materials

Article
Laboratory Evaluation of Storage Stability for Asphalt Binder
Modified with Crumb Rubber and Styrene–Isoprene–Styrene
Depending on Evaluation Factors and Blending Condition
Jihyeon Yun 1 , Shyaamkrishnan Vigneswaran 1 , Hyunhwan Kim 2 , Moon-Sup Lee 3, * and Soon-Jae Lee 2

1 Materials Science, Engineering, and Commercialization, Texas State University, San Marcos, TX 78666, USA;
yiy1@txstate.edu (J.Y.); gry14@txstate.edu (S.V.)
2 Department of Engineering Technology, Texas State University, San Marcos, TX 78666, USA;
k_h82@txstate.edu (H.K.); sl31@txstate.edu (S.-J.L.)
3 Korea Institute of Civil Engineering and Building Technology, Gyeong-si 10223, Republic of Korea
* Correspondence: truepath@kict.re.kr

Abstract: Modified asphalt binders are still considered important in asphalt pavement. However,
the comprehensive use of various modifiers is limited due to storage stability issues. Moreover,
there is a scarcity of detailed analyses regarding the degree of separation for asphalt binders among
each method despite the utilization of various methods to assess the storage stability of binders.
Therefore, a comprehensive analysis was conducted to assess the storage stability of asphalt binder
modified with a crumb rubber modifier (CRM) and styrene–isoprene–styrene (SIS), utilizing five
evaluation factors following the ASTM D7173 guidelines based on four mixing methods (A: high-
shear mixing method, B: low-speed agitating method, C: high-shear mixing method + low mixing
method, D: low-speed agitating method + low mixing method). To produce the modified asphalt
binder, the proportions of the CRM were 5% and 10% for each binder, and 10% SIS was added to
all binders. The results in this study convey that (1) the addition of the modifier led to an increase
in G*/sin δ with different mixing methods, but using mixing methods (C and D) for a relatively
long time resulted in a lower G*/sin δ, indicating suboptimal performance; (2) through the multiple
Citation: Yun, J.; Vigneswaran, S.; Kim, stress creep recovery (MSCR), rheological properties of Jnr and % rec exhibited trends similar to
H.; Lee, M.-S.; Lee, S.-J. Laboratory
G*/sin δ evaluation, highlighting an improved elastic recovery with a higher modifier content;
Evaluation of Storage Stability for
(3) storage stability assessment revealed consistent trends in high-shear mixing groups (A and C),
Asphalt Binder Modified with Crumb
while low-speed mixing groups (B and D) exhibited an elevated separation index (SI), suggesting a
Rubber and Styrene–Isoprene–Styrene
sensitivity to modification conditions; (4) evaluation using the MSCR method indicated that % rec
Depending on Evaluation Factors and
Blending Condition. Materials 2024, 17,
with a 3.2 kPa load is effective for the sensitive assessment of binder storage stability and Jnr showed
2091. https://doi.org/10.3390/ a limited sensitivity across varying loads, advocating for % rec for precise evaluation; and (5) despite
ma17092091 permitting various tests, achieving consistent results remains challenging. Future research should
explore diverse modifiers and optimal evaluation methods to enhance knowledge of binder behavior
Academic Editor: Gilda Ferrotti
and separation dynamics.
Received: 1 March 2024
Revised: 16 April 2024 Keywords: CRM; SIS; storage stability; SI
Accepted: 24 April 2024
Published: 29 April 2024

1. Introduction
Copyright: © 2024 by the authors.
In recent decades, there has been substantial growth and progress in the asphalt indus-
Licensee MDPI, Basel, Switzerland.
try. In particular, a range of modifiers have greatly enhanced the effectiveness of asphalt
This article is an open access article binders, addressing numerous issues that arise on road pavement [1–3]. Nevertheless,
distributed under the terms and irregular failure for asphalt pavement is on the rise, attributed to factors such as climate
conditions of the Creative Commons change and heightened traffic resulting from population density [4]. In addition, in the case
Attribution (CC BY) license (https:// of aged pavement, the deterioration of cracking damage is worsening [5]. Consequently,
creativecommons.org/licenses/by/ the significance of selecting an asphalt binder, modifier, and mixture design while taking
4.0/). into account diverse conditions and environments is acknowledged [6–8].

Materials 2024, 17, 2091. https://doi.org/10.3390/ma17092091 https://www.mdpi.com/journal/materials

Materials 2024, 17, 2091 2 of 18

Modified asphalt mixtures typically offer multiple benefits such as rutting and crack
resistance. However, owing to their heightened viscosity, precise temperature manage-
ment is essential throughout the production-to-construction process to ensure effective
compaction [9,10]. Furthermore, certain modified asphalt binders may incur higher costs,
potentially imposing an additional economic drawback on road construction and main-
tenance, underscoring the significance of comprehensive quality control for both asphalt
binders and mixtures [11]. For modified asphalt binders, one of the biggest challenges is
ensuring the stability of storage for quality control [12–14]. As an example, asphalt binders
stored in tanks may undergo a separation between the polymer and bitumen phases.
The separation process ultimately degrades the characteristics of the polymer-modified
binder and results in the loss of any advantages derived from the modification. Density
variations among materials are considered a major factor contributing to this imbalance
in storage [15–17].
Among the modifiers affecting the storage stability of modified asphalt binders, the
crumb rubber modifier (CRM) is considered the most susceptible. This is attributed to the
tendency of the CRM to settle due to its higher density compared to asphalt binders [18].
Numerous studies have been undertaken to address and resolve the issues related to
storage stability concerning the CRM. In investigations, it was observed that a CRM with
smaller particle sizes demonstrated enhanced storage stability performance, and certain
studies indicated an improvement in storage stability by incorporating nano materials
or a styrene block copolymer [19–22]. In certain research projects, the storage stability
of the binder has been ensured by employing a treated CRM or by subjecting the CRM
to a prolonged blending time until it becomes dissolved [23,24]. In addition, improving
the storage stability through the application of chemical additives has also been observed
in certain instances [25,26]. Therefore, diverse research studies aiming to enhance the
storage stability of CRM binders underscore the significance of the thorough assessment of
storage stability.
Since the issue of phase separation in modified asphalt binders was raised in the
1980s, numerous methods for evaluating storage stability have been suggested, utilizing a
tube, X-ray, microscopy, spectroscopy, etc. [27–32]. Regarding tube testing, it has gained
widespread recognition and adoption due to its ability to closely simulate the storage
conditions of modified binders, making it the most commonly employed method, and
various testing procedures are conducted on the final sample [33–37]. It is deemed appro-
priate to assess the phase separation of modified asphalt binders by examining the storage
stability through diverse experimental outcomes. Nevertheless, when appraising phase
separation using the binder with various experimental factors, variations in the level of
phase separation may occur, leading to ambiguous results for the tester [38].
This study, as shown in the flow chart (Figure 1), is based on ASTM D7173 guidelines [39]
and utilizes a dynamic shear rheometer (DSR) to examine the variations in storage sta-
bility results under the influence of five experimental factors. The modifiers employed
include styrene–isoprene–styrene (SIS), known as styrene block copolymers, and a CRM.
Four blending methods are introduced to assess how the storage stability is affected. More-
over, suggestions for future research plans and directions will be presented.
Materials 2024, 17, x FOR PEER REVIEW 3 of 19
Materials 2024, 17, 2091 3 of 18

Figure
Figure1.1.Flow
Flowchart
chartofofexperimental
experimentaldesign
design procedure in this
procedure in this study.
study.

2.2.Experimental
ExperimentalDesign
Design
2.1. Materials
2.1. Materials
In this research, the base asphalt binder chosen for modification with the CRM and
In this research, the base asphalt binder chosen for modification with the CRM and
SIS was the PG64-22 asphalt binder (Table 1). The CRM coming from passenger vehicles
SIS was the PG64-22 asphalt binder (Table 1). The CRM coming from passenger vehicles
through the ambient grinding process was selected, and its passing rate is detailed in
through the ambient grinding process was selected, and its passing rate is detailed in Table
Table 2. SIS was employed with physical properties similar to those utilized in prior
2.studies,
SIS wasas employed
outlined with physical
in Table properties
3. Aluminum similar
tubes to those
meeting utilized
the ASTM D in prior
7173 studies,
standard as
for
outlined in Table 3. Aluminum tubes meeting the ASTM D 7173 standard for storage
storage stability evaluation were employed. Figure 2 provides visual representations of sta-
bility
eachevaluation were employed.
material utilized Figure 2 provides visual representations of each material
in this study.
utilized in this study.
 RTFO aged residual G*/sin δ @ 64 °C 3.751 kPa >2.2 kPa
G*sin δ @ 25 °C 4245 kPa <5000 kPa
RTFO + PAV
Stiffness @ −12 °C 214 MPa <300 MPa
Aged residual
Materials 2024, 17, 2091 m-value @ −12 °C 0.318 > 0.3 4 of 18

Table 2. Passing rate of Crumb rubber modifier adopted in this study.

Table 1. Properties of base asphalt binder (PG 64-22).
Sieve Number (μm) Passing Rate (%)
Aging States Test Properties
30 (600) Test Result Minimum
100 Specification
Viscosity @ 135 ◦C 527 cP <3000 cP
Unaged binder 50 ◦(300) 57.7
G*/sin δ @ 64 C 1.373 kPa >1.00 kPa
100 (150) 14.2
RTFO aged residual G*/sin δ @ 64 ◦ C 3.751 kPa >2.2 kPa
200
◦
(75) 0.0
G*sin δ @ 25 C 4245 kPa <5000 kPa
RTFO + PAV
Stiffness @ −12 ◦ C 214 MPa <300 MPa
Aged residual Table 3. Properties
m-value @of SIS.
−12 ◦C 0.318 > 0.3

Polymer Structure Linear

Table 2. Passing rate of Crumb rubber modifier adopted in this study.
Styrene, wt % 15
SieveDiblock,
Number (µm)wt % Passing Rate (%)18
30 (600)
Melt flow, g/10min (200 °C/5kg) 100 11
50 (300)
Solution viscosity, cps 57.7 1240
100 (150)wt %
Ash, 14.2 0.3
Volatiles,
200 (75) wt % 0.0 0.2
Specific gravity 0.92
Table 3. Properties of SIS.
Tensile strength, psi (MPa) 3600 (25)
Elongation,
Polymer Structure % Linear 1250
Hardness,
Styrene, wt %shore A 15 33
Diblock, wt % 18
2.2. Production and g/10min
Melt flow, Sampling of ◦CRM+SIS
(200 C/5kg) Asphalt Binders 11
In this study, theviscosity,
Solution production
cps of the CRM+SIS-modified asphalt
1240 binder involved the
sequential additionAsh,
of awtCRM
% followed by SIS to the base asphalt
0.3 binder (Figure 3). The
proportions of theVolatiles,
CRM were wt %
5% and 10% for each binder, and 10% SIS was added to all
0.2
binders. The blending temperature was set at 200 °C, and the process followed these steps.
Specific gravity 0.92
• MethodTensile
A: High-shear mixing (8000 rpm) for 2 h.
strength, psi (MPa) 3600 (25)
• Method B: Low-speed agitating (700 rpm) for 2 h.
Elongation, % 1250
• Method C: High-shear mixing (8000 rpm) for 2 h + low mixing (300 rpm) for 6 h.
• Method D: Hardness,
Low-speed shore A 33
agitating (700 rpm) for 2 h + Low mixing (300 rpm) for 6 h.

(a) (b) (c)

Figure 2. Aluminum tube (a), crumb rubber (b), and SIS (c).
 Materials 2024, 17, 2091 5 of 18

2.2. Production and Sampling of CRM+SIS Asphalt Binders

Materials 2024, 17, x FOR PEER REVIEW 5
In this study, the production of the CRM+SIS-modified asphalt binder involved the
sequential addition of a CRM followed by SIS to the base asphalt binder (Figure 3). The
proportions of the CRM were 5% and 10% for each binder, and 10% SIS was added to all
Figure The
binders. 2. Aluminum tube (a), crumb
blending temperature rubber
was set (b),
at 200 and
◦ C, andSIS
the(c).
process followed these steps.

Figure
Figure 3. Schematic
3. Schematic illustration
illustration depicting
depicting themethod.
the mixing mixing method.

• Method A: High-shear
Following mixingprocess,
the blending (8000 rpm)a for 2 h. of the CRM + SIS asphalt binder fo
portion
• Method B: Low-speed agitating (700 rpm) for 2 h.
original condition sample was promptly set aside for rheological properties. S
• Method C: High-shear mixing (8000 rpm) for 2 h + low mixing (300 rpm) for 6 h.
•quently,
Methodthe
D: remaining binder was
Low-speed agitating (700 meticulously mixed
rpm) for 2 h + Low and(300
mixing poured into6 h.
rpm) for a vertically
tioned tube, ensuring an exact mass of 50 ± 0.5 g, before undergoing conditioning
Following the blending process, a portion of the CRM + SIS asphalt binder for the
oven at
original 163 ± 5 sample
condition °C for was
a duration
promptlyofset48aside
± 1 hfor
(Figure 4). Upon
rheological completion
properties. of this cond
Subsequently,
ing period, the tubes were transferred to a freezer set at –10
the remaining binder was meticulously mixed and poured into a vertically positioned± 10 °C to achieve thor
solidification
tube, ensuring an ofexact
the binder
mass offor50 a±minimum of undergoing
0.5 g, before 4 h, maintaining vertical
conditioning inorientation
an oven thro
atout. ± 5 ◦ Cbinders
163 Once for a duration of 48 ± 1 h (Figure 4). Upon completion of this conditioning
had sufficiently hardened, each tube was divided into three nearly
period, the tubes
segments andwere transferred
subjected to ato30a min
freezer set at –10
heating ± 10at◦ C163
cycle to achieve
± 5 °C thorough
to render solidi-
them fully
fication of the binder for a minimum of 4 h, maintaining vertical orientation throughout.
for the removal of the aluminum tube. Subsequently, binder specimens were meticul
Once binders had sufficiently hardened, each tube was divided into three nearly equal
prepared
segments andfor subsequent
subjected to a 30evaluations.
min heating cycle at 163 ± 5 ◦ C to render them fully fluid
for the removal of the aluminum tube. Subsequently, binder specimens were meticulously
prepared for subsequent evaluations.
 Materials 2024, 17, x FOR PEER REVIEW 6 of 19

Materials 2024, 17, 2091 6 of 18

Figure4.4.The
Figure Thevertically
verticallypositioned
positionedtube.
tube.

2.3.Binder
2.3. BinderEvaluation
Evaluation
2.3.1.
2.3.1.Rheological
RheologicalProperties
Properties
Due
Duetotothe thedependency
dependencyof ofasphalt
asphaltbinder
binderbehavior
behavioron onloading
loadingtimetimeandandtemperature,
temperature,
ananeffective
effectiveevaluation
evaluation of asphalt
of asphalt binders should
binders encompass
should both variables.
encompass The DSR
both variables. Theserves
DSR
asserves
an ideal tool for assessing rheological properties, such as the complex
as an ideal tool for assessing rheological properties, such as the complex shear mod- shear modulus and
phase angle,
ulus and across
phase medium
angle, across tomedium
high-temperature ranges during
to high-temperature asphalt
ranges binder
during testing.
asphalt By
binder
analyzing the viscoelastic behavior, DSR quantifies characteristics such
testing. By analyzing the viscoelastic behavior, DSR quantifies characteristics such as the as the complex shear
modulus
complex (G*)shear and phase angle
modulus (δ) ofphase
(G*) and the asphalt
angle binder.
(δ) of the G*asphalt
reflects binder.
the material’s overall
G* reflects the
resistance to deformation under cyclic shear stress, comprising both
material’s overall resistance to deformation under cyclic shear stress, comprising both elastic (recoverable)
and viscous
elastic (non-recoverable)
(recoverable) and viscous elements. On the other
(non-recoverable) hand, δ On
elements. signifies the proportion
the other hand, δ signi- of
non-recoverable strain. When subjected to a load, asphalt binder
fies the proportion of non-recoverable strain. When subjected to a load, asphalt binder exhibits both elastic and
viscous deformations. Consequently, through the integration of G* and δ, the viscoelastic
exhibits both elastic and viscous deformations. Consequently, through the integration of
parameter G*/sin δ is calculated at a vibration speed of 10 rad/s. This parameter provides
G* and δ, the viscoelastic parameter G*/sin δ is calculated at a vibration speed of 10
insight into the material’s viscoelastic properties, aiding in the characterization of asphalt
rad/sec. This parameter provides insight into the material’s viscoelastic properties, aiding
binder behavior under varying conditions.
in the characterization of asphalt binder behavior under varying conditions.
The multiple stress creep recovery (MSCR) test represents an advancement within
The multiple stress creep recovery (MSCR) test represents an advancement within
the framework of the Superpave asphalt binder specification. One key benefit of the
the framework of the Superpave asphalt binder specification. One key benefit of the MSCR
MSCR test lies in its ability to streamline the evaluation process by obviating the necessity
test lies in its ability to streamline the evaluation process by obviating the necessity for
for multiple distinct tests such as elastic recovery, toughness, ductility, etc., which are
multiple distinct tests such as elastic recovery, toughness, ductility, etc., which are tailored
tailored to elucidate polymer deformation within asphalt binders. By consolidating these
to elucidate polymer deformation within asphalt binders. By consolidating these assess-
assessments into a single MSCR test, comprehensive insights into both the performance
ments into a single MSCR test, comprehensive insights into both the performance and
and composition of the asphalt binder can be gleaned. The methodology of the MSCR
composition
test draws upon of the asphalt principles
established binder canofbecreep gleaned. The methodology
and recovery testing to of the trends
assess MSCR for test
draws upon established principles of creep and recovery testing
permanent deformation in a binder. This involves subjecting the asphalt binder sample to assess trends for per-
tomanent
a creepdeformation
load lastingin1as,binder.
followed Thisbyinvolves subjecting
a recovery periodthe of 9asphalt bindera sample
s. Initially, low stress to a
of 0.1 kPa is applied for 10 creep/recovery cycles, which is subsequently augmentedkPa
creep load lasting 1 s, followed by a recovery period of 9 s. Initially, a low stress of 0.1 to
is applied
3.2 kPa for an foradditional
10 creep/recovery
10 cycles. cycles, which test
The MSCR is subsequently
from traditional augmented
PG testing to 3.2
lieskPa for
in its
an additional 10 cycles. The MSCR test from traditional PG
material response. While PG systems typically measure the high-temperature parameter testing lies in its material re-
G*/sin δ through the application of oscillatory loads at very low strain rates, the MSCRδ
sponse. While PG systems typically measure the high-temperature parameter G*/sin
through
test employsthehigher
application
stress of
and oscillatory loads
strain levels, at very
thereby low strain
providing rates,
a more the MSCR
accurate test em-
depiction of
ploys higher
pavement stress and
behavior. strain levels,
However, MSCRthereby
and PGproviding
systems are a more
bothaccurate depiction
widely utilized toofassess
pave-
ment behavior.
asphalt binders. However,
Therefore,MSCR and were
both tests PG systems are both
considered widely
in this utilized
research to assess
(Figure 5). asphalt
binders. Therefore, both tests were considered in this research (Figure 5).
Materials 2024,
Materials 2024,17,
17,2091
x FOR PEER REVIEW 7 of 19
7 of 18

Figure5.5.Test
Figure Testprocedures
proceduresforfor rheological
rheological properties.
properties.

2.3.2.
2.3.2.Separation
SeparationIndex
Index (SI)
(SI)
This research involved
This research involved thethe
analysis
analysisof aofmodified
a modified asphalt binder,
asphalt withwith
binder, the SI derived
the SI derived
from both top and bottom test outcomes, following the test methods of the ASTM D7173
from both top and bottom test outcomes, following the test methods of the ASTM D7173
guidelines. Initially, SI was computed using Equation (1), utilizing the maximum value
guidelines. Initially, SI was computed using Equation (1), utilizing the maximum value of
of G*/sin δ between the top and bottom sections, denoted as (G*/sin δ)max , with the
G*/sin δ between the top and bottom sections, denoted as (G*/sin δ)max, with the average
average value from the top and bottom parts represented by (G*/sin δ)avg . Following this
value from the
methodology for top and bottom
SI calculation, theparts
SI wasrepresented
assessed using by (G*/sin
Equationsδ)avg(2)
. Following this method-
and (3), employing
ology
Jnr and for SI calculation,
% recovery the SI
for each was assessed
applied using Equations
load. Subsequently, (2) and (3), employing
a comparative analysis was Jnr and
% recovery for each applied load. Subsequently,
conducted between the SI results obtained from each source. a comparative analysis was conducted
between the SI results obtained from each source.
(G*/sin δ)max − (G*/sin δ)avg
Separation index = (G ∗/ sin 𝛿)max − (G ∗/ sin 𝛿) ×avg
100% (1)
𝑆𝑒𝑝𝑎𝑟𝑎𝑡𝑖𝑜𝑛 𝑖𝑛𝑑𝑒𝑥 = (G*/sin δ)avg × 100% (1)
(G ∗/ sin 𝛿)avg
(Jnr)max − (Jnr)avg
Separation index = (Jnr)max − (Jnr)× avg
100% (2)
𝑆𝑒𝑝𝑎𝑟𝑎𝑡𝑖𝑜𝑛 𝑖𝑛𝑑𝑒𝑥 = (Jnr)avg × 100% (2)
(Jnr)avg
(%rec)max − (%rec)avg
Separation index = × 100% (3)
(%(rec)
%recmax − (% rec)avg
)avg
𝑆𝑒𝑝𝑎𝑟𝑎𝑡𝑖𝑜𝑛 𝑖𝑛𝑑𝑒𝑥 = × 100% (3)
(% rec)avg
3. Results and Discussion
3.1. Rheological Properties for Original Condition
3. Results and Discussions
3.1.1. G*/sin δ
3.1. Rheological Properties for Original Condition
The rheological properties of the binder were assessed by evaluating G*/sin δ. Overall,
3.1.1.
the G*/sinofδthe modifier resulted in an increase in G*/sin δ, showing that as the CRM
addition
content increased,
The rheologicalthere was a clear
properties tendency
of the binder forwereG*/sin δ to by
assessed increase (Figure
evaluating 6). This
G*/sin δ. Over-
outcome
all, the addition of the modifier resulted in an increase in G*/sin δ, showing that to
is attributed to the CRM’s absorption of the light oil in the binder, leading as the
aCRM
relative increase
content in asphaltene
increased, content
there was and
a clear gelling of
tendency forthe CRM.
G*/sin In increase
δ to the SIS binder
(Figure with
6). This
5% CRM, the
outcome results obtained
is attributed to the from
CRM’sMethod B showed
absorption of thea slight
light increase,
oil in thewhich
binder,is thought
leading to a
to be due to the uneven dispersion of SIS at high temperatures, resulting in the partial
relative increase in asphaltene content and gelling of the CRM. In the SIS binder with 5%
reaggregation of SIS. This result affected the binder using 10% CRM, which shows an
CRM, the results obtained from Method B showed a slight increase, which is thought to
uneven trend and the lowest resulting gap among each mixing method. In each mixing
be due to the uneven dispersion of SIS at high temperatures, resulting in the partial reag-
method for CRM 10% + SIS 10% asphalt binder, G*/sin δ was relatively lower in groups
Cgregation of SIS.utilize
and D, which This result affected the
the low-speed mixingbinder using 10%
approach for 6CRM, which shows
h, compared an uneven
to groups A
trend and the lowest resulting gap among each mixing method. In each mixing method
for CRM 10% + SIS 10% asphalt binder, G*/sin δ was relatively lower in groups C and D,
which utilize the low-speed mixing approach for 6 h, compared to groups A and B. This
Materials 2024, 17, x FOR PEER REVIEW 8 of 19
Materials 2024, 17, 2091 8 of 18

is attributed to the suboptimal performance of SIS, a styrene block copolymer, due to pol-
and B. This is attributed to the suboptimal performance of SIS, a styrene block copolymer,
ymer molecular chain bond cracking induced by the prolonged reaction at high tempera-
due to polymer molecular chain bond cracking induced by the prolonged reaction at high
tures. Consequently, it is evident that there are significant differences depending on the
temperatures. Consequently, it is evident that there are significant differences depending on
modifying method and duration, underscoring the need to consider various conditions to
the modifying method and duration, underscoring the need to consider various conditions
ensure optimal performance under field conditions (e.g., rpm for the modification, tem-
to ensure optimal performance under field conditions (e.g., rpm for the modification,
perature, etc.).
temperature, etc.).

Figure 6. G*/sin δ of asphalt binders in each mixing method for the original condition.
Figure 6. G*/sin δ of asphalt binders in each mixing method for the original condition.

3.1.2.
3.1.2.Jnr
Jnrand
and%%rec recδδ
AAcomprehensive
comprehensiveanalysis analysisofofrheological
rheologicalproperties
properties was
was conducted
conducted using
usingJnr Jand
nr and%
rec, which
% rec, which employ
employ a relatively
a relatively higher
higherload
loadcompared
comparedtotothe theG*/sin
G*/sinδδevaluation
evaluationmethodmethod
(Figures
(Figures77and and8).8).Overall,
Overall, similar
similarto the findings
to the findingsfrom the G*/sin
from δ evaluation,
the G*/sin the Jnr the
δ evaluation, value Jnr
value exhibited
exhibited a decreasing
a decreasing trend with trendanwith an increase
increase in CRMincontent,
CRM content,
while the while% recthe value
% rec
value showed
showed an increasing
an increasing trend. Notably,
trend. Notably, when applying
when applying a low loada low(0.1
load (0.1the
kPa), kPa),
Jnr the
value Jnr
value tended to be lower and the % rec value tended to be
tended to be lower and the % rec value tended to be higher, indicating a better elastic higher, indicating a better
elastic recovery
recovery of the binder
of the binder under relatively
under relatively lower loadlower load conditions
conditions compared compared
to higher to higher
ones.
ones. Moreover,
Moreover, minimal minimal
deviation deviation
among amongresults wasresults was observed
observed betweenbetween
loads inloadsthe SIS in as-
the
SIS asphalt
phalt binder binder
with 10% with
CRM,10% suggesting
CRM, suggesting that a CRM
that a higher highercontent
CRM content
renders renders
the binder the
binder
more more enabling
elastic, elastic, enabling
effectiveeffective elastic recovery
elastic recovery irrespectiveirrespective of the load
of the applied applied load
magni-
magnitude.
tude. This trendThis trend was similarly
was similarly reflected
reflected in the
in the % rec% rec results.
results. Furthermore,a aprolonged
Furthermore, prolonged
modification time (Methods C and D) led to a decline in
modification time (Methods C and D) led to a decline in the binder’s elastic recovery, the binder’s elastic recovery,
mir-
mirroring the observations from the G*/sin δ evaluation. This phenomenon
roring the observations from the G*/sin δ evaluation. This phenomenon is attributed to the is attributed to
the cracking of polymer chains in SIS due to a prolonged
cracking of polymer chains in SIS due to a prolonged exposure to high temperature andexposure to high temperature
and reaction
reaction duration.
duration. Additionally,
Additionally, a notable
a notable decrease
decrease in elasticity
in elasticity was was observed
observed whenwhen ap-
applying a load of 3.2 kPa in Methods C and D of the group
plying a load of 3.2 kPa in Methods C and D of the group using long-term modification,using long-term modification,
indicatingaaheightened
indicating heightenedsensitivity
sensitivityin inevaluating
evaluatingbinder binderelasticity
elasticityunder
underrelatively
relativelyhigher
higher
loads compared to G*/sin δ evaluation. These findings underscore
loads compared to G*/sin δ evaluation. These findings underscore the clearer depiction of the clearer depiction of
reduced elasticity in the modified binder when subjected to
reduced elasticity in the modified binder when subjected to prolonged modification atprolonged modification at high
temperature,
high temperature, as observed
as observedin thisin study.
this study.
Materials
Materials2024,
2024,17,
17,x2091
FOR PEER REVIEW 9 of 19
9 of 18

Materials 2024, 17, x FOR PEER REVIEW 10 of 19

Figure 7. Jnr of asphalt binders in each mixing method for the original condition.
Figure 7. Jnr of asphalt binders in each mixing method for the original condition.

Figure 8. % rec of asphalt binders in each mixing method for the original condition.
Figure 8. % rec of asphalt binders in each mixing method for the original condition.
 3.2. Storage Stability Results
3.2.1. SI Result Based on G*/sin δ
Materials 2024, 17, 2091 10 of 18
The binder’s storage stability was assessed by calculating the SI utilizing the G*/sin δ
value as a factor (Figure 9). In general, within the groups employing high-shear mixing
methods (Groups
3.2. Storage A and
Stability C), there was a consistent distribution of G*/sin δ values from top
Results
to bottom,
3.2.1. SI accompanied
Result Based onby a downward
G*/sin δ trend in SI values. It is considered that this phe-
nomenon Thearises duestorage
binder’s to the stability
uniformwas dispersion
assessed by of calculating
the modifier thefacilitated
SI utilizing bythe the high-shear
G*/sin δ
value as a factor (Figure 9). In general, within the groups employing
mixer. Nevertheless, for the SIS binder employing 5% CRM in Method C, the SI was mar- high-shear mixing
methods
ginally higher (Groups A and
than that of C),
thethere was a consistent
SIS binder utilizing distribution
10% CRM. of G*/sin
This δ values
suggests thatfrom
with pro-
top to bottom, accompanied by a downward trend in SI values. It is considered that
longed modification time, the SIS binder that dispersed within the modified asphalt
this phenomenon arises due to the uniform dispersion of the modifier facilitated by the
binder tends mixer.
high-shear to re-agglomerate,
Nevertheless, for potentially
the SIS binderexerting
employing a detrimental impact C,ontheasphalt
5% CRM in Method
binder performance,
SI was but in than
marginally higher the result
that ofof thethe
SISSIS binder
binder using10%
utilizing 10% CRM,
CRM. Thisa higher
suggestscontent
of CRM hindered
that with prolongedthe modification
reaggregation of the
time, SIS.SIS
On the other
binder hand, the
that dispersed groups
within that chose the
the modified
low-speed agitating
asphalt binder tendsmethod (B and D)
to re-agglomerate, showed
potentially high aSIdetrimental
exerting results. In the group
impact utilizing
on asphalt
binder performance, but in the result of the SIS binder using
Method B, it was observed that the G*/sin δ value exhibited a notably higher magnitude10% CRM, a higher content
of CRM
at the bottom. hindered
This isthe reaggregation
thought to occur of due
SIS. On the other
to the uneven hand, the groups
dispersion ofthat
the chose the
SIS modifier at
low-speed agitating method (B and D) showed high SI results. In the group utilizing
an elevated modifying temperature, leading to re-agglomeration and the subsequent set-
Method B, it was observed that the G*/sin δ value exhibited a notably higher magnitude
tlingatof
theabottom.
higher Thisconcentration
is thought totowards
occur due the
to bottom.
the uneven Conversely,
dispersion of with themodifier
the SIS addition of a
CRM up to 10%, certain SI values showed a tendency to decrease.
at an elevated modifying temperature, leading to re-agglomeration and the subsequent This phenomenon is
attributed
settling to
of athe increased
higher CRM particles,
concentration towards the which
bottom. areConversely,
consideredwith to impede
the addition the of
entangle-
a
CRM up to 10%, certain SI values showed a tendency to decrease.
ment of SIS at elevated temperatures. For Method D, the observed trend indicated lower This phenomenon is
attributed
SI values to the increased
compared to Method CRM particles, which are considered
B. This discrepancy can betoattributed
impede theto entanglement
the generally re-
of SIS at elevated temperatures. For Method D, the observed trend indicated lower SI
duced G*/sin δ values resulting from prolonged modification at a high temperature, which
values compared to Method B. This discrepancy can be attributed to the generally reduced
induces
G*/sindegradation in the polymer
δ values resulting from prolongedmolecular chain bonds
modification of SIS.
at a high Consequently,
temperature, which it was
observed
induces degradation in the polymer molecular chain bonds of SIS. Consequently, itto
that SIS, as a styrene block copolymer, exhibits significant sensitivity both the
was
modification
observed that method
SIS, asand temperature,
a styrene meaning
block copolymer, that it
exhibits is imperative
significant to identify
sensitivity the opti-
to both the
malmodification
modification conditions
method when employing
and temperature, meaning thatit asitaismodifier.
imperative to identify the optimal
modification conditions when employing it as a modifier.

Figure 9. G*/sin
Figure δ of δasphalt
9. G*/sin binders
of asphalt in in
binders each mixing
each mixingmethod
method for
for top,
top, middle, andbottom
middle, and bottomparts
parts after
conditioning.
after conditioning.
 3.2.2. SI Result Based on Jnr and % Rec
Using the MSCR evaluation method, the storage stability of the binder was asse
by calculating the SI based on the Jnr and % rec values as factors (Figures 10 and 11).
Materials 2024, 17, 2091 11 of 18
overall pattern observed in the SI results mirrored that of the SI results obtained from
G*/sin δ values. This indicates that the analysis of the modifier’s behavior based on
mixing3.2.2.
method aligns
SI Result Basedalmost
on Jnr andconsistently
% Rec with the assessment of the G*/sin δ value.
SI values obtained
Using the using Jnr showed
MSCR evaluation consistent
method, the storageresults across
stability both
of the loading
binder conditions w
was assessed
out notable variations. This is considered to occur because the range of Jnr The
by calculating the SI based on the Jnr and % rec values as factors (Figures 10 and 11). values is
overall pattern observed in the SI results mirrored that of the SI results obtained from the
tively narrow, typically
G*/sin δ values. This less thanthat
indicates 10the Kpa −1 , andofdoes
analysis not varybehavior
the modifier’s significantly
based onwhen
the calc
ing themixing
SI. Conversely, whenconsistently
method aligns almost computing with% therec, it becomes
assessment apparent
of the G*/sin that
δ value. The the
SI resu
values obtained
value fluctuates dependingusing J showed consistent results across both loading conditions
nr on the applied load. This is attributed to the increased se without
notable variations. This is considered to occur because the range of Jnr values is relatively
tivity of SI determination, as the result range spans from 0% to 100%, allowing for m
narrow, typically less than 10 Kpa−1 , and does not vary significantly when calculating
discernible
the SI.variations in % computing
Conversely, when rec values. % Specifically, with thethat
rec, it becomes apparent application
the resultingofvalue
a 3.2 kPa l
the % fluctuates
rec values were notably
depending higher
on the applied for
load. This allis binders,
attributed toalso
the showing that some
increased sensitivity of resul
SI determination, as the result range spans from 0% to 100%,
certain mixing methods were nearly double compared to when a 0.1 kPa load was app allowing for more discernible
variations in % rec values. Specifically, with the application of a 3.2 kPa load, the % rec
These outcomes are attributed to the enhanced clarity in measuring the binder’s elast
values were notably higher for all binders, also showing that some results of certain mixing
when subjecting
methods wereit to adouble
nearly relatively
compared higher
to when load.
a 0.1 kPaTherefore, when These
load was applied. assessing
outcomes the SI o
binderare
using the MSCR
attributed evaluation
to the enhanced clarity method,
in measuring it the
is anticipated thatwhen
binder’s elasticity the subjecting
storage stabili
it to a relatively higher load. Therefore, when assessing the SI of the binder using the
the binder will be scrutinized more sensitively by % rec applied with a 3.2 kPa load;
MSCR evaluation method, it is anticipated that the storage stability of the binder will be
can be scrutinized
utilized asmorea factor.
sensitively by % rec applied with a 3.2 kPa load; so, it can be utilized
as a factor.

Figure Figure
10. Jnr 10.
of Jasphalt binders
nr of asphalt binders inineach
each mixing
mixing method
method for top,
for top, middle, middle,
and bottom and
parts afterbottom parts after
conditioning.
ditioning.
als 2024, 17, x FOR PEER REVIEW 13
Materials 2024, 17, 2091 12 of 18

FigureFigure
11. %11.rec%ofrec
asphalt binders
of asphalt bindersinineach
each mixing method
mixing method for for
top,top, middle,
middle, and bottom
and bottom parts parts
conditioning.
after conditioning.

3.3. Comparative Analysis of the SI Based on Each Factor in Mixing Methods

3.3. Comparative Analysis of the SI Based on Each Factor in Mixing Methods
To evaluate the storage stability of the asphalt binder, the ASTM D7173 guidelines
To evaluate
mention theselection
that the storageof stability of purpose
a test for this the asphalt binder,
will vary dependingthe ASTM D7173 guide
on the polymer
modification system under evaluation and the specific information
mention that the selection of a test for this purpose will vary depending on sought by the user. Thethe pol
DSR test [40] is widely utilized for this purpose, while the MSCR Test [41] serves as an
modification system under evaluation and the specific information sought by the
alternative test option. Therefore, to derive factors for assessing storage stability, namely,
The DSR test [40]
calculating is widelytest
SI, individual utilized
methodsfor this
were purpose,
chosen (Figurewhile the MSCR
12). In general, Test in
variations [41] serv
an alternative testobserved
SI results were option.depending
Therefore, tochosen
on the derive factors
mixing method;forlower
assessing
SI resultsstorage
were stab
evident when employing the high-shear mixing approach. This is considered
namely, calculating SI, individual test methods were chosen (Figure 12). In general, to occur due
to differences in the reaction of the modifier, influenced by factors such as the modifica-
ationstion
in SI results
method, were observed
temperature, depending
and duration, on theinchosen
as mentioned the storagemixing method;
stability findings.lower
sults were evident
Moreover, whenwere
disparities employing
observed in the
thehigh-shear mixing
SI results across various approach.
test factorsThis is consid
within
each mixing method. Specifically, the evaluation of the MSCR test displayed
to occur due to differences in the reaction of the modifier, influenced by factors su variations
depending on the applied load, with higher SI results observed when a high load was
the modification method, temperature, and duration, as mentioned in the storage sta
applied. This is attributed to the heightened sensitivity of the high load to the elastic
findings. Moreover,
behavior disparities were observed in the SI results across various test fa
of the binder.
within each mixing method. Specifically, the evaluation of the MSCR test displayed
ations depending on the applied load, with higher SI results observed when a high
was applied. This is attributed to the heightened sensitivity of the high load to the e
behavior of the binder.
However, when evaluating Jnr as a factor, no significant difference was obse
across varying loads. This is likely because the result of the factor is less than 10 k
indicating a limited range that does not allow for the sensitive measurement o
binder’s SI. Therefore, for a more precise evaluation of SI, it is deemed preferable to u
% rec as a factor, given its broader range of values spanning from 0 to 100%, rather
deriving SI based on Jnr evaluations. Consequently, while the ASTM D7173 guidelines
mit the assessment of binder storage stability through DSR and MSCR tests, achie
Materials 2024, 17, x FOR PEER REVIEW 14 of 19
Materials 2024, 17, 2091 13 of 18

Figure 12. SI for each mixing method.

Figure 12. SI for each mixing method.

3.4. Statistical
However, Analysis
whenamong SI Results
evaluating Jnr as a factor, no significant difference was observed
across varying loads. This is likely because the result of the factor ispackage
less than −1 ,
A statistical analysis was conducted utilizing the IBM statistical for10the
kPasocial
indicating
sciences a limited
(SPSS) to carry range
out that does notof
an analysis allow for the
variance sensitive measurement
(ANOVA) of thesignificant
and Fisher’s least binder’s
SI. Therefore, for a more precise evaluation of SI, it is deemed
difference (LSD) comparison with a significance level of α = 0.05. The statistical preferable to utilize % rec as
design
wasa factor,
based given its broader
on evaluating rangeδ,of
G*/sin Jnrvalues
, and %spanning
rec in each from 0 to 100%,
mixing rather
method. Anthan deriving
ANOVA was
SI based on Jnr evaluations. Consequently, while the ASTM
initially performed to ascertain the significant differences among the sample means.D7173 guidelines permit theIn
assessment of binder storage stability through DSR and MSCR tests, achieving consistent
general, the SI results exhibited statistically significant differences depending on the mix-
results regarding the extent of separation of the modified binder between G*/sin δ, Jnr , and
ing method in the SIS asphalt binder with 5% CRM added. Specifically, in Method A, it
% rec parameter values has proven challenging.
was established that all SI results were statistically similar. However, significant differ-
ences
3.4. were observed
Statistical Analysis between
among SIthe SI results of different mixing methods (B, C, D), as
Results
shown A in statistical
Table 4. Similarly,
analysis was in conducted
the SIS asphalt binder
utilizing withstatistical
the IBM 10% CRM added,
package forcomparable
the social
results were found among the SI results in each method within the
sciences (SPSS) to carry out an analysis of variance (ANOVA) and Fisher’s least significant high-shear mixing
group (Table (LSD)
difference 5). Significant
comparison differences were notedlevel
with a significance amongof αthe SI results
= 0.05. in the low-speed
The statistical design
agitating
was basedgroup, except forG*/sin
on evaluating Method δ, JC.
nr , Consequently,
and % rec in each notable
mixingdistinctions
method. Anwere ANOVA generally
was
observed
initiallyamong
performed mixing methodsthe
to ascertain andsignificant
factors used to evaluate
differences SI. In
among summary,
the optingIn
sample means. for
general, the SI results exhibited statistically significant differences depending
the high-shear mixing method yielded a consistent pattern of SI results for each parameter on the mixing
method
value. in the SIS this
Nonetheless, asphalt binder with
uniformity 5% CRM
stemmed fromadded.
onlySpecifically, in Method
using a similar and lowerA, it was
SI by
established
factors that all
to calculate theSISIresults were
results. Thisstatistically
highlightssimilar.
the need However, significant differences
for comprehensive considera-
were
tion observed
between testbetween
methodsthe SI results
and evaluation of different
factors mixing methods
to analyze (B, C,
a broad D), asofshown
range in
SI results
Table 4.
effectively. Similarly, in the SIS asphalt binder with 10% CRM added, comparable results
were found among the SI results in each method within the high-shear mixing group
(Table 5). Significant differences were noted among the SI results in the low-speed agitating
group, except for Method C. Consequently, notable distinctions were generally observed
among mixing methods and factors used to evaluate SI. In summary, opting for the high-
shear mixing method yielded a consistent pattern of SI results for each parameter value.
Nonetheless, this uniformity stemmed from only using a similar and lower SI by factors to
calculate the SI results. This highlights the need for comprehensive consideration between
test methods and evaluation factors to analyze a broad range of SI results effectively.
Materials 2024, 17, 2091 14 of 18

Table 4. Statistical analysis of CRM5% + SIS10% asphalt binder for SI based on testing and mixing methods (α = 0.05).

CRM5% + SIS10%
G*/sin δ (kPa) Jnr (0.1 kPa−1 ) Jnr (3.2 kPa−1 ) % rec (0.1 kPa−1 ) % rec (3.2 kPa−1 )
A B C D A B C D A B C D A B C D A B C D
A - S S S N S S S N S S S N S S S N S S S
B - S S S N S N S N S N S S S S S S S S
G*/sin δ (kPa)
C - S S S S S S S S S S N S N S S S S
D - S S S S S S S S S S S S S S S S
A - S S S N S S S N S S S N S S S

Jnr B - S N S N S N S S S S S S S S
(0.1 kPa−1 ) C - S S S S S S S S S S S N S
D - S N S N S S S S S S S S
A - S S S N S S S N S S S

Jnr B - S N S S S S S S S S
CRM5% +
SIS10% (3.2 kPa−1 ) C - S S S S S S S N S
D - S S S S S S S S
A - S S S N S S S

% rec B - S N S S S S
(0.1 kPa−1 ) C - S S S S S
D - S S S S
A - S S S

% rec B - S N
(3.2 kPa−1 ) C - S
D -
N: non-significant; S: significant.
Materials 2024, 17, 2091 15 of 18

Table 5. Statistical analysis of CRM10% + SIS10% asphalt binder for SI based on testing and mixing methods (α = 0.05).

CRM10% + SIS10%
G*/sin δ (kPa) Jnr (0.1 kPa−1 ) Jnr (3.2 kPa−1 ) % rec (0.1 kPa−1 ) % rec (3.2 kPa−1 )
A B C D A B C D A B C D A B C D A B C D
A - S N S N S N S N S N S N S N S N S N S
B - S S S S S S S S S S S S S S S S S S
G*/sin δ (kPa)
C - S N S N S N S N S N S N S N S N S
D - S S S S S S S S S N S N S S S S
A - S N S N S N S N S S S N S S S

Jnr B - S S S N S S S S S S S S S S
(0.1 kPa−1 ) C - S S S N S N S N S N S N S
D - S S S N S S S S S N S N
A - S N S N S S S N S S S

Jnr B - S S S S S S S S S S
CRM10% +
SIS10% (3.2 kPa−1 ) C - S N S N S N S N S
D - S S S S S S S N
A - S N S N S N S

% rec B - S N S S S S
(0.1 kPa−1 ) C - S N S N S
D - S S S S
A - S N S

% rec B - S N
(3.2 kPa−1 ) C - S
D -
N: non-significant; S: significant.
Materials 2024, 17, 2091 16 of 18

4. Summary and Conclusions

The storage stability of asphalt binders was examined by utilizing G*/sin δ, Jnr , and
% rec as factors to assess a 10% SIS binder with the inclusion of a 5% and 10% CRM
content, both before and after conditioning using four mixing methods. The findings of
this investigation led to the following conclusions.
(1) Overall, the addition of the modifier increased the G*/sin δ values, correlating with the
CRM increase. Additionally, different mixing methods and modifier contents resulted
in varied effects on G*/sin δ. Groups with a low-speed mixing for 6 h exhibited lower
G*/sin δ values, indicating a suboptimal SIS performance based on the chain cracking
of SIS. These results emphasize the importance of considering modifying the methods
and duration for optimal binder performance.
(2) The rheological properties using Jnr and % rec revealed consistent trends similar to
G*/sin δ evaluation, indicating a decreasing Jnr value and increasing % rec value
with a higher CRM content. In general, under a low load (0.1 kPa), lower Jnr and
higher % rec values suggest improved elastic recovery than under a load of 3.2 kPa.
Moreover, using higher loads (3.2 kPa) and a long-term modification method showed
a significant decrease in elasticity, highlighting increased sensitivity compared to the
G*/sin δ evaluation. These findings emphasize the clearer understanding of reduced
elasticity in modified binder under prolonged high-temperature modification.
(3) The storage stability of the binder was evaluated using G*/sin δ, revealing consistent
trends in the high-shear mixing groups (A and C) with a downward SI trend, indicating
uniform modifier dispersion. The low-speed mixing groups (B and D) showed an ele-
vated SI, possibly due to the uneven SIS dispersion causing re-agglomeration. Method
D exhibited a lower SI compared to Method B, which is attributed to the increased
G*/sin δ values of bottom part from prolonged high-temperature modification, indicat-
ing SIS sensitivity to modification conditions. Thus, SIS exhibits significant sensitivity
to both the modification method and temperature during asphalt binder modification.
(4) The storage stability of the binder was evaluated using the MSCR method, which
involved calculating the SI based on Jnr and % rec values. Jnr -based SI values showed
consistency across loading conditions due to the narrow range of Jnr values, whereas
the % rec-based SI exhibited fluctuation, attributed to its wider range. Particularly, at
a 3.2 kPa load, the % rec values significantly increased, indicating enhanced elasticity
measurement under higher loads. Thus, % rec with a 3.2 kPa load is effective for the
sensitive evaluation of binder storage stability using the MSCR method.
(5) Jnr , a factor in evaluating the storage stability, shows no significant difference across
varying loads, likely due to its limited range (<10 kPa−1 ), hindering sensitive SI
measurement. Thus, % rec is preferred for precise SI evaluation, offering a broader
range (0 to 100%). In addition, despite the ASTM D7173 guidelines permitting DSR
and MSCR tests for binder assessment, achieving consistent results regarding modified
binder separation between G*/sin δ, Jnr , and % rec parameters remains challenging.
These results also unveiled variances through statistical analysis.
(6) This research exclusively employed a CRM and SIS; hence, the investigation into the
behavior of other modifiers is required. In the future, a comprehensive analysis will
likely necessitate the inclusion of diverse modifiers and a deeper examination of their
direct influence on asphalt mixtures. Furthermore, to assess the degree of separation
between the binder and the modifier, along with conducting a phase separation analy-
sis of the binder, it is crucial to consider suitable evaluation factors. It is anticipated
that endeavors will be required to establish an optimal evaluation method.

Author Contributions: Conceptualization, S.-J.L.; Formal analysis, M.-S.L.; Data curation, J.Y. and
S.V.; Writing—original draft, J.Y.; Writing—review & editing, H.K.; Supervision, S.-J.L. All authors
have read and agreed to the published version of the manuscript.
Materials 2024, 17, 2091 17 of 18

Funding: This research was supported by a grant from a government funding project (2024 National
Highway Pavement Management System).
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: Data are contained within the article.
Conflicts of Interest: The authors declare no conflicts of interest.

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