buildings
Article
Development of Ultra-High-Performance Silica Fume-Based
Mortar Incorporating Graphene Nanoplatelets for
3-Dimensional Concrete Printing Application
Husam A. Salah 1 , Azrul A. Mutalib 1, *, A. B. M. A. Kaish 1, * , Agusril Syamsir 2
Citation: Salah, H.A.; Mutalib, A.A.;
Kaish, A.B.M.A.; Syamsir, A.; Algaifi,
H.A. Development of
Ultra-High-Performance Silica
Fume-Based Mortar Incorporating
Graphene Nanoplatelets for
3-Dimensional Concrete Printing
Application. Buildings 2023, 13, 1949.
https://doi.org/10.3390/
buildings13081949
Academic Editor: Ahmed Senouci
Received: 23 May 2023
Revised: 29 June 2023
Accepted: 10 July 2023
Published: 31 July 2023
Copyright: © 2023 by the authors.
Licensee MDPI, Basel, Switzerland.
This article is an open access article
distributed under the terms and
conditions of the Creative Commons
Attribution (CC BY) license (https://
creativecommons.org/licenses/by/
4.0/).
Buildings 2023, 13, 1949. https://doi.org/10.3390/buildings13081949
and Hassan Amer Algaifi 2
1 Department of Civil Engineering, Faculty of Engineering and Build Environment, Universiti Kebangsaan
Malaysia (UKM), Bangi 43600, Malaysia; p97967@siswa.ukm.edu.my
2 Institute of Energy Infrastructure (IEI), Universiti Tenaga Nasional, Jalan IKRAM-UNITEN,
Kajang 43000, Malaysia; agusril@uniten.edu.my (A.S.); enghas78@gmail.com (H.A.A.)
* Correspondence: azrulaam@ukm.edu.my (A.A.M.); amrul.kaish@ukm.edu.my (A.B.M.A.K.)
Abstract: Although the use of 3D printing in civil engineering has grown in popularity, one of the
primary challenges associated with it is the absence of steel bars inside the printed mortar. As a
result, developing 3D printing mortar with ultra-high compressive, flexural, and tensile strengths is
critical. In the present study, an ultra-high-performance mortar incorporating silica fume (SF) and
graphene nanoplatelets (GNPs) was developed for 3D printing application. The concrete mixture
added SF to the concrete mixture in the range between 0% and 20%, while GNPs were added
as a partial replacement by cement weight from 0.5% to 2%. The flowability and the machinal
properties of the proposed mortar, including compressive (CS), tensile (TS), and flexural strength
(FS), were investigated and assessed. Microstructure analysis involving FESEM and EDX was also
investigated and evaluated, while response surface methodology (RSM) was considered to predict
and optimize the optimum value of GNPs and SF. Workability results show that the flowability is
reduced when the amount of graphene increases. Based on the predicted and experimental results,
ultra-high-strength mortar can be developed by including 1.5% of GNPs and 20% of SF, in which
the CS jumped from 70.7 MPa to 133.3 MPa at the age of 28 days. The FS and TS were 20.66 MPa
and 14.67 MPa compared to the control mix (9.75 MPa and 6.36 MPa), respectively. This favorable
outcome was credited to the pozzolanic activity of SF and the effectiveness of GNPs in compacting
the pores and bridging the cracks at the nanoscale level, which were verified by FE-SEM and EDX.
In addition, the developed quadratic equations proved their accuracy in predicting and optimizing
the mechanical properties with low error (less than 0.09) and high correlation (R2 > 0.97). It can be
concluded that the current work is an important step forward in developing a 3D printing mortar.
The lack of reinforcement in the printed mortar structure has been a considerable difficulty, and the
SF and GNPs have increased the compressive, flexural, and tensile strengths of the mortar. Thus,
these improvements will encourage the industry to utilize sustainable materials to produce more
affordable housing.
Keywords: ultra-high-performance mortar; graphene; 3D printing mortar; mechanical properties;
optimization modeling
1. Introduction
Traditional concrete construction often faces challenges such as high costs, decreased
safety, and increased time and effort [1–3]. To address these issues, the civil engineering
community has turned its attention towards adopting a new construction technique known
as 3D concrete printing [4–6]. This unique technique, paired with precise structural opti-
mization [7,8], holds the key to massive benefits by substantially decreasing the wastage of
building materials. Furthermore, the removal of formwork not only reduces both money
and time but also opens up a world of possibilities for projects of all sizes, from small-scale
https://www.mdpi.com/journal/buildings
Buildings 2023, 13, 1949 2 of 20

to large-scale constructions. It is important to embrace the sustainability perspective, using

a logical approach when selecting the most efficient 3D concrete printing technology. A thor-
ough study needs to take place to determine the regions where this advanced technology
offers the most potential and benefits compared to traditional building methods. Despite
the available research falling short of fully investigating the sustainability implications of
3D concrete printing, the limited studies provide solid evidence of its enormous potential
when it requires complex designs for conventional construction [9].
Three-dimensional concrete printing is one of the latest technologies that has shifted
from laboratory experiments to developing different types of projects such as multi-story
units, gardens, bridges, etc. [10]. All of these developments require Portland cement PC,
and the high demand for utilizing PC is excessively predicted to be 4–8 Gt/yr by 2100 from
the perspective of shared socioeconomic pathways [11,12]. PC production causes high
CO2 emissions, accounting for 7–10% of global anthropogenic CO2 emissions and 2–3%
of energy consumption, and it is projected that cement production will increase by 50%
by 2050 [13–15]. To reduce CO2 emissions, scientists found four methods [16–18], which
currently follow the standard proposed by the World Business Council for Sustainable
Development (WBCSD) and International Energy Agency (IEA) in the cement industry [19].
This technology offers numerous benefits to the construction industry, including
cost-effectiveness, reduced effort, and improved safety compared to traditional concrete
construction [20,21]. However, a major challenge in 3D printing concrete is the absence
of steel reinforcement during the printing process. This has prompted researchers to
focus on designing 3D-printed concrete with ultra-high mechanical properties, ensuring
high compressive, tensile, and flexural strength. The research and development of 3D
concrete printing have progressed through sequential steps. In the first step, researchers
focused on developing 3D-printed concrete having low compressive strength. Subsequently,
efforts were made to enhance the 3D printing concrete mix to achieve high-quality results,
including high compressive, flexural, and tensile strength, as there is no steel reinforcement.
For example, Wolfs, Bos [22] started to develop 3D concrete printing with a compres-
sive and flexural strength of 30 MPa and 5 MPa, respectively. Cement I 52.5, fine aggregate
(less than 1 mm), polypropylene (PP) fibers, rheology modifiers, and additives were used
to achieve the aim of their study. The water-to-cement ratio was kept constant (0.495).
Similarly, Ding, Xiao [23] developed 3D printing green mortar with a low compressive and
flexural strength of 19.31 MPa and 2.15 MPa, respectively. After that, Lee, Kim [4], in turn,
tried to use pozzolanic additives such as silica fume (SF) and fly ash (FA) as partial replace-
ments for cement (OPC) to enhance the strength of 3D printing concrete. The outcome
exposed that the compressive strength of the reference mixture using mold-casting samples
was 66 MPa after 28 days, while it decreased to 22.54 MPa using printed cubical samples.
Similarly, Narelle, Hempel [24] developed 3D printing concrete involving 55% cement I
52.5, 15% silica fume, 30% fly ash, and a water-to-binder ratio of 0.42. It was found that the
compressive strength of 3D printing mortar incorporating pozzolanic additives increased
by 30% compared to that of the control mixture (71.8 MPa). The strength enhancement was
linked to the pore refinement at the micro-scale level in the presence of pozzolanic additives
inside the cement-based matrix. Arunothayan et al. [25], in the same context, used fiber to
improve the mechanical properties of 3D printing concrete, and it is in good agreement
with [26]. To further enhance the strength gained at the nanoscale level, nanomaterials were
also taken into account in 3D printing mortar. For example, Panda, Lim [27] suggested
adding 0.5% of nano clay in a 3D-printable mortar mixture incorporating high fly ash
content up to 60%, 2% silica fume, and 38% ordinary Portland cement. The water-to-cement
ratio was 0.3, and the sand-to-binder ratio was 0.83. Sikora, Chung [28] used nano-silica in
the range between 2% and 6% in printable cement mortar containing OPC, limestone filler,
and fine aggregate.
In addition, other researchers shifted their attention to utilizing nanocarbon materials,
namely graphene, as cement replacements [29]. However, its incorporation in 3D printing
concrete is still in its infancy, and very little research has been conducted on the impact of
Buildings 2023, 13, 1949 3 of 20

graphene on ultra-high-strength 3D printing mortar. Indeed, graphene is regarded as one

of the most robust materials in the globe, as the tensile strength of graphene reaches up to
130 GPa, and its Young’s modulus is recorded up to 1 TPa [30]. According to K. Cui and
J. Chang [31], the research found that adding MLG can significantly enhance compressive
strength and flexural strength on the 28th day by 22.2% and 43.3%, respectively. Shanmuga
Priya, Mehra [32] also concluded that the GO serves as a beneficial reinforcement material
inside the concrete matrix. Although GO has benefits when mixed with cement, an excess
of oxygen functional groups in GO can cause problems in the cement-based matrix. This is
because the positive charge of Ca2+ , Na+ , and K+ in the cement matrix and the negative
charge of GO can cause agglomeration due to van der Waals forces, resulting in the
formation of a weak zone within the cement-based matrix [33]. In another study conducted
by Kei cui et al. [19], which studied the impact of CNTs on the UHPC with two different
dosages (0.09%, 0.15%), the results show great strength of the concrete, which contain CNTs
with a large aspect ratio of 250–1500. Therefore, instead of GO, researchers have focused on
using reduced graphene oxide [34,35] and graphene powder (graphene nanoplatelets) [36]
to improve cementitious materials. For example, Jiang, Sevim [37] noticed that the highest
compressive strength of concrete was 17% when the GNPs were incorporated into the
concrete mixture at a dosage of 0.025% by cement weight. The result was in line with
Wang, Jiang [38], who found that the flexural strength of a cement composite increased
by approximately 20% (average) when the content of GNPs was just 0.05%. In contrast,
Du, Gao [39] stated that adding a high level of graphene nanoplatelets (up to 1.5%) can
significantly densify concrete pores. This is in good agreement with Du and Dai Pang [40],
who demonstrated that incorporating 2.5% of graphene nanoplatelets in cement mortar can
significantly increase the refinement of the mortar microstructure compared to the control
mix without GNPs. Jiang, Sherif [41] also reported that the graphene nanoplatelets are
able to bridge the inevitable cracks inside the concrete and enhance the tensile strength
by 8–48%.
Based on the overmentioned, the development of ultra-high mechanical properties of
3D printing mortar is in urgent demand to promote the use of 3D printing technology in the
construction field. In addition, incorporating graphene in a cement-based matrix not only
enhances the compressive strength by filling the concrete pores at the nanoscale level but
also acts as reinforcement by bridging the cracks. Therefore, to fill the gap in the present
literature, ultra-high-performance 3D printing mortar incorporating graphene nanoplatelets
and silica fumes has been developed. The dosage of GNPs varied from 0% to 1.5% at
intervals of 0.5%, while silica fume content ranged between 0% and 20% of the cement
replacement. The proposed mortar’s mechanical properties, such as compressive, flexural,
and tensile strength, are investigated and analyzed via both experimental and mathematical
modeling. Response surface methodology (RSM) is also used as a mathematical and
statistical tool to predict and find the optimum content of graphene nanoplatelets and
silica fume, as well as to derive a quadratic equation for further prediction in the future.
Microstructural tests such as field emission scanning electron microscopy (FE-SEM) are also
adopted to evaluate the behavior of the proposed mortar at the micro- and nanoscale levels.

2. Experimental and Theoretical Program Set-Up

2.1. Materials Preparation
The proposed high-strength mortar comprises cement, silica fume, graphene, natural
sand, superplasticizer, and water. Figure 1 depicts the graphene morphology purchased
from GrapheneCA Inc. (NYC, New York, NY, USA). It can be seen that graphene is com-
posed of multiple layers, which are well known as graphene nanoplatelets. A rapidly
hardened and early-strength cement (cement I 52.5 R) was used as it was recommended
for ultra-high-strength 3D printing mortar. Silica fume was, in turn, used as a mineral ad-
mixture, which was supplied by Elkem company. Table 1 shows the chemical composition
of both silica fume and cement as determined by X-ray fluorescence (XRF) spectroscopy.
It can be seen that the silica fume is rich in SiO2 (greater than 93%), which is in line with
 from GrapheneCA Inc. (NYC, New York, NY, USA). It can be seen that graphene is com-
posed of multiple layers, which are well known as graphene nanoplatelets. A rapidly
hardened and early-strength cement (cement I 52.5 R) was used as it was recommended
for ultra-high-strength 3D printing mortar. Silica fume was, in turn, used as a mineral
admixture, which was supplied by Elkem company. Table 1 shows the chemical compo-
Buildings 2023, 13, 1949 4 of 20
sition of both silica fume and cement as determined by X-ray fluorescence (XRF) spectros-
copy. It can be seen that the silica fume is rich in SiO2 (greater than 93%), which is in line
with previous studies [7].studies
previous A laser[7].
diffraction particle size
A laser diffraction analyzer
particle was also
size analyzer used
was alsoto deter-
used to determine
mine and analyzeand theanalyze
particlethesize distribution of silica fume and cement. Based on Figure
particle size distribution of silica fume and cement. Based on Figure 2, the
2, the size of silicasize
fume particles
of silica fumewas smaller
particles wasthan the than
smaller cement
the particles, with median
cement particles, par- particle
with median
ticle sizes of 12.74sizes
µ mofand 13.505
12.74 µ m,13.505
µm and respectively. This factThis
µm, respectively. confirmed the advantage
fact confirmed of
the advantage of the
undersized silica fume to fully react with calcium hydroxide
the undersized silica fume to fully react with calcium hydroxide ions and ultimately pro- ions and ultimately provide
vide more gel productmore gelin product
the mortarin the mortar matrix.
matrix.

Figure 1. GrapheneFigure 1. Graphene

morphology morphology
(FESEM image).(FESEM image).

Table 1. Chemical composition of silica fume and cement based on XRF analysis.
Table 1. Chemical composition of silica fume and cement based on XRF analysis.
Mass Percentage %
Elements Mass Percentage %
Elements Cement SF
Cement SF
CaO 69.79 0.26
CaO 69.79 0.26
SiO2 15.91 96.1
SiO2 Al2 O3 15.91 3.44 96.1 0.75
Al2O3 SO3 3.44 4.33 0.75 0.18
MgO 0.99 0.4
SO3 Fe2 O3
4.33 3.94
0.18 0.11
Buildings 2023, 13, x FOR PEER MgO
REVIEW Na2 O 0.99 0.0771 0.4 0.26 5 of 21
Fe2O3 K2 O 3.94 0.92 0.11 0.83
Na2O 0.0771 0.26
K2O 0.92 0.83 100

90

80

70
Undersize (%)

60

50

40

30

20

10

0
1000 100 10 1 0.1 0.01
Particle diameter [nm] Cement Silica Fume

Figure 2. Particle size distribution for both

Figure 2. both silica
silica fume
fume and
and cement.
cement.

As the fine aggregate, local natural sand was also used. The natural sand’s particle
size distribution and fineness modulus were determined using a sieve analysis test in ac-
cordance with ASTM C33-18 [42]. It was found that the sand met the grading requirements
 1000 100 10 1 0.1 0.01
Particle diameter [nm] Cement Silica Fume

Figure 2. Particle size distribution for both silica fume and cement.
Buildings 2023, 13, 1949 5 of 20

As the fine aggregate, local natural sand was also used. The natural sand’s par
sizeAs distribution and fineness modulus were determined using a sieve analysis test i
the fine aggregate, local natural sand was also used. The natural sand’s particle size
cordance with
distribution ASTMmodulus
and fineness C33-18 [42].
were It was found
determined that
using the sand
a sieve met
analysis the
test in grading requirem
accordance
in which
with ASTMthe passing
C33-18 [42]. Iton allfound
was sieves (4.75
that the mm–0.075
sand met themm) was
grading located between
requirements in whichthe high
lowpassing
the limits onof all
thesieves
specification, as shown
(4.75 mm–0.075 mm) inwasFigure
located3.between
In addition,
the hightheand
fineness
low modu
limits of the specification, as shown in Figure 3. In addition, the fineness
water absorption, and specific gravity of sand were 2.3, 2.6, and 1.2%, respectively modulus, water
absorption, and specific gravity of sand were 2.3, 2.6, and 1.2%, respectively. For workability,
workability, it is interesting to note that three different superplasticizers were used
it is interesting to note that three different superplasticizers were used and tested. Based on
tested.
the optimumBased on the
results optimum
that gave a high results that gave
slump without a high slump
any segregation, without any
Superplasticizer RPFsegrega
Superplasticizer
RAPIDCAST RPFwas
W, which RAPIDCAST
purchased fromW, Real
which was
Point Sdnpurchased from
Bhd, was taken Real
into Point Sdn
account
was
for ourtaken
studyinto
at a account forof
dosage level our
1%study at a weight.
by cement dosage level of 1% by cement weight.

Figure3.3.The
Figure The grading
grading of natural
of natural sand sand according
according toC33.
to ASTM ASTM C33.

2.2. Mix Proportions

2.2. Mix Proportions
The research has a set of three scenarios that were methodically designed to com-
The research
prehensively examine has
theabehavior
set of three scenarios that were methodically
of ultra-high-performance mortar injecteddesigned
with the to com
hensively
potent examine
mixture theof
consisting behavior of and
silica fume ultra-high-performance mortar
graphene. These situations injected
established with the po
fifteen
mixtureexperiments,
separate consisting of silica fume and detailed
as comprehensively graphene. These
in Table situations
2. In this initialestablished
scenario, thefifteen s
UHP mortar mixture as
rate experiments, contained a range of GNPs
comprehensively concentrations
detailed in Table varying from
2. In this 0% toscenario,
initial 2% of the U
the cement weight, with consistency at every 0.5% increment. It is important to note that
silica fume was purposefully avoided, adding an element of tension to the research process.
The mortar, equipped with unparalleled strength provided by graphene (0% to 2%), was
further reinforced in the second and third scenarios by incorporating 10% and 20% silica
fume. These remarkable combinations pushed boundaries for technological advancement
to unprecedented heights. The cement-to-fine-aggregate ratio was set as the optimum at 1:1
by mass in all of the developed mixtures, while the water-to-cement ratio of 0.26 ensured
excellent stability in the mixture. Notably, adding silica fume at concentrations of 0.1 and
0.2 provided a distinct presence for the mortar. A minimum of 1% superplasticizer dosage
was effectively incorporated to ensure continued consistency and facilitate subsequent
comparisons and assessments, maintaining the water content at a constant level across
every mixture. The 3D printing mortar workability has been carefully gauged, with this
experiment flow table illustrated in Figure 4, in strict conformity to the revered standards
set out by ASTM C230 [43].
 this experiment flow table illustrated in Figure 4, in strict conformity to the revered stand-
ards set out by ASTM C230 [43].

Table 2. Mix proportions of the proposed mortar.

Buildings 2023, 13, 1949 6 of 20
Cement Water Fine Aggregate Superplasticizer 1%
Mix Code NO. GNPs (%) SF (%)
(Kg/m3) (Kg/m3) (Kg/m3) (Kg/m3)
M1 0 Mix proportions
Table 2. 0 of916 229mortar. 916
the proposed 9.16
M2 0.5 0 916 229 916 9.16
Cement Water Fine Aggregate Superplasticizer 1%
Mix Code NO. GNPs (%)
M3 1SF (%) 0 (kg/m 9163 ) 229 (kg/m3 ) 916 (kg/m3 ) 9.16 (kg/m3 )
M1 M4 0 1.5 0 0 916
916 229 229 916 916 9.16 9.16
M2 M5 0.5 2 0 0 916
916 229 229 916 916 9.16 9.16
M3 1 0 916 229 916 9.16
M4
M6 1.5 0 0 10 916
916
229 229 916 916
9.16 9.16
M5 M7 2 0.5 0 10 916
916 229 229 916 916 9.16 9.16
M6 M8 0 1 10 10 916
916 229 229 916 916 9.16 9.16
M7 0.5 10 916 229 916 9.16
M8 M9 1 1.5 10 10 916
916 229 229 916 916 9.16 9.16
M9 M101.5 2 10 10 916
916 229 229 916 916 9.16 9.16
M10 2 10 916 229 916 9.16
M11 M11 0 0 20 20 916
916 229 229 916 916 9.16 9.16
M12 M120.5 0.5 20 20 916
916 229 229 916 916 9.16 9.16
M13 1 20 916 229 916
M13 1 20 916 229 916 9.16 9.16
M14 1.5 20 916 229 916 9.16
M15 M14 2 1.5 20 20 916
916 229 229 916 916 9.16 9.16
M15 2 20 916 229 916 9.16

Figure 4. Workability
Figureof4.graphene-based mortar using
Workability of graphene-based flow using
mortar table.flow table.

2.3. Compressive Strength Test

2.3. Compressive Strength Test
The compressive strength of the proposed mortar was determined at 3, 7, 14, and
The compressive
28 days.strength
Based on of
thethe proposed
guidelines mortar
of ASTM was determined
C109-109M at 3, 7, 14,
[44], the procedure wasand 28 out
carried
days. Based on using
the guidelines of ASTM C109-109M [44], the procedure was carried out
a cubic sample measuring 50 × 50 × 50 mm with three replicates. The cubic sample
was placed
using a cubic sample on the compression
measuring machine
50 × 50 × 50 and three
mm with exposed to a constant
replicates. Theload ratesample
cubic of 1000 N/s
until failure occurred, as stipulated by the standard. The cubic compressive strength (CS)
in MPa was then calculated using Equation (1), which takes into account the measured
failure load as well as the sample area denoted by A in mm2 and the total applied load
denoted by P in N.
P
CS = (1)
A

2.4. Flexural Strength Test

ASTM C348-21 [45] was also considered to determine the mortar’s flexural strength
using center point loading. Cured prism beams with dimensions of 40 × 40 × 160 mm were
used to conduct the test at the ages of 3, 7, 14, and 28 days. The spacing between the two
support rollers was set to 120 mm, while the loading rate was maintained at 50 N/s. The
Buildings 2023, 13, 1949 7 of 20

flexural strength (FS) in MPa was calculated using Equation (2). It is worth mentioning that
three replicate specimens were employed, and the mean value was taken for evaluation.

FS = 0.0028 P (2)

2.5. Tensile Strength Tests

ASTM C496/C496M [46] was taken into account to obtain the splitting tensile strength
of the proposed mortar. A cylinder sample with a dimension of 50 × 100 mm was consid-
ered to obtain the 3rd-day, 7th-day, 14th-day, and 28th-day tensile strength. The sample was
subjected to a constant loading rate of 1.0 MPa/min using the universal testing machine.
Then, the splitting strength (TS) in MPa was determined using Equation (3), where L is the
cylinder length and D is the cylinder diameter. It is worth noting that triplicate specimens
were used, and the average was considered for evaluation.

2P
TS = (3)
πDL

2.6. Microstructure Test

The field emission scanning electron microscope (FE-SEM) and energy-dispersive
X-ray (EDX) were employed to observe the microstructure of the mortar samples and
identify the chemical components in the mixture. At the 28-day mark, the cubic sample
was compressed, and a small specimen of less than 10 mm was extracted from it. Before
being analyzed with the SEM, this specimen was dried in an oven at 60 degrees Celsius to
remove any moisture content. The specimens were coated with gold before scanning to
improve image resolution. The sample was scanned using ZEISS MERLIN Field Emission
Scanning Electron Microscopes equipped with an energy-dispersive X-ray analyzer.

2.7. Optimization Modeling Using RSM Model

In recent years, many published academic papers recognized the response surface
methodology (RSM) as an effective optimization tool. This is because the RSM model uses
a combination of mathematical and statistical analysis to precisely assess the significant
relationship between dependent and independent variables [47,48]. This study used RSM
to predict and optimize the compressive strength (CS), flexural strength (FS), and tensile
strength (TS) of the ultra-high-performance mortar incorporating both silica fume and
graphene. The silica fume, graphene, and curing duration were considered independent
variables, while CS, FS, and TS were the output of the model (dependent variables). Table 3
shows the maximum and minimum values of each independent variable. The present
models were developed using Design Expert 13 software.

Table 3. Min. and max. values of the independent variables.

Independent Variables Unit Code Level (High) Level (Low)

Graphene % X1 2 0.5
Silica Fume % X2 20 0
Curing duration days X3 28 3

As shown in Equation (4), a second-order polynomial equation was used to determine

the computational relationship among the variables. The linear and constant coefficients
were denoted by βi and βo , while quadratic and interactive coefficients were denoted by βij
and βii , respectively. Moreover, the models’ dependability and sensitivity were assessed
using error and correlation statistical parameters involving the scatter index (SI), mean
absolute percentage error (MAPE), and the coefficient of determination (R2 ), as shown in
Buildings 2023, 13, 1949 8 of 20

Equations (4)–(7), where Ya and Yp represent the actual and predicted strength, while n
and Ya are the number of variables and average actual strength, respectively.

k k k
Y = β o + ∑ β i Xi + ∑ β ii Xi2 + ∑ β ij Xij (4)
i =1 i =1 i =1
q
2
1
n ∑in=1 Ya − Yp
SI = (5)
Ya
n Ya − Yp
1
MAPE =
n ∑ Ya
(6)
i =1

2
2 ∑in=1 Yp − Ya
R =
2 (7)
∑in=1 Ya − Ya

3. Results and Discussion

3.1. Mechanical Properties Analysis
This section of the research will illustrate the results and discuss them accordingly.
The flow table was observed after each concrete mixture in order to follow the flow table
test results required for a 3D concrete printer. Figure 5 shows all of the results found and
recorded to understand the potential and the effect of using GNPs in 3D concrete printers.
The results showed a significant decrease in the diameter of the flow table test when the
GNP content increased. According to Tay et al. [49], the study shows that mixtures with a
slump of 4 to 8 mm and a slump flow value of 150 to 190 mm have good buildability as
well as produce a smooth layer. As a result, the range of printing materials can be identified
through their slump together with slump flow values. The slump values start to decrease
with an increasing amount of GNPs and SF in the concrete mixture, and this is due to
the nanoparticles that the graphene contains to bond the concrete; thus, the slump
Buildings 2023, 13, x FOR PEER REVIEW 9 ofresults
21
decrease significantly.

Figure 5. Flow table test results.

Figure 5. Flow table test results.
Figure 6 presents the plotted charts of the experimental compressive and flexural
Figure 6 presents the plotted charts of the experimental compressive and flexural
strength obtained from different mortar mixes at interval times (3, 7, 14, and 28 days).
strength obtained from different mortar mixes at interval times (3, 7, 14, and 28 days). Each
Each mix involved a specific amount of silica fume and graphene nanoplatelets in accu-
mix involved a specific amount of silica fume and graphene nanoplatelets in accurately
rately assessing each parameter’s contribution to the mortar strength. For instance, Figure
assessing each parameter’s contribution to the mortar strength. For instance, Figure 6a
6a shows the relationship between compressive strength and five mortar mixtures incor-
porating only graphene, which varied from 0% to 2% with an interval of 0.5%. At the same
time, Figure 6b,c present the compressive strength evolution using another graphene-
based mortar mixture containing 10% and 20% silica fume, respectively. Overall, it can be
inferred that the compressive and flexural strength increased with increased curing dura-
Buildings 2023, 13, x FOR PEER REVIEW 10 of 21

Buildings 2023, 13, 1949 9 of 20

In the same context, flexural strength results tend to have a similar trend of compres-
sive
showsstrength. As shownbetween
the relationship in Figure 6d–f, the flexural
compressive strength strength was
and five enhanced
mortar withincorpo-
mixtures the in-
crease in curing duration for all mortar mixtures. In addition, adding 1.5%
rating only graphene, which varied from 0% to 2% with an interval of 0.5%. At the same GNPs and 20%
SF significantly increased the flexural strength from 9.9 MPa to 20.66 MPa
time, Figure 6b,c present the compressive strength evolution using another graphene-basedafter 28 days,
which
mortarismixture
double containing
the time of10%
the control
and 20% mixture. Thisrespectively.
silica fume, is because the GNPs play
Overall, it canabe
great role
inferred
in bridging the cracks and enhancing flexural strength. This fact is also in good
that the compressive and flexural strength increased with increased curing duration. Fur- agreement
with Tong,approximately
thermore, Fan [52], who 85%
foundof that the flexural
the strength strength of
enhancement ultra-high-performance
was con-
attained within seven days,
crete was improved by more than 50% owing to the presence of both carbon
which can be attributed to the use of cement I 52.5 R in the current research. This kind of nanofibers
and GNPs.
cement is known for its quick setting and high-strength characteristics.

(a)
(b)

(c) (d)

(e) (f)

Figure
Figure 6.6.Experimental strength
Experimental of the
strength proposed
of the mortar
proposed incorporating
mortar 0%, 10%,
incorporating and 20%
0%, 10%, andSF.
20%(a–c)
SF.
compressive strength, (d–f) flexural strength.
(a–c) compressive strength, (d–f) flexural strength.
Buildings 2023, 13, 1949 10 of 20

From another point of view, it can be seen that the control mixture (without graphene
and silica fume) showed the lowest compressive strength, in which its value was 42.4 MPa,
58.9 MPa, 65.7 MPa, and 70.7 MPa at the age of 3, 7, 14, and 28 days. In addition, the
highest compressive strength after 28 days (133.33 MPa) was achieved when the graphene
and silica fume content were 1.5% and 20%, respectively. In other words, the compressive
strength jumped from 70.7 MPa to 133.33 MPa in the presence of GNPs (1.5%) and SF (20%).
This remarkable positive result was attributed to two main reasons. The first reason is the
graphene’s efficiency in filling the pores inside the mortar mixture, minimizing the void
and tiny cracks. In other words, the excellent dispersion of GNPs inside the mortar matrix
would enhance its microstructure and thus increase the compressive strength. This fact is
in line with Du, Gao [39], who found that the optimal addition of graphene was 1.5% for
the pore refinement. Behind this value, there is no further improvement as the graphene
particles face difficulties dispersing inside the mortar matrix.
Meanwhile, the second reason behind the improvement of compressive strength was
the pozzolanic activity of silica fume. This is because SF is a very fine amorphous silica
whose particle size reaches 0.1 µm [49]. In addition, SF is rich in silica (SiO2 ), while the
cement-based mortar is rich with calcium hydroxide Ca(OH)2 produced during cement
hydration [50]. The chemical reaction between (SiO2 ) and Ca(OH)2 leads to the formation
of extra and further calcium silicate hydrate (C-S-H) gels inside the mortar matrix. The
C-S-H is the sole main parameter to densify the mortar microstructure. This is consistent
with previous research in published academic papers. For example, Zhang, Zhang [51]
stated that the size of SF and its high content of amorphous silicon dioxide are the main
reasons behind the high pozzolanic activity compared to other pozzolanic materials.
In the same context, flexural strength results tend to have a similar trend of com-
pressive strength. As shown in Figure 6d–f, the flexural strength was enhanced with the
increase in curing duration for all mortar mixtures. In addition, adding 1.5% GNPs and
20% SF significantly increased the flexural strength from 9.9 MPa to 20.66 MPa after 28
days, which is double the time of the control mixture. This is because the GNPs play a great
role in bridging the cracks and enhancing flexural strength. This fact is also in good agree-
ment with Tong, Fan [52], who found that the flexural strength of ultra-high-performance
concrete was improved by more than 50% owing to the presence of both carbon nanofibers
and GNPs.
Similarly, the tensile strength of the proposed mortar increased with the increasing
age of all mixtures, as shown in Figure 7. For instance, the tensile strength of the proposed
mortar incorporating 1% of GNPs and 10% SF was 6.03 MPa, 8.37 MPa, 9.34 MPa, and 10.05
at the age of 3, 7, 14, and 28 days. It was also found that the highest tensile strength was
obtained when the GNPs and SF were 1.5% and 20%, respectively. The tensile strength
jumped from 6.6 MPa to 14.67 MPa at the age of 28 days, which was attributed to two
reasons, as discussed earlier. This fact is also in line with Jiang, Sherif [41], who found that
including GNPs raised the tensile strength of the cement-based composites up to 48%.
The results achieved previously show the potential of utilizing the concrete mix design
in 3D concrete applications due to the negligence of the steel fibers and the reinforce-
ment steel bar, which cause difficulties in the extrusion process for some types of 3D
concrete printers.
 mortar incorporating 1% of GNPs and 10% SF was 6.03 MPa, 8.37 MPa, 9.34 MPa, and
10.05 at the age of 3, 7, 14, and 28 days. It was also found that the highest tensile strength
was obtained when the GNPs and SF were 1.5% and 20%, respectively. The tensile
strength jumped from 6.6 MPa to 14.67 MPa at the age of 28 days, which was attributed
Buildings 2023, 13, 1949
to two reasons, as discussed earlier. This fact is also in line with Jiang, Sherif [41],11who
of 20
found that including GNPs raised the tensile strength of the cement-based composites up
to 48%.

(a) (b)

(c)

Figure
Figure7.7.Experimental
Experimentaltensile
tensilestrength
strengthof
ofthe
theproposed
proposedmortar;
mortar;(a)
(a)0%
0%SF,
SF, (b)
(b) 10%
10% SF,
SF, (c) 20% SF.

3.2. The
Prediction
resultsUsing the RSM
achieved Model show the potential of utilizing the concrete mix de-
previously
sign inResponse
3D concrete applications
surface due was
methodology to the negligence
also of the steel
used to predict fibers and
and optimize the
the reinforce-
compressive,
tensile,
ment and
steel flexural
bar, whichstrength of ultra-high-performance
cause difficulties mortarfor
in the extrusion process containing
some typesSF of
and3DGNPs.
con-
For prediction
crete printers. purposes, three second-order polynomial equations were developed to
estimate the CS, TS, and FS using three independent variables involving SF, GNPs, and
age, as shown in Equations (8)–(10).

CS = 22.22 + 23.18 × X1 − 0.798 × X2 + 3.96 × X3 + 0.1 × X1 × X2 + 0.024 × X1 × X3

(8)
+0.04 × X2 × X3 − 8.95 × X12 + 0.11 × X22 − 0.09 × X32

TS = 1.21 + 3.32 × X1 + 0.146 × X2 + 0.405 × X3 + 0.001 × X1 × X2 − 0.005 × X1 × X3

(9)
+0.0053 × X2 × X3 − 1.3 × X12 + 0.003 × X22 − 0.009 × X32

FS = 2.85 + 3.23 × X1 + 0.06 × X2 + 0.59 × X3 + 0.02 × X1 × X2 − 7.8E − 17 × X1 × X3

(10)
+0.006 × X2 × X3 − 1.29 × X12 + 0.008 × X22 − 0.014 × X32

The accuracy and reliability of these equations were also evaluated using several
mathematical and statistical parameters. For instance, as shown in Figure 8a,c,e, the
coefficients of determination (R2 ) of CS, TS, and FS were greater than 0.9, confirming
that the correlation between experimental and predicted results is robust. The proposed
equations have the ability to predict mechanical properties with high accuracy. This is in
good agreement with Algaifi, Bakar [53], who stated that when the R2 is more significant
 𝐹𝑆 = 2.85 + 3.23 × 𝑋1 + 0.06 × 𝑋2 + 0.59 × 𝑋3 + 0.02 × 𝑋1 × 𝑋2 − 7.8𝐸 − 17 × 𝑋1 × 𝑋3
(10)
+0.006 × 𝑋2 × 𝑋3 − 1.29 × 𝑋12 + 0.008 × 𝑋22 − 0.014 × 𝑋32
The accuracy and reliability of these equations were also evaluated using several
mathematical and statistical parameters. For instance, as shown in Figure 8a,c,e, the coef-
ficients of determination (R2) of CS, TS, and FS were greater than 0.9, confirming that the
Buildings 2023, 13, 1949 12 of 20
correlation between experimental and predicted results is robust. The proposed equations
have the ability to predict mechanical properties with high accuracy. This is in good agree-
ment with Algaifi, Bakar [53], who stated that when the R2 is more significant than 0.7, the
than 0.7, the
predicted and predicted
experimental and experimental
results results
are relatively are Also,
similar. relatively
Othman,similar.
ChongAlso, Othman,
[54] suc-
cessively
Chong [54]developed
successivelythe RSM model to
developed predict
the RSM themodelmechanical
to predict properties of concrete
the mechanical con-
properties of
taining tire
concrete powder and
containing tireeggshell
powderinandwhich the value
eggshell of R2 was
in which thegreater
value of R20.98.
than wasIn addi- than
greater
tion, the
0.98. statistical the
In addition, errorstatistical
parameters involving
error SI andinvolving
parameters MAPE were SI0.028
and andMAPE0.015, indicat-
were 0.028 and
ing that
0.015, the modelthat
indicating is accurate.
the modelSimilarly, to assess
is accurate. the models’
Similarly, suitability,
to assess the error
the models’ distri- the
suitability,
bution
error (residuals) (residuals)
distribution obtained byobtained
the proposed
by theequations
proposedwas also considered.
equations This is be- This
was also considered.
cause, according to Hammoudi, Moussaceb [55], a high value
is because, according to Hammoudi, Moussaceb [55], a high value of R is not of R2 is not enough
2 to enough
con- to
sider the equation accurate. As shown in Figure 8b,d,f, the residual
consider the equation accurate. As shown in Figure 8b,d,f, the residual errors forerrors for CS, TS, andCS, TS,
FS were regular. In addition, the majority of the residuals are small and close to zero. Such
and FS were regular. In addition, the majority of the residuals are small and close to zero.
a fact indicates that the proposed equations can be regarded as accurate and reliable.
Such a fact indicates that the proposed equations can be regarded as accurate and reliable.

Buildings 2023, 13, x FOR PEER REVIEW 13 of 21

Figure 8. The
Figure The correlation
correlationand
andresidual error
residual distribution
error between
distribution the experimental
between and predicted
the experimental and predicted
results of
results of (a,b)
(a,b) compressive
compressivestrength, (c,d)
strength, tensile
(c,d) strength,
tensile andand
strength, (e,f)(e,f)
flexural strength.
flexural strength.

Meanwhile, the typical probability technique was also used to evaluate the distribu-
tion of the data. Indeed, this technique has a strong reputation in the research community
for evaluating data distribution [56]. As illustrated in Figure 9a–c, the data were distrib-
uted and almost fell on a straight line, indicating that they were almost normally distrib-
uted. This is in line with Algaifi, Mustafa Mohamed [57], who developed a mathematical
Buildings 2023, 13, 1949 13 of 20

Meanwhile, the typical probability technique was also used to evaluate the distribution
of the data. Indeed, this technique has a strong reputation in the research community for
evaluating data distribution [56]. As illustrated in Figure 9a–c, the data were distributed
and almost fell on a straight line, indicating that they were almost normally distributed.
This is in line with Algaifi, Mustafa Mohamed [57], who developed a mathematical model
to predict the mechanical properties of alkali-activated mortar incorporating nano-silica
powder, granulated blast-furnace slag (GBFS), and fly ash (FA). The outcome of their
research demonstrated the feasibility of their RSM model, as the CS, TS, and FS residuals
were normally distributed and presented using a typical probability technique. Similarly,
Buildings 2023, 13, x FOR PEER REVIEW 14 of 2
Salah et al. [58] verified the developed RSM model using a typical probability plot in which
the data were located along a straight line.

Figure 9. Typical Plot of Residuals. (a) compressive strength, (b) tensile strength, and (c) flexural
Figure 9. Typical Plot of Residuals. (a) compressive strength, (b) tensile strength, and (c) flexural strength.
strength.
Using the proposed above equations, a contour plot and three-dimensional response
Using the proposed above equations, a contour plot and three-dimensional respons
surface diagram were also developed to further illustrate the evolution of the compressive,
surface diagram were also developed to further illustrate the evolution of the compres
tensile, and flexural strength of the proposed mortar (output) as shown in Figure 10a–c,
sive, tensile, and flexural strength of the proposed mortar (output) as shown in Figur
respectively. These figures are also essential to establish the relationship between the output
10a–c, respectively. These figures are also essential to establish the relationship between
and independent thevariables
output and (input) as wellvariables
independent as to explain
(input) the impact
as well as toof the independent
explain the impact of the inde
variables on thependent
mortarvariables
strength.onThe dependent variable was depicted
the mortar strength. The dependent variable on thewasvertical
depicted on th
(Z-axis), while vertical
the independent variables were plotted on the horizontal and vertical and ver
(Z-axis), while the independent variables were plotted on the horizontal
(X-axis) axes (Y-axis). The area
tical (X-axis) axesin(Y-axis).
red color
Therefers to red
area in the color
maximumrefers strength value, while
to the maximum strength value
the blue area indicates
while the blue area indicates the minimum strength. It can be seen athat
the minimum strength. It can be seen that there was risethere
in the
was a rise in
CS, TS, and FS ofthethe
CS,proposed
TS, and FSmortar when themortar
of the proposed silica fume
whenincreased up toincreased
the silica fume 20%, andupthe to 20%, and
content of graphene nanoplatelets
the content increased
of graphene up to 1.5%.
nanoplatelets Beyond
increased up tothis value,
1.5%. a reduction
Beyond this value,ina reduction
in the mechanical properties was recorded. This result is in line with the experimenta
results, which were discussed in detail in Section 3.1.
Buildings 2023, 13, 1949 14 of 20

Buildings 2023, 13, x FOR PEER REVIEW 15 of 21

the mechanical properties was recorded. This result is in line with the experimental results,
which were discussed in detail in Section 3.1.

Figureevolution
Figure 10. The predicted 10. The predicted evolution
of mechanical of mechanical
properties properties of ultra-high-strength
of ultra-high-strength mortar contain-
mortar containing
graphene and silicaing graphene
fume; and silica fume;
(a) compressive (a) compressive
strength, strength,
(b) flexural (b) flexural
strength, and (c)strength, and (c) tensile strength
tensile strength.
 Buildings 2023, 13, x FOR PEER REVIEW 16 of 21
Buildings 2023, 13, 1949 15 of 20

3.3. Microstructure Analysis

3.3. Microstructure Analysis
The micrographs were obtained using SEM of the microstructure of concrete samples
The micrographs
containing GNPs afterwere obtained
28 days using
of the Kai SEM
Cui of theAn
process. microstructure of concrete
inadequate hydration samples
rate causes
containing
unreacted GNPsobjectsafter 28 days
within of the Kaicement
the hydrated Cui process.
paste,An inadequate
blocking hydration
the mixture fromrate causes
reaching
unreacted
its required objects within
strength. Thethe hydrated
GNP quantity cement
used inpaste, blockingincreased
the mixtures the mixture thefrom reaching
durability and
its required strength. The GNP quantity used in the mixtures increased
strength of the concrete mixes, resulting in the creation of C-S-H and the chemical inter- the durability
and
actionstrength
withinofPortlandite
the concrete mixes,2)resulting
(Ca(OH) and silicaininthe creation
silica fumeof inC-S-H and the
conjunction withchemical
GNPs.
interaction within Portlandite (Ca(OH)
The microscopy results clearly demonstrated 2 ) and silica
that the strength and dispersion of GNPs.
in silica fume in conjunction with C-S-H
The microscopy results clearly demonstrated that the strength and dispersion
gel in the cemented cement paste had improved. Figure 11 illustrates the internal charac- of C-S-H gel
in the cemented
teristics cement paste
of the concrete had at
samples improved. Figure of
magnifications 11 10
illustrates
µm (a, c)theand
internal
2 µmcharacteristics
(b, d), accord-
of the concrete samples at magnifications of 10 µm (a, c) and
ingly. GNPs contain many different layers, which improve their toughness 2 µm (b, d), accordingly.
andGNPs
make
contain many different layers, which improve their toughness and make them excellent for
them excellent for reinforcing composite materials. GNPs have the potential to increase
reinforcing composite materials. GNPs have the potential to increase toughness, strength,
toughness, strength, and resistivity, as previously stated by researchers [59]. Binding the
and resistivity, as previously stated by researchers [59]. Binding the microstructure at the
microstructure at the nano level adds more to the reinforcement effect.
nano level adds more to the reinforcement effect.

Figure11.
Figure 11.Image
Imageof
ofFESEM
FESEMtest
testfor
forthe
theconcrete
concretespecimen
specimencontaining
containingGNPs;
GNPs;(a,c)
(a,c)magnification
magnificationof
of
10 µm and (b,d) magnification of 2 µm.
10 µm and (b,d) magnification of 2 µm.

The EDX
The EDX test
test results
results were
were utilized
utilized to
to illustrate
illustrate the
the impact
impact ofof GNPs
GNPs with
with different
different
concentrationsininthe
concentrations theconcrete
concreteat at
thethe hydration
hydration ageage of 28th
of 28th days,
days, as shown
as shown in Figure
in Figure 12. The12.
The microstructure characteristic of concrete containing GNPs was deferred
microstructure characteristic of concrete containing GNPs was deferred with increasing with increas-
ing carbon
carbon content,
content, which which refers
refers to the
to the graphene
graphene concentration
concentration atat 0.5%,1%,
0.5%, 1%,1.5%,
1.5%,and
and2%2%
cement replacement. The wall effect and nanofiller migration effect enrich
cement replacement. The wall effect and nanofiller migration effect enrich the ITZ with the ITZ with
nanofillersand
nanofillers andaffect
affectthe
thewalls
wallscontaining
containing GNPs,
GNPs, enhancing
enhancing the
the ITZ
ITZ microstructures
microstructures [60].
[60].
Moreover, when
Moreover, when the 0D,0D, 1D,
1D,and
and2D 2Dnanomaterials
nanomaterialsare combined
are combined into thethe
into mixture, it can
mixture, it
absorb
can a tremendous
absorb a tremendous amount
amount of water in the
of water composite,
in the composite, enhancing
enhancing the the
capacity andand
capacity de-
creasing the
decreasing local
the water-to-binder
local water-to-bindercontent
content[61].
[61].
Buildings
Buildings2023,
2023,13,
13,x1949
FOR PEER REVIEW 1716ofof21
20

(a) (c)

(b) (d)

Figure 12. EDX test Image for the concrete samples that contain graphene nanoplatelets, (a) 0.5%
Figure 12. EDX test Image for the concrete samples that contain graphene nanoplatelets, (a) 0.5%
GNPs of 10 µ m, (b) 1% GNPs, (c) 1.5% GNPs, and (d) 2% GNPs.
GNPs of 10 µm, (b) 1% GNPs, (c) 1.5% GNPs, and (d) 2% GNPs.

3.4.
3.4.Numerical
NumericalOptimization
OptimizationUsingUsingthe theRSM
RSMModel
Model
Optimization
Optimizationof ofthe
theindependent
independentvariables
variablesinvolving
involvingGNPs,
GNPs,SF, SF, and
and age
age was
was numer-
numeri-
ically
cally obtained using desirability
desirability functions
functions that
that were
were provided
provided byby the
the RSM
RSM model.
model. In Inthe
the
current
currentliterature,
literature,desirability
desirabilityfunctions
functionsarearewidely
widelyacknowledged
acknowledgedas asthe
themost
most effective
effective
solution
solutionfor for obtaining
obtaining the the optimal
optimal values
values ofof the
the involved
involved parameters.
parameters. ItIt was
was calculated
calculated
based on the maximum value of the proposed mortar’s CS,
based on the maximum value of the proposed mortar’s CS, TS, and FS strength. TS, and FS strength. It is note-
It is
worthy
noteworthythat the
thatdesirability functions
the desirability yield multiple
functions solutions,
yield multiple all of which
solutions, all ofhave
whicha dimen-
have a
sionless desirability
dimensionless scale ranging
desirability betweenbetween
scale ranging one andone zero. The
and value
zero. Theof value
one refers to refers
of one a de-
sirable strength,
to a desirable while zero
strength, while indicates a thoroughly
zero indicates undesirable
a thoroughly strength.
undesirable The desirability
strength. The desir-
ability function
function (DR) can (DR)be can be defined
defined using using Equation
Equation (11), where
(11), where ‘n’ denotes
‘n’ denotes the number
the number of in-of
involved
volved variables.
variables.
DR = (d1 × d2 × d3 × d4 × . . . dn )(1/n) (11)
𝐷𝑅 = (𝑑1 × 𝑑2 × 𝑑3 × 𝑑4 × … 𝑑𝑛 )(1/𝑛) (11)
The optimization results of the three independent variables can also be graphically
The optimization results of the three independent variables can also be graphically
depicted, as shown in Figure 13. It can be seen that the optimal values GNPs and SF were
depicted, as shown in Figure 13. It can be seen that the optimal values GNPs and SF were
1.5% and 20%, respectively. Using the optimal value, a maximum strength was recorded in
1.5%
which and
the20%, respectively.
CS, TS, and FS were Using theMPa,
129.95 optimal
14.05value,
MPa, aandmaximum
19.2 MPa, strength was recorded
respectively. This fact
in which the CS, TS, and FS were 129.95 MPa, 14.05 MPa, and 19.2 MPa,
is almost in line with our experimental results, which were explained in detail in Section respectively. This
3.1.
fact is almost
It should alsoinbeline with
noted thatourtheexperimental
validation ofresults, which were
the optimization explained
process in detail
was carried outinusing
Sec-
tion
three3.1. It should also
experimental be noted
tests. It wasthat the validation
found that the errorof the optimization
percentage process
between thewas carried
experiment
out using three experimental tests. It was found that
and solutions obtained from the desirability function was less than 5%. the error percentage between the
experiment and solutions obtained from the desirability function was less than 5%.
13, x FOR Buildings
PEER REVIEW
2023, 13, 1949 18 of 21 17 of 20

Figureof13.
Figure 13. Optimization Optimization
GNPs, SF, andof GNPs,
age SF,the
using anddesirability
age using the desirability function.
function.
4. Conclusions
4. Conclusions The current study set out a daunting objective to develop ultra-high-strength mortar
The current study
designedsetfor
outfuture
a daunting objective
applications in 3D to develop
printing ultra-high-strength
endeavors. mortar potential
Utilizing the unrivaled
of silica fume and graphene nanoplatelets, the present study aimed
designed for future applications in 3D printing endeavors. Utilizing the unrivaled poten- to set new ground
tial of silica fume rules. The predicted
and graphene findings and
nanoplatelets, the findings
the present studyfrom experiments
aimed to set neware incorporated to
ground
reveal the following prominent conclusions by methodically
rules. The predicted findings and the findings from experiments are incorporated to optimizing the mechanical
re-
characteristics, which include compressive, flexural, and tensile strength, using predicted
veal the following prominent conclusions by methodically optimizing the mechanical
results and experimental data for a theoretical approach:
characteristics, which include compressive, flexural, and tensile strength, using predicted
i. The results of the flow table showed a significant decrease in the flow of concrete
results and experimental data for a theoretical approach:
slurry with the increase in the concentration of GNP. The results confirmed the vital
i. The results of the flow role oftable showed ainsignificant
nanoparticles binding the decrease
mixture and in the flow the
reducing of concrete
amount of water in
slurry with the increase in the concentration of GNP. The results confirmed the vital
the mixture.
ii.
role of nanoparticles Adding both GNPs
in binding and SF and
the mixture to the mortar, with
reducing a water-to-cement
the amount of water in ratio
theof 0.23 and
mixture. a cement-to-sand ratio of 1:1, enhanced the compressive strength to an incredible
ii. Adding both GNPs and MPa,
133.3 SF toproducing
the mortar, a long-lasting impact as well as
with a water-to-cement excellent
ratio improvement.
of 0.23 and a
iii. Beyond a threshold of 1.5% GNPs, mechanical properties began to deteriorate, indi-
cement-to-sand ratio of 1:1, enhanced the compressive strength to an incredible 133.3
cating a possible impairment of hydration and pozzolanic activity due to excessive
MPa, producing a long-lasting impact as well as excellent improvement.
GNP contents (clustering). As a result, the ideal values of 1.5% GNPs and 20% SF
iii. Beyond a thresholdindicated
of 1.5% by GNPs, mechanical
the desirability properties
function proved began to deteriorate,
to be crucial indi-to develop
for the mortar
cating a possible impairment of hydration and pozzolanic activity due to excessive
its full potential.
GNP contents iv. (clustering). As
The tensile and a result, thestrengths
flexural ideal values of 1.5%
increased GNPs
by more thanand 20%
50% SF using an
when
optimally function
indicated by the desirability measuredproved
mixturetoofbe 1.5% GNPs
crucial forand
the20% SF due
mortar to the exceptional
to develop
its full potential. densification of the slurry microstructure and the sealing of irreparable cracks.
v. The study focused on decreasing the porousness
iv. The tensile and flexural strengths increased by more than 50% when using an opti- of the concrete to achieve ultra-
high-performance mortar, where the FE-SEM images demonstrated that GNPs
mally measured mixture of 1.5% GNPs and 20% SF due to the exceptional densifica-
could fill the pores in the mortar and connect the cracks to each other.
tion of the slurry
vi.
microstructure and the sealing of irreparable cracks.
The strong confluence of the RSM model and experimental data results demon-
v. The study focused on decreasing
strates the porousness
their remarkable of the concrete
resemblance alongsidetothe achieve ultra-high- of CS, TS,
error percentages
performance mortar, where the FE-SEM images demonstrated
and FS, all falling below 5%. The above indicates the enormousthat GNPs could fill
potential of the
the pores in the mortar and connect
suggested the cracks
three nonlinear to each
equations forother.
accurately predicting the mechanical char-
vi. The strong confluence acteristics of mortar.
of the RSM model and experimental data results demonstrates
vii. A strong correlation,
their remarkable resemblance alongside exceeding
the error 0.97, between anticipated
percentages of CS, TS,and andobserved
FS, all outcomes
attests to the model’s unchanging
falling below 5%. The above indicates the enormous potential credibility and resilience. The
of the suggested three difference be-
tween the anticipated and adjusted R2 is 0.2 percent or less, demonstrating the
nonlinear equations for accurately predicting the mechanical characteristics of mor-
RSM model’s enormous promise for future research. Moreover, statistical error
tar. parameters with anticipated and adjusted values less than 0.03 and 0.09, respec-
vii. A strong correlation, exceeding
tively, reinforce0.97,
thebetween
model’s anticipated
efficiency and and observed outcomes
correctness, leaving noat- opportunity
tests to the model’s forunchanging
controversy. credibility and resilience. The difference between the
anticipated and adjusted R2 is 0.2 percent or less, demonstrating the RSM model’s
enormous promise for future research. Moreover, statistical error parameters with
anticipated and adjusted values less than 0.03 and 0.09, respectively, reinforce the
model’s efficiency and correctness, leaving no opportunity for controversy.
Buildings 2023, 13, 1949 18 of 20

Author Contributions: Writing—original draft preparation, H.A.S.; Conceptualization, H.A.S. and

H.A.A.; methodology, H.A.A.; software, H.A.A.; validation, A.B.M.A.K. and A.S.; formal analysis,
A.A.M. and A.B.M.A.K.; investigation, A.B.M.A.K.; resources, A.S.; data curation, H.A.S.; writing—
review and editing, H.A.S. and H.A.A.; supervision, A.A.M.; funding acquisition, A.A.M. All authors
have read and agreed to the published version of the manuscript.
Funding: The UKM Centre of Research Management and Instrumentation Management (CRIM),
UKM, and the Dana Impak Perdana Grant (DIP-2021-014).
Data Availability Statement: The data presented in this study are available on request from the
corresponding author.
Acknowledgments: In obtaining the intended results, the authors would like to thank Universiti
Kebangsaan Malaysia (UKM) for financing and supporting this study.
Conflicts of Interest: The authors declare no conflict of interest for the publication of the review paper.

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