, in
the last decade, several nano-scale fillers have been found to
effect dramatic reductions in PTFE wear [10], decreasing in
some instances the wear rate to hitherto unachieved 10
7
mm3/N m levels [11]. Nano-scale fillers have been thought
to reduce wear by a number of mechanisms, including: pre-
venting frictional destruction of PTFE banded structure [10],
enhancing transfer film-countersurface adhesion [10,12], or
inducing changes to the PTFE matrix structure that are more
wear-resistant [13–15]. However, a comprehensive under-
standing of the mechanism of low wear of these nano-compos-
ites has not yet been fully developed.
While nano-fillers such as carbon nanotubes, alumina and
zinc oxide nanoparticles have been studied for wear reduction,
so far there is no report in the literature on the use of graphene
as a wear suppressant additive in polymers. Graphene is a two-
dimensional sheet of sp2 bonded carbon atoms arranged in a
hexagonal lattice. Both individual graphene sheets and graph-
ene platelets (i.e. few-layered graphene) show enormous
potential as fillers for composite applications. In fact, several
studies with graphene have reported significant increase in
Young’s modulus, tensile strength, fracture toughness, and fa-
tigue resistance of polymers at one to two orders of magnitude
lower weight fraction than other competing nano-fillers such
as nano-particles, nano-clays and carbon nanotubes [16–21].
Graphene is intriguing from the point of view of wear suppres-
sion since it has in-plane dimensions of the order of several mi-
crons coupled with nano-meter scale sheet thickness. The
microscale dimensions of the graphene sheets might enable
it to effectively interfere with the debris generation processes
in polymers, while the nano-meter scale thickness, low density
and the planar geometry of graphene generates a huge interfa-
cial contact area with a very large number density of graphene
sheets in the polymer matrix. Moreover, sliding of individual
graphene planes within few-layered graphene platelets might
further enhance the lubrication effect. In this paper, we report
the ability of graphene platelets to drastically reduce wear rates
in PTFE to as low as 10 7 mm3/N m which is four orders of
magnitude lower than in baseline PTFE. The excellent wear
suppression performance of graphene additives coupled with
their potentially low production cost (top down synthesis by
exfoliation of graphite) makes this technology very promising
for industrial scale applications.
2. Materials and experimental protocol
PTFE granular resin with a typical particle size of 30 lm
(Dupont 7C) was used as the matrix material in this study.
The graphene platelets (GPL) were obtained by the one-step
Please cite this article in press as: Kandanur SS et al. Suppression of wear in graphene polymer composites. Carbon (2011), doi:10.1016/
j.carbon.2011.10.038
thermal exfoliation and reduction of graphite oxide
(Supplementary Section). In this method, graphite oxide is
subjected to a thermal shock (rapid rate of heating
2000 C/min) which exfoliates and reduces the graphite
oxide into GPL [22,23]. Fig. 1 shows a transmission electron
microscopy (TEM) image of a graphene platelet manufactured
by this process. The platelets are several micrometers in
in-plane dimensions and are comprised of 3–4 graphene
sheets (inset in Fig. 1) within each platelet. The total platelet
thickness is less than 2 nm. The rough, wrinkled surface
texture of the GPL, which may enable strong mechanical
interlocking and enhanced load transfer with polymer chains
is also visible in the TEM image. Commercially prepared
micro-scale graphite ( 325 mesh powder, size <44 lm) was
also tested as a control filler material to enable comparative
studies with GPL–PTFE composites. GPL–PTFE composites
with filler contents of 0.02, 0.05, 0.12, 0.32, 0.8, 2, 5 and
10 wt%, and graphite–PTFE composites with filler contents
of 2 and 10 wt%, were prepared for wear testing. The methods
used for composite preparation are provided in the Supple-
mentary Section. Fig. 2 shows a typical scanning electron
microscopy (SEM) image of the freeze-fractured surface of
the 2 wt% GPL–PTFE composite. There is no indication of large
agglomeration of the graphene platelets. High resolution SEM
(inset in Fig. 2) shows individual GPL fillers embedded in the
PTFE matrix; the wrinkled surface texture of the GPL is clearly
discernable in the inset image.
A multi-station high-throughput tribometer [15] was em-
ployed for wear testing in a reciprocating pin-on-flat configu-
ration in ambient air at room temperature. The composite
was milled into 10 mm long pins with a 4 mm · 4 mm
square cross-section that served as the contact surface during
wear testing. Stainless steel 304 flats, finished by polishing
with 0.3 lm alumina in distilled water on cloth wheel and
subsequently cleaned ultrasonically in a methanol bath, were
used as countersurfaces. The average roughness of the pol-
ished steel were in the range Ra = 0.015–0.03 lm. The design
Fig. 1 – Transmission electron micrograph (TEM) of a typical
graphene platelet deposited on a TEM grid [16,23]. The
platelet is several micrometers in in-plane dimensions
(scale bar is 0.5 lm). Inset shows a high resolution TEM
image of the edge of the platelet indicating that the
platelet thickness is less than 2 nm. The platelet is
comprised of 3–4 individual graphene sheets.
 CARBON xxx (2011) xxx–xxx
Fig. 2 – Scanning electron microscopy (SEM) image of a
freeze-fractured 2 wt% graphene platelet–PTFE composite.
Inset shows the wavy edges of graphene platelets within
the matrix. There is no indication of large agglomeration of
the graphene platelets from the SEM images.
of the pin holder and the countersurface flat holder of the
multi-station tribometer has been previously described in de-
tail elsewhere [15]. For the wear tests in this study normal
load, corresponding contact pressure, sliding speed, and
reciprocating stoke length were 50 N, 3.125 MPa, 0.1 m/s and
40.5 mm, respectively. Sliding was stopped periodically and
mass loss-based wear measurements of the composite pins
were made. The mass losses were converted to wear volumes
using the composite densities. Plots of wear volume as a func-
tion of sliding distance were obtained for each pin and sliding
for each pin was conducted for a duration long enough to en-
able identification of a steady-state region in which wear vol-
ume increased approximately linearly with sliding distance.
The slope of the identified steady-state wear volume-sliding
distance behavior was calculated using linear regression
and was divided by the 50 N normal load to obtain steady-
state wear rates (units of mm3/N m). For each pin, a 95% con-
fidence interval was determined on the steady-state wear rate
estimate from the linear regression.
3. Results and discussion
The wear volume-sliding distance records for unfilled PTFE
and PTFE filled with varying amounts of graphene are shown
in Fig. 3a. Unfilled PTFE wears rapidly, accumulating 33 mm3
of worn volume after a mere 1.5 km of sliding. It is clear that
the 0.02, 0.05 and 0.12 wt% GPL composites also show rapid
wear behavior, with their data points crowding near the verti-
cal axis similar to those of unfilled PTFE. The effectiveness of
the GPL as a potential wear suppressant is first seen in the
0.32 wt% composite which wears more gradually than unfilled
PTFE, needing 20 km of sliding before accumulating as much
wear volume as unfilled PTFE did after 1.5 km. Further
improvement in wear resistance is witnessed for the 0.8 and
2 wt% composites, with the former accumulating only
12 mm3 in wear volume after 26 km of sliding and the lat-
ter losing 4 mm3 after 51 km of sliding. This trend of in-
crease in wear resistance with increasing filler contents
continued for the 5 and 10 wt% composites with their data
points crowding near the horizontal axis as a consequence
Please cite this article in press as: Kandanur SS et al. Suppression of wear in graphene polymer composites. Carbon (2011), doi:10.1016/
j.carbon.2011.10.038
3
Fig. 3 – (a) Wear volume as a function of sliding distance for
unfilled PTFE and for PTFE with varying contents (wt%) of
graphene platelet filler. (b) The wear volume-sliding
distance records for the slow wearing 2%, 5% and 10%
composites. The steady-state behavior for each composite is
indicated by a trendline, the slope of which was used to
compute the steady-state wear rate for the composite. The
uncertainty in the wear volume measurements was
±0.05 mm3.
of their extremely slow wear rates. The response of these
highly wear-resistant 2, 5 and 10 wt% composites are more
clearly visible in Fig. 3b that is obtained by expanding the
scale of the wear volume axis from Fig. 3a. It is clear from
Fig. 3b that even the low wear 2, 5 and 10 wt% composites ini-
tially show a transient higher wear rate behavior, during
which they accumulate a few mm3 of wear volume, before
they transition to a lower steady-state wear behavior that is
indicated with the help of trendlines. The transition from
transient behavior to steady-state behavior for the compos-
ites in Fig. 3b seems to occur within the first 7–15 km of
sliding.
The results of Fig. 3a and b are summarized in Fig. 4 which
shows a plot of steady-state wear rates as a function of the GPL
content. While no reduction from the 0.4 · 10 3 mm3/N m
steady-state wear rate of unfilled PTFE was observed in the
0.02, 0.05 and 0.12 wt% composites, significant decreases were
observed thereafter, with the 0.32 wt% composite displaying a
0.3 · 10 4 mm3/N m wear rate. The steady-state wear rates
continue to decrease with further increasing filler contents
and the exceptional wear suppressing ability of GPL is clear
in the 10 wt% composite that displays an extremely low 10
7
mm3/N m wear rate. The results suggest that even lower
wear rates can be attained at graphene contents greater than
those studied here, since a monotonic decrease continues
with no minimum observed up to 10% loading (see Fig. 4).
The linearity of this decrease on the displayed
4 CARBON x x x ( 2 0 1 1 ) x x x –x x x

countersurface of the rapidly wearing unfilled PTFE (Fig. 5a).

Fig. 4 – Steady-state wear rate as a function of filler content
for graphene platelet–PTFE composites. The wear rate of
unfilled PTFE is indicated by the broken line. Error bars for
the data points are indicated in the plot. The wear rate is
found to decrease with approximately the square of the
graphene platelet content. The monotonic decrease
continues with no minimum observed for up to 10 wt% of
graphene loading.
log–log axes is particularly notable, indicating a wear rate
which decreases with approximately the square of the graph-
ene content. The wear suppressing ability of graphene addi-
tives compares favorably with that of carbon nanotubes
which have also been reported [24] to reduce wear rates in
PTFE by 2 orders of magnitude to 10 5 mm3/N m.
Fig. 5 compares the wear debris present by the sides of the
wear tracks on the countersurfaces of the high wear rate
unfilled PTFE and the extremely low wear rate 10 wt% GPL/PTFE
composite. Large plate-like wear debris, hundreds of microme-
ters in in-plane dimensions, is seen throughout over the
Noticeably smaller wear debris, generally much less than
100 lm in dimensions, is seen on the countersurface of the
low wear rate 10 wt% GPL–PTFE composite along the edges of
the wear track (running along the left side of Fig. 5b). Fig. 5c
and d presents the wear surfaces of the unfilled and graph-
ene-filled PTFE. Atop the otherwise smooth wear surface of
the unfilled PTFE, the large plate-like debris are again seen
(Fig. 5c), either in the process of detachment or as back-trans-
ferred debris cycling in attachment to the countersurface then
returning to the polymer surface until eventual ejection from
the contact. The wear surface of the graphene-filled PTFE dis-
played a ‘mudflat cracking’ appearance, as also reported by
Burris et al. [25] for comparably wear-resistant PTFE when filled
with 80 nm alpha-phase alumina particles. These mudflat
surface regions are of approximate 10 lm scale and, as also
reported for the wear-resistant alumina-filled PTFE nanocom-
posites [25], these regions appear to be secured into place by
PTFE fibrils which span the shallow cracks separating them.
As discussed previously, unfilled PTFE has been known to
wear by ejecting large plate-like debris hundreds of microme-
ters in in-plane dimensions and a few micrometers in thick-
ness. A popular model for PTFE wear suggests that wear
occurs as a result of propagation at a depth of few micrometers
of sub-surface cracks parallel to the sliding surface, with debris
formation occurring when these cracks eventually connect
with the surface. Micro-scale fillers, by virtue of their size, are
able to interfere with such debris formation phenomena [2]
as matrix wear exposes them to the sliding surface, where they
accumulate yet still extend many micrometers back into the
subsurface, and have been found to reduce wear by 2–3 orders

Fig. 5 – (a) Scanning electron micrograph of the countersurface of unfilled PTFE showing wear debris hundreds of
micrometers in in-plane dimensions. (b) The countersurface of the low wear rate 10% graphene platelet–PTFE showing wear
debris that is finer compared to that generated by the rapidly wearing unfilled PTFE. (c) Wear surface of unfilled PTFE showing
large plate-like debris on the surface. (d) Corresponding wear surface of the 10% graphene platelet–PTFE composite
displaying wear-resistant ‘mudflat’ features.

Please cite this article in press as: Kandanur SS et al. Suppression of wear in graphene polymer composites. Carbon (2011), doi:10.1016/
j.carbon.2011.10.038
 CARBON xxx (2011) xxx–xxx
of magnitude [26]. Our results indicate that graphene platelets,
with their micro-scale in-plane dimensions and large aspect
ratio are well suited to interfering with debris formation in
PTFE. This is evidenced by the noticeably smaller wear debris
size demonstrated in Fig. 5. Moreover the nanoscale thickness
of these sheets implies that at a given weight fraction of addi-
tives the number density of graphene platelets in the matrix far
exceeds that of conventional micro-fillers. This will cause sub-
surface matrix cracks to be deflected through a tortuous path
by the high aspect ratio, two-dimensional graphene platelets.
The aspect ratio of a 2D sheet such as graphene is the ratio of
the length or width of the sheet divided by the sheet thickness
which is estimated as 1000 for our graphene platelets [16,17].
In fact, efficient deflection of matrix cracks by such high aspect
ratio graphene platelets has been shown to cause dramatic
improvements in fracture toughness and fatigue performance
in graphene-epoxy composites [16,17] and more recently in
graphene-ceramic composites [27]. For these reasons graphene
platelets are expected to outperform micro-scale fillers in reg-
ulating the debris size. Indeed the impressive 10-fold and
50-fold wear rate reductions seen for the 0.32% and the 0.8%
composites are vastly superior to those seen in traditional PTFE
micro-composites with comparable filler contents. Further,
traditional PTFE micro-composites have not been known to
achieve even at significantly higher filler contents the extre-
mely low 3 · 10 7 mm3/N m wear rates exhibited by 5 wt%
graphene platelet–PTFE composites. For example, 0.32,
0.8 wt% of 1 lm alumina–PTFE microcomposites were seen to
exhibit wear rates as high as that of unfilled PTFE and even
when the micro-alumina filler content was increased to
5 wt%, the wear rate decreased to only to 10 5 mm3/N m level
[15] as opposed to the more dramatic wear reductions dis-
played by the 5 wt% GPL–PTFE composite.
To illustrate the wear superiority of the GPL composite
over conventional micro-composites, we show a head-to-
head comparison (Fig. 6) of wear rate with graphene and mi-
cro-graphite fillers at the same weight fractions. The 2 wt%
Fig. 6 – Wear volume as a function of sliding distance for
graphite–PTFE and graphene platelet–PTFE composites. The
uncertainty in the wear volume measurements was
±0.05 mm3. The steady state wear rate for the 2 and 10 wt%
graphite–PTFE composites was 2 · 10 5 mm3/N m and
2.9 · 10 6 mm3/N m, respectively. By contrast the 2 and
10 wt% GPL–PTFE composites showed significantly lower
wear rates of 10 6 mm3/N m and 10 7 mm3/N m,
respectively.
Please cite this article in press as: Kandanur SS et al. Suppression of wear in graphene polymer composites. Carbon (2011), doi:10.1016/
j.carbon.2011.10.038
5
graphite–PTFE microcomposite lost as much as 25 mm3 of
wear volume after 23 km of sliding and registered a stea-
dy-state wear rate as high as 2 · 10 5 mm3/N m, while the
2 wt% GPL–PTFE composite lost only a few cubic millimeters
of wear volume after comparable sliding distances and dis-
played a steady-state wear rate 30 times lower. Even when
the graphite filler content was increased to 10 wt%, the wear
rate of the graphite–PTFE composite never reached the low
10 7 mm3/N m levels of the 5 and 10 wt% GPL–PTFE compos-
ites. In fact, the 2.9 · 10 6 mm3/N m wear rate of the 10 wt%
graphite–PTFE microcomposite was higher than even that of
the 2 wt% GPL–PTFE composite.
4. Conclusions
To conclude, graphene platelets served as excellent wear
reducers when incorporated as fillers in a PTFE matrix. The
otherwise high 0.4 · 10 3 mm3/N m steady-state wear rates
of PTFE were found to decrease 10-fold and 50-fold upon
the inclusion of merely 0.32 and 0.8 wt%, respectively, of
graphene platelets. More dramatic 1700-fold and 4000-fold
decreases in wear rates were observed when the filler content
was increased to 5 and 10 wt%, respectively, The wear-resis-
tant graphene platelet–PTFE composites generated debris that
was much finer compared to the large plate-like debris gener-
ated by unfilled PTFE. Graphene platelets were significantly
more effective in PTFE composite wear reduction than con-
ventional micro-scale graphite with even the 10 wt% graph-
ite–PTFE micro-composites being unable to achieve low
10 7 mm3/N m wear rates displayed by the graphene plate-
let–PTFE composites.
Acknowledgements
N.K. acknowledges funding support from the US Office of Na-
val Research (Award N000140910928) and the US National Sci-
ence Foundation (Award: 0900188).
Appendix A. Supplementary data
Supplementary data associated with this article can be found,
in the online version, at doi:10.1016/j.carbon.2011.10.038.
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