Construction and Building Materials 151 (2017) 1827

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Construction and Building Materials

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

Recycled glass as a supplementary filler material in spent coffee grounds

geopolymers
Arul Arulrajah a,, Teck-Ang Kua a, Suksun Horpibulsuk b,a,, Mehdi Mirzababaei c, Avirut Chinkulkijniwat d
a
Department of Civil and Construction Engineering, Swinburne University of Technology, Hawthorn, Victoria 3122, Australia
b
School of Civil Engineering and Center of Excellence in Innovation for Sustainable Infrastructure Development, Suranaree University of Technology, Nakhon Ratchasima
30000, Thailand
c
School of Engineering and Technology, Central Queensland University, 120 Spencer Street, Melbourne, Victoria 3000, Australia
d
School of Civil Engineering and Center of Excellence in Civil Engineering, Suranaree University of Technology, Nakhon Ratchasima 30000, Thailand

h i g h l i g h t s

 Recycled glass (RG) evaluated as a supplement to spent coffee ground (CG) geopolymers.
 RG provides mechanical and chemical strength supplementation to CG geopolymer.
 Heat-treated activated RG + CG geopolymers can achieve 10 MPa at 7-days compressive strength.

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

Article history: Recycled glass (RG) is a demolition waste, rich in silica and with a high shear strength and has been used
Received 26 April 2017 as a replacement material for sand in various construction applications. Spent coffee grounds (CG) is a
Received in revised form 6 June 2017 waste material derived from brewing coffee and has been recently studied as a recycled construction
Accepted 8 June 2017
material, due to its physical resemblance to sandy soils. Geopolymerization, is a green process which pro-
duces cementitious compounds using aluminosilicate-rich materials and alkaline liquids. In this research,
a new geopolymer construction material was produced using RG as a supplementary filler material to
Keywords:
stabilize CG. Fly ash (FA) and slag were used as the precursors to induce geopolymerization in this
Construction
Glass
new RG + CG construction product. To maximize the potential strength of the geopolymer, fine RG was
Coffee grounds added into geopolymer mixes in proportions of 25%, 50%, and 75% to observe the effects on the final
Geopolymer RG + CG product strength. The mixes were compressed into cylindrical specimens, cured at room temper-
Recycling ature (i.e., 21 C) and 50 C for 7 and 28 days, and tested for their unconfined compressive strength (UCS)
to observe the effect of the various RG replacement ratio on the strength of CG geopolymers. Scanning
electron microscopy (SEM) and Energy-dispersive X-ray spectroscopy (EDS) were used to further explain
the role of RG in influencing strength development. Higher RG contents were found to lead to higher UCS
values. A lower liquid-to-precursor (L/P) ratio was required to achieve a saturation point in strength
development. RG was found to provide mechanical strength and supplementary chemical bonding
strengths by dissolving and contributing Si+ ions to form geopolymeric substances.
2017 Elsevier Ltd. All rights reserved.

1. Introduction to hold liquid, and as a construction material in building facades,

Glass is an amorphous solid which constitutes largely of silica
(SiO2) [1]. It is widely used to make containers, beakers, and bottles
Corresponding authors at: Department of Civil and Construction Engineering,
Swinburne University of Technology, P.O Box 218, Hawthorn, Victoria 3122,
Australia (A. Arulrajah). School of Engineering, Suranaree University of Technology,
Nakhon Ratchasima 30000, Thailand (S. Horpibulsuk).
E-mail addresses: aarulrajah@swin.edu.au (A. Arulrajah), suksun@g.sut.ac.th
(S. Horpibulsuk).
doors and windows due to its transparent nature, which allows
maximum sunlight into a building. Glass is an easily recyclable
product which can be crushed, melted and then remolded into var-
ious shapes and sizes [2]. However, currently large quantities of
used glass are either landfilled or stockpiled for future use because
current logistics and recasting technologies do not result in an eco-
nomical nor efficient glass recycling process [3]. On the other hand,
other wastes containing silica are widely recycled. For example,
post-consumer glassware can be ground, mixed with foaming
agents, and heated to produce a porous foamed-glass which is

http://dx.doi.org/10.1016/j.conbuildmat.2017.06.050
0950-0618/ 2017 Elsevier Ltd. All rights reserved.
 A. Arulrajah et al. / Construction and Building Materials 151 (2017) 1827 19

Table 1
Test plan for the strength assessment of RG + CG geopolymers.

Test type RG:CG:P (by dry mass) Na2SiO3: NaOH L/P (by mass) Curing temperature (C) Curing duration (days)
Modified proctor compaction 20RG:50CG:30FA 70:30 0.8, 1.0, 1.2, 1.4, 1.6 N/A N/A
35RG:35CG:30FA 70:30 0.4, 0.6, 0.8, 1.0, 1.2 N/A N/A
50RG:20CG:30FA 70:30 0.2, 0.4, 0.6, 0.8, 1.0 N/A N/A
20RG:50CG:30S 70:30 0.8, 1.0, 1.2, 1.4, 1.6 N/A N/A
35RG:35CG:30S 70:30 0.4, 0.6, 0.8, 1.0, 1.2 N/A N/A
50RG:20CG:30S 70:30 0.2, 0.4, 0.6, 0.8, 1.0 N/A N/A
UCS 20RG:50CG:30FA 70:30 0.8, 1.2, 1.6, 2.0 21, 50 7, 28
35RG:35CG:30FA 70:30 0.6, 1.0, 1.4, 1.8 21, 50 7, 28
50RG:20CG:30FA 70:30 0.4, 0.8, 1.2, 1.6 21, 50 7, 28
20RG:50CG:30S 70:30 0.8, 1.2, 1.6, 2.0 21, 50 7, 28
35RG:35CG:30S 70:30 0.6, 1.0, 1.4, 1.8 21, 50 7, 28
50RG:20CG:30S 70:30 0.4, 0.8, 1.2, 1.6 21, 50 7, 28

Fig. 1. SEM images of: (a) RG, (b) CG, (c) FA, and (d) Slag.

Table 2 (RG) in a number of construction activities. Medium and fine sized

Chemical composition of RG, FA, and Slag by XRF analysis. RG particles have been found to possess high shear strengths [7],
Chemical composition (%) RG CG FA Slag suitable for use as a recycled material in construction applications
SiO2 83.57 N.D. 75.45 35.21
such as embankment fills [8,9], masonry units [1012], and earth
Al2O3 2.43 N.D. 12.01 13.09 retaining structures [13]. Sand-sized RG can also be used as a fine
Fe2O3 0.86 4.13 3.96 0.45 aggregate, and has been previously bound with a fly ash geopoly-
CaO 12.53 32.15 2.72 43.55 mer to produce masonry units with a recorded 3-days UCS of
MgO N.D. N.D. N.D. 5.93
12 MPa [14]. Powdered RG was found to be a good pozzolan which
SO3 0.28 N.D. 0.78 0.85
K2O 0.33 45.31 2.97 0.92 may be used to potentially replace cement because of the large
TiO2 N.D. 18.41 N.D. N.D. total exposed surface which enables silica to be readily leached
by alkaline solutions [15,16]. However, the main concern with
N.D. = Not Detected.
using RG as a supplementary cementing agent or construction
material, is the alkali-silica reaction between the alkali found in
light-weight and possesses significant load-bearing strength [4]. concrete and alkaline activator liquids and the silica in RG.
Another example is silica fume, the by-product of silicon and Alkali-silica reaction is an expansive reaction which cracks con-
silicon-alloy manufacturing, is a waste product associated with cretes and reduces mortar durability, but using ground or pulver-
glass and is used as a supplementary cementing agent for concrete ized RG significantly minimizes the occurrence of alkali-silica
due to its high silica content [5]. reaction [17].
In Australia, approximately 1 million tons of waste glass is col- The aforementioned process, in which silica is leached by alka-
lected annually [6]. Crushed glass obtained from municipal and line solutions, is observed in the formation of geopolymers.
industrial sources in Australia is considered as a construction and Geopolymerization involves the breaking down of
demolition (C&D) waste [6] and can be reused as recycled glass aluminosilicate-rich materials by highly alkaline liquids to form
20 A. Arulrajah et al. / Construction and Building Materials 151 (2017) 1827

calcium silicate hydrate (CSH) [18] and aluminium-modified cal-
cium silicate hydrate (CASH) gels [19]. The aluminosilicates, ter-
med as precursors (P) in the geopolymerization process, are
industrial waste materials such as ashes from coal combustion
[20,21] and the burning of rice husk and sugar cane [22,23] which
are rich in silica. Slag, a residue from refining iron, is rich in calcium
oxide and silica is another precursor used in geopolymers. Like the
hydration of Portland cement, the formation of geopolymers
results in the formation of cementitious compounds, which can
be used to bind loose aggregates into a strong composite material.
However, unlike Portland cement, geopolymers are much greener
materials which produce zero carbon emissions [24]. Geopolymers
as alternative construction materials have increasingly garnered
the attention of researchers [2529] due to their low carbon foot-
print. The popularity of geopolymers as alternative construction
materials is also rising as civil engineers become increasingly
aware of innovative alternative construction materials, which will
promote a greener future [3034].
Spent coffee grounds (CG) is a granular, insoluble and highly
organic waste derived from coffee brewing [35]. Coffee is one of
the most popular beverages in the world [36], and estimations
undertaken in 2007 reported that the world produced 7.2 million
tons of spent coffee ground [37]; while in 2015 the figure rose to
8.6 million tons [38]. The highly organic CG is rich in nitrogen,
hence is commonly used as an agricultural fertiliser [39]. As
most of the CG generated in the world is diverted to landfills,
CG was also studied for its effects as a leachate absorbent [40].
More recently, CG was studied as a source of biodiesel fuel
[41] and even reused as a supplementary food ingredient in bak-
ery products [42].
distribution (PSD). Commercially available D-grade Na2SiO3 composed of 44.1% sili-
cic acid, sodium salt (1.6 < Molar Ratio  2.6) and 55.9% water, and reagent grade
NaOH with 97% purity were used.
RG and CG were the parent materials, which formed the bulk of the geopolymer.
RG was mixed with CG and Precursor at a CG:RG:P ratio of 50:20:30, 35:35:30, and
20:50:30. Precursor was fixed at 30% as done previously to enable comparison
between mixes with different RG ratios [44]. The P used in this experiment were
FA and Slag due to their efficiency in stabilizing other recycled construction mate-
rial such as crushed brick [48] and C&D aggregates [49,50]. Two series of specimens
were produced to contain either FA or Slag as their Precursor ratio. Sodium Silicate
(Na2SiO3) and Sodium Hydroxide (NaOH) were mixed for the alkaline liquid activa-
tor (L) used to induce geopolymerization. A ratio of 70Na2SiO3:30NaOH was
adopted as this ratio was found in past studies to be very efficient [14,44,51].
The dried granular solids comprising RG, CG and Precursor (FA or Slag) were
mixed at the desired ratio until homogeneity in colouration could be observed. Con-
currently, the 70Na2SiO3:30NaOH mixture was prepared. The dried material was
then mixed with L until an observable consistency was obtained. However, mixing
was limited to 10 min, particularly in Slag mixes, due to the high flocculation rate of
Slag geopolymers. Different L percentages were used, and the resultant mixes were
then subjected to modified Proctor compaction to obtain a maximum dry unit
weight versus L content curve to observe the influence of L on material compact-
ness. With material density obtained from compaction results, specimens were
statically compacted and reproduced in a 100 mm in height and 50 mm in diameter
split mold. These specimens were sealed in vinyl bags and cured at 21 C or 50 C.
The curing durations were 728 days. UCS tests were then conducted on the spec-
imens. Table 1 summarizes the material combination and test sequences used in
the UCS tests. Fragments obtained from the UCS tests were oven-dried for 24 h
and gold-coated to undergo scanning electron microscopy (SEM) and Energy-
dispersive X-ray spectroscopy (EDS) tests. SEM was conducted under 5 kV using a
Zeiss-SUPRA 40VP device. EDS was done at 20 kV using a peripheral INCA x-act
EDS instrument attached to the electron microscope.
100.0
90.0
Percentage Passing (%)

Due to the physical resemblance of CG with sandy soils, CG has 80.0

been evaluated as a construction material in embankment sub- 70.0
grades [4345]. These studies found that CG could indeed meet 60.0 RG
the structural strength requirements to be used as subgrade fill 50.0 CG
materials, but required proper treatment before becoming struc- 40.0 FA
turally adequate. Conventional soil stabilization methods employ- S
30.0
ing Portland cement and lime were found to be inefficient in 20.0
treating CG [45]. Fly ash (FA) and slag, wastes derived from the coal
10.0
combustion and iron mining industries respectively, were used as
0.0
precursors in CG geopolymers and achieved high compressive and 0.0 0.0 0.0 0.1 1.0 10.0
bearing strengths [44]. Particle Size (mm)
This research studied the effects of introducing RG as a supple-
mentary filler in CG geopolymers, with FA and Slag as precursors. Fig. 2. Particle size distribution of RG, CG, FA, and Slag.
The effects of different replacement ratios of RG on the geopolymer
density, optimum liquid content, and workability were evaluated
and analyzed. This research aims to further reinforce the usage of
green materials in infrastructure works by combining two tradi- 16.0
tional waste materials (RG and CG), into a valuable construction
material. Successful implementation of a recycled RG + CG material 15.0
Dry Unit Weight (kN/m)

as a construction fill material will furthermore reduce the demand 20RG:50CG:30FA

for increasingly scarce landfill space and provide an alternative 14.0
20RG:50CG:30S
solution for current waste management systems.
13.0
35RG:35CG:30FA

12.0
35RG:35CG:30S
2. Materials and methods
11.0 50RG:20CG:30FA
RG was sourced from a Construction and Demolition (C&D) waste recycling
plant in Melbourne, Australia. The RG was graded by the suppliers prior to collec- 10.0 50RG:20CG:30FA
tion, and was categorized as fine RG as all particles passed through the 4.75 mm
sieve. Fine RG was selected as it provides high shear strength compared to large-
sized RG. After procurement, RG was oven-dried at 100 C and then stored in air-
9.0
tight bags.
CG was sourced locally from cafes around Melbourne, Australia. CG was then 8.0
manually separated from other caf wastes such as teabags, serviettes, milk boxes
0.0 0.5 1.0 1.5 2.0
and capsules. The cleaned CG was then oven-dried at 50 C to avoid denaturing the L/P
highly organic particles [46]. Dried CG was then stored in air-tight bags for further
use. Commercially available FA and Slag from Australia were used. Sieve analysis Fig. 3. Modified Proctor compaction curve of CG geopolymers with different RG
was done on oven-dried RG according to ASTM [47] to determine its particle size replacement ratios.
 A. Arulrajah et al. / Construction and Building Materials 151 (2017) 1827 21

3. Results and discussions
SEM images captured on (a) RG, (b) CG, (c) FA, and (d) Slag in
Fig. 1 shows that RG and Slag are polygonal, CG particles are porous
and irregularly shaped, while FA particles are spherical. The XRF
results done on RG, FA, and Slag were summarized in Table 2.
XRF analysis undertaken on the RG particles shows that it is dom-
inantly composed of 83.57% of SiO2, with CaO being the second
dominant compound at 12.53%. Theoretically, this means that the
inorganic compounds found in RG are conducive for geopolymer-
ization as Si, Al, and Ca are required for the polymerization process
to take place. Fig. 2 presents the particle size distribution of the
materials used in the geopolymers and indicates that the RG and
CG are sand-sized particles, with RG resembling coarse-grained
sand and CG resembling medium-grained sand. On the other hand,
FA and Slag fall into the particle size range of fine-grained soils
similar to silt. All the materials used were uniformly graded, but
the fraction of smaller particles in RG is higher compared to the
particle distribution of the other materials. Mixing RG and CG
together with FA and Slag would increase the maximum dry unit
weight with the finer FA and Slag particles filling in the voids
between the larger particles.
Modified Proctor compaction tests done on the RG:CG:P mixes,
as shown in Fig. 3, indicate that with the increase of RG, the L con-
tent required to achieve maximum dry unit weight after com-
paction decreases. Compared to CG geopolymers utilizing solely
FA (L/P = 1.22.6) [43] or Slag (L/P = 1.52.5) [45], the optimum
range of L/P for RG + CG geopolymers to achieve maximum com-
paction is 0.21.6, which can be attributed to the porous CG being
replaced by RG particles which have lower water absorbency. Also,
increasing the ratio of RG in the geopolymer results in increased
dry unit weight of the mix due to the significantly denser RG par-
ticles, which replaces the lightweight CG. Moreover, due to
decreased microporosity with the inclusion of RG, the higher the
amount of RG, the lower the sensitivity of the mix towards
moisture variation. The maximum dry unit weight values recorded
by 20RG:50CG:30P specimens are 10.07 kN/m3 for FA and 11.12
kN/m3 for Slag, whereas the maximum dry unit weight values
recorded by 50RG:20CG:30P specimens are 13.87 kN/m3 for FA
and 14.92 kN/m3 for Slag. Comparatively, the maximum dry unit
weight of CG is 4.4 kN/m3 [35] and the maximum dry unit weight
of 70RG:30FA geopolymers is 18.1 kN/m3 [14].
Fig. 4 presents the 7-day UCS results of the RG + CG geopoly-
mers. Evidently, the UCS of CG geopolymers increases significantly
after the introduction of RG. Compared to CG + FA and CG + Slag
geopolymers, these supplemented geopolymers can easily gain
compressive strengths of more than 1 MPa. At 7 days, geopolymers
at the dry side of the Optimum Liquid Content (OLC) are relatively
inefficient, as the L/P ratio is too low to fully dissolve silica and alu-
mina to form cementitious compounds. At the wet side of OLC,
most mixes develop UCSs exceeding 1 MPa, except for the RG
+ CG + FA mixes cured at 21 C. RG + CG + FA specimens cured at
50 C gain strength with the increase of L/P because elevated tem-
perature curing favors geopolymeric reactions in FA geopolymers

20RG:50CG:30FA, 7 Days 20RG:50CG:30S, 7 Days

3.0 3.0
2.5 2.5
UCS (MPa)

UCS (MPa)

2.0 2.0
1.5 1.5
1.0 1.0
0.5 0.5
0.0 0.0
0.0 1.0 2.0 3.0 0.0 1.0 2.0 3.0
L/P L/P

35RG:35CG:30FA, 7 Days 35RG:35CG:30S, 7 Days

3.0 3.0
2.5 2.5
UCS (MPa)
UCS (MPa)

2.0 2.0
1.5 1.5
1.0 1.0
0.5 0.5
0.0 0.0
0.0 1.0 2.0 3.0 0.0 1.0 2.0 3.0
L/P L/P

50RG:20CG:30FA, 7 Days 50RG:20CG:30S, 7 Days

12.0 12.0
10.0 10.0
UCS (MPa)

UCS (MPa)

8.0 8.0
6.0 6.0
4.0 4.0
2.0 2.0
0.0 0.0
0.0 1.0 2.0 3.0 0.0 1.0 2.0 3.0
L/P L/P
21C 50C

Fig. 4. 7-days UCS of various CG + RG geopolymer mixes at different L/P ratios.

22 A. Arulrajah et al. / Construction and Building Materials 151 (2017) 1827

[52] as FA is high in silica content [53]. On the other hand, without
catalyzation of geopolymeric reaction by heat treatment, the
excess Al-Si precipitation in RG + CG + FA geopolymers hinders
geopolymeric reactions by preventing contact between reactive
materials [54]. Furthermore, the oversaturation of liquid in
50RG:20CG:30P mixes at L/P = 1.6 renders heat treatment ineffec-
tive in preventing excess Al-Si precipitation. Hence, it is important
for RG + CG geopolymers with FA as a precursor to be heat treated
for proper strength development. On the other hand, Slag speci-
mens do not show much variance in strength gain regardless of
curing temperature, confirming that geopolymers with Slag as a
precursors can be cured adequately without elevated curing tem-
peratures [55,56].
Fig. 5 presents the 28-day UCS results of the RG + CG geopoly-
mers. The trend of strength development relative to the change
in L/P is similar to that of the 7-day specimens. At 21 C, Slag
geopolymers performed remarkably and developed UCS similar
to those cured at 50 C; with an FA precursor, the increase of L/P
did not cause any significant variation in UCS. Mixes with high
L/P content have begun developing geopolymeric compounds in
contrast to the 7-days specimens, resulting in UCS values with
lower L/P values. At 50 C, similar to the 7-day specimens, the
UCS of 28-days specimens increases when L/P increases. However,
as the geopolymeric reactions at 28-days had manifested, the
geopolymers have saturation points in which the increase of L/P
still may result in UCS increases, however, the increment is not
proportionate to the increase of L/P. These saturation points are
1.2, 1.0, and 1.2 for 20RG:50CG:30P, 35RG:35CG:30P, and
50RG:20CG:30P respectively regardless of precursors used. Com-
pared to the OLC of these mixes, which are 0.4, 0.6, and 1.0 for
20RG:50CG:30P, 35RG:35CG:30P, and 50RG:20CG:30P respec-
tively, the saturation points are situated at much higher L/P ratios.
This indicates that for these geopolymers, a good balance between
L/P is more important than the maximum compaction of the gran-
ular solids, and that the geopolymeric bonds are the dominant con-
tributors to UCS compared to the interparticle friction created from
maximum material compactness. A balanced L/P ratio ensures that
the aluminosilicate in the mixes is fully utilized in the chemical
reaction to produce desirable calcium silicate hydrate (CSH) and
aluminium-modified calcium silicate hydrate (CASH) gels required
for geopolymerization [57,58].
Generally, the UCS of RG + CG geopolymers increases with the
increase of RG in the mix. This can be attributed to the shear strength
provided by RG particles [8]. Interestingly, 50RG:20CG:30S
specimens gain extremely high UCS values which exceed 10 MPa
at L/P > 1.2 after 7 days of curing. XRF results indicate that the Slag
used in this study has a dominant CaO composition of 43.55%.
OH- ions readily react with the abundant Ca (dissolved from CaO)

20RG:50CG:30FA, 28 Days 20RG:50CG:30S, 28 Days

3.0 3.0
2.5 2.5
UCS (MPa)

UCS (MPa)

2.0 2.0
1.5 1.5
1.0 1.0
0.5 0.5
0.0 0.0
0.0 1.0 2.0 3.0 0.0 1.0 2.0 3.0
L/P L/P

35RG:35CG:30FA, 28 Days 35RG:35CG:30S, 28 Days

3.0 3.0
2.5 2.5
UCS (MPa)
UCS (MPa)

2.0 2.0
1.5 1.5
1.0 1.0
0.5 0.5
0.0 0.0
0.0 1.0 2.0 3.0 0.0 1.0 2.0 3.0
L/P L/P

50RG:20CG:30FA, 28 Days 50RG:20CG:30S, 28 Days

12.0 12.0
10.0 10.0
UCS (MPa)

UCS (MPa)

8.0 8.0
6.0 6.0
4.0 4.0
2.0 2.0
0.0 0.0
0.0 1.0 2.0 3.0 0.0 1.0 2.0 3.0
L/P 21C 50C L/P

Fig. 5. 28-days UCS of various CG + RG geopolymer mixes at different L/P ratios.

 A. Arulrajah et al. / Construction and Building Materials 151 (2017) 1827 23

to form CSH [28], enabling the mix to achieve high early (7 days)
strengths. This observation is consistent with findings by Ismail
et al. [27]. The increased mechanical strength provided by RG parti-
cles, which possess a similar friction angle and shear strength as
compared to naturally occurring sand [59], and additional Si leached
from fine RG particles provided elevated compressive strength per-
formance and supplemented the formation of geopolymers.
Fig. 6 shows the difference in the UCS of specimens cured for 7
and 28 days using FA as a precursor. Evidently FA geopolymers
cured at room temperature exhibits decrease in UCS when the
L/P ratio goes beyond the optimum ratio. Alkaline activation causes
FA particles to dissolve and form NASH gels, which should merge
into larger masses with time [60]. However, due to excess Si in
the mix which excessively increases the Si/Al ratio [61], and with-
out the help of elevated temperature curing, the process is hin-
dered as seen in Fig. 6. Moreover, the addition of Si-rich RG
further increases the Si/Al ratio. Therefore, FA geopolymers cured
at room temperature performed poorly at 7 days. However, there
are large improvements in UCS after 28 days. With 50 C curing,
FA specimens develop higher overall UCS, and the difference
between the 7-day and 28-day specimens UCS was smaller.
Fig. 7 shows the difference in the UCS of specimens cured for 7
and 28 days using FA as a precursor. On the other hand, in Fig. 7 it
can be seen that Slag geopolymers develop high early strengths
regardless of curing temperature. Only 20CG:50RG:30S specimens
cured at 21 C at high L/P ratios show a significant difference in
UCS between 7-day and 28-day. As explained earlier, Slag geopoly-
mers gain early strength mainly by the formation of CSH, which is
independent of the Si/Al ratio. However, at 20CG:50RG:30S the
high amount of Si may start to hinder the geopolymerization pro-
cess due to excess unreacted compounds. This problem was not
present in 50 C -cured Slag geopolymers. On the other hand, com-
paring all 7-day to 28-day UCS results show that the UCS of spec-
imens is increased or maintained after prolonged curing.
Interestingly, at low L/P values of 0.40.8, all geopolymers per-
form relatively poorly, with UCS ranging from 500800 kPa. This is
attributed to insufficient L content, which results in poor dissocia-
tion of precursor material to form cementitious compounds,
regardless of heat treatment or prolonged curing. After reaching
the optimum L/P ratio, it is especially evident at 21 C curing that,
Slag geopolymers outperform their FA counterparts. In short, FA
geopolymers require heat treatment to develop high UCS, whereas

20RG:50CG:30FA, 21C 20RG:50CG:30FA, 50C

3.0 3.0
2.5 2.5
UCS (MPa)

UCS (MPa)

2.0 2.0
1.5 1.5
1.0 1.0
0.5 0.5
0.0 0.0
0.8 1.2 1.6 2.0 0.8 1.2 1.6 2.0
L/P L/P

35RG:35CG:30FA, 21C 35RG:35CG:30FA, 50C

3.0 3.0
2.5 2.5
UCS (MPa)
UCS (MPa)

2.0 2.0
1.5 1.5
1.0 1.0
0.5 0.5
0.0 0.0
0.6 1.0 1.4 1.8 0.6 1.0 1.4 1.8
L/P L/P

50RG:20CG:30FA, 21C 50RG:20CG:30FA, 50C

12.0 12.0
10.0 10.0
UCS (MPa)

UCS (MPa)

8.0 8.0
6.0 6.0
4.0 4.0
2.0 2.0
0.0 0.0
0.4 0.8 1.2 1.6 0.4 0.8 1.2 1.6
L/P L/P
7-Days Curing 28-days Curing
Fig. 6. 7-days and 28-days UCS development of CG + RG geopolymers with FA as a precursor.
24 A. Arulrajah et al. / Construction and Building Materials 151 (2017) 1827

20RG:50CG:30S, 21C 20RG:50CG:30S, 50C

3.0 3.0
2.5 2.5

UCS (MPa)

UCS (MPa)
2.0 2.0
1.5 1.5
1.0 1.0
0.5 0.5
0.0 0.0
0.8 1.2 1.6 2.0 0.8 1.2 1.6 2.0
L/P L/P

35RG:35CG:30S, 21C 35RG:35CG:30S, 50C

3.0 3.0
2.5 2.5

UCS (MPa)
UCS (MPa)

2.0 2.0
1.5 1.5
1.0 1.0
0.5 0.5
0.0 0.0
0.6 1.0 1.4 1.8 0.6 1.0 1.4 1.8
L/P L/P

50RG:20CG:30S, 21C 50RG:20CG:30S, 50C

12.0 12.0
10.0 10.0
UCS (MPa)

UCS (MPa)

8.0 8.0
6.0 6.0
4.0 4.0
2.0 2.0
0.0 0.0
0.4 0.8 1.2 1.6 0.4 0.8 1.2 1.6
L/P L/P
7-Days Curing 28-days Curing
Fig. 7. 7-days and 28-days UCS development of CG + RG geopolymers with Slag as a precursor.

Table 3
Comparison of EDS results for 20RG:50CG:30P geopolymers cured for 7 days at different temperatures.

Element 20RG:50CG:30FA 7 days, 20RG:50CG:30FA 7 days, 20RG:50CG:30S 7 days, 20RG:50CG:30S 7 days,

21 C 50 C 21 C 50 C
Weight% Atomic% Weight% Atomic% Weight% Atomic% Weight% Atomic%
C 45.64 56.03 32.83 42.67 29.91 39.9 18.49 26.39
O 38.95 35.89 47.15 46.01 47.11 47.19 52.72 56.49
Na 2.3 1.48 4.16 2.82 6.13 4.27 6.5 4.85
Mg N.D. N.D. N.D. N.D. 0.66 0.43 1.03 0.73
Al 2.98 1.63 3.82 2.21 1.25 0.74 1.99 1.26
Si 8.25 4.33 9.89 5.5 8.69 4.96 11.16 6.81
K 0.54 0.2 0.64 0.25 0.57 0.23 0.55 0.24
Ca 0.89 0.33 0.97 0.38 5.7 2.28 7.55 3.23
Fe 0.45 0.12 0.54 0.15 N.D. N.D. N.D. N.D.

N.D. = Not Detected.

Slag geopolymers develop relatively high UCS values regardless of
curing temperature.
EDS was used to scan the geopolymeric bonds occurring
within the RG + CG geopolymers. Table 3 compares the EDS
results of 50CG:20RG:30P specimens cured for 7 days. The car-
bon content represents CG: if the detectable percentage of car-
bon is large, it indicates that the geopolymeric material is not
effective in encapsulating the CG particles. FA specimens contain
trace amount of iron, whereas Slag specimens contain trace
amounts of magnesium. From Table 3, the percentage of carbon
in FA geopolymers was higher than Slag geopolymers. However,
at 50 C the percentage of carbon is significantly reduced.
Sodium, Aluminium, Silica, and Calcium levels in the geopoly-
meric compounds all show increase at 50 C curing, with the
increase more prominent in FA mixes, thus validating that ele-
vated temperature curing aids the formation of geopolymeric
 A. Arulrajah et al. / Construction and Building Materials 151 (2017) 1827 25

Table 4
Comparison of EDS results for CG:RG:Slag geopolymers with 20, 30, and 50% of RG.

Element 70CG:30S 7 days, 50 C 20RG:50CG:30S 7 days, 35RG:35CG:30S 7 days, 50RG:20CG:30S 7 days,

50 C 50 C 50 C
Weight% Atomic% Weight% Atomic% Weight% Atomic% Weight% Atomic%
C 29.91 39.9 18.49 26.39 15.87 23.15 11.66 18.94
O 47.11 47.19 52.72 56.49 52.18 57.15 46.8 55.46
Na 6.13 4.27 6.50 4.85 8.13 6.20 90 7.01
Mg 0.66 0.43 1.03 0.73 0.99 0.72 0.67 0.54
Al 1.25 0.74 1.99 1.26 1.48 0.96 2.44 1.76
Si 8.69 4.96 11.16 6.81 13.35 8.33 16.88 10.65
K 0.57 0.23 0.55 0.24 0.65 0.29 0.71 0.36
Ca 5.70 2.28 7.55 3.23 7.33 3.20 11.84 5.28
Fe N.D. N.D. N.D. N.D. N.D. N.D. N.D. N.D.

N.D. = Not Detected.

Element Weight% Atomic%

C 31.05 40.96
O 48.16 47.69
Na 5.19 3.58
Mg 0.78 0.51
Al 1.31 0.77
Si 6.84 3.86
K 0.3 0.12
Ca 6.38 2.52
(a)

Element Weight% Atomic%

C 24.86 34.16
O 49.7 51.27
Na 6.49 4.66
Mg 0.81 0.55
Al 1.62 0.99
Si 8.88 5.22
K 0.43 0.18
Ca 7.21 2.97
(b)

Element Weight% Atomic%

O 52.55 65.81
Na 10.46 9.12
Al 0.63 0.46
Si 30.11 21.48
K 0.28 0.15
Ca 5.97 2.98

(c)

Fig. 8. SEM of a 20RG:50CG:30 S specimen cured for 7 days at 21 C, and EDS results on (a) a large area of geopolymeric formation encompassing voids; (b) a smaller area of
relatively denser geopolymeric formation; and (c) an embedded RG particle.

substances. The levels of Na, Si and Ca are significantly higher in relies on the Al and Si whereas in Slag mixes, Ca and Si are
Slag geopolymers, indicating that the geopolymeric compound the main components in geopolymerization.
possesses a higher concentration of CSH and CASH gels. It can Table 4 shows that with the increase of RG in the dry material
also be deduced that the geopolymeric formation in FA mixes ratio, geopolymeric activities increase, as indicated by the increase
26 A. Arulrajah et al. / Construction and Building Materials 151 (2017) 1827
in Na, Si, and Ca and the decrease of carbon percentage in the
geopolymeric formation. As shown in Table 4, a geopolymer with-
out RG consists of 8% of Si that it doubles to 16% when CG is
replaced by 75% RG. Correlating the UCS and EDS results leads to
the inference that as RG increases, the resultant UCS of the mix
increases.
The SEM image of a Slag geopolymer specimen in Fig. 8 shows a
large polygonal particle cemented by geopolymeric substances.
The corresponding EDS results show significant difference in Silica
concentration at (a) a large area of geopolymeric formation encom-
passing voids, (b) a smaller area of relatively denser geopolymeric
formation, and (c) an embedded particle. With the presence of
voids in the geopolymer in (a), exposed CG is prone to detection.
A concentrated scanning area as shown in (b) may better represent
the typical element ratio in a geopolymeric compound. The polyg-
onal particle in (c) does not contain carbon, and is largely com-
posed of Si and O. RG and Slag are both polygonal but due to the
trace amount of detectable Ca, it can be deduced that the particle
is RG.
From the EDS results, it can be inferred that a fractional amount
of RG dissolves and contributes to the formation of geopolymeric
substances, but large RG particles can be found to be cemented
by the geopolymeric compounds. The RG used in this study has
particle sizes ranging from 0.075 mm to 4.5 mm, and fine RG par-
ticles contain easily dissolvable Si which is highly pozzolanic [62].
In a past study, fine RG particles lesser than 0.1 mm were found to
be effective pozzolans with properties similar to FA [63], whereas
another report considered RG finer than 0.3 mm to be an effective
precursor for geopolymers [62]. 10% of the RG used in this study is
finer than 0.3 mm in diameter hence act to supplement the forma-
tion of geopolymeric substances, as shown in the difference of Si
concentration in the geopolymeric formations with different per-
centages of RG in Table 4. The embedded glass particle supports
past observations that in a RG geopolymer, the geopolymeric for-
mation acts as a cementing agent that encapsulates and bonds
RG particles together [14]. The addition of RG in CG geopolymers
thus creates a highly favorable environment for UCS development
in which geopolymeric reaction is enhanced by the supplementa-
tion of Silica whereas large RG particles provide the mechanical
strength to the mix by acting as an aggregate.
Due to the porous surface of CG particles, it is much more water
absorbent whereas RG particles are smooth and non-porous hence
reducing the overall water absorption rate of the mix [64]. Hence
with the reduction of CG in the geopolymer mix, the amount of free
alkaline liquid which can react with the precursor increases dra-
matically and leads to the increase in UCS due to effective geopoly-
merization. Coupled with the high shear strength that
characterizes fine RG, the addition of RG into CG geopolymers leads
to the increased UCS in the resultant material.
4. Conclusions
RG was added as a supplementary material to observe how this
C&D waste material affects strength development in spent coffee
grounds (CG) geopolymers. CG has been known to form a green
material, which is lightweight and sufficiently strong to be used
as a road subgrade material when stabilized with fly ash (FA)
and Slag (Slag) geopolymers. An alkaline liquid ratio of 70%
Na2SiO3 and 30% NaOH was used to optimally induce
geopolymerization.
RG was found to reduce the L/P ratio of CG geopolymers to
achieve the saturation points for maximum UCS development.
However, the dry unit weight of CG geopolymers increased propor-
tionately along with the strength increase following the replace-
ment of CG by RG. This study ascertained that RG not only
provided mechanical strength to CG geopolymers due to high
inter-particle friction, but also supplemented the formation of
geopolymeric substances by providing readily dissolvable Si into
the mix.
L/P was an important parameter, which influenced strength
development in these geopolymers. At low L/P ratios, insufficient
alkaline liquid resulted in ineffective geopolymerization and
cementation, hence produced specimens with low UCS. By increas-
ing L/P, UCS increased until a saturation point was achieved. At sat-
uration point, RG supplemented CG + Slag geopolymers could
easily achieve UCS values exceeding 1 MPa after 7 days of curing,
regardless of a 21 C or 50 C curing environment. On the other
hand, CG + FA specimens required heat treatment to achieve high
early UCS. The highest recorded UCS at 7 days was 10.86 MPa
and corresponded with 20CG:50RG:30S at L/P = 1.2 cured at
50 C. Conclusively, CG + Slag geopolymers were recommended
for use due to their independency on the elevated temperature
curing.
RG is a waste material abundantly available throughout the
world. This research indicated that the addition of RG into the
CG geopolymer mix would contribute to streamlining waste man-
agement efforts, as large volumes of fill material are required
annually to construct roads and highways across the globe. A
green geopolymer encompassing the waste materials; RG CG,
FA, and Slag as an alternative construction material will indeed
promote a sustainable future for the construction industry.
Acknowledgements
The third author acknowledges the financial support from the
Thailand Research Fund under the TRF Senior Research Scholar
program Grant No. RTA5980005 and Suranaree University of
Technology.
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