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Process Biochemistry 45 (2010) 1065–1071

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Tansy fruit mediated greener synthesis of silver and gold nanoparticles

Shashi Prabha Dubey a,∗ , Manu Lahtinen b,1 , Mika Sillanpää a,∗∗
Laboratory of Applied Environmental Chemistry, Department of Environmental Sciences, University of Eastern Finland, FI-50100, Mikkeli, Finland
University of Jyväskylä, Department of Chemistry, P.O. Box 35, FI-40014 JY, Finland

a r t i c l e i n f o a b s t r a c t

Article history: In this paper we have reported the green synthesis of silver (AgNPs) and gold (AuNPs) nanoparticles by
Received 29 November 2009 reduction of silver nitrate and chloroauric acid solutions, respectively, using fruit extract of Tanacetum
Received in revised form 7 March 2010 vulgare; commonly found plant in Finland. The process for the synthesis of AgNPs and AuNPs is rapid,
Accepted 16 March 2010
novel and ecofriendly. Formation of the AgNPs and AuNPs were confirmed by surface plasmon spectra
using UV–Vis spectrophotometer and absorbance peaks at 452 and 546 nm. Different tansy fruit extract
concentration (TFE), silver and gold ion concentration, temperature and contact times were experimented
Tansy fruit extract
in the synthesis of AgNPs and AuNPs. The properties of prepared nanoparticles were characterized by TEM,
Metal nanoparticles
XRD, EDX and FTIR. Finally zeta potential values at various pH were analyzed along with corresponding
Zeta potential SPR spectra.
XRD © 2010 Elsevier Ltd. All rights reserved.

1. Introduction cles where plant extract is used for the synthesis of nanoparticles
without any chemical ingredients [10–14]. Leaf extracts of neem,
Science of the nanotechnology is supposed to have started by geranium, hibiscus, cinnamon, tamarind and coriander have also
the lecture of Richard Feyman on “There is Plenty of Room at the found suitable for the biosynthesis of silver and gold nanoparti-
Bottom” at the annual meeting of the American Physical Society cles [15–20]. Among various metal nanoparticles, AgNPs and AuNPs
at the California Institute of Technology in 1959. Due to the opti- have several effective applications as antibacterial, sensors and
cal, magnetic and electrical properties [1,2], nanomaterials have a detectors besides their biomedical applications [21–25].
long list of applicability in improving the human life and its envi- Tanacetum vulgare (tansy), a perennial herb is also known as
ronment. The first relation between human life and nanoscale was Common Tansy, Bitter Buttons, Cow Bitter, Mugwort, or Golden
developed naturally in ayurveda, which is 5000-year-old Indian Buttons. Around 1525, it was listed (by the spelling “Tansey”) as
system of medicine. It had some knowledge of nanoscience and “necessary for a garden” in Britain [26]. Tansy was considered a
technology before the term ‘nano’ was even formed, which modern cure for intestinal worms, rheumatism, digestive problems, fevers,
science has just started exploring in the 21st century [3]. Sev- sores, measles and less commonly it was used to treat menstrual
eral physical and chemical processes [4–6] for synthesis of metal irregularities and induce menstrual bleeding [27–30]. During the
nanoparticles were developed considering the real life application Middle Ages and later, high doses were used to induce abortions
of nanoparticles in the area of medicine [7], catalysis [8], detection [28,31,32]. Contradictorily, tansy was also used to help women con-
[9], etc. Recently the studies started under green chemistry for the ceive and to prevent miscarriages [27,28,33].
search of benign methods for the development nanoparticles and
searching antibacterial, antioxidant, and antitumor activity of natu-
ral products. Biosynthetic processes have received much attention
as a viable alternative for the development of metal nanoparti-

∗ Corresponding author at: Laboratory of Applied Environmental Chemistry,

Department of Environmental Sciences, University of Eastern Finland, FI-50100,
Mikkeli, Finland.
∗∗ Co-corresponding author. Tel.: +358 40 355 3410;
fax: +358 15 336 013. Inflorescence of T. vulgare
E-mail addresses:,
The principal chemical constituent of the herb is the volatile oil
(S.P. Dubey), (M. Sillanpää).
University of Jyväskylä, Department of Chemistry, P.O.Box 35, FI-40014 JY, Fin- or oil of tansy. In addition, a bitter, amorphous principle, tanacetin
land. (C11 H16 O4 ), is present [34] mainly in the flowers. Besides tanacetin,

1359-5113/$ – see front matter © 2010 Elsevier Ltd. All rights reserved.
1066 S.P. Dubey et al. / Process Biochemistry 45 (2010) 1065–1071

Fig. 1. Effect of Tansy fruit extract (TFE) quantity. (a) In silver nanoparticle (AgNPs) synthesis. (b) In gold nanoparticle (AuNPs) synthesis. (c) TEM images of silver and
nanoparticles at different leaf extract quantity. (I) S1 AgNPs at 1.8 mL TFE. (II) S2 AgNPs at 2.8 mL TFE. (III) S3 AgNPs at 4.8 mL TFE. (IV) A1 AuNPs at 1.8 mL TFE. (V) A2 AuNPs
at 2.8 mL TFE. (VI) A3 AuNPs at 4.8 mL TFE.

flower may contain several monoterpenoids [35]. The essential oil man filter paper (No. 40) was used for the filtration of boiled material to prepare the
content of tansy flowers is about twice as much as in the leaves [36]. aqueous fruit extract, which was used as such for metal nanoparticle synthesis.
Aqueous solution (1 mM) of silver nitrate and auric acid were prepared and
According to Leppig [37], the herb also contain the following con-
50 mL of those metal ion solutions were reduced using 1.8 mL of TFE at room temper-
stituents: tanacetin, tannic acid (tanacetum–tannic acid), traces of ature for 10 min. Below than this TFE quantity, the solution takes more than 20 min
gallic acid, volatile oil, a wax-like substance, albuminoids, tartaric, to get a significant SPR for both the metal nanoparticles. As a result brown–yellow
citric, and malic acids, traces of oxalic acid, a laevogyrate sugar, and pink–red solutions were formed, indicating the formation of silver and gold
resin, metarabic acid, parabin, and woody fiber. nanoparticles, respectively [38,39]. The effects of reaction conditions such as the
TFE amount, metal ion concentration, reaction temperature and contact time were
Here we have explored an inventive contribution for synthesis also studied.
of silver and gold nanoparticles using fruit extract of T. vulgare. The Spectral analysis for the development of nanoparticles at different reaction
procedure for the development of stable AgNPs and AuNPs is rapid, conditions were observed by UV–Vis spectroscopy (Perkin-Elmer Lamda-45 spec-
simple and viable. Synthesized nanoparticles were characterized trophotometer). AgNPs and AuNPs gave sharp peak in the range of visible region
of the electromagnetic spectrum. Transmission Electron Microscope (TEM) JEM-
by various methods, such as TEM, XRD, EDX, UV–Vis and FTIR.
1200EX, JEOL was used for the analysis of size and shape of developed nanoparticles.
3 ␮L of the sample was placed on copper grid making a thin film of sample on the
2. Materials and methods grid and kept for drying at room temperature for 15 min, then extra sample was
removed using the cone of a blotting paper and reserved in grid box. The presence
Fresh fruits of T. vulgare were collected from Mikkeli city. Silver nitrate and auric of elemental silver and gold was determined using energy dispersive X-ray analy-
acid were obtained from Sigma Aldrich chemicals. All glasswares were properly sis (EDX) with Zeiss Evo 50 instrument. Zetasizer (Malvern) instrumentation was
washed with water and dried in oven. used to analyze the surface charge and stability of synthesized nanoparticles at pH
Tansy fruits extract (TFE) was used as a reducing agent for the development of sil- (2–10). The pH of the solution was maintained by 1N HCl and 1N NaOH.
ver and gold nanoparticles. Properly washed 50 g of fresh tansy fruits were added in Resulting solutions of the developed nanoparticles of silver and gold were dried
250 mL ultrapure water in 500 mL Erlenmeyer flask and boiled for 10–15 min. What- at 80 ◦ C for X-ray powder diffraction measurements. The X-ray powder diffrac-
S.P. Dubey et al. / Process Biochemistry 45 (2010) 1065–1071 1067

Fig. 2. Effect of metal ion concentration. (a) In AgNPs synthesis. (b) In AuNPs synthesis. (c) TEM images of AgNPs and AuNPs at different metal concentrations. (I) S1 AgNPs
at 1 mM silver ion conc. (II) S2 AgNPs at 2 mM silver ion conc. (III) S3 AgNPs at 3 mM silver ion conc. (IV) A1 AuNPs at 1 mM gold ion conc. (V) A2 AuNPs at 2 mM gold ion
conc. (V) A3 AuNPs at 3 mM gold ion conc.

tion data was acquired by PANalytical X’Pert PRO diffractometer in Bragg–Brentano FTIR spectroscopy measurements were carried out to recognize the bio-groups
geometry using step-scan technique and Johansson monochromator to produce that bound distinctively on the silver and gold surface and involved in the synthesis
pure Cu K␣1 radiation (1.5406 Å; 45 kV, 30 mA). The ICDD PDF2 powder diffraction of these nanoparticles. Samples for the FTIR were prepared by drying native TFE and
database [40] implemented in HighScore Plus was used for the search-match phase resulting TFE with nanoparticles similarly as for powder diffraction measurements.
identification analyses. Hand-ground samples were measured by Bruker Tensor 27 FTIR spectrometer in
To estimate crystallite sizes of the produced nanoparticles, most isolated diffrac- attenuated total reflection mode (Pike Technologies, GladiATR for FTIR with dia-
tion peak positions were profile fitted using pseudo-Voigt function to establish the mond crystal) and using spectral range of 4000–400 cm−1 and resolution of 4 cm−1 .
full-width at half-maximum values (FWHM) needed for the crystallite size evalua- All the samples were analyzed twice to taking into account the potential preparation
tion made by Scherrer method. effects by placing a sample on the diamond crystal.

Fig. 3. Effect of temperature. (a) In AgNPs synthesis. (b) In AuNPs synthesis.

1068 S.P. Dubey et al. / Process Biochemistry 45 (2010) 1065–1071

Fig. 4. Effect of contact time. (a) In AgNPs synthesis. (b) In AuNPs synthesis.

3. Result and discussion b). In case of AgNPs, peak absorbance increases with metal ion
concentration from 1 to 3 mM but decreases at 3 mM gold ion con-
3.1. Effects of TFE quantity centration in case of AuNPs. TEM images of AgNPs and AuNPs at
different metal ion concentrations have been presented in Fig. 2c.
Different TFE quantities were used for the synthesis of AgNPs The particle size of AgNPs was found larger at higher metal ion
and AuNPs. The fruit extract quantity was varied from 0.5, 1.0, 1.8, concentration and red shift occurred in the SPR spectra which
2.8, 3.8, 4.8 mL in 50 mL of 1 mM silver nitrate and auric acid solu- in well correlation with the Mock et al.’s work [41]. In compari-
tion, respectively. With increase in TFE quantity from 0.5 to 4.8 mL son to AgNPs the AuNPs express larger sized nanoparticles which
in 50 mL of 1 mM metal ion solution, consistently an increase in were observed in TEM imaging at higher metal ion concentra-
peak absorbance was found in UV–Vis spectrum (Fig. 1a and b). tion.
Likewise, visual inspection of the solutions revealed color changes
from reddish yellow to deep red and light pink to dark pink on
both silver and gold solutions with an increase of TFE quantity in 3.3. Effect of reaction temperature
each reaction solution. Interpretation of TEM images of AgNPs and
AuNPs at 1.8, 2.8 and 4.8 mL of TFE suggests decrease in particle The SPR spectra were taken after 10 min heating of the sample at
size with an increase in TFE quantity (Fig. 1c). different temperature. By increasing reaction temperature from 25
to 150 ◦ C, an increase in peak sharpness was found in case of both
3.2. Effect of metal ion AgNPs and AuNPs (Fig. 3a and b). It may be due to increasing reac-
tion rate for NPs synthesis [11]. This sharpness in absorbance peak
Surface plasmon resonance spectra for AgNPs and AuNPs were depend on size of the synthesized nanoparticle as with higher tem-
obtained at 452 and 546 nm with brown–yellow and pink–red col- perature, particle size may be smaller, which results into sharpness
ors, respectively, at different metal ion concentration (Fig. 2a and of the plasmon resonance band of AgNPs and AuNPs [41,42].

Fig. 5. Effect of pH. (a) Zeta potential at different pH. (b) Effect of pH on SPR of AgNPs. (c) Effect of pH on SPR of AuNPs.
S.P. Dubey et al. / Process Biochemistry 45 (2010) 1065–1071 1069

3.4. Effect of reaction time

Formation of nanoparticles started within 10 min and spectra

were recorded after at 10 min, 1, 2, 3, 4 and 5 h. Effect of the reac-
tion time on AgNPs and AuNPs synthesis was also evaluated with
UV–Vis spectra and it is noted that with an increase in time the
peak become shaper (Fig. 4a and b). The reaction time found for the
development of nanoparticles in this study was found significantly
lower than in earlier reports [42,43].

3.5. Effect of pH on NPs stability

Zeta potential (ZP) values reveal details about the surface charge
and stability of the synthesized silver and gold nanoparticles. At dif-
ferent solution pH, there was little variation in the zeta potential
value of AuNPs. However, AgNPs demonstrate lower ZP value at
strongly acidic pH, whereas higher values were obtained at more
alkaline pH solutions (Fig. 5a). In overall, the results of zeta poten-
tial value for AgNPs and AuNPs are −26 and −31 mV, respectively, Fig. 6. Experimental diffraction patterns of silver and gold nanoparticle samples
indicating the stability of the synthesized nanoparticles which was AgNPs (a), and AuNPs (b). The peak positions of elemental Ag and Au are indicated
also supported by absorbance peaks in SPR spectra at various pH by  marks and positions of KCl phase by stick plot.
(Fig. 5b and c). It can be said that at acidic pH, the particle size are
comparatively larger than the basic pH, as blue shift was clearly ples. No other gold containing compounds than the metallic Au can
reported in the SPR spectra [41]. be recognized from the XRD pattern. The crystallite sizes of the
nanoparticles were estimated by the Scherrer method as Eq. (1):
3.6. Characterizations of the nanoparticles
D= (1)
ˇs cos 
TEM images showed that particles are mostly triangular and
spherical in shape, whereas some particles showed hexagonal in which D is the average size of the crystallites, K is the shape-
shapes as well. The sizes found for NPs are roughly in the range dependent Scherrer’s constant correlating to the true shape of
of 10–40 nm (Figs. 1c and 2c). crystallite (0.94 is used to correspond spherical crystallites with
The experimental powder diffraction (XRD) patterns of the pre- cubic symmetry);  is the radiation wavelength (1.5406 Å); ˇs is
pared silver and gold nanoparticles are shown in Fig. 6. On the the full peak width (given in radians) caused by structural broad-
XRD pattern of AgNPs, diffraction peaks at 38.13◦ , 44.21◦ , 64.47, ening due to crystallite size subtracted by instrumental broadening
77.37◦ , 81.47◦ , 98.01◦ 110.56◦ and 114.80◦ can be assigned to obtained by standard material (Si) in identical measurement con-
face-centered cubic (FCC) metallic silver (identified by PDF-2 ref. 4- ditions;  = diffraction angle.
0783). Whereas any peaks originating from potential silver oxides The FWHMs of the most isolated peaks at about 38.1◦ (1 1 1),
cannot be observed. However, two crystalline “impurity” phases 77.5◦ (3 1 1) and 114.8◦ (4 2 0) in 2 for both AgNPs and AuNPs
can also be identified from the pattern, which are AgCl (31-1238) (structurally isomorphous with silver) were used for size evalu-
and KCl (41-1476). ation. Average crystal size of 16 nm was determined for AgNPs,
In case of gold containing sample, the characteristic diffraction whereas for AuNPs somewhat smaller crystal size of 11 nm was
peaks of FCC metallic gold phase (4-0784) at 38.21◦ , 44.39◦ , 64.62◦ , obtained (Table 1). Elemental silver and gold peak found in the EDX
77.59◦ , 81.75◦ , 98.16◦ , 110.89◦ and 115.27◦ can be observed. Along study which is in accordance with the XRD results (Fig. 7).
with the AuNP phase, peak positions corresponding to a highly crys- The FTIR spectra of untreated and treated AgNPs and AuNPs
talline potassium chloride phase can be observed. By comparing samples are shown in Fig. 8. The untreated fruit extract sample
the XRD patterns containing either AgNPs or AuNPs, the content of show medium or strong absorption bands about at 3281, 2920,
crystalline KCl is significantly higher on AuNP than on AgNP sam- 1595, 1260, 1067 cm−1 suggesting –OH [44], aliphatic –CH stretch-

Fig. 7. EDX graph of AgNPs and AuNPs.

1070 S.P. Dubey et al. / Process Biochemistry 45 (2010) 1065–1071

Table 1 developed nanoparticles and produce a negative surface charge for

Average crystal size of AgNPs and AuNPs in samples.
AgNPs and AuNPs. This simple, low cost and greener method for
Sample Peak position (Miller indices) Mean value development of silver and gold nanoparticles may be valuable in
◦ ◦ ◦ environmental, biotechnological and biomedical applications.
38.1 (1 1 1) 77.5 (3 1 1) 114.8 (4 2 0)
(nm) (nm) (nm)

AgNPs 14 17 17 16 Acknowledgments
AuNPs 14 10 10a 11
Calculated from peak 110.9◦ instead of 115.2◦ because of peak overlap with KCl
The authors are pleased to acknowledge the European Commis-
peak. sion (Brussels) for the Marie Curie Research Fellowship for Transfer
of Knowledge (No. MTKD-CT-2006-042637) for financial support.


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