International Journal of Adhesion & Adhesives 134 (2024) 103802

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International Journal of Adhesion and Adhesives

journal homepage: www.elsevier.com/locate/ijadhadh

Performance assessment of composite modified bitumen integrated with

desulfurized crumb rubber and SBS modifier as waterproofing
adhesive layer
Jizhe Zhang a , Weidong Cao a, * , Weihua Li b , Shurong Lou b , Wenwu Zhang c , Zongliang Hou a, **
a
School of Qilu Transportation, Shandong University, Jinan, 250061, China
b
Shandong High Speed Group Weifang Development Co. LTD, Weifang, 262500, China
c
Shandong HI-SPEED Group, Shandong Expressway Building, 8# Longao North Road, Lixia District, Jinan, 250014, China

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

Keywords: Performance of the waterproofing adhesive layer played a critical role for governing duration of bridge deck
Waterproofing adhesive layer paving system due to harsh service conditions. To develop a new type of modified bitumen suitable for the layer
Composite modified bitumen (CMB) between bridge deck and overlaid asphalt, this study investigated the performance of composite modified
Desulfurized crumb rubber (DCR)
bitumen (CMB) integrated with desulfurized crumb rubber (DCR) and SBS modifier. The influence of DCR and
SBS modifier
Bonding strength
SBS additive on rheological behavior, high-temperature performance, low-temperature cracking resistance, and
adhesive performance of CMB was investigated by adopting various experimental tests, which including pene-
tration, ductility, softening point, Brookfield viscosity, dynamic shear rheometer (DSR), bending beam rheometer
(BBR), and bonding strength. The high-temperature stiffness and low-temperature flexibility of CMB was
improved after composite modification, which in turn contributed to the shear and cracking resistance. The black
diagram indicated that the formation of polymer network in the CMB improved the viscous flow resistance and
maintained elastic response at high in-service temperature. The bonding strength and moisture stability of the
composite bitumen-concrete interface were enhanced, with the properties exceeded the commercial SBS modi-
fied bitumen. The CMB binders R18S2 and R18S3 presented good performance and can be used for water-
proofing adhesive layer as a substitute of the commercial SBS modified bitumen.

1. Introduction waterproof bonding system played an important role on the service

performance of the overlaid pavement [5].
Reinforced concrete bridge is widely used in the road network. In Because of the importance of the waterproof bonding system, many
order to provide good driving comfort and supply adequate protection, attempts have been conducted to improve its properties. Zhou and Xu
the concrete bridge deck is normally overlaid by asphalt mixtures. Due [6] studied the adhesion properties of waterproof membranes subjected
to this complicated pavement structure, the bridge deck overlay has to to several service conditions, indicating that the coat material thickness,
suffer large shear stress under heavy vehicle loads [1]. It can often suffer concrete surface roughness and compaction temperature played an
large flexural deflection due to its complex supporting conditions and important role for the adhesion strength. The optimal parameters had
long-span, which in turn induces large strain to the overlaid asphalt been finally revealed and the related waterproof membrane material
pavement [2]. Because of these reasons, distresses of cracking and was designed based on the developed guidance. Liu et al. [7] developed
interfacial debonding usually presented at the asphalt overlays on con- a shear test device and employed to optimize the shear performance of
crete bridge decks due to repeated traffic loading and temperature ERS (Epoxy Bonding Chips Layer + Resin Asphalt + SMA) pavement
attacking [3,4]. It is recognized that the interface between overlaid interlayer. The influence of bonding material, aggregate type, surface
pavement and concrete bridge deck is vulnerable, and the quality of the treatment on the final properties of the ERS pavement system was

* Corresponding author.
** Corresponding author.
E-mail addresses: jizhe.zhang@sdu.edu.cn (J. Zhang), cwd2001@sdu.edu.cn (W. Cao), wfglsj@163.com (W. Li), sdgs144@163.com (S. Lou), 147849246@qq.com
(W. Zhang), hzl9602@mail.sdu.edu.cn (Z. Hou).

https://doi.org/10.1016/j.ijadhadh.2024.103802
Received 17 October 2023; Received in revised form 17 July 2024; Accepted 23 July 2024
Available online 25 July 2024
0143-7496/© 2024 Elsevier Ltd. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
J. Zhang et al. International Journal of Adhesion and Adhesives 134 (2024) 103802

investigated. It had been revealed that the irregular rough interface can the viscoelasticity and cracking resistance of bitumen. When the SBS
contribute to form interlayer with high shear resistance. The frequently modifier admixture exceeded 1 %, a network structure can be formed in
acceleration and brake of vehicles induce high shear stress and this is the bitumen structure and its performance was improved obviously
more susceptible to lead interlayer shear failure. In addition, high ser- [17]. To further understand the formation of polymer network as well as
vice temperature reduces the shear strength of interlayer which in turn the hybrid effect of SBS modifier and rubber powder, it would be
accelerates the shear failure. Guo et al. [8] evaluated the water important to systematically evaluate the optimization and performance
permeability, shear strength and extensional strength of different of the composite modified bitumen synthesized with crumb rubber
waterproof bonding materials. The results indicated that all waterproof powder and SBS modifier.
bonding materials had temperature sensitivity and their shear strength Inspired by previous researches, the main aim of this research was to
as well as tensile strength decreased when temperature elevated. Based investigate the influence of SBS/crumb rubber on the performance of
on comparison, the SBS modified bitumen presented better shear resis- CMB and characterize its possibility to be used as waterproofing adhe-
tance than other materials. Fang et al. [9] evaluated the shear resistance sive layer between bridge deck and asphalt overlayed surface. Perfor-
and fatigue life of different waterproof adhesive products by using direct mance of the developed CMB was evaluated by using Softening point
shear test and shear fatigue test. The influence of disposal schemes, test, Penetration test, Ductility test, Dynamic Shear Rheometer (DSR)
material selection, spreading approaches and material dosage on the test, and Bending-Beam Rheometer (BBR) test. In addition, the tensile
mechanical performance of waterproof cohesive layers were character- strength and moisture resistance of the bitumen-concrete interface was
ized with the fatigue prediction equation was finally established. Sun evaluated by using bonding strength test.
et al. [10] investigated the mechanical behavior of epoxy asphalt ad-
hesive (EAA) as the waterproof-bonding layer of the orthotropic steel 2. Materials and experimental methods
bridge decks. With respect to improve the properties of the EAA, atta-
pulgite clay was employed as a type of nano-filler and incorporated into 2.1. Materials
EAA. It is demonstrated that the incorporation of attapulgite enhanced
the tensile strength, modulus and adhesive behavior of EAA. Xu et al. The base bitumen (BA) used in this study was a type of heavy-duty
[11] investigated the influence of several critical factors on the adhesive road bitumen with a penetration grade of Pen 60/80, which was pro-
behavior of waterproofing adhesive layer (WAL) by using experimental duced by one Road Material Technology Co, Shandong, China. The
tests and finite-element (FE) modeling method. The results indicated commercial SBS modified bitumen (5 % SBS) selected as the control was
that the adhesive strength of WAL significantly influenced by the also produced by the same company. The DCR was a type of lightly
compaction temperature, environmental temperature, surface rough- pyrolyzed tire rubber obtained by twin-screw extruder at 220 ◦ C and
ness and overlay thickness. followed by mechanical disruption to obtain particle size of 40 mesh.
In order to achieve strong bonding between bridge deck and asphalt The SBS modifier was a type of linear SBS that was supplied by Sinopec,
layer, the methacrylate-based adhesive (MMA) was also used for pro- China. The basic performance of base bitumen and the SBS modified
duce waterproof adhesive layer (WAL). The n-butyl acrylate (nBA) was bitumen are listed in Table 1.
incorporated by using emulsion polymerization to overcome the brit-
tleness of MMA. This modification method improved the adhesion be- 2.2. Preparation of CMB
tween steel plate and asphalt surface. Molecular dynamics (MD)
simulation revealed that the van der Waals force experienced obvious In order to obtain the optimal proportion of CMB, the influences of
increase after nBA modification and this was the main reason for the both modifier dosages of SBS and DCR on the bitumen performance were
enhancement of adhesion [5]. To prevent the reflective cracks of asphalt investigated. The SBS dosage selected by mass to the base bitumen was
pavement caused by the negative bending moments of continuous beam 1 %, 2 %, 3 %, respectively and the DCR powder was 12 %, 15 %, 18 %,
bridge, a type of composite stress absorbing layer (CSAL) incorporating respectively. In this study, an external addition method was adopted and
geotextile and asphalt gravel seal, was developed [3]. Experimental the material mix designs are listed in Table 2.
results indicated that the CSAL was able to improve the cracking resis- By preparing CMB, the base bitumen was first packed in a bucket and
tance of bridge deck pavement by more than 5 times at low service kept at a constant temperature of 170 ◦ C in an oven for 1 h. The DCR and
temperatures. Moreover, its cracking resistance at a large deformation SBS modifier with predetermined dosages were then incorporated into
amplitude (2 mm) was also better than that of the asphalt rubber the hot bitumen with thoroughly mixing, and followed by 1 h condition
stress-absorbing membrane interlayer (ARSAMI). at 170 ◦ C. With respect to reduce the particle size of modifier to obtain
As abovementioned, the waterproofing adhesive layer played an CMB with homogeneous mixing, the high-speed shearing equipment
important role in the service properties of oveylaid asphalt mixtures. was employed at a shearing speed of 5000 rpm for 1 h, and the tem-
The commonly used SBS and rubber modified bitumen seem to hardly perature controlled at 180–190 ◦ C. Finally, the prepared CMB was
meet sufficient bonding durability. To effectively utilize complementary placed in an oven at 170 ◦ C for another 1 h to swell [18].
benefits of SBS additive and crumb rubber, a concept of SBS/crumb
rubber composite modified bitumen has been put forward by some re-
searches [12]. An economic analysis of SBS/crumb rubber composite
modified bitumen indicated that this type of modified bitumen not only Table 1
had better performance, but also had lower cost, which was of a great Conventional performance of base bitumen and SBS modified bitumen.
practical potential [13,14]. The rheological behavior, thermal-oxidative Technical index Base SBS modified Test
aging behavior and storage stability of SBS/rubber powder composite bitumen bitumen methoda
modified bitumen, were tested and the swelling mechanism and swelling 25 ◦ C Penetration/0.1 mm 60.3 58 T0604-
kinetics of waste rubber in the modified bitumen was analyzed [15]. A 2011
low dosage of rubber powder can effectively mitigate the problem of Ductility/cm > 100 30.7 (5 ◦ C) T0605-
(15 ◦ C) 2011
high viscosity and segregation of SBS/waste rubber powder in the Softening point/◦ C 45.1 80.2 T0606-
composite modified bitumen. Improvement of this type of composite 2011
modified bitumen can be also done by the furfural extracted oil, which 135 ◦ C Brookfield viscosity/ 0.52 2.50 T0625-
has a good swelling effect on the rubber powder, and it can increase the Pa⋅s 2011
ductility of SBS/rubber powder composite modified bitumen [16]. Liang a
Test methods were specified in Standard Test Methods of Bitumen and
et al. proposed that the SBS modifier and rubber particles can enhance Bituminous Mixtures for Highway Engineering (China).

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J. Zhang et al. International Journal of Adhesion and Adhesives 134 (2024) 103802

Table 2 2.3.6. Bending beam rheometer (BBR) test

Mix design of CMB. The BBR test was used to characterize the creep response of bitumen
Test number DCR dosage SBS modifier dosage Sample ID at low temperature. In this research, the BBR test was performed by
using asphalt samples after short term aging (Rolling Thin Film Oven
1 12 % – R12
2 12 % 1% R12S1 Test) at − 18 ◦ C and a stable load of 980 ± 50 mN was applied. The
3 12 % 2% R12S2 deflection of the bitumen beam was recorded to calculate creep stiffness
4 12 % 3% R12S3 (S) and m-value (m). Based on JTG E20-2011 standard, the creep stiff-
5 15 % – R15 ness (S) should be lower to reduce thermal stress, while a greater m-
6 15 % 1% R15S1
7 15 % 2% R15S2
value was desired to guarantee stress relaxation.
8 15 % 3% R15S3
9 18 % – R18 2.3.7. Bitumen-concrete bonding strength test
10 18 % 1% R18S1 In order to characterize the bonding strength of the developed
11 18 % 2% R18S2
modified bitumen with concrete bridge decks, an adhesion test (Positest
12 18 % 3% R18S3
13 70# base bitumen BA AT-A equipment) was employed, as shown in Fig. 1. The Positest AT-A is
14 SBS modified bitumen SBS an equipment that can generate a constant rate of pull pressure to
separate the adhesive layer of bitumen-substrate interface. To simulate
the adhesive condition of the waterproof layer on concrete bridge deck,
2.3. Experimental methods a self-made concrete slab was employed as the substrate. The specimens
were prepared by pouring hot bitumen onto the concrete substrate and
2.3.1. Penetration test followed by pressing a pull-stub onto the bitumen film [19]. After
In order to investigate the influence of polymer additives on the cooling down, the exceed bitumen around the edge was removed and a
grade level of modified bitumen, the penetration test was performed. good bitumen-concrete bonding was finally obtained. The test was
The penetration test was used to measure the depth of a standard needle performed at 20 ◦ C and the tensile strength was obtained automatically.
penetrated into the bitumen vertically under a certain load, time and Except for the test in dry condition, samples were experienced in the
temperature. This test was performed at 25 ◦ C with the load of 100 g and water bath at 20 ◦ C for different duration periods (3 days and 7 days)
loading time of 5 s, with detailed procedures described at T0604-2011. and the residual tensile strength was employed to reflect the moisture
stability of the bitumen-concrete bonding.
2.3.2. Ductility test
Ductility test was performed to evaluate the prolongation of bitumen 3. Results and discussion
at a certain temperature and a certain speed until to fail. Ductility in-
dicates to the ability of bitumen to withstand plastic deformation, 3.1. Penetration of CMB
reflecting both low temperature crack resistance and shearing sensitivity
of bitumen. In this study, ductility test was carried out at 5 ◦ C to char- The penetration values of composite modified binders prepared with
acterize the cracking resistance of CMB at low temperature in accor- different dosages of DCR and SBS modifier are shown in Fig. 2. The base
dance with T0605-2011. bitumen had the highest penetration, followed by the commercial SBS
modified bitumen (the control). The addition of DCR and SBS modifier
2.3.3. Softening point test reduced the penetration value. Under the same DCR dosage, incorpo-
Softening point test was used to measure the temperature at which rating the SBS modifier resulted in a reduction in penetration. Similarly,
steel ball first touches bottom shelf at a certain heating rate. This tem- the penetration value can also be reduced by increasing the DCR dosage,
perature is a critical indicator at which the bitumen changes from visco- but its improvement effect was not as obvious as increasing the SBS
elastic state to viscous state. The softening point is an indicator to reflect modifier dosage. The penetration values of DCR modified binders (S12
the deformation resistance of bitumen with higher value indicating and S15) were higher than that of the control. Further increasing DCR
better high temperature stability. The specific testing procedures are
described according to T0606-2011.

2.3.4. Brookfield viscosity test

A rotational viscometer (Brookfield DV-2) was used to measure the
rotational viscosity of composite modified binders. The selection of rotor
size is based on the viscosity of the bitumen tested to make sure the
torque level is in the right range. The viscosity was obtained by deter-
mining the torque required to spin the spindle-shaped shaft in the
bitumen at different temperatures (120 ◦ C, 140 ◦ C, 160 ◦ C and 180 ◦ C).
The spinning speed was 20 rpm with the torque guaranteed at 10 %–98
% of the equipment range by changing the shaft size. The specific testing
procedures are described in the Chinese standard JTG E20-2011
(T0625).

2.3.5. Dynamic shear rheometer (DSR) test

The rheological properties of modified bitumen were evaluated by
using DSR under sinusoidal loading mode (T0628-2011). The test was
performed in the temperature range of 40 ◦ C–88 ◦ C by using tempera-
ture sweep mode at a fixed shear frequency of 10 rad/s. The parallel
plate with the diameter of 25 mm was selected and the film thickness
was controlled at 1 mm. Parameters of complex shear modulus (G*) and
phase angle (δ) were obtained automatically.
Fig. 1. Equipment and specimen used for bitumen-concrete bonding
strength test.

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J. Zhang et al. International Journal of Adhesion and Adhesives 134 (2024) 103802

temperature performance are.

It has been reported that at low temperature, the interaction between
molecules in the base bitumen becomes weakened significantly, while
the SBS modifier has good deformation capacity to resist it [20]. In the
modified bitumen, the network cross-linking structure produced by two
modifiers can be deformed along the direction of the induced external
forces. Meanwhile, excellent elasticity of DCR can dissipate stress
effectively. Thus, the ductility value increased continuously with the
increase of SBS modifier and DCR. However, when the dosages of the
SBS modifier and DCR exceeded to a certain level, swelling would be
insufficient due to excessive light components from the base bitumen so
that its low temperature ductility was reduced. Based on China specifi-
cations JTG F40-2004, most of the composite modified binders exceeded
the required value.

3.3. Softening point of CMB

Softening point is an important indicator to evaluate high tempera-

ture stability and temperature sensitivity of bitumen. The softening
Fig. 2. Penetration of composite modified binders. point values of the CMB with different dosages of DCR and SBS modifier
are shown in Fig. 4. In a certain range, a higher softening point value
dosage or incorporating SBS modifier reduced the penetration, with indicating better high temperature stability. The softening point of each
values lower than that of the control. Previous researches have reported CMB was greater than that of the base bitumen, indicating that both two
that the light components in the bitumen would be adsorbed by the DCR modifiers of DCR and SBS modifier improved its high temperature sta-
and the SBS modifier, and resulted in a swelling effect [15]. Subjected to bility significantly. When the DCR dosage was constant, the softening
high-speed shearing at high temperature, DCR and SBS modifier were point of the CMB tends to gradually increased with the increase of SBS
homogenously dispersed in the bitumen and formed a three-dimensional modifier. If the SBS modifier dosage was constant, the softening point of
network structure. This network structure restricted the mobility of the CMB showed a trend of decreasing at first and then increasing with
bitumen so as to decrease the penetration. the addition of DCR. This implied that when the DCR was excessive, it
would lead to its insufficient swelling in the bitumen. During the prep-
aration of modified bitumen, SBS modifier and DCR should be dispersed
3.2. Ductility of CMB
in the bitumen uniformly. Both two modifiers absorb the light oil frac-
tions of base bitumen and undergo swelling, resulting in more viscous
Ductility results of CMB designed with different dosages of DCR and
and thus an increase in the softening point [21].
SBS modifier are shown in Fig. 3. Based on JTG F40-2004, the ductility
of polymer modified bitumen should be ≥ 20 cm at 5 ◦ C so as to guar-
3.4. Viscosity of CMB
antee its low-temperature performance. Incorporating DCR with 12 %
dosage can improve the ductility from 0.8 cm to 17.0 cm, and increasing
Viscosities of the composite modified binders were measured by
the DCR dosage has limited contribution to this parameter. With respect
using the Brookfield viscometer, and the results are shown in Fig. 5. The
to composite modification, further incorporating SBS modifier resulted
Brookfield viscosity is mainly used to predict the production and
in obvious increase in the ductility with the value reached to over 25.0
compaction performance of the related asphalt mixtures. It is clear that
cm. This indicated that the low temperature performance and plasticity
the viscosity of composite modified binders decreased with the increase
of the developed CMB would be much greater than that of the base
of testing temperature. The addition of SBS modifier or DCR resulted in
bitumen, and close to that of the control. Similarly, ductility of the CMB
an obvious increase in terms of the viscosity, especially at 120 ◦ C and
tended to increase after adding the SBS modifier. The greater the
140 ◦ C. This would imply that the addition of these two polymer
ductility value is, the better the bitumen plasticity and the low

Fig. 3. Ductility of composite modified binders. Fig. 4. Softening point of composite modified binders.

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J. Zhang et al. International Journal of Adhesion and Adhesives 134 (2024) 103802

Fig. 6. Complex shear modulus of composite modified binders.

Fig. 5. Viscosities of composite modified binders at different temperatures.

decreased gradually with the increase of temperature. By comparing
with the base bitumen, composite modified binders obtained greater
components improved the elasticity and viscosity of the CMB. With
complex modulus, indicating that the addition of SBS modifier and DCR
respect to evaluate the temperature sensitivity of the prepared com-
improved the deformation resistance and high temperature stability of
posite modified binders, the parameter of viscosity temperature index
related binders. This could be due to that the SBS modifier and DCR
(VTS) was employed.
formed a network cross-linking structure with the base bitumen, which
Table 3 lists the linear analysis of viscosity versus temperature for
in turn improved the elasticity and the deformation resistance of com-
composite modified binders. The equation of linear regression was ob-
posite modified binders [22]. Compared with the control, six composite
tained by taking double logarithm of viscosity and logarithm of Kelvin
modified binders, R12S3, R15S2, R15S3, R18S1, R18S2, R18S3 behaved
temperature, where the absolute value of the equation slope was called
better high temperature stability and deformation resistance. Among
viscosity temperature index (VTS). The VTS is often used to evaluate the
them, R18S3 CMB had the smallest variation and the best performance.
temperature sensitivity of bitumen in pavements. A smaller VTS value
means a slow change of binder viscosity with temperature, indicating
3.5.2. Phase angle of CMB
better temperature stability. Based on this principle, four modified
The phase angles of composite modified binders designed with
binders, R12S3, R15S2, R18S1 and R18S3, behaved better temperature
different dosages of desulfurized rubber powder DCR and SBS modifier
stability.
are shown in Fig. 7. The phase angle δ is an angle created when the si-
nusoidal stress input into the material is not synchronized with the si-
3.5. Rheological performance of CMB nusoidal strain response generated by the material. A bitumen with
larger phase angle δ indicating greater proportion of viscosity compo-
3.5.1. Complex shear modulus of CMB nents. The phase angle δ showed a decreasing trend with an increase of
The complex shear moduli of composite modified binders were the SBS modifier and DCR dosage. This indicated that both SBS modifier
measured by using the DSR and the related results are shown in Fig. 6.
The complex shear modulus G* is an indicator of total resistance of a
material to the repeated shear deformation, which consists of two parts:
the real part of the storage elastic modulus and the imaginary part of the
loss elastic modulus. A large G* value of the bitumen indicating good
deformation resistance. The complex shear modulus of each CMB

Table 3
Viscosity versus temperature analysis of composite modified binders.
Sample ID Regression equation R2 VTS

R12 y =− 2.5108x + 7.0514 0.9961 2.5108

R12S1 y =− 2.2736x + 6.4528 0.9904 2.2736
R12S2 y =− 2.1074x + 6.0395 0.9992 2.1074
R12S3 y =− 1.6576x + 4.8821 0.9164 1.6576
R15 y =− 2.2977x + 6.5155 0.9997 2.2977
R15S1 y =− 2.0233x + 5.8184 0.9990 2.0233
R15S2 y =− 1.8633x + 5.42 0.9895 1.8633
R15S3 y =− 2.1776x + 6.2596 0.9840 2.1776
R18 y =− 2.1824x + 6.2372 0.9985 2.1824
R18S1 y =− 1.7841x + 5.2176 0.9961 1.7841
R18S2 y =− 2.1565x + 6.2021 0.9974 2.1565
R18S3 y =− 1.9932x + 5.7956 0.9833 1.9932
BA y =− 3.3814x + 9.2189 0.9998 3.3814
SBS y =− 2.966x + 8.2658 0.9991 2.9660
Fig. 7. Phase angles of composite modified binders.

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J. Zhang et al. International Journal of Adhesion and Adhesives 134 (2024) 103802

and DCR are dispersed in the bitumen and restricts the flow of it. The Table 4
DCR has a certain elasticity, which enhances the resistance to permanent Fitting results of the rutting parameter VS temperature of CMB binders.
deformation of the CMB. At the temperature below 64 ◦ C, the elasticity Sample ID Fitting data
recovery of each CMB was higher than that of the control. As the tem-
Equation A B R2
perature exceeded 64 ◦ C, the elasticity recovery properties of two
− 0.112x
composite modified binders, R18S2 and R18S3, were nearly equivalent R12 y = 9324.6e 9324.6 − 0.112 0.9985
R12S1 y = 12826e− 0.109x 12826 0.109 0.9989
to that of the control.
−
R12S2 y = 11501e− 0.104x 11501 − 0.104 0.9994
R12S3 y = 9558.5e− 0.098x 9558.5 − 0.098 0.9994
3.5.3. Rutting parameter of CMB R15 y = 6712.2e− 0.103x 6712.2 − 0.103 0.9988
Rutting parameter can be calculated by G*/sinδ, which is an indi- R15S1 y = 10833e− 0.104x 10833 − 0.104 0.999
R15S2 y = 11081e− 0.102x 11081 0.102 0.9991
cator of high temperature performance of related asphalt pavement. The −
R15S3 y = 9865.7e− 0.098x 9865.7 − 0.098 0.9993
higher rutting parameter indicating stronger rutting resistance of the R18 y = 5313.1e− 0.096x 5313.1 − 0.096 0.9985
related pavement at high temperature. As shown in Fig. 8, the rutting R18S1 y = 9205.8e− 0.1x 9205.8 − 0.1 0.9992
parameter of each CMB decreased gradually with the increase of tem- R18S2 y = 7573.6e− 0.094x 7573.6 − 0.094 0.9993
perature. Among them, the base bitumen had the smallest rutting R18S3 y = 8253.1e− 0.093x 8253.1 − 0.093 0.9996
BA y = 16084e− 0.131x 16084 0.131 0.9988
parameter than that of other modified binders. Compared with the
−
SBS y = 5909.4e− 0.095x 5909.4 − 0.095 0.9994
control, five composite modified binders, R12S3, R15S3, R18S1, R18S2,
R18S3, showed greater rutting parameters, indicating their better tem-
perature stability. Among them, the high temperature stability of R18S2 3.5.4. Black diagrams
was equivalent to that of the control basically, and the best high tem- Black diagrams are plotted by using the value of complex modulus
perature stability belongs to R18S3. versus phase angle and employed as a indicator of thermo-rheological
The development of rutting parameter with the change of tempera- simple and complex materials [23]. The black diagrams for the CMB
ture was used to characterize the temperature stability of modified are presented in Fig. 9. The phase angle of base bitumen reduced
binders. The change of rutting parameter with temperature can be gradually with the decrease of complex modulus, indicating
expressed by the following equation: thermo-rheological simplicity of this binder. By only adding DCR, the
/ increase of DCR dosage produced an increase in the elastic response with
G∗ sin δ = AeBT (1) the phase angle declining at the same level of complex modulus. It was
noticed that the black diagrams of DCR modified binder cannot seen
Where, G*/sinδ is the rutting parameter, KPa; T is the temperature, ◦ C;
obvious plateau region and the binder still exhibited time-temperature
A, B is the regression coefficient.
superposition principle (TTSP) applicability. Under the same DCR
Based on this equation, a smaller absolute value of B indicated better
dosage, incorporation of SBS modifier resulted in the black diagrams
temperature stability of the CMB. The regression results of the rutting
shifts to lower phase angles and made the plateau region more obvious
parameter and temperature for different composite modified binders are
with the constant phase. This phenomenon suggests that the composite
shown in Table 4. In general, the temperature stability of the CMB
modification by using DCR and SBS modifier can contribute to the for-
increased with an increase of the SBS modifier (or DCR). This indicated
mation of polymer network, which improved the viscous flow resistance
that the addition of both modifiers can increase the non-deformability
and maintain elastic response of related binder at high in-service tem-
and deformation recovery of the bitumen, which improved the tem-
perature. The CMB binders (R12S3, R15S3, R18S2, and R18S3) showed
perature stability of bitumen. It was also found that five CMB binders
relatively similar even better elastic response behavior compared with
(R12S3, R15S2, R18S1, R18S2 and R18S3) and the control had small B
the control.
value and excellent high temperature stability. Therefore, using hybrid
modifiers can be considered to enhance high temperature stability and
permanent deformation resistance of CMB. 3.6. Low temperature cracking resistance of CMB

The cracking resistance of modified binders were measured at

− 18 ◦ C by using the bending beam rheometer (BBR) test, and the results
are presented in Figs. 10 and 11, respectively. It has been recognized

Fig. 8. Rutting parameters of composite modified binders. Fig. 9. Black diagrams of composite modified binders.

6
J. Zhang et al. International Journal of Adhesion and Adhesives 134 (2024) 103802

Fig. 12. Bonding strength of different concrete-bitumen substrate interfaces in

both dry and wet conditions.
Fig. 10. Creep stiffness values of CMB at − 18 ◦ C.
highest bonding strength of the concrete-bitumen interface was ob-
tained after composited modification and the moisture conditioning
deteriorated the adhesive performance. In the dry condition, incorpo-
rating DCR improved the bonding strength of the modified bitumen in
comparison with the base bitumen, but further increasing DCR dosage
from 12 % to 18 % cannot improve the adhesive behavior obviously. At
the same DCR dosage, adding SBS modifier not only had no contribution
to the adhesive performance, but also reduced the bonding strength as
the DCR dosage exceeded 15 %. It demonstrated that the DCR played an
important role in improving the bonding performance of composited
modified bitumen in the dry condition. In order to characterize the
moisture resistance of concrete-bitumen substrate interfaces, the resid-
ual bonding strength defined as the ratio of bonding strength after 7 days
of moisture to that of the value in the dry condition, as shown in Fig. 13.
It revealed that using DCR can improve the bonding strength in dry
condition, but it seemed to hardly contribute to the residual bonding
strength after moisture conditioning. As the SBS modifier was added, the
residual bonding strength of CMB was enhanced gradually with the in-
crease of SBS modifier dosage. By comparing with the control, several
specimens showed higher residual bonding strength due to composite
modification, especially R18S2 and R18S3. It indicated that the CMB by
Fig. 11. M-values of CMB at − 18 ◦ C. incorporating DCR and SBS modifier can obtain better adhesive per-
formance with concrete in both dry and wet conditions.
that the bitumen behaves good cracking resistance if having small creep With respect to utilize CMB for waterproofing adhesive layer on
stiffness and/or big m-values. Due to its high creep stiffness and low s- concrete bridge, the CMBs should have good high-temperature stability,
value, the base bitumen does not show good cracking resistance. In
contrast, the commercial SBS modified bitumen behaved much better
cracking resistance because of the addition of elastomer component. The
addition of DCR resulted in a decreased creep stiffness and an increased
m-value. It indicated that the DCR had positive effect on the cracking
resistance of modified bitumen. As the DCR increased to 12 %,
increasing its dosage cannot resulted in further increase in terms of the
m-value. This is because large amount of DCR dosage absorb more light
oil fractions from the base bitumen, which reduced the deformability of
related modified bitumen. At the same DCR dosage, adding the SBS
modifier reduced the creep stiffness of the related CMB. It demonstrated
that the DCR can improve the flexibility of bitumen and result in a better
low-temperature performance. However, the SBS modifier had limited
contribution to the m-value.

3.7. Bonding strength and moisture resistance of concrete-bitumen

interfaces

The Positest AT-A equipment was used to evaluate the bonding

strength of concrete-bitumen interfaces in both dry and wet conditions Fig. 13. Residual bonding strength of different concrete-bitumen substrate
and the results are presented in Fig. 12. For each type of bitumen, the interfaces after 7 days of moisture condition.

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J. Zhang et al. International Journal of Adhesion and Adhesives 134 (2024) 103802

low-temperature cracking resistance and moisture resistance. Based on National key research and development plan of China
these requirements, parameters of ductility, softening point, rutting (NO.2022YFB2603300, NO.2022YFB2603303), Shandong Trans-
parameter, creep stiffness, m-values, and residual bonding strength were portation Technology Plan (2020B66, 2019B47-1) and the Fundamental
employed for comprehensive analysis. It can be demonstrated that the Research Funds for the Central Universities, CHD (300102210507).
R18S2 and R18S3 obtained comparable high-temperature stability and
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Acknowledgement

The authors would like to acknowledge the financial support of