Journal of Cleaner Production 389 (2023) 136070

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Journal of Cleaner Production

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Microscopic characteristics of interface transition zones of hot mix asphalt

containing recycled concrete aggregates
Mengyun Zhang a, Changjiang Kou a, b, *, Aihong Kang a, b, Peng Xiao a, b, Haotian Hu c
a
College of Civil Science and Engineering, Yangzhou University, Yangzhou, 225127, China
b
Academy of Urban Planning and Development, Yangzhou University, Yangzhou, 225127, China
c
Jiangsu Sutong Bridge Co., Ltd, Nantong, 226000, Jiangsu, China

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

Handling Editor: Zhen Leng The understanding of microscopic characteristics of interface transition zones (ITZs) between recycled concrete
aggregates (RCAs) and asphalt mastic contributes to the treatment strategy of RCAs and the optimum design of
Keywords: hot mix asphalt. For this purpose, on ITZs samples cutting from stone mastic asphalt (SMA) mixture containing
Hot mix asphalt RCAs, scanning electron microscopy, nano-indentation and energy dispersive spectroscopy were performed to
Recycled concrete aggregates
examine the micromechanical properties, morphological characteristics, and chemical composition properties.
Interface transition zones
Results indicate that the addition of RCAs increased the high-temperature stability, and decreased the low-
Microscopic characteristics
Micromechanical properties temperature cracking resistance, the water stability, and the indirect tensile cracking resistance of SMA. The
microscopic characteristics of aggregate, residual mortar, asphalt mastic, and their ITZs show significant dif­
ferences. In terms of micromechanical parameters, the ITZs between the aggregate and the residual mortar (ITZs-
A-R) has a thickness of 25 μm and an average elastic modulus of 24.01 GPa while the ITZs between the residual
mortar and the asphalt mastic (ITZs-R-A) own a thickness of 26 μm and an average elastic modulus of 28.68 GPa.
Correspondingly, the asphalt mastic adjacent to the RCAs indicates a denser appearance than that unconnected to
the RCAs. Therefore, the penetration of asphalt binder helps improve the strength of the porous attached mortar.
The energy dispersive spectroscopy presents that the ITZs-A-R is dominated by substances containing calcium
oxide and aggregates and the ITZs-R-A is principally composed of asphalt, mineral, powder, and substances
containing calcium silicate. The thicknesses of ITZs determined by chemical composition are similar to that
determined by nano-indentation. Incorporating RCAs leads to a more complex mechanical composition system
and the performance degradation of hot mix asphalt. The microscopic characteristics of the ITZs should be taken
into account during the strengthening treatments of RCAs and the measurement of the mechanical properties of
hot mix asphalt incorporating RCAs.

1. Introduction
Construction and demolition waste (C&DW) are one of the key par­
adoxes in the field of construction engineering as China’s urbanization
process progresses and natural gravel resources grow increasingly
scarce. Waste concrete is a major component of C&DW (Tam, 2008; Kim
and Kim, 2007). Recycled concrete aggregates (RCAs) obtained by
processing and crushing waste concrete are proven to be used in pre­
paring RCAs hot mix asphalt (RCAM), which can pave asphalt pave­
ments of different grades. Asphalt mixtures that use RCAs instead of
natural aggregates (NAs) have been shown to perform satisfactorily
(Radevic et al., 2017; Sun et al., 2018; Alvarez et al., 2020). It can
encourage the effective recycling of building waste and lessen the need
for mining natural sand and gravel. As a result, considering the devel­
opment of road construction, the application of RCAs for asphalt pave­
ments seems extremely promising.
The feasibility of using RCAs in hot mix asphalt has received
mounting attention from researchers. Unlike NAs, RCAs are composite
materials that have minor damage and porous residual mortar attached
to the surface (Paranavithana and Mohajerani, 2006; Shi et al., 2016).
Only some of the engineering specifications are met by RCAs in com­
parison to NAs, but they have higher water absorption, lower specific
gravity, higher abrasion, and higher crushing pressure values (Pedro
et al., 2014; Poon et al., 2002; JTTE Editorial Office, et al., 2021). The

* Corresponding author. College of Civil Science and Engineering, Yangzhou University, Yangzhou, 225127, China.
E-mail address: changjiang.kou@yzu.edu.cn (C. Kou).

https://doi.org/10.1016/j.jclepro.2023.136070
Received 7 November 2022; Received in revised form 25 December 2022; Accepted 15 January 2023
Available online 18 January 2023
0959-6526/© 2023 Elsevier Ltd. All rights reserved.
M. Zhang et al.
RCAs surface becomes uneven, heterogeneous, and porous as a result of
the mortar layer adhesion, which worsens RCAM mechanical and
physical qualities. (Poon et al., 2004; Ghaffar et al., 2020; Mercante
et al., 2012). Therefore, moisture can easily intrude and remain in the
highly developed pores of the residual mortar in RCAs (Huang et al.,
2021). As a result, the adhesion between RCAs and asphalt is more
severely degraded than with NAs. The feasibility of RCAs applied to
asphalt mixtures was demonstrated (Wu et al., 2013; Hou et al., 2014;
Zou et al., 2020). The RCAM asphalt absorption and stability increase
with increasing RCA content. (Espino-Gonzalez et al., 2021). RCAs was
incorporated into the asphalt mixtures upon which the freeze-thaw
splitting tensile strength ratio, modulus of elasticity, and dynamic
modulus of the asphalt mixtures decreased (Mills-Beale and You, 2010;
Xiao et al., 2018; Yan et al., 2017). However, it is recommended that
RCAs be limited to an appropriate content to ensure that the asphalt mix
meets the performance requirements for water stability (Perez et al.,
2012). In addition, numerous studies have shown that the use of RCAs
increases the low-temperature cracking tendency of asphalt mixtures.
The indirect tensile strength of asphalt mixtures containing RCAs was
lower than that of natural aggregates asphalt mixture (AM) (Bhusal
et al., 2011). On the other hand, coarse RCAs could improve the
high-temperature rutting resistance of asphalt mixture (Shen and Du,
2004; Shen and Du, 2005). Although RCAs reduced the spalling resis­
tance of asphalt-stabilized materials, they substantially increased the
resistance to permanent deformation (Gomez-Meijide and Perez, 2016;
Pasandin and Perez, 2015). In summary, the performance of asphalt
mixtures containing RCAs over their service life is very different from
that of conventional mixtures.
The performance of RCAM is directly associated with the bond
strength of the interface between the materials. By using SEM, the
cementitious substance was found to produce narrow regions around the
aggregate particles that were thought to represent the interface transi­
tion zones (ITZs) (Zhu et al., 2017). The interaction mechanism at the
asphalt-aggregate interface is critical. In addition, the interface bond
strength influences the overall performance of the composite, and
identifying the ITZs between the asphalt and the aggregate helps to
control the mechanisms of fracture behavior in asphalt pavements
(Matzenmiller and Gerlach, 2006). ITZs turned out to be the weak point
of RCAM (Zhu et al., 2017; Mo et al., 2011). ITZs in the RCAM were
divided into the residual mortar interface and the aggregate interface
(Hu et al., 2022). Interface damage at the residual mortar and asphalt
mastic is the main source of damage; as the content of RCAs increases,
more interface damage occurs inside RCAM. It is therefore valuable to
study the nature of the transition zone at the interface of RCAM. How­
ever, the investigation of the mechanical properties and damage pat­
terns of RCAM is directly impacted by the lack of information regarding
the microscopic characteristics of the ITZs between RCAs and asphalt
mastic.
The microstructure of the ITZs can be explored by several instru­
mental techniques (nano-indentation (NI), scanning electron micro­
scopy (SEM), energy dispersive spectroscopy (EDS), etc.) to help
understand the complex mechanical behavior of the ITZs between RCAs
and asphalt mastic (Hu et al., 2015; Jiang et al., 2019; Lv et al., 2019).
ITZs between the aggregate and cement paste was studied by SEM
(Sidorova et al., 2014; Xie et al., 2015). The micromechanical properties
of asphalt mastic, ITZs, and granite aggregates was also investigated
(Barbhuiya and Caracciolo, 2017). The mechanical behavior of the ITZs
was measured by nano-indentation and the influence of aggregate type
on the thickness of ITZs was evident, while ITZs produced by limestone
are thinner than those produced by basalt and gabbro (Hu et al., 2020).
Similarly, the thickness of ITZs in asphalt mixtures with more porous
cement mortars and bricks (40 μm) was thicker than that of dense
recycled granite and natural limestone (30 μm) through NI tests (Huang
et al., 2021). It was identified that the ITZs range from about 30 μm to
60 μm near the surface of the aggregate (Karki et al., 2016). The rigidity
and modulus values of the ITZs are between those of limestone
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Journal of Cleaner Production 389 (2023) 136070
aggregates and asphalt marl (Khorasani et al., 2013). The thicknesses of
the ITZs between RCAs and mortar and the ITZs between NAs and
mortar were about 40–50 μm and 55–65 μm, respectively (Lee and Choi,
2013; Tasong et al., 1999). The distribution of chemical elements in the
focal region was studied using energy dispersive spectroscopy (EDS)
combined with SEM imaging to obtain more accurate thicknesses and to
identify each phase of the asphalt mixture by analyzing the character­
istic elements (Li and Stang, 1997). However, current research is yet
limited in grasping the microscopic mechanical properties of the nano­
scale ITZs between RCAs and asphalt mastics. The microscopic data
obtained from existing studies on multiphase interfaces vary consider­
ably, so the preparation of samples suitable for ITZs testing, the test
methods to accurately characterize micro and nano properties and the
effects of variability require in-depth research work.
Therefore, the understanding of microscopic characteristics of ITZs
between RCAs and asphalt mastic contributes to RCA treatment strategy
and the optimum design of hot mix asphalt. For this purpose, on ITZs
samples cutting from stone mastic asphalt (SMA) mixture containing
RCAs, scanning electron microscopy, nano-indentation and energy
dispersive spectroscopy were performed to examine the micro­
mechanical properties, morphological characteristics, and chemical
composition properties. . Based on this, it is possible to further explore
how ITZs affect hot mix asphalt performance, which will enhance the
caliber of RCAs and optimize recycling.
2. Materials and methods
2.1. Raw materials
2.1.1. RCAs and NAs
The aggregates used in the experiments include crushed production
of RCAs and NAs. RCAs are derived from waste cement concrete. Fig. 1
shows RCAs in different particle size ranges. RCAs with a particle size
greater than 26.5 mm have no mortar adhering to their surface, while
RCAs below 9.5 mm contains a large amount of residual mortar and have
greater variability in performance, which will affect the hot mix asphalt
performance. Therefore, the RCAs employed in this investigation had a
particle size range of 9.5–26.5 mm. Table 1 shows the general charac­
teristics of the RCAs and NAs employed in this investigation.
A reduction in density, a rise in water absorption, a high crushing
value, and a significant loss of Los Angeles abrasion are all character­
istics of RCAs. Despite having a crushing value of up to 23% and a Los
Angeles abrasion loss of up to 23.98% less than NAs, RCAs nonetheless
meet the standards of China’s technical specifications for the building of
highway asphalt pavement (JTG F40-2004) (Ministry of Transport of P.
R. China, 2004).
2.1.2. Asphalt binder
He chosen asphalt binder is styrene butadiene styrene (SBS) modified
asphalt, and Table 2 displays some of its fundamental technical
characteristics.
2.2. Mixture design
To replace NAs with the corresponding particle size in this study,
RCAs with a range of 9.5–26.5 mm were chosen. There was a 37.5%
overall replacement rate. Considering the RCAs properties, the RCAM
mineral gradations are modified by combining the volume correction of
the RCAs replacement rate with the natural fine aggregate curve fitting
method. Fig. 2 depicts the stone mastic asphalt mixture gradation curve.
The asphalt mixture was subsequently compacted using a Superpave
gyratory compactor into cylinder specimens with dimensions of 150 mm
in diameter and 115 mm in height. Using the Superpave asphalt mixture
design approach, the optimal asphalt content for hot mix asphalt con­
taining 37.5% RCAs was found to be 6.0%.
M. Zhang et al. Journal of Cleaner Production 389 (2023) 136070

Fig. 1. RCAs in different particle size ranges.

Table 1
General properties of RCAs and NAs.
Technical properties Particle size range/mm Criteria

RCAs NAs

9.5–13.2 13.2–16 16–19 19–26.5 9.5–13.2 13.2–16 16–19 19–26.5

Apparent relative density 2.686 2.679 2.689 2.691 2.716 2.715 2.707 2.716 >2.45
Relative density of gross volume 2.295 2.323 2.395 2.450 2.677 2.683 2.685 2.699 –
Water absorption/% 6.34 5.72 4.57 3.66 0.52 0.45 0.30 0.23 <3.0
Mortar adhesion rate/% 31.5 29.4 33.6 29.5 / / / / –
Crush value/% 21.3 23.5 22.8 24.4 10.0 10.4 9.9 10.4 <30
Abrasion value/% 25.0 24.2 24.6 22.1 18.0 17.4 17.9 18.4 <35

2.3. Experimental methods

Table 2
Basic characteristics of asphalt.
2.3.1. Performance tests
Technical indexes Measure Criteria The applicability and mechanical qualities of AM and RCAM were
value
examined through a variety of lab tests. The Standard Test Methods of
Ductility (5 cm/min,5 ◦ C)/cm 46 ≥30 Bitumen and Bituminous Mixtures for Highway Engineering following
Soften point/◦ C 65 ≥55
criteria were used to test each property separately: high-temperature
Penetration Index (PI) 0.5 − 0.4–1.0
Penetration (25 ◦ C)/0.1 mm 64 60–80
stability, low-temperature cracking resistance, and water stability
Elasticity Recovery (25 ◦ C)/% 78 ≥65 (JTG E20-2011).
Kinematic viscosity (235 ◦ C)/Pa⋅s 1.8 ≤3 Uniaxial penetration test (T0713) for assessing the high-temperature
Residues after Penetration ratio/% 71.8 ≥60 capabilities of asphalt mixes2 Low-temperature bending beam test
RTFOT (T0715) for assessing the low-temperature cracking resistance of asphalt
Mass change rate/% − 0.06 ≤±1.0
Residual ductility at 15 ◦ C/ 36 ≥20 mixes.
cm 3 Marshall Stability test (T0709) and Freeze-thaw splitting test
(T0729) for evaluating the water stability of asphalt mixtures.

Fig. 2. Mixture gradation curve.

3
M. Zhang et al.
IDEAL-CT test was adopted to evaluate the indirect tensile cracking
resistance of hot mix asphalt at the intermediary temperature of 25 ◦ C.
Samples with dimensions of 150 mm in diameter and 62 mm in thickness
were created. The rate of load is 50 mm/min (Zhou et al., 2017). When
the load reached 0.1 kN, the test ended. The load grew initially as
displacement increased before starting to decrease. To assess the com­
binations’ resistance to fracture, cracking test index (CTIndex) and
determining work of fracture (Wfb) were utilized.
2.3.2. Nano-indentation test
2.3.2.1. Nano-indentation test sample preparation. The homogeneity of
the sample surface is highly correlated with the accuracy of NI tests
(Miller et al., 2008). Therefore, during sample preparation it is crucial to
remove the detrimental impact of uneven surfaces on test findings.
(1) A cylindrical Superpave Gyratory Compactor (SGC) specimen
was formed by a rotary compaction method. A test sample of
approximately 1–1.5 cm in length and 1 cm in height was cut
using a precision cutter, including a uniformly flat test area of
RCAs-residual mortar-asphalt mastic.
(2)The epoxy resin was stirred slowly in the same direction; a pro­
portion of it was poured into a cylindrical mold. The cut sample was
placed in the mold with epoxy resin and held under vacuum for 15
min until no air bubbles were produced. Then it was placed at normal
temperature until the epoxy resin adhesive was cured. The cut
sample was cured to a flat cylindrical sample of 2–3 cm diameter and
placed in an electric vacuum drying oven with the mold at a
controlled temperature of 20–30 ◦ C.
(3) Metallographic grinding machines with 100, 400, 800, 1600, and
2500 grit metallographic sandpaper were used to smooth the
surface of the test sample after it was cooled under water. It took
approximately 30 min of polishing to get the entire surface to
reflect light.
(4) Finally, the NI test sample cutting from hot mix asphalt con­
taining RCAs was obtained after washing it with anhydrous
ethanol for 1–5 min and air-drying it. The preparation process of
a test sample is shown in Fig. 3.
Fig. 3. Sample preparation for NI test.
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Journal of Cleaner Production 389 (2023) 136070
(5) The polished samples were subsequently examined using a 3D
confocal laser microscope to get the surface morphology data in
order to confirm the surface quality following polishing and
grinding. The surface roughness was measured using the root
mean square (RMS) of the surface morphology. The test result
demonstrates that the average RMS roughness of the cut-cured
sample from hot mix asphalt after polishing is 127.03 nm,
which meets the uniformity prerequisite of the scored sample.
2.3.2.2. Elastic modulus. A brand-new technique for evaluating the
micro-mechanical performance of multi-phase mixtures is called NI. It
may specify differences in the mechanical properties of ITZs in the
mechanical properties of ITZs and recognize and categorize various
phases of asphalt mixes (Huang et al., 2021). To examine the test piece
and ascertain the micromechanical characteristics of the ITZs, this study
employed a Hysitron Triboindenter (TI950). Each sample was subjected
to a grid NI test utilizing a nanoindenter with a Berkovich tip. A 25 ◦ C
test temperature was used. Within 10,000 nm, the indentation depth
was under control. 3000 μN was chosen as the asphalt mix maximum
load per phase. It was decided to put the single loading time at 20 s
(Tarefder and Faisal, 2012, 2014).
He loading rate and the emptying rate are equal. Through an optical
microscope, the area of interest covering RCAs, ITZs, and asphalt mastic
was chosen as the indent position of the test, and the indent position
diagram is shown in Fig. 4. The distance between adjacent points was set
to 10 μm. The two test locations on the longitudinal line were spaced
apart by 10 m. By using optical microscopy, the position of the inden­
tation for the test was determined to be the region encompassing the
aggregate, the ITZs, and the asphalt mastic.
2.3.3. Electron microscope observation
In this study, ITZs’ precise microstructure was obtained using scan­
ning electron microscopy (SEM) (Sanchez-Cotte et al., 2020; Hou et al.,
2016). Small pieces of epoxy-coated RCAM were manufactured, much
like with the NI test sample preparation procedure. After curing, samples
with dimensions of roughly 10*10*5 mm in length, breadth, and height
were cut using a precision cutter. The cut samples include RCAs, residual
mortar, and asphalt mastic in a consistent and even test area. Fig. 5
M. Zhang et al. Journal of Cleaner Production 389 (2023) 136070

Fig. 4. Indent position diagram.

Fig. 5. Sample preparation for SEM test.

depicts the sample preparation procedure for the SEM test.

2.3.4. Elemental analysis test

To obtain more information about the elements and compound
composition of the ITZs, the elemental analysis method was used to
identify the ITZs between RCAs and asphalt mastic, along with exam­
ining the distribution of chemical elements in the focus area. In this
study, the energy dispersive spectrometer (EDS) was used to scan the
surface of the hot mix asphalt containing RCAs to obtain the elemental
composition and distribution of the ITZs. EDS test samples were pre­
pared in the same way as SEM samples. The EDS image had a dwell time
of 0.1 m/s, a scan time of 512 × 384 pixels, and a scan time of the 30s
(Neto et al., 2019).

3. Results and discussion

3.1. Performance of RCAM

Fig. 8 listed the uniaxial penetration test results. Fig. 6 illustrates that
the ultimate load and penetration strength of the stone mastic asphalt
mixture containing 37.5% RCAs increased by 63.68% and 29.17%
respectively compared to AM. This demonstrates that the RCAM dura­
bility at high temperatures has drastically increased. This is mainly
because the surface of the RCAs itself is rougher than that of the NAs,
and the friction between the aggregates is greater and less prone to
misalignment. Under wheel loading, the embedded effect between the
RCAs is enhanced and the structure becomes more stable, thus
improving the stability at high temperatures of the hot mix asphalt.
Fig. 7 displays the outcomes of the low-temperature bending beam
test. With the incorporation of RCAs, the failure strain of the RCAM
decreased, and the failure stiffness modulus increased. This shows that
the incorporation of RCAs makes the cracking resistance at a low tem­
perature of the hot mix asphalt worse.
Fig. 8 illustrates the results of the freeze-thaw splitting test and the
Marshall stability test. The water stability of the stone mastic asphalt
Fig. 6. High-temperature performance.
mixture somewhat deteriorated with the addition of RCAs. The stone
mastic asphalt mixture contains finer RCAs and contains relatively more
residual mortar and pores, resulting in its water stability decreasing as
the RCAs are incorporated.
Fig. 9 displays the IDEAL-CT test results. Compared with AM of the
same gradation, the CTIndex of stone mastic asphalt mixture with RCAs
was reduced by 8.16%. The trend of Wfb is the same as the CTIndex. As
RCAs are incorporated, less energy is required to produce cracks in the
RCAM. RCAM is more prone to cracking.
3.2. Microstructure of ITZs in RCAM
SEM images were used to visually confirm that there was a distinct
boundary between the ITZs-R-A and the asphalt mastic. The density
variation with crystal distribution was used to identify the ITZs areas.

5
M. Zhang et al.
Fig. 7. Low-temperature bending beam.
Fig. 8. Marshall stability and freeze-thaw splitting.
Fig. 9. IDEAL splitting.
The asphalt mastic was applied to the RCAs surface. As the position of
the asphalt mastic-mortar phase connection, the ITZs-R-A has an inter­
nal gap of 2–5 μm, as shown in Figs. 10 and 11. It could be brought on by
the buildup of mineral dust and fine aggregate particles that reach the
region of the interface and obstruct the asphalt mastic ability to
penetrate.
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Journal of Cleaner Production 389 (2023) 136070
Fig. 10. Joint seams in ITZs-R-A.
Fig. 11. The internal structure of ITZs-R-A.
The hydrate in the ITZs-A-R zone contains free silica, a small quantity
of whisker-like calcarenite crystals, and some well-crystallized floccu­
lated CH. Comparatively speaking, the ITZs-A-R adheres better than the
ITZs-R-A. It is true that there are gaps between ITZs-A-R and RCAs, but
with time, the chemical reaction causes the hydration products to
gradually close the pores, improving integrity between ITZs-A-R and the
mortar interface, as illustrated in Fig. 12. Uncompacted holes may be
seen inside the ITZs-A-R, as shown in Fig. 13, because an improved
agglomeration effect has not been created, since the inside of the ITZs-A-
R is distant from the aggregate,
The performance of the ITZs is seriously impacted by numerous
uncompacted pores and joints between the interfaces, which results in
compressive stress and weakens the rigidity of the bond between the
asphalt mastic and the aggregate. It might be one of the reasons that ITZs
are prone to break down first.
3.3. Micromechanical properties of ITZs in RCAM
3.3.1. Elastic-mechanical characteristics of RCAM
In sequence of extension from the aggregate, the following five
different phases make up the joint interface of the RCAs and asphalt
mastic: aggregate, ITZs-A-R, residual mortar, ITZs-R-A, and asphalt
mastic. Because the ITZs are heterogeneous, single-phase testing was
necessary to determine the phase composition by choosing the matching
M. Zhang et al.
Fig. 12. Chemical composition in ITZs-A-R.
Fig. 13. The internal structure of ITZs-A-R.
regions from several samples. The NI test area is shown in Fig. 14. Each
phase included indentation testing on a 10*10 grid. Each indentation
loading-unloading curves was recorded, and using the Oliver-Pharr
method, the modulus of individual materials in Table 3 were calcu­
lated from the elastic unloading curve.
The grid indentation approach, as shown in Fig. 15, also depicts the
features of the indentation curve for each phase in addition to the me­
chanical properties of the various phases. The maximum indentation
depth makes it easier to identify multi-phase interface indentations and
Fig. 14. Single-phase material testing area for RCAM.
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Journal of Cleaner Production 389 (2023) 136070
Table 3
Average modulus and coefficient of variation of different materials.
Material Residual mortar Asphalt mastic Aggregate
Modulus/GPa 30.23 1.62 50.65
Coefficient of Variation/% 31.2 15.8 12.5
Fig. 15. Indentation curves for aggregate, residual mortar, and asphalt mastic.
enables for the obvious identification of the various phases. The asphalt
mastic phase has an average modulus of 1.62 GPa and a maximum
indentation depth of over 2000 nm. For the same test method, the
aggregate shows good mechanical properties, with an indentation depth
of 800–1000 nm and an average modulus of 50.65 GPa. The residual
mortar displays a loading-depth diagram that is similar to the NA with
an indentation depth of 1000–1500 nm. However, as demonstrated by
the loading and modulus distinctions, the load-depth curves charac­
terize the aggregate, residual mortar, and asphalt mastic well and can
distinguish between the different zones well.
3.3.2. Elastic-mechanical characteristics of ITZs-R-A
In this investigation, a suitable test region, as shown in Fig. 16, was
chosen, and indentation tests on the ITZs-R-A were performed. Fig. 17
depicts the obtained load-displacement curve. The results demonstrate
that the indentation modulus is much higher in the old slurry matrix
near to the ITZs-R-A than in the asphalt area. Using the modulus data
from the NI tests, indentation modulus contour maps for the area of the
ITZs-R-A were created and used to investigate the mechanical properties
individually, as shown in Fig. 18. The morphology of ITZs can be
distinguished distinctly in Fig. 18. However, the modulus contour maps
were not equally distributed due to the asphalt mastic and residual
mortar, as well as considerable variations in the longitudinal and lateral
averaging statistics. In this work, frequency statistics for modulus
M. Zhang et al.
Fig. 16. ITZs-R-A test area.
Fig. 17. Load-displacement curve in ITZs-R-A.
Fig. 18. Modulus contour map of ITZs-R-A.
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Journal of Cleaner Production 389 (2023) 136070
contour images were obtained for appropriate intervals, and statistical
averages and deviations were then applied to modulus histograms over
the ITZs-R-A. The modulus frequency diagram across the ITZs-R-A is
given in Fig. 19 to detect the indentation modulus distribution in specific
directions and estimate the thickness of the ITZs-R-A.
Fig. 19 depicts the modulus of elasticity trend from the asphalt
mastic phase to the residual mortar phase. The material is in the asphalt
mastic phase between 0 and 40 μm on the grid distance, with a modulus
of around 0–5 GPa. The modulus fluctuates because to the minor amount
of mineral fines in the mastic phase. In the ITZs-R-A, the modulus is
between 10 GPa and 25 GPa between 40 and 66 μm on the grid distance.
Beyond 66 μm, the modulus increases in the test area at the mortar side.
The thickness of the ITZs-R-A is 26 μm baed on the analysis of the lateral
variation of characteristics surrounding the aggregate. The findings
indicate that 28.68 GPa is the average modulus of the ITZs-R-A.
3.3.3. Elastic-mechanical characteristics of ITZs-A-R
A grid area with 100 indentation points was tested in the ITZs-A-R
test area in Fig. 20 to determine the distribution of the mechanical
properties in the ITZs-A-R. Fig. 21 shows the load-displacement curve
that was obtained. Figs. 22 and 23 depict the modulus contour map and
modulus frequency diagram of ITZs-A-R, which were created using the
same technique as ITZs-R-A.
Fig. 23 depicts the modulus of elasticity trend from the mortar phase
to the aggregate phase. The grid distance is between 0 and 15 μm, in the
mortar phase, when the modulus of the material is low, 0–3 GPa, and the
tiny amount of material included in the mastic phase leads its average
modulus to fall and become prone to numerical variations. The modulus
in the ITZs-A-R is between 10 and 30 GPa between 15 and 40 μm. The
material’s modulus of elasticity rises steadily as it gets closer to the
aggregate zone at a distance of 10 μm, and subsequently, the growth
rates of both indicators decrease as the distance grows for each sample.
The modulus of the material gradually increases above 85 μm before
slowing down as it approaches the dense zone. It can be observed from
Fig. 10 that the ITZs-A-R is primarily dispersed in the outside half of the
NA and has a consistent thickness distribution.
The ITZs-A-R is 25 μm thick after examining the lateral change of
characteristics around the aggregate. ITZs-A-R has an average modulus
of 24.01 GPa, which is 1.3–1.5 times that of residual mortar. It has been
found in available studies that the thickness of ITZs between the
aggregate and the asphalt mastic in AM is in the range of 5 μm–20 μm
Fig. 19. Modulus frequency diagram of ITZs-R-A.
M. Zhang et al.
Fig. 20. ITZs-A-R test area.
Fig. 21. Load-displacement curve in ITZs-A-R.
(Zhu et al., 2017). In addition, the range of elastic modulus of ITZs in the
AM is 10–40 GPa and the average modulus is 26.60 GPa. By comparing
the mechanical properties of ITZs in AM and RCAM, it is discovered that
due to the introduction of mortar, the thickness of ITZs in RCAM is larger
than that in AM. The weakening of the bonding force between the phases
in RCAM results in the overall deterioration of RCAM performance. The
ITZs-A-R has a smaller elastic modulus than ITZs-R-A. The residual
mortar in RCAs should be further modified to improve the performance
of RCAM.
3.4. Element variation across ITZs in RCAM
3.4.1. Chemical properties of ITZs-R-A
A specimen containing the joint between the bituminous mastic and
mortar was prepared as a test sample of the ITZs-R-A. The EDS ITZs-R-A
area and the distribution of elements inside it are depicted in a layered
image in Fig. 24 that highlights the various element classes, contents,
and distribution. The RCAM is principally composed of calcium (Ca),
silicon (Si), carbon (C), and oxygen (O). The electronic image and the
chemical composition reveal a clear ITZs-R-A between the asphalt
9
Journal of Cleaner Production 389 (2023) 136070
Fig. 22. Modulus contour map of ITZs-A-R.
Fig. 23. Modulus frequency diagram of ITZs-A-R.
mastic and the residual mortar.
By performing an EDS line scan, more detailed information can be
obtained regarding the thickness and chemical content of the ITZs-R-A
along the mortar-ITZs-asphalt line. The distribution of the primary
characteristic elements (C, O, Si, and Ca) as well as the fluctuation in
values of the EDS elemental lines in the transition zone are shown in
Figs. 25 and 26. As can be seen from Figs. 25 and 26, the distribution of
Ca and Si in the mortar region of the mortar-ITZ-asphalt continues to
remain high, while the variation in counts of both C and O along the
entire scan line of the samples remains relatively evenly distributed and
may cause elevated variations in C and O with the modified asphalt in
the asphalt mix. Observations of the EDS line scan showed that the ITZs-
R-A had elemental contents between the coarse aggregate and the
asphalt mastic and contained a large distribution of high peak values of
Ca, Si, and O, which demonstrates that the ITZs-R-A exists in the RCAM.
The thickness of the ITZs-R-A is 32 μm.
3.4.2. Chemical properties of ITZs-A-R
Specimens containing the location of the mortar-natural aggregate
M. Zhang et al. Journal of Cleaner Production 389 (2023) 136070

Fig. 24. EDS surface scan of the ITZs-R-A area layered image.

Fig. 25. EDS line scanning results along the residual mortar-ITZs-R-A-asphalt mastic line.

joint were prepared as ITZs-A-R test samples. Fig. 27 shows a single-
element surface scan image of the ITZs-A-R area. In comparison with
the mortar layer images, the increase and superimposition of the point-
level facets in the images imply a richer elemental composition, and the
dispersion is complicated by the multi-phase connection.
The composition of the ITZs-A-R differs significantly between the
tested areas, as seen in Fig. 27. Aggregate and residual mortar is both
composed principally of calcium oxide and its derivatives, with the
natural aggregate having a lower calcium content than the mortar layer,
but a higher carbon content. Significant increase in aluminum and sili­
con content around the area close to the mortar layer.
The fluctuation in the counts of the EDS elemental lines in the ITZs
with the distribution of the primary elements (C, O, Si, and Ca) is
depicted in Figs. 28 and 29, respectively. Observation of the EDS line
scan shows that the elemental content of the ITZs-A-R lies between the
asphalt mastic and the coarse aggregate, resulting in large fluctuations
in calcium, silicon, and oxygen elements within the transition zone,
which proves that the ITZs-A-R does exist in RCAM. According to the
elemental profile of the sample, the thickness of the ITZs-A-R obtained
by the EDS-based approach is 27 μm. This conclusion is consistent with
the NI test results. The thickness of the ITZs in the AM by EDS line scan
was measured to be 12 μm. (Zhu et al., 2017). In line with the findings of

10
M. Zhang et al.
Fig. 26. Distribution of key characteristic elements in the ITZs-R-A.
Fig. 27. EDS surface scan of ITZs-A-R area layered image.
the NI experiments, the thickness of the ITZs in RCAM is greater than AM
due to the introduction of RCAs. This results in an overall inferior per­
formance of RCAM than AM, which is consistent with the performance
test findings.
4. Conclusions and findings
Pores and micro-cracks characterize the ITZs between RCAs and
asphalt mastic, which can easily lead to stress concentration and struc­
tural damage. These low strength zones are where failure in the hot mix
asphalt is mostly generated and developed. This paper provides a
micromechanical properties, morphological characteristics and chemi­
cal composition properties study on the ITZs between RCAs and asphalt
mastic in hot mix asphalt. The effect of RCAs on the ITZs performance,
elastic modulus and thickness was investigated.
(1) ITZs in hot mix asphalt are successfully identified by using the
difference in mechanical properties between RCAs and asphalt
11
Journal of Cleaner Production 389 (2023) 136070
mastic. The ITZs-A-R has a 25 μm thickness and an average
modulus of elasticity of 24.01 GPa. The ITZs-R-A has a thickness
of 26 μm and an average elasticity modulus of 28.68 GPa. This is
consistent with the EDS scanning results.
(2) The ITZs-A-R has a smaller elastic modulus than ITZs-R-A. To
enhance RCAM performance, more modifications to the residual
mortar in RCAs are necessary. Based on this, it is possible to
further explore how ITZs affect hot mix asphalt performance.
(3) The thickness of the ITZs in RCAM is greater than that of AM due
to the introduction of RCAs. It results in an overall inferior per­
formance of RCAM than AM, which is consistent with the per­
formance test results.
(4) The asphalt mastic adjacent to the RCAs displays a denser
appearance than that unconnected to the RCAs. The penetration
of asphalt binder aids in increasing the strength of the porous
mortar.
M. Zhang et al. Journal of Cleaner Production 389 (2023) 136070

Fig. 28. EDS line scan results along the residual mortar-ITZs-A-R-aggregate line.

Fig. 29. Distribution of key characteristic elements in the ITZs-A-R.

CRediT authorship contribution statement the work reported in this paper.

Mengyun Zhang: Conceptualization, Software, Formal analysis, Data availability

Investigation, Data curation, Writing – original draft, Visualization.
Changjiang Kou: Conceptualization, Methodology, Software, Valida­
tion, Formal analysis, Writing – original draft, Writing – review &
editing, Visualization, Project administration, Funding acquisition.
Aihong Kang: Methodology, Validation, Writing – review & editing,
Supervision. Peng Xiao: Methodology, Validation, Writing – review &
editing, Supervision. Haotian Hu: Investigation, Data curation.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
Data will be made available on request.
Acknowledgments
All authors gratefully acknowledge the financial support from Na­
tional Natural Science Foundation of China (Grant Number 51908487),
Natural Science Foundation for Youths of Jiangsu Province (Grant
Number BK20190913), Yangzhou University High-level Talent Support
Program, Postgraduate Research & Practice Innovation Program of
Jiangsu Province (SJCX21_1582), the Jiangsu Science and Technology
Association Promotion Project for the Youths (Grant Number 2021-090)

12
M. Zhang et al.
and the Qing Lan Project of Jiangsu Province.
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