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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.
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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.
Table 1
The chemical composition of materials.
Materials SiO2 Al2O3 CaO Fe2O3 K2O TiO2 NaO2 MgO SO3 Loss
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Table 2
The physical properties of OPC.
water requirement of normal consistency/% Fineness/% Setting time/min Flexural strength/MPa Compressive strength/MPa
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.
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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.
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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.
Fig. 9. Apparent density (a) and bulk density (b) of modified CGA.
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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
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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.
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].
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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.
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].
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Table 5
Statistical results of peak stress, peak strain, and limit strain under 100% and 60% substitution rates of modified CGA concrete.
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).
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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
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.
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Data availability
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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