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Journal of Building Engineering 72 (2023) 106649

Contents lists available at ScienceDirect

Journal of Building Engineering


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

Wrapped coal gangue aggregate enhancement ITZ and mechanical


property of concrete suitable for large-scale industrial use
Shaohui Zhang a, b, **, Mengyuan Cao b, KaiFeng Zhang d, Jian Yuan e, Yan Wang b, c, *
a
College of Civil Engineering, Xi’an University of Architecture and Technology, Xi’an, 710055, China
b
College of Materials Science and Engineering, Xi’an University of Architecture and Technology, Xi’an, 710055, China
c
State Key Laboratory of Green Building in Western China, Xi’an University of Architecture and Technology, Xi’an, 710055, China
d
China West Construction North Co., Ltd., Xi’an, 710055, China
e
Rocket Force University of Engineering Xi’an, 710055, China

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

Keywords: The disadvantages of coal gangue such as low strength, high water absorption, and weak bonding
Coal gangue aggregate ability with concrete matrix limit its large-scale application as coarse aggregate. Inspired by the
Surface modification traditional Chinese culture of Roll Rice Dumpling, this paper uses six cement-based paste materials
Crush index to wrap the surface of coal gangue aggregate (CGA) to enhance its performance and ITZ per­
Mechanical property formance. The density, crushing index, water absorption of modified CGA and the strength, water
Vickers hardness
absorption, load-deflection curve, stress-strain curve, Vickers hardness, and microstructure of
Interfacial transition zone
modified coal gangue aggregate concrete (CGAC) were studied, and the relationship between
modified CGA properties and CGAC properties was also analyzed. The results showed that the
apparent density and bulk density of modified CGA only changed 0.078%–5.6% and 0.71%–2.1%.
The crushing index is significantly reduced by 15.9%–57.5% due to the hard shell formed by the
wrapping material in the CGA. The compressive strength and splitting tensile strength of modified
CGAC are significantly improved, and its flexural toughness can be increased by up to 95.2%. The
modified CGAC shows good ductility, and its peak stress and ultimate strain are increased by
35.5%–60.6% and 46.3%–258.3%, respectively. The microhardness of modified CGA and ITZ
increased by 97.7%–158.6% and 27.9%–129.2% respectively, and the structure of ITZ was dense,
the modified CGAC had higher mechanical properties. The cost of modified CGAC can be saved by
30.4%, and the carbon emission is only 73.3% of the same grade traditional concrete. Through
this technology, we hope to provide an application framework for the industrialization, large-
scale, and high value utilization of coal gangue waste.

1. Introduction
Coal gangue as China’s largest industrial waste, has accumulated more than 700 million tons of emissions, annual emissions of
more than 70 million tons [1]. Coal gangue accumulation has brought serious challenges to the environment [2,3]. Large amounts of
coal gangue discharge and storage destroy and occupy large amounts of land resources [4]. Water pollution, soil quality decline,
ecosystem degradation, and biodiversity loss are very serious in coal gangue storage area. Coal gangue contains toxic heavy metals
such as lead, cadmium, mercury, arsenic and chromium [5]. These elements enter or penetrate into the soil through rainwater,

* Corresponding author. College of Materials Science and Engineering, Xi’an University of Architecture and Technology, Xi’an, 710055, China.
** Corresponding author. College of Civil Engineering, Xi’an University of Architecture and Technology, Xi’an, 710055, China.
E-mail addresses: zhangshaohui@xauat.edu.cn (S. Zhang), wangyanwjx@126.com (Y. Wang).

https://doi.org/10.1016/j.jobe.2023.106649
Received 11 January 2023; Received in revised form 19 April 2023; Accepted 23 April 2023
Available online 25 April 2023
2352-7102/© 2023 Elsevier Ltd. All rights reserved.
S. Zhang et al. Journal of Building Engineering 72 (2023) 106649

seriously affecting the soil or water environment and may be toxic to the human body, endangering the entire ecosystem and causing
secondary pollution [6]. The spontaneous combustion characteristics of coal gangue will produce flue gas and acidification compo­
nents during the combustion process, and the dust produced by weathering is also one of the culprits of haze [7]. How to effectively use
these industrial solid wastes, transform waste into available resources, and reduce environmental pollution is imminent. The
comprehensive utilization rate of coal gangue in developed countries is higher, such as Europe and the United States has more than
90%. However, the utilization in developing countries such as China remains is still quite low [8]. To this end, the Chinese government
has issued the Management Measures for Comprehensive Utilization of Coal Gangue, which explicitly prohibits the construction of per­
manent coal gangue dumps and improves the utilization rate of coal gangue.
Coal gangue is a mixture of carbonaceous, argillaceous and sandy shale. The main chemical components are SiO2 (about 46.7%),
Al2O3 (about 15.45%), and a small amount of CaO, Fe2O3 and other metal oxides [9]. These chemical and mineral properties similar to
natural aggregates (NA) make it possible to use coal gangue as aggregate to prepare concrete [10]. The C15 ~ C40 concrete can be
prepared by using coal gangue aggregate (CGA) instead of NA [11]. Due to the difference of coal forming conditions and coal mining
conditions, the structure of coal gangue is more loose, porous and flake particles than NA, and its performance fluctuates greatly. When
coal gangue is used as coarse aggregate in concrete, concrete is easily destroyed from the interface transition zone (ITZ), and the CGA
itself is crushed [12]. The water absorption of CGA concrete was significantly higher than that of NA concrete [13], and the high
carbon content of CGA and its weak interface bonding with concrete matrix pose a potential threat to the durability of concrete.
Therefore, the dosage of CGA (CGA) must be strictly controlled, otherwise the mechanical properties and durability of concrete will be
reduced [14–16]. It is necessary to modify CGA to make up for the defects of CGA, so as to improve the mechanical properties and
durability of concrete, expand the use range and realize the high value utilization of coal gangue [17].
At present, there are four methods to improve the activity of coal gangue, namely thermal activation [18], mechanical activation
[19], microwave activation [20] and composite activation [21,22]. Mechanical activation should control grinding time to prevent
particle agglomeration and avoid energy waste. In addition, the grinding process cannot completely change the mineral phase of coal
gangue [18]. The key to calcination of coal gangue is the selection of calcination temperature and calcination time. The optimal
calcination temperature of specific clay minerals may lead to the recrystallization or decomposition of other mineral components (such
as carbonate). Therefore, it seems complicated to ensure complete dehydroxylation of all clay minerals in coal gangue [23]. Microwave
activation of coal gangue is rarely reported, and the selection of parameters such as irradiation power and irradiation time is worth
exploring [24]. In addition, it also involves cumbersome processes, requires complex equipment, and consumes additional energy,
which runs counter to the low-carbon and green advocated in the field of civil engineering. The above methods are likely to damage the
coal gangue matrix and it is necessary to systematically study the differences and efficiency between different modification methods
[18].
We have learned from the traditional Chinese culture “roll rice dumpling”. It is to shake the dumplings into wet dumpling powder to
make dumplings. Inspired by this process, we tried to improve the performance of CGA and interface between aggregate and concrete
by wrapping a layer of cement paste on the surface of CGA. In this study, six aggregate modification methods suitable for large-scale
industrial applications were selected. The effects of different modification methods on the apparent density, bulk density, crush index,
water absorption, moisture content, and microstructure of CGA were compared and analyzed. The compressive strength, splitting
tensile strength, water absorption, load-deflection curve, and stress-strain curve of concrete with modified CGA were also analyzed.
Furthermore, the width and hardness of the ITZ were quantitatively analyzed based on the microhardness measurement, and the
morphology of the ITZ was analyzed by SEM. This study intends to provide an application framework for the industrialization, large-
scale, and high-value utilization of coal gangue.

Fig. 1. Particle size distribution of CGAraw.

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2. Raw materials and methods


2.1. Raw materials
The block coal gangue is mechanically broken and sieved into CGAraw with particle size of 5–20 mm, and its particle size distri­
bution is shown in Fig. 1. The chemical composition of CGAraw tested by X-ray Fluorescence is shown in Table 1. The main chemical
components of CGAraw are SiO2 (58.39%) and Al2O3 (27.52%) and mineral composition is mainly composed of quartz, anorthite, and
kaolinite, as shown in Fig. 2.
Ordinary Portland cement (OPC, Strength grade of 42.5), fly ash (FA), and silica fume (SF) were used, whose chemical compositions
and physical properties were shown in Tables 1 and 2. The river sand (medium sand) with bulk density and apparent density of 1478
and 2586 kg/m3 was adopted as fine aggregate, and its fineness modulus is 2.6. The polycarboxylate superplasticizer with a water
reduction rate of 25% was adopted.

2.2. Methods
2.2.1. Modification method of CGAraw
CGAraw is modified by six methods, namely, cement-based wrapping modification (CM), epoxy resin wrapping modification (EM),
epoxy resin + cement-based wrapping modification (ECM), cement-based + FA wrapping modification (CFM), cement-based + SF
wrapping modification (CSM), and calcination modification (CAM).
CM, CFM, and CSM test steps are as follows (Fig. 3). The CGAraw was soaked in water for 1 h (20 mm above the top of the aggregate),
and then the cement, cement + 10% FA and cement + 10% SF were added into pre-wetted CGAraw to stir and shake until the surface of
CGAraw was completely wrapped. After resting for 12 h, the covered CGAs was placed in the standard curing room (20 ± 2 ◦ C and 95%
RH) for curing to the ages of 1, 3, 7, and 28 days. The mass ratio of cement-based materials wrapped on the aggregate surface to
aggregate is 1:28.
EM test steps are as follows. Add an appropriate amount of epoxy resin (High permeable-liquid type) into the air-dried CGAraw and
stir until the surface of CGAraw is completely wrapped. Then the aggregate is spread to prevent aggregate particles from bonding
together, and the test is carried out after 1 day of rest. The mass ratio of coal gangue and epoxy resin is 88:1.
ECM test steps are as follows (Fig. 4(a) and (b)). Add an appropriate amount of epoxy resin and polyvinyl alcohol solution (con­
centration of 9%) in CGAraw, stir and shake to the surface of CGAraw to form a bonding layer. Then cement-based materials were added
to stir and shake to form cement shell on the CGAraw. After 1 day of rest, the wrapped aggregate was curing in the standard curing room
((20 ± 2 ◦ C and 95% RH)) for 7 days. The mass ratio of coal gangue and epoxy resin + cement-based is 88:1.
CAM test steps are as follows (Fig. 4(c)). The CGAraw was dried at 105 ◦ C, then the aggregate is laid in a square crucible with 30 cm,
25 cm wide, 10 cm high, and 2 cm wall thickness, and calcined in a muffle furnace at 600 ◦ C for 45 min.

2.2.2. Test method of modified CGA performance


The apparent density (ρ0), bulk density (ρ1), crush index (Qe) (The schematic diagram of the test device is shown in Fig. 5), water
absorption (w), and moisture content (Z) of modified and unmodified CGCAs were tested according to Chinese Standard GB/T 14,685
[25].

2.2.3. Preparation and performance test method of modified CGA concrete


The mix proportion of modified CGA concrete is shown in Table 3. The CGA replaces NA with equal volume [23] and the
replacement rates are 100% and 60%, respectively. The untreated coal gangue aggregate concrete is used as the control group.
The compressive strength, splitting tensile strength and stress-strain test are conducted according to the Chinese standard GB/T
50,081 [26]. The schematic diagram of the stress-strain test device is shown in Fig. 6. Water absorption test of modified CGCAs
concrete according to ASTM C1585 [27] (Fig. 7).
The specimens of 40 × 40 × 20 mm were cut from concrete, and soaked in ethanol solution for 48 h, and then dried at 60 ◦ C for 48 h.
Subsequently, the samples were ground with 600 mesh and 800 mesh SiC, and rinsed rapidly with ethanol solution. The treated
samples were placed in a sealed bag for the morphology analysis of the ITZ.
The microhardness test and data processing steps of specimens ITZ are as follows. The CGA concrete was sliced after curing for 60
days, with the size of 40 mm * 40 mm * 20 mm. First, the test block is impregnated with epoxy resin in the vacuum chamber. Then
different types of sandpaper (180#, 320#, 600#, 1200#, and 2000#) were used to pre-polishing the surface (Fig. 8 (a)). Then 1 μm
diamond spray polishing agent was used for 5min (Fig. 8(b)). The test point is shown in Fig. 8(c).
The test loads are 4.903 N (500gf) and 9.806 N (1000gf) and the loading time is 15s. The indentation area (S) and microhardness
(HV) are calculated by E.q. (3) and (4). In order to reduce the discreteness of test data, six groups of data were tested at each point in

Table 1
The chemical composition of materials.

Materials SiO2 Al2O3 CaO Fe2O3 K2O TiO2 NaO2 MgO SO3 Loss

NA 8.42 3.99 82.78 0.89 1.33 0.26 – – – –


CGAraw 58.39 27.52 0.59 6.65 4.03 0.90 – – – –
OPC 19.68 4.72 61.83 3.66 1.27 2.73 0.43 1.31 0.05 2.23
FA 49.71 16.57 19.90 5.70 0.30 2.40 0.35 1.20 0.35 2.57
SF 91.04 0.97 1.63 1.04 0.36 0.21 0.28 1.20 0.82 1.77

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Fig. 2. XRD pattern of CGAraw and NA.

Table 2
The physical properties of OPC.

water requirement of normal consistency/% Fineness/% Setting time/min Flexural strength/MPa Compressive strength/MPa

Initial setting Final setting 3d 28d 3d 28d

26.5 3.6 135 225 3.9 7.1 19.8 44.6

Fig. 3. The schematic diagram of the wrapping process and photographs of CM, CFM, and CSM.

Fig. 8(c), and the average value was taken as the final result.

d2
S= (3)
2 sin(θ/2)

HV = 1.854F/d (4)

Where, HV is Vickers hardness (MPa); S is the indentation area (mm2); d is the average length of the indentation diagonal (mm); F is the
test force (N); θ is the contact angle between the indenter and the specimen surface, θ = 136◦ .

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Fig. 4. The schematic diagram of the wrapping process and photographs of modified aggregates of EM and ECM.

Fig. 5. Measuring instrument for crushing index.

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Table 3
The mix proportion of modified CGCAs concrete (kg/m3).

Numbering Cement Water Fine aggregate Modified CGA (Replacement rate 100%) Modified CGA (Replacement rate 100%)

NA Modified CGCAs

CGA 1043 – –
PCGA
CM 400 152 740
EM
ECM – 443 626
CAM

Note: The codes of CGA, PCGA, CM, EM, ECM and CAM refer to concrete prepared by untreated aggregate, pre-wetting of untreated aggregate, cement-based modified
aggregate (Curing for 7-d), epoxy resin modified aggregate, epoxy resin + cement-based modified aggregate (Curing for 7-d), and calcined modified aggregate,
respectively.

Fig. 6. The schematic diagram of stress-strain test device.

Fig. 7. The schematic diagram of water absorption test device.

Fig. 8. Preparation and testing of microhardness test samples.

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3. Results and discussion


3.1. Properties of modified CGA
3.1.1. Apparent density and bulk density of modified CGA
The apparent density and bulk density of modified CGA is shown in Fig. 9. Compared with unmodified CGA, the apparent density
and bulk density of CGA modified by various modification methods were improved, but the increase was not significant, which were
0.078%–5.6% and 0.71%–2.1%, respectively. Among them, The CM, CFM, CSM, and CAM have great influence on the apparent
density, and the apparent density of CGA modified by CM, CFM, and CSM increases with the increase of curing age. It can be found that
CGA modified by CM, CFM, CSM, and CAM can meet the requirements of Chinese Standard 14,685–2011 [25].

3.1.2. Crush index of modified CGA


The crushing index of modified CGA is shown in Fig. 10. The crushing index decreased significantly after CGA modified by EM and
ECM, with the amplitudes of 49.1% and 57.5%. After the aggregate is wrapped by epoxy resin, a hard shell is formed on the outer
surface of the aggregate (as shown in Fig. 4 (b)). When the aggregate is stressed, the micro-cracks inside the aggregate are limited by
the hard shell on the outer surface, thereby improving the compressive performance of the aggregate [28]. The crushing index of the
CGA modified by CM, CFM, and CSM did not decrease significantly after curing for 1 day. With the continuous hydration of cement and
the “pozzolanic effect” of FA and SF [29] the hardened cement-based material wrapped on the outer surface of the aggregate and
formed a hard wrapping layer (as shown in Fig. 3 (b)).
The crushing index of roasted CGA decreased by 21.6%. This is due to the dehydroxylation of kaolinite during the calcination of
CGA [30]. When the CGA is calcined at 500 ◦ C, the hydroxyl group of kaolinite in aggregate is decomposed and begins to decompose
into amorphous metakaolinite [8,31] (the decomposition process is shown in E.q. (10)), which improves the chemical reaction activity
of kaolinite.

Al2O3⸱2SiO2⸱2H2O500 ◦ C →Al2O3⸱2SiO2⸱2H2O (g) (10)

The unmodified CGA belongs to Class II according to the crushing index (according to the standard, the crushing index ≤20%
belongs to Class II) [25]. After being modified by EM and ECM, the crushing index of CGA can meet the requirements of class I (the
crushing index of class I crushed aggregate in the standard should be less than 10%). The CGA modified by CAM, CM, CFM, and CSM
(before curing 3 days) still belongs to class II, but that of CGA modified by CM, CFM, and CSM after curing 7 days can meet the re­
quirements of class I.

3.1.3. Water absorption and moisture content of modified CGA


The water absorption of modified CGA is shown in Fig. 11. After modification by various methods, the water absorption of CGA
increased greatly except EM, and the growth rate was 41.7%–150%. Moreover, after modified by CM, CFM, and CSM, the water
absorption of aggregate increased with the increase of curing age except CM curing for 1 d. The outer surface of the CGA is wrapped by
a layer of cement, cement + FA, or cement + SF. These wrapping materials themselves absorb water rapidly, resulting in a sharp
increase in the water absorption of the aggregate.
After calcination modification, the water absorption of the CGA also showed increase by 66.7%, which is due to the loss of all free
water and part of the chemically bound water in the aggregate during the calcination process, as shown in E.q. (10) [8,31,32]. In
addition, calcination can also cause aggregate cracking, which also increases the water absorption of the CGA [23]. EM is the only
modification method for the decrease of aggregate water absorption among all the aggregate modification methods, with a decrease of
58.3%. The resin is wrapped in the outer layer of the aggregate, and the impermeable performance of the resin reduces the water
absorption property of the aggregate.
The moisture content of modified CGA is shown in Fig. 12. The change trend of moisture content of modified CGA is consistent with
that of water absorption, that is, except for EM and CAM, the moisture content of CGA modified by other modification methods has

Fig. 9. Apparent density (a) and bulk density (b) of modified CGA.

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Fig. 10. Crush index of modified CGA.

Fig. 11. Water absorption of modified CGA.

been greatly improved, the increase rate is 18.2%–154.5%, and even 318.2% (CFM modified curing for 1 day). The modification
processes of ECM, CM, CSM, and CFM need to be soaked water treatment (see the description in Section 2.2.1), which increases the
moisture content in the aggregate. After EM and CAM modification, the moisture content of the aggregate decreased sharply, only
0.4% and 0.1%. Compared with the untreated aggregate, the reductions were 63.6% and 90.9%, respectively. In EM treatment, the

Fig. 12. Moisture content of modified CGA.

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aggregate does not need soaking water treatment. After CAM treatment, all the free water and part of the chemical bond water in the
aggregate are lost during the calcination process [33], the moisture content of the aggregate decreases.

3.2. Mechanical properties of modified CGA concrete


3.2.1. Compressive and splitting tensile strength of modified CGA concrete
The compressive strength and splitting tensile strength of concrete with 100% CGA modified by various modification methods
(Fig. 13) have been greatly improved, with an increase of 13.0%–32.9% and 7.4%–39.6%, respectively. CM has the most obvious
improvement effect on the strength of concrete among all the modification methods, and the compressive strength and splitting tensile
strength increase by 29.5% and 29.4%, respectively, although the improvement effect is not obvious at early curing (3 days). The early
compressive strength of CGA, PCGA, CM, EM, CAM, and CSM concrete increases greatly with the curing age, especially in 3–7 days,
which is due to the internal curing effect of CGA [34].
The crushing index has the most significant influence on the strength of concrete among all the evaluation indexes of aggregate
[35]. The performance of CGA is poor, and its crushing index is as high as 16.7%, so the strength of concrete prepared by CGA is the
lowest in all groups [23]. After modification of CGA, its own performance has greatly improved, the crushing index is greatly
decreased, and the interface bonding performance with concrete is enhanced (see Figs. 21 and 22), the strength of concrete prepared is
greatly increased [36]. The outer surface of the CM modified aggregate is covered with a cement coating, and the interface bonding
performance between the aggregate and the concrete is excellent (see section 3.2.6), so the concrete strength is high. A layer of epoxy
resin was wrapped in the outer layer of CGA modified by EM, which is relatively smooth (see Fig. 4 (b)), and its interface with concrete
was poor (described in Section 3.2.5). The strength of the concrete with CGA modified by EM is basically consistent with that of
unmodified aggregate concrete. Although the aggregate modified by ECM is also wrapped by epoxy resin, there is still a layer of cement
wrapped in its outer layer, which has less defects in the ITZ with the concrete matrix. The strength of concrete with ECM aggregate is
higher than that of with EM. After calcination, the hydroxyl groups in kaolinite on the CGA surface are decomposed [8,31] (the
decomposition process is shown in E.q. (10)). The pozzolanic activity of Si and Al on the aggregate surface further promotes the
hydration of cement, consumes more Ca(OH)2 and improves the early strength of concrete [23,37].
Compared with concrete with CGA 100% replacing NA, the most obvious feature of the compressive strength and splitting tensile
strength of concrete with 60% replacement rate (Fig. 14) is that the strength during the whole curing period is higher than that of 100%
replacement, which are 5.56%–43.4% and 7.14%–38.7% respectively. This is because the compressive strength of NA is significantly
higher than that of CGA. The strengthening effects of CGA modified by various modification methods on the compressive and splitting
tensile strength of concrete with 60% replacement are similar to those with 100% replacement. In addition, it can be seen from the
failure section of concrete that the failure of CGA is that the aggregate is crushed, while the NA is not crushed but destroyed from the
IZT, as shown in Fig. 15, which is also consistent with the performance analysis of aggregate in Section 3.1.

3.2.2. Water absorption of modified CGA concrete


From Fig. 16 (a) and (b), it can be seen that the water absorption of CGA concrete with 100% replacement rate is the highest in 1–5
min, between 0.013–0.038 mm. And the water absorption of concrete with CGA modified by CAM is the largest, which is increased by
33.3%–100%. After 10 min, the water absorption of CGA concrete modified by different methods decreased gradually with time, and
maintains at about 0.001–0.005 mm. The water absorption of CGA concrete under each modification method under 60% replacement
rate is less than 100% replacement rate. It can be seen from Fig. 16(c) and (d) that under the replacement rate of 100% and 60%, the
cumulative water absorption of concrete with CGA modified by each method increases with time. The difference is that the pre-wetted
CGA (PCGA) concrete has the largest cumulative water absorption at 100% replacement rate (after 60 min), while the CM treatment
makes the cumulative water absorption of concrete decrease, compared with the untreated aggregate concrete.
The reason for the decrease of water absorption of CGA concrete in the late stage is that as the continuous entry of water into the

Fig. 13. The compressive strength (a) and splitting tensile strength (b) of concrete with CGA 100% replacing NA.

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Fig. 14. Compressive strength (a) and splitting tensile strength (b) of concrete with CGA 60% replacing NA.

Fig. 15. Failure section morphology of CGA concrete with 60% replacement rate.

pores of concrete through capillarity [38]. In addition, even if the capillary pores form a strong connected network in concrete, for
example, there are larger capillary pores in the ITZ, and the water adsorption rate is still slow. This is because after water enters, stable
or metastable meniscus morphology is formed at the air-water interface, which hinders the entry of water and reduces the later water
absorption [39].
The slope of the curve can be obtained by fitting the curves in Fig. 16 (c) and (d) with the linear regression method, namely, the
water absorption rate of concrete, and the results are shown in Fig. 17. The water absorption rate of modified CGA concrete with 100%
substitution is significantly higher than that of 60% substitution, with a range of 26.2% and 61.5%. This is because CGA has higher
water absorption than NA. At 100% replacement rate, the water absorption of modified CGA concrete (CM, EM, CAM, and ECM) is
lower than that of unmodified and pre-wetted CGA concrete (CGA and PCGA). Although the water absorption of modified CGA is
higher than that of unmodified CGA (see 3.1.3 description), the bonding performance between modified CGA and concrete matrix is
better, and the defects in the ITZ are less (see 3.2.5 and 3.2.6 description), which reduces the channel of water into concrete and makes
the water absorption rate of modified CGA concrete lower [40].

3.2.3. Load-deflection curve of modified CGA concrete


The peak load, ultimate deflection, and flexural toughness of all groups of CGA concrete at 60% substitution rate are greater than
those at 100% substitution rate (see Fig. 18 and Table 4), with the ranges of 2.7%–19.1%, 5.2%–21.5%, and 0.61%–35.6%, which is
consistent with the effect of CGA substitution rate on the compressive strength and flexural strength of concrete. Whether 100% or 60%
of NA are replaced by unmodified and modified CGA, an obvious characteristic of their load-deflection curves is that the post-peak
response is not observed. It can also be observed that the pre-peak curve slope of unmodified CGA concrete is greater than that of
various modified CGA concrete. The PCGA has little effect on the flexural toughness of concrete in all modification methods, only
increasing by 7.0%. In contrast, CM has the best enhancement effect on the flexural toughness of concrete, increasing by 95.2%. This is
because the compressive performance of modified CGA has been greatly improved, which corresponds to a significant decrease in the
crushing index (see 3.1.2 analysis). The interface adhesion between modified CGA and concrete is better (see 3.2.5 and 3.2.6 analysis).
EM modification has a negative impact on the flexural toughness of concrete, and the flexural toughness of concrete decreases by
16.3% at 60% substitution rate. This is the same as the reason why the compressive strength of concrete is not significantly enhanced
because the epoxy resin wrapped on the outer surface of CGA is too smooth and has poor interfacial adhesion with concrete (see
analysis in 3.2.6).

3.2.4. Stress-strain curve of modified CGA concrete


Fig. 19 shows the failure mode of concrete with CGA100% replacing NA under axial compression load. The failure of unmodified

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Fig. 16. Water absorption in time t (Fig. 16(a) and (b)) and cumulative water absorption (Fig. 16 (c) and (d)) of 100% and 60% replacement rate of modified
CGA concrete.

Fig. 17. Water absorption rate of concrete under 100% and 60% replacement rate of modified CGA.

(CGA) and unmodified-prewet (PCGA) CGA concrete is relatively serious, and a large number of spalling and falling blocks appear on
the surface. The CGA itself is crushed (Fig. 19 (a), (b), and (d)), which is inconsistent with the failure of NA. The failure of NA concrete
is destroyed from the ITZ between aggregate and matrix [41]. This is consistent with the evolution of compressive strength, splitting
tensile strength, and load-deflection curve of concrete, that is, the performance of unmodified, unmodified pre-wetted and EM
modified CGA concrete is poor. Conversely, the CM, CAM, and ECM modified CGA concrete only observed many small cracks on the

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Fig. 18. Load deflection curve of modified CGA concrete with 100% (a) and 60% (b) substitution rate.

Table 4
Statistical results of peak load, ultimate deflection, and flexural toughness under 100% and 60% substitution rates of modified CGA concrete.

Aggregate replacement rate CGA PCGA CM EM CAM ECM

Peak load (KN) 100% 16.14 14.00 19.71 16.94 16.55 17.78
60% 16.57 16.15 21.30 15.37 19.71 19.73
Ultimate deflection (mm) 100% 1.15 1.43 1.63 1.49 1.36 1.29
60% 1.21 1.34 1.98 1.35 1.63 1.44
Flexural toughness (N⋅mm) 100% 7915 7662 11,706 9163 8633 8976
60% 7963 8521 15,544 7833 11,707 11,060

Fig. 19. The failure modes of concrete with modified CGA100% replacing NA.

Fig. 20. The stress-strain curves of modified CGA concrete with 100% (a) and 60% (b) substitution rate.

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surface, and did not appear large area spalling and falling block phenomenon.
Fig. 20 shows the stress-strain curves of concrete with modified CGA 100% (Fig. 20 (a)) and 60% (Fig. 20 (b)) replacing NA. At
100% substitution rate, the slope and peak stress of the ascending segment of CM and CAM modified CGA concrete are higher than
those of unmodified, PCGA, EM, and ECM concrete, and the area surrounded by the curve is larger (see Table 5). The CGA concrete
shows high ductility, and the peak stress increases by 36.2%–60.6% and 35.5%–59.7%, respectively. Conversely, the ultimate strain of
concrete with unmodified and unmodified pre-wetted CGA concrete are 46.3%–150.0% and 109.8%–258.3% higher than those of
various modification methods, respectively. In addition, the EM and ECM modified CGA did not improve the ductility of concrete, and
even had a negative impact. The peak stress and peak strain of EM modification are lower than those of unmodified. The effect of
modified CGA on the stress-strain curve of concrete at 60% substitution rate is similar to that at 100% substitution rate. However, the
peak stress and ultimate strain of CM and CAM modified CGA concrete are higher than those of 100% replacement rate, and the area
around the curve is larger, indicating that the ductility of 60% replacement rate concrete is better than that of 100% replacement [42].
This is also consistent with the strength and load-deflection of concrete. In addition, at the substitution rate of 60%, the slope of the
curve rise section of all groups is close, which is quite different from that under the substitution rate of 100%. This indicating that when
the substitution rate is 60%, CGA has little effect on the elastic modulus of concrete [43].

3.2.5. Vickers hardness characteristics of ITZ of modified CGA concrete


Fig. 21 shows the change of Vickers hardness of aggregate, ITZ, and mortar of CGA, ECM and CM samples. Compared with the
unmodified group (CGA), the HV value of aggregate and ITZ increased most significantly after CM modification, which increased by
97.7%–158.6% and 27.9%–129.2%, respectively. This shows that the modified treatment enhances the performance of coal gangue
aggregate and the ITZ between coal gangue aggregate and concrete, which is consistent with the crushing index of aggregate (3.1.2
description) and the strength of concrete (3.2.1 description). The hardness of aggregate and ITZ of unmodified group is significantly
lower than that of mortar. After modification, the gap between the three gradually narrowed, until after CM modification, the hardness
of aggregate and ITZ is higher than that of mortar. This shows that the modified CGA changes the phenomenon that the ITZ in concrete
is a weak zone. This study has proved that this has obvious benefits to the mechanical properties of concrete, and also potentially
indicates that it can also improve the durability of concrete.

3.2.6. Microstructure of modified CGA concrete


The ITZ structure between the unmodified CGA (Fig. 22(a)) and the concrete matrix is loose, and there are obvious micro-cracks,
corresponding to the lower hardness of the ITZ (Fig. 21) and the lower compressive strength and splitting tensile strength of CGA
concrete (Fig. 13). The ITZ structure between the aggregate and the concrete matrix after modification is dense and the bonding
performance is good, which corresponds to the higher ITZ hardness and higher strength of concrete [44]. Among them, the obvious ITZ
boundary can not be distinguished after CM modification. As a comparison, the ITZ structure after EM and ECM modification is also
dense, but there are still obvious boundary traces. Although the ITZ structure of the aggregate after CAM is also dense, the micro-cracks
can be observed in the aggregate.

3.3. Relationship between modified CGA and mechanical properties of concrete


The relationship between aggregate properties and ITZ hardness and corresponding concrete strength is shown in Fig. 23. It can be
seen that the crushing index of unmodified and modified CGA is negatively correlated with the 3d compressive strength of concrete,
while the later compressive strength increases first and then decreases with the increase of crushing index of aggregate. The influence
of crushing index on concrete strength is not the higher the better, but there is a threshold. On the contrary, the compressive strength of
concrete is positively correlated with the ITZ.

Fig. 21. Microhardness of ITZ of CGA, ECM, and CM samples.

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S. Zhang et al. Journal of Building Engineering 72 (2023) 106649

Fig. 22. Micromorphology of modified CGA concrete.

Table 5
Statistical results of peak stress, peak strain, and limit strain under 100% and 60% substitution rates of modified CGA concrete.

Aggregate replacement rate CGA PCGA CM EM CAM ECM

Peak stress (MPa) 100% 24.86 21.93 35.21 24.93 35.03 25.86
60% 26.3 32.6 37.17 22.13 33.06 30.9
3
Peak strain/10− 100% 2.05 3.1 1.3 0.7 2.14 1.35
60% 0.95 1.35 2 2.1 1.34 0.8
3
Ultimate strain/10− 100% 3.0 4.3 2.0 1.2 1.62 2.05
60% 0.68 2.3 2.05 2.65 1.09 1.45

Fig. 23. Relationship between compressive strength of concrete and crushing index of aggrehate (a) and ITZ (b).

4. Analysis of economic and environmental benefits and application prospect


The strength of unmodified CGA concrete is at C25 grade, and the strength grade of modified CGA concrete can be increased to C35.
It is completely feasible to use modified CGA instead of NA to prepare concrete [33]. Large-scale industrial utilization pays more
attention to the economic benefits of solid waste. We compared the production cost of modified CGA concrete with the production cost
of traditional PC, as shown in Table 6, in order to evaluate its sustainability [9]. The production cost of traditional C35 concrete is
338.33 ¥/m3, and the production cost of modified coal gangue aggregate concrete is 233.89–235.31 ¥/m3, saving 30.4%–30.8%.
Application of modified CGA instead of NA replacement rate up to 100%. This increases the market competitiveness of modified CGA
and contributes to the large-scale application of industry. For environmental benefits, the carbon emission modified CGA concrete is
308 kg/m3, which is 73.3% of the traditional concrete with the same strength grade. In the large-scale use of solid waste while also

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S. Zhang et al. Journal of Building Engineering 72 (2023) 106649

Table 6
Comparison of economy and carbon emission between modified CGA concrete and traditional PC.

Unit price ¥/t Carbon emission Traditional PC (C35) MCGA concrete (C35)
t CO2-eq/t 3
Mix proportion t/m Mix proportion t/m3

Preparation of concrete raw materials Water 4.1 0.01232 0.25 0.152


NA 110 0.08 1.16 /
CGAs 35 / / 1.043
Cement 450 0.7 0.466 0.4
Wrapper material FA 90 / / 0.003725
SF 380 / / 0.003725
Cement 450 0.7 / 0.03725
Total cost 338.33 233.891; 234.232; 235.313
CO2 emissions t/m3 0.422 0.308

Note: 1: CM, 2: CFM, and 3: CSM; Carbon emission data from China Products Carbon Footprint Factors Database (2022).

achieving energy saving [45]. We believe that this study can greatly improve the utilization rate of the largest solid waste in China, and
provide support for the realization of the carbon peaking and carbon neutrality goals.
Filling mining is an effective technical means to alleviate surface subsidence, which is of great significance to green coal mining,
improving resource recovery and reducing environmental pollution [46]. Paste filling good fluidity, high strength, easy filling
operation, form a supporting role, is currently the main material of coal mine filling [47]. But many coal mines are deterred from
applying the technology due to its huge cost. The modified CGAC process is simple, the strength of the filler can be increased by 30%–
40%, and the cost can be saved by more than 30%. The coal gangue waste from coal mining can also be directly used in coal mine
filling, thus realizing zero emission from coal mining. Modified coal gangue concrete can also be used for roadway support in coal
mining process. Reinforced coal gangue concrete, steel gangue concrete and sprayed coal gangue concrete [48] provide a solid ma­
terial foundation for coal mine safety, efficient construction and green production.

5. Conclusions
(1) The apparent density and bulk density of modified CGA changed little, only between 0.078%–5.6% and 0.71%–2.1%. The crush
index of CGA modified by CM, CFM, CSM, EM, and ECM is significantly reduced, and the maximum reduction is 57.5%, which
meets the requirement of high-strength concrete. The water absorption of modified CGA increased greatly except EM, with a
growth rate of 41.7%–150%.
(2) The modified CGA significantly improved the compressive strength, splitting tensile strength, and flexural toughness of concrete
by 13.0%–32.9%, 7.4%–39.6%, and 95.2% respectively, and the effect of CM was the best. The slope and peak stress of the
ascending segment of CM and CAM modified CGA concrete are higher than those of unmodified, PCGA, EM, and ECM concrete,
and the area surrounded by the curve is larger. However, the modification treatment had a negative effect on the water ab­
sorption of concrete, and the water absorption increased by 41.2%–57.8%.
(3) The hardness of modified CGA and ITZ increased by 97.7%–158.6% and 27.9%–129.2% respectively due to the formation of
hard protective shell on the surface of aggregate. The ITZ structure between the modified CGA and the concrete matrix is dense
and the bonding performance is good, which corresponds to the high ITZ hardness and high mechanical properties of the
concrete.
(4) The cost of modified CGAC can save 30.4%–30.8%, and the carbon emission is only 73.3% of the traditional concrete of the
same strength grade. Modified CGAC is suitable for large-scale industrial applications, such as coal mine filling and roadway
support concrete to achieve zero emission of coal mining.

Compliance with ethics guidelines


All authors (Shaohui Zhang, Yan Wang, Mengyuan Cao, KaiFeng Zhang, Ditao Niu) declare that they have no conflict of interest or
financial conflicts to disclose.

CRediT authorship contribution statement


Shaohui Zhang: Methodology, Formal analysis, Investigation, Writing – original draft, Writing – review & editing. Mengyuan
Cao: Methodology, Investigation. KaiFeng Zhang: Validation. Jian Yuan: Investigation. Yan Wang: Conceptualization, Methodol­
ogy, Formal analysis, Investigation, Resources, Writing – original draft, Writing – review & editing, Supervision, Funding acquisition.

Declaration of competing interest


The authors declare that they have no known competing financial interests or personal relationships that could have appeared to
influence the work reported in this paper.

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S. Zhang et al. Journal of Building Engineering 72 (2023) 106649

Data availability

Data will be made available on request.

Acknowledgments
The funding support was provided by the National Natural Science Fund for Excellent Young Scholars (52222806), National
Natural Science Foundation of China (52078414), Key Project of Scientific Research Program of Shaanxi Provincial Education
Department (20JY037), Shaanxi Province Science Fund for Distinguished Young youths (2022JC-20), Key Project of Innovation Fund
for Doctoral Students in Xi’’an University of Architecture and Technology (2021XYBPY004).

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