Hybrid Biocomposites Based On Used Coffee Grounds and Epoxy Resin
Hybrid Biocomposites Based On Used Coffee Grounds and Epoxy Resin
Research Article
Hybrid Biocomposites Based on Used Coffee Grounds and Epoxy
Resin: Mechanical Properties and Fire Resistance
1 2
Tuan Anh Nguyen and Quang Tung Nguyen
1
Faculty of Chemical Technology, Hanoi University of Industry (HaUI), No. 298 Cau Dien Street, Bac Tu Liem District,
Hanoi 100000, Vietnam
2
Institute of Technology HaUI, Hanoi University of Industry (HaUI), No. 298 Cau Dien Street, Bac Tu Liem District,
Hanoi 100000, Vietnam
Copyright © 2021 Tuan Anh Nguyen and Quang Tung Nguyen. This is an open access article distributed under the Creative
Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the
original work is properly cited.
Studies on using biomaterials hybridized with other materials to produce biomaterials have been paid more attention due to their
low cost, abundance, renewability, and degradability. Therefore, these materials are ecofriendly and nontoxic to humans. A large
number of used coffee grounds (SCGs) are often discarded and replacements are necessary for dealing with environmental
problems. This work developed sustainable materials by reusing SCGs. Used coffee grounds were mixed with epoxy resin at
different amounts: 30 wt %, 40 wt %, 50 wt %, and 60 wt %. SCGs were treated with 0.5 N NaOH, at SCGs/NaOH ratio of 1 : 2. SEM
images showed that the material with 30 wt % SCGs has good compatibility without phase division on the SCGs-epoxy interface.
Results of mechanical properties of epoxy composites with 30 wt % SCGs are as follows: tensile strength of 44.81 ± 10 MPa, flexural
strength of 80.07 ± 0.16 MPa, compressive strength of 112.56 ± 0.11 MPa, and Izod strength and impact of 8.21 ± 0.19 kJ/m2. In
terms of flame-retardant properties, the oxygen index is limited to 20.8% ± 0.20 and the burning rate according to UL94HB is
27.02 ± 0.29 mm/min. The obtained results indicate that it is possible to produce biohybrid composites from epoxy resin and
SCGs. This work offers an ecofriendly alternative method to use the waste of the coffee industry. It contributes to improvements of
the general characteristics of composites such as mechanical, thermal, and flame-retardant properties. This work proved that SCGs
have a high potential to be used in a wide range of composite materials for civil engineering applications.
coffee grounds are a promising source of industrially im- studied the debrowning process of coffee grounds and
portant sugars and polyphenols [7]. Coffee grounds can be reinforced polylactic acid (PLA) resins [29], in addition to
considered a green, biodegradable material. The idea of researching and using used coffee grounds to make multi-
recovering used coffee grounds by introducing them as functional materials on plastic substrates such as epoxy and
reinforcements and fillers for polymer materials is likely to polylactic acid (PLA). They used coffee grounds as a versatile
be widely studied. Some studies have used different polymers green energy source. Extraction of biodiesel from coffee
such as polypropylene (PP), polylactide (PLA), and poly- grounds has been studied to significantly increase the
vinyl alcohol (PVA). Research results show that when profitability of biodiesel production, especially for the for-
adding used coffee grounds to epoxy resin, some mechanical mation of glycerol carbonate. Coffee grounds after extrac-
properties are slightly reduced but not much, and some tion of oil are an ideal material to make garden fertilizer, a
other mechanical properties are also significantly improved. raw material for ethanol, and a type of fuel [25, 30].
Coffee grounds can be said as the best material for com- There is a need for research and development of new
posites [8, 9]. Suaduang et al. studied the inclusion of coffee green composites to meet the growing industry demand for
grounds in polylactic acid at the concentrations of 5 wt.%, structural applications. In this study, used coffee grounds at
7.5 wt.%, and 10 wt.%. The results show that the elongation 30 wt %, 40% wt %, 50 wt %, and 60 wt % concentrations
at break is improved with increasing coffee grounds content were added to epoxy resin to form hybrid green composites.
[10]. Tarazona et al. used 30 wt % and 35 wt % coffee grounds Mechanical properties such as tensile strength, flexural
in making green composites based on epoxy resin, with 35 strength, compressive strength, and Izod impact strength
wt % coffee grounds for best mechanical properties [11]. In were investigated. The SEM method was used to study the
addition, to increase the applicability of coffee grounds, morphology and structure of the materials. Fire resistance
coffee grounds have been treated with alkalis at different was investigated by LOI and UL94-HB methods.
concentrations. This method can change the structure and,
under optimal conditions, does not break the basic structure 2. Materials and Methods
[12]. To improve the mechanical properties and fire
retardancy of epoxy materials, environmentally friendly 2.1. Materials
additives have been studied. Additive nanoclay, multiwalled
carbon nanotubes are incorporated into epoxy resin to (i) Epikote 240 epoxy (EP 240) was obtained from
improve mechanical properties while increasing fire bisphenol F, of Shell Chemicals (USA) with 24.6%
retardancy [13–15]. Besides, fly ash waste from thermal epoxy content, equivalent to epoxy group 185–196,
power plants is also recycled by using it as an additive to and viscosity 0.7 ÷ 1.1 Pa s at 25°C (see Table 1).
composite materials to improve fire resistance [16–19]. The (ii) Curing agent used was diethylenetriamine (DETA),
study of mechanical properties of fiber-reinforced com- from Sigma-Aldrich; chemical formula of DETA is
posites is of great interest to many scientists. Mostafa et al. H2N(CH2)NH(CH2)2NH2, with MW of 103 g.mol-1
studied the tensile properties of fiber/fabric-reinforced and specific gravity at 25°C: 0.95 g/cm3.
composites. One of the research results only shows that the (iii) Spent coffee grounds (SCGs) were collected from
degree of residual stress induced in the composite com- coffee shops in Hanoi City, Vietnam. Coffee was
ponents does not only depend on the degree of pretreatment produced by Trung Nguyen Coffee Company,
of the fiber but also on the elastic properties of the composite Vietnam.
[20]. Therefore, the initial fiber treatment before processing
(iv) NaOH was obtained from Sigma-Aldrich, Vietnam.
is very important. The structure of composite materials is
also studied through tensile and thermal testing [21]. Recent
research activities show that biological compounds such as 2.2. Methods
sisal fibers [22], lemon and lime peels [23], cellulose and silk
[24], and various fillers obtained from the outermost skins of 2.2.1. Sample Preparation. SCGs were washed with distilled
onions, potatoes, and carrots [25] are an approach to cre- water (7 to 10 washes) at room temperature to achieve a
ating biomaterials with desired specific properties. Banana neutral pH level. The SCGs were then dried in a drying oven
fiber and eggshell powder obtained from agricultural and at 80°C for 8 hours. The SCGs were then sieved to obtain less
postconsumer waste are used as biomaterial fillers to rein- than 50 µm in size and selected SCGs were stored for later
force concrete [26]. In addition, chicken waste (femur and use in all studies.
beak) and fish bones were used as an adsorbent to remove Pretreatment of spent coffee grounds: SCGs were soaked
Cd2+ from aqueous solutions [27]. Saberian et al. had an with NaOH 0.5 N (SCG/NaOH 0.5 N ratio � 1 : 2) for 5 hours
overview study on recycling used coffee grounds as building at 50°C. Then, each sample of the treated SCGs was dried at
materials. They concluded that SCGs have a high potential 80°C in a drying cell for 8 hours and stored in a glass bottle
for use as composites in building materials in a wide range of for use in the next analysis [12].
civil engineering applications. However, research is limited Dried SCGs were added to the epoxy resin at the following
and there is a lack of evidence of successful practical ap- mass percent: 30 wt %, 40% wt %, 50 wt %, and 60 wt % SCGs.
plications in the field of building materials [28]. The mixture was mechanically stirred at 1500 rpm at 80°C for
However, the inherent brown color of SCG places a limit 90 min. The mixture is allowed to cool at room temperature;
on the color of the composite product and thus Li et al. then, add a DETA curing agent (50 grams of epoxy resin
International Journal of Chemical Engineering 3
Table 1: Properties of epoxy Epikote 240 resin. (v) The morphology of the samples was carried out with
Properties Test method Unit Value
a scanning electron microscope (SEM, SU3800,
HITACHI, Japan), measured at Materials Room 1,
Epoxy group content SMS 2026 mmol/kg 5100–5400
Faculty of Mechanical Engineering Technology,
Epoxy molar mass∗ g 185–196
Viscosity at 25°C ASTM D445 Pa.s∗∗ 0.7–1.1 Hanoi University of Industry, Vietnam.
Colour ASTM D1209 Pt-Co 200 max
Density at 25°C ASTM D4052 kg/L 1.12
∗
No. of grams of resin containing 1 g equivalent of epoxide (weight per 3. Results and Discussion
equivalent, WPE, is an alternative term).∗∗1 Pa.s � 10 poise.
3.1. Morphology. The structural morphology of the hybrid
requires 12 grams of DETA) to the mixture. Stir the mixture at SCGs/epoxy composites was evaluated by SEM and is
300 rpm for about 7–10 minutes and then pour the mold. To presented in Figure 2.
cure at room temperature for 24 hours, dry at 80°C for 3 hours. From Figure 2, it can be seen that when mechanically
One week later, remove the mold to get the product. The stirring at 1500 rpm at 80°C, the coffee grounds moved
product is stored in hygroscopic plastic containers and measured strongly and the impact performance was strong, thus en-
for properties. A summary of the pretreatment process of SCG hancing the penetration into the plastic substrate and in-
and the fabrication of epoxy composites is presented in Figure 1. creased dispersion. The size of the coffee grounds is reduced.
Also, from the morphological structure of the SCGs-epoxy
hybrid material (see Figure 2), it is shown that the NaOH-
2.2.2. Analysis
treated coffee grounds give an effective wetting ability to the
epoxy resin base, along with the strong surface adhesion
(i) Fire-Retardant Evaluation Method.
between the phase of materials (according to Figure 2, the
(i) Limiting oxygen index (LOI) according to JIS K720 overall image SEM of the destroyed material surface at 45
standard (Japan): the sample bars used for the test resolution). We can also observe microcracking that appears
were 150 × 6.5 × 3 mm3. The average values of the normal to the grain contour, and this harms the compati-
five specimens were reported. bility (Figure 2, red circle area and white arrow). However,
(ii) The horizontal burning tests (UL-94HB): standard bar the crack size is small and the path length is short. The
specimens are to be 125 ± 5 mm long by 13.0 ± 0.5 mm compatibility is not good due to the appearance of phase
wide, provided in the minimum thickness of 3.0 separation on the epoxy-SCGs interface. This is completely
(−0.0 + 0.2) mm (ASTM D635-12). The average values normal because when the surface of SCGs has not been
of the five specimens were reported. modified much, the compatibility will decrease. Phase
separation is highly efficient when the surface of the SCGs is
The UL 94 flame-retardant and oxygen limit tests are modified and the input content is at the right level [8].
conducted at the Polymer Materials Research Center, Hanoi The dispersion of ESCG particles is homogeneous as
University of Technology, Vietnam. depicted in Figure 3. On the interface between SCGs-epoxy,
(ii) Method for Determining Mechanical Properties. the interaction is very good, and wetting and mechanical
(i) Tensile strength was determined according to ISO properties can be improved. However, observing
527-1993 standard on an INSTRON 5582-100 kN Figure 3(d), there is a separation between epoxy materials
machine (USA) with a tensile speed 5 mm/min, and SCGs (two white arrows). However, observing
temperature 25°C, and humidity 75%. The average Figure 3(d), there is a separation between epoxy materials
values of the five specimens were reported. and SCGs (two white arrows). This delamination is the result
of the force transfer process acting on the coffee grounds
(ii) The flexural strength was determined according to
filler; the coffee grounds have received the force and are
ISO 178-1993 on an INSTRON 5582-100 kN
loaded instead of the epoxy base material. The addition of
machine (USA) with a bending speed of 5 mm/
coffee grounds filler changed the path of the crack. Ob-
min, a temperature of 25°C, and a humidity of
servation on the interface of the crack showed that the
75%. The average values of the five specimens
addition of coffee grounds filler caused a change in the
were reported.
direction of the crack. The upper adhesive bond fracture type
(iii) Compressive strength was determined according to in Figure 3(d) shows a good interaction between the fillers of
ISO 604–1993 standard on an INSTRON 5582- waste coffee beans powder and epoxy.
100 kN machine (USA), with a compression speed Figures 2 and 3 show that with the addition of coffee
5 mm/min and temperature of 25°C. The average grounds to the content of 60 wt %, the compatibility is
values of the five specimens were reported. observed on the phase division surface. However, due to the
(iv) Izod impact strength was determined according to high content, the coffee grounds particles have agglomerated
the ASTM D265 standard on the Tinius Olsen into larger particles than the shape of the coffee grounds (see
machine (USA), measured at Research Center for Figures 2 and 3). There is a phase separation on the coffee
Polymer Materials, Hanoi University of Science and grounds-epoxy interface because at the position where force
Technology. The average values of the five speci- is applied, the amount of object is different. This can lead to
mens were reported. deterioration of mechanical properties.
4 International Journal of Chemical Engineering
Dry at 80°C, 8 hr
Wash distilled
Sieve 50 mesh
size SCG
Soak in NaOH
At 50°C, 5 hr
0.5 N solution
Dry at 80°C, 8 hr
Epoxy/DETA
Glass fiber/
epoxy/DETA
SCGs-epoxy hybrid material When the coffee grounds content was reduced to 50%,
although no agglomeration of coffee grounds was observed,
large cracks were still clearly visible on the SCGs-epoxy
interface (Figures 4(a) and 4(b)). At the same time, because
Epoxy
the content of coffee grounds is still high, the viscosity of the
mixture is large, leading to the existence of air bubbles (holes
in Figures 4(b) and 4(c)). In a certain region, epoxy-SCGs
SCGs still exist without any cracks (Figure 4(d)).
From the results of the morphology and structure (SEM
image, Figure 5), the fracture surface of the SCGs-epoxy
hybrid material, the cracks, and agglomeration (clustering)
of the SCGs are almost absent. Cracks are reduced and voids
are no longer present (mixed viscosity decreases).
The SEM images in Figure 6 show the difference in
structural morphology compared with the SEM images of
Figure 2: SEM images of SCGs/epoxy, 60 wt % SCGs, ×45. Figures 2–5. Figure 6(c) shows that the coffee grounds are in
International Journal of Chemical Engineering 5
(a) (b)
Epoxy SCGs
SCGs
(c) (d)
the form of beans with sizes ranging from about 20 to 50 µm, Only the Izod impact strength increased slightly compared
already completely embedded in the plastic mass. The coffee to the rest of the models. Possibly due to the good com-
grounds have been separated from each other, not as clumps, patibility on the epoxy-SCGs interface, this interaction is
and the particles are covered with epoxy resin. Cracks still strong enough to increase the impact strength. However,
appear on the fracture surface; however, the fracture tra- other durability tends to decrease, but not much. This is
jectory tends to change due to the influence of SCGs. The consistent with the argument in the structural morphology
compatibility is clearly shown in Figure 6(c), and phase section. In terms of tensile strength, in the presence of SCGs,
separation was not observed. Wetting was performed on the the tensile strength of the samples decreased especially at 60
SCGs-epoxy interface. Possibly at 30 wt % SCGs, the best wt % SCGs. This can be explained by the low compatibility,
compatibility was achieved compared with 40 wt %, 50 wt %, adhesion, and dispersion, as well as the uneven geometric
and 60 wt % concentrations. It is promising this is the rate at structure of the coffee grounds. At the concentrations of 50
which mechanical properties and flame retardancy will be wt % and 60 wt % SCGs, there is phase separation on the
improved [10]. Through SEM images of the fracture surface SCGs-epoxy interface and the association between SCGs and
of the material, it shows that delamination or fracture occurs epoxy resins is not high. As the SCGs particles are well
with the form between the particles and the epoxy-based dispersed in the epoxy matrix, the overall polymer-SCGs
resin (broken on the epoxy-SCGs phase-divided surface particle interaction has been improved. When increasing
interface). from 30 wt % SCGs to 60 wt % SCGs, the mechanical
strength, in general, tends to decrease. This is completely
consistent with the general rule [8, 10]. Patil et al. studied the
3.2. Mechanical Properties. The mechanical properties of inclusion of treated natural fibers (sweet lemons and limes)
SCGs/epoxy materials are presented in Figure 7. granules reinforced with 10%, 20%, and 30% volume frac-
From the results of mechanical properties in Figure 7, it tion in epoxy resin, resulting in mechanical properties.
is shown that when increasing the content of SCGs from 30 Studies show that 30% is the best. At 30% volume fraction
wt % to 60 wt %, the general mechanical properties (tensile (sweet lemon and lime), the tensile strength reached
strength, flexural strength, and compressive strength) tend 35.16 MPa and 48.22 MPa, respectively. Meanwhile, the
to decrease. This is a common characteristic of materials flexural strength of the sweet lemon sample reached
when using fillers of natural origin (kaolin, talc, or CaCO3). 72.11 MPa and the common lemon reached 79.32 MPa
6 International Journal of Chemical Engineering
(a) (b)
(c) (d)
[23, 25, 26]. From Figure 7, it is shown that, for the 30 wt % coffee grounds sample that has not been treated by NaOH
SCGs sample, the best tensile strength (44.81 MPa) and with lower mechanical properties than the model that has
similarly flexural strength of 80.07 MPa is higher than the been treated with 30SCGs-epoxy and other samples. It is
remaining samples. This shows that the research results in clear that the treatment with NaOH aids SCGs to bind the
this work are completely grounded. Thus, used coffee epoxy resin matrix to form a hybrid material. Therefore, the
grounds mixed with epoxy at 30 wt % are the most feasible, mechanical properties of the samples with treated coffee
suitable for composite materials reinforced with biological grounds have much higher mechanical strength.
materials (coffee grounds, lemon, sweet lemon, etc.).
The results of the measurement of mechanical properties 3.3. Fire-Retardant Property. Flame-retardant properties of
in Figure 7 also show that the 30SCG-epoxy sample is a used SCGs/epoxy materials are shown in Figure 8.
International Journal of Chemical Engineering 7
SCGs
60 90
80
50
Flexural strength (MPa)
Tensile strength (MPa)
70
40 60
50
30
40
20 30
20
10
10
0 0
Neat epoxy
30SCG-epoxy
30SCGs-epoxy
40SCGs-epoxy
50SCGs-epoxy
60SCGs-epoxy
Neat epoxy
30SCG-epoxy
30SCGs-epoxy
40SCGs-epoxy
50SCGs-epoxy
60SCGs-epoxy
160 10
Neat epoxy
30SCG-epoxy
30SCGs-epoxy
40SCGs-epoxy
50SCGs-epoxy
60SCGs-epoxy
Neat epoxy
30SCG-epoxy
30SCGs-epoxy
40SCGs-epoxy
50SCGs-epoxy
60SCGs-epoxy
SCGs (wt %) SCGs (wt %)
(c) (d)
Figure 7: Mechanical properties of hybrid materials SCGs-epoxy, with SCGs at different concentrations: 30 wt %; 40 wt %; 50 wt %; and 60
wt %. 30SCG-epoxy: 30 wt % SCG untreated used coffee grounds.
21.5 45
21 40
20.5 35
UL94-HB (mm/min)
20 30
LOI (%)
19.5 25
19 20
18.5 15
18 10
17.5 5
17 0
Neat epoxy
30SCG-epoxy
30SCGs-epoxy
40SCGs-epoxy
50SCGs-epoxy
60SCGs-epoxy
Neat epoxy
30SCG-epoxy
30SCGs-epoxy
40SCGs-epoxy
50SCGs-epoxy
60SCGs-epoxy
Composites Composites
(a) (b)
Figure 8: Flame-retardant properties of SCGs/epoxy materials with SCGs at different concentrations: 30 wt %, 40 wt %, 50 wt %, and 60 wt
%. 30SCG-epoxy: 30 wt % SCG untreated used coffee grounds.
From Figure 8, it can be seen that the content of SCGs retardant property improve (LOI index reaches 20.8%,
also affects the fire retardancy of epoxy resin more or less. burning rate V � 27.02 mm/minute, see Figure 8).
When the content of SCGs increases, the compatibility From Figure 9, at magnifications of 10.0 k and 20.0 k, we
decreases leading to an unstable structure and this is the can see that used coffee grounds can exist in small sizes. We
cause of the reduced fire retardancy of the material. Espe- observed that the SCGs particles bonded to the epoxy resin
cially at the combined ratio of 30 wt % SCGs, which is a fairly very strongly; they formed with the epoxy into a smooth,
good compatibility ratio, the mechanical properties are high defect-free substrate. This has had a huge impact on the
and the flame retardancy is better than other ratios. mechanical properties especially the flame-retardant prop-
At the combination of 30 wt % SCGs, the material erties. It is demonstrated that a 30 wt % SCGs blend provides
structure achieved good compatibility (as commented in the mechanical properties and flame retardancy at the specified
structure section via the SEM image above). Looking at the level. This may be related to successful oil removal during
SEM image in Figure 6(c), Coffee grounds are soaked in NaOH treatment. The absence of oil along with reduced
epoxy resin and surrounded by epoxy resin. It is this particle size may allow for better homogeneity in epoxy,
compact structure, without holes, that makes the flame- improved surface interaction between SCGs-epoxy [8].
International Journal of Chemical Engineering 9
SCGs
SCGs
(a) (b)
Figure 9: SEM images of fracture surface of 30SCGs-epoxy materials (30 wt % SCGs) at different magnifications: (a) ×10.0 k and (b) ×20.0 k.
(a) (b)
Glass fiber
(c) (d)
Figure 10: Structural morphology of SCGs/epoxy/glass fiber composites, with SCGs of 30 wt % content.
The mechanical properties obtained give similar values with industrial glass fibers is also considered through SEM
to other biosynthetic materials, confirming feasibility of images, mechanical properties, and fire retardancy.
using used coffee composites production facilities From the structural morphology, mechanical properties
[5, 8, 11, 23, 25]. and flame retardancy of materials include different SCGs
In this article, after selecting 30 wt % of used coffee concentrations. 30 wt % SCGs will be selected for further
grounds as appropriate, we included this ratio to process research into fiberglass reinforced composites. The mor-
glass fiber-reinforced epoxy composite materials. To eval- phological structure of the SCGS/fiberglass/epoxy material is
uate higher applicability, the compatibility of coffee grounds shown in Figure 10. From the SEM image in Figure 10, it is
10 International Journal of Chemical Engineering
(a) (b)
Figure 11: SEM images of the residual of composites: 30 wt % SCGs/epoxy/glass fiber material (assessed according to the UL
94-HB method).
35 35
30 30
UL94-HB (mm/min)
25 25
LOI (%)
20 20
15 15
10 10
5 5
0 0
Neat epoxy
30SCGs-epoxy
Glass fiber/epoxy
30SCGs/glass fiber/epoxy
Neat epoxy
30SCGs-epoxy
Glass fiber/epoxy
30SCGs/glass fiber/epoxy
Composites Composites
(a) (b)
Figure 12: Flame-retardant properties of SCGs/fiberglass/epoxy materials, with 30 wt % SCGs and 40 mass parts fiberglass.
shown that the bond between the fiber and the epoxy/SCGs work show that there is almost no effect when mixed at
resin is relatively good; the compatibility here is very good different concentrations. If the application is in the field of
and there is no flaking (Figure 10(a)). Fiberglass fibers are building materials with fire resistance, it is possible to mix
dislodged from the epoxy/SCGs and break when an external other flame-retardant additives to have a resonant perfor-
force is applied to the rough surface (Figure 10(c)). Si- mance [31].
multaneously, crack development in the epoxy matrix was Figures 11(a) and 11(b) show that the ash after burning
prevented by glass fibers (white arrows, Figure 10(d)). has areas of the porous structure (Figure 11(b)); there are
Observation of Figure 10(b) shows that the broken glass fiber dense, continuous areas without pores (Figure 11(a)). This is
has a rough surface that shows the damage with more energy determined by the fine dispersion states of the SCGs, the role
consumption. It proves that when the coffee grounds ad- of the binder between the SCGs, and the epoxy that will
ditive is present, the compatibility does not decrease, but promote flame retardancy.
rather increases. The epoxy-SCGs-glass fiber interface is From the results of Figure 11(b), it was found that when
strongly bonded and interactive. testing the fire-retardant properties of the reinforced ma-
In the case of flame cy, SCGs act as a filler of biological terial with glass cloth, it was found that only the epoxy resin
origin to solve the problem of a green environment. As for and part of the coffee grounds were burned. The glass cloth
the flame-retardant properties, the research results in this remains intact (Figure 11(b), red arrow). In this case, the
International Journal of Chemical Engineering 11
glass cloth acts as a flame retardant. Therefore, the research Conflicts of Interest
on putting used coffee grounds additives into glass fiber-
reinforced composites is a prospect in the future, applying to The authors declare that there are no conflicts of interest
multifunctional structures with high fire resistance or other regarding the publication of this paper.
materials construction material [32].
The flame-retardant properties of glass fiber-reinforced Acknowledgments
SCGs/epoxy materials are shown in Figure 12. From the
results of mechanical properties and flame retardants, it is The authors thank the Faculty of Chemical Technology,
shown that when 30 wt % of SCGs are combined with fibers Hanoi University of Industry, Vietnam, for funding this
glass for processing epoxy-based composites, mechanical work.
properties and flame-retardant properties are kept at the
specified level. Composite materials in the presence of SCGs,
the mechanical properties, and fire retardant are almost References
similar to those of epoxy-based composites reinforced with [1] F. Taleb, M. Ammar, M. Ben Mosbah, R. Ben Salem, and
glass fiber. Therefore, this result has scientific significance as Y. Moussaoui, “Chemical modification of lignin derived from
it can be used. Coffee waste has partially replaced epoxy resin spent coffee grounds for methylene blue adsorption,” Scien-
to make composite materials. tific Reports, vol. 10, no. 1108, pp. 1–13, 2020.
[2] International Coffee Organization, Coffee Market Report April
2021, International Coffee Organization, London, UK, 2021,
4. Conclusions https://ico.org.
[3] S. I. Mussatto, L. F. Ballesteros, S. Martins, and J. A. Teixeira,
In this study, the development of hybrid biocomposites
“Extraction of antioxidant phenolic compounds from spent
based on epoxy and SCGs was completed, the mass percent coffee grounds,” Separation and Purification Technology,
of SCGs used were 30 wt %, 40 wt %, 50 wt %, and 60 wt %. vol. 83, pp. 173–179, 2011.
The following conclusions are drawn from the current [4] L. F. Ballesteros, J. A. Teixeira, and S. I. Mussatto, “Chemical,
investigation: functional, and structural properties of spent coffee grounds
and coffee silverskin,” Food and Bioprocess Technology, vol. 7,
(i) Hybrid epoxy biocomposite material developed
pp. 3493–3503, 2014.
with used coffee grounds as reinforcement for epoxy [5] D. Garcı́a-Garcı́a, A. Carbonell, M. D. Samper, D. Garcı́a-
resins performs well at 30 wt %. Sanoguera, and R. Balart, “Green composites based on
(ii) Test results of mechanical properties of used coffee polypropylene matrix and hydrophobized spend coffee
grounds hybrid epoxy composite material at 30 wt ground (SCG) powder,” Composites Part B, Composites Part
%, tensile strength 44.81 ± 0.10 MPa, flexural B: Engineering, vol. 78, pp. 256–265, 2015.
strength 80.07 ± 0.16 MPa, compressive strength [6] R. Campos-Vegaa, G. Loarca-Pina, H. A. Vergara-Castaneda,
112.56 ± 0.11 MPa, and Izod impact strength of and B. Dave Oomah, “Spent coffee grounds: a review on
current research and future prospects,” Trends in Food Science
8.21 ± 0.19 kJ/m2.
& Technology, vol. 45, no. 24e36, pp. 1–13, 2015.
(iii) Test the flame-retardant properties of the bio- [7] D. S. Scully, A. K. Jaiswal, and N. Abu-Ghannam, “An in-
composite hybrid with 30 wt % of used coffee vestigation into spent coffee waste as a renewable source of
grounds, the limiting oxygen index is 20.8 ± 0.20%, bioactive compounds and industrially important sugars,”
and the rated burning speed according to the UL94- Bioengineering, vol. 3, no. 33, pp. 1–13, 2016.
HB method is 27.02 ± 0.29 mm/min. The results show [8] Y. Leow, P. Y. Michelle Yew, P. L. Chee, X. J. Loh, and D. Kai,
that used coffee grounds do not have much effect on “Recycling of spent coffee grounds for useful extracts and
green composites,” RSC Advances, vol. 11, no. 2682, pp. 1–11,
the flame-retardant properties of epoxy resins.
2021.
(iv) The surface morphology of the SEM images was [9] M. Müller, T. Martin, V. Šleger, M. Hromasová, and V. Kolář,
revealed when mixing 30 wt % of used coffee “Research of hybrid adhesive bonds with filler based on coffee
grounds (SCGs) with epoxy. The obtained bio- bean powder exposed to cyclic loading,” Manufacturing
composites had better structural compatibility at Technology, vol. 20, no. 5, pp. 1–9, 2020.
other mixing concentrations. On the SCGs-epoxy [10] N. Suaduang, S. Ross, G. M. Ross, S. Pratumshat, and
interface, no phase separation is observed. S. Mahasaranon, “Effect of spent coffee grounds filler on the
physical and mechanical properties of poly(lactic acid) bio-
(v) This study offers a solution to use coffee grounds as an composite films,” Materials Today: Proceedings, vol. 17,
environmentally friendly material to improve the pp. 2104–2110, 2019.
amount of waste generated by the coffee industry, [11] E. R. T. Tarazona, L. S. Oliveira, J. C. Rubio, and A. S. Franca
contributing to improving the general properties of Reparation, “Preliminary characterization and mechanical
composite materials in terms of mechanical properties. properties of epoxy composites reinforced with spent coffee
grounds,” in Proceedings of the 2017 8th International Con-
ference on Mechanical and Aerospace Engineering, pp. 1–4,
Data Availability Prague, Czech Republic, July 2017.
[12] C. Wongsiridetchai, W. Chiangkham, N. Khlaihiran et al.,
The experimental data used to support the findings of this “Alkaline pretreatment of spent coffee grounds for oligo-
study are included within the article. saccharides production by mannanase from Bacillus sp.
12 International Journal of Chemical Engineering
GA2(1),” Agriculture and Natural Resources, vol. 52, no. 3, [27] R. Foroutan, S. J. Peighambardoust, S. Samira Hosseini,
2018. A. Akbari, and B. Ramavandi, “Hydroxyapatite biomaterial
[13] T. A. Nguyen, Q. T. Nguyen, and T. P. Bach, “Mechanical production from chicken (femur and beak) and fishbone
properties and flame retardancy of epoxy resin/nanoclay/ waste through a chemical less method for Cd2+ removal from
multiwalled carbon nanotube nanocomposites,” Journal of shipbuilding wastewater,” Journal of Hazardous Materials,
Chemistry, vol. 2019, pp. 1–9, Article ID 3105205, 2019. vol. 413, Article ID 125428, 2021.
[14] T. A. Nguyen, “Mechanical and flame-retardant properties of [28] M. Saberian, J.Li Anita Donnoli, E. Bonderenkoa et al.,
nanocomposite based on epoxy resin combined with epoxi- “Recycling of spent coffee grounds in construction materials: a
dized linseed oil, which has the presence of nanoclay and review,” Journal of Cleaner Production, vol. 289, Article ID
MWCNTs,” Journal of Chemistry, vol. 2020, pp. 1–8, 2020. 125837, 2021.
[15] T. A. Nguyen, T. M. Huong Pham, T. H. Dang, T. H. Do, and [29] S. Li, C. Shi, S. Sun et al., “From brown to colored: polylactic
Q. T. Nguyen, “Study on mechanical properties and fire re- acid composite with micro/nano-structured white spent
sistance of epoxy nanocomposite reinforced with environ- coffee grounds for three-dimensional printing,” International
mentally friendly additive: nanoclay I.30E,” Journal of Journal of Biological Macromolecules, vol. 174, pp. 300–308,
Chemistry, vol. 2020, pp. 1–13, 2020. 2021.
[16] T. A. Nguyen, Q. T. Nguyen, X. C. Nguyen, and V. H. Nguyen, [30] N. Kondamudi, S. K. Mohapatra, and M. Misra, “Spent coffee
“Study on fire resistance ability and mechanical properties of grounds as a versatile source of green energy,” Journal of
composites based on Epikote 240 Epoxy Resin and thermo- Agricultural and Food Chemistry, vol. 56, pp. 11757–11760,
electric fly ash: an ecofriendly additive,” Journal of Chemistry, 2008.
vol. 2019, pp. 1–8, Article ID 2635231, 2019. [31] T. A. Nguyen, “Mechanical and flame-retardant properties of
[17] T. A. Nguyen, “Effects of the amount of fly ash modified by nanocomposite based on epoxy resin combined with epoxi-
stearic acid compound on mechanical properties, flame re- dized linseed oil, which has the presence of nanoclay and
tardant ability, and structure of the composites,” International MWCNTs,” Journal of Chemistry, vol. 2020, pp. 1–8, 2020.
Journal of Chemical Engineering, vol. 2020, pp. 1–6, 2020. [32] N. T. Anh, “Mechanical and flame-retardant properties of
[18] T. A. Nguyen and Q. T. Nguyen, “Study on synergies of fly ash exoxy epikote 240/epoxidized linseed oil composites using
with multiwall carbon nanotubes in manufacturing fire re- fiber-glass,” Mehran University Research Journal of Engi-
tardant epoxy nanocomposite,” Journal of Chemistry, neering & Technology, vol. 39, no. 1, 2001.
vol. 2020, pp. 1–9, 2020.
[19] T. A. Nguyen and T. M. Huong Pham, “Study on the
properties of epoxy composites using fly ash as an additive in
the presence of nanoclay: mechanical properties, flame re-
tardants, and dielectric properties,” Journal of Chemistry,
vol. 2020, pp. 1–11, 2020.
[20] N. H. Mostafa, Z. N. Ismarrubie, S. M. Sapuan, and
M. T. H. Sultan, “Fibre prestressed composites: theoretical
and numerical modelling of unidirectional and plain-weave
fibre reinforcement forms,” Composite Structures, vol. 159,
pp. 410–423, 2017.
[21] N. H. Mostafa, Z. N. Ismarrubie, S. M. Sapuan, and
M. T. H. Sultan, “Effect of equi-biaxially fabric prestressing on
the tensile performance of woven E-glass/polyester reinforced
composites,” Journal of Reinforced Plastics and Composites,
vol. 35, no. 14, pp. 1093–1103, 2016.
[22] C. Militello, F. Bongiorno, G. Epasto, and B. Zuccarello, “Low-
velocity impact behaviour of green epoxy biocomposite
laminates reinforced by sisal fibers,” Composite Structures,
vol. 253, pp. 1–6, Article ID 112744, 2021.
[23] A. Y. Patil, N. Umbrajkar Hrishikesh, G. D. Basavaraj,
G. R. Chalageri, and K. G. Kodancha, “Influence of bio-de-
gradable natural fiber embedded in polymer matrix,” Mate-
rials Today: Proceedings, vol. 5, pp. 7532–7540, 2018.
[24] M. Kostag, K. Jedvert, A. Omar, and El Seoud, “Engineering of
sustainable biomaterial composites from cellulose and silk
fibroin: fundamentals and applications,” International Journal
of Biological Macromolecules, vol. 167, pp. 687–718, 2021.
[25] Y. Thoppil, S. H. Zein, J. S. Yaradoddi et al., “Techno-eco-
nomic analysis and feasibility of industrial-scale biodiesel
production from spent coffee grounds,” Journal of Cleaner
Production, vol. 307, Article ID 127113, 2021.
[26] S. Niyasom and N. Tangboriboon, “Development of bioma-
terial fillers using eggshells, water hyacinth fibers, and banana
fibers for green concrete construction,” Construction and
Building Materials, vol. 283, Article ID 122627, 2021.