3.9 5.

Article

Characterization of Sustainable
Asphalt Binders Modified with
Styrene–Isoprene–Styrene (SIS)
and Processed Oil

Navid Hemmati, Jihyeon Yun, Mithil Mazumder, Moon-Sup Lee and Soon-Jae Lee

https://doi.org/10.3390/su15129464
 sustainability

Article
Characterization of Sustainable Asphalt Binders Modified with
Styrene–Isoprene–Styrene (SIS) and Processed Oil
Navid Hemmati 1 , Jihyeon Yun 1 , Mithil Mazumder 1 , Moon-Sup Lee 2, * and Soon-Jae Lee 1

1 Department of Engineering Technology, Texas State University, San Marcos, TX 78666, USA;
[email protected] (N.H.)
2 Korea Institute of Civil Engineering and Building Technology, Goyang-si 10223, Republic of Korea
* Correspondence: [email protected]

Abstract: The current study aims to evaluate the viscosity and rheological properties of PG 64-22
modified with Styrene–Isoprene–Styrene (SIS) and Processed Oil (PO) to enhance asphalt binder
properties. Performance properties were measured at high, intermediate, and low temperatures.
PG 64-22 was blended with SIS and Processed Oil at three levels (5%, 10%, and 15% by weight of
binder) and two concentrations (6% and 12% by weight of binder), respectively. Modified binders
underwent two short and long artificial aging processes, through the spinning of the thin film in
an RTFO oven and a pressure aging vessel (PAV). The Superpave binder evaluations were carried out
using a rotational viscometer (RV), dynamic shear rheometer (DSR), and bending beam rheometer
(BBR). According to the findings of the research, the addition of SIS caused higher values of viscosity,
but when co-modified with processed oil, there was a substantial decrease in viscosity values. As
a result, workability was improved. (1) It was observed that a greater reduction in viscosity was
achieved when the processed oil was present at a higher concentration at 135 ◦ C compared to a lower
concentration. (2) The study showed that the incorporation of processed oil led to a reduction
in rutting performance of the asphalt binder. However, the addition of SIS resulted in a notable
enhancement of rutting resistance. (3) The role of processed oil as co-modifier at concentrations of
6% and 12% caused significant decreases in G*sin δ, based on the susceptibility of asphalt molecules
to accept oil molecules in their network links. (4) The extracted measurements from the BBR tests
indicated that modification with SIS and PO improved the low-temperature cracking resistance
Citation: Hemmati, N.; Yun, J.;
significantly. Comparison of asphalt binders modified with 6% and 12% PO and the same SIS content
Mazumder, M.; Lee, M.-S.; Lee, S.-J.
Characterization of Sustainable
showed significant changes in modification with 12% PO rather than 6%.
Asphalt Binders Modified with
Styrene–Isoprene–Styrene (SIS) and Keywords: processed oil; SIS; cracking resistance; modified binders
Processed Oil. Sustainability 2023, 15,
9464. https://doi.org/10.3390/
su15129464
1. Introduction
Academic Editor: Edoardo Bocci
Asphalt binders are the most commonly used material for road construction. Currently,
Received: 14 March 2023 due to the increasing population and number of vehicles, more dynamic loads are applied
Revised: 4 June 2023 on asphalt pavements, resulting in severe defects and problems. Derived from petroleum
Accepted: 6 June 2023
refineries, asphalt binder is a complex chain of molecules that exhibits moderate polarity,
Published: 13 June 2023
molecular weight, and functionality [1]. Due to excessive dynamic loads and harsh weather
conditions, the top layers of asphalt pavements are more susceptible to damage than
the other structural layers [2]. Due to the reduction in the viscosity of asphalt binders
Copyright: © 2023 by the authors.
at excessive high temperatures, surface rutting occurs, which may create many severe
Licensee MDPI, Basel, Switzerland. problems on roads and highways. Thermal cracking is a common issue that arises at
This article is an open access article low temperatures and is caused by the loss of viscoelastic properties in the molecular
distributed under the terms and configuration of the binder [3]. Due to the conversion of aromatics to asphaltene during
conditions of the Creative Commons the aging of binders, greater viscosity has been observed in older asphalt binders than in
Attribution (CC BY) license (https:// virgin asphalt binders [4].
creativecommons.org/licenses/by/ Modification of asphalt binders has been considered and studied for decades as
4.0/). an available solution to optimize the quality of asphalt binders. Enhancing the viscosity of

Sustainability 2023, 15, 9464. https://doi.org/10.3390/su15129464 https://www.mdpi.com/journal/sustainability

Sustainability 2023, 15, 9464 2 of 17

asphalt binders helps to increase the resistance against dynamic loads and harsh situations
at ambient temperatures [5]. The selection and mixing design of modifiers is very important;
however, the laboratory performance may be different from that in situ [6]. On the con-
struction site, workability and handling of modified asphalt should be considered due to its
higher viscosity and high melting temperature [7]. The asphalt industry commonly employs
several modifiers, including Styrene–Butadiene–Styrene (SBS), Styrene–Butadiene–Rubber
(SBR), Crumbed Rubber Modifier (CRM), Polyethylene (PE), and Styrene–Isoprene–Styrene
(SIS) [8]. The presence of these modifiers enriches the viscosity; this means an improvement
will be achieved in rutting resistance, but it causes difficulties in workability and pumping
during the construction of asphalt pavements [9].
As a modifier, SIS increases the viscosity and improves the rutting resistance of asphalt
binder [10,11]. Due to the increase in viscosity, the stiffness of SIS-modified asphalt binders
consequently increases, which may cause thermal and fatigue cracking [12]. Co-modifiers
such as oil compounds help to improve the ability of asphalt binder to handle obstacles,
since they are susceptible to alternate properties of asphalt binders [13,14]. Due to the high
solubility rate of oil in asphalt, studies have shown its inclusion leads to asphalt rejuvena-
tion and dynamic viscosity reduction in addition to the reduction in stiffness [15–18]. As
a co-modifier of asphalt binder, processed oil is known to reduce viscosity and enhance its
resistance to stiffness at low temperatures, thereby preventing thermal cracking defects [19].
However, there is not a lot of research on the impact of oil compounds as co-modifiers with
primary modifiers at various temperature ranges in asphalt binders. The study of road
performance of modified asphalt mixtures is a crucial area of research in civil engineering
and materials science. It involves investigating the effects of modifying asphalt, the binder
used in asphalt concrete, with various additives or modifiers to enhance its performance.
This research aims to improve the overall performance of asphalt concrete, which is used in
road construction. Evaluating the road performance of modified asphalt mixtures helps
engineers to understand how the modified asphalt behaves under different conditions and
to assess its ability to withstand heavy loads, resist deformation, and maintain its integrity
over time. By studying road performance, researchers can determine the optimal dosage
and combination of modifiers, develop guidelines for their use, and ensure the durability
and longevity of asphalt pavements.
The present investigation was conducted to explore the impacts of incorporating
processed oil and SIS on the characteristics of asphalt binders. The research was designed
to determine the effects of different levels of processed oil and SIS on the viscosity and
stiffness of the asphalt binder, as well as its resistance to rutting, thermal cracking, and
fatigue cracking. This research focused on the rheological and cracking characteristics of
asphalt binders that had been modified with SIS and processed oil. This study utilized the
RTFO and PAV to evaluate the impact of short-term and long-term aging on the asphalt
binder. To assess the high-temperature viscosity of modified asphalt binders, measurements
were carried out with a rotational viscometer (RV) at temperatures between 135 ◦ C and
180 ◦ C at 15 ◦ C intervals. The outcomes were studied as a function of SIS and PO contents.
The dynamic shear rheometer (DSR) was employed to analyze the rutting resistance of
asphalt binders in their original state, short-term-aged state after RTFO, and long-term-
aged state after RTFO + PAV. Finally, the bending beam rheometer (BBR) was utilized
to determine the low-temperature cracking resistance of long-term-aged binders after
RTFO+PAV at −12 ◦ C and −24 ◦ C. The study design is illustrated in Figure 1.
Sustainability 2023, 15, 9464 3 of 17

Figure 1. Experimental design flow chart. (a) Control binder preparation process, containing
processed oil. (b) Samples preparation process, containing 6% processed oil and SIS. (c) Samples
preparation process, containing 12% processed oil and SIS.

2. Research Methodology
2.1. Components
A base asphalt binder with a performance grade of 64-22 (PG64-22) was employed as
the raw material both for the control and to be modified using processed oil and SIS. The
properties of the base binder, according to AASHTO PP6 standards, are presented in Table 1.
SIS, which has a linear molecular structure and consists of 15 wt%, was selected as the
primary modifier. The characteristics of SIS can be found in Table 2. To enhance workability
and improve low-temperature performance, processed oil was added as a co-modifier. PO
is a blackish byproduct of petroleum refining that is typically used for slicking industrial
equipment to decrease friction. The characteristics of the PO are presented in Table 3 based
on different ASTM standards.
ff
Sustainability 2023, 15, 9464 4 of 17

Table 1. Asphalt binder PG64-22 properties.

Aging States Test Properties Test Condition PG 64-22

Viscosity (cP) At 135 ◦C 538
Original
G*/sin δ (kPa) At 64 ◦C 2.20
Short-term-aged residual
G*/sin δ (kPa) At 64 ◦ C 3.40
RTFO
G*sin δ (kPa) At 25 ◦ C 4400
Long-term-aged residual ◦C
Stiffness (MPa) At −12 187
RTFO+PAV
m-value At −12 ◦C 0.32
Note: From the [19].

Table 2. Properties of SIS.

Parameter Unit Value

Styrene Grade 4113 A/4113 N
Polymer Structure Linear
Styrene wt% 15.0
Melt Flow g/10 min (200 ◦ C/5 kg) 11.0
Viscosity mPa-s 1240.0
Ash Content wt% 0.3
Volatiles wt% 0.2
Specific Gravity 0.92
Tensile Strength psi (MPa) 3600 (25)
Elongation % 1250.0
Hardness, Shore A 33.0

Table 3. Properties of processed oil.

Test Test Condition Unit Value Specification

Relative Density At 15 ◦ C 1.0049 D4052
Flash Point Cleveland Open Cup ◦C 228.0 D92
At 98.9 ◦C cm2 /minute 13.554 D 445
Kinematic Viscosity
At 100 ◦ C cm2 /minute 12.918 D 445
Pour Point ◦C +15 D 97
Viscosity
0.9555 D 2140
Gravity Constant
Aromatic % 41.9 D 2140
Hydrocarbon Type Naphtenic % 26.2 D 2140
Paraffinic % 31.9 D 2140
Note: From the [19].

2.2. Preparation Process

At a designated temperature of 170.0 ± 5 ◦ C, processed oil was added into the base
binder while mixing was on-going. SIS was added at various concentrations after reaching
the target temperature, and the duration of mixing was set at 10 min using 8000 rpm. To
maintain the original characteristics of the binder, the mixing temperature was manually
monitored and controlled not to exceed its boiling point.
Sustainability 2023, 15, 9464 5 of 17

Two distinct concentrations of processed oil were utilized as modifiers in this study,
comprising 6% and 12% of the sample’s weight of the unmodified binder. Once the ten-
minute mixing process was complete, SIS was introduced directly to the agitation vessel
in three separate concentrations of 5%, 10%, and 15% as a fraction of sample weight. To
keep the coherence throughout the whole tests, the modifiers were sourced from the same
product package.
Two long-term and short-term aging processes were performed to age the samples.
The short-term aging process proceeded artificially at 163 ◦ C for 85 min. This was followed
by a long-term aging treatment, which was performed under 2 bars of pressure at 100 ◦ C
for 20 h in the PAV. Once the aging treatments were completed, the tests mentioned in
the study design flowchart were conducted to investigate the impact of modification via
SIS–PO. The appearance of the PO is depicted in Figure 2.

Figure 2. Processed oil (PO).

2.2.1. Fundamental Attribute Assessments

tt
To assess the asphalt mixture regarding its workability and handling, a rotational
viscosity (RV) test was conducted over a temperature range of 135–180 ◦ C at 15 ◦ C intervals,
using a constant velocity of 20 rpm. The test was performed on 10.5 g samples via cylindrical
spindle number 27, and the timespan of the RV test was fixed at 20 min per sample for data
collection. The determination of the asphalt binder’s viscoelastic properties and resistance
to rutting involved the measurement of complex shear modulus (G*) and the sine of the
phase angle (δ) at 82 ◦ C, enabling the calculation of G*/sin δ. To assess the fatigue cracking
tt binder, G* and sin δ factors were measured at 25 ◦ C. The
resistance of the modified asphalt
◦
modified asphalt binder’s stiffness values
◦
δ were investigated at two temperatures of −12 C δ
and −24 C using BBR (Canon, Huntington, NY, USA) equipment based on the standards
of AASHTO T 313. To measure the creep stiffness of the samples, which had dimensions of
δ
125 × 6.35 × 12.7 mm3 , they were molded and placed in a bath.ff
− −
2.2.2. Data Analysis
ff
The investigation applied a statistical analysis technique known as Analysis of Vari-
ance (ANOVA) using the Social Sciences Statistical Program (SSSP 28) with Fisher’s Min-
imum Significant Difference (MSD) contrast and a significance level of α = 0.05. The
primary parameters examined in this study were the PO concentrations of 0%, 6%, and
12%, and SIS concentrations of 0%, 5%, 10%, and 15%. ANOVA was executed to identify
significant dissimilarities among sample averages. To assess the differentiation between
two populations, the Mean Square Deviation (MSD) was calculated based on the deviation
between sample means, withff a comparison made for each pair of means. If the differenceα
between two sample means equaled or exceeded the MSD value, it indicated a statistically

ff
Sustainability 2023, 15, 9464 6 of 17

significant distinction between the population means. The study utilized a confidence level
of 95%, ensuring a 95% probability of accuracy for each finding.

3. Results and Discussion

3.1. Viscosity
The flowability of asphalt binder within an asphalt plant, its ability to fully coat the
aggregate in a HMA mixture, and its capacity to create a new pavement surface upon
placement and compaction are influenced by its high-temperature viscosity. This viscosity
is a crucial factor in determining the optimal working temperature (Asphalt Institute,
2003) [20]. Figures 3 and 4 present the results obtained from the standard RV test of PG
64-22 asphalt binder modified with PO and SIS across a temperature range of 135 ◦ C to
180 ◦ C. Figure 3 illustrates that the viscosity of the modified asphalt binder with 6% PO
increases as the amount of added SIS (0%, 5%, 10%, and 15%) increases at each temperature
level. The viscosity values of the 6%-processed-oil-modified binder containing 0%, 5%, 10%,
and 15% SIS at 135 ◦ C were observed to be 331, 966, 2681, and 5356 cP, respectively. Figure 4
illustrates that the measured viscosity values for the binder modified with 12% processed
oil with the previous SIS contents at 135 °C were 234, 681, 1687, and 3812 cP, respectively.
It shows that an increase in processed oil content caused viscosity reduction for each
SIS content (0, 5, 10, and 15%) of 26, 29, 37, and 28%, respectively. With an increase in
temperature to 150 ◦ C, the viscosity values for asphalt binder modified with 6% processed
oil and 0, 5, 10, and 15% SIS were 162, 462, 1368, and 2874 cP, respectively. For asphalt
binder modified with 12% processed oil and 0, 5, 10, and 15% SIS, the viscosity values
were measured 118, 337, 887, and 2218, respectively. At 150 ◦ C, there was a reduction in
viscosity of 27, 27, 35, and 22% at 0, 5, 10, and 15% SIS content, respectively, due to the
increase in processed oil concentration from 6% to 12%. Subsequently, the same pattern
of reduction was observed at 165 ◦ C. At 180 ◦ C, with SIS contents of 0, 5, 10, and 15% for
both modified binders, reductions of 50, 28, 31, and 17% were observed, respectively, with
12% processed oil.

ff of SIS content on the viscosity of PG 64-22 binder modified with 6% processed oil.
Figure 3. Effect
Sustainability 2023, 15, 9464 7 of 17

ff of SIS content on the PG 64-22 binder’s viscosity modified with 12% processed oil.
Figure 4. Effect

While an increase in SIS significantly raised the value of G*/sin δ, the introduction of
processed oil as a co-modifier led to a reduction in viscosity due to the high rate of diffusion
in asphalt molecules and the restructuring of the chains of asphaltene molecules; this results
in an improvementffin workability. A higher concentration of processed oil (12% compared
to 6%) in the modified asphalt binders led to a greater reduction in viscosity and good
workability. These results show how processed oil can be effective at improving handling,
pumping,α coating, and compaction on the construction site, by joining with SIS to improve
viscosity and workability simultaneously. Figures 3 and 4 show a reduction in viscosity
which satisfies Superpave’s specifications [20]; except for the ones containing 15% SIS at
135 °C, the binders all had a viscosity lower than 3000 cP. Due to the properties of processed
oil, it seems that this effectiveness can be maintained by conjugating other common modi-
fiers, such as Styrene–Butadiene–Styrene, Styrene–Butadiene–Rubber, Crumbed Rubber
Modifier, etc.
Tables 4 and 5 display the statistical significance of changes in viscosity values caused
by variations in processed oil content, SIS content, and temperature. The findings indicate
that altering the temperature in accordance with changes in processed oil and SIS content
can significantly affect the viscosity values of binders.

Table 4. Viscosity data analysis of modified PG 64-22 with 6% processed oil as a function of SIS
content (α = 0.05).

Viscosity 135 ◦ C 150 ◦ C 165 ◦ C 180 ◦ C

SIS% 0 5 10 15 0 5 10 15 0 5 10 15 0 5 10 15
0 - S S S S S S S S N S S S S S S
◦C 5 - S S S S S S S S S S S S S S
135
10 - S S S S S S S S S S S S S
15 - S S S S S S S S S S S S
0 - S S S S S S S S N S S
◦C 5 - S S S S S S S S N S
150
10 - S S S S S S S S S
15 - S S S S S S S S
Sustainability 2023, 15, 9464 8 of 17

Table 4. Cont.

Viscosity 135 ◦ C 150 ◦ C 165 ◦ C 180 ◦ C

SIS% 0 5 10 15 0 5 10 15 0 5 10 15 0 5 10 15
0 - S S S S S S S
5 - S S S S S S
165 ◦ C
10 - S S S S S
15 - S S S S
0 - S S S
5 - S S
180 ◦ C
10 - S
15 -
S: significant N: Non-significant.

Table 5. Data analysis of viscosity values of modified PG 64-22 with 12% processed oil as a function
of SIS content (α = 0.05).

Viscosity 135 ◦ C 150 ◦ C 165 ◦ C 180 ◦ C

SIS% 0 5 10 15 0 5 10 15 0 5 10 15 0 5 10 15
0 - S S S S S S S S S S S S S S S
5 - S S S S S S S S S S S S S S
135 ◦ C
10 - S S S S S S S S S S S S S
15 - S S S S S S S S S S S S
0 - S S S S S S S S N S S
5 - S S S S S S S S N S
150 ◦ C
10 - S S S S S S S S N
15 - S S S S S S S S
0 - S S S S S S S
◦C 5 - S S S S S S
165
10 - S S S S S
15 - S S S S
0 - S S S
◦C 5 - S S
180
10 - S
15 -
S: significant N: Non-significant.

3.2. Rutting Properties

According to the specifications of Superpave [20], a greater G*/sin δ in dynamic shear
rheometer (DSR) tests means more resistance and effectiveness against the high temperature
rutting defect. The G*/sin δ values were examined at different states of aging, including
original and short-term RTFO, at the temperature of 82 ◦ C. Figure 5 shows the values of
G*/sin δ at their original state. Due to the application of processed oil as a co-modifier,
a decrease in rutting resistance values was expected; however, the G*/sin δ values show
an increase for asphalt binders modified with both 6 and 12% processed oil, because of
the addition of SIS. Therefore, the inclusion of SIS has enhanced the resistance of asphalt
binders against rutting, while the processed oil contents have altered the workability of
the binder. As presented in Figure 5, the G*/sin δ values for the asphalt binder modified
with 6% processed oil demonstrated significant increases of 410%, 297%, and 260% upon
the addition of 5%, 10%, and 15% SIS, respectively. Conversely, for the modified asphalt
binders containing 12% processed oil, a rise in the values of G*/sin δ was observed by
358%, 267%, and 214% due to the incorporation of 5%, 10%, and 15% SIS, respectively. As
a result of the higher proportion of processed oil, the rate of growth in values of G*/sin δ
was moderate in comparison to the binder that was modified with 6% processed oil.
 δ

δ
Sustainability 2023, 15, 9464 9 of 17

Figure 5. Influence of SIS concentration on G*/sin δ values for PG 64-22 binders modified with
6% and 12% processed oil at 82 ◦ C. δ

Table 6 presents the statistical analysis and significance of variations in G*/sin δ

values for the initial state of modified asphalt binders. The binders contained 6% δ and
12% processed oil, with SIS contents ranging from 5% to 15%. Notably, significant alter-
ations were observed in the asphalt binder modified with 6% processed oil when 15% SIS
was added. Conversely, for the asphalt binder modified with 12% processed oil, significant
changes were noted with the addition of both 10% and 15% SIS.

Table 6. Analysis of G*/sin δ values for PG 64-22 at original state, and modified with processed oil
and SIS (α = 0.05). δ
α
G*/sin δ SIS % 0 5 10 15
δ
0 - N N S
PG 64-22
5 - N S
and
10 - S
Processed Oil 6%
15 -
0 - N S S
PG 64-22
5 - S S
and
10 - S
Processed Oil 12%
15 -
S: significant N: Non-significant.

Figure 6 illustrates the G*/sin δ of asphalt binders modified with 6% and 12% processed
oil at a short-term-aged state, after the addition of 5%, 10%, and 15% SIS. The findings
indicate that, in the case of the asphalt binder modified with 6% processed oil, the G*/sin δ
values exhibited increases of 220%, 255%, and 197%, respectively. Conversely, for the
asphalt binder modified with 12% processed oil, the G*/sin δ values experienced increases
of 383%, 267%, and 187%, respectively. These results provide further affirmation of the
notable influence of processed oil on G*/sin δ values, an effect primarily attributed to its
impact on the viscosity of asphalt binders.
 δ
δ
ffi
Sustainability 2023, 15, 9464 δ ff tt 10 of 17

Figure 6. ff δ δ values of RTFO-aged PG 64-22 binder modified with

Effect of SIS concentration on G*/sin
6% and 12% processed oil at 82 ◦ C.

Table 7 presents the noteworthy variations in G*/sinδ δ observed under short-term-

aged conditions, resulting from adjustments in the content of SIS and processed oil. The
results demonstrate that the inclusion of SIS in both modified binders containing 6% and
12% processed oil yielded significant changes. These findings underscore the influence
of SIS on the viscoelastic properties of asphalt binders, as well as its capacity to improve
resistance against rutting
tt at elevated temperatures.

Table 7. G*/sin δ δ values data analysis of short-term-aged PG 64-22, modified with processed oil and
SISα(α = 0.05).

G*/sin δδ SIS % 0 5 10 15
0 - S S S
PG 64-22
5 - S S
and
10 - S
Processed Oil 6%
15 -
0 - S S S
PG 64-22
5 - S S
and
10 - S
Processed Oil 12%
15 -
S: significant N: Non-significant.

3.3. Fatigue Cracking

Figure 7 depicts the test results and values of G*sin δ for asphalt binders modified
with 6% and 12% processed oil after long-term aging (RTFO+PAV), as observed from the
DSR test. G* represents stiffness, while δ indicates the viscoelasticity of the binder. All
binders containing 0%, 5%, 10%, and 15% SIS were tested at 25 °C to investigate the fatigue
cracking resistance. For the asphalt binder modified with 6% concentration of processed oil
and 5%, 10%, and 15% concentrations of SIS, a decrease was observed in the values of G*
sin δ of 25%, 56%, and 72%, respectively. On the other hand, the asphalt binder modified
with 12% processed oil and the same contents of SIS showed a more severe reduction in
 ff δ
℃ to investigate the fatigue
cracking resistance
Sustainability 2023, 15, 9464 11 of 17
δ

δ
values of G* sin δ. These reductions were 7%, 72%, and 66%, for 5%, 10% and 15% of
SIS, respectively. These results demonstrate the impact of processed oil as a co-modifier
δ
alongside SIS; it reduces G* sin δ values and improves fatigue cracking resistance.

Figure 7. G*sinδ δ values of PG 64-22 binder modified with processed oil as a function of SIS content
at 25 ◦ C and long-term aging with RTFO + PAV.

The data analysis of changes in fatigue cracking resistance of modified asphalt binders
containing 6% processed oil and 12% processed oil and 0%, 5%, 10%, and 15% SIS is
presented in Table 8. The obtained values show that the application of SIS as modifier in
conjunction with processed oil as co-modifier enhanced the fatigue cracking resistance of
both modified asphalt binders significantly, regardless of the percentage of content.

Table 8. Analysis of G*sin δ values for PG 64-22 modified with processed oil and SIS after long-term
δ
aging with RTFO+PAV (α = 0.05).
α
G*sin δδ SIS % 0 5 10 15
0 - S S S
PG 64-22
5 - S S
and
10 - S
Processed Oil 6%
15 -
0 - S S S
PG 64-22
5 - S S
and
10 - S
Processed Oil 12%
15 -
S: significant N: Non-significant.

3.4. Thermal Cracking Resistance and Characteristics

To comply with the specifications of Superpave asphalt binders, the maximum per-
mitted value of creep stiffness for asphalt binders is 300 MPa. Lower stiffness values are
desirable to reduce tensile stress in the asphalt binder. The BBR tests were performed at
temperatures of −12 ◦ C and −24 ◦ C on modified asphalt binders. These binders consisted
of 6% processed oil and 12% processed oil, incorporating SIS contents of 0%, 5%, 10%, and
15%. Figures 8 and 9 illustrate the stiffness values of the asphalt binders at −12 ◦ C and
 ff

ff
−
Sustainability 2023, 15, 9464 12 of 17
ff
ff
ff
−24 ◦ C. The stiffness values obtained from the BBR test for the asphalt binder modified
with 6% processed oil, with varying SIS contents (0%, 5%, 10%, and 15%), were 247 MPa,
185 MPa, 105 MPa, and 22 MPa, respectively. Similarly, for the asphalt binders modified
with 12% processed oil, at the same temperature and SIS contents, the stiffness values were
recorded as 117 MPa, 83 MPa, 38 MPa, and 9.8 MPa, respectively.

Figure 8. ffEffect of SIS content on stiffness

ff of RTFO+PAV-aged PG 64-22 binders containing 6% and
12% processed oil at− −12 ◦ C.

Figure 9. Effect of SIS content on stiffness of RTFO+PAV-aged PG 64-22 binders containing 6% and
12% processed oil at −24 ◦ C. −

The influence of SIS and processed oil content on the stiffness values of modified
asphalt binders containing 6% and 12% processed oil was examined at −24 ◦ C. The re-
Sustainability 2023, 15, 9464 13 of 17

sults of the study demonstrate the notable impact of incorporating SIS and processed oil
on the stiffness values. Specifically, for the asphalt binder modified with 6% processed
oil, the stiffness values at 0%, 5%, 10%, and 15% SIS content were 765 MPa, 683 MPa,
363 MPa, and 84 MPa, respectively. Similarly, the stiffness values for the asphalt binder
modified with 12% processed oil, with the same SIS contents, were determined to be
690 MPa, 627 MPa, 242 MPa, and 57 MPa, respectively. These findings indicate that the
inclusion of SIS and processed oil in modified asphalt binders enhances their resistance to
low-temperature cracking.
Tables 9 and 10 display the data analysis and significance and non-significance of
changes in matter for binders modified with 6% and 12% processed oil, with varying
concentrations of SIS (0%, 5%, 10%, and 15%). It is notable that the inclusion of SIS in the
modified binders that contain processed oil results in a significant effect at both −12 ◦ C
and −24 ◦ C. The only instance where a change was found to be non-significant was in
the modified binder that contained 12% processed oil and 5% SIS, as compared to 0%,
at −24 ◦ C.

Table 9. Statistical analysis of the effect of SIS content on stiffness of PG 64-22 modified with 6% and
12% processed oil after long-term aging at −12 ◦ C (α = 0.05).

Stiffness SIS % 0 5 10 15
0 - S S S
PG 64-22
5 - S S
and
10 - S
Processed Oil 6%
15 -
0 - S S S
PG 64-22
5 - S S
and
10 - S
Processed Oil 12%
15 -
S: significant N: Non-significant.

Table 10. Statistical analysis of the effect of SIS content on stiffness of modified PG 64-22 with 6% and
12% processed oil after long-term aging, at −24 ◦ C (α = 0.05).

Stiffness SIS % 0 5 10 15
0 - S S S
PG 64-22
5 - S S
+
10 - S
Processed Oil 6%
15 -
0 - N S S
PG 64-22
5 - S S
+
10 - S
Processed Oil 12%
15 -
S: significant N: Non-significant.

Figures 10 and 11 depict the m-values for asphalt binders modified with 6% processed
oil and 12% processed oil at −12 ◦ C and −24 ◦ C. The processed oil contained SIS in
varying percentages of 0, 5, 10, and 15%. The addition of SIS did not cause a significant
increase in the m-values of either of the modified asphalt binders. For the asphalt binder
modified with 6% processed oil, the m-values at −12 ◦ C were 0.311, 0.32, 0.352, and 0.385 at
SIS concentrations of 0, 5, 10, and 15%, respectively. The asphalt binder modified with
12% processed oil showed increases in m-values of 0.325, 0.337, 0.411, and 0.442 at SIS
concentrations 0, 5, 10, and 15%, respectively. At −24 ◦ C, the m-values for the asphalt
binder modified with a processed oil content of 6% and SIS concentrations of 0, 5, 10,
and 15% were 0.15, 0.163, 0.154, and 0.293, respectively. The asphalt binder modified
with 12% processed oil had m-values of 0.141, 0.145, 0.252, and 0.337, respectively, at the
same temperature.
 ff
Sustainability 2023, 15, 9464 14 of 17

Figure 10. Impact of SIS content on m-values of long-term-aged PG 64-22 binders, modified with
− of −12 ◦ C.
6% processed oil and 12% processed oil, at the temperature

Figure 11. ffEffect of SIS content on m-values of long-term-aged PG 64-22 binders, modified with
− of −24 ◦ C.
6% processed oil and 12% processed oil, at the temperature

The inclusion of processed oil in combination with SIS has a direct impact on the
−
effectiveness −
of modified asphalt binders. The high penetration rate of processed oil and
−
the resulting improvements in viscosity and viscoelasticity are the main factors contributing
to the observed trends− in the m-values of both modified asphalt binders.

− α
Sustainability 2023, 15, 9464 15 of 17

Tables 11 and 12 depict the m-values of asphalt binders modified with varying levels
of SIS at −12 ◦ C and −24 ◦ C. The introduction of 10% and 15% SIS as a modifier resulted in
noticeable changes at −12 ◦ C for asphalt binders modified with both 6% processed oil and
12% processed oil. At −24 ◦ C, significant changes were observed in the modified asphalt
binders with added SIS, except for the binder containing 5% SIS.

Table 11. Data analysis results of the impact of SIS content on m-values of PG 64-22 modified with
6% processed oil and 12% processed oil after long-term aging, at −12 ◦ C (α = 0.05).

m-Value SIS % 0 5 10 15
0 - N S S
PG 64-22
5 - S S
and
10 - S
Processed Oil 6%
15 -
0 - N S S
PG 64-22
5 - S S
and
10 - S
Processed Oil 12%
15 -
S: significant N: Non-significant.

Table 12. Data analysis results of the impact of SIS content on m-values of PG 64-22 modified with
6% and 12% processed oil at long-term aging with RTFO+PAV, at −24 ◦ C (α = 0.05).

m-Value SIS % 0 5 10 15
0 - N N S
PG 64-22
5 - N S
and
10 - S
Processed Oil 6%
15 -
0 - N S S
PG 64-22
5 - S S
and
10 - S
Processed Oil 12%
15 -
S: significant N: Non-significant.

4. Conclusions
To study the impact of processed oil and SIS on the characteristics of modified asphalt
binder at three states of aging, including original, short-term, and long-term, mechanical
tests and other rheology experiments were performed. Various tests, such as rotational
viscosity, DSR, and BBR, were performed to assess the characteristics of modified asphalt
binders in their different aging states. The outcomes of the research shed light on the
combination of processed oil and SIS, resulting in the following deductions:
1. Although the addition of SIS increases viscosity, the presence of processed oil as
a co-modifier leads to a substantial improvement in viscosity values. The modified
asphalt binders containing 12% processed oil exhibit a more considerable reduc-
tion in viscosity for all SIS contents (5%, 10%, and 15%) when contrasted with the
6% processed oil modification.
2. DSR testing revealed that the inclusion of processed oil mitigates the negative impact
of SIS and enhances both viscosity and rutting performance at high temperatures.
A decrease in G*/sin δ values was observed in modified asphalt binders at original
and short-term (RTFO) aging states, which provides evidence of the positive effects of
co-modification using processed oil and SIS.
3. Values extracted from DSR, and evaluation of fatigue cracking tests showed a significant
decrease due to addition of processed oil and SIS. The addition of processed oil had
a positive effect on the viscosity and viscoelasticity of long-term-aged asphalt and
its rejuvenating. Therefore, the application of processed oil along with SIS showed
effectiveness in improving the resistance against fatigue cracking.
Sustainability 2023, 15, 9464 16 of 17

4. The results of the BBR test indicated that the incorporation of processed oil and SIS
caused a significant reduction in stiffness of asphalt binder modified with different
contents of processed oil and SIS, while the same positive effect of this conjugation
was observed in m-values. These results show the important role of processed oil in
viscoelasticity of asphalt binders.
5. Simultaneous application of processed oil and SIS had a positive effect on the resis-
tance of asphalt binders at high and low temperatures, which shows how processed
oil can be effective as a co-modifier in mixture design. It is desirable to study the
impact of processed oil in conjunction with other modifiers such as SBS, CRM, SBR,
and other common ones.

Author Contributions: Conceptualization, S.-J.L.; Validation, S.-J.L.; Resources, M.-S.L.; Writing—original

draft, N.H. and J.Y.; Writing—review & editing, M.M. All authors have read and agreed to the
published version of the manuscript.
Funding: This research was supported by a grant from a government funding project (2023 National
Highway Pavement Management System).
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: The data used to support the findings of this study are included within
the article.
Conflicts of Interest: The authors declare no conflict of interest.

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