Journal of Cleaner Production 289 (2021) 125727

Contents lists available at ScienceDirect

Journal of Cleaner Production

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

Review

Natural rubber as a renewable and sustainable bio-modifier for

pavement applications: A review
Anwaar Hazoor Ansari a, b, *, Fauzan Mohd Jakarni a, **, Ratnasamy Muniandy a,
Salihudin Hassim a, Zafreen Elahi a, b
a
Department of Civil Engineering, Faculty of Engineering, Universiti Putra Malaysia, 43400, Serdang, Selangor, Malaysia
b
Department of Civil Engineering, Faculty of Engineering, Balochistan University of Information Technology, Engineering, and Management Sciences, 87300
Quetta, Pakistan

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

Article history: The increasing demand for non-renewable resources such as bitumen is a significant problem in the
Received 24 June 2020 pavement industry. Flexible pavement primarily relies on and consumes a large quantity of bitumen,
Received in revised form which has become a significant problem in terms of environmental sustainability and economic
1 December 2020
standpoints. Hence, researchers strive to explore alternative solutions such as bitumen modifiers to
Accepted 26 December 2020
Available online 30 December 2020
prolong the lifespan of flexible pavements. One such modifier is natural rubber (NR), and it has exhibited
some beneficial effects for bitumen and asphalt mixtures. However, its adoption as a modifier in the
Handling editor: Prof. Jiri Jaromir Kleme
s pavement industry is constrained. Hence, the main objective of this review is to analyse the literature in
depth to reveal the possibilities of alternative uses of NR as a modifier in the pavement industry. NR in
Keywords: the forms of latex and cup lump was observed to improve the physical, rheological, and mechanical
Natural rubber performance of bitumen. The uncross-linked polymer of fresh NR can easily swell and be absorbed by
Cup lump bitumen. In addition, the effect of blending variables is interdependent on the physical properties of the
Latex modified bitumen. However, NR decreases the workability of the asphalt mixture, which can be
Bitumen
compensated for by warm mix additives. The optimum content of NR for bitumen to improve pavement
Bio-modifier
performance is 4e6 wt.%. Meanwhile, NR absorbs 24.9 kg of CO2 to produce 1 kg of NR latex. This paper
Sustainability
also discusses improved field condition indicators of NR-modified pavements. Finally, recommendations
for future research and development are provided to promote the utilisation of NR in the forthcoming
sustainable pavement industry.
© 2020 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. Method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
3. Physical and chemical properties of natural rubber . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.1. Natural rubberebitumen system and interaction process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
4. Natural rubber as bitumen modifier . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
4.1. Natural rubber production for bitumen modification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
5. Physical and rheological properties of natural-rubber-modified bitumen . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
5.1. Natural rubber as latex for bitumen modification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
5.2. Coagulated natural rubber for bitumen modification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
5.3. Chemical additives as co-modifier for natural rubber modified bitumen . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
6. Performance properties of natural rubber asphalt mixture-latex and coagulated . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11

* Corresponding author.
** Corresponding author. Department of Civil Engineering, Faculty of Engineering,
Universiti Putra Malaysia (UPM), 43400, UPM, Serdang, Selangor, Malaysia.
E-mail addresses: gs52876@student.upm.edu.my (A.H. Ansari), fauzan.mj@upm.
edu.my (F.M. Jakarni).

https://doi.org/10.1016/j.jclepro.2020.125727
0959-6526/© 2020 Elsevier Ltd. All rights reserved.
A.H. Ansari, F.M. Jakarni, R. Muniandy et al. Journal of Cleaner Production 289 (2021) 125727

7. Field performance of natural rubber modified asphalt mixture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12

8. Challenges in expanding natural rubber applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
9. Conclusions and recommendations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
Acknowledgement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14

1. Introduction conducted in the United Kingdom in the 1950e1960s (Wen et al.,

2017). The production of global NR has increased from approxi-
Environmental sustainability is an emerging concept of the mately 6.9 to 13 million metric tons (MMT) from 2001 to 2017.
modern millennium development goals. It is defined as the use of However, the price has significantly decreased since 2011 and is
non-renewable resources in a manner that satisfies present-day likely to continue to decrease (Board, 2018). Fluctuation in the
demands without compromising the requirements of forth- production and rate of rubber has created significant demand for
coming generations (Aziz et al., 2015; Kuhlman and Farrington, the alternative use of NR (Zborowski and Kaloush, 2007). Hence,
2010). However, the global demand for non-renewable resources the use of NR as a modifier for asphalt can generate a win-win
is currently a significant concern. Hence, to ensure the concept of condition by benefiting the financial burdens of the rubber tree
sustainability, researchers are giving high priority to alternative or farmers. In addition, it can cost-effectively enhance the road
bio-renewable sources (Vinod et al., 2020). The bio-based economy, structures that are under deprived conditions in various NR-
in which energy generated from organic renewable sources is used producing countries. Therefore, this review focuses on the NR
irrespective of natural fossil fuel, is of particular interest globally. modification of bitumen for the construction of road pavements,
Thus, this ultimately saves the sources of energy from rapid aiming to highlight possible solutions for the above problems and
depletion, and the safety of the environment is ensured (Demirbas encouraging and promoting the concept of sustainability. Conse-
and Balat, 2006). Concerning the economy of any country, energy quently, a comprehensive overview of the technical development
and environment are the utmost demanding problems. Hence, bio- over the last few decades has been summarized and discussed. The
based sources are assets to countries as they are renewable, envi- physical, rheological, and mix-performance characterization of NR
ronmentally friendly, efficient, and less costly (Al-Sabaeei et al., with bitumen and chemical additive as a co-modifier is also
2020b; Mohan et al., 2006). reviewed.
The road network is the principal sector for global asset man-
agement. Approximately 95% of the world’s roads are created from
2. Method
flexible pavements, and bitumen is used as a traditional binder for
road materials (Aziz et al., 2015). Bitumen is a natural constituent
The identification of the most related articles was followed by a
that results in the refinement of crude oil with thermoplastic
four-step sample selection approach, i.e., database selection, pre-
behaviour and waterproofing properties (Zhu et al., 2014). The
liminary searching, selecting the sample, and refining the sample.
highest usage of bitumen is in the construction of road pavements,
The procedure for selecting review samples is shown in Fig. 1.
which is approximately 85% of its total consumption (Institute,
However, various data sources can be utilized for index publication,
2015). The use of unmodified bitumen reduces the service life of
i.e., Scopus, Google Scholar, the Web of Science, and PubMed.
the road and increases the volatility of road performance and cost.
Therefore, after initial analysis and comparison, the Web of Science
Considering the performance and service life of a road, many
contained the most related research and was used as the key search
studies were conducted over the past decades on polymer-
database. Google Scholar was used to further refine the sample.
modified bitumen (PMBs) with significantly increased benefits
Initial keyword searching was performed in the database, and 1102
(Ko€k et al., 2014; Yildirim, 2007). PMBs significantly improve the
papers related to NR and bitumen were found. This review includes
performance of the asphalt mixture and service life cycle of high-
only articles in English, published in databases such as SCI-
way pavements, but they also have disadvantages (Padhan et al.,
expanded, SSCI, A&HCI, CPCIeS, and ESCI. For sample selection,
2015). A polymer with virtuous properties can increase the elas-
all irrelevant studies were excluded from the initial search through
ticity and flexibility of the asphalt mixture, ultimately improving
a reading of the title and abstract. Papers that were challenging to
the thermal cracking and fatigue characteristics of asphalt mixtures
screen were analysed thoroughly, and finally, 29 articles that were
(Al-Mansob et al., 2014; Pasandín and Pe rez, 2015). The declination
highly related to the topic were selected. For the timely update of
of oil reserves has caused an increasing demand for alternative
the sample, Google Scholar was used and a total of 32 articles were
pavement binders and modifiers (Fini et al., 2011). Consequently,
finalized for an in-depth review.
extensive research has been conducted to partially replace tradi-
After the introduction and method section, the remainder of the
tional bitumen with bio-binders derived from biomasses to
article is structured as follows: Section 3 describes the physical and
enhance their feasibility (Fini et al., 2011; Peralta et al., 2012; Wen
chemical properties of NR and the interaction with bitumen; Sec-
et al., 2013). Thus, industries are becoming broader in the use of
tion 4 describes NR as a bitumen modifier and its production for
natural rubber (NR) as a modifier to replace bitumen up to some
such a modification; Section 5 discusses the physical and rheo-
proportion.
logical properties and the chemical additives of NR-modified
NR is extracted from trees through tapping and is used to modify
bitumen; Section 6 presents the performance-based properties of
bitumen as a biopolymer. NR as a biopolymer has been effectively
NR-modified mixtures; the full-scale field performance is discussed
utilized over many decades in the manufacturing of tires and gloves
in Section 7, followed by challenges in expanding NR applications in
and for building and road construction (Ibrahim et al., 2014). Most
Section 8; Section 9 concludes the review-based study. Fig. 2 pre-
of the research on the modification of bitumen with NR was
sents the detailed framework of this review study.

2
A.H. Ansari, F.M. Jakarni, R. Muniandy et al.
Fig. 1. Four-step sample selection procedure.
3. Physical and chemical properties of natural rubber
NR is a multipurpose agricultural product and is used in
approximately 50,000 products worldwide (Nair, 2010). Rubber
was first used during the Olmec civilization and its usage was
sustained among the Mayans (Yucatan peninsula in Mexico) and
Incas (Andes highlands, Peru) (Greve, 2000). A Spanish rector, P.
Martyre d’Anghiera, was first to write about rubber in his book ‘De
Orbo Novo’ in 1530. However, the worthwhile use of rubber
remained unidentified among Europeans for approximately 200
years (Shinzo Kohjiya and Ikeda, 2014). Hence, NR became a
scientifically imperative reserve and an indispensable material af-
ter the discovery of vulcanization (Mathew, 1992; Nakao and
Kohjiya, 2014).
NR is created from a runny, milky white liquid called natural
rubber latex (NRL) that drips from the bark of tropical and sub-
tropical plants through tapping. Approximately 99% of global NR
comes from the tree species Hevea brasiliensis. After the NR tree is
tapped, NRL is collected in a cup to avoid it flowing to other parts of
the tree. Primarily, there are two main methods of collecting NR;
the first is the preservation of latex as a liquid by adding some
quantity of ammonia and proceeding to the pattern the rubber in
soft slabs. The second is collecting latex in hard form by letting it
coagulate in the collection cups by itself or by adding formic acid to
3
Journal of Cleaner Production 289 (2021) 125727
convert to faster to cup lump natural rubber (CLNR) (Groover,
2010). Sometimes, a latex film formed on a tapping cut (lace) and
dripped on the ground (scrap) is also collected with a cup lump
(Baker et al., 2012). Higher-grade rubber forms are then processed
from CLNR to form pale creep, ribbed smoke sheet, block rubber,
and air-dried sheet (Bhowmick, 2000). In addition, it is also used to
form technically specified rubber (TSR10 and TSR20) and viscosity-
controlled grade rubber (TSR10 CV and TSR20 CV (Franta, 2012).
NRL exists as a colloid in which rubber particles are suspended
in the serum. It also contains many non-rubber components such as
phospholipids, proteins, carbohydrates, and inorganic salts. NR is
significantly affected by non-rubber ingredients (Nawamawat et al.,
2011). Table 1 shows the fresh latex composition of the NR.
Conversely, Hevea brasiliensis is essentially pure poly-cis-1,4
isoprene (comprising 99.9% of cis 1,4 structural units) and its par-
ticles vary in size from 0.15 to 3 mm; it has the chemical formula
C5H8 with a molecular weight of 105e106 Da (Shinzo Kohjiya and
Ikeda, 2014). Fig. 3 shows the chemical structure of cis-1,4-
polyisoprene in NRL extracted from Hevea brasiliensis. Non-
isoprene structural units and backbone may also be bonded the
ends of its macromolecules. These may also be epoxide, ester,
aldehyde, and eventually lactone groups. In addition, some of the
non-rubber additives that are present in the latex remain in the
rubber. Their content may be different but generally vary in the
A.H. Ansari, F.M. Jakarni, R. Muniandy et al. Journal of Cleaner Production 289 (2021) 125727

Fig. 2. Framework of the article.

range of 5e10 (Matador Rubber, 2007; Nakao and Kohjiya, 2014). NR undergoes easy cross-linking or vulcanization. Therefore,
Despite their small amount in rubber, they have significant effects almost all rubber products must be three-dimensionally structured
on the NR properties. networks to exhibit a stable elasticity (Ikeda et al., 2018). NR pri-
Because of the presence of a double bond in its repeated units, marily exhibits elasticity owing to its high stretch ratio and

4
A.H. Ansari, F.M. Jakarni, R. Muniandy et al. Journal of Cleaner Production 289 (2021) 125727

Table 1 a significant effect on the properties of the modified binder spe-

Composition of fresh NRL (Bhowmick, 2000; Matador
Rubber, 2007).
Constituent Content%
Rubber 30e40
Protein 1.0e1.5
Resins 1.5e3.0
Minerals 0.7e0.9
Carbohydrates 0.8e0.1
Water 55e60
Fig. 3. Chemical structure of cis-1, 4-polyisoprene in NRL extracted from Hevea
brasiliensis.
resilience characteristics, mostly owing to a chain of polyisoprene.
Under loading, it behaves like a linear chain, and when the load is
released, it wrinkles back (Greve, 2000). NR has a flexible molecular
chain owing to its amorphous mass of coiled structures that make it
too soft to be used for any useful purpose (Tinavallie A/P
Grumoorthy, 2013). It has gained interest owing to its various
beneficial properties such as high tensile strength, elasticity, flexi-
bility, crack growth resistance, and low heat build-up (Sriring et al.,
2018). In addition, NR also exhibits some viscoelastic properties and
various behaviours. Before cross-linking, it is like a viscous liquid,
and when vulcanized or cross-linked, it becomes solid or more
elastic (Mathew, 1992). NR also tends to crystallise upon cooling at
low temperatures or by stretching it in a specific direction. There-
fore, the unstrained rubber achieves maximum crystallisation
at
26  C and has a crystalline melting point of 25  C (Tinavallie A/P
Grumoorthy, 2013). Crystallisation limits movement between
neighbouring molecular chains and results in a substantial increase
in hysteresis and ultimate strength. Table 2 summarizes the prop-
erties of NR.
3.1. Natural rubberebitumen system and interaction process
cifically for storage stability and transport (Abdelrahman and
Carpenter, 1999). The stability or the phase behaviour of polymer-
modified bitumen originates from the material’s physical and
chemical nature, which affect bitumen properties (Zhu et al., 2019).
For example, the bitumen frequently has varying chemistry owing
to various crude oil sources, and this will affect the compatibility
with the NR. However, the solubility parameter has been reported
to be approximately 16.9 MPa0.5 for NR and in the range
17.2e18.8 MPa0.5 for bitumen (Mark et al., 2013; Zhu et al., 2019).
This similarity in parameters indicates that bitumen behaves as a
swelling agent for NR. The interaction process has two main stages:
rubber swelling (physical diffusion process) and degradation (a
chemical process that creates new substances) (Abdelrahman and
Carpenter, 1999; Wang et al, 2017, 2020a). When NR interacts
with the preheated bitumen, the low molecular weight fraction of
bitumen (maltenes) is dispersed and absorbed by the network of
the polymers, causing it to swell.
Vulcanized (cross-linked) and non-vulcanized (uncross-linked)
rubber have different behaviours and interaction stages when
interacting with the bitumen. The uncross-linked polymer consists
of long chains forming folded coils that are entangled with each
other without any links and can be easily dispersed, swollen, and
ultimately absorbed by the solvent (Fig. 4a). In contrast, the cross-
linked network of rubber, which has constraints owing to the links
between chains of polymers, may swell because of being absorbed
by the solvent, but hardly any dissolution occurs (Mark et al., 2013;
Wang et al., 2020a) (Fig. 4b). However, the equilibrium of swelling
can vary by scenario and significantly relies on the
bitumenepolymer combination and thermal conditions (Wang
et al, 2019, 2020b).
From the perspective of the chemical degradation of rubber, the
cross-linked polymers counteract the degradation of the rubber
network. However, the high temperature, high shearing energy,
and extended mixing time destroy the complex vulcanized struc-
ture of rubber (Zanzotto and Kennepohl, 1996). Thus, reduction in
the molecular weight of the rubber occurs because of the scission
process of chemical bonds of cross-linking (disulphide bonds,
carbonesulphur bonds) and backbone chain bonds (carbon-
ecarbon bonds). As discussed earlier, uncross-linked NR can swell
up and absorb easily in the bitumen because of the non-existence of
cross-linking bonds, which require high energy and much time for
de-vulcanization.

NR-modified bitumen is typically produced by mixing rubber

and bitumen at high temperatures for a certain time. In polymer 4. Natural rubber as bitumen modifier
science, bitumen is frequently considered a low-molecular-weight
solvent, and rubber can be considered a high-molecular-weight From a historical perspective, the use of granulate NR as a
polymer (Lesueur, 2009). The interaction of bitumen and NR has bitumen modifier for paving roads began in the 1840s (Sienkiewicz

Table 2
Summary of natural rubber properties (Niranjan Karak, 2009).

Item Attribute Properties

Molecular behaviour Glass transition temperature
70  C

Hardness range 30e100 shore A
Maximum tensile strength 27.58 MPa @ 21.11  C
Maximum elongation 50% @ 21.11  C
Advantages Physical resistance Excellent resistance
Excellent tear strength
Excellent abrasion
Impact strength
Environmental resistance Good compression resistance
Excellent water resistance
Good low-temperature flexibility
Chemical resistance Good oxidation resistance
Excellent resistance to alcohol and oxygenated solvents

5
A.H. Ansari, F.M. Jakarni, R. Muniandy et al.
Fig. 4. Molecules representation of (a) uncross-linked polymers (b) cross-linked polymers (Mark et al., 2013; Wang et al., 2020a).
et al., 2017). Bitumen modification was performed even before
refined bitumen was produced; people had been modifying natural
bitumen with NR to create more wear-resistant bitumen, and few
patents were also granted (Yildirim, 2007; Zhang et al., 2010). NR is
a remarkable modifier that can be efficiently added to bitumen
(Zborowski and Kaloush, 2007). Owing to good tear strength,
resistance against fatigue, and higher stability, NR extends the
stability of asphalt pavements (Colin Ruggles, 2005). Thus, some
studies supported NR as a modifier owing to its excellent low-
temperature properties and minimal loss of hysteresis on dy-
namic loading (Vasavi Swetha, 2014). Accordingly, NR enhanced the
cost-effectiveness of road pavements and increased service life
with low maintenance (Polacco et al., 2006). The mixing of NR in
bitumen increases the thermal sensitivity. It aids in dissipating low-
temperature developed stresses whereas, at higher temperatures, it
controls the flow of the asphalt mixture by functioning as a
membrane and enhancing the shear strength (Wen et al., 2017). NR
also has the potential to improve long-term pavement performance
owing to its essential elastomeric properties (Shaffie et al., 2015).
Table 3 summarizes the reviewed literature on the use of NR at
various concentrations.
4.1. Natural rubber production for bitumen modification
NR has been used in various forms to modify bitumen. However,
latex (liquid) and coagulated (solid) NR are the major forms used
for the modification (Mustafa Kamal et al., 2020; Poovaneshvaran
et al., 2020; Saowapark et al., 2019; Wen et al., 2017). The pro-
duction of NR is very simple and does not require any intricate
process to furnish products for modification (Al-Sabaeei et al.,
2020a; Azahar et al., 2019). NR production and its types are dis-
cussed in detail in Section 3. In postproduction, the NRL-modified
bitumen was observed to be a cost-effective system owing to its
ability to be added directly to bitumen. Conversely, the coagulated
form of NR must be sufficiently small (2 cm) to improve the
bitumenerubber interaction by increasing the rubber surface area
(Azahar et al., 2019). In contrast to NR, other modifiers such as
crumb rubber (CR), which is recycled from end-of-life tires (ELTs),
has emerged as a viable waste modifier for pavement applications
(T. Wang et al., 2018). The size of CR varies from 4.75 to 0.075 mm,
and the fine particles of CR have been demonstrated to achieve
maximum swelling at a faster rate than coarse particles, resulting in
different interaction levels in the binder matrix (Nanjegowda and
Biligiri, 2020; Venudharan and Biligiri, 2017). Additionally,
6
Journal of Cleaner Production 289 (2021) 125727
because of the large surface area of fine particles, the absorption of
light fractions of the bitumen matrix is much faster than that of
coarse particles, rendering stiffness to the liquid phase of the binder
(Ghavibazoo and Abdelrahman, 2013; Shen et al., 2009). Thus, an
increase in the CR particle size enhances anti-rutting performance
and fatigue resistance. In contrast, reducing CR can produce a more
homogenous bitumenerubber blend and improve the storage sta-
bility and low-temperature performance of binders (Ghavibazoo
et al., 2013; Qian et al., 2020). However, CR-modified bitumen
with finer sizes significantly increases the cost because of the
required additional grinding (Wang et al., 2020a). However, the
average size of rubber particles used for the modification is
0.56 mm, and 80% of rubber particles used are smaller than 0.8 mm;
nevertheless, only 25% are smaller than 0.4 mm in diameter (Bressi
et al., 2019; Picado-Santos et al., 2020). NR and CR exhibit different
behaviours when interacting with bitumen, and the latter requires
a higher temperature, shearing speed, and time for degradation of
the complex rubber structure. The detailed chemical interaction is
discussed in Section 3.1.
The production of 1 t of CR from ELTs consumed a large amount
of energy as well as 384 kW h of electric power, 2.99 L of diesel oil,
0.22 m3 of water, 0.04 kg of lubricant oil, and several supporting
materials (Bartolozzi et al., 2012). Further, the shredding of ELTs
was reported to consume 72e73% of electric power (Gautam et al.,
2018). According to (ASTM, 2009), the minimum amount of CR
should be 15 wt% of bitumen to achieve desirable properties.
However, the average NR content is between 6 and 10 wt% of
bitumen. This indicates that a higher rubber content lowers the
workability of the mixture, which ultimately requires higher mix-
ing and compaction temperatures. Furthermore, with increasing
concerns about global warming, the production of CR accounts for
10% of the global warming potential and toxicity in freshwater
(Bartolozzi et al., 2012; Nanjegowda and Biligiri, 2020). However,
NR was reported to absorb 24.9 kg of CO2 to produce 1 kg of NRL
(Satakhun et al., 2019).
Despite the higher energy concerns, CR contains sulphur-based
benzothiazole that functions as a persuader in asphalt rubber
fumes and generates carcinogenic compounds as well as a low
concentration of polycyclic aromatic hydrocarbons which have the
potential to cause respiratory problems for workers exposed to
fumes (Burr et al., 2001; T. Wang et al., 2018). However, NR as an
organic biopolymer does not generate any hazardous compound in
the production of rubberized bitumen. Despite all discussed pa-
rameters, the NR industry also experiences fluctuations in demand
A.H. Ansari, F.M. Jakarni, R. Muniandy et al. Journal of Cleaner Production 289 (2021) 125727

Table 3
Summary of the reviewed literature on the use of natural rubber at various concentrations.

Reference Type of natural rubber Bitumen Replacement Viscosity @ 135  C Softening point Penetration Complex modulus G*
grade (%) (Pa.s) (oC) (dmm) (kPa)

Poovaneshvaran et al. (2020) Latex 60/70 5,10 1.5,3.7 50,54 59,56 1.0,3
Tuntiworawit et al. (2005) Latex 60/70 1,3,5,7,9,11,13 0.5e5.2 47e60 65e82 1.4e4.0
Suaryana and Sofyan (2019) Latex 60/70 7.0 e 53.8 53 e
Bakar et al. (2018) Latex 80/100 5,10,15 e 47.5e48.8 76.3e75.4 1.31e1.93
Prastanto et al. (2019) Latex 60/70 3,5,7 0.54e0.96 e e e
Sutanto et al. (2018) Latex 60/70 4,6,8 e 54e61.1 62e44 e
Shafii et al. (2017) Latex 80/100 1,2,3,5,7,9,12 e 47e50 72e107 e
E.Shaffie, A. K. Arshad (2018) Latex 80/100 2,4,6,8,10,12 e 53.4e57.4 55.9e49.8 e
Wen et al. (2017) Latex 60/70 3,5,7 1.1e3.2 e e 2.37e4.57
Sani et al. (2019) Latex 60/70 3,6 1.2,1.8 51,55 57,44 1.2e1.4
Fernando and Nadarajah Latex 80/100 2,3,4 e 53e60 74e62 e
(1969)
Ibrahim et al. (2017) Latex 80/100 2,4,6,8 e 48.9e52.7 95.4e97.4 e
Saowapark et al. (2019) Latex 60/70 0.6,2,3.2,4.5 0.32e1.2 48e58 64e56 e
Khadivar and Kavussi (2013) Latex 60/70 3,4,5 e 60.1e64 52.5e51 2.51e5.2
Chowdhury et al. (2017) Latex VG 40 1,2,3,4,5 0.31e0.30 58.3e61.3 36e30 e
Nair et al. (1998) Latex 80/100 5,10,20,30 e 44e29 85e340 e
Mazlina Mustafa kamal (2016) Cup lump 60/70 5.0 e 60 30 6.0
Abdulrahman et al. (2019) Cup lump 60/70 2.5,5,7.5 1.57e2.5 54e63 38e33 e
Azahar et al. (2019) Cup lump 60/70 5,10,15 1.0e3.1 47e43 48.4e153.5 2.2e11
Mustafa Kamal et al. (2019) Cup lump 60/70 5 1.5 60 59 6.86
Daniel et al. (2019) Cup lump 60/70 2.5,5.0,7.5,10 0.8e2 42e49 62e43 2.7e7
Othman et al. (2018) Cup lump 60/70 5.0 e 63 63.3 e
Ismail et al. (2012) Epoxidized natural 80/100 5.0 e 55 63 3.2
rubber
Al-Mansob et al. (2014) Epoxidized natural 80/100 3,6,9,12 0.46e0.69 50.6e57 73e53 12.1e11
rubber
Vichitcholchai and Panmai Ribbed smoked sheet 60/70 2,4,6,8,10 0.64e6.8 50e56 55e78 e
(2012)

and supply, which can be due to a shift towards the synthetic
rubber industry and a parallel increase in palm oil plantations
(Azahar et al., 2016). The low price and high cost of rubber pro-
duction create a large demand for the alternative usage of NR
(Zborowski and Kaloush, 2007). Thus, NR as a sustainable and
renewable bio-modifier for the pavement industry can mitigate the
financial burdens of rubber smallholders and simultaneously
enhance the pavement structures cost-effectively. Further insight
into the expansion of NR applications is provided in Section 8.
5. Physical and rheological properties of natural-rubber-
modified bitumen
To modify bitumen and optimise its properties, NR is used in
both latex and coagulated forms. However, some chemical addi-
tives are also used as co-modifiers to mitigate some deficiencies in
using NR.
5.1. Natural rubber as latex for bitumen modification
To date, a variety of studies have reported enhancement in the
physical and rheological properties of NRebitumen. Various raw
latices were analysed with low and high ammonium addition in
1969. The results revealed that field latex with a high percentage of
ammonium is effective in reducing penetration and increasing the
softening point compare with low-ammonium latex (Fernando and
Nadarajah, 1969). The pronounced enhancement is because of the
high ammonium in the latex as low-ammonium field latex behaves
inefficiently in the laboratory as it requires sufficient time to swell
and mix with bitumen. For better performance in terms of visco-
elastic properties, it must be thoroughly blended with bitumen, as
undissolved NRL limits the enhancement of performance.
According to the conclusions by Saowapark et al. (2019), the
physical properties of bitumen are enhanced when NRL is incor-
porated into bitumen. The penetration was observed to decrease
when 0.6e4.5 wt% of NRL was added to 64e57 dmm bitumen
compared with the penetration of 67 dmm of neat bitumen.
Consequently, a similar linear trend was observed for the softening
point of the bitumen, which increased to 58  C. A similar study was
conducted by Shaffie et al., in which bitumen was modified by
adding 4 to 12 by wt.% of bitumen to NRL. The experimental results
revealed a decrease in penetration up to 49.8 dmm for a very high
percentage of NR when using an 80/100 grade bitumen. Similarly,
the softening was enhanced from 44 to 57.4  C on the too-high
content of NR. The stiffening of the bitumen might be due to the
macromolecules of the NR. The chains disperse within the bitumen,
sharing the penetration load while holding the bitumen molecules
together. Thus, increasing the content of NR macromolecules re-
sults in penetration resistance and greater load-bearing bitumen.
In other comprehensive studies, Wen et al. (2017) and
Saowapark et al. (2019) observed an enhancement in the viscosity
of bitumen. The results indicated that rotational viscosity at 135  C
was observed to linearly increase with the increase in NRL content.
Thus, the highest viscosity occurs at 3.2 Pa s for 9% NRL (Fig. 5a) and
at approximately 1.2 Pa s for 4.5% NRL (Fig. 5b). This suggests that
there is a clear association between the NR molecules and bitumen,
which provide better compatibility and higher viscosity. However,
the results indicated that a higher percentage of NRL in bitumen
requires high temperature for mixing and compaction during the
laying out process of pavements. For lower energy consumption
and enhanced properties, the optimum amount of NRL is recom-
mended for modification.
Further reviewing the latex modification of bitumen, the
blending speed and time of the modified bitumen are worth
considering. The decomposition of latex in bitumen only occurs
when the time and speed are sufficiently high to disperse the latex.
Shaffie et al. (2018) and Shafii et al. (2017) evaluated the effects of
variables such as speed, time, and temperature on the physical
properties of NRL-modified bitumen. All variables were considered
to be interdependent for the superior blending of latex and

7
A.H. Ansari, F.M. Jakarni, R. Muniandy et al.
Fig. 5. Effect of natural rubber content on the rotational viscosity at 135  C (Saowapark et al., 2019; Wen et al., 2017).
bitumen. A 20% increase in blending speed was observed to
promptly reduce the time required by approximately 30% for a
sufficiently homogenous bitumen. Other studies investigated the
high blending speed for NR-modified bitumen (Bindu et al., 2020;
Wen et al., 2017). The results indicated that the use of high speed
(>4000 rpm) and temperature (150e160  C) reduced the time to
disperse the NR with bitumen to 30e40 min. Note that while
increasing the blending speed, the time duration decreased to
achieve the same dispersion.
To further understand the effect of NRL on bitumen properties,
many researchers have studied the dynamic rheological properties
by using a dynamic shear rheometer (DSR) test. According to the
Superpave specification, the obtained rheological properties must
be within the viscoelastic range, simulating the road-traffic con-
dition of loading. The complex shear modulus (G*) and phase (d)
angle are the fundamental parameters obtained from the DSR. For a
better understanding, the process of NRL modification and its ef-
fects on the rheological properties and viscoelastic behaviour of
bitumen is worth analysing. Thus, Bakar et al. (2018) investigated
G* and d. They observed an increasing trend on the values of G* and
d for an NRL content in the range of 3e7 wt.%. The G* values were
more prominent within a temperature range of 46e58  C at a very
high concentration of NRL. In contrast, the d values approaching 90
as the temperature increases indicated a sufficient viscous behav-
iour, but after adding 7% NRL, the phase angle decreased towards
the elastic range. Wen et al. (2017) observed NRL performance in
terms of G* and d similar in a similar manner to (Bakar et al., 2018).
Incorporation of NRL into the bitumen by 3e9% reduced the tem-
perature susceptibility. The results indicated that G* values nar-
rowed between low and high temperatures, indicating that the NRL
appeared to be useful for enhancement. The value of d is generally
more sensitive to the structure and bitumen modification (Ren
et al., 2020), as its values increase at high temperatures and are
compensated when the dosage of NRL is added to the bitumen.
The theoretical rutting parameter under the Strategic Highway
Research Program (SHRP) specifications (G*/sin d) is the measure of
permanent deformation of bitumen under cyclic load, and it is
considered to reflect the fatigue resistance at intermediate tem-
peratures. The reflective values of resistance against load for the
rutting and fatigue parameters must be higher than 1.0 kPa and less
than or equal to 5000 kPa, respectively, at a frequency of 10 rad/s
for the maximum design temperature. However, for low-
temperature cracking, the creep stiffness (S) and creep rate (m-
8
Journal of Cleaner Production 289 (2021) 125727
value) can be calculated using a bending beam rheometer accord-
ing to the AASHTO M320 (S < 300 MPa and m-value>0.30)
specifications.
In a recent study by Daniel et al. (2019), the effect of adding
0e10% NRL to bitumen on G*/sin d versus temperature was ana-
lysed. Increasing the content of NRL resulted in an improvement in
permanent deformation compared with the base bitumen (Fig. 6a).
The Superpave performance grade improved up to PG82 at 10%
NRL. Similar trends were reported by Bakar et al. (2018) for G*/sin d
versus temperature (Fig. 6b). Bitumen stiffness is an essential
parameter to ascertain fatigue cracking at intermediate tempera-
tures (Thodesen et al., 2009). Fatigue is an intricate process that can
occur in pavements owing to repeated bending loads, which cause
microdamage in the pavements (Wang et al., 2012). This damage
ultimately results in a decrease in stiffness, thus decreasing the
applied load capacity and capability to resist additional damage.
Owing to its elastic behaviour, NRL can modify bitumen and
dissipate the energy by rebounding and not cracking the pave-
ments. Wen et al. (2017) reported on the fatigue parameter and
demonstrated that as the NRL content increases, the fatigue results
at intermediate temperatures decrease compared with the neat
bitumen. The decreases in the G* sin d for modified bitumen with
3%, 5%, and 7% NRL at 25  C were 20.1%, 34.11%, and 42.3%,
respectively. Thus, the incorporation of NRL can increase the fatigue
resistance. Similarly, in studies by (Al-Sabaeei et al., 2020a; Sani
et al., 2020), the incorporation of NRL enhanced the fatigue resis-
tance of bitumen.
Wen et al. (2017) conducted further investigations of NRL-
modified bitumen and concluded that NRL increases its elastically
at low-temperature conditions. The S-values of a modified binder
with NRL increased at
6  C and
12  C by 31% and 41.9%,
respectively. However, there was no significant change in m-values
at
6  C and failure occurred at
12  C. Therefore, the NRL
enhanced bitumen flexibility at lower temperatures by reducing
the stiffness. In addition, some researchers have indicated that the
m-value of the rubber modified binder is slightly degraded while a
reduction in the bitumen stiffness occurs (Abdelrahman, 2006;
Billiter et al., 1997; Ghavibazoo and Abdelrahman, 2014). In sum-
mary, rubber-modified bitumen exhibits improved thermal
cracking resistance compared with the original binder.
Overall, these studies consistently indicated that as it changes
the rheological properties and flow of bitumen, latex acts as a
membrane that boosts the shear strength and resists flow. Hence,
A.H. Ansari, F.M. Jakarni, R. Muniandy et al.
Fig. 6. Effect of temperature and NRL on the rutting parameter (Bakar et al., 2018; Daniel et al., 2019).
the incorporation of NRL increases the complex modulus of
bitumen. Thus, this results in the enhancement of the rutting
parameter and the intermediate and low-temperature properties of
bitumen according to the SHRP specifications. All the metrics dis-
cussed above support the hypothesis that NR has elastomeric
properties, which enhance bitumen performance. Despite several
advantages, NRL also has some limitations. NRL contains 55e60%
water (Table 1), which directly affects the properties of bitumen
and its mixture by creating foaming and frothing during the
blending process and is a significant concern for its long-term
implementation.
5.2. Coagulated natural rubber for bitumen modification
Raw rubber in the form of a cup lump has been identified to
modify bitumen as a biopolymer. The chemical properties of CLNR
are similar to those of NRL. In addition, CLNR is appropriate for
mixing with bitumen because of its low water content. Insufficient
literature is available on CLNR-modified bitumen as it is in the
initial phase of evaluation and implementation. A recent study by
Azahar et al. (2019) investigated the compatibility of CLNR to
analyse its effects on engineering parameters of modified bitumen.
The CLNR was pre-treated using toluene solvent to soften it for
blending with a bitumen. The penetration resistance decreased by
20% when a 5 wt% CLNR dosage was added to the bitumen. Incor-
poration of CLNR hardened the bitumen, thus also enhancing the
softening properties by 8%. The elasticity and stiffness of the
bitumen were due to the globular particles and porous surface of
the CLNR, which can absorb bitumen enormously (Intapun et al.,
2010) (Fig. 7). A linear trend was observed for the viscosity anal-
ysis at 135  C as the percentage content of CLNR increased the
viscosity was enhanced. The results for 5%, 10%, and 15% for treated
CLNR were 1.1, 1.6, and 3.1 Pa s, respectively.
A similar study conducted by Abdulrahman et al. (2019) inves-
tigated the physical properties of warm mix asphalt by adding CLNR
as a modifier. The trends of the results were similar to those by
(Azahar et al., 2019; Mustafa Kamal et al., 2020). The increase in
bitumen viscosity might be due to the rubber-to-bitumen reactivity
and the formation of the cross-linking skeleton. This can be
attributed to the bitumen chain movement, which is limited by the
layers of treated rubber at a higher temperature. Another form of
CLNR is epoxidized natural rubber (ENR), and its potential use for
the enhancement of bitumen was recognized in the 1980s. Chem-
ically modified NRL with a proxy formic acid with the process of
epoxidation is called ENR (Fig. 8).
9
Journal of Cleaner Production 289 (2021) 125727
ENR offers improved heat and chemical resistance owing to its
ability to resist crystallisation in conjunction with a higher glass-
transition temperature. These properties result in improved
damping and adhesion. Moreover, the physical properties of
bitumen by using ENR were analysed by Al-Mansob et al. (2014)
who observed that bitumen seemingly improve stiffness by
reducing penetration (64%) and increasing softening (11%). How-
ever, when ENR was added, the ductility initially declined and
subsequently began to increase, indicating a performance
improvement. The storage stability test revealed that up to 6% ENR
is stable for bitumen used at high temperatures. ENR has also been
used to enhance the rutting parameter under the SHRP specifica-
tion. However, the optimum addition of ENR to improve the rutting
resistance is 6 wt% bitumen (Al-Mansob et al, 2014, 2017a).
Al-Mansob et al. (2016) further investigated the fatigue behav-
iour of ENR-modified bitumen (6 wt%) at intermediate tempera-
tures and analysed aged conditions. The decreasing magnitude of
G* sin d after the ageing of bitumen at temperatures greater than
20  C was smaller than that of unaged bitumen. In contrast, long-
term aged modified bitumen exhibited a decrease of 47.6% in the
G* sin d compared with the unaged modified bitumen. The age-
hardening and intermediate temperature resistance of the ENR
bitumen could be due to the improved properties of ENR and good
compatibility between bitumen and rubber. Similar to the findings
by Al-Mansob et al. (2016), Azahar et al. (2019) also investigated the
CLNR at 5, 10, and 15 wt% of bitumen for fatigue behaviour at in-
termediate temperatures. The results indicated a declining trend
with increasing CLNR content. However, the CLNR-modified
bitumen failed at 24 and 19  C with 4510 and 4794 kPa, respec-
tively, which was lower than that of neat bitumen at 26  C
(4022 kPa). The findings at intermediate temperatures for modified
bitumen revealed that CLNR can increase the fatigue resistance for
an extended service life of pavements. Moreover, CLNR modifica-
tion enhances the bitumen energy dissipation by rebounding and
reduces the cracking process owing to NR elasticity.
NR sheets with different forms can also be used with bitumen,
and examples are ribbed smoked sheets (RSSs), creep rubber, and
block rubber. Despite various forms and shapes, these NR sheets
have methods of mixing with bitumen, and their chemical nature is
similar to that of NRL. Research conducted by Vichitcholchai and
Panmai (2012) revealed that using RSS significantly affected the
properties of bitumen. However, the RSS ratio must be maintained
to reduce the cause of heterogeneity. They also concluded that 6%
by weight of NR in bitumen enhanced the physical properties and
developed high torsional recovery-toughness and tenacity.
A.H. Ansari, F.M. Jakarni, R. Muniandy et al.
Fig. 7. Field emission scanning electron microscope morphology of cup lump rubber (Azahar et al., 2019).
Fig. 8. Epoxidation of natural rubber (Al-Mansob et al., 2014).
Additionally, the rubber sheet is reliable during blending with
bitumen as it reduces foaming and frothing.
5.3. Chemical additives as co-modifier for natural rubber modified
bitumen
Several researchers have investigated the incorporation of NR in
bitumen and observed a decisive enhancement in rheological and
performance testing (Azahar et al., 2019; Poovaneshvaran et al.,
2020; Shaffie et al., 2017). However, the addition of NR to
bitumen for modification decreases the workability of the asphalt
mixture. Hence, this could occur owing to the improvement in
aggregates-mastic adhesion and increase in the viscosity of the
bitumen. Thus, high mixing and compaction temperatures are
required during construction to gain the desired workability. High
energy consumption and greenhouse emission are concerns that
are parallel to promising results from the modification of bitumen
(Behnood, 2019). The generation of many fumes and pollution of
the environment while heating the asphalt mixture at high tem-
peratures also increases the end cost of production. Therefore,
several researchers have investigated various warm mix asphalt
(WMA) additives to increase the workability, resulting in approxi-
mately 25% fuel savings (Kheradmand et al., 2014; T. Wang et al.,
2018). Thus, the addition of 5.0% of CLNR and 0.5% Evotherm was
reported to reduce the viscosity of bitumen by approximately 14%,
in turn reducing the compaction and mixing temperature for the
modified bitumen (Fig. 9). Because of the oily nature of Evotherm, it
increases the penetration and softening point temperature by
reducing the molecular weight of bitumen because of the deag-
glomeration of macromolecules (Abdulrahman et al., 2019).
Sani et al. (2019) reported that the addition of 0.1% Zycotherm as
a co-modifier with NRL reduced the rotational viscosity values.
However, a dominant improvement was observed in the high-
10
Journal of Cleaner Production 289 (2021) 125727
temperature values of the complex modulus stiffness. Addition-
ally, the rutting parameter of the modified bitumen with 0.1%
Zycotherm and 3% NRL was observed to increase the failure tem-
perature from 64 to 76  C. The reason for the improvement in the
rheological properties could be the continuous agglomerated
globule network of microstructures formed in the modified matrix.
Similarly, the organic additive cashew nutshell liquid (CNSL) was
incorporated into an NR-modified bitumen as WMA and 2 wt% was
observed to be the optimum. The CNSL reduced the viscosity by
34.74% at 140  C (Fig. 10), and CNSL aided in reducing the mixing
temperature by 20  C (Bindu et al., 2020). The reduction in viscosity
is due to the chemical interaction between CNSL and bitumen, in
which solubilisation of asphaltenes occurs owing to the CNSL
components. Through the organic nonpolar radical, it promotes an
equilibrium interaction, which decreases the viscosity of bitumen
(Oliveira et al., 2011).
In the context of high energy requirement and emission of
greenhouse gases during the mixing and compaction of the asphalt
mixture, another method to improve the workability of the mixture
by reducing the viscosity is the production of the foamed based or
rubberized foamed WMA (H. Wang et al., 2018). Foaming tech-
niques have been widely adopted by the pavement industry and
have exhibited significant potential for sustainable development
(Fu et al., 2011; Martinez-Arguelles et al., 2014; Shu et al., 2012). In
the pavement industry, foaming technology can be classified into
two different techniques: water-based methods (foamed bitumen
is produced by the injection of a small amount of water 1e6% by wt.
of bitumen into pre-heated bitumen) and water-bearing additives
(solid additives that retain moisture and create bubbles when it
comes into contact with pre-heated bitumen) (Mohd Hasan et al.,
2017).
The process of foaming significantly increases the volume of
bitumen (5e15 times from the original) (Mohd Hasan et al., 2017).
A.H. Ansari, F.M. Jakarni, R. Muniandy et al.
Fig. 9. Effect of Evotherm on the rotational viscosity (Abdulrahman et al., 2019).
Fig. 10. Viscosity variation with different % of cashew nutshell liquid (Bindu et al.,
2020).
However, the quality of foam bitumen is affected by air pressure
and water content. An excessive amount of water content and air
pressure increases the expansion ratio of foamed bitumen, which
ultimately lowers the surface area of the air bubble and causes a
deficient coating of aggregates (Ozturk and Kutay, 2014). Wang and
Li (2008) studied the models of bubble growth using the quasi-
static diffusion-driven process and indicated that bubble growth
in the polymer foaming process was affected by the properties of
the material (viscosity, surface tension, gas diffusivity, and relaxa-
tion time) and also by foaming process parameters, for instance,
temperature, gas concentration, and pressure. NRL contains
approximately 50e60% water in total colloids (Table 1). Sani et al.
(2019) and Wen et al. (2017) reported that the addition of NRL
into pre-heated bitumen generates excessive bubbles. Wen et al.
(2017) further investigated NRL-modified bitumen (7%) and
observed that modified bitumen demonstrated a uniform fluores-
cence response. However, the high-magnification modified
bitumen exhibits an interesting network composed of an excessive
number of bubbles. This is due to the presence of moisture in the
latex. The results also corresponded to the presence of 4.2% solid
rubber and 3.8% water, and a reduction in the viscosity was also
reported. Yu et al. (2013) recommended 1% of water as a foaming
agent for neat bitumen and 3% for styrene-butadiene-styrene
polymer-modified bitumen. As discussed earlier, NRL can produce
foaming rubber-modified binders such as WMA. Thus, the water
content present in 7% NRL for creating foaming rubber-modified
11
Journal of Cleaner Production 289 (2021) 125727
bitumen is similar to that recommended in a previous study (Yu
et al., 2013). Fu et al. (2011) reported that the foamed bitumen
properties can be enhanced by incorporating anti-strip agents to
enhance the adhesion ability of bitumen. However, bitumen
modified with NRL foamed rubber seemingly performs better as
NRL has more elastic and adhesion properties to adhere to aggre-
gates and bitumen and strengthens its performance.
In addition to the WMA, to reduce the viscosity and stiffness of
rubber-modified bitumen, polyphosphoric acid (PPA) and sulphur
can be used combination with lower-content NRL. Thus, 3.2% NRL,
2% PPA, and 0.3% sulphur was considered a suitable combination for
the improved performance of the modified bitumen (Saowapark
et al., 2019). The chemical interaction between PPA and bitumen
is the reason for enhanced bitumen properties through the pro-
duction of a phosphate ester group owing to the presence of the
hydroxyl group in bitumen (Shvedov et al., 1965).
6. Performance properties of natural rubber asphalt mixture-
latex and coagulated
Researchers have also conducted studies on the performance
properties of modified NR asphalt mixtures and demonstrated the
enhancement of deformation and fatigue resistance of pavement. A
study conducted by Shaffie et al. (2017) summarized the perfor-
mance properties of asphalt using CLNR as a modifier. Adding 8%
CLNR increases the rutting depth by 41% in contrast to the un-
modified asphalt mix (Fig. 11a). In another study, Siswanto (2017)
reported the results for deformation decrement in a similar
manner as (Shaffie et al., 2017). The deformation decreased by
36.28% upon addition of 6 wt% latex compared with the original
state of the asphalt mix (Fig. 11b). A study conducted by Al-Mansob
et al. (2017b) used ENR as an asphalt mixture modifier and reported
a significant enhancement in permanent deformation and followed
the same trends as (Shaffie et al., 2017; Siswanto, 2017).
A recent studyinvestigated the performance properties of a cup
lump modified mixture at a dosage of 5% (Mohd Azahar et al.,
2019a). The results revealed an enhancement in the dynamic
creep and resilient modulus properties by 126% and 27%, respec-
tively. However, similar trends were observed for the permanent
deformation, as concluded by (Shaffie et al., 2017; Siswanto, 2017).
Compared with a conventional mixture, the improvement is
possibly due to the elastic response of the NR incorporating. NR in
pavements primarily functions as an elastic band that aids to
A.H. Ansari, F.M. Jakarni, R. Muniandy et al.
Fig. 11. Deformation at various % of natural rubber (Shaffie et al., 2017; Siswanto, 2017).
disintegrate stresses. Consequently, polyisoprene elastomeric
behaviour simultaneously holds the pavement together where
cracks are likely to develop (Colin Ruggles, 2005; Shafii et al., 2017).
NR built-in elastomers have proven that NR has the potential to
enhance pavement long-term performance in asphalt mixtures
with improvement in the cohesion and adhesion properties of
bitumen (Shaffie et al., 2015). Table 4 summarizes the few reviewed
laboratory studies of asphalt mixtures using NR for modification.
7. Field performance of natural rubber modified asphalt
mixture
NR modification has demonstrated beneficial improvement in
bitumen and mixture performance at a laboratory scale. The vali-
dation of modification at full-scale field performance is recom-
mended for new innovative materials and procedures. Very few
studies have been conducted on the on-field performance of NR-
modified pavements and have exhibited some enhancement
owing to the elastomeric properties of NR. A study was conducted
by Othman et al. (2018) on modified asphalt mixtures incorporating
CLNR in the Jalan Kuala LumpureKuantan Road, Daerah Temerloh,
Pahang, Malaysia. They concluded that 5% of CLNR-modified
bitumen utilized in asphalt pavement has better field perfor-
mance after six months of construction. The results indicated
rutting of less than 5 mm, which is a good indicator of rutting
conditions. In addition, the 94% roughness indicated an improve-
ment in skid resistance and structural condition compared with all
AC14 pavements. The improvement in the field performance could
be owing to the improved adhesion between aggregates. Some
studies also investigated the chemical interaction of bitumen with
the isoprene unit of NR, which also contributes to performance
improvement (Mohd Azahar et al., 2019b). Another study by Razali
et al. (2019) concluded that CLNR-modified pavement was con-
structed without any significant modification in the construction
process. The outcomes indicated no significant improvement in
comparison with a control section and suggested that a more
extended period was required to validate the results accurately.
Similarly, NRL-modified bitumen was utilized as a seal coat
(Fernando and Nadarajah, 1969). Latex was observed to improve
temperature-dependent properties, and a 2% rubberized bitumen
seal coat extended the service life of the pavement. The neat
bitumen without rubber, which was laid in the same section,
developed cracks. However, the rubberized seal coat did not exhibit
signs of failure; hence, a minimum of 2% of latex was
12
Journal of Cleaner Production 289 (2021) 125727
recommended. Table 5 summarizes the pavement conditions in-
dicators of the few NR-modified pavement sections.
8. Challenges in expanding natural rubber applications
NR, among any other biomaterials, is highly significant for
various applications owing to its pure elastomeric properties. In
increasing the demand for NR for multiple products, all the bot-
tlenecks in the efficient process must be eradicated. However, the
major global contributors, i.e., Malaysia, Thailand, and Indonesia,
have always been apprehensive because of some factors for
expanding the NR industry. Thus, the shift towards the synthetic
rubber industry and price variation are the major barriers to
expanding the NR industry. Primarily, a factor that affects the pri-
ority of buyers is the price, which always is considered to estimate
gain profit and loss analysis when producing high-end products.
Owing to the unpredictable NR demand for excellent production,
there is instability in the rates of NR. The primary source of NR has a
significant supply, as the NR industrial production was 13 MMT in
2017 compared with synthetic rubber (15 MMT) (Board, 2018). In
the total production, approximately 40% of rubber is in a natural
state, while the industry consumes the remainder for
manufacturing synthetic rubber products (ResearchInChina, 2017).
The commercialization of NR into synthetic rubber because of a lack
of proper and satisfying demand for NR, which creates a gap that
has been filled by synthetic rubber. Consequently, the products of
synthetic rubber have high quality and valuable usage globally, e.g.,
aircraft and heavy-truck tires. In contrast, the major NR-producing
countries are experiencing challenges in the global demand and
supply because of the parallel emerging growth of palm oil plan-
tations. Since decades ago, it has emerged as the cheapest edible oil,
whereas Southeast Asian countries have earned economic growth
and interest in global trade owing to palm oil plantations. Consid-
ering the facts discussed and the economic value of NR, an initiative
must be undertaken to mitigate the challenges of expansion of the
NR industry before this valuable raw material completely loses its
commercial value.
9. Conclusions and recommendations
The aim of this review is to promote NR applications by
reviewing the available literature. It reveals the possibility of NR
usage in the construction of sustainable pavements by reducing
preconceptions and hesitation. In addition, it highlights the usage,
A.H. Ansari, F.M. Jakarni, R. Muniandy et al. Journal of Cleaner Production 289 (2021) 125727

Table 4
Summary of laboratory studies of asphalt mixtures using natural rubber for modification.

Reference Objective Experimental Plan Conclusion

Shaffie et al. Investigate and characterize the Superpave mix design was performed to prepare a Rubber addition enhanced the rutting resistance of the
(2017) improvement in asphalt mixtures using mixture with SP 19-mm gradation; the bitumen was 80/ mixture compared with the unmodified mixture.
CLNR. 100, and 8% CLNR by weight of bitumen was added
following the wet blending procedure.
Siswanto Study the effect of latex on the Four asphalt dense-graded mixtures at 0%, 2%, 4%, and 6% The addition of latex enhanced the permanent
(2017) permanent deformation of asphalt were prepared to add latex (60% dry rubber content) by deformation of the asphalt concrete wearing course, and
concrete wearing course. weight of 60/70 grade bitumen and were tested for the addition of 6% indicated promising improvement.
deformation in wheel tracking machine.
Al-Mansob Investigate the performance ENR-modified bitumen was prepared by mixing 3, 6, 9 The ENR-modified mixture exhibited a high resilient
et al. characterization of hot mix asphalt and 12 ENR by weight of bitumen at 4000-rpm shearing modulus at intermediate and high temperatures, and
(2017b) incorporating ENR. speed for 60e66 min, and the temperature was 160  C. improved the rutting compared with unmodified
The asphalt mix design was based on Superpave, and SP mixtures; it was also less susceptible to fatigue cracking
19-mm gradation was followed and tested for rutting, and moisture damage.
dynamic creep, resilient modulus, and fatigue test.
Chowdhury Laboratory investigation of NR latex and The VG40 bitumen was modified using NRL and warm Incorporation of latex in the mixture resulted in better
et al. Zyco Therm (warm mix additive) on mix additive at 1e5% and 0.15% by weight of bitumen, moisture performance; the tensile strength ratio of NR
(2017) moisture performance of asphalt respectively, and Marshall mix design with dense was slightly lower than that of NRewarm additive
mixtures. gradation was followed and tested for moisture, i.e., mixture; however, both were greater than the minimum
indirect tensile test, retained stability, and boiling test. requirement of 80%.
Prastanto Evaluate the performance of rubberized The dosage of NR was set at 3%, 5%, 7%, and 9%, and The study concluded that the addition of 5%e7% NR
et al. hot mix asphalt at a laboratory scale. cationic NR, pre-vulcanized NR, and semi-solid rubber improved the physical properties of asphalt mixture
(2019) were used for modification. The penetration 60/70 grade instability and flow.
bitumen was used, and the wet blending process was
followed. The Marshall mix design was used for dense
mixture preparation and tested for stability and flow.
Shaffie et al. To investigate the stripping The penetration grade 80/100 was used for modification The NR-modified asphalt mixture exhibited better
(2015) performance and volumetric properties and 8% of NRL by weight of the bitumen. The Superpave resistance for stripping as the tensile strength ratio was
of NRL-modified hot mix asphalt. mix design procedure was followed to obtain an higher than that of an unmodified mix.
optimum asphalt content, and the mixture was
evaluated in indirect tensile and boiling tests to evaluate
stripping performance.

Table 5
Summary of the pavement conditions indicators of natural rubber modified pavements sections.

Reference Year Location and pavement section details NR concentration Pavement condition parameters
Investigated
Condition Rutting Surface Crack Texture
Parameter Roughness Distribution Depth
Index

Othman 2017 The study was conducted at Jalan Kuala Lumpur 5.0% NR was used through the wet Good 100% 94% 100% 100%
et al. eKuantan (FT02), Daerah Temerloh, Pahang, blending process. Fair 0% 6.0% 0% 0%
(2018) Malaysia. The total length was 1.5 km for Cup lump Poor 0% 0% 0% 0%
modified asphalt and 500 m for the control section. Bad 0% 0% 0% 0%
The construction method used was a mill and paved
50-mm wearing course. The pavement was evaluated
after one month of constriction
Mazlina 2014 A 2.0-km road was constructed at Kota Tinggi, Johar, A mixture of 95:5 bitumen-to- Good 100 70% 100% 10%
Mustafa Malaysia, using CLNR. The IKRAM road scanner as rubber ratio was used, and rubber Fair 0% 20% 0% 90%
kamal used to measure pavement condition after 8 months and bitumen were preblended Poor 0% 10% 0% 0%
(2016) of construction. Bad 0% 0% 0% 0%
Razali et al. 2016 CLNR as an additive on maintenance project at Route Homogenous CLNR-modified Good 100 100 100 100
(2019) 4, Jalan KupangeGerik, Baling, Kedah, Malaysia, the bitumen was produced and Fair 0% 0% 0% 0%
length of the section was divided into two parts: aggregates were added to produce Poor 0% 0% 0% 0%
500 m for the CLNR-modified pavement and 220 m cup lump asphalt. Bad 0% 0% 0% 0%
for the control section. The pavement condition was
measured after six months of construction.

advancement, and challenges encountered when modifying using
NR, which affects the bitumen properties. Previous studies on NR-
modified bitumen have indicated that it is one of the biopolymers
used as a modifier for pavement performance to mitigate failures.
The following conclusions can be drawn based on the review.
 Modifying bitumen with NR and putting it into practice can
promote sustainable pavement construction by preventing the
swift depletion of non-renewable resources.
 Fresh NR is an uncross-linked polymer consisting of long chains
forming folded coils and entangled with each other without any
links and can be easily dispersed, swollen, and ultimately
absorbed by bitumen.
 The chemical interaction and restructuring the molecules of
bitumen and NR further strengthens the viscoelastic behaviour
of bitumen. Thus, it can resist more strain energy before any
failure and is ultimately significant in long-term pavement life.
 The strength and rubberized bitumen depend solely on the type
of NR used. The presence of more than 50% of water in the latex
produces foaming and frothing during blending, which ulti-
mately reduces long-term performance. However, low-water-
content rubber (CLNR) has a solid shape, although it is unsta-
ble during storage at high rubber content and temperatures.
 NR as an organic biopolymer does not generate any hazardous
compound in the production of rubberized bitumen. However,

13
A.H. Ansari, F.M. Jakarni, R. Muniandy et al.
NR was estimated to absorbs 24.9 kg of CO2 to produce 1 kg of
NRL.
 The effect of blending variables is interdependent on the phys-
ical and chemical properties of the modified bitumen. For
example, CLNR requires a high shearing speed for a homoge-
neous bitumen.
 In general, the optimum content of NR is 4e6% for improved
rheology and pavement performance.
 NR content has a significant function in the high and low-
temperature properties of rubberized bitumen.
 High NR content results in the low workability of asphalt mix-
tures, which ultimately requires high mixing and compaction
temperatures. Therefore, warm mix additives are utilized, and
they enhance the workability of the mixture and simultaneously
reduce high energy consumption.
 The utilisation of 5% CLNR in asphalt pavement exhibits better
field performance after six months of construction and less than
5-mm rutting occurs, which is a good indicator of rutting
conditions.
In summary, the consumption of NR for the construction of
highway pavements can result in many benefits. First, it reduces the
dependence on petroleum-based modifiers as it is a low-cost and
environmentally friendly biopolymer. Consequently, extensive use
of NR owing to its low cost can simultaneously enhance the eco-
nomic growth of the industry and the service life of roads with low
maintenance costs, which would significantly improve the ride
quality. However, there is still a very low utilisation of NR, and the
reason could be the limited studies and a wide disparity in results
and recommendations. Thus, this review can aid to overcome these
limitations and recommend a few considerations for future
research to increase the utilisation of NR as a new biopolymer
modifier for bitumen.
 The physical and chemical interaction mechanism between NR
and bitumen should be investigated further.
 More studies should be conducted to develop a method for NR
in latex form to blend with bitumen. It produces foaming and
frothing during the blending procedure, which is a significant
concern for long-term implementation.
 CLNR, which requires a very minimal manufacturing process,
has been utilized recently and has gained interest as a bitumen
modifier. However, no prominent method of blending and pre-
treatment of CLNR with bitumen exists to achieve homogenous
blended bitumen with good storage stability at high
temperatures.
 The addition of NR of more than 5% by wt. of bitumen signifi-
cantly increases the viscosity. Thus, an increase in the viscosity
of the binder requires a higher mixing and compaction tem-
perature during the pavement laying process. Hence, the co-
modifier must be used to optimise the binder performance for
sustainable pavements.
 Further evaluation of the performance of asphalt mixtures with
different gradations and types of NR is required to fully under-
stand the behaviour of modified mixtures.
 Further, a prompt in situ evaluation of the field performance of
existing pavement is recommended, and it is a quintessential
research topic.
 NRL contains approximately 50e60% water in the total colloids,
and NRL can produce a foaming-rubber-modified binder such as
WMA. Evaluation of the optimum NRL content and other pa-
rameters for injection to produce the foaming WMA is
recommended.
 Insufficient research has been conducted for the ageing and
low-temperature performance of the NR-modified bitumen.
14
Journal of Cleaner Production 289 (2021) 125727
Thus, the performance of the modified bitumen should be
evaluated using an in-depth analysis of the ageing and low-
temperature properties.
 The NR-modified binder must be evaluated for the adhesion and
cohesion properties to optimise the NR content for better
performance.
 Finally, the actual cost-effectiveness of NR-modified pavements
on an industrial scale is recommended to commercialize the
product.
Declaration of competing interest
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgement
/Authors would like to thank the Ministry of Higher Education
Malaysia and Universiti Putra Malaysia for the award of Funda-
mental Research Grant Scheme (FRGS) FRGS/1/2017/TK06UPM/02/
1 (Project Code: 03-01-17-1894FR) as well as all the people whom
are directly and indirectly involved in this study.
References
Abdelrahman, M., 2006. Controlling performance of crumb rubberemodified
binders through addition of polymer modifiers. Transp. Res. Rec. J. Transp.
Res. Board 64e70. https://doi.org/10.1177/0361198106196200108, 1962.
Abdelrahman, M.A., Carpenter, S.H., 1999. Mechanism of interaction of asphalt
cement with crumb rubber modifier. Transp. Res. Rec. J. Transp. Res. Board 1661,
106e113. https://doi.org/10.3141/1661-15.
Abdulrahman, S., Hainin, M.R., Idham, M.K., Hassan, N.A., Warid, M.N.M., Yaacob, H.,
Azman, M., Puan, O.C., 2019. Physical properties of warm cup lump modified
bitumen. IOP Conf. Ser. Mater. Sci. Eng. 527, 012048 https://doi.org/10.1088/
1757-899X/527/1/012048.
Al-Mansob, R.A., Ismail, A., Alduri, A.N., Azhari, C.H., Karim, M.R., Yusoff, N.I.M.,
2014. Physical and rheological properties of epoxidized natural rubber modified
bitumens. Construct. Build. Mater. 63, 242e248. https://doi.org/10.1016/
j.conbuildmat.2014.04.026.
Al-Mansob, R.A., Ismail, A., Yusoff, N.I.M., Albrka, S.I., Azhari, C.H., Karim, M.R., 2016.
Rheological characteristics of unaged and aged epoxidised natural rubber
modified asphalt. Construct. Build. Mater. 102, 190e199. https://doi.org/10.1016/
j.conbuildmat.2015.10.133.
Al-Mansob, R.A., Ismail, A., Rahmat, R.A.O.K., Borhan, M.N., Alsharef, J.M.A.,
Albrka, S.I., Karim, M.R., 2017a. The performance of Epoxidised Natural Rubber
modified asphalt using nano-alumina as additive. Construct. Build. Mater. 155,
680e687. https://doi.org/10.1016/j.conbuildmat.2017.08.106.
Al-Mansob, R.A., Ismail, A., Yusoff, N.I.M., Rahmat, R.A.O.K., Borhan, M.N., Albrka, S.I.,
Azhari, C.H., Karim, M.R., 2017b. Engineering characterisation of epoxidized
natural rubber-modified hot-mix asphalt. PloS One 12, e0171648. https://
doi.org/10.1371/journal.pone.0171648.
Al-Sabaeei, A.M., Mustofa, B.A., Sutanto, M.H., Sunarjono, S., Bala, N., 2020a. Aging
and rheological properties of latex and crumb rubber modified bitumen using
dynamic shear rheometer. J. Eng. Technol. Sci. 52, 385. https://doi.org/10.5614/
j.eng.technol.sci.2020.52.3.6.
Al-Sabaeei, A.M., Napiah, M.B., Sutanto, M.H., Alaloul, W.S., Usman, A., 2020b.
A systematic review of bio-asphalt for flexible pavement applications: coherent
taxonomy, motivations, challenges and future directions. J. Clean. Prod. 249,
119357. https://doi.org/10.1016/j.jclepro.2019.119357.
ASTM, 2009. ASTM D6114/D6114M - 09 Standard Specification for Asphalt-Rubber
Binder. ASTM Int. West Conshohocken, , PA, USA. https://doi.org/10.1520/
D6114_D6114M-09.
Azahar, N.B.M., Hassan, N.B.A., Jaya, R.P., Kadir, M.A.B.A., Yunus, N.Z.B.M.,
Mahmud, M.Z.H., 2016. An overview on natural rubber application for asphalt
modification. Int. J. Agric. For. Plant. 2, 212e218.
Azahar, N.M., Hassan, N.A., Jaya, R.P., Hainin, M.R., Yusoff, N.I.M.,
Kamaruddin, N.H.M., Yunus, N.Z.M., Hassan, S.A., Yaacob, H., 2019. Properties of
cup lump rubber modified asphalt binder. Road Mater. Pavement Des. 220,
1e21. https://doi.org/10.1080/14680629.2019.1687007.
Aziz, M.M.A., Rahman, M.T., Hainin, M.R., Bakar, W.A.W.A., 2015. An overview on
alternative binders for flexible pavement. Construct. Build. Mater. 84, 315e319.
https://doi.org/10.1016/j.conbuildmat.2015.03.068.
Bakar, S.K.A., Ezree Abdullah, M., Mustafa Kamal, M., Abd Rahman, R., Putra Jaya, R.,
Buhari, R., Arifin Hadithon, K., 2018. Influence of ageing process on rheological
characteristic of waste natural rubber latex modified bitumen. J. Phys. Conf. Ser.
1049 https://doi.org/10.1088/1742-6596/1049/1/012100, 012100.
A.H. Ansari, F.M. Jakarni, R. Muniandy et al.
Baker, C.S.L., Fulton, W.S., 2012. Updated by staff, 2012. Rubber, natural. In: Kirk-
Othmer Encyclopedia of Chemical Technology. John Wiley & Sons, Inc., Hobo-
ken, NJ, USA https://doi.org/10.1002/0471238961.1821020202011105.a01.pub2.
Bartolozzi, I., Antunes, I., Rizzi, F., 2012. The environmental impact assessment of
asphalt Rubber : life cycle assessment. In: Asphalt Rubber Conference 2012
Munich.
Behnood, A., 2019. Application of rejuvenators to improve the rheological and
mechanical properties of asphalt binders and mixtures: a review. J. Clean. Prod.
231, 171e182. https://doi.org/10.1016/j.jclepro.2019.05.209.
Bhowmick, A.K., stephens, H.L., 2000. Handbook of Elastomers, second ed. CRC
Press, New York. https://doi.org/10.1201/9781482270365.
Billiter, T.C., Davison, R.R., Glover, C.J., Bullin, J.A., 1997. Physical properties of
asphalt-rubber binder. Petrol. Sci. Technol. 15, 205e236. https://doi.org/
10.1080/10916469708949653.
Bindu, C.S., Joseph, M.S., Sibinesh, P.S., George, S., Sivan, S., 2020. Performance
evaluation of warm mix asphalt using natural rubber modified bitumen and
cashew nut shell liquid. Int. J. Pavement Res. Technol. 13, 442e453. https://
doi.org/10.1007/s42947-020-0241-7.
Board, M.R., 2018. Natural Rubber Statistics.
Bressi, S., Fiorentini, N., Huang, J., Losa, M., 2019. Crumb rubber modifier in road
asphalt pavements: state of the art and statistics. Coatings 9. https://doi.org/
10.3390/COATINGS9060384.
Burr, G., Tepper, A., Feng, A., Olsen, L., Miller, A., 2001. Crumb-Rubber Modified
Asphalt Paving: Occupational Exposures and Acute Health Effects. NIOSH
Publications Office, 2001-0536-2864.
Chowdhury, P.S., Kumar, S., Sarkar, D., Of, I., Data, P., 2017. Effect of natural rubber
and zycotherm on moisture performance of asphalt mixtures. In: International
Conference on Advances in Construction Materials and Systems, pp. 421e428.
Daniel, N.H., Hassan, N.A., Idham, M.K., Jaya, R.P., Hainin, M.R., Ismail, C.R.,
Puan, O.C., Azahar, N.M., 2019. Properties of bitumen modified with latex. IOP
Conf. Ser. Mater. Sci. Eng. 527 https://doi.org/10.1088/1757-899X/527/1/012063,
012063.
Demirbas, M.F., Balat, M., 2006. Recent advances on the production and utilization
trends of bio-fuels: a global perspective. Energy Convers. Manag. 47,
2371e2381. https://doi.org/10.1016/j.enconman.2005.11.014.
Fernando, M.J., Nadarajah, M., 1969. Use of natural rubber latex in road construction.
Rubber Res. Inst. Malaya 22, 430e440.
Fini, E.H., Kalberer, E.W., Shahbazi, A., Basti, M., You, Z., Ozer, H., Aurangzeb, Q., 2011.
Chemical characterization of biobinder from swine manure: sustainable mod-
ifier for asphalt binder. J. Mater. Civ. Eng. 23, 1506e1513. https://doi.org/
10.1061/(ASCE)MT.1943-5533.0000237.
Franta, I., 2012. Elastomers and Rubber Compounding Materials. Elesvier, New York.
Fu, P., Jones, D., Harvey, J.T., 2011. The effects of asphalt binder and granular material
characteristics on foamed asphalt mix strength. Construct. Build. Mater. 25,
1093e1101. https://doi.org/10.1016/j.conbuildmat.2010.06.067.
Gautam, P.K., Kalla, P., Jethoo, A.S., Agrawal, R., Singh, H., 2018. Sustainable use of
waste in flexible pavement: a review. Construct. Build. Mater. 180, 239e253.
https://doi.org/10.1016/j.conbuildmat.2018.04.067.
Ghavibazoo, A., Abdelrahman, M., 2013. Composition analysis of crumb rubber
during interaction with asphalt and effect on properties of binder. Int. J. Pave-
ment Eng. 14, 517e530. https://doi.org/10.1080/10298436.2012.721548.
Ghavibazoo, A., Abdelrahman, M., 2014. Effect of crumb rubber dissolution on low-
temperature performance and aging of asphalterubber binder. Transp. Res. Rec.
J. Transp. Res. Board 2445, 47e55. https://doi.org/10.3141/2445-06.
Ghavibazoo, A., Abdelrahman, M., Ragab, M., 2013. Effect of crumb rubber modifier
dissolution on storage stability of crumb rubberemodified asphalt. Transp. Res.
Rec. J. Transp. Res. Board 2370, 109e115. https://doi.org/10.3141/2370-14.
Greve, H.-H., 2000. Rubber, 2. Natural. In: Ullmann’s Encyclopedia of Industrial
Chemistry. Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim, Germany, p. 14.
https://doi.org/10.1002/14356007.a23_225.
Groover, M.P., 2010. Summary for policymakers. In: Intergovernmental Panel on
Climate Change. Cambridge University Press, Cambridge, pp. 1e30. https://
doi.org/10.1017/CBO9781107415324.004. Climate Change 2013 - The Physical
Science Basis.
Grumoorthy, Tinavallie A/P., 2013. Improving the Ductility and Elastic Recovery of
Bitumen -natural Rubber Latex Blend. University Tun Abdul Rahman.
Ibrahim, S., Daik, R., Abdullah, I., 2014. Functionalization of liquid natural rubber via
oxidative degradation of natural rubber. Polymers 6, 2928e2941. https://
doi.org/10.3390/polym6122928.
Ibrahim, A., Ahmad, A., Kamarudin, F., Mansor, S., Shafika, I., Bahri, S., 2017.
Peformance of Bituminous-modified binder using natural rubber latex as green
enhancer. In: International Malaysia-Indonesia-Thailand SIC, Symposium on
Innovation and Creativity (IMIT-SIC), pp. 1e4.
Ikeda, Y., Kato, A., Kohjiya, S., Nakajima, Y., 2018. Basic science of rubber. In: Rubber
Science. Springer Singapore, Singapore, pp. 19e53. https://doi.org/10.1007/978-
981-10-2938-7_2.
Institute, A., 2015. The Bitumen Industry A Global Perspective Production, Chem-
istry, Use,specification and Occupatinal Exposure, third ed. Asphalt Institute Inc.
and European Bitumen AssociationeEurobitume. Asphalt Institute Inc. and
European Bitumen AssociationeEurobitume, USA.
Intapun, J., Sainte-Beuve, J., Bonfils, F., Tanrattanakul, V., Dubreucq, E., Vaysse, L.,
2010. Effect of microorganisms during the initial coagulum maturation of Hevea
natural rubber. J. Appl. Polym. Sci. 116 https://doi.org/10.1002/app.32331 n/a-n/
a.
Ismail, A., Al-mansob, R.A., Izzi, N., Yusoff, B., Karim, M.R., 2012. Effect of toluene as
15
Journal of Cleaner Production 289 (2021) 125727
disperser on the bitumen modified with epoxidized natural rubber with aging
simulation. Aust. J. Basic Appl. Sci. 6, 97e101.
Karak, Niranjan, 2009. Fundamentals of Polymers: Raw Materials to Finish Products.
PHI Learning Pvt. Ltd, New Delhi.
Khadivar, A., Kavussi, A., 2013. Rheological characteristics of SBR and NR polymer
modified bitumen emulsions at average pavement temperatures. Construct.
Build. Mater. 47, 1099e1105. https://doi.org/10.1016/j.conbuildmat.2013.05.093.
Kheradmand, B., Muniandy, R., Hua, L.T., Yunus, R.B., Solouki, A., 2014. An overview
of the emerging warm mix asphalt technology. Int. J. Pavement Eng. 15, 79e94.
https://doi.org/10.1080/10298436.2013.839791.
Kohjiya, Shinzo, Ikeda, Y., 2014. Natural Rubber: Production, Properties and Appli-
cations. Elsevier Science.
€ k, B.V., Yılmaz, M., Akpolat, M., 2014. Evaluation of the conventional and rheo-
Ko
logical properties of SBSþSasobit modified binder. Construct. Build. Mater. 63,
174e179. https://doi.org/10.1016/j.conbuildmat.2014.04.015.
Kuhlman, T., Farrington, J., 2010. What is Sustainability? Sustainability 2,
3436e3448. https://doi.org/10.3390/su2113436.
Lesueur, D., 2009. The colloidal structure of bitumen: consequences on the rheology
and on the mechanisms of bitumen modification. Adv. Colloid Interface Sci. 145,
42e82. https://doi.org/10.1016/j.cis.2008.08.011.
Mark, J.E., Erman, B., Roland, M., 2013. The Science and Technology of Rubber. Ac-
ademic press.
Martinez-Arguelles, G., Giustozzi, F., Crispino, M., Flintsch, G.W., 2014. Investigating
physical and rheological properties of foamed bitumen. Construct. Build. Mater.
72, 423e433. https://doi.org/10.1016/j.conbuildmat.2014.09.024.
Mathew, M.R.S.N., 1992. Natural Rubber,Biology, Cultivation and Technology.
Elsevier Science.
Mazlina Mustafa kamal, K.A.H., 2016. Rubberised bitumen e an innovative and
sustainable technology for road pavements. In: 13th Universiti Malaysia Ter-
engganu International Annual Symposium on Sustainability Science and Man-
agement (UMTAS 2016). Diterbitkan Oleh Penerbit UMT Universiti Malaysia
Terengganu (UMT) 21030 Kuala Terengganu, pp. 123e127. Terengganu.
Mohan, D., Pittman, C.U., Steele, P.H., 2006. Pyrolysis of wood/biomass for bio-oil: a
critical review. Energy Fuel. 20, 848e889. https://doi.org/10.1021/ef0502397.
Mohd Azahar, N., Abdul Hassan, N., Jaya, R.P., Md Nor, H., Mohd Satar, M.K.I.,
Mashros, N., Mohamed, A., 2019a. Mechanical performance of asphalt mixture
containing cuplump rubber. J. Teknol. 81, 179e185. https://doi.org/10.11113/
jt.v81.13857.
Mohd Azahar, N., Abdul Hassan, N., Putrajaya, R., Rosli Hainin, M., Che Puan, O.,
Athma Mohd Shukry, N., Azril Hezmi, M., 2019b. Engineering properties of
asphalt binder modified with cup lump rubber. IOP Conf. Ser. Earth Environ. Sci.
220, 012014 https://doi.org/10.1088/1755-1315/220/1/012014.
Mohd Hasan, M.R., You, Z., Yang, X., 2017. A comprehensive review of theory,
development, and implementation of warm mix asphalt using foaming tech-
niques. Construct. Build. Mater. 152, 115e133. https://doi.org/10.1016/
j.conbuildmat.2017.06.135.
Mustafa Kamal, M., Hadithon, K.A., Abu Bakar, R., 2019. Warm mix asphalt aditive in
natural rubber modified bitumen. MATEC Web Conf. 266, 04005 https://
doi.org/10.1051/matecconf/201926604005.
Mustafa Kamal, M., Arifin Hadithon, K., Abu Bakar, R., 2020. Natural rubber modified
asphalt. IOP Conf. Ser. Earth Environ. Sci. 498, 012001 https://doi.org/10.1088/
1755-1315/498/1/012001.
Nair, K.P.P., 2010. Rubber (Hevea brasiliensis). In: The Agronomy and Economy of
Important Tree Crops of the Developing World. Elsevier, pp. 237e273. https://
doi.org/10.1016/B978-0-12-384677-8.00008-4.
Nair, N.R., Mathew, N.M., Thomas, S., Chatterjee, P., Siddiqui, M.A., 1998. Physical
and rheological characteristics of liquid natural rubber modified bitumen.
J. Appl. Polym. Sci. 68, 53e61. https://doi.org/10.1002/(SICI)1097-
4628(19980404)68:1<53::AID-APP6>3.0.CO;2-M.
Nakao, T., Kohjiya, S., 2014. Computer simulation of network formation in natural
rubber (NR). In: Chemistry, Manufacture and Applications of Natural Rubber.
Elsevier, pp. 216e246. https://doi.org/10.1533/9780857096913.1.216.
Nanjegowda, V.H., Biligiri, K.P., 2020. Recyclability of rubber in asphalt roadway
systems: a review of applied research and advancement in technology. Resour.
Conserv. Recycl. 155, 104655. https://doi.org/10.1016/j.resconrec.2019.104655.
Nawamawat, K., Sakdapipanich, J.T., Ho, C.C., Ma, Y., Song, J., Vancso, J.G., 2011.
Surface nanostructure of Hevea brasiliensis natural rubber latex particles. Col-
loids Surf. A Physicochem. Eng. Asp. 390, 157e166. https://doi.org/10.1016/
j.colsurfa.2011.09.021.
Oliveira, M.S.C., Morais, S.M. de, Magalh~ aes, D.V., Batista, W.P., Vieira, I.G.P.,
Craveiro, A.A., de Manezes, J.E.S.A., Carvalho, A.F.U., de Lima, G.P.G., 2011.
Antioxidant, larvicidal and antiacetylcholinesterase activities of cashew nut
shell liquid constituents. Acta Trop. 117, 165e170. https://doi.org/10.1016/
j.actatropica.2010.08.003.
Othman, Z., Hainin, M.R., Warid, M.N.M., Idham, M.K., Kamarudin, S.N.N., 2018. Cup
lump modified asphalt mixture along jalan Kuala Lumpur-Kuantan, daerah
Temerloh, Pahang. MATEC Web Conf. 250 https://doi.org/10.1051/matecconf/
201825002007, 02007.
Ozturk, H.I., Kutay, M.E., 2014. Sensitivity of nozzle-based foamed asphalt binder
characteristics to foaming parameters. Transp. Res. Rec. J. Transp. Res. Board
2444, 120e129. https://doi.org/10.3141/2444-14.
Padhan, R.K., Gupta, A.A., Badoni, R.P., Bhatnagar, A.K., 2015. Improved performance
of a reactive polymer-based bituminous mixes e effect of cross-linking agent.
Road Mater. Pavement Des. 16, 300e315. https://doi.org/10.1080/
14680629.2014.995210.
A.H. Ansari, F.M. Jakarni, R. Muniandy et al.
Pasandín, A.R., Pe rez, I., 2015. The influence of the mineral filler on the adhesion
between aggregates and bitumen. Int. J. Adhes. Adhes. 58, 53e58. https://
doi.org/10.1016/j.ijadhadh.2015.01.005.
Peralta, J., Raouf, M.A., Tang, S., Williams, R.C., 2012. Bio-renewable asphalt modi-
fiers and asphalt substitutes. In: Gopalakrishnan, K., van Leeuwen, J., Hans),
Brown, R.C. (Eds.), Sustainable Bioenergy and Bioproducts: Value Added Engi-
neering Applications. Springer London, London, pp. 89e115. https://doi.org/
10.1007/978-1-4471-2324-8_6.
Picado-Santos, L.G., Capita ~o, S.D., Neves, J.M.C., 2020. Crumb rubber asphalt mix-
tures: a literature review. Construct. Build. Mater. 247, 118577. https://doi.org/
10.1016/j.conbuildmat.2020.118577.
Polacco, G., Stastna, J., Biondi, D., Zanzotto, L., 2006. Relation between polymer
architecture and nonlinear viscoelastic behavior of modified asphalts. Curr.
Opin. Colloid Interface Sci. 11, 230e245. https://doi.org/10.1016/
j.cocis.2006.09.001.
Poovaneshvaran, S., Mohd Hasan, M.R., Putra Jaya, R., 2020. Impacts of recycled
crumb rubber powder and natural rubber latex on the modified asphalt rheo-
logical behaviour, bonding, and resistance to shear. Construct. Build. Mater. 234,
117357. https://doi.org/10.1016/j.conbuildmat.2019.117357.
Prastanto, H., Firdaus, Y., Puspitasari, S., Ramadhan, A., Falaah, A.F., 2019. Study of
physical characteristic of rubberized hot mix asphalt based on various dosage of
natural rubber latex and solid rubber. IOP Conf. Ser. Mater. Sci. Eng. 509 https://
doi.org/10.1088/1757-899X/509/1/012049, 0e8.
Qian, C., Fan, W., Yang, G., Han, L., Xing, B., Lv, X., 2020. Influence of crumb rubber
particle size and SBS structure on properties of CR/SBS composite modified
asphalt. Construct. Build. Mater. 235, 117517. https://doi.org/10.1016/
j.conbuildmat.2019.117517.
Razali, R., Hainin, M.R., Hassan, N.A., Idham, M.K., Malek, M.S.C., Warid, M.N.M.,
Yaacob, H., Mohamed, A., Ismail, C.R., 2019. Field performance of asphalt
pavement maintenance using cup lump rubber modified asphalt (CMA). IOP
Conf. Ser. Mater. Sci. Eng. 527, 012064 https://doi.org/10.1088/1757-899X/527/
1/012064.
Ren, S., Liu, X., Wang, H., Fan, W., Erkens, S., 2020. Evaluation of rheological be-
haviors and anti-aging properties of recycled asphalts using low-viscosity
asphalt and polymers. J. Clean. Prod. 253, 120048. https://doi.org/10.1016/
j.jclepro.2020.120048.
ResearchInChina, 2017. Global and China Natural Rubber Industry Report, 2017-
2021. Research in China.
Rubber, Matador, 2007. Rubber Chemistry, Virtual Education in Rubber Technology.
Ruggles, Colin, 2005. The Use of Natural Rubber Latex in Modified Asphalt Road
Binders in the UK.
Sani, A., Mohd Hasan, M.R., Shariff, K.A., Jamshidi, A., Ibrahim, A.H.,
Poovaneshvaran, S., 2019. Engineering and microscopic characteristics of nat-
ural rubber latex modified binders incorporating silane additive. Int. J. Pave-
ment Eng. 1e10. https://doi.org/10.1080/10298436.2019.1573319, 0.
Sani, A., Mohd Hasan, M.R., Shariff, K.A., Jamshidi, A., Poovaneshvaran, S.,
Shahid, K.A., 2020. Physico-mechanical and morphological properties of wax
latex-modified asphalt binder. Iran. J. Sci. Technol. Trans. Civ. Eng. https://
doi.org/10.1007/s40996-020-00422-9.
Saowapark, W., Jubsilp, C., Rimdusit, S., 2019. Natural rubber latex-modified as-
phalts for pavement application: effects of phosphoric acid and sulphur addi-
tion. Road Mater. Pavement Des. 20, 211e224. https://doi.org/10.1080/
14680629.2017.1378117.
Satakhun, D., Chayawat, C., Sathornkich, J., Phattaralerphong, J., Chantuma, P.,
Thaler, P., Gay, F., Nouvellon, Y., Kasemsap, P., 2019. Carbon sequestration po-
tential of rubber-tree plantation in Thailand. IOP Conf. Ser. Mater. Sci. Eng. 526
https://doi.org/10.1088/1757-899X/526/1/012036.
Shaffie, E., Ahmad, J., Arshad, A.K., Kamarun, D., Kamaruddin, F., Mara, U.T., 2015.
Stripping performance and volumetric properties evaluation of hot mix asphalt
( HMA ) mix design using natural rubber latex polymer modified binder ( NRMB
). In: InCIEC. springer, singapore, pp. 873e884.
Shaffie, E., Wan Hanif, W.M.M., Arshad, A.K., Hashim, W., 2017. Rutting resistance of
asphalt mixture with cup lumps modified binder. IOP Conf. Ser. Mater. Sci. Eng.
271, 012056 https://doi.org/10.1088/1757-899X/271/1/012056.
Shaffie, E., Arshad, A.K., Ahmad, J., Hashim, W., 2018. Effect of mixing variables on
the physical properties of modified bitumen using natural rubber latex. Int. J.
Civ. Eng. Technol. 9, 1812e1821.
Shafii, M.A., Lai Yew Veng, C., Mohamad Rais, N., Ab Latif, A., 2017. Effect of blending
temperature and blending time on physical properties of NRL-modified
bitumen. Int. J. Appl. Eng. Res. 12, 3844e3849.
Shen, J., Amirkhanian, S., Xiao, F., Tang, B., 2009. Influence of surface area and size of
crumb rubber on high temperature properties of crumb rubber modified
binders. Construct. Build. Mater. 23, 304e310. https://doi.org/10.1016/
j.conbuildmat.2007.12.005.
Shu, X., Huang, B., Shrum, E.D., Jia, X., 2012. Laboratory evaluation of moisture
susceptibility of foamed warm mix asphalt containing high percentages of RAP.
Construct. Build. Mater. 35, 125e130. https://doi.org/10.1016/
j.conbuildmat.2012.02.095.
Shvedov, V.P., Orlov, Y.F., Shevyakov, A.M., 1965. Spectra of phosphate esters in the
900?1400 cm?1 region. J. Appl. Spectrosc. 2, 36e38. https://doi.org/10.1007/
BF00658082.
16
Journal of Cleaner Production 289 (2021) 125727
Sienkiewicz, M., Borze˛ dowska-Labuda, K., Wojtkiewicz, A., Janik, H., 2017. Devel-
opment of methods improving storage stability of bitumen modified with
ground tire rubber: a review. Fuel Process. Technol. 159, 272e279. https://
doi.org/10.1016/j.fuproc.2017.01.049.
Siswanto, H., 2017. The effect of latex on permanent deformation of asphalt concrete
wearing course. Procedia Eng 171, 1390e1394. https://doi.org/10.1016/
j.proeng.2017.01.452.
Sriring, M., Nimpaiboon, A., Kumarn, S., Sirisinha, C., Sakdapipanich, J., Toki, S., 2018.
Viscoelastic and mechanical properties of large- and small-particle natural
rubber before and after vulcanization. Polym. Test. 70, 127e134. https://doi.org/
10.1016/j.polymertesting.2018.06.026.
Suaryana, N., Sofyan, T.S., 2019. Performance evaluation of hot mixture asphalt
using concentrated rubber latex, rubber compound and synthetic polymer as
modifier. Civ. Eng. Dimens. 21, 36e42. https://doi.org/10.9744/ced.21.1.36-42.
Sutanto, M., Bala, N., Al Zaro, K., Sunarjono, S., 2018. Properties of crumb rubber and
latex modified asphalt binders using superpave tests. MATEC Web Conf. 203,
05007 https://doi.org/10.1051/matecconf/201820305007.
Thodesen, C., Xiao, F., Amirkhanian, S.N., 2009. Modeling viscosity behavior of
crumb rubber modified binders. Construct. Build. Mater. 23, 3053e3062.
https://doi.org/10.1016/j.conbuildmat.2009.04.005.
Tuntiworawit, N., Lavansiri, D., Phromsorn, C., 2005. The modification of asphalt
with natural rubber latex. Proc. East. Asia Soc. Transp. Stud. 5, 679e694.
Vasavi, D. wetha, Rani, K. urga, 2014. Effect of natural rubber on the properties of
bitumen and bituminious mixes. Int. J. Civ. Eng. Technol. 5, 976e6308.
Venudharan, V., Biligiri, K.P., 2017. Effect of crumb rubber gradation on asphalt
binder modification: rheological evaluation, optimization and selection. Mater.
Struct. 50, 129. https://doi.org/10.1617/s11527-017-0994-x.
Vichitcholchai, N., Panmai, J., 2012. Modification of asphalt cement by natural
rubber for pavement construction. Rubber Thai. J. 39, 32e39.
Vinod, A., Sanjay, M.R., Suchart, S., Jyotishkumar, P., 2020. Renewable and sustain-
able biobased materials: an assessment on biofibers, biofilms, biopolymers and
biocomposites. J. Clean. Prod. 258, 120978. https://doi.org/10.1016/
j.jclepro.2020.120978.
Wang, H., Li, W., 2008. Selective ultrasonic foaming of polymer for biomedical
applications. J. Manuf. Sci. Eng. 130 https://doi.org/10.1115/1.2823078.
Wang, H., You, Z., Mills-Beale, J., Hao, P., 2012. Laboratory evaluation on high
temperature viscosity and low temperature stiffness of asphalt binder with
high percent scrap tire rubber. Construct. Build. Mater. 26, 583e590. https://
doi.org/10.1016/j.conbuildmat.2011.06.061.
Wang, S., Cheng, D., Xiao, F., 2017. Recent developments in the application of
chemical approaches to rubberized asphalt. Construct. Build. Mater. 131,
101e113. https://doi.org/10.1016/j.conbuildmat.2016.11.077.
Wang, H., Liu, X., Apostolidis, P., Scarpas, T., 2018. Review of warm mix rubberized
asphalt concrete: towards a sustainable paving technology. J. Clean. Prod. 177,
302e314. https://doi.org/10.1016/j.jclepro.2017.12.245.
Wang, H., Liu, X., Apostolidis, P., Erkens, S., Scarpas, T., 2019. Numerical investigation
of rubber swelling in bitumen. Construct. Build. Mater. 214, 506e515. https://
doi.org/10.1016/j.conbuildmat.2019.04.144.
Wang, H., Apostolidis, P., Zhu, J., Liu, X., Skarpas, A., Erkens, S., 2020a. The role of
thermodynamics and kinetics in rubberebitumen systems: a theoretical over-
view. Int. J. Pavement Eng. 1e16. https://doi.org/10.1080/
10298436.2020.1724289, 0.
Wang, H., Liu, X., Apostolidis, P., Erkens, S., Skarpas, A., 2020b. Experimental
investigation of rubber swelling in bitumen. Transp. Res. Rec. J. Transp. Res.
Board 2674, 203e212. https://doi.org/10.1177/0361198120906423.
Wen, H., Bhusal, S., Wen, B., 2013. Laboratory evaluation of waste cooking oil-based
bioasphalt as an alternative binder for hot mix asphalt. J. Mater. Civ. Eng. 25,
1432e1437. https://doi.org/10.1061/(ASCE)MT.1943-5533.0000713.
Wen, Y., Wang, Y., Zhao, K., Sumalee, A., 2017. The use of natural rubber latex as a
renewable and sustainable modifier of asphalt binder. Int. J. Pavement Eng. 18,
547e559. https://doi.org/10.1080/10298436.2015.1095913.
Yildirim, Y., 2007. Polymer modified asphalt binders. Construct. Build. Mater. 21,
66e72. https://doi.org/10.1016/j.conbuildmat.2005.07.007.
Yu, X., Wang, Y., Luo, Y., 2013. Impacts of water content on rheological properties
and performance-related behaviors of foamed warm-mix asphalt. Construct.
Build. Mater. 48, 203e209. https://doi.org/10.1016/j.conbuildmat.2013.06.018.
Zanzotto, L., Kennepohl, G.J., 1996. Development of rubber and asphalt binders by
depolymerization and devulcanization of scrap tires in asphalt. Transport. Res.
Rec. 1530, 51e58.
Zborowski, A., Kaloush, K.E., 2007. Predictive equations to evaluate thermal fracture
of asphalt rubber mixtures. Road Mater. Pavement Des. 8, 819e833. https://
doi.org/10.1080/14680629.2007.9690101.
Zhang, F., Yu, J., Wu, S., 2010. Effect of ageing on rheological properties of storage-
stable SBS/sulfur-modified asphalts. J. Hazard Mater. 182, 507e517. https://
doi.org/10.1016/j.jhazmat.2010.06.061.
Zhu, J., Birgisson, B., Kringos, N., 2014. Polymer modification of bitumen: advances
and challenges. Eur. Polym. J. 54, 18e38. https://doi.org/10.1016/
j.eurpolymj.2014.02.005.
Zhu, J., Balieu, R., Wang, H., 2019. The use of solubility parameters and free energy
theory for phase behaviour of polymer-modified bitumen: a review. Road
Mater. Pavement Des. 1e22. https://doi.org/10.1080/14680629.2019.1645725, 0.