polymers

Article
Analysis of the Influence of Production Method, Plastic Content
on the Basic Performance of Waste Plastic Modified Asphalt
Haibin Li 1, * , Lichang Zhou 1 , Jianmei Sun 1 , Sirui Wang 2 , Mingming Zhang 1 , Yihong Hu 1
and Ahmed Abdulakeem Temitope 3

1 School of Architecture and Civil Engineering, Xi’an University of Science and Technology, Xi’an 710054, China
2 Shaanxi Transportation Holding Group Co., Ltd., Xi’an 710064, China
3 School of Material Science and Engineering, Chang’an University, Xi’an 710064, China
* Correspondence: [email protected]

Abstract: The sustainable reuse of waste plastic as an alternative construction material has numerous
environmental and economic advantages. New opportunities to recycle waste plastic in asphalt for
road construction would mitigate landfill issues and significantly reduce global carbon emissions.
With a clear aim to contribute to a more efficient reuse of waste plastic, this paper reutilized two
types of waste plastic (polypropylene (PP) and polyethylene (PE)) as asphalt modifiers to improve
the performance of asphalt pavement as well as to achieve the purpose of sustainable recycling waste
plastic. Therefore, the optimal preparation parameters of plastic-modified asphalt were recommended
by the orthogonal test. Then, the dispersion and modification mechanisms of plastic particles in
plastic-modified asphalt were further studied by Fourier Transform Infrared Spectroscopy (FTIR) and
Thermogravimetric Differential Scanning Calorimetry (TG-DSC). The results show that the asphalt
containing PP and PE shows better overall performance at high temperatures compared with the base
Citation: Li, H.; Zhou, L.; Sun, J.; asphalt. Furthermore, PE-modified asphalt and PP-modified asphalt exhibited optimal properties
Wang, S.; Zhang, M.; Hu, Y.;
when prepared at 3000 rpm for 30 min at 170 ◦ C. Moreover, the results of the expansion mechanism
Temitope, A.A. Analysis of the
show that the main reaction process of plastic asphalt is a physical change. Finally, PP-modified
Influence of Production Method,
asphalt and PE-modified asphalt generally perform well and are suitable for high-temperature
Plastic Content on the Basic
Performance of Waste Plastic
areas. Consequentially, the results of this research promote the recycling of waste plastic, ultimately
Modified Asphalt. Polymers 2022, 14, advocating the recycling of waste materials and environmental protection of pavement construction.
4350. https://doi.org/10.3390/
polym14204350 Keywords: road engineering; waste plastic; polypropylene (PP); polyethylene (PE); modified asphalt;
basic performance; mechanism analysis; SBS modified asphalt
Academic Editor: Victor
Tcherdyntsev

Received: 24 September 2022

Accepted: 12 October 2022 1. Introduction
Published: 15 October 2022
Asphalt pavement is widely used for its smooth surface and driving comfort. However,
Publisher’s Note: MDPI stays neutral with the high temperature in southern and western China in summer, as well as the sudden
with regard to jurisdictional claims in increase in traffic volume, heavy overload, and drainage traffic, asphalt pavement defects
published maps and institutional affil- are becoming more and more prominent [1]. The properties of base asphalt are not so good
iations. that the road asphalt maintenance budget every year exceeds the budgetary allocation for
new asphalt pavement construction. It has become clear that these base asphalt pavements
are incapable of meeting the high-temperature stability, low-temperature crack resistance,
anti-aging, and durability requirements of modern transportation. Therefore, it is necessary
Copyright: © 2022 by the authors.
to choose a more effective, more economic, and simpler asphalt modifier to improve its
Licensee MDPI, Basel, Switzerland.
performance [2].
This article is an open access article
The production and usage of plastic products have made great contributions to almost
distributed under the terms and
all different industries as well as exacerbating the waste of resources and increasing pollu-
conditions of the Creative Commons
tion worldwide. The management of waste plastic remains a global challenge for developed
Attribution (CC BY) license (https://
and developing countries alike. Plastic pollution, also known as “white pollution”, causes
creativecommons.org/licenses/by/
4.0/).
crop yield reduction, animal deaths, and land occupation, which affect sustainable land

Polymers 2022, 14, 4350. https://doi.org/10.3390/polym14204350 https://www.mdpi.com/journal/polymers

Polymers 2022, 14, 4350 2 of 19

use. China, the world’s largest consumer of plastics, is facing a huge challenge now. More
than 63 million tons of plastic had been produced in this country by 1.4 billion people in
2021 alone; the recycling rate is only about 30%, which results in the filling of landfills at an
alarming rate [3]. Efficient and economical approaches to dealing with these waste plastics
have been urgently needed. Currently, attention to the field of waste recycling has continu-
ously increased. Waste plastic is one of the most popular types. The successful application
of recycled plastic would significantly reduce plastic pollution, improve efficiency in the
utilization of resources, and decrease the carbon footprint. Additionally, it is an effective
way to reduce production costs.
As high molecular polymers, plastics are generally divided into thermosetting plastic
and thermoplastic. The physical and chemical properties of plastic are stable and can
be used for the modification of base asphalt. Due to the stable physical and chemical
properties of plastic, the usage of waste plastic, such as polyethylene (PE) [4–6], high-
density polyethylene (HDPE) [7], low-density polyethylene (LDPE) [7], polypropylene
(PP) [8–10], ethylene-vinyl acetate (EVA) [11], polyvinyl chloride (PVC) [12], polyethylene
terephthalate (PET) [13,14], and polystyrene (PS) to improve the performance of asphalt
is one of the research hotspots in road engineering. Many factors including construction
ability, availability, cost, and expected performance are important in the choice of modifier
for asphalt. Therefore, from an environmental and economic point of view, the use of
recycled waste plastic materials instead of raw materials could have several advantages
such as help easing landfill pressures and reducing demands of extraction from quarries
and other natural sources.
The application of recycled waste plastic-modified asphalt, whether it is EVA, PP, or PE-
modified asphalt, will effectively change the structure of raw asphalt collage and form new
collage structures, thus improving the high-temperature resistance, moisture susceptibility,
and other properties of the asphalt mixture, and furthermore improving the pavement
quality, saving maintenance costs, and extending the service life of asphalt pavement.
Modarres and Hamedi [13] applied shredded PET fine particles to asphalt mixes and
the results showed that PET particles improved the fatigue behavior and stiffness of the
asphalt mixes. Xu et al. [14] found that the overall properties of rubber asphalt could
be improved by the application of chemically recycling waste PET. Jianmin Ma et al. [7]
analyzed the effects of four typical recycled plastics (including HDPE, LDPE, PP, and PS)
on the performance of asphalt, it was found that high-temperature binder grades improved
while low-temperature grades were relatively unaffected. Plastics increase strength but
reduce strain tolerance in ductile failure. So, the study proposed that only binder course
layers should be modified to prevent undue risk for premature and excessive surface
cracking. Dalhat and Al-Abdul Wahhab [9] reported that following extensive research,
PP and PE significantly improved the rutting and fatigue performance as well as the
resilient modulus (MR) of base asphalt. Hınıslıoğlu and Ağar [15] concluded that for
optimum Marshall stability, flow, and Marshall quotient (MQ), 4% PE should be mixed
with base asphalt at 165 ◦ C for 30 min. PE existed in many variations; Ho, et al. [16] found
that PE with lower molecular weight and wider molecular weight distribution were more
suitable materials for asphalt modification. Through exhaustive research, Costa et al. [17,18]
confirmed the superiority of EVA and PE-modified asphalt over base asphalt. Köfteci [19]
proved that 4% PE material content gave modified asphalt better stability values than base
asphalt. Martin-Alfonso, et al. [20] indicated that PE considerably improved the viscoelastic
properties as well as water sensitivity and fatigue resistance of ordinary base asphalt.
Abed and Bahia [21] also noted that PE obviously improved the penetration grade as well
as the strength properties of base asphalt, when compared with an unmodified asphalt
mixture. Khurshid, et al. [22] found that PE-modified asphalt had better stability, rutting
resistance, and load-bearing capacity when used in asphalt mixtures. In other research,
Mansourian, et al. [23] reported better low-temperature properties and rutting resistance in
asphalt following EVA and PE dosing.
 Polymers 2022, 14, 4350 3 of 19

Although there are many studies on using waste plastic as asphalt modifiers, few of
them consider the climatic factors of the used areas. Problems caused by high temperatures
in combination with high traffic volume and heavy loads remain to be solved. On the other
hand, improper disposal of waste plastic causes harm to water bodies and soil, and there-
fore, rationally, it must be used in order to realize its sustainable development. Thus, the
objective of this paper is to comprehensively study the reutilization of waste plastic (PP and
PE) in asphalt and to improve the performance of asphalt in high-temperature areas. The
optimal preparation parameters of plastic-modified asphalt are recommended by orthogo-
nal test. Then, the dispersion and modification mechanism of plastic in modified asphalt is
further studied by Fourier Transform Infrared Spectroscopy (FTIR) and Thermogravimetric
Differential Scanning Calorimetry (TG-DSC). The evaluation of plastic-modified asphalt
will enable further enhancement of the performance of the pavement. This would also
bring new knowledge to the construction materials industry to develop new products for
different environments and accelerate the reuse of waste resources.

2. Materials and Methods

2.1. Materials
2.1.1. Asphalt
This paper selected the South Korean 90# (SK-90#) base asphalt to prepare the modified
asphalts. The basic performance indexes of the SK-90# asphalt were shown in Table 1.

Table 1. Basic performance indexes of SK-90# asphalt.

Specification
Test Unit Measured Value
Requirement
Penetration (25 ◦ C, 100 g, 5 s) 0.1 mm 85 80~100
Ductility (5 cm/min, 15 ◦ C) cm >100 >100
Softening point ◦C 48.3 >45
Density (15 ◦ C) g/cm3 1.030
Aging Quality change % 0.120 ≤±0.8
(TFOT) test Residual penetration % 73.6 ≥57
(163 ◦ C, 5 h) Residual ductility cm 11.7 ≥8

2.1.2. Plastic
Polymers 2022, 14, x FOR PEER REVIEW In this paper, two different kinds of waste plastic (PE and PP) were selected which had
a large consumption at present. The corresponding physical appearances were shown in
Figure 1, and the physical and chemical indexes were shown in Tables 2 and 3, respectively.

(a) (b)
Appearances
Figure 1.1.
Figure of recycled
Appearances PE pelletsPE
of recycled andpellets
PP pellets.
and (a) PP
PE pellets (b) PP
pellets. (a)pellets.
PE pellets (b) PP pel
Table 2. Basic indicators of recycled PE pellets.
Table 2. Basic−3indicators of recycled
◦ PE pellets.
Density/g·cm Melting Point/ C Melt Rate/g·10 min−1 Elongation Break Rate/%
0.91~0.92 cm−3
Density/g· 43Melting 0.2~5.0
Point/° C 20~800
Melt Rate/g·10 min−1 Elongation
0.91~0.92 43 0.2~5.0 20

Table 3. Basic indicators of recycled PP pellets.

 Figure 1. Appearances of recycled PE pellets and PP pellets. (a) PE pellets (b) PP pellets.

Table 2. Basic indicators of recycled PE pellets.

Density/g·cm−3 Melting Point/°C Melt Rate/g·10 min−1 Elongation Break Rate/%

Polymers 2022, 14, 4350 0.91~0.92 43 0.2~5.0 20~8004 of 19

Table 3. Basic indicators of recycled PP pellets.

Table 3. Basic indicators
Density/g· cmof−3 recycled PP pellets.
Melting Point/°C Elongation Break Rate/%
0.90~0.91
Density/g ·cm−3 Melting 135~159
Point/◦ C 150~600
Elongation Break Rate/%
0.90~0.91 135~159 150~600
2.1.3. Preparation of Plastic Modified Asphalt
2.1.3.According
Preparationtoofthe preparation
Plastic Modifiedprocess
Asphaltand relevant technical specifications of modi-
fied asphalt, the plastic content, shearing time, shearing temperature, and shearing speed
According to the preparation process and relevant technical specifications of modified
were selected as key parameters in the preparation process of plastic-modified asphalt
asphalt, the plastic content, shearing time, shearing temperature, and shearing speed were
[24]. Theas
selected specific preparation
key parameters process
in the is as follows:
preparation process of plastic-modified asphalt [24]. The
specific preparation process is as follows:asphalt was heated to 165 °C ± 5 °C until it turned
As is shown in Figure 2, the base
into liquid. Then,inaccording
As is shown to the
Figure 2, the baseresearch
asphalt [25,26], the appropriate
was heated to 165 ◦ C ± 5amount
◦ C until of PE (0, 2%,
it turned
4%,
into6%, 8%)Then,
liquid. and PP (0, 2%, 4%,
according 6%,research
to the 8%, 10%, 12%) the
[25,26], wasappropriate
predetermined to add
amount into
of PE (0,the
2%,base
asphalt.
4%, 6%, 8%)Nineandgroups
PP (0,of specimens
2%, 4%, 6%, 8%,with no12%)
10%, less than three specimens
was predetermined in each
to add into group
the basewere
prepared
asphalt. Nine under different
groups shearingwith
of specimens timesno(30
lessmin,
than60 min,specimens
three 90 min), shearing temperatures
in each group were
prepared
(170 °C, 180 under
°C, different shearing
190 °C), and timesrates
shearing (30 min,
(300060r/min,
min, 90 min),
4000 shearing
r/min, 5000 temperatures
r/min).
(170 ◦ C, 180 ◦ C, 190 ◦ C), and shearing rates (3000 r/min, 4000 r/min, 5000 r/min).

Figure 2.
Figure Preparation of
2. Preparation ofplastic-modified
plastic-modifiedasphalt.
asphalt.

In this study, SBS-modified asphalt was simultaneously prepared for comparative

In this study, SBS-modified asphalt was simultaneously prepared for comparative
analysis of plastic-modified asphalt. The mixing time was 45 min, and the temperature
analysis of plastic-modified asphalt. The mixing time was 45 min, and the temperature
was limited to 175 ± 5 ◦ C. A shearing rate of 3000 r/min was adopted. SBS content was
was limited to 175 ± 5 °C. A
maintained at 5% by weight, the shearing rate
standard of 3000
value r/min on
was based was adopted.
Standard SBS
Test contentofwas
Methods
maintained at 5% by weight, the standard value was based on Standard
Bitumen and Bituminous Mixtures for Highway Engineering (JTG E20-2011). Test Methods of
Bitumen and Bituminous Mixtures for Highway Engineering (JTG E20-2011).
2.2. Experimental Methods
2.2. Experimental
2.2.1. OrthogonalMethods
Test
2.2.1.To optimize the
Orthogonal Testcomposition of plastic-modified asphalt, an orthogonal test was
adopted in this study. Penetration, softening point, and viscosity were selected as the
To optimize the composition of plastic-modified asphalt, an orthogonal test was
main indicators to measure the basic physical properties of plastic-modified asphalt. The
adopted in this study. Penetration, softening point, and viscosity were selected as the
parameters (shearing time, shearing temperature, and shearing rate) were taken as control
factors that affected the properties of plastic-modified asphalt. After the preliminary test of
the research team, different shearing times (30 min, 60 min, 90 min), shearing temperatures
(170 ◦ C, 180 ◦ C, 190 ◦ C), and shearing rates (3000 r/min, 4000 r/min, 5000 r/min) in the
preparation process of plastic modified asphalt were taken as cross-testing to explore the
law and influence of various factors of plastic modified asphalt. The orthogonal test scheme
is shown in Table 4.
Polymers 2022, 14, 4350 5 of 19

Table 4. Orthogonal test design table.

Tests Shearing Time/min Shearing Temperature/◦ C Shearing Rate/r·min−1

l 30 170 3000
2 30 180 4000
3 30 190 5000
4 60 170 4000
5 60 180 5000
6 60 190 3000
7 90 170 5000
8 90 180 3000
9 90 190 4000

2.2.2. Physical Property Tests

According to the test methods T0604-2011, T0606-2011, T0625-2011, and T0605-2011 in
the JTG E20-2011, the penetration, softening point, viscosity, and ductility tests of plastic-
modified asphalt were carried out.
1. Penetration refers to the vertical penetration distance of a standard needle under
constant load (100 g) for 5 s at a temperature of 25 ◦ C. It is measured in 0.1 mm units
and is used to assess the hardness of asphalt.
2. The softening point is the average value of the temperature. The steel ball passes
through the asphalt plate and falls from a height. When the steel ball just touches the
bottom plate at a specified distance, the water temperature at this time is the softening
point of the asphalt.
3. The 135 ◦ C viscosity is a basic characteristic that reflects the frictional resistance
between the internal molecules of asphalt during flow deformation.
4. The 5 ◦ C ductility refers to the length at which the prepared sample is stretched at a
certain temperature and a certain speed to break.

2.2.3. Fourier Transform Infrared Spectroscopy (FTIR)

FTIR belongs to the molecular absorption spectrum, which is widely used in the
qualitative and quantitative analysis of organic materials [27]. In order to verify the effect
of plastic from the microscopic point of view, the functional groups of the plastic-modified
asphalt and base asphalt were observed and tested by an infrared spectrometer. The FTIR
(Nicolet Is10 Fourier Transform Infrared Spectrometer produced by Thermo Scientific,
Madison, WI, United States) was used to determine the different functional groups of
plastic and plastic-modified asphalt in wave numbers ranging from 4000 cm−1 to 500 cm−1 .
The samples were cut into small pieces and placed in the IR cell.

2.2.4. Thermogravimetric Differential Scanning Calorimetry (TG-DSC)

The thermal stability of plastic-modified asphalt was analyzed by thermogravimetric
analysis (TG) and differential scanning calorimetry (DSC). There are mainly two technolo-
gies used in this test, differential scanning calorimetry, and thermogravimetric analysis,
which can detect the physical changes and chemical reactions of the samples in the ex-
perimental process. The comprehensive heat analytical instrument was used to analyze
the base asphalt and the plastic-modified asphalt. The heating rate and nitrogen flow rate
of the test were set to 10 ◦ C/min and 20 mL/min, respectively, and the temperature was
continuously increased to 800 ◦ C.

3. Results and Discussion

3.1. Orthogonal Test Analysis
3.1.1. Optimal Preparation Parameters of PE Modified Asphalt
According to the orthogonal test in Table 4, a total of nine groups of orthogonal tests
were carried out, and the results were shown in Table 5. The variance analysis results of
the orthogonal test were listed in Tables 6–8. In order to better analyze the orthogonal test
Polymers 2022, 14, 4350 6 of 19

results, the sum of factor test results K and extreme difference R is proposed to describe the
data. Ki is the sum of values, and column-level number is i. In addition, the variance of
the three levels is R (extreme difference) which is used to quantify the influencing degree
of factors to the test index. The larger of R value, the greater impact of the factor on the
test parameter.

Table 5. Properties of PE-modified asphalt.

Factor Softening Point/ ◦ C 25 ◦ C Penetration/0.1 mm 135 ◦ C Viscosity/Pa·s

Test l 65.1 47.0 0.618
Test 2 61.9 47.3 0.609
Test 3 63.6 46.4 0.628
Test 4 63.3 47.5 0.606
Test 5 62.9 47.3 0.612
Test 6 62.6 48.4 0.600
Test 7 62.5 47.2 0.617
Test 8 61.6 49.3 0.594
Test 9 63.1 47.4 0.609

Table 6. PE Calculation results of softening point test R and K values of PE modified asphalt.

Shear
Factor Shear Time/min Shear Rate/r·min−1 Softening Point/◦ C
Temperature/◦ C
Test l 30 170 3000 65.1
Test 2 30 180 4000 61.9
Test 3 30 190 5000 63.5
Test 4 60 170 4000 63.3
Test 5 60 180 5000 62.9
Test 6 60 190 3000 62.6
Test 7 90 170 5000 62.5
Test 8 90 180 3000 61.6
Test 9 90 190 4000 63.1
K1 190.5 190.9 189.3 /
K2 188.8 186.4 188.3 /
K3 187.2 189.2 188.9 /
R 3.3 4.5 1.0 /

Table 7. Calculation results of penetration test R and K values of PE modified asphalt.

Shear 25 ◦ C
Factor Shear Time/min Shear Rate/r·min−1
Temperature/◦ C Penetration/0.1 mm
Test l 30 170 3000 47.0
Test 2 30 180 4000 47.3
Test 3 30 190 5000 46.4
Test 4 60 170 4000 47.5
Test 5 60 180 5000 47.3
Test 6 60 190 3000 48.4
Test 7 90 170 5000 47.2
Test 8 90 180 3000 49.3
Test 9 90 190 4000 47.4
K1 140.1 141.7 144.7 /
K2 143.2 143.9 142.2 /
K3 143.9 142.2 140.9 /
R 3.8 2.2 3.9 /
Polymers 2022, 14, 4350 7 of 19

Table 8. Calculation results of viscosity test R and K values of PE modified asphalt.

Shear 135 ◦ C
Factor Shear Time/min Shear Rate/r·min−1
Temperature/◦ C Viscosity/Pa·s
Test l 30 170 3000 0.618
Test 2 30 180 4000 0.609
Test 3 30 190 5000 0.628
Test 4 60 170 4000 0.606
Test 5 60 180 5000 0.612
Test 6 60 190 3000 0.600
Test 7 90 170 5000 0.617
Test 8 90 180 3000 0.594
Test 9 90 190 4000 0.609
K1 1.855 1.814 1.812 /
K2 1.818 1.815 1.823 /
K3 1.820 1.827 1.857 /
R 0.037 0.012 0.045 /

Tables 6–8 listed the effect of different preparation parameters on the penetration,
softening point, and viscosity of PE-modified asphalt. From Tables 7 and 8, according
to the R values, the factors that affect the penetration and viscosity were shearing rate,
shearing time, and shearing temperature, in that order. However, the temperature became
the foremost factor affecting the softening point, as the R-value of the shearing temperature
(4.5) exceeds that of the shearing rate (1.0). Based on Tables 6–8, it can be explained that
the shearing rate, shearing time, and shearing temperature had some negative effects on
the properties of specimens. Table 6 displayed the softening point with various factors.
The large values of K represented the high softening point that indicated less sensitivity to
the high-temperature properties of plastic-modified asphalt. According to the K values in
Table 6, the softening point was the best when the shearing time, shearing temperature, and
shearing rate were 30 min, 170 ◦ C, and 3000 rpm, respectively. From the above analysis,
the optimal preparation parameters of PE-modified asphalt were determined, in which the
shearing time was 30 min, the shearing temperature was 170 ◦ C, and the shearing rate was
3000 rpm.

3.1.2. Optimal Preparation Parameters of PP Modified Asphalt

According to the orthogonal test scheme in Table 4, a total of 9 groups of orthogonal
tests are carried out, and the test data results were shown in Table 9.

Table 9. Properties of PP-modified asphalt.

Factor Softening Point/◦ C 25 ◦ C Penetration/0.1 mm 135 ◦ C Viscosity/Pa·s

Test l 63.4 54.5 0.670
Test 2 61.6 52.3 0.679
Test 3 60.9 51.8 0.682
Test 4 62.6 51.6 0.684
Test 5 61.4 51.4 0.687
Test 6 60.8 51.3 0.687
Test 7 62.0 52.5 0.676
Test 8 61.2 51.0 0.690
Test 9 60.6 51.5 0.685

The variance analysis results of the orthogonal tests were listed in Tables 10–12.
Tables 10–12 listed the effect of different preparation parameters on the penetration, soften-
ing point, and viscosity of PP-modified asphalt. From Tables 10 and 12, according to the R
values, the factors affecting the softening point and viscosity were shearing temperature,
shearing time, and shearing rate, in that order. However, the shearing rate became the
foremost factor affecting penetration, as the R-value of the shearing rate (4.1) exceeds
Polymers 2022, 14, 4350 8 of 19

that of temperature (4.0). Based on the data in Tables 10–12, it can be explained that the
shearing rate, shearing temperature, and shearing time also had some negative effects on
the properties of specimens. Table 10 displayed the softening point of specimens with
various factors. The large values of K represented the high softening point that indicated
less sensitivity to the high-temperature properties of plastic-modified asphalt. According to
the K values in Table 10, when the shearing time, shearing temperature, and shearing rate
were 30 min, 170 ◦ C, and 3000 rpm, respectively, the softening point was the best. From
the analysis above, the optimal preparation parameters of PP-modified asphalt, and the
optimal preparation parameters of the specimen were determined: the shearing time was
30 min, the shearing temperature was 170 ◦ C, and the shearing rate was 3000 rpm.

Table 10. PE Calculation results of softening point test R and K values of PP modified asphalt.

Shear Shear Shear Softening

Factor
Time/min Temperature/◦ C Rate/r·min−1 Point/◦ C
Test l 30 170 3000 63.4
Test 2 30 180 4000 61.6
Test 3 30 190 5000 60.9
Test 4 60 170 4000 62.6
Test 5 60 180 5000 61.4
Test 6 60 190 3000 60.8
Test 7 90 170 5000 62.0
Test 8 90 180 3000 61.2
Test 9 90 190 4000 60.6
K1 185.9 188.0 185.4 /
K2 184.8 184.2 184.8 /
K3 183.8 182.3 184.3 /
R 0.7 1.9 0.37 /

Table 11. Calculation results of penetration test R and K values of PP modified asphalt.

Shear Shear 25 ◦ C
Factor Shear Time/min
Temperature/◦ C Rate/r·min−1 Penetration/0.1 mm
Test l 30 170 3000 54.5
Test 2 30 180 4000 52.3
Test 3 30 190 5000 51.8
Test 4 60 170 4000 51.6
Test 5 60 180 5000 51.4
Test 6 60 190 3000 51.3
Test 7 90 170 5000 52.5
Test 8 90 180 3000 51.0
Test 9 90 190 4000 51.5
K1 158.4 158.6 156.8 /
K2 154.3 154.7 155.4 /
K3 155.0 154.6 155.7 /
R 4.1 4.0 1.4 /
Polymers 2022, 14, x FOR PEER REVIEW 9 of 20

Polymers 2022, 14, 4350 Table 12. Calculation results of viscosity test R and K values of PP-modified asphalt. 9 of 19

Shear
Factor Shear Time/min
Shear Rate/r·min−1 135 °C Viscosity/Pa·s
Temperature/°C
TestTable
l 12. Calculation
30 results of viscosity
170 test R and K values
3000 of PP-modified asphalt.
0.670
Test 2 30 180 4000 0.679
Shear Shear Shear 135 ◦ C
Test 3 Factor30 190 5000
Time/min Temperature/◦ C Rate/r·min−1 0.682Viscosity/Pa·s
Test 4 60 170 4000 0.684
Test 5 Test l 60 30 180 170 5000 3000 0.687 0.670
Test 2 30 180 4000 0.679
Test 6 60 190 3000 0.687
Test 3 30 190 5000 0.682
Test 7 Test 490 60 170 170 5000 4000 0.676 0.684
Test 8 Test 590 60 180 180 3000 5000 0.690 0.687
Test 9 Test 690 60 190 190 4000 3000 0.685 0.687
K1 Test 2.031
7 90 2.030 170 2.047 5000 / 0.676
K2 Test 2.028
8 90 2.056 180 2.048 3000 / 0.690
K3 Test 2.051
9 90 2.054 190 2.045 4000 / 0.685
R K 1 0.023 2.0310.026 2.030 0.003 2.047 / /
K2 2.028 2.056 2.048 /
K3 2.051 2.054 2.045 /
3.2. Influence ofRPlastic Contents on Physical Properties
0.023 of Base Asphalt 0.003
0.026 /
3.2.1. Effect of PE Contents on the Modified Asphalt
According to the
3.2. Influence previous
of Plastic studies
Contents on [28–30], different dosages
Physical Properties (0, 2%, 4%, 6%, 8%) of
of Base Asphalt
PE were selected, and PE-modified asphalt was prepared
3.2.1. Effect of PE Contents on the Modified Asphalt with the optimal preparation
parameters.According
Figure 3 shows the curves of softening point, penetration,
to the previous studies [28–30], different dosages and(0,
ductility
2%, 4%,of6%,
PE-8%) of
modified
PE asphalt with various
were selected, contents of PE.
and PE-modified asphalt was prepared with the optimal preparation
parameters. Figure 3 shows the curves of softening point, penetration, and ductility of PE-
modified asphalt with various contents of PE.

Softening point 25 ℃ Penetration 5 ℃ Ductility

Softening point (℃) / 25 ℃ Penetration (0.1mm)

100 10

9
90

8 5 ℃ Ductility (cm)
80
7
70
6
60
5

50
4

40 3

30 2
0 2 4 6 8
PE dosage (%)

Figure 3. Influence curve of softening point, penetration, and ductility with different PE dosages.
Figure 3. Influence curve of softening point, penetration, and ductility with different PE dosages.
It can be seen from Figure 3 that the softening point was improved after adding PE.
ItWhen
can betheseen from of
content Figure 3 that thefrom
PE increased softening
4% to point
6%, thewas improved
softening pointafter adding
showed PE.
a significant
When increase
the contentof 42%.
of PE The reasonfrom
increased was4%that
towhen PEsoftening
6%, the content was
pointincreased,
showed a phase separation
significant
appeared,
increase of 42%. Theshowing
reasonthat
wasthe plastic
that whenphase was distributed
PE content in the
was increased, continuous
phase separationphase of
asphalt. In this way, the plastic phase was swelled by absorbing the
appeared, showing that the plastic phase was distributed in the continuous phase of as- light components in
phalt. asphalt, thereby
In this way, the improving
plastic phase thewas
performance
swelled byofabsorbing
modified asphalt.
the light Itcomponents
can be seenin that the
penetration
asphalt, decreasedthe
thereby improving after adding PE.ofThe
performance reason asphalt.
modified was thatItthe
cancombination
be seen thatof theplastics
in asphalt
penetration formed
decreased a good
after three-dimensional
adding network
PE. The reason was structure,
that the whichof
combination also madeinasphalt
plastics
harden, finally leading to a decrease in penetration. Meanwhile, the ductility of asphalt
was decreased. When the content of PE increased from 4% to 6%, the ductility at 5 ◦ C had
an obvious decrease in a leap of 52%. With the increase of the plastic contents, some defects
 asphalt formed a good three-dimensional network structure, which also made asphalt
harden, finally leading to a decrease in penetration. Meanwhile, the ductility of asphalt
was decreased. When the content of PE increased from 4% to 6%, the ductility at 5 °C had
an obvious decrease in a leap of 52%. With the increase of the plastic contents, some de-
Polymers 2022, 14, 4350 10 of 19
fects on the surface or inside would produce tiny holes under the action of stress concen-
tration and then develop into very fine lines. When the deformation developed further
and the straight orientation molecular chain was broken, it would turn into micro cracks.
The smallonparticles
the surface or inside
of plastic would
played theproduce tiny holes
role of stress under the and
concentration, action
theofmodifier
stress concentration
par-
and then develop into very fine lines. When the deformation developed
ticles caused a large number of fine lines or shear bands under external tension, thus further
re- and the
straight orientation molecular chain was broken, it
ducing the room temperature crack resistance of PE-modified asphalt.would turn into micro cracks. The small
particles of plastic played the role of stress concentration, and the modifier particles caused
a large
3.2.2. Effect number
of PP of fine
Contents on lines or shear bands
the Modified Asphaltunder external tension, thus reducing the room
temperature crack resistance of PE-modified asphalt.
According to the previous study [31], different dosages (0, 2%, 4%, 6%, 8%, 10%, 12%)
of PP were selected,
3.2.2. Effect ofand
PP the PP-modified
Contents asphalt was
on the Modified prepared with the optimal prepa-
Asphalt
ration parameters. The curves of softening point, penetration, and ductility are shown in
According to the previous study [31], different dosages (0, 2%, 4%, 6%, 8%, 10%,
Figure 4.
12%) of PP were selected, and the PP-modified asphalt was prepared with the optimal
preparation parameters. The curves of softening point, penetration, and ductility are shown
in Figure 4.
90
Softening point
Softening point (℃) / 25 ℃ Penetration (0.1mm)

25 ℃ Penetration 10
5 ℃ Ductility
9
80
8

5 ℃ Ductility (cm)
70 7

60 5

4
50
3

2
40
0 2 4 6 8 10 12
PP dosage (%)

Figure 4. Influence curve of softening point, penetration, and ductility with different PP dosages.
Figure 4. Influence curve of softening point, penetration, and ductility with different PP dosages.
It can be seen from Figure 4 that the softening point of asphalt was obviously improved
It can beadding
after PP. The
seen from softening
Figure 4 thatpoint decreasedpoint
the softening as theofdosage
asphaltof was
PP increased.
obviouslyWhen
im- the PP
proved content was less
after adding PP.than
The 6%, the softening
softening point increased
point decreased as the slowly,
dosageand when
of PP the PP content
increased.
When the increases
PP contentfromwas
6% less
to 8%,thanthe
6%,softening point point
the softening of theincreased
plastic-modified asphalt
slowly, and whenincreases
the PP content increases from 6% to 8%, the softening point of the plastic-modified asphalt from
significantly, and the increment is about 14%, and when the PP content increases
increases8% to 10%, the and
significantly, softening point rises
the increment slowly.
is about 14%, It can
and be seen
when thethat
PP the penetration
content and 5 ◦ C
increases
from 8%ductility
to 10%, theof PP-modified
softening pointasphalt
risesdecrease
slowly. Itwith
can the increase
be seen that in
thePP dosage. Atand
penetration low5content,
plastic improved the penetration of base asphalt, however, with
°C ductility of PP-modified asphalt decrease with the increase in PP dosage. At low con- the increasing of plastic,
the content of oxidized substances (such as resins or asphaltenes)
tent, plastic improved the penetration of base asphalt, however, with the increasing of began to accumulate,
plastic, which damaged
the content the structure
of oxidized of the (such
substances asphalt
ascomponents and inhibited
resins or asphaltenes) the to
began stretching
accu- effect
mulate, of the performance
which damaged theof base asphalt.
structure of the asphalt components and inhibited the stretch-
The softening point
ing effect of the performance of base of asphalt
asphalt.increased and the penetration decreased for the PE
and PP-modified asphalts with the contents increasing. However, when the content of
PE and PP was less than 8%, the low-temperature ductility decreased slightly after the
initial decreasing trend. In addition, when the PP content was higher than 8%, the ductility
decreased by 0.4, while the softening point increased by 4.9 and penetration decreased by
3.7. Furthermore, in order to maximize the improvement effects of PE and PP on asphalt
performance in high-temperature areas, the recommended optimal dosages of PE and PP
were 5% and 9% respectively.
Polymers
Polymers 2022,
2022, 14,
14, x4350
FOR PEER REVIEW 1211ofof20
19

3.3.
3.3. Comparative
ComparativeAnalysis
AnalysisofofBasic
BasicPerformances
Performances with
with SBS
SBS Modified
Modified Asphalt
Asphalt
With the high-temperature melt mixing method, PE-modified asphalt,
With the high-temperature melt mixing method, PE-modified asphalt, andand PP-mod-
PP-modified
ified asphalt were prepared under the optimal preparation parameters and
asphalt were prepared under the optimal preparation parameters and optimal dosage, optimal dos-
age, respectively. Compared with base asphalt and SBS-modified asphalt, the results
respectively. Compared with base asphalt and SBS-modified asphalt, the results of penetra- of
penetration, softening
tion, softening point, ductility,
point, ductility, and viscosity
and viscosity were in
were shown shown in5.Figure 5.
Figure

(a) (b)

(c) (d)
Figure
Figure5.5.Comparative
Comparativeanalysis
analysis ofof
matrix
matrixasphalt and
asphalt SBSSBS
and modified asphalt.
modified (a) Softening
asphalt. point.
(a) Softening (b)
point.
Penetration. (c) Ductility.
(b) Penetration. (d) Viscosity.
(c) Ductility. (d) Viscosity.

Figure
Figure 55 shows
shows that
that all
all the
the indexes
indexes adequately
adequatelymeet meetthethespecification
specificationrequirements.
requirements.
Moreover, with the
Moreover, with theaddition
additionofofPEPE and
and PP,PP,
thethe softening
softening pointpoint increased
increased by 35.8%
by 35.8% and
and 44.1%
44.1% respectively,
respectively, which indicated
which indicated better high-temperature
better high-temperature propertiesproperties of plastic-modi-
of plastic-modified asphalt.
fied asphalt.
However, However,
the the SBS
SBS modifier hadmodifier
a more had a more influence
significant significantoninfluence on base
base asphalt, asphalt,
increasing
increasing the softening point of asphalt by 59.1%. The penetration decreased
the softening point of asphalt by 59.1%. The penetration decreased by 42% and 43.5% by 42% and
43.5% respectively,
respectively, whichwhich has similar
has similar effectseffects with
with the themodifier
SBS SBS modifier
on theonasphalt.
the asphalt. Mean-
Meanwhile,
while, the highest
the highest influence
influence of these
of these modifiers
modifiers couldcould
be onbethe
onviscosity
the viscosity
of theof asphalt
the asphalt
[32].[32].
PE-
PE-modified asphalt
modified asphalt andand PP-modifiedasphalt
PP-modified asphaltincreased
increasedthetheviscosity
viscosity of
of asphalt by by 61.4%
61.4%
and82.5%
and 82.5%respectively,
respectively, indicating
indicatinggood goodworkability
workabilityand andconsistency
consistencyin inroad
roadconstruction.
construction.
Furthermore,
Furthermore, the softening points of the PE-modified asphalt and
softening points of the PE-modified asphalt and PP-modified PP-modified asphalt are
asphalt
obviously higher than that of base asphalt, while the penetration was
are obviously higher than that of base asphalt, while the penetration was lower than thatlower than that of
base
of asphalt,
base which
asphalt, whichindicates
indicates thethebetter high-temperature
better high-temperature performance
performance of plastic-modified
of plastic-mod-
asphalt.
ified When
asphalt. compared
When with with
compared the SBS themodifiers, the waste
SBS modifiers, plasticplastic
the waste modifiers adequately
modifiers ade-
meet the
quately requirements
meet of the specification,
the requirements whilst only
of the specification, whilstlagging behindbehind
only lagging these expensive,
these ex-
speciallyspecially
pensive, producedproduced
modifiers,modifiers,
by small margins.
by smallThis furtherThis
margins. confirms theconfirms
further efficacy of plastic
the effi-
modifiers as viable economical substitutes for their expensive counterparts.
cacy of plastic modifiers as viable economical substitutes for their expensive counterparts.

3.4. Mechanism
3.4. MechanismAnalysis
AnalysisofofPlastic-Modified
Plastic-Modified Asphalt
Asphalt
3.4.1. Effects of Functional Groups on Plastic-Modified Asphalt
3.4.1. Effects of Functional Groups on Plastic-Modified Asphalt
The functional groups of asphalt can be divided into the following characteristic peaks:
The functional groups of asphalt can be divided into the following characteristic
the strong absorption at 2880~2980 cm−1 is the C-H stretching vibration absorption peak of
peaks: the strong
cycloalkanes and absorption
alkanes, theatvariable
2880~2980
anglecmvibration
−1 is the C-H stretching vibration absorption
absorption peaks of CH3 and CH2 is
peak
at 1450of cm
cycloalkanes
−1 and 1370 and
cmalkanes, the variable
−1 , the strong angle
stretching vibration
vibration absorption
absorption peaks
band of CH3
of aromatic
and CH
C=C and multi conjugated hydrogen bound C=O are at about 1600 cm−1 . The presenceof
2 is at 1450 cm−1 and 1370 cm−1, the strong stretching vibration absorption band of
aromatic
Carboxylic C=C and
acid, multi and
Ketone, conjugated
Quinonehydrogen
is shown at bound C=Ocmare
the 1700 −1 at about 1600
absorption cmand
peak,
−1. The
the
presence
absorption ofpeak
Carboxylic acid,cmKetone,
at 700–900 −1 showsandtheQuinone is shown
out-of-plane at the
vibration of 1700 cm−1components.
aromatic absorption
 peak, and the absorption peak at 700–900 cm−1 shows the out-of-plane vibration of aro-
matic components.
Polymers 2022, 14, 4350 As shown in Figure 6, the SK-90# base asphalt was characterized by strong absorp- 12 of 19

tion peaks of C-H, stretching vibration from 2850 cm−1 to 2990 cm−1; an obvious absorption
peak of CH2 variable angle vibration stretching was from 760 cm−1 to 960 cm−1 and CH3
Asvibration
variable angle shown in Figure 6, the
was near SK-90#
1480 cm−1base
. asphalt was characterized by strong absorption
peaks of C-H, stretching vibration from 2850 cm−1 to 2990 cm−1 ; an obvious absorption
peak of CH2 variable angle vibration stretching was from 760 cm−1 to 960 cm−1 and CH3
variable angle vibration was near 1480 cm−1 .

0.4
SK-90# Matrix asphalt

0.5

0.6
Absorbance (a.u.)

0.7

0.8

0.9

1.0

500 1000 1500 2000 2500 3000 3500 4000

Wavenumber (cm−1)
Figure 6. FTIR image of SK-90# matrix asphalt.
Figure 6. FTIR image of SK-90# matrix asphalt.
The main characteristic peaks of PE and PP were depicted in Figure 7. The strong
absorption peaks from 2850 cm−1 to 2990 cm−1 were C-H stretches vibration of PE, and
The main characteristic peaks of PE and PP were depicted in Figure 7. The strong
the absorption peaks of CH3 and CH2 variable angle vibration were near 1480 cm−1 and
absorption
760 peaks
cm−1 . from 2850 cm
Meanwhile,
−1 to 2990 cm−1 were C-H stretches vibration of PE, and the
PP also showed strong absorption peaks of C-H stretching vibration
absorption
frompeaks
2850 cm of CH
− 1 and cm
to3 2990 CH −12 , variable
but it wasangle vibration
characterized by were near 1480
the absorption cmof
peaks
−1 and 760
CH3 and
cm−1. Meanwhile, PP also showed strong absorption −
peaks1 of C-H −
stretching
CH2 variable angle vibration stretching from 1280 cm and 1490 cm which was unlike 1 vibration
from 2850thecm
PE.−1 to 2990 cm−1, but it was characterized by the absorption peaks of CH3 and
CH2 variableTheangle main characteristic
vibration stretchingpeaksfrom
of plastic-modified
1280 cm−1 and asphalt
1490 cm and base asphalt
−1 which were
was unlike
the PE. depicted in Figure 8. When the asphalt was modified with PE and PP, the out-of-plane
vibration of aromatic components was obvious, such as the C-H stretching vibration
absorption peaks of cycloalkanes and alkanes at 2850 cm−1 to 2990 cm−1 , the CH3 and CH2
variable angle vibration absorption peaks at 1450 cm−1 and 1370 cm−1 , and the absorption
peaks at 700~900 cm−1 . New absorption peaks were not found in the whole functional
group region when compared with base asphalt. Meanwhile, in Figure 8b, there was a
stronger absorption band in the range of 2760~3000 cm−1 which was very close to the
position of the infrared absorption peak of the base asphalt. Moreover, some absorption
peaks even coincide with the base asphalt which showed there was no chemical reaction
between plastic and base asphalt. The mixing process was a mainly physical reaction. The
PE and PP absorbed light components in asphalt and swelled during the shearing process.
ymers 2022, 14, x FOR PEER REVIEW 14 of 20

Polymers 2022, 14, 4350 13 of 19

0.8
PE pellets

Absorbance (a.u.)
0.9

1.0

500 1000 1500 2000 2500 3000 3500 4000

−1
Wavenumber (cm )

(a)

0.80
PP pellets

0.85
Absorbance (a.u.)

0.90

0.95

1.00

1.05
500 1000 1500 2000 2500 3000 3500 4000
−1
Wavenumber (cm )

(b)
Figure 7.Figure
The functional groupsgroups
7. The functional change of different
change plastic
of different pellets.
plastic (a)(a)
pellets. PEPE
pellets.
pellets.(b)
(b)PP
PPpellets.
pellets.

The main characteristic peaks of plastic-modified asphalt and base asphalt were de-
picted in Figure 8. When the asphalt was modified with PE and PP, the out-of-plane vi-
bration of aromatic components was obvious, such as the C-H stretching vibration ab-
sorption peaks of cycloalkanes and alkanes at 2850 cm−1 to 2990 cm−1, the CH3 and CH2
variable angle vibration absorption peaks at 1450 cm−1 and 1370 cm−1, and the absorption
 stronger absorption band in the range of 2760~3000 cm−1 which was very close to the po-
sition of the infrared absorption peak of the base asphalt. Moreover, some absorption
peaks even coincide with the base asphalt which showed there was no chemical reaction
between plastic and base asphalt. The mixing process was a mainly physical reaction. The
PE and PP absorbed light components in asphalt and swelled during the shearing process.
Polymers 2022, 14, 4350 14 of 19

0.4
SK-90#
PE 5%
0.5
PE 2%

0.6
Absorbance (a.u.)
0.7

0.8

0.9

1.0

500 1000 1500 2000 2500 3000 3500 4000

−1
Wavenumber (cm )

(a)

0.4
SK-90#
PP 4%
0.5 PP 9%

0.6
Absorbance (a.u.)

0.7

0.8

0.9

1.0

500 1000 1500 2000 2500 3000 3500 4000

Wavenumber (cm−1)

(b)
Figure 8. The functional
Figure 8. Thegroups change
functional of plastic-modified
groups asphalt and matrix
change of plastic-modified asphalt.
asphalt (a) PE-mod-
and matrix asphalt. (a) PE-
ified asphalt and SK-90#. (b) PP-modified asphalt and SK-90#.
modified asphalt and SK-90#. (b) PP-modified asphalt and SK-90#.

3.4.2. Thermogravimetric Analysis

Figures 9–11 were the TG-DSC curves of base asphalt, PE-modified asphalt, and PP-
modified asphalt, respectively. Figure 9a showed the TG-DSC spectrum of SK-90# base
asphalt. The TG curve presented a downward trend which was three weight loss stages
in the test process of base asphalt. The first weight loss stage occurred in the temperature
range of 150~400 ◦ C, and the weight loss was about 10%.
 °C, base asphalt tended to be stable and the residual mass of asphalt was 17.6%. From the
curve, the base asphalt was endothermic and exothermic at 0~40 °C and 400~600 °C, re-
spectively. It can be found that the exothermic peak appeared at 460 °C with the maximum
mass loss rate of base asphalt. In the process of rapid mass change, a large number of
chemical reactions and the exothermic reactions occurred in the complex components of
Polymers 2022, 14, 4350 15 of 19
base asphalt. The concentration time of the exothermic process was short due to the com-
plex chemical reaction.

(a)

(b)
Polymers 2022, 14, x FOR PEER REVIEW 17 of 20
Figure
Figure9.9.TG-DSC
TG-DSCspectrum
spectrumofof
base
baseasphalt
asphaltand
andPE-modified
PE-modifiedasphalt.
asphalt.(a)(a)TG-DSC
TG-DSCspectrum
spectrumofofbase
base
asphalt. (b) TG-DSC spectrum of PE modified asphalt.
asphalt. (b) TG-DSC spectrum of PE modified asphalt.

10. TG-DSC
Figure 10.
Figure TG-DSCspectrum
spectrumofofPP-modified
PP-modifiedasphalt.
asphalt.

10
PP modified asphalt
PE modified asphalt
8

6
mw/mg)

4
Polymers 2022, 14, 4350 16 of 19
Figure 10. TG-DSC spectrum of PP-modified asphalt.

10
PP modified asphalt
PE modified asphalt
8

Heat flux/(mw/mg) 4

-2

-4

-50 0 50 100 150

Temperture/℃

FigureFigure 11. Thermal

11. Thermal analysis
analysis curve curve of plastic-modified
of plastic-modified asphalt.
asphalt.

FigureAfter 290 ◦ C, the

9b showed the weight
thermalofanalysis
base asphalt decreased
spectrum obviously, asphalt.
of PE-modified which meant
It canthat
be base
seen that the thermal analysis spectrum of PE-modified asphalt was obviously different of
asphalt underwent a process of combustion during the mass loss. The second stage
◦ C. In this stage, base asphalt lost 80% of its weight, which
from mass lossasphalt.
the base occurred at 380~540
Firstly, from the TG curve, it can be seen that the mass of the test
samplewas also the
showed a most masstrend.
downward loss among
When thetemperature
the three stages. When
rose the 360
to about temperature reached
°C, the mass
560 ◦ C, base asphalt tended to be stable and the residual mass of asphalt was 17.6%. From
loss of asphalt began to change obviously. At this time, the test sample began to decom-
◦ C and 400~600 ◦ C,
pose the curve, the
by heating, andbase
theasphalt was endothermic
curve changed andthe
gently until exothermic at 0~40 was
test temperature about 500
respectively. It can be found that the exothermic peak appeared at 460 ◦ C with the maximum
°C. This was because some physical changes occurred in the PE pellets beyond 360 °C.
mass loss rate of base asphalt. In the process of rapid mass change, a large number of
Some components with similar structures in the asphalt were adsorbed by these PE parti-
chemical reactions and the exothermic reactions occurred in the complex components
cles. Under the action of some lightweight components, PE pellets swelled, and the struc-
of base asphalt. The concentration time of the exothermic process was short due to the
tural composition of the asphalt was changed, which increased its viscosity and changed
complex chemical reaction.
the polyethylene state from a crystalline state to an amorphous state. Compared with the
Figure 9b showed the thermal analysis spectrum of PE-modified asphalt. It can be
temperature range of 290 °C to 500 °C, the PE-modified asphalt mass loss was diminished
seen that the thermal analysis spectrum of PE-modified asphalt was obviously different
by 33.3% from 360 °C to 500 °C, which indicated that the process of PE-modified asphalt
from the base asphalt. Firstly, from the TG curve, it can be seen that the mass of the test
mass loss was shorter. It showed that the addition of PE pellets reduced the contents of
sample showed a downward trend. When the temperature rose to about 360 ◦ C, the mass
light components, such as saturated phenanthrene and aromatic components. Addition-
loss of asphalt began to change obviously. At this time, the test sample began to decompose
ally, it increased the contents of asphaltene and gum in base asphalt under high-temper- ◦
by heating, and the curve changed gently until the test temperature was about 500 C.
atureThis
melting,
was which
because made
somethe asphaltchanges
physical have better high-temperature
occurred performance.
in the PE pellets beyond 360 ◦ C. Some
components with similar structures in the asphalt were adsorbed by these PE particles.
Under the action of some lightweight components, PE pellets swelled, and the structural
composition of the asphalt was changed, which increased its viscosity and changed the
polyethylene state from a crystalline state to an amorphous state. Compared with the
temperature range of 290 ◦ C to 500 ◦ C, the PE-modified asphalt mass loss was diminished
by 33.3% from 360 ◦ C to 500 ◦ C, which indicated that the process of PE-modified asphalt
mass loss was shorter. It showed that the addition of PE pellets reduced the contents of
light components, such as saturated phenanthrene and aromatic components. Additionally,
it increased the contents of asphaltene and gum in base asphalt under high-temperature
melting, which made the asphalt have better high-temperature performance.
Figure 10 shows the trend of the thermal analysis spectrum of PP-modified asphalt
which was similar to that of PE-modified asphalt. However, the changing trend of PP-
modified asphalt began earlier. The main reason was that the lightweight components in
the base asphalt were absorbed by the PP pellets. Due to the high-speed shearing action,
the PP pellets were scattered in the base asphalt. During this process, the required energy
was less in the range of room temperature to 600 ◦ C, which indicated that the PP pellets
started the physical reaction much easier than PE pellets. Although the DSC curve changed
very little, there was still some mass loss from inception until 360 ◦ C, which was still
Polymers 2022, 14, 4350 17 of 19

similar to PE-modified asphalt. When the test temperature rose to about 460 ◦ C, the mass
loss of the test sample tended to be flat. All the results were consistent with the previous
research conclusions.
As shown in Figure 11, PE-modified asphalt had a larger endothermic peak area
than PP-modified asphalt. When the plastic pellets were added, the DSC curve of the
corresponding modified asphalts became smoother, and the corresponding peak was
smaller, which could prove that the temperature stability of PE-modified asphalt was more
stable than that of PP-modified asphalt. The reason was that the addition of PE pellets made
the asphalt components more complex, the swelling and cross-linking reaction between
plastic and asphalt was more sufficient under high-temperature conditions, the contents
of light components in the asphalt were reduced, and the PE pellet was not completely
swollen, existing as small particles in the modified asphalt.
Meanwhile, with the temperature increasing, the adsorption between molecules made
the remaining components in the asphalt have no obvious change, and the DSC curve
only showed a gentle peak. When the temperature was between −40 ◦ C and 30 ◦ C, the
asphalt changed from a solid state to a liquid state with performance changing. At this
time, the performance of asphalt mainly depended on the solid components part. In this
temperature range, the exothermic peak of PE-modified asphalt was naturally larger than
that of PP-modified asphalts because its temperature sensitivity was obvious.
Furthermore, when the modified asphalt changed from a solid state to a liquid state,
the volume of flowing components increased and the intermolecular force decreased rapidly.
Due to the existence of pellets, the light components in plastic-modified asphalt existed
in crystallized forms. When the temperature increased, the amount of solid matter and
components in this part of the asphalt changed obviously. That meant the phase state with
an obvious exothermic peak changed sharply. As a result, these plastic-modified asphalts
were more suitable to be used in high-temperature regions.

4. Conclusions
Introducing waste plastics into the asphalt as a modifier was one of the most innova-
tive, reasonable, and effective ways to recycle them owing to the economic benefits and
reduced negative impact on the environment. Therefore, this paper put forward a way of
using waste PE and PP as asphalt modifiers. The optimal process conditions and prepara-
tion parameters were proposed, the performance of PE-modified asphalt and PP-modified
asphalt were studied and the reaction mechanism was revealed. The conclusions were
summarized as follows:
(1) The performance of base asphalt can obviously be affected by PE and PP. The proper
preparation parameters were 30 min shearing time, 170 ◦ C shearing temperature, and
3000 r/min shearing rate. The optimal dosage for the PE and PP were recommended
to be 5% and 9% respectively.
(2) When compared with SBS modifiers, the waste plastic, adequately met the require-
ments of the relevant specification, whilst only lagging behind these expensive spe-
cially produced modifiers, by small margins. As in the case of the softening point,
where the waste plastic modified asphalts were only lower by an average of 8.2%
than the special modifiers, indicating the efficiency of waste plastic modifiers as an
economical substitute.
(3) The plastic-modified asphalt and the base asphalt had similar functional groups,
especially the positions of the C-H stretching absorption peaks, CH3 , and CH2 variable
angle absorption peaks of the cycloalkanes and alkanes. There were no new absorption
peaks which indicated that the mixing process of asphalt and waste plastic was a
physical swelling reaction.
(4) The plastic-modified asphalt showed better thermal stability with a mass loss of about
33.3%. Due to the absorbing and light-reducing components of asphalt, the mass loss
process of plastic-modified asphalt was shorter. The temperature sensitivity of waste
Polymers 2022, 14, 4350 18 of 19

plastic-modified asphalt was reduced since the endothermic peak area and exothermic
peak area of the DSC curve increased obviously.
(5) The good high-temperature performance of plastic-modified asphalt made it more
suitable in high-temperature regions. Since PE was the most produced plastic type,
it is recommended to reuse it as a modifier in asphalt; it will therefore achieve an
additional environmental conservation aim and provide a new way for the recycling
of waste materials.
The preparation, modification mechanism, and basic properties of PE and PP-modified
asphalt were focused on in this study, and further studies will focus on more types of plastic,
low-temperature performance improvement, and compatibility. In particular, the use of
molecular simulation techniques is strongly recommended for further investigation of
asphalt compatibility and modification mechanisms at the molecular level.

Author Contributions: H.L.: conceptualization, methodology, validation, investigation, writing—

original draft. L.Z.: conceptualization, writing—review and editing. J.S.: writing—review and
editing. S.W.: supervision. M.Z.: methodology, writing—review and editing. Y.H.: supervision.
A.A.T.: supervision, project administration, resources. All authors have read and agreed to the
published version of the manuscript.
Funding: This research was funded by the Key Research and Development Projects in Shaanxi
Province (2022SF-328), Science and Technology Project of Shaanxi Department of Transportation
(No.19-10K, No.19-28K).
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: All the data used in this article are in the manuscript.
Conflicts of Interest: The authors declare that they have no conflict of interest.

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