Syeda A. Hussain1 and Michelle S.

Hoo Fatt2

The Behavior of Carbon Black-Filled

Natural Rubber under High Strain Rates3

REFERENCE: Hussain, Syeda A. and Fatt, Michelle S. Hoo, ‘‘The Behavior of Carbon
Black-Filled Natural Rubber under High Strain Rates,’’ Tire Science and Technology,
TSTCA, Vol. 34, No. 2, April – June 2006, pp. 119-134.

ABSTRACT: Tensile tests were conducted to obtain the deformation and failure characteris-
tics of unfilled natural rubber 共NR兲 and natural rubber with 25, 50, and 75 phr of N550 carbon
black filler under quasistatic and dynamic loading conditions. The quasistatic tests were per-
formed on an electromechanical INSTRON machine, while the dynamic test data were ob-
tained from tensile impact experiments using a Charpy impact apparatus. In general, the
modulus of the stress-extension ratio curves increases with increasing strain rate up to about
407, 367, 346, and 360 s−1 for unfilled, and 25, 50, and 75 phr for filled NR, respectively.
Above these strain rates, the unfilled and filled natural rubber stress-extension ratio curves
remained unchanged. The modulus increased with increasing strain rate because there was
little time for stress relaxation. Above a critical strain rate, no change in modulus was ob-
served because the time of the experiment was short compared to the lowest characteristic
relaxation time of the material. Dynamic stress-extension ratio curves did not have the very
sharp upturn at break, which is observed from strain-induced crystallization in natural rubber
under quasistatic loading. Strain-induced crystallization appeared to be suppressed at high
rates of loading. In fact, the highest dynamic tensile strength for the 25- and 50-phr carbon
black-filled natural rubbers was smaller than those under quasistatic loading, while the highest
dynamic tensile strength of the 75-phr carbon black-filled NR was greater than that in the
static test. This indicated that high amounts of carbon black fillers will impede strain-induced
crystallization in natural rubber.

KEY WORDS: natural rubber, N550 carbon black, high strain rate, deformation and fracture

Introduction

The strain rates in tires can be well above those obtained from conventional
quasistatic tests, which are generally below 1 s−1. Consider a standard 205/
60R15 pneumatic tire. This tire has a width of 205 mm, an aspect ratio of 60,
and a rim diameter of 15 in. Assume that when it is mounted on a vehicle
traveling at a speed of V mph, the tire has a footprint of roughly 8 in due to the
weight of the vehicle. As the tire rolls, a material point in the tire tread is first
loaded as it enters the footprint and then unloaded as it leaves the footprint. The
material point is loaded from the weight of the vehicle as well as the friction

1
Graduate Student, Department of Mechanical Engineering, The University of Akron, Akron, Ohio
44325-3903.
2
Associate Professor, Department of Mechanical Engineering, The University of Akron, Akron,
Ohio 44325-3903.
3
Presented at the twenty fourth annual meeting of the Tire Society, Akron, Ohio, September 20–21,
2005.

119
120 TIRE SCIENCE AND TECHNOLOGY

TABLE 1 — Estimated loading and unloading time in footprint and strain rate to reach 100% in
standard 205/60R15 tire (calculations based on loading time being twice as large as unloading
time).

Vehicle speed Loading and unloading Strain rate 共s−1兲

共mph兲 time in footprint 共ms兲 for strain of 100%
35 13 115
55 8.3 180
65 7.0 214
75 6.1 245
85 5.3 283
95 4.8 312
125 3.6 416

between tire and road free. Outside the footprint, these loads do not act on the
material point. Since 8 in has to be in contact with the ground during every
revolution, the total loading/unloading time in the material per revolution is
8 in⫻ 3 600共sec/ hr兲 / 63 360共in/ miles兲 ⫻ V共mph兲. Table 1 shows the total load-
ing and unloading time for different car speeds. The faster the vehicle travels,
the shorter the loading/unloading time is of the tread in the footprint. Assume
that the loading time is twice as long as the unloading time 关1兴 and consider
rubber undergoing a strain of 100%. A local strain of this value is not unrea-
sonable for a tread in the footprint area. For a vehicle traveling at the speed of
65 mph, the strain rate involved in stretching the rubber to 100% is 214 s−1
关=3 / 共2 ⫻ 0.007 s兲兴. The faster the vehicle travels, the higher this strain rate
becomes. The third column in Table 1 shows calculated strain rates for a 100%
strain at the various vehicle velocities. For an automobile traveling between 35
and 125 mph, the strain rates vary from 155 to 416 s−1. These rates are clearly
not quasistatic.
The above analysis serves as a motivation for the development of consti-
tutive models to predict rubber material response at high strain rates. This paper
is concerned with the acquisition of high strain rate material properties, which
will become essential material as input data for high strain rate constitutive
models for unfilled and filled natural rubber. The deformation and fracture char-
acteristics of unfilled styrene butadiene rubber 共SBR兲 under high strain rates
have been studied extensively by Bekar et al. 关2–4兴. It was found that in gen-
eral, the modulus of SBR increases with increasing strain rate up to a critical
value of strain rate. Beyond this critical value, the modulus does not change
with increasing strain rate. The stress-extension ratio curve at this point was
termed a “locking” curve. It was proposed that the increase in modulus at high
rates of loading resulted from the lack of relaxation time in the chain molecules.
Three deformation and fracture regimes were identified for unfilled SBR. In the
first regime, which occurred from quasistatic to about 190 s−1, the tensile
 HUSSAIN AND FATT ON THE BEHAVIOR OF CARBON BLACK-FILLED
121

FIG. 1 — Molecular structure of cis-1,4-polyisoprene.

strength and fracture strain increased with increasing strain rate. The second
regime occurred between 190 and 325 s−1, and in this regime, the tensile
strength increased but the fracture strain decreased with increasing strain rate.
In the third regime, which occurred above 325 s−1, both the tensile strength and
fracture strain decreased with increasing strain rate.
A similar study on natural rubber 共NR兲 will be performed in this paper.
Unlike SBR, NR has the unique ability to undergo strain-induced crystalliza-
tion. Natural rubber contains a high degree of long-chain branching 关5,6兴, which
is associated with the presence of small numbers of non-hydrocarbon groups
distributed along the chains 关6兴. It has a cis-1,4-polyisoprene structure, as
shown in Fig. 1, and contains macromolecules that are configured identically.
This allows them to pack together as crystallites either at low temperature 共the
maximum packing rate occurs at about −25 ° C兲 or at room temperature upon
stretching 关7兴. Strain-induced crystallization leads to important mechanical
properties such as high green strength, tear strength, and gum tensile strength.
Synthetic SBR, on the other hand, cannot crystallize and is about 90% weaker
when compared to NR. Carbon black is often used as a filler material to im-
prove the strength of SBR. It can increase the strength of SBR more than
tenfold. Carbon black is also used to improve the tearing strength and abrasion
resistance of NR. It has been mentioned in Ref. 关8兴 that carbon black has very
little effect on the tensile strength of NR since most of the strength of NR is due
to strain-induced crystallization.
Among the different types of fillers available, carbon black fillers are the
most widely used. Carbon black fillers can be divided into three categories 关9兴:
共1兲 Small particle size abrasion furnace blacks 共N100–N300 series兲, which
give vulcanizates highest strength properties and highest changes in
stiffness with strain amplitude.
共2兲 Semi-reinforcing furnace blacks 共N500–N700 series兲, which give
slightly lower strength properties and smaller changes in stiffness with
strain amplitude.
共3兲 Diluent thermal blacks 共N880–N990兲, which give much lower strength
properties and smaller changes in stiffness with strain amplitude.
The 100, 200, and 300 series are used in tire tread, while the 500 and 600 series
are used for the tire carcass. The N550 carbon black chosen for this study is not
only used to make tires but also automotive belts, seals, weather strip, O-rings
and gaskets, engine mounts, antivibration dampeners, and wiper blades.
122 TIRE SCIENCE AND TECHNOLOGY

TABLE 2 — Unfilled natural rubber formulation.

Amount
Ingredients 共phra兲
NR 100
Process oil 2
Stearic acid 2
Zinc oxide 5
6 PPD 1
Sulphur 2.75
MBTS 1
TMTD 0.1
a
Parts by weight per 100 parts by weight of rubber. Cure for 20 min at 300 ° F 共150 ° C兲
and 300 psi.

We will investigate the differences in the deformation and fracture behavior

of unfilled and carbon black-filled NR under high strain rates and what is
observed under quasistatic loading. Natural rubber, unfilled and filled with three
amounts of N550 carbon black, 25, 50, and 75 phr, will be used to examine the
effect of carbon black on the high strain rate properties of NR. High-speed
tensile tests will be conducted on rubber specimens to obtain stress-extension
ratio curves at strain rates in the range 10– 103 s−1, using a tensile impact
apparatus developed earlier by Bekar et al. 关2兴. The quasistatic test data will be
obtained from an electromechanical INSTRON machine.

Materials

Samples of unfilled and carbon black-filled NR with formulations listed in

Tables 2 and 3 are prepared according to standard ISO 2393 methods 关10兴. The
various components are first weighed as specified in Tables 2 and 3. The NR is
then shredded and carbon black N550 is added at various amounts 共25, 50, and
75 phr兲 and mixed in with the shredded NR. In the next step of preparation, the
antioxidants 共6 PPD兲, accelerators 共TMTD兲, antiozonants 共MBTS兲, reinforcing
agents and pigments 共zinc oxide兲, and softening agents 共stearic acid兲 are added
to the NR and carbon black mixture and mixed thoroughly in a Banbury ma-
chine. For the carbon black to be well dispersed in the rubber, the viscosity of
the rubber must not be too low. If the viscosity of the rubber is too low, then the
shear stresses will be insufficient to break the filler agglomerates into aggregates
and thoroughly disperse them in the rubber. Hence oil is added toward the end
of the mixing cycle. The final stage involves curing of this mixture. Curing
times, temperatures, and pressures are determined from an oscillating disk-type
rheometer 共ODR兲 and are listed in Tables 2 and 3.
 HUSSAIN AND FATT ON THE BEHAVIOR OF CARBON BLACK-FILLED
123

TABLE 3 — Carbon black-filled natural rubber formulations.

Amount
Ingredients 共phra兲
NR 100
Process oil 5
Stearic acid 2
Zinc oxide 5
Carbon black N 550 25, 50, 75
6 PPD 1.5
Sulphur 2.75
MBTS 1
TMTD 0.1
a
Parts by weight per 100 parts by weight of rubber. Cure for 20 min at 300 ° F 共150 ° C兲
and 300 psi.

Once the curing times and temperatures have been determined, the rubber
samples are placed in a hydraulic press and stamped for 20 min at a temperature
of 300 ° F and a pressure of 300 psi. The size of the die is chosen such that the
stamped samples are 152.4 mm⫻ 152.5 mm⫻ 2.54 mm thick 共6 in⫻ 6 in
⫻ 0.1 in thick兲. ASTM D412 关11兴 dumbbell and strip specimens are used for the
quasistatic and dynamic tests, respectively. The gage dimensions are 25.4 mm
⫻ 6.35 mm⫻ 2.54 mm thick 共1 in⫻ 0.25 in⫻ 0.1 in thick兲. The dumbbell speci-
mens are cut from a die and press, while the strip specimens are cut using a
razor and hammer. An additional 12.7 mm 共0.5 in兲 on either side of the 25.4-
mm 共1-in兲 gage length is allowed to grip the strip specimen. It is standard
practice not to test rubber within 16 hours of vulcanization 关12兴. Cross linking
does not stop exactly when the rubber is taken out from the mold. It continues
as the rubber cools to room temperature and even proceeds slowly at room
temperature. In addition to this, the rubber ages due to oxidation. Antioxidants
共6 PPD兲 were added to the formulation of the unfilled and filled natural rubber
to slow down this process. Both cross linking and aging cause variations in the
mechanical properties of the rubber, and it has been recommended that the time
between vulcanization and testing be no longer than 60 days for some rubber
components 关13兴. To extend the testing period beyond 60 days, the specimens
are sealed in plastic bags and stored at a reduced temperature of approximately
40 ° F. Decreasing the temperature would slow down any chemical reaction
according to Arrhenius equation.

Experimental Setup

Quasistatic Tests
Quasistatic tests are conducted on ASTM D412 dumbbell specimens using
an electromechanical INSTRON machine. The specimens are held in place by
124 TIRE SCIENCE AND TECHNOLOGY

FIG. 2 — Schematic diagram of tensile impact test: (a) Side view of Charpy hammer impact and (b)
top view of experiment.

means of pneumatic grips. Extension of the test piece is measured with a long-
travel, balanced elastomeric clip-on extensometer attached to the central portion
of the specimen. Displacement or strain-controlled tests are performed and the
stress-extension ratio curves are obtained at a constant strain rate of 0.1 s−1.
Four to five tests are conducted on the specimens made from the unfilled and
carbon black-filled rubber in order to ensure repeatability of data.

High-Speed Experiments
The tensile impact experiment that is used to obtain the deformation and
fracture characteristics of natural rubber under tensile impact loading was de-
veloped by Bekar et al. 关2兴 and is shown in Figs. 2共a兲 and 2共b兲. As shown in Fig.
2共a兲, the Charpy impact pendulum is used to impact a specially designed slider
bar connected to two copper cables. The copper cables are directed around
pulleys and attached to sliding guided bases with grips that hold opposite ends
of the specimen 关see Fig. 2共b兲兴. The guided bases are allowed to slide freely
along steel rails via linear bearings. On top of the guided bases are specially
designed grips, which not only hold opposite ends of the specimen but are also
attached to dynamic load cells and displacement transducers. The piezoelectric
force sensors 共PCB load cells兲 mounted on each guided base record the impact
tensile force as the copper cables pull on the guided base. The extension of the
specimen is recorded by two RDP D5 linear variable differential transformers
 HUSSAIN AND FATT ON THE BEHAVIOR OF CARBON BLACK-FILLED
125

共LVDTs兲, which have a range of ±150 mm. Since the extensions are measured
by grip displacement, ASTM D412 strip specimens are used instead of dumb-
bell specimens. An 8-channel PCB 482A22 signal conditioner is used with the
force sensors, and two RDP S7AC transducer amplifiers are used with the
LVDTs. The data acquisition device used in the experiment is DATAQ DI-720-
USB. It has the ability to collect 250 000 data per second. Since there are two
load cells and two displacement transducers or four channels, each channel can
obtain up to 62 500 data points per second, which is deemed sufficient for this
type of application.
Elongation and force must be converted to extension ratio and stress. The
extension ratio, ␭, is the ratio of the specimen’s current length, L, to the original
length, Lo,
⌬ + Lo
␭ = L/Lo = 共1兲
Lo
where ⌬ is the elongation. The engineering strain, e, is thus related to the
extension ratio by
e = ␭ − 1. 共2兲
The true stress, ␴, is the tensile force, F, divided by the current cross-sectional
area, A,
F
␴= . 共3兲
A
Assuming incompressible material 共often a good assumption for rubber in ten-
sion and shear since the bulk modulus is much greater than the shear modulus兲
one can relate the true stress to the engineering stress, s, by
␴ = s␭. 共4兲

Results and Discussion

QuasiStatic Test Results

Cauchy stress-extension ratio curves for filled and unfilled NR at strain
rates of 0.1 s−1 are shown in Fig. 3. The stars indicate break points, i.e., exten-
sion ratio at break and tensile strength, whereby the specimen breaks in the gage
center. The general trend observed from the quasistatic tests on NR is that the
strength and stiffness increase with higher amounts of carbon black, up to about
25 phr. Beyond this amount, the strength decreases with increasing carbon
content while stiffness increases but at a slower rate. The increase in stiffness
with percentage of carbon filler has been well documented 关14兴, but the de-
126 TIRE SCIENCE AND TECHNOLOGY

FIG. 3 — Static stress-extension ratio curves of unfilled and filled natural rubber.

crease in strength with increasing amounts of carbon filler has not been men-
tioned as much in the literature. The decrease in tensile strength and fracture
strain of NR with increasing carbon black filler could be caused by the carbon
black agglomerates. A large structured filler aggregate 共see Fig. 4兲 has a huge
void volume in which the rubber molecules get trapped or occluded during
shear mixing 关7兴. This bound rubber is prevented from crystallizing.

Dynamic Stress-Extension Ratio Curves

High-speed tensile tests were conducted on unfilled and filled NR with 25,
50, and 75 phr of N550 carbon black. Figures 5–8 show the dynamic stress
strain curves of each blend of NR. The static stress-extension ratio curve 共strain
rate of 0.1 s−1兲 is included on these graphs for reference. Again the stars indi-
cate break points, i.e., extension ratio at break and tensile strength, whereby the
specimen breaks in the gage center. For the unfilled NR and some of the 25-phr

FIG. 4 — Structure of carbon black agglomerate.

 HUSSAIN AND FATT ON THE BEHAVIOR OF CARBON BLACK-FILLED
127

FIG. 5 — Dynamic stress-extension ratio curves for unfilled natural rubber.

carbon-filled NR, the specimen broke in the grips and break points could not be
found. Using dumbbell specimens in the high-speed experiments would have
prevented this from happening, but the specimen extension could only be mea-
sured from the grip displacement in the present experimental setup. Future work
using dumbbell specimens and a high-speed camera is planned to achieve mea-
surements of the tensile strength and breaking elongation for the unfilled and
25-phr carbon-filled NR.
Unfilled Natural Rubber. The dynamic stress-extension ratio curves indicate
that stiffness increases with strain rate but beyond 407 s−1, the stiffness is al-
most unchanged, i.e., a “locking” curve is approached. This locking curve was
also identified in the unfilled SBR 关2–4兴 and is associated with the so-called
instantaneous response of the material. The instantaneous response curve rep-
resents the material’s stiffness without any measurable stress relaxation. The
increase in stiffness with increasing strain rate is due to a lack of time for stress
relaxation. The static stress-extension ratio curve also appears to be stiffer than
the dynamic stress-extension ratio curves, especially when the extension ratios
are large, i.e., greater than 3. This is possibly due to a reduction in the time
needed for strain-induced crystallization to occur. Recall that NR is inherently
stiff and strong because of strain crystallization. Contrary to the case of SBR,
128 TIRE SCIENCE AND TECHNOLOGY

FIG. 6 — Dynamic stress-extension ratio curves for natural rubber with 25-phr N550.

high rates of loading do not necessarily increase the stiffness and strength of
NR.
It should be emphasized that this locking curve appears for the material
over a very large strain region. A locking curve for the material may occur at
strain rates a few orders of magnitude higher if one were concerned with a very
small strain region, one in which the material stress-strain curve is often mod-
eled as linear elastic. Time-dependent or viscoelastic behavior of elastomers is
linked to complicated molecular adjustments resulting from macroscopic me-
chanical deformations 关15兴 that may occur at different length and time scales.
Alfrey 关16兴 describes the morphology of an elastomer in terms of convolutions,
curls, and kinks. Convolutions represent the long-range contour of an entire
molecular chain, which forms entanglements. Curls are shorter-range molecular
contours that develop between entanglements and cross links, and kinks are
molecular bonds within a curl. Under stress, the molecules slide except at the
entanglements and cross links. Relaxation, intermolecular slippage accompa-
nied by some reversible breaking or swapping of bonds, takes place during this
time and the various types of slippage are distinguished by different relaxation
times. Relaxation on a local scale involves relatively rapid readjustments of the
kinks in the molecular chains. Relaxation on a long-range scale involves very
slow rearrangements of the convolutions with respect to each other. Readjust-
ments can be restricted when the elastomer is deforming at very high rates
because certain relaxation mechanisms do not have time to occur. Thus, the
 HUSSAIN AND FATT ON THE BEHAVIOR OF CARBON BLACK-FILLED
129

FIG. 7 — Dynamic stress-extension ratio curves for natural rubber with 50-phr N550.

long-range relaxation mechanisms, which are concerned with motion of convo-

lutions and curls and take place on the order of say 100 or more milliseconds,
may not have time to occur if the load is applied in less than this time. The lack
of these long-range relaxation mechanisms is what leads to the locking curve
observed in our experiments. To see the same locking curve due to lack of
relaxation on a local scale, one will have to perform experiments in the small
strain region where this phenomenon is more dominant and subject the materi-
als to much higher loading rates. The long travel LVDTs used in our experi-
ments have an error of ±3.8 mm 共±0.15 in.兲 and for a 1-in.-guage specimen,
strains below 15% cannot be determined accurately. Thus it is impossible to find
a locking curve in the small strain region in the current experimental setup.
Carbon Black-Filled Natural Rubber. The dynamic stress-extension ratio
curves of carbon black-filled NR in Figs. 6–8 show similar trends to the unfilled
NR in that the modulus increases with increasing strain rate up to a critical
value of strain rate. Above the critical strain rate, a locking curve becomes
130 TIRE SCIENCE AND TECHNOLOGY

FIG. 8 — Dynamic stress-extension ratio curves for natural rubber with 75-phr N550.

evident for each material. The critical strain rate for locking is 346, 367, and
360 s−1 for the 25-, 50-, and 75-phr carbon-filled NR, respectively. Surprisingly,
the strain rates at which locking occurs for the filled natural rubbers are almost
the same, about 360 s−1. The static stress-extension ratio curves for NR with
25-phr carbon black is stiffer than the dynamic stress-extension ratio curves
when extension ratios are greater than 3. Thus a reduction in time for strain-
induced crystallization is also playing a role in determining the dynamic prop-
erties of 25-phr filled NR.
For the 50 and 75 phr, the quasistatic tensile stress-extension ratio curve is
below the locking curve. Strain-induced crystallization is not as prevalent in
these materials possibly due to the high amounts of carbon black in them. Table
4 shows a comparison of the static and highest dynamic Cauchy stress at 300%
strain 共extension ratio of 4兲 for the unfilled and filled NR. A strain of 300% was
chosen to reveal the effect of strain-induced crystallization. The static stress at
300% strain is about 26% higher than the highest dynamic stress at 300% for
 HUSSAIN AND FATT ON THE BEHAVIOR OF CARBON BLACK-FILLED
131

TABLE 4 — Comparison of static and highest dynamic Cauchy stress at 300% strain.

NR with NR with NR with

25-phr 50-phr 75-phr
Unfilled carbon carbon carbon
NR black black black
Static Cauchy stress 1 150 3 800 8 856 10 060a
at 300% strain 共psi兲
共strain rate at 0.1 s−1兲
Highest dynamic 1 500 3 000 11 500 14 500a
Cauchy stress at
300% strain 共psi兲
a
Extrapolated value.

the 25 phr. This is because the material has enough time to crystallize. It takes
30 seconds for the specimen to reach a 300% strain at a strain rate of 0.1 s−1,
but only 5 ms to reach a 300% strain at a strain rate of 588 s−1. Thirty seconds
is about five orders of magnitude higher than 5 milliseconds, and it would
appear that strain-induced crystallization, as in the case of stress relaxation,
needs finite time to become noticeable. The static stresses at 300% strain are
23% and 28% lower than the highest dynamic stress at 300% for the 50 and 75
phr, respectively. Apparently, the percentage of carbon black affects the extent
of strain crystallization in NR. Filler reinforcement rather than strain-induced
crystallization is more important in highly filled NR.
Break points, indicating tensile strength and extension ratio at break at
constant strain, can be obtained for most of the filled NR tests. This is because
the carbon black filler is toughening the material held in the grip. A comparison
of the tensile strength during static and dynamic loading is shown in Table 5.
The tensile strength quoted in Table 5 is the Cauchy or true stress and not the
engineering stress, which is often given in the literature. Break point for the
lower strain rate could not be determined since a constant strain rate until break

TABLE 5 — Comparison of static and highest dynamic tensile strength.

NR with NR with NR with

25-phr 50-phr 75-phr
Unfilled carbon carbon carbon
NR black black black
Static tensile 20 833 22 638 16 863 8 856
strength 共psi兲 共strain
rate at
0.1 s−1兲
a
Highest dynamic 12 974 14 538 17 342
tensile strength 共psi兲
a
Test data could not be found.
132 TIRE SCIENCE AND TECHNOLOGY

could not be maintained in the tests. No dynamic tensile strength was obtained
for the unfilled NR due to the fact that the specimen broke in the grip instead of
the center of the gage area. For the 25- and 50-phr carbon black-filled NR, the
highest dynamic tensile strength is below the static tensile strength. However,
the highest dynamic tensile strength is about double that of the static tensile
strength for the 75-phr carbon-filled NR. The high content of carbon black filler
in the 75-phr carbon-filled NR has evidently changed the morphology of NR to
the point that the material is not undergoing any substantial strain-induced crys-
tallization. The dynamic tensile strength of the 75-phr filled NR is higher than
the static value because there is not enough time for the material to relax.
Another interesting observation from Table 5 is that the highest dynamic tensile
strength increases from 25 to 75 phr carbon black filler in the NR, while the
opposite trend is observed for the static tensile strength. Thus carbon black filler
can increase the tensile strength of NR due to filler reinforcement but only at
high rates of loading. This conclusion is very important in predicting damage of
tire treads that experience high rates of loading.

Conclusions and Recommendations

High-speed tensile tests were conducted on unfilled and 25-, 50-, and 75-
phr carbon black-filled natural rubber using a Charpy tensile impact apparatus.
In general, the modulus of the stress-extension ratio curves increase with in-
creasing strain rates up to about 407, 367, 346, and 360 s−1 for unfilled, and 25-,
50-, and 75-phr filled NR, respectively. Above these strain rates, the unfilled and
filled NR stress-extension ratio curves remained unchanged. The dynamic
stress-extension ratio curves from these tests were compared to those obtained
in quasistatic tests using an electromechanical INSTRON machine. It was found
that the general shape of the dynamic stress-extension ratio curves was different
from those of the quasistatic tests. The initial modulus 共modulus at low strain兲
of the dynamic stress-extension curves was very high and then decreases with
extension ratio, while that of the static curve was initially low and increases
with increasing extension ratio. Dynamic stress-extension curves also do not
have the very sharp upturn at break, which is characteristic of strain crystalliz-
ing natural rubber under quasistatic loading.
The unfilled and 25-phr carbon black-filled NR were stiffer at large strains
共greater than 400% and 200%, respectively兲 under quasistatic loading than they
were under high rates of loading. This was probably due to insufficient time for
strain-induced crystallization in these materials at high strain rates. When the
static stress at 300% strain was compared to the highest dynamic stress at 300%
strain, it was found to be 26% higher for the 25-phr NR, but 23% lower for the
50-phr NR and 28% lower for the 75-phr NR. This indicated that high amounts
 HUSSAIN AND FATT ON THE BEHAVIOR OF CARBON BLACK-FILLED
133

of carbon black hindered strain-induced crystallization, which was also becom-

ing less evident at higher rates of loading. This conclusion can be further sub-
stantiated by noting that static tensile strengths of the 50- and 75-phr carbon
black-filled natural rubbers were even lower than that of the 25-phr carbon
black-filled and unfilled natural rubbers.
The highest dynamic tensile strengths for 25- and 50-phr carbon black-
filled natural rubbers were found to be lower than those from the static tensile
tests for these materials. This again indicated that during high rates of loading,
natural rubber may not have time to undergo strain-induced crystallization. The
above dynamic tensile tests corresponding to the highest dynamic tensile
strength lasted less than 30 milliseconds and this time may be short compared to
the crystallization time. In contrast to the 25- and 50-phr carbon-black-filled
NR, the highest dynamic tensile strength for the 75-phr carbon black-filled NR
was greater than that from the static tensile test. Thus very high amounts of
carbon black impede strain-induced crystallization and the dynamic tensile
strength of a highly filled NR is determined primarily from filler reinforcement.
Future work is planned to analyze the effect of different filler types on the high
strain rate properties of natural rubber. A similar study will also be carried out to
investigate the effect of fillers on high strain rate properties of SBR, which is
not a strain crystallizing rubber.

Acknowledgments
This research was supported by the National Science Foundation under
Grant No. CMS-0528060. The authors would like to thank Robert Seiple and
the Applied Polymer Research Center for providing raw materials and technical
support in the preparation of rubber specimens. They also thank Steve Gerbertz,
Dr. Michael J. Hovan, and Mohammed R. Karim for their assistance during the
high-speed experiments.

References

关1兴 Vickers, H. H. and Robison, S. B., “Measurements of Tread Motions and Application to Tire
Performance,” Proceedings of the International Rubber Conference, Washington DC, Nov.
8–13, 1959, pp. 128–141.
关2兴 Bekar, I., Hoo Fatt, M. S., and Padovan, J., “Deformation and Fracture of Rubber Under
Tensile Impact Loading,” Tire Science and Technology Journal, Vol. 30, No. 1, 2002, pp.
45–58.
关3兴 Hoo Fatt, M. S., Bekar, I., and Padovan, J., “Tensile Impact of SBR—Rate-Dependent Defor-
mation and Fracture Characteristics,” EUROMECH Colloquium on Constitutive Equations for
Polymer Micro-Composites: On the Border of Mechanics and Chemistry, Vienna, Austria, July
15–17, 2002.
关4兴 Hoo Fatt, M. S., and Bekar, I., “High-Speed Testing and Material Modeling of Unfilled Styrene
134 TIRE SCIENCE AND TECHNOLOGY

Butadiene Vulcanizates at Impact Rates,” Journal of Materials Science, Vol. 39, No. 23, 2004,
pp. 6885–6899.
关5兴 Bruzzone, M., Corradini, G., De Chirico, A., Guiliani, G., and Modini, G., “Branching and
Molecular Weight Distribution in 1, 4-cis-polyisoprenes and Effect on the Dynamic Proper-
ties,” Proceedings of the 4th International Synthetic Rubber Symposium, London, Sep. 30—Oct.
2, 1969, pp. 83–87.
关6兴 Angulo-Sanchez, J. L. and Caballero-Mata, P., “Long Chain Branching in Natural Hevea
Rubber—Determination by Gel Permeation Chromatography,” Rubb. Chem. Technol., Vol. 54,
No. 1, 1981, pp. 34–41.
关7兴 Gent, A. N. 共editor兲, Engineering with Rubber: How to Design Rubber Components, 2nd ed.,
Hanser Publishers, Munich, 2001.
关8兴 Bateman, L., The Chemistry and Physics of Rubber-Like Substances, MacLaren and Sons Ltd.,
London, 1963.
关9兴 Gregory, M. J., “Selection of Carbon Black Fillers for Natural Rubber Springs,” Rubb. Chem.
Technol., Vol. 52, No. 5, 1979, pp. 996–1007.
关10兴 ISO 2393: Rubber Test Mixes—Preparation, Mixing and Vulcanization—Equipment and Pro-
cedures, 2nd ed., 1994.
关11兴 Annual Book of ASTM Standards, Vol. 09.01, 1998.
关12兴 ASTM D 3182–89: Standard Practice for Rubber—Materials, Equipment and procedures for
Mixing Standard Compounds and Preparing Standard Vulcanized Sheets, 1994.
关13兴 ASTM D 3183–84: Standard Practice for Rubber—Preparation of Pieces for Test Purposes
from Products, 1998.
关14兴 Roberts, A. D., 共editor兲 Natural Rubber Science and Technology, Oxford University Press,
Oxford, 1988.
关15兴 Ferry, J. D., Viscoelastic Properties of Polymers, 3rd ed., Wiley, New York, 1980.
关16兴 Alfrey, T., Mechanical Behavior of High Polymers, Interscience, New York, 1948.