Petroleum Science and Technology

ISSN: 1091-6466 (Print) 1532-2459 (Online) Journal homepage: https://www.tandfonline.com/loi/lpet20

A comparative evaluation of crumb rubber and

devulcanized rubber modified binders

Amirhossein Ghasemirad, Seyed Mohammad Asgharzadeh & Nader

Tabatabaee

To cite this article: Amirhossein Ghasemirad, Seyed Mohammad Asgharzadeh &

Nader Tabatabaee (2017) A comparative evaluation of crumb rubber and devulcanized
rubber modified binders, Petroleum Science and Technology, 35:11, 1091-1096, DOI:
10.1080/10916466.2017.1303717

To link to this article: https://doi.org/10.1080/10916466.2017.1303717

Published online: 11 Sep 2017.

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PETROLEUM SCIENCE AND TECHNOLOGY
, VOL. , NO. , –
https://doi.org/./..

A comparative evaluation of crumb rubber and devulcanized rubber

modified binders
Amirhossein Ghasemirada , Seyed Mohammad Asgharzadehb , and Nader Tabatabaeea
a
Department of Civil Engineering, Sharif University of Technology, Tehran, Iran; b Department of Civil and Environmental
Engineering, Tarbiat Modares University, Tehran, Iran

ABSTRACT KEYWORDS
One of the most prominent uses of ground tire rubber (GTR) is in rubber- devulcanized rubber; ground
modified asphalt industry. Besides improving performance properties of tire rubber; modified binder;
binders, GTR induces some drawbacks like weak storage stability and inferior MSCR; performance grading;
storage stability
low temperature (LT) performance. This study sought to rectify these short-
comings through using devulcanized rubber (DVR) in place of common GTR.
Binder performance grading, multiple stress creep and recovery, and storage
stability tests were conducted. More resistance against traffic loads at high
temperatures was observed as DVR’s advantages over GTR, while its weaker
LT characteristics and lower storage stability can prevent it from being a viable
alternative.

1. Introduction
Nowadays, regarding the increased traffic loads and adverse atmospheric effects, different types of pave-
ment distresses exist in road pavement, which makes additives a beneficial means to enhance the quality
and performance of asphalt. One of the most well-known binder additives is the ground tire rubber
(GTR), also known as crumb rubber. ASTM D8 defines the rubber-modified asphalt binder as “a blend
of asphalt cement, reclaimed tire rubber and certain additives in which the rubber component is at least
15% by weight of the total blend and has reacted in the hot asphalt cement sufficiently to cause swelling
of the rubber particles.”
Studies have shown that rubber-modified binder possesses improved performance properties. The
reported enhanced properties include better rutting (Wang et al., 2012) and fatigue resistance (Ameri
et al., 2017), improved creep and recovery properties (Wang et al., 2012), reduced temperature suscepti-
bility (Lee et al., 2008), improved resistance to oxidative aging (Cheng et al., 2014), and increased resis-
tance to low temperature (LT) cracking (Puga and Williams, 2016). However, the usage of crumb rubber
modified asphalt binder has its own drawbacks, one of which is the tendency of the rubber particles to
separate from the binder during storage at high temperatures, which results in weak storage stability of
crumb rubber modified asphalt binder at these temperatures (Cheng et al., 2011). The storage stability
of rubber-modified binders is shown to become even worse as the rubber particle size increases (Liang
et al., 2015), or when crumb rubber particles are produced in the cryogenic process rather than grinding
at ambient temperatures (Presti, 2013). Many efforts have been made to improve the storage stability
of rubber-modified asphalt binders, one of which is using various types of modifiers that form bonds
between the components of rubber-modified binder (Sienkiewicz et al., 2017). Other researchers have
used reclaimed rubber to resolve the low compatibility of crumb rubber and asphalt binder (Yu et al.,
2011). Rubber reclamation in general can be carried out by using rubber surface-activating agents, or

CONTACT Seyed Mohammad Asgharzadeh sm.asgharzadeh@modares.ac.ir Department of Civil and Environmental

Engineering, Tarbiat Modares University, Tehran, Iran.
©  Taylor & Francis Group, LLC
1092 A. GHASEMIRAD ET AL.

treating ground tire rubber by gamma or microwave irradiation, or modifying through the devulcaniza-
tion process (Hassan et al., 2013). Other types of rubber-modified binders such as wet process Terminal
Blend (TB) rubberized binders, produced under a special manufacturing process, still present phase seg-
regation problems at high temperatures (Han et al., 2016).
In tire manufacturing, rubber undergoes vulcanization to form the rigid 3D network of polymeric
chains, while during devulcanization the inter-molecular links in the chemical network, including
carbon–sulfur and sulfur–sulfur bonds, break down, which finally results in shorter length of the poly-
meric chains (Hassan et al., 2013). The resulting devulcanized rubber (DVR) has been found to mix and
disperse more easily in the matrix and to have improved compatibility with asphalt binder (Dong et al.,
2011; Yu et al., 2011).
Little work has been devoted to investigating the effects of the modification of devulcanized crumb
rubber on asphalt binders. Dong et al. (2011) reported that rubberized asphalt concrete made with DVR-
modified binder has improved rutting and cracking resistance properties. Yu et al. (2011) observed higher
compatibility between DVR and binder. Considering these benefits, it appears that DVR-modified bitu-
men can alleviate some of the shortcomings of GTR-modified binder such as its lower storage stability.
However, like all other additives, the optimum mixing conditions and optimum content of DVR modifier
should be first determined. This was performed in this research by evaluating the performance proper-
ties of DVR-modified binders at different temperature ranges and under different mixing conditions. In
addition, a research concerning both the performance characteristics of DVR-modified binder and its
storage stability was missing in the literature. Furthermore, these characteristics should be compared to
those of GTR-modified binder if one is going to substitute DVR for GTR in rubberized binders. The
objectives of this research were to determine the physical properties of DVR-modified binders and iden-
tify its optimum mixing characteristics, compare the rheological properties and storage stability of GTR-
and DVR-modified binders, and finally determine whether DVR can be a proper substitute for GTR in
rubberized binders.

2. Materials and testing

A base asphalt of performance grading (PG) 58–22 with SARA fractions (ASTM D4124) of 10.6% asphal-
tene, 11.2% saturates, 44.6% naphthene aromatics, and 33.6% polar aromatics was used in this research.
The high aromatic content of this binder is indicative of good compatibility with modifiers such as
crumb rubber (Asgharzadeh and Tabatabaee, 2013). The GTR was produced by Yazd Tire Company
using ambient grinding technology on scrap truck tires and had a density of 1,100 kg/m3 . The asphalt
rubber blends were made of 15% GTR relative to weight of the neat asphalt, mixed with the base binder
using a high shear mixer with a speed of 5,000 rpm at 180°C for 60 min. The rubber particle maximum
size of 0.25 mm was selected so that the negative effect of large particle size on DSR test results would
decrease. The devulcanized crumb rubber was also provided by the same company and from the same
source of scrap tires the GTR was produced. Regarding the costs of the devulcanization processes, the
DVR was approximately twice more expensive than GTR. Specifications of DVR are presented in Table 1.
Upon devulcanization, the rubber crumbs became soft and sticky, which made determination of its gra-
dation through sieve analysis impossible. The mixing conditions for binder modifications were selected
as described in Table 2. The binders were labeled as DVR-X-Y, which denotes a blend with X percent
DVR relative to the weight of the base binder mixed for Y minutes at 180°C.

Table . Properties of used devulcanized rubber.

Mooney Tensile
Acetone viscosity (@ strength Elongation Hardness Density
Property extract (%) Ash (%) °C) (ML  + ) (kg/cm ) (%) (Shore-A) (g/cm )

Test ASTM D ASTM ASTM D ASTM ASTM D ASTM ASTM
method D D D D
Amount  Max . Max  Max  Min  Min 55 ± 5 1.13 ±
0.02
 PETROLEUM SCIENCE AND TECHNOLOGY 1093

Table . Binder mixing conditions and PG grading.

Mixing conditionsa Continuous performance temperature (°C)

Modifier content Mixing time LT LT Standard Nominal Continuous
Binder (%) (min) HT IT S-value m-value HT-LT PG grade ITb (°C) span (°C)

Base binder na na . . − . − . .–. –  

GTR-   . . − . − . .–. –  
DVR-   . . − . − . .–. –  
DVR-   . . − . − . .–. –  
DVR-   . . − . − . .–. –  
DVR-   . . − . − . .–. –  
DVR-   . nac nac nac .–LT –LT nac nac
a Mixing temperature and speed for all modified binders are °C and , rpm, respectively.
b Nominal IT = (HT grade + LT grade)/ + °C
c Binder was too stiff for making proper specimens.

The rheological properties and performance grading of the base, GTR-, and DVR-modified binders
were determined according to Superpave standards, using DSR, BBR, and RV apparatus. The multiple
stress creep and recovery (MSCR) test was also conducted according to ASTM D7405 on the short-
term aged binders. All modified binders were subjected to the high-temperature storage stability test in
accordance with ASTM D7173, using aluminum tubes. The DSR test at the pertinent high temperature
(HT) grade of the binder was carried out on the top and bottom portions of aluminum tubes that were
cut into three parts of equal length.

3. Results and discussion

3.1. Superpave PG tests

Table 2 shows the results of PG grading of all binders. Continuous grades were determined by interpola-
tion to determine the temperatures at which the physical criteria were met. As shown in Table 2, the use
of 15% DVR resulted in high temperature properties close to those of GTR-modified binder. Increasing
the DVR content to 25% in DVR25-30 improved the HT grade by two PG grades (from 70 to 82), but
caused binder viscosity to rise to 10.2 Pa·s at 135°C, making its practical pumpability seriously inap-
propriate. This makes DVR15-60 and GTR15-60 the top HT-performing binders. Also, in the binders
containing 15% DVR, increasing the mixing time from 15 to 60 min constantly enhanced the HT grade,
one of its reasons would be the increase in heat aging of the binders. However, increasing the mixing time
of DVR from 60 to 90 min caused a noticeable softening of the binder, as is evident from the decline in
HT from 78.7 to 71.9°C with a small 1.3°C improvement in LT. This suggests the breakdown of the poly-
mer network, which may occur due to rubber particle dissolution (Wang et al., 2016; Shu and Huang,
2014). Rubber particle dissolution happens only in large mixing time and temperatures (Shu and Huang,
2014).
Table 2 shows that in all cases asphalt binder modification noticeably improved intermediate tem-
perature (IT) performance. DVR15-30 and DVR15-15 exhibited the best performance, and DVR15-60
showed the least IT improvement.
Binder GTR15-60 showed the best LT performance. A comparison between values in the LT-m-value
and LT-S-value columns in Table 2 shows that the m-value was by far the controlling parameter for
LT grade. This is the case for most binders. It is interesting to note that DVR modification improved
LT up to 1.5°C based on m-value, whereas the LT-S-value improved up to 7.4°C compared to the cor-
responding values for base binder. Previous studies (Lee et al., 2008) have also reported a significant
decrease in creep stiffness with slight changes in the logarithmic creep rate (m-value) for GTR and found
that m-value is not necessarily an appropriate parameter for modified binders (Velasquez et al., 2011).
All in all, it is implied that the optimum mixing duration for DVR in terms of performance is about
60 min.
1094 A. GHASEMIRAD ET AL.

Table . Binder viscosity test results.

Rotational viscosity (mPa·s) (viscosity ratioa )

Binder °C °C °C

Base binder . (.) . (.) . (.)

GTR- . (.) . (.) . (.)
DVR- . (.) . (.) . (.)
a Numbers in parentheses show the ratio of modified binder viscosity to base binder viscosity.

Table 3 shows the viscosity results for base binder, GTR15-60 and DVR15-60 (the DVR-modified
binder under its optimum mixing condition) binders. As can be seen, both GTR and DVR binders would
increase the viscosity noticeably; however, this increment was less in the case of DVR than that of GTR,
which is counted as an advantage of DVR modification over GTR.

3.2. MSCR test

AASHTO MP19 recommends the use of letters S, H, V, or E suffixes after the HT grades to indicate
suitability for withstanding “Standard,” “Heavy,” “Very heavy,” or “Extremely heavy” traffic levels and
traffic loading rates, based on Jnr3.2 values. Table 4 shows that binders with higher PG grades, including
GTR15-60, DVR15-60, and DVR25-30, were all graded S at their HT PG grade. All other binders having a
HT grade of 70°C, labeled as H, could carry high levels of traffic. MSCR testing at a reference temperature
of 64°C was also conducted to compare the recoverable and non-recoverable creep compliance for the
modified binders. It can be seen in Table 4 that DVR25-30, having the lowest Jnr3.2 , attained an E grade.
The next was DVR15-60 that showed one of the best performances that made it superior to the GTR15-
60 binder. The criterion JnrDiff ࣘ 75% was not met by any of the modified binders in Table 4; although this
result does not prove invalidity, it suggests that all the modified binders were highly sensitive to different
stress levels. Also regarding the R values at 64°C, Table 4 shows that GTR has better elastic properties
than DVR. However, among DVR15 binders, DVR 15–60 showed the maximum percentage of recovery
at 3,200 Pa (R3.2 ).
Figure 1 shows the creep compliance for the modified binders at 100 and 3,200 Pa stress levels at
64°C. In both stress levels, the highest strain level in the creep-loading portion of the test corresponded
to GTR15-60 and the lowest strain level to the highly modified binder DVR25–60. Among the DVR-
modified binders containing 15% modifier, DVR 15–60 recorded the lowest strain level in the creep
portion. Figure 1 also shows that the GTR-modified binder recorded the maximum rate of recovery of
all modified binders and continued recovering after the 9-s recovery portion of the test. On the whole,
regarding MSCR test results, DVR15-60 can again be considered as the binder with optimum mixing
conditions among DVR15-modified binders.

Table . MSCR test results at HT PG grade and °C.

@ HT PG grade @ °C

Binders Jnr. a Jnr. a JnrDiff (%)b Grade Jnr. a Jnr. a JnrDiff (%)b Grade R. (%)c R. (%)c

Base binder . . . S . . . S . .
GTR- . . . S . . . V . .
DVR- . . . H . . . V . .
DVR- . . . H . . . V . .
DVR- . . . S . . . E . .
DVR- . . . H . . . V . .
DVR- . . . S . . . E . .
a J is shown in (kPa)−1 .
nr
Jnr3.2 −Jnr0.1
nrDi f f = × 100%, with Jnr0.1 representing the non-recoverable creep compliance in a  Pa loading.
bJ
Jnr0.1
c R = ε p −εu × 100%, in which ε is the peak strain and ε is the unrecovered strain at each -s cycle
εp u p
 PETROLEUM SCIENCE AND TECHNOLOGY 1095

1.E-3 GTR15-60 1.E-3 GTR15-60

DVR15-15 DVR15-15
9.E-4 3200 Pa DVR15-30
100 Pa DVR15-30
@64°C DVR15-60
8.E-4 @64°C DVR15-60 8.E-4
DVR15-90 DVR15-90
DVR25-30 7.E-4 DVR25-30

6.E-4 6.E-4
J (1/Pa)

J (1/Pa)
5.E-4
4.E-4 4.E-4
3.E-4
2.E-4 2.E-4
1.E-4
0.E+0 0.E+0
0 1 2 3 4 5 6 7 8 9 10 0 1 2 3 4 5 6 7 8 9 10
Time (s) Time (s)
(a) 100 Pa (b) 3200 Pa

Figure . MSCR creep compliance and recovery curve for modified binders at °C.

3.3. Storage stability test

Standard ASTM D7173 testing was used to compare the separation tendency and storage stability of
the modified binders at high temperatures. Ring and ball softening points and DSR tests are usual to
be performed for this comparison (Zhang and Hu, 2015). Past experience using the softening point test
showed improvement in the storage stability of DVR-modified binders (Dong et al., 2011). DSR testing
at HT grade of each binder was used to examine the binder storage stability. Considering the positive
effect of sulfur as a cross-linking agent on the storage stability of polymer-modified binders through
vulcanization (Zhang and Hu, 2015; Sienkiewicz et al., 2017), 0.1% sulfur relative to the weight of binder
was introduced into the blend along with the GTR to create a reference binder (GTR15-60+Sul0.1-60)
for evaluation of storage stability. Table 5 shows that the non-cross-linked GTR binder exhibited a higher
complex modulus at the top of the tube and the DVR asphalt exhibited a higher complex modulus at the
bottom of the tube. The aggregation of modifier at the top or bottom portion of the tube resulted in harder
binders with higher complex modulus values. The swelling of crumb rubber particles from absorption
of binder aromatics (Cheng et al., 2011) lowers their density and results in accumulation at the top of
the blend. This swelling process did not occur for DVR, which caused settlement of the modified binder.
Table 5 shows that DVR did not improve the homogenization and long-term storage stability of the
binder. These findings contradict the findings of a previous work (Dong et al., 2011).

Table . Binder storage stability test results.

log G∗ Max−log G∗ Min
Binder Sample no. Part Test temp. (°C) G∗ (Pa) log G∗ logG∗ Average × 100

GTR-+Sul.-  Top  . . .%

Bottom  . .
 Top  . . .%
Bottom  . .
GTR-  Top  . . .%
Bottom  . .
 Top  . . .%
Bottom  . .
DVR-  Top  . . .%
Bottom  . .
 Top  . . .%
Bottom  . .
1096 A. GHASEMIRAD ET AL.

4. Summary and conclusion

The present study evaluated DVR as a potential substitute for GTR for modification of asphalt binders.
To this end, the properties of DVR-modified binders were compared to those of GTR-modified binder
and the base binder. It was found that DVR and GTR offered the best high temperature performances
for 60 min of mixing time. Regarding high temperature MSCR test results, it was found that at the same
modifier content of 15%, DVR-modified binder showed more resistance to traffic loadings rather than
GTR-modified binder. Also, DVR modification slightly improved the continuous LT grade over the base
binder, whereas GTR-modified binder offered more improvement in LT performance. The storage sta-
bility test results showed that the tendency of DVR to separate from the pertinent modified binder was
more than that for GTR. Finally, DVR-modified binder, mixed by 15% and for 60 min, proved to be the
best substitute for GTR-modified binder in terms of performance; however, its weaker storage stability
and higher material cost and similar dosage and mixing conditions to GTR-modified binder can make
it a non-economically viable alternative.

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