Fibers and Polymers 2015, Vol.16, No.

1, 181-187 ISSN 1229-9197 (print version)

DOI 10.1007/s12221-015-0181-z ISSN 1875-0052 (electronic version)

Leather Fibres as Reinforcement for Epoxy Composites: A Novel Perspective

Rethinam Senthil, Sathyaraj Weslen Vedakumari, Thiagarajan Hemalatha, Bhabendra Nath Das1, and
Thotapalli Parvathaleswara Sastry*
Bioproducts Laboratory, Central Leather Research Institute, Chennai 600 020, India
1
Shoe Design and Development Centre, Central Leather Research Institute, Chennai 600 020, India
(Received May 6, 2014; Revised August 26, 2014; Accepted September 1, 2014)

Abstract: Developing composite materials with better mechanical and electrical properties is the need of hour, particularly in
developing and third world countries. Keeping this objective in view, composite material was prepared, in sheet form,
containing leather fibres (LF), isolated from used leather products. Reinforced composite material was produced using LF as
reinforcing material for epoxy resin (ER) laminates. To impart additional strength, charcoal carbon nano particles (CCNP)
were incorporated (LF:ER:CCNP) in the composite. Fourier transform infrared spectroscopy (FTIR) and thermo gravimetric
analysis (TGA) of the samples have revealed the chemical nature and thermal stability of the composites, respectively, while
SEM pictures revealed the fiber-matrix interface. LF:ER:CCNP possessed good mechanical properties viz., tensile strength,
elongation at break (%), flexural strength, hardness etc, in addition to its electrical property. Hence, the composite possess
multifunctional applications, it addition to its cost effectiveness and environmental pollution abatement.
Keywords: Leather fibres, Epoxy resin, Reinforced composites, Charcoal carbon nano particles, Tensile strength

Introduction from used leather wastes, for the manufacture of leather

The use of natural cellulosic fibres, viz., flax, hemp, sisal,
kenaf, banana and jute, is gaining promising attention in
recent years for their use in polymer composites production,
as an alternative to traditional fibres such as glass, carbon,
and aramid [1]. According to the latest estimates 20-30 %
leather solid waste is generated by the leather products
industry. Also, enormous amount of pairs of chappals, shoe
waste and end products of leather industry constitute to
major solid wastes [2]. Improper disposal of these leather
wastes causes environmental pollution, therefore proper
optimized utilization of these wastes into valuable end
products will be a promising solution [3,4]. Leather waste is
composed of extra-cellular matrix, highly ordered type I
collagen fibre [5]. Hence, in this study we have isolated fibre
from waste leather. This leather fibre (LF) is different from
conventional fibres such as plant, glass or carbon in its
physico-chemical and mechanical properties [6,7]. Thermal
stability and uniform separation of leather fibre contribute to
its enhanced mechanical properties [8].
Leather fibres were taken up for this study owing to their
inherent eco-friendly nature, low cost, low density, bio-
degradability, recyclability and significant processing advantages,
in particular equipment abrasion, energy consumption,
pollutant emission, dermal and respiratory irritation are all
reduced. Major limitations in the use of leather fibres are
their short length, high moisture absorption and low microbial
resistance [9]. Sastry et al. [10] have reported the preparation of
leather products such as insole, chappals, key chain and dog
chews etc from tannery solid leather waste, while Senthil et
al. [9] have demonstrated the preparation of leather boards
*Corresponding author: sastry56@gmail.com
products.
In recent years, a lot of research is focussed on reinforcing
thermoplastic and thermo setting polymers with organic and
inorganic nano-sized particles for their use in the field of
automotive engineering, aerospace development, marine
technology, electronic devices, construction industries etc.
Epoxy resin (ER) is a widely used thermo setting material.
Reinforcement of epoxy resin with different types of particles
can markedly change its mechanical, thermal, and tribological
properties [1,11]. Natural fibre composites such as hemp
fibre-epoxy, flax fibre-polypropylene (PP), and china reed
fibre-PP are particularly attractive in automotive applications
because of lower cost and lower density [12]. Leather fibre,
which is a thermal insulative material, can act as a better
reinforcing material when combined with epoxy resin, and
this composite can be used for construction purposes.
Carbon-based nano particles (CNP) have attracted significant
attention due to their unique physical, chemical, and electrical
properties. Potential applications of CNPs extend into everyday
settings viz., building blocks in photovoltaic and optoelectronics
[13], as fillers in composite materials to improve structural
and electrical properties [14], sensors [15] etc. Charcoal
carbon nano particles, possess good electrical conductivity
and when combined with reinforced material it can be made
into weightless film, which can be used in chips, sensor
materials etc.
The objective of this study is to prepare a reinforced
composite material (RCM), in sheet form, containing epoxy
resin and leather fibres, impregnated with charcoal carbon
nano particles (LF:ER:CCNP). This product was characterized
for its physico-chemical properties using FTIR, TGA and
SEM. Mechanical properties such as tensile strength, flexural
test, impact test and hardness properties were assessed. In

181
182 Fibers and Polymers 2015, Vol.16, No.1
addition, electrical conductivity of the composite was also
analysed.
Experimental
The epoxy-LY 556 and hardner-HY 951 were purchased
from M/s. Java Enterprises, (Chennai, India). Leather wastes
were collected from Central Leather Research Institute,
Chennai, India. Other chemicals used were of analytical
grade.
Preparation and Characterisation of LF
Waste leather shoes uppers, leather chappals, leather
wastes form leather product industry etc were collected.
Only the leather portions of these waste leather products
were carefully separated and it was dried under sunlight for
2 h. These leather wastes were cut into small pieces using
Swing ARM Clicker (Porielli S.20, VIGEVANO-ITALIA)
(Figure 1(a)). The cut leather waste was converted into leather
fibre (LF) with the help of fibrizer machine (SDL868, USA)
(Figure 1(b)). Coarse and uneven fibres were removed using
mechanical stainless steel sieve [9].
LF was characterized for its mechanical properties and
surface morphology. Mechanical properties such as tensile
strength (MPa) and percentage of elongation at break (%)
were measured using Universal testing machine (INSTRON
model 1405) at an extension rate of 5 mm/min. Scanning
electron microscopic (SEM) analysis was carried out on
LEICA stereo scan 440 instrument. The samples were coated
Figure 1. Instruments used to prepare leather fibre; (a) swing arm
clicker machine and (b) fibrizer machine.
Rethinam Senthil et al.
with gold ions using an ion coating unit. The micrographs
for LF were taken at different magnifications by operating
the instrument at 15 kV accelerating voltage.
Preparation and Characterisation of CCNP
Charcoal was subjected to ten stage milling process with a
seven bladed universal rice milling machine at room
temperature. After milling, the milled powder was filtered
(420 micron) twice and the powder was collected in a
chamber. This procedure reduced the grain size. Powdered
sample from charcoal was subjected to SEM and energy-
dispersive X-ray spectroscopy (EDX) analysis, using LEICA
stereo scan 440 instrument.
Preparation of RCM
Fabrication of RCM was done using leather fibre, epoxy
resin and charcoal carbon nano particles (LF:ER:CCNP).
Fabrication is the process of manufacturing by shaping pliable
raw material using a rigid frame or model called a pattern.
Epoxy resin and hardener were mixed in 100:33.3 ratio [1]
and 2 % CCNP was added to this matrix [16]. ER and CCNP
was agitated properly using magnetic stirrer at room temperature.
Release agent (poly vinyl acetate) was applied on the glass
mould and it was allowed to dry for few seconds. The epoxy
mixture was poured on to this surface, upon which two
layers of LF were added. LF was introduced into the mould
layer by layer. Excess amount of mixture was removed using
rollers. Mould was closed and pressure was applied using
250 kg. After 12 h of curing at room temperature, the mould
was removed and was post cured for 3 h at 140 oC [17]. The
composite (RCM) was removed from the mould and it was
cut for required dimensions as per ASTM standards.
Three specimens were fabricated by compression moulding
(i) only epoxy resin (ER) (ii) leather fibre (2 layered) with
epoxy resin composite (LF:ER) (iii) leather fibre (2 layered),
epoxy resin and carbon nano particles composite (LF:ER:
CCNP).
Characterization
Fourier transform infrared (FTIR) measurements were
carried out to determine the formation and changes in the
functional groups on the prepared LF:ER:CCNP composite.
The spectrum was measured at a resolution of 4 cm-1 in the
frequency range of 4000-500 cm-1 using Nicolet 360 FTIR
Spectrometer. Thermo gravimetric analysis (TGA) was used
to analyze the thermal stability of LF:ER and LF:ER:CCNP
composites. All the measurements were performed using
High Resolution 2950 TGA thermo gravimetric analyzer
(TA Instrument). Samples weighing between 10 and 20 mg
were placed in a platinum pan and test were carried out in a
programmed temperature range of 0 to 800 oC at a heating rate
of 5 oC/min under nitrogen atmosphere at flow rate of 50 ml/
min. SEM and EDX analysis of LF:ER and LF:ER:CCNP
composites were done using scanning electron microscope
Leather Fibres as Reinforcement for Epoxy Composites Fibers and Polymers 2015, Vol.16, No.1 183

(SEM Model LEICA stereo scan 440). Mechanical properties overcome the limitations of LF (such as short length), by
were analysed using dumb-bell shaped ER, LF:ER and incorporating CCNP in ER:LF, which will act as fillers [19]
LF:ER:CCNP composites of 4 mm wide and 10 mm length. and improves the functional properties of polymer composite.
Tensile strength (MPa) and elongation at break (%) were
measured using a INSTRON (model 1405) at an extension
rate of 5 mm/min. Flexural strength was also assessed using
Universal testing machine (UTM model Autograph DCS-
5000, Shimadzu). Impact strength was measured according
to ASTM D256-04 standards. Hardness test was assessed
using Brinell Hardness Testing machine (model D638). The
specimens were tested under the loading condition of 60 kgf.

Electrical Characterization
The electrical conductivity of the fabricated LF:ER:CCNP
composites was analysed using cyclic voltmeter model (CHI
600D). The experiments were carried out at room temperature
[18].

Results and Discussion

The study uses a novel approach to prepare multifunctional

reinforced composite materials using solid leather wastes.
Though polymer composites are prepared using various
fibres, this study is a maiden attempt to use leather fibre for
reinforcement in polymer composites. The prepared LF:ER:
CCNP composite possessed better mechanical and electrical
properties as well as smooth surface. The study aims to

Figure 3. (a) SEM image (magnification 300×) and (b) EDX

analysis of CCNP.

Figure 2. Leather fibres; (a) photographic image and (b) SEM Figure 4. Photographic images of (a) LF:ER composite and (b)
image. LF:ER:CCNP composite.
184 Fibers and Polymers 2015, Vol.16, No.1
Preparation and Characterisation of LF
LF (Figure 2(a)) was prepared using the fibrizer machine.
The fibre size was 2.0 cm in length and 0.7 mm in diameter
[9]. Since the leather fibre consisted more of collagen, it had
a tensile strength of 0.38+0.01 MPa and elongation at break
(%) of 0.38+0.04. SEM images revealed the smooth surface
morphology of LF (Figure 2(b)).
Preparation and Characterisation of CCNP
Under SEM, charcoal powder appeared as irregular
shaped particles with size ranging from 30-100 nm. Such
small size proves that they are under nano scale form (Figure
3(a)). The EDX test results (Figure 3(b)) showed that the
CCNP specimen contaied a large amount of carbon (96.06 %)
and remaining natural minerals such as Na, Mg, Ca, Cl, K,
Nb and traces of silicon.
Preparation of RCM
RCM (LF:ER) prepared without CCNP was smooth and
its colour depended upon the source of LF (Figure 4(a)),
Figure 5. FTIR of (a) ER and (b) LF:ER:CCNP.
Figure 6. TGA of (a) LF:ER and (b) LF:ER:CCNP.
Rethinam Senthil et al.
while LF:ER:CCNP (Figure 4(b)) was black in colour due to
the incorporation of CCNP and it also possessed smooth
surface and was weightless in nature.
Characterisation
The FTIR spectra of ER (Figure 5(a)) exhibited peaks at
1754 cm-1 and 1100 cm-1 representing C=O and C-O stretching
vibrations respectively. Peak at 910 cm-1 represented the
stretching of C-O of oxirane group of epoxy resin. In addition,
LF:ER:CCNP (Figure 5(b)) composite contained peaks at
3440 and 1600 cm-1 corresponding to amine N-H stretch and
NH bending of proteins respectively, present in leather fibre.
Peaks at 1700 cm-1 are due to the aromatic C=C bending of
the epoxy resin.
TGA result depicted the thermal stability of the composites
LF:ER (Figure 6(a)) and LF:ER:CCNP (Figure 6(b)). A two
step weight loss was observed around 300 and 480 oC. The
initial weight loss around 150 oC could be attributed to the
loss of water molecules. Collagen present in LF degraded at
300-340 oC [20] and degradation of other organic compounds
Leather Fibres as Reinforcement for Epoxy Composites
Figure 7. SEM images of (a) LF:ER and (b) LF:ER:CCNP.
Figure 8. EDX spectra of (a) LF:ER and (b) LF:ER:CCNP.
occured between 270 and 500 oC. Epoxy resin, the thermally
stable component of the composite degrades between 350 to
450 oC [21], while a residual matter of about 10 % remained
indicating the complete decomposition of the composite.
The surface morphology of LF:ER (Figure 7(a)) and
LF:ER:CCNP (Figure 7(b)) was revealed by SEM. Better
adhesion between LF and epoxy matrix was observed in
LF:ER composites, while smooth surface was observed on
LF:ER:CCNP, which might be due to coating of carbon nano
particles on to the leather fibres. EDX analysis (Figure 8(a)-
(b)) of the composites determined the local distribution of
Fibers and Polymers 2015, Vol.16, No.1 185
the elements based on weight percentage and atomic weight
percentage. Carbon was the significant element in the
composites due to their organic nature. The atomic weight
percentage of carbon (68 %) was higher in LF:ER:CCNP
composites due to the incorporation of CCNP, compared to
LF:ER composite.
Mechanical properties of polymer composites play a
major role in determining their application perspectives
(Table 1). Keeping this point in view, tensile properties of
the ER, LF:ER and, LF:ER:CCNP were studied. LF:ER:
CCNP displayed maximum tensile strength and elongation
186 Fibers and Polymers 2015, Vol.16, No.1 Rethinam Senthil et al.

Table 1. Mechanical properties of the epoxy resin and composites

Tensile strength Elongation Flexural strength Impact Hardness Youngs Flexural
Samples
(MPa) at break (%) (MPa) strength (J/m2) (BHN) modulus (GPa) modulus (GPa)
Epoxy resin (ER) 26.81±5.63 19.33±2.10 211±10.14 1.51±0.18 48±2 0.7±0.02 2.53±0.11
LF:ER composite 104.24±1.93 87.96±3.42 681.33±11 5.41±0.38 55±2 2.54±0.04 3.22±0.07
(leather fibre:epoxy resin)
LF:ER:CCNP 115.94±3.53 103.53±5.22 806.66±20.81 8.55±0.35 57±3 3.1±0.1 4.8±0.19
(leather fibre:epoxy resin:
charcoal carbon nanoparticles)
Data are presented as mean± standard deviation (SD) of three individual experiments (n=3).

at break (%) values compared to the rest. This enhanced

strength may be due to the impregnation of CCNP on LF:
ER. The flexural test results of the composites revealed that
there was not much difference between LF:ER and LF:ER:
CCNP. LF:ER:CCNP exhibited higher impact strength
compared to the other 2 samples, which could be due to the
reinforcing effect of LF and CCNP. Hardness, the resistance
of a material to permanent indentation, was measured for the
composites. From the results, it was evident that there was
not much difference in Brinell hardness value among the
composites, since epoxy resin matrix is the major contributor of
hardness. The mechanical properties of short fiber reinforced
composites are highly determined by the fiber-matrix
interface [1]. Collagen in leather fibres has become integral
Figure 9. Cyclic voltammogram of LF:ER:CCNP.
parts of epoxy matrix and has modified the fiber-epoxy
interface. From the above results, it is clearly evident that
LF:ER:CCNP possessed better mechanical properties for use Preparation of leather fiber reinforced epoxy composites is
in various applications. Inclusion of CCNP has improved the an attempt towards biodegradable thermoplastic matrices.
mechanical properties of the composites, because these Also, since the leather portion used in the composites is
nanoparticles provide reinforcement effect with a combination derived from waste leather materials, they would be profitable
of high stiffness and toughness. This effect is probably compared to conventional composites and they possess
caused by changes in the morphology of the polymer matrix environmental significance as well. Since these composites
due to the presence of nanoparticles. It is generally agreed possess better mechanical properties they may find applications
that the large surface to volume ratio of the nanoscale inclusions in interior decorations.
play significant role in improving the mechanical property
of the composites [22]. The formation of a nanostructured Conclusion
network of finely dispersed particles, which strongly binds
to the polymer is probably responsible for the reinforcement The aim of this study was to investigate the potential of
[23]. Kotsilkova et al. [17] reported that the dispersion leather fibres/charcoal carbon nano particles as reinforcement
microstructure of carbon nanoparticles play a main role in materials for epoxy composites. The novelty of the study lies
the reinforcement of nanocomposites. The network structure in the incorporation of leather fibres, first of its kind, for the
and the interface polymer layer, surrounding nanoparticles preparation of reinforced epoxy composites. The study also
increases the relaxation strength and results in improvement envisions the production of cost effective composites, by
of mechanical properties. conversion of wastes into wealth, simultaneously decreasing
the environmental pollution. Leather fibres acted as better
Electrical Characterization reinforcement material for epoxy resin and impregnation of
Carbon, which is known to possess good electrical con- CCNP enhanced the strength as well as electrical conductivity
ductivity, has been impregnated in LF:ER:CCNP, and hence of the LF:ER:CCNP composite. The results depict the
was assessed for its electrical behaviour. The composite preparation of a smooth surfaced composite with better
produced 1.1 A current at 0.29 V, 1.25 A current at 1 V, mechanical and electrical properties, which could have
1.7 A current at 1.3 V [24] (Figure 9). multifunctional applications.
Leather Fibres as Reinforcement for Epoxy Composites
Acknowledgements
The award of DST fellowship to R. Senthil and S. Weslen
Vedakumari and CSIR fellowship to T. Hemalatha is
gratefully acknowledged.
References
1. I. M. De Rosa, C. Santulli, and F. Sarasini, Mater. Des., 41,
2397 (2010).
2. J. Kanagaraj, K. C. Velappan, N. K. Chandrababu, and S.
Sadulla, J. Sci. Ind. R., 65, 541 (2006).
3. B. Assamoi and Y. Lawryshyn, Waste Manage., 32, 1019
(2012).
4. G. Laufenberg, B. Kunz, and M. Nystroem, Bioresour.
Technol., 87, 198 (2003).
5. T. P. Sastry, R. K. Sehgal, and T. Ramasamy, J. Environ.
Sci. Eng., 4, 205 (2005).
6. L. A. Pothan, S. Thomas, and N. R. Neelakantan, J. Reinf.
Plast. Compos., 8, 744 (1997).
7. F. A. AI-Sulaiman, Appl. Compos. Mater., 9, 369 (2002).
8. H. Ozgunay, S. Colak, M. M. Mutlu, and F. Akyuz, Pol. J.
Environ. Stud., 6, 867 (2007).
9. R. Senthil, T. Hemalatha, B. S. Kumar, T. S. Uma, B. N.
Das, and T. P. Sastry, Clean Technol. Environ. Policy., doi:
10.1007/s10098-014-0776-x (2014).
10. T. P. Sastry, R. K. Sehgal, and T. Ramasami, J. Environ.
Fibers and Polymers 2015, Vol.16, No.1 187
Sci. Eng., 47, 250 (2005).
11. L. Rajabi, Z. Mohammadi, and A. A. Derakhshan, Iran. J.
Chem. Eng., 10, 16 (2013).
12. J. D. Foulk, D. E. Akin, and R. B. Dodd, SAE, 1, 6 (2000).
13. P. Avouris, M. Freitag, and V. Perebeinos, Nat. Photonics.,
2, 341 (2008).
14. T. Hanemann and D. V. Szabó, Materials, 3, 3517 (2010).
15. M. Knite, S. Zike, J. Zavickis, and A. Linarts, Mat. Sci.
Appl. Chem., 28, 29 (2003).
16. Y. X. Zhou, P. X. Wu, Z. Y. Cheng, J. Ingram, and S.
Jeelani, Express Polym. Lett., 2, 40 (2008).
17. R. Kotsilkova, D. Fragiadakis, and P. Pissis, J. Polym. Sci.
Pt. B-Polym. Phys., 43, 522 (2005).
18. Y. Tu, Y. Lin, W. Yantasee, and Z. Ren, Electroanalysis,
17, 79 (2005).
19. S. I. Lee and D. J. Yoon, Key. Eng. Mater., 290, 321
(2008).
20. L. Bozec and M. Odlyha, Biophys. J., 101, 228 (2011).
21. Y. F. Duann, T. M. Liu, K. C. Cheng, and W. F. Su, Polym.
Degrad. Stabil., 84, 305 (2004).
22. S. N. Nicolopian, M. L. Friedman, U. Stalnova, and V.
Popov, Adv. Polym. Sci., 96, 1 (1990).
23. E. Reynaud, T. Jouen, C. Gauthier, G. Vigier, and J. Varlet,
Polymer, 42, 8759 (2001).
24. Z. Ounaies, C. Park, K. E. Wise, E. J. Siochi, and J. S.
Harrison, Combust. Sci. Technol., 63, 1637 (2003).