Journal of Food Measurement and Characterization

https://doi.org/10.1007/s11694-018-9974-2

ORIGINAL PAPER

Optimization of polyphenols extraction from orange peel

S. Haya1 · F. Bentahar1 · M. Trari2

Received: 11 May 2018 / Accepted: 8 November 2018

© Springer Science+Business Media, LLC, part of Springer Nature 2018

Abstract
The aim of the present study was to optimize the phenolic recovery from orange peel by investigating the effect of several
parameters on the extraction yield. The phenols were extracted in a batch reactor and the effects of the concentration and
the nature of the solvent (methanol, ethanol and hexane: 0–100% V/V), were studied. The Folin–Ciocalteau reagent (FCR)
was used for the determination of the total phenolic content (TPC) and the antioxidant activity was investigated using the
stable free radical: 2,2-diphenyl-1-picrylhydrazyl (DPPH). TPC corresponds to the gallic acid equivalent (GAE)/g dry weight
(DW) and its value (115.52 mg) was obtained at 25 °C with a stirring speed of 400 rpm in neutral medium (pH ~ 6) and a
particle size of 605 µm. The results indicated that the polyphenols content varies considerably with the solvent polarity and
the highest extraction yield was obtained with aqueous organic solvent. The inhibitory concentration ­(IC50) obtained for
DPPH inhibition was found to be 0.5%, while the DPPH inhibition showed a noticeable inhibitory activity of orange peel
with a percentage of 97%; such high value constitutes an originality of the present study.

Keywords Orange peel · Inhibitory concentration ­(IC50) · Total phenol content (TPC) · 2,2-Diphenyl-1-picrylhydrazyl
(DPPH)

Introduction C is an important water-soluble antioxidant, which protects

Phenolic compounds are ubiquitously present in vegetables,
fruits, pips, tea and juices, thus highlighting their impor-
tance in the human diet. These compounds are known to
display a wide range of physiological activities related
to the protection against various forms of environmental
stress [1]. Fruits and vegetables intake have long been asso-
ciated with a reduced risk of chronic diseases, especially
cardiovascular disease and certain types of cancer. Among
the dietary sources of polyphenols, orange is of particular
interest. This staple crop is widely consumed all over the
world and is therefore an ideal source of health-promoting
antioxidants for the human diet [2, 3]. Oranges are a main
source of vitamin C and polyphenolic compounds; vitamin
* M. Trari
solarchemistry@gmail.com; mtrari@usthb.dz
1
Laboratoire “Phenomenes de Transfert”, Faculté de Génie
Mécanique et Génie des Procédés, USTHB, El Alia,
16111 Algiers, Algeria
2
Laboratory of Storage and Valorization of Renewable
Energies, Faculty of Chemistry, USTHB, El Alia,
16111 Algiers, Algeria
compounds in extracellular and intracellular spaces in most
biological systems and reduces the copherol radicals [4].
The extraction process is a widely used unit operation in
the food industry to obtain desired components in the food
matrices [5, 6]. The extracted molecules may be used as food
additives or exert peculiar effects on the human health [7,
8]. For the extraction of phenolic compounds, conventional
methods based on the solid–liquid extraction using organic
solvents have been used. However, these techniques require
long extraction time, resulting in low yields. Therefore, sev-
eral studies devoted to the extraction of antioxidant have
explored the effect of different techniques for the recovery
of phenolic compounds from orange peel [9]. The highest
content of total polyphenol (PT) was obtained by solvent
extraction in batch mode followed by ultrasound-assisted
extraction after extraction by microwave, fourth extraction
in the presence of supercritical fluid ­(CO2), and finally a high
pressure extraction.
Other works aiming to optimize the process parameters
for the extraction of phenolic compounds on the pectin from
orange peel [10]. The treatment the authors have chosen was
the extraction by microwave at 25 °C at different powers in

13
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acidic media, the extraction yield increased from 6.7 to 9.2%
with increasing the S–L ratio.
It is well known that the natural antioxidants extracted
from herbs, wastes and spices have high activity and are used
in many food applications. Among these substances, the phe-
nolic compounds are widely distributed in the plants with
the ability to scavenge free radicals by single electron trans-
fer [11]. The nature of the solvent can affect the extraction
rates through the equilibrium-solvent that can be explained
on the basis of the transition state theory. To our knowledge,
the experimental design for optimizing the physical param-
eters has not been reported in the literature, compared to
different varieties of the extracted materials. The originality
of the present study is to extract a product rich in phenolic
compounds with a high extraction yield in short time. It
also concerns the evaluation of the recovered polyphenols
to reduce DPPH with a degradation percentage of 97%.
The influences of binary and ternary solvents systems as
well as the solvent polarity constitute a first approach to the
work in the composition of the mixture between methanol;
ethanol and hexane. The parametric study and the effects of
the solid–liquid ratio, agitation speed, temperature, pH and
granulometry on the yield of extracted polyphenols were
also undertaken. Hence, the objective of the present study
was to evaluate the effect of some physico-chemical param-
eters, namely, the solid–liquid (S–L) ratio, temperature, pH,
agitation speed and particle size on the extraction yield of
PT and TPC from orange peel, along with the antioxidant
activity.
Materials and methods
Chemicals
Na2CO3 (purity ≥ 99.9%), Folin–Ciocalteu phenol reagent
(FCR), gallic acid (purity 98%), Absolute ethanol (≥ 99.4%
V/V), Hexane (99% V/V) and Methanol (99% V/V) were
purchased from Sigma-Aldrich Chemical. All other chemi-
cals were of analytical grade and the stock solutions were
prepared with distilled water.
Sample materials
“Valencia” orange fruit was collected from the experimen-
tal field in Algeria, during the period September–December
2011. The orange Peels were dried in a free area to avoid
their transformation and degradation and powdered by a
blender. The dried powder was ground, stored in hermetic
boxes at ambient temperature, immediately packed, pro-
tected from light to avoid the reactions of transformations
and stored until their use.
13
S. Haya et al.
Preparation of extracts
One gram of powdered orange peel was extracted with
100 mL of distilled water; the mixture was then shaken at
25 °C, natural pH ~ 6.8 (not adjusted) and a stirring speed
of 400 rpm/10 min, this time corresponds to the extraction
period. After completing the extraction process, the orange
peel extract was filtered (pore diameter: 0.45 µm) in order
to get clear crude extract solution. Subsequently, the crude
extract was subjected to antioxidant assays for analysis, done
in triplicate.
Determination of total phenol content
TPC of orange peel extracts was determined with FCR
[12]; the sample (0.5 mL) was mixed with 2.5 mL of FCR.
Then, 2.5 mL of saturated ­Na2CO3 solution was added,
followed by incubation at 45 °C for 15 min. GA was used
to calibrate the
( standard) curve by using the equation:
y = 0.0076 × R2 = 0.997 and the results were expressed
in mg of GAE/g of DW. The absorbance was measured at
765 nm with a Perkin Elmer Lambda 1 UV–Vis Spectropho-
tometer; TPC was calculated from the following formula:
{ / }
TPC = VTE × CGAE DW
where TPC is total phenolic content, ­VTE the total volume
extract, ­CGAE the concentration in mg gallic acid equivalent
and DW the dry weight.
Statistical design of experiments
Full factorial design
A common experimental design is one with all input factors
set at two levels namely high (+ 1) and low (−1). A design
with all possible high/low combinations of all input factors
is called a full factorial design in two levels. If there are k
factors, each at two levels, a full factorial design has ­2k runs.
The amount of extracted polyphenol (y) from orange
peels depends on the solid/liquid ratio, agitation speed (N),
temperature and pH. A full 24 factorial design is given in
Table 1 and the factor levels are coded as − 1 (low), 0 (cen-
tral point) and 1 (high).
To determine the influence of each factor, the experi-
ments were carried out by systematically varying the
studied factors, keeping the others parameters con-
stant. A suitable experimentation technique should be
selected to assess possible interactions with a minimum
of experiments [13, 14]. In the statistical design, the
factors involved in an experiment were simultaneously
changed. The advantage was that not only the effects of
individual parameters but also their relative importance
Optimization of polyphenols extraction from orange peel

Table 1  Levels of different Experiments S/L N (rpm) T (°C) pH X1 X2 X3 X4 Concentration

process variables in coded and (g/100 mL) (mg GAE/L)
non-coded for the extraction of
polyphenol Y

1 1 100 25 2 −1 −1 −1 −1 14.40
2 5 100 25 2 +1 −1 −1 −1 115.52
3 1 400 25 2 −1 +1 −1 −1 42.5
4 5 400 25 2 +1 +1 −1 −1 103.94
5 1 100 85 2 −1 −1 +1 −1 11.38
6 5 100 85 2 +1 −1 +1 −1 14.01
7 1 400 85 2 −1 +1 +1 −1 12.63
8 5 400 85 2 +1 +1 +1 −1 11.84
9 1 100 25 10 −1 −1 −1 +1 13.35
10 5 100 25 10 +1 −1 −1 +1 75.26
11 1 400 25 10 −1 +1 −1 +1 35.69
12 5 400 25 10 +1 +1 −1 +1 110.78
13 1 100 85 10 −1 −1 +1 +1 23.94
14 5 100 85 10 +1 −1 +1 +1 27.23
15 1 400 85 10 −1 +1 +1 +1 26.57
16 5 400 85 10 +1 +1 +1 +1 26.84
17 3 250 55 6 0 0 0 0 47.36

The Test No. 17 was imposed by the design experiment is the average speed (250 rpm) between the max-
ima (400 rpm) and minima (100 rpm)

Table 2  Analysis of variance (ANOVA) DPPH radical scavenging activity

Source DF Sum of squares Mean squares F. ratio
The antioxidant activity of the extract was measured by
Model 15 21207.704 1413.85 the DPPH method [15]. DPPH solution (~ 6×10−5 mol)
Error 0 0.000 Prob > F was freshly prepared, 77 µL of sample extract was added
C. total 15 21207.704 to 3 mL of DPPH reagent and the test tube was incubated
in the dark at room temperature. The absorbance was
measured at 517 nm, by UV–Vis spectrophotometry. The
percentage inhibition of radicals was calculated from the
in a given process where the interactions of two or more formula:
variables can be derived. The regression analysis was
performed to estimate the response function as a second Radical scavenging activity (%)
order polynomial: {( )/ }
= 100 × Acontrol − Asample Acontrol
∑ ∑∑ ∑∑∑
Y = a0 + ai Xi + aij Xi Xj + aijk Xi Xj Xk
∑∑∑∑ Acontrol is the absorbance of DPPH solution without extract
+ aijkl Xi Xj Xk Xl and ­Asample the absorbance with DPPH. The inhibitory con-
centration ­(IC50) was taken as the amount of antioxidant
where Y is the predicted response and a­ 0, ­ai, ­aij, ­aijk, ­aijkl required to decrease the initial DPPH concentration by 50%.
the coefficients estimated by regression, which represent the
linear, quadratic and cross products of ­Xi, ­Xj, ­Xk and ­X1 on
the response. A statistical program JMP.8 was used for the Results and discussion
regression analysis of data and the equations were validated
by the ANOVA statistical test (Table 2). The significance of Determination of the total polyphenols content
each term in the equation is to estimate the goodness of the
fit in every case. The effect of physical parameters on the extraction of phe-
All experiments were realized with particles of mean nolic compounds from orange peel was determined on the
diameter of 231 µm, determined during the characteriza- base of single factor experiment.
tion of the solid (Table 1).

13
 S. Haya et al.

Solid–liquid (S–L) ratio
The S–L ratio is important during the mass transfer between
the solid and the solvent. The effect on the extraction yield
(Fig. 1) shows that the quantity of extracted phenol increases
with raising the mass of the solid. Since the volume of the
solvent used in each experiment is constant, the extraction
rate increases with the mass of the solid. The maximal TPC
(42 mg GAE/g DW) is obtained for S–L ratio of 4 g/100 mL,
and this could be explained by the fact that higher the mass
of solid, greater the offered contact area. A decrease in the
quantity of extracted matter is noticed beyond this value,
due to the insufficiency of solvent to wet the solid particles,
600
S/L (%)
1 compounds [12, 17].
2
500
3
4 Effect of pH
Concentration(mg GA/l)
because a high mass of solid causes a saturation of the
medium. So, it is necessary to search a compromise between
the efficiency and the installation of technological limitation.
Effect of temperature
The thermal effect on the polyphenols extraction from
orange peel (Fig. 2) shows that the yields extract increases
significantly in the temperature range (25–30 °C) and tends
to saturation at 70 °C while the extract mass increases. The
decreased extraction rate at 85 °C is mainly due to the deg-
radation of phenols to phenolic acids, (chlorogenic and neo-
chlorogenic acid) [16]. However, the increase of PT above
80 °C (52.8 mg GAE/g DW), is caused by a fast mass trans-
fer between both phases, due to the increased intraparticle
distribution of the solid, and higher solubility of phenolic

400 5

pH is a crucial parameter for controlling the separation

300 between the solid and aqueous phases, and acts on both
the solubility and ionization state of the solid [18]. It was
200 studied in the range (2–10) and its effect shows that the
better extraction of the phenolic compounds occurs at
100
pH ~ 6, because of their solubility under the working con-
ditions (Fig. 3). By contrast, the rate does not change sig-
0
0 2 4 6 8 10 12 14
nificantly in acid medium as confirmed by the TPC (38.8 g
Time (min) extract/100 g DW). On the other hand, a notable improve-
ment in the extraction yield was obtained at higher pHs
Fig. 1  Extraction yield as a function of time at different solid–liquid (> 6), caused by interaction forces, which are appreciably
ratios brought up between ­H+ and ­OH− ions on the solid surface,

Fig. 2  Effect of temperature on 12 55

the yield of phenolic extraction
from orange peel
10
50
Yield (gGA/100gDW)

Yield (gextract/100gDW)
8

45
6

4 40

2
35

0
30
0 10 20 30 40 50 60 70 80 90

Temperature (°C)

13
Optimization of polyphenols extraction from orange peel

Fig. 3  Effect of pH on the yield 12

of phenolic extraction from 48
orange peel
10 46

Yield (gGA/100gDW)

Yield (gextract/100gDW)
44
8
42

6 40

38
4
36

2 34

32
0
0 1 2 3 4 5 6 7 8 9 10 11

pH

thus favouring the phenols extraction [19]. The results are
expressed in mg gallic acid equivalent; the comparison of
the extract and gallic Acid (mg Equivalent) is made after
the antioxidant activity.
Effect of agitation speed
The high amount of polyphenols extracted at equilibrium
(48.33 mg GAE/g DW) is obtained at a speed 400 rpm,
which assures a good diffusion of ions toward orange peel
particles [20, 21]. The sorption of the malachite green from
potato peel also showed that a speed of 400 rpm gives a good
sorption performance [22].

The effect of the agitation speed (100, 200, 300 and

400 rpm) on the extraction of polyphenols from orange
peels was also studied, keeping the other parameters con-
stant. Figure 4 shows that the amount of phenols increases
with the agitation speed, due to the diffusion rate of the solid
from the bulk liquid toward the solid particles because of the
enhanced turbulence and decreased liquid boundary layer.
Effect of particle size
The granulometry of the particles also influences the het-
erogeneous reaction kinetics through the exposed surface
area and the maximal capacity of particles depends on the
specific surface area of the solid. Figure 5 shows that TPC

Fig. 4  Effect of stirring speed 12 50

on the yield of phenolic extrac-
tion from orange peel
48
10
Yield (gGA/100gDW)

Yield (gextract/100gDW)
46
8

44
6
42

4
40

2
38

0 36
0 100 200 300 400

stirring speed(r.p.m)

13
 S. Haya et al.

Fig. 5  Effect of particle size on 3,0

the yield of phenolic extraction 1,2
orange peel, D is the average
diameter 2,5
1,0

Yield (gGA/100gDW)

Yield (gextract/100gDW)
2,0
0,8

1,5
0,6

1,0
0,4

0,5 0,2

0,0 0,0
0 200 400 600 800 1000
D(µm )

does not vary significantly with the diameter; this could be
explained by the adherence of the particles between them
that prevents the penetration of the solvent and therefore
decreases the surface of the mass transfer. According to
Khan et al. lower yields observed with particles of smaller
sizes were due to the remaining particles on the solvent sur-
face during the extraction process [23]; the yield decreases
as the particle size decreases and for sizes greater than
605 µm, the extraction yield reaches 272.36 mg GAE/g DW,
due to the interfacial resistance. Consequently, the particles
with large diameter induce a lower diffusion and decrease
the extraction rate [24, 25].
Effects of the solvent on the extraction yield
and polyphenol content
The nature of solvent affects the equilibrium constants
of reactions by differential stabilization of the reactants/
products. The equilibrium is shifted toward the sub-
stance that is preferentially stabilized, demonstrating the
effects of four extracting solvents (Table 3). The solu-
bility of phenolic compounds depends on their chemi-
cal nature and varies from simple to highly polymerized
compounds. This structural diversity is responsible for
the great variability of the physicochemical properties,
influencing the polyphenols extraction [26]. Moreover,
the solubility of phenols depends on the polarity of the
solvent and methanol and hexane give the best extrac-
tion yields with a preference for hexane whereas the
low yield is observed with ethanol [27, 28]. The major-
ity of chemical groups, like phenols, are extractable by
water, in agreement with the literature data [8, 29] and
the extraction efficiency is attributed to the high solu-
bility of phenols in the polar methanol. Water, aqueous
mixtures of ethanol, hexane and methanol are generally
used for the extraction of phenolic compounds [30]. We
also tested the influence of binary and ternary systems
on TPC obtained from orange peel (Table 3). The mix-
ture water/solvent can facilitate the chemicals extraction
and this may be the reason why the yields of aqueous

Table 3  Extraction total phenol Solvent Extraction yield (%) TPC (mg GAE/mL)
content (TPC) yield of orange
peel Water 34.44 ± 0.25 111.84 ± 0.25
100% (Ethanol) 0.20 ± 0.01 17.5 ± 0.23
Water–ethanol (30%–70%) 0.25 ± 0.01 241.44 ± 1.97
100% (Methanol) 2.78 ± 0.08 79.34±0.93
Water–methanol (90–10%) 3.277 ± 0.02 253.34 ± 2.29
100%(Hexane) 1.76 ± 0.02 105.13±0.2
Water–hexane (70%–%30) 2.9 ± 0.48 185.52± 1.11
Hexane–water–ethanol (25–50%–25%) 0.074 ± 0.17 130.26± 3.28
Ethanol–water–methanol (25–50%–25%) 16.55 ± 1.11 235.52±1.31
Methanol–water–hexane (25–50%–25%) 3.87 ± 1.89 44.078 ±1.97

13
Optimization of polyphenols extraction from orange peel
methanol, ethanol, and hexane extracts are higher than
those of water, methanol and ethanol used separately.
TPC of the water extract is 111.84 mg GAE/L and
decreases in the order given in Table 3. The addition
of water to the extraction system improves the yield of
phenolic glycolyses and phenols with a higher degree
of polymerization. On the other hand, the increase of
the volume of water in the solvent can polymerize the
non-phenolic compounds like carbohydrates and pro-
teins, with the phenolic compounds, thus increaing the
extracted amount [31].
Experimental design
To examine the combined effect of four independent vari-
ables, the experiments on the extraction yield of polyphe-
nol were performed. Equation represents the mathematical
model relating the polyphenol concentration with the inde-
pendent variables:
y = 41.61625 + 19.06625X1 + 4.72375X2 − 22.3075X3
+ 0.835X4 − 2.05125X1 X2 − 18.3925X1 X3 + 4.56X2 X3
+ 1.485X1 X4 + 2.775X2 X4 + 6.00875X3 X4 + 1.245X1 X2 X3
+ 3.335X1 X2 X4 + 1.69875X1 X3 X4 − 2.38125X2 X3 X4
− 3.28625X1 X2 X3 X4
The experimental and predicted values of the polyphenol
concentration are given in Table 1. According to the last
equation, the agitation speed and the S–L ratio has a posi-
tive effect on the polyphenols extraction. By contrast, the
temperature has a negative effect while a negligible effect is
observed in acidic medium in the ranges of each selected var-
iable. Both the mass transfer and the concentration of poly-
phenol increase with raising the agitation speed. The number
of active sites on the solvent produces more ·OH radicals and
increases the extraction efficiency. The negative sign for the
thermal effect is due to the fact that an increased tempera-
ture causes a degradation of phenols, and a transformation
of phenolic acids. The maximal concentration of extracted
polyphenol is equal to 115.52 mg GAE/L under the optimal
conditions: 100 rpm, 5 g/100 mL, at pH ~ 2 and 25 °C.
Antioxidant activity
DPPH is a stable organic radical with an absorption band
at 517 nm [32]. Through this study it was concluded that
at concentration 5%, DPPH is almost completely degraded,
with an elimination percentage of 97%, showing the good
antioxidant power of orange peel with ­IC50 of ~ 0.5% and
this constitutes originality in this work. I­ C50 is inversely
proportional to the antioxidant capacity, as it expresses the
Table 4  Evaluation of IC50, anti-radical power and stoichiometry
value
Compound IC 50 (%) Anti-radical power Stoichiometry
(per g/GAE g DPPH)
Orange peel 0.5 ± 0.01 4.10−3 10
Gallic acid 0.3 ± 0.02 7.8.10−3 6
amount of the antioxidant required to decrease the DPPH
concentration by 50% [33]. ­IC50 is obtained by interpolation
from a linear regression analysis; values lower than ­IC50
indicates a high antioxidant activity (Table 4). So, one can
conclude that the orange peel is an efficient antioxidant with
a significant anti-radical power and ­IC50 value of 4×10−3 g−1
GAE/g DPPH.
Conclusion
The aim of this study was to investigate the influence of
physical parameters on the extraction yields of phenolic
compounds. The main novelty concerns the extraction of
phenolic compounds with a high yield in short time and
the recovery of polyphenols with reduce 2,2-diphenyl-1-pic-
rylhydrazyl. The duration that ensures an optimal extrac-
tion rate was found to be 10 min and the yields of poly-
phenols extraction increased significantly with raising the
temperature from 25 to 30 °C, in neutral medium leading
to a high amount of polyphenols at equilibrium (115.52 mg
GAE/L). Furthermore, an increase in the total phenolic
content (272.36 mg GAE/L) was recorded with particles
size of 605 µm. Solvents with different polarities (ethanol,
methanol and hexane) at various concentrations showed
a significant effect on the extraction yields. Antioxidants
extractions were improved by combined solvents. In addi-
tion, the obtained extracts with the solvent–water mixtures
were distinguished from those obtained with pure organic
solvents. However, water remains the best extraction solvent.
The extraction yields increased with increasing the water
content in ethanol, methanol, and hexane. The peel extract
is rich in polyphenols and the results of DPPH tests were in
accordance with those obtained in TPC determination. The
DPPH method was applied for evaluating the antioxidant
activity. Orange peel constitutes an important source of anti-
oxidant which can find various applications in the food, and
cosmetics industries.
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