Science of the Total Environment 907 (2024) 167794

Contents lists available at ScienceDirect

Science of the Total Environment

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

Review

Global insights into micro-macro mechanisms and environmental

implications of limestone calcined clay cement (LC3) for sustainable
construction applications
Nauman Ijaz a, Wei-Min Ye a, Zia ur Rehman b, *, Zain Ijaz a, Muhammad Faisal Junaid c
a
Department of Geotechnical Engineering, College of Civil Engineering, Tongji University, Shanghai 200092, China
b
School of Civil Engineering and Surveying, University of Portsmouth, Portland Building, Portland Street, Portsmouth PO1 3AH, United Kingdom
c
Department of Materials Engineering and Physics, Faculty of Civil Engineering, Slovak University of Technology, Bratislava 810 05, Slovakia

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• Hydration chemistry and phase assem­

blage of SCMs were critically discussed.
• Effect of SCMs on rheological, mechan­
ical, and durability properties
• Environmental implications and poten­
tial research areas were discussed.
• Potential application of LC3 in various
fields of construction was determined.
• LCA showed LC3 a cost-effective blend
with low carbon footprints.

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

Editor: Daniel CW Tsang Limestone calcined clay cement (LC3) has gained attention in the research paradigm, and useful data is available
in scattered form, necessitates comprehensive review to provide global insight into important research questions,
Keywords: i.e., micro-macro response, and environmental implications, keeping in view the future research directions. In
Low carbon limestone calcined clay cement this regard, the current article provides a comprehensive insight into LC3, focusing on its micro-macro mecha­
(LC3)
nisms and critically examining different aspects such as chemical composition, hydration chemistry with special
Hydration chemistry
attention on phase assemblage, impacts of various salts and carbonation, rheological properties, mechanical
Durability
Sustainable applications behavior, high-temperature exposure, and compatibility with different admixtures. Additionally, this article
Environmental and economic aspect explores the sustainable and environmentally friendly applications of LC3, with an emphasis on its economic and
environmental advantages highlighted by pertinent data and lifecycle assessments (LCA). Comprehensive data
was gathered from a micro-macro perspective considering SCMs from different regional sources, and compari­
sons were drawn with Ordinary Portland Cement (OPC). Further, comparative economic and environmental
aspects for different grades of LC3 and OPC were evaluated and analyzed considering energy demand, cost-
effectiveness, and energy efficiency. The micro-macro characteristics of LC3 are found to be majorly

* Corresponding authors at: School of Civil Engineering and Surveying, University of Portsmouth, Portland Building, Portland Street, Portsmouth PO1 3AH, United
Kingdom.
E-mail address: engr.zrehman@gmail.com (Z. Rehman).

https://doi.org/10.1016/j.scitotenv.2023.167794
Received 5 August 2023; Received in revised form 19 September 2023; Accepted 11 October 2023
Available online 17 October 2023
0048-9697/© 2023 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY-NC license (http://creativecommons.org/licenses/by-
nc/4.0/).
N. Ijaz et al. Science of the Total Environment 907 (2024) 167794

dependent on its constituent, particularly clinker composition and alumina content in SCMs, which varies
regionally. This review study outlines the critical research directions, i.e., enhancement of mechanical behavior
and rheology, incorporation of super plasticizers and waste materials for resource conservation, and improve­
ment of carbonation resistance for durability to make LC3 a sustainable and first-choice cement.

1. Introduction: the necessity for innovative cement!
The escalating accumulation of greenhouse gases (GHGs), primarily
carbon dioxide (CO2), has resulted in global warming and poses a pro­
found threat to the planet (Izumi et al., 2021; Talaei et al., 2019). The
cement industry, responsible for 40 % of global CO2 emissions and
projected to contribute 10–15 % in the future, necessitates urgent action
(Anderson et al., 2016; Junaid et al., 2022). Extensive research reveals
cement production’s substantial environmental impact, accounting for
3.8 Gt of CO2 emissions in 2012 (Miller et al., 2016a, 2016b; Samad and
Shah, 2017; Salman et al., 2021). Recent stats showed that the annual
global cement output is roughly 4.5 gigatons, with consumption hov­
ering around 4.27 gigatons (Dinga and Wen, 2022). Concurrently, the
sector’s carbon emissions are increasing by 4.7 % each year (Hasanbeigi,
2019; Chatziaras et al., 2016). As the construction sector continues its
rapid expansion, immediate implementation of new policies and inno­
vative technologies becomes imperative to effectively mitigate CO2
emissions and address the pressing climate emergency, thereby charting
a path toward a more sustainable future (Ngo et al., 2018; Sanjayan and
Nematollahi, 2019).
Meanwhile, cement manufacturing emphasizes sustainability and
reduced energy consumption (Barcelo et al., 2014; Sousa and Bogas,
2021). Modern clinker plants maximize thermodynamic efficiency
(Fierro et al., 2020; Herrera et al., 2017; Z. Liu et al., 2015). Besides,
partially replacing clinker with Supplementary Cementitious Materials
(SCMs) reduces environmental impact (Chung et al., 2020; Olafusi et al.,
2019; Sonebi et al., 2016). However, commonly used SCMs, such as fly
ash, slag, silica fume, etc., have limited accessibility, reactivity and
affect the cement performance differently, restraining their global
acceptability (Lee et al., 2018; Mangi et al., 2018; Panesar and Zhang,
2020; Franco de Carvalho et al., 2019; Juenger et al., 2019; Miller, 2018;
Teixeira et al., 2019; Wu et al., 2011; Gao et al., 2021; Y. Gao et al.,
2018; J. Liu et al., 2019). In this regard, ternary blended cement (TBC)
enables higher clinker replacement without compromising performance
(Antoni et al., 2012a, 2012b; Dhandapani et al., 2022; Vaasudevaa et al.,
2021; Dhandapani et al., 2021).
In the field of TBC, a noteworthy development is the introduction of
limestone calcined clay cement (LC3), which replaces traditional clinker
with calcined clay/metakaolin (CC/MK) and limestone powder (LSP)
(Antoni et al., 2012a, 2012b). LC3’s notable feature lies in its ability to
reduce clinker consumption by nearly 50 % (Fig. 1), while promoting the
formation of a dense microstructure, resulting in improved mechanical
strength and enhanced durability (Dhandapani et al., 2021; Antoni,
2013). LC3 utilizes globally available clay and limestone waste sources,
offering easy implementation without specialized training (Akindahunsi
et al., 2020; Avet et al., 2018; Dixit et al., 2021; Huang et al., 2020a;
Krishnan et al., 2018a; Krishnan et al., 2018b; Lin et al., 2021a, 2021b;
Emmanuel et al., n.d.; Joseph and Krishnan, 2014; Sharma et al., 2021a,
2021b). In the realm of LC3, different review articles have been docu­
mented so far, which were predominantly focused on specific aspects or
limited geographical regions. For instance, Scrivener et al. (2018a,
2018b) provided a comprehensive analysis of calcined clay behavior and
its pozzolanic reactivity at different temperatures. Sharma et al. (2021a,
2021b) discussed the effect of raw material properties and mixture
design on the chemistry and strength behavior of LC3 cement.
Homayoonmehr et al. (2021) examined the influence of CC/MK on the
fresh properties and corrosive behavior of concrete. Fernandez et al.
(2011) offered valuable insights into clay minerals and their impact on
pozzolanic activity. Other reviews centered on economic and life cycle
assessments of LC3, such as the case study by Sánchez Berriel et al.
(2016) on the economic and environmental aspects of LC3 in Cuba’s
cement industry. However, a comprehensive state-of-the-art review
bridging the micro-macro behavior of LC3 from a global perspective,
encompassing diverse raw material sources and origins, and elucidating
their consequential effects on rheological, mechanical, and durability
characteristics remains conspicuously absent. Therefore, this review
endeavors to bridge this critical gap by providing an extensive and
authoritative analysis of these facets while elucidating the immense
potential of LC3 in advancing sustainable, economic, and
environmentally-friendly applications within the construction industry.
Given the discussion above, this article presents a comprehensive
review that delves into the global understanding of the micro-macro
mechanisms of LC3, considering its applicability in the construction
industry and proposing avenues for future research. The availability of
SCMs, their mineralogical and chemical compositions, the detailed
physical and chemical integration of these SCMs, the rheological fea­
tures, and the mechanisms influencing strength development are thor­
oughly discussed (Fig. 2). Furthermore, LC3’s durability under various
conditions, such as salt exposure, carbonation, and temperature effects,
and its compatibility with superplasticizers are analyzed. Importantly,

Fig. 1. LC3 composition; a) comparison of LC3 with OPC; b) typical LC3 recipe.

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N. Ijaz et al. Science of the Total Environment 907 (2024) 167794

the economic and environmental dimensions of LC3 are critically

explored, focusing on its cost-effectiveness and energy efficiency. This
study conducts a scoping and bibliometric review of LC3’s micro and
macro mechanisms, extracting key information from over 380 rigor­
ously selected articles from 1000 initially screened in databases like Web
of Science, Google Scholar, and Scopus using the Joanna Briggs Institute
Critical Appraisal System. Through thematic and content analyses, key
trends and patterns were identified, resulting in a comprehensive
narrative and visual overview of LC3 behavior. (Fig. 2).

2. SCMs accessibility

The prime SCMs in LC3 are CC/MK and LSP, which have significant
potential for global acceptance due to their wider availability (Ito and
Wagai, 2017; Martirena, 2017), unlike the traditional SCMs such as fly
ash, blast furnace slag, burnt shale, silica fume, natural pozzolan, etc.,
(Fig. 3) (Sandanayake et al., 2020; Shubbar et al., 2019; Teixeira et al.,
2019; Shi et al., 2008; Antoni et al., 2012a, 2012b). Though the use of
industrial wastes as SCMs contributes toward waste reduction and car­
bon emission, however, face significant challenges that limit their uni­
versal adoption as viable alternatives to OPC on a global scale. These Fig. 3. Comparison of availability of different SCMs reserves (Scrivener et al.,
challenges include limited accessibility to quality sources (Fig. 3), var­ 2018a, 2018b).
iable pozzolanic reactivity, restricted potential for clinker substitution,

THE ACTUCAL RESEARCH STATUS

ACTIONS
Materials Assessment

Hydration Chemistry
Low Carbon
Requirement Limestone Rheology
CONCERNS related to Value Research
resource conservation for new Calcined
Strength
and environmental cementing Clay
protection. addition dimensions
material. Cement LC3 Applications
OPC (LC-3)
Manufacturing Economical &
Environmental Aspect

THE FORMULATION OF PAPERS

Literature overview Keyword's determination Database

Data collection

Low carbon limestone calcined clay

Paper selection cement (LC3); rheological properties;
hydration chemistry; long-term durability;
LC3 applications; economical and
Main points
environmental aspect.

Micro Behavior Macro Behavior Life Cycle Assessment

SCMs composition, sourcing, & accessibility Rheology Economical aspect

Review areas

Role of calcined clay/metakaolin Mechanical Behavior Environmental aspect

Role of limestone powder Superplasticizers

Role of Gypsum
Application of LC3
Effect of various salts and carbonation on
hydration product

Future Research Dimensions and Summarization

Fig. 2. Methodology flowchart.

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N. Ijaz et al.
and diverse impacts on cement performance characteristics. These fac­
tors collectively act as constraints on their global acceptability.
Recent studies have demonstrated that CC/MK, in combination with
LSP, can effectively replace ~50 % of cement clinker owing to better
pozzolanic properties, offering comparable strength to traditional OPC
(Akindahunsi et al., 2020; François Avet et al., 2018). Clays found in
diverse regions globally exhibit varying concentrations of kaolinite
content and occur alongside associated minerals such as quartz, lime­
stone, iron-bearing phases, and other minerals derived from rocks
(Sionneau et al., 2008; Uwins et al., 1993). Whereas kaolinite-rich clays,
widely distributed worldwide, provide ample reserves for cement pro­
duction, especially in humid and hot climates where chemical weath­
ering is more intense (Lin, 2007; Satola et al., 2020; Net et al., 2002;
Srivastava et al., 1998). Fig. 4(a) presents a cartographic representation
of the global distribution of key clay minerals, including kaolinite, illite,
smectite, and vermiculite, with a particular emphasis on the abundant
reserves of kaolinite clay (Ito and Wagai, 2017). Fig. 4(b) provides a
quantitative analysis of global kaolinite clay mining, segmented by re­
gion. Notably, India leads in this sector, accounting for 16.9 % of
worldwide production, followed sequentially by China, Uzbekistan, and
the United States by 14.2 %, 12.2 %, and 9.1 %, respectively. These
clays, comprising silicon and aluminum oxides, constitute about ¾th
portion of the crust and are abundant near the earth’s surface (Fig. 5)
(Fernandez et al., 2011; Momma and Izumi, 2011; Tan and Chi-Lung,
2009). Such clays result from the weathering process of diverse rock
types, making them widely accessible in various geological settings
(Scrivener et al., 2018a, 2018b; Snellings, 2016; Hazen et al., 2013).
Meanwhile, it is essential to note that in LC3, the required kaolinite
content is lower than for pure kaolinitic clay used in the ceramics and
paper industries. Therefore, it would not compete with the need for
resources from other industries. For instance, numerous low-grade clays
in India are considered waste and overburdened in existing quarries
(Joseph and Krishnan, 2014). By leveraging these ‘waste’ resources, the
LC3 system not only avoids opening new quarries but also does not
impinge upon valuable agricultural lands. Therefore, the LC3 approach
could potentially align with policies aimed at preserving farmland, as it
uses materials that are already disregarded and do not compete with
agricultural needs. Besides, such clays need low calcination tempera­
tures to activate their pozzolanic reactivity compared to clinkers,
significantly reducing the potential carbon footprint.
Further, the cement plants always have ample access to LSP, a con­
ventional raw material for cement manufacturing. LSP concentration is
usually around 15 % in LC3 blends, but other materials not suitable for
clinker production can be incorporated into the blend. For instance,
Fig. 4. Global distribution and extraction of kaolinite clay, a) distribution (Ito and Wagai, 2017); b) extraction (Michele, 2022).
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Science of the Total Environment 907 (2024) 167794
periclase is produced during clinker production when a limestone
enriched in high dolomite content is used, resulting in expansion,
considered a low-quality overburden and undesirable material. Whereas
in LC3 cement, such limestone with high dolomite content can be suc­
cessfully used (John et al., 2018). In this way, limestone quarries can be
used more efficiently, as these materials can be employed safely in un­
derground applications (Scrivener, 2014). With the same limestone
reserve, the amount of cement produced can be doubled under similar
conditions. Moreover, factors such as reduced transportation, no calci­
nation energy, and usage of low-grade limestone significantly support
the sustainable use of LSP as an SCM in clinker replacement.
3. Micro-mechanism
The hydration reaction mechanism involved in traditional Ordinary
Portland Cement (OPC) is well understood (Bhatty et al., 1986; Dodson,
1990). Whereas, in the LC3 system, the presence of SCMs (i.e., CC/MK,
LSP, and GY) could considerably alter the extent and nature of the re­
action and hydration products. Under this section, a comprehensive
discussion of the hydration chemistry of LC3, along with the individual
roles of SCMs, was carried out. For contextual understanding and
comparison, a brief overview of OPC hydration chemistry is also
presented.
3.1. Hydration chemistry of LC3
In the realm of cement production, prior to the emergence of LC3,
various studies delved into the individual merits of CC/MK and LSP as
influential components. CC/MK, renowned for its remarkable reactivity
as a pozzolanic material, garnered attention in notable works (Fernan­
dez et al., 2011; Souza and Dal Molin, 2005). Similarly, the utilization of
LSP as a filler material in cement production was explored by different
researchers (Dunster et al., 1993; Poon et al., 2001; Bonavetti et al.,
2001; Kakali et al., 2000). Building upon these individual investigations,
Antoni et al. (2012a, 2012b) embarked on a pioneering endeavor,
combining the synergistic effects of CC/MK and LSP to achieve a sub­
stantial clinker replacement of ~50 % in cement production. The
groundbreaking composition comprised 50 % clinker, 30 % CC/MK, 15
% LSP, and 5 % gypsum (GY). The subsequent sub-sections unravel the
intricacies of these SCMs, exploring their distinct roles and profound
impacts on the global of cement production.
3.1.1. Role of CC/MK
In LC3 systems, CC/MK plays a vital role as a readily available and
N. Ijaz et al. Science of the Total Environment 907 (2024) 167794

Fig. 5. Structure and optimal formulas a) kaolinite; b) illite; c) montmorillonite (Fernandez et al., 2011).

pozzolanic SCM for replacing clinker. Its reactivity and hydration 2018b; K. L. Scrivener, 2014). However, higher calcination tempera­
chemistry in the LC3 system are influenced by factors such as kaolinite tures beyond 900 ◦ C adversely affect the pozzolanic reactivity attributed
content and calcination temperature. CC/MK integrates chemically with to sintering and recrystallization into cristobalite, spinel, and mullite
hydration byproducts and contributes to both chemical and physical (Alujas et al., 2015a; Alujas et al., 2015b). Fig. 6 presents the effect of
integration. This section presents a comprehensive analysis of CC/MK’s different calcination temperatures on the XRD pattern of CC/MK. The
pozzolanic reactivity and hydration chemistry in the LC3 system, calcination results in dehydroxylation, which induces the formation of
considering a diverse range of factors. penta-coordinated aluminum ions responsible for CC/MK reactivity
(Coleman and Mcwhinnie, 2000; Fernandez et al., 2011). The chemical
a) Kaolinite grade (KAG) and Thermal Activation of CC/MK composition of CC/MK from different regions and sources by mass (%) is
tabulated in Table 1.
In the LC3 system, the KAG and protocols for thermal activation of Besides, some CC/MK exhibits a reddish color on cooling, resulting
pozzolanic reactivity of kaolinite clay are critically important to un­ from the oxidation of iron into hematite (Fe2O3). However, studies
derstand before discussing its role as a physical and chemical integrator. reveal no change in pozzolanic reactivity despite oxidation (Zunino
In this regard, numerous studies on CC/MK reactivity regarding clay Sommariva, 2020). Further, coloring can be managed by controlling the
feed purity and processing parameters have been documented in the atmosphere, and such techniques are quite renowned in the brick in­
literature (Khatib and Clay, 2004; Lagier and Kurtis, 2007; Martirena, dustry. Moreover, grinding of clinkers and SCMs together could lead to
2017; Wild et al., 1996). The clay feed from different sources comprised bimodal grain size distribution owing to the softer nature of SCMs,
different percentages of kaolinite content (KAC), which defines the KAG which might lead to the high fineness of CC/MK and LSP, while the
responsible for sufficient pozzolanic reactivity, while in natural depo­ clinker stays coarser (Krishnan and Bishnoi, 2018; Pérez et al., 2018).
sition, clay also contains other clay minerals (i.e., montmorillonite and
illite) as impurities, which could act as a diluent (Fernandez et al., 2011;
Kostuch et al., 2000) (Fig. 4). Whereas thermal activation of several clay
minerals are known to cause partial or complete breakdown of the
crystal lattice structure, resulting in the formation of high reactivity
anhydrous solid termed CC/MK (Alujas et al., 2015a, 2015b; Fernandez
Lopez, 2009). Studies reveal that among different clays, kaolinite clays
with a 1:1 layered structure of alumina and silica bonded with hydrogen
and Vanderwall forces tend to offer a more porous structure, leading to
serving as an effective filler and potentially easing the reaction and
resulting in a denser and stronger cement. Besides, the hydroxyl group
tends to enhance the chemical bonding with cement components, i.e.,
Ca2+, which aids in water retention for better hydration and improves
adhesion with aggregates (Khalifa et al., 2020; Wu et al., 2021). Whereas
illite and montmorillonite clays have a 2:1 structure and exhibit limited
reactivity owing to the aluminum groups trapped between silicate
layers, making them less likely to react with the alkaline environment
created by the cement (Fernandez et al., 2011). Further, different studies
reported that the dehydroxylation of clay feed with low-grade kaolinite
content of approximately 40 % at a low calcination temperature of
around 700-850 ◦ C (Eq. (5)) is sufficient to induce comparable strength
Fig. 6. The effect of calcination temperature on the XRD pattern of kaolinite
compared to OPC (Cao et al., 2021; John et al., 2018; Scrivener et al.,
clay (Alujas et al., 2015a, 2015b).

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Table 1
Composition of CC/MK in different regions of the world.
Calcined clay 1 2 3 4 5 6 7

Origin North America South Asia South-East Asia South America

Calcination Flash Furnace Furnace Furnace Furnace Flash Furnace

XRF composition
SiO2 52 54.7 51.8 58.4 44.9 50.3 67.6
Al2O3 43.8 42.4 17.5 32.3 42.7 22.6
Fe2O3 0.3 13.6 1.9 8.9 15.4 0.6 6.1
CaO – 0.3 0.1 0.6 1.3 – 0.5
MgO – 1 0.1 0.8 0.8 – –
SO3 0.1 – – – – – –
Na2O 0.3 – 0.1 – 0.4 – –
K2O 0.1 0.4 0.1 2.3 0.2 0.1 0.3
TiO2 1.5 1.1 2.4 0.8 2.4 1.8 1.5
P2O3 0.2 – 0.1 0.1 0.4 0.1 –
MnO – – – 0.1 0.4 – –
Others 0.1 – 0.2 0.2 0.2 0.2 –
LOI 1.5 1.9 1 0.5 1.7 3.6 1.4
Calcined kaolinite content (%) 95 38.9 79.4 17 50.3 66.2 35
BET-specific surface (m2/g) 9.6 23.1 15.3 18.7 25.7 12.9 18.5
Dℽ50 (μm) 5.1 8.5 5.3 5.9 10.9 4 23.5

The less efficient inter-grinding of cement has also been attributed to a
layering of the grinding medium with particles of fine powders, such as
CC/MK, during the grinding process (Katsioti et al., 2009; Sohoni et al.,
1991). In this regard, alkanolamine-based grinding aids such as dieth­
ylisopropanolamine (DEIPA), triiso-propanolamine (TIPA), and trie­
thanolamine (TEA) demonstrated to be efficient in improving the
hydration of ferrite and aluminate phases during LC3 inter-grinding
(Zunino and Scrivener, 2021a). Moreover, the grinding aids increase
the fineness and compressive strength for a given specific energy con­
sumption of the grinding mill (Assaad and Issa, 2014; Katsioti et al.,
2009).
b) Physical Integration
Physical integration of CC/MK refers to its effects as a filler material
that happens instantaneously. Besides, the physical impact of CC/MK
also influences clinker hydration (De la Varga et al., 2018; De Weerdt
et al., 2011; Lothenbach et al., 2011; Zunino and Lopez, 2016, 2017).
Compared to conventional cementitious systems, these physical effects
cause clinker to hydrate more quickly (Bentz et al., 2017; Zunino and
Scrivener, 2019). The physical integration can lead to three major
contributions to the LC3 system:
• Nucleation site provision: CC/MK played a pivotal role in enhancing
the hydration reaction and subsequently improving the mechanical
and durability characteristics of the LC3 system. CC/MK is an
amorphous thermally activated aluminosilicate that provides a high
specific surface area for potential hydration reactions (Dhandapani
et al., 2018; Hanpongpun, 2019; Tchakouté et al., 2020). The
physical interaction between CC/MK in the LC3 system is primarily
associated with the nucleation site provision, which acts as “anchors”
for generating hydration products (Hameed et al., 2020). These
nucleation sites refer to appropriate locations on the surfaces of CC/
MK particles where the preliminary phases of CSH and other hy­
dration products can emerge more readily than on the crystalline
surfaces of typical Portland cement particles. Therefore, CC/MK’s
highly reactive surface can easily interact with Ca2+ ions generated
during the early stages of clinker hydration (Zunino and Scrivener,
2019). This effectively initiates the development of CSH/CASH
phases, resulting in faster hydration kinetics. Thereby, CC/MK effi­
ciently improves the usage of LSP, which is otherwise a weakness in
many alternative cementitious systems. Moreover, it is critical to
emphasize the synergistic benefits of CC/MK when combined with
LSP in the LC3 system. The CC/MK not only speeds up the hydration
processes but also allows for better usage of CC/MK and LSP com­
ponents, which may have somewhat slower reaction kinetics than
OPC (Zunino and Scrivener, 2022a). This further has a broader
impact on various properties ranging from better strength growth,
decreased permeability, and increased resilience to chemical attack.
• Modified water to cement ratio: secondly, CC/MK particles exhibit a
slower reactivity compared to the highly reactive clinker phases
(Juenger et al., 2019). When CC/MK replaces clinker in cement, it
increases the water-to-cement ratio while maintaining a constant
water-to-binder ratio (Zunino and Scrivener, 2021b). This is due to
its fine particle morphology and high specific surface area, which
substantially elevates the particle packing density of the cement
matrix, thereby effectively reducing interstitial void spaces. More­
over, this fine-tuned microstructural optimization allows for an
elevated water-to-cement ratio without compromising the work­
ability of the mix (Berodier and Scrivener, 2014b). Furthermore, the
inherent pozzolanic characteristics of CC/MK actively participate in
chemical interactions with Ca(OH)₂, a by-product generated during
the hydration of C3S and C2S in the cement matrix (Zunino and
Scrivener, 2019). These interactions result in the formation of sup­
plementary CSH/CASH phases. The formation of these additional
phases necessitates a higher consumption of water, thereby not only
enhancing the mechanical properties of the composite but also
introducing the potential for a dynamically self-adjusting water-to-
cement (w/c) ratio throughout the curing process. In addition, CC/
MK addition subsequently impacts the rheological properties of the
LC3 system, depending on the fineness, particle shape, and specific
surface area, which requires w/c ratio adjustment to maintain a
consistent level of workability. Besides, the synergy of CC/MK with
other LC3 components, i.e., clinker, LSP, and GY, might induce a
reduction in porosity, thereby changing the water absorption rate
and influencing the overall LC3 w/c ratio. A better understanding of
the complex integeration of CC/MK in LC3 system permits better
control over w/c ratio which subsequently enable to optimize the
performance parameters in terms of compressive strength and
durability.
• Particle packing and shearing: this concept is particularly of more
significance owing to the presence of CC/MK as a prime ingredient in
the LC3 system, which has subsequently multiple implications taken
into account rheology, mechanical behavior, and long-term dura­
bility characteristics (Canbek et al., 2022b). Owing to its fine nature,
CC/MK particles fit effectively in the interstitial spaces between the
bigger cement particles and aggregates (Chen et al., 2023). This
produces a denser, more compact particle arrangement, regarded as

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N. Ijaz et al. Science of the Total Environment 907 (2024) 167794

“improved particle packing.” This results in a reduction in the overall
porosity due to better packing, which subsequently improves the
concrete strength and endurance, and resistance to chemical attacks
like chloride and sulphates (Sui et al., 2019). Moreover, the fine CC/
MK particles tend to contribute to shear-induced alignment during
mixing, which results in better orientation of other composites, such
as layered silicate, which subsequently improves the mechanical
behavior and resistance to cracking (Bright Singh and Murugan,
2022). The CC/MK’s particle size, shape, and specific surface area
have an impact on the shearing behavior, which subsequently in­
fluences the rheological properties, i.e., plastic viscosity, yield stress,
etc. Besides, CC/MK works in a synergistic way with other LC3
components when integrated with LSP and further enhances the LC3
properties. Its effects on particle packing and shear behavior
contribute to optimizing the overall performance of the LC3 mix.
c) Chemical integration
The role of CC/MK in the LC3 system is multifaceted, taking into
account CC/MK reactivity, influence on hydration products, the inter­
play of CC/MK with C3S and C2S in clinker composition and phase
assemblage modification, which contributes toward the overall perfor­
mance and behavior of LC3 system.
• CC/MK reactivity: the fundamental reactive elements in CC/MK
typically consist of silica and alumina, which exhibit varying degrees
of dissolution in an alkaline milieu depending on the clay’s type,
structure, and additional constituents. The pozzolanic characteristics
of CC/MK define the chemical integration, which can be succinctly
explained by its reaction with a saturated solution of portlandite (Ca
(OH)2) derived from the hydration of cement (i.e., C3S and C2S)
(Table 2) that defines the main idea of LC3 (Wilson et al., 2018). This
chemical interaction yields the formation of key hydrate phases,
including an aluminum-substituted calcium silicate (C(A)SH) phase,
strätlingite (C2ASH8), and calcium aluminate hydrate phases of the
AFm type (C4AH13) that enhanced the strength parameters and
significantly reduce the porosity through space-filling thereby
influencing the phase assemblage (Table 2) (Antoni et al., 2012a,
2012b; Avet and Scrivener, 2018b; Silva and Glasser, 2015).
• Influence of hydration products: the integration of alumina from CC/
MK into CSH product formed during the hydration reaction and has a
more complex structure owing to different dissolution rates of SCMs,
KAC, and heat flows (L’Hôpital et al., 2015, 2016; Avet et al., 2019a,
2019b; Mishra et al., 2019). The study reveals the fibrillar structure
for the C(A)SH phase with no notable variation in solid (~2.8) and
bulk (~1.8) densities in ternary systems comprising CC/MK and LSP
(Avet et al., 2019a, 2019b). The remainder of the alumina interacts
with the carbonate phases to generate carbo-aluminate phases
through a synergetic reaction in the presence of LSP and GY in the
LC3 system (Antoni et al., 2012a, 2012b). Following that, the pres­
ence of additional aluminates (i.e., from CC/MK) in the pore-solution
causes the production of carbo-aluminate phases, which restrict

Table 2
Holistic overview of hydration chemistry involves possible reactions and physical integration of OPC and LC3 system.
Type Ingredients Hydration chemistry Physical integration Remarks

Chemical reactions Hydration product

OPC 1) Clinker (95 %) 1) Dissolution The physical integration in OPC

a) Tricalcium silicate C3S + 6H2O → C3S2H3 + 3Ca(OH)2 CSH and CH system is limited in comparison to
(C3S) LC3.
b) Dicalcium silicate C2S + 4H2O → C3S2H3 + Ca(OH)2 CSH and CH 2) Nucleation and crystal
(C2S) growth
c) Tricalcium C3A + 6H2O → C3AH6 CAH
aluminate (C3A)
d) Tetracalcium C4AF + 7H2O → C4(A,F)H13 AFm and AFt phases
aluminoferrite
(C4AF).
2) Gypsum (5 %) C3A + 3C$ + 26H2O → C6AS3H32 Ettringite 3) Hardening and
Calcium sulphate C6AS3H32 + 2C3A + 4H → 3C4ASH12 (in Monosulfate microstructure development
dihydrate the absence of sulfate ion provided by
(CaSO4⋅2H2O) gypsum)
LC3 1) Clinker (50 %) Calcined clay 1) Mococarbonate instead of
a) Tricalcium Silicate C3S + 6H2O → C3S2H3 + 3Ca(OH)2 CSH and CH 1) Nucleation site provision monosulphate is produced as AFm
(C3S) 2) modified water to cement phase, which provides enough
b) Dicalcium silicate C2S + 4H2O → C3S2H3 + Ca(OH)2 CSH and CH ratio 3) particle packing and sulphate to preserve the Ettringite.
(C2S) shearing
c) Tricalcium C3A + 6H2O → C3AH6 (further react Ettringite
aluminate (C3A) with C$) C3A + 3CaSO4⋅2H2O + 26H →
C6A$3H32
d) Tetracalcium C4AF + 4CH + 14H → C4(A,F)H13
aluminoferrite (further react with GY and LSP)
(C4AF).
2) Gypsum (5 %) Synergy C4AF + 4CH + C$ + 2Cc + Ferrite-rich Limestone powder
Calcium sulphate 12H → C4(A,F)cH13 monocarbonate phase 1) Dilution effect. 2) The physical integration in the
dihydrate (C$) LC3 system is much more
3) Calcined clay (30 %) AS2 + 3.1CH + 4.6H → C-(A)-S-H, Strätlingite, 2) Reduction in inter-particle significant owing to distinctive
Metakaolin (AS2) C1.5A0.1SH4 + C2ASH8 + Calcium Aluminate capillary space. compositions and functionalities.
0.9C4AH13 Hydrate phase of AFm
type
4) Limestone powder AS2 + 5.4CH + 0.4Cc + Monocarbonate or 3) Shearing action.
(30 %) 1.2C$ + 20H → hemicarbonate as AFm
2C1.5A0.1SH4 + phases
0.4C4AcH12 + 0.4C6A
$3H32
Calcium carbonate (Cc) C3A + 0.5 Cc + 0.5CH +
0.5C$ + 11.5H →
C4Ac0.5H12

7
N. Ijaz et al.
ettringite conversion to mono-sulfate (Ms) (V. L. Bonavetti et al.,
2001; Dhandapani and Santhanam, 2017; Matschei et al., 2007a).
Moreover, the carbo-aluminates claimed to be more stable phases
over a broad range of relative humidity (10–90 %). Besides, the
structural dehydration in the C(A)SH and strätlingite phase is
consistent with a decline in relative humidity. In comparison,
strätlingite is controlled by the quantity of reactive alumina required
to produce an A/S ratio of 1 (Lothenbach et al., 2008). It is important
to note that strätlingite forms in pure metakaolin-portlandite systems
but not always in CC/MK blended cement due to its incompatibility
with portlandite. The presence of LSP suppresses strätlingite forma­
tion, favoring monocarbonate and hemicarbonate AFm phases
(Table 2). However, strätlingite appears in CC/MK blends at later
high hydration stages, even in the presence of Ca(OH)2, owing to the
local heterogeneities in the dense microstructure.
• Interplay of CC/MK with C3S and C2S in clinker composition: be­
sides, the concentration of C3S and C2S contents in the clinker
portion played a critical and decisive role. Moreover, it has also been
reported that the CC/MK reaction capacity in the LC3 system in­
creases linearly with C3S and C2S content (Avet et al., 2018; Krishnan
and Bishnoi, 2020). Further, the reactivity of CC/MK was found to be
increased as a function of time and KAG (Fig. 7) (Avet and Scrivener,
2018a, 2018b). Besides, some studies also reported a drop in CC/MK
reactivity at a higher aging period associated with the formation of
low CH content, along with low internal relative humidity in the LC3
system (Briki et al., 2021a, 2021b). This phenomenon is mainly
ascribed to the pore size, which plays a critical role in maintaining
the internal relative humidity in the LC3 system, while the increase
in pore size beyond a certain threshold (>13 nm) results in a
reduction in internal relative humidity which outcomes in reduced
pore solution in the capillary pores (Briki et al., 2021a). Therefore, at
a later age, enhancement of CC/MK reactivity is related to filling
capillaries with pore solution. Also, the findings indicate that both
hydrates’ development appears to slow down below a pore radius
range of between 3 and 5 nm (Briki et al., 2021a, 2021b).
• Influence on phase assemblage: in the LC3 system, CC/MK modifies
the phase assemblage and alters the mechanical and durability pa­
rameters. CC/MK enhances the development of CSH/C(A)SH for­
mation, the binding phase that controls strength and durability.
Moreover, CC/MK also results in the intricate formation of carbonate
aluminate phases by interacting with LSP-driven carbonate in a
synergetic manner, offering the potential for a more durable and
adaptable phase assemblage (Avet and Scrivener, 2018a, 2018b;
Fig. 7. Percentage of reacted CC/MK as a function of a) time and b) calcined KAC (Avet and Scrivener, 2018a).
8
Science of the Total Environment 907 (2024) 167794
Dhandapani et al., 2018). Besides, the grade of CC/MK is also critical,
considering the phase assemblage and porosity. Higher KAC in LC3
curtails clinker hydration and boosts portlandite consumption.
Compared to the OPC system, carbo-aluminate hydrates are formed
instead of monosulphate. Studies showed that the ettringite levels
stay consistent, with the highest KAC blend producing the least
carboaluminate hydrate (Avet and Scrivener, 2018a, 2018b). Hy­
drate volumes for 50.3 % and 95.0 % KAC in LC3 blends are com­
parable, showcasing the use of low-grade CC/MK (Fig. 8). Beisdes,
the porosity LC3 blend with 95.0 % KAC shows significant pore
refinement compared to OPC, mirroring the refinement of the LC3
blend. In contrast, at 28 days, only the 50.3 % KAC blend exhibits
further refinement. Moreover, the peak refinement was also found in
the LC3 blend with 17.0 % KAC (Fig. 9).
3.1.2. Role of LSP
a) Physical integration
In the realm of binder systems, the physical integration of LSP en­
capsulates the impact of fillers, notably through the dilution effect, the
reduction in inter-particle capillary space, and shearing action, each
contributing to the overall performance and behavior of the LC3 system.
• Dilution effect: in the LC3 system, a part of LSP will undergo physical
integration by inducing a “dilution effect” that has manifold impli­
cations on several micro-macro properties. In general, the clinker
replacement with filler materials reduces the binder’s reactive
component and its hydration mechanism and mechanical charac­
teristics (Di Salvo Barsi et al., 2020; Kakali et al., 2000; Z. Shi et al.,
2016). However, the fine particulate size and elevated specific sur­
face area of LSP have been observed to positively influence early-
stage hydration, particularly when integrated within the diverse
compositional context of the LC3 system (Gupta et al., 2017). By
adjusting the water-to-binder ratio, this early hydration boost can
counteract the dilution effect in later stages (Briki et al., 2021a,
2021b). Also, LSP fillers increase the effective water-to-binder ratio,
improving the degree of clinker phase hydration despite the inherent
dilution effect. Moreover, the LSP incorporation leads to ease the
concrete placement by inducing better workability, low water de­
mand, and optimized particle packing. Additionally, LSP’s ability to
moderate the heat of hydration reduces the risk of thermal cracking
and expands the preliminary setting duration, providing logistical
advantages for construction scenarios (Oey et al., 2013; Puerta-Falla
N. Ijaz et al.
Fig. 8. Phase assemblage of hydration of OPC and LC3 with 17, 50.3, and 95 % of KAC in CC/Mk; a) 3 days; b) 28 days (Avet and Scrivener, 2018a, 2018b).
Fig. 9. MIP analysis of PC and LC3-50 blends with 17, 50.3, and 95 % of KAC in CC; a) 3 days; b) 28 days (Avet and Scrivener, 2018a, 2018b).
et al., 2015). The diluting effect further promotes a synergistic
conjunction with other cementitious elements, increasing their
reactivity and boosting the mechanical and durability of the finished
concrete. Overall, the introduction of LSP offers a rich benefit profile
that, when properly adjusted, may significantly enhance the effi­
ciency and sustainability of LC3 systems.
• Shearing action: apart from the dilution effect, the LSP as a filler
material in the LC3 system, also induced shearing action, which
tends to have intricate implications on the cement hydration kinetics
(Zunino Sommariva, 2020). The LSP-induced shearing force acti­
vates dormant reaction sites on the cement grains, considerably
enhancing the hydration kinetics (Berodier and Scrivener, 2014b).
This results in the forming of new surfaces that act as nucleation sites
for developing hydration products, enhancing the workability and
strength behavior at an early age (Kandagaddala et al., 2023).
Studies also showed the alteration of hydration kinetics by the in­
clusion of fine limestone or quartz similar to those observed with
different shearing rates, a behavior akin to the influence of varying
shear rates during mixing on pure cement systems (Berodier and
Scrivener, 2014b). Beyond the inherent characteristics of the filler,
such as hardness and particle size, shearing action has an influence
on the kinetics of hydration (Berodier and Scrivener, 2014b).
Notably, this shear-induced hydration kinetics acceleration may be
amplified by the surface morphology of LSP, its particle size distri­
bution, and the electrostatic and Vander Waals interactions resulting
from particle polarity. These shear-dependent interactions are
further modulated by the rheological characteristics of the LC3 sys­
tem, such as yield stress and plastic viscosity. Even the compatibility
with admixtures that may influence rheology, such as super­
plasticizers, can alter the shear-induced activation of cement grains
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Science of the Total Environment 907 (2024) 167794
in a synergistic manner (Kandagaddala et al., 2023; Muzenda et al.,
2020). The observed early-age performance advantages result from
the intricate interaction between the shear forces, produced surfaces
for nucleation, and faster hydration kinetics (de Matos et al., 2022;
Lin et al., 2022). When it comes to improving LC3 formulations,
early-age strength and workability are essential, particularly in ap­
plications that call for early strength development and superior fin­
ishing attributes.
• Particle packing: the filler effect of LSP in the LC3 system also has
implications in enhancing the particle packing effectiveness, which is
not only multi-faceted but also beneficial considering the overall
performance (Long et al., 2021a, 2021b; H. Sui et al., 2022).
Considering the fine nature of LSP particles, its inclusion in the LC3
system leads toward the optimization of the granular packing of the
binder matrix. Subsequently, the setting time and the early-age
mechanical characteristics of the LC3 system are immediately
impacted by this increase in packing density (Chen et al., 2016; Knop
et al., 2014; Lecomte et al., 2016; Marchetti et al., 2017; Sun et al.,
2017). The LSP’s particle size distribution, specific surface area, and
morphological traits are important technical factors that affect this
packing effect. Studies reveal that even a slight concentration of LC3
between 10 and 15 % results in observable improvements in packing
density. Similarly, other studies showed an increase in packing
density by approximately 11.6 % with an increase in LSP from 5 to
35 % (Knop and Peled, 2016), and is considered a low-cost filler
material (Barkat et al., 2019; Boel and De Schutter, 2006; Burroughs
et al., 2017; P. R. Da Silva and De Brito, 2015; Li et al., 2017; Salami
et al., 2014; Ye et al., 2007). This is especially helpful since limestone
grinds to a finer consistency during the grinding process than clinker
because it is naturally softer. Moreover, studies have shown that such
N. Ijaz et al.
fine grinding results in even greater particle packing, improving the
packing effectiveness of inter-ground binders, including LSP. Be­
sides, the inter-particle interactions, particularly in terms of surface
area and interaction sites, might be impacted by the high fineness of
grounded LSP (Zunino and Scrivener, 2020). This may lessen the
requirement for water and hence decrease the water-to-cement ratio
by improving the rheological characteristics of the LC3 system
(Muzenda et al., 2020). Additional advantages of such an enhanced
microstructure include increased durability and higher resistance to
microcracking. Furthermore, increasing packing density may be
significantly aided by the shape of the LSP particle. The cohesiveness
and structural integrity of the cement matrix may be improved by the
more effective interlocking of irregularly shaped particles. The dis­
tribution and shape of hydration products may be impacted by an
optimal packing structure, which can also have an impact on the LC3
system’s long-term mechanical performance and durability (Dhan­
dapani et al., 2018). Overall, a complex interaction of various pa­
rameters, including particle size, shape, and surface properties,
contributes to the particle packing efficiency of limestone powder in
LC3 systems.
b) Chemical integration
• Ca-rich surface induced nucleation of CSH: the addition of LSP in the
The chemical integration of LSP within the LC3 matrix encompasses
a complex range of mechanisms. This includes enhancement of the ki­
netics of the C3S reaction, the creation of nucleation sites for CSH pre­
cipitation, and its consequential implications on the composite phase
assemblage in the cementitious system. LSP dissolution releases car­
bonate ions, leading to ettringite preservation and carbo-aluminate
formation, resulting in a dense structure compared to OPC (Fig. 10).
These interactions, key to understanding LSP’s impact on phase
assemblage, are further examined to dissect their chemical
characteristics.
• Enhancing the kinetics of C3S reaction: in the LC3 system, the LSP
played a critical role in accelerating the kinetics of the C3S hydration
process, which is a significant predictor of early-age strength in
cementitious systems (Krishnan et al., 2019; Zunino Sommariva,
2020). LSP promotes this acceleration through a variety of sophis­
ticated ways. Initially, the calcite surfaces in LSP function as extra
nucleation sites for CSH gel, catalyzing its production and thereby
improving C3S hydration rates (Krishnan et al., 2019; Lin et al.,
2022). Second, LSP changes the pore solution chemistry by adding
carbonate ions, which interact with Ca2+ ions, improving the disso­
lution kinetics of C3S and speeding up the hydration process
(Krishnan et al., 2019). Studies reported that Ca2+ concentration
increases in OPC systems with 40 % LSP, escalating ionic activity
potential and driving precipitation (Berodier and Scrivener, 2014b).
Fig. 10. Microstructure of OPC and LC3 at 28 days; a) OPC; b) LC3 (Hay et al., 2022b).
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Science of the Total Environment 907 (2024) 167794
Third, LSP stabilizes additional hydration byproducts like ettringite
and carbo-aluminates, preventing them from converting to less sta­
ble phases and guaranteeing a steadier hydration rate throughout
time. This was further verified by calorimetric heat profiles corrob­
orating that the incorporation of LSP expedites the hydration kinetics
of C3S, notably abbreviating the dormancy phase relative to other
SCMs (Bentz et al., 2017; Krishnan et al., 2018b; Lothenbach et al.,
2008). Fourth, the increased ionic strength of the pore solution due
to carbonate ions increases ionic conductivity, enhancing ion trans­
port critical for C3S hydration (Ejbouh et al., 2023). Fifth, when LSP
is used in conjunction with SCMs such as CC/MK, a synergistic effect
occurs, increasing the reactivity of these SCMs and improving C3S
hydration kinetics (Krishnan et al., 2019; Zunino Sommariva, 2020).
Finally, the LSP acts as a pH buffer, keeping the environment alkaline
and allowing for continuous C3S dissolution and subsequent CSH
production (Scrivener et al., 2018a; Avet and Scrivener, 2020; Wil­
son et al., 2022). In essence, the chemical incorporation of LSP in LC3
systems accelerates C3S hydration through a complex interplay of
nucleation effects, pore chemistry modification, phase stabilization,
and synergistic interactions with SCMs, thereby improving both the
early-age mechanical properties and durability of LC3-based
cementitious systems.
LC3 system causes subtle but significant alterations in the nucleation
kinetics of CSH, which is an important phase in the overall hydration
process that contributes to cementitious strength. In the LC3 system,
LSP’s high specific surface creates localized regions wherein Ca2+
ions from the LSP adsorb preferentially (Puerta-Falla et al., 2016).
Due to the reduced Gibbs free energy (refers to thermodynamic po­
tential) for nucleation in these calcium-rich zones, this microenvi­
ronment serves as a “hotbed” for the nucleation of CSH (Skibsted and
Snellings, 2019; Zhao et al., 2023). Essentially, the localized increase
in Ca2+ ions concentration functions as a catalytic environment for
the CSH nucleation, expediting the phase’s formation kinetics.
Further, the complex interplay between pH, ionic strength, and zeta
potential also comes into focus. These characteristics are intrinsically
connected to the electrostatic stability of CSH particles in colloidal
solution. Carbonate ions in LSP may bind with metal ions (referred to
as cations) in the LC3 system, altering the zeta potential and, hence,
the stability and shape of CSH throughout its nucleation and devel­
opment phases (Hay and Celik, 2022; P. Hou et al., 2021; Sposito
et al., 2021). Further, the morphological studies indicate changes in
CSH d-spacing and crystallite dimensions, demonstrating the influ­
ence of LSP on the CSH structure (Hassannezhad et al., 2022; Hay
et al., 2022a; Berodier and Scrivener, 2014a). Besides, LSP addition
also impacts the thermodynamic solubility product (K_sp) of multiple
phases in the LC3 system. In other words, the K_sp value determines
the concentration of specific phases (such as CSH, carbo-aluminates,
N. Ijaz et al.
etc.) that will dissolve in the pore solution and the concentration that
will precipitate out and form the solid phases. Thus, LSP intrusion
alters the K_sp, which changes the phases and impacts the nucleation
and stability rate. Overall, the LSP presence in the LC3 system acts as
a chemical pivot that alters thermodynamic, local ionic environment,
and morphological characteristics and accelerates and stabilizes the
CSH nucleation, affecting early-age and long-term mechanical
performance.
• LSP-induced alterations in phase assemblage: the chemical integra­
tion of LSP in the LC3 system is critical in regulating the phase
assemblage of the hydration product. Carbonate ions from the LSP
combine with accessible aluminates (i.e., from CC/MK) in the sys­
tem, exhibit enhanced reactivity, and interact in two distinct ways, i.
e., carboaluminate hydration phases and ettringite stabilization in
assemblage phases (V. L. Bonavetti et al., 2001; Kakali et al., 2000;
Machner et al., 2018b). These phases add to the compositional va­
riety and alter the mechanical and rheological properties of the LC3
system. Based on the amount of carbonate, two forms of carbo-
aluminates could form, i.e., hemicarbo-aluminate (Hc) and mono-
carbo-aluminate (Mc) with half and one molecule of the carbonate
ion, respectively (Table 2) (Avet and Scrivener, 2018b). However, it
is often found that Hc leads to the formation of Mc, and the direct
formation of Mc is not frequently recorded. Besides, the stoichio­
metric calculations showed that ettringite and carbo-aluminates
phases have comparable effects and reduce porosity (Avet, 2017).
Moreover, it was also revealed that the Hc and Mc formation reached
its maximum in a 50 % CC/MK system. This implies that the pro­
duction of Hc and Mc does not need an excess of Al3+ ions. Several
documented studies on the ternary blend of LSP and CC/MK have
reported similar effects as that of pure CC/MK preferentially to form
CASH rather than CO3-AFm. As a result, low-grade clays could pro­
vide an alternative mean of CC/MK and further require investigation.
Furthermore, these carbo-aluminate phases are greatly influenced by
several factors, including LSP’s particle size distribution, purity, and
reactive aluminate concentration (from CC/MK) (Krishnan et al.,
2019; Shah et al., 2022; Zunino and Scrivener, 2021b). The type and
concentration of carbo-aluminate phases are influenced by the
equilibrium between carbonate ions derived from the LSP and alu­
minates from CC/MK. The factors above have significant conse­
quences on the hydration kinetics, the microstructural development,
and the final mechanical characteristics of the LC3 binder system
(Sharma et al., 2021b). In addition, it was also found that the heat
flow for the alite reaction is similar in both LC3 and OPC, whereas
the secondary aluminate peak is more pronounced in LC3 owing to
the higher absorption of sulfate in CSH during the alite peak.
Whereas the third peak refers to AFm (i.e., Hc and Mc) phases is more
pronounced in LC3, which ensures the synergetic reaction of CC/MK
and LSP (Zunino Sommariva, 2020) (Fig. 11). In general, in the
typical recipe of an LC3 system, these AFm phases in combination
occupy up to 25 % of hydrated cement paste volume. Regardless of
the lower clinker content, CASH continues to make up around 50 %
of the paste volume (Fig. 8) (Avet, 2017; Krishnan, 2019; Krishnan
and Bishnoi, 2020).
c) Type and grade of LSP
In the LC3 system, low-grade LSP played a critical role, taking into
account the granularity and chemical composition. Overall, LSP played a
dual role, considering its chemical and physical integration. A part of
LSP actively participates in the development of complicated carbo-
aluminate hydrate phases through chemical integration. These phases
subsequently improve the cement matrix’s microstructural integrity and
long-term durability. Such chemical integration involves intricate ion
exchange and crystalline transformation, which tends to stabilize the
carbo-aluminate phases (Andrés et al., 2015).
Meanwhile, a significant amount of LSP is still chemically inert and is
11
Science of the Total Environment 907 (2024) 167794
Fig. 11. Comparison of heat profile of LC3 and OPC (Zunino Sommar­
iva, 2020).
used as a micro-filler. This inert property is not only passive; it actively
contributes to the microstructure’s densification, increasing mechanical
strength and decreasing permeability. The use of lower-purity limestone
and even industrial by-products is made possible by LSP’s dual func­
tionality, which allows it to serve as both a reactive and a filler
component (Krishnan et al., 2018a, 2018b). This expands the range of
raw materials that may be included in the LC3 system. Other carbonate-
rich materials, such as dolomite and marble dust, have also shown
comparable reactivity profiles in addition to standard calcite-based LSP.
Despite having different kinetics, they all work together to create and
stabilize ettringite, which is necessary for both early-age strength and
long-term durability. The ramifications of these variances in kinetic
profiles on hydration chemistry, setting times, and final mechanical
performance call for a sophisticated understanding (Krishnan and
Bishnoi, 2018; Machner et al., 2018b; Matschei et al., 2007b; J. Xu et al.,
2019; Zajac et al., 2018a).
3.1.3. Role of gypsum (GY)
GY played a pivotal role in the hydration chemistry of LC3, similar to
OPC. The incorporation of GY leads to two important observations.
Firstly, adding GY influences the hydration process of C3A and C3S,
causing the calorimetric peak associated with aluminate to occur after
the peak associated with silicate. The temporal segregation allows for an
uninterrupted period of initial hydration for C3S, accelerating its role in
early-stage strength development (Hay et al., 2022b; Zunino and
Scrivener, 2022b). Secondly, the presence of sulfate ions derived from
GY plays a crucial role in promoting the abundant development of
ettringite (termed as AFt) (Luan et al., 2023). The importance of this
cannot be overstated, as it not only contributes to the initial increase in
strength but also enhances the microstructural density of the cement,
hence improving its durability properties. Meanwhile, filler action
induced supplementary sulfate to be adsorbed on CSH phases, increasing
sulfate requirement in all types of bulk volume replacement binders
(Zunino and Scrivener, 2019). Mishra et al. (2019) reported that the
adsorption of sulfate by CSH/CASH in the LC3 system affects the con­
centration of aluminate accessible for the formation of the carbo-
aluminate phase, particularly at high temperatures. A similar observa­
tion was also documented in other types of cement, i.e., the adsorption
of sulfate by CSH. Besides, owing to the formation of the Hc phase
initially subjected to the considerably slower dissolution of the car­
bonates, its conversion into Mc is preferred thermodynamically in the
long term (Damidot and Glasser, 2015; Krishnan et al., 2019). Therefore,
N. Ijaz et al.
early reactive aluminates in some SCMs would demand careful GY
content selection to separate the aluminate peak from the silicate re­
action (Antoni et al., 2012a, 2012b; Adu-Amankwah et al., 2018; Zajac
et al., 2018b; Zunino and Scrivener, 2019). Besides, elevated quantities
of GY have the potential to undermine the resilience to sulfate attack,
particularly in situations with high sulfate concentrations. The impact of
GY also encompasses thermal stability since it induces modifications in
phase stability at varying temperatures. Ultimately, the impact of GY on
the pore structure may lead to reduced permeability, hence providing
more protection against harmful compounds.
3.2. Hydration chemistry of OPC
In comparison to LC3, the hydration process of OPC begins with the
physical integration, first initiated by the dissolution of key constituents
- tricalcium silicate (C3S), dicalcium silicate (C2S), tricalcium aluminate
(C3A), tetracalcium aluminoferrite (C4AF), and gypsum (CaSO4.2H2O)
in water. This dissolution liberates crucial ions that nucleate to form the
initial structure of emerging solid phases, thus catalyzing crystal growth.
These crystals interlock and harden over time, culminating in a complex
microstructure that fills capillary pores, bolstering the material’s
strength and durability. Alongside the physical integration, chemical
interactions are concurrently taking place. Hydration reactions among
the chief constituents lead to the formation of semi-amorphous or
amorphous crystalline cement hydration products, such as calcium sil­
icate hydrate (CSH) and calcium hydroxide (Ca(OH)2) (Constantinides
et al., 2003; Jennings, 2000, 2008; Jennings et al., 2007; Petersen and
Ulm, 2017). In particular, C3S plays a vital role in early structure
development, as well as in the creation of aluminum hydrates. A note­
worthy product of chemical integration is ettringite (C6AS3H32) (Talero,
1996), formed from the interaction of C3A and gypsum (GY). Ettringite
eventually transitions into mono-sulfate (C4ASH12) as GY is depleted.
Thus, the OPC hydration process is underpinned by a simultaneous
interplay of both physical changes and chemical reactions, resulting in
an integrated system that holistically combines the material’s physical
attributes and chemical nature. It is pertinent to mention here this study
used the term OPC, which is identical to CEM I type cement under Eu­
ropean EN 197–1, as both kinds are 95 % clinker and, exhibiting closely
analogous hydration chemistry with minor compositional differences,
which is regarded as inconsequential for this analysis and comparison
with LC3. Table 2 provides a holistic overview of these major physical
and chemical integrations occurring in the OPC system is presented in
Table 2.
3.3. Salts and carbonation effect on LC3
The concrete structures could lead to deterioration and degradation
when exposed to different salt solutions such as chloride, sulfates, and
alkalis. For instance, an alkali-silica reaction could lead to the formation
of expansion gel, which induces cracking within the concrete structure,
and a subsequent sulfate ion intrusion might lead to major deterioration
(Lee et al., 2018). Besides, carbonation is another important factor that
could have a detrimental effect on the integrity of the structure.
Therefore, it is critically imperative to analyze these parameters (such as
chloride, sulfate, alkali content, and carbonation) in the formulation of
the LC3 system, considering the long-term durability. Different studies
evaluate the durability properties of the LC3 system considering chlo­
ride, sulfate, alkali, and carbonation resistance (Shi et al., 2017; Mar­
aghechi et al., 2018; Krishnan et al., 2021). This section is focused on the
effect of such salts on the micro-mechanism, i.e., chemical hydration of
LC3, and the corresponding impact on the formation of mineralogical
products responsible for macro response, i.e., strength development.
3.3.1. Alkali-silica reaction
Alkali silica reaction (ASR) is a complex phenomenon that causes the
formation of ASR gel induced by the reaction of pore fluid hydroxyl ion
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with reactive silica from aggregate. The hydrophilic nature of ASR gel
absorbs more water, causing expansion and cracking in the concrete
matrix (Guo et al., 2019; X. Hou et al., 2004, 2005; T. Kim and Olek,
2014). Besides, the type and concentration of alkali content (such as
KOH and NaOH) have a significant impact on early days strength (i.e.,
an increasing trend was observed due to accelerated reaction of silica
and alumina phase), whereas at higher alkali content (i.e., >1 % by
mass) there is a significant reduction in later age strength (Hanpongpun,
2019). The inclusion of SCMs have found to have a positive impact in
curtailing the ASR gel expansion that falls under three ways: 1) dilution
of Portland cement reduces alkali content in concrete; 2) production of
densifying paste matrix that decelerates ions’ migration in ASR; 3)
limiting the dissolution of silica in aggregates (Aquino et al., 2001;
Nguyen et al., 2020b; Nguyen et al., 2020c; Rajabipour et al., 2015;
Scrivener et al., 2018a; Turk et al., 2017). It was reported that the CC/
MK releases alumina into the pore solution, which inhibits the dissolu­
tion of reactive silicate minerals (Chappex and Scrivener, 2013). A study
reported a 50–60 % reduction in ASR expansion compared to the OPC
system upon the inclusion of highly reactive CC/MK and silica fume
(Aquino et al., 2001). Whereas the incorporation of LSP and fly ash also
reported a reducing trend in ASR expansion (Turk et al., 2017). Also, it
was revealed that in the LC3 model reactant system, the presence of
supplementary calcium-rich phases appears to inhibit ASR gel formation
or to create high Ca/Si ASR products, relatively stiff CSH, and CASH
with reduced expanding capacity (Nguyen et al., 2020c). Also, a study
evaluated the LC3–65 (refers to 65 % replacement of clinkers with
SCMs) and LC3–50 having CC/MK percentage of 50 % and high-reactive
aggregate; after 28 days of curing under moist conditions were subjected
to soaking at 38 ◦ C under 0.32 M solutions of NaOH, the LC3 system
reported negligible ASR expansion (Scrivener et al., 2018a; Zunino
Sommariva, 2020).
3.3.2. Sulfate resistance
The pozzolanic reactivity of SCMs played an integral role in miti­
gating the potential adverse effect of sulfate exposure (Boubekeur et al.,
2019; Favier and Scrivener, 2018; Schmidt et al., 2009; Z. Shi et al.,
2019). A study reported that binary and the ternary blend of CC/MK and
CC/MK + LSP considerably enhanced the sulfate resistance and, after
almost two years of exposure to sulfate attack, exhibited negligible
expansion of <0.05 % (Z. Shi et al., 2019). Besides, the individual effect
of LSP in a binary blend poses an adverse effect, i.e., it considerably
enhances the sulfate expansion at an early curing age (Z. Shi et al.,
2019). Moreover, it is also revealed that an external sulfate attack in the
LSP cement could lead to the formation of thaumasite (Sotiriadis and
MrózMr, 2018). However, the incorporation of SCMs, i.e., CC/MK, was
shown to be effective in suppressing thaumasite attacks (Skaropoulou
et al., 2013). Thus, CC/MK was found to be a major factor in countering
the sulfate attack, which is attributed to the lower concentration of C3A
due to OPC substitution and its pozzolanic nature, which results in the
formation of extra gel which fills the pores within the cement matrix
(Cao et al., 2021; Kirsanova and Kramar, 2015; M. Zhang et al., 2013). It
is also reported that the higher concentrations of sulfate in the pore
solution are also necessary for an LSP-SCM binder for the conversion of
carboaluminate into sulphoaluminate and subsequently ettringite,
which could further improve the potential for sulfate resistance (Z. Shi
et al., 2019). Moreover, the carbonates utilize the majority of the
available alumina and function as a supplementary buffer, whereas the
sulfate-related phases are constrained, prolonging the formation of
ettringite. Nonetheless, research reveals that Mc ultimately loses sta­
bility when exposed to sulfate and chloride; however, this impact has to
be elucidated further (V. L. Bonavetti et al., 2001).
3.3.3. Chloride resistance
SCMs played a critical role in enhancing the concrete’s resistance to
chloride penetration, thereby mitigating the detrimental effects of
chloride ingress. Different studies reported that the role of CC/MK is
N. Ijaz et al.
significant in providing chloride resistance, whereas the individual
impact of LSP in a binary blend permits chloride penetration with the
highest total chloride content (Nguyen et al., 2020a; Shi et al., 2017; Sui
et al., 2019). Besides, the optimal interaction of LSP with SCMs
increased chloride binding, reducing the time-dependent chloride
diffusion coefficient and improving service life estimates (Ipavec et al.,
2011). A study reported that the presence of CC/MK coupled with LSP
induced higher binder capacity in comparison to the binary substitution
of LSP (Machner et al., 2018a; Sui et al., 2019).
Moreover, compared to OPC, the chloride binding capacity is
enhanced by adding CC/MK either with or without LSP, whereas CaCl2
showed the strongest binding than NaCl (Shi et al., 2017). Further, it was
also documented that in certain pH environments, the efficacy of LSP is
limited, considering the improvement in binding capacity (Ipavec et al.,
2011).
The chloride penetrability behavior significantly depends on the
pore structure and binding capacity attributed to physical and chemical
effects (Ipavec et al., 2011). In the LC3 system, the AFm phases
considerably induced pore structure refinement, thus improving the
resistance to chloride ion ingress (Maraghechi et al., 2018; Shi et al.,
2017). The AFm phases tend to reduce the pore structure, reducing pore
size and capillary pore connectivity. In addition, the AFm phases are also
in synergy with other hydration products, like CASH/CSH resulting in a
more robust structure. Whereas taking into account the binding capac­
ity, the AFm phases exhibit affinity to the Clˉ ions, which further results
in improved durability and significantly reduces the Clˉ induced corro­
sion in steel reinforcement. This is attributed to the binding of the Clˉ
ions by AFm phases, which efficiently eliminates the Clˉ from the pore
solution and subsequently reduces its precipitation, which triggers the
corrosion process. A study compared the threshold for corrosion for
embedded steel and chloride ion diffusion of OPC and LC3 systems and
found that the LC3 system exhibits high resistivity against the ion
transport and ensures an extended service life period (Pillai et al., 2019).
The ternary mixes of CC/MK and LSP showed improved chloride pene­
trability, which was controlled by the pore network’s enhanced tortu­
osity (Mathieu Antoni, 2013; Dhandapani and Santhanam, 2020). Other
studies also reported that Mc becomes unstable and converted into
different forms of AFm under chloride exposure (Bonavetti et al., 2001;
Machner et al., 2018a). Overall, the quantitative evaluation of the LC3
system, considering the binding capacity, exhibits a significant reduc­
tion in Clˉ penetration depth compared to other traditional and binary
blends with fly ash, slag, CC/MK, and limestone combinations, owing to
the higher amount of AFm (Maraghechi et al., 2018; Z. Shi et al., 2017)
which is significantly beneficial in increasing the durability of the
Fig. 12. Role of binding capacity on the chloride penetration depth of various
cement blends (Sui et al., 2019).
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concrete structure (Fig. 12) (Sui et al., 2019).
3.3.4. Carbonation
It is generally recognized that blended cement concrete has a higher
carbonation rate than OPC concrete, and the same is true for LC3 con­
crete (Morandeau et al., 2015). Though SCMs inclusion could reduce the
carbonation depth (CD) and lessen the CO2 ingress, owing to lower
alkalinity in the pore solution resulting from CH consumption, end up
with the enhanced CD (Duan et al., 2013). So, the effect of SCMs on
carbonation kinetics would either enhance or delay, which ultimately
governs the CD (Bakera and Alexander, 2019). Besides other factors,
such as curing duration and exposure conditions, including temperature
and internal and external relative humidity, exposure cycles also played
a major role in carbonation performance. Different pertinent literature
reported an increase in CD with SCMs incorporation, which is linked
with CH consumption and alkalis content that regulates the pH (H. S.
Kim et al., 2007; Morandeau et al., 2015; Pacheco Torgal et al., 2012;
Saillio et al., 2015; San Nicolas et al., 2014). Besides the percentage
content of SCMs, the w/c ratio is also reported to have a strong effect on
the increase in CD (David Newlands, 2011; Jones, 2011; Meddah et al.,
2018). Generally, the CD increases with an increase in SCMs content.
However, at low CC/MK content (i.e., 10–15 % of CC/MK), some studies
reported a reduction or no notable determinantal effect on CD (Bakera
and Alexander, 2019; Barbhuiya et al., 2015; Vejmelková et al., 2010).
On the other hand, the carbonation of LSP cement composites revealed
that the Hc phase interacts with CO2 and acts as a carbonation sink for
converting to Mc. Similar to CASH phases, the carbo-aluminate phases
also do not bind alkalis, which could induce improvement in the alka­
linity reserve of the cement paste matric, though this premise needs
further evaluation (Shah and Bishnoi, 2018). Further, the synergetic
effect of CC/MK and LSP in the LC3 system was found to exhibits
comparatively higher CD compared to the OPC system considering 28
and 84 days of aging (Bahman-Zadeh et al., 2022).
4. Macro-mechanisms
4.1. Rheological properties of LC3
The rheology of a ternary mix of the LC3 system is quite complex and
requires considerable importance, as it has a substantial impact on its
practical application. In this regard, the key differences in the rheolog­
ical behavior between conventional OPC and new ternary LC3 are crit­
ically important to understand. The rheological properties are mainly
governed by interparticle forces resulting in non-Newtonian behavior
(Hatem et al., 2013; Houlsby, 1991). The concrete performance and
cementitious material efficacy are crucial and dependent on rheology.
Therefore, to achieve the required engineering properties such as con­
trol segregation, formwork, pump pressure, surface finish, etc., rheo­
logical properties should be properly balanced (Ferraris, 2017). Under
this section, a critical discussion on the rheological properties of LC3 and
its comparison to OPC has been carried out.
4.1.1. Workability and setting time
Workability and setting time (i.e., initial and final setting time)
depend upon several factors such as fineness, water-cement ratio, alkali
or salt content, atmospheric condition, GY content, etc., that also play a
critical role in strength development (Scanlon, 1994; Tattersall, 1976,
1991). CC/MK has a strong water absorption affinity. Clinker replace­
ment could considerably impair workability and delay the setting time
(Cao et al., 2021; Joseph and Krishnan, 2014; Paiva et al., 2012). Jiang
et al. (2015) reported a reduction in the fluidity of freshly prepared
mortar with the increase in OPC replacement with CC/MK content at a
given W/C ratio ascribed to irregular morphology and high specific area.
Some studies reported different setting time modifications for equiva­
lent clinker replacement with CC/MK or LSP (Cassagnabère et al.,
2013a, 2013b; Courard et al., 2003; Cao et al., 2021; Madandoust and
N. Ijaz et al.
Mousavi, 2012). For instance, the binary addition of LSP in the range of
10–35 % reduces the setting time (Di Salvo Barsi et al., 2020; Kakali
et al., 2000; Wang et al., 2021). Whereas beyond 35 % (i.e., at 45 %), an
increasing trend was observed. While at a similar percentage (i.e., at 45
%), the binary addition of CC/MK also exhibits an increasing trend;
however, the magnitude of increase in the case of CC/MK was found to
be much more pronounced compared to LSP. An overall increase of 26.6
% and 34.4 % in initial and final setting times was reported, considering
the combined effect of CC/MK and LSP in the standard LC3 recipe
compared to the OPC (Ez-zaki et al., 2021). Besides, it was found that
with the increase in fineness and use of higher quality CC/MK, the
setting time tends to be faster (Joseph and Krishnan, 2014; Scrivener
et al., 2018b). The reduction in setting time at low partial substitution
could be linked to the higher specific surface area (SSA) of CC/MK
content, which tends to absorb more water and lessen the free water
availability in the cement-clay matrix. Whereas for the latter, the in­
crease in setting time is associated with delayed pozzolanic reactivity
during the early age, which is linked with the hydration rate of clinkers
and subsequently delayed precipitation of portlandite and consequently
the setting time (Courard et al., 2003; Wild et al., 1996). Similarly,
Kawashima et al. (2012) reported that the addition of nano-clay (up to
1.5 % by mass of cement) particles facilitates the stiffening behavior of
freshly prepared cement paste. Such behavior is owed to the non-
availability of free water caused by flocculation between the particles
with no connection to the adsorption phenomena of nano clay particles.
Besides, the presence of additional GY content of 5 % in the LC3 system
is also an important influencing factor that affects the setting time
(Wang et al., 2021). However, the reduction in workability owing to
higher clinker replacement was identified as an adverse characteristic
(Ferreiro et al., 2017; Muzenda et al., 2020).
4.1.2. Yield stresses, thixotropy, and plastic viscosity
In essence, fresh cementitious materials exhibit yield stresses (static
and dynamic), plastic viscosity, and thixotropy, which pertain to flow­
ability, internal resistance, and time-dependent microstructural recov­
ery when the stress is removed (Beigh et al., 2020; Y. Chen et al., 2019;
Koehler, 2013; Mahaut et al., 2008; Moller et al., 2009). Overall, the
static yield stress is higher than the dynamic yield stress (Qian et al.,
2019). Mahaut et al. (2008) examined the evolution of yield stress for
cement pastes over time and found that the evolution of structuration at
rest is connected to the gradual and reversible creation of a solid
structure via flocculation. Different studies reported that SCMs (i.e., CC/
MK and LSP) substitution induces a significant increase in the yield
stresses, thixotropy, and plastic viscosity (Ferreiro et al., 2017; Kawa­
shima et al., 2013; Vance et al., 2013b). Whereas CC/MK as SCM is well
recognized as a viscosity modifier to improve flocculation strength (Qian
and Kawashima, 2018). Muzenda et al. (2020) reported that with the
increase in clinker substitution, the static and dynamic yield stresses
gradually increased at different rates. For example, at the standard LC3
recipe, the static and dynamic yield stresses at the time interval of 30.0
min were found to be increased by 325.3 % and 1094.1 %, whereas at
the time interval of 60.0 min, the increase was 100.2 % and 682.1 %
compared to the referenced conventional OPC. A similar kind of
increasing trend was also reported by Nair et al. (2020).
Besides, the individual effect of SCMs (CC/MK and LSP) as a clinker
substitute is crucial to determining the dominating influence of the
specific SCMs in a standard LC3 system. A study reported that in the LC3
system, the major SCMs ingredient responsible for the increase in yield
stresses, thixotropy, and plastic viscosity is CC/MK owing to its high
specific surface area and agglomeration (Muzenda et al., 2020; Ez-zaki
et al., 2021; Nair et al., 2020). Neto and Campiteli (1990) reported an
increase in yield stress and a reduction in plastic viscosity at 15 % LSP.
Vance et al. (2013a, 2013b) reported insignificant variation in yield
stress and plastic viscosity at coarser LSP. The results revealed a direct
correlation between yield stress and plastic viscosity with SSA and an
inverse relationship with the thickness of water film (Vance et al.,
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Science of the Total Environment 907 (2024) 167794
2013b). Some other studies reported that the combined synergetic effect
of CC/MK and LSP could lead to induce greater effects in corresponding
properties compared to individual effects (Andrade Neto et al., 2021;
Antoni et al., 2012a, 2012b; Malacarne et al., 2021; Scrivener et al.,
2018b; Sfikas et al., 2014). In addition, the particle size distribution
(PSD) of SCMs also played a critical role in defining the rheology. For
instance, the SCMs substitution with coarser limestone (i.e., 15 m size)
by 5 % induced a reduction in yield stresses, whereas finer content of
size range 0.7–0.3 m induced an increase in yield stresses (Nair et al.,
2020). Vance et al. (2013a, 2013b) also reported a similar trend of
reduction in yield stress and insignificant variation in plastic viscosity at
coarser LSP substitution.
4.1.3. Plastic and autogenous shrinkage
Plastic shrinkage refers to the reduction in volume occurring right
after mixing to the setting of fresh mortar corresponding to water
interaction with the surrounding environment, whereas autogenous
shrinkage refers to the uniform reduction of internal moisture caused by
cement hydration. This phenomenon ultimately exhibits cracking
behavior (Mehta and Monteiro, 2014; Tazawa., 1999). The major
driving forces that contribute to this shrinkage and corresponding
cracking behavior fall under four phases; 1) rapid evaporation rate
(Radocea, 2015); 2) differential settlement (Kovler and Roussel, 2011;
Qi et al., 2003); 3) differential thermal dilation (Lura et al., 2007); 4)
autogenous shrinkage in the plastic phase (Jensen et al., 2004; Lura
et al., 2007; Schachinger et al., 2002). Practically all these factors occur
simultaneously and contribute to shrinkage and cracking behavior.
Studies reveal that the physical, chemical, and mineralogical properties
of SCMs could induce considerable variation in shrinkage behavior
(Akkaya et al., 2007; Giergiczny, 2019; Mokarem et al., 2005; Nguyen
et al., 2022), whereas in the LC3 system, in particular, LSP is crucial in
controlling shrinkage (Bouasker et al., 2008; Rezvani et al., 2019;
Rezvani and Proske, 2017). It was found that the LC3 system performed
significantly superior to the conventional OPC system in restraining the
plastic shrinkage (i.e., bleeding and drying regime) values by a factor
greater than two (Ez-zaki et al., 2021). Whereas compared to the con­
ventional OPC system, the individual effect of CC/MK and LSP tend to
reduce the plastic shrinkage with different magnitudes, while the syn­
ergetic effect of CC/MK in the presence of LSP in the LC3 system has a
more dominating effect (Ez-zaki et al., 2021). Different studies associate
this notable improvement with pore network refinement that suspends
the development and succeeding evaporation of the bleed layer,
resulting in a solid network against compressibility (Hu et al., 2013;
Maraghechi et al., 2018).
Meanwhile, some studies reported that the autogenous shrinkage of
the LC3 system was found to be comparable with the OPC system
(Dhandapani et al., 2018; Ston et al., 2018), while some other studies
reported higher autogenous shrinkage than conventional OPC (Du and
Pang, 2020; Nguyen et al., 2022). Scrivener et al. (2018a, 2018b) re­
ported that higher autogenous shrinkage in LC3 mixes is linked to the
coupling effect of chemical evolution due to high pozzolanic reactivity,
crystal growth, and capillary pressure as a result of porosity refinement
(Du and Pang, 2020; X. Gao et al., 2012; Sabir et al., 2001). This implies
that the filler effects of the LSP and the CC/MK increased the hydration
of clinker constituents, resulting in a greater shrinkage, thus counter­
balancing the reduced clinker content (Hay et al., 2022b).
In conclusion, the overall effect of the LC3 system in curtailing the
plastic shrinkage is much superior to the conventional OPC system,
which is critical for crack initiation, whereas higher autogenous
shrinkage is linked to high pozzolanic reactivity in the LC3 system,
which further supports the higher clinker replacement up to 50 %.
4.2. Mechanical response of LC3
In the LC3 system, the mechanical properties and durability char­
acteristics are the governing factors that uphold structural integrity.
N. Ijaz et al.
Various important aspects of SCMs, such as particle fineness, dosages,
clinker composition, etc., play a critical role in early and later age
strength development. Besides, in the LC3 system, the AFm phases
occupy 10–25 % of the hydrated phase assemblage (Fig. 9) (Avet and
Scrivener, 2018b; Dhandapani and Santhanam, 2020). These phases are
extremely sensitive to their exposure environment and exhibit a pro­
clivity for phase transitions under circumstances of chemical exposure
(such as sulfate, chloride, alkali, etc.), temperature, and CO2 environ­
ment (Baquerizo et al., 2015; Herrera et al., 2017; Ipavec et al., 2011;
Krishnan et al., 2021; Mishra et al., 2019; Vizcaíno Andrés et al., 2015).
Therefore, under this section, a special discussion is carried out on the
effect of various parameters on strength and durability characteristics.
4.2.1. Impact of fineness, dosages, and grade of SCMs on strength
It is believed that the fineness of individual LC3 components is
critically more important considering the strength development
compared to total fineness. Among different components, the fineness of
the clinker portion is crucial in strength development, along with SCMs,
whereas in the case of SCMs beyond a certain degree of fineness, the
impact is limited (Adu-amankwah et al., 2019; Dhandapani et al., 2021).
This is linked with portlandite availability for secondary reaction in the
presence of CC/MK and LSP (Zunino et al., 2021).
The CC/MK played an integral role in controlling the compressive
strength of the LC3 system based on its filler effect (physical integration)
and pozzolanic reactivity (chemical integration). Primarily, the CC/MK
particles are fine; therefore, the LC3 is documented to have a high SSA
compared to conventional OPC. Studies reported faster strength devel­
opment at early ages associated with the degree of fineness and majorly
on pozzolanic reactivity of CC/MK (Avet and Scrivener, 2018b; Curcio
et al., 1998; M. H. Zhang and Malhotra, 1995; Zunino and Scrivener,
2021b). The pozzolanic reactivity of CC/MK is mainly dependent on its
KG, i.e., the KAC (Avet and Scrivener, 2018b), while other associated
minerals in CC/MK, such as iron oxide have no evidence of reactivity
and therefore have no significant role (F. H. Avet, 2017). Different
pertinent studies reported in the literature incorporated CC/MK with a
mean size diameter ranging between 1 and 12 μm with KAC ranging
between 20 and 95 % (Akcay and Tasdemir, 2018; Ding, n.d.; Madan­
doust and Mousavi, 2012; Razak and Wong, 2005; Tafraoui et al., 2016).
For instance, Zunino and Scrivener, 2021b, used CC/MK having SSA and
Dv 50 of 13.56 m2/g and 5.13 μm with KAC ≥ 40 % induced similar
strength properties compared to the control OPC system. Whereas the
use of very fine CC/MK with KAC < 40 % poses a significant determi­
nantal effect on the strength and workability. A study showed that in the
LC3 system with an increase in CC/MK grade in terms of KAC (i.e., in the
range of 40 %–63 %) coupled with high SSAs (i.e., in the range of
1.13–8.96 m2/g) of LSP not only exhibits comparable strength but also
exceeds the conventional OPC strength with the aging period (Zunino
Sommariva, 2020) (Fig. 10). Further, the role of CC/MK in strength
development was found to be more prominent at later ages, i.e., 3 or 7
days owing to synergetic reaction (Mishra et al., 2019). In contrast, at 1-
day strength, the CC/MK contribution toward the strength development
is insignificant (Avet and Scrivener, 2018b). Similarly, some other
studies reported that a cost-effective and ideal range of KAC in clays is
between 40 and 63 %, which permits the use of low-grade clays with
lower KAC (Zolfagharnasab et al., 2021). In comparison, higher grades
do not significantly contribute to strength development (Avet and
Scrivener, 2018b; Scrivener et al., 2018a). This is attributed to the fact
that even with clays of lower quality, unreacted clinker, and CC/MK
both persist since there is not enough space for the cement hydration
products (Avet and Scrivener, 2018b; Scrivener et al., 2018a). Besides,
the individual effect of CC/MK as a clinker replacement up to 25 % has
reported potential benefits i.e., increase in strength, durability and
better resistance to chloride and sulfate resistance owing to densification
of pore microstructure in the particular interfacial transition zone (Paiva
et al., 2012; Perlot et al., 2013; C. S. Poon et al., 2006; K. L. Scrivener
et al., 2004; Sullivan et al., 2018). On the contrary, the high fineness of
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Science of the Total Environment 907 (2024) 167794
CC/MK is reported to have a determinantal effect due to a reduction in
workability and resulting agglomeration (Sullivan et al., 2018). Fig. 13
presents the variation compressive strength of LC3 corresponds to
different grades CC/MK and aging period.
Meanwhile, the fineness of LSP also played an essential part in
enhancing the nucleation and packing efficiency coupled with the
chemical dissolution rate. While high fineness of LSP is not only bene­
ficial for early age strength but also compensates for the dilution effect
owing to physical integration (V. Bonavetti et al., 2003; S. H. Liu and
Wang, 2014; Livesey, 1991). It was found that LSP with higher fineness
(i.e., 1 μm) exhibits higher strength development, whereas the coarse
LSP (i.e., 10 μm) exhibits adverse effects on strength development (Knop
and Peled, 2016; Moon et al., 2017).
Overall, the LSP with a mean average particle size in the range of
5–10 μm is widely used in the literature, whereas a very fine LSP (i.e.,
<1 μm) could induce high plastic shrinkage and increase the plasticizer
demand. The use of bi-modal LSP could be beneficially comprised of
enough fines that could undergo chemical integration, whereas the
coarse section of LSP could retain the rheological properties. Moreover,
a comprehensive analysis of a large database exhibits a 15 % strength
reduction beyond 25 % LSP dosage (Elgalhud et al., 2016). Whereas
higher dosages reduced the ultimate strength despite the presence of
SCMs, owing to an imbalance in hydration level trade and dilution effect
(P. R. Da Silva and De Brito, 2015; Diab et al., 2016; Kenai et al., 2007;
Mohammadi and South, 2016; Proske et al., 2018; Santhanam et al.,
2020; S. Sui et al., 2019; Vance et al., 2013a; Maciej Zajac et al., 2020).
Numerous studies document that an LSP dosage of <20 % leads to a
similar slightly marginal reduction in later age strength compared to
that of OPC (Arora et al., 2016; Bolte et al., 2019; Carrasco et al., 2005;
Han et al., 2016; Krishnan et al., 2018b; Mounanga et al., 2011; Vance
et al., 2013a; MacIej Zajac et al., 2014; Y. Zhang and Zhang, 2008).
Besides, some studies documented slightly reduced strength with the
LC3 system, which can be overcome by providing a marginal concrete
cover. Fig. 14 presents the variation in compressive strength of the LC3
blend considering LSP with varying degrees of fineness. In addition,
Table 3 presents the comparative data to illustrate the global insights of
supplementary cementitious materials (SCMs) sourced from various
regions, highlighting their impact on the strength behavior of LC3 in
comparison to Ordinary Portland Cement (OPC). The tabulated data
considers various integral parameters critically important for strength
development to enable a comprehensive comparison between LC3 and
OPC.
Fig. 13. Compressive strength changes with different CC/MK grades and aging
periods, compared to OPC (indicated by dotted lines) (Avet et al., 2016; Avet
and Scrivener, 2018a, 2018b).
N. Ijaz et al.
Fig. 14. Comparison of compressive strength of LC3 incorporating different
grades of LSP (Zunino Sommariva, 2020).
4.2.2. Effect of temperature on strength
SCMs blended cement’s hydration characteristics are strongly
influenced by temperature (Lothenbach et al., 2008; Mishra et al.,
2019). This is attributed to variation in microstructural changes owing
to the variation in hydration product formation due to change in hy­
dration rate induced by high temperature (Cao et al., 2023). Clinker
replacement by SCMs increases the early age hydration reaction to high
pozzolanic nature, whereas high temperature could further induce sig­
nificant changes. For instance, at a higher temperature, the CC/MK
blended LC3 system could result in the enhanced formation of AFm
phases attributed to the increased availability of the Al2O3/SO3 ratio
(Williams et al., 2016). LSP is also another vital component of LC3 that
contributes to the formation of carboaluminate phases by accelerating
the clinker hydration attributed to dilution and filler effect, which re­
straint the ettringite transformation into monosulfate (MacIej Zajac
et al., 2014). These carbonate aluminate and ettringite phases in LC3 are
found to be quite sensitive to temperature variation, i.e., tends to be
more soluble at a higher temperature (Hirljac et al., 1983.; Mishra et al.,
2019). In addition, Mishra et al. (2019) reported that despite reduced
clinker content, the heat of hydration of both LC3 and OPC is similar at
an elevated temperature of 20 ◦ C and 50 ◦ C, and LC3 exhibits a shorter
induction period (Krishnan et al., 2019; Shah et al., 2020; Zumrawi,
2015; Zunino and Scrivener, 2019). Different pertinent studies docu­
mented a reduction in compressive strength at higher curing tempera­
tures, and this behavior is particularly more pronounced in the LC3
system compared to OPC, mainly attributed to the solubility of AFt and
AFm phases (Mishra et al., 2019). Meanwhile, some other studies re­
ported the effect of very high temperatures between 400 and 800 ◦ C on
CC/MK blended cement and documented a high reduction in strength
beyond 400 ◦ C in comparison to that of OPC (Nadeem et al., 2014; Poon
et al., 2003; Poon and Azhar, 2003; Lin et al., 2021a, 2021b). In com­
parison, some other studies show a comparable reduction in the strength
of LC3 compared to OPC at 400o C (Cao et al., 2023).
4.3. Admixtures compatibility with LC3
The compatibility of admixtures with the LC3 system is of critical
importance to meet the specific rheological properties and their
extended effects on mechanical parameters such as strength. The con­
ventional OPC system is well-understood, and suitable admixtures such
as superplasticizers, water, and air-entraining admixtures, etc., are well-
developed and commercially available and are in practice. However, the
LC3 system differs from the OPC system in terms of its composition
owing to the substitution of 50 % of the clinkers with SCMs. The nature
and surface of the particles present in the cement composition played a
16
Science of the Total Environment 907 (2024) 167794
critical role in defining the role of different types of admixtures, such as
adsorption ability, variation in surface charge, specific surface area, the
morphology of clay particles, etc., which could notably modify the
admixture efficiency (Lorentz et al., 2020). For instance, clay particles
have a higher tendency to exchange cations to balance intrinsic electric
charges, which could significantly alter the performance of air-
entraining and water-reducing admixtures, which mainly function
based on electrostatic forces (Teh et al., 2009). When chemical admix­
tures are introduced, the clay’s cations quickly interchange with the
organic molecules in the admixture. As a result, less quantity of ad­
mixtures are dispersed and adsorb on the clay’s surface, thus consuming
a considerable portion, consequently necessitating greater doses to
achieve the desired workability, which ultimately affects setting time,
long-term strength gain, and correspondingly the duration of formwork
(Batis et al., 2005; Cassagnabère et al., 2013a, 2013b; Justice and Kurtis,
2007; Ng and Justnes, 2015; Paiva et al., 2012; Perlot et al., 2013).
Different studies evaluated and analyzed the potential compatibility
of LC3 with commercially available superplasticizers such as sodium
lignosulfonate, polycarboxylic ether (PCE), polymelamine formalde­
hyde (SMF), naphthalene formaldehyde condensates (SNF), etc. (Avet
et al., 2019b; Huenger et al., 2020; Nair et al., 2020; Nehdi, 2014;
Zaribaf et al., 2015). Studies reveal that water-reducing admixtures
comprised of polycarboxylate ether (PCE) as an active component are
more compatible with the LC3 system compared to that of sulfonated
naphthalene formaldehyde (SNF) (M. Antoni et al., 2015; Huenger et al.,
2020; Nair et al., 2020; Nehdi, 2014). Such PCE-based admixtures are
found to curtail slump retention. Besides, the use of retarders doesn’t
pose a notable impact on slump retention improvement. Moreover, some
studies also reported a reduction in the need for PCE-based admixtures
in LC3 compared to the conventional OPC system (Schmid et al., 2018a,
2018b; Schmid et al., 2020). Narula et al. (2020) reported that in the
LC3 system, the water hydrophobic admixture performs superiorly in
reducing porosity and adsorption rate in comparison with crystalline
admixture. Some other studies reported that the type of clay (i.e., 1:1
and 1:2 layered structure) and quantity of quartz in CC/MK played a
decisive role in controlling the rheological properties of LC3 and efficacy
of admixtures (Daukšys et al., 2010; Kameda and Morisaki, 2017; Spo­
sito et al., 2020).
Besides taking advantage of the high yield stress and viscosity of the
LC3 system, the further introduction of high-range water reducers
further enhances the structure and yield stress of LC3, which makes it a
promising candidate for 3D-printed concrete (Beigh et al., 2020; Vance
et al., 2013b). Further, it has been demonstrated that a pumpable and
sprayable cementitious composite can be engineered despite the
changed rheology of LC3 (Zhu et al., 2021).
Therefore, it is preferable to optimize rather than maximize the KAC
in the clays to enhance the functionality of LC3. An integrated strategy
to maximize both strength and workability might be devised, much to
the strategy to maximize KAC based on reaction stoichiometry (Krishnan
et al., 2019). Similar research revealed that silica fume and LC3 particle
packing improved the structural recovery, dynamic yield stress, and
static yield stress of 3D-printable concrete (Long et al., 2021a, 2021b).
Based on the documented studies, it is deduced that PCE-based plasti­
cizers are found to be quite effective in the LC3 system. Besides, the
evaluation, assessment, and optimization of different potential admix­
tures, along with their attributes and shortcomings, need to be exam­
ined. Overall, limited studies are documented, and this area needs to be
established.
5. Application of LC3
LC3 is considered to be the replacement for OPC in the construction
sector. Therefore, most of its applications are concentrated on cement-
based construction utilities, i.e., conventional concreting, 3D concrete
printing, plastering, roof tiles, prefab material, concrete bricks, paver,
cementing additive, etc. However, the usage of LC3 on a large scale is
 Table 3

N. Ijaz et al.
Global insight into the effect of various parameters on the mechanical behavior of LC3.
Type Ingredients Chemical composition Clinker Specific Dv50 Compressive strength Superplasticizer Origin Reference
Composition surface area (μm) (MPa) type
CaO SiO2 Al2O3 Fe2O3 MgO K2O TiO2 SO3 LOI
(%) (m2/kg)

OPC 64.6 19.0 4.2 3.9 0.9 0.6 0.2 1.7 1.4 – – 340 23.6 M-30: 40.3 ± 0.5, M50: Polycarboxylic India (Dhandapani et al.,
47.8 ± 1.5 (28D, 20 ◦ C) ether 2018)
LC3 CC/MK 0.1 58.4 25.0 5.1 0.2 0.2 1.4 0.0 9.6 – – 520 20 M-30: 41.1 ± 0.5, M50:
LSP 48.5 10.1 1.7 1.6 0.5 0.1 0.2 0.0 37.1 – – 48.89 ± 1.6 (28D, 20 ◦ C)
OPC 63.2 21.6 5.4 2.7 2.4 1.1 0.3 2.2 0.6 – – – 18.3 61 ± 2 (180D, 20 ◦ C); 14 – Korea (Lin et al., 2021a,
± 1.2 (180D, 900 ◦ C) 2021b)
LC3 CC/MK 0.2 64.2 23.9 6.4 0.5 3.2 0.8 0.0 0.7 – – – 12.3 41± 1.1 (180D, 20 ◦ C); 8
LSP 59.2 0.3 0.2 0.1 0.3 0.0 0.0 0.1 39.6 – – – 7.4 ± 1.1 (180D, 900 ◦ C)
OPC 64.6 19.7 4.7 3.0 1.5 0.6 0.3 2.2 3.2 C3S 51.2 – 8.5 51.5 + 2.5 (28D, 23 ± – Australia (Nguyen et al.,
2 ◦ C) 2018)
LC3 CC/MK 0.5 70.4 22.3 2.3 0.2 0.2 1.1 0.0 1.8 C2S 16.5 – 21.2 36.72 + 1.5 (28D, 23 ± France
LSP 57.5 0.4 0.1 0.1 57.5 0.3 0.0 0.0 42.6 C3A 6.5 – 43.4 2 ◦ C) Australia
C4AF 7.3
OPC 61.7 20.5 4.5 3.1 3.2 0.4 0.2 2.6 2.1 C3S 57.6 268.1 13.8 – BASF US (Canbek et al.,
LC3 CC/MK 0.0 51.4 43.0 0.3 0.0 0.1 1.6 0.1 1.4 C2S 34.1 2211.1 3.8 55 ± 2.8 (28D, 23 ± MasterGlenium 2022a)
LSP 55.0 0.8 0.3 0.3 1.8 0.0 0.0 0.0 41.8 C3A 1.9 924.3 13.4 2 ◦ C) 7920
C4AF 4.4
OPC 65.2 19.2 4.9 3.3 1.2 0.5 0.3 2.4 2.6 C3S 67.7 – 12.8 61.8 ± 2.2 (28D, 20 ◦ C) – Thailand (Hanpongpun,
LC3 CC/MK 2.1 40.7 30.4 20.1 0.6 0.1 2.7 0.0 2.5 C2S 7.95 30,200 4.6 52.5 ± 1.3(28D, 20 ◦ C) 2019)
LSP 55.0 0.1 0.0 0.0 0.2 0.0 0.0 0.0 42.5 C3A 6.57 1800 7.2
C4AF 9.21
OPC 63.9 19.5 4.4 3.1 2.1 0.8 0.3 3.3 1.5 C3S 66.5 1410 14.2 67.5 ± 2.5 (28D, 20 ◦ C) Unkown Switzerland (Zunino and
LC3 CC/MK 0.0 52.0 43.8 0.3 0.0 0.3 1.5 0.1 1.5 C2S 4 13,560 5.1 78.7 ± 1.8 (28D, 20 ◦ C) Scrivener, 2021b)
LSP 55.0 0.1 0.0 0.0 0.0 0.0 0.0 0.0 42.5 C3A 4.9 3600 3.9
17

C4AF 9.6
OPC 64.2 21.0 4.6 2.6 1.8 0.9 0.1 2.8 1.3 C3S 62.1 – 14.1 48.8 (28D) Rheobuild Switzerland (Antoni et al.,
LC3 CC/MK 0.0 50.6 46.9 0.4 0.1 0.2 1.3 0.1 0.0 C2S 15.2 – 12.2 55.8 (28D) 5500 USA 2012a, 2012b)
LSP 56.5 0.0 0.1 0.1 0.1 0.0 0.0 0.0 43.1 C3A 6.4 – 1–3 Switzerland
C4AF 6.2
OPC 63.6 19.3 5.7 3.6 1.6 1.2 0.3 3.2 0.0 C3S 66.3 1940 6.8 44.3 (28D) ± 1.6 Unknown China (S. Sui et al., 2019)
LC3 CC/MK 0.2 49.7 41.8 2.3 0.1 0.1 0.1 0.0 0.1 C2S 6.11 9190 5.0 46.2 (28D) ± 0.3
LSP 55.0 5.7 0.0 0.0 0.2 0.0 0.0 0.0 42.6 C3A 7.64 2060 7.5
C4AF 11.9
OPC 63.4 20.0 5.0 2.9 1.8 0.8 0.3 3.2 0.0 – – 10.7 52.6 ± 1.9 (M50); 82.5 Polycarboxylate Switzerland (Avet et al., 2019a,
± 2.7 (M70) ether 2019b)
LC3 CC/MK 0.2 49.7 41.8 2.3 0.1 0.1 3.4 0.0 1.9 – – 8200 8.4 57.2 ± 1.7 (M50); 72.3
LSP 55.0 0.1 0.0 0.0 0.2 0.0 0.0 0.0 42.6 – – 1800 7.2 ± 3.8 (M70)
OPC 64.0 21.4 4.7 4.3 1.4 0.7 2.4 0.9 – – – 16.5 45.3 ± 1.2 (28D) Polycarboxylate Iran (Zolfagharnasab

Science of the Total Environment 907 (2024) 167794

LC3 CC/MK 2.1 16.2 55.4 17.4 1.2 0.4 0.1 1.7 – – – 18.5 52.5 ± 0.5 (28D) ether et al., 2021)
LSP 49.1 3.3 0.7 0.2 2.8 0.1 0.1 43.4 – – – 8
OPC 64.0 21.4 4.7 4.3 1.4 0.7 2.4 0.9 C3S 59.6 – 16 52 ± 2 (28D) Polycarboxylate Iran (Bahman-Zadeh
LC3 CC/MK 2.1 16.2 55.4 17.4 1.2 0.4 0.1 1.7 C2S 16.5 – 18.5 51.5 ± 0.5 (28D) ether et al., 2022)
LSP 49.1 3.3 0.7 0.2 2.8 0.1 0.1 43.4 C3A 5.3 – 8
C4AF 12.9
OPC 52.2 34.1 7.4 2.6 4.0 0.7 0.3 1.2 0.0 – – – – Malawi (Kafodya et al.,
LC3 CC/MK 0.7 46.7 36.0 3.4 0.2 0.4 0.4 0.1 11.3 – – – – 39.2 ± 3.8 (28D) – 2023)
LSP 47.3 6.5 1.7 0.6 9.2 0.1 0.1 0.3 34.3 – – – –
OPC 63.2 21.0 5.3 4.8 1.1 0.5 0.3 3.2 – – – 1490 7.4 149 ± 8 (28D, 20 ◦ C) Glenium ACE 460 Switzerland (Wang et al., 2021)
LC3 CC/MK 6.4 50.2 25.6 7.6 3.3 3.2 0.9 2.1 – – – 7550 8.9 124 ± 7 (28D, 20 ◦ C) Germany
LSP 74.2 7.9 2.1 0.8 12.9 0.5 0.0 0.0 – – – 1690 17.8
OPC 65.1 20.2 5.2 3.2 1.3 0.5 0.3 3.4 0.3 – – – 20 33.7± 1.6 (28D, 20 ◦ C); Polycarboxylic Australia (Cao et al., 2023)
22.5 + 3.8 (28D, 400 ◦ C)
LC3 CC/MK 0.0 66.1 29.3 2.7 0.2 0.5 0.8 0.0 0.3 – – – 12 31 ± 1.4 (28D, 20 ◦ C);
LSP 55.0 0.1 0.0 0.0 0.1 0.0 0.0 0.0 42.6 – – – 20 ± 1.6 (28D, 400 ◦ C)
N. Ijaz et al.
still under development and requires more effort for its widespread
applicability in the construction sector. To appraise the performance of
the application of LC3, OPC is taken as the benchmark, considering LC3
as a potential replacement. In this section, the documented evidence
about different construction applications is discussed.
5.1. LC3 in concrete technology
Several studies have been reported in the last few years to prepare
different concrete, i.e., lightweight, normal weight, and self-compacting
concrete, and 3D concrete printing using LC3, and compared it with
OPC-based concrete. Reddy et al. (2021) prepared 40-grade concrete by
following IS 10262–2019 and using OPC and LC3 and fly as modified
cement. They reported a 5 % increase in compressive and flexural
strength and exhibited enhanced durability and strength in the case of
LC3 compared to other cementing materials with improved water ab­
sorption and desorption characteristics. Moreover, Pillai et al. (2019)
prepared 35 and 50 grades of concrete by using LC3 and appraised the
service life of such concrete for a typical bridge pier and girder. They
claimed a higher service life of LC3 as compared to conventional
cementing material. Further, the life cycle assessment of concrete pro­
duced by the aforementioned SCMs showed that the carbon footprint of
LC3 and fly ash-based modified cement was much lower than the OPC.
Nguyen et al. (2020a, 2020b, 2020c) reported the mechanical and
chloride resistivity performance of LC3-based concrete, which was
found to be considerably superior compared to OPC-based concrete.
Furthermore, the application of LC3 is also assessed for reinforced
concrete, i.e., steel, rubber, etc. The performance of LC3 is found to be
comparable and superior for steel and rubber reinforcement, respec­
tively, in comparison to OPC.
Besides, some limited studies are documented in literature focusing
on lightweight concrete. For instance, Salem et al. (2019) reported that
intrusion of SCMs, i.e., CC/MK in lightweight concrete, has significantly
improved the strength and resistance against chloride diffusion. Zhou
et al. (2022) examined the LC3-based lightweight concrete and reported
that flexural and compressive strength is slightly reduced with reduced
porosity and pore size coupled with reduced environmental impact.
Huang et al. (2020a, 2020b) reported the bond-slip behavior between
the LC3 concrete interface and steel bars exhibits higher bond-slip
Fig. 15. Applications of LC3; a) LC3 concerting; b) Swiss Embassy building in Delhi made up of LC3 prefab material; c) check dam in Orchha; d) LC3-prefab
materials; e) LC3-pavements; f) LC3 for Biennale.
18
Science of the Total Environment 907 (2024) 167794
stiffness than the OPC concrete-rebar interface, whereas the bond
strength is comparable to that of OPC concrete with 28-day compressive
strength.
Meanwhile, in recent years, the use of LC3 has gained considerable
attention owing to its high yield stresses and viscosity of the LC3
mixture, which make it a potential candidate for 3D concrete printing.
Tao et al. (2022) evaluated the efficacy of LC3 coupled with perforated
fly ash cenospheres as an internal curing agent in 3D concrete printing
and reported that shrinkage is significantly reduced by 80 % and rheo­
logical properties meet the 3D specifications. Long et al. (2021a, 2021b)
reported that LC3 mortar with 5 % SF by weight significantly improves
printability with excellent shape retention and better rheological prop­
erties (i.e., dynamic and yield stresses). Moreover, compared to plain
mortar, optimal mortar’s embodied energy (EE) and embodied carbon
emissions (CO2) decreased by 50.2 % and 45.2 %, respectively. Chen
et al. (2020) reported that medium-grade CC/MK performs better than
low-grade and high-grade clays in terms of buildability and printability.
Similarly, Chen et al. (2019) reported that an increase in CC/MK could
increase extrusion pressures and green strength, reduce the initial
setting time, and enhance compression strength at 1, 7, and 28 days.
Based on the preceding analysis, several practical applications of LC3
have emerged across a range of concrete grades. These include its use in
concreting, residential construction, small check dam construction,
production of prefab materials, tuff paver tiles, and biennale, among
others, as illustrated in Fig. 15.
5.2. LC3 as mortar
In the essence of increasing cement demands, the use of LC3 as a
mortar could be a good low-carbon alternative. In this regard, numerous
studies are documented in the literature highlighting the potential ef­
ficacy of LC3 and its comparison with conventional OPC. For instance,
Marangu (2020) reported conducted a comparative study on cement
mortar using LC3, OPC, and modified PC with volcanic ash considering
different w/c ratios (~0.5–0.6). Among cement mortars, the LC3-based
mortar exhibits an appreciable increase in compressive strength and
notable resistance against the salt solution (NaCl) and chloride ingress,
creating a denser structure. Nguyen et al. (2020a, 2020b, 2020c) re­
ported that LC3 mortar exhibits better resistance to ASR compared to
N. Ijaz et al.
OPC mortar pastes. Zolfagharnasab et al. (2021) reported that low-grade
CC/MK has a promising potential to be used in LC3 mortar with
enhanced durability to counter the chloride ingress, though the
compressive strength is found to be lower than OPC mortar.
5.3. LC3 in geotechnical engineering
Besides the primary application of LC3 in concrete technology,
recent studies showed its potential interest in the field of geotechnical
engineering. From the geotechnical perspective, the OPC has been
widely employed for ground treatment of problematic soils such as
expansive soils, loess, contaminated soils, organic soil, etc. Such soils
exhibit low bearing capacity and are comprised of adverse soil charac­
teristics, such as low shear strength, swell-shrinkage behavior, cracking
phenomena, etc. Recent studies showed the potential benefits of LC3 in
the treatment of such problematic soils. For instance, Ijaz et al. (2022)
carried out a comprehensive study and revealed the stabilization
mechanism by which LC3 stabilized the problematic expansive soil. The
LC3 intrusion results in the formation of CSH/CASH gel coupled with
space-filling ettringite phases produced in a high pH environment
responsible for strength development, eradication of swelling behavior,
and inducing low permeability. The synergetic reaction of CC/MK and
LSP played an important role in the formation of space-filling ettringite,
which is responsible for the development of dense microstructure
(Fig. 16) (Ijaz et al., 2022).
Reddy et al. (2019) evaluate the LC3 efficacy for the treatment of
zinc (Zn)-contaminated soil. The results show that, following a 14-day
curing period, LC3 works effectively in limiting Zn-leachability consid­
erably below the equivalent hazardous waste management regulation
limit. A similar trend was also reported in the case of lead (Pb)
contaminated soil, wherein toxic characteristics of leached Pb were
found to be well below the regulatory limits with enhanced compressive
strength (Reddy et al., 2020a, 2020b). Also, Reddy et al. (2020a, 2020b)
Fig. 16. Schematic illustration of LC3 stabilization mechanism of expansive soil; a) untreated; b) LC3 treated (Ijaz et al., 2022).
19
Science of the Total Environment 907 (2024) 167794
reported the efficacy of LC3 treatment of soil with coupled contamina­
tion of Zn/Pb, considering a possible scenario. The formation of space-
filling ettringite significantly immobilizes the Zn/Pb movement and
ameliorates the strength characteristics. Overall, the LC3 was found to
be quite effective in dealing with geotechnical engineering problems
regarding ground improvement. However, these studies are still in their
initial phases and are restricted to laboratory experimentation. Broad
application of LC3 in the soil stabilization is an open to research urging
full-scale investigation of LC3 impact on mechanical durability and
physico-chemical response.
6. Economic and environmental aspects
Economic and environmental aspects are regarded as major pillars of
the sustainability index which have been well addressed by LC3,
considering the serviceability and safety of the material along with en­
gineering performance (Cancio et al., 2017; Joseph, 2016; Martirena
and Scrivener, 2018; Sánchez Berriel et al., 2016; Sharma et al., 2021a).
For this purpose, different life cycle assessment (LCA) based studies for
LC3 and its counterparts are critically examined.
The cement production must consider the system boundaries that can
be either Cradle-to-Gate or Gate-to-Gate. The Cradle-to-Gate system
encompasses extracting raw materials until they reach the
manufacturing plant. This approach provides a comprehensive overview
but is limited due to data variability and discrepancies in machinery use
across different regions. On the other hand, the Gate-to-Gate system
focuses solely on the operations within the processing plant, from the
initial processing of raw materials to the creation of the end product.
This approach offers more standardized data as it excludes the energy
demand and carbon emissions related to the transportation of raw ma­
terials. It typically provides a similar outcome irrespective of the loca­
tion/region. Fig. 17 illustrates a comprehensive comparison of various
critical steps involved in the manufacturing and usage of OPC and LC3,
N. Ijaz et al. Science of the Total Environment 907 (2024) 167794

Fig. 17. Comparison of production scheme from cradle to grave of OPC and LC3.

considering the cradle-to-grave approach. It is important to note that the
manufacturing process of LC3 involves more recyclable resources,
thereby presenting a more sustainable manufacturing scheme over OPC.
Cement manufacturing is an intricate process globally, leveraging
various raw materials and energy resources, heavily contingent on
regional geological availability, industry regulations, and technical
advancement (Di Filippo et al., 2019). Literature reveals that the budget
allocation required to establish and run an LC3 plant is less than that
required to construct and run an OPC plant of equivalent capacity
(Cancio et al., 2017; Joseph, 2016). This entails the conservation of

Table 4
Comparison of OPC and LC3 considering material needs and energy consumption at the pilot, industrial, and BAT levels.
Details Unit Pilot level Industrial level BAT level

OPC PPC LC3 OPC PPC LC3 OPC PPC LC3

Input data
Fuel type km Cuban crude oil Pet-coke + cuban crude oil Gas + waste
Kaolinite clay lead distance 150 60–150 <100
Clay calcining technology Wet rotary kiln Retrofitted calciner Optimized flash calciner
Clinker technology Wet rotary kiln 4 stage pre-heaters + pre-calciner 6 stage pre-heaters + pre-calciner

Foreground data per ton of cement

Materials
Raw materials
Limestone, crushed for mill kg 841 459 717 1056 900 459 1056 900 459
Iron kg 45 25 38 28 24 25 28 24 25
Clay kg 117 64 100 318 271 64 318 271 64
Clinker from Cienfuegos kg 197 165 106
Kaolinite clay kg 390 390 390
Additions
Gypsum kg 62 50 70 62 50 70 62 50 70
Limestone kg 44 150 44 150 44 150
Zeolite kg 200 200 200
Energy for clink erization
Pet coke kg 101 86 55
Crude oil kg 167 143 91
Waste oil kg 53 45 29
Gas kg 20 17 11
Electricity kWh 70 60 38 80 68 44 23 19 13
Energy for clay calcination kg 31 23
Gas kg 5
Crude oil kg
Waste oil kg 14
Electricity kWh 20 16 5
Grinding + packing + other
Electricity kWh 51 51 31 52 51 24 31 31 15

20
N. Ijaz et al.
material inventory as well as energy consumption required for the
production process (Diab et al., 2016; Joseph, 2016).
Meanwhile, a detailed comparative study that gives a brief idea
about the lead distance of the raw material, consumption index of ma­
terial and energy, and extraction process by considering three different
scenarios, i.e., pilot study, industrial level, and best available technology
(BAT) for OPC, Portland pozzolan cement (PPC) and LC3 (Table 4). The
results showed that LC3 could considerably reduce the cost in terms of
raw materials, energy for clinkerization, calcination, grinding, and
packing, whereas BAT technology performs superiorly among the three
(Sánchez Berriel et al., 2016). Overall, studies reveal that the LC3
technology successfully fulfills the criteria pertaining to 1) technical
feasibility, 2) economic viability, 3) low capital investment, and 4) easy
accessibility of raw materials. However, the literature reveals that the
economic and resource conversation-related advantages of LC3 are
highly region-specific, as different practices are being followed in
various regions for LC3 production. The disparity in the production
process leads to different characteristics and conservation schemes. The
following discussion brings different practices in material inventory and
energy consumption of different regions into light based on pertinent
literature.
• Clinkerization, a crucial, energy-intensive phase in cement produc­
tion, varies globally based on regional resources and practices
(Zhang et al., 2020). Considering the clinker aspect in OPC and LC3
production, the key ingredient in both types of cement is limestone,
which is universally procured from licensed mining operations,
abiding by national and local regulations (Kanagaraj et al., 2023).
Whereas LC3 leverages of pozzolanic behavior of CC/MK (calcined at
750-800 ◦ C) to reduce the clinker content significantly to one-half,
thus, ultimately leading to lower energy consumption (Wang et al.,
2021). Meanwhile, dry process clinkerization is standard in India for
water conservation, while regions with ample water supply, like
South America, employ wet process clinkerization (Prakasan et al.,
2020). Whereas developed regions like Europe tend to implement the
semi-dry or semi-wet process, balancing environmental concerns and
energy efficiency (Madlool et al., 2011).
• The energy source for cement production also varies regionally.
While coal is the primary energy source in many developing coun­
tries, natural gas, petroleum coke, or alternative fuels like biomass
are commonly used in developed countries (Chatziaras et al., 2016).
Countries rich in natural resources, such as Russia and the Middle
East, rely more on natural gas, while others, like the U.S., leverage
petroleum coke (Yang et al., 2017).
• Coal characteristics, including calorific value and ash content, can
vary regionally. Indian coal, with a low calorific value (10 MJ/kg to
20 MJ/kg) and high ash content (35 % to 50 %), contrasts with
Australian or South African coal, known for higher calorific values
and lower ash content (Degereji et al., 2012; Kanagaraj et al., 2023).
This variation impacts the efficiency of cement plants and necessi­
tates coal imports in regions with lower-quality coal.
• Gypsum addition in cement manufacturing presents cost variability
based on the source. Some regions opt for natural gypsum extraction,
while others, due to cost constraints or environmental regulations,
employ industrial byproducts like phosphogypsum from the fertilizer
industry (Calderón-Morales et al., 2021). In countries like China, the
use of flue gas desulfurization gypsum is quite common (Xu et al.,
2017).
• Embracing sustainability measures like waste utilization and
biomass for fuel is an emerging trend worldwide, albeit with regional
variations. Developed regions, especially Europe, are at the forefront
of employing alternative raw materials and fuels, driven by strict
environmental regulations and advanced technologies. However, in
developing countries, the adoption rate might be slower due to
technological and regulatory constraints.
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Science of the Total Environment 907 (2024) 167794
By considering these variables, it provides a more comprehensive
understanding of the globally diverse landscape of cement production,
revealing its intricate interplay of geological, regulatory, technological,
and economic factors. In addition, Table 5 offers a detailed economic
analysis, shedding light on the cost-effectiveness, energy consumption,
energy efficiency, and carbon efficiency for each cubic meter of OPC and
LC3 concrete of grades M40, M45, and M70 based on published litera­
ture (Kanagaraj et al., 2023; Yu et al., 2021). Reportedly, for normal
strength LC3, the production costs of different grades of concrete were
~5–10 %, lower than of OPC. Whereas the cost-effectiveness was found
to be 12–16 % higher than the OPC, highlighting the superiority of LC3.
In addition, the energy efficiency of LC3 concrete was found to be
significantly increased by ~30–80 %. Furthermore, the carbon effi­
ciency of different LC3 grades of concrete was significantly increased by
~45–90 % compared with OPC concrete. Similarly, other studies also
reported a significant reduction in carbon emission for LC3 systems
taking into account the distinct technological levels: Pilot, Industrial,
and BAT. Fig. 18(a) and (b) shows the material responsible for CO2
emission, which is roughly 30 % lower for the LC3 system (Sánchez
Berriel et al., 2016). A similar outcome was also reported in a study
conducted on the number of cement factories in India. This investigation
demonstrates that LC3–50 saves 30 % of CO2 emissions when compared
to OPC at the cement level and roughly 10 % when compared to a
Portland Pozzolanic (fly ash) blend. Some studies reported the CO2
emission for 50 MPa grade concrete and found it to be significantly
lower in comparison to that of OPC and OPC blended with 30 % fly ash/
15 % ground granulated blast slag (GGBS) (Fig. 18c) (Gettu et al., 2019;
Scrivener et al., 2018b).
Meanwhile, adapting existing production equipment for LC3
manufacturing requires due attention. From a capital expenditure
perspective, the transition to LC3 technology generally incurs lower
upfront costs than establishing a new OPC production facility of
equivalent capacity. Several studies corroborate this, suggesting that
modifying an existing cement plant for LC3 production is more cost-
effective than erecting a new clinker production line (Diab et al.,
2016; Joseph, 2016; Sánchez Berriel et al., 2016). Moreover, this
financial advantage is amplified in regions experiencing a surge in
cement demand. Notably, the retrofitting process typically involves
upgrading existing clinker kilns to incorporate clay calciners, a modifi­
cation that has demonstrated financial efficacy (Cancio et al., 2017). The
technical modifications for such upgrades are generally well-understood
and can often be integrated seamlessly into existing production lines.
This ease of integration minimizes production downtime, thereby pre­
serving revenue streams. Additionally, various calcination methodolo­
gies have been evaluated for their economic and operational efficiency,
providing a range of options tailored to specific plant configurations and
regional raw material availabilities. Therefore, not only does LC3 pro­
duction offer environmental benefits through reduced carbon emissions
and provides a feasible and economically sound option for cement
producers looking to modernize their operations.
7. Research status
Overall, the literature review manifests that research on LC3 has
been conducted from many aspects, including but not limited to
rheology, mineralogical and microstructural analyses, durability,
strength behavior, material assessment, resources conversation, envi­
ronmental protection, sustainability, and life cycle assessment (LCA).
A systematic analysis of the database used for the current review
article was also performed, considering the co-occurrence of keywords
and fields of studies manifested by different studies. For this purpose,
VOSviewer software was used to visualize the co-occurrence analysis of
different keywords regarding publication. Considering all the articles
cited in the current, approximately 3000 keywords were analyzed by
setting the co-occurrence level at 5 (Fig. 19a). The analysis showed that
rheology, durability, microstructure, and sustainability are the most
N. Ijaz et al. Science of the Total Environment 907 (2024) 167794

Table 5
Comparative evaluation of cost-effectiveness, energy demand, energy efficiency, and carbon efficiency of 1m3 of concrete of OPC and LC3.
Materials Rates ($/Mt) E-CG CO2-e (kg- OPC
(GJ/t) CO2-e/t)
Kanagaraj Yu et al., M40 M45 M70
et al., 2023 2021a*
Qty Cost ED CO2- Qty Cost ED CO2- Qty Cost ED CO2-
e e e

OPC 130.5 102.6 4.3 840 412 53.77 87 95 % 395.9 40.62 92 95 % 428 55.85 89 96 %
% % %
CC/MK 115.3 51.3b* 2.5 330 – – – – – – – – – – – –
LSP 36.2 – 3.8 – – – – – – – – – – – –
GY 120.6 0.057 140 – – – – – – – – – – – –
SF 391.6 384.6 0.036 520 – – – – – – – – 27 10.48 0 0%
FA 13.1 51.3 0.033 4.0 – – – – – – – – 80 1.05 0 0%
CA 24.1 19.2 0.083 4.8 1234 29.79 5% 2% 1106 21.24 5% 2% 1219 29.43 5% 2%
SD 26.6 28.2 0.083 4.8 648 17.2 2% 1% 664 18.72 3% 1% 589 15.64 4% 1%
SP 3916.0 2949.0 29.1 1180 4.12 16.13 6% 2% 2.67 10.46 6% 1%
Total cost ($/m3) 116.89 80.6 122.9
28 Days compressive strength (CS) (MPa) 46.5 55.5 79.9
Cost efficiency (CE) (MPa/$/m3) 0.4 0.68 0.65
Energy efficiency (EE) (MPa/GJ) 21 30 36
Carbon efficiency (CA-E) (MPa/t-CO2) 129 162 213

Materials Rates ($/Mt) E-CG CO2-e LC3

(GJ/t) (kg-CO2-
Kanagaraj Yu et al., M40 M45 M70
e/t)
et al., 2023 2021a*
Qty Cost ED CO2- Qty Cost ED CO2- Qty Cost ED CO2-
e e e

OPC 130.5 102.6 4.3 840 206 26.88 60 75 % 199.9 20.51 65 % 77 % 255 33.28 62 76 %
% %
CC/MK 115.3 51.3b* 2.5 330 123.6 7.12 21 18 % 119.94 6.1529 22.7 18 % 153 8.88 21 18 %
% % %
LSP 36.2 – 3.8 61.8 4.47 0% 0% 59.97 3.0765 0 0.1 77 5.53 0% 0%
GY 120.6 0.057 140 20.6 2.48 0% 1% 19.9 1.0209 0.10 1.3 26 3.14 0% 1%
%
SF 391.6 384.6 0.036 520 – – – – – 0 – – – – –
FA 13.1 51.3 0.033 4.0 – – – – – – 0 – – – – –
CA 24.1 19.2 0.083 4.8 1324 31.96 7% 3% 1106 21.24 7% 2% 1294 31.24 6% 2%
SD 26.6 28.2 0.083 4.8 645 17.12 4% 1% 664 18.72 4% 2% 579 15.37 3% 1%
SP 3916.0 2949.0 29.1 1180 4.12 16.13 8% 2% 0.452 1.33 1% 0% 5.1 19.97 8% 2%
Total cost ($/m3) 106.2 72.05 117.4
28 Days compressive strength (CS) (MPa) 48.25 56.5 79.9
Cost efficiency (CE) (MPa/$/m3) 0.45 0.784 0.68
Energy efficiency (EE) (MPa/GJ) 39 37.4 52
Carbon efficiency (CA-E) (MPa/t-CO2) 254 232 313

Note: FA: fly ash; SF: silica fume; CA: coarse aggregate; SD: sand; SP: superplasticizer; LSP: limestone powder; CC/MK: calcined clay/metakaolin; GY: gypsum; Qty:
quantity; E-CG: energy required for collecting and grinding; ED: energy demand; a*: HK based rates in US$ for M45 grade; b*: procured item is a mixture of CC/MK, LSP
and GY with an overall rate.

prominent fields of investigation considering LC3. Further, the research
trend is also emerging toward the assessment of different materials for
the preparation of LC3. Besides, it is also pertinent to mention here that
mostly work has been done in concrete technology, whereas its potential
application in other fields of construction is yet to be evaluated. Further,
the year-wise research publication trend shows that the research on LC3
is emerging with each passing year (Fig. 19b). However, more efforts are
still required to resolve associated challenges with LC3 by pacing up the
research in coming years.
8. Discussion on future prospective research areas
Based on a comprehensive literature review, the findings demon­
strate the promotion of the use of LC3 in concrete technology due to its
economic and environmental benefits. The potential area of interest,
along with technical criticalities that need to be given due attention to
pave the way for LC3 in concrete technology as well as in other areas of
engineering, are discussed as under:
The heterogeneous nature of SCMs, specifically CC/MK and LSP,
often introduces variances in chemical composition owing to the po­
tential presence of impurities. These impurities could induce changes in
phase composition and, consequently, influence the strength develop­
ment of LC3. As such, it is paramount that future research endeavors
undertake rigorous investigations utilizing thermodynamic modeling or
mass balance techniques. These methodologies offer an avenue for
quantitative by applying statistical methods evaluating the implications
of prevalent impurities on strength development. Moreover, it would be
advantageous to design studies that seek to optimize the processing and
preparation of these SCMs, with the aim of minimizing the potential
impurities, which could provide critical guidance for the construction
industry.
The grade of CC/MK is crucial in governing and ensuring sufficient
pozzolanic reactivity, thereby significantly influencing LC3 perfor­
mance. Consequently, it is imperative to develop and standardize test
methods that accurately quantify CC/MK quality and reactivity in
cement plants, considering factors such as calcination temperature,
grinding conditions, and color control. Simultaneously, the alite content
in clinker, given its pivotal role in producing sufficient hydration by-
products like CH that react with CC/MK to form cementitious phases,
warrants a comprehensive investigation to standardize the minimum
required content. The development of such standards could enable
comparable strength to OPC. Future research should also focus on

22
N. Ijaz et al.
Fig. 18. Cost and CO2 comparison; a) CO2 emission producing materials of LC3 and OPC; b) environmental and monetary cost comparison of LC3 and OPC (Sánchez
Berriel et al., 2016); c) CO2 emission comparison of 50 MPa grade concrete (R. Gettu et al., 2019; Scrivener et al., 2018b).
leveraging advanced statistical techniques to optimize calcination and
grinding conditions and developing sophisticated computational
models, potentially employing machine learning for accurately pre­
dicting strength development. Together, these focused research di­
rections can significantly contribute to enhancing the understanding of
LC3 and facilitating its widespread adoption in the construction
industry.
While 2:1 clay is acknowledged to possess lower reactivity compared
to kaolinitic clays, their significance cannot be overlooked, especially
given the non-availability of kaolinitic clays in certain regions. This
presents an opportunity to expand the clay types utilized in the LC3
system through the integration of 2:1 clay with clinkers and LSP. Future
research could probe into innovative modification techniques such as
thermal treatment, mechanochemical activation, or chemical alteration
to enhance the reactivity of 2:1 clay. This approach could potentially
lead to the development of novel LC3 mix designs that leverage these
clays, thereby enhancing both the versatility and performance of LC3 in
varying regional contexts, thus expanding its potential application in the
construction industry.
Besides, LC3 displays promising resistance to various salt exposures;
its carbonation resistance falls short compared to OPC, indicating a
crucial area for further exploration. Future research should adopt a
comprehensive approach, examining the carbonation kinetics in LC3,
23
Science of the Total Environment 907 (2024) 167794
investigating induced phase transformations and microstructural
changes through advanced microscopic and spectroscopic techniques,
and understanding carbonation-triggered corrosion via electrochemical
analysis. Evaluating the carbonation’s impact on mechanical properties
such as compressive strength, flexural strength, and modulus of elas­
ticity should also be integral to future inquiries.
The intricate rheological properties of LC3 compared to OPC un­
derscore a need for more nuanced exploration. Particularly, the “dy­
namic” nature of the w/c ratio of LC3 systems suggests opportunities for
innovative mix design strategies that consider the evolving microstruc­
ture during curing. Moreover, future research should be targeted toward
unraveling the effects of the bi-modal gradation of both CC/MK and LSP
on these properties, taking advantage of its physical integration aspect
as a filler. Key influential parameters such as gradation, SSA, and
chemical interactions between these constituents and elements like
clinker could significantly impact the chemical integration, workability,
and early-age strength development of LC3. Moreover, the application of
advanced characterization techniques and modeling approaches can
shed light on the complex interplay between these factors and their
combined effect on the hydration kinetics, microstructure, durability,
and overall performance of LC3. The potential of the bi-modal approach
to enhance the workability of LC3 mixtures and improve its resistance to
various aggressive agents warrants comprehensive exploration, which
N. Ijaz et al.
Fig. 19. a) Keywords co-occurrence overlay visualization using VOSviewer software; b) yearly publication record.
helps in the establishment of standardized guidelines for LC3..
The adoption of LC3 presents promising potential for mitigating
plastic shrinkage, but the in-depth understanding of its impact on
autogenous shrinkage, long-term drying, and creep behavior remains
underdeveloped. Future studies should scrutinize these areas and addi­
tionally examine the influence of LC3 on the temporal microstructural
development of the cement matrix. Simultaneously, it is crucial to
explore the behavior of LC3 under various thermal conditions to gauge
its stability and durability across its lifecycle. Consideration should also
be given to the synergistic effects of LC3 with different aggregate types,
with potential implications for optimizing LC3 concrete’s performance
and sustainability.
The mechanical behavior of LC3 has been widely evaluated, but the
role of clinker, particularly its characteristics and fineness, necessitates
further scrutiny. Future research focused on an in-depth understanding
of LC3’s additional mechanical properties, such as elastic modulus,
tensile strength, bond strength, fatigue strength, fracture toughness,
impact resistance, and different shrinkage types, will enrich LC3’s
comprehensive performance evaluation. Along with these aspects, the
influence of temperature fluctuations on LC3, including its impact on
strength development and stability, should be investigated, considering
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Science of the Total Environment 907 (2024) 167794
durability issues related to accelerated curing, high ambient tempera­
tures, and adiabatically rising temperatures. LC3’s resistance to fire also
merits extensive study, adhering to standards like ASTM E119.
Addressing these technical aspects in future research will reinforce
LC3’s broader usability and acceptance in diverse structural
applications.
Future research for the standardization and optimization of different
superplasticizers within the LC3 system must delve into a multidimen­
sional investigation encompassing compatibility with LC3’s unique
composition, effectiveness on rheological behavior, impacts on both
early and late strength development, and the implications on long-term
durability. Furthermore, understanding the time-dependent effects on
properties like setting time and bleed characteristics is equally impor­
tant. As sustainability is key in modern construction practices, the
environmental impact of employing various superplasticizers in LC3
must be evaluated.
With its versatile and promising characteristics, LC3 signifies a po­
tential replacement for OPC across a wide range of applications within
both concrete technology and geotechnical engineering. These appli­
cations extend to concreting, plastering, 3D concrete printing, roof tiles
production, prefab materials, concrete bricks, paving, soil stabilizer, and
N. Ijaz et al.
as a cement additive. Crucially, its utilization in pre-stressed and post-
tensioned concrete needs further exploration. Also, emerging evidence
supports LC3’s efficacy as a soil stabilizer for problematic soils and as an
agent in curbing heavy metal mobility. However, validation of these
prospective uses requires a shift from laboratory test outcomes to large-
scale field studies under real environmental conditions. Therefore, the
concentration of future studies should pivot toward these practical field
investigations.
While LC3’s production offers strategic benefits, including lower fuel
costs and compatibility with existing OPC infrastructure, more
comprehensive region-specific cost-benefit analyses and lifecycle as­
sessments are needed to fully evaluate its environmental and economic
implications. Future research should focus on examining the effects of
regional raw material variations on LC3 production, optimizing the
calcination process, integrating carbon capture technologies, leveraging
waste heat recovery, and exploring varied end-of-life scenarios for LC3-
based concrete. These key technical considerations, investigated via
extensive lifecycle assessments, will serve to illuminate more sustainable
and economically viable practices for LC3 production, informing its
potential optimization across diverse regional contexts.
9. Summary
LC3 is found to be a viable and environmentally friendly alternative
in the construction industry, reducing the carbon emissions traditionally
associated with OPC by a substantial margin. The important conclusions
of this study are outlined below:
• At the microstructural scale, LC3 exhibits advantageous pozzolanic
reactivity due to the incorporation of SCMs such as CC/MK and LSP.
The use of SCMs in the production of low-carbon LC3 plays a sig­
nificant role in the development of CSH/CASH, strätlingite, and
calcium aluminate hydrate phases of the AFm type. This results in
LC3 exhibiting comparable mechanical strength with reduced
porosity to that of OPC. Nevertheless, there exists a few challenges at
this stage in particular, including the adverse effects of impurities in
SCMs on the behavior of strength, as well as the need for a modified
substitution of clay with a ratio of 2:1 in areas where the availability
of kaolinite resources is limited.
• LC3 demonstrates superior behavior than OPC in mitigating alkali-
silica reactions and resisting sulfate-induced degradation, making
it advantageous for applications in aggressive environmental con­
ditions. Its heightened resilience to chloride ingress also strengthens
its suitability for marine settings or other chloride-rich contexts.
However, the LC3 resistance to carbonation necessitates further
investigation and potential supplementary protective measures to
enhance its long-term durability.
• The mechanical behavior of LC3 shows a strong similarity to that of
traditional cementitious systems. Nevertheless, the efficacy of this
performance might be influenced by multiple factors. The fineness,
dosages, and grades of the incorporated SCMs play a crucial role in
determining the final compressive strength of the formulation.
Moreover, the temperature conditions have a significant impact on
the mechanical integrity of the LC3 system. Therefore, the successful
use of LC3 as a viable substitute for conventional cement choices
depends heavily on the accurate adjustment of SCMs and the
implementation of rigorous environmental regulations. Moreover,
the superplasticizer type and dosage in LC3 is critical for combining
workability with mechanical integrity, underscoring its value as a
sustainable cement alternative.
• The LC3 technology exhibits a wide variety of applications, including
various uses such as structural concrete and the production of pre­
fabricated components like roof tiles and concrete bricks, along with
its application as a problematic soil stabilizer. The findings of
regional studies provide evidence for the reliability and durability of
the material under examination. However, optimizing calcination
25
Science of the Total Environment 907 (2024) 167794
and grinding parameters is key for scaling LC3 production, especially
given the complexity introduced by the bi-modal gradation of CC/
MK and LSP. Precise particle size control is essential for both hy­
dration kinetics and workability.
• LC3 has significant benefits from both environmental and economic
standpoints, considering higher energy efficiency and global avail­
ability of SCMs leads to a substantial reduction in its carbon foot­
print. LCA studies provide empirical evidence that supports the
sustainability credentials of a given subject. From an economic
standpoint, the compatibility of LC3 with the current OPC infra­
structure leads to a reduction in capital expenditures. However, it is
important to note that the heightened need for water and super­
plasticizers may result in an increase in operating costs. Future
research should continue exploring the optimization of LC3 systems
and extending its range of applications. This study will pave the
evidence-informed from the practical application in the field and
future studies for further development.
CRediT authorship contribution statement
Nauman Ijaz: Conceptualization, Investigation, Validation, Formal
analysis, Writing – original draft, Writing – review & editing. Wei-Min
Ye: Supervision, Project administration, Resources, Writing – review &
editing. Zia ur Rehman: Conceptualization, Validation, Formal anal­
ysis, Investigation, Writing – review & editing. Zain Ijaz: Conceptuali­
zation, Validation, Formal analysis, Investigation, Writing – review &
editing. Muhammad Faisal Junaid: Validation, Formal analysis,
Investigation, Writing – review & editing.
Declaration of competing interest
No conflict of interest exists in the submission of this manuscript.
Data availability
Data will be made available on request.
Acknowledgment
The support from the National Key Research and Development Pro­
gram of China (2019YFC1509900) and Shanghai Super Post-Doctoral
Funding is greatly acknowledged.
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