Cement and Concrete Composites 139 (2023) 105042

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Cement and Concrete Composites

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

Investigation on the reactivity of recycled brick powder

Shujun Li a, b, Gaofeng Chen a, b, Yasong Zhao a, b, Zhenhai Xu a, b, Xu Luo a, b, Cheng Liu a, b,
Jianming Gao a, b, *
a
School of Materials Science and Engineering, Southeast University, Nanjing, 211189, China
b
Jiangsu Key Laboratory for Construction Materials, Nanjing, 211189, China

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

Keywords: Knowing the reactivity of recycled brick powder (RBP) is fundamental for its correct and efficient utilization. In
Recycled brick powder this work, the dissolution behavior of RBP in NaOH solution and the degree of reaction in cement matrix were
Dissolution kinetics studied to investigate the reactivity of RBP. The results revealed that the main active species of RBP, Si and Al,
Degree of reaction
showed obvious lasting dissolution with a significant non-steady state dissolution stage, indicating that the re­
Reaction rim
action proceeds slowly. The dissolution mechanism controlled by the phase boundary reaction, with activation
energies of 82.74 kJ/mol and 75.79 kJ/mol for Si and Al dissolution, respectively, further confirmed this finding.
The strength activity index, thermogravimetric analysis, selective dissolution, BSE-IA-Mapping and MAS NMR all
confirmed reactivity of RBP. Additionally, reaction rims were observed around RBP particles in cement paste.
The low Ca/Si and Ca/Al ratios and their significant increases in a direction from the particle boundary to the
paste demonstrate that the rim was a hybrid phase composed of the original RBP components and the reaction
products.

1. Introduction grinding power consumption of WCBs is very low, approximately

Using construction and demolition waste (CDW) to produce con­
struction materials has become an attractive way to reduce the amount
of CDW and the carbon footprint of the construction industry [1].
Recycling waste clay bricks (WCBs) has been a key component in this
field [2]. As early as the 1990s, the reuse of WCBs has received attention
due to its detectable pozzolanic activity [3–5]. Due to the increasing
number of WCBs, recycling has become more urgent. According to the
available statistics [6,7], the amount of WCBs has become enormous; in
China and India, WCBs account for more than 30% of CDW. How to
promote the reuse of WCBs reasonably and efficiently becomes
increasingly important.
At present, WCBs recycling is broadly divided into two aspects. One
is coarse and fine aggregates after screening and crushing [8], and the
other is to be further destroyed to produce supplementary cementing
materials (SCMs) [9]. The former is mainly used in low-strength and
light-weight concrete due to its high porosity and low strength [10,11],
while the latter is more widely used. When WCBs are prepared as SCMs,
or recycled brick powder (RBP), it has several advantages: (i) due to the
reduced particle size, the pozzolanic activity of the material is more fully
utilized, and its low-strength defects are further limited [12]; (ii) the
one-twentieth of that of cement clinker [13]; and (iii) there is a clear
need for RBP as access to traditional SCMs becomes unsustainable with
increasingly stringent carbon emission regulations [14].
In recent years, many researchers have conducted studies on the
feasibility of RBP, covering almost all the macroscopic properties of
RBP-containing mortar and concrete [15–17]. These findings show that
introduction of less than 25% of RBP has the capacity to enhance the
matrix resistance to chloride ions and sulfate attack and gains significant
mechanical properties at a later stage due to RBP’s pozzolanic activity,
which also accelerates the carbonization rate at a relatively high RBP
replacement [18], a common issue with pozzolanic SCMs. Overall, RBP
presents great potential for practical application based on its observable
behavior. However, the unsolved critical issues, such as reactivity and its
mechanism of RBP, still hinder the further understanding of its
application.
RBP is similar to calcined clay in raw materials but exhibits differ­
ential activities due to the calcination temperature. Calcined clays are
typically burned ranging from 500 to 900 ◦ C to produce more active
components, i.e., the amorphous form [19–22]. The most common
baking temperatures for clay bricks range between 850 and 1150 ◦ C, and
they are usually baked near or above 1000 ◦ C to obtain high-performing

* Corresponding author. School of Materials Science and Engineering, Southeast University, Nanjing, 211189, China.
E-mail address: Jmgao@seu.edu.cn (J. Gao).

https://doi.org/10.1016/j.cemconcomp.2023.105042
Received 2 November 2022; Received in revised form 9 March 2023; Accepted 19 March 2023
Available online 24 March 2023
0958-9465/© 2023 Elsevier Ltd. All rights reserved.
S. Li et al. Cement and Concrete Composites 139 (2023) 105042

products. Whereas, at baking temperatures near 1000 ◦ C, most clay Table 2

minerals undergo partial recrystallization, leading to a reduction in Chemical compositions of cement and RBP (wt.%).
amorphous content [23]. As a result, clay bricks exhibit lower activity Cement RBP
than calcined clay but still show a pozzolanic activity [4]. Currentlly,
SiO2 19.5 65.0
there has been numerous studies on the reactivity of RBP, but the ma­ Al2O3 4.5 19.3
jority of studies focused on determining RBP’s activity using the CaO 62.7 1.8
compressive strength index method and the Frattini testing method Fe2O3 3.0 6.5
[24], or the evaluation of RBP activity through the calcium hydroxide MgO 1.6 1.7
Na2O 0.1 1.2
(CH) content in blended cement paste [25], leading to a lack of quan­ K2O 0.8 2.6
titative and qualitative understanding of RBP reactivity. SO3 2.3 0.4
As is widely acknowledged, the reaction mechainisms of traditional Others 4.0 1.3
SCMs such as fly ash (FA), granulated blast furnace slag (GGBS), and LOI 1.5 1.6
silica fume (SF) have been well ascertained. This knowledge has pro­
vided technical and economic guidance for their utilization, successfully
promoting their practical application. However, systematic and in-depth
investigation on the RBP reaction mechanisms, and even the evaluation
of its reaction degree, are lacking, impeding the further development of
RBP as an SCM.
Therefore, this paper aims to investigate the reactivity and mecha­
nism of RBP, specifically focusing on RBP produced by WCBs with
baking temperatures exceeding 1000 ◦ C due to its wide distribution and
generation. The reactivity of SCMs generally refers to their chemical
activity, that is, participating in chemical reactions to form hydration
products and following the solubility-precipitation reaction mechanism
[26]. Thus, the RBP reactivity investigation was divided into two parts:
i) investigating the dissolution behavior of RBP in alkaline solutions
with a pH similar to that of pore solution in concrete; ii) quantifying the
reaction degree of RBP at different ages in hydrated cement, iii) estab­
lishing the RBP reaction mechanism base on above exploration. This will
provide a comprehensive and thorough understand the reactivity of
RBP.

2. Materials and methods

2.1. Materials Fig. 1. Particle size distribution and Blaine specific surface.

Portland cement (PC) P•I 42.5, provided by Fushun Cement Co., Ltd,
China was used in this study. Its physical properties and chemical
composition are presented in Tables 1 and 2, respectively. WCBs were
collected from a construction waste disposal site in Nanjing. These WCBs
were screened, crushed, sieved, and ground to produce RBP. The
chemical composition, mineral composition, and particle size distribu­
tion of RBP are shown in Table 1 and Figs. 1 and 2, respectively. The fine
aggregate used was the standard sand produced by Xaimen ISO Standard
Sand Co., Ltd, with a fineness modulus ranged between 2.3 and 3.0. Tap
water was used for preparing mortar and paste. The sodium hydroxide
used was an analytical reagent (>95 wt% pure) produced by Macklin
Biochemical Co., Ltd. Deionized water, produced by Aladdin Bio-Chem
Technology Co., Ltd, was used for the dissolution test.
During the baking of clay bricks, the minerals (e.g., kaolinite, illite,
and montmorillonite) were gradually sintered, and mullite crystallized
at above 1000 ◦ C. In this work, Mullite and Kyanite were detected in
WCBs after several tests, and a representative result of one sample is
shown in Fig. 2. Therefore, it can be confirmed that the baking tem­
perature of these clay bricks was higher than 970 ◦ C. In addition, the

Table 1
Physical properties of cement and RBP.
Specific surface areaa Density (g/ Flexural Compressive Fig. 2. X-ray diffraction pattern of RBP.
(m2/kg) cm3) strength strength
(MPa) (MPa)

3d 28d 3d 28d

Cement 344.2 3.11 5.5 8.7 28.4 46.1

RBP 427.1 2.72 - - - -
a
: Specific surface area was measured by the Blaine method.

2
S. Li et al. Cement and Concrete Composites 139 (2023) 105042

amorphous content was determined between 15 and 20% using a semi- continuously for 0.5 h. This is to avoid the impact of the test apparatus
quantitative method. probe (silica) on the test results and to dissolve possible precipitation.
Given that the dissolution of the active component in RBP in NaOH
2.2. Sample preparation solution follows the following reactions:
[ ]−
Al2 O3 + 3H2 O + 2OH− →2 Al(OH)4 (2)
2.2.1. Mortar samples
The moulding process for mortar specimens followed the standard [ ]−
SiO2 + H2 O + OH− → SiO(OH)3 (3)
GB/T 17617-2021 (equivalent to EU 196–2005). Each testing group
consisted of three specimens with dimensions of 40 × 40 × 160 mm3. [ ]2−
The mix proportion, specifing the quantity of materials employed in SiO2 + 2OH− → SiO2 (OH)2 (4)
moulding each group of mortar specimens, has been tabulated in The maximum degree of reaction of RBP in the NaOH solution under
Table 3. The maintenance procedure of the specimens was also followed the test conditions was calculated from Eq. (5):
the aforementioned standards.
61
MSi + 102 MAl
RRBP = 29 54
(5)
2.2.2. Paste samples 50
The moulding process of the paste samples complied with the stan­
dard GB/T 1346–2011, and the water-to-binder ratio was 0.5. The Where RRBP is the reaction fraction of RBP in solution (%); MSi is the
maintenance procedure for these sample was the same as that for the concentration of Si in the solution (ppm); MAl is the concentration of Al
mortar samples. Until the specified age, the central part of the samples in the solution (ppm).
was collected and prepared into blocks with a side length of less than 10
mm, which were then impregnated in anhydrous ethanol to stop the 2.4. RBP in cement paste
hydration process. The samples were dried in a vacuum oven at 60 ◦ C for
72 h before microscopic testing. To quantify the reactivity of RBP in cement paste, thermogravimetric
analysis (TGA), selective dissolution, magic angle spinning nuclear
2.2.3. Samples for backscattered electron images analysis magnetic resonance (MAS NMR), and BSE-IA were used.
The preparation of backscattered electron images analysis (BSE-IA)
samples is described below. The dried paste samples were the first cast in 2.4.1. TGA
molds with epoxy resin. After that, the molds containing the samples TGA was performed using a Simultaneous Thermogravimetry-
were placed in a vacuum chamber for 30 min to allow the epoxy resin to Differential Scanning Calorimetry instrument (STA 449 F5 Jupiter).
fully penetrate the pores of the samples to mitigate microstructure The method for semi-quantification of portlandite was adapted from the
damage during the polishing. After 24 h, the demolded hardened sam­ method proposed by Taehwan et al. [27]. The detailed calculation
ples were removed for sanding and polishing. Five types of sandpaper process is shown in Fig. 3, and the formula for calculating CH content is
(P400, P800, P1200, P2500, and P7000) were used for the sequential Eq (6):
sanding of the samples. The speed of the polishing machine was 1000 r/ ( )
min. The samples were polished with silk flannel containing 0.25 μm PCH =
WLCH 74.1 WLCC 74.1
× + × × 100% (6)
diamond suspension. The grinding and polishing times were determined W50 18 W50 44
by observing the sample surface with a crystallographic microscope.
Anhydrous ethanol was selected as a coolant in the grinding and pol­ Where PCH is the content of hydration products (CH) in the sample,
ishing process. WLCH is the weight difference corresponding to the CH peak determined
by the tangential method, WLCC is the weight difference corresponding
2.3. RBP in NaOH solution to the Calcium carbonate (CC) peak determined by the tangential
method, W50 is the mass of sample at 50 ◦ C.
RBP was dissolved in 0.1 mol/L NaOH solution (pH = 13), roughly
equivalent to the pore solution in concrete. A solid-liquid ratio of 1:200 2.4.2. Selective dissolution
was used to ensure adequate dissolution of RBP. Polypropylene conical The selective dissolution method was widely used to determine the
flasks with alkali resistance and deionized water were used to ensure the degree of reaction of SCMs due to their time-saving and convenience.
accuracy of the test results. 20 ◦ C, 60 ◦ C, and 80 ◦ C were selected to
investigate the effect of temperature on RBP dissolution. The release rate
of the ions (r in mol/m2/s) was denoted as Eq (1),
C×V
r= (1)
m×S×x×t

Where C is solubility of the (element in the solution (mol/L); m is mass of

the sample (g); S is initial specific surface area of the sample (m2/g); V is
Volume of the solution (L);x is atomic fraction of the element in RBP
(calculated from the chemical composition of RBP).
At each age (0.5, 1, 2, 4, and 8 h and 3, 7, 28, and 90 days), an in­
dividual testing sample (200 mL NaOH + 1 g RBP) was acidified using
HCl, the pH of the solution was adjusted between 4 and 5, and stirred

Table 3
Mixing proportions of mortar samples (g).
Sample codes W/B Cement RBP Water Sand

MC 0.5 450 225 1350

Fig. 3. Calculation example of CH in a cement paste (90-day cement paste
–
MB 0.5 315 135 225 1350
containing RBP).

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S. Li et al. Cement and Concrete Composites 139 (2023) 105042

The principle is that the hydration products and unhydrated cement

were chemically dissolved in preference, leaving unreacted SCMs [28].
However, many researchers found errors in the results obtained by se­
lective dissolution, mainly due to the insufficient dissolution of cement
clinker (alite) and CH in solvent [29]. To obtain reliable results, the
selective dissolution of paste samples containing RBP was carried out
according to the method proposed by Dong et al. [30], and the calcu­
lation formula was Eq. (7) [31].
Wur
− FC Fuc
DoRRBP = 1 − 1− Wn
× 100 (7)
FRBP Fur

Where
WL − Lc
wn = (8)
1 − Lc

m0 − m950
wL = (9)
m0

Lc = (1 − β)Lp + βLb (10)

Wur is the mass fraction of the undissolved residue in the blended cement
paste at each age, Wn is the non-evaporated water content in hardened
paste, FC is the mass fraction of cement in blende cement, Fuc is mass
fraction of undissolved cement residue, Fur is mass fraction of undis­
solved RBP residue, FRBP is the mass fraction of RBP in the blended
cement, Lc is LOI of unhydrated blended cement containing RBP, Lp is
LOI of cement, Lb is LOI of RBP, β is the mass fraction of RBP in blended
cement, wL is LOI of blended cement paste containing RBP, m0 is the
mass of the blended cement paste before calcination. m950 is the mass of
the blended cement paste after being fired at 950 ◦ C. Fig. 4. Extraction process for RBP particles.

2.4.3. MAS NMR

RBP after time t.
MAS NMR was used to investigate the degree of reaction of RBP in
cement pastes, and its corresponding mode was deconvolution trans­
3. Results and discussion
formed [32,33]. The resonance frequency and spin rate of the 29Si NMR
instrument (Bruker 400 M) were set to 79.48 MHz and 10 kHz, respec­
3.1. Dissolution of RBP in NaOH solution
tively. The pulse length and relaxation delay used were 4.97 μs and 6.5
μs, respectively. Deconvolution of the spectrums was performed in Peak
3.1.1. Species dissolved in RBP
Fit using a Gaussian model. Considering the inevitable peak drift in 29Si
The results of the dissolution of RBP in NaOH solutions at different
or 27Al spectra, each deconvolution calculation aimed at obtaining the
temperatures (20 ◦ C, 40 ◦ C, and 80 ◦ C) for 4 h are presented in Fig. 5.
best fit with an equal number of peaks (software calculations determined
The results showed that the dominant dissolved element species of RBP
peak locations).
observed in NaOH solutions at 20 ◦ C, 60 ◦ C, and 80 ◦ C were Si, Al, and
2.4.4. BSE-IA
BSE-IA allows the identification of individual phases in a blended
cement paste according to their brightness, which depends on their
average atomic number [34]. This method has been widely used to
quantitatively evaluate the degree of reaction of SCMs in recent years
[35]. However, the RBP particles in BSE images exhibited similar grey
values to those of the C-(A)-S-H gels, leading to unreliable statistics of
the degree of reaction of RBP. Here, a method for marking RBP particles
in BSE images, referring to the elemental labeling method proposed in
Ref. [36], was developed to calculate the degree of reaction of RBP and
is shown in Fig. 4. The 1000× magnification of BSE images were used for
the labeling of RBP particles, and each pixel in the image corresponds to
approximately 0.27 μm in the real No. 15 BSE images were used for the
results statistics, corresponding to 90 elemental images. Image J was
used for binarization and statistics of the output images, and the
calculation formula is shown in Eq. (11).
Afanhydrous RBP (t = 0) − Afanhydrous RBP (t)
RRBP = (11)
Afanhydrous RBP (t = 0)

Where RRBP is the area fraction of RBP (equivalent to the volume frac­
tion), Afanhydrous RBP (t = 0) is remaining area fraction of the initial Fig. 5. Results of RBP dissolution in NaOH solution at different temperatures
unreacted RBP, Afanhydrous RBP (t) is remaining area fraction of unreacted for 4 h.

4
S. Li et al.
Ca, followed by Fe, K, and Mg after 4 h of dissolution. It is important to
mention that the dissolution of Na was not discussed due to the use of a
NaOH solution. The dissolved Si and Al were primarily derived from the
dissolution of aluminosilicate glass in RBP, as confirmed by subsequent
MAS NMR tests. Additionally, the dissolution of Ca was also noteworthy.
When the dissolution temperature was 20 ◦ C, the dissolution amount of
Ca was greater than that of Al but slightly lower than that of Si. When the
temperature was further increased to 80 ◦ C, the amount of Ca dissolved
only slightly increased. This indicates that Ca in RBP had an extremely
high dissolution rate during the initial period, but it decreased rapidly.
The above phenomenon has been attributed to the presence of "weak"
sites in the polymerized network [37]. The non-bridging oxygen com­
bined with cations (e.g., Ca2+) in the form of ionic bonds was the weak
link in the dissolution process. This causes the eraly release of Ca into the
solution. As a result, an early rapid release of Ca was observed.
3.1.2. Effect of dissolution time
Section 3.1 indicates that the mian dissolved elemental species in
RBP were Si, Al, and Ca. The amount and rate of dissolution of these
elements are therefore investigated in this section. Fig. 6 illustrates the
release amounts of Si, Al, and Ca in the RBP NaOH solution at different
times. During the initial period (<1 h), the release amounts of Ca were
higher than those of Si and Al. The release amounts of Ca in the solution
were still higher than those of Al until 3 h but increased slowly in the
following time. Concerning Si and Al, their release amounts in solution
exhibited an obvious increasing trend with time. However, Si release
was significantly higher than Al release, which is similar to conventional
SCMs [38,39].
The release rates of Si, Al, and Ca in RBP NaOH solution were
calculated using equation (1), as shown in Fig. 7. During the entire
testing period, the release rate of Ca was the highest, followed by Al and
Si, indicating that the dissolution ratio of Ca in RBP relative to the
original Ca content was significantly higher than that of Si and Al, which
further verified the preferential destruction of Ca in the glass network.
The preferential release of Al compared to Si can be explained by the
electron density polarization in the network covalent bond. Si4+ has a
charge/radius ratio more than twice that of Al3+ (Al3+: 0.39 Å and Si4+:
0.26 Å), and thus the electron density polarization of neighboring oxy­
gen ions is stronger [40]. Therefore, the Al–O site in a Si–O–Al linkage is
more easily destroyed, leading to a preferential release of Al [41].
Notably, a valuable characteristic was observed in the dissolution of
RBP. It can be noticed that under the experimental conditions, the
release rate of Ca, Al, and Si decreased continuously throughout the
Fig. 6. Concentration of Si, Al, and Ca in RBP NaOH solution.
5
Cement and Concrete Composites 139 (2023) 105042
Fig. 7. Logarithm of the release rate of Si, Al, and Ca in RBP NaOH solution.
observation time. However, these release rates displayed a remarkable
phase variation, decreasing rapidly before 7 days, but the trend was no
longer significant for the rest of the period. Generally, the dissolution
stage with a rapid change of the release rate was called the " non-steady
state" dissolution stage, and the subsequent dissolution stage with a
relatively stable release rate was called the "steady state" dissolution
stage. Under similar experimental conditions, the duration of the non-
steady stage of Si and Al dissolution for GGBS and FA is very short,
generally ending within a few hours [42]. The longer duration of the
non-steady stage indicates a longer time required for the activity
development of RBP compared with GGBS and FA. This explains the
continuous and slow strength growth of the RBP-containing cementi­
tious material in the later stage from a dissolution perspective [43].
3.1.3. Effect of dissolution temperature
Figs. 8 and 9 show the concentration of Si and Al in RBP NaOH so­
lution at different temperatures. As expected, the elevated temperature
significantly increased the concentration of Si and Al. The concentration
of Si increased from approximately 1 mmol/L to 4 mmol/L, and the
concentration of Al increased from approximately 0.5 mmol/L to 2
mmol/L in 8 h when the temperature was raised from 20 ◦ C to 80 ◦ C.
Also, it is worth noting that higher temperatures resulted in higher
amounts of dissolved Si and Al. When the temperature was elevated
from 60 ◦ C to 80 ◦ C, the concentration of Si and Al increased signifi­
cantly, from approximately 4 mmol/L to 7.4 mmol/L and from 2.4
mmol/L to 3.44 mmol/L, respectively. This suggests that it is feasible to
increase RBP reactivity using high-temperature curing. Additionally, the
calculated results of Si and Al release rates show that the elevated
temperature significantly increased the Si and Al release rates and
greatly reduced the duration of the non-steady phase of Si and Al
dissolution. The dissolution of the glass in alkali solutions is governed by
the surface chemistry controlled by the surface product layer and liquid
film. Increasing temperature can increase the diffusion coefficient,
thereby promoting the release of Si and Al [44]. Furthermore, the in­
crease in temperature can also increase the activity of OH− and reduce
Al(OH)-4 adsorption, thereby increasing the dissolution of Si [45].
3.1.4. Dissolution kinetics
The dissolution of RBP in alkali solutions is a typically heterogeneous
non-catalytic solid-liquid reaction. Clarifying the dissolution behavior of
RBP facilitates the understanding of its reaction mechanism. The
shrinking core model (SCM) has been widely employed to investigate
the reaction behaviour of solid reactants in solution. It is described by
three mechanisms: (1) The dissolution behavior of particles is controlled
S. Li et al. Cement and Concrete Composites 139 (2023) 105042

Fig. 8. Concentration of Si and Al in RBP NaOH solution at different temperatures.

Fig. 9. Release rates of Si and Al in RBP NaOH solution at different temperatures.

by the diffusion of liquid film on the surface, which is expressed in Eq. chemical reaction rate constant; CAg is the concentration of A in the
(12); (2) The dissolution of particles is controlled by the chemical re­ filtrate; n is the order of reaction concerning A; De is diffusion coefficient
action on the surface of reactants, which is expressed by Eq. (13); (3) The through the product layer.
dissolution of particles is controlled by phase boundary reactions and Fig. 10 illustrates the fitting results of dissolved Si and Al in RBP
product layer diffusion, which was expressed by Eq. (14). NaOH solution at 20 ◦ C using an SCM, and the linear behavior was
employed to evaluate the fitting results. It can be found that compared
2bkc CAg
(12) with Eqs. (11) and (12), Eq. (13) shows the best fitting value of 0.982 for
2
1 − (1 − α)3 = kt k=
ρb R2
the experimental data of Si and Al dissolution from RBP in NaOH solu­
bkc CAg tion at 20 ◦ C. Similarly, the dissolution of Si and Al in RBP exhibits the
(13)
1
1 − (1 − α)3 = kt k=
ρb R same trend at 60 ◦ C and 80 ◦ C, as shown in Table 4. However, it should
be noted that this trend was no longer distinct with increasing temper­
2bkDe CAg atures. Therefore, it can be confirmed that the dissolution of Si and Al
(14)
2
1 − 3(1 − α)3 + 2(1 − α) = kt k= from RBP in NaOH solution was controlled by the phase boundary re­
ρb R2
actions and the product layer diffusion.
Where α is the fraction of B converted to a product in the solid particles To further understand the dissolution kinetics of Si and Al in RBP
at time t; ρb is the density of solid particles; r is the initial radius of solid NaOH solution, ln (k) versus 1/T was plotted based on Arrhenius Eq.
particles, b is moles of B consumed per mole of reacted A; kc is the (15), and the activation energy was calculated as shown in Fig. 10.

Fig. 10. Plots of 1-(1- α)2/3, 1-(1- α)1/3, and 1–3(1-α)2/3-2(1-α) versus time for the dissolved Si and Al in RBP NaOH solution.

6
S. Li et al. Cement and Concrete Composites 139 (2023) 105042

Table 4 SCMs replacement of cement (Rc ). The correlation between SAI and Rc is
Fitting results of dissolved Si and Al in RBP NaOH solutions at a different tem­ generally satisfied: SAI ≥ 100% − Rc at given ages (7 or 28 days).
perature from the SCM model. Furthermore, the development of the pozzolanic activity of SCMs is also
Element Temperature (◦ C) R2 considered in the individual criteria and thus supplemented with SAI ≥
Eq. (11) Eq. (12) Eq. (13)
100% − Rc + Δ, Δ > 0 at a longer age (90 days). The water-binder and
binder-sand ratios of mortar specimens are commonly approximately
Si 20 0.880 0.886 0.988
1:2 and 1:3, respectively.
60 0.911 0.913 0.993
80 0.962 0.979 0.981 Figs. 12 and 13 show the compressive strength of mortar specimens
Al 20 0.857 0.869 0.982 and SAI of RBP. The investigated RBP exhibited an acceptable SAI value
60 0.882 0.885 0.962 at 28 days, slightly greater than 70%. Notably, the SAI of the RBP
80 0.957 0.961 0.988 increased steadily with an increasing curing time, indicating the
development of RBP activity at later ages. This is supported by findings
in sect. 3.2 that the dissolution of active Si and Al in RBP exhibited a
(15)
Ea
k = Ae−
significantly longer non-steady stage and continuous low dissolution
RT

rates for a longer time. Therefore, RBP-contained mortars exhibited an

Where k is the kinetics/rate constant; A is the frequency factor; Ea is the
observable development of compressive strength. The SAI line graph
activation energy; R is the universal gas constant; T is the thermody­
reflects this trend more clearly. Overall, the investigated RBP showed
namic temperature.
promising activity: SAI exceeded 70% at 28 days and continued to grow
Fig. 11 shows that the activation energies Ea of Si and Al dissolved in
after that. In addition, the longer-term SAI was worth considering for
RBP NaOH solution (pH = 13) were 82.74 kJ/mol and 75.79 kJ/mol,
evaluating RBP activity.
respectively. According to the definition of Ea , Ea can reflect the ease of
dissolution of Si and Al in RBP. However, Ea is calculated in k, which is
3.2.2. CH content
different for the same material in solutions of different solutes and pH
Investigating the variations of CH content in the matrix is a common
[44]. It is difficult to compare Ea of different pozzolanic materials, but
method to study the reactivity of SCMs with pozzolanic activity [50]. In
some evaluation and discussion can still be conducted in light of relevant
the case of CH saturation, the silicate or aluminosilicate network formers
studies. In this study, the Ea of Si and Al during the dissolution process
were depolymerized and dissolved into the solution, and the depoly­
(75.79–82.74 kJ/mol) is higher than that of the common pozzolanic
merized silicates and aluminates entered the solution following Eqs. (16)
material reaction (approximately between 30 and 50 kJ/mol) [46–48],
and (17):
and similar to that of ferronickel slag (49.45–80.47 kJ/mol) [49]. The
[ ]−
reason for the slow reaction rate of RBP is understood from the ≡ Si − O − Si ≡ + 3OH− → SiO(OH)3 (16)
perspective of dissolution kinetics. The lower Ea of Al dissolution than
[ ]− [ ]− )
that of Si dissolution indicates that Al in RBP had a faster dissolution rate ≡ Si − O − Al ≡ + 7OH− → SiO(OH)3 + Al(OH)4 (17)
under alkaline conditions and also demonstrates that the solubility of Si
is highly dependent on temperature. When Ca2+ ions are in contact with these silicate and aluminate species,
C–S–H and calcium aluminate hydrate C4AH13 are formed following Eqs.
3.2. Reactivity of RBP in cement paste (18) and (19), while AFt and AFm are formed when sulfate ions are
present following Eqs (20) and (21) [51]：
3.2.1. Strength activity index [ ]−
Y SiO(OH)3 + XCa2+ + (Z − X − Y)H2 O + (2X − Y)OH− → CX − SY − HZ
The strength activity index (SAI) is one of the most fundamental
(18)
methods for evaluating the reactivity of SCMs and has been widely used
worldwide. There are national and regional standards for SAI, such as [ ]−
2 Al(OH)4 + 4Ca2+ + 6H2 O + 6OH− →C4 AH13 (19)
GB/T 1596–2017, BS-EN 450-1-2012, and ASTM C311-2013. In the
standards mentioned above, the SAI is established based on the rate of

Fig. 11. Arrhenius plots of dissolution of Si and Al from RBP in NaOH solution
(pH = 13). Fig. 12. Compressive strength of mortar specimens.

7
S. Li et al.
Fig. 13. SAI of RBP.
[ ]−
2 Al(OH)4 + 3SO2−4 + 6Ca2+ + 4OH− + 26H2 O + →C4 A
• 3CaSO4 •32H2 O
[ ]−
2 Al(OH)4 + 6Ca2+ + • 3CaO • Al2 O3
• 3CaSO4 •32H2 O + 10OH− → 3[3CaO • Al2 O3 • CaSO4 •12H2 O] + 5H2 O
Thus, the pozzolanic activity can be investigated according to the
variation of the CH content in the system. Fig. 14 presents the variation
of CH content in pastes containing RBP and QP at different ages. On the
first day, the CH content of cement paste mixed with RBP was signifi­
cantly lower than that of pure cement paste due to the dilution of cement
clinker. After curing for 3 days, the difference in CH content between the
paste containing RBP and pure cement was more obvious, and the CH
content increased slightly compared with that of the pure paste. The
difference in CH content between RBP-containing paste and pure cement
paste became more and more significant with age because the CH con­
tent of RBP-containing pastes gradually decreased after 28 days of
curing, indicating the occurrence of the pozzolanic reaction. This is
consistent with the findings in Sect. 3.1.2, verifying that the develop­
ment of the pozzolanic activity of RBP required a long time. From the
Fig. 14. CH content in blend paste and cement paste samples at different ages.
Cement and Concrete Composites 139 (2023) 105042
growth rate of CH content in RBP-blended paste, the pozzolanic reaction
between RBP and CH produced by cement hydration probably occurred
at an early age (after 3 days), but this reaction was weak because of the
low amorphous content in RBP and the inhomogeneous mineral phase
composition that prevented the dissolution of active ingredients. Until
the CH in the system gradually slowed down, the consumption of CH by
RBP was only detectable when the active components of RBP were
continuously dissolved.
3.2.3. Selective dissolution and BSE-IA-Mapping
Quantitative evaluation of the degree of reaction of RBP in cement
paste is essential to investigate its reactivity. In this section, selective
dissolution and BSE-IA-Mapping were employed to evaluate the degree
of reaction of RBP at different ages. In addition, the RBP dissolution data
from the previous section are also used for the discussion in this section.
Fig. 15 shows the degree of reaction of RBP determined using se­
lective dissolution, BSE-IA-Mapping, and RBP dissolution in 0.1 mol/L
NaOH.The three methods gave similar trends in the degree of reaction of
RBP that the reaction degree increases with time. As expected, these
methods provide slightly different results. The RBP reactivity of NaOH
leaching at the same age was the highest, reaching 12% at 90 days.
However, it should be added that the actual degree of reaction was
greater than this value since other dissolved elemental species, such as
Ca, Na, and K, were not included in the statistics. The reaction degree of
(20)
RBP determined using selective dissolution was slightly higher than that
of BSE-IA-Mapping. The 180-day degree of reaction of RBP determined
by the two methods was 15.1% and 13.2%, respectively.
A higher degree of reaction can be expected using the NaOH disso­
(21) lution. The alkalinity of the NaOH solution (pH = 13) used in the
experiment was close to that of the pore solution in concrete, but the pH
of the pore solution can reach 13.8 with the hydration process [52]. In
theory, the polymeric network of silicate and aluminate tetrahedra in
RBP will be attacked by higher amounts of OH− in a higher alkalinity
environment, accelerating the rate of hydrolysis and thus leading to a
higher degree of reaction. However, in the pore solution, the dissolution
of Si and Al in the polymeric network will be influenced by the solution
components. When Ca and Al in the solution reach a specific concen­
tration, they will be enriched on the surface of SCMs particles and form a
Ca-modified aluminate layer. This phenomenon has only been
confirmed in the dissolution experiment of synthetic glass [35]. Current
studies on inhibiting SCMs dissolution by Ca and Al seem to support the
reaction site adsorption theory [38], but the presence of Ca and Al un­
doubtedly hinders the dissolution of Si and Al in SCMs.
Fig. 15. Degree of reaction of RBP determined by different methods.
8
S. Li et al. Cement and Concrete Composites 139 (2023) 105042

The resulting higher degree of reaction using selective dissolution

compared with BSE-IA-Mapping is due to an inherent error. Even
considering the loss of cement residue and RBP during dissolution, mass
loss in manual operation was unavoidable, leading to an overestimation
of the degree of reaction of RBP. It is worth noting that the results
measured by these two methods varied slightly, with a maximum dif­
ference of less than 2%, which might be attributed to the relatively low
reactivity of RBP. Overall, although the three methods gave differing
degrees of reaction of RBP, valuable reactivity could be identified: the
degree of reaction of RBP in cement paste was not high but showed long-
lasting reactivity.

3.2.4. MAS NMR

To further investigate the RBP reactivity, MAS NMR was employed.
Fig. 16 presents the 29Si MAS NMR spectrum of initial RBP and RBP
residues at different ages and their deconvolution analysis results. The
initial RBP and RBP residues showed a broad and overlapping peak
between − 80 and − 125 ppm, indicating the inhomogeneous presenta­
tion of different Q4 structures. The peaks at − 87, − 91, − 94, − 101,
− 107, − 112, and − 117 were assigned to Q4 (mAl, m = 0–4). Glass
components and crystalline phases such as quartz and mullite contribute
to the formation of these sites [53,54].
Additionally, a clear downward trend at approximately − 100 ppm to
− 80 ppm was observed in the 29Si spectra of samples with age, indi­
cating an ongoing reaction for RBP in cement paste. This spectrum
segment corresponds to the peaks at the Q4 (3Al) and Q4 (4Al) sites. The
significant reduction in the intensity of these peaks with time suggests
that the presence of Al–O sites contributed to the reaction of RBP. This is
attributed to the fact that Al–O sites are more easily destroyed than the
Si–O sites in alkaline solutions, and thus more Al–O sites allow for a
higher degree of dissolution of the glassy structure. This observation is
consistent with the finding in Sect. 3.2 that Al in RBP is released more
rapidly than Si, demonstrating that the dissolution of RBP in the hard­
ening cement is similar to that in the simulated solution (NaOH) tested.
In addition, this finding that peaks in the Q4 (3Al) and Q4 (4Al) sites
show a dramatical reduction in intensity at 180 days more directly
confirms that the C-(A) -S-H gel is the main reaction product of RBP in
hardened cement.
More detailed results of the deconvolution calculations are shown in
Fig. 17. Three different trends are observed for alterations in the content
of different structures of Q4 with time. Q4 (0Al) exhibits a significant
increase in content with increasing age, while the content of Q4 (1Al)
Fig. 17. Deconvolution results of 29
Si MAS NMR spectra of RBP based on area
percentage (%).
and Q4 (2Al) alter slightly. Clearly, Q4 (3Al) and Q4 (4Al) show a sig­
nificant decrease with time. The significant decrease in the content of Q4
(3Al) and Q4 (4Al) undoubtedly indicates that Si in Q4 (3Al) and Q4 (4Al)
is more actively involved in the reaction of RBP in cement paste. In
contrast, the dramatic increase in the content of Q4 (0Al) shows the low
reactivity of Si in this site. Ref. [33] demonstrates that Si of Q4 (0Al) sites
in FAis almost non-reactive with less than 0.4%, and the findings of
Ref. [32] also support this conclusion. Based on this conclusion, Eq. (22)
is used to calculate the reactive Si in RBP in cement paste at different
ages, and the corresponding calculation results are shown in Fig. 16.
SiReacted = 1 −
Q4 (0Al)Initial
(22)
Q4 (0Al)T
Where SiReacted is the fraction of reacted Si in RBP (wt%); Q4 (0Al)Initial
is the fraction of Q4 (0Al) in the initial RBP from the convolution
calculation of the 29Si spectrum; Q4 (0Al)T is the fraction of Q4 (0Al) in
RBP in cement paste at the time of T from the convolution calculation of
the 29Si spectrum.
Fig. 18 shows that the amount of reactive Si from RBP in cement
paste calculated based on the 29Si spectrum has a similar increasing
trend to that in NaOH solution. The results of 29Si MSS NMR spectra and
dissolution experiments showed that the Si reactivity reached about
24% and 12% at 180 and 90 days, respectively, but the former showed a
slightly higher level at the same age. The dissolution of RBP in NaOH
solution (pH = 13) provides a nearly ideal condition for the dissolution

Fig. 18. Reacted Si in RBP subjected to cement paste and NaOH solution (pH
Fig. 16. NMR Spectra of RBP and RBP residues at different ages. = 13).

9
S. Li et al.
of reactive Si, so the level of reactive Si obtained under this condition
can be used as the approximate upper limit of RBP reactive Si in cement
paste. The level of reacted Si obtained from the deconvolution calcula­
tions of 29Si Mass NMR spectra is inevitably affected by some variables,
for example, the selection of site locations and used fitting function, and
the conditional qualification about the function. Moreover, the results
provided by this method are coupled with slightly significant errors.
However, it can be confirmed that RBP exhibited a continuous reaction
both in the NaOH solution and in the cement paste according to the
experimental results; the reactivity of RBP is further clarified.
Fig. 19 shows the 27Al MAS spectra of initial RBP and RBP resides at
different ages. It is generally accepted that the 27Al MAS NMR is more
suitable for qualitative evaluation than quantitative calculations owing
to the wide peak locations, asymmetrical natural and complicated
linking environments [55]. The deconvolution of Al spectra was,
therefore, not conducted in this study. Three distinct peaks were iden­
tified in the spectrum of initial RBP at approximately 2, 13 and 55 ppm.
According to available studies, peaks at 2 and 55 ppm can be confirmed
to be associated with octahedral and tetrahedral Al, respectively, but the
Al structure represented by the peak at 12 ppm is not well defined.
Typically, the octahedral and pentahedral Al is assigned to around
30–40 ppm and − 10 to 20 ppm, respectively. Thus, the peak at 13 ppm is
suspected to be tetrahedral Al with a differential structure. The RBP
residues exhibited a peak distribution similar to the initial RBP but
decreased peak intensity of octahedral Al with age. The reduced peak
intensity, confirmed by comparison with the intensity of tetrahedral Al
peak, indicates that the Al from the vitreous Al phase and the crystalline
mullite in RBP took part in the reaction in blend cement paste. This is
also consistent with the results obtained from 29Si spectrum that Q4(3Al)
and Q4(4Al) show a significantly decreased content with increasing age,
especially after 28 days, further revealing the reactivity of RBP.
3.2.5. Energy-dispersive spectroscopy (EDS)
The combination of BSE and EDS can provide detailed information
on the distribution of elements and thus provide an in-depth investiga­
tion of the reactivity of RBP. Regions of the cement pastes containing the
RBP particles were first observed in the BSE images to obtain detailed
information on the reaction of RBP. The greyscale (brightness) of phases
in BSE pictures correlates with their atomic number, and higher
brightness indicates a higher atomic number for the phase, providing a
preliminary evaluation of the phase composition and distribution.
Through numerous observations, it was found that “reaction rims”
appeared around the RBP particles at 28 days and became more distinct
with increasing time. Typical reaction rims are shown in Fig. 20 (marked
by green arrows). Similar reaction rims are frequently found in FA or
slag-blended cement [56,57]. Obviously, the reaction rims around RBP
particles were much less significant. This is attributed to the lower
reactivity of RBP than FA and GGBS, and this finding also more directly
confirms the existence of RBP activity.
To obtain more detailed information on the reaction rim around the
27
Fig. 19. Al NMR Spectra of RBP and RBP residues at different ages.
10
Cement and Concrete Composites 139 (2023) 105042
RBP particle, the 180-day reaction rims were further analyzed using
point element analysis, as shown in Fig. 21. A significant directional
trend of increase or decrease in the content of elements can be observed
in the reaction rim. The Si content shows a continuous decrease along
the RBP particle boundary to the paste, indicating that there may be a Si
release process. However, Ca and Al present the opposite distribution
characteristics to Si, demonstrating that the dissolution and reaction of
the active elements in the RBP particles are inhomogeneous. These
speculations are further verified by the variation in the distribution of
the Ca/Si ratio in this region: The change of Ca/Si ratio distribution in
this region further confirmed the above speculation: with the increase of
the Ca/Al ratio, the RBP particle boundary extended vertically outward,
but the value was very small (less than 0.3), which was much lower than
the known C–S–H gel interface, indicating that the reaction edge might
be a hybrid phase. It contains the original RBP particle component (i.e.,
quartz phase) and hydration products. In addition, another special zone
(Zone 2) was found, which showed clear signs of erosion and reaction.
Data from the point element analysis shows that the Ca/Si ratio in this
region was higher than that in phases from the RBP particle, supporting
the idea that the rim region was a hybrid phase.
In addition to particles rich in the quartz phase, another type of RBP
particle is more abundant, namely the silica-aluminum phase. Similar
regions were also found around such particles, as shown in Fig. 22.
Although not obvious in BSE images, the elemental distribution map
clearly shows the existence of the reaction rim. The reaction rims around
these two types of particles exhibit similar Ca/Si values and distribution,
but the region located around the silica-aluminum phase particles show
an extremely high Ca/Al ratio due to the higher Al content. Comparing
the Al contents of the different localities, these Al probably belong to or
are derived from silica-aluminum phase particles. Furthermore, it is
noteworthy that the Na content in this region shows a clear decreasing
extending particle interface in a vertical outward direction, suggesting
that silica-aluminum phase RBP particles abundant of Na (possibly
feldspar particles) can dissolve Na for reaction to produce possible
C–N–S–H gels.
The observed reaction rim can be understood as a modified layer
formed by an interface-coupled dissolution-reprecipitation reaction. The
free energy difference required to drive this reaction is provided by the
difference in solubility between the parent and product phases in the
solution. Both reactions occur at the particle interface; only a small
amount of material needs to be dissolved in the boundary layer at the
interface at any one time. Another important property supporting the
continuation of the reaction is the high porosity of silica, a common
feature of silica or "gel" layers, which enables mass transfer through the
corrosion zone and from the reaction interface at a wide range of pH
conditions [58,59]. Meanwhile, the porous nature of the RBP particle
itself further enhances this possibility. Therefore, since the original RBP
particle is not in equilibrium with the interface solution, the reaction can
proceed through the difference in solubility between the original RBP
particle and the reaction product, even if the surrounding solution is
S. Li et al. Cement and Concrete Composites 139 (2023) 105042

Fig. 20. Representative regions of cement pastes containing RBP particles at different ages.

Fig. 21. BSE image and results of elemental distribution analysis of the reaction rim at 180 days.

filled with the associated ions. However, as the thickness of the reaction
rim increases, the reaction is increasingly controlled by transport of
material through the pore of the reaction rim. As a result, the reaction
rims exhibit a differential Ca distribution. The difference in the distri­
bution of Si and Al is probably due to the formation of precipitation
(products) that reduce the concentration of Si and Al in the boundary
layer adjacent to its original particle constituents. To better understand
the formation of the reaction rim, a schematic representation of the
reaction is depicted in Fig. 23.
4. Conclusions
In this work, the reactivity of RBP, derived from WCBs with an
original baking temperature above 1000 ◦ C, was investigated in

11
S. Li et al. Cement and Concrete Composites 139 (2023) 105042

Fig. 22. BSE image and results of elemental distribution analysis of the reaction rim at 180 days.

• The primary reactive species in RBP, Si and Al, exhibited obvious

• SAI, TGA, selective dissolution, BSE-IA-Mapping, and MAS NMR all
Fig. 23. Schematic diagram of formation of the reaction rim.
combination with its dissolution kinetics in NaOH solutions and degree
of reaction in the cement matrix. The main findings are summarized
below.
lasting dissolution behavior with a significant “non-steady state”
dissolution stage, indicating that the RBP reaction proceeded slowly.
This finding was verified by the dissolution mechanism controlled by
the phase boundary reaction, with activation energies of 82.74 kJ/
mol and 75.79 kJ/mol for Si and Al dissolution, respectively.
Furthermore, an increase in temperature was found to accelerate the
dissolution of RBP substantially.
confirmed the reactivity of RBP. Regarding the SAI, it is worth
considering the complement of a 90-day observation indicator for a
more reliable assessment. Selective dissolution and BSE-IA-Mapping
provided a comparable evaluation of the degree of reaction for RBP
in cement pastes, which was approximately 15% at 180 days. NMR
tests identified reactive Si and Al in RBP primarily from the Q4
(3,4Al) and Al (IV) sites, respectively.

12
S. Li et al.
• Observations of reaction rims surrounding RBP particles in the
cement paste suggest that the reaction rim is a hybrid phase
composed of both original RBP components and newly-formed
products. The significant increase in Ca/Si, Ca/Al, and Ca/Na ra­
tios from the particle boundary towards the cement paste further
supports this finding.
The results in this work indicate that RBP derived from WCBs with an
original baking temperature above 1000 ◦ C has low reactivity and ex­
hibits a reaction mechanism that significantly differs from conventional
SCMs, such as FA and GGBS. However, RBP obtained from WCBs with an
original baking temperature below 1000 ◦ C is expected to exhibit
improved activity and a more intriguing reaction mechanism. Another
important aspect to note is the congruent or incongruent dissolution of
RBP, which can contribute to a deeper understanding of the reaction
mechanisms. Further investigation of these aspects is therefore war­
ranted. It is believed that the pursuit of these endeavors can yield a more
thorough understanding of the reaction mechanism of RBP, thereby
facilitating its diverse and tiered utilization, ultimately resulting in
improved utilization efficiency of RBP.
CRediT authorship contribution statement
Shujun Li: Software, Validation, Investigation, Resources, Data
curation, Writing - original draft, Writing - review & editing. Jianming
Gao: Formal analysis, Conceptualization, Writing - review & editing,
Funding acquisition, Project administration. Gaofeng Chen: Software,
Data Curation. Yasong Zhao: Investigation, Zhenhai Xu: Investigation.
Xu Luo: Supervision. Cheng Liu: Software.
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.
Data availability
Data will be made available on request.
Acknowledgments
The authors deeply appreciate the financial support provided by the
National Natural Science Foundation of China (No. 52130210) and the
Jiangsu Key Laboratory of Construction Materials for technical support.
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