Journal of Cleaner Production xxx (xxxx) xxx

Contents lists available at ScienceDirect

Journal of Cleaner Production

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

Environmental and economic perspective of waste-derived activators

on alkali-activated mortars
Mariam Abdulkareem a, *, Jouni Havukainen a, Jutta Nuortila-Jokinen b,
Mika Horttanainen a
a
Lappeenranta-Lahti University of Technology, School of Energy Systems, Department of Sustainability Science, P.O.Box 20, 53851, Lappeenranta, Finland
b
Lappeenranta-Lahti University of Technology, Research Platform RE-SOURCE, P.O.Box 20, FI-53851, Lappeenranta, Finland

a r t i c l e i n f o a b s t r a c t

Article history: Alkali-activated binders have been considered a low carbon alternative to cement and are produced by
Received 9 January 2020 reacting aluminosilicate precursor with an alkali-activator. However, alkali-activators have been
Received in revised form observed to be a major contributor to the environmental burdens of alkali-activated materials regarding
13 August 2020
various environmental impact categories. Therefore, this study aims to perform an environmental impact
Accepted 11 October 2020
Available online xxx
assessment using life cycle assessment methodology on alkali-activated mortars produced from chem-
ically modified one- and two-part waste-derived activators (waste glass and rice husk ash) in comparison
Handling editor Bin Chen to conventional one- and two-part alkali-activated mortars, to estimate the influence of activator on
environmental impact of mortar. Additionally, a simplified cost analysis of the different mortar com-
Keywords: positions was conducted. A sensitivity analysis was performed on the key parameters, and allocating
Waste-derived activator emissions to waste glass and rice husk ash. Results show that waste glass and rice husk ash-derived
Waste glass alkali-activated mortar resulted in up to 62%, 61%, 76% and 56% reduced emission respectively in
Rice husk ash climate change, fossil depletion, terrestrial acidification and photochemical ozone creation formation
One-part alkali-activated mortar
when compared to conventional alkali-activated mortar counterpart. Sensitivity analysis indicated that
Two-part alkali-activated mortar
waste glass and rice husk ash are not so sensitive to mass allocation, with a maximum of 5% increased
Life cycle assessment
emissions observed in the above-mentioned impact categories. Additionally, sensitivity analysis on so-
dium hydroxide demonstrated that production from chlorine-alkali electrolysis using technology-mix
produced improved environmental performance in comparison to production from brine solution and
diaphragm route, respectively. Sensitivity analysis on sodium silicate using an alternative inventory data
indicated the emissions can increase regarding one-part or decrease regarding two-part alkali-activated
mortars. Results from cost analysis indicated up to 19% cost savings from waste-derived alkali-activated
mortar compared to conventional alkali-activated mortar. In conclusion, chemically modified waste-
derived activators are a promising alternative in improving environmental performance of alkali-
activated materials if their usage also reduces or substitutes the need for conventional alkali-activators.
© 2020 The Author(s). 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/).

1. Introduction cement production results respectively from thermally decom-

posing carbonates (mainly limestone) into oxides and CO2, to
Cement production has rapidly grown in recent years with an produce clinker; and during generation of high amount of energy
estimate of 4.7 billion tonnes produced globally in 2016 (from combustion of fossil fuels) needed to heat raw materials (over
(CEMBUREAU, 2017), and an estimated contribution between 4% 1000
C) (Andrew, 2018). There are different types of cement
and 8% of global CO2 emissions (Andrew, 2018). CO2 emissions from binders categorized from CEM I e V, containing cement clinker in
the range of 5%e100% (BS EN 197-1, 2011) with different percent-
* Corresponding author. Lappeenranta-Lahti University of Technology, School of ages of industrial by-products and/or wastes materials such as blast
Energy Systems, Department of Sustainability Science, P.O.Box 20, FI-53851, Lap- furnace slag, silica fume, pozzolana, fly ash, burnt shale and lime-
peenranta, Finland. stone, to partially replace cement binder for an improved envi-
E-mail addresses: Mariam.Abdulkareem@lut.fi (M. Abdulkareem), Jouni. ronmental performance among other reasons (CEMBUREAU,
Havukainen@lut.fi (J. Havukainen), Jutta.Nuortila-Jokinen@lut.fi (J. Nuortila-
Jokinen), Mika.Horttanainen@lut.fi (M. Horttanainen).
2015a; 2015b; 2015c).

https://doi.org/10.1016/j.jclepro.2020.124651
0959-6526/© 2020 The Author(s). 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/
).

Please cite this article as: M. Abdulkareem, J. Havukainen, J. Nuortila-Jokinen et al., Environmental and economic perspective of waste-derived
activators on alkali-activated mortars, Journal of Cleaner Production, https://doi.org/10.1016/j.jclepro.2020.124651
M. Abdulkareem, J. Havukainen, J. Nuortila-Jokinen et al. Journal of Cleaner Production xxx (xxxx) xxx

In addition to integrating industrial by-products with clinker for

an improved environmental performance of cement, there has
been increased research in reducing environmental impact of
cement binders through development of alternative types of
binders such as alkali-activated binders (AABs) sometimes referred
to as geopolymer binders (Provis, 2018). Geopolymers are largely
used to describe low calcium alkali-activated aluminosilicate
binders, thus, categorized as a sub-group of alkali-activated mate- Fig. 2. One-part alkali-activated binder.
rials (Heath et al., 2014; Provis, 2018). Davidovits (1994) defined the
concept of geopolymers as polycondensation of polymeric alumi-
nosilicates and alkali-silicates, yielding three-dimensional poly- materials, to avoid problems of waste disposal and associated
meric frameworks. They do not require very high temperatures environmental burdens. To further promote alkali-activated ma-
during production, thus, reducing high fuel consumption terials as a feasible and beneficial option, precursors and activators
(Davidovits, 2015). By and large, AABs are produced by reacting should be locally available to minimise transportation costs and
solid aluminosilicate raw materials (precursor) with an alkali- emissions. The downside of AABs is not having a standardised
activator to form a hardened binder (Tong et al., 2018; Vinai and approach when compared to OPC, thus, not making it a solution
Soutsos, 2019). These aluminosilicate precursors can be in the suitable for all circumstances (Provis, 2018). Additionally, they can
form of virgin raw materials such as metakaolin, or in the form of be susceptible to cracking, failures and deterioration as a result of
industrial side-streams with a high Si/Al ratio such as coal fly ash their brittleness. This can however be overcome by reinforcement
(CFA) and granulated blast furnace slag (GBFS), which have with fibres or other suitable materials (Alomayri, 2017).
demonstrated good results in production of AABs (Provis, 2018). The environmental sustainability of alkali-activated materials is
AABs can be produced in two pathways namely one-part and highly dependent on alkali-activators (commonly used are sodium
two-part pathways (Luukkonen et al., 2018a). hydroxide and sodium silicate). More information on production of
these chemicals can be found in the supplementary material. So-
 Two-part AABs as depicted in Fig. 1 are more conventional and dium silicate as an activator is known to produce a more compact
are produced by reacting solid aluminosilicate precursor with a and dense material with higher mechanical strength in comparison
concentrated aqueous solution of alkali silicate and hydroxide, to hydroxide-activated materials. Thus, a higher quantity of sodium
and water. They are mainly suitable for precast applications silicate is used when both chemicals are used as activators
(Luukkonen et al., 2018a). However, with respect to large scale (Mohseni, 2018; Nematollahi et al., 2015). However, sodium silicate
production of two-part AABs, impracticalities of handling large has also been observed to be a major contributor to the environ-
amounts of corrosive, viscous and hazardous alkali solutions led mental burdens of alkali-activated materials regarding various
to increased research in the development of one-part AAB impact categories such as global warming potential (GWP), acidi-
(Luukkonen et al., 2018a). fication potential (AP), abiotic depletion potential (ADP), toxicity
 One-part AAB as depicted in Fig. 2 is produced by reacting solid potentials etc. (Abdulkareem et al., 2019a; Habert et al., 2011;
aluminosilicate precursor with solid alkali silicate, thereby McGuire et al., 2011). These emissions are mainly as a result of the
producing a dry mixture binder similarly to cement. One-part high energy consumption required during their production (Fawer
AABs are more suited for in situ applications where handling et al., 1999). Furthermore, a study carried out by Abdulkareem et al.
of viscous alkali solutions can be more challenging, making (2019b) comparing the environmental assessment of one-part and
them more scalable in future as it is similar to cement in terms two-part alkali-activated mortars (AAMs) demonstrated that one-
of usage and packaging (Luukkonen et al., 2018a; Provis, 2018). part AAM had higher environmental impact when compared to
its two-part counterpart mainly as a result of the additional energy
AABs (especially one-part AABs) can be a potential alternative to required to produce sodium silicate powder which is required in
Ordinary Portland cement (OPC). Although, they are not likely to the production of one-part AAM (Abdulkareem et al., 2019b).
fully replace OPC, they can serve as a supplementary binder to OPC Although, the powder activator is a more desirable option when
thereby reducing CO2 emissions from the cement industry compared to the aqueous activator regarding handling and use, it is
(Luukkonen et al., 2018a). Some advantages of AABs over OPC however not desirable due to its higher environmental burdens.
include but are not limited to high resistance against acids, high In a bid to develop activators with reduced environmental im-
temperature resistance, high strength and high durability (Weil pacts, while retaining high mechanical properties of alkali-
et al., 2005). However, these advantages also depend strongly on activated materials, there has been increased research in the pro-
mixture composition of materials, curing time and temperature duction of sodium silicate from other silica rich waste materials
(Weil et al., 2005). Besides, alkali-activated materials provide such as rice husk ash (Tchakoute
et al., 2016; Tong et al., 2018),
means of reusing and recycling waste materials as secondary raw sugarcane bagasse ash (Norsuraya et al., 2016; Tchakoute
et al.,
2017), waste glass (Passuello et al., 2017; Vinai and Soutsos, 2019)
and silica fume (Bajza et al., 1998; Rousekova
et al., 1997) etc. Most
of these studies are however focused on the mechanical properties
of alkali-activated materials from these waste derived activators
(chemically modified by caustic solution) and not on the environ-
mental impacts. As a result, this study will focus on environmental
impact assessment of waste-derived AAMs in comparison to con-
ventional AAMs, to estimate and compare their environmental
performance. In addition, a simplified cost analysis of these
different mortar compositions will be conducted to assess their
economic sustainability.
Fig. 1. Two-part alkali-activated binder.

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M. Abdulkareem, J. Havukainen, J. Nuortila-Jokinen et al. Journal of Cleaner Production xxx (xxxx) xxx

2. Materials and method NaOH (8.7%), RHA (24%) and water (67.3%) in mass (Gursel et al.,
2016; Tong et al., 2018). To produce alkali-activated mortar from
2.1. Materials RHA-derived activator, fly ash and GBFS were blended manually
and sand was subsequently added to the mix. Afterward, the acti-
2.1.1. Waste glass (WG) cullet vator was added to the mix and subsequently cured at room tem-
Glass production has large similarities with sodium silicate perature (Tong et al., 2018). From this mixture, a two-part waste-
production as it involves reaction of silica sand and soda ash at a derived AAM is produced.
temperature of more than 1100
C (EU, 2007). Thus, making silicon
dioxide the main component of glass. WG cullet is a potential 2.2. Life cycle assessment methodology
source of silicate with amorphous silica content of 70e75% (Vinai
and Soutsos, 2019). Glass production is quite extensive which Life cycle assessment (LCA) addresses “environment aspects and
means that there is a high amount of WG available for open and potential environmental impacts throughout a products’ life cycle
closed-loop recycling. However, composition, colour and contami- from raw material acquisition through production, use, end-of-life
nation of WG can reduce the amount of glass that can be reused in treatment, recycling and final disposal” (EN ISO 14040, 2006; EN
closed-loop recycling of glass (Vinai and Soutsos, 2019). Over 12 ISO 14044, 2006). LCA framework is actualised in four phases
million tons of glass bottles and jars are collected and recycled in which are: goal and scope definition, life cycle inventory (LCI)
Europe with an average glass recycling rate of 74% (FEVE, 2019). phase, life cycle impact assessment (LCIA) phase and interpretation
Alkali-activator from WG can be produced using hydrothermal phase. Additionally, to establish confidence in LCA results, it is
or fusion methods. Hydrothermal method involves heating of WG recommended to conduct assessment procedures such as sensi-
in an alkaline solution while fusion method involves heating WG tivity analysis, consistency check and completeness (EN ISO 14040,
and NaOH powder at a very high temperature. Hydrothermal 2006).
method produces aqueous alkali-activator while fusion methods
produce powder alkali-activator (Vinai and Soutsos, 2019). Hence, 2.2.1. Goal and scope of study
making possible production of one-part waste-derived alkali acti- The goal of this study is to estimate and compare environmental
vator. The environmental impacts of producing powder activator impacts of chemically modified waste-derived alkali-activated
from WG cullet using the fusion method was assessed following the mortar (one- and two-part) in comparison to conventional alkali-
production process reported by Vinai and Soutsos (2019). WG cullet activated mortars (one- and two-part), to estimate the influence
was milled by means of Retsch PM 400 ball mill for 10 min and then of activator on environmental impact of mortar. The results are
reacted with NaOH powder by heating in an electric furnace at compared to assess if waste-derived activators improve environ-
150
C for 1 h. The mass proportion of WG cullet and NaOH was 48% mental performance of AAMs. In addition, a simplified cost analysis
and 52% respectively. The advantage of this procedure is that it was carried to compare the cost of these different mortars to assess
produces a powder activator as opposed to a liquid activator. their economic sustainability. The functional unit is defined as the
Mortar produced from WG-derived activator is prepared by mixing environmental burdens generated due to the activities involved in
required amounts of sand, CFA, GBFS and activator. The mixtures the production of 1 m3 of AAM with compressive strengths be-
were cured at room temperature (Vinai and Soutsos, 2019). From tween 52 MPae60 MPa at 28 days. It is assumed that the scenarios
this mixture, a one-part waste-derived AAM is produced. will have similar applications with similar service life.
The system boundary (Fig. 3) utilized in this study contains the
2.1.2. Rice husk ash main production steps of cradle-to-gate AAM including raw ma-
Rice husk ash (RHA) is an agricultural waste material resulting terial production, waste treatment and mixing of constituents in
from combustion of rice husk, which is a residual stream from the which the associated emissions and energy consumptions are
pod of rice grains (Gursel et al., 2016). Rice husk is generated while calculated. Transportation is excluded from this study as it is
milling paddy and has a number of applications such as in fertilizer assumed all raw materials considered have similar transportation
and substrate, raw material for brick production and renewable distances. The use phase and end-of-life phase are also excluded
energy source from biomass etc. (Tong et al., 2018). Gasification or from this study as it is assumed that comparable and similar im-
controlled burning of rice husks in kilns or power plants is an pacts are expected from these phases.
effective way of disposing rice husks thereby producing high
quality RHA suitable as a supplementary cementitious material 2.2.2. Scenario description
(SCM) (Gursel et al., 2016; Meryman, 2009). RHA is rich in silica, Four scenarios were considered in this study namely.
approximately 90%, similarly to glass (Norsuraya et al., 2016; Tong
et al., 2018) and has been considered a potential source of sili-  S1 e one-part mortar (conventional powder activator)
cates for alkali-activated binders (Ghosh, 2013; Kamseu et al., 2017;  S2 e two-part mortar (conventional aqueous activator)
Liu et al., 2016; Ma et al., 2012; Tong et al., 2018). Temperature and  S3 e one-part mortar (WG-NaOH derived powder activator)
duration of combustion process are important during combustion  S4 e two-part mortar (RHA-NaOH derived aqueous activator)
of rice husk, as shorter duration and higher temperatures are ex-
pected to maximize the amorphous content of RHA and induce S1 and S2 represents reference scenarios for conventional alkali-
formation of crystalline SiO2. The RHA share of rice husk is 18e22% activators in the production of one-part and two-part AAM
of dry content by weight. Market availability of amorphous RHA respectively. S3 and S4 represent scenarios derived from chemically
with silica content of about 95% makes industrial production of modified WG and RHA alkali-activators to produce one-part and
silicate from RHA possible (Tong et al., 2018). two-part AAMs respectively. The synthesis conditions for the AAMs
The environmental impacts of producing alkali-activator from are defined at laboratory scale. Table 1 illustrates mix proportions
RHA using the hydrothermal method was assessed following the of these scenarios. All mortars have similar quantities of constitu-
production process reported by Tong et al. (2018). RHA was milled ents and equivalent magnitude of compressive strengths at 28 days
for 15 min by means of Retsch PM400 to produce a fine RHA to aid comparison. All mortars were cured at room temperature,
powder. RHA powder was dissolved in a NaOH solution, heated and hence, avoiding energy required for thermal curing. WG and RHA
kept under magnetic stirring. The composition of the solution is are considered as wastes in this study and allocated no
3
M. Abdulkareem, J. Havukainen, J. Nuortila-Jokinen et al. Journal of Cleaner Production xxx (xxxx) xxx

Fig. 3. System boundary depicting production of alkali-activated mortar.

Table 1
Mix proportions of mortars.

Constituent (kg/m3) S1 52 MPa a

S2 58 MPa b
S3 58 MPa c
S4 60 MPa b

Coal fly ash 0 321 313 326

GBFS 373 214 208 217
Sand 1445 1471 1432 1493
WG-NaOH powder 0 0 126 0
RHA-NaOH solution 0 0 0 196
Sodium silicate 109d 157e 0 0
Sodium hydroxide pellets 0 26 0 36
Water 241 131 231 99

WG e waste glass.RHA e Rice husk ash. NaOH - Sodium hydroxide. GBFS - Granulated blast furnace slag.
a
Yang et al. (2010).
b
Tong et al. (2018).
c
Vinai and Soutsos (2019).
d
Sodium silicate powder.
e
Sodium silicate solution.

environmental burdens based on the EU directive that states “a system boundary are quantified. LCI data for processes such as
substance is considered as by-product and not waste if it fulfils NaOH, sand, electricity and water were sourced from GaBi database.
certain criteria which are 1) further use of the substance is certain; LCI for sodium silicate solution and sodium silicate powder were
2) the substance can be used directly without any further pro- sourced from Ecoinvent database while LCI for CFA, GBFS, RHA and
cessing other than normal industrial practice; 3) the substance is WG were collected from literature. Table 2 shows data sources for
produced as an integral part of a production process; 4) further use the different processes considered in this study. In this study,
is lawful (European Parliament and Council, 2008)”. As a result, pedigree matrix (see supplementary material for more details) is
only impacts incurred during treatment of WG and RHA will be applied to assess the quality of data utilized in this study. Data
considered. sources are evaluated based on five independent characteristics
Selected scenarios focus on AAM recipes with comparable namely, reliability, completeness, temporal correlation, geograph-
compressive strength. Data for these scenarios were collected from ical correlation, and further technological correlation. Each inde-
literature studies. It was ensured that these data were closely pendent characteristic is scored between 1 and 5 based on 5 quality
related with respect to system boundaries and masses of sub- levels (Weidema et al., 2013).
stances to ease comparison and consistency. Additional scenarios RHA beneficiation process include electricity for milling
were not taken into consideration as there are limited information (0.0432 MJ/kg) and electricity of 0.74 MJ/kg to dissolve RHA in
on waste-derived AAMs with comparable compressive strength NaOH by heating at 80
C for 3 h (Tong et al., 2018). Due to sim-
within the scope of this study. For instance, one-part RHA-NaOH plifications in the analysis of heat required to dissolved RHA in
derived mortar studied by Luukkonen et al. (2018b), obtained a NaOH, the estimated energy is more than actual energy needed
compressive strength of 32 MPa at 28 days which is high enough, (Tong et al., 2018). WG cullet beneficiation include electricity con-
however, not as high as compressive strength of mortars in the sumption for milling glass (0.18 MJ/kg) (Vinai and Soutsos, 2019).
scope of this study. Also, Puertas and Torres-Carrasco (2014) and Electricity required to heat glass powder with NaOH was 0.072 MJ/
Torres-Carrasco and Puertas (2015) carried out a study on two-part kg. This value is according to technical specifications obtained for
WG-derived activator focusing on paste preparation and not industrial ovens with required capacity (Vinai and Soutsos, 2019).
mortar, which is out of scope of this study. Thus, the limitations of The synthesis conditions for some of the alkali-activated mortars
this study include the limited number of scenarios for waste- are defined at laboratory scale. Thus, energy consumed might be
derived AAMs. more conservative when compared to industrial scale production.
For GBFS and CFA, they are assumed to come into the system
boundary with no environmental burdens, since they are consid-
2.2.3. Inventory analysis
ered wastes. However, GBFS which is used as a supplementary
Life cycle inventory (LCI) is the phase where inputs and outputs
cementitious material (SCM), goes through the processes of
as well as produced emission of all unit processes included in the
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M. Abdulkareem, J. Havukainen, J. Nuortila-Jokinen et al. Journal of Cleaner Production xxx (xxxx) xxx

Table 2
Data sources with data quality indexes.

Type of data Source Data quality indexes Pedigree

matrix

Sodium hydroxide GaBi database 2019 e EU-28: Sodium hydroxide (caustic soda mix, 100%) (3,3,2,2,2)
Sodium silicate Ecoinvent database e EU-28: Sodium silicate production, hydrothermal liquor, product in 48% solution state (2,2,5,1,1)
solution
Sodium silicate powder Ecoinvent database e EU-28: Sodium silicate production, spray powder, 80% (2,2,5,1,1)
Sand GaBi database 2019 e EU-28: Sand 0/2 (3,3,4,3,4)
Water GaBi database 2019 e EU-28: tap water (3,3,4,4,3)
Electricity GaBi database 2019 e FI: electricity grid mix (3,3,4,3,4)
Coal fly ash Coal fly ash beneficiation (Kawai et al., 2005) (4,4,5,5,2)
GBFS GBFS beneficiation (Marceau and VanGeem, 2003) (2,3,5,4,1)
Waste glass Waste glass beneficiation (Vinai and Soutsos, 2019) (2,4,1,3,1)
Rice husk ash Rice husk ash beneficiation (Tong et al., 2018) (2,4,2,3,1)

GBFS e granulated blast furnace slag.

granulation, drying, crushing and grinding (Marceau et al., 2007). 3. Results

Thus, materials and energy required to process GBFS were
modelled according to data from Marceau and VanGeem (2003). 3.1. Environmental assessment of mortars
With respect to CFA, emission associated with treatment process
was adopted from Kawai et al. (2005). Environmental impacts of The results generated as presented in Fig. 4 are based on the
capital good such as trucks, equipment, buildings were not environmental assessment of mix proportions of different mortars
considered in this study. Although, capital goods can have a sig- (Table 1). They illustrate the studied environmental impacts and
nificant influence on the total results (Liikanen et al., 2017), how- contribution of different input materials and energy to respective
ever, scope of this study is limited to materials and energy needed impact categories. Here, S3 and S4 are compared to S1 and S2 (see
to produce alkali-activated mortars. section 2.2.2 for a detailed description of scenarios).
As seen in Fig. 4, the most contributing materials to S1 and S2
are sodium silicate powder and sodium silicate solution respec-
2.2.4. Life cycle impact assessment tively. While WG-NaOH activator contribute the most to S3 and
The environmental impact categories that will be employed in RHA-NaOH activator and sodium hydroxide are the most contrib-
assigning LCI results to specific environmental issues will be based uting materials to S4. All the other materials had minimal contri-
on four impact categories: climate change, terrestrial acidification, bution of less than 10% in the respective impact categories, except
fossil depletion and Photochemical ozone creation (POC) (human for S3 and S4 where GBFS contributed 14% in fossil depletion
health). This is because, cement binder production is associated impact category and in photochemical ozone creation (POC) for-
with environmental issues such as consumption of energy, raw mation where sand contribute 14% to S4. Overall, chemically
materials and emissions to air, land, and water. Also, fuel handling modified waste-derived mortars in S3 and S4 have shown to have
and storage can be a potential source of soil and groundwater lower impacts than conventional mortars in S1 and S2. This is
contamination (Stajanca and Estokova, 2012). The associated because of substituting conventional activator with waste-derived
impact categories to these environmental issues will therefore be activator. This is also in agreement with other reported studies
relevant for assessment of emissions from binder and mortar pro- (Heath et al., 2014; McLellan et al., 2011; Passuello et al., 2017; Tong
duction processes (Chen et al., 2010; Van Den Heede and De Belie, et al., 2018).
2012). Results of other environmental impact categories (fine par- As seen in Fig. 4, with respect to climate change (excluding
ticulate matter formation, freshwater consumption, freshwater biogenic carbon), S3 and S4 both had 62% lower emissions when
ecotoxicity, freshwater eutrophication; human toxicity, ionizing compared to S1; 58% and 59% reduced emissions when compared
radiation, land use, marine ecotoxicity, metal depletion, strato- to S2 respectively leading to a potential reduction in greenhouse
spheric ozone depletion, terrestrial ecotoxicity) are given in the gases thereby reducing global mean temperature. This is a result of
supplementary material. Environmental performance modelling WG-NaOH and RHA-NaOH as alkali-activators respectively in S3
was conducted using GaBi 9.1.0.53 software and selected method and S4. Environmental impact of the waste-derived activators
was ReCiPe 2016 v1.1 (midpoint hierarchist time-frame) method mainly come from the treatment process and reaction of the wastes
(Thinkstep, 2019). ReCiPe indicators provide information on the with NaOH to produced sodium silicate. NaOH is the major
environmental issues associated with inputs and outputs of the contributor to the waste-derived activators, contributing 98% of
product system (EN ISO 14040, 2006). It is a widely adopted emissions in WG-NaOH activator and 69% emissions in RHA-NaOH
method due to its robustness (Hischier et al., 2010). activator. More information of environmental assessment of the
activators can be found in the supplementary material.
In the fossil depletion impact category, S3 had reduced fossil fuel
2.2.5. Sensitivity analysis extraction by 61% and 53% respectively, when compared to S1 and
Sensitivity analysis “is a procedure to determine how changes in S2. While S4 had reduced fossil fuel extraction by 59% and 51%
data and methodological choices affect life cycle assessment re- respectively, when compared to S1 and S2. High fossil fuel extrac-
sults” (EN ISO 14040, 2006). Sensitivity analysis is conducted to 1) tion from S1 and S2 are as a result of sodium silicate powder and
identify key parameters or factors influencing a product system and sodium silicate solution consuming 1 MJ/kg and 0.6 MJ/kg of fossil
the effect of different conditions on the product system 2) study fuel respectively, during production (Fawer et al., 1999). Fossil
uncertainty in a model input and apportioning of different sources depletion of WG-NaOH and RHA-NaOH mainly comes from sodium
of uncertainty in a model input (Guo and Murphy, 2012). For this hydroxide used during the reaction process to produce alkali-
study, sensitivity analysis will be based on the first option of how activator signifying lower fossil fuel extraction.
different factors influence a product system.
5
M. Abdulkareem, J. Havukainen, J. Nuortila-Jokinen et al. Journal of Cleaner Production xxx (xxxx) xxx

Fig. 4. LCIA results for the different scenarios.

With respect to terrestrial acidification, S3 and S4 had 75% lower in this study for sodium hydroxide is “EU NaOH from chlorine-alkali
emissions respectively when compared to S1 and S2, thereby electrolysis, 100% NaOH, using membrane, diaphragm and
reducing potential acidity of plant species. While, with respect to amalgam technology mix”. The alternative production methods
POC, S3 and S4 had reduced POC by 51% and 52% respectively when used for sensitivity analysis include “RER NaOH from brine solution,
compared S1, and reduced POC by 56% and 57% respectively, when 100% NaOH” and “DE NaOH using diaphragm route, 100% NaOH”.
compared to S2, reducing ozone creations leading to reduced fre- These are all collected from GaBi database. More information on the
quency and severity of respiratory diseases in human health. As emission factors of these different LCI can be found in the supple-
discussed in earlier impact categories, the major contributors are mentary material.
the activators and the avoided burden gained from using waste The highest impact was observed in RER NaOH in all impact
materials thereby lowering emissions from S3 and S4. Results categories, while EU NaOH had the least emissions. It can be
showing all impact categories can be found in the supplementary deduced that producing sodium hydroxide from brine solution
material. This shows that waste-derived activators can completely (RER NaOH) and diaphragm route (DE NaOH) respectively, caused
substitute conventional alkali-activators while also producing more environmental impacts compared to using a technology mix
materials of equivalent strengths. This is also in line with other of membrane, diaphragm and amalgam production method (EU
reported studies (Passuello et al., 2017). Furthermore, this con- NaOH) (Fig. 5). To further reduce the environmental footprints of
strues the fact that majority of environmental impacts from alkali- sodium hydroxide, more efficient production processes can be
activated materials are associated with the type of alkali-activator practiced which in overall improves the environmental footprint of
used (Abdulkareem et al., 2019a, 2019b) and a waste-derived acti- alkali-activated materials.
vator can significantly increase their environmental performance.

3.2.2. Sensitivity analysis on sodium silicate using different LCI data

3.2. Sensitivity analysis
Sodium silicate is a significant contributing material to the
overall LCA results. Sodium silicate powder and sodium silicate
Sensitivity analysis is conducted on the key parameters influ-
solution was utilized in S1 and S2, respectively. As a result, sensi-
encing the system. Based on the results, sodium silicate and NaOH
tivity analysis in this section was mainly between S1 and S2, using
are the major contributing materials to the environmental burdens
different LCI data. The original LCI data used is from Ecoinvent
of AAMs. Consequently, sensitivity analysis will be performed on
database while the alternative LCI data employed is from Fawer
these chemicals. Additionally, influence of allocation is determined
et al. (1999).
for WG and RHA respectively.
With respect to climate change and POC, Fawer et al. (1999)
exhibited higher impacts when compared to Ecoinvent in S1, at
3.2.1. Sensitivity analysis on sodium hydroxide using different an estimate of 48% and 71% respectively. However, results were
production methods contrariwise for S2 with decreased emissions at 13% and 12%
High amounts of sodium hydroxide are required to chemically respectively. In fossil depletion category, higher environmental
modify waste glass (S3) and RHA (S4) to produce alkali-activators. impact was observed in Fawer when compared to Ecoinvent for
Also, additional sodium hydroxide is required in the development both S1 and S2 at 63% and 3% respectively, while results were the
of aqueous alkali-activated mortar in S2 and S4 (see Table 1). Thus, other way round with respect to terrestrial acidification with
the sensitivity analysis was mainly between S2, S3 and S4, using decreased emissions of 15% and 51% respectively. These results as
different production methods. The main production method used shown in Fig. 6, show the interconnectedness of LCI data from both
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M. Abdulkareem, J. Havukainen, J. Nuortila-Jokinen et al. Journal of Cleaner Production xxx (xxxx) xxx

Fig. 5. Sensitivity analysis using different production methods for sodium hydroxide.

Fig. 6. Sensitivity analysis using alternative LCI data sources for sodium silicate.

Fawer et al. (1999) and Ecoinvent database. Conversely, a study 3.2.3. Sensitivity analysis on waste glass and RHA
carried out by European Commission on best available techniques Waste glass (WG) and RHA were assumed to be waste in this
(BAT) for manufacture of inorganic chemicals (EU, 2007), detailing study and only associated emissions from the treatment processes
inputs and outputs on sodium silicate solution, demonstrated that were considered. Based on this assumption, a sensitivity analysis
between 33% and 67% reduced environmental impact can be was performed to determine how mass allocation of these waste
actualised for the studied impact categories when compared to materials influence overall results of the study. Data for WG and
Fawer et al. (1999) and Ecoinvent database (see supplementary rice were collected from Ecoinvent. Allocation of RHA was esti-
material). This is because of reduced energy consumption and us- mated from rice (non-basmati) production. As discussed earlier,
age of more efficient technologies as document by BAT (EU, 2007). RHA share in rice husk is 18e22% of dry content by weight while
However, the study did not have detailed information for sodium 20% of rice husk is generated from rice paddy, which makes it
silicate powder. Nonetheless, it can be assumed that reduced approximately 4% of RHA from rice paddy. Thus, an estimate of 4%
emissions are also achieved. of emissions from production of rice (non-basmati) is allocated to
RHA (more details can be found in the supplementary material).
Fig. 7 presents the influence of allocating emissions to WG and RHA.
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M. Abdulkareem, J. Havukainen, J. Nuortila-Jokinen et al. Journal of Cleaner Production xxx (xxxx) xxx

Fig. 7. Sensitivity analysis based on mass allocation of RHA and waste glass.

Scenarios S3 and S4 are particularly focused on since they contain b) Cost of two-part RHA-NaOH alkali-activator: Price of RHA was
these respective wastes materials. According to Fig. 7, it can be seen collected from industrial trading sites (alibaba, 2019). Consid-
that WG and RHA are not so sensitive to the allocation procedure in ering the required mass proportion for RHA required for alkali-
all the analyzed impact categories, thus, overall, making S3 and S4 a activator production, average cost of RHA required for activator
more environmentally friendly option than S1 and S2. is 16 V/ton. Considering mass proportion of NaOH pellet
required to chemically modify RHA, cost of NaOH pellet was
estimated to be 36 V/ton of activator. Market price for electricity
in Finland was estimated 0.064 V/kWh as at 2018, thus, elec-
3.3. Cost analysis of mortars
tricity cost for producing alkali-activator from RHA has been
estimated to be 14 V/ton. In total, 69 V/ton has been estimated
To determine the viability of the AAMs considered in this study,
to produce aqueous alkali-activator of which 52% of the cost is as
financial cost comparison is required. Thus, this study examines a
a result of NaOH.
simplified cost of materials needed to generate the cost of a given
formulation of mortar. Sodium silicate provides a significant reac-
Prices of CFA and GBFS were collected from industrial trading
tive part of silica in combination with NaOH to produce conven-
sites with an average price of 35 V/ton and 43 V/ton respectively
tional alkali-activator. From data available on industrial trading
(alibaba, 2019). Price of water and sand were based on Finnish
websites (alibaba, 2019), conventional sodium silicate powder and
market prices, at an average price of 5 V/ton and 8 V/ton, respec-
solution was estimated to cost an average of 414 V/ton and 203
tively. Based on mass proportion of the different input materials,
V/ton respectively. NaOH pellets was estimated to cost an average
414 V/ton. The cost associated with production of the waste-
derived alkali-activator are as follows:

a) Cost of one-part WG-NaOH alkali-activator: Based on European

statistics, material price for recyclates such as waste glass is 55
V/ton (eurostat, 2019). Thus, considering the mass proportion of
WG needed for alkali-activator production, cost of WG was
estimated to be 29 V/ton of activator. Additionally, based on
mass proportion of NaOH pellet required to chemically modify
WG powder, cost of NaOH pellets was estimated to be 199 V/ton
of activator. Since it is assumed in this study that all wastes are
locally available, negligible transportation costs have been
considered. Electricity required for milling glass cullet to glass
powder is estimated to be 50 kWh/ton (Vinai and Soutsos,
2019). Thus, 26 kWh/ton is estimated for milling of glass
cullet. With market price of electricity for Finland estimated to
be 0.064 V/kWh as of 2018, 1.7 V/ton is required to mill glass
and energy cost for producing alkali powder from waste glass
has been estimated to be 38 V/ton. In total 268 V/ton has been
estimated to produce powder alkali-activator from WG, of
which 74% of the cost is a result of cost of NaOH. Fig. 8. Simplified cost analysis for the different alkali-activated mortars.

8
M. Abdulkareem, J. Havukainen, J. Nuortila-Jokinen et al. Journal of Cleaner Production xxx (xxxx) xxx

cost of the different mortars was calculated as presented in Fig. 8. 5. Conclusions

Error bars were used to depict the price range of the different
mortars. S3 and S4 AAM are slightly cheaper than S1 and S2 AAM, This study highlights the relevance of using waste-based acti-
however, there is also possibility of S1 and S2 been cheaper if the vators to produce alkali-activated mortars in developing environ-
lower values of the error bars are considered. These prices may vary mentally friendly materials. This study lays emphasis on one-part
quite much because there are no standardised prices for waste (powder) WG-derived alkali-activated mortar and two-part
materials (RHA, CFA and GBFS) as compared to OPC. With indus- (aqueous) RHA-derived alkali-activated mortar. In addition, a
trially produced AAMs and standardised prices, cheaper price of simplified cost analysis was carried to compare the cost of these
production can be achieved. different mortars to assess their economic sustainability. Conclu-
sions from this study include:

4. Discussion and perspectives - Waste glass and rice husk ash derived alkali-activated mortar
resulted in up to 62%, 61%, 76% and 56% lower emissions
Alkali-activated mortars are considered a low carbon alternative respectively, in all the four studied impact categories (climate
to cement mortars. However, producing a more compact and dense change, fossil depletion, terrestrial acidification and photo-
material with higher mechanical strength highly depends on the chemical ozone creation formation) when compared to con-
quantity of alkali-activator. Alkali-activators have also been high- ventional one- and two-part alkali-activated mortar.
lighted as the most contributing material to the environmental Additionally, one-part WG-derived alkali-activated mortar
impact of alkali-activated materials, with many studies recom- without additional sodium hydroxide during mortar produc-
mending using waste-derived alkali-activators as a substitute to tion, exhibits possibility of producing mortar almost completely
conventional alkali-activators. Furthermore, reduced emissions from side-streams (waste glass, fly ash and granulated blast
from sodium silicate can be achieved when fossil fuels are replaced furnace slag) while maintaining equivalent compressive
with renewable energy (Abdulkareem et al., 2019a). Despite this strength as conventional alkali-activated mortars.
been a sustainable alternative in producing alkali-activator, virgin - Waste glass and rice husk ash demonstrated little sensitivity to
raw materials are still consumed and a high energy consumption in mass allocation procedure, with increased emissions from 0.2%
production. WG and RHA have high volumes globally, containing to 5% in the above-mentioned impact categories, thus, making
significant shares of silicon oxide which is one of the major ele- the waste-derived alkali-activated mortar a more environmen-
ments required in developing alkali-activators. Hence, producing tally friendly option.
alkali-activator from these waste materials, will mean avoidance of - Sodium hydroxide was consistent in this study in chemically
virgin materials consumption and enhancing circularity of wastes. modifying waste glass and RHA to produce alkali-activators and
It should be noted RHA is predominantly produced in rainfed in the development of aqueous alkali-activated mortar. Thus, a
upland regions where rice is grown and incinerated. Therefore, sensitivity analysis was carried out on sodium hydroxide using
RHA might not be as available in some countries. On the other hand, data from different production methods. The default production
other silica rich agro-wastes such as straw can be used to replace method used in this study is “EU-28 sodium hydroxide from
RHA for countries where rice is not locally produced. WG is avail- technology-mix” while the alternative production method for
able almost everywhere, but its production is more distributed sensitivity analysis includes “RER sodium hydroxide from brine
regionally where only large cities produce significant amounts. solution” and “DE sodium hydroxide using diaphragm route”.
Therefore, collection from larger areas to the place of utilisation will Results illustrated that increased emissions between 1% and
be needed. Furthermore, material availability and quality of in- 153% was observed from the alternative production routes.
dustrial side-streams such as CFA and GBFS, are crucial to the Thus, sodium hydroxide production from technology-mix,
development of AAMs. These industrial side-streams are depen- demonstrated improved environmental performance than so-
dent on production quantity and method of production which can dium hydroxide from brine solution and diaphragm route,
lead to variability in their chemical compositions (Provis, 2018). respectively. However, with continuous improvement in the
GBFS is increasingly used in the cement industry, which can reduce emissions profile of the chlor-alkali industry, lower emissions
its availability for alkali-activated materials. Also, the adoption of can be expected when assessing sodium hydroxide production
renewable energy will limit the availability of CFA, which is a in future.
product of energy production from coal combustion. Consequently, - Sensitivity analysis on sodium silicate using an alternative LCI
research can investigate more materials that do not require much data (Fawer et al., 1999) showed that with respect to S1, 48%,
beneficiation (grinding, granulating, and high temperature pro- 63%, and 71% increased impact was observed respectively, for
cesses) and has zero to low conventional value for sustainable climate change, fossil depletion, and POC and 15% reduced
material productions. Thus, further studies will investigate the impact in acidification category. With respect to S2, between
scale of supply and demand of these materials and their proposed 12% and 51% of reduced impact is observed for all impact cate-
application. gories except fossil depletion which had a 3% increase. This is all
To further increase the environmental sustainability of waste- realised when alternative LCI data is compared to the original
derived activators and industrial side-streams, it is important, LCI data.
they are locally available. However, this usually is not the case, and - With respect to costs of producing waste-derived alkali-acti-
in some instances, raw materials must be transported from one vated mortars, analysis show that, a range of 9%e19% of cost
region to another. Transportation implies added cost in production savings can be achieved from using waste-derived alkali-acti-
and additional emissions. Depending on where the waste is sourced vated mortars compared to its conventional counterpart. Addi-
and where it is produced, transportation burdens might lower net tionally, local availability of primary and secondary raw
environmental and economic benefits of using wastes. Additionally, materials needed for production of alkali-activated materials
increased environmental performance can be actualised by utilis- will impact positively on the total cost of production.
ing waste heat or renewable energy in the production of waste-
derived alkali-activators and beneficiation processes of side- It can be concluded that significant environmental impact re-
streams. ductions are not only achieved from waste-derived alkali-activated
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M. Abdulkareem, J. Havukainen, J. Nuortila-Jokinen et al. Journal of Cleaner Production xxx (xxxx) xxx

mortars, but also provides a useful alternative to utilising waste Concr 131e149.
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CYCLE ASSESSMENT . PRINCIPLES AND FRAME- WORK (ISO 14040: 2006).
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quite safely that usage of waste glass or rice husk ash as an activator Assessment d Requirements and Guidelines, ISO 14044. https://doi.org/
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Habert, G., D’Espinose De Lacaillerie, J.B., Roussel, N., 2011. An environmental
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The authors declare that they have no known competing research trends. J. Clean. Prod. 19, 1229e1238. https://doi.org/10.1016/
financial interests or personal relationships that could have j.jclepro.2011.03.012.
appeared to influence the work reported in this paper. Heath, A., Paine, K., McManus, M., 2014. Minimising the global warming potential of
clay based geopolymers. J. Clean. Prod. 78, 75e83. https://doi.org/10.1016/
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Acknowledgements Hischier, R., Editors, B.W., Althaus, H., Bauer, C., Doka, G., Dones, R., Frischknecht, R.,
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Development Fund, through the urban innovative actions initiative Kamseu, E., Beleuk a  Moungam, L.M., Cannio, M., Billong, N., Chaysuwan, D.,
for co-financing the Urban Infra Revolution project under the Melo, U.C., Leonelli, C., 2017. Substitution of sodium silicate with rice husk ash-
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Supplementary data to this article can be found online at Liikanen, M., Havukainen, J., Hupponen, M., Horttanainen, M., 2017. Influence of
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management systems e a comparison of case studies in Finland and China.
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