GEOPOLYMER AS MATRIX APPLIED IN COMPOSITES WITH

NATURAL FIBERS

E. A. S. Correia1, M. E. O. Alexandre2
1
Universidade Federal da Paraíba - UFPB, João Pessoa/PB – Brazil
2
Instituto Federal de Educação, Ciência e Tecnologia da Paraíba-IFPE, João Pessoa, Brasil

ABSTRACT
The development of new technologies has boosted searches for obtaining competitive and
ecologically viable materials cost benefit attractive to the market. The main goal of this work
was to develop and study geopolimérica matrix composites reinforced with fibres of vegetable,
for application as alternative non-conventional material in several areas. Noted the technical
feasibility of such materials through the results achieved when subjected to mechanical and
physic-chemical associated with the modern techniques of microestruturais characterizations.
The bursting and compression module, array and composite material, was compatible with the
minimum established resistance and validated in the market when compared to the similar hues
screeds. When subjected to pressure, low energy composites showed outstanding degree of
packaging, lower porosity, resistivity and better ductility and excellent stage of deformation.

Keywords: Geopolymer1, Natural Fibers2, Composites 3.

1. INTRODUCTION

Advances in the development of composite materials have brought significant results as to

its applicability (MATTOSO,1996). However it is notable that some reinforcements traditional
expose their limitations and compromises its mechanical performance. This is because with time,
these materials lose their tenacity and endurance due to the alkalinity of the array. The relentless
quest for the most versatile building materials, with greater economic potential and low cost,
have targeted searches to work with natural fibres (AZIZ, 1987), which in addition to improving
the mechanical performance of the array, has good resistance to chemical instability establishing
a greater resistance to the matrix, however still exists the need to find satisfactory conditions for
optimizing the interface, as well as enhance operationalization in productive scale.
The technique of applying natural fibres such as strengthening agent in arrays slabs have
been used since the mid-1940s when James Hardie and Copy Pty Ltd has replaced asbestos by
pulp cellulose as strengthening agent in cement-based laminates. In Brazil, this technique began
to be developed by the research and Development Center in Bahia, applying natural fibers in
concrete matrix (SIVARAJA, 2009). This new line of research brings to light a new variable for
composite materials, opening up new fields of application, in addition to using renewable
resources, which contribute to the reduction of contamination of the environment.
 Compound as aluminosilicates form a matrix resistant high temperature (BARBOSA,2003;
COLEMAN,2005), have high power to accession and satisfactory ability to cure at room
temperature, the Geopolymer (DAVIDOVITS,2002; DUXTON,2006) like most arrays screeds,
has a low mechanical strength, which limits its scope. To obtain a significant gain in strength,
especially when subjected to mechanical tests, inserting vegetable fiber composite qualities
raises and extends its scope.

2. MATERIALS AND METHODS

2.1. Materials

As a source of silicon and aluminum matrix used the supplied by Caulisa SA kaolin, kaolin
processing industry located in the municipality of Juazeirinho, PB; the vegetable fibres were
provided by COSIBRA – Company Sisal of Brazil. Sodium silicate was provided by
Pernambuco Chemistry S/A with a silica (SiO2/Na2O ratio, by mass) roughly 2.5 and pH around
13.

2.2. Synthesis process

The process of synthesis occurred in two steps. In the first stage was calcined
kaolin(DUXTON2006), in a muffle furnace at 750 ° C for 2 h, so that the entire exercised by
kaolinite in metacaulinita(PALOMO,2003; VAN JAARSVELD,2002), then use the sodium
silicate in appropriate proportion with Activator alkaline, the bubbles have been eliminated
through intermittent vibration. In the second step the fibers with approximately 60 mm in length
were arranged in two layers of 3 mm and interspersed by matrix in the ratio of 3%, until filling
mold, this process was repeated until all layers were released by filling in a uniform manner
throughout the mold cavity.
Again, the bubbles have been eliminated by placing the template fully populated on a
shaking platform. After the molding process, shapes underwent a process of cure in an oven at 55
° C for 48 hours. After this period, the mold rested for over 48 hours under ambient temperature,
so that ultimately were subjected to the tests of characterization.

(a) (b)
Figure 1: Three-point bending test during and after the break
 (a) (b)
Figure 2: Tests simple and diametric compression

2.3. Characterization of materials

The characterization of materials, precursors and of the bodies evidence instrumental

techniques was carried out as described below:-the determination of the moisture content of the
fibres(LADCHUMANANANDASIVAM,2005; GHAVAMI,1999) of the Agave Sisalana was
conducted according to standard (American Society for Testing and Materials) ASTM 1413-76;
the analyses via wet (titration) were held in order to determine the concentration of acidic groups
of samples; The content of water-soluble extractives was determined by standard TAPPI T212
om-98. -Images of the surfaces of vegetable fibres were obtained from secondary electrons and
Spread in a scanning electron microscope JSM 5800 LV a JEOL brand.
The accelerating voltage of the electron beam generated from a tungsten filament was equal
to 10 kV.
Compression test, conducted in the laboratory of Rural Constructions – Seals/UFCG, was
used the Universal type compression machine. Test compression was accomplished using the
cylindrical body of evidence with the following dimensions: 5 cm in diameter and 10 cm in
height, as in Figure 2. The test of resistance to traction in bending Universal Machine was used
for the testing of 03 points, as shown in Figure 1, with the following schedule: 03 batches with 5
bodies of evidence each with dimensions 4cmx4cmx16cm, at the age of 30 days, both tests with
speed 2 mm s-1.Chemical analysis was held at the Rapid laboratory Scale of UFPB in Sequential
x-ray Fluorescence Spectrometer XRF-1800 model of Shimadzu.

3. RESULTS AND DISCUSSION

3.1. Geopolymer Formulations of folder

The chemical composition(PALOMO,2003) of metacaulinita activated

alkaline(FERNÁNDEZ-JIMÉNEZ,2005; GLUKHOVSKY, 1980; and GOMES,2007) with
sodium silicate PQ-1.65, was analyzed by x-ray Florescence (XRF) in laboratory scale rapid
UFPB.
 Table1: Chemical compositions of the Geopolymer folder.

constituents SiO2 Na2O Al2O K2O Cl Fe2O3 CaO TiO2 SO3 P2O5 NiO
% 72.7895 12.9737 12.8665 0.4329 0.3769 0.3008 0.1291 0.0537 0.0409 0.0295 0.0064

3.2. Physico-chemical properties of fibres

As the Lignocellulosic are highly hygroscopic materials is very important to the

determination of the moisture content of The soluble in cold water include organic salts, sugars,
resins and tannins.

Table 2: Physico-chemical properties of vegetable fibres

Parameters Agave Sisalana Ananás Comosos

Moisture content (%) 10,48 10,11
Acidic groups (mol/l) 0, 00186 0,00146
Water-soluble extractives (%) 6,84 7,19
pH 7,69 6,96
Density (g/m3) 1,32-1,45 1,30-1,44
Lignin (%) 6-11 5-12
Cellulose(%) 65-73 70-83
Hemicellulose(%) 13,33 18
Diameter (μm) 50-300 50-105
Hygroscopicity (%) 10-13 9-11
L/D 103 460
Angle expiral(°) 20 15
Length (cm) 30-140 20-120

One of the limitations of plant fibers in the production of composites is the high hygroscopicity
and the high content of soluble extractives present on the surface, which hinders the physical
interaction of the matrix with the reinforcing agent, the low density of pineapple fiber in relation
to fiber of agave, provides a high aspect ratio (L / D), favorable for the anchoring of the
pineapple fiber in the geopolymer matrix, another positive aspect is the high lignin content in this
fiber, which acts as plasticizing agent, optimizing the stability of the interface.

3.3. Mechanical strength properties

3.3.1. Three point bending tests

Been tested 45 bodies of evidence, 15 in 3 batches of five and 30 in 6 batches of five

following batches for array, matrix, with agave sisalana and matrix with pineapple comosos at a
ratio of 3% by volume for randomly distributed reinforcing agent with approximately 25 mm in
length. Bending tests were conducted at three points on a machine SHIMADZU AG-X , with
load cell of 50 kN, where the body of evidence was positioned with the load applied at the center
of even with going to encyclopedia of 120 mm and with a speed of 2 mm/min, defined by NBR
13279 (2005) and temperature about 25 °C. Figure 1 (a) shows the outline of the test. The results
obtained are represented in the form of graph (Stress x Strain), figures 3 and 4.

Média
Stress (MPa)

Strain (%)
Figure 3: Array behavior in three-point bending tests.

Média
Média
Stress (MPa)

Tensão (MPa)

(a) Strain (% ) (b) Strain (%)

Figure 4: Behavior of composites with agave sisalana (a) and with pineapple comosos (b) for the three points
bending tests.
 Compression tests were conducted on a machine SHIMADZU AG-X 100, with load cell of
100 kN, where the bodies of evidence were positioned as Figure 2 (a) (b) and with a speed of 2
mm/min, defined by NBR 7215 (1991), and temperature about 25 ° c. The results obtained are
represented in chart form (Stress x Strain), figures 5, 6,7 and 8.

3.3.2. Axial compressão tests

Média
Stress (MPa)

Strain(%)

Figure 5: Average curve for simple compression test with the array.

Média Média
Stress (MPa)

Stress (MPa)

(a) Strain(%) (b)Strain(%)

Figure 6: Average curves for simple compression tests with composites of agave sisalana pineapple (a) and
ananás comosos (b)
3.3.3 Diametral compression test

Média
Stress (MPa)

Strain(%)

Figure 7: Average curve to diametral compression test with the array.

Média Média
TStress (MPa)

TStress (MPa)

(a) Strain (%) (b) Strain (%)

Figure 8: Average curves for compression tests with diametral composites agave sisalana pineapple (a) and
ananás comosos (b)
 Figure 3 shows that the mean value obtained for bending stress was 1.4Mpa for matrix,
a reasonable value for the standards found in the literature for ceramic materials, in Figure 4, we
can see values between 2 and 3 MPa for reinforced matrices with plant fibers, the values
obtained for rupture moduli are also expressive and occur with a higher deformation rate than the
matrix without reinforcing agent.

3.4. Micro-structural studies

Figure 5: Microstructure of the surface of the Figure 6: Microscopy in composite with

fibres of sisal in natura. leaf of sisal fiber in Geopolymer.

Figure 7: Microstructure of the surface of the Figure 8: Microscopy in composite with

fibres of ananás in natura. leaf of ananás fiber in Geopolymer

The morphological changes observed in the matrix fibers were observed through SEM, in
this work we used in natura fiber because the matrix already has high alkalinity (pH = 13), so we
avoid the embrittlement of the reinforcing agent by excessive chemical treatment; in Figure 6,
we observed empty spaces in the fiber-matrix interface, but these spaces are minimized in Figure
8, where pineapple fiber was used as reinforcement, this occurs due to the low content of soluble
extractives present in this pineapple fiber, which is lower in around 11%.
3.5. Termogravimétricas Analyses
shows the TG / DTG curves
14 0,3
for sisal fibers in natura and
TGA - FLS DTG-FLS treated with NaOH (2%) for
TGA - FLSM DTG-FLSM
12 48h and exposed to air for
0,2 15 days, we can see two

Deriv.Weight(% mg/min)
10 stages of decomposition of
10-12% water, 50- 65%
Weight (% mg)

0,1
8 polysaccharides and about
30% residues. We observed
6
0,0 from the results that the
untreated sample had a
4
higher decomposition rate
-0,1
around 300-400 ° C.
2

0 -0,2
0 100 200 300 400 500 600 700 800 900

Temperature (°C)

Figure 9: TG and DTG curves for fibers of agave sisalana in natura and mercerizadas

FLS
60
FLSM A two-stage exothermic
peak at 360 ° C and 460 ° C
50 at the end of the
40
experimental period was
observed in the DTA curve
30
(Figure 10) for sisal fiber, an
Weight (% mg)

20 endothermic event between

65-75 ° C and another in the
10
400-420 ° C range. transition
0 temperature, marked thermal
degradation occurred
-10
between 300-400 ° C and
-20 coincides with TG / DTG
0 100 200 300 400 500 600 700 800 900
analysis.
Temperature (°C)

Figure 10: DTA curves for agave sisalana in natura and mercerizadas
 shows the TG / DTG curves for
coman pine fiber, under the
14 0,10
same conditions previously
TGA - FLA DTG - FLA reported, where we can observe
TGA - FLAM DTG - FLAM
two stages of decomposition,
12 0,05
the first at 60 ° C, referring to
the loss of water and the second
10

Deriv.Weight(%/min)
0,00 a365 ° C, referring to the main
decomposition. A residue of 1.5
Weight (%)

8
-0,05 to 2.5% was noted at 800 ° C.
The DTG curve presented two
6
-0,10
stages of decomposition, the
first one at 60 ° C,
4 corresponding to the heat of
-0,15
vaporization and the second at
2 355 ° C, where the
-0,20 decomposition was maximum.
0 100 200 300 400 500 600 700 800 900
Temperature (°C)

Figure 11: TG and DTG curves for fibers of ananás comosos in natura and mercerizadas.

20
DTA - FLA The analysis of the DTA curve
DTA - FLAM
showed small positive thermal
Temperature difference (°C/mg)

events and scarce significant

0 calorific points according to
figure 12, the in natura fiber
presented discrete and negative
exothermic results, however for
-20
mercerized fibers we observed a
maximum peak around 415 ° C.

-40

0 300 600 900

Temperature (°C)

Figure 12: DTA curves for ananás comosos in natura and mercerizadas
4. CONCLUSIONS

The presence of plant fibers in the matrix gives a tendency of growth in the flexural
strength, until an optimal content, with later reduction of this property, the capacity to absorb
energy (tenacity) was the most sensitive property influenced by the addition of the fibers. The
composites with coman pine fibers presented high values for specific energy (toughness) and
flexural strength in relation to the specimens with agave sisalana fibers, for all the stresses used.
This is probably due to the higher number of fibers per unit volume of the matrix, because the
coman pineapple fibers have a larger aspect ratio (L / D) due to the smaller diameter and the
higher fiber concentration in the interface region, higher lignin content of these fibers also
provides greater stiffness and elasticity.
A thermoanalitic curves showed that the fibers have stability around 300ºC, and can be
applied in refractory materials, thermal and acoustic insulation. The fibers of pineapple leaf have
great potential in the application in mechanical engineering in composite materials for the
manufacture of carcasses of automobiles, bumpers, car panels, in boats, water boxes, telephone
booth, mailboxes, garbage dump , etc., still arouse particular interest of the civil construction for
geopolymer matrix composites developed for ecologically correct interior design.

5. ACKNOWLEDGMENTS

We acknowledge all the partners and friends who collaborated to the development that job,
providing us every necessary material to confection our specimens between them, the COSIBRA
S.A., Caulisa S.A. and Chemistry S.A. Acknowledge too, all the laboratories who collaborated to
analyzes and characterizations our specimens made in the LABEME and LSR in the Federal
University of Paraíba. The characterization was made in the LACOM on UFPB, and a
mechanical test was executed in mechanical laboratory of the IFPB and Rural Constructions
laboratory – LaCRA/UFCG.
.

6. REFERENCES

Aziz, M. A., Paramasivam, P., Lee, S. L., “Natural fibre reinforced composite building materials
for low-income”, In: Symposium on Building Materials for Low-Income Housing, p. 129-137,
Bangkok, Thailand, 1987.

Barbosa, V.F.F. & Mackenzie, K.J.D., Thermal behaviour of inorganic geopolymers and
composites derived from sodium polysialate. Mater. Res. Bull. 38, 319-331 (2003)

Coleman, N. J.; Page, C. L. “Aspects of the pore solution chemistry of hydrated cement pastes
containing MK: lime hydration”. Cement and Concrete Research, Oxford, v. 27, n. 1, p. 147-154,
1997. Colloids and Surfaces A: Physicochem Eng Aspects, 268, pp. 1–6, 2005.
Davidovits, J., “Properties of geopolymer cements”. Proceedings First International Conference
on AlkalineCements and Concretes, Kiev, Ukraine, volume 131, 1994. “derived from sodium
polysialate”. Materials Research Bulletin, 38, pp. 319–331, 2002.

Duxton, P. “The structure and thermal evolution of metakaolin geopolymers”. Thesis of Doctor
of Philosophy in Engineering of Department of Chemical and Biomolecular Engineering, the
University of Melbourne, 2006.

Fernández-Jiménez, A.; Palomo, A.; Criado, M. “Microestructure development of alkali-

activated fly ash cement: a descriptive model”. Cement and Concrete Research, v. 35, p. 1204-
1209 (2005).

Ghavami, K., Toledo Filho, R. D., Barbosa, N. P., Behavior of composite soil reinforced with
natural fibres.Cement and Concrete Composite Vol. 21, p. 39-48,1999.

Glukhovsky, V.D.; Rostovskaja G.S.; Rumyna, G.V.; Rostovskaja. “Characterization of

Environmentally-Friendly Alkali Activated Slag Cements and Ancient Building Materials .” 7th Int.
Cong. Chem. Cem., Vol.3, Paris, Theme 5, pp. 164–168 (1980).

Gomes, K.C.; Torres, S.M.; de Barros, S.; Barbosa, N.P. “Geopolymer Bonded Steel Plates.
ETDCM8- 8th Seminar on Experimental Techniques and Design in Composite Materials”. 3-6
October 2007 – Sant’Elmo Beach Hotel – Castiadas – Costa Rei – Sardinia (Italy). (2000b).

Hardjito, D. and Rangan, B. (2005). Development and properties of low-calcium fly ash based
geopolymer concrete. Perth, Australia: Curtin University of Technology.

Mattoso, L.H.C.; Ferreira, F.C.; Curvelo, A A S. “Sisal fiber: morphology and applications in
polymer composites”, In: International Symposium on Lignocellulosics-Plastics Composites, 1,
São Paulo-SP, Mar. 1996,Proceedings.

Nguyen, V., Bui, D.T. and Dang, V.T. (2008). Recent research geopolymer concrete. The 3rd
ACF International Conference-ACF/VCA.

Palomo, A.; de La Fuente, J.I.L. “Alkali-activated cementitious materials: Alternative matrices

for the immobilisation of hazardous Wastes” - Part I. Stabilisation of boron. Cement and
Concrete Research 33(2): 281-288. (2003).

R. Ladchumananandasivam, M. E. DE O. Alexandre, L.H. Carvalho and W. S. Cavalcanti,

“Effect of Water Sorption in Unsaturated Polyester/ Pineapple Leaf Fibre (PALF) Composites”,
International Composite Conference: Developments in Composites:Advanced,Infrastructural,
Natural & nano-composites.

Rowell, R. M.; Sanadi, A. R.; Caulfield, D. F.; Jacobson, R. E. Utilization of natural fibers in
plastic composites: Problems and oppurtunities. In: Leâo, A. L.; Carvalho, F. X.; Frollini, E.
Lignocellulosic-Plastics Composites, São Paulo: USP/UNESP, p.21-51, 1997.
Satyanarayana, K., Kulkarni, A., Sukumaran, K., Pillai, S., Cherian, P. and Rohatgi, P. 1983.
Performance of banana fabric-polyester resin composites. In: Composite structures. Proceedings
of the International Conference, London, Applied Science. Ed. Marshall, I.H., pp. 535-48.

Sivaraja M, Kandasamy S. Characterization of natural fibres as concrete composites forenergy

absorption. International Journal of Materials and Product Technology, Nos. 1-4, 36(2009) 385
95.

Van Jaarsveld, J. S., Van Deventer, J. J., & Lukey, G. (2002). The effect of composition and
temperature on the properties of fly ash- and kaolinite-based geopolymers. ChemicalEngineering
Journal, 89(1-3), 63-73. Retrieved from http://www.sciencedirect.com/science/article/B6TFJ
45CW8XH-3/2/23e663b72b8e26b2ff2f45ba3d875405