Materials Focus

Vol. 3, pp. 17, 2014

(www.aspbs.com/mat)

Copyright 2014 by American Scientific Publishers

All rights reserved.
Printed in the United States of America

Ag Grafted ZnO Nanoplates for Photocatalytic

Applications
Vidur Raj, Pranauv Balaji, Monika Joshi , and Manish Kumar
Amity Institute of Nanotechnology, Amity University Uttar Pradesh, Sector125 Express Highway, Noida, U.P., India

ABSTRACT

KEYWORDS: Optical Material, Chemical Synthesis, X-Ray Diffraction, Photocatalysis.

1. INTRODUCTION
Photocatalysis using nanoparticles have potential applications in optical devices like Organic LEDs, Solar energy
conservation (Solar cells), Water treatment using UV rays
and environmental pollution treatment etc.1 Compared
with other semiconductor nanostructures, ZnO have been
studied extensively over the last decades due to their
unique physical and chemical properties. ZnO is one of the
most widely used photocatalytic metal-oxide nanostructured semiconductors with a wide band gap of 3.2 eV and
a large exciton binding energy of 60 meV.2 It is an intrinsically n-type semiconductor of wurtzite structure and has a
good chemical, thermal and catalytic stability at room temperature. Due to these properties, ZnO is widely applied in
various applications in optical devices,3 transistors,4 piezoelectric devices,5
6 gas sensor,7
8 mechanical devices,9 UV
detectors10
11 and photoluminescence devices.12
However, photocatalytic efficiency of pure semiconducting nanomaterial is very low due to the fast recombination
of photo-generated electron hole pair and the inability to
utilize visible light due to the large wide band gap. Therefore, considerable efforts have been made for the development of a photocatalytic system that can be more active
in visible light (>400 nm).13 To date, many approaches

Author to whom correspondence should be addressed.

Email: mjoshi@amity.edu
Received: xx Xxxx xxxx
Accepted: xx Xxxx xxxx

Mater. Focus 2014, Vol. 3, No. xx

2169-429X/2014/3/001/007

including (i) functionalization of ZnO with photosensitizes that absorbs UV light, (ii) doping with metals and
(iii) doping with non metals have been applied to enhance
the photocatalytic activity of semiconductors like ZnO.14
Doping and making composite with metals are widely
studied ways of enhancing the photocatalytic activity of
metal oxide semiconductor. The interaction of metal with
semiconductor improves the electrical and optical properties due to the shifting of the Fermi level and the formation of a Schottky barrier for trapped electrons has
earlier been reported.15 These trapped electrons are transferred to the dye, which are further degraded through
the hydroxyl and super hydroxyl radicals generated by
UV illuminator.16 Therefore, the photocatalytic activity of
metal-semiconductor shows significant enhancement compare to pure ZnO.
Noble metal such as (Ag and Au) shows unique electron
storage and light absorption properties.17 Compared with
all other metal-semiconductor nanostructures, Ag/ZnO
nanocomposites have drawn particular attention, not only
because ZnO nanostructures can be easily prepared by
a series of simple methods,1821 but also that silver displays the most efficient plasmon resonance in the visible
region among all metals by virtue of its favorable frequency dependence of the real and imaginary parts of
the dielectric function.22 ZnO nanorods with noble metals
shows improved electrical, optical, magnetic and chemical properties.23 Ag nanoparticles have lots of peculiar and
exciting physical chemical and catalytic properties that are
different from massive silver. Therefore, incorporation of
doi:10.1166/mat.2014.1192

ARTICLE

Herein, ZnO nanoplates were synthesized by chemical method and Ag nanoparticles were grafted on ZnO
nanoplates surface by sonochemical method. The formation of the nanocomposites was investigated using
X-ray diffractometer (XRD) and Field Emission Scanning Electron Microscopy (FE-SEM). Optical properties of
the nanocomposite were investigated using Photoluminescence spectroscopy (PL) and UV-Visible spectroscopy
(UV-Vis). FESEM investigation confirms that the nanoplates were uniformly distributed and Ag nanoparticles
were grafted on the surface on ZnO nanoplates. The photocatalytic activity of Ag/ZnO nanocomposites was
evaluated in terms of their efficiency of the photo excitation of methyl orange dye (MeO) under UV illuminator.
A photo excitation of Ag/ZnO showed enhanced photocatalytic activity compared to pure ZnO Nanoplates. This
enhanced UV activity of Ag/ZnO nanocomposite makes it a potential candidate for optoelectronic devices for
Solar Energy conservation, water splitting and Light Emitting devices etc.

Raj et al.

Ag Grafted ZnO Nanoplates for Photocatalytic Applications

ARTICLE

silver (Ag) can enhance the photocatalytic efficiency of

semiconducting nanoparticle (ZnO) by acting as an electron sink for the exited electrons and thus increases the
generation of electron hole pairs in ZnO. Moreover, the
enhancement was not due to the electrons generated by
visible light excitation of surface plasmon resonance but
due to the plasmon resonance enhanced local electric field
of the incident light.24 These enhanced properties have
been utilized in photovoltaic cells, photo-catalysts, solar
cells and optoelectronic devices.
In the present article, Ag/ZnO nanocomposites have
been synthesized by varying the concentration of Ag. The
photocatalytic activity of Ag/ZnO nanocomposite under
UV-Visible irradiation was studied by photo degradation of organic dye (MeO). The nanocomposite shows
enhanced photocatalytic activity compared to the pure
ZnO. The results indicated that optical absorption of
Ag/ZnO nanocomposite showed enhanced photocatalytic
activity at 10 mM concentration of silver.

Fig. 1. XRD image of ZnO Nanoplates and Ag/ZnO nanocomposite.

2.2. Grafting of Ag Nanoparticles on ZnO Nanoplates

0.2 g of synthesized ZnO Nanoplates were dissolved in
50 ml of D. W. and ultrasonicated for 2 hr. 10 mM
of Ag(NO3  (AR Grade) and 1 mM Tri sodium citrate
(Na3 C6 H5 O7  (MERCK) was added to the above solution.
The solution was stirred for 2 hr at room temperature. The
resultant solution was centrifuged and obtained a blackish
brown colored powder. The same experiment was repeated
by varying the concentration of Ag (NO3  to 5 mM and
2.5 mM concentrations.

and 44.25 corresponds to (111) and (200) planes of

Ag nanoparticles with face centered cubic structure (fcc)
respectively. It is indicated that the crystallization of ZnO
Nanoplates is not affected by grafting of Ag nanoparticles, indicating a good crystalline property of the Ag/ZnO
nanocomposites.
The synthesized material was investigated by FESEM
(Zeiss Ultra Plus-40-98) at room temperature for its
morphology and composition. Figures 2(A)(D) shows
FESEM micrograph of the synthesized ZnO nanoplates.
The Nanoplates formed were evenly distributed throughout the sample. The nanoplates are arranged in the form
of beautiful uniform flowers with bush like structure. The
petals of nanoflowers are pyramidal in shape with a diameter of 30 nm70 nm and a length of few micrometers.
The images reveal that Ag nanoparticles are sparsely distributed on the ZnO Nanoplates. Figure 2(E) shows the
EDX mapping of Ag/ZnO nanocomposite. The EDX mapping shows the presence of materials like Zn, O, Ag and
some of the other stray molecules like C etc. confirming
the presence of Ag grafted ZnO. The FESEM micrograph
and EDX mapping measurement reveals the presence of
Ag nanoparticles grafted on to the surface of the ZnO
Nanoplates.

3. CHARACTERIZATION TECHNIQUES

4. RESULTS AND DISCUSSION

The changes of crystalline phase structure of Ag/ZnO

nanocomposite were investigated using X-ray diffractometer (Bruker, D-2 Phaser) at room temperature. Figure 1
shows the comparative XRD image of uncoated ZnO
Nanoplates and ZnO Nanoplates coated with Ag nanoparticles. Three prominent peaks at 2 = 3162, 34.44 and
36.10 corresponds to the diffraction of the (100), (002)
and (101) planes of ZnO respectively. All diffraction peaks
can be indexed as wurtzite structure ZnO. The intensity
of (101) plane is higher than other two planes suggesting
that most of the ZnO Nanoplates are with (101) planes.
XRD image of ZnO decorated with Ag nanoparticles are
obtained two prominent additional peaks at 2 = 3838

The photocatalytic degradation of organic dyes or toxic

pollutant is a commonly used approach to characterize
the efficiency of the photo catalyst. The photo-catalytic
activity of Ag/ZnO nanocomposite was evaluated by the
photo-degradation of methyl orange (MeO) placed under
UV illuminator for a fixed interval of time. Figure 3
shows a series of UV-Vis absorption spectra of (3A) ZnO
Nanoplates (3B) Ag/ZnO nanocomposite obtained from
the suspension of 10 M solution of organic dye (Methyl
Orange (C14 H14 N3 NaO3 S)MeO) with 1 mg of each of
the nanomaterials. On increasing the exposure time of UV
irradiation the absorption peak intensity decreases indicating the photo-decomposition of the organic dye (MeO)

2. MATERIALS AND METHODS

2.1. Synthesis of ZnO Nanoplates

50 ml of 1 M NaOH was prepared and 1 g of poly ethylene glycol (PEG) was added and stirred for 1 hr. 0.5 M
Zn(COOCH3 2 (H2 O)2 (MERCK) was added drop-wise in
above solution. The mixture was then stirred at 60  C for
2 hr. A white precipitate was collected and washed several
times with D. W. and Ethanol (C2 H5 OH).

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Ag Grafted ZnO Nanoplates for Photocatalytic Applications

used. The two plots clearly indicate that after an exposure

for 12 hr with a time interval of 3 hr the photo-catalytic
activity of pure ZnO Nanoplates has been enhanced by
grafting of Ag on the Nanoplates.
The semiconducting metal oxides like ZnO on exposure to UV irradiation excite the material resulting in the
formation of electron hole pairs in the system. These electron hole pairs generated will interact with the molecules
attached on their surface forming reactive radicals such as

etc. from the oxygen in the metal oxide netO

2 , OH
work and hydroxyl groups on their surface respectively.25
These radicals are responsible for the catalysis of the reaction for decomposing the organic pollutant materials. The
main limiting factor in this reaction is the electron hole
pair recombination in the system. This problem is overcome when grafted or composited with noble metals (Ag,
Au) on semiconductor metal oxide materials. The noble
metal (Ag, Au) in the system acts as an electron sinks
which capture the electron from the generated electron
hole pair in semiconductor and prohibits the recombination of them. Thus, enhancing the photo-catalytic activity
Mater. Focus, 3, 17, 2014

of the synthesized nanocomposite compared to the pure

ZnO nanomaterials.
To study the photodegradation behaviour of Ag/ZnO
nanocomosite, an aqueeous solution of MeO was irradiated in the presence and abscence of nanocomposite.
Figure 4(a) shows the degradation of MeO (in terms of
the UV-visible absorption intensity) as a function of time
for bare ZnO nanorods and Ag/ZnO nanocomosite. The
Blue plot indicates no change in the absorption intensity under dark conditions. The Ag/ZnO nanocomposite
shows higher photocatalytic activity compared to bare ZnO
nanorods. The rate of decolarization of MeO as a function
of absorption intensity can be calculated using the following equation:
% = C0 Ct /C0 100
Where, C0 and C are the initial and reaction concentration
of MeO after a time t, respectively.
Figure 4(b) shows a plot of C/C0 curve as a function of
time of MeO degradation in the presence and abscene of
catalyst. The photodegradation of the dye does not occur
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Fig. 2. FESEM micrograph (A)(D) ZnO Nanoplates with sparsely grafted Ag nanoparticle. (E) EDX mapping evaluation of the synthesized nanoparticle with presence Zn, O, Ag.

Raj et al.

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Ag Grafted ZnO Nanoplates for Photocatalytic Applications

Fig. 3. UV-Vis spectra of photodegraded MeO by photocatalyst for (a)

bare ZnO and (b) Ag/ZnO nanocomposite, as a function of UV illumination time.

in the abscence of catalyst. The degradation curve of MeO

by ZnO and Ag/ZnO shows similar profile, suggesting a
similar way of degradation by both the catalyst. However,
the degradation rate of Ag/ZnO nanocomposite is higher
then bare ZnO nanorods. The kinetics of the photocatalytic efficency of the nanocomposite were evaluated by
calculating k using the first order kinetic model derived
from the Langmuir-Hinshelwood Kinetic equation.In this
model,the the first order rate constant (k) can be calculated
using the following equation:
lnC/C0  = kt
The first order rate constant (k) for zinc oxide and zinc
oxide grafted with silver were calculated from the slope
of the graphs to be 0.03814 hr1 and 0.16299 hr1
respectively. The results indicated that Ag/ZnO nanocomposite shows higher degradation rate compare to bare
ZnO nanoplates. Thus, the photocatalytic activity of ZnO
nanoplates enhances after the grafting pf Ag nanoparticles.

5. PHOTO CATALYTIC MECHANISM

Figure 5(a) shows the schematic diagram of the mechanism of enhanced photocatalytic dye degradation of MeO
by Ag/ZnO nanocomposites and Figure 5(b) shows the
chemical structure of MeO. The transfer of electron in
4

Fig. 4. (a) Shows the UV absorbance versus UV illumination time.

(b) Shows the photocatalytic degradation of MeO versus time. Inset
shows C/C0 versus time at 10 mM of Ag/ZnO nanocomposite, bare ZnO.

metal and semiconductor takes place when they are in the

contact and the direction of the electron transfer depends
on the energy states and band structure of the metal and
the semiconductor. In case of Ag/ZnO nanocomosite the
Fermi level of ZnO lies lower than the Fermi level of Ag.
Therefore, the conduction band of the ZnO undergoes a
shift, and hence the interference of Ag is responsible for
band bending. The process of band bending in Ag/ZnO
nanocomposite forms the Schottky barrier for trapped electrons. These trapped electrons are transferred to MeO for
photo-degradation.
In case of ZnO nanoplates on UV illuminator, ZnO leads
to generate electron and hole pairs (Eq. (1)). The generated electrons can be trapped by electron acceptors to
produce superoxide radical ions ( O
2  (Eq. (2)) and the
holes can be trapped by the hydroxyl group to produce
super hydroxyl radicals ( OH ) (Eq. (3)).
ZnO + h
h +
 + e c
O2 + e c

O
2

(2)

h +
OH  OH


h +
 + H2O OH + H

(1)

(3)
+

(4)

Further, methyl orange (MeO) on absorption of UV-light

goes to an excited state (MeO ), these excited state can
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Ag Grafted ZnO Nanoplates for Photocatalytic Applications

Fig. 5. (a) Shows the mechanism of the photocatalysis. (b) Shows the
structure of methyl orange.

Mater. Focus, 3, 17, 2014

Fig. 6. (a) PL spectra of ZnO Nanoplates; (b) PL spectra of Ag/ZnO

nanocomposite.

nanocomposite decreases on increasing the percentage of

Ag nanoparticles. This indicates that due to the surface
plasmon resonance (SPR) affect of Ag the electron hole
pair recombination decreases.32 At 10 mM concentration
of Ag two sharp peaks at around 361 nm and 470 nm
were observed. The change of the peaks towards right hand
side (red shift) is due to change in interaction between
Ag and ZnO Nanoplates. The red shift suggested that Ag
nanoparticles are very small (few nm) in size and easily
incorporate on the ZnO surface. On modification of ZnO
Nanoplates by Ag nanoparticles PL spectra in Figure 6(b)
shows decrement in the visible region peak whereas an
increment in the UV region peak. Also decreasing the
concentration of Ag has decreased the intensity of visible
region of PL spectra. At 25 mM conc. of Ag the visible
band due to structural defects almost diminished and only
UV peak was obtained. The PL result also suggested that
at 10 mM concentration of Ag the nanocomposite have
only point defects, shows very good crystal quality, which
is a good agreement with XRD results.
The optical absorption spectra of pure ZnO nanoplates
and AgZnO nanocomposites were shown in Figures 7(a)
and (b) respectively. Figure 7(a) shows the absorption
spectra of ZnO nanoplates. A broad peak at around 360 nm
corresponds to the characteristic peak of ZnO Nanoplates.
The optical absorbance peak of noble metals, Ag or Au
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either donate or accept electron and generate radical cation

(MeO+ ) or radical anion(MeO).26
The photo generated hole hvb+ can also reacts with
water molecule in solution leads to generate superoxide
radical anion (Eq. (4)). These super hydroxyl radicals and
holes are responsible for decomposition of MeO and produce colorless MeO.
In case of ZnO, most of the photo generated charges
can recombine, thus the photodecomposition efficiency of
MeO decreases. On the other hand, in case of Ag/ZnO
nanocomposites Ag acts as an electron acceptor causes a
fast removal of photo generated electron to the conduction
band of ZnO and this process decreases the recombination
rate of photo generated electronhole pair. Therefore, the
photocatalytic activity of Ag/ZnO composite shows significant enhancement over pure ZnO. In this process of
photo-degradation a small quantity of Ag/ZnO nanocomposite can initiate the degradation, which can further use
using recycle process.
The PL spectrum of uncoated ZnO Nanoplates is shown
in Figure 6(a) which was investigated using Shimadzu RF
5301PC at room temperature. A sharp peak at 362 nm
is observed that corresponds to radiative recombination,
occurs due to the recombination between the electrons in
the conduction band and the holes in the valence band.27
This peak is also known as a UV range emission peak.28
The two small peaks at 387 nm and 469 nm are also
observed that corresponds to UV range emission and blue
range emission.29
30 The blue emission is considered to be
due to the deep level defect produced during the growth.
Oxygen vacancies and zinc interstitial related defects are
considered as the most probable region for generation of
blue emission.31 Figure 6(b) shows the PL spectra of the
Ag/ZnO nanocomposite. The UV emission band of the

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Ag Grafted ZnO Nanoplates for Photocatalytic Applications

ARTICLE

6. CONCLUSION
In summary, a simple method was developed to synthesize Ag/ZnO nanocomposite and their photocatalytic activities were evaluated by the degradation of Methyl Orange
(MeO) under UV light irradiation. The grafting of Ag
nanoparticles was found to be enhanced the photocatalytic
activity compared to bare ZnO Nanoplates. The enhanced
photocatalytic activity of Ag/ZnO nanocomposite is due
to the behavior of Ag nanoparticles as a sink for electrons from the electron hole pair generated by irradiation
in metal-oxide semiconductor material. The XRD results
reveals that the grafting of Ag nanoparticles does not affect
the crystalline of the ZnO Nanoplates but the morphology
of the nanocomposites varied with the increased amount
of Ag. Optical properties of Ag/ZnO nanocomposites were
improved compared to the pure ZnO Nanoplates. The
optical properties of Ag nanoparticles on ZnO surfaces
were investigated by varying the concentration of Ag. The
amount of Ag content was found to control the absorption
band due to the surface plasmon resonance effect. From
the Photo luminescence and absorption spectra it is concluded that at 10 mM concentration of Ag the composite
film shows best optical properties.

Fig. 7. (a) Optical absorption spectra of ZnO Nanoplates; (b) optical

absorption spectra of Ag/ZnO nanocomposite.

is always sharp and intense compare to the nanocomposite. For pure Ag the absorbance peak at 420 nm which
corresponds to the surface plasma resonance effect. The
position and broadening of the peak depends on the size
of the metal and the semiconductor.
The aim of the grafting of Ag nanoparticles on ZnO
nanoplates is to enhance the photocatalytic efficiency in
the visible region. After the grafting of silver nanoparticles, new broad peaks at around 380 nm, 395 nm
and 440 nm appears in all samples containing Ag with
molar ratio of 2.5 mM, 5 mM and 10 mM respectively
(Fig. 7(b)), which corresponds to the surface plasmon resonance of Ag nanoparticles.33 In comparison to the narrow absorption peak of pure ZnO Nanoplates, the observed
broad bands are evidence of strong interactions between
ZnO and silver nanoparticles. After the grafting of Ag
nanoparticles the peaks were shifted towards the visible
range compared to the pure ZnO nanoplates. These results
suggested that the grafting of silver nanoparticles helps to
reduce the band gap. The results indicated that for 10 mM
concentration of Ag a broad peak appears at 430 nm. The
absorption at 430 nm originates with a good incorporation
of small size Ag nanoparticles (few nm) in ZnO matrix.111
From the absorption curve it was concluded that at 10 mM
concentration surface plasmon resonance (SPR) is maximum, which is a good agreement with PL results.
6

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