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Experimental Investigation on Ambient-Cured One-Part Alkali-


Activated Binders Using Combined High-Calcium Fly Ash (HCFA)
and Ground Granulated Blast Furnace Slag (GGBS)

Citation for published version:


Teo, W, Shirai, K, Lim, JH, Jack, LB & Nikbakht, E 2022, 'Experimental Investigation on Ambient-Cured
One-Part Alkali-Activated Binders Using Combined High-Calcium Fly Ash (HCFA) and Ground Granulated
Blast Furnace Slag (GGBS)', Materials, vol. 15, no. 4, 1612. https://doi.org/10.3390/ma15041612

Digital Object Identifier (DOI):


10.3390/ma15041612

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materials
Article
Experimental Investigation on Ambient-Cured One-Part
Alkali-Activated Binders Using Combined High-Calcium Fly
Ash (HCFA) and Ground Granulated Blast Furnace Slag (GGBS)
Wee Teo 1, * , Kazutaka Shirai 2 , Jee Hock Lim 3 , Lynne B. Jack 4 and Ehsan Nikbakht 5

1 School of Energy, Geoscience, Infrastructure and Society (EGIS), Heriot Watt University Malaysia,
Putrajaya 62200, Malaysia
2 Faculty of Engineering, Hokkaido University, Sapporo 060-8628, Japan; shirai.kazutaka@eng.hokudai.ac.jp
3 Department of Civil Engineering, Universiti Tunku Abdul Rahman, Bandar Sungai Long, Cheras,
Kajang 43000, Malaysia; limjh@utar.edu.my
4 School of Energy, Geoscience, Infrastructure and Society (EGIS), Heriot-Watt University,
Edinburgh EH14 4AS, UK; l.b.jack@hw.ac.uk
5 Department of Civil and Environmental Engineering, Universiti Teknologi Petronas,
Seri Iskandar 32610, Malaysia; ehsan.nikbakht@utp.edu.my
* Correspondence: t.wee@hw.ac.uk; Tel.: +60-127560230

Abstract: The challenges of handling user-hostile alkaline solutions in the conventional alkali-
activated binders (AAB) have initiated the development of “just add water” or one-part solid-based
AAB systems. This paper aims to present a preliminary investigation on the development of one-part
 ambient-cured alkali-activated binders produced by synthesising high-calcium fly ash (HCFA) and

ground granulated blast furnace slag (GGBS) using sodium metasilicate anhydrous. Three test
Citation: Teo, W.; Shirai, K.; Lim, J.H.;
series were conducted in this study to investigate the effects of GGBS/binder, activator/binder and
Jack, L.B.; Nikbakht, E. Experimental
Investigation on Ambient-Cured
water/binder ratios on the fresh and hardened properties of the one-part synthesis AAB system. It
One-Part Alkali-Activated Binders was found that the SiO2 /Al2 O3 molar ratio plays an important role in the attainment of compressive
Using Combined High-Calcium Fly strength and limits the amounts of solid activators effective in contributing to the alkali-activation
Ash (HCFA) and Ground Granulated reaction process. The optimum SiO2 /Al2 O3 molar ratio was found between 3.20 and 3.30. The
Blast Furnace Slag (GGBS). Materials test results revealed that the optimum proportion between HCFA and GGBS was discovered at a
2022, 15, 1612. https://doi.org/ GGBS/binder ratio of 0.50. The optimum activator/binder ratio was between 0.08 and 0.12, and it
10.3390/ma15041612 is recommended that the water/binder ratio should not exceed 0.50. This study demonstrated the
Academic Editors: Paola Palmero, potential of the one-part synthesis method in the production of alkali-activated binder for practical
Jean-Marc Tulliani and structural applications.
Paola Antonaci
Keywords: one-part; alkali-activated binder; high-calcium fly ash; ground granulated blast furnace slag
Received: 9 January 2022
Accepted: 17 February 2022
Published: 21 February 2022

Publisher’s Note: MDPI stays neutral 1. Introduction


with regard to jurisdictional claims in
Ordinary Portland Cement (OPC) is one of the most widely used construction materials
published maps and institutional affil-
worldwide. It is strong, durable, cheap, and abundant in raw materials all over the world.
iations.
OPC manufacturing processes are known to be highly energy-intensive, which releases
huge amounts of carbon dioxide (CO2 ) emissions into the environment. It is generally
known that for every tonne of OPC, almost one tonne of CO2 is emitted. Given that the
Copyright: © 2022 by the authors.
cement industry is responsible for up to 7% of the world’s carbon emissions [1], there
Licensee MDPI, Basel, Switzerland. is an urgent driving need to develop more technically viable solutions or alternatives to
This article is an open access article conventional OPC with minimised energy consumption and carbon emissions.
distributed under the terms and Alkali-activated binder (AAB) is considered one of the promising contenders as a
conditions of the Creative Commons viable substitute for OPC. This binder is produced by synthesising aluminosilicate source
Attribution (CC BY) license (https:// materials of geological origin or industrial by-products with highly alkaline activators.
creativecommons.org/licenses/by/ The most commonly used aluminosilicate sources for alkali activation are fly ash (FA),
4.0/). ground granulated blast furnace slag (GGBS), metakaolin (MK), rice husk ash (RHA)

Materials 2022, 15, 1612. https://doi.org/10.3390/ma15041612 https://www.mdpi.com/journal/materials


Materials 2022, 15, 1612 2 of 22

and palm oil fuel ash (POFA) [2–7]. AAB has been regarded as an important element of
“sustainable cementing binder systems” for the future [8,9]. It offers a potential reduction
in CO2 emissions by as much as 80% or more, when compared to OPC [10]. Due to its
great potential, over the past decades, there has been growing interest in the development
and application of AAB. This is clearly reflected by the large number of research articles
published in various state-of-the-art reports [8,11–14].
There are basically two methods of producing AAB, either a one-part mix or a two-part
mix formulation. Most of the research on AAB is primarily focused on the two-part mix
type, also known as a solution-activated mixture. This type of AAB can be produced by
synthesising aluminosilicate sources with highly concentrated alkaline solutions made up
of sodium hydroxide (NaOH) and sodium silicate (Na2 SiO3 ). Both NaOH and Na2 SiO3 are
known for being hazardous and highly corrosive and handling such user-hostile solutions
can be extremely challenging, especially in large quantities for commercial applications.
One-part or “just add water” AAB is developed specially with the intention of tackling the
challenges of handling solution-based alkaline activators. Both aluminosilicate sources and
alkaline activators are in solid form (powder-based) and then blended to make the one-part
binder system. The activation process begins once water is added to the solid mixture. The
whole mixing and handling process is thus similar to conventional OPC concrete. The use
of the one-part system could increase the commercial viability of AAB for mass production
and large-scale applications in the construction industry.
Over the past decades, there have been several attempts at the synthesis of one-
part AAB with various combinations of aluminosilicate sources and solid activators.
Yang et al. [15] and Yang and Song [16] developed cementless binders using FA and GGBS
as the source materials and activated by either sodium silicate powder or a combination
of sodium silicate and sodium hydroxide powders. GGBS-based AAB achieved higher
compressive strength than FA-based AAB, with more notable strength development at
an early age. The FA-based AAB they produced showed very low 28-day compressive
strengths, in some cases less than 1 MPa. Hajimohammadi et al. [17] successfully produced
a one-part geopolymer system utilising geothermal silica and solid sodium aluminate. They
found that samples with less water content had a greater extent of crystallite formation,
possibly due to the rapid dissolution of the aluminate source and the relatively slower
dissolution of the silica source in the early stages of geopolymerisation. Hajimohammadi
and van Deventer [18] studied the effects of water content and Si/Al ratio on the reac-
tion mechanisms and physical properties of fly ash one-part systems synthesised by solid
sodium silicate. They found that the rates of release of Si and Al nutrients from source
materials greatly affect their availability for reaction and their extent of participation in a
geopolymer gel structure. In one-part mix systems, the usual crystalline phases that appear
in fly ash geopolymers are missing, and by increasing the Si/Al ratio, the extent of Si
contribution in the final geopolymer gel is reduced. Participation of more Si in the stages of
gel formation can be anticipated for samples with a lower water content. Waste valorisation
of FA and red mud to produce a one-part mix AAB was investigated by Choo et al. [19].
They found that one-part alkali-activated FA could be synthesised at ambient temperatures
using red mud as the solid alkali activator. However, the resulting compressive strengths
were low, less than 2 MPa. This is possibly due to the low pH level (<11) of the mate-
rials they produced, which would have hindered the active polycondensation reaction.
Kim et al. [20] found that calcium oxide (CaO) is a more effective activator for GGBS than
calcium hydroxide (Ca(OH)2 ) in terms of achieving higher compressive strengths and
producing more C-S-H gels.
Synthetic alkali silicates are the most widely used activators in either one-part or
two-part AAB mixtures [21]. For one-part AAB, synthetic sodium metasilicate anhydrous
has been proven to be highly effective for strength development [22–24]. Ma et al. [24]
investigated three different types of commercial sodium metasilicate powders, namely
Na2 SiO3 -anhydrous, Na2 SiO3 .5H2 O and Na2 SiO3 .9H2 O, respectively. In terms of strength
development, Na2 SiO3 -anhydrous achieved the highest followed by Na2 SiO3 ·9H2 O, and
Materials 2022, 15, 1612 3 of 22

Na2 SiO3 ·5H2 O was the lowest. The N-A-S-H gels developed in Na2 SiO3 -anhydrous and
Na2 SiO3 ·9H2 O-activated geopolymers appear to be better geopolymerised compared to
Na2 SiO3 ·5H2 O-activated geopolymers. To further minimise the CO2 emissions, alkalin-
ity and cost associated with Na2 SiO3 -anhydrous activated geopolymers, Ma et al. [25]
explored the possibility of partially replacing a portion of Na2 SiO3 -anhydrous with sodium
carbonate (Na2 CO3 ). The results showed that increasing the Na2 CO3 content decreases
the compressive strength and the quantity of gelatinous products, which eventually led to
many large micro-cracks and high porosity. Although a combined composite activator is an
attractive and cleaner solution, somehow this may sacrifice the performance and economic
benefit. To improve the commercial practicality of geopolymers, Askarian et al. [26] studied
various types of solid activators, such as sodium silicate, calcium hydroxide, sodium oxide,
lithium hydroxide, potassium carbonate and their combinations. They found that under the
ambient-cured condition, the highest compressive strength was obtained from a precursor
made up of 50% fly ash and 50% slag activated by a combination of sodium silicate, calcium
hydroxide and lithium hydroxide.
Regarding the precursor materials, the majority of the studies used low-calcium FA
as the aluminosilicate source. The use of high-calcium FA for one-part AAB systems is
extremely rare due to its flash setting and low workability characteristics [27]. In this study,
high-calcium FA combined with GGBS is synthesised using sodium metasilicate anhydrous
to produce an ambient-cured one-part AAB system. The use of GGBS enables to eliminate
the necessity of heat curing [5]. The effect of GGBS/binder, solid activator/binder and
water/binder ratios on the fresh and hardened properties of one-part AAB systems are
thoroughly investigated in this paper. Optimum proportion ratios as well as their statistical
correlations are proposed to pave the way for one-part AAB technology to be deployed in
future construction practices.

2. Experimental Programme
2.1. Materials
2.1.1. High-Calcium Fly Ash (HCFA)
Fly ash (FA) used in this study was obtained locally from YTL Cement Bhd Malaysia. The
oxide analysis of the FA determined by X-ray fluorescence (XRF) analysis is shown in Table 1.
The pozzolanic compounds level of the FA used in this study (SiO2 + Al2 O3 + Fe2 O3 ) is 61.9%
and can therefore be classified as Class C fly ash according to ASTM C618-12a [28] (i.e., >50%).
The FA contains a relatively high percentage of CaO (18.94%), greater than 10%, and
therefore is classified as high-calcium fly ash (HCFA).

Table 1. Oxide composition of HCFA and GGBS from XRF (by mass).

Material SiO2 Al2 O3 Fe2 O3 CaO MgO Na2 O K2 O TiO2 MnO


HCFA (%) 35.07 13.71 13.12 18.94 8.66 4.02 1.18 0.79 0.14
GGBS (%) 32.15 10.60 0.39 43.46 6.58 0.28 0.36 0.65 0.24

2.1.2. Ground Granulated Blast Furnace Slag (GGBS)


Ground granulated blast furnace slag (GGBS) used in this study was obtained from
the same supplier (YTL Cement Bhd Malaysia). The oxide composition of the GGBS is
shown in Table 1. It was off-white in colour and contained at least two-thirds by mass
of glassy slag and possesses hydraulic properties when suitably activated. The sum of
CaO, MgO and SiO2 in the GGBS constituted 86.8% of the total mass, while the basicity
ratio (CaO + MgO)/(SiO2 ) was 1.56, both of which satisfy the requirements specified in
BS EN 197-1: 2011 [29] (i.e., two-thirds for the sum of CaO, MgO and SiO2 (by mass) and
>1.0 for the basicity ratio).
Materials 2022, 15, 1612 4 of 22

2.1.3. Solid Activator


One-part or “just add water” geopolymers correspond to using a solid-based alkaline
activator to synthesise geopolymer composites. The solid alkali activator used in this
study was sodium metasilicate anhydrous, which is a similar solution to that adopted by
Nematollahi et al. [22]. The chemical contents of the sodium metasilicate anhydrous used
in this study were 51.10% Na2 O and 46.53% SiO2 , with a modulus ratio (Ms) and relative
density of 0.91 and 2.4, respectively.

2.2. Design Mix Proportions


The main purpose of this research is to investigate the main influencing parameters
in the development of appropriate mix proportions of an ambient-cured one-part alkali-
activated paste. The mixture consists of four main ingredients: high-calcium fly ash
(HCFA), ground granulated blast furnace slag (GGBS), solid activator (sodium metasilicates
anhydrous) and water. Three test series were planned in sequence to investigate the three
main influencing parameters, namely the ratios of GGBS/binder, activator/binder and
water/binder, summarised as follows:
1. Series A: This test series was the first series conducted to define the appropriate binder
proportion between HCFA and GGBS. The GGBS/binder ratio was taken as the main
parameter in this investigation. The activator/binder and water/binder ratios were
kept constant in this series at 0.12 and 0.40, respectively. A total of 8 mixes with
various proportions between HCFA and GGBS were conducted.
2. Series B: This test series was intended to evaluate the effect of the activator/binder
ratio on the one-part alkali-activated paste. After the evaluation of Series A, the opti-
mum GGBS/binder ratio will be used in this series. Additionally, the water/binder
ratio was kept constant at 0.40. In total, there are 6 mixes in this series.
3. Series C: In this final test series, the main variable will be the water/binder ratio. In
total, there are 4 mixes in this series. The GGBS/binder ratio and activator/binder
ratio used are based on the results obtained from Series A and B, respectively.
According to Yang et al. [15,16], the SiO2 /Al2 O3 molar ratio and calcium content
(CaO) in the source material, and the Na2 O/SiO2 molar ratio in the alkaline activator, play
very important roles on the alkali-activation mechanisms and mechanical properties of
the one-part geopolymer pastes. Recognising the importance, the above-proposed test
series will also include those molar ratios in their investigation. The effect of SiO2 /Al2 O3 ,
Na2 O/SiO2 and H2 O/Na2 O molar ratios will form part of the main study in test series A,
B and C, respectively.

2.3. Mixing, Casting and Curing


All mixes were prepared by using a 5-litre planetary mixer. Solid and dry materials,
which are comprised of FA, GGBS and solid activator, were first added into the mixer and
then dry-mixed for 3 min. The water was then gradually added to the dry materials and
the mixing continued for a further 3 min to produce the fresh and uniform paste. The fresh
paste was then cast into 50 mm cube moulds for the compressive strength test.
Immediately after casting, the moulds were covered with plastic film to avoid water
evaporation and then left overnight for demoulding the following day. After being de-
moulded, the specimens were fully wrapped with a plastic sheet and left to cure under
ambient conditions in the laboratory until the day of testing.

2.4. Test Methods


Two test methods were adopted in this experiment programme. Firstly, the flow table
test (or flow test) as per the standard ASTM C230 [30] was conducted immediately after
mixing to determine the consistency of the fresh geopolymer paste. The target flow spread
diameter was aimed for a minimum of 200 mm so that desirable rheological properties and
self-compacting capability of the paste can be achieved. Secondly, compressive strength
tests were conducted at 3, 7, 14 and 28 days of age. A total of twelve 50 mm cube moulds
Materials 2022, 15, 1612 5 of 22

were cast in each mixture to determine the compressive strength. Prior to testing, each
specimen was weighed to obtain their respective densities.

3. Results and Discussion


3.1. Test Series A: Proportion of HCFA and GGBS
As mentioned in the preceding section, test series A consisted of 8 mixes where the
primary variable is the binder proportion between HCFA and GGBS or the GGBS/binder
ratio. The activator/binder and water/binder ratios were kept constant at 0.12 and 0.40,
respectively. Table 2 summarises the mixture proportions and the molar ratios of critical
chemical compounds in the mixtures for this test series.

Table 2. Mixture proportions (by weight) for test series A.

HCFA GGBS Activator Water Molarity


Mix No. A/B W/B
% kg/m3 % kg/m3 kg/m3 kg/m3 Si/Al Na/Si H/Na (Na + K)/Al
A1 100 1153.85 0 0 0.12 138.46 0.40 461.54 2.965 0.25 3.94 0.827
A2 90 1047.14 10 116.35 0.12 139.62 0.40 465.40 3.012 0.242 4.091 0.812
A3 80 938.64 20 234.66 0.12 140.80 0.40 469.32 3.062 0.235 4.254 0.796
A4 70 828.29 30 354.98 0.12 141.99 0.40 473.31 3.113 0.227 4.43 0.780
A5 60 716.05 40 477.37 0.12 143.21 0.40 477.37 3.167 0.219 4.621 0.763
A6 50 601.87 50 601.87 0.12 144.45 0.40 481.49 3.224 0.211 4.83 0.745
A7 40 485.69 60 728.54 0.12 145.71 0.40 485.69 3.284 0.203 5.06 0.726
A8 0 0 100 1258.13 0.12 150.98 0.40 503.25 3.56 0.17 6.238 0.639
HCFA: high-calcium fly ash, GGBS: ground granulated blast furnace slag, A/B: activator/binder ratio,
W/B: water/binder ratio, Si/Al: molarity ratio of SiO2 /Al2 O3 , Na/Si: molarity ratio of Na2 O/SiO2 ,
H/Na: molarity ratio of H2 O/Na2 O, (Na + K)/Al: molarity ratio of (Na2 O + K2 O)/Al2 O3 .

3.1.1. Fresh Paste Properties


Figure 1 shows the flow characteristics of each fresh mixture immediately after mixing
(except for A1). Based on observation, the flow characteristics of mixtures A1, A2 and A3
form a thick and highly cohesive paste. The fresh mixture tends to flow by gravity and
shows a viscous property. Due to the highly cohesive paste, no flow spread diameter
readings were taken for those mixtures. The observed fresh properties’ behaviour was
mainly due to the low reactivity of HCFA. When activated with a solid activator, the HCFA
remained either unreactive or partially reactive. Sasui et al. [31] revealed that low reactivity
of Class C FA limits the leaching of major elements such as Si, Al and Ca to the matrix,
which could prolong the setting time and limit the formation of calcium silicate hydrate
(C-S-H) gel for strength development.
GGBS is more reactive than FA in improving flowability. The results show that an
increase in the replacement level of HCFA by GGBS between 30% and 50% dramatically
improved the flowability of the mixtures. Mixture A4 with a 30% replacement level of
GGBS (GGBS/binder = 0.30) obtained an average flow spread diameter of 196.5 mm, which
corresponds to 96.5% flow. The highest average flow spread diameter of 214.75 mm (114.8%
flow) was achieved with mixture A6, with a 50% replacement level (GGBS/binder = 0.50).
This replacement level is considered to be the threshold level. As observed from Figure 1,
when GGBS exceeded 50% (A7 and A8), the mixture became stiff with a quick setting
time. Similar observations were also reported by other researchers [5,32] on the effect of an
increase of GGBS content with a decrease in the initial and final setting times.
With a further increase in the replacement level of GGBS, there was a dramatic change
in the flowability of the mixture. As shown in Figure 1, mixtures A4, A5 and A6 exhibited
better flowability spread than mixtures A2 and A3. The results of flow table tests taken
from mixtures A4, A5 and A6 are plotted in Figure 2. Also included in the figure are the
percentage flow and the variation of the SiO2 /Al2 O3 molar ratio.
corresponds to 96.5% flow. The highest average flow spread diameter of 214.75 mm
(114.8% flow) was achieved with mixture A6, with a 50% replacement level (GGBS/binder
= 0.50). This replacement level is considered to be the threshold level. As observed from
Materials 2022, 15, 1612 Figure 1, when GGBS exceeded 50% (A7 and A8), the mixture became stiff with a quick 6 of 22
setting time. Similar observations were also reported by other researchers [5,32] on the
effect of an increase of GGBS content with a decrease in the initial and final setting times.

A2 A3 A4

A5 A6 A7

A8
Figure
Figure 1.
1. Flow
Flow characteristic
characteristic from
from test
test series
series A.
A.

3.1.2. Density
The dry density of one-part alkali-activated paste in each mixture was measured at
3, 7, 14 and 28 days. All results are presented in Table 3 and Figure 3. The density was
evaluated by weighing the mass and dimensions of three 50 mm cubes per age and taking
the average value.

Table 3. Density of one-part alkali-activated pastes from test series A (kg/m3 ).

Mix No. 3 Days 7 Days 14 Days 28 Days


A1 1906.67 1917.33 1922.67 1916
A2 1950.67 1922.67 1934.67 1921.33
A3 1948 1920 1921.33 1928
A4 1962.67 1949.33 1942.67 1953.33
A5 1958.67 1949.33 1950.67 1948
A6 1972 1961.33 1956 1954.67
A7 1957.33 1958.67 1966.67 1966.67
A8 1952 1961.33 1964 1953.33
Materials 2022,15,
Materials2022, 15,1612
x FOR PEER REVIEW 7 of2322
7 of

Mix No A4 A5 A6
Average diameter (mm) 196.50 178.75 214.75
Percentage flow (%) 96.5 78.8 114.8
Percentage flow (%) = difference between the flow spread and the inner base diameter of cone (100
mm) divided by the inner base diameter of the cone.

Figure2.2.Correlation
Figure Correlationof
ofSiO
SiO22/Al
/Al22OO3 3molarity
molarityratio
ratioand
andaverage
averageflow
flowspread
spreaddiameters
diameterstaken
takenfrom
from
mixtures
mixturesA4,
A4,A5
A5 and
and A6.
A6.

3.1.2.Generally,
Density dry density increases in relation to the SiO2 /Al2 O3 molar ratio and re-
placement level of GGBS. As can be seen from Figure 3, the densities increased along with
The dry density of one-part alkali-activated paste in each mixture was measured at
the steady increase of the SiO2 /Al2 O3 molar ratio due to the increase in the replacement
3, 7, 14 and 28 days. All results are presented in Table 3 and Figure 3. The density was
level of GGBS or the GGBS/binder ratio. It is evident that the increases in densities were
evaluated by weighing the mass and dimensions of three 50 mm cubes per age and taking
more pronounced when the GGBS/binder ratio exceeded 0.30. On average, the dry den-
the average value.
sities achieved 1955 kg/m3 at 28 days. It is interesting to note that mixture A8 with a
Generally, dry density increases in relation to the SiO2/Al2O3 molar ratio and replace-
GGBS/binder ratio of 1.0, despite having the highest SiO2 /Al2 O3 molar ratio (3.56), did
ment level of GGBS. As can be seen from Figure 3, the densities increased along with the
not exhibited the highest densities. As a matter of fact, it had lower densities at 28 days
steady increase of the SiO2/Al2O3 molar ratio due to the increase in the replacement level
compared to mixture A7.
of GGBS or the GGBS/binder ratio. It is evident that the increases in densities were more
Based on the observation, mixtures with combined HCFA/GGBS (such as mixtures A2–A6)
pronounced when the GGBS/binder ratio exceeded 0.30. On average, the dry densities
demonstrated the highest rates of dry density gain at an early age of 3 days, with densities
achieved 1955 kg/m3 at 28 days. It is interesting to note that mixture A8 with a
ranging from 1951 to 1972 kg/m3 . A slight decrease in density could be observed at later
GGBS/binder ratio of 1.0, despite having the highest SiO2/Al2O3 molar ratio (3.56), did not
ages, typically around a 0.5–1.5% reduction. This phenomenon is probably due to the low
exhibited the highest densities. As a matter of fact, it had lower densities at 28 days com-
alkali-activation reaction and water evaporation at later ages of curing.
pared to mixture A7.
3.1.3. Based on the observation,
Compressive Strength mixtures with combined HCFA/GGBS (such as mixtures
A2–A6) demonstrated the highest rates of dry density gain at an early age of 3 days, with
The results of the compressive strength obtained at 3, 7, 14 and 28 days with all
densities ranging from 1951 to 1972 kg/m3. A slight decrease in density could be observed
mixtures are presented in Table 4 and Figure 4. It should be noted that setting and hardening
at later ages, typically around a 0.5–1.5% reduction. This phenomenon is probably due to
of mixture A1 with 100% HCFA did not occur satisfactorily and strength development
the low alkali-activation reaction and water evaporation at later ages of curing.
failed to take place throughout the whole age of curing. As mentioned in Section 3.1.1, this
is mainly due to the low reactivity of HCFA that limits the leaching of Ca to the matrix. As
Table 3. Density of one-part alkali-activated pastes from test series A (kg/m3).
mentioned by Luukkonen et al. [33], the composition of binding phases of alkali-activated
bindersMixis No. 3 Days
greatly affected by the Ca content:7 Days 14 Days and C-A-S-H
N-A-S-H, C-(N)-A-S-H 28 Days gels are
formed in A1 low-, intermediate-,
1906.67 and high-calcium
1917.33 systems, respectively.
1922.67 Yang et al.
1916 [16] and
Kim et al.A2 [20] observed that in
1950.67 high-calcium one-part
1922.67 systems, the
1934.67 main binding
1921.33phase is
Materials 2022, 15, x FOR PEER REVIEW 8 of 23

A3 1948 1920 1921.33 1928


Materials 2022, 15, 1612
A4 1962.67 1949.33 1942.67 1953.33 8 of 22
A5 1958.67 1949.33 1950.67 1948
A6 1972 1961.33 1956 1954.67
A7 1957.33 1958.67 1966.67 1966.67
likely to be crystalline C-S-H and also C-A-S-H gels. It is well-documented [31,34] that the
A8 1952 1961.33 1964 1953.33
formation of C-S-H/C-A-S-H gels produces a compact matrix and improves the strength.

Density of one-part alkali-activated pastes 3 ), at the 3, 7, 14 and 28


Figure
Figure 3. 3.
Density of one-part alkali-activated pastes fromfrom test series
test series A (kg/m
A (kg/m 3), at the 3, 7, 14 and 28
days
days curing
curing periods.
periods.

It is obviousStrength
3.1.3. Compressive from Figure 4 that with GGBS introduced into the mixture, the gain of
compressive strength significantlystrength
The results of the compressive developed. As can
obtained at 3,be7,seen
14 and from
28 the
days result, strength
with all mix- gain
was directly proportional to the replacement levels of GGBS
tures are presented in Table 4 and Figure 4. It should be noted that setting and hardening and the SiO 2 /Al 2 O3 molar
ratio. The higher the content of GGBS, the greater the compressive
of mixture A1 with 100% HCFA did not occur satisfactorily and strength development strength development.
Tableto4take
failed alsoplace
includes the strength
throughout gainage
the whole ratio, taken as
of curing. Asthe ratio of in
mentioned compressive
Section 3.1.1,strength
this at
isamainly
designated
due toagetheto thereactivity
low compressiveof HCFA strength at 28 days.
that limits It is noteworthy
the leaching of Ca to thethat early-age
matrix.
Asstrength
mentioned development
by Luukkonen was etsignificant
al. [32], thein composition
the first 7 days. The compressive
of binding strength could
phases of alkali-acti-
reachbinders
vated up to 70–80%
is greatly ofaffected
the compressive
by the Castrength
content: at 28 daysC-(N)-A-S-H
N-A-S-H, depending on andthe replacement
C-A-S-H
level
gels areofformed
GGBS.inAs shown
low-, in Table 4, the
intermediate-, andstrength gain attainment
high-calcium at 3 and 7 days
systems, respectively. Yangfor mixture
et al.
A6and
[16] withKim a GGBS/binder ratio of
et al. [20] observed 0.50
that inwas 71% and 80%,
high-calcium respectively.
one-part systems, the It ismain
interesting
bindingto note
that at
phase 14 days,
is likely to bethe strength C-S-H
crystalline attainment wasC-A-S-H
and also shown as fairly
gels. It isconstant between [33,34]
well-documented mixtures A2
andthe
that A7,formation
regardless ofof the GGBS replacement
C-S-H/C-A-S-H gels produceslevel,awith an average
compact matrix of and84.7% of compressive
improves the
strength attained at 28 days.
strength.
It is obvious from Figure 4 that with GGBS introduced into the mixture, the gain of
compressive strength strength
Table 4. Compressive significantly developed.
of one-part As can bepastes
alkali-activated seen from
fromtesttheseries
result,
A. strength
gain was directly proportional to the replacement levels of GGBS and the SiO2/Al2O3 mo-
lar Compressive
ratio. The higherStrength (MPa) of GGBS, the greater the compressive
the content Strength Gain strengthRatiodevelop-
Mix No.
3 Days ment. 7Table
Days 4 also includes
14 Days the strength 28 Days gain ratio, ftaken
/f
3 28
as the ratio
f /f
7 28
of compressive
f14 /f28
strength at a designated age to the compressive strength at 28 days. It is noteworthy that
A1 0.00 0.00 0.00 0.23 0 0 0
early-age strength development was significant in the first 7 days. The compressive
A2 5.81 22.49 41.09 49.49 0.12 0.45 0.83
A3 24.12 strength could reach up
46.31 to 70–80% of 64.88
54.89 the compressive0.37 strength at 28 days 0.71 depending0.85 on
A4 39.45 51.64 61.28 73.11 0.54 0.71 0.84
A5 49.24 60.28 67.79 76.65 0.64 0.79 0.88
A6 57.09 64.07 68.63 80.07 0.71 0.80 0.86
A7 57.43 67.68 74.51 90.88 0.63 0.74 0.82
A8 49.92 70.07 77.88 78.45 0.64 0.89 0.99
f3 : Compressive strength at 3 days, f7 : compressive strength at 7 days, f14 : compressive strength at 14 days,
f28 : compressive strength at 28 days.
Materials
Materials2022,
2022,15,
15,x 1612
FOR PEER REVIEW 10 of
9 of2322

CorrelationofofSiO
Figure4.4.Correlation
Figure SiO2/Al
2 /Al O3 molar
2O23 molar
ratio
ratio and
and compressive
compressive strength
strength atat
3,3,7,7,1414and
and2828days
daysofof
one-part alkali-activated pastes from test series A (N/mm 2 ).
one-part alkali-activated pastes from test series A (N/mm ). 2

Mixture A8 with 100% GGBS showed a lower compressive strength at an early


3.1.4. Discussion of Results from Test Series A
age of 3 days and subsequently gained strength, with a higher compressive strength at
7 andThe14GGBS/binder
days compared ratiotowas investigated
mixtures A6 andinA7.this It
series. FA used to
is important in note
this study
that at is 14
a Class
days,
C-type high-calcium (Ca) fly ash (HCFA). Despite the high Ca content,
the compressive strength actually attained almost its full strength of 78.45 MPa at 28 days. its reactivity is
found to be either unreactive or partially reactive. Ca content has long
Despite the fact that mixture A8 had the highest SiO2 /Al2 O3 molar ratio (3.56), its compres- been known for its
rapid setting property,
sive strength at 28 daysand was hence lowlower
actually workability, and through
than mixtures A6 and theA7. coexistence
The results of showed
C-S-H
phase
that atit 28
improves the mechanical
days, mixtures A6 and properties
A7 achieved of compressive
the final products [27].of
strengths However,
80.1 andthis 90.9does
MPa,
not fully reflect in the results obtained from this series. Although
respectively. This is an interesting observation and in line with findings reported by other the flow characteristic
ofresearchers
mixture A1[18,27].in fresh conditions
According to exhibited
Chindaprasirta thicket and highly
al. [27], cohesive
increased SiOpaste, there was
2 content would
nolead to a decrease in compressive strength. They suggested that the optimum SiO2of
sign of setting and hardening of the paste after 28 days of curing. As a matter /Alfact,
2 O3
the compressive
molar ratio should strength development
fall between 3.20 andof3.70.mixture
Based A1onfailed to take
our test place at all.
observations from mixtures
A6, The
A7 and addition
A8, our of GGBS
optimum into SiO
the2proportion
/Al2 O3 molar improved
ratio was thearound
reactivity 3.20oftothe precursor
3.30. Once it
material
passed the andlimit,
enhanced the early
a decrease strength development
in compressive strength could at ambient curing
be observed. Asconditions.
depicted inThe mix-
flowability
ture A8, with performed
a SiO2 /Al wellO
2 3 between
molar GGBS/binder
ratio equal to ratios
3.56, it of 0.30 and
demonstrated 0.50.
a When
lower the ratio
compressive
exceeded
strength at 0.50, the flowability
28 days compared and setting A6
to mixtures time dramatically
and A7. reduced, as shown in mix-
tures A7 and A8. Obviously, compressive strength development increases along with the
3.1.4. content.
GGBS Discussion An of Results balance
optimum from Test Series A
between flowability in fresh conditions and compres-
sive strength is required in
The GGBS/binder order
ratio was toinvestigated
achieve a feasible
in thismixture.
series. Based
FA used on inthethis
results
studyfromis a
this
Classseries,
C-typethe optimum (Ca)
high-calcium proportion betweenDespite
fly ash (HCFA). HCFAthe andhighGGBS was found
Ca content, at a
its reactivity
GGBS/binder
is found to beratio of 0.50.
either This was
unreactive deduced reactive.
or partially based onCa thecontent
results of
hasflowlongspread diameter
been known for
its rapid setting property, and hence low workability, and through
and compressive strength from mixture A6. It achieved a compressive strength of 80 MPa the coexistence of C-S-H
atphase
28 daysit improves
with a flow the spread
mechanicaldiameterproperties of the
of 214.75 mm final products
(114.8% flow).[27]. However, this does
not The
fullyrelationship
reflect in theofresults obtained
compressive from this
strength series.
at 28 daysAlthough
with respectthe flow characteristic
to GGBS/binder ra-of
mixture
tios A1 ininfresh
is plotted Figureconditions exhibited
5. Generally, a thickshowed
the results and highly goodcohesive
correlations paste, there was
between com- no
sign of setting
pressive strength and
and hardening
GGBS/binder of the pastewith
ratios, aftera28 days of curing.
calculated correlationAs acoefficient
matter of fact,
(R2) the
of
compressive
0.956. The trend strength
showed development
that compressive of mixture A1 failed
strength increasedto take
withplace at all.
the GGBS/binder ratio,
reached a maximum at a GGBS/binder ratio of approximately 0.70, which of
The addition of GGBS into the proportion improved the reactivity the precursor
corresponds to
amaterial
SiO2/Al2O and enhanced
3 molar ratio the early and
of 3.348, strength
then development at ambient
decreased afterward. It iscuring conditions.
noteworthy The
that the
flowability performed well between GGBS/binder ratios of 0.30 and 0.50. When the
Materials 2022, 15, 1612 10 of 22

ratio exceeded 0.50, the flowability and setting time dramatically reduced, as shown in
mixtures A7 and A8. Obviously, compressive strength development increases along with
the GGBS content. An optimum balance between flowability in fresh conditions and
compressive strength is required in order to achieve a feasible mixture. Based on the
results from this series, the optimum proportion between HCFA and GGBS was found at a
GGBS/binder ratio of 0.50. This was deduced based on the results of flow spread diameter
and compressive strength from mixture A6. It achieved a compressive strength of 80 MPa
at 28 days with a flow spread diameter of 214.75 mm (114.8% flow).
The relationship of compressive strength at 28 days with respect to GGBS/binder
ratios is plotted in Figure 5. Generally, the results showed good correlations between
compressive strength and GGBS/binder ratios, with a calculated correlation coefficient (R2)
of 0.956. The trend showed that compressive strength increased with the GGBS/binder ratio,
reached a maximum at a GGBS/binder ratio of approximately 0.70, which corresponds to a
SiO2 /Al2 O3 molar ratio of 3.348, and then decreased afterward. It is noteworthy that the
predicted maximum compressive strength at a SiO2 /Al2O3 molar ratio of 3.348 corresponds
well to our test observations, which found that the optimum SiO2 /Al2 O3 molar ratios were
close, in the range between 3.20 and 3.30.

3.2. Test Series B: Activator to Binder Ratio


The main objective of test series B was to evaluate the optimum activator/binder
(A/B) ratio. The GGBS/binder ratio was kept at 0.50 following the results obtained from
test series A. The water/binder ratio was kept constant at 0.40. Table 5 summarises the
mixture proportions and the molar ratios of critical chemical compounds in the mixtures
for this test series. A total of six mixes including mixture A6 taken from test series A are
listed in Table 5.

3.2.1. Fresh Paste Properties


The flow characteristics of all mixtures in test series B are presented in Figures 6 and 7.
The flowability of the fresh state has been visually observed on all mixtures. As a general
trend, all mixtures, except mixture B5, exhibited considerable flowability spread, with
average flow spread diameters exceeding 200 mm. Based on the observation, mixture
B5 displayed a highly cohesive and viscous paste with a fast setting time. The flow
characteristics of the mixtures were greatly influenced by the Na2 O concentration in the
solid activators and source materials, which were commonly denoted by the Na2 O/SiO2
molar ratio. Table 5 summarises the Na2 O/SiO2 molar ratios of the mixtures in this
test series. Figure 7 shows the relationship between average flow spread diameters and
Na2 O/SiO2 molar ratios of the mixtures.

Table 5. Mixture proportions (by weight) for test series B.

HCFA GGBS Activator Water Molarity


Mix No. A/B W/B
% kg/m3 % kg/m3 kg/m3 kg/m3 Si/Al Na/Si H/Na (Na + K)/Al
B1 50 627.03 50 627.03 0.04 50.16 0.40 501.62 2.918 0.118 9.54 0.408
B2 50 620.54 50 620.54 0.06 74.47 0.40 496.43 2.995 0.143 7.67 0.492
B3 50 614.19 50 614.19 0.08 98.27 0.40 491.35 3.071 0.167 6.41 0.577
B4 50 607.97 50 607.97 0.10 121.59 0.40 486.37 3.148 0.19 5.51 0.661
A6 50 601.87 50 601.87 0.12 144.45 0.40 481.49 3.224 0.211 4.83 0.745
B5 50 595.89 50 595.89 0.14 166.85 0.40 476.71 3.301 0.232 4.30 0.829
HCFA: high-calcium fly ash, GGBS: ground granulated blast furnace slag, A/B: solid activator/binder ratio,
W/B: water/binder ratio, Si/Al: molarity ratio of SiO2 /Al2 O3 , Na/Si: molarity ratio of Na2 O/SiO2 , H/Na: mo-
larity ratio of H2 O/Na2 O, (Na + K)/Al: molarity ratio of (Na2 O + K2 O)/Al2 O3 .
Materials 2022, 15, x FOR PEER REVIEW 11 of 23

predicted maximum compressive strength at a SiO2/Al2O3 molar ratio of 3.348 corre-


Materials 2022, 15, 1612 11 of 22
sponds well to our test observations, which found that the optimum SiO2/Al2O3 molar
ratios were close, in the range between 3.20 and 3.30.

Materials 2022, 15, x FOR PEER REVIEW 12 of 23

The flow characteristics of all mixtures in test series B are presented in Figures 6 and
7. The flowability of the fresh state has been visually observed on all mixtures. As a gen-
eral trend, all mixtures, except mixture B5, exhibited considerable flowability spread, with
average flow spread diameters exceeding 200 mm. Based on the observation, mixture B5
displayed a highly cohesive and viscous paste with a fast setting time. The flow charac-
teristics of the mixtures were greatly influenced by the Na2O concentration in the solid
Figure
Figure 5. 5. Relationship
activators andofsource
Relationship of compressive
materials,
compressive strength
which
strength at were
28 daysat 28 days
commonly
with GGBSwith GGBS
denoted
to binder to
thebinder
byratios Na ratios
2O/SiO
(GGBS/B (GGBS/B ratio).
2 molar
ratio).
ratio. Table 5 summarises the Na2O/SiO2 molar ratios of the mixtures in this test series.
3.2. Test From
Series7Figure
Figure B:shows 7,
theitrelationship
Activator toisBinder
evident that initially,
between
Ratio flowability
average flow increased
spread diameters andwith the increase
Na2O/SiO 2 of
theThe molar
Na2main ratios
O/SiO of the
2 molar mixtures.
objective of ratio between
test series B was0.118 and 0.167,
to evaluate which corresponded
the optimum activator/binderto mixtures
B1–B3 From
with Figure 7, it is evident
activator/binder that
ratios ofinitially,
0.04 to flowability
0.08. increased
Mixtures B2 andwithB3 theachieved
increase ofthe highest
(A/B) ratio. The GGBS/binder ratio was kept at 0.50 following the results obtained from
the Na2O/SiO2 molar ratio between 0.118 and 0.167, which corresponded to mixtures B1–
average
test series A. flow
Thespread diameter
water/binder ratio with
was keptcomparatively
constant at 0.40.close values
Table at 263.25the
5 summarises and 266 mm,
B3 with activator/binder ratios of 0.04 to 0.08. Mixtures B2 and B3 achieved the highest
respectively.
mixture Further
proportions and increasing
the molar the
ratios Na
of O/SiO
critical
2 molar
chemical
2 ratio beyond
compounds
average flow spread diameter with comparatively close values at 263.25 and 266 mm, re-
in 0.167
the led
mixtures to a decline in
for thisspectively.
test series.
flowability, which A total
impliedof six mixes
that anyincluding
higher mixture
amount
Further increasing the Na2O/SiO2 molar ratio beyond A6
of taken
Na O from test
exceeding series
a
2 0.167 led to a decline A
Na are
O/SiO
2 in 2 molar
listed
ratioinflowability,
ofTable
0.1675.inwhich
the solid
implied activators can significantly
that any higher amount of Na2reduce the flowability
O exceeding a Na2O/SiO2 molarof fresh pastes.
ratio of 0.167
The results revealedin thethat
solidmixture
activatorsB3canwith
significantly reduce the flowability
an activator/binder ratio ofoffresh
0.08 pastes.
(corresponds to
Table 5.TheMixture proportions (by weight) for test series B.
a Na2 O/SiO2 molar ratio = 0.167) proved to be the optimum amount of solid to
results revealed that mixture B3 with an activator/binder ratio of 0.08 (corresponds activator in
Mix HCFA GGBS a Na2O/SiO 2 molar ratio = 0.167) proved to be the optimum amount of solid activator in
Activator Water Molarity
termstermsofA/B
flowability.
of flowability.
Interestingly,
W/B
Interestingly,
a similar
a similar
finding was also reported by Oderji
finding was also reported by Oderji et al. [35].
et al. [35].
No. % kg/m3 % kg/m 3 kg/m 3 kg/m 3 Si/Al Na/Si H/Na (Na + K)/Al
B1 50 627.03 50 627.03 0.04 50.16 0.40 501.62 2.918 0.118 9.54 0.408
B2 50 620.54 50 620.54 0.06 74.47 0.40 496.43 2.995 0.143 7.67 0.492
B3 50 614.19 50 614.19 0.08 98.27 0.40 491.35 3.071 0.167 6.41 0.577
B4 50 607.97 50 607.97 0.10 121.59 0.40 486.37 3.148 0.19 5.51 0.661
A6 50 601.87 50 601.87 0.12 144.45 0.40 481.49 3.224 0.211 4.83 0.745
B5 50 595.89 50 595.89 0.14 166.85 0.40 476.71 3.301 0.232 4.30 0.829
HCFA: high-calcium fly ash, GGBS: ground granulated blast furnace slag, A/B: solid activa-
tor/binder ratio, W/B: water/binder ratio, Si/Al: molarity ratio of SiO2/Al2O3, Na/Si: molarity ratio
of Na2O/SiO2, H/Na: molarity ratio of H2O/Na2O, (Na + K)/Al: molarity ratio of (Na2O +
K2O)/Al2O3.

B1 3.2.1. Fresh Paste Properties B2 B3

B4 B5
Figure 6. Flow characteristics from test series B.
Figure 6. Flow characteristics from test series B.
Materials2022,
Materials 2022,15,
15,1612
x FOR PEER REVIEW 13 12
ofof2322

Mix No B1 B2 B3 B4 A6 B5
Average diameter (mm) 238.00 263.25 266.00 249.75 214.75 126.68
Percentage flow (%) 138 163.3 166 149.8 114.8 26.7
Percentage flow (%) = difference between the flow spread and the inner base diameter of cone (100
mm) divided by the inner base diameter of the cone

Figure
Figure 7. CorrelationofofNa
7. Correlation Na 2 O/SiO
2O/SiO 2 molarity
2 molarity ratioratio and average
and average flow spread
flow spread diameters
diameters from
from test test
series
series
B. B.

3.2.2. Density
3.2.2. Density
The dry densities of the one-part geopolymer paste in each mixture measured at 3, 7, 14
The dry densities of the one-part geopolymer paste in each mixture measured at 3, 7,
and 28 days are presented in Table 6 and Figure 8. The density was evaluated by weighing
14 and 28 days are presented in Table 6 and Figure 8. The density was evaluated by weigh-
the mass and dimensions of three 50 mm cubes per age and taking the average value. For
ing the mass and dimensions of three 50 mm cubes per age and taking the average value.
mixture B5, only one cube was prepared for ages of 3, 7 and 14 days due to the damage of
For mixture B5, only one cube was prepared for ages of 3, 7 and 14 days due to the damage
specimens during the demoulding process.
of specimens during the demoulding process.
Figure 8 shows that at all ages, the dry density increased with the increase in the
Table 6. Density of one-part alkali-activated pastes from test series B (kg/m3 ).
amounts of solid activators or the Na2O/SiO2 molar ratio. The main reaction product in
high-calcium
Mix No. one-part systems 3-Day is likely crystalline
7-Day C-S-H and also C-A-S-H gels.
14-Day It is gen-
28-Day
erally understood that a high Na2O/SiO2 molar ratio (or Na2O concentration) promotes
B1 1925.33 1885.33 1880 1868
high levels
B2 of the alkali-activation
1898.67 process,1910.67
which leads to the1894.67
formation of more C-S-H/C-
1906.67
A-S-H gels
B3 and a denser morphology
1921.33 [3,36,37].
1910.67 1918.67 1932
Generally,
B4 the rate 1966.67
of dry density gain1942.67
was demonstrated1948 to be the highest 1942.67
at the early
age of 3A6 days, with densities 1972ranging between1961.33
1899 and 1976 kg/m1956 3, and then it1954.67
decreased
B5 1976 * 1960 * 1964 *
at later ages, with the highest reduction up to 3.0%. These observations were clearly 1966 re-
* vealed
The result is based on only one cube specimen due to damage of cube specimens during the
in mixtures B1, B4, A6 and B5. The reduction is probably due to the low alkali- demoulding stage.
activation reaction and water evaporation at a later age of curing.
Figure 8 shows that at all ages, the dry density increased with the increase in the
amounts of solid activators or the Na2 O/SiO2 molar ratio. The main reaction product
Table 6. Density of one-part alkali-activated pastes from test series B (kg/m3).
in high-calcium one-part systems is likely crystalline C-S-H and also C-A-S-H gels. It is
Mix understood
generally No. that3-Day
a high Na2 O/SiO 7-Day
2 molar ratio (or14-Day
Na2 O concentration) 28-Day
promotes
high levels B1 of the alkali-activation
1925.33 process, which leads to the1880
1885.33 formation of more C-S-H/C-
1868
A-S-H gels B2 and a denser1898.67morphology [3,36,37].
1910.67 1894.67 1906.67
B3 1921.33 1910.67 1918.67 1932
B4 1966.67 1942.67 1948 1942.67
A6 1972 1961.33 1956 1954.67
B5 1976 * 1960 * 1964 * 1966
Materials 2022, 15, 1612 13 of 22
* The result is based on only one cube specimen due to damage of cube specimens during the
demoulding stage.

Density 3 at the 3, 7, 14 and


Figure8.8.Density
Figure ofof one-part
one-part alkali-activated
alkali-activated pastes
pastes from
from testtest series
series B (kg/m
B (kg/m 3), at),
the 3, 7, 14 and 28
28 days
days curing
curing periods.
periods.

Generally, the rate of dry density gain was demonstrated to be the highest at the
early age of 3 days, with densities ranging between 1899 and 1976 kg/m3 , and then it
decreased at later ages, with the highest reduction up to 3.0%. These observations were
clearly revealed in mixtures B1, B4, A6 and B5. The reduction is probably due to the low
alkali-activation reaction and water evaporation at a later age of curing.

3.2.3. Compressive Strength


The results of compressive strength for test series B measured at 3, 7, 14 and 28 days
are presented in Table 7 and Figure 9. Similar to dry densities, the compressive strength
increased with the amount of solid activators or the activator/binder ratios. Figure 9 also
shows the relationship between compressive strengths and the Na2 O/SiO2 molar ratio.

Table 7. Compressive strength of one-part alkali-activated pastes from test series B (N/mm2 ).

Compressive Strength (MPa) Strength Gain Ratio


Mix No.
3 Days 7 Days 14 Days 28 Days f3 /f28 f7 /f28 f14 /f28
B1 16.27 22.89 27.68 31.09 0.52 0.74 0.89
B2 25.80 34.51 40.39 47.04 0.55 0.73 0.86
B3 34.79 41.60 56.31 59.89 0.58 0.69 0.94
B4 40.73 53.57 64.83 70.81 0.58 0.76 0.92
A6 57.09 64.07 68.63 80.07 0.71 0.80 0.86
B5 55.60 * 66.48 * 78.24 * 79.86 0.70 0.83 0.98
* The result is based on only one cube specimen due to damage of cube specimens during the demoulding stage.
f3 : Compressive strength at 3 days, f7 : compressive strength at 7 days, f14 : compressive strength at 14 days,
f28 : compressive strength at 28 days.
Si/Al ratio. From their microstructural analysis, it showed that for samples with a high
Si/Al ratio, the microstructure was less dense with larger pore formation. In terms of me-
Materials 2022, 15, 1612 14 of 22
chanical strength, they also indicated lower compressive strengths with increased Si/Al
ratios.

CorrelationofofNa
Figure9.9.Correlation
Figure Na2O/SiO
2 O/SiO 2 molar
2 molar
ratio
ratio and
and compressive
compressive strength
strength atat
3,3,7,7,1414and
and2828days
daysofof
one-partalkali-activated
alkali-activatedpastes
pastesfrom
fromtest
testseries
seriesBB(N/mm
(N/mm 2
one-part 2). ).

Mixture B1 with an activator/binder ratio of 0.04 achieved a compressive strength


3.2.4. Discussion of Results from Test Series B
of 31.1 MPa at 28 days. As shown in mixtures B2, B3 and B4, the compressive strength
at 28This testincreased
days series investigated
by 51.3%,the influence
92.6% of the solid
and 127.8%, activator/binder
respectively, compared(A/B) toratio on
mixture
the fresh and mechanical properties of an ambient-cured one-part
B1. The highest compressive strength at 28 days was attained from mixture A6 with an alkali-activated binder.
Sodium metasilicate
activator/binder (Naof
ratio 2SiO3) anhydrous was used as the solid alkaline activator. Often,
0.12 at the value of 80.1 MPa, which corresponds to a 157.5%
the activator concentration
increase compared to mixture is expressed
B1. It should by the
beNa 2O/SiO2 molar ratio. It is well-docu-
noted that there was no sign of further
mented that the Na 2 O/SiO 2 molar ratio
increments in compressive strength in mixture B5 when plays a vital role
theinactivator/binder
the alkali-activation process
ratio increased
[3,36–38].
to 0.14. As a matter of fact, mixture B5 achieved an almost identical compressive strength
valueHigh Na2O/SiO
to mixture A6, 2 molar
of 79.8ratios
MPa,encouraged
at 28 days. more alkali activation with the aluminosil-
icate materials
Table 7 presents the strength gainHCFA/GGBS)
(in this case, combined ratios calculatedandatled
3, 7toandthe14formation
days for ofall more C-
mixtures.
S-H/C-A-S-H gel, denser morphology, lower porosity and therefore
In terms of compressive strength development, all mixtures could gain at least 50% and higher compressive
strength.
70% of the Ascompressive
demonstrated from our
strength at 28results, dry
days at densities
the early age andof compressive
3 and 7 days,strength in-
respectively.
creased with the Na2O/SiO
The activator/binder molar
ratio2had ratio. However,
a significant effect onthere appeared compressive
the early-age to be a limit strength
on the
effective amounts
development. Asof solid activators
demonstrated in the contribution
in mixtures A6 and B5,toa the higheralkali-activation
activator/binder reaction
ratio
process.
resultedOur resultsstrength
in higher indicated gainthat thisatlimit
ratios is greatly
3 and influencedtoby
7 days compared the SiO
mixture 2/Al
B1. 2O3 molar
After 7 days,
ratio. According
the strength gaintoappeared
Section 3.1,to bethemore
optimum SiO2/Al
consistent 2O3 molar
throughout allratio shouldItfall
mixtures. between
is interesting
3.20 and that
to note 3.30.atAny mixtures
14 days, exceeding
mixture this range
B5 attained almostof the SiOto
equal 2/Al
its2O 3 molar
full ratio would
compressive not
strength
show
at 28 further increases
days, with in compressive
a strength gain ratio of strength, even when provided
0.98. Additionally, as mentioned with earlier,
high amounts
mixture
ofB5solid
did activators,
not indicateasany signdemonstrated
clearly of further increments
in mixturein compressive
B5 in this series.strength at 28 days and
achieved an almost identical
The relationship strength
of flowability value of
(in terms to average
mixture flow
A6. This
spread observation
diameters) implied
and com-that
there is probably
pressive strength at a limit
28 dayson the
witheffective
respectamounts of solid activators
to activator/binder ratios isneeded
plottedtoincontribute
Figure 10.to
Itthe alkali-activation
is evident reaction
that flowability process.
and compressive strength showed good correlations with ac-
tivator/binder ratios. The calculated source
The GGBS/binder ratio of the material
correlation was kept
coefficients constant
(R2) in this series
for flowability and at 0.50.
com-
The SiO /Al
pressive strength
2 O molar ratio of the mixtures increased due to the increase
2 3 were 0.987 and 0.996, respectively. Both predicted trends follow closely of the amount
of Na2 SiO3 solid activators. Mixture B5 had a SiO2 /Al2 O3 molar ratio equal to 3.30. As
explained in Section 3.1.3, according to Chindaprasirt et al. [27], there is a limit on the extent
of SiO2 content in relation to compressive strength. Once past the limit, it would lead to
a decrease in compressive strength. Our findings from test series A suggested that our
Materials 2022, 15, 1612 15 of 22

optimum SiO2 /Al2 O3 molar ratio fell between 3.20 and 3.30, which somehow explained
why mixture B5 exhibited no further increase in strength.
According to Hajimohammadi et al. [18], a higher SiO2 /Al2 O3 (Si/Al) molar ratio
could potentially decrease the amount of Si contribution in the final geopolymer gel and
the geopolymerisation reaction rate in FA one-part geopolymers. This is mainly due to
the formation of larger unreactive silica oligomers instead of small reactive species at a
high Si/Al ratio. From their microstructural analysis, it showed that for samples with a
high Si/Al ratio, the microstructure was less dense with larger pore formation. In terms
of mechanical strength, they also indicated lower compressive strengths with increased
Si/Al ratios.

3.2.4. Discussion of Results from Test Series B


This test series investigated the influence of the solid activator/binder (A/B) ratio
on the fresh and mechanical properties of an ambient-cured one-part alkali-activated
binder. Sodium metasilicate (Na2 SiO3 ) anhydrous was used as the solid alkaline acti-
vator. Often, the activator concentration is expressed by the Na2 O/SiO2 molar ratio.
It is well-documented that the Na2 O/SiO2 molar ratio plays a vital role in the alkali-
activation process [3,36–38].
High Na2 O/SiO2 molar ratios encouraged more alkali activation with the aluminosil-
icate materials (in this case, combined HCFA/GGBS) and led to the formation of more
C-S-H/C-A-S-H gel, denser morphology, lower porosity and therefore higher compres-
sive strength. As demonstrated from our results, dry densities and compressive strength
increased with the Na2 O/SiO2 molar ratio. However, there appeared to be a limit on the
effective amounts of solid activators in the contribution to the alkali-activation reaction
process. Our results indicated that this limit is greatly influenced by the SiO2 /Al2 O3 molar
ratio. According to Section 3.1, the optimum SiO2 /Al2 O3 molar ratio should fall between
3.20 and 3.30. Any mixtures exceeding this range of the SiO2 /Al2 O3 molar ratio would not
show further increases in compressive strength, even when provided with high amounts of
solid activators, as clearly demonstrated in mixture B5 in this series.
The relationship of flowability (in terms of average flow spread diameters) and com-
pressive strength at 28 days with respect to activator/binder ratios is plotted in Figure 10.
It is evident that flowability and compressive strength showed good correlations with
activator/binder ratios. The calculated correlation coefficients (R2) for flowability and com-
pressive strength were 0.987 and 0.996, respectively. Both predicted trends follow closely
to the actual test results. The results showed that mixtures with an activator/binder ratio
beyond 0.12 (such as mixture B5, activator/binder ratio = 0.14, SiO2 /Al2 O3 ratio = 3.301)
did not reveal a noticeable improvement in compressive strength. Whereas in terms of
flowability, a pronounced effect in reducing the flowability of the mixture could be observed
after the activator/binder ratio exceeded 0.08.
Given the above interpretation, it could be deduced that activator/binder ratios in the
range between 0.08 and 0.12, which corresponds to a Na2 O/SiO2 molar ratio from 0.167
to 0.211, are the optimum ratios in satisfying flowability performance and attainment of
reasonable compressive strength as high as 80 MPa. It should be emphasised that one of
the issues associated with the use of excessive alkali in some conventional alkali-activated
formulations is efflorescence, especially for ambient-cured alkali-activated cements [26].
Therefore, the selection of an optimum activator/binder ratio must also consider reducing
the amount of activators used so as to increase the economic and environmental benefits of
one-part alkali-activated cement.

3.3. Test Series C: Water to Binder Ratio


Test series C aimed to investigate the influence of the water/binder (W/B) ratio
between 0.40 and 0.55 on the fresh and mechanical properties of the one-part alkali-activated
binder. Following the outcomes from test series B, an A/B ratio of 0.08 was selected in the
study. The GGBS/binder ratio was kept constant at 0.50 following the results obtained
ability, a pronounced effect in reducing the flowability of the mixture could be observed
after the activator/binder ratio exceeded 0.08.
Given the above interpretation, it could be deduced that activator/binder ratios in the
range between 0.08 and 0.12, which corresponds to a Na2O/SiO2 molar ratio from 0.167 to
0.211, are the optimum ratios in satisfying flowability performance and attainment of rea-
Materials 2022, 15, 1612 sonable compressive strength as high as 80 MPa. It should be emphasised that one of16the of 22
issues associated with the use of excessive alkali in some conventional alkali-activated
formulations is efflorescence, especially for ambient-cured alkali-activated cements [37].
Therefore,
from test the selection
series of anofoptimum
A. A total four mixesactivator/binder ratio B3
including mixture must alsofrom
taken consider reducing
test series B are
the
listed in Table 8, which summarises the mixture proportions and the molar ratios benefits
amount of activators used so as to increase the economic and environmental of critical
ofchemical
one-partcompounds
alkali-activated
in thecement.
mixtures for this test series.

Figure 10. Relationship of average flow spread diameters and compressive strength at 28 days with
Figure 10. Relationship of average flow spread diameters and compressive strength at 28 days with
activator to binder ratios (A/B ratio).
activator to binder ratios (A/B ratio).

Table 8. Mixture proportions (by weight) in test series C.


3.3. Test Series C: Water to Binder Ratio
HCFA Test series C aimed Activator
GGBS to investigate the influence
Water of the water/binderMolarity(W/B) ratio be-
Mix No. A/B W/B
% kg/m3 tween
% 0.40 and
kg/m 3 0.55 on the fresh
kg/m 3 and mechanical properties
kg/m 3 Si/Al of the one-part
Na/Si alkali-activated
H/Na (Na + K)/Al
B3 50 614.19 binder.
50 Following
614.19 the outcomes
0.08 98.27 from0.40 test series B, an A/B ratio of 0.08 was
491.35 6.412selected in the
C1 50 578.65 study.
50 The GGBS/binder
578.65 0.08 ratio
92.58 was kept
0.45 constant
520.78 at 0.50 following the7.214 results obtained
3.071 0.167 0.577
C2 50 547 50 547 0.08 87.52 0.50
from test series A. A total of four mixes including 547 mixture B3 taken from 8.015
test series B are
C3 50 518.63 50 518.63 0.08 82.98 0.55 570.49 8.817
listed in Table 8, which summarises the mixture proportions and the molar ratios of criti-
HCFA: high-calcium fly ash, GGBS: ground granulated blast furnace slag, A/B: solid activator/binder ratio,
cal chemical
W/B: compounds
water/binder in the
ratio, Si/Al: mixtures
molarity ratio offor
SiO this
/Al test series.molarity ratio of Na O/SiO , H/Na: mo-
O , Na/Si:
2 2 3 2 2
larity ratio of H2 O/Na2 O, (Na + K)/Al: molarity ratio of (Na2 O + K2 O)/Al2 O3 .
Table 8. Mixture proportions (by weight) in test series C.
3.3.1. Fresh Paste Properties
Mix HCFA GGBS Activator Water Molarity
TheA/B
flow W/B
characteristic results from test series C are presented in Figure
No. % kg/m3 % kg/m 3 kg/m 3 kg/m 3 Si/Al Na/Si H/Na (Na + 11. The
K)/Al
influence of the W/B ratio in the one-part alkali-activated binder behaved exactly the same
B3 50 614.19 50 614.19 0.08 98.27 0.40 491.35 3.071 0.167 6.412 0.577
as the water/cement (W/C) ratio in the conventional OPC-based binder. Water content is
an important parameter that affects flowability. The increase of the W/B ratio increased
the flowability of the mixtures. Another usual way of expressing the amount of water
demand in one-part alkali-activated binder studies is the H2 O/Na2 O molar ratio [33].
The H2 O/Na2 O molar ratios of all mixtures are tabulated in Table 8 and also plotted in
Figure 11. As clearly demonstrated in Figure 11, the average flow spread diameters steadily
increased with the H2 O/Na2 O molar ratios.
as the water/cement (W/C) ratio in the conventional OPC-based binder. Water content is
an important parameter that affects flowability. The increase of the W/B ratio increased
the flowability of the mixtures. Another usual way of expressing the amount of water
demand in one-part alkali-activated binder studies is the H2O/Na2O molar ratio [32]. The
H2O/Na2O molar ratios of all mixtures are tabulated in Table 8 and also plotted in Figure
Materials 2022, 15, 1612 17 of 22
11. As clearly demonstrated in Figure 11, the average flow spread diameters steadily in-
creased with the H2O/Na2O molar ratios.

Mix No B3 C1 C2 C3
Average diameter (mm) 266 315 348.75 381.25
Percentage flow (%) 166 215 248.8 281.3
Figure 11.
Figure 11. Average
Average flow
flow spread
spread diameters
diameters from
from test
test series
series C.
C.

3.3.2.
3.3.2. Density
Density
Similar
Similar to
to the
the previous
previous test series,
series, the
the density
density was
was measured
measuredby byweighing
weighingthe themass
mass
and
and dimensions
dimensions ofofthree
three5050mmmm cubes
cubes perper
ageage
andand taking
taking the average
the average value.value. The
The dry dry
den-
density results
sity results taken
taken from from
thisthis
test test series
series are summarised
are summarised in Table
in Table 9 and9 and Figure
Figure 12. Also
12. Also in-
included
cluded ininFigure
Figure1212 are
are thethe curves
curves forfor
thethe
H2H2 O/Na
O/Na 2 O molar
2O molar ratio.
ratio. The The results
results showshow
that that
an
an increase
increase of the
of the W/BW/Bratioratio or H
or the the H2 O/Na
2O/Na 2 O molar
2O molar ratio
ratio led to led to a reduction
a reduction of density.
of density. This
This
was was expected
expected as anasincrease
an increase of water
of water content
content wouldwould result
result in more
in more pores,
pores, which
which leads
leads to
to reduction
reduction ofof density.AsAs
density. shownininTable
shown Table9 9and
andFigure
Figure12,
12,the
thedensities
densitiesofofmixtures
mixturesC1,
C1,C2C2
and C3 measured at 28 days decreased by 2.83%, 6.8% and 11.65%, respectively, compared
to mixture B3.

Table 9. Density of one-part alkali-activated pastes from test series C (kg/m3 ).

Mix No. 3 Days 7 Days 14 Days 28 Days


B3 1921.33 1910.67 1918.67 1932
C1 1897.33 1883.47 1878.13 1877.33
C2 1812 1813.33 1814.93 1800.8
C3 1727.73 1717.33 1697.87 1706.93

3.3.3. Compressive Strength


Table 10 summarises the compressive strength results of this series. Similar to dry
density, the obtained results showed that the compressive strength decreased with the
increase of the W/B ratio or the H2 O/Na2 O molar ratio, as clearly shown in Figure 13.
The trends consistently agreed throughout all ages of curing in relation to increased water
content. In comparison with mixture B3, the compressive strength at 28 days of mixtures
C1, C2 and C3 was found to reduce by 6%, 19.6% and 35.4%, respectively.
Table 9. Density of one-part alkali-activated pastes from test series C (kg/m3).

Mix No. 3 Days 7 Days 14 Days 28 Days


B3 1921.33 1910.67 1918.67 1932
C1 1897.33 1883.47 1878.13 1877.33
Materials 2022, 15, 1612 C2 1812 1813.33 1814.93 1800.8 18 of 22
C3 1727.73 1717.33 1697.87 1706.93

Figure12. Densityofofone-part
12.Density one-partalkali-activated
alkali-activatedpastes
pastesfrom
fromtest
testseries
seriesCC(kg/m
(kg/m 3 ), at the 3, 7, 14 and
Figure 3), at the 3, 7, 14 and
2828 days
days ofof curing
curing periods.
periods.

Table 10. Compressive strength of one-part alkali-activated pastes from test series C (MPa).
3.3.3. Compressive Strength
Table 10 summarises
Compressive the compressive strength resultsStrength
Strength (MPa) of this Gain
series. Similar to dry
Ratio
Mix No. density, the obtained results showed that the compressive strength decreased fwith the
3 Days 7 Days 14 Days 28 Days f3 /f28 f7 /f28 14 /f28
increase of the W/B ratio or the H2O/Na2O molar ratio, as clearly shown in Figure 13. The
B3 34.79 41.60 56.31 59.89 0.58 0.69 0.94
trends consistently agreed throughout all ages of curing in relation to increased water
C1 25.92 39.08 45.36 56.29 0.46 0.69 0.81
C2 23.21 content. In comparison
34.92 with mixture48.17
39.81 B3, the compressive0.48 strength 0.72 at 28 days of mixtures
0.83
C3 19.31 C1, C2 and 23 C3 was found 30.67to reduce by 6%, 19.6% and
38.71 0.5035.4%, respectively.
0.59 0.79
f3 : Compressive strength at 3 days, f7 : compressive strength at 7 days, f14 : compressive strength at 14 10.
The strength gain ratios in this test series are calculated and summarised in Table days,
Based on the observation,
f28 : compressive strength at 28 there
days. was a noticeable reduction in the strength gain ratios with
high W/B ratios. This could especially be witnessed between mixtures B3 (W/B = 0.40) and
C3 (W/B The= strength gain of
0.55) at ages ratios in this
7 and test series
14 days. Again, arethis
calculated and summarised
may probably be attributedin Table
to the10.
Based on the observation, there was a noticeable reduction in the strength gain ratios with
increase in the distribution and size of the pores with the increase in the W/B ratio.
high W/B ratios. This could especially be witnessed between mixtures B3 (W/B = 0.40)
and 10.
Table C3Compressive
(W/B = 0.55) at agesofof
strength 7 and 14
one-part days. Again,
alkali-activated this may
pastes probably
from test series Cbe(MPa).
attributed to
the increase in the distribution and size of the pores with the increase in the W/B ratio.
Compressive Strength (MPa) Strength Gain Ratio
Mix No. 3.3.4. Discussion of Results from Test Series C
3 Days 7 Days 14 Days 28 Days f3/f28 f7/f28 f14/f28
B3 34.79 The effects of 56.31
41.60 water/binder or59.89 H2 O/Na2 O molar 0.58 ratios on the0.69fresh and mechanical
0.94
properties of one-part alkali-activated binders was investigated in this series. It is well-
recognised that water content plays an important role that greatly affects the flowability and
strength. With the increase of the water content, the flowability of the mixtures increased,
whereas the density and compressive strength decreased.
The relationship of flowability (in terms of average flow spread diameters) and com-
pressive strength at 28 days with respect to water/binder ratios is plotted in Figure 14. It
is evident that the results showed excellent correlations of flowability and compressive
strength with water/binder ratios. The flowability performance is directly proportional to
the water/binder ratio. On the other hand, compressive strength is inversely proportional
to the water/binder ratio. The calculated correlation coefficients (R2) for flowability and
compressive strength were 0.9987 and 0.9981, respectively.
C1 25.92 39.08 45.36 56.29 0.46 0.69 0.81
C2 23.21 34.92 39.81 48.17 0.48 0.72 0.83
C3 19.31 23 30.67 38.71 0.50 0.59 0.79
Materials 2022, 15, 1612
f3: Compressive strength at 3 days, f7: compressive strength at 7 days, f14: compressive strength19atof 22
14 days, f28: compressive strength at 28 days.

Materials 2022, 15, x FOR PEER REVIEW 21 of 23


Figure13.
Figure Compressivestrength
13.Compressive strengthatat3,3,7,7,1414and
and2828days
daysofofone-part
one-partalkali-activated
alkali-activatedpastes
pastesfrom
fromtest
test
seriesCC(N/mm
(N/mm 2
2). ).
series

3.3.4. Discussion of Results from Test Series C


The effects of water/binder or H2O/Na2O molar ratios on the fresh and mechanical
properties of one-part alkali-activated binders was investigated in this series. It is well-
recognised that water content plays an important role that greatly affects the flowability
and strength. With the increase of the water content, the flowability of the mixtures in-
creased, whereas the density and compressive strength decreased.
The relationship of flowability (in terms of average flow spread diameters) and com-
pressive strength at 28 days with respect to water/binder ratios is plotted in Figure 14. It
is evident that the results showed excellent correlations of flowability and compressive
strength with water/binder ratios. The flowability performance is directly proportional to
the water/binder ratio. On the other hand, compressive strength is inversely proportional
to the water/binder ratio. The calculated correlation coefficients (R2) for flowability and
compressive strength were 0.9987 and 0.9981, respectively.
As explained by Hajimohammadi et al. [18], water content greatly influenced the dis-
solution of SiO2 from the precursor material and alkali activator. An increase of water
content would reduce the alkalinity of the system and lead to lower dissolution of SiO2. It
is expected that higher alkalinity affects the dissolution of SiO2 more than it affects the
dissolution of Al2O3 from source materials. Therefore, more participation of SiO2 in stages
of gel formation could be observed from mixtures with lower water content. Based on this
interpretation, appropriate low water/binder ratios should be considered. So far, our test
results suggest that the water/binder ratios should not exceed 0.50 to yield satisfactory
performance in flowability
Figure 14. Relationship and compressive
of average strength.and compressive strength at 28 days with
flow spread diameters
Figure 14. Relationship of average flow spread diameters and compressive strength at 28 days with
water to binder ratios (W/B ratio).
water to binder ratios (W/B ratio).
As explained by Hajimohammadi et al. [18], water content greatly influenced the
4.dissolution
Conclusions of SiO2 from the precursor material and alkali activator. An increase of water
content wouldofreduce
The effects GGBS/binder, activator/binder
the alkalinity andand
of the system water/binder ratios
lead to lower on the fresh
dissolution of and
SiO2 .
mechanical properties of ambient-cured one-part alkali-activated pastes have been inves-
It is expected that higher alkalinity affects the dissolution of SiO2 more than it affects the
tigated. Combined HCFA and GGBS were used as the precursor materials in this study,
with sodium metasilicate anhydrous as the solid alkali activator. The following conclu-
sions can be derived from this study:
1. There was a definite limit on the SiO2 content in contributing to compressive strength.
Materials 2022, 15, 1612 20 of 22

dissolution of Al2 O3 from source materials. Therefore, more participation of SiO2 in stages
of gel formation could be observed from mixtures with lower water content. Based on this
interpretation, appropriate low water/binder ratios should be considered. So far, our test
results suggest that the water/binder ratios should not exceed 0.50 to yield satisfactory
performance in flowability and compressive strength.

4. Conclusions
The effects of GGBS/binder, activator/binder and water/binder ratios on the fresh
and mechanical properties of ambient-cured one-part alkali-activated pastes have been
investigated. Combined HCFA and GGBS were used as the precursor materials in this
study, with sodium metasilicate anhydrous as the solid alkali activator. The following
conclusions can be derived from this study:
1. There was a definite limit on the SiO2 content in contributing to compressive strength.
Based on our test results, the maximum compressive strength was achieved at the
SiO2 /Al2 O3 molar ratio somewhere between 3.20 and 3.30. Once it passed the limit,
the compressive strength decreased.
2. The addition of GGBS with HCFA improved the reactivity of the precursor materials.
It enhanced the flowability and compressive strength development in the ambient-
cured condition. The optimum GGBS/binder ratio was found at 0.50. It was deduced
based on flowability and compressive strength test results from mixture A6, where it
achieved a compressive strength of 80 MPa at 28 days with a flow spread diameter of
214.75 mm (114.8% flow).
3. The optimum activator/binder ratio was found in the range between 0.08 and 0.12,
which satisfied both the flowability performance (>100% flow) and the attainment of
compressive strength up to 80 MPa. There was a limit on the effective amounts of
solid activators in the contribution to the alkali-activation reaction process, which was
greatly influenced by the SiO2 content or the SiO2 /Al2 O3 molar ratio.
4. Increased water content would increase the flowability, but it reduced the compressive
strength and density. Low water/binder ratios should be considered in all cases as
this greatly affects the dissolution and participation of SiO2 in stages of gel formation.
It is recommended that the water/binder ratio should not exceed 0.50.
This paper has summarised findings from a preliminary investigation on the fresh
and mechanical properties of one-part alkali-activated binder pastes. The obtained results
were shown to be promising. However, the microstructure and morphology analysis
was limited and may require further investigation. Future research will focus on the
development of tensile strain-hardening characteristics for alkali-activated composites.
The effects of different types of aluminosilicate materials and commercially available solid
alkali activators on the tensile strain-hardening behaviour of ambient-cured one-part alkali-
activated composites will be thoroughly studied in future work.

Author Contributions: Conceptualisation, W.T.; methodology, W.T.; formal analysis, W.T.; investiga-
tion, W.T. and J.H.L.; writing—original draft preparation, W.T.; writing—review and editing, L.B.J.,
K.S., J.H.L. and E.N.; visualisation, W.T.; supervision, W.T. and L.B.J.; project administration, W.T.;
funding acquisition, W.T. and K.S. All authors have read and agreed to the published version of
the manuscript.
Funding: This research was funded by the Ministry of Education (MOE) Malaysia through the
Fundamental Research Grant Scheme (FRGS), grant number: FRGS/1/2018/TK01/HWUM/02/3,
and in part by the 2020 MAEDA Foundation Research Grant through with Hokkaido University,
Sapporo, Japan.
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: Not applicable.
Materials 2022, 15, 1612 21 of 22

Acknowledgments: The authors would like to thank former research Ng Wei Yean for her contribu-
tion to the laboratory work.
Conflicts of Interest: The authors declare no conflict of interest. The funders had no role in the design
of the study; in the collection, analyses, or interpretation of data; in the writing of the manuscript, or
in the decision to publish the results.

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