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Cement and Concrete Research xxx (xxxx) xxx–xxx

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Cement and Concrete Research


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

Carbon dioxide reduction potential in the global cement industry by 2050


Sabbie A. Millera,⁎, Vanderley M. Johnb,⁎, Sergio A. Paccac, Arpad Horvathd
a
Department of Civil and Environmental Engineering, University of California, Davis, United States
b
Department of Construction Engineering, University of São Paulo, Brazil
c
School of Arts, Sciences, and Humanities, University of São Paulo, Brazil
d
Department of Civil and Environmental Engineering, University of California, Berkeley, United States

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

Keywords: This paper, which is a contribution to the UNEP series on Eco-Efficient Cements, examines the role of material-
Carbon dioxide emissions based solutions to reducing CO2 emissions from cement production considering factors that could influence
Alternative cementitious materials implementation. Global urbanization has led to an increase in demand for cement and cement-based materials.
Global mitigation strategies With its growth in consumption, the associated CO2 emissions from its production are raising concern. However,
Bulk cement
the role of mitigation strategies in a global context that account for regional material availability and degree of
Bagged cement
market adoption have yet to be considered. This work shows that the 2 °C scenario targets for 2050 can be met
Calcined clays
Alkali-activated materials through increased use of calcined clay and engineered filler with dispersants. The introduction of new Portland
Fillers clinker-based cement alternatives, use of alkali-activated materials, and improvement of efficiency of cement use
could further contribute to reduction goals. There are currently-available technologies for reduction that could
be rapidly implemented.

1. Introduction environmental improvements to cement manufacturing through appli-


cation of life-cycle assessment (LCA) methodology (e.g., [10]), as well
As urbanization changes the global landscape, demand to expand as examination of the role of alternative cementitious materials on re-
the built environment is growing. This demand reflects both a need to ducing the environmental impacts from cement (e.g., [11,12]). In such
repair infrastructure (e.g., roads, buildings) in countries where old studies, consideration has been given to the role of concrete strength
systems have lost functionality and a need to build new infrastructure (e.g., [13–15]) and research has been conducted to examine the role of
in countries that are expanding current systems [1]. To meet this in- material properties on guiding concrete mixture proportions (e.g.,
creased demand in infrastructure systems, production of the most [16–19]). These studies, however, lack a global perspective. The pre-
common infrastructure materials has grown, with the pace of cement mier work in the field of global assessment was the 2009 World Busi-
production outstripping not only all other materials, but also popula- ness Council for Sustainable Development (WBCSD) and International
tion growth [2–5]. This upturn in materials production is a cause for Energy Agency (IEA) Cement Roadmap [20], which examined the role
concern regarding environmental impact. In 2012 alone, the production of several mitigation methods and the amount of raw materials avail-
of cement was approximately 3.8 giga tonnes (Gt), equivalent to ap- able, globally and regionally. In addition to this work, a study by Miller
proximately 3.2 Gt of CO2 emissions worldwide, approximately 8% of et al. [6] considered the role of using currently available methods to
the annual anthropogenic CO2 emissions [6]. In three years, the pro- reduce greenhouse gas emissions from cement and concrete at a global
duction of cement, globally, rose to over 4.5 Gt [7] and, with it, so too scale by using LCA methodology. Beyond these, little consideration has
did CO2 emissions. been given to the role any set of mitigation strategies would have when
With increased awareness of the CO2 emissions from cement pro- scaled up to the world to the best of the authors' knowledge. Further,
duction at this large scale, there has been increased focus on reduction existing research on improvements to mixtures has failed to consider
strategies, including a variety of approaches such as consideration of global impacts on material flows as well as mitigations best suited to
equipment efficiency, fuel substitution (including increased use of developing regions, which are expected to have high rates of cement
biofuels), strategic concrete composition for specific applications, use of production in the coming years.
alternative raw materials, and use of material substitutes [8,9]. Re- In this research, which is a contribution to the UNEP series on Eco-
search in this area has also included examination of the role of Efficient Cements, the global use of material-based technologies that


Corresponding authors.
E-mail addresses: sabmil@ucdavis.edu (S.A. Miller), vmjohn@usp.br (V.M. John).

http://dx.doi.org/10.1016/j.cemconres.2017.08.026
Received 22 November 2016; Received in revised form 14 April 2017; Accepted 29 August 2017
0008-8846/ © 2017 Elsevier Ltd. All rights reserved.

Please cite this article as: Miller, S.A., Cement and Concrete Research (2017), http://dx.doi.org/10.1016/j.cemconres.2017.08.026
S.A. Miller et al. Cement and Concrete Research xxx (xxxx) xxx–xxx

are capable of reducing CO2 emissions in the cement industry are ex- [25]. New approaches to the inclusion of limestone filler based on en-
amined. These methods are presented in the context of 2 °C scenario gineered filler and dispersion, which allow for a reduction of water,
reduction targets set out by the IEA for cement production accounting make 70% of binder substitution possible. However, because of the
for projections in growth of cement consumption to the year 2050 [21]. water reduction, the net benefit is lower than the clinker fraction in the
We explore material-based strategies to reduce emissions that are not cement. Therefore, we estimate that when fully developed, the tech-
dependent on carbon capture and storage (CCS) technologies, which nology may allow for an average net benefit equivalent to a clinker
have not been fully developed and may be cost-prohibitive. Further- substitution of 35%.
more, this work examines the role of market adoption and discusses the
ability for different regions of the world to implement material-based 2.1.3. New cements and clinkers
mitigation strategies based on considerations for currently known ma- The second group of materials assessed to reduce CO2 emissions
terial reserves. from the production of concrete are (a) alkali-activated binders, based
on Provis [26], (b) Belite-Ye'elimite-Ferrite clinkers (BYF), based on
2. Materials and methods Gartner and Sui [27], and (c) Carbonatable Calcium Silicate clinkers
(CCSC), based on Gartner and Sui [27]. Use of these materials is not as
2.1. Materials assessed for potential contribution to carbon dioxide well established in industrial practice; although incorporation of some
reduction of these new cements has started for certain applications (e.g., use of
geopolymers in concrete construction in Australia [26]). Due to the
2.1.1. Baseline case maturity of these technologies, availability of raw materials, and po-
While there are multiple ways of reducing CO2 emissions from the tential change in cost relative to the production of OPC, it is possible
production of concrete, this assessment focuses on the role of material these materials will face more limited market application than the first
alternatives. The first material that will be considered in this assessment group of materials discussed. Nevertheless, since potential use of this
is the baseline production of ordinary Portland cement (OPC). Based on second group is more developed than CCS technology for the cement
projections for production of common supplementary cementitious industry, this assessment (i.e., at production levels and CO2 emission
materials (SCMs), such as fly ash or slag, cement production can be reduction goals for the 2 °C scenario in 2050) assumes that incorpora-
estimated to reach the ~71% clinker fraction goal by 2050 set by the tion of these materials could be implemented at lower cost than CCS
Cement Roadmap [20], with limestone filler accounting for approxi- technology.
mately 10% of cement by mass. If a 50% average clinker fraction were Alkali-activated binders and geopolymers can use several sources of
targeted instead, it is possible to estimate that use of fly ash and/or slag silicates and alumina with a variety of activators to produce cementi-
with limestone filler would have 40% of the cement market share. For tious material [28]. They can harden quickly, and studies have shown a
the remaining 60% of the market, the cement could still contain 10% potential for reduction in CO2 emissions relative to OPC [15]. As a
limestone filler, but other SCM use could be explored. result of the range of material inputs and fuel sources that could be used
In this assessment, OPC is modeled as containing 85% clinker, 5% in the production of these materials, a broad range is associated with
gypsum, and 10% limestone by mass. The quantity of replacement of their ability to alter the CO2 emissions from common cement produc-
this OPC by alternative materials was used to determine CO2 emission tion [15]. If fly ash and slag are used as the sources of the solid pre-
reduction values. Clinker substitution by filler, calcined clay and filler, cursor, a low CO2 footprint for the production of geopolymers can be
or use of alternative cements will be developed as an addition to the found when these material inputs are modeled as byproducts from other
10% limestone content and 5% gypsum content already consider in the industries with little to no associated emissions from production. The
mitigation scenario. main limitation to this method of producing geopolymers is that it is
dependent on diverting flows of fly ash and slag that could otherwise be
2.1.2. Innovative use of currently applied materials used as supplementary cementitious materials with conventional ce-
The first group of materials assessed can act to partially replace ments made from Portland clinker, so limited additional mitigation is
Portland clinker through innovative versions of already in-use SCMs. expected. However, other industrial by-products or co-products could
The materials considered at this phase of assessment are: (a) the com- also be used as the solid precursor to geopolymers if they can provide
bination of calcined clay with limestone filler, based on Scrivener et al. adequate sources of silicates and alumina; further, fly ash that might
[22], and (b) increased use of engineered filler with dispersants, based not be suitable as an SCM could be viable as a solid precursor for
on John et al. [23]. These materials have a high potential for scale-up geopolymers [26]. These products have the potential to offer low CO2
by industry because these materials utilize globally available raw ma- embodied materials for the production of alkali-activated materials.
terials, require modest changes in existing production lines, and require Because at a global scale, mitigation strategies for CO2 emissions from
no new quarries or large investments. As such, the main limitations for the production of concrete often assume use of fly ash and slag flows as
their adoption are those imposed by technical performance of cement in cementitious materials [20], this assessment considers use of calcined
different applications and the familiarity of industry and clients. clay as the source of silicates and alumina as well as other industrial
With regard to the calcined clay pozzolans, CO2 emissions benefits byproducts. When other sources of silicates and alumina are modeled,
are expected both from the ability to reduce raw-material derived CO2 such as using calcined clay as an input, the mitigation potential for
emissions as well as from reducing thermal energy required during alkali-activated materials drops. However, with improved production
processing. This assessment considers calcined clay combined with methods for alkali-activators, lower CO2 emissions from the production
clinker-based cement and limestone filler, which not only dilutes the of the associated cements can be expected. Evaluations of availability of
binders, but also increases chemical reaction and improves the rheo- materials for this research are cautious and are based primarily on the
logical behavior of the system. In this work, it is assumed that as a current availability of resources. Consideration is mainly given to
global average it is possible to replace 50% of the clinker by a combi- economic reserve, availability at low cost as byproducts, rather than
nation of between 25 and 35% of calcined clay and 15% of limestone reserve base, physical availability [29]. Future use of SCMs in geopo-
filler. lymers could change if the market were prepared to pay for their pro-
The second innovative use of currently applied materials considers duction or in markets where the availability of SCMs exceeded that of
increased use of fillers, here modeled as limestone filler. The use of the resources to produce OPC. Of course, any changes in production
limestone filler, with purity similar to clinker grade, is currently well that could affect allocation of environmental impacts would then need
established at about 7% global average [24]. Data show it can be in- to be included in calculation of emissions generated.
creased to about 10% without significant loss of strength due to dilution For the production of BYF clinkers, there is a twofold benefit

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S.A. Miller et al. Cement and Concrete Research xxx (xxxx) xxx–xxx

relative to the production of OPC. First, the BYF clinkers require a these materials were based on calculations by Gursel and Horvath [33]
different raw material feed than typical Portland clinkers, namely, they using regional electricity mixes for processing of clinker and other ce-
require lower limestone content [27]. This reduced limestone in the mentitious products based on calculations by Miller et al. [6]. For more
clinker lowers the quantity of raw material-derived CO2 emissions from detail on modeling inputs and assumptions made, see the Supplemen-
the pyroprocessing stage of clinker production. Second, the production tary Material.
of BYF occurs at a slightly reduced kiln temperature [27], which re- Similar calculations were conducted in the assessment of CO2
duces the fuel energy required and the associated fuel-related emis- emission factors for the material alternatives proposed as mitigation
sions. Both of these factors result in lower expected CO2 emissions strategies. These included assessment of emission factors for calcined
while using existing clinker processing infrastructure. Yet, due to high clay in which assessments were based on two datasets for production:
amount of ettringite, BYF cements may suffer from loss of strength due Berriel et al. [34] and Vieira et al. [35]. These models were extended to
to carbonation if used in thin porous components. Additionally, avail- different regional fuel and electricity mixes used in the production of
ability of abundant high-alumina mineral, not captured by the more cement and values were estimated for the carbon dioxide emissions
valuable aluminum industry, is the key for the competitiveness of this expected to result from the production of calcined clay as well as a
technology. As such, there are some potential limitations to widespread cementitious blend containing 35% calcined clay, 15% limestone filler,
implementation. and the remainder as clinker.
For the production of CCSC, there are more avenues for potential The CO2 emissions associated with the production of alkali-acti-
CO2 reductions than those proposed by BYF. Again, reductions can be vated cements were calculated in two phases. First, emissions asso-
expected in raw material-derived CO2 emissions because raw material ciated with production of the alkali-activator were determined. Because
sources differ from those used in OPC and fuel-derived emissions would different raw materials, raw material sources, and processing can be
be expected to be lower than for OPC, totaling in an estimated over 30% implemented in the production of these activators, a range of emissions
reduction in CO2 emissions relative to OPC [27]. The additional benefit was considered. On the low end of emissions, a carbon emissions model
noted in the use of CCSC clinkers is a result of their being cured in a was developed for the production of sodium silicate based on raw
CO2-rich environment, beneficially utilizing CO2. Similarly to BYF, material-derived carbon dioxide emissions and the energy efficiency
CCSC clinkers can be processed in conventional cement kilns. However, associated with the production of glass, which contains similar che-
these clinkers possess a greater number of limitations. They are not mical constituents, resulting in CO2 emissions of approximately
fully developed and there are no available standards. These clinkers 0.9 kg CO2/kg material, dry basis, based on communication with
require curing in an environment saturated with CO2, thus capturing Gartner [36]. To capture a higher emissions factor, data from Habert
the process CO2. As such, their market is limited to industrialized and Ouellet-Plamondon [15] were used to find a factor of approxi-
concrete plants, particularly for thin or porous sections, without steel mately 1.8 kg CO2/kg material, dry basis. These activators were then
reinforcement, which is a relatively small market in developing coun- considered to be used with calcined clay as the source of silicates and
tries where cement demand is expected to grow. alumina with a 25–50% range of activator needed by mass, depending
on properties of raw material inputs and application requirements [26].
2.2. Calculation of emissions factors For the production of BYF and CCSC, CO2 emissions factors were
calculated by adapting the LCA model for the production of Portland
Emission factors for all alternative materials were calculated using clinker. Using adjusted raw-material derived CO2 emissions and
life-cycle assessment (LCA) methodology. These assessments were thermal energy demands for these technologies as noted by Gartner and
conducted to determine CO2 emissions associated with the production Sui [27], reductions in total emissions were calculated. It must be noted
of the materials, considering raw material use, energy demand, fuel that CO2 capture during curing was not considered for CCSC technology
mixes, electricity mixes, transportation, and raw material-derived CO2 because concrete batching was considered outside the scope of assess-
emissions. The life-cycle phases considered were from raw material ment. Lower cumulative CO2 emissions would be expected with a larger
acquisition through cement production (i.e., cradle to gate) and as- scope of analysis.
sessments were based on production of 1000 kg of material. Process For more detail on the LCA approach, the scope of the assessment
flow diagrams detailing the considered phases are shown in Fig. 1. applied herein, and details on how emissions factors were calculated,
To perform these assessments, production was considered at re- see the Supplementary Material. Also considered in the Supplementary
gional levels and, using weighted averages, outcomes were combined to Material are alternatives, which have not been included in this assess-
develop global emissions factors. To capture data inputs, such as kiln ment due to their limited reduction potential, e.g., Reactive Belite-rich
efficiencies and regional production, several datasets were combined. Portland cement (RBPC).
The Getting the Numbers Right (GNR) database [24] reported kiln use For this assessment, emissions factors for production of OPC and the
by region as well as kiln efficiency in terms of MJ/t clinker for each kiln alternative materials were performed based on cradle-to-gate calcula-
type. These data were used to find energy for clinker production by tions incorporating current kiln technologies, energy mixes, and pro-
region. Fuel mixes were estimated based on data from GNR [24] and duction statistics (discussed in more detail in the Supplementary
the IEA [30]; CO2 emissions from fuel were calculated based on values Material). The factors developed based on regional assessments were
reported by the Intergovernmental Panel on Climate Change [31] for then aggregate to develop factors for a global assessment. These ag-
stationary combustion in manufacturing industries and construction. In gregated factors for alternative materials were then examined at dif-
the production of clinker, these kiln efficiencies, fuel types, and elec- ferent potential global market adoption rates and compared using 2050
tricity requirements for processing were considered as well as raw projected cement production and the 2 °C scenario CO2 emission re-
material-derived emissions, which were assumed to be 0.507 kg CO2/kg duction goals. Because this research focuses on the role of alternative
of clinker [32]. materials in contributing to CO2 emission reduction goals in the ce-
Models for the CO2 emissions from each of the materials were as- ment-based materials industry, assessments focused on the degree of
sessed separately, then compared to one another at different levels of market adoption necessary at a global scale. Due to the scope of this
replacement. For models of cement containing solely clinker and assessment, models projecting change in commodity cost and its role on
gypsum, the use of Portland clinker was modeled with additional pro- reserve base, local implementation plans, and the influence of socio-
cessing and the inclusion of 5% gypsum by mass. Beyond this cement, economic factors on use of alternative materials as well as change in
the production and consumption of SCMs, namely blast furnace slag, fly technology efficiency and change of energy mixes were not included.
ash, natural pozzolans, and limestone filler, in cement or as cementi-
tious replacement were considered. Carbon dioxide emission factors for

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S.A. Miller et al. Cement and Concrete Research xxx (xxxx) xxx–xxx

Fig. 1. Process flow diagrams for cementitious materials assessed


Ordinary Portland Cement (OPC) (note: fuel requirements and transportation considered at all per-
Crushing, tinent stages).
Raw Material Grinding, and Pyroprocessing Finish Grinding
Acquisition and Milling
Milling

Mineral Additions

Cement with Calcined Clay

Crushing,
Raw Material Grinding, and Pyroprocessing Finish Grinding
Acquisition and Milling
Milling

Mineral Additions

Clay Calcination

Cement with Increased Filler*

Crushing,
Raw Material Grinding, and Finish Grinding Batching for Use End of Life
Pyroprocessing
Acquisition and Milling Application
Milling

Mineral Additions

Alkali-Activated Cement

Crushing,
Raw Material Grinding, and Heat Processing Finish Grinding
Acquisition and Milling
Milling

Clay Calcination

Mineral Additions

Belite- -Ferrite (BYF)**

Crushing,
Raw Material Grinding, and Pyroprocessing Finish Grinding
Acquisition and Milling
Milling

Mineral Additions

Carbonate Calcium Silicate Clinkers (CCSC)***

Crushing,
Raw Material Grinding, and Pyroprocessing Finish Grinding
Acquisition and Milling
Milling

Mineral Additions

* Contains more limestone filler than OPC


** Contains different raw materials than OPC and requires less heat in pyroprocessing
*** Contains different raw materials than OPC and requires less heat in pyroprocessing & carbonation benefits not considered

2.3. Raw material availability 30–40 Mt of geopolymer, based on [38,39]. However, there are ex-
tensive reserves of soda ash and silica, which are needed to develop the
One of the most notable constraints on the use of material alter- product [40]. Therefore, it is assumed in the model that geopolymers
natives in cement production is limitation in availability. Due to the composed of activated clay may have a limited market adoption, con-
high consumption levels of cement globally, mitigation requires that sidered in this research as between 0 and 15% of the market share. Due
the material alternatives be available in large quantities. First, the fu- to extensive amounts of industrial waste or byproducts that could be
ture availability of common SCMs used today must be considered. For viable as the solid precursor to geopolymers, these materials were not
fly ash and slag, two prevalent SCMs globally, annual consumption considered to be a limiting factor; however, further research into the
levels are nearing current production levels [6]. Projecting to 2050, the viability of different waste flows and their influence on material
ratio of available blast furnace slag to cement production has been es- properties in cement-based composites should be conducted.
timated to be approximately the same as observed today, around For BYF, the critical materials are bauxite and other high-alumina
370 million tonnes (Mt) in 2050, about the same value estimated in the minerals of which the fraction of Al2O3 is 16.4% [41]. Bauxite extrac-
Cement Roadmap 2009 [20]. There is no available estimate of fly ash tion in 2016 was 274 Mt worldwide. Economically explorable reserves
production in 2050, apart from the 368 Mt estimated by the Cement are 28 Gt, but resources are estimated to be 55–75 Gt, and 91% of the
Roadmap 2009, a value lower than the estimated 590 Mt in 2005 and reserves are located in only 15 countries [42] (Fig. 2c). Al2O3 content in
623 Mt estimated for 2010. Therefore, production of blast furnace slag bauxite is circa 40% [43], and there are reserves to increase bauxite
and fly ash together are projected to be around 16% of cement pro- production. If all of today's bauxite extraction is diverted to BYF ce-
duction in 2050. Global cement production and ratios of annual pro- ment, it will be possible to produce around 650 Mt of cement. This
duction of these popular SCMs are shown in Fig. 2. value suggests material availability is not a hindering factor, but be-
Filler and calcined clay plus limestone filler face limitation due to cause the aluminum industry may offer a more economically competi-
limits of clinker substitution as opposed to material availability. In tive use of the material, there is a potential limitation associated with
addition to limits from clinker substitution, high filler substitution will the opportunity cost. As a result, the degree of market adoption is
require the introduction of dispersant organic admixture at the cement considered to be between 0 and 15% for this research.
plant. In order to scale up the technology, the production of these Because there are no published studies on future market share of
dispersants must increase; however, this increase is not expected to be industrialized cement-based components, which excludes dry-mixed
problematic and thus is not considered a limitation [37]. mortar and the early stages of development of this technology, new
These low ratios and current prevalence of these materials as SCMs technologies such as carbonation-hardening CCSC that require special
suggest they may be used as SCMs rather than as a solid precursor to industrial facilities was limited to 15% of market share in 2050. This is
geopolymers. However, as mentioned before, remaining ash and other considered an optimistic value, justifiable because it helps to make
industrial byproducts could be used in production of geopolymers. evident the mitigation potential of the technology. CCSC can be formed
For production of geopolymers with calcined clay, to scale up it is using simple calcium silicates, such as wollastonite (raw material
necessary to increase the production of sodium silicate. Today, pro- availability shown in Fig. 2d). Again, considering both material avail-
duction is estimated to be only 6 Mt, sufficient to produce only ability and specialized industrial facilities, in this research, the degree

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S.A. Miller et al. Cement and Concrete Research xxx (xxxx) xxx–xxx

Fig. 2. Maps of material resources showing (a) avail-


ability of fly ash relative to cement production by region
(calculated based on Miller et al. [6]); (b) slag relative to
cement production by region (calculated based on Miller
et al. [6]); (c) country based production of alumina and
bauxite [58], which is necessary for the production of
BYF; and (d) resource availability of wollastonite [59],
which can be used in the production of CCSC.

of market adoption for CCSC technology is assessed between 0 and assessment weighted by regional hydraulic cement production (more
15%. detail on the emissions factors calculated can be found in the Supple-
mentary Material). Based on the assessments conducted, it can be seen
2.4. Mitigation potential that each of the materials assessed offer different carbon emission
profiles. The natural minerals, such as natural pozzolans or limestone
The mitigation potential (tonnes of CO2, tCO2) of a technology is a filler, have the lowest carbon emission factors, followed by the in-
function of the specific mitigation potential, smp (kg CO2/t), multiplied dustrial byproducts, which have no allocated emissions from produc-
by the amount of cement produced, which can be expressed as the tion, but are allocated emissions associated with collection, refinement,
fraction of market shares of the total market of 4566 Mt forecasted in and transportation. Calcined clay alone offers over a 50% reduction in
2050 [21]. Therefore, we are not addressing the time scale of the in- CO2 emissions relative to Portland clinker and gypsum, but it is con-
troduction of each technology, which is not the same for all technolo- sidered to be a blended material with clinker and limestone filler as a
gies and may become a relevant factor: mitigation strategy. The alkali-activated cements have a wide range of
associated emissions based on material inputs, showing the potential to
smp = Ct − Cc
either reduce or increase CO2 emissions relative to Portland clinker and
where Ct is the CO2 footprint of the technology, and Cc is the CO2 gypsum. This finding suggests that further refinement of materials used
footprint of the cement it displaces from the market, in our case, and appropriate application of geopolymers must be examined to pro-
Portland cement with 10% of filler and 5% of gypsum. An underlying vide the best mitigation of CO2 emissions. Finally, BYF and CCSC
assumption in our model is that all technologies will produce cements clinkers show a reduction in CO2 emissions relative to Portland clinker
that on average will have the same efficiency in terms of the amount of by 25–40%. The CO2 emissions for CCSC clinker could have an even
cement needed to fulfill the desired performance, for example, me- lower CO2 emissions factor of approximately 0.19 kg CO2/kg material
chanical strength. This assumption is not accurate in all situations since (or 65% lower than the factor listed) if carbonation were within the
efficiency depends on the end use, an aspect that is not possible to scope of assessment.
model accurately at a global scale. The mitigation potential calculated
is then compared to projected 2 °C scenario mitigation goals for cement 3.2. Mitigation potential
production. Again, because this research approaches this issue from a
global perspective, quantity of implementation at the local level and Using the emission factors calculated and projections for cement
rate of implementation were not considered. Rather, global totals based consumption in the year 2050, mitigation strategies relative to use of
on current reserves and cumulative material replacement were con- OPC were assessed. Fig. 3 presents potential reductions in CO2 emis-
sidered regardless of time or location of implementation. sions from innovative use of currently applied material alternatives in
the cement industry. Fig. 3a shows an estimate of the mitigation po-
3. Results tential of a combination of 25% to 35% of calcined clay with fixed 15%
of limestone filler with minimum 50% clinker content. The mitigation
3.1. Emissions factors for materials considered currently allocated by carbon capture and storage (CCS) can be reached
if this technology were scaled up to 50–60% of the cement market.
Table 1 contains selected of the emissions factors calculated in this Another option is substitution of binder by 25–35% of engineered fillers

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S.A. Miller et al. Cement and Concrete Research xxx (xxxx) xxx–xxx

Table 1
Carbon dioxide emission factors for cementitious materials including 95% clinker Portland cement, supplementary cementitious materials, and fillers currently used, as well as alternative
cementitious materials and filler. Factors were developed by regional assessment and weighted by regional production.

Clinker Fly ash Slag Natural Calcined clay Limestone filler Calcined clay based alkali- Fly ash based alkali-activated BYF CCSCa
+ gypsum pozzolans activated cement cement

0.86 0.04 0.09 0.007 0.21–0.33 0.008 0.50–1.08 0.09–0.25 0.62–0.65 0.53

BYF: Belite-Ye'elimite-Ferrite.
a
Carbonated calcium silicate cement, modeled without carbon capture.

combined with dispersant, a technology that compensates dilution by


reducing the amount of water, that will deliver mitigation originally
attributed to CCS with slightly lower market share, between 37% and
55% (Fig. 3b). These two technologies, which are based on minerals
and production processes with which the cement industry is familiar, if
further developed and adapted can be combined to cope with peculia-
rities of each market, giving flexibility to companies. The engineered
filler combined with dispersant is certainly more challenging to develop
and deploy. However, this method can be employed among the more
capable industrial users of cements.
Apart from these two mitigation methods, other technologies that Fig. 4. Estimate of mitigation potential of new cement technologies as a function of the
do not rely on Portland clinker were explored, namely use of alkali- market share for the year 2050 low-demand scenario. These technologies are at earlier
activated cement, as well as CCSC and BYF clinkers. As a whole, there is stage of development and, as such, there is greater uncertainty associated with emission
less accumulated industrial knowledge about these technologies than factors. For this plot, “Alkali-Activated Cement (1)” represents use of calcined clay as the
about the previous one and greater uncertainty regarding costs and solid precursor and “Alkali-Activated Cement (2)” represents use of waste fly ash as the
solid precursor, as discussed in the text. The horizontal grey line presents a reference of
market limitations. Additionally, limited industrial knowledge of these
the mitigation target from the 2 °C change scenario from CCS technologies.
alternative materials results in greater uncertainty in modeling CO2
emissions from production. Fig. 4 presents an estimate of the potential
mitigation from each of the three new cements and clinkers assessed applied (0.33 kg CO2/kg material) with an average of the two sodium
considering uncertainty associated with emission factors and expected silicate values reported (1.35 kg CO2/kg material) used at 40% by mass
potential replacement levels. of the geopolymer. The sensitivity assessment of this material considers
To address the uncertainty in the CO2 emission factors for the al- both the range of use of the alkali-activator (varying between 25% and
ternative materials to OPC, sensitivity ranges were incorporated. The 50%) and the emission factor for the alkali-activator. These results
market for CCSC is limited to the production of industrial components show a formulation with 55% of sodium silicate with 1.1 kg CO2/kg
because carbonation hardening requires dedicated industrial facilities. (dry-basis) will result in no improvement from Portland cement with
To capture uncertainty, the emission factor was made to vary 15% 10% of limestone filler. As such, calcined clay geopolymers will only
below and above the nominal CO2 footprint. BYF is also not fully de- provide a strong means for mitigation if sources of sodium silicate with
veloped; as such, its CO2 footprint and its estimates for cost are subject a much lower (~ 50%) CO2 emission factor than currently available
to change. The degree of market adoption of this cement will depend on were introduced in the market and/or low-content activator formula-
availability and costs of aluminum-rich minerals in various regions. The tions were developed. Otherwise the technology can actually lead to an
emission factor was considered to vary 15% above and below the increase in CO2 emissions.
average CO2 footprint. Fly ash and blast furnace slag-based geopolymers could be expected
As discussed in Section 2, the CO2 emission factors for geopolymers to have much lower CO2 footprint than Portland cement, depending on
are affected by the source of silicates and alumina, the source of alkali- the amount of sodium silicate. However, to scale up in the market, they
activator, and the relative quantities of these materials. This assessment might need to divert SCMs from the Portland cement market, causing
considers a calcined clay geopolymer with sodium silicate activator. In the CO2 emission of Portland cements to increase by the same amount.
the model for the average mitigation potential shown in Fig. 4, the more Consequently, fly ash- and granulated blast furnace slag-based geopo-
conservative (higher) CO2 emissions factor for calcined clay was lymer technology will contribute to CO2 mitigation only if (a) they use

Fig. 3. Expected mitigation potential re-


flected as a percent increase in (a) sub-
stitution of cement for a combination of
25–35% calcined clay plus 15% of lime-
stone filler, and (b) potential of filler sub-
stitution varying between 25% and 35% as
a function of market share for the year
2050 low-demand scenario. The horizontal
lines reference the mitigation targets from
the 2 °C change scenario for total targeted
reduction in emissions from cement in-
cluding CCS (upper gray line) and the tar-
geted mitigation share from CCS alone
(lower gray line).

6
S.A. Miller et al. Cement and Concrete Research xxx (xxxx) xxx–xxx

SCMs with higher efficiency than ordinary Portland cement, an aspect uncertainty [21]. The assumptions made in the modeling of emission
that it is not yet proven, or (b) they increase the fraction of use of such factors are described in more detail in the Supplementary Material.
materials that can be utilized, e.g., using fly ashes that are not suitable Calculations and comparisons drawn in this research are based on
for SCM in Portland cement. The mitigation potential of using fly ash- mass material alternatives and mass of cement produced. Because ce-
or slag-based geopolymers is currently unknown for a global perspec- ment is not the end-product used in applications, this research was not
tive; however, to present a range of potential mitigation possible from able to capture the role of material properties or durability of cement-
use of alkali-activated material, the use of fly ashes not suitable as SCMs based products in comparing mitigation alternatives. Additionally,
in geopolymers are presented in this assessment. Plotting these data SCMs, such as calcined clay and limestone fillers, often have lower
shows the use of industrial by-product, if allocated only processing CO2 density than Portland clinker, which would affect the volume of ce-
emissions and none from the production of the primary product, could ment, a key factor in several applications. The changes in material
result in geopolymers that have markedly lower CO2 emissions per kg of properties and volume-based comparisons were outside the scope of
production than OPC. These geopolymers have a great potential to this assessment, but should be considered in future work.
offset CO2 emissions relative to OPC. The models presented in this work also were not able to capture the
These three technologies are at varying stages of development, but rate of learning in industry and of implementation, nor did they capture
CCS for the cement industry is also not fully developed. However, they potential changes in material properties resulting from implementation
are potentially of interest for the industry because they can be cheaper of the mitigation strategies. These areas should be examined in greater
than CCS in most situations and will require much less energy than CCS. detail in further assessments.
At this stage of knowledge, BYF and CCSC seem to be the more pro-
mising technologies for CO2 mitigation than geopolymers. Geopolymer
mitigation contributions depend on the availability in the world market 4.2. Concrete mixture proportioning and full life-cycle impacts of concrete
of alkali-activators with much lower CO2 footprint than the current
literature shows, and geopolymer formulations that require a low This research focuses on cradle-to-production gate CO2 emissions
amount of sodium silicate, particularly if the material uses calcined from the production of cement and cement material alternatives;
clay. however, because concrete is a structural material that is often in ser-
It is worth noting that these calculations are based on current vice for an extended period of time, there are many other factors that
equipment efficiency, electricity mixes, transportation emission factors, could be applied at later stages of the material life cycle to mitigate CO2
and thermal energy mixes. With improvement in these areas, a reduc- emissions. While not all of these mitigation strategies can be easily
tion in CO2 emissions could be expected. Furthermore, these new ma- scaled to a global assessment to determine their role in reducing CO2
terial alternatives to OPC can further benefit from dilution with en- emissions, it is worth discussing these factors as they can contribute to,
gineered filler and dispersants, increasing their mitigation potential. if not outweigh, some of the cradle-to-production gate impacts. A few of
these considerations are briefly discussed below.
4. Discussion Strategic mixture proportioning can contribute to reducing CO2
emissions from the production of concrete. For example, the use of
4.1. Uncertainty and limiting assumptions appropriate levels of SCMs, use of the appropriate binder content, use of
chemical admixtures, or changes in aggregate type and gradation, can
This research incorporates several sources of uncertainty and sev- influence properties achieved and environmental impacts of concrete
eral limiting assumptions. A synopsis of these uncertainties and as- mixtures (e.g., [13,16,17,44–46]). To this extent, use of concrete effi-
sumptions follows. ciently by designing members with appropriate strength or other ma-
First, considering how emission factors were calculated, it must be terial characteristics can contribute to a reduction in concrete needed
noted that some uncertainty arises from data availability. Estimations and, thus, potentially contribute to lower associated emissions for a
for equipment efficiency were not representative of all cement produ- structural element. (e.g., [16,19,47]). Further, it has been shown that if
cers in the world and data are better for some regions than others. designs were to occur with higher specified age for strength, different
Furthermore, the datasets used to assess equipment efficiency, energy mixture proportions could be used in concrete structures and could
mixes, transportation, and material production methods were not all contribute to lower levels of OPC needed to meet the same application
from the same year, potentially affecting calculations. The application requirements [18].
of weighted averages to electricity and thermal energy mixes may not The durability of concrete, which would influence both main-
have accurately captured individual production processes. Varying tenance and replacement [48], has the potential to overshadow benefits
sources of data for these inputs, with potential variation in scopes of gained through manufacturing processes. Research on the influence of
assessment, also lead to greater levels of uncertainty. These types of durability mechanisms on the longevity of infrastructure materials has
uncertainties are discussed in more detail in Miller et al. [6]. shown that time-dependent loss of material properties or other me-
In modeling the emissions factors for mitigation strategies, there chanisms leading to deterioration can offset potential benefits gained
were several additional factors contributing to uncertainty. Among through implementation of beneficial production methods or use of
these, the use of life-cycle inventory data from various sources for the low-impact constituents [48–50]. Beyond the volumes of cement-based
mitigation strategies can lead to a level of uncertainty and there is in- material that could be altered due to durability leading to changes in
herent variability in each of the processes modeled. While variations frequency of replacement, the emissions from maintenance have been
were compensated for by the use of similar transportation, processing, shown to have potentially dramatic effects on total CO2 emissions as-
and energy input models, the uncertainty in comparisons drawn could sociated with concrete structures [51].
not be fully removed. Additionally, the use of weighted averages of In addition to the role mixture proportioning, structural design,
emission factors by region projecting forward could not capture dif- durability through intended service life, and maintenance can have on
ferences in production at the local scale nor could it capture differences emissions, carbonation during the use of a concrete structure containing
depending on region or individual application. These data are based on cement with CH and carbonation of concrete rubble after demolition
present technology, but with deployment of energy efficiency measures, can change the emissions profile associated with a structure (e.g.,
alternative fuel sources, and the adaptation of material-based alter- [52,53]). However, it should be noted that use of alternative materials
natives, further reductions may be expected. Furthermore, estimates in the production of concrete to reduce clinker content will also reduce
and assumptions were made to determine cement production projec- the uptake of CO2 through carbonation.
tions, which while not developed in this research, contribute to

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S.A. Miller et al. Cement and Concrete Research xxx (xxxx) xxx–xxx

4.3. Role of industrialization industrialization of cement production are starting to appear. For ex-
ample, the National Climate Change Program of China recommended a
The attractions of using cement are manifold, including ease of use, reduction in the quantity of concrete and mortar mixed on construction
readily available raw materials, and affordability. Yet when cement and sites, resulting in an expected 2.4% reduction in cement consumption
cementitious products are manufactured or applied by untrained per- [55–57]. Further, implementation of such strategies could significantly
sonnel, the knowledge or means to optimize mixture proportioning can aid in meeting mitigation goals globally.
be limited, leading to higher consumption than that needed for tech-
nical performance. At larger scales of production, employment of spe- 4.4. Other material substitutes and mitigation strategies
cialized personnel for improved quality control and optimization of
production becomes possible. For example, a study of construction in This research focused on several key material substitutes that could
Brazil showed a median waste rate of approximately 50% for bagged contribute to the reduction of global CO2 emissions in the production of
cement used to make site-mixed concrete and just below 50% for ag- cement. However, there are several other strategies that could be im-
gregates. In contrast, the median waste of ready-mixed (bulk) concrete plemented, including the often-discussed improved equipment effi-
was below 10% [54]. ciency and alternative fuel mixes. Additionally, other material sub-
This increased ability to have specialized technicians and improved stitutes may prove to be viable options with more research and
quality control associated with larger scales of production, which could development. For example, magnesium oxides derived from magnesium
be expected to grow with industrialization, has the potential to con- silicates (MOMS) have been discussed as potentially being net carbon
tribute to a reduction in cement consumption and associated environ- dioxide neutral or negative. While energy would be needed during
mental impacts. However, with the exception of a study published by processing, there would be no raw material-derived carbon dioxide
Lafarge-WWF [47] that discussed a potential reduction in greenhouse emissions. Carbonation of the material, if it resulted in greater carbon
gas emissions by 15% from efficient use of cement, which would be dioxide uptake than emitted during processing, could potentially result
facilitated by industrialization, the role of industrialization in mitiga- in this material being either carbon neutral or net negative in terms of
tion is not a well-examined field in the literature. CO2 emissions. Because the raw materials needed are abundant, albeit
Because industrial applications, such as ready-mixed concrete, dry- not uniformly distributed globally, further examination of this class of
mix mortar, precast components, etc., tend to use bulk delivery, the materials as an alternative cementitious binder could be a fruitful area
share of cement used in less monitored applications can be estimated by of research. Due to lack of data, the mitigation potential of this or other
the market share of bagged cement. Based on data representing the new materials is not estimated in this work.
percent of cement sold in bags relative to national gross domestic
product (GDP), it is estimated that 42% of cement produced is sold in 5. Conclusions
bags and 58% is sold in bulk. Data show that the share of bagged ce-
ment decreases with GDP per capita increase (Fig. 5), but there is large This research examined future viable global CO2 mitigation strate-
scatter. In developing countries, which consume about 90% of cement, gies for the cement industry. The estimates show that it is possible for
the share of bulk cement is below 60%. In China, which produces about the cement industry to fulfill the 2 °C scenario mitigation targets
40% of the world's cement, bag cement sales are around 40–45% of the without requiring CCS if application of the discussed material alter-
market. In India, the second largest cement consumer, bag cement sales natives gets underway.
are much higher, 85–90% of total sales. The large scatter suggests that Of the several material alternatives examined, two clinker sub-
local governmental incentives can play a role in promoting in- stitution methods, calcined clay with limestone filler and engineered
dustrialization, but the trend indicates increased GDP is correlated with limestone filler combined with dispersant, would facilitate high levels
distribution of cement through bulk channels. of substitution. Due to their raw material availability and limited re-
Through large-scale production, facilitated by industrialization, quired infrastructure changes, these methods are expected to have few
more efficient mixture proportioning and concrete application could limits to implementation and could contribute significantly to CO2 re-
contribute to reduced emissions from the cement industry. The cen- ductions.
tralization of cement and concrete production would aid the inclusion Beyond these methods, the development of alternative cement
of materials such as those discussed in this research as well as other technologies was shown to have potential to contribute to global mi-
SCMs. Further, if the 15% reduction from improved efficiency esti- tigation of CO2 emissions from the cement industry. Clinkers with
mated by the WWF-Lafarge report [47] were achieved, a reduction of Ye'elimite as the most reactive phase (BYF, CCSC) can be produced in
approximately 530 Mt of CO2 could be expected based on the calcula- conventional cement kilns but require aluminum rich minerals, sul-
tions from this research. This value represents approximately 96% of phates and carbonates. CCSC uses widely available, not so pure lime-
the 2 °C mitigation target from CCS technologies. Benefits from stone and silicon, processed in conventional cement kilns. They require
curing in a CO2-rich environment capturing the process CO2. Therefore,
their market is limited to industrialized concrete plants, particularly for
thin or porous sections, without steel reinforcement.
Despite limitations, these materials offer promising alternatives for
certain regions and applications. Additionally, alkali-activated mate-
rials produced with calcined clay or industrial waste products appear to
be a scalable technology. Due to raw material inputs, these materials
would likely only contribute to mitigation of CO2 emissions if the
emissions from the alkali-activator could be reduced. As such, further
research and strategic implementation could solidify the benefits
achievable through the use of these materials.
It should be noted that these new technologies are likely more at-
tractive for regions where the cement industry is expanding production
Fig. 5. Percent of cement market supplied as bagged cement and bulk cement relative to capacity because the new plants can be built with capacity for these
GDP per capita. Data from LafargeHolcim Corporate Strategy Estimates as of the first material alternatives. In addition to material substitution alternatives,
quarter of 2016 and from the World Bank [60]. Data cover countries responsible for industrialization of concrete manufacturing has a significant potential
approximately 90% of total cement production.
to increase the efficient use of cement and lead to savings in greenhouse

8
S.A. Miller et al. Cement and Concrete Research xxx (xxxx) xxx–xxx

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