Cleaner Materials 2 (2021) 100031

Contents lists available at ScienceDirect

Cleaner Materials
journal homepage: www.elsevier.com/locate/clema

The utilization of waste plastics in asphalt pavements: A review

Yuetan Ma a, Hongyu Zhou a, Xi Jiang a, Pawel Polaczyk a, Rui Xiao a, Miaomiao Zhang a, Baoshan Huang b,⇑
a
Department of Civil and Environmental Engineering, The University of Tennessee, Knoxville, TN 37996, USA
b
Edwin G Burdette Professor, Department of Civil and Environmental Engineering, The University of Tennessee, Knoxville, TN 37996, USA

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

Keywords: Plastics are commonly used in all aspect in daily life. Lacking suitable approaches for waste treatment, a huge
Waste plastics generation of waste plastics will cause the main global environmental issues. The most common types of waste
Asphalt pavement plastics in the US municipal solid waste (MSW) stream include high‐density polyethylene (HDPE), low‐density
Compatibility polyethylene (LDPE), polypropylene (PP), polystyrene (PS), polyethylene terephthalate (PET), Ethyl Vinyl
Low‐temperature performance
Acetate (EVA), and polyvinyl chloride (PVC). Hot mix asphalt (HMA) is considered the ideal place to reuse
waste plastics in high‐value applications because of its high usage in highway construction. This paper compre-
hensively reviewed various types of waste plastics in asphalt pavement via wet and dry processes. In general,
the incorporation of waste plastics into asphalt mixtures presented improvements in rutting resistance, fatigue
resistance, and moisture resistance. However, compatibility and low‐temperature performance problems
remained during the application of plastic modified asphalt. Different approaches are adopted to improve
the above limitations, including polymer additives, chemical additives, and nanomaterials. Additional studies
should be focused on the aging effect, pavement performance monitoring, the stabilization among polymers,
and the economic and environmental concerns of using plastics in asphalt pavements.

Contents

Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
Background . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
Types of plastics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
Approaches to incorporate plastics into the asphalt . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
Objective . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
Plastic modified asphalt through the wet process. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
Polyethylene (PE) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
Physical properties and modification mechanism of PE modified asphalt.. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
Compatibility of PE modified asphalt. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
Low-temperature performance of PE modified asphalt. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
Improvement of compatibility and low-temperature properties of PE modified asphalt. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
Ground tire rubber (GTR). . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
Styrene butadiene styrene (SBS) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
Chemical additives. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
Nanomaterials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
Polypropylene (PP) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
Ethyl Vinyl Acetate (EVA). . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
Polyvinyl chloride (PVC). . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
Plastic modified asphalt through dry process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
Plastics with high melting points. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
Plastics with low melting points. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
Field projects . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10

⇑ Corresponding author.
E-mail address: bhuang@utk.edu (B. Huang).

https://doi.org/10.1016/j.clema.2021.100031
Received 31 July 2021; Revised 24 September 2021; Accepted 18 November 2021

2772-3976/© 2021 The Authors. Published by Elsevier Ltd.

This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
Y. Ma et al. Cleaner Materials 2 (2021) 100031

Economic and environmental effects.. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10

Conclusions and future concerns. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
Declaration of Competing Interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11

Introduction applications and melting point. Regarding the exact melting tempera-
ture of the plastics, different mixing temperatures should be consid-
Background ered during asphalt modification. A majority of asphalt mixtures are
produced below 180 °C; however, some plastics, such as PVC, and
Nowadays, the utilization of waste materials in pavement construc- PET, cannot melt and blend with asphalt to coat aggregates
tion has gained many attentions to consume the waste materials with- (Brasileiro et al., 2019; Geyer et al., 2017).
out compromising the pavement qualities (Ma and Huang, 2020; Ma
et al., 2020a). U.S. government also promotes to apply cleaner materi-
als and sustainable technologies to extend the life cycle of pavements Approaches to incorporate plastics into the asphalt
(Ma et al., 2021a). Plastics have become a widespread commodity that
infiltrated every aspect of human life. The production of plastics pre- In general, there are two approaches to incorporate recycled plas-
sented a growth from 2 million metric tons in 1950 to 322 million met- tics in asphalt mixtures: the wet process and the dry process. Fig. 2
ric tons in 2015 (Geyer et al., 2017). The cumulative amount of plastic shows the wet process and dry process of incorporating plastics in
production reached 8.3 billion metric tons in 2017. Lacking awareness asphalt plants. In the wet process, polymers are blended with bitumen
of being recycled or reused, plastics have rapidly become a major con- at high temperatures to produce bituminous binders before mixing
cern of municipal solid waste (MSW) (Abd El‐Rahman et al., 2018). with aggregate (Ghuzlan et al., 2013b; Kalantar et al., 2012). There-
Fig. 1 presents the number of tons of plastics generated, recycled, com- fore, the wet process requires more machinery and equipment to shred
bustion with energy recovery, and landfilled from American Chemistry the plastics into powders and mix them with hot asphalt binder after-
Council. In 2018, plastics generation was approximately 35.7 million ward. Studies concluded that the blending of plastics and asphalt
tons in the United States, which was 12.2% of the MSW generation. through the wet process is a physical procedure in which plastic parti-
Among all generated plastics, only 8.7% of them can be recycled, cles could absorb the lightweight components in asphalt to form a dis-
while 75.6% and 15.7% of the plastics were landfilled and combusted persion of viscoelastic phase at high temperatures. Plastics with
with energy recovery, respectively (Abd El‐Rahman et al., 2018). Hot relatively low melting points, especially PE, are suitable for this pro-
mix asphalt (HMA) mixture is considered as a promising approach to cess (Fang et al., 2013; Ge et al., 2016).
reuse waste plastics in a large volume. Hence, waste plastics are inves- In the dry process, recycled plastics are added directly into the mix-
tigated as potential modifiers for asphalt binders or substitutes for ture as either aggregate replacement or mixture modifiers (Movilla‐
aggregates to achieve sustainable pavements. Quesada et al., 2019). The aggregate replacement approach is com-
monly used with recycled plastics with a high melting point, such as
PET and PS, while the mixture modifier approach applies to virtually
Types of plastics all types of recycled plastics (e.g., PE, PP, PET, and PS) except for poly-
vinyl chloride (PVC) due to the concern of hazardous chloride emis-
There exist numerous types of plastics with various compositions sions (Ahmadinia et al., 2012; Modarres and Hamedi, 2014). When
and engineering properties. Melting point is one physical property recycled plastics with a melting point below the mixture production
for asphalt modification since plastics need to melt first and become temperature are used for mixture modification via the dry process,
part of the asphalt binders. Table 1 classifies the plastics based on their they will melt upon mixing with the hot aggregates and produce

Fig. 1. Tons of plastics for generation and different treatments.

2
Y. Ma et al. Cleaner Materials 2 (2021) 100031

Table 1
Types of plastics with different applications and melting points.

Types of plastics Applications Melting point (°C)

High-density Polyethylene (HDPE) Toys, shampoo bottles, pipes, and housewares 130–149
Low linear density polyethylene (LLDPE) food packing film and geomembranes 125
Low-density Polyethylene (LDPE) plastic bags, trays, containers, and agricultural film 110–120
Polypropylene (PP) plastic containers, piping system, and automotive parts 160–165
Polystyrene (PS) Test tubes, package, CD case, food container 210–249
Polyvinyl Chloride (PVC) window frames, profiles, cable insulation, and garden hoses 100–260
Ethyl Vinyl Acetate (EVA) Toys, home tools 75–102
Polyethylene Terephthalate(PET) Plastic bottles, food packaging 250–255
Other plastics: Acrylonitrile butadiene styrene Car parts; building insulations; e-wastes Depend on plastic types
(ABS); Polyurethane (PU); Polycarbonate (PC)

plastic‐coated aggregates with potentially improved physical and sur-
face characteristics (Modarres and Hamedi, 2014). Hence, the dry pro-
cess seemed simple and energy‐saving by adding the shredded plastics
powders directly into hot aggregates.
Objective
The objective of this study is to conduct a literature review of using
various plastics for asphalt modification via wet process and dry pro-
cess. Plastics modification asphalt through the wet process will be first
reviewed, including the modified effect, modification mechanisms,
and potential problems. Different approaches to improving the proper-
ties of plastic‐modified binder blends will be summarized afterward.
Plastic modified asphalt through the dry process will also be reviewed,
including the typical plastics with high melting points and low melting
points. Finally, future concerns of using plastics in asphalt will be pro-
posed. The overall sketch of this literature review is shown in Fig. 3.

Fig. 2. Wet process and dry process of incorporating plastics into batch asphalt plant (Brasileiro et al., 2019).

3
Y. Ma et al.
Fig. 3. Literature review flow chart.
Fig. 4. Microstructures of HDPE and LLDPE modified asphalt, (a) HDPE, (b) LLDPE (González et al., 2006).
Plastic modified asphalt through the wet process.
Polyethylene (PE)
Physical properties and modification mechanism of PE modified asphalt.
Polyethylene, accounting for 34% of the total plastics market, is
plastic with the greatest market production. PE can be mainly divided
into two categories: LDPE with a density between 0.91 and 0.94, and
HDPE with a density more than 0.94, which are manufactured by poly-
merization at high and low pressure, respectively (Ghuzlan et al.,
2013a). PE is usually a type of thermoplastic material moldable at a
certain elevated temperature and becomes rigid and solid upon cool-
ing. However, it can be modified to thermosetting material, such as
cross‐linked polyethylene. Initial studies are mainly focused on the
use of PE for asphalt modification through the wet process (-
Hınıslıoglu, 2004; Little, 1993; Little, 1991). The mixing temperature
varies from 150 to 180 °C with a percentage of PE addition between
1% and 10%. In general, the PE modifiers could increase the softening
point and decrease the penetration of the binder blends, indicating a
more rigid behavior of the asphalt mixtures and a higher resistance
to the permanent deformation of pavements (García‐Morales et al.,
2006; Gawande et al., 2012).
Furthermore, the addition of PE modifiers could reduce the strip-
ping, raveling and enhance the binder cohesion to the aggregates
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Cleaner Materials 2 (2021) 100031
(Daly et al., 1993; Flynn and Bridges, 1993; Stuart et al., 2000). The
basic modification mechanism is that PE tends to crystallize as solid
particles below the melting point in asphalt. The PE particles still exist
in solid states when the asphalt binder becomes soft at high pavement
service temperatures, enhancing the rutting resistance of the modified
binder blends. In terms of the microscale, certain plastic content could
combine with the asphalt to form a network that prevents the move-
ment of the molecular chain of asphalt (Dalhat and Al‐Abdul
Wahhab, 2015).
Compatibility of PE modified asphalt.
The crystal phase of PE could serve as high strength fillers during
modification and enable PE particles to remain intact in asphalt bin-
ders; hence, the binder blends tend to encounter phase separation
and suffer a compatibility issue between PE and asphalt (Yeh et al.,
2005). Many factors, including the types and contents of PE, may influ-
ence the compatibility between PE and asphalt binders. González et al.
investigated the application of HDPE and LLDPE in asphalt modifica-
tion. A severe phase separation for HDPE was detected compared to
LLDPE (Fig. 4). Hence, the dosages of LLDPE for asphalt modification
are recommended not to exceed 3% to improve the binder properties
and mitigating the phase separation of modifiers (González et al.,
2006). Fig. 5 displays the microstructures of asphalt modified with dif-
ferent content of LDPE. The micrographs the binder blends with less
Y. Ma et al.
Fig. 5. Optical micrographs of different PE modified binder blends. A) 2% wt LDPE; B) 5% wt LDPE; C) 15% wt. LDPE; D) 25% wt. LDPE; E) 50% wt LDPE
(Fuentes-Audén et al., 2008).
than 5% present dispersion of discontinuous polymer‐rich phase in
asphalt, while a continuous polymer phase and large disperse of
asphalt phase are noticed at 15% or higher LDPE content (Fuentes‐
Audén et al., 2008). A higher concentration of polymers tends to yield
various asphalt morphologies and narrow dispersion of asphalt dro-
plets in polymer‐rich continuous phases known as phase inversion
(Garcia‐Morales et al., 2004). Due to the swelling of maltenic com-
pounds, the increasing polymer concentration would change the rheo-
logical behaviors of binder blends from predominantly viscous
behavior (0–5% wt LDPE) to gel‐like behaviors (LDPE ≥ 15% wt).
Therefore, a lower LDPE concentration (less than 5%) is suitable for
pavement engineering, whereas higher LDPE content (greater than
15%) can be used for roofing membrane in building constructions.
Polacco et al. further evaluated different PE‐based polymers for
asphalt modification with high shear mixers. The special design of
high shear mixer allows the mixtures enter and move rapidly between
the two plates, making the mixtures of asphalt and polymers more
homogeneous. The rotational rate of the mixers can be adjusted based
on the type of polymers (Hasan et al., 2012). Testing showed that
LLDPE modifiers significantly altered the rheological and viscosity of
the base binder, indicating a possible formation of cross‐link structure
between LLDPE and asphalt binder (Polacco et al., 2005). Ho et al.
pointed out that PE generally improves the rutting resistance but
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Cleaner Materials 2 (2021) 100031
decreases the low temperature cracking resistance of the binder
blends; however, the low temperature cracking resistance and phase
separation tendency of modified binders were dependent on the
molecular weight of the polymers. Specifically, LDPE with lower
molecular weight showed little phase separation in storage stability
tests and cigar tube tests, which is more suitable for asphalt modifica-
tion (Ho et al., 2006; Punith and Veeraragavan, 2007). In terms of
HDPE modifiers, studies demonstrated that the improvement of mix-
ture properties in mixture stability and rutting resistance was more
pronounced for HDPE than LDPE (Costa et al., 2013; Khan et al.,
2016). However, HDPE could suffer a more severe phase separation
during high‐temperature storage, indicating that compatibility issue
occurs between HDPE and asphalt binder, even though a high‐shear
mixer was applied during blending (Moghadas Nejad et al., 2017).
Low-temperature performance of PE modified asphalt.
The low‐temperature properties of PE‐modified asphalt are the
major concerns of using PE in asphalt pavement. The strategic high-
way research program (SHRP) concludes that 80% of pavements sub-
jected to low temperature cracking attribute to the break of asphalt
binder at low temperatures. From the binder perspective, Fraas’s
breakpoint (FBP), ductility tests, direct tension (DT) test, and bending
beam rheometer tests (BBR) are commonly adopted to evaluate the
Y. Ma et al.
low‐temperature performance of the modified asphalt binder (Tang
et al., 2018; Wang et al., 2017b). Researchers believed that PE modi-
fiers could not improve the low‐temperature properties of the asphalt
binder in terms of the FBP in which higher FBP reflects worse low‐
temperature properties (Wang et al., 2017a). Du et al. summarized
the FBP of various polymer‐modified asphalt binders and concluded
that the FBP of rubber‐modified asphalt is the lowest. The FBP of PE
modified asphalt is higher than the base asphalt, indicating the worse
low‐temperature properties of the modified binder blends (Du et al.,
2020). It was also reported that the ductility of the binder blends
decreases with the addition of PE (Attaelmanan et al., 2011; Fang
et al., 2013; Ho et al., 2006). BBR and DT tests are two types of tests
to predict the critical cracking temperature of the asphalt binders. Test
results showed that PE modified asphalt had a higher critical cracking
temperature than the base binder, indicating a lower cracking resis-
tance at low temperatures (Lee and Hesp, 1994).
Improvement of compatibility and low-temperature properties of PE
modified asphalt.
PE modified asphalt could improve the high‐temperature perfor-
mance, fatigue resistance, and moisture resistance; however, PE mod-
ified asphalt have not been widely used in the practical projects mainly
due to the two reasons: (1) the compatibility between the asphalt and
remains due to the segregation of PE particles; (2) the low‐temperature
flexibility of PE is poor, which exaggerate the low‐temperature crack-
ing issue of the modified binder blends. Different approaches have
been adopted to improve the compatibility and low‐temperature prop-
erties of the PE‐modified binder blends. The aforementioned review
Fig. 6. Microstructures of different modified binder blends. (a) 4% PE, (b) 4% PE and 4% GTR; (c) 4% PE and 8% GTR; (d) 4% PE and 12% GTR; (e) 4% PE 4%
GTR with compatibilizer; (f) GTR/PE composites (Ma et al., 2021c).
6
Cleaner Materials 2 (2021) 100031
indicated that the types and contents of PE might affect the compatibil-
ity of the binder blends in which the segregation effect can be miti-
gated by using the PE with fewer quantities and molecular weight
(Costa et al., 2013; Ho et al., 2006; Punith and Veeraragavan, 2007).
Besides, the addition of rubberized polymers such as ground tire rub-
bers (GTR), styrene–butadienestyrene (SBS), and additives including
polyphosphoric acid (PPA), maleic anhydride (MAH) also present
notable improvement of the compatibility and low‐temperature crack-
ing resistance of the binder blends (Fu et al., 2007; Li et al., 2003).
Ground tire rubber (GTR)
Approximately one billion waste tires end their service life each
year globally, which are the majority segments of “black pollution”.
The waste tires are usually ground into tiny sizes, known as the ground
tire rubbers (GTR), and mixed with PE as a co‐modifier to mitigate the
phase separation of PE particles for binder modification (Huang et al.,
2002; Mashaan et al., 2013; Wang et al., 2018). Generally, natural rub-
bers start to degrade at 143 °C and accelerate the degradation rate as
the temperature exceeds 200 °C (De et al., 2005). As for the asphalt
modification through the wet process, rubbers can be partially
digested into asphalt in which rubber particles tend to swell and soften
due to the absorption of the aromatic oils asphalt binder (Huang et al.,
2002; Lee et al., 2008). However, the increased temperatures and mix-
ing time would cause excessive degradation of rubbers and the reduc-
tion in performance of modified asphalt binders (Lo Presti, 2013). Wu
et al. concluded that a higher temperature would destroy their cross‐
link structures and facilitate the dissolution of rubber particles (Wu
et al., 2016). Yan et al. found that the addition of 10% GTR into 5%
PE modified asphalt could improve the ductility of the binder blends
Y. Ma et al.
Fig. 7. Reaction mechanism of vulcanization of TOR.
up to 50% (Yan et al., 2015). Studies also demonstrated that the com-
plex modulus of GTR modified asphalt is increased at high tempera-
tures and declined at low temperatures, which proved that GTR
could enhance the rutting resistance of the binder blends and reduce
the risk of low‐temperature cracking potential of the pavements
(Huang, 2008). However, the high molecular weight of GTR will also
lead to the precipitation of the rubber particles (Xu et al., 2017). One
approach to solving the compatibility among PE, GTR, and asphalt is to
use the GTR/PE composites. The pre‐degraded rubbers are alloyed
with PE to form a stabilized compound (Ma et al., 2021b; Wang
et al., 2014). Fig. 6 (a) to (f) displays the microstructures for different
GTR and PE blends conducted by Ma et al. The test results reflect those
rubber particles have the ability to scissor the PE into smaller sizes. At
the same time, the GTR/PE composites enable a homogenous disper-
Fig. 8. Micrographs (100×magnification) of HDPE-SBS modified asphalt with 0.4%. LLDPE-MAH after 48 h storage test; top section (left); bottom section (right)
(Zhang et al., 2013).
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Cleaner Materials 2 (2021) 100031
sion of PE particles and the dissolution of GTR particles into asphalt
(Ma et al., 2021c). A network between PE particles and rubberized
asphalt was formed to strengthen the asphalt properties at high and
low temperatures (Liang et al., 2020; Ma et al., 2021c; Wang et al.,
2014; Zhang et al., 2016b).
Meanwhile, polymer additives such as Trans‐polyoctenamer (TOR)
were also adopted to improve the compatibility and thermal stability
of rubber asphalt by promoting the cross‐linking structure between
polymer and asphalt (Ren et al., 2020). TOR is a polymer with many
unsaturated bonds with high reactivity. The reaction mechanism of
TOR vulcanization is presented in Fig. 7. The double bonds in TOR
could undergo a cross‐linking reaction with sulfur component on the
surface of crumb rubbers, anticipating to mainly occur at carbon–car-
bon double bonds (Mu et al., 2020). Studies found that the application
of TOR to crumb rubber has outstanding effects on cracking, moisture,
and aging resistance of the asphalt mixtures (Zhang et al., 2021).
Nowadays, researchers tried to apply the TOR and cross‐linking agent
(i.e. elemental sulfur) in plastic modified asphalt, aiming at improving
the network between asphalt and plastics (Padhan et al., 2018).
Styrene butadiene styrene (SBS)
SBS is considered an effective polymer to improve the low‐
temperature performance of the PE‐modified binder blends. Most nota-
bly, asphalt modified with SBS copolymer, a thermoplastic elastomer
(TPE), has good processability, balanced properties at service temper-
atures, and is compatible with most asphalts (Fu et al., 2007; Peng
et al., 2013; Wang et al., 2015). As SBS dissolves in the poor solvation
of asphalt, the polystyrene blocks are more affected by heat, while the
butadiene blocks are affected by heat and solvation in the asphalt mal-
tenes. The maltenes lack the solvency to dissolve the butadiene leaving
the butadiene mid‐blocks swollen and dispersed in the asphalt matrix,
thereby elastic nature to the asphalt binder (Fawcett and McNally,
2003). However, several cases occur when SBS modified asphalt is
subjected to aging: (1) the degradation of SBS polymers; (2) the
destruction of phase structures during short‐term aging; and (3) the
oxidation of base asphalt during long‐term aging (Allen et al., 2000).
The thermal oxygen degradation and ultraviolet of SBS will break
the C = C bonds of butadiene in SBS, making the phase structure
inevitable in SBS modified asphalt (Zhao et al., 2011). The separation
potential of SBS modified asphalt at high temperatures is another dis-
advantaging of using SBS. Therefore, a series of additives are usually
applied to collaborate with SBS and PE to overcome the separation
and aging problems.
Chemical additives
PE grafted with MAH has proven an effective additive to improve
low‐temperature resistance, indicated by a lower creep stiffness and
a higher m‐value of BBR tests (Li et al., 2014). Zhang et al. evaluated
Y. Ma et al.
Fig. 9. Possible mechanism of PE-MAH during asphalt modification (Ma et al., 2016).
the high‐temperature storage stability of the HDPE‐SBS with LLDPE‐
MAH modified asphalt. They found that the difference of softening
point between the top and bottom sections of the samples is less than
2.5 °C, indicating no substantial phase separation of polymers and
asphalt. Optical micrographs for the top and bottom of the 0.4%
LLDPR‐MAH modified asphalt are shown in Fig. 8 (Zhang et al.,
2013). Ma et al. proposed the modification mechanism between PE
and MAH during asphalt modification. The schematic illustration is
displayed in Fig. 9. It is believed that polymer undergoes a reaction
between the epoxide ring of the polymer and carboxylic groups of
asphaltene (Polacco et al., 2004). The functional group of PE‐MAH,
including ring anhydride and carbonyl group, could interact with the
active groups in asphalt such as amino‐group, hydroxyl, and carboxyl
groups (Wang et al., 2014). As shown in Fig. 9, PE‐MAH can
strengthen the cross‐link interaction between maleic anhydride groups
and active groups in asphalt. The cross‐link could form a network
when PE‐MAH reaches a certain content. Due to the lower melting
point, PE‐MAH is usually in flow state during mixing and compaction,
which will fill the voids between the aggregates. When the tempera-
ture goes lower, PE‐MAH could maintain its shape and limit the move-
ments of the aggregates. Hence, the low‐temperature performance of
asphalt mixtures is significantly improved (Ma et al., 2016). Chen
et al. also concluded that MA could improve the interfacial adhesion
between PE and asphalt, reflected by the decreased non‐recoverable
creep compliance and increased permanent recovery (Chen et al.,
2021).
PPA, another widely used additive modifier, is produced from
dehydration of H3PO4 at high temperatures or heating P2O5 dispersed
in H3PO4. Literature has proved that chemical modification with PPA
could enhance the high‐temperature performance without mitigating
the low‐temperature performance of the binder blends (Huang et al.,
2016; Qian et al., 2019). PPA often works with SBS or styrene‐
butadiene rubber (SBR) by assisting the dispersion of SBS/SBR parti-
cles and shifting the asphalt structures from solution to gel. The addi-
tion of sulfur contributes to the dynamic vulcanization and the
improvement of thermal stability since vulcanization is a chemical pro-
cess in which polymer molecules interact to form a network under
high temperatures (Liang et al., 2017b).
8
Cleaner Materials 2 (2021) 100031
Nanomaterials
Nanomaterials including nano‐clays, nano‐SiO2, ZnO, and TiO2 are
also reported to collaborate with PE, aiming at enhancing the rheolog-
ical properties, low‐temperature performance, aging resistance, mois-
ture resistance, and storage stability of the binder blends (Fang
et al., 2012; Yao et al., 2013; Zhang et al., 2016a). Yao et al. found that
the nano‐SiO2 can improve the rutting, fatigue, and anti‐aging resis-
tance of the modified binder blends (Yao et al., 2013). Zhang et al. pre-
pared modified asphalt with two or three different nanomaterials
(ZnO, CaCO3, TiO2). It was observed that nanoparticles were well dis-
persed, and the compatibility of PE and asphalt was significantly
improved (Zhang et al., 2016a). Moreover, the ductility of composite
modified asphalt increases by adding Montmorillonite (OMMT) since
PE chains are absorbed by the strong surface energy of OMMT, which
favors the interaction between the polymer and asphalt (Fang et al.,
2012).
Polypropylene (PP)
Polypropylene is the second productive plastic, accounting for 21%
of the total plastic market at the global level (Geyer et al., 2017). Com-
pared to the PE modifier, PP is more challenging to mix homoge-
neously with asphalt through the wet process due to the higher
melting point. The common mixing temperature varies between 160
and 190 °C, while the percentage of PP for modified asphalt produc-
tion ranges between 3% and 5% (Brasileiro et al., 2019). The incorpo-
ration of ground PP powders into asphalt would notably reduce the
penetration and increase the viscosity and softening point of the mod-
ified binder blends, which has a pronounced rutting resistance than PE
modified asphalt (Dalhat and Al‐Abdul Wahhab, 2015). However, PP‐
modified asphalts are more susceptible to phase separation owing to a
lack of compatibility between PP and asphalt binder (Al‐Abdul
Wahhab et al., 2016). The addition of PP tends to reduce the ductility
of the modified binder blends significantly. To be specific, 5% of PP
results in approximately a 20% reduction of ductility, which is harmful
to the low‐temperature performance (Al‐Hadidy and Yi‐qiu, 2009).
Such reduction can be mitigated when PP is subjected to the reaction
with MA (Ahmedzade et al., 2015). Additives including Isotactic
Y. Ma et al.
polypropylene (iPP) and maleated polypropylene (MPP) could facili-
tate the dispersion and interaction of PP into the asphalt by increasing
the amorphous content and enhancing the amorphous region in
asphalt (Al‐Hadidy and Yi‐qiu, 2009). The addition of SBS or plas-
tomeric polybilt (PB) could improve the storage stability of PP modi-
fied binder blends but was not sufficient to mitigate the phase
separation issue, limiting the utilization of PP in asphalt modification
through the wet process (Al‐Abdul Wahhab et al., 2016).
Ethyl Vinyl Acetate (EVA)
EVA is a thermoplastic polymer that is manufactured by copolymer-
ization of ethylene (E) and vinyl acetate (VA) (Abd El‐Rahman et al.,
2018). The variations E and VA can be adjusted and controlled during
copolymerization to achieve different properties of the modifiers. The
segment of E is crystalline that provides a more rigid modified binder
blends at high temperatures, while VA presents non‐crystalline and
polarity properties in which a higher content of VA could enhance
the flexibility, elasticity, and storage stability of the binder blends
(Liang et al., 2017a). BBR tests from Yuliestyan et al. reflected that
m‐value increases notably with higher VA content, which improves
the low‐temperature behaviors of asphalt. In contrast, higher VA con-
tent causes poor resistance to the long‐term aging effect (Yuliestyan
et al., 2016). The modified binder blends were commonly prepared
at around 175 °C with a shear speed of 3000 to 4000 rpm in relation
to the mixing process. Similar to PE and PP modifiers, the addition of
EVA leads to an increment in the viscosity of the modified binder
blends, while in contrast with them, the ductility of EVA modified
asphalt increases as well. Studies showed that using 5% EVA in asphalt
tends to increase around 20% of the ductility. The increment will be
more pronounced when EVA was grafted with 2% MA (Luo and
Chen, 2011). Meanwhile, the rutting resistance at high temperatures
was still improved compared to the base binder, indicated by a larger
value of complex modulus and lower value of phase angle (Garcı´a‐
Morales et al., 2004). Researches showed that phase separation occurs
at a low content of EVA; however, as the EVA content increases, a
phase inversion occurs to form cross‐linking structures between
asphalt and EVA (Liu et al., 2017). Moreover, Sureshkumar et al.
revealed that the addition of nanoclays increases the interactions
between EVA and asphalt because clays exhibit higher polarity than
the EVA alone (Sureshkumar et al., 2010).
Polyvinyl chloride (PVC)
PVCs are mainly from pipes or window frames. The chemical bonds
between chloride and carbon increase the stiffness and hardness of
PVC (Fang et al., 2009). One study conducted by Ziari et al. shows that
waste PVC can enhance the rutting and fatigue resistance of the base
binder, whereas the low‐temperature cracking resistance may be com-
promised (Ziari et al., 2019). Kofteci et al. investigated three types of
PVC wastes, including cable window and blind wastes. The test results
concluded that the PVC derived from waste blinds presents the highest
brittleness, followed by the waste window and waste cable (Köfteci
et al., 2014). Fang et al. used an extruder to produce nanocomposites
with PVC and OMMT. The extruded compounds were added to the
base asphalt. It was found that numerous PVC molecular chains were
Table 2
Summary of binder properties modified with different plastics through wet process (based on literatures).
Type of Plastics Rutting resistance Fatigue cracking resistance
PE ↑ ↑
PP ↑ ↑
EVA ↑ ↑
PVC ↑ ↑
Cleaner Materials 2 (2021) 100031
interacted with OMMT lamella due to the large surface energy of
OMMT and the polarity of PVC chains, improving the compatibility
of the binder blends (Fang et al., 2014). PVC wastes are usually shred-
ded into powders for asphalt modification through wet processes, but
heating PVC will emit chloride, which is harmful to human health and
the environment. Therefore, further studies should be focus on solving
the emission issue during asphalt modification.
The wet process is more suitable for plastics with low melting
points such as PE. However, the modified binder blends encounter
compatibility problems with the asphalt‐plastic system. The plasticity
of the modifiers also leads to the low‐temperature cracking potential
of the asphalt mixtures. The major advantages and disadvantages of
different plastics through wet process are summarized in Table 2. In
general, plastics with higher melting point would have better rutting
and fatigue cracking resistance. However, the ductility and low‐
temperature cracking resistance would be compromised. In addition,
the binder blends would encounter more severely phase separation
between the asphalt and plastics.
Various strategies proved to improve the weakness of plastic mod-
ified asphalt through wet processes, including higher shear mixing
speed, higher mixing temperature, rubberized polymers, chemical
additives, and nanomaterials. The synergistic effects of the additives
tend to have more pronounced improvements in compatibility and
low‐temperature properties. As for the plastics with high melting
points such as PP and PET, it is energy‐consuming to provide heat to
dissolve such polymers into the asphalt. Furthermore, a severe phase
separation would occur due to the polymers’ large molecular weight
and strong chemical bonds. Therefore, the dry process is considered
especially for the rigid and hard polymers with high melting points.
Plastic modified asphalt through dry process
Generally, the dry process is applicable for all types of recycled
plastics by incorporating the plastic wastes into hot aggregates before
adding asphalt. In this process, plastics act as various functions such as
asphalt modifiers aggregates coating or aggregates replacement
depending on the size and properties of the plastics. Plastics with high
melting points are usually applied as aggregates substitution, whereas
the plastics with low melting points could form a thin film to wrap the
aggregates.
Plastics with high melting points
PET is a thermoplastic polymer with a high melting point, which is
mainly used to produce drinking bottles. PET has a specific gravity of
1.32, a tensile strength ranging from 300 to 350 MPa, an elasticity
modulus of 13 GPa, and an elongation of 7.5% (Yoo and Al‐Qadi,
2014). The majority of approaches of using PET in asphalt are dry pro-
cesses in which PET bottles are shredded into smaller sizes to replace
the aggregates. Pre‐mixing PET and hot aggregates should be carried
out to wrap the aggregates with the shredded PET plastics. In Hassani’s
study, approximately 5 to 15% of PET wastes, with sizes between 2.36
and 4.75 mm, were added to replace the aggregates in asphalt mix-
tures. The test results showed that the Marshall stability was similar
to the control samples, indicating that waste PETs can be used as
aggregates in the asphalt mixtures (Hassani et al., 2005). Dalhat
Low-temperature cracking resistance Phase separation Environmental concerns
↓ √ –
↓ √ –
↑ √ –
↓ √ √
9
Y. Ma et al.
et al. noticed that the processed PETs with finer dimensions (No.8 to
No. 40) have better moisture resistance than PETs with sizes ranging
from passing No.8 to No.10 (Dalhat et al., 2019). Researchers quanti-
fied the benefits that the addition of 12% PET extended the pavement
service life 2.81 times and saved around 20% asphalt layer thickness
(El‐Naga and Ragab, 2019). It is well acknowledged that the addition
of PET results in better rutting and fatigue resistance and mitigates the
moisture and thermal cracking resistance (Ahmadinia et al., 2012;
Ahmadinia et al., 2011; Baghaee Moghaddam et al., 2014). Phase sep-
aration and a decrease in specific gravity of asphalt mixtures occur due
to the non‐uniform distribution of PET (Ameri and Nasr, 2016).
Few studies tried to convert the PET to a liquid state by glycolysis
reaction to modify the base asphalt through the wet process (Ameri
and Nasr, 2016; Gürü et al., 2014). Mashaan et al. proposed that the
ideal content of PET for asphalt modification is 6–8%, corresponding
with the improved rutting and fatigue resistance (Mashaan et al.,
2021). Guru et al. introduced two novel additive materials, Thin Liq-
uid Polyol PET (TLPP) and Viscous Polyol PET (VPP), for asphalt mod-
ification. Two additives were determined to improve stripping, fatigue
resistance, and low temperature cracking resistance of the binder
blends (Gürü et al., 2014). Leng et al. combined Triethylenetetramine
(TETA) with PET through aminolysis reaction to synthesize a PET‐
derived additive, which was added to reclaimed asphalt pavement
(RAP) to improve both rutting and cracking resistance (Leng et al.,
2018).
Plastics with low melting points.
Researchers also tried to use plastics with lower melting points
through the dry process. In the beginning, Awward and Shbeed evalu-
ated the addition of PE into asphalt mixtures via the dry process. Both
LDPE and HDPE were added directly into the hot aggregates at 180 to
190 °C. The melted PE formed a thin film to coat the aggregates sur-
face. It was found that the incorporation of LDPE and HDPE increased
the Marshall stability and flow of the controlled asphalt mixtures. The
optimum PE content was recommended as 12% since the VMA, and air
voids decreased as the PE content is less than 12%, whereas increased
as the PE content is larger than 12% (Awwad and Shbeeb, 2007). Sim-
ilar studies with PE improved rutting resistance, indirect tensile
strength, resilient modulus, and fatigue resistance (Melbouci et al.,
2014; Vasudevan et al., 2012). Arabani et al. concluded that PE treat-
ment favors adhesion between the asphalt and aggregates and reduces
the free energy of the adhesion in the presence of water, contributing
to improved moisture resistance of the asphalt mixtures (Arabani and
Hamedi, 2011). Haider et al. found that PE modified asphalt mixtures
through wet process showed better adhesion and moisture resistance
than those modified though dry process (Haider et al., 2020). PP fibers
were also demonstrated to improve the Marshall stability of the
asphalt mixture; nevertheless, they did not affect the fatigue resistance
(Lastra‐González et al., 2016). Bajpai et al. evaluated the properties of
PP coated aggregates and summarized that PP coating favors the
impact, crushing, stripping, and abrasion resistance of aggregates
(Bajpai et al., 2017). In addition, GTR is sometimes mixed with PE
and PP against the plastic deformation and cracking of the asphalt mix-
tures during the dry process (Cao, 2007). Digestion time is one of the
critical parameters that determine the performances of asphalt mix-
tures. An appropriate digestion time before compaction could assist
the interaction between asphalt and polymers. Generally, an approxi-
mately 90 mins digestion time is necessary before compaction. The
maximum rubber sizes and quantities are recommended to be less than
0.6 mm and 1% weight of the aggregates, respectively (Moreno et al.,
2011). The main difference between plastics and GTR in the dry pro-
cess is that the former can improve the interaction between aggregates
and polymers. At the same time, the latter provides a digestion proce-
dure to modify the asphalt (Lastra‐González et al., 2016).
10
Cleaner Materials 2 (2021) 100031
Field projects
Most of the studies focused on the material properties of plastic
modified asphalt based on the laboratory tests. Field projects should
also be conducted to validate the pavement performances of incorpo-
rating the waste plastics. In India, Vasudevan et al. incorporated plas-
tic wastes with PE, PP, and PS into the pavement. Field monitoring
reflected that pavement with plastics is more suitable for heavy traffic
due to the improved binder, increased strength, and better surface con-
dition of the asphalt mixtures (Vasudevan et al., 2012). White and
Reid conducted a project by adding 200,000 plastic bags, 63,000 glass
bottles, and more than 4500 printer cartridges into asphalt pavement,
showing improved rutting and fatigue resistance comparing to the
unmodified asphalt road. The cost was higher than plain asphalt road
due to the lack of producers, but was not as much as other polymer
modified pavements (White and Reid, 2018). Chin and Damen also
conducted a project of using HDPE, LDPE, and PET in asphalt pave-
ment. Field tests indicated that the incorporation of plastics in asphalt
pavement could improve the moisture resistance, enhance binding
properties, and facilitate the high temperature performances without
increasing construction costs and releasing the toxic gases (Chin and
Damen, 2019). However, the long‐term performance of asphalt pave-
ment containing waste plastics need further monitoring and
investigation.
Economic and environmental effects.
In terms of economic and environmental effects, the use of plastics
in asphalt pavements benefits improved pavement performance, the
reduction of landfills, and the necessity of using virgin polymers,
resulting in possible cost savings and environmental protection in
the long term (Li et al., 2019; Ma et al., 2020b). The melting of plastics
may also release some hazardous emissions, which are harmful to the
environment. Vasudevan et al. used waste plastic in a road with 1 km
length and 3.75 m width, saving approximately 1 ton of asphalt bin-
der, while the pavement life lasted around 7 years (Vasudevan et al.,
2012). Sojobi et al. showed that using PET wastes in road construction
could consume the PET wastes by several million tons and also prolong
the service life of the pavements (Sojobi et al., 2016).
To quantify the economic and environmental effects, life cycle cost
analysis (LCCA) and life cycle assessment (LCA) are required to evalu-
ate the use of different plastics in asphalt pavement. Poulikakos et al.
conducted LCA using PET, glass, GTR in road construction and found
that the reduction of materials cost, greenhouse gas, and energy‐
saving was 8.5%–33.9% 266.3%‐860%, and 13.9%‐76.1%, respec-
tively (Poulikakos et al., 2017). Via‐Cortavitarte et al. used the LCA
tool to compare different PS wastes in asphalt mixtures. It was
observed that the addition of PS enlarged the pavement life expectancy
without increasing the environmental impacts during construction.
The social and environmental benefits are promising since the emis-
sions derived from the extraction and processing of the asphalt could
be avoided (Vila‐Cortavitarte et al., 2018). Lack of quantitative data
considering the pavement performance, economic impacts of using
various plastics into asphalt pavements, and insufficient LCA and
LCCA in this area need further investigation in future studies.
Conclusions and future concerns.
In summary, the paper shows a comprehensive literature review of
using plastics in asphalt pavements. The commonly used plastics for
asphalt modification through the wet process and dry process were
reviewed. The following findings are concluded:
Y. Ma et al.
• The wet process is suitable for plastics with low melting points,
improving the rutting resistance, moisture resistance, and fatigue
resistance of the binder blends. Plastics with higher melting point
tend to increase more viscosity but reduce more ductility of the bin-
der blends.
• The incorporation of plastics into asphalt through the wet process
may encounter two potential concerns: the phase separation and
low‐temperature performance of the binder blends. Plastics with
high melting points tend to exaggerate such concerns.
• Several approaches can be adopted to mitigate the compatibility
and low‐temperature problems including the addition of rubber-
ized materials, chemical additives, nanomaterials, etc. To be speci-
fic, rubberized materials aim to increase the ductility of the binder
blends, chemical additives are conducive to the formation of poly-
mer networks, and nanomaterials could provide enough surface
area and improve the dispersion and interaction between plastics
and asphalt.
• The dry process is applicable for all plastic types to enhance the rut-
ting and moisture resistance of asphalt pavements. Plastics with
high melting points are usually applied as aggregates substitution,
whereas the plastics with low melting points could form a thin film
to increase the adhesion among asphalt, plastics, and aggregates.
• Field projects of asphalt pavement containing plastics reflect that
the incorporation of plastics in asphalt pavement could improve
the moisture resistance, enhance binding properties, and facilitate
the high temperature performances without increasing construc-
tion costs and releasing the toxic gases. Quantitative data need to
be collected for further LCA and LCCA evaluation.
For future studies, in terms of wet process, innovative approaches
are also needed to improve the compatibility between asphalt and
plastics, especially the plastics with high melting points. Effective com-
patibilizers should be developed to stabilize the nanomaterials, plas-
tics, and other polymer additives to improve the low‐temperature
properties of the binder blends. In addition, the aging effects of
plastic‐modified asphalt mixtures require more tests and validation
to evaluate the long‐term performance of plastic‐modified asphalt.
Regarding the dry process, the mechanisms of using plastics and the
interactions among asphalt, aggregates, and plastics are worthy of
investigation. The homogeneity problem of coating between plastics
and aggregates needs to be solved to improve the workability during
construction. From the project level, more test sections are promoted
to be constructed with different types of plastics, and the pavement
performances are necessary to be monitored for the long‐term perfor-
mance evaluation. Finally, LCA and LCCA are supposed to quantify the
economic and environmental impacts of the addition of various plas-
tics throughout the whole life cycle.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
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