Food Chemistry 125 (2011) 255–261

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Food Chemistry
journal homepage: www.elsevier.com/locate/foodchem

Analytical Methods

Microwave steam diffusion for extraction of essential oil from orange peel:
Kinetic data, extract’s global yield and mechanism
Asma Farhat a,c, Anne-Sylvie Fabiano-Tixier c,*, Mohamed El Maataoui b, Jean-François Maingonnat c,
Mehrez Romdhane a, Farid Chemat c
a
Unité de Recherche Modélisation, Analyse et Commande de Systèmes, Ecole Nationale d’Ingénieurs de Gabès, 6029 Gabès, Tunisia
b
UMR 406, Université d’Avignon et des Pays de Vaucluse, INRA, 84000 Avignon, France
c
UMR 408, Université d’Avignon et des Pays de Vaucluse, INRA, 84000 Avignon, France

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

Article history: The microwave steam diffusion (MSDf) apparatus for extraction of essential oils from orange peel (by-
Received 8 February 2010 products) was studied. MSDf has been compared with conventional steam diffusion (SDf). A response sur-
Received in revised form 15 June 2010 face methodology (RSM) was realised to investigate the influence of process variables by a central com-
Accepted 29 July 2010
posite design (CCD) approach. The statistical analysis revealed that the optimal conditions for the
extraction of orange essential oil were a steam mass flow rate of 25 g min1 and a microwave power
of 200 W. Cytohistological investigations using light microscopy provided evidences for rapid and pro-
Keywords:
nounced cell and tissue alterations of oil glands with MSDf in comparison with SDf. The essential oils
Microwave extraction
Green process
extracted by MSDf for 12 min were quantitatively (yield) and qualitatively (aromatic profile) similar to
By-product those obtained by SDf for 40 min. Extraction of essential oils from orange peel with MSDf was better than
Essential oil SDf in terms of energy saving, cleanliness and reduced waste water.
Mechanism Ó 2010 Elsevier Ltd. All rights reserved.

1. Introduction chemical and food industry in order to replace the conventional

Extraction is one of the key technologies for sustainable growth
of the agro-food industry and economy of the process industry, and
also often requiring up to 50% of investments in a new plant and
more than 70% of total process energy used in food industries
(Clark & Macquarrie, 2002). Existing extraction technologies suffer
from considerable technological and scientific bottlenecks which
are difficult to overcome, such as reduction of energy consumption,
and fulfilment of increasingly stringent legal requirements on
emissions product/process and materials safety and control.
Therefore, in the last few years there has been an increasing de-
mand for novel green process technologies, starting from the idea
that pollution and hazards have to be eliminated at the source,
thus reducing environmental impact and costs (Nelson, 2003). As
a consequence, an increased interest exists for improvement, de-
sign and development of new green processes for the extraction
of essential oil from bio-product. Thus, auxiliary techniques as
ultrasound and microwave irradiation have been used to enhance
extraction performances (Cravotto et al., 2008; Pérez-Serradilla, Ja-
pon-Lujàn, & Luque de Castro, 2007; Romdhane & Gourdon, 2002).
Recently, much attention has been given to the application of
microwave dielectric heating in many various processes in the
* Corresponding author.
E-mail address: anne-sylvie.fabiano@univ-avignon.fr (A.-S. Fabiano-Tixier).
extractive methods. Microwave extraction is now recognised as
efficient technique that dramatically reduces extraction time, in-
creases the yield and the quality of the extract (Abert Vian, Fernan-
dez, Visinoni, & Chemat, 2008; Chemat et al., 2006; Ferhat, Meklati,
& Chemat, 2007; Ferhat, Meklati, Smadja, & Chemat, 2006; Ferhat,
Meklati, Visinoni, Abert Vian, & Chemat, 2008; Letellier & Budzin-
ski, 1999; Teo, Tan, Hong Yong, Hew, & Ong, 2008).
Citrus is the largest fruit crop in the world (100 million cubic
tons per year) and the orange account for 60% (Oreopoulou & Tzia,
2006). The remaining orange peel account for approximately 45%
of the total bulk (Yeoh, Shi, & Langrish, 2008). Consequently, signif-
icant amounts of orange peel are available as a by-product. The or-
ange peel, if treated as waste materials, may create environmental
problems, particularly water pollution, due to the presence of bio-
materials such as essential oil (Berna, Tàrrega, Blasco, & Subirats,
2000; Ferhat et al., 2006, 2007, 2008), pectin (Yeoh et al., 2008;
Zhongdong, Guohua, Yunchang, & Kennedy, 2006) and sugar. This
problem could be turned into an asset, if potentially marketable ac-
tive principles such as essential oil could be extracted from the
peel. After extraction, the peel could be a high protein stock feed
in dry form, increasing the potential return for the orange juice
industry and reducing the pollution (Yeoh et al., 2008). Orange
essential oil is used to add the orange aroma to products such as
carbonated drinks, ice creams, cakes, air-fresheners and perfumes
(Braun & Cohen, 2007). Recently, other applications make use of

0308-8146/$ - see front matter Ó 2010 Elsevier Ltd. All rights reserved.
doi:10.1016/j.foodchem.2010.07.110
256 A. Farhat et al. / Food Chemistry 125 (2011) 255–261
the d-limonene, major component of orange essential oil, as green
solvent for extraction of fats and oils from olive seeds in combina-
tion with microwave energy (Virot, Tomao, Ginies, Visinoni, & Che-
mat, 2008).
The aim of present study is to operate and optimise a green pro-
cess for the extraction of essential oil from orange peel: Microwave
steam diffusion (MSDf). The effect of mass flow rate of steam and
microwave power was studied using the response surface method-
ology (RSM). Optimal operating conditions were determined in or-
der to achieve optimal extraction time. Extraction mechanism was
proposed to understand the action of MSDf using kinetic data and
cytohistological investigations.
2. Materials and methods
2.1. Plant material
In this study, about 100 kg of orange (Citrus sinensis L. Osbeck
from Valencia late cultivar, Spain) peel were collected locally after
juice extraction (which separates the external part of the orange
(peel), giving a yield approximately of 20% (w/w) of orange peel
with respect to the whole fruit). Moisture content determination
was carried out by conventional Dean–Stark distillation apparatus.
The initial moisture content of orange peel was 90%. Fresh plant
material was employed in all extractions.
2.2. Microwave steam diffusion apparatus and procedure
Microwave steam diffusion (MSDf) has been performed in a
Milestone NEOS microwave laboratory oven (Milestone, Bergamo,
Italy, www.milestonesrl.com) illustrated in Fig 1. It is a multimode
Steam
Generator
Microwave oven
Packed bed
Reactor
Support
Cooler
Essential oil
Aqueous phase
Receiving flask
Waste-water
Fig. 1. Schematic diagram of the experimental apparatus of microwave steam
diffusion (MSDf).
reactor 2.45 GHz with a maximum delivered power of 1000 W var-
iable in 10 W increments, equipped with Pyrex extraction vessels
with a capacity of 1500 ml. Time, temperature and power were
controlled. During experiments temperature was monitored by
temperature sensor optic fibres which were inserted in the centre
and outer layer of orange peels and also in the bulk reactor. Tem-
perature variations in different parts of plant material and reactor
were measured continuously and data were saved automatically. A
Wattmeter (W) has been added at the generator entrance, in order
to measure power consumption.
In a typical MSDf procedure at atmospheric pressure, batch of
250 g of fresh orange peel were packed into cylindrical Pyrex reac-
tor. The raw material forms the packed bed. The saturated steam
was produced by electrical steam generator, passes through the or-
ange bed, whilst the mixture was continuously heated in a micro-
wave cavity. The combination of microwaves with saturated steam
favours the release of essential oils trapped inside the cells of plant
tissues. A mixture of hot ‘‘crude juice” and steam moves thus nat-
urally downwards by earth gravity into a spiral condenser outside
the microwave cavity. The extraction was continued until no
essential oil was obtained. The essential oil is collected, dried with
anhydrous sodium sulphate and stored at 4 °C until analysed.
Extractions were performed at least three times, and the mean val-
ues were reported.
2.3. Steam diffusion apparatus and procedure
For rigorous comparison, the same glassware and same operat-
ing conditions have been used for conventional steam diffusion
(the same process but without use of microwaves). In this system,
the vapour produced by the steam generator crosses the orange
peel bed, charged with the essential oil then passes through the
condenser to a receiving Florentine flask. The extraction was con-
tinued at 100 °C until no distillate was obtained. The essential oil
is collected, dried with anhydrous sodium sulphate and stored at
4 °C until used. A Wattmeter (W) has been added at the generator
entrance, in order to measure the power consumption. Extractions
were performed at least three times, and the mean values were
reported.
2.4. Design of experiment
Box–Wilson design, also called Central Composite Design (CCD),
was used to achieve optimal conditions of the process with a min-
imal number of possible experiments. The type of CCD used in this
study was central composite face-centred (CCF) experimental de-
sign to determine the optimal conditions of MSDf. The application
of a CCF design is a convenient way to optimize a process with five
levels (a, 1, 0,+1, and + a) for each factor. In this design, the star
points are at the centre of each face of the factorial space, thus
±a = ±1. This design is needed to evaluate the effects and interac-
tions of tow independent variables, namely mass flow rate of
steam (Gv), and power (Pw). The microwave irradiation power
was varied between 50 and 200 W whereas the values of mass flow
rate of steam were examined from 10 to 40 g min1. A total of 12
different combinations, including 22 full factorial design (±1) with
four axial points (±a) and four replicates of centre point (coded 0),
chosen in random order according to a CCF configuration for tow
factors, was employed for response surface modelling.
The selected optimisation response was the extraction time of
orange essential oil obtained by MSDf denotes t (min). The exper-
imental designs used were constructed and the experimental re-
sults were processed by using the software STATGRAPHICS PLUS
(Version 5.1, Statistical Graphics Corporation, Rockville, USA,
2000). An analysis of variance (ANOVA) with 95% confidence level
was then carried out for each response variable in order to test the
 A. Farhat et al. / Food Chemistry 125 (2011) 255–261
model significance and suitability. The F-value in ANOVA is the ra-
tio of mean square error to the pure error obtained from the repli-
cates at design centre and the P-value defines the significance of
the different variables. A description of significant effects obtained
from ANOVA for extraction time t (min) was presented by a Stand-
ardised Pareto Chart (Živorad, 2004).
2.5. Gas chromatography–mass spectrometry
Essential oils composition was determined by gas chromatogra-
phy coupled to mass spectrometry (GC–MS) analysis on a Hewlett–
Packard 6890 gas chromatograph coupled to a 5973A mass spec-
trometer, using two fused-silica-capillary columns with different
stationary phases. The non-polar column was HP5MS™ (30 m 
0.25 mm  0.25 lm film thickness) and the polar one was a Stabil-
wax™ consisting of Carbowax™-PEG (60 m  0.25 mm  0.25 lm
film thickness). GC–MS spectra were obtained using the following
conditions: carrier gas He;flow rate 0.7 ml min1;split 1:20;injec-
tion volume 0.1 ll; injection temperature 250 °C; oven tempera-
ture progress from 60 to 280 °C at 2 °C min1; the ionisation
mode used was electronic impact at 70 eV. Most constituents were
tentatively identified by comparison of their GC Kovats retention
indices (RI), determined with reference to an homologous series
of C5–C28 n-alkanes and with those of authentic standards available
in the authors’ laboratory. Identification was confirmed by com-
parison of their mass spectral fragmentation patterns with those
stored in the MS database (National Institute of Standards and
Technology and Wiley libraries) and with mass spectra literature
data (Adams, 1995;Arctander, 1994).
The relative percentage of the components was electronically
calculated from GC-FID peak areas. A Hewlett–Packard 6890 GC-
FID system was used for gas chromatography analysis, fitted with
a fused-silica-capillary column with an apolar stationary phase
HP5MS™ (30 m  0.25 mm  0.25 lm film thickness). The column
temperature programme was 60 °C for 8 min increased at
2 °C min1 to 250 °C and held at 250 °C for 15 min. Injection was
performed at 250 °C in the split-less mode; 1 lL of sample was in-
jected. A flow rate of 0.3 ml min1 carrier gas (N2) was used. Flame
ionisation detection was performed at 320 °C.
2.6. Cytohistology
A cytohistological study was carried out to assess the effects of
extraction methods at cellular and tissular levels. For this purpose,
rind fragments (5  5 mm) from each treatment and from control
were fixed in formalin–acetic acid–alcohol (1/1/8, V/V/V), rinsed
in tap water and stored in 70% alcohol until required. They were
then dehydrated in a graded alcohol series (80–100%) and embed-
ded in methacrylate resin. Sections (3 lm thickness) were serially
cut using a rotation microtome and stained to specifically visualise
polysaccharides and proteins (El Maâtaoui & Pichot, 1999). Obser-
vation and photographs were made using a light microscope (Leica
DM 2000) equipped with a digital camera (DFC 30F).
3. Results and discussion
3.1. Central composite design results
The effect of mass flow rate of steam Gv (g min1), and micro-
wave power Pw (W) on extraction of essential oil from orange peels
in terms of extraction time t (min) was evaluated by response sur-
face methodology. ANOVA for extraction time obtained by MSDf
gave a coefficient of determination (R2) of 91.8%, which indicates
a close agreement between experimental and predictive values.
ANOVA data for extraction time are also shown on a Pareto Chart
257
Standardized effects
Gv : Mass flow rate +
-
Pw: Microwave power
G v Pw
Pw Pw
Gv Gv
0 1 2 3 4 5
Fig. 2. Standardised Pareto chart.
(Fig. 2), which represents the significant effects of all variables (lin-
ear and quadratic) and their interactions. The length of the bars is
proportional to the absolute magnitude of the estimated effects
coefficients whilst the dashed line represents the minimal magni-
tude of statistically significant effects (95% of the confidence inter-
val) with respect to response. It can be seen that mass flow rate of
steam has the most important influence on extraction time fol-
lowed by microwave power, interaction of microwave power and
mass flow rate of steam and squared term of power. The experi-
mental data built after running 12 trials allowed us to fit all the re-
sponses as a function of mass flow rate of steam and power. The
second-order polynomial equations of the response surfaces ob-
tained are as follow:
tðminÞ ¼ 9:58  17:66Gv  24:16Pw þ 16:25G2v þ 20:5Gv Pw
þ 18:75P2w ð1Þ
where t denotes extraction time (min), Gv the mass flow rate of
steam (g min1) and Pw is the microwave power (W).
Response surface optimisation can be found depending on the
two key variables, namely, mass flow rate of steam and microwave
power. The optimal conditions obtained from the first derivatives
of the second-order polynomial equation were derived a second
time. The derivatives were then equalled to 0 and solved in an
equation system. The coded values obtained from these equations
were thus decoded and rounded in order to be applied to the de-
vice. On the basis of the results obtained by CCF design, the optimal
extraction time of orange essential oil obtained by MSDf is 12 min
for the following optimal operating conditions: (i) Mass flow rate
of steam: Gv = 25 g min1, (ii) Microwave power: Pw = 200 W.
3.2. Composition of essential oil
The retention time, molecular formula, content, and total con-
tent of chemical compositions in essential oils obtained from fresh
orange peel are listed in Table 1. The essential oils extracted by
MSDf or SDf are rather similar in their composition. The same
number of volatile secondary metabolites is found in the essential
oils isolated by MSDf or SDf, with similar yields. Limonene is the
most abundant component in the essential oil extracted from or-
anges peel with equivalent relative amounts for both extraction
methods: 94.88% and 95.03%, respectively, for MSDf and SDf. Linal-
ool, an oxygenated monoterpene, is present at 0.29% and 0.22%,
respectively for MSDf and SDf. Therefore, in this application, micro-
wave irradiation highly accelerated the extraction process, without
major modifications in the volatile oil composition, phenomenon
which was already described (Chemat et al., 2006). The influence
of microwave energy on extraction is strictly thermal and the
microwave energy quantum is given by the usual equation
W = h.m. Within the frequency domain of microwaves and hyper-
258 A. Farhat et al. / Food Chemistry 125 (2011) 255–261

Table 1 1.8
Chemical compositions of orange peel essential oils obtained by MSDf and SDf. Yield (%)
No. Compounds RIa RIb MSDf SDf 1.6
(%) (%)
Monoterpenes 98.23 98.13
B C B’
1.4
C’
1 a-Pinene 926 1023 0.45 0.43
2 Sabinene 961 1121 0.53 0.32
3 b-Pinene 974 1109 0.04 0.02
4 b-Myrcene 988 1165 1.59 1.54 1.2
5 a-Phellandrene 1001 1268 0.28 0.23
6 D3-Carene 1014 1290 0.24 0.28
1.0
7 Limonene 1030 1206 94.88 95.03
8 c-Terpinene 1103 1285 0.22 0.28
Oxygenated monoterpenes 0.43 0.35 0.8
9 Linalool 1125 1538 0.29 0.22
10 Citronellal 1167 1478 0.01 0.01
11 Terpin-4-ol 1191 1590 0.01 0.02 0.6
12 a-Terpineol 1203 1677 0.02 0.01
13 Nerol 1237 1781 0.02 0.02
14 Neral 1268 1670 0.01 0.01 0.4
15 Geranial 1284 1714 0.06 0.05
16 Perilla alcohol 1313 1991 0.01 0.01
0.2
Sesquiterpenes 0.16 0.13
17 a-Copaene 1357 1491 0.01 0.01
A A’ time (min)
18 b-Elemene 1373 1583 0.01 0.01 0.0
19 (E)-Caryophellene 1391 1594 0.01 0.01 0 10 20 30 40 50 60
20 trans-a-Bergamotene 1437 1577 0.01 0.01
21 a-Humulene 1450 1657 0.02 0.01 Fig. 3. Yield profile of oranges essential oil obtained by MSDf (j) and SDf (h) as
22 (E)-b-Farnesene 1453 1650 0.01 0.01 function of the extraction time.
23 Valencene 1488 1705 0.09 0.07
Oxygenated sesquiterpenes 0.04 0.03
24 Caryophellene oxide 1570 1977 0.02 – of SDf. The overall yield of essential oils obtained from orange peel
25 b-Sinensal 1701 2341 0.01 0.02 was 1.54% and 1.51% by MSDf and SDf, respectively. Thus, one of
26 Nootkatone 1799 2250 0.01 0.01 the advantages of the MSDf method is rapidity. For both tech-
Other oxygenated compounds 0.41 0.53 niques, the behaviour is similar and two phases are observed in
27 n-Nonanal 1126 1400 0.15 0.30 the process of extraction kinetics. The first part (AB or A’B’) is rep-
28 Decanal 1211 1497 0.18 0.15
resented by an increasing line, which characterises the rapid in-
29 Undecanal 1318 1592 0.06 0.05
30 a-Terpinyl acetate 1335 1684 0.01 0.02 crease in the yield and representing approximately 96% of the
31 Citronellyl Acetate 1342 1645 0.01 0.01 total yield, suggesting that the essential oil is easily accessible by
the steam. The second part (BC or B’C’) corresponds to a horizontal
Total oxygenated compounds (%) 0.88 0.91 line which marks the end of the extraction process. The same re-
Total non oxygenated compounds 98.39 98.26
marks were noticed by Farhat, Ginies, Romdhane and Chemat
(%)
Extraction time (min) 12 40 (2009) for the extraction of essential oil from lavender flowers by
Yield (%) 1.54 1.51 the same process.
a
Retention indices relatives to C5–C28 n-alkanes calculated on non-polar
HP5MS™ capillary column. 3.4. MSDf extraction mechanism
b
Retention indices relatives to C5–C28 n-alkanes calculated on polar Carbowax™-
PEG capillary column.
Our proposed mechanism will refer to cytohistological analysis
and to kinetic temperature profile of extraction.

frequencies (300 MHz–300 GHz), the corresponding energies are,

respectively, 1.24  106 to 1.24  103 eV. These energies are
much lower than the usual ionisation energies of biological com-
pounds (13.6 eV), covalent bond energies like OH (5 eV), hydrogen
bonds (2 eV), Van der Waals intermolecular interactions (lower
than 2 eV) and even lower than the energy associated to Brownian
motion at 37 °C (2.7  103 eV). From this scientific point of view,
direct molecular activation of microwaves should be excluded.
Some kind of step by step accumulation of the energy, giving rise
to a high-activated state should be totally excluded due to fast
relaxation.
3.3. Extraction kinetics
Fig. 3 shows the evolution of the extraction yield according to
the extraction time. No striking differences were found in oil yield
with the both techniques, the only difference observed is the dura-
tion of extraction. An extraction time of 12 min with MSDf pro-
vides yields comparable to those obtained after 40 min by means
3.4.1. Cytohistological analysis
Fig. 4(a,b and c) are micrographs of the untreated orange peel,
which can be compared with structures of MSDf treated orange
peel in Fig. 4a’ and b’ and SDf treated orange peel in Fig. 4c’. Sec-
tions from peel fragments collected before extraction (controls)
showed a gross histological structure, typical of the genus Citrus
(Bennici & Tani, 2004; Knight, Klieber, & Sedgley, 2001; Liang,
Wu, Lun, & Lu, 2006; Margosan, Aung, Wergin, & Erbe, 2001).
The oil containing part (flavedo) consisted of epidermal and hypo-
dermal layers that surround a massive parenchyma with numerous
gland cavities (GC) (Fig. 4a). Peripheral tissues exhibited thick-
walled cells whereas the inner parenchyma (IP) of oil glands
showed highly vacuolated cells with thin walls (Fig. 4b and c).
Comparative analysis of section from MSDf (Fig. 4a’ and b’) and
SDf (Fig. 4c’) extracted peel show similar cytohistological altera-
tions. Both procedures resulted in cell flattening, cell disintegra-
tion, cell wall loosening and gland opening (Fig. 4). However,
MSDf appeared to induce noticeable gland destructuration partic-
ularly in the inner parenchyma (compare Fig. 4a’, b’ and c’). All
 A. Farhat et al. / Food Chemistry 125 (2011) 255–261
Fig. 4. Structure of orange flavedo prior (a, b, c), after MSDf extraction (a’, b’) and after SDf extractions (c’). GC = gland cavity, E = epidermis, and IP = inner parenchyma cells.
Bars = 25 lm (a and a’), 15 lm (b, c and b’), 18 lm (c’).
the sectioned specimen after MSDf treatment were characterised
by absence of a structured inner parenchyma (Fig. 4a’). In many
cases this tissue persisted only in form of masses of scattered cell
debris bordering gland cavities (Fig. 4b’). As can be seen in
Fig. 4c’, SDf extraction resulted in inner parenchyma flattening
without cells dissociation. These observations suggest that micro-
wave radiation has a stronger destructive effect on the oil-contain-
ing structures of orange peel. Indeed, it has been reported that the
main essential oil-accumulating structures in Citrus fruits are the
gland cavities and their inner parenchyma (Margosan et al.,
2001). Similar effects were pointed out by Ferhat et al. (2006) using
microwave extraction of essential oils from orange peel. When the
glands were subjected to the pressure, build-up within the glands
could have exceeded their capacity for expansion, and caused their
rupture more rapidly than in conventional extraction.
3.4.2. Kinetic temperature profile
Fig. 5 shows temperature profiles during MSDf and SDf extrac-
tion. For both processes, two phases are observed in the process of
extraction. The first part is represented by an increasing line until
the temperature reaches 100 °C and thus achieves the distillation
of the first essential oil droplet. In the second part, the extraction
temperature is approximately equal to water boiling temperature
at atmospheric pressure in the case of SDf whereas it was equal
to 105 °C in the case of MSDf until the end of extraction. However,
one of the most important differences was observed between the
both extraction methods, is the ability of MSDf process to quickly
raise the temperature of the sample to the desired extraction tem-
perature. Thus, this rapid increasing of extraction temperature
259
gives to acceleration of extraction rates under microwaves and
could be due to a synergy combination of the two transfer phe-
nomena mass and heat acting in the same way. This could be ex-
plained by the fact that in the case of SDf, mass transfer occurs
from the inside to the outside whilst heat transfer occurs from
the outside to the inside. For microwave extraction, the two trans-
port phenomena are in the same direction from the inside to the
outside of the peel, which facilitates oil diffusion from the inside
of the peel to steam by an increase in the of temperature rate
due to the use of microwave.
The results obtained with these both analyses explain the abil-
ity of MSDf process to accelerate the rate of extraction by rapid in-
crease of temperature resulting with rupture of the cells and the
glands of plants materiel more rapidly than conventional SDf and
these results are confirmed by the cytological study.
3.5. Cost, cleanliness, scale-up and safety considerations
The reduced cost of extraction of essential oil is clearly advan-
tageous for the proposed MSDf method in terms of energy and
time. The MSDf procedure required an extraction time of 12 min
versus 40 min of conventional SDf. The energy required to perform
the two extraction methods are, respectively, 300 kWh kg1 essen-
tial oil for SDf and 120 kWh kg1 essential oil for MSDf. Also, the
waste waters rejected were 85 L kg1 essential oil for MSDf against
290 L kg1 essential oil for SDf. Regarding environmental impact,
the calculated quantity of carbon dioxide rejected in the atmo-
sphere is higher in the case of SDf (238 kg CO2 kg1 essential oil)
than for MSDf (95 CO2 kg1 essential oil). The power consumption
260 A. Farhat et al. / Food Chemistry 125 (2011) 255–261
Fig. 5. Temperature profiles as a function of time during MSDf and SDf extractions of essential oil from orange peels.
has been determined with a Wattmeter at the microwave genera-
tor entrance and the electrical heater power supply. These calcula-
tions have been made according to the literature: to obtain 1 kWh
electricity from fuel, 800 g of CO2 will be rejected in the atmo-
sphere during combustion of fossil fuel (Bernard, 2001).
MSDf could also be used to produce larger quantities of essen-
tial oils by using existing large-scale microwave extraction reac-
tors. These microwave reactors are suitable for the extraction of
10, 20, or 100 kg of plant material per batch (Chemat, 2009). These
reactors could be easily modified and used for MSDf extractions.
4. Conclusions
A rapid and green process of extraction of essential oil was
developed in this study: Microwave steam diffusion (MSDf). This
green microwave extraction process offers important advantages
over traditional steam diffusion, namely; shorter extraction times
(12 min versus 40 min for SDf), lower energy consumption, lower
cost and reduced waste water. The aim of this work was to confirm
the efficiency of this microwave process and to explain how micro-
wave extraction highly accelerated the extraction process, without
causing considerable changes in the volatile oil composition and
properties. Besides, the light microscopy was used to confirm
how the essential oil present in the cells of orange peel diffuses
outside the plant material. The result showed that after MSDf
and SDf, all observed cells reduced their volume and appeared to
have imploded, whilst maintaining the whole cuticles. Finally, in
this study, we present MSDf as a green, cleaner, environmentally
friendly, economic procedure and efficient extraction method of
essential oil from orange peel.
Acknowledgements
Authors gratefully acknowledge their physician colleague
Charles Danquigny.
References
Abert Vian, M., Fernandez, X., Visinoni, F., & Chemat, F. (2008). Microwave
hydrodiffusion and gravity, a new technique for extraction of essential oils.
Journal of Chromatography A, 1190, 14–17.
Adams, R. P. (1995). Identification of essential oil components by gas chromatography/
mass spectroscope. Carol Stream, IL: Allured Publ..
Arctander, S. (1994). Perfume and flavor chemicals. Carol Stream, IL: Allured Publ.
Bennici, A., & Tani, C. (2004). Anatomical and ultrastrucural study of the secretory
cavity development of Citrus sinensis and Citrus limon: Evaluation of
schizolysigenous ontogeny. Flora, 199, 464–475.
Berna, A., Tàrrega, A., Blasco, M., & Subirats, S. (2000). Supercritical CO2 extraction of
essential oil from orange peel; effect of the height of the bed. Journal of
Supercritical Fluids, 18, 227–237.
Bernard, J. (2001). Sciences et vie, 214, 68.
Braun, L., & Cohen, M. (2007). Herbs and natural supplements. An evidence-based
guide. Australia: Elsevier.
Chemat, F. (2009). Essential oils and aromas: Green extractions and applications.
Dehradun: HKB Publishers.
 A. Farhat et al. / Food Chemistry 125 (2011) 255–261
Chemat, F., Lucchesi, M. E., Smadja, J., Favretto, L., Colnaghi, G., & Visinoni, F. (2006).
Microwave accelerated steam distillation of essential oil from lavender: A rapid,
clean and environmentally friendly approach. Analytica Chimica Acta, 555,
157–160.
Clark, J., & Macquarrie, D. (2002). Handbook of green chemistry and technology.
Weinhiem: Blackwell Science Ltd..
Cravotto, G., Boffa, L., Mantegna, S., Perego, P., Avogadro, M., & Cintas, P. (2008).
Improved extraction of vegetable oils under high-intensity ultrasound and/or
microwaves. Ultrasonics Sonochemistry, 15, 898–902.
El Maâtaoui, M., & Pichot, C. (1999). Nuclear and cell fusion cause polyploidy in the
megagametophyte of common cypress. Cupressus sempervirens L. Planta, 208,
345–351.
Farhat, A., Ginies, C., Romdhane, M., & Chemat, F. (2009). Eco-friendly and cleaner
process for isolation of essential oil using microwave energy. Experimental and
theoretical study. Journal of Chromatography A, 1216, 5077–5085.
Ferhat, M. A., Meklati, B. Y., Visinoni, F., Abert Vian, M., & Chemat, F. (2008). Solvent
free microwave extraction of essential oils Green chemistry in the teaching
laboratory. Chimica Oggi, 26, 48–50.
Ferhat, M. A., Meklati, B. Y., & Chemat, F. (2007). Comparison of different
isolation methods of essential oil from Citrus fruits: Cold pressing,
hydrodistillation and microwave ‘dry’ distillation. Flavour and Fragrance
Journal, 22, 494–504.
Ferhat, M. A., Meklati, B. Y., Smadja, J., & Chemat, F. (2006). An improved microwave
Clevenger apparatus for distillation of essential oils from orange peel. Journal of
Chromatography A, 1112, 121–126.
Knight, T. G., Klieber, A., & Sedgley, M. (2001). The relationship between oil gland
and fruit development in Washington Navel orange (Citrus sinensis L. Osbeck).
Annals of Botany, 88, 1039–1047.
Letellier, M., & Budzinski, H. (1999). Microwave assisted extraction of organic
compounds. Analusis, 27, 259–271.
Liang, S. J., Wu, H., Lun, X., & Lu, D. W. (2006). Secretory cavity development and its
relationship with the accumulation of essential oil in fruit of Citrus medica L;
261
var. sarcodactylis (Noot.) Swingle. Journal of Integrative Plant Biology, 48(5),
573–583.
Margosan, D. A., Aung, L. H., Wergin, W. P., & Erbe, E. F. (2001). The nature of oil
gland and its associated tissues in the pericarp of Citrus limon (L.) Burn. F. by
confocal microscopy. Phyton-International Journal of Experimental Botany, Sp. Iss,
SI, 107–119.
Nelson, W. M. (2003). Green solvents for chemistry: Perspectives and practice. Oxford
University Press.
Oreopoulou, V., & Tzia, C. (2006). Utilization of plant by-products for the recovery of
proteins, dietary fibers, antioxidants and colorants. In Utilization of by-products
& treatment of waste in the food industry. Springer.
Pérez-Serradilla, J. A., Japon-Lujàn, R., & Luque de Castro, M. D. (2007). Simultaneous
microwave-assisted solid–liquid extraction of polar and non polar compounds
from alperujo. Analytica Chimica Acta, 602, 82–88.
Romdhane, M., & Gourdon, C. (2002). Investigation in solid-liquid extraction:
Influence of ultrasound. Chemical Engineering Journal, 87, 11–19.
Teo, C. C., Tan, S. N., Hong Yong, J. W., Hew, C. S., & Ong, E. S. (2008). Evaluation of
the extraction efficiency of thermally labile bioactive compounds in Gastrodia
elata Blume by pressurized hot water extraction and microwave-assisted
extraction. Journal of Chromatography A, 1182, 34–40.
Virot, M., Tomao, V., Ginies, G., Visinoni, F., & Chemat, F. (2008). Green procedure
with a green solvent for fats and oils’ determination. Microwave-integrated
Soxhlet using limonene followed by microwave Clevenger distillation. Journal of
Chromatography A, 1196, 147–152.
Yeoh, S., Shi, J., & Langrish, T. A. G. (2008). Comparisons between different
techniques for water-based extraction of pectin from orange peels. Desalination,
218, 229–237.
Zhongdong, L., Guohua, W., Yunchang, G., & Kennedy, J. F. (2006). Image study of
pectin extraction from orange skin assisted by microwave. Carbohydrate
Polymers, 64, 548–552.
Živorad, R. L. (2004). Design of experiments in chemical engineering. Weinheim:
Wiley-VCH Verlag GmbH & Co. KGaA.