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Performance Evaluation of Recycled Aggregate Concrete Incorporating Limestone Calcined Clay Cement (LC3)
Performance Evaluation of Recycled Aggregate Concrete Incorporating Limestone Calcined Clay Cement (LC3)
A R T I C L E I N F O A B S T R A C T
Handling Editor: Zhen Leng Recycled aggregate concrete (RAC) incorporating limestone calcined clay cement (LC3) holds promise as a so
lution to the depletion of natural resources for construction materials and is a way to mitigate the environmental
Keywords: impacts of energy-intensive cement production. The ternary binder system demonstrates an overwhelming in
Recycled aggregate concrete fluence on the phase assemblage of RAC matrix, and the kinetics of hydration reaction are altered from the early
Limestone calcined clay cement
formation stage. The pore structure is significantly refined, and the porosity is reduced. The ameliorated
Strength
microstructure contributes to the significant improvement of the chloride penetration resistance of RAC without
Chloride resistance
Electrical resistivity noticeably compromising its mechanical strength. For RAC incorporating 50% LC3, the reduction ratio of the
Pore structure chloride rapid migration coefficient could reach 94% while the strength loss ratio is only 12% at 300 days
compared to the reference group. The electrical resistance of RAC using LC3 is also remarkably improved because
of the formation of a denser matrix as well as the reduction of available OH− in the pore solution of LC3 blends.
According to a life cycle assessment analysis, the environmental impact of RAC is significantly reduced with the
maximum reduction ratio being 42% due to the incorporation of LC3 because cement is the largest contributor to
both carbon emissions and energy consumption. The combination of recycled aggregate and LC3 is a promising
approach to improving the overall performance of RAC and mitigating the environmental impacts for concrete
production.
1. Introduction microcracks pre-exist in RCA (Poon et al., 2004); and old and new
interfacial transition zones (ITZ) are present in RAC (Li et al., 2016;
Reusing waste concrete is an effective way to promote a sustainable Liang et al., 2022; Xiao et al., 2013a). RCA with complicated micro
construction industry. The application of recycled aggregate concrete structures usually exhibits high porosity, high water absorption, and low
(RAC) not only alleviates the burden placed on natural resources for particle strength (Bosque et al., 2017; Li et al., 2012; Zhao et al., 2020).
construction materials, but also mitigates the tremendous environ Consequently, the overall performance of RAC is generally inferior to
mental pressure of construction and demolition (C&D) waste disposal. that of normal concrete (Guo et al., 2018, Tang et al., 2021; Meng et al.,
Substantial studies concerning the workability, mechanical strength, 2020).
and durability of RAC have been carried out (Adessina et al., 2019; In order to improve the interfacial properties and the performance of
Kurda et al., 2018; Liang et al., 2015; Mistri et al., 2020; Santos et al., RAC, many researchers have suggested incorporating supplementary
2017; Wang et al., 2021; Ying et al., 2017), and many achievements cementitious materials (SCMs) such as fly ash, ground granulated blast
have been made (Ding and Xiao, 2014; Marinkovic et al., 2017; furnace slag (GGBFS), metakaolin, and silica fume in RAC (Bravo et al.,
Velay-Lizancos et al., 2018; Xiao et al., 2012; Ying and Xiao, 2013; Ying 2015; Kim et al., 2013; Kou and Poon, 2013; Sim and Park, 2011). The
et al., 2020). Nevertheless, recycled coarse aggregate (RCA) obtained by addition of SCMs generally promotes the secondary hydration between
crushing and grinding waste concrete exhibits inherent defects. A SCMs and Ca(OH)2, with the newly formed C–S–H gels filling the pores
certain amount of old adhered mortar is left on the surface of conven and microcracks present in RAC (Kou et al., 2008; Limbachiya et al.,
tional aggregate (Otsuki et al., 2003; Xu et al., 2021); crushing caused 2012; Somna et al., 2012; Sunayana and Barai, 2018). Others have
* Corresponding author. Guangdong Provincial Key Laboratory of Durability for Marine Civil Engineering, Shenzhen University, Shenzhen, 518060, China.
E-mail address: ywzhou@szu.edu.cn (Y. Zhou).
https://doi.org/10.1016/j.jclepro.2022.132820
Received 7 December 2021; Received in revised form 18 May 2022; Accepted 19 June 2022
Available online 1 July 2022
0959-6526/© 2022 Elsevier Ltd. All rights reserved.
M. Guo et al. Journal of Cleaner Production 366 (2022) 132820
shown that the performance of RAC can be ameliorated, especially from performance than the reference Portland cement concrete by compre
a durability point of view (Guo et al., 2018). Sunayana and Barai (2017) hensively considering the trade-off between the mechanical properties,
reported that the elasticity modulus and mechanical strength of RAC environmental impacts, and economic potential.
using fly ash were comparable to those of natural aggregate concrete by Although substantial progress has been made concerning the prop
applying the particle packing method. The addition of fly ash contrib erties of LC3 blends, the ways this ternary binder system improves the
utes to the reduction of both the water absorption ratio and the electrical performance of RAC has not yet been studied, to the best knowledge of
resistivity of RAC (Kurda et al., 2019). The impermeability of RAC was the authors. As an environmentally friendly SCM, LC3 promises to not
remarkably improved by incorporating ultra-fine silica fume and met only increase the greenness of RAC but also ameliorate the microstruc
akaolin (Cakir, 2014). According to Abbas et al. (2009), the RAC resis tural properties of RAC. This work aims to provide a preliminary
tance to chloride ingress was improved by the addition of fly ash and investigation concerning the influence of LC3 on the properties of RAC.
GGBFS as a partial replacement for ordinary Portland cement (OPC). Specifically, the influence of the replacement of OPC by LC3 on the
Xiao et al. (2013b) concluded that the resistance to penetrability of properties of concrete using 100% RCA was studied. The mechanical
chloride ions in RAC with mineral admixtures can meet the required strength and the resistance to chloride ingress were investigated first.
engineering codes. The RAC mixes containing 50% GGBFS gave the best Then, the qualitative and quantitative analysis of the hydration phases
performance with respect to strength, permeability coefficient, and of the RAC matrix as well as the pore size distribution were carried out.
resistance to chloride ingress (Berndt, 2009). Kou et al. (2011) pointed To further evaluate the corrosion risk of reinforcement in RAC con
out that using metakaolin and silica fume demonstrated beneficial ef taining LC3, the electrical resistance of RAC was investigated and an
fects on both the short and long-term properties of the concrete, whereas equivalent circuit model was proposed. Finally, the potential environ
fly ash and GGBFS merely contributed to the long-term performance. mental impact was evaluated by conducting a life cycle assessment
The improvements seen on the performance of RAC with mineral ad analysis of RAC incorporating LC3.
mixtures is higher compared to the case of natural aggregate concrete.
Fathifazl et al. (2009) demonstrated that, by using SCMs, the cement 2. Experiment program
content of RAC can be reduced without adversely affecting its long-term
properties. 2.1. Materials and mixture design
Despite the advantageous effects of common SCMs mainly including
fly ash and GGBFS, the reduced consumption of coal due to its increasing In this study the RCA was obtained by crushing unknown waste
environmental impacts limits the supply of fly ash, and the amount of concrete collected from a local C&D waste site in Shenzhen, China. After
available GGBFS is less than 10% of the produced cement worldwide screening and cleaning, the particle size range was kept at 5–20 mm. The
(Scrivener et al., 2018). To address the inadequacy of traditional SCM, crushing index of RCA was 18.48%, and the water absorption ratio was
limestone calcined clay cement (LC3) appears to be an excellent alter 5.89%. OPC 52.5R was used in this work. Calcined clay and limestone
native (Chen et al., 2020; Lin et al., 2021; Maraghechi et al., 2018; Shi powder at the mixing ratio of 2:1, as suggested by Scrivener et al.
et al., 2019). Both kaolinite clay and limestone are abundant worldwide, (2018), were used to replace OPC, and three replacement ratios
which ensures an adequate supply (Krishnan and Bishnoi, 2020; Sharma including 0, 35%, and 50% were investigated. The used calcined clay,
et al., 2021). The production of both materials consumes low amounts of made from kaolin tailings in Maoming, south China, is locally abundant.
energy, and the resulting CO2 emission is largely reduced compared to Its mineralogical composition, determined by XRD-Rietveld method, is
conventional cement clinkers (Scrivener et al., 2018). The past decades presented in Table 1. Gypsum was also added into the mixture to adjust
have witnessed substantial studies concerning the hydration features, the reaction process of aluminates at early age. Fig. 1 shows the particle
mechanical strength, and durability of LC3-based cementitious materials size distribution curves of the binders that were used. The chemical
being conducted (Krishnan and Bishnoi, 2020; Berriel et al., 2016). compositions are summarized in Table 2.
According to Muzenda et al. (2020), calcined clay contributes to an in The mixture proportions of the studied RACs are shown in Table 3.
crease of static and dynamic yield stress, initial thixotropic index, and The water-to-cement (w/c) ratio was set to be 0.4 for all the mixtures.
plastic viscosity, while limestone has an opposite effect. Avet et al. Quartz-based river sand was used and its water absorption ratio is 1.2%.
(2019) found that significant incorporation of aluminum is observed for Considering the relatively high water absorption ratio of RCA, supple
LC3-50 mixtures compared to the control OPC. Avet and Scrivener mentary water was added to compensate for the water absorbed by RCA.
(2018) reported that the refinement of pore connectivity is significant in Polycarboxylate-based high-range water reducer (HRWR) was used to
LC3 paste. The decrease of pore size leads to the increase of the super adjust the flowability of recycled concretes incorporating LC3. The
saturation level, which is necessary for the further growth of hydration following mixing procedure was applied to achieve good dispersion of
products. To achieve the maximum strength, the proportion of calcined the mixture. First, RCA and sand were put into the mixer and dry mixed
clay to limestone could be optimized by considering the amount of for about 2 min. Then, the cementitious binders including OPC, calcined
soluble and reactive alumina in calcined clay (Ferreiro et al., 2017). clay, limestone powder, and gypsum were added and the mixing process
Antoni et al. (2012) demonstrated that, in LC3 blends, the content of lasted for 3 min. Finally, the water containing HRWR was gradually
gypsum dominates the rapid reaction process of aluminates and plays an poured into the mixer and mixed for about 3 min. The fresh slurry was
important role in determining the early-age strength. Moreover, the put into the molds and cured in room environment for 24 h. Moreover, in
kaolinite content of clay considerably affects the rheological properties order to evaluate the influence of LC3 on the phase composition of
as well as the strength development of LC3 paste (Karen et al., 2019). concrete, cement pastes corresponding to the three types of RAC were
Avet et al. (2018) found that an increase of metakaolin content in cast. The w/b ratio of the three types of paste all being 0.4 was the same
high-grade calcined clays becomes less important for determining the to that of concrete. After demolding, the specimens were placed in a
content of reacted metakaolin. Dhandapani and Santhanam (2017) re standard curing room at 23 ± 3 ◦ C and 95% relative humidity until
ported that the permeability of LC3 blends is much lower than that of the reaching the specified age of testing.
OPC and fly ash binder systems. The substitution ratio of cement clinker
by LC3 could reach 50% without compromising the mechanical strength
(Scrivener et al., 2018). The studies of Dhandapani et al. (2018) indicate Table 1
the superiority of LC3 binder over OPC and fly ash based binder in Mineralogical composition of calcined clay.
producing durable concrete, especially in chloride environment. Yu Composition Quartz Illite Glass
et al. (2021) further demonstrated that concrete made with
Calcined clay 13.27% 38.13% 48.53%
ultrahigh-volume limestone-calcined clay shows higher overall
2
M. Guo et al. Journal of Cleaner Production 366 (2022) 132820
limewater and were then used to measure the chloride rapid migration
coefficient (DRCM). A specific constant direct voltage was applied and the
duration of the RCM test depended on the measured initial current. After
the test, a AgNO3 solution was sprayed on the split cylinders to deter
mine the chloride penetration depth (Xd). The observed white color area
that represents the chloride penetration zone is demonstrated in Fig. 2.
In addition, a mercury intrusion porosimeter (MIP) was employed to
characterize the micropore structure of the RAC matrix at 28 days. By
removing coarse aggregate, the mortar was used for testing. To termi
nate the hydration process of the sample, the selected small particles
were put into absolute ethyl alcohol for at least 3 days and then vacuum
dried for 24 h at 60 ◦ C. The porosity and the pore size distribution were
determined by applying pressures ranging from 0 to 210 MPa. X-ray
diffraction (XRD) analysis was conducted to investigate the hydrated
phase composition of RAC matrix owing to the addition of LC3, espe
cially the content variation of Ca(OH)2 with curing age. Dried samples
were ground into fine powders and were then used for testing. A Cu Kα
radiation (λ = 1.54 Å) at 40 kV and 40 mA with 2θ value ranging from 5◦
to 65◦ was used for the scanning at a speed of 0.02◦ /step and 0.04 s per
step angle. Based on the obtained XRD patterns, the matrix-flushing
Fig. 1. Grading curves of cementitious binders. method was used to carry out the quantitative component analysis
(Chung, 1974), and the synthetic corundum was used as the flushing
agent. In addition, thermogravimetric analysis (TGA) was conducted to
Table 2
evaluate the pozzolanic reaction degree resulting from the use of
Chemical composition of cementitious binders.
calcined clay. The dried fine powders were heated up from 30 ◦ C to
Property Cement Calcined clay Limestone powder Gypsum 800 ◦ C in an N2 atmosphere at a rate of 10 ◦ C/min. The weight loss was
MgO (%) 1.78 0.31 0.77 3.39 recorded for further analysis. A scanning electron microscopy-energy
Na2O (%) 0.28 – – – dispersive spectrometer (SEM-EDS) point analysis was conducted to
Al2O3 (%) 3.51 39.41 0.13 5.83
identify the chemical composition of hydration phases. Samples were
SiO2 (%) 15.41 53.73 0.31 14.05
P2O5 (%) 0.07 0.04 – 0.05
impregnated by epoxy resin and were grinded by 400, 800, 1200 grit SiC
SO3 (%) 4.21 0.09 – 35.87 papers, respectively, for about 1 min. Then, the samples were polished,
K2O (%) 0.10 4.23 0.04 1.40 respectively, with 3, 1 and 0.25 μm diamond suspension. The duration
CaO (%) 69.86 0.10 98.72 37.05 for each grade was about 1 min. Before testing, the samples were coated
Fe2O3 (%) 3.74 2.06 2.03
with a thin layer of carbon for achieving better conductivity. During the
–
SrO (%) 0.07 – 0.04 0.33
test, the accelerating voltage was set to be 15 kV with a working distance
of 10 mm.
2.2. Test methods Because the electrical resistivity of heterogeneous concrete reflects
the distribution and interconnectivity of pores and the interfaces be
To investigate the macro-mechanical properties of recycled concrete, tween the solid and liquid phases, it was used to explore the micro
the compression tests were carried out with 100 × 100 × 100 mm3 cubes structural characteristics of the cementitious material in regard to the
at 7, 28, and 300 days. A 2000 kN MTS machine was used for loading at a resistance to ionic ingress. In this work, electrical impedance spectros
rate of 0.2 MPa/s. To evaluate the influence of LC3 on RAC’s resistance copy (EIS) (PARSTAT4000+) with an AC frequency ranging from 1 Hz to
to aggressive agents, rapid chloride migration (RCM) tests were per 1 MHz was used to measure the electrical response of concrete speci
formed according to GB/T50082-2009. Ф100 × 50 mm2 cylinders were mens. The amplitude of the excitation signal was 10 mV. The single-
tested at 28 and 300 days. The specimens were vacuum saturated in frequency current was applied to the specimen through outer
Table 3
Mixture proportion of recycled concrete (kg/m3).
Mixture type RCA Sand Cement Calcined clay Limestone powder Gypsum Effective water Absorbed water HRWR
3
M. Guo et al. Journal of Cleaner Production 366 (2022) 132820
electrodes, and the amplitude and phase shift of the resulting voltage
were obtained, and the impedance at each frequency was calculated. For
each order with a magnitude, 10 points of data were collected, and the
impedance spectrum was thus acquired.
Fig. 3. Compressive strength of the three RAC mixture types. Fig. 5. Evaluation of DRCM for the three mixture types.
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M. Guo et al. Journal of Cleaner Production 366 (2022) 132820
3.3. Microstructural characteristics confirms that Ca(OH)2 is largely consumed by the pozzolanic reaction of
metakaolin as well as the formation of carboaluminates.
3.3.1. Hydrate phase assemblage
The replacement of OPC by LC3 shows no negligible effect on the 3.3.2. Pore structure analysis
hydrate phase assemblages of paste matrix based on the XRD pattern For each concrete type, the porosity of paste matrix is illustrated in
analysis, as shown in Fig. 6. The main formed phases in the LC3 binder Table 6. It is remarked that the replacement of OPC by LC3 reduces the
matrix include portlandite (CH), calcium carbonate (CaCO3), ettringite porosity of paste matrix and that the reduction ratio reaches 25% for
(AFt), and a siliceous AFm-type phase strätlingite. According to the LC3-50. Fig. 10 presents the pore volume fraction in each matrix type.
SEM-EDS point analysis (Fig. 7 and Fig. 8), a significant amount of The incorporation of LC3 contributes to the pore size refinement of paste
aluminum is incorporated in the hydrated phases of LC3 blends. The Al/ matrix. The volume of pores with diameter less than 20 nm is dramat
Ca ratio increases with the increasing of LC3 replacement ratio. Inner C- ically increased, while the volume of larger capillary pores is signifi
A-S-H instead of C–S–H is generated while outer C-A-S-H is intermixed cantly reduced owing to the addition of LC3. The threshold pore entry
with other hydrated phases such as CH and AFt. Because the aluminates radius of paste matrix containing LC3 is also decreased, which could
in both calcined clay and cement react with CaCO3 from limestone to remarkably reduce the pore connectivity of the microstructure and in
form mono- (Mc) and hemi-carboaluminates (Hc), the two additional crease the tortuosity of ion permeation route. In addition, the reactive
hydrate phases that make the microstructure of matrix denser are found aluminates in calcined clay facilitate the formation of AFm-type phases,
to coexist in LC3-35 and LC3-50 blends (Fig. 8). In addition, as the which contributes to the improvement of chloride binding capacity of
calcined clay also introduces quartz and illite, the phases of SiO2 and the LC3 blends (Weerdt et al., 2011; Shi et al., 2017). All of these phe
illite are also observed in the XRD patterns of LC3-based blends. nomena are a good explanation for the reduction of DRCM, as described
For OPC-based paste matrix, the AFt peaks that are observed at 7 and in section 3.2.
28 days disappear at 300 days, while, for LC3-based paste matrix, the
peaks always exist from the early hydration stage to the late stage. As
pointed out by Avet et al. (2018), the incorporation of limestone gives 3.4. Electrochemical properties
rise to the stabilization of ettringite, the content of which does not vary
greatly with the hydration stage. Besides, as the pozzolanic reaction of Fig. 11 shows the development of Nyquist curves of the three RAC
reactive silica and alumina introduced by calcined clay consumes a types. For RAC incorporating LC3, the characteristics of EIS spectra are
certain part of Ca(OH)2, and the formation of Mc and Hc phases also quite different from those of the reference group. To better interpret the
requires the presence of Ca(OH)2, the calcium hydroxide content is electromechanical behavior of LC3-based RAC, an equivalent circuit
significantly reduced because of the replacement of OPC by calcined model was proposed, as illustrated in Fig. 12. The bulk matrix along with
clay and limestone, as illustrated in Table 5. For the reference group, the the microcracks is considered as continuous media, the circuit model of
CH content rises with curing age owing to the progressive hydration which is described as (Rm1Cm1)Rm2Cm2 (Fan et al., 2018). The contin
process, while, for LC3 blends, the CH content reduces with the curing uous matrix acts as a resistor Rm1 and the interconnected pores provide a
age due to the remarkable consumption for pozzolanic reaction and capacitor effect Cm1; Rm2 represents the resistor effect of the whole
carboaluminates formation process. In contrast, the peaks of CaCO3 are conductive path; Cm2 represents the capacitor effect of the almost whole
enhanced in the LC3 groups mainly owing to the addition of limestone non-conductive path in RAC. The RCA in combination with ITZ is rep
powder. resented by a circuit model Cr2 (Rr1Cr1). The interphase between RAC
TGA analyses were also performed to further investigate the forma and matrix acts as a resistor Rr1 and RCA between continuous ITZs
tion of hydrated phases in the different binder systems. Four major provides a capacitor effect Cr1. Since it is difficult for the current to pass
endothermic peaks that correspond to the dehydration of C–S–H/C-A-S- through the RCA with excessively large particle size, Cr2 represents the
H/AFt, Hc/Mc, Ca(OH)2, and CaCO3 are observed, as illustrated in capacitor effect caused by the hindrance of large RCA. With this model,
Fig. 9. The contents of Hc/Mc phases are significantly increased owing the interface between the electrode and the specimen is represented by a
to the replacement of OPC by calcined clay and limestone, which co circuit model Celec-inter(Relec-interW) (Snyder et al., 2003), where W rep
incides with the above XRD results. A higher content of calcium car resents the Warburg diffusion element. Thus, the total resistance of
bonate is also observed in LC3 blends. Furthermore, the reduction of CH concrete would be:
content is significant owing to the incorporation of LC3, which further
Z = Zm + Zr + Ze (2)
1
Zm = 1
(3)
Rm2
+ Rm1 +1 1 + jωCm2
jωCm1
1
Zr = 1
(4)
Rr1 +jωC1
+ jωCr2
r1
1
Re + AW ω− 2 (1 − j)
Ze = ( 1 ) (5)
1 + jω Re + AW ω− 2 (1 − j) Ce
where Zm, Zr, and Ze refer to the impedance of continuous matrix, RAC
along with ITZ and the interface between electrode and specimen,
respectively; j is the imaginary number; ω is the angle frequency; AW
represents the Warburg constant.
Fig. 11 shows the fitting curves of the three RAC types predicted by
the proposed circuit model. It can be seen that the diameter of the semi-
circle of Nyquist curves rises with the increasing replacement ratio of
OPC by LC3. As mentioned in section 3.3.1, the calcined clay introduces
a remarkable amount of aluminum that leads to the formation of a
Fig. 6. XRD patterns for different pastes at 7, 28, and 300 days. distinctive C-A-S-H gel system compared to OPC-based binder. The new
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M. Guo et al. Journal of Cleaner Production 366 (2022) 132820
6
M. Guo et al. Journal of Cleaner Production 366 (2022) 132820
Fig. 8. Chemical composition of the inner product C-(A)-S-H of cement pastes at 28 days.
Table 5
Relative content of Ca(OH)2 calculated by matrix-flushing method.
Age (days) RAC-PC RAC-LC3-35 RAC-LC3-50
Table 6
Pore structural characteristics of paste matrix.
Specimen RAC-PC RAC-LC3-35 RAC-LC3-50
7
M. Guo et al. Journal of Cleaner Production 366 (2022) 132820
Fig. 12. Scheme representation of the microstructure of RAC and the corresponding equivalent circuit model.
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M. Guo et al. Journal of Cleaner Production 366 (2022) 132820
5. Conclusions
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M. Guo et al. Journal of Cleaner Production 366 (2022) 132820
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The authors would like to express their gratitude to Shaocong Chen Fathifazl, G., Abbas, A., Razaqpur, A.G., Lsgor, O.B., Fournier, B., Foo, S., 2009. New
mixture proportioning method for concrete made with coarse recycled concrete
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thank the Instrumental Analysis Center of Shenzhen University for the Ferreiro, S., Herfort, D., Damtoft, J.S., 2017. Effect of raw clay type, fineness, water-to-
cement ratio and fly ash addition on workability and strength performance of
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from the National Natural Science Foundation of China (NSFC) (Grants doi.org/10.1016/j.cemconres.2017.08.003.
No. 51908369 and 52178236), the Ministry of Science and Technology GB/T 50082-2009, 2009. Chinese Standards, Standard for Test Methods of Long-Term
Performance and Durability of Ordinary Concrete.
of China (Grant No. 2018YFE0125000), NSFC and Guangdong province Guo, H., Shi, C.J., Guan, X.M., Zhu, J.P., Ding, Y.H., Ling, T.C., Zhang, H.B., Wang, Y.L.,
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