Construction and Building Materials 385 (2023) 131518

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Construction and Building Materials

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Using diatomite as a partial replacement of cement for improving the

performance of recycled aggregate concrete (RAC)-Effects and mechanism
Hongru Zhang a, *, Bingjian He a, Baojun Zhao b, Paulo JM Monteiro c
a
College of Civil Engineering, Fuzhou University, Fuzhou 350108, Fujian, PR China
b
China State Construction Hailong Technology Co. LTD., Shenzhen 518110, Guangdong, PR China
c
Department of Civil and Environmental Engineering, University of California, Berkeley, CA 94720, USA

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

Keywords: This work proposes that diatomite can be used to improve the performance of recycled aggregate concrete (RAC).
Recycled aggregate concrete A calcined diatomite sample with an amorphous silica content over 90% was added to the RAC mixture as a
Diatomite partial replacement of the ordinary Portland cement (OPC) at varying rates from 0 to 20 wt%. Test results show
Modification
that both the strength and impermeability of RAC can be obviously enhanced with the greatest enhancement
Hydration
Pore structure
observed at a replacement level of 15 wt% for which the 28-day compressive/splitting tensile strengths were
Interfacial transition zone (ITZ) improved by 29.2% and 33.9%, respectively, and the chloride diffusion coefficient was reduced by 86.27%. The
microscopic measurements confirmed the nucleation effects and the high pozzolanic reactivity of diatomite
which both contributed to the more complete hydration of cement in RAC. It was also found that the proportion
of large capillary pores in the new mortar was reduced by using diatomite, meanwhile the average porosity of the
new interfacial transition zone (ITZ) became smaller. This work suggests that the calcined diatomite used for
improving RAC performance should be no larger than 15 wt% of cement, as the scarcity of CH at a higher
replacement ratio would hamper the pozzolanic reactions, meanwhile the diluted cement clinkers would have a
negative effect on the pore structure of RAC.

1. Introduction
The past 5 to 6 decades have witnessed the rapid development of
China in many aspects, especially in the construction industry. The
accelerating urbanization and the long-lasting reconstruction of old
cities have brought prosperity to the regional economy, but they have
also led to serious environmental problems, among which the excessive
discharge of construction and demolition waste (C&DW) is a critical one.
In China, the annual discharge of C&DW has been rising drastically since
the year 2015, and in the year 2019, the number has exceeded 1.85
billion tons [1]. In light of this, recycled aggregate concrete (RAC) which
helps dispose of C&DW in an environmentally friendly way and enables
the production of more sustainable concrete mixtures attracts increasing
attention. The most commonly used recycled aggregate (RA) for pre­
paring RAC is produced from waste concrete which accounts for about
1/3 of the total amount of C&DW [2].
It has been widely accepted that RAC prepared with RA coming from
waste concrete has inferior mechanical performance and durability
compared to normal concrete [3–7], especially at a higher replacement
ratio of natural aggregate (NA) with RA (e.g., higher than 30%) [8,9].
This has limited the wide application of RAC in structural use, which can
be seen from the strict limits on the use of RA and RAC in certain sce­
narios as required by the technical standards on recycled concrete
structures in many countries or regions like mainland China, Hong Kong,
Korea, Japan, and Netherlands [10–12]. For example, as required by the
Chinese Standard JGJ/T 443–2018 [13], the amount of Class II and III
coarse RA (characterized by relatively lower density, larger water ab­
sorption/crushing index, and higher contents of fine powder/clay
clump/elongated &flaky particles/other impurities) is suggested not to
exceed 50% of the total mass of coarse aggregate in multi-story ­
buildings or high-rise buildings. The classifications of coarse RA can be
found in the national standard of China GB/T 25177–2010 [14]. In Hong
Kong, China, concrete with 100% recycled coarse aggregate can be used
in benches, stools, planter walls, concrete mass walls, and other minor
concrete structures where specifically permitted in the contract, ac­
cording to the specifications facilitating the use of recycled aggregates
by the Works Bureau Technical Circular 12/2002 [12]. In South Korea,
the coarse RA could be used to prepare concrete with target strength

* Corresponding author.
E-mail address: hrzh@fzu.edu.cn (H. Zhang).

https://doi.org/10.1016/j.conbuildmat.2023.131518
Received 2 November 2022; Received in revised form 17 April 2023; Accepted 20 April 2023
Available online 28 April 2023
0950-0618/© 2023 Elsevier Ltd. All rights reserved.
H. Zhang et al.
between 21 and 27 MPa and the replacement rate should be no larger
than 30% [15]. In Japan, recycled aggregate was not allowed to be used
in high-strength concrete; for normal-strength concrete, only Type H
recycled coarse aggregate (the other two types were Type M and Type L
RA with lower apparent density, larger water absorption, inferior
abrasion resistance, and higher contents of fine powder and impurities)
could be used to partial replace the natural coarse aggregate but the
replacement rate should not exceed 5% as per JIS A 5308–2019 [16]. In
Europe, International Union of Laboratories and Experts in Construction
Materials, Systems and Structures (RILEM) specifies that the Type I
recycled aggregate originating primarily from masonry rubbles and
Type II primarily from concrete rubbles could be used to prepare con­
crete at the maximum allowable strength levels of C16/20 and C50/60,
respectively. Only Type III aggregate which consists of a blend of recy­
cled aggregates and natural aggregates with the latter accounts for no
less than 80 wt% could be used for preparing concrete at any target
strength [17].
Many modification techniques have been proposed to improve the
RAC performance, thereby breaking the limits for RAC’s application in
real projects, especially in structural use. Some of the modifying tech­
niques aim to remove or enhance the old mortar via thermal treatment
[18], microwave-assisted grinding [19], CO2 curing [20], aggregate
surface treatment [21,22], or biological deposition [23], et al. However,
new problems arise as the elimination of old mortar is usually accom­
panied by large energy consumption or undesirable air/water/noise
pollution while the enhancement of old mortar requires operating yards
and extended time for the surface treating process. Because of this, the
performance of RAC should be improved by more easily handling and
more environmentally-friendly approaches. Some researchers proposed
to take the new RAC mix design methods like the scattering-filling
coarse aggregate (SFCA) process [24] or the equivalent mortar volume
(EMV) method [25–27] for improving the RAC performance while some
other researchers suggested that incorporating pozzolans should be
another easy-handling choice for enhancing the RAC performance. The
commonly employed pozzolans for the purpose of modifying the
strength and durability of RAC include slag, silica fume, fly ash, coal
bottom ash, metakaolin, rice husk ash, etc. [28–35]. It is now well
known that the amorphous components present in these pozzolans can
convert calcium hydroxide (CH) to calcium silicate hydrates (C-S-H) via
pozzolanic reactions thereby enhancing both the cement matrix and the
interfacial transition zone (ITZ) of RAC [36,37]. Some pozzolans (e.g.,
silica fume, rice husk ash, and nano silica) also present a seeding effect
that can facilitate the formation and growth of C-S-H, thereby contrib­
uting to the performance improvement of RAC. Using these pozzolans at
an appropriate dosage can improve the RAC compressive strength and
splitting tensile strength by 10% to 35%, and 12% to 45%, respectively,
as previously reported by other researchers [7,28–34,36,37].
In light of the significant advantages of using pozzolans in RAC’s
performance modification, this work proposes that the RAC properties
can also be enhanced by diatomite, a natural pozzolan. Diatomite is a
material of sedimentary and biogenic origin formed from the accumu­
lation of algae shells that were fossilized due to the silica deposit on the
diatom skeletons [38]. Diatomite was widely spread in many countries.
USGS (U.S. Geological Survey) reported a total of 2300 thousand metric
tons diatomite mined around the world in the year 2021 with huge re­
serves that cannot be estimated yet [39]. The United States accounted
for an estimated 36% of the global production; followed by Denmark
with 17%, Turkey with 9%, China with 6%, and Argentina, Mexico, and
Peru each with 4% [40]. Smaller quantities of diatomite were mined in
21 additional countries. The amorphous silica (opaline) content in
diatomite ranges from 25% to 100% [41], making it a natural pozzolan.
Due to the high open porosity (e.g., 50% to 70%) and the large specific
area and high-water absorption (as high as 1 kg/kg [36], diatomite has
been widely used in filtration, drilling mud thickener, chromatography,
etc. In cementitious materials, diatomite is usually suggested to be used
in high-performance concrete and ultra-high-performance concrete
2
Construction and Building Materials 385 (2023) 131518
[42–44], serving as a source of internal curing water and supplementary
cementitious materials (SCMs), or in fireproof cement, insulation ma­
terials, and as an absorbent in explosives manufacture because of its
excellent resistance to heat and chemical action [45].
Till now, using diatomite for the purpose of modifying the RAC
performance is rarely reported in published papers [46]. However, the
results as reported in a few studies dealing with the use of diatomite in
normal mortar or concrete are promising. For instance, Li et al. [47]
reported that a green mortar prepared with the intermix of fly ash and
diatomite can reach 60 to 70 MPa at an OPC replacement level of 40% to
60%; the diatomite can be used to replace up to 30% OPC without
jeopardizing the mechanical properties of mortar. In another work of Li
et al. [48], mortars with the diatomite dosage of 10 to 30 wt% were
found to have higher compressive strengths than those prepared with
the white Portland cement at 7, 28, and 90 days. Regarding the use of
diatomite in concrete, Tagnit-Hamou et al. [43] used diatomite as the
partial replacement of OPC to prepare concrete, and they found that the
concrete with 30% OPC replaced by diatomite develops the highest
compressive strength of 51 MPa which represents an increase of about
1.3 times that of the reference concrete. Moreover, the chloride ion
permeability index was reduced by 6 and 2.5 times with a replacement
level of 15% and 30%, respectively. HASAN et al. [42] reported that the
flexural strength of the high-strength concrete beams can be enhanced
by 4.46% with the addition of diatomite micro particles (5 wt% of the
binder amount) as a mineral additive. A research work carried out by
Wei et al. showed that the calcined diatomite of 2% added to RAC can
decrease the relative penetration coefficient by 59% [49]. The high
pozzolanic reactivity due to the relatively large content of amorphous
silica can help facilitate the cement hydration in RAC [50,51]; further­
more, the diatomite after grinding can also induce filling effect by the
action of the finer grains to improve the pore structure of the cement
matrix [52]. This explains why the addition of diatomite can guarantee
the high strength and low permeability of mortar/concrete. However,
currently the use of diatomite at a high dosage in concrete as the sup­
plementary cementitious material (SCM) is basically hampered. This is
due to not only the particle shape of the diatomite skeletons (i.e., usually
thin and being either radial symmetry or line symmetry) which has an
unfavorable effect on the paste consistency, but also the large water
absorption causing an increase in the water demand of concrete
[43,53,54]. Therefore, if diatomite is to be used for modifying the RAC
performance, the amount of diatomite needs to be adjusted and the
optimal dosage should be determined by experimental investigation.
The present paper aims to modify the RAC performance by using
diatomite as the SCM to partially replace cement during the RAC prep­
aration. The purposes are two-fold. First, such a trial has been rarely
referred in published articles as mentioned above, while this work can
verify the feasibility of this approach in improving the RAC perfor­
mance. The optimal replacement level (if there is a one) will also be
determined via experimental investigation. The second purpose is to
better understand the modification effects of diatomite on the RAC
performance in terms of the changes in the hydration process, the pore
structure, as well as the microhardness of the mortar phase and the
interfacial transition zone (ITZ) phase compared to the case without
diatomite. Using diatomite as SCM for preparing RAC mixtures should
be a new approach for improving the RAC performance which could
thereby promote the wider application of RAC in structural use. The use
of diatomite in concrete can also partially offset the local deficiency in
traditional SCMs like fly ash, slag, and silica fume as reported in many
countries [48,55] given its abundant reserve and promising long-term
supply in China and other regions.
H. Zhang et al. Construction and Building Materials 385 (2023) 131518

2. Materials and methodology and 2.0, respectively.

2.1. Materials
2.2. Mix proportions and concrete casting
2.1.1. Cement and diatomite
A total of 5 groups of RAC were prepared by this work. Portland
The cementitious materials used in this study include the ordinary
cement was replaced by an equivalent weight of diatomite ranging be­
Portland cement (OPC) and calcined diatomite obtained from Jilin
tween 0 and 20%. The mixture proportions can be found in Table 4. The
Province, China. The OPC (Lianshi 42.5) is equivalent to CEM I 42.5 N
number contained in the label for the five concrete groups is consistent
according to EN197-1 [56]; the representative physical properties of
with the replacement rates of OPC by diatomite, i.e., 5%, 10%, 15% and
OPC are listed in Tables 1. The calcined diatomite employed by this
20%, respectively. Target compressive strength of the prepared RAC was
present work was more commonly used as a filter aid in the food pro­
30 MPa. In all concrete mixtures, a fixed water-to-binder ratio of 0.50
duction industry. The chemical compositions of OPC and diatomite are
was selected; the binder herein refers to the blend of OPC and diatomite
listed in Table 2a. Table 2b is the mineralogical compositions of OPC
as the SCM. Considering the higher water requirements of both RA with
which was provided by the supplier. The specific surface area of diato­
the presence of the adhering porous old mortar and the diatomite
mite was 59, 200 m2/kg and the density was 450 kg/m3.
skeletons with a large open porosity, the RA was pre-wetted to be surface
According to Table 2a, the calcined diatomite used in this work
saturated dry (SSD) before the concrete casting, meanwhile a poly­
showed higher silica content and lower calcium content compared to
carboxylate superplasticizer (solid content of 20%) was added to the
OPC. The diatomite was almost pure with a SiO2 content up to 92.13%.
concrete mixtures, to ensure a good workability of the fresh concrete.
According to ASTM C618-19 [57], it can be classified as Class N natural
The superplasticizer employed by this work also contained defoaming
pozzolan.
agent which accounted for about 0.05 wt% of the solid content. Note
The skeletons of diatoms contained in the diatomite samples present
that the superplasticizer dosage for the five concrete groups was
varying shapes but the same porous characteristic, as shown by the SEM
adjusted by a series of trials in order to achieve comparable fluidity
pictures (Fig. 1). The size distribution of the diatomite tested by the laser
among the five concrete groups. As shown by Table 4, the super­
granulometry is shown in Fig. 2 compared to OPC. The diatomite and
plasticizer dosage increased with the replacement rate of OPC by diat­
OPC particle size ranged from 2 to 21 μm and 2 to 30 μm, respectively;
omite; the slump slightly fluctuated between 190 and 200 mm.
the average particle size was 6.16 and 9.33 μm, respectively. The diat­
To prepare the concrete mixture, the diatomite was first mixed with
omite sample’s great fineness is consistent with its original function as a
OPC for 60 s to allow the good dispersion of diatomite in OPC. Next, the
filter aid. The partial replacement of OPC by the finer diatomite particles
deionized water mixed with the superplasticizer was poured by half into
may impact the workability, mechanical properties, and durability of
the dry mixture, and they were stirred for another 60 s. Afterward, RA,
the prepared RAC, which will be discussed in the following sections. The
sand, and the remained half of the water suspension of the super­
XRD pattern of the diatomite samples (Fig. 3) shows a broad peak
plasticizer were added. After a 2-minute mixing, the mixture was poured
(hump) between 20◦ and 26◦ 2θ, indicating the presence of a large
into molds. The prepared specimens were then moist cured in a curing
proportion of amorphous silica phase (opal-A). Quartz is also identified
chamber at a temperature of 20 ± 2 ◦ C and relative humidity above 95%
but in a very low concentration, according to Fig. 3.
for 28 days. Note that a total of five groups of blended pastes with the
diatomite dosage varying at the same range to that in the five groups of
2.1.2. Recycled coarse aggregate
RAC mixtures were also cast, to help understand the role of diatomite in
Recycled aggregates (RA) were purchased from a ready mix plant.
the hydration process of the blended binder. The mixture proportions of
The production of RA from waste concrete included two crushing pro­
the five groups of paste samples with varied replacement ratios of OPC
cesses, two grinding processes, one sieving process, and a final cleaning
by diatomite are shown in Table 5.
process. The parent concrete came from a 25-year-old apartment
building located in Tonglu, Zhejiang Province, China. The RA had a
particle size ranging between 4.75 and 31.5 mm. The representative 2.3. Test methods
physical properties of the RA, i.e., the apparent density, the water ab­
sorption, and the crushing value, were tested following the standard GB/ 2.3.1. Compressive and tensile splitting strengths
T 14685–2011[58], which were 2680 kg/m3, 2.32 wt%, and 14.6 wt%, The compressive and splitting tensile strengths of concrete were
respectively. The content of the old cement mortar adhering to the RA determined using a DYE-2000 compression machine with the highest
particles was measured by a thermal treating procedure proposed by loading capacity of 2, 000 kN. The compressive and splitting tensile
Reference [59]; the old mortar accounted for about 13.2% of the RA by strengths were measured at the ages of 7, 14, and 28 days, as per the
mass. The grain size distribution of RA is illustrated in Fig. 4, which national Standard of China GB/T 50081–2002 [60].
complies with the Chinese National Standard GB/T 14685–2011. No
natural coarse aggregate was used. 2.3.2. Chloride permeability
The chloride permeability of RAC was evaluated by the diffusion
2.1.3. Fine aggregate coefficient of chloride, i.e., DRCM, measured by the rapid chloride
The fine aggregate used in this study was local river sand from Min migration (RCM) technique, following the instructions stated in the
River. The size distribution is shown in Table 3. The water absorption Chinese Standard GB/T 50082–2009 [61].
and the fineness modulus of the employed sand were tested to be 2.3%
2.3.3. Measurements on the microscale

Table 1 2.3.3.1. The hydration process and the hydration products. The hydration
Typical physical properties of OPC. process and the hydration products of the binary paste with OPC
Specific surface LOI Setting time(min) Bending Compressive replaced by diatomite at varying replacement rates were identified and
area (m2/kg) (%) strength strength analyzed by the scanning electron microscopy (SEM), the X-ray
(MPa) (MPa)
diffraction (XRD, X/Pert Pro MPD) technique, the thermogravimetric
Initial Final 3d 28 3d 28 d
set set d analysis (TGA), and the combination of these techniques in some cases.
The paste was cured in the saturated Ca(OH)2 solution till the target ages
363 1.04 135 180 5.9 8.1 27.2 44
for each measurement. Before testing, the hydration was arrested by

3
H. Zhang et al. Construction and Building Materials 385 (2023) 131518

Table 2
A) chemical compositions of cement and diatomite (%) and b) mineralogical compositions of cement provided by the supplier (%).
SiO2 Al2O3 Fe2O3 MgO CaO Na2O K2O SO3 TiO2 MnO

OPC 24.78 4.26 3.88 3.06 60.44 0.32 0.35 2.27 0.28 0.15
Diatomite 92.13 4.13 1.20 0.39 0.46 0.54 0.68 0.03 0.13 0.02

Clinker Gypsum Calcite Free lime Quartz Others

82.2 5.80 2.90 1.20 1.70 6.20

Fig. 1. The SEM picture of diatomite (40,000 × ). Fig. 3. The XRD pattern of the diatomite sample.

Fig. 4. Particle size distribution of the employed RA.

Fig. 2. Particle size distribution of cement and diatomite.

Table 3
using the solvent-exchange method with isopropanol [62]. The size distribution of the river sand.
For the SEM observation, small particles (size of 5 to 8 mm) of the Grain size (mm) 4.75 2.36 1.18 0.6 0.3 0.15 <0.15
paste samples were first knocked off from the 100-mm paste cubes,
Cumulative residual 0 0.5 3.9 23.5 72.5 96.4 100
which were moist cured at the target ages. Cement hydration was then (%)
arrested by soaking these particles in abundant isopropanol for 72 h,
with the isopropanol renewed every 24 h. After gold spray on the sample
surface, the morphology of the hydration products was detected by using
a QUANTA 250 scanning electron microscope (SEM).

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H. Zhang et al. Construction and Building Materials 385 (2023) 131518

Table 4
Concrete mixture proportions (kg/m3) and the measured slump (mm).
Concrete groups Mass of each component per cubic meter of concrete Slump
OPC DE Water Sand RA Superplasticizer

RAC 360 0 180 708 1154 1.8 190

RAC-5 342 18 2.16 190
RAC-10 324 36 2.52 200
RAC-15 306 54 2.88 200
RAC-20 288 72 3.24 195

The thermogravimetric (TG) measurements were carried out on a

Table 5
Netzsch STA 449F3 analyzer to determine the total CH content of pastes
The mixture proportions of the OPC-diatomite composite paste samples.
prepared with OPC replaced by diatomite at varying replacement rates.
Paste groups OPC DE Water Superplasticizer The peasized paste particles taken from samples cured at 1, 7, 14, and
P-0 1600 0 800 0 28 days were soaked in isopropanol to arrest cement hydration. After­
P-5 1520 80 1.6 ward, they were dried in the oven at a temperature of 45℃ until the
P-10 1440 160 3.2 mass did not change. Then the small particles were ground to powder,
P-15 1360 240 4.8
P-20 1280 320 6.4
passing a #200 sieve, and then placed in a Pt/Rh crucible with a
perforated lid under a nitrogen flow of 70 ml/min and heated from 45 ℃
to 1000 ℃ at 10℃/min.
As for the XRD measurements, the paste was first ground in iso­
propanol and then dried at 40℃ in a vacuum oven for 12 h. In the XRD 2.3.3.2. Pore structure. The pore structure of the cement mortar phase
measurement, Cu-Кα radiation with a wavelength of 1.54 Å in the 5 to and the ITZ phase in RAC as modified by the diatomite was assessed by
65◦ of 2θ range was utilized, and the voltage was set to be 45 kV and the the mercury intrusion porosimetry (MIP) technique and the image
current was 40 mA. The scanning step was set as 0.01313◦ and each step processing of the backscattered electron (BSE) pictures, respectively.
took for 118.32 ms. After 28 days, small peasized chunks were hammered down from the

Fig. 5. The processing procedure of the BSE pictures: (a) the BSE images being divided into parallel strips to the outline of the coarse aggregate, (b) the grey-value
histogram, and (c) the cumulative grey value curves obtained from one single strip.

5
H. Zhang et al. Construction and Building Materials 385 (2023) 131518

100 mm concrete cubes, and the coarse aggregate was carefully removed
by using tweezers. The remained new cement mortar (about 1 g in mass)
was first dried for 72 h at a temperature of 45 ± 2℃, the pore structure
was measured and analyzed by the Quanta PoreMaster-60 MIP. The pore
size distribution (PSD) curve can then be obtained by relating the
intruded volume at a given pressure to the pore size evaluated at the
same pressure [63]. In the MIP measurement, the upper limit of the
pressure under the low-pressure modes and the high-pressure modes
was set to be 20 psi and 50, 000 psi, respectively. The relation between
the applied pressure (P) and the size of the connected pores (d) of the
tested samples can be expressed by the Washburn-Laplace formula (see
Eq. (1). In Eq. (1), the contact angle θ of mercury was taken as140◦ , and
the surface tension of mercury γ as 0.480 N/m. Therefore, the MIP
measurement can provide the size distribution of pores ranging between
0.003 and 1080 μm.
4γcosθ
d= − (1)
P
The sample processing procedure of the concrete samples taken for
the BSE observation mainly refers to Reference [64]. The BSE pictures
were first taken in the vicinity of the target ITZ. After noise reduction, Fig. 7. The schematic diagram for the arrangements of testing points across ITZ
these images were split into strips (width of 10 μm) parallel to the in the microhardness measurement.
outline of the coarse aggregate or the old mortar (Fig. 5a) using Pho­
toshop software. Afterward, these strips were processed by the Image- schematically shows the arrangements for the testing points in the
Pro plus software to obtain the gray-value histogram (e.g., Fig. 5b) microhardness measurement across the target ITZ1 and ITZ3. As shown
and the cumulative grayscale curve (e.g., Fig. 5c). The threshold of the in Fig. 7, the interval between every two adjacent indents in each row
grey value was then determined as the overflow point on the cumulative was 20 μm while that between the two rows was 10 μm. The interlaced
grayscale curve. For example, in Fig. 5c, the overflow point was at the indents can help obtain more microhardness data across the target ITZ
grey value of 53, which means the pixels with a grey value below 53 without inducing interference between adjacent indents. The static load
should be identified as pores. In this way, the porosity of each strip can for the microhardness measurement on both the ITZ and mortar phases
be calculated, and the distribution of the porosity across the target ITZ was set to be 0.01 kgf, while on the virgin aggregate phase, it was set as
can be plotted afterward. 0.05 kgf. The contact time for each testing point was 5 s. The micro-
Note that different from the natural aggregate concrete, there are hardness (MH, in MPa units), which is actually the Vicker hardness,
three types of ITZ contained in RAC, as reported by the authors in their can then be calculated as follows [66,67]:
previous works [65] (see Fig. 6). The new ITZ includes ITZ1 between the
unwrapped old virgin aggregate and the new cement mortar, and ITZ3 MH =
2P(sinα/2)
× 9.81 (2)
between the old and new cement mortar, while ITZ2 embedded in the RA d2
particles was identified as the old ITZ. The BSE images of the old ITZ
where P is the applied force in the unit of kgf; α is the indenter diagonals
were not taken for the pore structure analysis, as the effect of the partial
angle which is 136◦ in this measurement, and d (unit: mm) is the average
replacement of cement by the diatomite on the old ITZ2 may probably be
diagonals of the indentation.
marginal.

3. Results and discussion

2.3.3.3. The micro-mechanical properties of ITZ. The micro-mechanical
property of the new ITZ phases (i.e., ITZ1, ITZ3) was tested by the
THSV-1–800 M− AXY microhardness tester at the age of 28 days. The
sample processing procedure was the same as that for the BSE mea­
surement. Similarly, the replacement of cement with diatomite should
not lead to obvious changes in the microhardness of the old ITZ2, so the
microhardness of ITZ2 was not tested in this present work. Fig. 7
Fig. 6. The illustration for the different types of ITZs contained in (a) RAC and
(b) NAC [65].
3.1. Concrete properties on the macro scale
3.1.1. Compressive strength
Fig. 8a shows the compressive strength of the five groups of concrete
with OPC partially replaced by diatomite at the ages of 7, 14, and 28
days. According to Fig. 8, RAC prepared with the blended binder of OPC
and diatomite presents greater compressive strength than the reference
RAC at all ages. At the age of 28 days, the compressive strength of the
reference RAC failed to reach the target strength level, i.e., 30 MPa,
while that of those with diatomite was from 34.9 to 38.1 MPa. The
improved strength should be attributed to both the filling effects and the
pozzolanic effects of the employed diatomite, which will be discussed in
detail in Section 3.2.
Fig. 8b gives the relative changes in fc for these RAC groups
compared to the reference RAC so that the enhancement of compressive
strength at varying dosages of diatomite can be better compared. Basi­
cally, the improvement in the compressive strength became more sig­
nificant with the increasing replacement rate of OPC by diatomite up to
a dosage of 15%, while afterwards it began to drop. It is reasonable that
the compressive strength would be better enhanced if more diatomite
participated in or facilitated the cement hydration so that both the
mortar phase and the ITZ phase in RAC would be enhanced. However,

6
H. Zhang et al.
Fig. 8. Compressive strength and the relative change compared to the reference RAC: (a) fc, and (b) the relative change in fc.
the excessive diatomite added to RAC to replace OPC would lead to the
dilution of cement clinkers so less calcium hydroxide (CH) would be
available for the pozzolanic reaction between diatomite and CH. This
would hinder the further enhancement of compressive strength of RAC
with the increasing dosage of diatomite. As is seen from Fig. 8b, the
compressive strength of RAC at a diatomite dosage of 15% can be
improved by 15.4%, 13.1%, and 29.2% at the ages of 7, 14, and 28 days,
respectively, while the improvements diminished to be 5.0%, 11.0%,
and 22.4% at 20% though fc is still higher comparing to that of the
reference RAC. Fig. 8b also shows that the improvement in the
compressive strength by diatomite is more significant at 28 days than at
an early age, e.g., 7 days or 14 days. This is likely due to more complete
reactions between diatomite and the cement hydration products at later
ages given that the samples were stored at an appropriate temperature
and humidity.
3.1.2. Splitting tensile strength
Similar results can be found in the splitting tensile strength (i.e., fst)
of RAC as modified by the diatomite at different replacement rates of
OPC (see Fig. 9). The most significant improvement in the splitting
tensile strength of RAC can also be observed at a replacement ratio of
15%; the improvements were 14.8%, 15.2%, and 33.9% at the ages of 7,
14, and 28 days, compared to that of the reference RAC at the same ages.
According to Fig. 19b, the enhancement in the tensile strength by
diatomite was also more significant at 28 days than at earlier ages,
especially at 7 days.
It is well known that the concrete specimens would undergo a brittle
Fig. 9. Splitting tensile strength and the relative change compared to the reference RAC: (a) fst, and (b) the relative change in fst.
7
Construction and Building Materials 385 (2023) 131518
f
fracture in the measurement of splitting tensile strength and the con­
crete would break along the relatively weak material phases present in
the specimens. Therefore, the analysis of the fracture section can help
identify the relatively weak material phases under the tensile loads.
Fig. 10 provides the pictures of the fracture sections of three concrete
groups, i.e., the reference RAC, RAC-15, and RAC-20, after the mea­
surements of fst. As shown by Fig. 10, the fracture paths through
different phases were outlined in certain colors. The red color outlined
the fracture paths along the ITZ. Such fracture can be easily recognized
on the fracture sections by the peeling of the old virgin aggregate or the
old mortar off the new mortar matrix. Note that the recycled coarse
aggregate could also fracture under the tensile stress, and the fracture
may break through either the old mortar phase or in some cases through
the old virgin aggregate instead of through the weaker ITZ. These
fracture paths were outlined in blue and green in Fig. 10, respectively.
By making comparisons between Fig. 10a and Fig. 10b, it can be seen
that the replacement of 15% OPC by diatomite leads to an increased
preference for fracture via the old mortar phase and a diminished
preference via the ITZ (mainly the new ITZ between the new and old
cement mortar, or between the unwrapped old virgin aggregate and the
new cement mortar) compared to the case with the reference RAC. This
change indicates the likely enhancement of the ITZ phase at a proper
replacement ratio of OPC by the diatomite. In contrast, the increase in
the fracture preference via the old mortar is no longer obvious at a
relatively higher replacement ratio (i.e., 20%, see Fig. 10c). More frac­
ture paths via the new ITZ can be observed on the fracture section of
RAC-20, which is quite similar to that of the reference RAC. Therefore,
fs
H. Zhang et al.
Fig. 10. The fracture sections of three concrete groups in the measurement of splitting tensile strength, i.e., (a) the reference RAC, (b) RAC-15, and (c) RAC-20.
even if the higher dosage of diatomite may benefit the densification of
new ITZ by promoting the conversion of CH to C-S-H, the excessive
diatomite skeletons which were unreacted and remained in the new ITZ
may still render the new ITZ vulnerable to tension due to the very porous
structure of diatomite.
The relationship between the splitting tensile strength (i.e., fst) and
the compressive strength (i.e., fc) for the five groups of RAC was also
8
Construction and Building Materials 385 (2023) 131518
discussed in this work. It can be seen from Fig. 11 that the spitting tensile
strength increased as the compressive strength increased, but the in­
crease is apparently slower than that of the latter. The empirical
formulae expressing the relationship between these two strengths for
normal concrete can be found in the regulations released by China,
Japan, Europe, the United States, etc., which are also provided in Fig. 11
[68–71]. As is seen from Fig. 11, the relationship between fst and fc
H. Zhang et al.
f f
f f
f f
f f
Fig. 11. The relationship between fst and fc and that given by different regu­
lations [68–71].
obtained from the five groups of RAC could be hardly expressed by a
certain formula due to the quite limited amount of data as well as the
data dispersion. Still, Fig. 11 shows that the data collected from the 5
groups of RAC are all below the lines given by the regulations of the
abovementioned countries. It indicates that a much lower splitting
tensile strength should be expected from the RAC samples at the same
compressive strength level to that of the normal concrete, regardless of
the use of diatomite or not. Even though that the splitting tensile
strength of RAC was proved to be even better enhanced by the use of
diatomite than the compressive strength (see the results shown in Sec­
tions 3.1.1 and 3.1.2), still the adverse effects brought out by the use of
coarse of RA on tensile strength could be hardly made up as RA intro­
duced a larger quantity of ITZ to concrete compared to the conventional
NA (see Fig. 6 in Section 2.3.3). The obviously lower splitting tensile
strength of RAC than the expected level also indicates the higher brit­
tleness of RAC than the normal concrete. Fig. 11 also shows that the
partial replacement of OPC by diatomite could slightly reduce the RAC
brittleness but the reduction is quite limited.
D
D
Fig. 12. Diffusion coefficient of chloride ions and the relative change compared to the reference RAC: (a) DRCM, and (b) the relative change in DRCM.
9
Construction and Building Materials 385 (2023) 131518
3.1.3. The chloride permeability
The diffusion coefficients of chloride ions tested by RCM, i.e., DRCM,
of the five concrete groups are shown in Fig. 12a. The drastic drop in
DRCM indicates an enhanced chloride impermeability of RAC by the
partial replacement of cement with diatomite. As shown in Fig. 12b, a
5% replacement of OPC by diatomite can reduce the DRCM of RAC by
35.21%, and when the replacement increases to 15%, the reduction can
reach up to 86.27%. Therefore, replacing OPC with diatomite even by
just a low ratio (e.g., lower than 20%) can greatly enhance RAC’s
resistance to the chloride ingress, which should be favorable to extend
the service life of reinforced RAC structures serving in marine environ­
ments. The beneficial effects by the introduction of diatomite on the
chloride impermeability of concrete are in close agreement with the
findings of previous studies [43,49], which is likely attributed to both
the filling effects and the pozzolanic effects of the fine diatomite as
utilized by this work. These effects will be discussed in detail based on a
series of microscopic measurements. Fig. 12b also shows that the
improvement in RAC’s resistance to chloride ingress would no longer be
further enhanced at a diatomite dosage over 10%; the likely explanation
should be the diluted cement clinkers at a high replacement ratio which
may reduce the total amount of hydration products and cause the in­
crease in the porosity of RAC.
3.2. Concrete properties on the microscale
3.2.1. The hydration process and the hydration products
Fig. 13a to d are the SEM pictures of diatomite taken at the ages of 0,
7, 14, and 28 days in the blended paste prepared with OPC and diato­
mite; the replacement ratio of cement by diatomite is 15%.
Fig. 13a shows a well-preserved diatomite cell that presents the
characteristic honeycomb texture taken before the diatomite particles
reacted with the hydration products of OPC. At 7 days (Fig. 13b), it can
be seen that the honeycomb surface of the diatomite cells was weath­
ered; a large amount of fibrous hydration products associated with C-S-H
can be observed to grow both on the surface and in the pores of the
diatomite skeletons, meanwhile, the edge of the diatomite skeleton
seems to be dissolving with the pores near the edge getting finer. This
phenomenon indicates that the diatomite is likely to induce both the
nucleation effects and the pozzolanic effects in the process of cement
hydration. The porous texture of the diatomite skeletons can provide
favorable sites for the growth of C-S-H gel, meanwhile the amorphous
silica can react with the hydration products of OPC, i.e., CH, to generate
H. Zhang et al. Construction and Building Materials 385 (2023) 131518

Fig. 13. The texture of the diatomite particles in the blended paste (i.e., P-15) at different ages: (a) before hydration, (b) at 7 days, (c) at 14 days, and (d) 28 days,
respectively.

Fig. 14. The diatomite in the binary system whose edge is turning grey.

10
H. Zhang et al.
more C-S-H. The pozzolanic reaction between the diatomite particle and
the cement hydration products can be further proved by the BSE picture
taken from the RAC-15 sample (see Fig. 14), in which the edge of a
diatomite particle is apparently turning grey. In Fig. 13b, some needle-
like hydration products which should be ettringite (AFt) can also be
observed in the vicinity of the dissolving diatomite particles. With the
passage of time, the honeycomb texture of diatomite can hardly be
observed at 14 days, as the surface of the skeleton was covered by more
fibrous and reticular hydration products (Fig. 13c). At the age of 28
days, most diatomite particles were almost fully encompassed by the
fibrous and leafy-like C-S-H and needle-like AFt, which were bridging
and binding together surrounding the diatomite skeletons (Fig. 13d).
The XRD patterns obtained from the OPC-diatomite paste are shown
in Fig. 15 (28 days).
As mentioned above, the XRD diffractogram of the calcined diato­
mite samples clearly shows an amorphous silica hump around 2θ = 22◦
(Fig. 4), while after 28 days of hydration, the amorphous hump around
2θ = 22◦ was no longer detected in the OPC-diatomite binary system and
was replaced by the signal of portlandite (CH) and calcium silicate hy­
drate (C-S-H). In Fig. 15, the three humps at 2θ of 29.4◦ , 32.1◦ , and 50.1◦
which are assigned to a C-S-H gel [72] imply that the gel should be quite
disordered [73]. In both the pure cement paste and the cement-
diatomite pastes, the main crystalline product is portlandite, but the
intensity of portlandite at 2θ = 34.2◦ and 47◦ is significantly smaller in
the blended pastes compared to that in the OPC control; moreover, the
intensity of CH is diminishing as more OPC is replaced by the diatomite.
As for another characteristic peak of CH at 2θ around 18◦ , Fig. 15 shows
that the diffraction intensity also underwent a decrease given that the
diatomite dosage was no greater than 10%. However, the peak height
began to increase when the diatomite dosage was over 10% (see P-15
and P-20). The trend is different from that observed from the other two
CH peaks at 2θ = 34.2◦ and 47◦ as described above. It is difficult to
Fig. 15. The X-ray diffractogram for the blended pastes cured at 100% relative humidity for 28 days.
11
Construction and Building Materials 385 (2023) 131518
explain such a difference as the reason may be multifaceted. First, it is
widely known that the preferred orientation has an influence on the XRD
results which cannot be eliminated [74,75]. There is thereby a likeli­
hood that the difference between the three characteristic CH peaks as
influenced by the diatomite dosage may be attributed to the preferred
orientation effects which would vary from one sample to another. Given
that the preferred orientation effects are not considered by this present
work, the decreasing height of the CH peak at 2θ around 18◦ from P-0 to
P-10 implies that the CH content may be reduced with the partial
replacement of OPC by diatomite, while the increasing peak height at a
diatomite dosage greater than 10% (e.g., 15% and 20%) indicates that
the CH content may be increasing, though it is still lower than that in the
blank paste. CH is known as the main product of the primary cement
hydration. Replacing part of OPC by diatomite would lead to the dilution
of cement clinkers thereby reducing the CH generated through the pri­
mary OPC hydration. Besides, the diatomite can further consume CH via
the pozzolanic reaction to generate C-S-H gel and this process is also
known as the “secondary hydration” of cement [76,77]. Therefore, the
changes of the CH content in the paste samples should be attributed to
the competing effects of the primary cement hydration and the sec­
ondary hydration with the incorporation of diatomite, which however,
cannot be quantitively evaluated merely according to the height of the
CH diffraction peaks obtained by the XRD measurement. Instead, the
quantitative analysis on the CH content should be conducted based on
the TG analysis which is going to be discussed below.
Fig. 15 also indicates that the anhydrous clinker phases contained in
the OPC (e.g., C3S and C2S at 2θ = 26.6◦ , 29.3◦ , and 32.5◦ ) underwent a
reduction in amount with more OPC replaced by diatomite, which is
reasonable as the cement clinkers would be diluted by the use of diat­
omite. There is another likelihood that diatomite may accelerate the
dissolving of cement clinkers by inducing the nucleation effects. Besides,
Fig. 15 shows that the AFm peak in the cement-diatomite pastes greatly
H. Zhang et al. Construction and Building Materials 385 (2023) 131518

diminishes compared to the reference cement paste. In P-15 and P-20 between 600 and 800 ℃) must be counted in [52]. The evolution of the
with relatively higher proportions of diatomite, the AFm phase can content of portlandite over the hydration age in the five pastes is shown
hardly be identified in the XRD diffractogram at the age of 28 days. This in Fig. 16b. Apparently, with more cement replaced by diatomite, the
is reasonable considering the diluted cement clinkers by diatomite and content of CH in the binary paste after 28-day hydration dropped
the conversion of high Ca/Si C-S-H to lower Ca/Si C-S-H [78] with significantly, especially at a replacement higher than 5%. This is
diatomite as an extra Si4+ supplement. The generation of low Ca/Si C-S- consistent with the findings concluded from the XRD measurement and
H is responsible for reducing soluble Ca2+ and the decreasing alkalinity is likely ascribed to the pozzolanic effects and the dilution effects by the
of pore solution, which is not favorable for the stabilization of the AFm replacement of OPC with diatomite.
phases [79,80]. As proposed by References [81,82], the pozzolanic reactivity of a
Note that the usefulness of the XRD testing is greatly limited because pozzolan can be accessed by the normalized CH content, i.e., CHnorm , of
it cannot identify hydraulic binding phases. Besides, as mentioned the composite cementitious paste prepared with the target pozzolan and
above, the XRD measurement conducted by this work could only pro­ cement respecting that of the plain paste, which can be calculated by the
vide qualitative analysis on the compositions of hydration products following formula:
while the quantitative information has to be achieved via other tech­
CH(t)
niques, e.g., TGA. CHnorm (t) = (3)
mc × CHplainpaste (t)
Fig. 16a gives the TG-DTG curves obtained from the five groups of
pastes with cement replaced with diatomite by 0, 5, 10, 15, and 20%,
where CH(t) and CHplainpaste (t) are the CH content (g/g of ignited
respectively, at the age of 28 days. The weight loss between 50 ℃ to 400
weight) of the composite cementitious paste containing the target
℃ is associated with C-S-H. Fig. 16 shows that all the blended pastes
pozzolan and that of the plain paste at the age t, respectively; mc rep­
have more C-S-H than the plain paste after 28 days’ hydration, con­
resents the weight proportion of cement accounting for the composite
firming that the diatomite can indeed facilitate the cement hydration.
cementitious materials. Lower CHnorm indicates a more significant
With the replacement ratio below 15%, the amount of C-S-H increased
pozzolanic effect of the target pozzolan in the composite cementitious
with the diatomite dosage. At a replacement higher than 15%, however,
paste.
the amount of C-S-H underwent a significant reduction. This is probably
The content of CHnorm in the binary paste with cement replaced by
due to the scarcity of Ca(OH)2 (CH) at a high dosage of diatomite which
diatomite at varying replacement ratios were compared in Fig. 17.
is essential for the pozzolanic reactions. This result agrees with the
As is seen from Fig. 17, basically, the content of CHnorm in P-15 is
compressive strength data in which the enhancement in the compressive
lower than that in other paste groups, indicating the overall more suf­
strength of RAC underwent a drop when the diatomite dosage exceeded
ficient pozzolanic reaction at a 15% replacement. Fig. 17 also shows that
15%. The less significant improvement in the compressive strength of
the CHnorm of the cement-diatomite paste, all experienced a rise from 1
RAC-20 compared to the reference RAC with a higher content of diat­
day to 7 days. It is known that cement hydration was very quick at an
omite can thus be linked to the lack of portlandite ascribed to the
early age (the hydration of OPC would be 75% complete within the first
dilution effects.
7 days). In view of this, the pozzolanic effect of diatomite (if any), which
The dehydration of CH is observed from the weight loss between 430
should have led to a consumption of CH, would be less significant
℃ and 500 ℃, as shown in Fig. 16. The determination of the amount of
compared to the early cement hydration, which can produce a large
portlandite can help access the pozzolanic effects of diatomite in the
amount of CH within a short period of time. Moreover, the SEM obser­
binary system but note that at a temperature over 600 ℃, decarbonation
vation has confirmed the nucleation effects of diatomite in the binary
of CaCO3 is observed, indicating the carbonation of the paste samples.
paste, which can promote cement hydration, thereby generating more
Even though in this work, the samples were very carefully cured (in
CH than that consumed by the pozzolanic reaction. This explains why
saturated CH solution) and processed (being ground in isopropanol),
the normalized CH content experienced a rise from 1 to 7 days. At a later
carbonation cannot be completely avoided during the sample drying in
age, after 7 days, the hydration reaction of cement may have already
the normal oven instead of the vacuum oven. Therefore, the amount of
slowed down, and the pozzolanic reaction began to play a more
portlandite that is equivalent to CaCO3 (decomposition occurring

Fig. 16. TG-DTG analysis of the cement-diatomite pastes at the age of 28 days: (a) the TG-DTG curves obtained from 100 to 1000 ℃, and (b)the content of Ca(OH)2.

12
H. Zhang et al.
CH
Fig. 17. The content of CHnorm in pastes.
predominant role than the nucleation effect in the binary system,
thereby causing a significant drop in CHnorm from 7 to 14 days. The
normalized CH content was all below 1.0 at 14 days, namely, it was
lower than that in the reference plain cement paste. The age of 28 days
has witnessed a rise in the CHnorm content again compared to that at 14
days, which indicates that the pozzolanic reaction may probably
diminish after 14 days. The reason for the hampered pozzolanic reaction
at this stage may be attributed to the coated diatomite by the reticular C-
S-H (see Fig. 13d), which prevented the access of diatomite to CH [78]. It
can also be seen from Fig. 17 that the pozzolanic reactivity was
enhanced with more cement replaced by up to 15%; at a higher
replacement, i.e., 20%, the normalized CH content was comparable to or
even higher than that in P-15, indicating the diminishing pozzolanic
reactivity which should be ascribed to the diluted cement clinkers by
excessive diatomite causing the scarcity of CH for the pozzolanic
reaction.
Diatomite can also change the hydration degree of cement. The hy­
dration degree of the cement-diatomite system can be determined by
analyzing the content of non-evaporable water according to the TG test
results. The content of non-evaporable water (Wn) was obtained as the
difference in mass between the sample heated at 105℃ and 1000℃
normalized by the mass after heating to 1000℃ [82]. As typically
assumed that amorphous silica does not consume water chemically to
react with CH [81,83], and the hydration of 1 g cement produces about
0.23 g non-evaporable water, the hydration degree can thereby be
calculated by following Eq. 4 below:
Wn (t)
DoH = × 100 (5)
mc Wn (∞)
where mc is the mass ratio of cement to the composite cementitious
materials composed of cement and diatomite in this present work; Wn(t)
is the non-evaporable water content of cement paste at any time t (g/g of
ignited weight), and Wn (∞) is the non-evaporable water content at t→∞
corresponding to full hydration of 1 g of cement, which is about 0.23 g as
mentioned above.
Fig. 18 compares the hydration degree between the five cement-
diatomite paste samples at the ages of 1, 7, 14, and 28 days. Fig. 18
confirms again that the partial replacement of cement with diatomite by
up to 20% can improve the hydration degree at any age. At a very early
age, i.e., 1 day, the hydration degree increased with more cement
replaced by diatomite due to the enhancing pozzolanic effects and
nucleation effects, given that CH was supplied in abundance at this
13
Construction and Building Materials 385 (2023) 131518
Fig. 18. The hydration degree of cement at different ages.
stage. The dilution of clinker contributed to the higher hydration degree
at the early age, too. As derived from Fig. 18, the hydration degree
within the first 24 h was 48.8% for the reference cement paste, and it
was improved to 63.5% for the P-20 paste. At later ages, however, the
most significant improvement in the hydration degree was observed at a
replacement of 15%, and at a higher replacement of 20%, the hydration
degree began to drop. The possible reason is related to the scarcity of CH
as mentioned above. The hydration degree at 28 days in the P-15 sample
reached 86.5%, which was 23.2% higher than that of the reference
cement paste.
3.2.2. The pore structure
Fig. 19a and b gives the cumulative pore volume and the differential
pore size distribution (PSD) curve of the new cement mortar sampled
from the prepared RAC specimens cured after 28 days. It is known that
the capillary pores present in concrete can be further classified into three
categories, i.e., the small/medium/large capillary pores with the size
ranging from 2.5 to 10 nm, 10 to 50 nm, and 50 to 10,000 nm, respec­
tively [84]. The size ranges of the three categories of capillary pores are
also given in Fig. 19.
The MIP results indicate an obvious change in the proportions of
capillary pores with the increasing replacement ratio of OPC by the
diatomite. By comparing the intrusion curves shown in Fig. 19a, it can
be seen that the RAC modified by diatomite contained a larger propor­
tion of medium capillary pores while the large capillary porosity was
obviously lower than that of the reference RAC. Fig. 19 shows that the
peaks of the PSD curve of the reference RAC falls in the range from 100
to 1000 nm which means that the most probable pores in RAC should be
the large capillary voids. As for the RAC groups with OPC partially
replaced by diatomite at a rate no larger than 15%, the peak of the PSD
curves shifts to the left compared to that for the reference RAC. The most
probable pore size for RAC-5 and RAC-10 is quite close to the size range
for medium capillary voids. Such a change indicates that the pores may
be refined with the use of diatomite at an appropriate replacement rate.
As the diatomite dosage increases to 20%, however, the peak of the PSD
curve shifts back to the right and the peak is even higher than that for the
reference RAC. It indicates that the most probable pore size was
enlarged at this high diatomite dosage.
The influence of capillary pores on the concrete performance has
been long studied by previous researchers. It is once proposed by Mehta
et al. [84] that the capillary voids larger than 50 nm which referred to
macropores in modern literature are probably more influential in
determining the strength and impermeability characteristics of concrete,
while the pores smaller than 50 nm should have only marginal effects on
the mechanical properties of concrete. Uzal et al. [85] suggested that the
H. Zhang et al. Construction and Building Materials 385 (2023) 131518

Table 6
Representative pore structure indexes of the 5 RAC groups at 28 days.
RAC Total The The Average The most
group porosity, proportion proportion pore probable
% of pores of pores diameter, pore
smaller than larger than nm diameter,
50 nm, % 100 nm, % nm

RAC 20.1 17.94 72.19 50.40 266

RAC- 19.3 36.22 46.91 29.88 47
5
RAC- 21.3 33.71 45.26 70.67 73
10
RAC- 20.5 35.96 49.73 31.84 112
15
RAC- 18.8 24.48 62.40 48.72 266
20

d be confirmed by the reduction in the average pore diatomite, too. The
Fig. 19. MIP results: (a) the integral curves and (b) the differential curves of
the pore size distribution of paste in the five concrete groups.
increase in the proportion of pores larger than 100 nm may lead to an
obvious drop in the compressive strength of concrete. In light of this, the
proportion of pores smaller than 50 nm, i.e., the small and medium
capillary porosity, and that of pores larger than 100 nm (large capillary
porosity) in the mortar of the five groups of RAC were derived from
Fig. 19 and shown in Table 6. Some other representative pore structure
indexes, including the total porosity, the effective porosity, the average
diameter, and the most probable pore diameter as derived from the MIP
curves, were also listed in Table 6.
It can be seen from Table 6 that the proportion of pores smaller than
50 nm increased while that for pores larger than 100 nm was greatly
reduced in RAC with the increasing diatomite replacement ratio from
0 up to 15%. For instance, at the replacement ratio of 5%, the volume
fraction of pores smaller than 50 nm was doubled, and that of pores
larger than 100 nm was reduced by as large as 35.02%, compared to the
reference RAC. Therefore, the partial replacement of cement by
diatomite (no larger than 15%) should help make pores finer, which can
pore-filling effects due to the small size of the diatomite particles, the
nucleation effects as well as the pozzolanic effects which helps generate
more C-S-H in the cement-diatomite binary cementitious system,
contribute to the pore structure improvement together. Also, it is known
that the permeability of cement paste or concrete should be largely
dependent on the proportion of large capillary pores [84]. Hence, the
reduced proportion of pores larger than 100 nm, as shown in Table 6 can
explain why the RAC’s impermeability of chloride ions was significantly
improved by the replacement of cement with diatomite, as discussed in
Section 3.1.3.
It is noteworthy that the increase in the diatomite replacement is not
always beneficial for the pore structure of RAC. Table 6 and Fig. 19b
show that both the average pore diameter and the most probable pore
diameter increase as the diatomite dosage rises from 5% to 20%. At a
replacement rate of 20%, the average or the most probable pore diam­
eter became comparable to that in the reference RAC. This is reasonable
as the diatomite skeletons themselves are porous, which means that the
use of diatomite would introduce more pores larger than the pores be­
tween C-S-H gels. The dilution effects due to the high replacement of
cement by diatomite would also contribute to an increased fraction of
large pores in RAC. The marginally improvement in the pore structure
with the higher dosage of diatomite explains why the enhancement in
strength/chloride impermeability for RAC would not keep rising with
the increasing replacement rates of OPC by diatomite. Also note that the
porosity of the new mortar would be influenced not only by the dosage
of diatomite, but also by the concrete admixture. As mentioned in Sec­
tion 2.2, an increasing dosage of superplasticizer was added to the RAC
mixture as the replacement rate of OPC by diatomite increased from 0 to
20% in order to ensure the comparable fluidity between these RAC
mixtures. The usage of a larger dosage of superplasticizer was likely to
influence the porosity and the pore size in concrete mixtures as reported
by previous researchers [86,87], even though deforming agent was
already incorporated in the employed superplasticizer. The porosity as
well as the proportion of pores at certain size ranges may thereby fluc­
tuated due to different dosages of superplasticizer added to the RAC
mixture which however was not sufficiently considered by this work. It
is recommended that such an effect should be further eliminated by
reliable techniques, e.g., by the incorporation of extra deforming agent
with the dosage finely adjusted.
As for the porosity distribution across ITZ, it was analyzed by the
image processing technique on the BSE pictures captured in the vicinity
of ITZ, as mentioned in Section 2.3.3. Figs. 20 and 21 give the repre­
sentative BSE pictures captured around the new ITZ, i.e., ITZ1 and ITZ3,
in different RAC. Note that the BSE pictures of RAC-10 were corrupted so
they were not incorporated in these two figures. The old ITZ2, which lay
between the old virgin aggregate and the old cement mortar, was sup­
posed to be hardly influenced by diatomite because it was embedded
inside the RA. Therefore, the porosity distribution across ITZ2 was not

14
H. Zhang et al.
Fig. 20. BSE pictures taken in the vicinity of ITZ1, in (a) RAC (1000 × ), (b) RAC-5 (1000 × ), (c) RAC-15 (1000 × ), and (d) RAC-20 (1000 × ), respectively.
discussed by this work.
In Fig. 20, diatomite particles can be rarely observed in the vicinity of
ITZ1 in RAC-5 (see Fig. 19b), because of the sufficient pozzolanic reac­
tion after 28-days hydration, given that the diatomite dosage was rela­
tively low. In contrast, some unreacted diatomite particles can be
observed around ITZ1 in the RAC groups with higher diatomite dosages,
e.g., 15% or 20% (see Fig. 20c and d). A similar phenomenon can be
found with ITZ3, as shown in Fig. 21.
The unreacted diatomite (at least for the case at 28 days) in RAC-15
and RAC-20 should have enlarged the porosity of ITZ1/ITZ3, while the
porosity distribution results as obtained by processing a series of
representative BSE pictures captured in the vicinity of new ITZ were just
opposite (see Fig. 22). Fig. 22a shows that the porosity within ITZ1 in
RAC with cement partially replaced by diatomite was basically lower
than that in the reference RAC, and the porosity level dropped with the
increase of the diatomite dosage. With regard to ITZ3, the porosity
fluctuated a little bit within ITZ3, but the trend was similar to that for
ITZ1; the higher replacement rate of cement by diatomite corresponded
to a more significant reduction in the porosity. This result indicates that
15
Construction and Building Materials 385 (2023) 131518
the beneficial effect of diatomite in reducing the ITZ porosity is likely to
be more significant than the adverse effect induced by the porous
structure of diatomite itself and the dilution of cement clinkers, given
that the diatomite replacement ratio is no larger than 20%. Besides, the
thickness of the two new ITZs in RAC was reduced with the use of
diatomite, too. As is seen in Fig. 22, the thickness of ITZ1 and ITZ3
changed from 70 μm to 60 μm and 80 μm to 70 μm, respectively.
3.2.3. Microhardness
Probably due to the reduced porosity, the new ITZ1 and ITZ3 in RAC
with cement partially replaced by diatomite present higher microhard­
ness levels than those in the reference RAC, as is seen from Fig. 23. Take
ITZ3 for example, the average microhardness was 207, 220, 229, 255,
and 256 MPa for the reference RAC and the RAC prepared with 5% to
20% cement replaced by diatomite, respectively. The greatest
enhancement was observed in RAC-15 and RAC-20, for which the ITZ3
microhardness was enhanced by up to 23.7% compared to that for the
reference RAC. Similar results can be found in the microhardness of the
new cement mortar. The average microhardness of the new cement
H. Zhang et al. Construction and Building Materials 385 (2023) 131518

Fig. 21. BSE pictures taken in the vicinity of ITZ3 in (a) RAC (1000 × ), (b) RAC-5 (1000 × ), (c) RAC-15 (1000 × ), and (d) RAC-20 (1000 × ), respectively.

Fig. 22. Porosity distribution across (a) ITZ1, and (b) ITZ3 in different RAC.

16
H. Zhang et al. Construction and Building Materials 385 (2023) 131518

Fig. 23. Microhardness distribution across (a) ITZ1, and (b) ITZ3 in different RAC.

mortar was 508, 541, 550, 580, and 577 MPa for the five RAC groups, as the improved pore structure of the mortar and ITZ should be responsible
derived from Fig. 23. The most significant enhancement in the micro­ for the greatly enhanced compressive and splitting tensile strengths of
hardness of new mortar was observed in RAC-15 and RAC-20, too, which RAC prepared with cement partially replaced by diatomite compared to
was about 14%. The reason for the enhancement in the microhardness of the reference RAC. As reported in Sections 3.1.1 and 3.1.2, the greatest
the new ITZ and new cement mortar by the partial replacement of enhancements in the 28-day fc and fst were 29.2% and 33.9%,
cement with diatomite is similar to that in the reduction of ITZ porosity, respectively.
as already discussed above. Increasing the amount of diatomite can It is worth noting that the pozzolanic reactivity requires an optimal
benefit the micro-mechanical properties of the new ITZ and new mortar replacement ratio of cement by diatomite, according to the normalized
in RAC, but the benefit is no longer increasing when the diatomite CH content, i.e., CHnorm , as discussed in Section 3.2.1. The optimal
replacement ratio exceeds 15%. replacement ratio in terms of pozzolanic reactivity in this work was
observed at 15%; the weakened pozzolanic reactivity at a higher
replacement ratio (i.e., 20%) should be ascribed to the scarcity of CH in
3.3. Discussion on the effects of the partial replacement of OPC by
the system due to the diluted clinkers by excessive diatomite. The
diatomite on the RAC performance
excessive diatomite resulted in not only the weakening pozzolanic
reactivity, but also the insignificant improvement in the pore structure
As discussed above, the partial replacement of OPC by diatomite can
of the cement mortar in RAC (see the relatively larger proportion of large
improve both the compressive and tensile strengths of RAC given that
pores and also larger average pore size according to Table 6, Section
the replacement ratio is no larger than 20%. Test results on the micro-
3.2.2). These two adverse effects, as well as the directly diluted clinkers,
scale show that the calcined diatomite used in this work was charac­
explains why the improvement in compressive and tensile strengths of
terized by the small particle size (smaller than cement), the porous
RAC by the diatomite began to drop when the diatomite replacement
honeycomb-like structure, and the high content of amorphous silica.
rate exceeded 15%.
These characteristics are responsible for three main effects of diatomite
The decreasing proportion of large capillary pores for the cement
inducing on the cement-diatomite system, i.e., the pore-filling effect, the
mortar of RAC, as well as the diminishing porosity of the new ITZ1 and
nucleation effect, and the pozzolanic effect. The replacement of OPC
ITZ3, contributes to the obvious reduction in the chloride diffusivity of
with diatomite also leads to the dilution of cement clinkers, known as
RAC, too. According to the results discussed in Section 3.1.3, the
the dilution effect. The nucleation effect has been confirmed by the SEM
reduction in DRCM of RAC can be as large as 86.72%. Moreover, only a
observation. The porous structure of the diatomite skeletons was found
5% replacement of OPC by diatomite can already significantly reduce
to provide a quantity of favorable sites for the growth of C-S-H, thereby
DRCM of RAC by 35.21%. This result suggests that the partial replace­
promoting the hydration of cement. The pozzolanic reaction between
ment of OPC by diatomite should have a promising prospect in preser­
the diatomite and the hydration products of cement was confirmed not
ving the performance of reinforced RAC structures serving in marine
only by the BSE observation (see the turning-grey edge of diatomite in
environments. It is also interesting to note that the DRCM keeps
the binary paste, Fig. 14) but also by both the XRD and TG analysis. The
decreasing as the diatomite dosage increases from 15% to 20% while the
pozzolanic reaction directly led to the conversion of CH towards C-S-H
proportion of pores larger than 100 nm in the new mortar increased
in the cement matrix of RAC, thus being predominantly responsible for
from 49.73% to 62.4%. More large pores contained in the new mortar
the reduction in the content of CH as verified by the TGA results. Both
should have adverse effects on the chloride impermeability of concrete.
the nucleation effects and pozzolanic effects of diatomite can contribute
However, it is widely accepted that the chloride permeability of concrete
to the generation of more C-S-H and also improve the hydration degree
should be more largely dependent on the ITZ phase rather than the
of the cement-diatomite binary system, as confirmed by the analysis of
mortar phase, as the permeability of the former was times larger than
non-evaporable water content (Wn) according to the TG/DTG curves
that of the latter as commonly referred in the published literature
(see Fig. 17, Section 3.2.1). The more thorough cement hydration and
[84,88]. It is likely that the reduced porosity of ITZ with the addition of
the generation of more C-S-H usually correspond to better compactness
more diatomite (see the discussion in Section 3.2.2) induced even more
of the paste or mortar, meanwhile the fine diatomite particles can help
obvious enhancement on the chloride impermeability than the adverse
further fill the pores. Therefore, the pore structure of both the mortar
effects induced by the increasing large pores in the new mortar. As a
and ITZ in RAC was improved as discussed in Section 3.2.2 according to
result, the DRCM keeps decreasing as the diatomite dosage increased
the MIP measurements, and the processing of BSE images captured in
from 5% to 20%.
the vicinity of ITZ, respectively. The increasing C-S-H content, as well as

17
H. Zhang et al.
Moreover, the partial replacement of OPC by diatomite would help
further reduce the carbon emission of RAC. A previous study carried out
by Li et al. [48] reported that the carbon emission for mining diatomite
was about 2.7 kg CO2-eq/t taking that the density of the diatomite was
450 kg/m3. This is far less than the CO2 emission by the OPC production
as it is now well known that the production of every ton of OPC is
accompanied by an equivalent amount of carbon dioxide released. Ac­
cording to the data reported by previous researchers, the CO2 emission
of OPC by considering the vehicle transportation and the limestone
mining is 660 to 820 kg CO2-eq/t [89–91]. Taking that the carbon
emission of OPC was 660 kg CO2-eq/t, the replacement of OPC by
diatomite at the replacement rates from 5% to 20% could reduce the CO2
emission for preparing 1 m3 RAC by 11.88 kg to 47.52 kg, which is
remarkable. The added CO2 emission by the use of diatomite (2.7 kg
CO2-eq/t), however, can be ignored given that the largest dosage of
diatomite used for producing 1 m3 RAC was merely 0.072 t. Also note an
increasing dosage of polycarboxylate superplasticizer was added to the
RAC mixture with the increasing replacement rates of OPC by diatomite
in order to ensure the fluidity of the RAC mixture. The use of a larger
dosage of superplasticizer would lead to extra carbon emission for
producing RAC, too. Xiao et al. reported that the production of super­
plasticizer is responsible for a carbon emission of 1064 kg CO2-eq/t [92].
Since the dosage of superplasticizer was only 0.5% to 0.9% of the binder
(see Table 4 in Section 2.2), the extra carbon emission by the use of
superplasticizer would be 1.9 to 3.4 kg per m3 RAC, which is also quite
limited compared to the reduced carbon emission by less OPC used for
the concrete preparation. In light of this, the environmental profit of
RAC can be further enhanced compared to the conventional natural
aggregate concrete by the partial replacement of OPC by diatomite at an
appropriate rate, not to mention that the RAC strength and the dura­
bility were greatly improved at the same time. Apparently, these bene­
fits can ensure a better prospective of RAC applied in practical use.
However, it is noteworthy that the calcination and grinding operation
conduced on diatomite should be responsible for higher CO2 emission
compared to the as-received diatomite sample as referred in Li et al.’s
work. Further investigation should be carried out on this topic by col­
lecting more detailed information on the carbon emission for the pro­
cessing procedures of diatomite.
Note that the fine diatomite employed by this present work is typi­
cally used as a filter aid in the food production industry which is usually
produced from normal diatomaceous earth via calcination, grinding,
and sieving. Hence, this type of diatomite is supplied at a high price in
China which ranges between 250 and 300 US dollars per ton, which
means that its practical use will be greatly limited by the drastically
increased cost. However, the authors suggest that the cost can be
reduced to an acceptable level by using spent diatomite filter aid from
different industries. The amorphous silica content in the spent diatomite
filter aid is supposed not to be changed obviously compared to that in
the unused diatomite, so it may probably present the still high pozzo­
lanic reactivity in the RAC mixture. Moreover, the use of spent diatomite
filter aid as a partial replacement to cement in preparing RAC can help
further reduce the carbon footprint of concrete preparation, thereby
making RAC a more environmentally-friendly building material. Letelier
et al. once reported their trial to use both brewery spent diatomite and
recycled aggregate to prepare RAC and drew a conclusion that a 5% of
brewery spent diatomite and a 25% of RA can be used as a replacement
of cement and natural coarse aggregates without significant loss in the
mechanical properties when compared to a control concrete [46]. This
work, however, is mainly focused on the changes of the mechanical
performance of RAC by changing the replacement of OPC by brewery
spent diatomite and the replacement of NA by RA, respectively; the
modification effects of diatomite on the durability and long-term prop­
erties of RAC was not discussed in-depth, which deserves further
investigation in the following research. The possible challenge of using
the spent diatomite filter aid is that the open pores of the diatomite
skeletons may be filled with impurities through filtering; the unclean
18
Construction and Building Materials 385 (2023) 131518
pores may weaken the nucleation effects by reducing the favorable sites
for the growth of C-S-H gels. This adverse effect, if any, needs to be
evaluated in further studies by experimental investigation, however.
The study dealing with the effects of the spent diatomite filter aid from
different industries in modifying the RAC performance is already being
carried out by the authors’ group; the comparisons between different
types of diatomite, including the as-receiving low-grade diatomite earth,
the ground diatomite, the calcined diatomite, and the diatomite filter aid
(spent or not) in the modification effects on the RAC performance, and in
the environmental impacts, as well, will be discussed in detail and re­
ported in elsewhere.
4. Conclusions
This work proposes a new technique to improve the mechanical
performance and durability of RAC by using diatomite as a partial
replacement of OPC. A calcined diatomite filter aid was made use of, and
the improvements in the RAC performance, including the compressive
strength, the splitting strength, and the chloride permeability, were
experimentally investigated and discussed at varying replacement rates
of OPC by diatomite from 0 to 20%. The mechanism for the improved
RAC performance was discussed in terms of the changes in the hydration
products and the changes in the pore structure and micro-mechanical
properties of the mortar and ITZ phases in RAC, respectively. The
main findings can be summarized as follows:
1. Both the compressive and splitting tensile strengths of RAC can be
obviously enhanced by the partial replacement of OPC with diato­
mite by up to 20 wt%. The greatest enhancement was observed at a
replacement level of 15 wt%, for which the compressive strength and
splitting tensile strength at 28 days were improved by 29.2% and
33.9%, respectively.
2. The chloride impermeability of RAC was also greatly enhanced by
using diatomite as a partial alternative to OPC. A 5% replacement
can already significantly reduce the diffusion coefficient of chloride,
i.e., DRCM, by 35.21%; when the replacement increases to 15%, the
reduction can reach 86.27%.
3. The porous diatomite skeletons can provide a quantity of favorable
sites for the growth of C-S-H, as confirmed by the SEM observation.
The analysis of the XRD and TGA results obtained from the binary
paste of cement mixed with diatomite showed that the diatomite
presented significant pozzolanic reactivity, especially from 7 to 14
days. Both the nucleation effects and the pozzolanic reactivity of
diatomite contributed to the more complete cement hydration in the
binary cementitious system.
4. The use of diatomite can also improve the pore structure of both the
new mortar and new ITZ phases in RAC. The large capillary pores
(larger than 100 nm) in the new mortar can be reduced by as large as
35.02%, meanwhile the average pore diameter/ the most probable
pore diameter became smaller at a replacement level no larger than
15%. The porosity within the new ITZ was also obviously reduced
which led to the enhancement in the ITZ microhardness.
5. The pozzolanic reactions were found to be hampered at a diatomite
replacement higher than 15% (e.g., 20% in this work) due to the
scarcity of CH. The excessive diatomite would also dilute the cement
clinkers in RAC which led to insigificant improvement in the pore
structure of the RAC. It is thereby suggested that the replacement
ratio of OPC by diatomite should be no more than 15% in this case.
CRediT authorship contribution statement
Hongru Zhang: Methodology, Investigation, Writing – original
draft, Funding acquisition. Bingjian He: Investigation, Writing – review
& editing, Validation. Baojun Zhao: Investigation, Project administra­
tion. Paulo JM Monteiro: Conceptualization, Supervision, Writing –
review & editing.
H. Zhang et al.
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
This work was supported by the National Natural Science Foundation
of China (grant number 52178121), and the Science and Technology
Project of China Overseas Holdings Limited (grant number COHL-2021-
Z-1-02).
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