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Industrial Crops & Products 112 (2018) 556–560

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Industrial Crops & Products


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

Curcuma longa L. plant residue as a source for natural cellulose fibers with T
antimicrobial activity

Manikandan Ilangovana, , Vijaykumar Gunaa,b, Chunyan Huc,d,e, G.S. Naganandaa,

Narendra Reddya,
a
Centre for Incubation, Innovation, Research and Consultancy, Jyothy Institute of Technology, Thataguni Post, Bengaluru 560082, India
b
Visvesvaraya Technological University – Research Resource Centre, Jnana Sangama Belagavi-590018, India
c
College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai 201620, PR China
d
National Engineering Research Center for Dyeing and Finishing of Textiles, Donghua University, Shanghai 201620, PR China
e
National Cashmere Products Engineering & Technical Research Center, Erdos Cashmere Group, Ordos, Inner Mongolia 017000, PR China

A R T I C L E I N F O A B S T R A C T

Keywords: Natural cellulose fibers extracted from stems of Curcuma longa L. have properties similar to fibers from lig-
Curcumin longa nocellulosic crop residues and also inherit antimicrobial properties. Turmeric contains curcumin, the natural
Natural cellulose fibers compound known to have many medicinal benefits including anti-cancer activity. Turmeric plants are mainly
Antibacterial properties cultivated for its rhizome (tuber) but the plant generates considerable amounts of stem and leaves as residues.
Valorization
Leaves and stems of turmeric plants have been reported to contain oil and other extractives having antimicrobial
and anti-insecticidal activities. Such extracts are of limited quantity and hence it is difficult to justify the eco-
nomic feasibility of using the residues for large scale applications. Natural fibers have a large market and offer
higher value addition and options to develop various products. However, fibers obtained from lignocellulosic
sources do not have inherent antimicrobial properties. Turmeric stems were treated with alkali solution to obtain
natural cellulose fiber bundles. These fibers had cellulose content of about 50%, lignin content of 12% and about
10% ash. Alkali treatment removed surface substances resulting in smooth fiber bundles. Cellulose in the fibers
showed typical diffraction peak at 22.7° belonging to the 002 plane. Tensile strength of the fibers at 2.5 g/den
(325 MPa) was similar to jute. Fibers showed antimicrobial activity against both gram positive and gram ne-
gative bacteria. Turmeric fibers could be useful for wound dressings, textiles, composites and other applications.

1. Introduction 2017).
Agricultural residues such as stalks, leaves and husks have been
Multipurpose agricultural crops that yield more than one produce/ used to develop fibers, composites, filters, sorbents for waste water etc.
processed products are limited. Most of the major crops such as wheat, Among the various uses, fibrous applications are most promising due to
corn, rice, sugarcane etc are grown primarily for their produce. the high value addition possible. Fibers have been extracted from
Unfortunately, the amount of produce generated from these crops is cornhusks, stalks, wheat and rice straw, cotton stalks and other agri-
considerably low compared to the waste or residues they generate. For cultural residues with properties similar to that of the fibers in current
instance, the corn collected is much low in quantity compared to the use (Anandamurthy et al., 2017; Reddy, 2015). Properties of textiles
stalks, leaves, husks and cobs generated as byproducts or residue. and composites made from fibers extracted from agricultural residues
Generally, these residues are either burnt or buried in the ground. This have been found to be suitable for automotive composites and other
means that the natural resources and energy used to grow the crop are areas (Vinayaka et al., 2017; Bhuvaneswari et al., 2017).
not utilized efficiently. Owing to the large amounts available at low cost Curcumin longa, commonly referred to as turmeric is an herb used
and in a sustainable route, considerable efforts are being made to utilize for its medicinal properties. India is the largest producer of turmeric
the agricultural residues for industrial applications (Reddy and Yang, with annual production of about 25 M tonnes. Turmeric is grown in
2009a,b,c). Similar to the agricultural residues, high yield and low re- about 180,000 ha in India and the yield is about 39 t per hectare. It
source intensive biomass such as switchgrass and water hyacinth are typically takes about 225 days for the plants to be mature. Although
also considered for various industrial applications (Guna et al. 2016, considerable quantity of turmeric is produced, the most valuable


Corresponding authors.
E-mail addresses: narendra.r@ciirc.jyothyit.ac.in, nreddy3@outlook.com (N. Reddy).

https://doi.org/10.1016/j.indcrop.2017.12.042
Received 7 September 2017; Accepted 17 December 2017
0926-6690/ © 2017 Elsevier B.V. All rights reserved.
M. Ilangovan et al. Industrial Crops & Products 112 (2018) 556–560

component curcumin yield from turmeric is about 6–7% depending up acetic acid solution for about 10 min, rinsed and dried.
on the variety and the conditions during growth (Hossain and Yukio,
2005). Since turmeric is a rhizome, the stem and leaves above the 2.3. Composition
ground are not considered useful and are generally disposed as waste.
Unfortunately, the amount of residues generated is considerably higher Composition of the untreated turmeric stems and the fibers ex-
than the turmeric harvested. tracted were determined in terms of cellulose, hemicellulose, solubles,
Several attempts have been made to utilize parts of the turmeric lignin and ash. The compositional analysis was done using standard test
plant in addition to the rhizome and curcumin extracted from the tur- methods. Cellulose and hemicellulose were determined using the acid
meric. About 40% oil is extracted when turmeric is processed to obtain and neutral detergent procedure. Neutral detergent was added into the
the yellow pigment curcumin (Negi et al., 1999). Four different frac- biomass at 1:100 ratio along with decalin and anhydrous sodium sul-
tions were separated from the oil. Ar-Turmerone, turmerone and cur- fite. Beaker was boiled for 5–10 min and continued to heat for 60 min.
lone were found to be the major compounds in the oil with one of the Similar procedure was also followed to determine the acid detergent
fractions having considerably higher antimicrobial activity (Negi et al., fiber. Residue obtained after treatment was called Acid Detergent Fiber
1999). Curcumin was also reported to correct cystic fibrosis (Egan et al., (ADF) and neutral detergent fiber (NDF) which represent cellulose and
2004). Fractionation of curcumin yields three curcuminoids having hemicellulose, hemicellulose and lignin, respectively. ADF and NDF
enzyme inhibition activity. Other compounds extracted from curcumin values were used to determine the% cellulose and hemicellulose. About
have exhibited antifungal and mosquitocidal activity (Roth et al., 2 g of sample was placed in a crucible and heated in a muffle furnace for
1998). Given such unique and distinct applications, it is reasonable that 5 h at 550 °C to determine the ash content. Weight of the sample after
curcumin is considered a novel and highly valuable biocompound. burning was recorded and the difference in weight was used to calcu-
Since curcumin only forms a minor part of the crop, it is highly practical late the% ash content. Klason lignin was determined using the sulfuric
to use other parts of the plant for value added applications. Such efforts acid hydrolysis approach. Samples were treated with 72% sulfuric acid
will not only add value to the crops but will also decrease the amount of (1:5 ratio) and allowed to stay at room temperature for about 2 h under
waste generated. constant stirring. Later, the solution was diluted with water at 1:540
In addition to the tuber, other parts of the turmeric plant have also ratio and boiled for 6 h under reflux. After the thorough boiling, the
been reported to have medicinal and other properties. Arutselvi et.al, residue in the flask was washed several times until the pH was neutral.
studied the photochemical content and potential antimicrobial activity Weight of the residue was determined after drying and used to calculate
of the extractants from turmeric leaves (Arutselvi et al., 2012). Leaf the% lignin. The flavonoid and phenolic contents in the turmeric plant
extractants were composed of flavanoids, cardiac glycosides and phe- and extracted fibers were determined using qualitative and quantitative
nols and showed antimicrobial activity against S.pyrogens, B.subtilis and methods based on established protocols (Sadasivam and Manickam,
C. albicans (Arutselvi et al., 2012). In another study, hexane extracts 1997; Nagananda et al., 1986; Tripathi et al., 2002).
from turmeric leaves contained labda-8(17),12-diene-15,16 dial. These
compounds were found to effectively inhibit growth of Candida albi- 2.4. Tensile properties
cans, Candida kruseii and Candida parapsilosis. One of the extract (12-
diene-15,16 dial) was also found to act as mosquitocide against A. ae- Tensile strength, elongation and modulus of the fibers were de-
gyptii larvae when used at a concentration of 10 μg mL−1 and also acted termined using a universal tensile tester (MTS Mechatronics,
against three different types of beetle (R. dominica, S. oryzae and T. Ichalakarnji, India). Samples were tested using a gauge length of 1 inch
castaneum) (Roth et al., 1998). Similar to the rhizome, oil extracted and crosshead speed of 18 mm/min according to ASTM standard D
from the leaf contained about 60 compounds, prominent among them 3822-14. A 500 N load cell was used for testing. All tests were done at
being alpha-phellandrene (18.2%), 1,8-cineole 04.6%) and p-cymene room temperature and about 30 fibers each from three different ex-
(13.3%) (Sharma et al., 1997). tractions were tested. The average and ± one standard deviation of the
Although some efforts have been made to identify and utilize parts values has been reported.
of turmeric plant other than the rhizome, to the best of our knowledge,
turmeric residues have not been studied to understand their potential as 2.5. Morphology
sources for natural cellulose fibers. In this research, we have extracted
natural cellulose fibers from the stalks of the turmeric plant and char- A Hitachi (Model SU 3500) scanning electron microscope was used
acterized the structure and properties of the fibers. In addition, we have to observe the morphology of the turmeric stems before extraction and
studied the potential antimicrobial properties of the fibers. the fibers obtained after extraction. Changes in the surface and cross-
sections were studied. Samples were sputter coated in an Ion beam
2. Materials and methods coater for 60 s before observation. Images were collected using the
secondary electron detector operating at 15 kV.
2.1. Raw material
2.6. X-ray diffraction studies
Turmeric plants were collected from a field on campus after the
rhizome was harvested. Leaves and stalks were dry and used directly Turmeric stems and fibers were powdered in a Wiley mill for the X-
without any treatment. Laboratory grade sodium hydroxide, acetic acid ray powder diffraction studies. Samples were powdered and placed in a
and other chemicals required for fiber extraction were purchased from Teflon holder. Readings were taken on a Bruker D8 Advanced Eco X-ray
local vendors. diffractometer having Bragg-Brentano Focusing geometry. A Cu-Kα ra-
diation at a wavelength (λ = 1.54 Å) was used for the measurement. A
2.2. Extraction of fibers SSD 160 recorded the diffraction intensities for 2θ angles varying from
5 to 40°. Readings obtained were analyzed using Origin and the peak
Turmeric plants were treated with 1 M sodium hydroxide solution positions were identified.
for 30 min at 90 °C. Material to the alkali solution ratio was maintained
at 1:10. After treatment, the liquid that contained dissolved hemi- 2.7. Thermogravimetric analysis
cellulose, lignin and other extractives was decanted and disposed.
Fibers extracted were thoroughly washed several times until the pH of Thermal degradation of the turmeric stalk and fibers were de-
the fibers in water was about 7. Later, the fibers were immersed in 10% termined using a Shimadzu DTG 60 thermogravimetric analyzer. About

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M. Ilangovan et al. Industrial Crops & Products 112 (2018) 556–560

10–15 milli grams of the powdered specimen was placed in the analyzer protective layer without the individual fibers being visible.
and heated from room temperature to 600 °C at a heating rate of 20 °C/ Longitudinal strips of about 50 μm in width are seen which should be
minute. Tests were conducted under nitrogen atmosphere flowing at a the fiber bundles (Fig. 1a). Higher magnification image shows spherical
rate of 50 ml/min. deposits on the surface which are a few microns in diameter (Fig. 1b).
In cross-sectional view, the stalks are seen to be quiet porous and have
2.8. Antimicrobial activity bundles of fibers connected together (Fig. 1c). Width of the bundle is
about 5–30 μm. During the treatment, the connecting places and com-
Ability of the turmeric plants and the extracted fibers to resist ponents between these bundles are removed resulting in individual fi-
common bacteria was studied. Four common bacterial strains bers. Fiber bundles have a much smoother surface than the untreated
(Staphylococcus aureus, Escherichia coli, Serratia marcescens and Bacillus stems. A number of fibrils are held together to form the fiber bundle as
cereus) were selected. Out of the four bacteria, two were gram positive seen (Fig. 1d). Some of the spherical deposits seen on the surface of the
and two were gram negative. Master cultures maintained on nutrient stalks are retained even after extraction and are seen on the fibers
agar at our institution were used for the study. Initial culture was (Fig. 1e). Bundles of fibers are composed of individual fibrils which
prepared by inoculating fresh organisms into Mueller-Hinton broth and have a width of about 2–5 μm similar to that in most lignocellulosic
later incubating at 37 °C for 12 h. Turmeric plant and fibers were fibers (Fig. 1f). Length and width of the individual fibers plays a major
powdered and two concentrations (50 or 100 mg) were added into test role in determining the properties of the fibers. Raw materials with
tubes. To the test tubes, about 10 ml of Muller-Hinton broth was added longer and finer individual fibrils can produce finer fibers as with linen
and later autoclaved. About 50 μl of broth containing the bacteria was whereas shorter fibrils result in coarser fibers as with rice, wheat straw
added into each test tube and incubated on a shaker incubator at 37 °C and other unconventional natural cellulose fibers.
for 6 h. Control samples that did not contain the turmeric plants or the
fibers were also incubated. At desired time intervals, the absorbance of 3.3. X-ray diffraction
the solution in the test tubes was measured on a spectrophotometer at a
wavelength of 600 nm. At least three trials were conducted for each Major differences in the position and number of peaks can be ob-
condition and the average and standard deviations are reported. served between the X-ray diffraction patterns of turmeric stalk and fi-
bers obtained from the stalks (Fig. 2). Minor peak at the prominent
3. Results and discussion cellulose 002 crystal plane at 22° suggests that the stalks have lower
composition of cellulose. Increase in the intensity of the 002 plane peak
3.1. Composition of the fibers in the fibers substantiates the compositional analysis which showed
that the fibers had 84% higher cellulose content. Additional peaks (24,
Considerable changes in the composition of the turmeric stem can 27°) seen in the stalks but absent in the fibers should be from the mi-
be observed due to the treatment with alkali. Composition of biomass nerals or impurities that are removed during extraction. Using the area
and fibrous materials varies drastically depending on the function, under the diffraction curve, the% crystallinity of the fibers was found to
growth and extraction conditions. For example, cotton is mostly cellu- be about 33% compared to 30% in the untreated stalks. A prominent
lose (> 90%) whereas coir contains only about 30–35% cellulose and peak seen only in the treated fibers at about 28° is from the calcium
up to 30% lignin. As expected, fiber extraction results in the removal of carbonate that was probably due to the washing of the fibers in the hard
some of the non-cellulosic substances. Consequently, amount of cellu- water.
lose in the fibers was 84% higher compared to that in untreated stalk
(Table 1). About 50% decrease in hemicellulose content also occurred 3.4. Thermal degradation
due to the treatment. The fibers have relatively high amounts of lignin
and ash but typical levels of cellulose and hemicellulose compared to Thermal degradation profile of the fibers is shown in Fig. 3 in
other natural fibers. Before treatment, the fibrous cellulose is protected comparison with the untreated fibers. Although both the fibers and
by the lignin and hemicellulose. Although it is necessary to remove the stalk had similar residual content of about 10%, their degradation be-
lignin and hemicellulose to obtain the fiber bundles, excessive removal havior was different. Throughout the temperature range, the weight
will result in shorter fibers not suitable for high value applications. loss of the stalk was higher than that of the fibers which is probably due
Extent of removal of the non-cellulosic components depends on the to the presence of impurities that have lower thermal stability. Rate of
treatment conditions and should be controlled depending on the degradation of the fibers was also considerably higher than that of the
properties of the fibers desired. The flavonoid content in the fibers was stalks suggesting that the substances present in the stalk provide better
about 25% lower and the phenol content decreased by about 20% thermal insulation. Stability of the fibers up to 300 °C (about 20%
compared to that in the untreated raw material. Phenolic concentration weight loss) is high and hence the fibers would be suitable for most
in the fibers is considerably high compared to other common lig- applications.
nocellulosic fibers.
3.5. Tensile properties
3.2. Morphology
Tensile properties of turmeric fibers are typical to those of many
Before treatment, the surface of the turmeric stalks is covered with a other lignocellulosic fibers. Strength and elongation of the fibers are
similar to that of jute whereas modulus is considerably lower. Turmeric
Table 1 fibers are also coarser than the fibers in common use (Table 2). Since
Composition of the turmeric plants and fibers extracted from the plants. turmeric fibers are from an agricultural waste unlike jute or linen which
are exclusively grown for fibers, the raw material is not ideally suited
Composition Turmeric Stalk Turmeric Fibers
for extraction of fibers. For instance, the single cells in turmeric fibers
Cellulose, % 30.7 ± 0.5 56.5 ± 0.6 should be considerably smaller than in cotton or linen (Reddy and
Hemicellulose, % 26.1 ± 1.0 12.4 ± 0.2 Yang, 2009b). This makes it difficult to extract finer fibers. In addition
Lignin, % 17.7 ± 1.6 14.8 ± 1.3 to the single cells, composition of the raw material and extraction
Ash, % 15.4 ± 0.5 10.2 ± 1.2
conditions used make a significant difference on the fiber properties.
Flavonoids, μg/ml 260 ± 0.2 196 ± 0.1
Phenols, μg/ml 226 ± 0.2 180 ± 0.1 Turmeric fibers are extracted from an agricultural residue using a
simple process which makes the fibers inexpensive. Although it may be

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Fig. 1. Scanning electron images reveal the longitudinal and cross-sectional features of the turmeric plants and fibers extracted from them. A and B are the surface features of the
untreated stems and C is the cross-section of the untreated stem. D, E and F show the surface of the treated fibers at different magnifications after removal of the non-cellulosic substances.
Fiber bundles composed of individual fibers/cells are clearly seen in the SEM pictures of the fibers.

biomass, the untreated sample had higher% inhibition, most notably for
S. marcescens. Differences in inhibition decrease drastically when the
concentration used was 10 mg/ml. Both the untreated and treated
material showed higher inhibition of S. aureus and E. coli compared to
the other two bacteria studied. Antibacterial activity of the samples is
related to the phenolic content in the material. As discussed earlier, the
phenolic content is high in the untreated material and hence it shows
better activity. Considerable amounts of phenolic materials are re-
moved during fiber extraction and hence we observe a decrease in the
antibacterial activity of the fibers. Nevertheless, the inhibition of
common bacteria (S. aureus and E. coli) by the fibers is 59 and 50%
respectively suggesting that the fibers could be used for treating
wounds, purification of water and other applications.

4. Conclusions

Natural cellulose fibers extracted from the discarded stems of tur-


Fig. 2. X-ray diffractogram of the turmeric plant stem (before extraction) and the fibers meric plants have structure and properties similar to that of other lig-
extracted from the stems. nocellulosic fibers. In addition, the fibers retain high level of inhibition
against common bacteria including E. coli and S. aureus. Since turmeric
difficult to process the fibers as cotton, jute and linen due to their coarse is a rhizome, only the root is currently utilized and the large amounts of
diameter, the fibers can be used for composites, as blends with common biomass generated is disposed as waste. We demonstrate that residues
fibers and for other applications. of turmeric plants can be utilized to obtain fibers with unique proper-
ties. Composition, morphological and tensile properties of the turmeric
fibers are similar to several lignocellulosic fibers. Turmeric fibers could
3.6. Antimicrobial properties be ideal for developing materials for medical applications.

There was considerable difference between the antibacterial activity Acknowledgements


of the fibers and the turmeric plant. Extent of antibacterial activity also
varied depending on the type of bacteria evaluated. As seen from Narendra Reddy expresses his sincere thanks to the Department of
Table 3, the untreated sample showed considerably higher inhibition of Biotechnology, Ministry of Science and Technology, Government of
all four bacteria at both concentrations studied. At 5 mg per ml of the India for funding through the Ramalingaswami Re-entry Fellowship.

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M. Ilangovan et al. Industrial Crops & Products 112 (2018) 556–560

Fig. 3. TGA (left) and DTG (Right) curves for the degradation of the turmeric stems and extracted fibers.

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