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Materials Research Bulletin 46 (2011) 2560–2566

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Materials Research Bulletin


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Green synthesis of zinc oxide nanoparticles by aloe barbadensis miller leaf extract:
Structure and optical properties
Gunalan Sangeetha a, Sivaraj Rajeshwari a,*, Rajendran Venckatesh b
a
Department of Biotechnology, School of Life Sciences, Karpagam University, Eachanari Post, Coimbatore 641 021, Tamilnadu, India
b
Faculty of Chemistry, Government Arts College, Udumalpet 642 126, Tamilnadu, India

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

Article history: Biological methods for nanoparticle synthesis using microorganisms, enzymes, and plants or plant
Received 29 January 2011 extracts have been suggested as possible ecofriendly alternatives to chemical and physical methods. In
Received in revised form 17 June 2011 this paper, we report on the synthesis of nanostructured zinc oxide particles by both chemical and
Accepted 29 July 2011
biological method. Highly stable and spherical zinc oxide nanoparticles are produced by using zinc
Available online 26 August 2011
nitrate and Aloe vera leaf extract. Greater than 95% conversion to nanoparticles has been achieved with
aloe leaf broth concentration greater than 25%. Structural, morphological and optical properties of the
Keywords:
synthesized nanoparticles have been characterized by using UV–Vis spectrophotometer, FTIR,
A. Nanostructures
Photoluminescence, SEM, TEM and XRD analysis. SEM and TEM analysis shows that the zinc oxide
B. Chemical synthesis
C. Optical properties nanoparticles prepared were poly dispersed and the average size ranged from 25 to 40 nm. The particles
D. X-ray diffraction obtained have been found to be predominantly spherical and the particle size could be controlled by
E. Electron microscope varying the concentrations of leaf broth solution.
ß 2011 Elsevier Ltd. All rights reserved.

1. Introduction It is non-toxic, self-cleansing [13,14], compatible with skin,


antimicrobial, dermatological and is used as an UV-blocker in
Nanomaterials, controlled to nano crystalline size (less than sunscreens and many biomedical applications [15]. Furthermore,
100 nm), can show atom-like behaviors which result from higher ZnO appears to strongly resist microorganisms [16] and some
surface energy due to their large surface area and wider band gap reports show considerable antibacterial activity of CaO, MgO and
between valence and conduction band when they are divided to ZnO [17], which is attributed to the generation of reactive oxygen
near atomic size [1]. Transition metal oxides with nanostructure species on the surface of these oxides.
and semiconductors with dimensions in the nanometer realm In spite of these merits, ZnO is bio-safe, biocompatible with
have attracted considerable interest in many areas of chemistry, unique ability like structure-dependent properties, electrical and
physics, material science, biotechnology, information technology thermal transport properties, which could be varied with respect
and environmental technology as next generation technologies to particle size, shape, morphology, orientation and aspect ratio,
[2–4]. In recent years, zinc oxide (ZnO), an important semicon- have resulted in increased interest in obtaining this nano metal
ductor with tremendous scientific and technological interest, oxide material [18–20]. Several physical and chemical procedures
having a direct wide gap (3.37 eV, 387 nm, deep violet/borderline have been used for the synthesis of large quantities of metal
ultraviolet (UV)) and a large exciton-binding energy (60 meV) [5], nanoparticles in relatively short period of time. Approaches such as
is a highly preferred multitasking metal oxide having a vast list of simple solution-based methods, chemical precipitation [21,22],
attractive properties. Due to its unique optical and electrical sol–gel [23], solvothermal/hydrothermal [24–26], electrochemical
properties [6,7], it is regarded as a potential material in and photochemical reduction techniques are most widely used
optoelectronic applications operating in the visible and near [27,28]. Chemical methods lead to the presence of some toxic
ultraviolet spectral regions. ZnO nanoparticles have been widely chemicals adsorbed on the surface that may have adverse effects in
used in many industrial areas such as solar cells, UV light-emitting medical application [29]. Increasing awareness towards green
devices, gas sensors, photocatalysts, pharmaceutical and cosmetic chemistry and other biological processes has led to the develop-
industries [8–12]. Additionally, metal nanoparticles have a ment of an eco-friendly approach for the synthesis of nanopar-
surface plasmon resonance absorption in the UV–visible region. ticles. The use of environmentally benign materials like plant leaf
extract [30], bacteria [31], fungi [32] and enzymes [33] for the
synthesis of silver nanoparticles offers numerous benefits of eco-
* Corresponding author. Tel.: +91 422 2611146; fax: +91 422 2611043. friendliness and compatibility for pharmaceutical and other
E-mail address: rajeshwarishivaraj@gmail.com (S. Rajeshwari). biomedical applications, where toxic chemicals are not used for

0025-5408/$ – see front matter ß 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.materresbull.2011.07.046
G. Sangeetha et al. / Materials Research Bulletin 46 (2011) 2560–2566 2561

the synthesis protocol. Although biosynthesis of gold nanoparticles 2.2. Characterization


by plants such as alfalfa [34,35], Cinnamomum camphora [36], neem
[37], Emblica officinalis [38], lemon grass [39], and tamarind [40] Optical properties of ZnO nanoparticles were characterized
have been reported, the potential of plants as biological materials based on UV absorption spectra and photoluminescence (PL). The
for the synthesis of nanoparticles is yet to be fully explored. The sample was sonicated for uniform dispersion and the aqueous
present investigation describes for the first time, synthesis, component was subsequently analyzed at room temperature for
characterization and optical properties of ZnO nanoparticle optical band gap (Eg) using UV–Vis spectrophotometer (UV-2450,
prepared by both chemical and biological (green) techniques Shimadzu). Photoluminescence (PL) spectra were recorded on a
using Aloe vera. Aloe vera (Aloe barbadensis Miller) a perennial Perkin-Elmer LS-55 B. The chemical composition was studied by
succulent belonging to the Liliceal family, is a cactus-like plant that using FTIR spectrometer (Perkin-Elmer 1725X). The shape, size and
grows in hot, dry climates [41]. Aloe gel is the mucilaginous jelly microstructures of the products were characterized by using
obtained from parenchyma cells of the Aloe vera plant. Different scanning electron microscopy (Model JSM 6390LV, JOEL, USA). The
researchers have described different processing techniques of the size and morphology were examined by TEM, JEOL model JEM
gel with regard to its sterilization and stabilization, i.e., cold 3010 Electron microscope. Size distribution and the average size of
processing or heat treatment. For many years, aloe vera has been the nanoparticles were estimated on the basis of TEM micrographs
reported to possess immunomodulatory, anti-inflammatory, UV with the assistance of Sigma-Scan Pro software (SPSS Ins, Version
protective, antiprotozoal, and wound healing properties [42–45]. 4.01.003). Phase purity and grain size were determined by X-ray
In order to find the efficiency of aloe vera plant in synthesis of diffraction (XRD) analysis recorded by diffractometer (SEIFERT PTS
nanoparticles, total leaf and gel broth extracts have been used for 3003). All experiments were done in triplicates and the data were
the study. The effect of reaction conditions (broth concentration) analyzed using Origin Pro 7.5 SRO software (OrginLab Corporation,
on synthesis rate and particle size of the zinc oxide nanoparticles USA) and the results were recorded for different aloe leaf broth
has also been investigated. concentrations (0–50%).

3. Results and discussion


2. Experimental details
The study reports the formation of nanoparticles when exposed
2.1. Synthesis by chemical and biological method to aloe extract by monitoring changes in colour as particle size
increased. White precipitate formed was the end product in
Zinc nitrate (99% purity) and NaOH (pellet min. 99%) were used synthesis I whereas in synthesis II, pale white precipitate appeared.
as the starting material and were supplied by Sigma–Aldrich Fig. 1 shows the synthesis of nanoparticles by chemical and
Chemicals, India. The Aloe vera leaves were harvested from local biological method with 25% aloe leaf and gel broth extracted
agricultural fields, Coimbatore, Tamilnadu. Aloe vera extracted solution. At a reaction period of 3 h, around 50–60% conversion
solution was prepared by two different processes. In the first was achieved for aloe leaf and gel broth, whereas only 20%
process, about 250 g portion of thoroughly washed Aloe vera conversion was noticed in chemical synthesis. Increasing the
leaves were finely cut and boiled with de-ionized water in reaction duration to 5–6 h improved level of conversion to almost
medium flame. The resulting product was ground to get complete 100% in aloe gel broth and 95% in leaf broth, but in chemical
extract. The solution was boiled, filtered and stored in refrigerator synthesis the duration exceeded and only 50% conversion was
for further experiments. In the second process, the inner gel noticed after 6 h. It was found >58% nanoparticle synthesis was
portion was extracted from the aloe leaves, crushed and ground to achieved after 4 h. The average ZnO nanoparticle size achieved by
thin paste by adding enough de-ionized water and filtered by using gel (35 nm) and leaf broth (34 nm) was more or less similar
using fine mesh. The resulting extract was stored at 10 8C for whereas the average size was found to be increased to 60 nm in
further experiments. chemical synthesis.
Two different methods were used for synthesizing ZnO
nanoparticles of varying particle sizes. In synthesis I (chemical
method), zinc nitrate was dissolved in distilled water under
constant stirring. While at room temperature, sodium hydroxide
solution was added drop by drop. After completion of reaction,
the solution was allowed to settle for overnight and the
supernatant liquid was discarded. The white precipitate formed
was washed thoroughly with double distilled water to remove all
the ions and then centrifuged at 3000 rpm for 10 min. The
obtained precipitate was dried in a hot air oven at 80 8C for 6 h.
During drying, complete conversion of Zn(OH)2 into ZnO took
place. In synthesis II (biological method), a typical procedure was
employed, where aloe leaf and aloe gel broth extracts at different
concentrations (50%, 25%, 15%, 10%, 5%) were prepared with
distilled water and the volume was made up to 250 ml. Later, zinc
nitrate was dissolved in the aloe extract solution under constant
stirring using magnetic stirrer. After complete dissolution of the
mixture, the solution was kept under vigorous stirring at 150 8C
for 5–6 h, allowed to cool at room temperature and the
supernatant was discarded. The pale white solid product
obtained was centrifuged twice at 4500 rpm for 15 min after
thorough washing and dried at 80 8C for 7–8 h. The resulting
dried precursor was crushed into powder and stored in air tight Fig. 1. Synthesis of ZnO nanoparticle by (a) 25% Aloe gel broth, (b) 25% Aloe leaf
container for further analysis. broth, (c) 0% Aloe broth.
2562 G. Sangeetha et al. / Materials Research Bulletin 46 (2011) 2560–2566

Fig. 2 shows the effect of leaf broth with varying concentration


(5–50%) on ZnO nanoparticle synthesis with time duration of 6 h.
The rate of synthesis increased with increase in leaf broth
concentrations. With a leaf broth concentration of 5%, the level
of conversion to nanoparticle achieved was only around 35% after
7 h. Increasing the leaf broth concentration to more than 25%
resulted in almost 100% conversion after 6–7 h. In synthesizing
gold or silver nanoparticles close to 100% conversion was achieved
with a leaf broth concentration of 5% [46,47]. It is thus not only
duration but also higher leaf broth concentrations that are required
to achieve levels of zinc oxide nanoparticle synthesis comparable
to those for gold and silver.
UV–Visible absorption spectra of the ZnO particles synthesized
from the mixture with and without ALE at room temperature are
presented in Fig. 3. It is generally recognized that UV–Vis spectra
could be used to examine the size and shape controlled
nanoparticles in aqueous suspension [48]. All the samples exhibit
strong UV absorption spectra with the absorption peak ranging
from 358 to 375 nm due to its surface plasmon resonance and
attains a plateau above 3.3 eV (375 nm). Similar observation has
been reported on the rapid synthesis of stable silver, gold and bi-
metallic Ag/Au core shell nanoparticles using 20 g of leaf biomass
of Azadirachta indica and 1 mM aqueous AgNO3, within 4 h with
90% reduction of the metal ions [49]. A clear shift in the absorption
Fig. 3. UV–Vis spectra of ZnO nanoparticle with (A) 0% ALE, (B) 5% ALE, (C) 10% ALE,
onset is discernible in ZnO nanoparticles prepared with ALE (D) 15% ALE, (E) 25% ALE, (F) 50% ALE.
(Fig. 3B–F). The peaks show significant blue shift for ALE
concentration ranging from 5 to 25% absorption whereas
broadened red shift of ZnO nanoparticles were noticed for
concentrations above 25%. The observed red shift implies that
the particle size increases with increased ALE concentrations.
On the other hand, sample without ALE (Fig. 3a) shows a red
shift of the UV–Visible absorption which can be attributed to the
larger particle size. The optical absorption spectra of noble metal
nanoparticles are known to exhibit unique optical properties due
to the property of Surface Plasmon Resonance (SPR), which shift to
longer wavelengths with increasing particle size. The size and
shape of metal nanoparticles and dielectric constant of the
medium and surface adsorbed species determine the spectral
position of plasmon band absorption as well as its width [67].
According to Mie’s theory, only a single SPR band is expected in the
absorption spectra of spherical nanoparticles, whereas anisotropic
particles could give rise to two or more SPR bands depending on

Fig. 4. PL spectra for ZnO nanoparticle. (A) Chemical method, (B) biological method.

Fig. 2. Effect of various concentration of Aloe leaf extract (ALE) on the time course of
ZnO nanoparticle synthesis. Fig. 5. FTIR spectra for ZnO nanoparticle with 0–50% ALE.
G. Sangeetha et al. / Materials Research Bulletin 46 (2011) 2560–2566 2563

the shape of the particles. The number of SPR peaks increases as the The particles obtained from both the synthesis show an
symmetry of the nanoparticle decreases [68–70]. excitation wavelength at 325 nm which is in accordance with
Fig. 4 represents the Photoluminescence (PL) spectra of ZnO results in the literature [50,51]. A relatively sharp, weak UV
particles obtained from synthesis I and II. All the samples with emission band at 3.23 eV (384 nm) and a broad stronger emission
different concentrations of ALE show similar excitation and band in the green part of the visible spectrum with a maximum
emission spectra but their luminescence intensities are different. intensity at 2.4 eV (520 nm) is observed and studied extensively.
The emission intensity decreases gradually and may be likely due ZnO nanoparticles synthesized without ALE (Fig. 4a) show the
to concentration quenching. The UV luminescence of ZnO lowest emission while nanoparticles synthesized with ALE
nanomaterials is commonly attributed to the direct recombination (Fig. 4b–f) show decreasing intensity with increasing concentra-
of excitons through an Exciton–excition scattering [71]. The visible tion ranging from 5 to 50%. The highest peak may correspond to the
luminescence originates from the radioactive recombination of a absorption peaks in the UV–Vis measurement and the band gap of
photo-generated hole with an electron occupying the oxygen ZnO nanoparticles. The broad green band at 2.38 eV is attributed to
vacancy [72]. the radioactive recombination of photogenerated hole with an

Fig. 6. SEM photographs for ZnO nanoparticles with (a) 0% ALE, (b) 5% ALE, (c) 10% ALE, (d) 15% ALE, (e) 25% ALE, (f) 50% ALE.
2564 G. Sangeetha et al. / Materials Research Bulletin 46 (2011) 2560–2566

electron belonging to a singly ionized vacancy in the surface and been assigned to stretching vibrations of the primary and
subsurface [52,53]. The emission shifts from green to red by secondary amines, O–H stretching of alcohols and C–H stretching
increasing the concentration of ALE which reflects the change in of alkanes. The corresponding bending vibration for primary and
the excition energy in the absorption spectra and increase in the secondary amines is also noticed. The peaks around 1640 and
particle size of ZnO nanoparticles. These PL signals are attributed to 1540 cm 1 are due to the amide I and amide II regions that are
band-edge free excitons and bound excitons, respectively [54]. characteristic of proteins/enzymes [57]. The intense bands
Fig. 5 shows the FTIR spectra of zinc oxide nanoparticles observed at 924, 1020, 1150 and 1380 cm 1 have been assigned
synthesized by chemical and biological method. The spectrum to alcohols and phenolic groups, C–N stretching vibrations of
obtained for synthesis I (Fig. 5a) clearly shows ZnO absorption aliphatic and aromatic amines [56], respectively. The peaks in the
band near 528 cm 1. The peaks at 3451, 1552, 1393 and 922 cm 1 region between 600 and 400 cm 1 are allotted to Zn–O [55,58] are
indicate the presence of –OH stretching of intramolecular clearly represented in the Fig. 5.
hydrogen bond, C5 5O stretching and C–C stretching of alkanes The mechanism by which nanoparticles are formed in the
[55,56]. Similar spectra are obtained for the nanomaterials biosynthesis procedures is still not clear. The overall observation
produced via synthesis II (Fig. 5b–e). The amide linkages between proves the existence of some phenolic compounds, terpenoids or
the amino acid residues in the proteins give rise to additional peaks proteins that are bound to the surface of ZnO nanoparticles that
in the infrared region (2900–3700 cm 1) of the electromagnetic remained despite repeated washing. The stability of ZnO nanopar-
spectrum. The bands observed at 3450, 3266 and 2932 cm 1 have ticle may be due to the free amino and carboxylic groups that have

Fig. 7. TEM images for ZnO nanoparticles with (a) 0% ALE, (b) 5% ALE, (c) 10% ALE, (d) 15% ALE, (e) 25% ALE, (f) 50% ALE.
G. Sangeetha et al. / Materials Research Bulletin 46 (2011) 2560–2566 2565

interacted with the zinc surface. The bonds of functional groups precursors have been completely decomposed and no other crystal
such as –CO–C–, –C–O– and –C5 5C– are derived from heterocyclic products have been retained after the decomposition process. All
compounds and the amide bands derived from the proteins are samples with aloe extract had preferred orientation along the
present in the leaf extract and are the capping ligands of the (1 0 1) plane. It has been observed that the preferred orientation of
nanoparticle [56,59,60]. Moreover the proteins present in the (1 0 1) for the ZnO nanoparticles slightly shifted to the left when
medium prevent agglomeration and aids in the stabilization by aloe extract was used when compared to ZnO prepared without
forming a coat, covering the metal nanoparticles. aloe extract (Fig. 8). As the concentration increased, the typical
The SEM and TEM monographs in Figs. 6a–f and 7a–f clearly tendency of increasing intensity of samples was determined using
shows the distribution of ZnO nanoparticles prepared with or the Scherrer’s formula, D = 0.9l/(B cos u) [65,66], where D is the
without aloe broth extract. The powders obtained were homoge- crystal size, l the X-ray wavelength, u the Bragg’s angle in radians,
neous and agglomerated with a particle size ranging from below 25 and B the full width at half maximum of the (1 0 1) peak in radians.
to 55 nm with some deviations. The images show spherical shape The average particle size of the products was around 35 nm, a trend
and hexagonal nanoparticles, which are in accord with the XRD. that generally matched the tendency shown in the TEM and SEM
Owing to the uniform distribution of oxidized metal anions in the images.
three-dimensional polymeric network structure, the agglomera-
tion could be induced by densification resulting in the narrow 4. Conclusions
space between particles [61,62]. Addition of aloe vera extract to the
zinc nitrate did not change ZnO nanoparticles shape, but it caused The secrets gleaned from nature have led to the development of
an increase in nanoparticle size especially for higher concentration biomimetic approaches for the growth of advanced nanomaterials.
(50%) of aloe vera extract. Only a small difference is observed A simple, rapid biological procedure has been developed to
between nanoparticle size measured by XRD and TEM. The synthesize zinc oxide nanoparticles with tunable optical properties
difference in the obtained values of the particle size of the directed by particle size using varying concentration of Aloe vera
produced ZnO nanoparticle is due to the fact that TEM measure- leaf broth extracted solution. The zinc oxide nanoparticle shows
ments are based on the difference between the visible grain distinct poly dispersity and the particle size ranges from 25 to
boundaries, while XRD calculations measure the extended 45 nm with an average size of 35 nm. Maximum nanoparticles
crystalline region that diffracts X-rays coherently. So, the XRD show particle size of 30 nm with distinct cap, which may be due to
method has a more stringent criterion and leads to smaller sizes the flavonoids, proteins and other functional groups present in the
[63]. leaf broth of aloe vera and are likely to be responsible for the
The TEM images at higher resolution also reveal that formation of zinc oxide nanoparticles. The explored eco-friendly,
nanoparticles are not in physical contact but are separated by high efficient zinc oxide nanoparticles prepared from Aloe vera leaf
uniform inter-particle distance. The images clearly show the broth are expected to have more extensive applications in
presence of secondary material capping with a thickness of biomedical fields and in cosmetic industries.
10 nm which may be assigned to bioorganic compounds present
in the leaf broth [49–60]. This can be further confirmed by
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