sustainability-16-03328

sustainability
Article
Towards Sustainable Material: Optimizing Geopolymer
Mortar Formulations for 3D Printing: A Life Cycle
Assessment Approach
Charlotte Roux 1, * , Julien Archez 2 , Corentin Le Gall 2 , Myriam Saadé 2 , Adélaïde Féraille 2
and Jean-François Caron 2
1 MINES Paris—PSL Research University, CEEP (Centre Energie Environnement Procédés),

60 Boulevard Saint Michel, 75006 Paris, France
2 Navier Laboratory, Ecole des Ponts ParisTech, Gustave Eiffel University CNRS,
77454 Champs sur Marne, France
* Correspondence: charlotte.roux@minesparis.psl.eu
Abstract: Geopolymer-based concretes have been elaborated among others for their potential to
lower the environmental impact of the construction sector. The rheology and workability of fresh
geopolymers make them suitable for new applications such as 3D printing. In this paper, we aim to
develop a potassium silicate- and metakaolin-based geopolymer mortar with sand and local earth
additions suited for 3D printing and an environmental assessment framework for this material. The
methodology aims at the optimization of both the granular skeleton and the geopolymer matrix for
the development of a low-environmental-impact material suited for 3D printing. Using this approach,
various metakaolin/earth geopolymer mortars are explored from a mechanical and environmental
point of view. The environmental assessment of the lab-scale process shows an improvement for
the climate change category but a degradation of other indicators, compared to Portland-cement-
based concrete. Several promising options exist to further optimize the process and decrease its
environmental impacts. This constitutes the main research perspective of this work.
Citation: Roux, C.; Archez, J.; Le Gall,

Keywords: sustainable material; geopolymers; 3D printing; material characterization; environmental
C.; Saadé, M.; Féraille, A.; Caron, J.-F.
optimization; life cycle assessment
Towards Sustainable Material:
Optimizing Geopolymer Mortar
Formulations for 3D Printing: A Life
Cycle Assessment Approach.
Sustainability 2024, 16, 3328. https://
1. Introduction
doi.org/10.3390/su16083328 Concrete is responsible for 8% of global greenhouse gas (GHG) emissions and 5.2% of
particulate matter (PM10 ) emissions [1]. With the gradual awareness of the urgency of
Academic Editors: Uroš Klanšek
decarbonizing the concrete and cement industries, alternatives have been developed,
and Tomaž Žula
particularly to replace Portland cement, which largely contributes to the carbon footprint
Received: 13 March 2024 of concrete [2,3]. Some alternatives rely on the replacement of cement using by-products of
Revised: 9 April 2024 high-emitting industries such as coal and steel production, providing fly ashes and slags,
Accepted: 12 April 2024 respectively. Other emerging technologies aim at reducing emissions and energy use in
Published: 16 April 2024 cement production [4,5]. The wide adoption of such technologies, however, faces multiple
barriers, ranging from regulatory issues to supply, product confidence, and technical
obstacles [6].
In addition to being a major contributor to climate change, concrete production also
Copyright: © 2024 by the authors.
consumes notable amounts of natural resources such as aggregates and sand with a certain
Licensee MDPI, Basel, Switzerland.
quality. The world consumption of sand and aggregates is estimated to reach about
This article is an open access article
distributed under the terms and
41 billion tons per year and is expected to increase soon [7]. The sand supply has long been
conditions of the Creative Commons
taken for granted but nowadays faces issues of local resource depletion, impacts on the
Attribution (CC BY) license (https:// ecosystem, and climatic instabilities [8].
creativecommons.org/licenses/by/ In this context, geopolymers recently benefited from renewed interest. Geopolymers
4.0/). (GPs) are inorganic, amorphous three-dimensional alumino-silicate materials synthesized at
Sustainability 2024, 16, 3328. https://doi.org/10.3390/su16083328 https://www.mdpi.com/journal/sustainability

Sustainability 2024, 16, 3328 2 of 20
an ambient temperature through the activation of an aluminosilicate source (i.e., metakaolin)

by an alkaline solution [9]. The polycondensation reaction between alumina and silicates
occurring under basic alkali activation results in a geopolymer network. Such geopolymer
provides resistance to high temperatures, as well as high mechanical or chemical resistance
due to GP covalent bonds [10,11]. Sodium and potassium alkaline solution are largely used
as activators but another synthesis path involving phosphoric acid is also studied, to a
lesser extent [12].
Geopolymers are seen as an alternative to Ordinary Portland Cement (OPC), with
expected lower CO2 emissions [9]. Portland cement requires heating up to 1450 ◦ C for
several hours which causes the calcination of the limestone (clinkerization process). The
combustion of fuels to reach such a temperature and the decarbonization of limestone both
emit a high quantity of CO2 —about one ton of CO2 per ton of cement [13]. In comparison,
geopolymer production requires the use of a chemical solution of alkali silicates and the
heating of kaolin clay at a lower temperature (around 850 ◦ C), without the calcination of
limestone. The synthesis of raw material is, therefore, less emitting than the Portland cement
production process, when considering the CO2 emitted directly during the production
process [9]. However, its environmental advantage has to be rigorously confirmed in a life
cycle and multi-criteria perspective [14].
Life Cycle Assessment (LCA) is a method currently widely used to assess the envi-
ronmental impacts of products and services [15,16]. It is a multi-step and multi-criteria
approach developed to avoid impacts shifting along the value chain and among impact
categories. Multiple Life Cycle Assessment studies have been applied to geopolymer (GP)
matrices, concretes, and mortars, with the latter being constituted of a geopolymer matrix
and a granular skeleton [17–22]. So far, no scientific consensus has been reached about their
environmental performances, mainly because the results highly depend on the formulation
and raw materials used for their synthesis. Some authors show a significant reduction of
environmental impacts when using GP concrete based on slag, fly ash, and alkali-silicate
systems [18,23], while others confirm a slight reduction of GHG emissions using fly ash and
blast-furnace geopolymers [19]. They also highlight a trade-off between impacts on climate
change and other environmental categories such as abiotic resources, eutrophication, and
acidification, for which GP concrete presents higher impacts. GP concrete could even have
a higher carbon footprint than conventional concrete depending on upscaling commercial
scenarios for 3D printing concrete [24].
Most studies agree on the importance of the contribution to the impacts of alkali
activator production. To reduce the contribution of the geopolymer matrix, fillers such as
sand can be added to form the geopolymer mortar. Another way is to use raw earth instead
of sand [25] as GP chemistry makes it more prone to interact with the earth, especially
clays, than ordinary concrete [26,27]. In this way, from a circular economy perspective,
geopolymer synthesis could help recover excavated earth.
In addition to their potential intrinsic environmental performances, GP mortars could
be suited for 3D printing. Applied to the construction sector, this technique, currently
under development, is considered as a way to reduce the amount of construction materials
used [28]. Geopolymers present a totally different physic than 3D-printed rock analogs [29]
and a different setting than cement mortars—they are closer to polymeric glues than
hydrated mortars. They also may be highly completed with different fillers. For these
reasons, they become good challengers for this new way of building. Their interesting
durability properties would also be relevant in a growing number of applications (structural
materials, heat-resistant pavement, sewer pipes, sub-aqueous seawater, etc.) [30]. Improved
knowledge of geopolymers is thus broadly recommended to understand their potential
to mitigate carbon emissions in the construction sector [31–33] and precisely evaluate the
domain of environmental relevance for this technology. Specific work on geopolymer
mortars for 3D printing shows low embodied carbon per m3 compared to cementitious
material [34]. However, the contribution of transport and the curing and mixing process
are not clearly presented. Moreover, most formulations reviewed are based on used fly ash
and blast-furnace slags (Table 1), which are by-products of polluting industries and are only
available in limited quantities. Even if the use of fly ash and blast-furnace slags could be
envisioned in countries where electricity is still mainly coal-based, they remain by-products.
They might not be a long-term option for replacing cementitious blends on a large scale.
The development of a potassium silicate- and metakaolin-based geopolymer mortar with
low environmental impact, sufficient mechanical properties, and suitability for 3D printing
could therefore be beneficial for the construction sector. Its environmental impact must,
however, be thoroughly studied using a comprehensive Life Cycle Assessment.
Table 1. Comparison of embodied GHG emissions for GP concrete or mortar and Ordinary Portland
Concrete found in the literature.
Geopolymer (GP) GHG Emissions of GHG Emissions of Ref.

Ref Comments
Description GP (kgCO2 eq/m3 ) OPC (kgCO2 eq/m3 )
Carbon accounting and not full
Binder, suitable for 3D LCA (f.e. water carbon footprint
107 556 [34]
printing—FA50% + GGBS50% is set to zero). Reference binder
is 80% OPC and 20% FA.
Carbon accounting and not full
Binder, suitable for
LCA (f.e. water carbon footprint
3D printing—FA78.5% + 134 556 [34]
is set to zero). Reference binder
GGBS13.8% + SF7.7%
is 80% OPC and 20% FA.
Full, complete LCA, including
Slag and FA GP binder for
677 493 [24] sensitivity analysis
3D printing
on allocations.
Carbon accounting
“Standard” FA GP concrete 320 354 [35]
and not full LCA.
Also investigating MK-GP, but
clear figures are not available.
FA GP concrete 169 306 [19]
MK-GP impacts are higher than
FA-GP impacts.
Indian context, cement
FA and slag GP cement 267 895 [18]
and not concrete.
FA: Fly ash, GGBS: granulated blast-furnace slag.
The objective of this paper is to propose a formulation for a low-environmental-impact

geopolymer mortar to be used for 3D-printing applications exploiting locally available
materials. The research explores a lab-scale process developed in a French context. After a
brief description of the studied class of geopolymer, the article describes the LCA-based
approach used to optimize geopolymer formulation, relying on its environmental perfor-
mance. An initial formulation of a geopolymer mortar is tested, and its environmental
impacts are evaluated to identify the life cycle stages with the main impact. The article then
presents the results of formulation optimization using LCA and examines the influence of
LCA parameters such as transport. Based on a comparison of three 3D-printing materials,
it discusses potential improvements of the process to further decrease the environmental
impacts of metakaolin geopolymers, highlighting the need to improve the accuracy of
LCA data.
2. Materials and Methods

2.1. Methodological Approach
Our methodological approach is summed up in Figure 1. To understand the environ-
mental impacts of a printable geopolymer formulation, a first environmental assessment
was led using a GP matrix previously developed in the NAVIER laboratory and suitable
for 3D printing, as described in [36]. This first matrix serves as a reference for further
optimization. It is composed of 46%w metakaolin, 37%w potassium alkaline solution,
15%w wollastonite, and 2%w glass fibers and will be called GP–GfW in this study.
15%w wollastonite, and 2%w glass fibers and will be called GP–GfW in this study.
Based on the environmental impact of a geopolymer-based 3D-printing material, an
optimization of the matrix was undertaken to lower the environmental impacts while
maintaining sufficient mechanical property. Then, geopolymer formulations (matrix +
granular skeleton) were developed to decrease GHG emissions while maintaining printa-
bility and a minimum mechanical strength of 32.5 MPa (NF-EN 197-1 standard [37]).
Figure 1.
Figure 1. Methodological
Methodological approach.
approach.
The results
Based on thewere further analyzed
environmental impacttoofunderstand the influence
a geopolymer-based of certainmaterial,
3D-printing parameters an
on the environmental impacts of the formulation. The studied process
optimization of the matrix was undertaken to lower the environmental impacts while main-is a lab process and
is not optimized
taining sufficient as the processes
mechanical currently
property. Then, ingeopolymer
place withinformulations
the cement and concrete
(matrix sector
+ granular
are. Transport
skeleton) distances and
were developed modes were
to decrease GHGinvestigated in a maintaining
emissions while sensitivity analysis to under-
printability and a
stand howmechanical
minimum impacts could be decreased
strength of 32.5 MPaby (NF-EN
a scale effect.
197-1 The poor [37]).
standard quality of some data,
related
Thetoresults
low temporal representativity,
were further analyzed tofor instance, the
understand is also discussed.
influence of certain parameters
on the environmental impacts of the formulation. The studied process is a lab process
2.2. Raw
and Materials
is not optimizedand as
Sample Preparation
the processes currently in place within the cement and concrete
sector are. Materials
2.2.1. Raw Transport distances and modes were investigated in a sensitivity analysis to
understand how impacts could be decreased by a scale effect. The poor quality of some
Geopolymer formulations were synthesized at the NAVIER laboratory with potas-
data, related to low temporal representativity, for instance, is also discussed.
sium silicate solution (Geosil14515: [K] = 7.0 M, SiO2 = 19%w, K2O = 22%w and H2O =
59%w)
2.2. Rawand metakaolin
Materials aluminosilicate
and Sample Preparationsource (M1000: SiO2: 55%w Al2O3: 40%w, D50 = 10
µm) [38]. The developed
2.2.1. Raw Materials formulations differ from most GPs presented in the literature,
which are sodium silicate solution and industrial waste (fly ashes, ground granulated
Geopolymer formulations were synthesized at the NAVIER laboratory with potassium
blast slag)-based GPs [39]. Given their limited availability on the French territory and the
silicate solution (Geosil14515: [K] = 7.0 M, SiO2 = 19%w, K2 O = 22%w and H2 O = 59%w) and
uncertainties of their future supply, industrial wastes were not included in the tested for-
metakaolin aluminosilicate source (M1000: SiO2 : 55%w Al2 O3 : 40%w, D50 = 10 µm) [38].
mulations.
The developed formulations differ from most GPs presented in the literature, which are
A granular skeleton constituted partly of masonry sand (0–4 mm diameter) and
sodium silicate solution and industrial waste (fly ashes, ground granulated blast slag)-
partly of raw earth was then added to the geopolymer matrix to form a geopolymer mor-
based GPs [39]. Given their limited availability on the French territory and the uncertainties
tar. Raw earth was supplied locally from the excavation works of the “Grand Paris” pro-
of their future supply, industrial wastes were not included in the tested formulations.
ject. The earth was
A granular driedconstituted
skeleton in an ovenpartly
(24 h ofat masonry
100 °C) and
sandthen
(0–4sieved consecutively
mm diameter) into
and partly
four particle sizes (1.6–2.5 mm, 0.8–1.6 mm, 0.4–0.8 mm, and <0.4 mm).
of raw earth was then added to the geopolymer matrix to form a geopolymer mortar. Raw Qualitative tests
regarding
earth earth addition
was supplied infrom
locally geopolymers showed
the excavation waterofabsorption
works the “Grandissues.
Paris”The earthThe
project. has
a higher water demand than sand due◦ to the presence of clays (like illite
earth was dried in an oven (24 h at 100 C) and then sieved consecutively into four particle or smectite for
the earth used in this study), especially for the low granulometry (<0.8
sizes (1.6–2.5 mm, 0.8–1.6 mm, 0.4–0.8 mm, and <0.4 mm). Qualitative tests regarding mm). To quantify
earth addition in geopolymers showed water absorption issues. The earth has a higher
water demand than sand due to the presence of clays (like illite or smectite for the earth
used in this study), especially for the low granulometry (<0.8 mm). To quantify the water
absorption, the water demand of earth particles and sand was quantified by measuring
the quantity of water (in increments of 10 µL) to be added to 10 g of material to reach a
moist state. The moist state corresponds to a visual criterion where the sand or earth is
fully wet. Their values are reported in Table 2. Given that the earth absorbs most of the
water from the mix, the mortar becomes dry too quickly and the earth addition becomes
the
the
the
thewater
water
water
water absorption,
absorption,
absorption,
absorption, the
the
the water
the water
water
water demand
demand
demand
demand ofof
of
ofearth
earth
earth
earth particles
particles
particles
particles and
andsand
and sandwas
sand wasquantified
was quantified
quantified byby
by
the water absorption, the water demand of earth particles and andsandsand was was quantified
quantified by by
measuring
measuring
measuring
measuring the
the
the quantity
quantity
quantity
the quantity ofof
of water
water
water
of water (in
(in
(in increments
increments
increments
(in increments ofof
of1010
10 µL) µL)
µL) toto
to bebe
be added
added
added toto
to 1010
10 gggofof
of material
material
material
measuring the quantity of water (in increments of 10ofµL)10 to µL)betoadded
be added to 10tog 10of g of material
material
toto
to reach
reach
reach aaamoist
moist
moist state.
state.
state. The
The
The moist
moist
moist state
state
state corresponds
corresponds
corresponds toto
to aaavisual
visual
visual criterion
criterion
criterion where
where
where the
the
the sand
sand
sand oror
or
to reach a moist state. The moist state corresponds to a visual criterion where the sand5sand
to reach a moist state. The moist state corresponds to a visual criterion where the or
Sustainability 2024, 16, 3328 of 20
or
earth
earth
earth
earthisisisis
fully
fully
fully
fullywet.
wet.
wet.
wet. Their
Their
Their
Theirvalues
values
values
values are
are
are
arereported
reported
reported
reportedinin
in Table
in Table
Table
Table 2.2.2.2.
Given
Given
Given
Given that
that
that
thatthe
the
the
theearth
earth
earth
earth absorbs
absorbs
absorbs
absorbs most
most
most
most
earth is fully wet. Their values are reported in Table 2. Given that the earth absorbs most
ofof
of the
of the
the
thewaterwater
water
water from
fromthe
from the
the mix,
mix,
mix, the
the
the mortar
mortar
mortar becomes
becomes
becomes dry
dry
dry too too
too quickly
quickly
quickly and
andthe
and the
the earth
earth
earth addition
addition
addition
of the water fromfrom the
the mix, mix, the
the mortar mortar becomes
becomes dry toodry too quickly
quickly and and the
the earth earth addition
addition
becomes
becomes
becomes
becomes
impossible. impossible.
impossible.
impossible.
impossible.
The absorption The
The
The
Theabsorption
absorption
absorption
absorption
of water of ofof
ofwater
of
bywater water
water
water
the earth by
byby
bythe
the
the
the
modifies earth
earth
earth
earth modifies
modifies
modifies
modifies the
the
the ratio
the ratio
ratio
ratioof of
of
ofchemical
chemical
chemical
chemical
becomes impossible. The absorption by the earth the ratio ofthe
modifies chemical
ratio ofcomponents
chemical
components
andcomponents
components
components
consequently and
and
and
and consequently
consequently
consequently
consequently
the the
the
the
polycondensationthepolycondensation
polycondensation
polycondensation
polycondensation
reaction of the reaction
reaction
reaction
reaction
geopolymer. ofof
of the
of the
the
thegeopolymer.
geopolymer.
geopolymer.
geopolymer.
components and consequently the polycondensation reaction of the geopolymer.
Table
Table
Table
Table Granulometry
2.2.2.2.
Table Granulometry
Granulometry
2. and
Granulometryand
Granulometryandwater
andwater
water
and demand
waterdemand
waterdemandof
demand
demandofsand
of
ofsand
sand
of and
sandand
sandandearth
andearth
andearthused
earthused
earth in
used
used
usedinthis
in
in this
in study.
this
thisstudy.
study.
study.
this study.
Table 2. Granulometry and water demand of sand and earth used in this study.
Particle
Particle
Particle
Particle Type
Type
Type
Type Sand
Sand
Sand Earth
Earth
Earth
Particle
Particle TypeType SandSand
Sand Earth
Earth
Earth
Grain
Grain
Grain
Grainsize
size
size (mm)
size (mm)
(mm)
(mm) 0–4
0–4
0–4
0–4 1.6–2.5
1.6–2.5
1.6–2.5
1.6–2.5 0.8–1.6
0.8–1.6
0.8–1.6
0.8–1.6 0.4–0.8
0.4–0.8
0.4–0.8
0.4–0.8 <0.4
<0.4
<0.4
<0.4
Grain sizesize
Grain (mm)
(mm) 0–4 0–4 1.6–2.5
1.6–2.5 0.8–1.6
0.8–1.6 0.4–0.8
0.4–0.8 <0.4
<0.4
Water
Water
Water
Water
Water absorption
absorption
absorption
absorption
absorption േേേേ
± 0.02
Water absorption േ 0.13
0.13
0.13 0.06
0.06
0.06 0.28
0.28
0.28 0.58
0.58
0.58 0.75
0.75
0.75
0.13 0.13 0.06 0.06 0.28 0.28 0.58 0.58 0.75 0.75
0.13 0.06 0.28 0.58 0.75
0.02(mL/g)
0.02(mL/g)
0.02 (mL/g)
(mL/g)
0.02 0.02
(mL/g) (mL/g)
Picture
Picture
Picture
Picture
Picture
Picture
To
To
To
Tooptimize
optimize
optimize
optimizethe
the
the earth
the earth
earth quantity,
earth quantity,
thethe
quantity,
quantity, the
the
thegranular
granular
granular
granular skeleton
skeleton
skeleton
skeleton of of
of
ofthe
the
the
themix
mix
mix was
was
was
mix improved
was improved
improved
improvedfol-
fol-
fol-
ToTooptimize
optimize the
the earth
earth quantity,
quantity, the granular
granular skeleton
skeleton of
of the
the mix
mix was
wasimproved
improved fol- fol-
follow-
lowing
lowing
lowing
lowing the
the
the Fuller-Thompson
the Fuller-Thompson
Fuller-Thompson
Fuller-Thompson method
method
method
method [36],
[36],
[36], considering
[36], considering
considering
considering Equation
Equation
Equation
Equation (1).
(1).
(1).
ing
lowing the Fuller-Thompson
the Fuller-Thompson method
method [36],
[36],considering
considering Equation
Equation (1). (1).
(1).
pipi
pi ===(d_i/D)
pi (d_i/D)
=(d_i/D)
(d_i/D)0.45
0.45 (1)
(1)
(1)
(1)(1)(1)
0.45 0.45
0.45
0.45
pi
pi == (d_i/D)
(d_i/D) 0.45
where
where
where
where pipi
pipiisisisis
thethe
the percent
the percent
percent
percent passing
passing
passing
passing ith
ith
ith sieve,
ith sieve,
sieve,
sieve,didi
didi(mm)
(mm)
(mm)
(mm) isisisis
thethe
the opening
the opening
opening
opening size
size
size
sizeofof
ofthe
of the
the ith
the ith
ithith sieve,
sieve,
sieve, and
sieve, and
and
and
where
where pipiisis the the percent
percent passing
passing ith
ithsieve,
sieve, didi(mm)
(mm)isisthe the opening
opening size size of
of the
the ith sieve,
ith sieve, and D
and
DDD(mm)
(mm)
(mm)
D (mm) is is
is the the
the maximum
maximum
maximum particle
particle
particle size.
size.
size.
D (mm)
(mm) theismaximum
is the
is
the maximum
maximum particle
particle
particle size. size.
size.
An An
An Anoptimized
optimized
optimized
optimized granularity
granularity
granularity
granularity was
was
was
wasdesigned
designed
designed
designed to
totocompensate
to compensate
compensate
compensate for
for
for the
for the
the high
the high
high
high water
water
water
water absorption
absorption
absorption
absorption
AnAn optimized
optimized granularity
granularity waswas designed
designed totocompensate
compensate forfor
thethehigh
highwater
water absorption
absorption
ofof
of the
of the
the
the small
small
small
small earth
earth
earth
earthfractions
fractions
fractions
fractions (diameter
(diameter
(diameter
(diameter under
under
under
under 0.80.8
0.8 mm).
0.8 mm).
mm).
mm). The
The
The
The final
final
final
finalcomposition
composition
composition
composition consisted
consisted
consisted
consisted of
ofof
ofof
thethesmall
small earth earthfractions
fractions (diameter
(diameter under
under 0.80.8 mm).mm). The Thefinal
finalcomposition
composition consisted
consisted ofof of
sand
sand
sand
sand forfor
for
foraggregates
aggregates
aggregates
aggregates with
with
with
withaaadiameter
a diameter
diameter
diameter lower
lower
lower
lower than
than
than
than 0.8
0.8
0.8
0.8 mmmm
mm mm and
and
and
and earth
earth
earth
earth for
for
for coarse
for coarse
coarse
coarse aggregates,
aggregates,
aggregates,
aggregates,
sand
sand forforaggregates
aggregates with
with a diameter
a diameter lower
lower thanthan 0.80.8mm mm andandearth
earth forfor
coarse
coarse aggregates,
aggregates,
with
with
with
with aaasize
a size
size
size grain
grain
grain
grainhigher
higher
higher
higher than
than
than
than 0.8
0.8
0.8 mm.
0.8 mm.
mm.
mm. The
The
The
The optimized
optimized
optimized
optimized grain
grain
grain
grain size
size
size distribution
size distribution
distribution
distribution isisisis
exposed
exposed
exposed
exposed in in
in
with
with a size
a size grain
grain higher
higher than
than 0.80.8mm.
mm.The The optimized
optimized graingrain size
sizedistribution
distribution is is
exposed
exposed inin in
Figure
Figure
Figure
Figure 2.2.
2.
Figure
Figure 2. 2. 2.
Figure
Figure
Figure
Figure2.2.2.
Grain
Grain
2.Grain
Grainsize
size
sizedistribution
distribution
distribution
size of
distributionof 
of
of earth
earth
earth
and
and
and
earth 
and sand
sand
sand
sandininin
in the
the
theoptimized
optimized
optimized
the granularity.
optimized granularity.
granularity.
granularity.
Figure
Figure 2. 2.
GrainGrain size
size distribution
distribution ■
of of earth
earth and
and ■ sand
 sand in in
thethe optimized
optimized granularity.
granularity.
2.2.2. Sample Preparation
The nomenclature used in this work is Ma Sb Say Ez , where a and b characterize the ratio
between potassium silicate solution (S) and metakaolin (M), so a + b = 100%. Moreover, “y”
and “z” represent, respectively, the quantity in grams of sand (Sa) and earth (E) added to
form the geopolymer mortar for 100 g of geopolymer paste (a + b). The sample preparation
consisted of adding metakaolin into a silicate solution progressively while mixing with a
planetary mixer. After 3 min of mixing, sand and/or earth were added progressively to the
The nomenclature used in this work is MaSbSayEz, where a and b characterize the ratio
between potassium silicate solution (S) and metakaolin (M), so a + b = 100%. Moreover,
“y” and “z” represent, respectively, the quantity in grams of sand (Sa) and earth (E) added
to form the geopolymer mortar for 100 g of geopolymer paste (a + b). The sample prepa-
Sustainability 2024, 16, 3328 ration consisted of adding metakaolin into a silicate solution progressively while mixing 6 of 20
with a planetary mixer. After 3 min of mixing, sand and/or earth were added progres-
sively to the geopolymer paste and mixed for 5 min. The sample was then cast in a 40 × 40
geopolymer pastemold
× 160 mm closed and mixed forbubbles
and the 5 min. The
weresample
removed waswith
thenacast × 40 ×(50
in a 40needle
vibrating 160Hz,
mm1
closed mold
min). The and the
samples bubbles
were were after
demolded removed withstored
24 h and a vibrating needle
in a sealed (50 Hz,
plastic 1 min).
bag. The
The print-
samples were demolded after 24 h and stored in a sealed plastic bag. The printability
ability of the sample was quantified by overlaying manually the material with a syringe
of thea sample
with was quantified
15 mm diameter. by overlaying
The normal manually
compressive thewere
strengths material with aafter
evaluated syringe with
7 days on
a1215 mm diameter. The normal compressive strengths were evaluated after
(half 40-40-160 mm) samples using an MTS with a 100 kN load cell at 0.5 mm/min con-7 days on
12 (half
stant 40-40-160 mm) samples using an MTS with a 100 kN load cell at 0.5 mm/min
speed.
constant speed.
2.3. Environmental Characterization
2.3. Environmental Characterization
2.3.1. Environmental
2.3.1. Assessment: Methodological
Environmental Assessment: Methodological Choices and Perimeter
Choices and Perimeter of the LCA
of the LCA for
for
3D Printing
3D Printing Geopolymer
Geopolymer Mortars
Mortars
Definition of
Definition ofthe
thefunctional
functionalunit:
unit:The
Thefunctional
functionalunit
unitis is defined
defined as:as: “producing
“producing 1 m13mof3
of geopolymer
geopolymer mortar
mortar suitable
suitable for 3Dforprinting”.
3D printing”. The impact
The impact of the formulation
of the formulation or 3D-
or 3D-printing
printingon
process process on the mechanical
the mechanical propertiesproperties of these geopolymers
of these geopolymers has alreadyhas already
been been
studied in
studied
the past in theand
[40], pastaccording
[40], andtoaccording
the NF EN to the NFstandard,
197-1 EN 197-1the standard,
compressivethe compressive
strength of
strength
the mortarof the mortar
should should
reach reach
at least at MPa
32.5 least 32.5 MPa to
to ensure itsensure its suitability
suitability for 3D print-
for 3D printing. The
ing. The printability
material material printability
also needsalso needs
to be to beSuch
assured. assured. Such printability
printability was qualifiedwas by
qualified
manuallyby
manually overlaying
overlaying the material thewith
material with as
a syringe, a syringe, as a preliminary
a preliminary test [38]. test [38].
boundaries: The flowchart of the system is presented
System boundaries: presented in in Figures
Figures 33 and
and 4.
4. The
study is a cradle-to-gate assessment, and we included in the system the production of GP
mortar as well as upstream activities and processes. GP applications applications are not considered,
and consequently,
consequently, neither are transportation, use, and end-of-life. The equipment used to
neither are transportation, use, and end-of-life.
process the materials
materials (e.g., mixing
mixing unit, oven,
oven, molds) and the the land
land occupation
occupation generated
generated
by the
thelab
labwere
werealso
also excluded
excluded fromfrom
the the
systemsystem processes,
processes, as noas nowere
data dataaccessible.
were accessible.
More-
Moreover, no material
over, no material loss during
loss during the process
the process was was accounted
accounted for infor in study.
this this study. To consider
To consider the
the localized
localized characteristic
characteristic of this
of this supply,
supply, LCA LCA
datadata
werewere as much
as much as possible
as possible adapted
adapted to
to the
the French context.
French context.
Figure 3.
Figure 3. Granularity
Granularity flowchart
flowchart of
of the
the GP
GP studied
studied system.
system. Mixed
Mixed processes are ecoinvent
processes are ecoinvent processes
processes
adapted or modified for the study. Foreground processes are processes defined by the authors.
adapted or modified for the study. Foreground processes are processes defined by the authors.
The study was led using the open-source framework Brightway 2 and its graphic
interface Activity-Browser [41,42], relying on the database Ecoinvent 3.7 Cutoff [43,44].
x FOR PEER REVIEW
Sustainability 2024, 16, 3328 7 7of
of 21
20
4. Flowchart
Figure 4.
Figure Flowchart ofof the
theOPC
OPCstudied
studiedsystem.
system.Mixed
Mixedprocesses
processesare ecoinvent
are processes
ecoinvent adapted
processes or
adapted
modified
or forfor
modified thethe
study. Foreground
study. processes
Foreground areare
processes processes defined
processes by the
defined authors.
by the authors.
2.3.2. Life Cycle Inventory of Individual Processes

The study was led using the open-source framework Brightway 2 and its graphic
The Activity-Browser
interface assumptions made to derive
[41,42], theon
relying process inventory
the database for each
Ecoinvent 3.7component
Cutoff [43,44].of the
studied system are exposed below. Exhaustive information on the system modeling is
givenLife
2.3.2. in Supplementary
Cycle Inventory Materials,
of IndividualSection S1.
Processes
Metakaolin (MK): The considered metakaolin (MK) was provided by the French
The assumptions made to derive the process inventory for each component of the
company Ceradel under the label METAKAOLIN ARGICAL M1000 (Ceradel, Clérac,
studied system are exposed below. Exhaustive information on the system modeling is
France). According to commercial communication by Imerys, it was assumed that the MK
given in Supplementary Materials, Section S1.
was formed from a process involving high-purity kaolinite heated at 750 ◦ C in a rotary
Metakaolin (MK): The considered metakaolin (MK) was provided by the French com-
kiln. The modeling process considers 1.16 kg of kaolin production (ecoinvent process,
pany Ceradel under
contextualized usingthe label METAKAOLIN
a French electricity mix)ARGICAL and 2.5 MJM1000 (Ceradel,
of natural Clérac,to
gas heating France).
obtain
According to commercial
1 kg of metakaolin [22]. communication by Imerys, it was assumed that the MK was
formed from a process involving high-purity kaolinite heated
Potassium silicate solution (PSS): The potassium silicate solution (PSS) used in this at 750 °C in a rotary kiln.
The modeling
process process considers
is a commercial solution 1.16 kg of kaolin
distributed by theproduction
German chemical(ecoinvent process,Woellner
company contex-
tualized
(Ludwigshafen, Germany), under the name Geosil 14515. An existing process 1inkgthe
using a French electricity mix) and 2.5 MJ of natural gas heating to obtain of
metakaolin
ecoinvent database [22]. for sodium silicate was selected based on the same synthesis process
Potassium
(hydrothermal). A molar silicate solution
equivalent(PSS):was The potassium
applied in thesilicate
ongoing solution
flows, (PSS) usedsodium
to replace in this
process is a commercial solution distributed by the German
with potassium [45]. This process had a close solid ratio with the product Geosil 14515 chemical company Woellner
(Ludwigshafen,
used in this study Germany),
(48% mass under the name
of dried contentGeosil 14515. An
compared to existing
45% forprocess in theFinally,
this study). ecoin-
vent database for sodium silicate was selected based on the
water flow was added to the process to match the dried content of the Geosil 14515. This same synthesis process (hy-
drothermal).
way of designing A molar equivalent
a process for PSS was applied
was in theby
confirmed ongoing flows, toproducer.
the industrial replace sodium with
potassium [45]. This
Glass fiber: processintroduced
Previously had a closeinsolid ratio with developed
a formulation the productinGeosil 14515 used
the NAVIER in
labora-
this
torystudy (48% mass
and suitable for 3Dof dried
printingcontent
[36],compared
glass fiberstowere45% used
for thisin study). Finally,formulation.
our reference water flow
was addedfiber
The glass to the
cameprocess
from to match the
a French dried content
producer located in of the south
Geosilof 14515.
France This
(700way
kmoffrom
de-
signing a process for PSS was confirmed by the industrial
the lab), and the global market in the ecoinvent database was adjusted accordingly. A producer.
FrenchGlass fiber: Previously
electricity introducedfor
mix was considered inglass
a formulation developed in the NAVIER labor-
fiber production.
atoryWollastonite:
and suitable for 3D printing
Wollastonite [36], glassisfibers
production were used in
not represented inour
thereference
ecoinventformulation.
database. It
The glass fiber
is usually a mined came fromalthough
stone, a Frenchitproducer located inproduced.
can be artificially the south Here,of France
only(700
openkm from
mining
the lab),
was and the using
considered, globalthe market
asbestosin the ecoinvent
chrysotile database
global was adjusted
production processaccordingly.
as a reference. A
Transport
French distances
electricity mix were
wasalso adjusted,for
considered asglass
the lab providers
fiber production.are located in Mexico.
Other raw materials:
Wollastonite: WollastoniteThe other constituents
production is not were directlyintaken
represented from the ecoinvent
the ecoinvent database.
3.7isdatabases.
It usually a mined If possible,
stone,data for the
although French
it can context were
be artificially taken.Here,
produced. When notopen
only available,
min-
Swiss
ing was (CH) or European
considered, using(RER) data were
the asbestos considered.
chrysotile global production process as a reference.
Transportation
Transport distances were of thealso matrix components:
adjusted, as the labThe transportation
providers are locatedprocess was directly
in Mexico.
extracted
Otherfrom raw the Ecoinvent
materials: The3.7 library
other databasewere
constituents without changes.
directly takenWe fromusedthethe EURO4
ecoinvent
class for all transportation vehicles (trucks). For PSS and
3.7 databases. If possible, data for the French context were taken. When not available, MK, distances between the
actual production sites and the NAVIER
Swiss (CH) or European (RER) data were considered. laboratory were calculated. The following driving
distances were estimated
Transportation of theusingmatrixGoogle Maps: The transportation process was directly
components:
•
extracted from the Ecoinvent
MK: Clérac—Champs sur3.7 library
Marne: 535database
km. without changes. We used the EURO4
•
class for all
PSS: transportation vehicles (trucks).
Ludwigshafen—Champs sur Marne: For504PSSkm.
and MK, distances between the actual
production sites and the NAVIER laboratory were calculated. The following driving dis-
tances were estimated using Google Maps:
For the supply of cement, sand, and gravel, distances were estimated. A distance
of 50 km was taken to account for displacement from the cement factory to the lab. This
estimated distance is about 30 km for the aggregates (sand and gravel).
As the GP mortar was synthesized at the laboratory scale, and given the small number
of required materials, it was considered that the vehicles used belonged to the 3.5–7.5 T
category, for MK, G, and aggregates. As the process for Ordinary Portland Concrete (OPC)
is more usual, 16–62 T lorries were considered for its transportation.
Electricity: The electricity consumption of the process was evaluated at 4 kWh per m3
of produced concrete or mortar. This value is an expert-based estimation for regular con-
crete provided by the French National Project RECYBETON (https://www.pnrecybeton.fr/
accessed on 11 April 2024). It should be studied in more depth and adapted to GPs in
further research. The French low-voltage market for electricity included in Ecoinvent v3.7.1
was chosen for the inventory.
2.3.3. Environmental Indicators

The main environmental issue usually related to traditional concrete and mortar is its
impact on climate change (CC). This environmental category is thus a major focus of this
study. Nevertheless, other impact categories (listed in Table 3) were examined to provide
an overview of the environmental profile of the GP technology and avoid impact shifting.
Table 3. Abbreviations and units of the environmental indicator used in this study.
Impact Category Abbreviation Unit

Climate Change Total CC kg CO2 -eq
Freshwater and Terrestrial Acidification FTA mol H+ -eq
Freshwater Ecotoxicity Fex CTUe
Freshwater Eutrophication Feu kg P-eq
Marine Eutrophication Meu kg N-eq
Terrestrial Eutrophication Teu mol N-eq
Carcinogenic Effects CE CTUh
Ionizing Radiation IR kg Bq U235
Non-Carcinogenic Effects nCE CTUh
Ozone Layer Depletion OD kg CFC-11-eq
Photochemical Ozone Creation POCP kg NMVOC eq
Respiratory Effects, Inorganics RE disease incidences
Resources, Dissipated Water DW m3 water deprived
Resources, Fossils RF Megajoule
Resources, Land Use RLU soil quality index—dimensionless
Resources, Minerals, and Metals RMM kg Sb-Eq
Cumulative Energy Demand CED MJ-Eq
The LCA was first performed using the European consensus set of environmental
indicators reached around the International Life Cycle Data initiative (ILCD). The midpoint
set of indicators from the methodology ILCD 2.0 2018 was used [46,47]. To give an overview
of the impact at the damage level to raise potential impact shifting among categories, a
second assessment was performed using the ReCiPe2016, hierarchist method [48].
Although the cumulative energy demand is sometimes depreciated by LCA experts
and seen as additional information more than a full LCA indicator [49], it was still added
to the midpoint indicators because of its very frequent use in the construction sector. This
set of impact categories aims to provide a comprehensive overview to avoid or at least
quantify the phenomena of pollution transfers and impact shifts.
3. Results
3.1. Environmental Impact Assessment of Elementary Processes of Geopolymer Mortars and
Reference Situation
In order to identify the parameters to be further optimized, a first environmental
assessment of the reference formulation (GP–GfW) was performed. The impact factors of
3.1. Environmental Impact Assessment of Elementary Processes of Geopolymer Mortars an
erence Situation
In order to identify the parameters to be further optimized, a first environmen
sessment of the reference formulation (GP–GfW) was performed. The impact fact
the elementary processes of the geopolymer production system used for the calcu
the elementary processes of the geopolymer production system used for the calculation
are available in Supplementary Materials, Section S2. The contribution analysis of th
are available in Supplementary Materials, Section S2. The contribution analysis of this
mulation is exposed in Figure 5. Although the additions (wollastonite and glass fibe
formulation is exposed in Figure 5. Although the additions (wollastonite and glass fiber)
are not negligible,negligible,
not the main
the main driver fordriver for environmental
environmental impact inimpact
most in most categories
categories is the is the
sium silicate solution (PSS), followed by the metakaolin and transport. The electricit
potassium silicate solution (PSS), followed by the metakaolin and transport. The electricity
tribution appears to be negligible
contribution appears to be negligible in this study.in this study.
Figure 5. Reference
Figuresituation for 3D-printing
5. Reference situation for geopolymer formulation.formulation.
3D-printing geopolymer CC = climate
CC =change,
climate change,
FTA = freshwaterfreshwater and terrestrial
and terrestrial acidification,
acidification, FEx = freshwater
Fex = freshwater ecotoxicity,
ecotoxicity, FEu = freshwater
Feu = freshwater eu- eutro
tion, Meu = marine eutrophication, TEu = terrestrial eutrophication, CE = carcinogenic
trophication, Meu = marine eutrophication, Teu = terrestrial eutrophication, CE = carcinogenic effect, effec
ionizing radiation, nCE = non-carcinogenic effects, OD = ozone depletion,
IR = ionizing radiation, nCE = non-carcinogenic effects, OD = ozone depletion, POCP = photo- POCP = photoch
ozone creation, RE = respiratory effects, DW = water depletion, RF = fossil resources, RMM =
chemical ozone creation, RE = respiratory effects, DW = water depletion, RF = fossil resources,
als and metals resources, CED = cumulative energy demand.
RMM = minerals and metals resources, CED = cumulative energy demand.
3.2. Optimization3.2.ofOptimization
the Geopolymer of the Geopolymer
Formulation Formulation
to Lower to Lower GHG Emissions
GHG Emissions
Based on the
Based on the preliminary LCApreliminary
results, theLCA results, the
optimization optimization
of the of the matrix
matrix is undertaken to is under
to lower
lower the quantity of PSSthe quantity
while of PSS while
maintaining maintaining
sufficient mechanicalsufficient mechanical
properties. properties. A f
A formulation
that lowers thelation
matrixthat lowersbythe
quantity matrix quantity
integrating a maximumby integrating
of sand and a maximum of sand
earth additions andand earth
tions and is suitable for the 3D-printing process was then
is suitable for the 3D-printing process was then developed and characterized mechanically. developed and charact
mechanically.
3.2.1. The Geopolymer Matrix
In order to3.2.1.
obtainThea Geopolymer Matrix
geopolymer formulation adapted for 3D printing with sufficient
compressive strength and low GHG emissions,
In order to obtain a geopolymer the geopolymer
formulation matrixfor
adapted was3Dfirst opti-with suffi
printing
mized. Different compressive strength and low GHG emissions, the geopolymer matrixawas first
ratios of metakaolin/potassium silicate solution were investigated with
metakaolin mass percentage
mized. Different ranging
ratios from 40 to 60%. The mechanical
of metakaolin/potassium silicatecurves
solutionobtained for
were investigated
a M50 S50 geopolymer
metakaolinare displayed in Figure
mass percentage 6a. This
ranging formulation
from 40 to 60%.exhibits a 60 ± 3 curves
The mechanical Mpa obtain
compressive strength
a M50S50and a brittle failure.
geopolymer The compressive
are displayed in Figurestrength
6a. Thisand the climate exhibits
formulation change a 60 ± 3
impact, expressed in kgCO eq/m 3 of the different geopolymer matrices are presented
compressive strength and a brittle failure. The compressive strength and the c
2
in Figure 6b. Thechangecompressive strength presents
impact, expressed in kgCO small variations but stays in the same
2eq/m3 of the different geopolymer matrice
order of magnitude (from 51 to 60 Mpa). When the metakaolin content increases from
40 to 50%, the compressive strength slightly increases due to enhanced polycondensation
reaction [50]. It then slightly decreases with a further increase in metakaolin content, from
50 to 60%, probably because of the presence of unreactive particles and a decrease in the
paste workability [51]. The climate change impact per m3 increases slightly with increased
presented in Figure 6b. The compressive strength presents small variations but stays in
the same order of magnitude (from 51 to 60 MPa). When the metakaolin content increases
from 40 to 50%, the compressive strength slightly increases due to enhanced polyconden-
Sustainability 2024, 16, 3328 sation reaction [50]. It then slightly decreases with a further increase in metakaolin con-
10 of 20
tent, from 50 to 60%, probably because of the presence of unreactive particles and a de-
crease in the paste workability [51]. The climate change impact per m3 increases slightly
with increased PSS content. Indeed, the PSS has a bigger impact per mass unit than me-
PSS content. Indeed, the PSS has a bigger impact per mass unit than metakaolin (0.63 and
takaolin (0.63 and 0.58 kgCO2eq/kg, respectively, for the M40S60 and M60S40 formulations).
0.58 kgCO2 eq/kg, respectively, for the M40 S60 and M60 S40 formulations). However, the
However,
density ofthe thedensity
matrixof the matrix
increases increases
with with theproportion
the decreased decreased proportion
of PSS which of PSS
leadswhich
to an
leads to an increase in impact per volume unit. Since the values of
increase in impact per volume unit. Since the values of climate change impact are climate change impact
of the
are of the
same ordersame order of magnitude,
of magnitude, the M50 S50the M50Spresenting
matrix 50 matrix presenting better mechanical prop-
better mechanical properties seems
erties
optimal. In terms of buildability, printing testsprinting
seems optimal. In terms of buildability, show that tests show
every thatgeopolymer
tested every testedmatrix
geo-
polymer matrix is
is not adapted fornot
3Dadapted
printingforbecause
3D printing because
the paste thewhen
flows paste flows
severalwhen several
layers layers
are stacked
are stacked during printing. Their yield stress has then to be increased
during printing. Their yield stress has then to be increased to improve the buildability, to improve the
buildability, which means to be able to carry the weight of the layers [52]. For
which means to be able to carry the weight of the layers [52]. For that purpose, it is possible that pur-
pose,
to addit is possible to add
reinforcement reinforcement
elements such as elements such
glass fibers or as glass fibers[38]
wollastonite or wollastonite
or to change[38]the
or to change the volume fraction by adding, for instance,
volume fraction by adding, for instance, sand or earth [53]. sand or earth [53].
(a) (b)
Figure 6. (a) Compressive curves of a M50 S50 geopolymer and (b) • compressive strength and ■
Figure
climate6.change
(a) Compressive
in kgCO2 eq/m 3 asof
curves a M50S50 of
a function geopolymer
metakaolinand (b)  compressive
percentage and 
strengthmatrix.
in the geopolymer
climate change in kgCO2eq/m as a function of metakaolin percentage in the geopolymer matrix.
3
3.2.2. The Geopolymer Mortar

3.2.2. In
The Geopolymer
order Mortar
to decrease the matrix quantity and increase the buildability, sand was added
to the different geopolymer
In order to decrease the matrices.
matrixTo define the
quantity andmaximum
increase quantity of sand tosand
the buildability, be added,
was
two thresholds were determined. The first threshold corresponds to
added to the different geopolymer matrices. To define the maximum quantity of sand the quantity of sand
to
foradded,
be whichtwo the thresholds
mortar begins
weretodetermined.
shear underThe mixing. After reaching
first threshold this threshold,
corresponds sand
to the quan-
wasofcontinuously
tity sand for whichadded to a point
the mortar beginswhere a vibrating
to shear needle After
under mixing. couldreaching
not fluidize the mix
this thresh-
anymore. The admissible range of sand quantity suitable for 3D printing
old, sand was continuously added to a point where a vibrating needle could not fluidize lies between
these
the mixtwo thresholds;
anymore. The before the first,
admissible rangetheofmortar is not stackable,
sand quantity suitableand after
for 3D the second,
printing the
lies be-
mortar is not pumpable. These two thresholds are presented in Figure 7a for
tween these two thresholds; before the first, the mortar is not stackable, and after the sec- the different
geopolymer binders. The thresholds are almost similar for a quantity of metakaolin ranging
ond, the mortar is not pumpable. These two thresholds are presented in Figure 7a for the
from 40 to 50% of the binder. With higher proportions of metakaolin, a saturation level is
different geopolymer binders. The thresholds are almost similar for a quantity of me-
reached, and the value of the second threshold decreases. In that range, the water coming
takaolin ranging from 40 to 50% of the binder. With higher proportions of metakaolin, a
from the silicate solution is not sufficient in the geopolymer matrices, and the amount of
saturation level is reached, and the value of the second threshold decreases. In that range,
sand it is possible to add decreases.
the water coming from the silicate solution is not sufficient in the geopolymer matrices,
To ensure that the geopolymer mortar formulations are mechanically reliable, the
and the amount of sand it is possible to add decreases.
compression strength of the M60 S40 geopolymer binder was measured. This is reported in
To ensure that the geopolymer mortar formulations are mechanically reliable, the
Figure 7b as a function of the quantity of added sand. The mechanical strength decreases
compression strength of the M60S40 geopolymer binder was measured. This is reported in
slightly from 51 ± 3 MPa without sand to 44 ± 2 MPa with the addition of sand (M60 S40 Sa60 ).
Figure 7b as a function of the quantity of added sand. The mechanical strength decreases
Consequently, the addition of sand to form a printable geopolymer mortar has no significant
effects on the properties of the material.
tototo
ymersadd
add
add totothe
per the
to GP
the
unit GP
ofGPmatrix.
matrix.
matrix.
volume. Moreover,
Moreover,
Moreover,
Nevertheless, the
the geopolymer
the impactformulations
geopolymer
geopolymer
their formulations
formulations
depends on thewith
with
withhigh
highsilicate
high
quantity silicate content
silicate
it content
content
is possible
(M(M(M
40
40SS60
40 Sax,
S
60 Sax,
60 M
Sax,M M
45
45SS55
45 SSax,
55 Sax,
55 M
Sax, M M
40 S
40S60
40SSax)
60 Sax)
60 have
Sax)have
haveclimate
climate
climatechange
change
changeimpacts
impacts
to add to the GP matrix. Moreover, the geopolymer formulations with high silicate content impacts lower
lower than
lowerthan 3D-printed
than3D-printed
3D-printed con-
con-
con-
crete
(M crete
crete (529
(529
40S60Sax, kgCO
(529MkgCO
kgCO eq/m
2eq/m
45S55Sax,
2 2eq/m
3)3 or
M)40or
3 )S60generic
generic
orSax)generic mortar
have mortar
mortar (393
climate(393 kgCO
(393kgCO
kgCO
change 2 eq/m
2eq/m
2eq/m
impacts 3)3 while
) lower
3while keeping
keeping
) whilethan
keepingsufficient
sufficient
sufficient
3D-printed me-
me-
con- me-
chanical
crete (529properties
chanical
chanical properties
properties
kgCO 2eq/m (above
(above
3)(above 40
or generic4040MPa).
MPa).
MPa).These
These
mortar These formulations
(393formulations
formulations
kgCO2eq/m can
can
3)can then
then
while be
then selected
bebeselected
selected
keeping tototo
sufficientprogress
progress
progress
me-
Sustainability 2024, 16, 3328 toward
toward
toward
chanical aproperties
asustainable
asustainable
sustainable material
(abovematerial
material for
40 MPa). for3D
3D
for 3Dprinting.
printing.
printing.
These formulations can then be selected to progress 11 of 20
toward a sustainable material for 3D printing.
(a)
(a)(a) (b)
(b)(b)
(a) (b)
(c)
(c)(c)
(c)
Figure
Figure
Figure7.7.(a) quantity
7.(a)(a) quantity
quantityofofsand
ofsand added
sandadded
added different
inindifferent
indifferent
different geopolymer
geopolymer
geopolymer matrices
matrices
matrices with
with the
with the( ()
()
the )()
printable
printable domain
printable domain
domain
between
between
between the
the
the 
the  
first
firstand
first and
and
first 
and  
second
second thresholds
second
second thresholds
thresholds
thresholds (b)
(b) quantity
(b)
quantity
(b) quantity of
quantity of sandof
sand
of sandas
as
Figure 7. (a) quantity of sand added in different geopolymer matrices with the () printable domain a
sanda
asfunction
as a
function
a function of
ofcompressive
function
of of strength
compressive
compressive
compressive strength
strength
for
foran
for
strength
between MM
anan M
for
60
the SS40
60 an
6040 formulation
formulation
Sfirst
40 and
60
and
second and
S40 formulation
Mformulation (c)
and quantity
(c)(c)
quantity
quantity
and
thresholds ofof
(c)(b) kgCO
ofkgCO
kgCO
quantity
quantity /m
2of2/m
of
3 3for
/m
2kgCO for the
2the
3 for
sand /m
as asecond
the3second
second
for threshold
the
function threshold
threshold
second
of mortar
mortar formula-
mortar
threshold
compressive formula-
formula-
mortar
strength
tions.
fortions.
tions.
an M
formulations.
60 S 40 formulation and (c) quantity of kgCO 2 /m 3 for the second threshold mortar formula-
tions.
The value of climate change impact per volume unit (kgCO2 eq/m3 ) was then calcu-
lated for mortar formulations at the second threshold and is reported in Figure 7c. The
climate change impact decreases slightly with a decrease in silicate solution until it reaches
an optimum at 316 kgCO2 eq/m3 for the M50 S50 Sa191 formulation. It increases afterward.
This optimum can be explained by two phenomena: (i) the silicate solution has a big
impact on climate change and (ii) the formulation that contains a high quantity of silicate
solution allows us to add more sand, which decreases the final impact. The impact of the
M50 S50 Sa191 formulation is 3.7 times lower than the (M50 S50 ) matrix impact. The addition
of sand in the geopolymer formulation then drastically decreases the climate change impact
of geopolymers per unit of volume. Nevertheless, their impact depends on the quantity
it is possible to add to the GP matrix. Moreover, the geopolymer formulations with high
silicate content (M40 S60 Sax, M45 S55 Sax, M40 S60 Sax) have climate change impacts lower
than 3D-printed concrete (529 kgCO2 eq/m3 ) or generic mortar (393 kgCO2 eq/m3 ) while
keeping sufficient mechanical properties (above 40 MPa). These formulations can then be
selected to progress toward a sustainable material for 3D printing.
3.2.3. Optimization with Earth Addition

After optimizing the geopolymer formulation through the addition of sand, tests were
conducted using the mix of earth and sand determined in Figure 1. This mix was added
added in a 1:1 mass proportion with an M50S50 geopolymer matrix to obtain a printable
material (M50S50Sa66E34). The printability and buildability of this formulation were tested
with a manual extrusion tool, as shown in Figure 8a. As shown in previous work [38], this
preliminary test provides an indication of the buildability of the material.
Sustainability 2024, 16, 3328 The tested formulation presents a compressive strength equal to 31 ± 4 MPa. This is
12 of 20
lower than the geopolymer matrix due to the earth’s inclusion (Figure 8b) and a modifi-
cation of the polycondensation reaction. However, it is still acceptable for construction
applications.
in a 1:1 massThese results with
proportion showanthat
M50the
S50optimization
geopolymer of the granular
matrix to obtainskeleton allows
a printable us
material
to (M
add Slocal earth into the formulation to improve the circular economy while keeping
50 50 Sa66 E34 ). The printability and buildability of this formulation were tested with
sufficient
a manual mechanical
extrusionproperties and obtaining
tool, as shown in Figurea 8a.
mix As
adapted
shownforin3D printing.
previous work [38], this
preliminary test provides an indication of the buildability of the material.
Figure 8. Photos of (a) printed layers of the earth–sand–M50S50Sa66E34 mix extruded with a manual
tool and
Figure 8. Photos of ×
(b) a 40 × 160 mm
(a)40printed sample.
layers of the earth–sand–M50S50Sa66E34 mix extruded with a man-
ual tool and (b) a 40 × 40 × 160 mm sample.
The tested formulation presents a compressive strength equal to 31 ± 4 MPa. This
is Comparison
3.3. lower than of the
thegeopolymer matrix dueFormulation
Optimized Geopolymer to the earth’s
withinclusion (FigureMaterials
Other Printing 8b) and a modi-
fication
The environmental performance of the optimized formulations as printingconstruction
of the polycondensation reaction. However, it is still acceptable for materials
applications. These results show that the optimization of the granular skeleton allows us
was assessed in a comparative approach at a material scale. The robotic process necessary
to add local earth into the formulation to improve the circular economy while keeping
to print the material [54–56] was excluded from the scope of the study. The formulation
sufficient mechanical properties and obtaining a mix adapted for 3D printing.
with the addition of sand (M50S50Sa191—GP-S) and the formulation with the addition of
earth
3.3. and
Comparison S50Sa
sand (Mof50the 66E34)—GP-SE) were compared to two other 3D-printing formu-
Optimized Geopolymer Formulation with Other Printing Materials
lations—one based on Portland cement [54], named 3DCM, and one based on a geopoly-
The environmental performance of the optimized formulations as printing mate-
mer [36], with glass fibers and wollastonite additions (GP–GfW). The four formulations
rials was assessed in a comparative approach at a material scale. The robotic process
are summarized in Table 4.
necessary to print the material [54–56] was excluded from the scope of the study. The
formulation with the addition of sand (M S Sa —GP-S) and the formulation with
Table 4. Formulation of the 3D-printing mortars. 50 50 191
the addition of earth and sand (M50 S50 Sa66 E34 )—GP-SE) were compared to two other
3D Cement Mortar—
3D-printing formulations—one GP Mortar
based on Portland cement [54], named 3DCM, and one
Quantity Quantity GP Mortar «GP–S» GP Mortar «GP–SE»
«3DCM» based on a geopolymer «GP–GfW»
[36], with glass fibers and wollastonite additions (GP–GfW). The
(in kg/m3) (in kg/m )
3 (Section 3.2.2) (Section 3.2.3)
[54] four formulations are summarized [36] in Table 4.
OPC 540 MK 915.4 327.4 505
Silica Fume 480 Table 4. Formulation
PSS of the 3D-printing
736.3 mortars. 327.4 505
Sand 1033 Sand 0 1248.8 666.6
Water 3D Cement
212 Mortar— Wollastonite GP Mortar
298.5 0 0 «GP–SE»
Quantity Quantity GP Mortar «GP–S» GP Mortar
«3DCM» «GP–GfW»
(in kg/m3 )
Accelerator 6 Glass kg/m3 )
(infibers 39.8 0
(Section 3.2.2) 0
(Section 3.2.3)
[54] [36]
Plasticizers 8.8 Steamed earth 0 0 333.3
OPC 540 MK 915.4 327.4 505
Silica Fume 480 ConsideringPSS 736.3
the Portland cement-based 327.4most upstream requirements
mortar 3DCM, 505
Sand 1033are accounted forSand
in the market processes
0 of the ecoinvent databases. Electricity
1248.8 consump-
666.6
Water 212
tion for the 3D cement
Wollastonite
mortar was added
298.5
considering 40
kWh/m 3 and transport is also
0
Accelerator 6 Glass fibers 39.8 0 0
Plasticizers 8.8 Steamed earth 0 0 333.3
Considering the Portland cement-based mortar 3DCM, most upstream requirements

are accounted for in the market processes of the ecoinvent databases. Electricity consump-
tion for the 3D cement mortar was added considering 4 kWh/m3 and transport is also
accounted for, using the process “market for concrete, 50 MPa, global” contextualized to
Europe. The 4 scenarios are considered to have equivalent properties in terms of mechanical
resistance, pumpability and extrudability, making them suitable for 3D printing in the
Sustainability 2024, 16, x FOR PEER REVIEW 13
Sustainability 2024, 16, 3328 accounted for, using the process “market for concrete, 50 MPa, global” contextualiz
13 of 20
Europe. The 4 scenarios are considered to have equivalent properties in terms of me
ical resistance, pumpability and extrudability, making them suitable for 3D printing
perspective of structural uses. Relative results are provided for a clearer interpretat
perspective of structural uses. Relative results are provided for a clearer interpretation of
the results, 3D cement mortar (3DCM) being the reference/denominator (Figure 9).
the results, 3D cement mortar (3DCM) being the reference/denominator (Figure 9).
Figure 9. LCA ofFigure

GP-S and GP-SE
9. LCA mortar,
of GP-S andcompared to 3DCM
GP-SE mortar, (used as
compared to reference,
3DCM (used fixed
as at 100%) and
reference, fixed at 100%
GP–GfW (log scale).
GP–GfW (log scale).
With the currently

With tested formulations
the currently and in a French
tested formulations and incontext,
a French thecontext,
resultstheshow
results show
that the GP formulations present impacts equivalent to or higher than
the GP formulations present impacts equivalent to or higher than 3DCM,3DCM, except for except f
climate change,mate
for which GP-S has a lower impact ( − 23%). Secondly, the GP-S
change, for which GP-S has a lower impact (−23%). Secondly, the GP-S and G and GP-
SE perform significantly better than better
perform significantly the previous
than theformulation with a higher
previous formulation withshare of the
a higher share of th
matrix (GP–GfW). However, GP-SE does not perform better than GP-S due to
trix (GP–GfW). However, GP-SE does not perform better than GP-S due to a higher m a higher
matrix proportion. The climate
proportion. The change
climateimpact
changeofimpact
geopolymer mortar highly
of geopolymer mortar depends
highly on its
depends on it
formulation—whether by the nature or quantity of its raw material or by the optimization
mulation—whether by the nature or quantity of its raw material or by the optimizat
of the granularthe
skeleton.
granular skeleton.
Figure 10 shows the 10
Figure important
shows the contribution of transportation
important contribution of the material
of transportation of theformaterial f
GP mortar: from 7 to 47% according to certain categories (28% on average).
mortar: from 7 to 47% according to certain categories (28% on average). The same
The same fi
figures for 3DCM vary from
for 3DCM vary4from
to 42%
4 to(16%
42% on average).
(16% This is
on average). related
This to the
is related tolab-scale
the lab-scale and
and poor development of production sites for kaolinite. Another source of improvement
development of production sites for kaolinite. Another source of improvement c
clearly stands in the material
stands production
in the material itself: PSS
production and
itself: PSSMK andproductions
MK productions are significant
are significant co
contributors to utors
most to
categories, and further
most categories, and research should investigate
further research the improvement
should investigate the improvement
of the production process, especially
production on toxicity-related
process, especially impacts for
on toxicity-related PSS. Further
impacts for PSS.effort to effort t
Further
decrease the needed matrix quantity would also be very efficient as it will decrease
crease the needed matrix quantity would also be very efficient as it will decrease both
impacts from production
impacts from andproduction
transport. and transport.
Figure 11 shows the contribution of different environmental issues to damage to hu-
man health, biodiversity, and resources, using the ReCiPe2016 method endpoint level. If
climate change clearly dominates human health, other categories are not negligible, such
as toxicity (cancer and non-cancer) and particulate matter (which can be associated with
“respiratory effects”). On the biodiversity side, global warming dominates, followed by
terrestrial acidification, photochemical ozone formation, and land use. A multi-criteria
assessment is therefore essential to clearly prove the environmental relevance of the tech-
nology, restricting the evaluation to carbon footprint is not sufficient and could lead to
impact shifting.
Figure 10. Contribution analysis

Figure 10. of GP-SE
Contribution mortar.of GP-SE mortar.
analysis
100% 100% 100%
Figure 11 shows the contribution of different environmental issues to damage
90% 90%
man health, biodiversity, and resources, using the ReCiPe2016 method endpoint le
80% 80%
climate change clearly dominates human health,80% other categories are not negligible
70% 70%
as toxicity (cancer and non-cancer) and particulate matter (which can be associated
60% 60%
“respiratory effects”). On the biodiversity side,60% global warming dominates, follow
50% terrestrial acidification,
50% photochemical ozone formation, and land use. A multi-crite
40% sessment is therefore
40% essential to clearly prove 40% the environmental relevance of the
30% nology, restricting
30% the evaluation to carbon footprint is not sufficient and could le
20% impact shifting.20% 20%
10% Results for10%the GP materials are largely hampered by scale factors, as we com
0%
a lab-scale technology to a fully deployed technology that has benefited from many
0% 0%
of innovation
Human Health and improvements, and its small-scale production
Biodiversity units are close to
Ressources
users. Consequently, these direct results are to be taken with caution. A scale-up of t
Other (IR+OD+PhO)
technology will helpOther (Eu+EcoTx+Water)
assess its long-term potential. It should cover both the possible
Water mization of the geopolymerOzone Phelaboration process (equipment efficiency,
Mineral resource raw material
scarcity
Human toxicity
the overall value chainTerrestrial Acidification
(optimization of transport type and distance). This is a majo
Particulate matter of this workLand
spective anduse Fossil resource
is further detailed in the Section 4. scarcity
Global warming Global warming
Figure 11. Midpoint contribution to Endpoint for GP-S concrete, Human Health (left), Biodiversity
Figure(right)
(center), and resource 11. Midpoint contributionhierarchist
using ReCiPe2016, to Endpoint for GP-S concrete, Human Health (left), Biodi
method.
(center), and resource (right) using ReCiPe2016, hierarchist method.
Results for the GP materials are largely hampered by scale factors, as we compared a
lab-scale technology to a fully deployed technology that has benefited from many years
4. Discussion
of innovation and improvements, and its small-scale production units are close to final
4.1. Value Chain Optimization
users. Consequently, these direct results are to be taken with caution. A scale-up of the
The developed process is currently an under-optimized laboratory process com
GP technology will help assess its long-term potential. It should cover both the possible
to well-established conventional
optimization of the geopolymer elaboration materials
process such as
(equipment concreteraw
efficiency, mortars. This explain
materials)
the impact of transport is so high compared to 3DCM. To account for
and the overall value chain (optimization of transport type and distance). This is a majorthis bias, a sens
analysis was performed on transport type and
perspective of this work and is further detailed in the Section 4. transport distances; first, we imp
transport to 16–32 T EURO6 lorries (scenario T++) and secondly, we decreased tran
distances from 500 km to 50 km for MK and PSS (scenario T++D−). The results ar
sented in Figure 12 below, which provides a selection of seven indicators among the
important ones according to the endpoint assessment.
There is great room for improvement, which could be made thanks to the scale
This limited analysis based on only two parameters should be further investigated t
duce full scale-up scenarios, focusing both on process optimization and distributio
tions. Process improvements can be obtained thanks to bigger and more efficient e
4. Discussion
4.1. Value Chain Optimization
The developed process is currently an under-optimized laboratory process compared
to well-established conventional materials such as concrete mortars. This explains why the
impact of transport is so high compared to 3DCM. To account for this bias, a sensitivity
analysis was performed on transport type and transport distances; first, we improved
transport to 16–32 T EURO6 lorries (scenario T++) and secondly, we decreased transport
distances from 500 km to 50 km for MK and PSS (scenario T++D−). The results are
Sustainability 2024, 16, x FOR PEER REVIEW 16 of
presented in Figure 12 below, which provides a selection of seven indicators among the
most important ones according to the endpoint assessment.
Figure 12. Assessment of the reference lab process and scale-up scenarios, midpoint level, considering
Figure 12. Assessment of the reference lab process and scale-up scenarios, midpoint level, conside
3DCM mortar as a ing
baseline
3DCMscenario.
mortar as a baseline scenario.
There is great room

4.2. forOptimization
Matrix improvement, which could be made thanks to the scale effect.
This limited analysisThebased on only matrix
geopolymer two parameters
formulationshould be further
was selected basedinvestigated to
on its mechanical perfo
produce full scale-up
mancescenarios, focusing
and its climate change both on process
impact. optimization
This procedure and
could be distribution
further deployed to evalu
options. Process improvements
ate candidates incanall be obtained thanks
environmental impactto categories.
bigger andThe more efficient
authors wantequip-
to highlight th
ment, such as MK flash calcination
methodology set up to[57,58],
develop a change in energy
the geopolymer, suppliers,
which or a change
is simplified in
and restrained to on
PSS suppliers. Distribution options
single indicator in the could involve
first step the use of
for readability. alternative
They acknowledgeraw the
materials
importance of th
such as low-kaolinite metakaolin
multi-criteria that could
approach be produced from clays with a high content of
in LCA.
kaolinite [59]—an abundant
The LCA resource
results often available
also showed locally
that in France [60].
the formulation with Freight by train
sand (GP-S) exhibits bette
or by barge couldresults
also bethan the formulation
envisioned to furtherwithdecrease
earth (GP-SE). Theimpacts.
transport use of locally
Thisexcavated
representsearth could
however,
an important research be beneficial
perspective as awork.
of this strategy to reduce impacts related to the extraction of sand i
the context of aggregate scarcity and a lack of environmental regulation [7,8].
4.2. Matrix Optimization
Moreover, the use of sodium instead of potassium in the alkaline solution could als
produce
The geopolymer geopolymers
matrix formulationsuited
wasfor structural
selected applications
based while reducing
on its mechanical both the cost an
performance
the environmental burden [9]. Other synthesis processes could be investigated in a futur
and its climate change impact. This procedure could be further deployed to evaluate
study to use broadly available potash salts instead of potassium hydroxide in the confe
candidates in all environmental impact categories. The authors want to highlight the
tion of potassium silicate solution (waterglass).
methodology set up to develop the geopolymer, which is simplified and restrained to one
Finally, the printability of the formulation has been measured in a simple way, eve
single indicator in
if the first
better step for
methods readability.
exist, They acknowledge
like the squeeze the importance
test [61] or modified Vicat [62],offor
theinstance. I
multi-criteria approach in LCA.
[63], we developed an original and efficient in-line test for 3D concrete, the slug test, whic
The LCA results
is ablealso showed
to deduce thethat
yield the formulation
stress with sand
from the weight (GP-S)
of drops exhibits
falling better
from the nozzle, whic
results than the formulation with earth (GP-SE). The use of locally excavated earth could,
directly relies on the printability. In [36], we successfully adopted this method for the GP
GfW geopolymer used in this study for comparisons, and future tests will be conducte
for the formulations integrating earth, to confirm their printability.
4.3. Uncertainties
Uncertainty values are high, as the data suffers from some severe flaws, especially i
foreground processes. The estimation of this uncertainty is a critical issue for comprehen
however, be beneficial as a strategy to reduce impacts related to the extraction of sand in

the context of aggregate scarcity and a lack of environmental regulation [7,8].
Moreover, the use of sodium instead of potassium in the alkaline solution could also
produce geopolymers suited for structural applications while reducing both the cost and
the environmental burden [9]. Other synthesis processes could be investigated in a future
study to use broadly available potash salts instead of potassium hydroxide in the confection
of potassium silicate solution (waterglass).
Finally, the printability of the formulation has been measured in a simple way, even if
better methods exist, like the squeeze test [61] or modified Vicat [62], for instance. In [63],
we developed an original and efficient in-line test for 3D concrete, the slug test, which is
able to deduce the yield stress from the weight of drops falling from the nozzle, which
directly relies on the printability. In [36], we successfully adopted this method for the GP–
GfW geopolymer used in this study for comparisons, and future tests will be conducted for
the formulations integrating earth, to confirm their printability.
4.3. Uncertainties
Uncertainty values are high, as the data suffers from some severe flaws, especially in
foreground processes. The estimation of this uncertainty is a critical issue for comprehensive
LCA results [64]. For PSS, the data on potassium are inexistent, following an existing trend
in the chemical industry [65]. The values for alkali silicates come from a 25-year-old
study from Fawer and colleagues [45], as is the case in the vast majority of other LCA
studies such as [19,22,66]. It strongly affects the temporal and technological correlation
parameters and consequently gives high uncertainty to the related process. For MK, the
material comes from widely different processes, and a high variability is observed in the
literature [19,22,66]. Consequently, the technological correlation is low. Furthermore, an
uncertainty assessment is not explained in this article, although it is considered to be a
major perspective of this work.
The uncertainty related to the freshwater ecotoxicity indicator will hopefully soon be
reduced with ongoing work on improving the characterization factor of metals. In the mean-
time, this result has to be taken with caution. For instance, the most important contributing
elementary flows differ between the ILCD and Impact World+ indicators [67], with ques-
tions on both results and the overall contribution of this category in the environmental
assessment of GP mortar.
4.4. Damage Assessment Method

As endpoint characterization methods are subject to higher uncertainties than the
midpoint, a sensitivity analysis was performed using another method: ImpactWorld+ [67].
The results significantly differ, especially for biodiversity assessment and the contribution
of long-term effects regarding freshwater ecotoxicity, which clearly dominates the Impact-
World+ results. This impact category is subject to very high uncertainties, and this result
is the consequence of only a few compounds highly persistent in the environment. Here,
these are aluminum, copper, and iron, which come from upstream secondary processes
related to sulfidic tailing from copper production. There is an important debate on ecotoxi-
city characterization factors for metals, which could eventually lead to a decrease in their
contribution by at least two orders of magnitude [68,69]. There is also a current debate on
the possible overestimation of tailing releases to the environment [70]. Excluding long-term
effects to avoid this metal issue, the dominant category is climate change, closely followed
by land use (related to transport) and acidification. Details on stressor contribution to
freshwater ecotoxicity impacts are available in Supplementary Materials, Section S3.
The ReCiPe2016 method, a hierarchist scenario, used in this work does not consider
the long-term effects of ecotoxicity (over 100 years), which could potentially lead to an un-
derestimation of the impacts of very persistent compounds. However, stressor contribution
results were consistent with the ILCD method used for midpoint assessment. Uncertain
impacts must be assessed even if uncertain and ongoing important research efforts might
soon lead to a better comprehension of occurring phenomena and a reduction of related

uncertainties and variations among models.
4.5. Comparative LCA with 3D Printing Mortar Based on OPC

For simplicity reasons, the choice of a conventional equivalent was based on concrete
with 100% OPC. Although 100% OPC is still widely used, a wide range of alternative clink-
ers have been developed [71]. It would be highly consistent to further include the proposed
geopolymer in a wider perspective, comparing it to a wide scope of 3D-printing materials.
5. Conclusions and Perspective

The research presented in this paper focuses on geopolymer compositions iteratively
developed for structural applications, with the goal of lowering the environmental impact.
An LCA model for MK- and PSS-based geopolymer mortars was built. This model was
used to optimize the GP matrix and granular skeleton starting from an existing formulation,
through the reduction of GHG emissions. Two optimized formulations of GP mortars
suitable for 3D printing were then compared with a 3D-printed mortar based on Portland
cement. The results were completed by a sensitivity analysis of the transport of raw
materials. The conclusions of this LCA show that 3D-printed GP formulations are not yet
a mature technology, and short-term applications of this technology are not necessarily
environmentally beneficial. Nevertheless, GPs hold great potential as they can divide GHG
emissions by a factor close to two, with conceivable innovations. In the meantime, human
and environmental toxicities, mineral depletion, and fossil resources are increased by the GP
mortars—a trade-off already underlined by previous studies. The designed material shows
good extrudability and buildability and could be used in high-performance applications
thanks to its high compressive strength. Despite its low proportion of aggregates, this
material displays significant environmental assets as it contains an important share of earth
that is widely available and often treated as waste.
Some other prospective works lie ahead and are worth exploring. First, there is a need
for a prospective resource-availability assessment for the GP technology (alkali, kaolin
clays) to ensure that the required resources are widely available or to define locations that
could most benefit from the technology. Secondly, an environmental assessment of the large-
scale use of 3D printing in building applications must be conducted, as the literature is still
scarce. A robust uncertainty assessment should be undertaken with rigorous sampling for
processes specific to geopolymers. Furthermore, the social impact of such a new technique
is also worth exploring before its wider application.
Supplementary Materials: The following supporting information can be downloaded at: https://www.
mdpi.com/article/10.3390/su16083328/s1. Section S1: Process of Detailed Modelization; Section S2:
Impact Categories; Section S3: LCA Results: Stressor Contribution to Ecotoxicity.
Author Contributions: C.R.: Conceptualization, Writing—Original draft preparation, visualization,
validation—environmental assessment part; J.A.: Conceptualization, Writing—Original draft prepa-
ration, Visualization, validation—mechanical and workability characterization part; C.L.G.: Concep-
tualization, Methodology, Investigation, Software; M.S.: Writing—Original draft preparation, Critical
Review and Editing, A.F.: Writing—Review and Editing, supervision; J.-F.C.: Writing—Review and
Editing, supervision, Project administration, funding acquisition. All authors have read and agreed
to the published version of the manuscript.
Funding: This work was performed using the funds of the NAVIER research lab.
Informed Consent Statement: Not applicable.
Data Availability Statement: Data is contained within the article or Supplementary Materials. A
dataset for more detailed information is available on request from the authors.
Conflicts of Interest: The authors declare no conflicts of interest.
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1 MINES Paris—PSL Research University, CEEP (Centre Energie Environnement Procédés),

Citation: Roux, C.; Archez, J.; Le Gall,

Sustainability 2024, 16, 3328. https://doi.org/10.3390/su16083328 https://www.mdpi.com/journal/sustainability

an ambient temperature through the activation of an aluminosilicate source (i.e., metakaolin)

Geopolymer (GP) GHG Emissions of GHG Emissions of Ref.

The objective of this paper is to propose a formulation for a low-environmental-impact

2. Materials and Methods

2.3.2. Life Cycle Inventory of Individual Processes

2.3.3. Environmental Indicators

Impact Category Abbreviation Unit

3.2.2. The Geopolymer Mortar

3.2.3. Optimization with Earth Addition

Considering the Portland cement-based mortar 3DCM, most upstream requirements

Figure 9. LCA ofFigure

With the currently

Sustainability 2024, 16, x FOR PEER REVIEW 1

Figure 10. Contribution analysis

There is great room

however, be beneficial as a strategy to reduce impacts related to the extraction of sand in

4.4. Damage Assessment Method

soon lead to a better comprehension of occurring phenomena and a reduction of related

4.5. Comparative LCA with 3D Printing Mortar Based on OPC

5. Conclusions and Perspective

58. Deteuf, C. Imerys Metakaolin Production.pdf. 2016. Available online: https://geopolymer.org/fichiers/gpcamp-2016/Deteuf%

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