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This document discusses a study that evaluated asphalt modified with bio-oil and high rubber content under low temperature and short mixing time production conditions. The study prepared rubber and bio-oil modified asphalt (BRMA) with 20% crumb rubber content and 5%, 10%, or 15% bio-oil content at 160°C for 30 minutes of mixing. Tests found that bio-oil addition significantly reduced the viscosity increase typically caused by rubber modification. The BRMA showed improved high-temperature, elastic, and low-temperature performance compared to neat asphalt. However, Fourier transform infrared and fluorescence microscope tests indicated insufficient interaction between the rubber, bio-oil, and asphalt under the low-temperature, short

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0% found this document useful (0 votes)
44 views10 pages

1 s2.0 S0950061823033743 Main

This document discusses a study that evaluated asphalt modified with bio-oil and high rubber content under low temperature and short mixing time production conditions. The study prepared rubber and bio-oil modified asphalt (BRMA) with 20% crumb rubber content and 5%, 10%, or 15% bio-oil content at 160°C for 30 minutes of mixing. Tests found that bio-oil addition significantly reduced the viscosity increase typically caused by rubber modification. The BRMA showed improved high-temperature, elastic, and low-temperature performance compared to neat asphalt. However, Fourier transform infrared and fluorescence microscope tests indicated insufficient interaction between the rubber, bio-oil, and asphalt under the low-temperature, short

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juan daniel
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Construction and Building Materials 408 (2023) 133656

Contents lists available at ScienceDirect

Construction and Building Materials


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

Evaluation of asphalt modified with bio-oil and high rubber content: Low
temperature and short mixing time production condition
Yiyang Xue a, b, Dongdong Ge a, b, *, Songtao Lv a, b, Defeng Duan c, Yajun Deng d
a
Key Laboratory of Special Environment Road Engineering of Hunan Province, Changsha University of Science & Technology, Changsha 410114, Hunan, China
b
National Engineering Research Center of Highway Maintenance Technology, Changsha University of Science & Technology, Changsha 410114, Hunan, China
c
CCCC-SHB Fourth Engineering Co., Ltd., Luoyang 471013, Henan, China
d
Shenzhen Municipal Engineering Corp, Shenzhen 518034, Guangdong, China

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

Keywords: High rubber content modified asphalt needed high production temperatures due to the high viscosity, but the
Waste crumb rubber viscosity and production temperature could be decreased by adding bio-oil. Producing rubber and bio-oil
Bio-oil modified asphalt (BRMA) with good performance under low temperatures and short mixing time had signifi­
Production condition
cant environmental contributions. Therefore, this study prepared BRMA with crumb rubber content of 20 % and
Rheological performance
Interaction mechanism
bio-oil content of 5 %, 10 %, and 15 % under the low-temperature (160 ◦ C) and short-time (30 min) shear
Insufficient interaction conditions. The rheological characteristics of BRMA were evaluated by conventional and rheological property
tests. The interaction mechanism among rubber, bio-oil, and asphalt was assessed with the Fourier Transform
Infrared test (FTIR) and Fluorescence Microscope test (FM). The addition of bio-oil had a significant impact on
reducing the increase in asphalt viscosity that was typically caused by rubber modification. The high-
temperature performance, elastic performance, and low-temperature performance of BRMA were significantly
improved. The PG grade of neat asphalt was PG 64–22, 20 %R + 5 %Bio was PG 70–34, 20 %R + 10 %Bio was PG
70–34, and 20 %R + 15 %Bio was PG 64–40. Under the condition of low mixing temperature and short reaction
time, the FTIR test found that no new absorption peak appeared, and the bio-oil, rubber, and asphalt were mainly
physical mixing. Through the FM test, it was found that rubber reacted with asphalt at different degrees, and
some crumb rubber that did not fully react ensured that asphalt still had good elastic properties and deformation
resistance at high temperatures. The research provided theoretical guidance for similar application scenarios,
such as dry process rubber modified asphalt.

1. Introduction combining the characteristics of two waste materials. Many scholars


have studied the application of two kinds of waste materials in road
As the road industry continues to evolve, increasingly demanding engineering.
usage environments have led to higher performance requirements for Rubberized asphalt, as a representative of polymer-modified asphalt,
pavement materials, and the demand for high-quality asphalt materials was extensively applied in high-grade pavement construction due to its
is increasing [1,47]. Applying waste crumb rubber to asphalt modifi­ excellent performance [5]. According to researchers, adding only 10 %
cation was a good choice to solve the waste tires “black pollution” and crumb rubber to 90# asphalt could elevate its PG grading temperature
endow asphalt with better road performance. However, the high vis­ from 64 ◦ C to 80 ◦ C [6]. The rubber modified asphalt had good high-
cosity of rubberized asphalt was not conducive to engineering applica­ temperature performance due to the swelling reaction of crumb rub­
tion [2,3]. Biomass resources have made remarkable achievements in ber would absorb lightweight components, and the elastic characteris­
alleviating the consumption of asphalt resources. Adding bio-oil as an tics and deformation resistance were improved by the micro-skeleton
admixture was an effective way to decrease the viscosity and mixing effect of crumb rubber [7,8,48]. However, high viscosity, high energy
temperature of the mixture [4]. This study aimed to prepare BRMA by consumption, poor construction workability, and other problems have

* Corresponding author at: Key Laboratory of Special Environment Road Engineering of Hunan Province, Changsha University of Science & Technology, Changsha
410114, Hunan, China.
E-mail address: [email protected] (D. Ge).

https://doi.org/10.1016/j.conbuildmat.2023.133656
Received 26 April 2023; Received in revised form 5 September 2023; Accepted 2 October 2023
Available online 10 October 2023
0950-0618/© 2023 Published by Elsevier Ltd.
Y. Xue et al. Construction and Building Materials 408 (2023) 133656

seriously limited the utilization of high rubber content modified asphalt was beneficial to improve fatigue properties [36,37]. Xu et al. showed
in highway construction to this day [9,10]. Poor construction work­ that the utilization of microwave desulfurization in combination with
ability led to high energy consumption and environmental problems waste engine oil could effectively reduce the viscosity of rubber asphalt,
during construction [11]. Wang et al. showed that AASHTO M 320 leading to improved workability [38]. Li et al. overcame the high vis­
stated that when the viscosity of asphalt binder reached 3 Pa⋅s, the cosity and difficult construction of traditional rubber asphalt by adding
maximum service temperature was 135◦ C. The condition was conve­ waste oil as a viscosity reducer. At a temperature of 180 ◦ C, the use of
nient for storage and construction, but rubber modified asphalt was waste oil led to a 64.5 % decrease in the rotational viscosity of rubber
difficult to meet this requirement [12]. The mixing temperature of asphalt [39]. Gong et al. employed an epoxy asphalt rubber that was
rubber asphalt was 30 ◦ C ~ 50 ◦ C higher than that of traditional hot mix modified with waste cooking oil to reduce its viscosity and extend
asphalt [13]. Li et al. demonstrated that the rubber content was the most construction duration. Meanwhile, the compatibility of the modified
influential factor affecting the viscosity of rubber asphalt, with viscosity binder enhanced a lot, and the mechanical properties also met the
increasing exponentially as rubber content increased [14]. Khalili et al. specification requirements [40]. However, there are few researches on
demonstrated that enlarging the particle size of crumb rubber would low viscosity rubber modified asphalt based on bio-oil modification, and
result in a notable elevation in the viscosity of rubber asphalt, and it was the preparation process still needs to be optimized [41].
also concluded that increasing the crumb rubber content led to higher In summary, high rubber content modified asphalt had problems of
asphalt viscosity and elastic recovery percentage [15]. Nevertheless, high viscosity and poor construction workability. This limitation
incorporating more crumb rubber into asphalt resulted in negative im­ imposed a serious impediment to the advancement of high content
pacts on its ductility, toughness, and resistance to cracking [16,49]. rubber modified asphalt. The high viscosity could be reduced by bio-oil,
Singh et al. demonstrated that enlarging the size of crumb rubber par­ but there was no mature preparation method. This study hoped that the
ticles was advantageous in enhancing the deformation and rutting viscosity reduction of bio-oil would make it possible for rubber modified
resistance of rubberized asphalt [17]. Yang et al. believed that incor­ asphalt to have lower preparation temperature and shorter shear time.
porating a higher concentration of rubber into the asphalt mixture
would result in an increase in its hardness, as well as a potentially higher 2. Objective
required temperature for construction [18]. Moreover, the emission of
harmful gases during the construction of rubber asphalt was shown to In this study, the incorporation of bio-oil reduced the marked in­
have a significant increase when compared to that of neat asphalt, and crease in the viscosity of asphalt with high rubber content. The dry
the emission of harmful gases was more obvious in high-temperature rubber mixture was produced at shorter mixing times and lower tem­
environments. Reducing the construction temperature could reduce peratures in the field, even if there was a curing process between the
harmful gas emissions [3,19]. crumb rubber and asphalt, the reaction between the two was still
In order to reduce the viscosity of rubber modified asphalt and insufficient. However, the laboratory had not established a standard for
expand its application scenarios, many researchers have used bio-oil to the indoor simulation of the dry method. Therefore, this study attempted
modify rubber asphalt in recent years [20]. Biomass materials had sig­ to use 160 ◦ C − 30 min to prepare BRMA. To examine the impact of bio-
nificant advantages, such as huge reserves, renewable, extensive sour­ oil concentration on BRMA performance, BRMA was prepared with
ces, and high economic benefits. Bio-oil obtained by rapid pyrolysis of different content of bio-oil and 20 % crumb rubber. This study used
biomass [21], substrates after crop processing [22], and downstream crumb rubber and bio-oil combined modified asphalt under the low-
products of the oil industry [23] could be used as direct substitutes, temperature and short-time shear condition, hoping to prepare high
admixtures, and modifiers to produce bio-asphalt with different prop­ performance modified asphalt used under low construction tempera­
erties. The utilization of bio-based materials in road engineering was tures and achieve the goal of environmental protection. To investigate
beneficial in reducing greenhouse gas emissions [24]. As a modifier, bio- the impact of material design and preparation process on the properties
oil exhibited a notable capability to decrease the asphalt viscosity, while of BRMA, Brookfield Rotational Viscosity Test (RV), Dynamic Shear
simultaneously adding light components to strengthen low-temperature Rheometer test (DSR), Multiple Stress Creep Recovery test (MSCR),
crack resistance and aging resistance [25,26]. Hill B used pig manure as Bending Beam Rheological test (BBR), Fourier Transform Infrared test
raw materials to prepare bio-asphalt. The study findings revealed that (FTIR), and Fluorescence Microscope test (FM) were carried out.
incorporating bio-oil into asphalt led to enhancement in low-
temperature rupture resistance and mitigates the adverse impact of 3. Materials and test methods
RAP on performance [27]. The addition of isosorbide fractionation
bottom liquid as a warm mixing agent to the asphalt lowered the tem­ 3.1. Materials
perature of mixing and compaction. And the modified asphalt main­
tained a good high-temperature performance at the lowest compacted 70# neat asphalt was used in this study. All the fundamental char­
temperature of 120 ◦ C [28]. Podolsky et al. found that by only adding 1 acteristics of this neat asphalt met the specification requirements, as
% soybean oil into petroleum asphalt, construction temperature could shown in Table 1.
be lowered by 2 ◦ C to 3 ◦ C while maintaining excellent resistance against The particle size of the crumb rubber selected in this study was 0.3
low-temperature cracking and water damage [29]. mm, which was directly crushed from waste tires produced by Guangxi
Bio-oil could enhance the workability, compatibility, and storage Jiaoke New Material Technology Co., Ltd. Table 2 shows the basic
stability of rubberized asphalt during construction [30]. Researchers physical parameters of crumb rubber.
indicated that incorporating bio-oil into rubber modified asphalt resul­
ted in a considerable enhancement of the adhesive’s low-temperature
capabilities [31]. And the overall viscosity of the adhesive was Table 1
reduced clearly as well. Lower mixing and compaction temperatures Fundamental characteristics of 70# neat asphalt.
would reduce greenhouse gas emissions from rubber modified asphalt Properties Measured value Reference standard
adhesives during pavement construction [32,33]. The synergistic effect
Penetration at 25 ◦ C(0.1 mm) 67.3 AASHTO T 49
of bio-oil and rubber could greatly enhance the asphalt’s resilience to Softening point(◦ C) 48.7 AASHTO T 53
aging, and the anti-ultraviolet aging properties improved more signifi­ Ductility at 10 ◦ C(mm) 31.6 AASHTO T 51
cantly than the thermal aging properties [34,35]. Lei et al. highlighted Viscosity at 135 ◦ C(mPa⋅s) 462.5 AASHTO T 316
that the elastic properties would be enhanced by the interaction of bio- G*/sinδ(64 ◦ C) 1259.5 AASHTO T 315
G*/sinδ of aged asphalt(64 ◦ C) 2483.2 AASHTO T 315
oil with larger rubber particles, and the interaction with small rubber

2
Y. Xue et al. Construction and Building Materials 408 (2023) 133656

Table 2 Table 4
Basic indicators of crumb rubber. Detailed information of the sample.
Properties Requirements Result Crumb rubber content Bio-oil content Abbreviation
3
Density(g/cm ) ≤1.2 1.2 0% 0% Neat asphalt
Water content(%) ≤1.0 0.5 20 % 5% 20 %R + 5 %Bio
Metal content(%) ≤0.05 0.02 10 % 20 %R + 10 %Bio
Ash(%) ≤10 7 15 % 20 %R + 15 %Bio
Acetone extract(%) ≤10 7
Rubber hydrocarbon content(%) ≥48 56
Carbon black content(%) ≥26 30 AASHTO T 51.

3.2.4. Brookfield rotational viscosity test (RV)


This study used industrial waste vegetable oil as bio-oil, produced by
This study measured the viscosity of BRMA prepared by low-
Jinan Boao Chemical Co., Ltd, which was a by-product of the refining
temperature short-term shear using the Brookfield viscosity test in
process of industrial diesel oil. Table 3 shows the detailed parameters of
accordance with the specification AASHTO T 316, and analyzed the
this bio-oil.
impact of bio-oil content on the viscosity of BRMA, in order to verify the
feasibility of BRMA mixing in low temperature engineering. No.27 rotor
3.2. Test method was used in the Brookfield viscosity test, and the speed was 20 r/min.
Each asphalt was tested two times at 160 ◦ C.
3.2.1. Preparation of compound modified asphalt
The compound-modified asphalt preparation method referred to the 3.2.5. Dynamic shear rheometer test (DSR)
production methods of rubberized asphalt and bio-asphalt in relevant The DSR test measured the rutting index (G*/sinδ) at specific tem­
research literature. Rubber crumbs with a mass of 20 % asphalt were peratures and loading frequency referred to AASHTO T 315. The high-
determined to be used, and bio-oil contents were 5 %, 10 %, and 15 % of temperature sweeping processes were applied to the neat asphalt,
asphalt mass after conducting basic experimental studies. A method of modified asphalt, as well as asphalt binder subjected to short-term
preparing BRMA under the shear condition of low temperature (160 ◦ C) aging. High-temperature sweeps range from 46 ◦ C to 82 ◦ C, every 6 ◦ C
and short time (30 min) was proposed, which could simulate the dry for a temperature sweep. The asphalt after long-term aging was swept at
process of modifying asphalt with rubber at low mixing temperatures in intermediate temperatures. Intermediate-temperature sweeps range
the laboratory. First, the neat asphalt was heated in an oven at 135 ◦ C for from 16 ◦ C to 31 ◦ C, every 3 ◦ C for a temperature sweep. Simultaneously,
1 h until it reached a flowing state. Then 450 g asphalt and the designed the frequency sweep with a loading frequency of 0.1–10 Hz was per­
content of bio-oil were poured into the shear cup successively, and the formed at each test temperature. The tests were repeated three times for
glass rod was stirred for 2 min to ensure thorough mixing of the bio-oil each asphalt binder.
and asphalt. Finally, the mixture of bio-oil and modified asphalt was
sheared for 5 min at 135 ◦ C and 3000 r/min. After shearing, it was 3.2.6. Bending beam rheological testing (BBR)
heated to 160 ◦ C. In order to prevent clumping, the crumb rubber was The BBR test was conducted with reference to AASHTO T313 with
consistently incorporated into the bio-oil modified asphalt several times, the test instrument model CANNON TE-BBR. BBR tests were conducted
ensuring uniform distribution, and a glass rod was used to mix evenly at the range from − 12 ◦ C to − 30 ◦ C. Neat asphalt-PAV, 20 %R + 5 %Bio-
during the addition process. Then the BRMA was prepared under the PAV, 20 %R + 10 %Bio-PAV, and 20 %R + 15 %Bio-PAV were tested
condition of 3500 r/min shearing speed for 30 min. Detailed informa­ every 6 ◦ C, and every asphalt sample was repeated three times at the
tion of different types of asphalt binders studied in the manuscript is same temperature.
presented in Table 4.
3.2.7. Multiple stress creep recovery test (MSCR)
3.2.2. Rolling thin film oven test (RTFO)/ pressure aging vessel test (PAV) According to the DSR test results, the MSCR tests were performed in
The neat asphalt and BRMA were exposed to short-term aging ac­ accordance with AASHTO TP 70, with a temperature range of 52–76 ◦ C.
cording to the procedure outlined in AASHTO T 240 to obtain neat Neat asphalt-RTFO, 20 %R + 5 %Bio-RTFO, 20 %R + 10 %Bio-RTFO,
asphalt-RTFO, 20 %R + 5 %Bio-RTFO, 20 %R + 10 %Bio-RTFO, and 20 and 20 %R + 15 %Bio-RTFO were tested every 6 ◦ C. Each asphalt was
%R + 15 %Bio-RTFO. tested three times at the same temperature.
Subsequently, in order to simulate the thermal oxygen aging reac­
tion, the asphalt binder tested by RTFO was subjected to pressure aging 3.2.8. Fourier Transform Infrared test (FTIR)
according to AASHTO R 28. Neat asphalt-PAV, 20 %R + 5 %Bio-PAV, FTIR test could effectively analyze the functional groups in the
20 %R + 10 %Bio-PAV, and 20 %R + 15 %Bio-PAV were obtained after asphalt binder. The model of the FTIR instrument used in the test was
long-term aging. Thermo Fisher Nicolet iS50, 32 sweeps were performed across the
wavenumber range of 4000 cm− 1 to 650 cm− 1. The wave number curve
3.2.3. Conventional performance tests of absorbance could be obtained by sweeping.
The conventional performance of neat asphalt and BRMA was pre­
liminarily evaluated through softening point, penetration, and ductility 3.2.9. Fluorescence microscope test (FM)
tests to verify the feasibility of subsequent tests. Conventional tests were FM test could show different fluorescence characteristics of materials
performed according to specifications AASHTO T 53, AASHTO T 49, and at the micro-scale. In this study, the swelling degree and mixing uni­
formity of rubber powder in asphalt during low-temperature and short-
Table 3 time shearing were analyzed by FM test. The fluorescence microscope
Detailed parameters of Bio-oil. model used for the FM test was Leica DM4 M. BRMA was observed under
microscope magnification of 200x.
Properties Unit Result

Density(15 ◦ C) g/mL 0.93


Viscosity(60 ◦ C) Pa⋅s 73
Flash point ◦
C 231
Water content % 2.4

3
Y. Xue et al. Construction and Building Materials 408 (2023) 133656

4. Results and discussion

4.1. Conventional tests

At 25 ◦ C, the penetration of 20 %R + 5 %Bio was found to be com­


parable to that of neat asphalt. The penetration of BRMA increased
proportionally with the amount of bio-oil, and the growth rate was
getting faster. Compared with 20 %R + 5 %Bio, the penetration of 20 %
R + 10 %Bio increased by 23.4 %, while that of 20 %R + 15 %Bio
increased by 62.9 %. The increase of penetration was due to the addition
of bio-oil, which supplemented the lightweight components absorbed by
the crumb rubber. The penetration would increase proportionally with
the concentration of lightweight components [42]. As the bio-oil content
increased, there was a noticeable enhancement in its ability to reduce
the hardness of rubber modified asphalt.
The softening point of 20 %R + 5 %Bio increased by 29.8 %
compared with that of neat asphalt, which was a significant improve­
ment. The softening point of 20 %R + 15 %Bio was 18 % lower than that
of 20 %R + 5 %Bio. By adding bio-oil to asphalt, lighter components
were supplemented which helped to decrease the percentage of
Fig. 1. Viscosities of different types of asphalt binders.
asphaltene and subsequently reduced the softening point. A higher
concentration of asphaltene in asphalt would result in a higher softening
point [43]. As the content of bio-oil increased, the softening point of that the bio-oil could help the crumb rubber to dissolve and disperse
BRMA gradually decreased, but the BRMA exhibited better high- evenly.
temperature stability compared to the neat asphalt. According to the The preparation of BRMA by low-temperature and short-time
above data, the use of bio-oil negatively impacted the high temperature shearing had good construction workability, which could reduce the
performance of BRMA, crumb rubber was the main component of BRMA mixing temperature, energy consumption, and engineering costs of high
with good high temperature performance. rubber content modified asphalt mixture. It provided a novel approach
At a speed of 5 cm/min, neat asphalt and BRMA were tested for for utilizing bio-oil and crumb rubber waste materials with high content
ductility at 5 ◦ C. The ductility of neat asphalt was only 6.7 mm at this in road engineering.
test temperature. With 5 %, 10 %, and 15 % bio-oil content, the ductility
of BRMA rose by 24.4 times, 27.8 times, and 33.8 times of neat asphalt, 4.3. Rheological tests
respectively, which showed a linear upward trend. The combined action
of high rubber content with bio-oil significantly improved the ductility 4.3.1. Temperature sweep
of asphalt in low-temperature environments. In this study, the impact of crumb rubber and bio-oil on the prop­
In accordance with the mentioned analysis, the modified asphalt erties of BRMA in high temperatures was examined through the tem­
prepared by this method could realize the complementary advantages perature sweeping analysis of neat asphalt, BRMA, and asphalt after
and disadvantages of high rubber content and bio-oil. The combined RTFO. Fig. 2 displays the G*/sinδ value.
action of the high rubber content with high bio-oil content could provide The properties of BRMA were greatly improved compared with neat
good basic performance for the neat asphalt, which proved the feasi­ asphalt in high temperatures. During the temperature sweep from 46 ◦ C
bility of the follow-up test. to 82 ◦ C, the rate of decrease in G*/sinδ was observed to be significantly
higher for neat asphalt than that of BRMA, and the lower G*/sinδ slope
4.2. RV test of BRMA represented lower temperature sensitivity. The addition of bio-
oil resulted in a reduction of the G*/sinδ value of BRMA, but the G*/sinδ
The viscosity of BRMA, which was prepared using low-temperature of 20 %R + 5 %Bio and 20 %R + 10 %Bio was significantly higher than
and short-time shearing, was investigated using the Brookfield viscos­ that of neat asphalt. At 52 ◦ C, the G*/sinδ of 20 %R + 15 %Bio was
ity test, aiming to assess the construction workability of the dry process similar to that of the neat asphalt, but it was still significantly improved
of BRMA. In order to avoid further reaction of rubber in asphalt during under the test conditions above 52 ◦ C. The G*/sinδ at 70 ◦ C of neat
the test and better simulate the situation of BRMA in actual road use, the asphalt was 587 Pa, 20 %R + 15 %Bio, 20 %R + 10 %Bio, and 20 %R +
Brookfield viscosity test was performed at 160 ◦ C immediately after the 5 %Bio were 1.7, 2.6, and 4.3 times of that, respectively. The temper­
BRMA was obtained by shearing. ature sweeping results showed that although bio-oil had a negative
As shown in Fig. 1, the viscosity of 20 %R + 5 %Bio at 160 ◦ C was impact on the properties of BRMA in high temperatures, the combina­
1125 mPa⋅s, which was 8.2 times higher than the 137 mPa⋅s of the neat tion of high rubber content and bio-oil could provide good performance
asphalt. As the amount of bio-oil was increased, the viscosity of BRMA and stability for asphalt in high temperatures (Table 5).
experienced a significant decrease. Compared with 20 %R + 5 %Bio, the In the process of temperature rise, the slope of the G*/sinδ curve of
viscosity of 20 %R + 10 %Bio decreased by 41 %, and the viscosity of 20 neat asphalt-RTFO increased the most significantly, and the slope of the
%R + 15 %Bio decreased by 72 %. The viscosity of traditional rubber G*/sinδ curve of BRMA-RTFO changed relatively little. After short-term
asphalt at 160 ◦ C was about 3000 mPa⋅s [12], and the viscosity of 20 %R aging, comparing the slopes of G*/sinδ curves before and after, it was
+ 15 %Bio was 312 mPa⋅s. Compared with traditional rubber asphalt, observed that BRMA had significantly lower temperature sensitivity
the viscosity of 20 %R + 15 %Bio decreased by 89 %. It could be seen than neat asphalt, and BRMA had better anti-aging ability than neat
that the error bar of BRMA viscosity was significantly increased asphalt. Comparing the change in G*/sinδ between aged and unaged
compared with the neat asphalt, which was due to the interference of asphalt, the increase of G*/sinδ of neat asphalt-RTFO was the largest,
insufficiently dissolved rubber on the viscosity results. With the increase and the rise of G*/sinδ of BRMA-RTFO was obviously smaller. The
of bio-oil content, the viscosity error bar of BRMA decreased gradually. comparison results further confirmed the conclusion that the synergy
The error bar of 20 %R + 5 %Bio was the largest, but the error bar value between high-content rubber and bio-oil could improve the anti-aging
of 20 %R + 15 %Bio was close to that of neat asphalt. The results showed capability of asphalt and reduce its sensitivity to high temperature

4
Y. Xue et al. Construction and Building Materials 408 (2023) 133656

Fig. 2. Temperature sweep of original asphalt (a) and asphalt-RTFO(b).

the increase of sweeping frequency, the G* of neat asphalt-RTFO


Table 5
increased significantly and was higher than that of BRMA-RTFO. The
Conventional properties of different types of asphalt binders.
significant increase of G* suggested that the neat asphalt exhibited poor
Asphalt binder type Penetration Softening point Ductility aging resistance, leading to an increased susceptibility to variations in
(0.1 mm) (◦ C) (mm)
test conditions after aging. Due to the combination of the characteristics
Neat asphalt 67.3 48.7 6.7 of crumb rubber’s high elasticity and the anti-aging properties of bio-oil,
20 %R + 5 %Bio 70.7 63.2 163.7
the sensitivity of BRMA-RTFO to temperature and frequency changes
20 %R + 10 %Bio 87.2 57.2 186.3
20 %R + 15 %Bio 115.2 51.6 227
was reduced. Therefore, the G* of neat asphalt-RTFO was lower at low
frequency and higher at high frequency.

changes. 5. MSCR test


According to AASHTO T 315, PG grade was determined. Table 6
showed the high-temperature PG grades of different types of asphalt Through the MSCR test on the neat asphalt-RTFO and BRMA-RTFO
binders studied in the manuscript. under low stress (0.1 kPa) and high stress (3.2 kPa) conditions, the
test results of percentage of recovery and unrecoverable creep (Jnr) are
4.3.2. Master curve shown in Fig. 4 and Fig. 5.
Asphalt was a typical viscoelastic material with temperature and A higher percentage of recovery indicated that the asphalt binder
frequency equivalence. Under load, asphalt binder showed the same had better elasticity, and the ability to recover deformation after stress
viscoelasticity at high temperature instantaneous (high frequency) and was stronger [44]. The percentage of recovery values for various asphalt
low-temperature long time (low frequency). According to the principle binders under low stress (0.1 kPa) and high stress (3.2 kPa) conditions
of temperature-frequency equivalence, the master curves of neat asphalt are shown in Fig. 4. During the process of increasing the test tempera­
and BRMA were created using the results of temperature sweeping and ture from 52 ◦ C to 76 ◦ C, the percentage of recovery of asphalt samples
frequency sweeping. gradually decreased, and the decrease became faster at high tempera­
As shown in Fig. 3, the G* increased with the sweeping frequency tures. At the same time, the percentage of recovery of the same asphalt
increased, indicating that neat asphalt and BRMA had strong stiffness binder under low stress (0.1 kPa) and high stress (3.2 kPa) was
and resistance to deformation under low temperature/high frequency compared. The comparison results showed that the percentage of re­
conditions. The increase of bio-oil content in the BRMA resulted in a covery of asphalt under high-stress conditions had an obvious
reduction in G* value. However, neat asphalt exhibited the lowest G*, decreasing trend compared with low stress. The difference in the per­
but BRMA still had higher G* at a lower sweeping frequency. The results centage of recovery between the two stresses was greater under high-
indicated that incorporating crumb rubber could improve the elasticity temperature conditions, indicating that the asphalt binder’s elastic re­
and the ability to resist permanent deformation of BRMA at low fre­ covery characteristics under high-stress states were weak. The high-
quency (high temperature), while bio-oil would reduce the elasticity. temperature and high-stress environment would have a serious nega­
After the RTFO test, the G* of BRMA-RTFO was still higher than that of tive impact on the elastic capacity of asphalt binder.
neat asphalt-RTFO at low frequency (high temperature). However, with The order of percentage of recovery from strong to weak was: 20 %R
+ 5 %Bio > 20 %R + 10 %Bio > 20 %R + 15 %Bio > Neat asphalt. At
52 ◦ C, the percentage of recovery of neat asphalt under low stress was
Table 6 9.18 %, 20 %R + 5 %Bio, 20 %R + 10 %Bio, and 20 %R + 15 %Bio were
High-temperature PG grade. 9.3 times, 9.0 times, and 8.1 times of that, respectively. When the
Asphalt binder Neat 20 %R + 5 20 %R + 10 20 %R + 15 temperature rose by 70 ◦ C, the percentage of recovery of the neat asphalt
type asphalt %Bio %Bio %Bio decreased to 0, but the percentage of 20 %R + 5 %Bio, 20 %R + 10 %
PG-High PG 64 PG 70 PG 70 PG 64 Bio, and 20 %R + 15 %Bio were 61.94 %, 59.37 %, and 48.77 %,
Temperature respectively. The percentage of recovery of BRMA had been greatly

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Y. Xue et al. Construction and Building Materials 408 (2023) 133656

Fig. 3. The master curve of original asphalt (a) and asphalt-RTFO(b).

Fig. 4. Test results of deformation recovery rate R.

Fig. 5. The results of irrecoverable creep compliance Jnr.

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Y. Xue et al. Construction and Building Materials 408 (2023) 133656

improved, and the modification could bring good elastic recovery ability unit of strain. The capacity of asphalt binders to dissipate stress during
for asphalt so that asphalt could still maintain good elastic performance stress transfer was reflected by the m-value. A higher m-value was a
under high-temperature and high-stress environments. However, as the clear indicator of better stress relaxation capabilities and increased
content of bio-oil increased, the percentage of BRMA recovery gradually resistance to cracking.
reduced, and the rate of descent became faster. This indicated that Fig. 6 shows the S and m values of asphalt binder at − 12 ◦ C to
crumb rubber was the main component of the elastic effect in BRMA, − 30 ◦ C. Since the neat asphalt no longer met the specification re­
and the bio-oil had a negative impact on the BRMA’s elastic recovery quirements at − 18 ◦ C, testing was only conducted at − 12 ◦ C and − 18 ◦ C.
capacity. However, the deformation of 20 %+10 % Bio-PAV and 20 %+15 % Bio-
The value of Jnr reflected the irretrievable change in creep compli­ PAV was large under the test condition of − 12 ◦ C, and the test data could
ance of asphalt binder when subjected to stress. The ability of asphalt not be measured.
binders to resist unrecoverable strain under stress was inversely pro­ As shown in Fig. 6 (a), the lower the temperature, the faster the S
portional to the value of Jnr. During the process of temperature increase, increased, indicating that the hardness and brittleness of asphalt were
the Jnr values for different asphalt binders under low stress (0.1 kPa) more pronounced in low-temperature environments. During testing at
and high stress (3.2 kPa) increased, and the irreversible strain of asphalt identical temperatures, BRMA exhibited a noteworthy decline in its S
increased under stress. Moreover, the Jnr value under high stress was value relative to neat asphalt, with an increasingly pronounced reduc­
significantly higher than that under low stress, indicating that the tion in tandem with the augmented bio-oil content. At − 18 ◦ C, the S
deformation resistance of asphalt was significantly adversely affected by value of neat asphalt-PAV was 379 MPa, 20 %R + 5 %Bio-PAV, 20 %R +
the high temperature and high stress level in the application 10 %Bio-PAV, and 20 %R + 15 %Bio-PAV were 83.5 MPa, 52.1 MPa, and
environment. 35.8 MPa, respectively. These values represented reductions of 78 %, 86
The combination of high content rubber and bio-oil could signifi­ %, and 90 % compared to the neat asphalt binder. As the test temper­
cantly decrease the amount of unrecoverable creep compliance that ature decreased, there was a significant difference in the creep stiffness
occurs when the asphalt was placed under stress. However, the irre­ of BRMA with varying bio-oil contents. The rate of increase in creep
versible creep soft growth rate of BRMA increased as the bio-oil content stiffness of BRMA decreased as the bio-oil content increased. At − 30 ◦ C,
increased, suggesting that an excessive amount of bio-oil would the S values of 20 %R + 5 %Bio-PAV and 20 %R + 10 %Bio-PAV were
compromise the temperature and pressure stability of BRMA. It showed 465 MPa and 335.5 MPa, respectively, which could not meet the spec­
that in BRMA, bio-oil would reduce the rutting resistance, and crumb ification requirements, while 20 %R + 15 %Bio-PAV was 248 MPa,
rubber was the main score for BRMA to provide better elastic perfor­ which was still within the prescribed range. The results of the S value
mance and enhance asphalt’s resistance to permanent deformation. showed that bio-oil could significantly reduce the stiffness of asphalt at
Therefore, crumb rubber could bring elastic properties to asphalt. It was low temperatures, so asphalt had better low-temperature crack
essential to carefully regulate the amount of bio-oil utilized in the resistance.
mixture to ensure that BRMA and the mixture could better resist per­ The stress dissipation capacity of asphalt binder decreased signifi­
manent deformation under high-temperature environments. cantly at low temperatures, as evidenced by a decrease in the m-value.
The m-value of BRMA exhibited a more pronounced increase as the
content of bio-oil was raised, resulting in a marked improvement over
5.1. BBR test the neat asphalt. At a temperature of − 18 ◦ C, the m-value of neat
asphalt-PAV was 0.236, which was far below the specification re­
In this study, BBR tests were carried out at − 12 ◦ C to − 30 ◦ C to quirements. The m-values of 20 %R + 5 %Bio-PAV, 20 %R + 10 %Bio-
determine the change rule of S and m value to characterize the low PAV, and 20 %R + 15 %Bio-PAV were 0.376, 0.402, and 0.439, which
temperature crack resistance of aged asphalt binder. Creep stiffness (S) were 59 %, 70 %, and 86 % higher than the neat asphalt. As temperature
was a useful indicator of an asphalt binder’s ability to deform under low decreased, the m-value of BRAM with different bio-oil contents
temperature conditions. Asphalt hardness increased with an increase in decreased at the same rate, and the decrease rate was gentler than that of
S, meaning that a higher stress level was necessary to produce the same

Fig. 6. The test results of S (a) and m-value (b).

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Y. Xue et al. Construction and Building Materials 408 (2023) 133656

neat asphalt, indicating that BRMA was less sensitive to low tempera­
ture. At − 30 ◦ C, the m-values of 20 %R + 5 %Bio-PAV and 20 %R + 10 %
Bio-PAV were 0.244 and 0.271, which were below the specification
requirements, while the m-values of 20 %R + 15 %Bio-PAV was 0.3,
which was still within the prescribed range. By using a combination of
high rubber content and bio-oil, the stiffness of asphalt could be
reduced, relieve the increase of the hardness and brittleness of asphalt in
the aging process, and enhance the cracking resistance and stress
dissipation performance of asphalt at low temperatures.
According to the PG grade shown in Table 6, the frequency sweep of
the asphalt after PAV was carried out at intermediate temperatures. Neat
asphalt-PAV G*/sinδ was 65086 Pa at 25 ◦ C, 20 %R + 5 %Bio-PAV G*/
sinδ was 22680 Pa at 22 ◦ C, 20 %R + 10 %Bio-PAV G*/sinδ was 12987
Pa at 22 ◦ C, and 20 %R + 15 %Bio-PAV G*/sinδ was 12642 Pa at 16 ◦ C.
Table 7 shows the PG grade of different types of asphalt binders.

5.2. Microscopic properties

5.2.1. FTIR test


The FTIR spectra of BRMA and its modified materials are shown in
Fig. 7. The reaction mechanism between materials was determined by
comparing the changes of absorption peaks in the spectrogram. Fig. 7. FTIR spectra of different types of asphalt binders.
Table 8 displays the same absorption peaks of neat asphalt and
BRMA. The spectra of bio-oil, bio-oil modified asphalt, and BRMA
revealed significant changes in their absorption peaks with two new Table 8
strong peaks appearing prominently at 1750 cm− 1 and 1150 cm− 1, Same absorption peaks of neat asphalt and BRMA.
which were absent in neat asphalt. The absorption peaks observed at Wave number Functional Vibration mode
1750 cm− 1 and 1150 cm− 1 were unique characteristics of the ester group group
present in the bio-oil. The peak at 1750 cm− 1 could be attributed to the 960–700 cm− 1
Benzene ring C-H- bond rocking vibration
stretching vibration of the C = O bond in the ester group. This suggested 1370 cm− 1 –CH2 - C-H bond symmetric tensile bending
that the combination of bio-oil and asphalt was a result of physical vibration
blending. It could be clearly seen that compared to rubber modified 1455 cm− 1 Methyl group C-H bond stretching vibration
1600 cm− 1 Toluene C = C skeleton stretching vibration
asphalt and bio-oil modified asphalt, the spectrum of BRMA only
2356 cm− 1 CO2 stretching vibration
showed changes in the absorption peak area. The interaction between 2922––2852 Methylene –CH2 bond symmetric and antisymmetric
rubber crumbs and bio-oil in asphalt did not cause new absorption peaks cm− 1 stretching vibrations
in the spectrum of BRMA. It showed that in the process of preparing
BRMA by low-temperature short-time shearing, the crumb rubber only
existed a swelling reaction in asphalt, and no chemical change occurred, previous studies [46].
which was consistent with the findings from Zhang et al. [45]. The The microstructure of BRMA was observed by FM test verified that
spectrogram showed that the process of combining bio-oil, crumb rub­ the crumb rubber could not completely react with asphalt in the process
ber, and asphalt in BRMA prepared by low-temperature short-time of low-temperature and short-time shearing, these incompletely swollen
shearing was mainly physical blending. Through physical action, the crumb rubber could endow BRMA with good elastic recovery properties.
combination of crumb rubber and bio-oil provided the BRMA with The FM test results of BRMA well reflected the micro-morphology of
excellent performance in both high and low temperatures, as well as crumb rubber in the dry rubber asphalt mixture, establishing the sound
strong resistance to deformation. theoretical groundwork for future research on the BRMA and dry rubber
modified asphalt mixture.
5.2.2. FM test
In order to analyze the microstructure of the crumb rubber and 6. Conclusion
asphalt reaction, the FM test was used to observe the BRMA. Fig. 8 shows
the microstructure of BRMA observed under the Fluence Microscope. In this study, BRMA was prepared with varying contents of bio-oil (5
Because the crumb rubber without swelling reaction would not be %, 10 %, and 15 %) and crumb rubber (20 %) by low-temperature and
excited by fluorescence and would appear black under the fluorescence short-time shearing. The bio-oil and crumb rubber contents were
microscope, the reaction degree and dispersion could be clearly determined by conventional tests. The construction workability of
observed by the FM test. As shown in Fig. 8, the crumb rubber in BRMA BRMA was evaluated by the RV test. Rheological properties tests such as
prepared by low-temperature and short-time shearing was distributed DSR and BBR were conducted to investigate the high and low-
evenly, but the reaction degree was different. Part of the crumb rubber temperature characteristics of BRMA, and PG grades were carried out.
with large particles could not be completely swollen, so unswollen FTIR and FM tests were carried out to analyze the modification mech­
crumb rubber could be observed, as well as partially swollen and anism of BRMA. The conclusions are as follows:
completely swollen crumb rubber. Similar results have been observed in
(1) Bio-oil could significantly enhance the construction workability
Table 7 of rubber modified asphalt. As the level of bio-oil content rose,
PG grade of different types of asphalt binders. the viscosity of BRMA declined. At 160 ◦ C, the viscosity of 20 %R
+ 15 %Bio was 312 mPa⋅s, which was 72 % lower than that of 20
Asphalt binder Neat 20 %R + 5 % 20 %R + 10 20 %R + 15
type asphalt Bio %Bio %Bio %R + 5 %Bio.
(2) The PG grade of neat asphalt was PG 64–22, 20 %R + 5 %Bio was
PG Grade PG 64–22 PG 70–34 PG 70–34 PG 64–40
PG 70–34, 20 %R + 10 %Bio was PG 70–34, and 20 %R + 15 %

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Y. Xue et al. Construction and Building Materials 408 (2023) 133656

Fig. 8. The dissolution state of rubber in modified asphalt as observed by FM test.

Bio was PG 64–40. Crumb rubber was the main component to interests or personal relationships that could have appeared to influence
provide high-temperature deformation resistance in BRMA, and the work reported in this paper.
bio-oil gave BRMA good low-temperature crack resistance.
(3) The results of FTIR showed that bio-oil and crumb rubber were Data availability
physically blended to improve the properties of BRMA without
chemical reaction. The results of the FM test demonstrated that Data will be made available on request.
crumb rubber in BRMA was in an insufficiently reactive state.
(4) The BRMA exhibited a high elasticity recovery rate when Acknowledgements
compared to neat asphalt, and the unrecoverable deformation
was greatly reduced. The crumb rubber existed in the form of The manuscript was supported by the National Natural Science
granules, which might be the reason why BRMA had good Foundation of China (Grant numbers: 52108398, 52225806,
deformation resistance and elastic recovery performance at high 52078063), the Open Fund of Key Laboratory of Special Environment
temperatures. Road Engineering of Hunan Province (kfj210502).

The content of 20 %R + 10 %Bio was recommended based on PG


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