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Received: 6 October 2020 Revised: 22 January 2021 Accepted: 27 January 2021

DOI: 10.1002/pls2.10034

REVIEW

Waste plastics in asphalt concrete: A review

Brian P. Grady

School of Chemical, Biological, and


Materials Engineering, University of Abstract
Oklahoma, Norman, Oklahoma, USA Among possible applications for post-consumer waste plastics, one criterion is
that the application should be able to use very large amounts of material
Correspondence
Brian P. Grady, School of Chemical, because the amount of plastic waste is so large. Another key issue is econom-
Biological, and Materials Engineering, ics; very little cost should be involved in preparing waste plastics for a specific
University of Oklahoma, Norman, OK,
application. One of the few applications for post-consumer waste plastics that
USA.
Email: bpgrady@ou.edu could possibly meet both requirements is filler in asphalt concrete. Specifically,
if waste plastics in asphalt concrete were  10 wt%, then this application alone
could use all plastic waste currently being produced in the world. This review
examines the progress that has been made to incorporate waste plastics into
asphalt concrete and identifies key issues preventing this technology from
being applied commercially.

KEYWORDS
asphalt, bitumen, plastic, recycle

1 | INTRODUCTION of plastic in those new roads would be 10 wt%.[7] Reuse


of waste plastics in asphalt road construction is one of the
A recent article by Geyer[1] painted a stark picture of the very few applications, because of the large volumes of both
world's use of plastic and the buildup of waste plastic. As plastics and roads produced, that could effectively elimi-
shown in Figure 1, every year more than 100 pounds of nate landfilling or burning of plastic. The purpose of this
polymers are produced for every man, woman and child review article is to highlight studies that have described
on the planet. Recycling rates in the United States are low; incorporation of waste plastics into asphalt roads.
only about 9% of post-consumer plastic waste is Asphalt does not have a precise definition. In North
recycled.[4] In European countries that have banned land- America, the terms asphalt and bitumen refer to a highly
filling, the average recycling rate is 35%; the country viscous and sticky form of petroleum. Asphalt refers to
with the highest recycling rate in the world (Norway) still the bottoms from a distillation column of crude oil, while
only recycles about 45% of its plastic waste.[5] The vast bitumen refers to the form that occurs naturally without
majority of the remainder of the waste plastic in all of any processing. Outside of North America, the term bitu-
these countries is either burned for fuel value or buried in men refers to a highly viscous and sticky form of petro-
the ground. leum, no matter the source, while the terms asphalt
As is obvious by examining the top graph in Figure 1, refers to the product after mixing bitumen with aggre-
very few possible reuses of plastics could possibly absorb gate, for example, stone and sand.
the volumes required. In the United States, if all plastic dis- The formation of bitumen (using the term according
posed of in the United States (about 230 lbs/person/year)[6] to the North American convention) requires temperature
were put in newly constructed asphalt roads, the amount and pressure and hence forms far beneath the earth's

This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided
the original work is properly cited.
© 2021 The Authors. SPE Polymers published by Wiley Periodicals LLC. on behalf of Society of Plastics Engineers.

SPE Polymers. 2021;1–15. wileyonlinelibrary.com/journal/pls2 1


2 GRADY

This review is not the first review of this topic.[8–14]


This review differs in that the review is written for a read-
ership unfamiliar with asphalt and hence particular
attention is spent defining terms for tests, and, as much
as possible, confusing nomenclature is avoided. Further,
the clear division between plastics that melt and those
that do not is unique to this review versus other reviews.
Finally, previous reviews are organized among different
plastic types while this review is organized around differ-
ent properties of asphalt concrete and the effect that
waste plastics has on those properties.
This review is not comprehensive in two senses. First,
the focus is only on certain measurements. The measure-
ments were chosen because they are most directly related
to performance in roads. Second, not all papers are
referenced here; the author believes he looked at most if
not all papers that measured the quantities of interest,
but instead decided to choose representative results
rather than report all results.

1.1 | Asphalt concrete basics

Asphalt concrete is composed of binder and rocks at a


minimum. Typical weight fractions are approximately
FIGURE 1 World plastics production[2,3] 95% aggregate and 5% binder; volume fractions are typi-
cally 88% and 12%, respectively. The minimum amount
of binder required to properly wet the aggregate is typi-
surface. Tar has similar properties, but tar formation cally used; variations in binder amount occurs primarily
occurs either chemically in a reactor or column or occurs because aggregate can adsorb asphalt. Air also will be
naturally near the Earth's surface. Tar is not used exten- incorporated into the mixture. Recycling is already very
sively in road construction primarily because of its common in this industry; reclaimed asphalt shingles
greater changes in viscosity with temperature. Even more and/or reclaimed asphalt pavement may be in a formula-
confusing, in North America, the process to make roads tion as well. Because of variability in both binder and
from bitumen is very different than what is used for aggregate, testing in laboratory finished formulations is
asphalt. Bitumen roads are made by spraying bitumen, critical prior to application as a road. Major variables
then aggregate, then bitumen again. Asphalt roads are include viscosity of the binder with temperature, wetting
made by mixing the asphalt with the aggregate at ele- of the binder to the rock, and surface area (particle size)
vated temperatures, and then pouring out this composite of the rock. Table 1 lists the typical tests done on asphalt
onto the surface. Only asphalt roads are of interest in this concrete; note that the exact procedures used vary sub-
paper. stantially so only general guidelines are given. Of course,
If asphalt is the viscous form of petroleum, then the tests are done on both aggregate and asphalt binder indi-
term “asphalt roads” is imprecise because road material vidually, including size distribution for the former and
is mostly aggregate, with a small amount of asphalt. For viscosity versus temperature for the latter to help deter-
this review, the term asphalt binder (or just binder) will mine concrete composition and mixing temperature,
be used when referring to the liquid and asphalt concrete respectively. These tests will be discussed as appropriate
(or just concrete) the mixture of binder with aggregate. later in the manuscript. Also, Table 1 is not comprehen-
During the course of collecting information for this sive although every test that is referred to in this paper
review, the author found that if the term “asphalt” or does appear in this table.
“bitumen” is used alone in the title or abstract without Asphalt binder is usually mixed with aggregate at a
the terms binder or concrete, then the paper must be read facility far removed (miles to tens of miles) from the road
to determine whether the material studies was with or where the asphalt concrete is applied; the presumption is
without the aggregate. that little to no cooling occurs during transport.
GRADY 3

TABLE 1 Tests for asphalt concrete depends primarily on the temperature at which the com-
paction is done. The asphalt concrete is then left to solid-
Performance
Test Description property ify and is considered complete and ready for use when
the temperature reaches ambient temperature.
Stiffness Modulus is measured Deformation due
The composition of a hot-mix asphalt concrete
in compression or in to
deflection instantaneous (HMA) is as described above. HMAs may also
load include small amounts of additives; most commonly
Indirect A cylindrical specimen Failure due to interfacial agents to reduce viscosity via reduction in
tensile is stood on edge and instantaneous particle-particle friction as well as improving wetting
strength broken and the force load between rock and asphalt. The temperature of mixing is
(ITS) required to break is 150–180 C while compaction typically occurs 40 C less
measured than application temperature. Over the last 20 years or
Tensile ITS done after Failure due to so, warm-mix asphalt concretes (WMAs) have been
strength exposure to water instantaneous gaining significantly in market share. Mixing tempera-
ratio (TSR) and/or freeze/thaw load after tures used are lower, typically from 110–150 C. Formula-
cycles. The tensile absorption of
tions are more complicated because additives are needed
strength ratio is the water
so that the viscosity is low enough to apply the asphalt
ratio of the value
from the exposed concrete. Typical additives include waxes and interfacial
sample to the value agents. WMA also refers to foams, which involve
from the injecting water to make steam which also lowers the
measurement on the viscosity. The driving force for WMA processes are
sample prior to environmental because lower temperatures mean less
exposure emissions of organic materials to the atmosphere as well
Rutting A wheel runs over a Deformation due as less energy consumption to heat the asphalt binder
sample many times to cyclic load and aggregate. In addition, worker safety is improved
and rut depth after a
because of the lower exposure to emissions during appli-
certain number of
cation. From a plastics recycling perspective, the temper-
cycles is measured
ature at which the asphalt is mixed is critical because
Fatigue Load varies Weakening of the
this temperature will determine whether a specific plastic
sinusoidally on a ability to
sample, typically in withstand
melts during mixing.
on a beam in deformation
compression, until after
some modulus drop application of a 1.2 | Plastic waste composition
is reached, typically cyclic load
a drop of 50% The most important thermoplastic polymers are low-
density polyethylene (LDPE), linear-low-density polyeth-
ylene (LLDPE), high-density polyethylene (HDPE),
Regarding waste plastic that is a liquid at mixing temper- polypropylene (PP), polystyrene, polyvinyl chloride
ature; the introduction of the plastic can be done by (PVC), polyethylene terephthalate (PET), polyamide,
mixing with the binder (wet process) or the solid plastic polyurethane and acrylics (most commonly polymethyl
can be added with the aggregate (dry process). The for- methacrylate). Depending on the temperature at which
mer typically requires some process modification while asphalt is mixed and the composition of the polymer, the
the latter does not. Application has two steps, the first is polymer can become a high viscosity liquid or may
augering of the asphalt concrete onto the roadway at remain a solid. This difference is critically important in
some specified rate and the second is compaction, typi- studies of plastic waste in asphalt concrete for a variety of
cally with a steel roller, to remove trapped air from the reasons, including the importance of the polymer surface
asphalt concrete. The actual application temperature will and effect on binder viscosity. As can be concluded from
depend on the outside air temperature while, by chang- Figure 2, for an HMA about 70% of all plastic waste
ing the time between application and compaction, some would be a liquid, while for a WMA the percentage drops
control of compaction temperature is possible, although to 25%. Not surprisingly, 70% corresponds roughly to
typically compaction occurs immediately after applica- the fraction of papers that describe studies of plastics in
tion. The compaction step is extremely important for pro- asphalt concrete that involve plastics that melt during
ducing a long-lived asphalt concrete, which in turn mixing of binder with aggregate. The key failure of
4 GRADY

being fully soluble in the binder and the polystyrene


domains not soluble. These compounds increase fatigue
resistance because the polystyrene domains act as cross-
links and hence improve the flexibility of the binder.[15]
Reactive polymers, that is, acrylates, react with the
binder and improve the stiffness of the concrete. Reactive
copolymers can increase interfacial adhesion to a waste
polymer via reaction as will be discussed below.
The review is divided into three sections: cases where
the plastic is expected to melt in the binder during prepa-
ration, cases where the plastic is not expected to melt, and
a few cases where mixed feedstocks are used. In the discus-
sion below, rheological and mechanical properties are
F I G U R E 2 Adapted from Reference [1]. Temperature above described separately within each section. For the purposes
each bar is the approximate temperature at which the plastic will of this review, rheological refers only to measurements
become a melt. Polyurethane and polyamide have a range of made at temperatures and shear rates relevant for mixing,
temperatures ( ± 20 C). n/a means material will soften but never application, or compaction. Other rheological measure-
become a viscous liquid. Additives represents solids, colorants and
ments are correlated to mechanical performance and will
plasticizers that have been added. Data listed had PP and acrylic
be found in the mechanical or aging sections. The next
fiber listed as one entry so they were split in half for this chart
section starts with a fundamental description of what a
melted polymer will do in a binder since the final particle
plastics in asphalt concrete is poor interfacial adhesion size of the solid polymer that exists after cooling will be a
between the plastic and the asphalt binder and hence function of process that occur while the polymer is melted.
strategies that can be used for plastics that are not melts
(e.g. surface treatments) would be expected to be totally
ineffective for plastics that melt. Alternatively if the melt 2 | P L A S T I C TH A T ME L T S
can wet, or be made to wet, the aggregate, then having a DU R I N G M IX I N G
plastic that melts would be preferred.
Most studies do not use mixed waste streams, at least 2.1 | Droplet breakup and coalescence
partly because of the melt/solid issue. Obviously, there is
a significant economic benefit of being able to use a When a plastic is used that is a melt during mixing, drop-
mixed waste stream. Even more important perhaps is lets will form in the asphalt. To this author's knowledge,
that small amounts of impurities (pigments, food, oil, no plastic melt is soluble in the asphalt binder so the melt
grease) that are often part of any plastic waste stream are will form a separate phase in the liquid that will persist as
likely to not cause a problem with asphalt concrete the mixture cools. Because the viscosity of the polymer is
because their concentration will be too low. In this significantly higher than the viscosity of the asphalt binder
author's opinion, if a method can be developed that (e.g. the viscosity ratio is high), the asphalt should be
improves interfacial adhesion between the asphalt binder unable to disperse the polymer to any significant degree.
and the plastic, then this method will likely be effective The reason for this statement is described in the article by
for most post-consumer plastic waste streams without Stone[16]; for any pure shear flow with a viscosity ratio
significant cleanup of the waste stream. Because the tem- greater than 4 the drop rotates like a rigid body rather
perature at which the different components of a post- than stretches because of vorticity. A purely elongational
consumer plastic waste streams becomes a melt is not flow would be able to break up the drop irrespective of the
uniform suggests that some separation by type may be viscosity ratio; however, the elongational flow component
necessary. of typical asphalt mixers is not large.
Certain polymers are purposefully added to increase However, this simplified picture is misleading in that
mechanical properties of the asphalt concrete or change reductions in polymer droplet size do occur during
the interfacial interaction between the binder and the mixing. The polymer phase will be swollen significantly
aggregate; these polymers are not a subject of this review. by lower molecular weight species found in asphalt
However, those that are purposefully added do give some binder and hence the viscosity ratio is much smaller than
idea of how waste polymers might be viewed. Thermo- the ratios of pure polymer and pure binder. Depending
plastic elastomers, that is, styrene-butadiene-styrene on the polymer, the amount of asphalt contained in the
(SBS) terpolymers, phase separate with the butadiene polymer droplets can be many times the amount of
GRADY 5

polymer. Another consequence of extensive swelling is above the melting temperature of each material after
that the interfacial tension is small which also favors mixing, with the results reproduced in Figure 3. Each
droplet breakup; in one study with LDPE a value of particle grew substantially, to the point where the area
10−6 N/m was found at 180 C.[17] In fact, one study spe- fraction of the particles was much larger than the volume
cifically noted that a particular LLDPE had significantly fraction consistent with the 5 wt% added polymer. The
smaller drops during mixing versus HDPE and LDPE. authors concluded that swelling of the particles was
Because of the very small change in Hansen solubility occurring. Surprisingly, LLDPE showed a much smaller
parameters with branching, the authors attributed the growth in particle size than the other materials which
smaller drops in LLDPE due to a reduced melt elasticity could not be explained by the viscosity of the polymer
of the LLDPE versus the other PEs.[18] Another study since the melt flow index (MFI) was in the middle of the
noted that higher molecular weight LDPE (e.g. higher four polymers studied. Although crystallinities were not
melt elasticity) yielded larger drop sizes than its lower given, in general HDPE has the highest crystallinity so
molecular weight counterpart.[19] This result suggests crystallinity is likely not the cause of this difference even
that one way to improve properties of recycled plastics though crystalline regions will not swell. LDPE did have
that melt in asphalt is to reduce melt elasticity. Another the fastest increase in particle size; in this study this
way is suggested by increasing the elongational flow com- LDPE also had the highest MFI.[24] Another study, with
ponent of mixing; a study showed that rotor-stator mixers storage at 180 C, showed that LDPE also had more coa-
produce much better dispersions of various polymers in lescence than HDPE in binder.[25] As expected, func-
binder versus a stirred tank and the former have much tionalization of a non-reactive polymer with groups that
larger elongational flow components.[20] react with asphalt will slow coalescence.[26]
Coalescence is one reason restricting polymer loading
in binder because large inclusions will form if coales-
cence occurs. In fact, waste plastic bags (usually a mix- 2.2 | High temperature rheology of
ture of LDPE and LLDPE) have been shown to phase binder
separate from the binder into a separate layer at HMA
mix temperatures with no agitation.[21] Plastics com- The effect on the rheological properties of the asphalt with
monly found in post-consumer waste do not have any the addition of melted polymer is to increase the viscosity,
affinity for the aggregate and are not preferentially although at very high shear rates this difference is either
adsorbed on the aggregate surface. As stated previously, small or nonexistent. For example, the addition of only
the interface between the polymer particles and the 1 wt% of recycled HDPE to an asphalt binder raised the
highly viscous asphalt is weak and is considered the complex viscosity at low frequencies by more than an
source of the generally poor properties in measurements order of magnitude, while at a frequency of 103 s−1 the
sensitive to the interface as will be described below. viscosities were identical.[27] The shear rate during mixing
A smaller starting particle size prior to melting should is estimated to be 104–105 s−1 depending on equipment[28]
lead to smaller final particle size after melting. A dissipa- while that during compaction is 5 × 102 s−1.[29] The vis-
tive energy comparison using sinusoidal strains above the cosity during application is much lower. The conclusion
linear viscoelastic limit at room temperature was used to that mixing and compaction temperatures, and hence the
compare HDPE, LDPE and PP as fillers for asphalt binder viscosities at the shear rates relevant for these processes,
+ aggregate (at binder volume fractions much larger than are not affected by the addition of melted polymer has
typical) after high temperature high speed mixing, melting been made elsewhere as well.[30] However, another study
and cooling. LDPE had the best performance which was with recycled LDPE at a very large percentage (2:1 wt ratio
attributed to the particle size of the dispersed polymer of LDPE:binder) showed a  70% increase in torque at a
phase being significantly smaller.[22] Another approach to shear rate that was presumably quite high.[31] Weight per-
reduce coalescence is to reduce the temperature. WMA centages of HDPE between 2 and 6% showed that the elas-
allows lower mixing temperature, and in fact the polymer tic response increased more than the viscous response.[32]
might emulsify along with the binder if water is used. This The addition of agents or chemical modification of the
approach was used at low LDPE concentrations (4%) and polymer to promote bonding between a waste polymer
phase separation during storage at higher temperatures and the binder have been found to increase the viscosity
was reduced although this material was not used to make as expected.[33,34] Also, as measured by storage stability
an asphalt concrete.[23] Finally, the addition of reactive (which is related to drop coalescence), a study found that
groups can yield to smaller particle sizes.[19] there was an optimal mixing time between waste polyeth-
An interesting study examined the growth of various ylene packaging bags (typically a mixture of LDPE and
PE particles in asphalt binder at a temperature well LLDPE) and asphalt binder.[35]
6 GRADY

F I G U R E 3 Growth of polymer particle diameter with time in an asphalt binder at 163 C after mixing and cooling. MDPE is medium
density polyethylene. The y-axis in all plots is the percentage of particles with the mean diameter on the y-axis. Modified from
Reference [24]

135 C is a testing temperature for a viscosity test that concentration on viscosity at low shear.[39] Increasing the
is contained in a commonly used list of guidelines for temperature from below the melting temperature to
asphalt binder.[36] This temperature is near the solid– above the melting temperature at 2–5 wt% of filler for
liquid transition of many waste plastics; because of the HDPE and PP caused a reduction in viscosity difference
adsorption of low molecular weight binder components between filled and unfilled binder at low shear rates;
into the amorphous sections of the semicrystalline poly- however, the viscosity reduction was close to LDPE over
mers as well as possibly smaller crystallites that form the same concentration range which presumably did not
after mixing, the actual melting temperature has been go through that transition.[15]
measured to be 10 C less than the melting temperature
of the pure polymer when the polymer is melted and
then encapsulated in binder.[37,38] Not surprisingly, 2.3 | Mechanical properties of concrete
HDPE added to binder evaluated at a temperature
slightly above its melting point, for example, a WMA Overall, the addition of a polymer to a binder causes an
mixing temperature, shows a very strong effect of increase in binder stiffness, and related properties such
GRADY 7

as an increase in softening point and decrease in penetra- dry mixing.[41] A study comparing waste HDPE and PP
tion, which is not surprising since at the temperature of found that the former had 10% ITS improvement and
testing (typically between 25 and 80 C) the polymer will 17% TSR improvement at 4 wt% addition with none and
be a solid in the binder. There are many papers that have 8% for the latter with 3 wt% addition, respectively.[42] In
these or similar conclusions with respect to binder, and another case, ITS improved by 15% with 6% waste
the interested reader is referred to the review papers LDPE film addition while the TSR dropped from slightly
mentioned earlier. Since the increase in binder properties over 100% to 85%.[43] In another case, ITS did not
is of interest only in an indirect sense, this section will improve at 2 wt% for both HDPE and PP and improved
focus on properties of the concrete. Indirect tensile by 20% at 5 wt% polymer content.[44]
strength (ITS), tensile strength ratio (TSR), rutting tests Usually, the addition of plastic causes a rise in ITS up
and fatigue tests are tests used more-or-less universally to a certain amount, at which point the ITS begins to
on concretes and will be described below. Because the decrease. For example, adding LDPE increased the ITS
exact specifics of the test varies from state to state in by 20% up to 1 wt% LDPE; at 3% LDPE the ITS was 10%
the United States, and from country to country and the lower than the concrete with no LDPE.[31] Another study
values of the non-polymer containing concrete depend with waste LDPE found a maximum 20% improvement
on formulation, percentages rather than absolute values in ITS at 5 wt%; at 10 wt% the ITS was lower than the
will be used for most results below. Note that all percent- concrete without any plastic.[45] The addition of polypro-
ages of plastic added, unless otherwise noted, are weight pylene caused an increase in ITS by 15% at 2 wt% con-
percentages on a binder basis. tent; at 3 wt% the value dropped.[46] A study with very
high percentages (2, 4 and 6 wt% based on the mixture
weight, which corresponds to 30, 45 and 60 wt% on a
2.3.1 | ITSTSR binder basis) using both an HDPE/LDPE mix as well as
just PP showed 10–20% drops in ITS except for two data
The addition of a small amount of polymer causes an sets.[47] A study with 2 wt% waste polyethylene showed a
increase in both ITS and TSR typically. For example, a 50% increase in ITS while only a 20% increase was found
very small particle size (less than 100 nm average size) for 6 wt% virgin LDPE.[48] Figure 4 shows the type of
HDPE showed a  15% increase in ITS and an increase behavior that is common; an increase of ITS and TSR at
in TSR from 81 to 88% with 3 wt% HDPE addition.[30] low added fractions followed by a decrease above some
The value of the ITS was five times larger with 3 wt% fraction. This figure also confirms that the amount of
PP in one study without any change in the TSR.[40] A plastic required to show a decrease varies with formula-
comparison of HDPE and LDPE with four different rock tion and processing specifics.[49] Overall, TSR tends to
types consistently showed higher TSR for HDPE than qualitatively mirror the trends in ITS. These results are
LDPE at 9 wt% plastic with wet mixing outperforming consistent with the fact that the larger the inclusion, the

F I G U R E 4 Change in indirect tensile strength (ITS) (solid lines) and tensile strength ratio (dashed lines) with waste plastic
incorporation. Dark lines are dry mixed while light lines are wet mixed. Adapted from Reference [49]
8 GRADY

2.3.2 | Rutting

A commonly used specification for asphalt binder is the


ratio G*/sin δ measured at a frequency of 10 rad/sec,
where G* is the complex shear modulus and δ is the
phase angle. This parameter is correlated to the rutting
resistance and higher values of this parameter are
desired, that is, a higher modulus material with more
elasticity shows less rutting. The addition of virgin HDPE
of very small particle size (less than 100 nm) caused an
F I G U R E 5 Indirect tensile test results for unaged and aged increase in this parameter versus the base resin, with a
asphalt concrete samples made with 0.7 wt% (total mixture basis) corresponding improvement in the rutting resis-
polypropylene. Dark bars represent unaged samples while lighter tance.[30,54] Other studies of have found similar results
bars have been aged (aging reduced the ITS by about 25%). Aging for recycled LDPE[55,56] and LLDPE[57] The addition of
was done by holding the samples at elevated temperature in an
recycled HDPE along with crumb rubber from vehicle
oven and is meant to simulate aging during the first 5 years of
tires showed that the HDPE coated the rubber and
pavement life. Adapted from Reference [52]
improved G*/sin δ.[58] The addition of both has been
found to improve creep resistance, thought to be due to
more the ultimate properties of the concrete tend to the rubber, as well as rutting resistance.[59] Improve-
weaken (larger volume fractions will lead to larger inclu- ments in G*/sin δ were seen in another study using
sions because coalescence will occur more frequently recycled HDPE and crumb rubber as well which also
everything else being equal). Hence, the fraction where showed that a wax residue can help compatibility of these
this downturn in ITS and TSR occurs varies; not surpris- two waste materials in asphalt binder which was attrib-
ing since the final particle size will depend on the mixing uted to smaller particle sizes of the dispersed phase.[60]
procedures, the interfacial tension between the asphalt Desulfurizing the rubber was shown to improve this mea-
swollen particles and the asphalt, the viscosity of the surement in rubber mixtures with virgin LDPE, again
asphalt etc. attributed to better dispersion of the filler.[61]
Not surprisingly, higher temperatures tend to increase As noted elsewhere, the G*/sin δ parameter is not a
the percentage improvement in ITS with the addition of very good predictor of rutting performance. Another test
plastic, although of course the absolute value of ITS for asphalt binder, namely multiple stress creep recovery,
decreases as temperature increases. A very large increase has much better correlation.[62] In this test, a specific stress
in ITS of 47, 68, and 71% at 25, 35, and 45 C, respectively, is put on a sample at a given temperature, and the recov-
with 5 wt% waste LDPE was found for a porous asphalt ery is measured for a specified time interval that is con-
concrete ((produced using a much larger proportion of stant and then more stress is added and the recovery is
large aggregate and used in tropical regions with large measured etc. The Jnr, which is the permanent strain/
amounts of rainfall). A higher percentage increase in ITS stress (typically averaged over all 10 tests) is reported.
at 60 versus 25 C (50% vs. 20%) was also found at Improvements, that is reductions, in Jnr have been found
5 wt% HDPE addition with a marked decrease for both at for LDPE[63,64] and HDPE.[65,66] One study saw an increase
7 wt%; the TSR increased from 80 to 95% from 0 to 5 wt% in Jnr with the addition of LDPE which was attributed to a
and then fell to 87% at 7 wt% content.[50] In one case, the higher viscous part of the viscoelastic response.[67]
ITS was less for samples with a few percent added waste A more direct measure of rutting performance, that is
HDPE at low temperatures (5–20 C) while being higher the resistance of the road to undergo creep deformation
at higher temperatures; the TSR at room temperature due to tires running over the surface is the Hamburg
increased a few percent with added HDPE.[51] Similar wheel tracking test. In this test, a wheel with a specified
behavior for the ITS was found for PP-filled samples normal force passes over an asphalt concrete held a speci-
where the crossover temperature was 48 C.[52] fied temperature via immersion in a water bath. The tem-
A very interesting study[53] found that coating aggre- perature is specified by the category of mix used.
gate with polypropylene (heating the aggregate at 230 C Typically the deformation after a set number of passes
and then slowly adding crushed polypropylene to aggre- (typical values are a frequency of 1 Hz and 20,000 passes)
gate that is being mixed) does improve performance sig- is reported with a smaller deformation distance being
nificantly of the asphalt concrete as shown in Figure 5. better. Alternatively, the test is halted when some defor-
The concrete was mixed at 166 C so in all cases the PP mation is reached and the number of cycles required to
should melt. reach that deformation is reported. As expected from Jnr
GRADY 9

naturally occur, because mismatched thermal expansion


coefficients will yield tensile stresses in the system which
is the cause of interfacial debonding. With any failure
that is primarily driven by interfacial weakness, the key
mechanical test is one that has a tensile component.
Fatigue experiments (sinusoidal loadings) tend to accen-
tuate interfacial failures as well. The most common type
of test is a four point bend test. A detailed description of
the mechanics of this test are beyond the scope of this
review, however a tensile component occurs in the bot-
tom half of the sample and is maximum at the bottom
F I G U R E 6 Number of passes to reach 20 mm rutting depth in edge. The number of cycles required for a specific drop in
Hamburg wheel tracking test as a function of low-density modulus (typically 50%) is usually reported; clearly larger
polyethylene (LDPE) added to binder. Adapted from Reference [45] values are better. Again, because the absolute numbers
will depend strongly on sample and test conditions, per-
centage changes are reported.
results, improved rutting performance results with the In the case of three waste polyethylenes the number
addition of plastic; for example the addition of a small of cycles to failure was unchanged while both SBS copol-
particle size HDPE at 3 and 5 wt% loading levels led a ymer and crumb rubber increased the fatigue life.[32] In
decrease from 17 mm with no plastic to 10–5 mm, respec- one study, the number of cycles dropped by more than a
tively.[30] The reduction was much smaller but in the factor of 5 with 7% added HDPE.[73] 6 wt% waste LDPE
same direction for another study using waste HDPE at plastic dropped the number of cycles by 33% on both
similar loading levels.[51] A study with LDPE found a aged and unaged samples.[43] The addition of 0.5% waste
reduction from 15.7 mm to 3.4 mm with the addition of LDPE improved fatigue resistance by 25% with lime-
3 wt% polymer; increases to 6 and 9 wt% gave smaller stone aggregate in one case, while in the other with por-
improvements.[68] Large reductions were also found for phyry aggregate the fatigue resistance dropped by a factor
waste polyethylene film and LDPE.[48] Figure 6 shows of 3.[31] The fatigue life dropped by about 50% over a
the number of cycles required to reach a certain depth as range of initial strains for 2.5 wt% waste PE from bags at
a function of LDPE amount added to the binder in one 20, 30, and 40 C.[74] In one study, the fatigue life was a
study; such maximum are not as common as they are in few percent higher with the addition of 2 and 5 wt% PP
ITS results.[45] Two commercial materials made from a and HDPE.[44] Using both 7.5 wt% used motor oil and
proprietary mix of recycled plastics (one elastomeric, one 4 wt% HDPE improved fatigue resistance by about a fac-
plastomeric) show 50% reduction in rutting depth at tor of 5 versus a concrete without either of these, and by
conditions that produce a 10 mm rutting depth in the about a factor of 2 versus a concrete with only 5 wt% used
unmodified concrete and almost no change at conditions motor oil.[75] A factor of 5 increase in fatigue life was also
that produce a 2 mm rutting depth at 6 wt% plastic con- seen for 5 wt% PE from waste bags being added to a con-
tent.[69] Grafting groups that will react with the binder crete.[76] In a different study, a much smaller increase
improves rutting performance. For example, grafting 1% was found for 5 wt% of HDPE addition; about 16%
maleic anhydride onto waste polyethylene causes the improvement. However a wet sample showed a much
deformation to decrease by about a factor of 4 in a con- larger improvement with HDPE addition; about a factor
crete where the polyethylene was about 7 wt% of the of two.[66] A factor of two improvement was seen when
binder[70]; results on other polymers reactively modified adding both polyphosphoric acid and 4 wt% HDPE; the
with peroxides also show improvements in rutting resis- former can likely react with the HDPE.[15]
tance.[71] Finally, and perhaps most importantly, field
tests of asphalt concrete with 4.7 wt% waste PE bags
showed no wheel path cracking after 5 years while the 3 | PLASTICS THAT REMAINS
control section showed such cracking.[72] SOLID DURING MIXING

3.1 | High temperature rheology of


2.3.3 | Fatigue tests binder

Interfacial weakness between the polymer and the binder Dry mixing, that is, mixing of the polymer with the aggre-
will manifest itself in temperature variations that gate, versus wet mixing, that is, mixing with the binder
10 GRADY

prior to adding aggregate, should make little to no differ-


ence in terms of performance for polymers that remain
solid during mixing, unless the polymer is combined with
the aggregate at an aggregate temperature above the
melting point of the polymer.[77] The addition of a few
percent of a polymer solid also will likely not have any
appreciable influence on the viscosity at the high shear
rates involved in mixing and compaction. Viscosity mea-
surements at low temperatures and low shear rates how-
ever showed a factor of 4 increase with 10 wt% recycled
PET at a testing temperature of 135 C,[78] a factor of 3,
4 and 5, respectively, at 5, 10 and 15 wt% PET at 135 C
and very little at 163 C.[79] In one study, the viscosity
shows a slight minimum at 12 wt% PET; this result is
likely due to the fact that the PET was melted prior to
adding the PET to the binder.[77] The zero-shear viscosity
for 11 wt% PVC in binder between 0 and 55 C was orders
of magnitude larger than that of pure binder.[80] Again,
however, the high shear rates relevant during mixing
means that good coating of the aggregate should not be
affected by the addition of a solid polymer to the binder,
although the amount of binder may need to be adjusted
to account for the fact that the binder contains a solid
that will obviously not wet the aggregate.

F I G U R E 7 Variation in ITS (% basis) (top) and variation in ITS


3.2 | Mechanical properties of concrete and TSR as a function of PET added to binder. Top: Adapted from
Reference [81] top. Bottom: Adapted from Reference [82]

The same statements made in Section 2.3 apply here; the


addition of a solid polymer to a binder causes an increase
in stiffness, and related properties such as an increase in the introduction of 2 wt% PET.[84] Interestingly in
softening point and decrease in penetration. Also, this another study, with more air voids the addition of PET
section will focus on properties of the concrete: ITS, TSR, showed an optimal amount at 2 wt% which corresponded
rutting tests and fatigue. Finally, all percentages of plastic to an increase of 33% in ITS for a smaller PET particle
added, unless otherwise noted, are weight percentages on size (0.3–0.6 mm) and  10% for a larger PET particle
a binder basis. size (1–2 mm). TSR showed a maximum at the same wt
% and was again lower for the larger particle size (83%
and 75%, respectively, vs. 68% for the control) With less
3.2.1 | ITS/TSR voids, the asphalt concrete without any PET had the
highest ITS, with again the finer particle size having
Shown in Figure 7 are the results from studies using vari- higher ITS than the smaller particle size.[85] A small
ous contents of waste PET that had been cut up into amount (0.4 wt%) of polyamide 6–10 added to a binder
small pieces (top)[81] and waste PET washed and mix that also contained SBS improved the fatigue life by
reextruded (bottom)[82] before addition to the binder. The a few percent.[86] The addition of 5 and 10% PVC powder
same correspondence noticed earlier with there being an increased the ITS by 10% along with an increase of TSR
optimal amount of polymer for maximum ITS was seen from 81% to 87% with little difference between the
with both papers, and the latter also showed that ITS and two loading levels.[87] In another study with PVC in a
TSR are correlated with one another as well. In another porous asphalt concrete at 2 wt% loading there was no
study, with 10% PET added, the ITS increased by 10% but change in ITS but at 4 wt% loading the ITS dropped
the TSR dropped from 0.85 to 0.7.[83] A different study by 25%.[88]
that also used 10% PET in binder caused an increase in One possibility would be to form the waste plastic
TSR from 72% to over 90%.[78] ITS for a porous asphalt into fibers if not already in that form. Whether fiber ori-
concrete was improved significantly (a factor of 3) with entation occurs during application of a fiber in a road has
GRADY 11

not been determined to this author's knowledge; what 2.0


direction orientation should occur to maximize road lon- 1.8
1.6

Rut Depth (mm)


gevity has also not been determined. At loadings of 0.5
1.4
and 1 vol% of the concrete (on a per asphalt basis that 1.2
corresponds to roughly 5 and 10 wt%) the increase in ITS 1.0
was about 2.5% and 5% for samples containing PET fibers 0.8
and 0% and 10% for samples containing polyamide fibers. 0.6
0.4
TSRs increased from 80% for the sample without fiber to 0.2
84% for the sample with fiber for both polyamide and 0.0
PET.[89] The addition of polyamide 6–10 fibers at weight 0 2 4 6 8 10
wt % PET
fractions between 0.5 and 2 wt% on a total mix basis
(roughly 5–20% on a binder basis) caused an increase of
F I G U R E 8 Variation in rut depth in rutting test. Adapted from
about 15% in ITS at the optimal content of 1 wt% on a Reference [96]
total mix basis. An optimal TSR was also found at the
same fiber content which corresponded to a change from
81% to 88%.[90] A study on recycled carpet fabrics found percentages was much less significant than the reduction
that the critical pullout length (e.g where the mode of in ITS shown in Figure 7.[82] As shown in Figure 8, an
failure changed from interfacial failure to fiber breakage) optimal amount of PET added was found at 4 wt% in
from binder was 9.2 mm for a particular fiber; however another study.[96] In another case, PET was added to the
the addition of these fibers at 0.25–1 vol% on a total aggregate at concentrations from 0.1 to 1.1 wt% (on an
aggregate basis (approximately 1.5–6 wt% on a binder aggregate weight percent basis; the equivalent basis on a
basis) decreased the ITS by about 15% at the maximum binder basis is 2 to 22 wt%) and the sample with 0.5 wt
loading with no consistent differences between 6 and % on an aggregate basis was found to have the optimal
12 mm fibers.[91] rutting resistance improvement, from 9 to 6 mm.[97] As
was found with ITS and TSR as described above, a maxi-
mum in rutting resistance was found for addition of 1 wt
3.2.2 | Rutting % on a total weight basis of polyamide fiber.[90]

As with melts, there are some studies that look at asphalt


binder. An asphalt binder showed significant desirable 3.2.3 | Fatigue tests
increases in G*/sin δ and reductions in Jnr at temperatures
between 58 and 76 C with the addition of PET[92] A mono- Overall, data for plastics that do not melt during mixing
tonic increase in G*/sin δ was found with PET addition up is not as negative as for plastics that do melt during
to 15 wt%[79] and PVC addition up to 5 wt% PVC.[93] How- processing, although as mentioned previously the
ever, an optimum at 2 wt% was found in another study for amount of data for the former case is about a factor of
PVC addition with respect to G*/sin δ.[94] 3 less than the amount of data for the latter case. An
With respect to the concrete, some studies show a increase in fatigue life by a factor  10 occurred in one
monotonic improvement in rutting resistance with added case where 10 wt% waste PET was added to asphalt con-
solid plastic. A reduction from 5 to 0.5 mm was found with crete.[78] Roughly a half order of magnitude increase in
the addition of 14% waste PET material.[77] A similar study the number of cycles to failure occurred with the addition
at high percentages of PET (0.25% to 1 wt% on an aggre- of waste PET that had been cut into small pieces.[98]
gate basis, which roughly corresponds to 5–20 wt% on a Almost no change in fatigue life occurred at both 5 and
binder basis) showed a monotonic decrease in rutting 20 C for levels of PET added from 0 to 10%.[81] A mono-
depth with PET added amount. However, three particle tonic increase in fatigue life with the addition of PET
sizes were tested; for the two larger particle sizes, the rut- from 0.2 to 1 wt% on an aggregate basis (approximately
ting depth for the sample with 0.25 wt% on an aggregate 4–20 wt% on a binder basis) was found in another study
wt% basis was higher than the sample with no PET.[95] at three different microstrains; the increase at the highest
Again, most studies show a maximum improvement loading level averaged about a factor of 2 although the
at some intermediate added plastic amount. An optimal increase was only about a factor of 1.5 at the highest
amount of 7.5 wt% added PET for minimum rutting was strain.[99] A study that used design of experiments meth-
also found in the same study corresponding to the bottom odology that probed PET content from 0–1 wt% on an
part of Figure 7, i.e. the same weight fraction as the maxi- aggregate basis (approximately 0–20 wt% on a binder
mum in ITS. However, the increase in rutting at higher basis) along with temperature and strain found that PET
12 GRADY

the polymer to allow the HDPE to melt. The particle size


did not have a significant effect, except in the
preheating step.[103] A truly mixed waste, i.e. one that
was gathered from a municipal waste recycle facility
with no sorting, has been studied. With adding the
mixed waste to the aggregate, the ITS decreased by 5%
for a larger particle size and 40% for a smaller particle
size at 10 wt% (although at 20 wt% for the latter, the
ITS was 15% higher) Compared to the concrete without
plastic, the TSR was higher for the smaller particle size
and smaller for the higher particle size. The fatigue life
increased by as much as an order of magnitude with
the smaller particle size mixed waste at 9.5 wt%; how-
ever, the slope with the amount of strain was much
more steep meaning at very low applied strains the
two overlapped. This paper also concluded that mixing
some of the mixed waste with the binder and some
with the aggregate may yield the best results.[104]
Another strategy to mix waste plastics into asphalt
binder is to depolymerize or degrade the polymer into a
liquid first. PET was first chemically depolymerized using
ethanolamine and the resultant product was bis
(2-hydroxy ethylene) terephthalamide (BHETA). This
F I G U R E 9 Cycles to failure as a function of PET added to small molecule seemed to be soluble in the binder,
concrete with top representing 1 cm fibers and the bottom 2 cm i.e. the viscosity of the binder decreased. The addition of
fibers. Legend refers to strain and are in units of microstrain. various percentages to a binder containing 10 wt% crumb
Adapted from Reference [101] rubber increased G*/sin δ and, consistent with this result,
reduced Jnr as well.[105] Better performance in various
measurements was found when the terminal groups were
content over this range increased the fatigue life only amines instead of hydroxyls in BHETA indicating that
slightly, about 40% increase at the highest content stud- the identity of the terminal groups are important likely
ied.[100] Figure 9 shows the change in fatigue life as a because of the more facile reactivity of amines.[106] A sim-
function of PET fiber length and strain for the fatigue ilar approach, except in this case using glycolysis via pro-
test. Longer fibers tend to help more, and there does pylene glycol, was used as well. In this case, the reaction
seem to be an optimum that varies with strain and fiber was complete in one case and only 50% complete in the
length.[101] A study with polyamide fibers from between other. In both cases, the viscosity decreased and various
0.1 and 0.4 wt% on a mixture basis (roughly 2–5 wt% on a low temperature properties were improved. Most inter-
binder basis) showed that a monotonic increase in fatigue estingly perhaps, with enough of either material the vis-
life occurred with addition of the fibers, from 6000 cycles cosity was lowered enough so that WMA-type procedures
with no fibers to 7600 at the highest concentration of were possible without the addition of any other agent to
added fibers.[102] A study with PVC found a slight reduce binder viscosity.[107] Reacting BHETA with a
improvement in fatigue life of the binder at low strains diisocyanate in situ in the binder yielded a performance
while a more significant reduction at high strains.[87] similar to that found with SBS terpolymers, which is not
surprising since both belong to the broader polymeric
category of thermoplastic elastomers.[108]
4 | OTHER STRATEGIES Waste tire rubber and various polymers (HDPE,[73,109]
LDPE and LLDPE,[110] EPDM and HDPE,[111] PET[92,105,112]
Studies with mixed plastics are limited where at least one have been examined extensively. As the addition of
will melt during mixing of binder and aggregate and the rubber is beyond the scope of this review a detailed
other(s) will not. In one case, a mixture of HDPE, PVC description will not be provided, however the effect is as
and PET was used with the ITS increasing with a small one would expect in terms of increasing resilience. As
(2%) reduction in tensile strength ratio. The authors noted detailed previously, the addition of polymer improves
the importance of premixing the heated aggregate with mechanical properties except those related to fatigue. No
GRADY 13

interaction between these non-reactive polymers and the Surprisingly, very little has been done on chemically
rubber has been found. modifying the surface of a solid plastic to enhance com-
In one unique idea, layering polyethylene sheets patibility with asphalt, unlike the case of melts where
made from waste polymer between layers of asphalt will chemical modification has been studied. Alternatively, as
reduce crack propagation through the concrete.[113] noted in the manuscript, only one group has tried to
replace enough asphalt binder with a low viscosity degra-
dation product to allow for WMA conditions to be used;
5 | O V E R A LL SU M M A R Y one would expect that this might be a way to both replace
asphalt binder as noted above as well as improve the
Addition of plastic, whether they melt or not, increase environmental footprint of the laying of concrete in road
properties related to stiffness. For plastics that melt, construction.
oftentimes the amount of asphalt can be reduced which
causes a higher solids content at use temperature. Tensile DATA AVAILABILITY STATEMENT
strengths also typically increase, but in most cases, there No data are available as this is a review article
is an optimal amount of plastic to add which is on the
order of 10% of the binder content or 1% of the total mix. ORCID
The fact that an optimal amount exists is due to poor Brian P. Grady https://orcid.org/0000-0002-4975-8029
interfacial adhesion between the plastic and the binder.
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