Journal of Cleaner Production 271 (2020) 122484

Contents lists available at ScienceDirect

Journal of Cleaner Production

journal homepage: www.elsevier.com/locate/jclepro

Low-content crumb rubber modified bitumen for improving

Australian local roads condition
Muhammad Jamal , Filippo Giustozzi *
Civil and Infrastructure Engineering, RMIT University, Melbourne, VIC, 3001, Australia

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

Article history: A global trend for developing sustainable transport infrastructure by adopting various sources of recycled
Received 8 January 2020 material is being promoted by researchers and media daily. Recycling End of Life Tyres (EOLTs) in the
Received in revised form form of Crumb Rubber (CR) builds on decades of past tradition. Local councils in Australia welcome
13 May 2020
recycling practices and sustainability although a general lack of guidelines is commonly acknowledged
Accepted 28 May 2020
for low-traffic roads. This paper evaluates the benefits of low-content crumb rubber modified bitumen
Available online 1 July 2020
(CRMB) for its application on Australian local roads, often exposed to very hot summer temperatures.
^ as de
Handling editor: Cecilia Maria Villas Bo Blending conditions play a vital role in CRMB; these include temperature, mixing duration and applied
Almeida shear rate or shear mixer speed. In this study, the influence of blending conditions on the physical,
chemical, thermal and rheological properties of low-content CRMB is investigated. Two shear mixing
Keywords: rates (700 and 3500 rpm) and three mixing durations (30, 60 and 90 min) were chosen and rubber-
Recycling modified blends were prepared with 7.5% CR. Rheological tests such as master curve, black diagram,
Crumb rubber Cole-Cole analysis, and Multiple Stress Creep Recovery were investigated. It was observed that the
End-of-life tyres
mixing duration has minimal effect on low-content CRMB, however, the applied shear rate has an impact
Multiple stress creep recovery
in the sense that it produces a relatively stiffer e and oxidised e blend at higher mixing speeds. This was
Bitumen
also correlated to the outcome from Fourier Transform InfraRed analysis (FTIR). Overall, the use of low-
content CRMB in local Australian roads can significantly improve the rutting performance while facili-
tating the recycling of end-of-life tyres.
© 2020 Elsevier Ltd. All rights reserved.

1. Introduction other countries, all the end-of-life material must be reprocessed

According to the yearly book of Australian Infrastructure Sta-
tistics (Australian Infrastructure Statistics-Yearbook 2018, 2018),
the total length of Urban and Non-Urban roads is approximately
877,651 km and is mostly paved with asphalt. Of these, almost 70%
are local roads administered by Councils. Asphalt pavements con-
structed from conventional bitumen are continuously struggling to
achieve their design life under increased traffic volumes and heavy
loadings (Li et al., 2009). Therefore, there is a growing trend of
modifying the conventional bitumen in such a way that it can resist
rutting, fatigue and other road distresses. Modification of bitumen
with Crumb Rubber (CR) is one of the top priorities in developed
countries to address some of the environmental and health issues
associated with the improper disposal of waste tyres (Genever,
2017). In Australia, due to recent bans for exporting waste to
locally (Pickin and Donovan, 2020). Several initiatives are under-
way to introduce new CR asphalt technologies in Australia and
increase the use of CRMB in both asphalt and sealings. Although the
rubber asphalt and sealing technology are relatively well under-
stood, there is currently no uniform framework to meaningfully
characterise and specify the CRMB performance, hence hindering a
broad use of the technology.
Bitumen modification with CR was first introduced by Charles
McDonalds in the 1960s, since then, the process has significantly
evolved and many states in the USA e i.e. Arizona, Florida, and
California e have developed their own CRMB specifications. CRMB
is commonly acknowledged to have improved rutting and cracking
resistance of conventional bitumen (Lo Presti, 2013). The final
properties of CRMB primarily depends on the extent of CR-bitumen
interaction. When the CR particles interact with the bitumen, two

* Corresponding author.
E-mail address: filippo.giustozzi@rmit.edu.au (F. Giustozzi).

https://doi.org/10.1016/j.jclepro.2020.122484
0959-6526/© 2020 Elsevier Ltd. All rights reserved.
2 M. Jamal, F. Giustozzi / Journal of Cleaner Production 271 (2020) 122484
types of processes occur; swelling and depolymerization or
devulcanization. The swelling process is dominant at temperatures
below 190
C while depolymerization occurs at temperatures
higher than 190
C (Jamrah et al., 2015). However, a longer inter-
action time may also result in the depolymerization of CR particles,
even at temperatures below 190
C (Wang et al., 2019b).
Swelling of CR is basically a diffusion process where oils (mal-
tene fraction) from bitumen migrate into CR particles, which then
results in the swelling of CR particles (Artamendi et al., 2006). The
swelling process is influenced by the bitumen type, CR source and
composition, CR production method, CR particle size and
morphology (Airey et al., 2003; Behl et al., 2013; Liu et al., 2009;
Loderer et al., 2018; Santagata et al., 2012). A soft bitumen
commonly interacts better with the rubber particles compared to a
hard bitumen because the rate of swelling is high in case of a low-
viscosity bitumen (Thives et al., 2013). Similarly, a larger particle
will take more time to swell as compared to a finer particle because
the rate of maltenic oil penetration into CR particles is inversely
proportional to the CR particle size (depth of penetration) (Bressi
et al., 2019). And even if all the material-relevant factors are kept
constant, then the blending conditions - which include blending
temperature, digestion time, applied shear rate and CR content -
would play a significant role. Blending temperature is considered as
one of the most influential factors (Lo Presti et al., 2012). Navarro
et al. (Navarro et al., 2007), conducted a very important study to
understand the influence of blending temperature and processing
devices on the properties of CRMB. Temperature was varied from
90 to 250
C and CR was mixed using a four-blade impeller, a helical
stirrer, an anchor stirrer and a pilot plant. He reported that the CR
particles in CRMB does not swell further if the temperature is kept
between 90 and 120
C. However, higher processing temperature
(i.e. 160-180
C) leads to a partial depolymerization/devulcaniza-
tion (approx. 4%) of the rubber network, increasing the number of
components that are incorporated into the bitumen phase
(bitumen matrix) and consequently reducing both solid concen-
tration and rubber particle size. The mixing devices were found to
be not influencing the mixing process as all the blends mixed with
different mixing devices were giving the same amount of solubi-
lized CR and rheological performance. Conversely, other authors
have found a clear dependence of binder properties from the mixer
speed and the applied shear rate (Lo Presti et al., 2012). According
to Mohammadi and Khabbaz (2013), it takes two days for bitumen
to dissolve 30% of the rubber at low agitation (i.e. 500 rpm) and 4 h
if the agitation is increased to 1500 rpm at 190
C. Agglomeration is
another mechanism that can contribute to the increase of viscosity
during the modification process. Therefore, a high shear rate en-
sures the proper dispersion of the rubber within the bitumen
matrix and helps in improving the storage stability of the final
blend (Lo Presti et al., 2012).
Additional influential factors e other than temperature and
mixing devices e are the mixer speed and mixing duration. Mashan
and Ali (Nuha S. Mashaan et al, 2011) studied the effect of blending
time and CR content on the CRMB properties. He used CR from 4 to
20% by weight of bitumen, and two mixing times - i.e. 30 and
60 min - and mixed using a propeller blade mixer at 200 rpm. He
reported that the mixing duration does not significantly affect
CRMB properties while CR content does. Tayh and Yousif (2018)
conducted a laboratory study to examine the effect of varying
mixing speeds (250, 750, and 1250 rpm) and blade levels (low, mid,
and high position) on 10% CRMB properties. The rubberized
bitumen was characterized in terms of viscosity and resistance for
rutting at high in-service temperature. The outcomes of this study
showed that the blade level had no considerable impact on the
properties of the modified binder, while the shearing rate was of
great effect. Kim and Lee (2015) produced 10% CRMB with four
blending periods (1, 30, 60, and 90 min) at 177
C and a mixing rate
of 700 rpm. Viscosity values at 135
C and 120
C were used as
evaluating parameters. Similarly, Kok et al. (Ko € k et al., 2018) used
10% of CR to modify bitumen at 180
C for 30 min, 60 min, 90 min
and 120 min mixing time and 1000 rpm, 2000 rpm and 5000 rpm
rotation speed. The evaluation parameters used in this study were
penetration, softening point, ductility, viscosity and G*/sin (d). It
was concluded that penetration and softening point test did not
show the effectiveness of CR obtained at various mixing conditions.
Moreover, an overall stiffening of the binder at high mixing speeds
was associated to oxidation although this observation was not fully
justified by any chemical test such as FTIR, Gas Chromatography or
SARA analysis. Gonzalez et al. (Gonza lez et al., 2012) also investi-
gated the effect of the gap between the rotor and stator of the
mixer, digestion time and temperature, and reported that a
blending time longer than 45 min at 180
C leads to an exponential
increase in viscosity due to “primary ageing” of the bituminous
base. At the same time, a decrease in viscosity takes place because
of the increase in the amount of rubber digestion. Nevertheless, the
gap between the rotor and stator seems to hold small influence
over the amount of rubber digestion.
It is very clear from previous literature studies that the blending
temperature is one of the critical factors in influencing the CRMB
properties. Moreover, it is of a consensus that higher temperature
(>190
C) depolymerizes the CR particles and ages the binder. This
alters the purpose of modification because the CR properties are
not properly reflected in the final rubber-modified bitumen.
As most of the studies address the performance of CRMB at high
dosage (i.e. more than 15%) and compare its performance with
polymer-modified bitumen, the use of the CR technology in asphalt
is not well-adopted by local councils as the roads they administer
are mainly composed by standard e unmodified e bitumen. The
use of CRMB at high percentage of CR is therefore seen as an un-
necessary cost increase in their limited annual budgets. Due to the
recent government push in implementing recycling practices,
councils are now looking at incorporating small amount of recycled
material in their roads (Rahman et al., 2020). An attempt has been
made in this paper to introduce low-content CRMB as a possible
construction and maintenance alternative to use more recycled
materials and facilitate the disposal of end-of-life tyres, while
keeping costs under control. In Australia, due to the rapid increase
in population and traffic, the local roads system is under extreme
pressure to guarantee new households a durable infrastructure.
Although the initial cost would be higher compared to roads con-
structed with standard bitumen, the overall pavement thickness
can be decreased due to the rubber modification and durability
increased; this is expected to possibly equalize the whole-of-life
costs (Dehghani et al., 2013; Giustozzi et al., 2012). In an effort to
help develop specifications for local administrations, this study is
focused on modifying bitumen with low content of CR and on
testing its rheological performance and blending parameters, such
as the influence of blending duration and applied shear rate. These
parameters could be considered by future specifications for local
roads, rather than relying on international standards previously
developed for high CR contents. The available worldwide CR
specifications were critically reviewed and the following di-
vergences were identified:
i International specifications recommend a CR dose of 17e22%;
their recommended blending conditions are thus based on such
high concentration, which cannot directly be transposed for
blending low CR contents (i.e. 7.5%).
ii The available specifications do not specify any speed of the shear
mixer when characterizing the properties of CRMB. In fact,
probably due to the high concentration of CR, this factor only
 M. Jamal, F. Giustozzi / Journal of Cleaner Production 271 (2020) 122484
plays a secondary role on the final blend performance. However,
7.5% (or lower contents) is a relatively smaller quantity and the
susceptibility of primary ageing of the base binder while mixing
at high speed may be worth exploring.
iii The worldwide specifications are mostly reliant on viscosity
values to prove the correct blending of CR in the bitumen.
Although viscosity is an important parameter for evaluating
binder workability, it cannot be solely used to predict the in-
service performance of the binder within the asphalt mixture.
Therefore, this study used a more comprehensive approach for
the development of CRMB specifications based on performance
properties:
⁃ G*: Complex shear modulus, which relates to the stiffness of
the material at various temperature and frequency values;
⁃ d: Phase angle, which relates to the viscoelastic properties of
the material;
⁃ Jnr and %R: Non-recoverable creep compliance and Percent
Recovery, which relates to rutting/resistance to permanent
deformation in the field.
2. Material & methods
2.1. Crumb rubber
CR was collected from a local recycling plant in Victoria,
Australia. Its chemical composition, gradation, and surface texture
are given in Table 1, Figs. 2 and 3, respectively. SEM images were
taken using the Philips XL-30. It may be noted in Fig. 3a that CR
particles are of irregular shape and rough texture. The surface area
of CR particles was calculated using the MasterSize-3000 particle
characterization system. A dry sample of CR particles weighing 100
±1g was analysed for Particle Size Distribution (PSD). The specific
surface area was 19.04 m2/kg.
The composition of CR particles was determined using the
thermogravimetric technique by employing Perkin Elmer Pyris-1
Thermogravimetric Analyzer. Samples were decomposed by vary-


ing the temperature from 50 to 850
C at a rate of 20 C/min. From


0 to 750 C, the atmosphere was kept inert using Nitrogen gas while
from 750 to 850
C, Nitrogen was replaced with air. The reason of
this mixed atmosphere for decomposition can be better captured in
Fig. 1 where the variability of the two gases on the TGA outcome of
the same material is depicted.
Samples were first run in Nitrogen atmosphere from 0 to 850
C.
It may be noted from the decomposition curve under the nitrogen
atmosphere that after 550
C the curve becomes smooth which
means that the sample is not decomposing further, even if the
temperature is being increased up to 850
C. At this stage, what is
left of the original sample basically contains carbon black plus inert
filler. In the second trial, samples were decomposed in air (as at-
mosphere) from 0 to 850
C. It can be observed that air alone cannot
be used as an atmosphere because synthetic rubber and carbon
black would simultaneously be decomposing, and it would be
difficult to differentiate between them. Therefore, to determine the
carbon black content, and the decomposition of other components,
the atmosphere was kept inert from 0 to 750
C using Nitrogen and
was changed from Nitrogen to Air after 750
C. The sequence of
Table 1
Chemical Composition of CR Particles from TGA analysis.
Oils Natural Rubber Synthetic Rubber Carbon Black Inert Filler
%
6.5 40.0 17.5 29.3 6.7
3
decomposition peaks was identified as oils (300
C), Natural and
Synthetic Rubber (between 300 and 750
C), Carbon Black
(>750
C) and Inert filler (Ash) (Ghavibazoo and Abdelrahman,
2013).
According to Genever et al. (Genever, 2017), the amount of
natural rubber, synthetic rubber, and carbon black in Australian
passenger car tires is around 20.5, 37.2 and 29.8%, respectively,
while Australian truck tires show a different composition of 42,
18.9, and 34.8%, respectively. Hence, the composition of the CR used
in this study was defined as being closer to that of truck tyres.
2.2. Bitumen C-320
Standard Australian bitumen C320 was collected from SAMI
Bitumen Technologies Pty Ltd. Its physical properties are provided
in Table 2.
2.3. Sample preparation
The influence of blending parameters on the rheological prop-
erties of CRMB was evaluated in this study. CR at 7.5% dosage (by
weight of bitumen) was added into the bitumen at 177 ± 10
C. The
available specifications do not provide guidance about the mixing
speed of the mixer and the available body of literature shows a wide
range of mixing speeds ranging from 200 rpm (Dong and Zhao,
2018) to 8000 rpm (Yu et al., 2011). The most commonly used
mixing rate for CRMB is 700 rpm and, if SBS or other modifiers are
to be added in the mix, then a mixing speed of 3000þ rpm has been
used by various researchers. Therefore, for the present study, it was
decided to use two shear mixing rates; namely 700 rpm (low) and
3500 rpm (high) to evaluate benefits and drawbacks associated
with the mixing speed, if any. Although many specifications require
approx. 45e60 min reaction time, literature studies (Artamendi
et al., 2006; Gawel et al., 2006; Wang et al., 2019b, 2019a) show
how shorter reaction periods can lead to insufficient penetration of
the oil in the rubber while excessively long reaction time can cause
depolymerization. Therefore, in this study, a blending duration of
30 min (i.e. a shorter reaction time to evaluate whether the maltene
fraction was able to penetrate the rubber particles), 60 min (i.e.
commonly indicated by standards worldwide) and 90 min (i.e. to
evaluate the potential depolymerization) were selected to test
CRMB. The CR was mixed using a Silverson L5M-A shear mixer.
2.4. Rheological evaluation
To evaluate the influence of blending parameters on the rheo-
logical properties of CRMB, a Dynamic Hybrid Rheometer-3 (DHR3)
from TA Instruments was used in this study. Frequency sweep and
multiple stress creep and recovery (MSCR) tests were performed on
the samples. Frequency sweep test was conducted at 5, 20, 40 and
60
C by varying the frequency from 0.1 to 15 Hz. The strain was
kept constant during the test at 0.01%, to keep the binder in the
Linear Viscoelastic (LVE) range. From 5 to 20
C, the 8 mm diameter
parallel plate geometry with 2 mm thickness was used while the
25 mm diameter plate with 1 mm thickness was used from 40 to
60
C. The output from the system was in the form of storage (G0 )
and loss modulus (G00 ) at the corresponding frequencies and tem-
peratures. This data was further used to calculate the complex
shear modulus (G*) and Phase angle (d) using the following
equations;
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
2
G* ¼ G’ þ G}2 (1)
4 M. Jamal, F. Giustozzi / Journal of Cleaner Production 271 (2020) 122484

Fig. 1. Decomposition curves of CR under different atmospheric conditions.

Fig. 2. Crumb rubber particles gradation.

Fig. 3. a) SEM image CR particles b) PSD Analysis of CR particles.

Table 2
Physical properties of bitumen C320.

Penetration at 25
C Softening Point Viscosity at 135
C Viscosity at 177.5
C

o
(1/10 mm) ( C) (Pa$s) (Pa$s)
59.3 48.0 0.62 0.30
 M. Jamal, F. Giustozzi / Journal of Cleaner Production 271 (2020) 122484
 
G}
d ¼ tan1
G’
MSCR was conducted in accordance with AASHTO T350-19 at
60
C. Samples were tested at three stress levels (0.1, 3.2 and
6.4 kPa) for 1 s loading cycle followed by 9 s recovery cycle. Twenty
cycles of Creep and Recovery were applied at 0.1 kPa while ten
cycles were applied at the next stress levels, according to the
standard. In the calculation of Non-Recoverable Creep Compliance
(Jnr) and percentage of Recovery (%R), the first ten cycles at 0.1 kPa
were ignored (conditioning cycles) and only the following ten cy-
cles were considered. Three replicates of each sample were tested,
and their average is reported in the paper.
3. Results & discussion
3.1. Master curve
Master curves are a convenient graphical representation of
frequency sweep test data. They show the dependence of G* and
d on loading frequency. To develop a master curve, the test data
collected at different temperatures need to be shifted to a single
reference temperature using the time and temperature super-
position (TTS) principle. Many methods are available to shift
rheological data sets; among these, the Arrhenius equation, Wil-
liamseLandeleFerry (WLF) equation or regression analysis
(Booshehrian et al., 2013). Once the shift factors are determined,
the data is further fitted to one of the models available in the
literature (i.e. sigmoidal, Christensen and Anderson Model) (Jamal
et al., 2018).
In this study, shift factors are calculated by regression analysis
and the data is fitted into the Sigmoidal Model using the following
equation;
a where ‘A’ is the area under the relative peaks.
logjG* j ¼ d þ
1 þ ebgðlogfr Þ
where ‘G*’ is the complex shear modulus at a given frequency ‘fr’, ‘d’
is the minimum G* of the binder, ‘a’ is the difference between
maximum and minimum G* of binder and ‘fr’ is the reduced fre-
quency (Hz). ‘b’ and ‘g’ are shape parameters of the curve. ‘b’ de-
scribes the horizontal position of the turning point of the curve, and
‘g’ describes the slope of the curve (Al-Haddad, 2015). Data sets at
all temperatures are then shifted to 20
C as reference temperature
to develop master curves, as shown in Fig. 4.
It can be noted from Fig. 4a) that the blending duration has an
almost negligible effect on G* of low-content CRMB prepared at
700 rpm over the entire range of frequencies. However, in com-
parison with C320 bitumen, there is a clear difference in CRMB
stiffness at lower frequencies. The addition of CR into C320 bitumen
increased the overall stiffness of the binder and is more visible at
slow loading rates, which is a positive aspect - from the perfor-
mance point of view - to increase the resistance to rutting. How-
ever, at higher frequencies, the complex shear modulus of CRMB is
similar to neat binder. Similar behaviour has been observed when
the shear mixer speed is increased from 700 rpm to 3500 rpm. To
understand the effect of the shear mixer speed on G* of CRMB, a
comparison of blends prepared at 700 and 3500 rpm has been
separately shown in the following figure.
Fig. 5 shows that an increase in shear mixer speed produces a
vertical shift of the master curve, which is more noticeable at lower
€k et al., 2018) also noticed an increase in
frequencies. Baha et al. (Ko
CRMB stiffness, if mixed at higher mixing rates (i.e. 5000 rpm). This
vertical shift can be an indication of the ageing susceptibility of
CRMB at higher mixing rates. To investigate this further, the
5
Fourier-Transform InfraRed spectroscopy (FTIR) test was performed
(2) on the samples. Spectrum 100 FTIR Spectrometer by Perkin Elmer
was used to get the modified-bitumen spectrum in the range of
650e4000 cm1 wavenumber. The test was conducted in attenu-
ated total reflectance (ATR) mode due to consistency in the repli-
cates as compared to transmission mode (Dougan et al., 2014). For
each spectrum obtained using this method, a total of 32 consecu-
tive scans at a resolution of 2 cm1 were collected (Fig. 6).
Carbonyl and sulphoxide groups are usually used for qualifying
bitumen ageing (Subhy et al., 2018; Ye et al., 2019) (Ye et al., 2019).
FTIR spectroscopy qualitatively identifies different types of func-
tional groups present in organic compounds and is often used for
monitoring the carbonyl and sulphoxide groups formation in aged
asphalt binder (Zhang et al., 2018). The strong peaks observed in
Fig. 6 at 2920 cm1 and 2851 cm1 are the CeH stretches of alkanes.
The peak at 1599 cm1 is C]C stretching vibrations in the aro-
matics. The asymmetric deformation of CeH in CH2 and CH3 and
the symmetric deformation of CeH in the CH3 were found in the
range of 1410e1495 and 1360e1395 cm1, respectively. The small
peaks between 650 and 810 cm1 are the CeH vibrations in the
benzene ring (Zhang and Hu, 2015). The small peaks at about
1680e1750 cm1 and 980-1060 cm1 are attributed to C]O and
S]O stretch in carbonyl and sulphoxide compounds, respectively.
By measuring the area (Spectragryph Optical Spectroscopy, version
1.2) of the IR bands, the relative amount of newly formed carbonyl
and sulphoxide compounds was calculated using the following
equations (Dony et al., 2016; Porot et al., 2018);
Acarbonylð16801750Þ
CI ¼ (4)
ACH2ð14101495Þ þ ACH3ð13601390Þ
Asulphoxideð1060980Þ
SI ¼ : (5)
ACH2ð14101495Þ þ ACH3ð13601390Þ
(3)
Carbonyl and sulphoxide indices (CI & SI) of neat and CR
modified binders are shown in Fig. 7.
From Fig. 7, if a comparison is to be made between the ageing
indices of the two crumb rubber blends prepared at different
mixing speeds, it can be easily noted that the shear mixer speed has
a significant contribution on the sulphoxide index of CRMB. Blends
prepared using 700 rpm have an SI value of 0.135, although when
the mixer speed is increased to 3500 rpm, the SI value increased to
0.186.
No significant difference was noticed for the CI index instead.
3.2. Black diagram
Black diagram is a representation of raw rheological data
(complex shear modulus and phase angle) regardless of any shift-
ing occurring when developing master curves. In fact, the latter
procedure can be only applied to thermo-rheological simple ma-
terials (hence complying with the time-temperature superposition
principle) and it is commonly acknowledged that polymer-
modified bitumen shifts its thermo-rheological simplicity to more
complex behaviour. Black diagram is developed using the phase
angle and complex shear modulus of the binder without any
manipulation of the rheological data. Black diagrams have many
advantages; i.e., finding inconsistencies in the rheological data,
distinguishing between the thermo-rheological simple and com-
plex materials, compliance of DSR geometries and confirming
polymer modifications (Airey, 2011).
The influence of blending conditions on the Black diagrams has
been shown in the following figures.
6 M. Jamal, F. Giustozzi / Journal of Cleaner Production 271 (2020) 122484

Fig. 4. Master Curves of C-320 bitumen modified with 7.5% of CR at a) 700 rpm and b) 3500 rpm for 30, 60 and 90 min mixing.

Fig. 5. Influence of shear mixer speed on blends’ master curve prepared using 700 and 3500 rpm mixed for a duration of 60 min.

Fig. 8 shows that the blending duration does not affect the shape
and magnitude of CRMB black diagrams at both low and high
mixing speeds. However, there is a difference between the shape of
a CRMB black diagram and that of C320. The black diagram of
standard C320 bitumen is continuous and smooth which is in
agreement with previous studies where neat bitumen showed a
smooth transition when it switches from a viscoelastic solid to
viscoelastic fluid, hence showing a thermo-rheological simple
behaviour (Nivitha et al., 2018). Moreover, at 60
C, the phase angle
of C320 is close to 90
which shows that the material is in the fluid-
 M. Jamal, F. Giustozzi / Journal of Cleaner Production 271 (2020) 122484
Fig. 6. FTIR spectra of C-320 and CRMBs.
Fig. 7. Influence of shear mixer speed on the ageing indices of CRMB
viscous state. Although CRMB black diagram follows a similar trend
for smaller phase angles (i.e. low temperature of testing), it rapidly
discontinues after the phase angle achieves approx. 68
. The
rheological response at this point can be better explained by un-
derstanding the constituent material. When CR particles are added
into bitumen, some CR particles dissolve while some remain
insoluble. At low temperature, the system made by insoluble CR
particles and bitumen with soluble CR particles acts as a single unit
because the bituminous part of CRMB shrinks, pulling the insoluble
CR particles closer to each other. Thus, the overall stiffness of this
unit is lower than that of C320 alone because of the presence of CR
particles. However, when the temperature is increased, C320
bitumen simply melts and smoothly transfers from a glassy state to
viscous solid and then from viscous solid to viscous fluid (ther-
morheologically simple behavior). On the other hand, when the
temperature is increased for CRMB, due to its bi-phasic nature, the
bituminous phase melts and CRMB no longer acts as a single unit;
the insoluble CR instead acts as a suspended particle. The sus-
pended particles are not able to form any long-range network
because the viscosity of the liquid medium around the CR particles
7
is high, hence restraining any motion of CR particles. The chance of
any colloid-chemical activity is thus hindered and suspended CR
acts as inert particles. The bituminous phase at this point has a
small contribution towards resisting the external shearing forces,
which are mainly sustained by CR particles; this appears in the
form of a sudden drop in the black diagram. At this point the black
diagram can be divided into two sections; a polymer-dominant
phase for phase angle values above 68
(7.5% CR), and a bitumen-
dominant phase for lower values of the phase angle (i.e. low tem-
perature of testing). At low G* values of C320, the small rubber
content provides an increased elastic response by reducing the
phase angle values of approx. 10
.
To evaluate the relative effect of the mixer speed on the rheo-
logical properties, a comparison has been made for the blends
prepared at 700 and 3500 rpm mixed for 60 min (Fig. 9).
It can be noted from Fig. 9 that the rotational speed of the mixer
influences the rate of change of curve. At smaller phase angles, the
blend prepared at 3500 rpm has a higher complex shear modulus
than the one prepared with 700 rpm. However, after the phase
angle reaches 68
, a sudden drop in the complex shear modulus
value is identified which then leads to both types of blends showing
almost the same G* trend at corresponding phase angles. As
already discussed, this was identified as the rubber-dominant re-
gion; e.g. where the rubber addition provided the greatest contri-
bution to the bitumen rheological behaviour.
3.3. Cole-Cole plot
Cole-Cole plot is a way to show a graphical description of the
viscous and elastic part of the material’s stiffness under study. It
illustrates the contribution of elastic (storage modulus) and viscous
(loss modulus) components that contribute to the overall stiffness
of the material. A Cole-Cole plot is typically plotted between the
storage and loss modulus. The frequency at which G0 becomes equal
to G00 is called crossover frequency, the inverse of which is called
relaxation time. Therefore, a line at 45
angle in Cole-Cole plot is
usually drawn to indicate the location of G’ ¼ G00 points. Any ma-
terial above this line is in the viscous dominant phase (liquid like),
while any material below this line is in the elastic dominant phase
(solid like). The Cole-Cole plot for the C-320 and CRMB mixed at
8 M. Jamal, F. Giustozzi / Journal of Cleaner Production 271 (2020) 122484

Fig. 8. Black Diagrams of C320 Bitumen modified with CR at a) 700 rpm b) 3500 rpm.

Fig. 9. Influence of shear mixer speed on the black diagram of CRMB

 M. Jamal, F. Giustozzi / Journal of Cleaner Production 271 (2020) 122484 9

Fig. 10. Cole-Cole plot for C320 bitumen modified with CR at a) 700 rpm and b) 3500 rpm and mixed for 30, 60 and 90 min..

different durations and with different mixing rates is shown in greater the defects at molecular level, the poorer will be the
Fig. 10. interaction between bitumen and CR and higher will be the h value.
It can be noted from Fig. 10 that the blending duration has According to Rolere et al. (Rolere et al., 2017), h can be calculated by
minimal effect on the relative contribution of viscous and elastic simply plotting the G0 -G00 on a linear scale and fitting it to the
components at the entire range of stiffness values. However, the fourth-order polynomial; finally, the following equation is used to
major portion at lower stiffness values of C320 bitumen shows a calculate h;
greater viscous component which means that the material behaves
  ’ 
more like a liquid and loses its ability to store the applied energy. A 2 dG
h¼ arctan lim : (6)
major portion of this energy is dissipated, which appeared in the p dG} G’/0
form of greater loss modulus (G00 ) value. The addition of CR into
C320 bitumen increased the overall stiffness as well as the ratio The h values for the different blending conditions are presented
between the viscous and elastic component and made the binder in the following table.
more elastic at lower stiffness values. The credit for this improved It may be noted from Table 3 that the interaction between CR
elastic nature of the material goes to CR. When CR is added into particles bitumen is affected by both mixing duration and mixer
bitumen, oils from the bitumen migrates into the CR due to diffu- speed. At 700 rpm, the h value decreases after 60 min showing an
sion process which makes the particles swell, hence reducing the
inter-particle distance and increasing viscosity of the bituminous Table 3
component. The increase in viscosity of the bituminous component Influence of mixing duration and mixer speed on h values of CRMB.
provides sufficient resistance to flow, while the CR particles provide
Mixing Duration Mixer Speed
resistance to deformation and ability to store the applied the en-
ergy which makes the overall response of the material more elastic. (minutes) 700 3500
(rpm)
Perez et al. (Perez et al., 1988) studied polymers rheology and
30 0.5564 0.5649
introduced a new parameter ‘h’; the study found that h is linked to 60 0.5515 0.5716
the topographic defects of the polymers at the molecular level. The 90 0.5572 0.5793
10 M. Jamal, F. Giustozzi / Journal of Cleaner Production 271 (2020) 122484

Fig. 11. Influence of shear mixer speed on Cole-Cole plot of CRMB

Fig. 12. Influence of mixing speed and mixing duration on Jnr and %R of CRMB
 M. Jamal, F. Giustozzi / Journal of Cleaner Production 271 (2020) 122484
Fig. 13. Influence of the stress level on Jnr and %R of CRMB
improved interaction and increases at 90 min which is linked to
disturbance in the developed polymeric network (i.e. depolymer-
ization) with increased mixing duration. Moreover, by increasing
the mixer speed to 3500 rpm, the developed polymeric network is
optimal after just 30 min of mixing. This shows that e at low CR
content e increasing the mixer speed reduces the mixing time
required for swelling CR particles. However, the overall h values of
CRMB blends prepared at 3500 rpm are higher than those of blends
prepared at 700 rpm, showing relatively poor interaction.
From Fig. 11 it can be inferred that the influence of shear mixer
speed on the Cole-Cole plot is limited. Moreover, at lower stiffness
values, the CRMB Cole-Cole plot is more inclined towards the 45o-
line showing the elastic contribution due to CR modification.
3.4. Rutting potential (multiple stress creep recovery)
Jnr and %R were calculated from the MSCR test data at each stress
level for all the samples and are plotted in this section. Error bars
are also added to show the variability within the three replicates at
each test condition. It can be noted from Fig. 12 that C320 bitumen
has very high non-recoverable deformation and minimal %R at
60
C. With a softening point of just 48
C, standard bitumen cannot
withstand plastic deformation at high temperature. Air tempera-
ture in excess of 40e45
C is not uncommon during hot Australian
summers.
With a minimal addition of 7.5% of CR, CRMB non-recoverable
strain is reduced to half of the original C320. Moreover, a
11
significant improvement can be observed in the percent recovery of
C320 bitumen with the addition of CR. As far as the influence of
mixing is concerned, no significant difference in terms of Jnr and %R
value was observed with increasing the shear rate and mixing
duration although a slight improvement was noticed when
increasing the mixing speed (i.e. reduced Jnr and increased %Re-
covery at 3500 rpm) or extending the mixing time (i.e. reduced Jnr
and increased %Recovery after 90 min). The influence of different
stress levels on the non-recoverable strain and recovery is shown in
Fig. 13.
It can be noted that C320 bitumen has similar Jnr value at all the
stress levels, which produces further evidence that the test tem-
perature is quite high for it to resist to any applied stress. Similarly,
%R of C320 is minimal and was further reduced when the stress was
increased from 0.1 to 6.4 kPa. As far CRMB is concerned, it can be
concluded that a significant decrease in Jnr and increase in %R were
observed compared to standard bitumen, hence possibly improving
resistance to rutting in the field. Moreover, the shear mixer speed
was deemed to have an influence on Jnr and %R, although minimal
in magnitude. The blend prepared at 3500 rpm had lower Jnr and %R
value compared to the blend prepared at 700 rpm. This shows that
the 3500-rpm blend retains stiffer and less elastic behaviour at
60
C; this agrees with the observations made in the master curve
and black diagram sections and FTIR analysis. When increasing the
stress level up to 6.4 kPa, the benefits provided by the crumb rubber
modification are evident.
12 M. Jamal, F. Giustozzi / Journal of Cleaner Production 271 (2020) 122484
4. Conclusions
This study evaluated the possible benefits of adding a limited
quantity of crumb rubber into bitumen for improving local roads
condition when exposed to a warm environment. This is expected
to further facilitate the reuse of end-of-life tyre, especially in
countries where the current regulation does not allow any expor-
tation of waste material.
Based on the experimental results, the following conclusions
can be drawn;
- the mixing duration between 30 and 90 min does not have a
significant influence on the rheological properties of CRMB, if
the mixing temperature is kept below 190
C and the amount of
rubber is limited;
- the shear mixer speed influences the chemical and rheological
properties where a higher mixing rate enhances the ageing of
CRMB and this further increases the complex shear modulus
(and reduce the phase angle) of CRMB as compared to slow
mixing rates;
- small additions of CR into bitumen can significantly enhance the
rutting resistance of CRMB according to the MSCR test;
- On average, the addition of CR decreases Jnr by 63% whereas CR
improves %R by thirteen times at 3.2 kPa compared to standard
bitumen;
- CR also significantly enhances the properties of CRMB (i.e.
decreased Jnr and increased %Recovery) when the stress is
increased from 0.1 to 6.4 kPa compared to the standard bitumen.
Overall, the addition of small quantities of CR into standard local
roads mixes seems to better support the increasing traffic loads in
hot Australian conditions. The addition of CR should be modulated
with the proper design of the asphalt layer thickness and whole-of-
life cost considerations.
CRediT authorship contribution statement
Muhammad Jamal: Conceptualization, Formal analysis, Data
curation, Investigation, Methodology, Writing - original draft,
Writing - review & editing. Filippo Giustozzi: Conceptualization,
Formal analysis, Data curation, Methodology, Writing - review &
editing, Project administration, Funding acquisition, Supervision.
Declaration of competing interest
The authors declare not to have any conflict of interest.
Acknowledgments
Muhammad Jamal would like to acknowledge the support given
by Tyre Stewardship Australia under the scholarship “Crumb rub-
ber asphalt binder characterisation and specifications for road
pavement applications”.
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