Case Studies in Construction Materials 18 (2023) e01729

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Case Studies in Construction Materials

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Case study

Life cycle assessment to produce LC3 cements with kaolinitic waste

from the Amazon region, Brazil
Euler Santos Arruda Junior *, Nállyton Tiago de Sales Braga, Márcio Santos Barata
Post-Graduate Program in Architecture and Urbanism, Federal University of Pará, Augusto Corrêa Street, 1, Brazil

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

Keywords: The present study was developed with the aim of determining the environmental impact of the
Life cycle assessment production process (cradle-to-gate) of Limestone Calcined Clay Cements (LC3) produced with
LC3 kaolinitic residues from the Brazilian Amazon, through a life cycle assessment (LCA). For this
Kaolinitic residues
purpose, 6 LC3 mixtures were prepared from combinations of clinker, gypsum, and metakaolin:
Metakaolinite
Amazon
limestone filler in the ratios 2:1, 1.5:1 and 1:1, replacing 45% and 60% Ordinary Portland Cement
(OPC). The LC3 cements were compared with two cements already produced industrially. CO2
emissions associated with the transportation of raw materials to produce LC3 cements increased
significantly, especially for the cements where 60% clinker was substituted, with CO2 emissions
up to 2–3 times higher than for the reference cements. Despite that, LC3 cements showed a
reduction in energy demand of up to 28% and total CO2 emissions of up to 38% compared to
commercial cements. In this way, the conducted study demonstrates the high environmental
potential of LC3 cements with kaolinitic residues from the Amazon region for reducing pollutant
emissions in the manufacture of cement.

1. Introduction

Population growth and economic development, especially in emerging countries, are enhancing urbanization processes through
transportation, housing, and sanitation infrastructure systems in cities. In this context, the production of raw materials is increasing to
meet the needs of the construction industry. Of note is the process of cement production, which is responsible for up to 7% of CO2
emissions into the atmosphere, making it the construction material that contributes most to the release of pollutants into the envi­
ronment [48]. This is largely due to clinker production, i.e., the burning and decarburization of calcium carbonate at 1400 ◦ C to
produce clinker, the main component of cement. This process has the highest pollutant emission rate to the atmosphere - 842.69 kg
CO2/ton of clinker, accounting for practically 94% of the total greenhouse gas emissions associated with cement production [36].
As a result, in recent decades, various institutions and representatives of citizens, politics and the private sector, have developed
plans for the sustainable growth of society and the reduction of pollutant emissions, with the aim of stopping the increase in the Earth’s
temperature and climate change [46,47].
Orsini and Marrone [33] emphasize that the use of waste and alternative materials has high environmental potential, with the
prospect of reducing up to 40% of greenhouse gas emissions. Such techniques, combined with carbon capture and storage, renewable
energy sources, and product performance optimization, would enable significant environmental improvements and greater

* Corresponding author.
E-mail addresses: euler.junior@itec.ufpa.br (E.S. Arruda Junior), nallyton.braga@itec.ufpa.br (N.T. de Sales Braga), marciobarata@ufpa.br
(M.S. Barata).

https://doi.org/10.1016/j.cscm.2022.e01729
Received 7 October 2022; Received in revised form 19 November 2022; Accepted 30 November 2022
Available online 1 December 2022
2214-5095/© 2022 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
E.S. Arruda Junior et al. Case Studies in Construction Materials 18 (2023) e01729

eco-efficiency of products commonly used in the construction chain. In turn, Reis et al. [39] emphasize that the optimization of cement
production plants, the use of alternative fuels, and the reduction of the use of clinker in cement, combined with the industrialization of
production processes and distribution of concrete and mortar, would allow a reduction in CO2 emissions of up to 56% by 2050.
In this sense, cementitious compositions of calcined clay, limestone filler, and clinker (LC3) stand out. This type of cement is
highlighted in the literature due to its high application potential, wide availability of raw materials, and high clinker replacement
capacity [1,5,32]. What distinguishes LC3 from other cements with supplementary cementitious materials is the composition of their
raw materials: limestone, as a filler, is already normally used by the cement industry for the production of clinker and is highly
available for extraction; clay, in turn, although it requires a process of thermal activation of kaolinite, requires lower temperatures than
those used in the clinker production process, which allows a reduction in the energy necessary for its production [38].
Metakaolin, a product of calcination of kaolinitic clays at up to 900 ◦ C, forms hemicarboaluminates and monocarboaluminates
when reacting with the calcium hydroxide formed during the cement hydration process in the presence of limestone filler and water,
which are products chemically more stable and prevent the formation of ettringite and favor the refinement of the pores of the cement
matrix [34,50]. In this sense, the synergy between limestone fillers and pozzolanic materials offers advantages ranging from the
possibility of obtaining cement-based materials with higher mechanical strength to the reduction of clinker consumption and the
possibility of achieving carbon neutrality [27,28].
Several studies demonstrate the environmental feasibility of LC3 cements, which have the potential to reduce the emission of
pollutants and bring benefits to industry, local economies and populations in different regions of the world [10,18,30,33].
In Brazil, there are records of the development of cements with calcined kaolin and limestone fillers by the cement industry since
1991, from flint kaolin deposits with a kaolinite content of more than 85% found in the Brazilian Amazon [7,49]. The cements
produced reached a compressive strength of over 40 MPa after 7 days. In the 2000 s, studies conducted at the Federal University of Pará
demonstrated that replacing up to 60% of the clinker with calcined kaolin and limestone in proportions of less than 2, preferably 1,
with higher limestone content, gave better mechanical properties in both initial and final ages compared to ordinary Portland cement.
This performance was attributed to the high quality of the flint kaolin from the Amazon region, which allowed the admixture of up to
30% limestone to the mix [26]. Recent research, in turn, has addressed the pozzolanic activity index, the use of superplasticizing
admixtures, and the effect of the proportion of gypsum, calcined clay, and limestone in the composition of LC3 cements, as well as the
use of LC3 cements in colored concrete [3,4,8,17,31].
In this sense, life cycle analysis (LCA), used as a mechanism to evaluate the environmental characteristics and potential envi­
ronmental impacts of products and materials, has been addressed in several studies on LC3 cements. This technique is important in that
it makes it possible to identify and compare the environmental impacts associated with the replacement of clinker by supplementary
cementitious materials, particularly in terms of reducing the emission of pollutants and lowering energy consumption [12], higher
eco-efficiency of cementitious materials [18], and lower impact on human health [13].
The Brazilian Amazon not only has the most diverse types of kaolin deposits, from low to high kaolinite concentration, but also the
generation and deposition of kaolinite-rich residues from mining and secondary kaolin processing as cover for paper. Today, these
residues have no added value as they represent an environmental burden. Therefore, it is necessary to increase the knowledge of such
materials for the production of eco-efficient cements at the regional level. Therefore, a project was developed to evaluate the feasibility
of using Amazonian kaolinitic wastes in LC3 cements, focusing initially on the chemical, physical and mineralogical properties of the
raw materials and on the mechanical performance of the cements produced. These results were published in a preliminary study [2].
Subsequently, we analyzed the life cycle of these LC3 cements with the aim of determining the environmental impact of the production
process up to the cement plant. For this purpose, a total of six cements were produced from metakaolin and limestone filler in the ratios
2:1, 1.5:1 and 1:1, replacing 45% and 60% of OPC.

Table 1
Chemical composition, fire loss, and specific gravity of input materials.
Oxides Ordinary Portland Cement Kaolin Metakaolin Limestone
(FK)

MgO (%) 3,69 0,52 0,73 2,00

Al2O3 (%) 4,32 37,60 44,77 0,73
SiO2 (%) 17,79 46,49 52,74 3,19
P2O5 (%) 0,46 – – 0,58
SO3 (%) 4,26 0,35 – 0,44
K2O (%) 0,57 – – 0, 33
CaO (%) 64,40 – – 50,37
TiO2 (%) 0,21 0,54 0,21 0,31
Fe2O3 (%) 3,73 0,66 3,79 0,62
Fire loss (%) 1,05 13,85 0,37 42,26
Specific gravity (g/cm3) 3,08 2,55 2,58 2,75

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2. Materials and methods

2.1. Preliminary observations

The experimental program of the project to which this study belongs was divided into three preliminary stages: characterization of
raw materials, production of cements with additives, and evaluation of physical, chemical, mineralogical, and mechanical properties
of binders. The numerical results were analyzed and discussed in a previous publication [2], and the main considerations are used as
input parameters for the life cycle analysis conducted in the present study.
For the development of binders, flint-type kaolin (FK), originating from deposits in the middle valley of the Rio Capim, limestone
and gypsum were used. Ordinary Portland cement (OPC), type CEM I, and Portland composite cement (PCC), type CEM II, were used as
reference binders. OPC was also used for the composition of the LC3 cements. The chemical properties and specific gravity of the
starting materials are listed in Table 1. Further details can be obtained from [2].
A total of six cements were prepared from metakaolin and limestone filler in the ratios 2:1, 1.5:1 and 1:1 with 45% and 60%
replacement of OPC. All the samples were made with same gypsum percentage (Table 2). Table 2 also shows the results of specific
gravity and specific Blaine surface area of the reference cements and LC3 cements.
From the cements obtained, mortars were developed with standard sand in accordance with national regulations (ABNT NBR
7215) [11] in a mass ratio of 1:3 and a water/cement ratio of 0.48. The mortars were tested for their compressive strength at 1, 3, 7, 28
and 91 days of age, as shown in Fig. 1 [2]. In all the ratios considered, the LC3 cements showed a high development of compressive
strength in the first 7 days, with results above 40 MPa after 90 days. The positive results were generally associated with the high
reactivity of the metakaolinite used. These results demonstrate the environmental potential of ternary cements produced from
kaolinitic waste from the Brazilian Amazon.

2.2. Life cycle analysis

After the initial characterization of the raw materials, cement pastes and mortars, the final step began, which aimed to apply the
Life Cycle Assessment (LCA) to the cement manufacturing process to determine the environmental impact of LC3 cements through CO2
emissions and the energy required for the clinker manufacturing process. These results were then compared with those of ordinary
Portland cement and Portland-composite cement, both of which are produced on an industrial scale.

2.2.1. Definition of objective and scope

At the outset, the objective and scope of the study were defined. The objective of the study was to evaluate the carbon footprint and
energy demand in the rotary kiln of LC3 cements produced in the laboratory, taking into account the increasing production of this type
of cement on an industrial scale in Brazil. The environmental data were obtained from the Eco invent v.3 database [19] and from the
bibliography available in Brazil. The Life Cycle Impact Assessment (LCIA) was made through the IPCC method for a period of one
hundred years, as indicated in the standard ISO 14067 [21].
The scope of the study considered the production of fuels, extraction and production of raw and auxiliary materials, calcination of
clinker in a rotary kiln, electricity consumption for the production of clinker and fuels, grinding, raw and auxiliary materials, and
transportation of all materials used. The analysis considered the main fuel used by the Brazilian industry, petroleum coke, which
represents about 70% of the national thermal matrix. However, there is a strong mobilization for the use of alternative fuels, with an
increase of 520% in the use of waste and biomass between 1990 and 2019 [43]. Clinker mixing, cement packaging, and transportation
to the end user were not included in the study, so the analysis is from the cradle to the door of the industry.

2.2.2. Product system

In several studies LCA specific unit processes are identified by creating diagrams that represent the production chain of the
analyzed product [35]. The product system considered in this study is based on the main processes that exist in an industrial plant, as
shown in the product system flowchart. Fig. 2 shows the product system under study and its boundaries (cradle-to-gate). In the figure,
one can see the difference between the process of Portland cement and LC3 , as well as the boundary of the studied system. For Portland

Table 2
Proportion of materials, specific gravity, and specific surface area of cements.
Type Composition (%) Specific gravity (g/cm3) Specific Blaine surface area (cm2/g)

Clinker Gypsum Calcined FK Limestone

LC3 - 50 2:1 50 5 30 15 2,86 6210

LC3 - 50 1,5:1 27 18 2,87 5850
LC3 - 50 1:1 22,5 22,5 2,88 5670
LC3 - 35 2:1 35 40 20 2,79 7370
LC3 - 35 1,5:1 36 24 2,80 6910
LC3 - 35 1:1 30 30 2,81 6410
OPC Reference 3,08 3490
PCC Reference 3,02 4830

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Fig. 1. Compressive strength of the cements tested at ages of 1, 3, 7, 28, and 91 days. In all cases, the LC3 cements showed higher strength than the
reference cements after 28 days.

Fig. 2. Stablishing the boundaries of the LCA comparative study.

cement, the extraction of fuel and raw materials, transport, clinkerization, followed by the addition of limestone and gypsum fillers, as
well as grinding, were considered. In the case of LC3 , there is an additional step, namely calcination and separate grinding of the
kaolinite clay.

2.2.3. Functional unit

Given the functional equivalence of the cements in question, 1 ton of cement produced was considered the most appropriate
functional unit to be a reference for the processes evaluated in LCA.

2.2.4. Inventory analysis

In this study, the average composition of clinker precursor meal used by Queiroz [37] to produce 1 ton for the OPC, and PCC was
considered. The composition used is close to those found in the database of countries that consider the drying process of clinker
production. The data from the literature were adopted because it was not possible to obtain data from the local industry.
Measured, estimated, and calculated data were collected in the inventory analysis. Since this is an innovative building material that
has not yet been produced on an industrial scale, it was not possible to measure data directly from the industry. Therefore, a literature
review of case studies on the carbon footprint of Portland clinker was first conducted since the production processes are similar.
It was found that most of the greenhouse gas emissions in the life cycle of Portland clinker are associated with the calcination

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processes and the energy consumption of the rotary kiln. Since many of these studies were conducted abroad, it was considered
important to also evaluate the typical energy consumption of the Brazilian cement industry and the production of electricity and fuels,
taking into account the specificities of the country’s energy matrix [6]. In addition to the data estimated in the literature, measure­
ments were selected to be performed in the laboratory, such as the CaO composition in the clinker and the mass loss of the kaolin, in
order to determine the CO2 emissions in the calcination process and the energy consumption of the rotary kiln.

2.2.5. Transport
For the supply of raw materials, the distances between the cement plant and the respective raw material deposits were determined
(Fig. 3). The cement plant is located in the municipality of Primavera (PA), which is close to the limestone deposits, about 5 km away.
For iron ore, the distance of 813 km between Parauapebas, in the south of Pará, and Primavera was considered. For FK, the distance
between the mine site in Ipixuna and the processing plant is 228 km. In the case of gypsum, a distance of 649 km to the municipality of
Codó in Maranhão was considered. For the calculation of transport-related CO2 emissions, the total distances for each raw material
were doubled, since we considered the round trip.
For the extraction of limestone and FK, extraction data using wheel loaders were used, kept constant for calculation parameters. For
the transport of FK, extra-heavy trucks of 72 tons of consumptions taken from ECOINVENT, and Costa [14,19] were used, while for
limestone, trucks of up to 45 tons were stipulated [14].

2.2.6. Estimation of CO2 emissions during the calcination process

Estimates of emissions from Portland clinker precursor raw meal were determined using Eqs. (1 and 2), modified from the
Intergovernmental Panel on Climate Change methodology [23]. The same equations were used to calculate emissions from the clinker
process for LC3 cements. In the case of LC3 , the CaO content determined by X-ray diffraction (FRX) for the OPC was considered, using

Fig. 3. Distance from the raw materials to the cement plant.

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the proportional amount of CaO% to the incorporated substitutes as the basis for the calculations [2].

CO2Portland (kg/ton) = CtPortland*%CaO* (100− % Addition) (1)

44 10
CtPortland = [ ∗ ] (2)
56 (100 + %CaSO4)

Where:
CO2Portland = CO2 emissions in kilograms per ton of cement;.
CtPortland = constant calculated from Eq. (2);.
%CaO = Percentage of calcium oxide in the flour;.
%CaSO4 = Percentage of calcium sulfate in the sample;.
%Addition = Percentage of mineral additions incorporated.
The estimates were made for the production of 1 ton of cement, taking into account the addition of gypsum as well as the mineral
additions of limestone filler in PCC, as well as limestone filler and calcined clay in LC3 cements.

2.2.7. Estimation of energy consumption in the rotary kiln

The estimate of energy demand (DE, in GJ ton-1 cement) for the production of cement is based on the energy required to reach the
burning temperatures: 1450ºC for Portland clinker and 800ºC for metakaolinite. The values for energy consumption in the calcination
of clinker and kaolinite clay were obtained from the local industry per ton of calcined material. The energy demand (DE LC3, in GJ clay-
1) for the production of LC3 cements and OPC and PCC cements can be estimated using Eq. (3).

DE = [% Clinker Port⋅*DEPortand] + [%MK*DEmc] (3)

Where:
DE=Energy requirement of specific cement (LC3, OPC or PCC) in GJ Tonne-1 of cement.
% Clinker Port = Percentage of clinker in the cement;.
DEPortland= Energy requirement in GJ tonne-1 of clinker;.
% MK = Percentage of metakaolin in the cement;.
DEmc = Energy demand in GJ tonne-1 of metakaolin.

2.2.8. Comparative assessment of environmental impact

The evaluation was performed comparatively by relating the carbon footprint (CO2 emissions) and energy required for the
calcination process of the LC3 cements produced in the laboratory and the OPC and PCC cements, used as references.
To evaluate the efficiency of the LC3 binders more objectively, the adjusted clinker factor (clinker/cement ratio) proposed by
Damineli [15] was used (Eq. 4), to which a correction factor was applied to the percentage of calcined clay of each cement. This factor
assumes that the burning of fuels in clinker represents only 40% of total emissions [49], since there is no decarbonization fraction in
burning calcined clay and only 70% of the relative energy is consumed in calcination of clinker. Therefore, 70% of the relative energy
of 40% of total emissions is equivalent to a correction factor of 28%. In addition, two indicators of binder efficiency and global
warming proposed by Damineli et al. [15] were adopted. These are the CO2 intensity index (cics) (Eq. 5) and the binder intensity index
(bics) (Eq. 6), both of which are associated with compressive strength after 28 days. Normally, such indicators are applied to concrete,
but in the case of this study, the methodology was adapted for mortar. The aim was to comparatively evaluate the efficiency of LC3 and
reference cements by analyzing these two indicators together, in order to provide further guidance in the selection of the most suitable
cements from an eco-efficiency point of view.
(%Clinker + (%Calcined Clay ∗ 28%))
Clinker factor = (4)
Cement
c
cics = (5)
rc

l
bics = (6)
rc

Where:
%Clinker = % of clinker in the adjusted binder;.
%Calcined Clay = % of calcined clay.
Cement = normalized amount of cement (100%);.
c = total CO2 emissions (kg.m-3);.
rc = compressive strength (MPa), determined in Arruda Junior and Barata [2,7];.
l = total binder consumption (kg.m-3);.
Binder intensity index and CO2 intensity index allow a quick and objective comparison of different mixes. The higher the cics value,
the lower the environmental efficiency against global warming. Conversely, the higher the bics value, the more binder is required to
perform the same function, resulting in lower eco-efficiency, and serving as an economic indicator. Taken together, the two indicators

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provide a comprehensive approach to cement efficiency and use.

3. Results and discussion

3.1. Environmental impact of transport through CO2 emissions

The amount of raw meal needed to produce one ton of clinker is 1560 kg (local industry data), of which 95% is limestone, 4% is FK
and 1% is iron ore, according to the manufacturer. The use of heavy and extra heavy trucks was considered when calculating CO2
emissions related to the transport of raw materials. Table 3 shows the transport distances, the capacity of each truck, the fuel con­
sumption, the CO2 emission factor of the fuel and the total CO2 emissions per ton of transported raw materials.
Using the data on CO2 emissions per ton, it was possible to calculate the CO2 emissions generated by transporting raw materials to
produce one ton of cement (Fig. 4). The calculation of the quantities considered the shoaling of the material and the average annual
humidity of about 20% (18% in summer and 23% in winter) (data provided by the local industry).
In the specific situation of this work, using a kaolinitic residue far from the cement plant, there was a significant increase in CO2
emissions associated with the transport of LC3 cements raw materials, especially for those with 60% clinker replacement (LC3− 35),
whose percentage of calcined clay varied between 30% and 40%. The CO2 emissions of LC3 − 35 (2:1) were three times higher than
those of PCC. The smallest difference in emissions between LC3 and PCC occurred with a clinker replacement percentage of 50% and a
metakaolin to limestone ratio 1:1, since this cement has the lowest percentage of FK among the LC3 cements studied - about 22.5%.
Since the round trip of the vehicles transporting the raw materials was considered, the results presented are consistent with those of
similar studies: Malacarne et al. [30] found that the environmental impacts associated with the transportation are significant for
distances greater than 500 km. Stafford et al. [44], in turn, highlights the potential impact of transportation for cement production in
Brazil, as about 95% of transportation logistics are overland, with the use of trucks, over distances that can vary significantly
depending on the origin of the raw materials considered.
It is worth emphasizing that the transport distance of the starting materials has a direct effect not only on CO2 emissions but also on
the cost of the final product. Unpublished results show that for the Amazon region, all mixtures presented in this research are
economically viable with clay being transported up to 200 km by road compared to reference cements, similar to results found in the
literature [9].
The results show the importance of the proximity of the raw material to the industrial cement plant, as in the case of the LC3 , which
requires the proximity not only of the limestone deposit but also of the kaolinite clay deposits.

3.2. Estimation of energy consumption in the rotary kiln

The energy consumption in a rotary kiln was determined from the energy demand data of the raw materials of the mixtures. Table 4
shows the energy consumption data of Portland clinker and metakaolinite (MK) provided by the local industry.
For the LC3 cements, the data determined in the laboratory were adopted. The measured mass loss during calcination of kaolinitic
clay was 12.82%. In this sense, 1 ton of metakaolinite would be produced from 1282 tons of raw kaolin. The calculation of mass loss
was thus weighted according to the substitution contents, considering the mass loss of 35.89% of Portland clinker at 1450 ºC and of 12.
82% in the calcination of kaolin at 800 ºC to obtain metakaolinite.

3.3. Energy consumption

From these data, it was possible to estimate the energy demand (DE LC3, in GJ Ton-1 cement) of the production of LC3 in com­
parison to OPC and PCC, applying Eq. 3. The values of the energy consumption of the reference cements and LC3 produced in the
laboratory are presented in Fig. 5.
The energy demand of LC3 cements is lower compared to the cements OPC and PCC. For OPC, the percentage reduction in energy
demand of LC3 50 and 35 was 30% and 40%, respectively. For PCC, the reduction was lower, ranging from 10% to 25%. It should be
noted that these reductions in energy consumption are quite significant, since direct heating (clinkerization) represents about 79% of
energy consumption in the Brazilian cement industry [6]. Recent studies address the performance of supplementary cementitious
materials for variations in energy consumptions [40] and emphasize that the high mechanical performance of SCM can translate into
relevant environmental benefits such as lower CO2 emissions and reduced damage on human health, even when significant increases in
energy consumption are estimated.

Table 3
Fuel consumption and CO2 emissions per ton transported.
Material Distance Round trip distance Truck capacity Consumption (L/Ton/ Fuel consumption CO2 emission (kg/L) – CO2/
(km) (km) (Ton.) km) (L) Diesel Ton

Limestone 4 8 45 0,01216 1 4,38 3,22 0,31

Kaolin 228 456 72 0,0114 1 374,28 3,22 16,63
Iron ore 813 1626 72 0,0114 1 1334,62 3,22 59,32
Gypsum 649 1298 72 0,0114 1 1065,4 3,22 47,35

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Fig. 4. - CO2 emissions (kg/ton of cement) associated with the transport of raw materials.

Table 4
Data for estimating energy consumption in clinker production.
Raw material LOIa (%) kcal/kg Energy consumption (GJ/Ton clinker)

Portland clinker 35,89 740 3,10

Metakaolinite 12,82 450b 1,88
a
Loss of ignition.
b
According to Zampieri [49], the energy consumption related to clay calcination varies from 450 to 650 kcal/kg of pozzolan.

Fig. 5. Energy consumption for calcination and reduction of energy consumption of LC3 cements compared to reference cements.

The reductions are not linear with the percentage of replacement or with the clinker factor[12] . This is because LC3 uses calcined
clay as one of the mineral additives, which, unlike blast furnace slag (BFS), fly ash (FA), limestone filler, natural pozzolans, and others,
requires thermal activation. Although no decarbonization occurs when clays are burned, they require the combustion of fuel, which
accounts for between 50% and 70% of the energy required to calcine clinker. For this reason, its attenuating effect on energy demand is
lower compared to other pozzolans and is not proportional to its clinker replacement potential; it also requires investment in ma­
chinery and equipment [12]. For the LC3 - 50, where the clinker replacement percentage was 45%, reductions between 28% and 33%

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were achieved, while for the LC3 - 35 with 60% replacement, energy demand was reduced between 37% and 44%. The results are more
optimistic than those of Bumanis et al. [12], which found that a 75% replacement of clinker with alternative materials could result in
about a 30% reduction in energy consumption.
Considering the data, LC3 compositions with higher percentages of calcined clay show improvements in mechanical performance
and properties of concretes and mortars, but mixtures with higher percentages of incorporated limestone such as LC3 - 50 (1:1) and
LC3 - 35 (1:1) not only have the lowest energy demand for the replacement levels analyzed, but also achieve satisfactory mechanical
strength and meet the requirements of the construction market.
The results presented here are in contradiction to the literature recommendations, which are LC3 - 50 at a ratio of calcined clay to
limestone of 2:1, without the need to use kaolinitic clays with a kaolinite content greater than 65% to reduce the cost of acquiring clays
and, consequently, the cost of cement production [41]. In the case of the Amazon, which has a large supply of kaolinite-rich clays of
secondary origin, the difference is due precisely to the use of these clays, which made it possible to obtain highly reactive metakaolinite
and allow larger addition of limestone without significant loss of strength.

3.4. Estimate of CO2 emissions

Eqs. (1 and 2) were used to estimate precursor raw meal emissions for Portland clinker. The CaO content used in Eq. (1) was 64.4%,
obtained in the XRF (Table 1), which represents the full composition of the Portland clinker oxides produced from raw meal Portland.
The same equations were used to calculate the emissions from the clinker process in the LC3 produced, using the proportional
amount of CaO% to the degrees of substitution incorporated as the basis for the calculations performed. The amounts of CO2 resulting
from the chemical reaction of CaCO3 decomposition according to Eqs. (1 and 2) are shown in Fig. 6.
In parallel with the laboratory studies, the LCA of Brazilian Portland clinker was developed based on national industry estimates [6]
and internationally recognized databases [19]. Based on this analysis, it was possible to estimate the carbon footprint of Portland
cement produced in Brazil. Using the comparative data obtained in the laboratory for the LC3 cements, ordinary Portland cement and
Portland-composite cement, shown in Figs. 4, 5 and 6, the carbon footprint data for the LC3 cements were obtained (Figs. 7 and 8).
Fig. 7 shows the CO2 emissions of the individual cements evaluated and indicates the contribution of each process stage. Fig. 8, in turn,
allows an evaluation of the share of the individual steps in the total amount of CO2 emissions of the cements investigated. Other energy
consumptions of the industry, such as lighting and process heat, were kept constant in the analysis.
As shown in Fig. 7, reducing the proportion of clinker in the composition of cements reduced CO2 emissions, particularly those
associated with calcination, even in cements with higher percentages of calcined clay incorporation, the emissions from the production
of this pozzolana are 72% lower (Eq. 4) when they occurred with the same mass of clinker incorporation. It was also found that for
LC3 type cements, CO2 emissions related to fuel combustion and transport of raw materials play a greater role than for the reference
cements, even if they are small compared to the overall scenario (Fig. 8). Results for carbon dioxide emissions from the reference
cements ranged from 657 to 810 kg CO2/ton. cement produced. In the reference literature, these indices ranged from 632 to 950 kg
CO2/ton. cement for general applications [36].
LC3 cements, in turn, show a significant reduction in CO2 emissions compared to reference cements. Compared to PCC, the current
technological stage of cement production in the Amazon region, the reductions for LC3 − 50 cements with 45% clinker replacement
vary between 20% and 22%, depending on the ratio between MK and limestone, and between 35% and 38% for a clinker replacement
of 60% (LC3− 35). The results are consistent with the observations of Malacarne et al. [30] in a study that found that the widespread use
of LC3 type cements can lead to a reduction in greenhouse gas emissions of up to 38% compared to conventional cements. Maddalena
et al. [29] observed a 23–55% reduction in the carbon footprint of cements by introducing alternative materials in their composition.
The reductions are significant, but to a lesser extent than when using other mineral additions, such as BFS and FA [16]. Although

Fig. 6. CO2 emissions (kg/ton of cement) from the chemical reaction of decarbonization of calcite.

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Fig. 7. CO2 emissions of production for each cement evaluated.

Fig. 8. Contribution of each step of the process to the total CO2 emission for the cements evaluated.

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E.S. Arruda Junior et al. Case Studies in Construction Materials 18 (2023) e01729

the largest share of CO2 emissions is associated with the decarbonization of calcite, the share of combustion is also significant and, in
the case of clays, corresponds to between 50% and 70% of the fuel used in clinker production, as shown by local industry data.
To illustrate the effects of burning calcined clays in LC3 , the percentages of the two major constituents are compared: Decarbu­
rization and fuel combustion for each of the cements. Calcite decarburization and fuel combustion account for 58% of the total CO2
emissions for OPC and 38% of the total CO2 emissions for PCC. However, for LC3 cements, these proportions reach similar levels with
increasing clinker replacement and limestone content: for LC3 - 35, for example, decarbonization corresponds to 47% and fuel
combustion to 45% of total CO2 emissions.
According to the Cement Technological RoadMap published in 2019 by ABCP and SNIC [42], the national cement industry’s CO2
emission reduction targets for achieving levels that limit global temperature rise by up to 2 ◦ C in the long term should be 480 kg
CO2/ton of cement by 2030, 410 by 2040, and 310 kg CO2/ton of cement by 2050 (Fig. 9). If the changes are not effectively imple­
mented, the temperature increase threshold of up to 6 ◦ C will be reached.
Assuming a hypothetical scenario based on the results obtained in this work for mechanical resistance, energy demand and CO2
emissions, using LC3 - 50 (1:1) for the industrial segment corresponding to 34% of the production volume and LC3 - 35 (1:1) for the self-
building segment corresponding to 66% of the market, the weighted average of CO2 emissions in this scenario would be 433 kg CO2/t
of cement, reaching the target by 2040. It is possible to achieve the levels set for 2050 in the short term through the simultaneous use of
LC3 and alternative fuels such as biomass, whose CO2 emissions would be considered zero given the balance between the carbon
emitted by the extracted biomass and the carbon absorbed during the growth of new plants [22]. The combination of biomass and
LC3 could fulfill the goal of the cement industry in the Amazon region (northern region), since the state of Pará is responsible for more
than 50% of cement production in Amazon [42] and has great potential for biomass utilization and wide availability of high purity
kaolinitic clays with kaolinite content above 85%.
Another possibility would be the use of natural pozzolans available in the region, which are rarer and occur only locally, or by
mechanical activation of kaolinites [24,25,45], given the high degree of defects in the crystalline structure of some clays in the region
and the low CO2 emission factor of the Brazilian energy matrix, which is mainly based on hydropower plants. This technological
alternative is particularly promising if the industry adopts the energy cogeneration system through heat recovery from chillers, vertical
mills, and waste heat recovery plants (WHR), with a potential for electricity savings between 20% and 30% [42].
Another parameter that has been set as a target in the RoadMap is the reduction of the clinker factor from 0.67 to 0.52 by 2050. This
index is extremely relevant because clinkerization is the main factor associated with climate change because of cement production
[13]. This indicator is often used for binders using BFS, FA, or natural pozzolans, which, because they are industrial wastes or do not
need to be burned, are considered mineral additives with "zero" emissions, which significantly reduces the clinker factor. However, in
the case of LC3 , the clinker factor does not reflect the specifics of using calcined clays in combination with limestone, as this pozzolan
does produce significant CO2 emissions, but not to the same extent as clinker. In addition, the calcined clays chemically interact with
the limestone, increasing the efficiency of the binder, without the limestone filler being considered in the clinker factor.

3.5. Binder intensity index (bics) and CO2 intensity index (cics) indicators

Fig. 10 shows the indicators obtained with the LC3 cements and the reference cements. Looking at the clinker factor of LC3 cements
and comparing it with the target set in the RoadMap report [42], we conclude that to achieve the parameters set between 2030 and
2040, it would be sufficient to use LC3 − 50, gradually changing the proportions of MK and limestone over the years. From 2040, the
use of LC3 35 would be required.

Fig. 9. Key indicators for the Brazilian cement industry to reach 2 ◦ C by 2050.
Adapted from SNIC [42].

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Fig. 10. LC3 efficiency indicators. Considering the compressive strengths reached at 28 days, the LC3 cements showed great environ­
mental potential.

The joint analysis of bics and cics provides a more comprehensive approach to cement use efficiency than the clinker factor. When
analyzing the cics and bics of the cements in this study, there are no significant differences between the LC3 , either at 45% or 60%
clinker replacement. The results reflect the high efficiency of these binders and the potential to reduce global warming compared to
composite cements with limestone filler, which are currently the benchmark. The bics value of PCC was 8.7 kg.m-3/MPa, and 12.33 kg.
m-3/MPa in OPC. For LC3 cements, the bics ranged from 5.23 to 5.88 kg.m-3/MPa, which is considered by Damineli [15] as a realistic
target for concretes with normal strengths (up to 50 MPa) in the future. For the cics, the values were also reduced and vary between
4.90 kg.m-3/MPa for the LC3 - 50 (2:1) and 5.55 kg.m-3/MPa for the LC3 - 35 (1:1).
Damineli et al. (2013) states that low cics, of the order of 1.5 kg.m-3/MPa, is achieved only for strengths above 50 MPa in com­
bination with high bics, i.e., with high BFS or FA substitutions. However, since the availability of these additives is limited regionally,
they are not considered a viable solution, especially in the Amazon region of northern Brazil, where there are no steel mills or
thermoelectric plants. The ideal condition would be a low cics associated with a low bics, which, according to the authors of the
methodology, can only be achieved with a high clinker replacement and by optimizing the mix.
Figs. 11 and 12 were adapted from Damineli et al. [15] and allow the comparison of the results obtained in this study with ref­
erences in Brazil and in the international literature. As can be seen in Fig. 11, based on the binder index of the LC3 cement of this study
combined with the compressive strengths obtained, the cements with kaolinitic residues from the Brazilian Amazon are among the
lowest observed bics indexes, with mortar consumption in the range of 250 kg/m3 or less. The cics index of the LC3 cements also showed
consistent results with those in the reference literature and was lower than the values of the reference cements in this study.
The bics and cics values in LC3 cements were achieved by the high efficiency of the mixture of calcined clay and limestone. The
combination of the two additives, one active and the other inert, produces a stronger synergistic effect than the use of both additives
alone in the binary system with Portland cement.
The results of the indicators show that it is indifferent whether a clinker replacement of 45% or 60% or a ratio of MK:limestone of
2:1 or 1:1 is used. However, the analysis is not limited to the numerical results obtained. A more comprehensive evaluation is required,
including criteria for mechanical strength, carbon footprint, and economic analysis of production.
The LC3 50 (2:1), as expected, was the one with the highest compressive strengths due to the ratio of MC: limestone being ideal
from a stoichiometric point of view to form monocarboaluminates and C-A-S-H in greater amounts.
However, it is worth mentioning the performance of LC3 50 (1:1) with a greater dilution effect, due to the greater amount of
limestone in the mixture (22.5%) and a lower percentage of calcined material, both clinker and MC, which also showed resistance
superior to the reference cements already at 7 days of age (Fig. 1). The high concentration of kaolinite (97%) in the FC led to the
production of a highly reactive MC, the phase responsible for the pozzolanic activity of calcined clays, allowing limestone in­
corporations above the ideal stoichiometric calculation not damage the initial and final strengths, which were 38 MPa at 7 days and
49 MPa at 28 days, quite satisfactory for employment in the segment of the construction chain that industrializes concrete production
and mortar. As this segment represents in percentage terms around 25–30% of the Construction market civil engineering, the
replacement of composite cement with limestone filler by LC3 50 (1:1) may contribute significantly substantial contribution to
reducing the carbon footprint of the cement industry.
From an economic point of view and considering the implementation and operating costs, it is much more interesting to reduce the
proportion of calcined clay in the production line in order to reduce fuel consumption, processing operations and combustion, as well
as the daily production volume of pozzolan, all of which are closely related to the sizing and acquisition of the necessary equipment for
burning and grinding clays. The preparation of limestone filer is far less complex and costly than that of the pozzolan, which requires
calcination. Since there is no difference in efficiency between the binders, the choice should be the LC3 with the lowest ratio between
MK and limestone, i.e., 1:1.

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Fig. 11. Binder Index (bics) for different compressive strengths, obtained in Brazilian (left) and international (right) studies.
Adapted from Damineli et al. [15].

Fig. 12. CO2 index (cics) for different compressive strengths, obtained in Brazilian (left) and international (right) studies.
Adapted from Damineli et al. [15].

4. Conclusions

The present study was developed with the aim of determining the environmental impact of the production process of LC3 cements
made with kaolinitic residues from the Brazilian Amazon through a life cycle assessment. The results were compared with those of
cements already produced on an industrial scale. Among the conclusions of the analyzes conducted, the following should be
highlighted:

CO2 emissions related to the transport of raw materials to produce LC3 cements increased significantly, especially for the cements
where 60% clinker was replaced, with emissions two to three times higher than for the reference cements. Although they did not
have a major impact on overall emissions, the results show the importance of LC3 cement deposits and sediments being located
close to the industrial cement plant;

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LC3 cements generally show a 10–40% reduction in energy demand compared to reference cements. In this sense, LC3 cements with
a higher limestone content (LC3 - 50 1:1 and LC3 - 35 1:1) showed a lower energy demand and a satisfactory mechanical perfor­
mance, thus offering a greater environmental potential. This is due to the fact that the Amazonian clays are rich in kaolinite with a
high reactive potential. These results are in contradiction with some recommendations in the literature that consider the use of
LC3 − 50 cements with a higher proportion of calcined clays (2:1) rather than limestone to be more beneficial, without the need to
use kaolinitic clays with a kaolinite content greater than 65%;
LC3 cements show a significant reduction in CO2 emissions compared to reference cements, with up to 38% less CO2 emissions. In
absolute terms, the emissions of LC3 − 50 and LC3 − 35 averaged 520 and 415 kg CO2/ton of cement, respectively. For the reference
cements, they varied between 657 and 810 kg CO2/ton. Cement;
The use of LC3 cements and alternative fuels would enable the industry to meet the emission levels of polluting gases set by 2050 to
mitigate the impact of climate change on the planet.

Finally, considering aspects such as compressive strength, energy demand during calcination, CO2 emissions, eco-efficiency in­
dicators and a differentiated analysis by type of construction segment, it can be said that LC3 cements with 45% clinker replacement
with equal proportions of MK and limestone (LC3 50 1:1) are most suitable for the industrial segment of construction, while LC3 with
60% clinker replacement, also with equal proportions of MK and limestone (LC3 35 1:1), are suitable for the self-building segment.
Obviously, a more detailed economic analysis must be carried out, considering aspects related to the investment to be used, return on
investment, operating costs, logistics, availability, distance and quality of deposits, and economic feasibility of using kaolinitic residues
between other aspects not covered in this work.

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to
influence the work reported in this paper.

Data Availability

Data will be made available on request.

Acknowledgements

The authors thank the Federal University of Pará (UFPA) and the Post-Graduate Program in Architecture and Urbanism (PPGAU).
This research did not receive any specific grant from funding agencies in the public, commercial, or not-for-profit sectors. The authors
are thankful to the PROPESP/UFPA (PAPQ), Brazil, for providing the required funds to support the publication of this article.

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