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Research Note
A new process for extraction of essential oil from Citrus peels: Microwave
hydrodiffusion and gravity
Nabil Bousbia a,b, Maryline Abert Vian c, Mohamed A. Ferhat a, Brahim Y. Meklati a, Farid Chemat c,*
a
Centre de Recherche Scientique et Technique en Analyses Physico-Chimiques, CRAPC, Alger, Algeria
b
Institut National Agronomique, El Harrach, Alger, Algeria
c
UMR A 408, Scurit et Qualit des Produits dOrigine Vgtale, INRA, Universit dAvignon et des Pays de Vaucluse, 84000 Avignon, France
a r t i c l e i n f o a b s t r a c t
Article history: Attention is drawn to the development of a new and green alternative technique for the extraction of
Received 15 January 2008 essential oil from citrus peels. The process uses the hydro-diffusion phenomenon generated by micro-
Received in revised form 30 May 2008 waves to extract essential oil from the inside to the outside of the biological material and gravity to col-
Accepted 18 June 2008
lect and separate them. The present apparatus permits fast and efcient extraction, reduces waste, avoids
Available online 3 July 2008
water and solvent consumption, and allows substantial energy savings.
2008 Elsevier Ltd. All rights reserved.
Keywords:
Microwave
Extraction
Hydro-diffusion
Essential oil
Citrus
1. Introduction of attention due to the increasing energy prices and the drive to re-
duce CO2 emissions. These shortcomings have led to considering
Citrus essential oils are the most widely used essential oils in the use of new techniques in the extraction of natural substances,
the world. They are obtained as by-products of the citrus process- which typically use less solvent and energy, such as supercritical
ing. They are used as aroma avor in many food products, includ- uid extraction, ultrasound extraction, the controlled pressure
ing alcoholic and non-alcoholic beverages, candy, gelatins, In drop process, and sub-critical water extraction. Researchers in
pharmaceutical industries they are employed as avoring agents many universities are working on novel techniques that could lead
to mask unpleasant tastes of drugs. In perfumery and cosmetic, to compact, safe, efcient, energy saving, and sustainable extrac-
they are used in many preparations. The traditional way to extract tion processes (Luque de Castro et al., 1999; Pollien et al., 1998;
essential oils is by cold pressing the citrus peels. The oil is present Reverchon, 1997; Vinatoru, 2001; Jimenez-Carmona et al., 1999;
in oil sacs or oil glands located at different depths in the peel and Rezzoug et al., 2000; Ganzler et al., 1986; Lucchesi et al., 2004).
the cuticles of the fruit. Peel and cuticle oils are removed mechan- In this study, a new and original process for the extraction of nat-
ically by cold pressing and since cold pressing yields a watery ural substances using microwave hydro-diffusion and gravity
emulsion, this emulsion is then centrifuged to separate out the (MHG) was designed and developed (Fig. 1). This green extraction
essential oil. Distillation is also used in some countries as an eco- process is an original combination of microwave heating and grav-
nomical way to recover the oils. During distillation, the Citrus peels ity working at atmospheric pressure. MHG was conceived for the
exposed to boiling water or steam, release their essential oils extraction of natural substances from different plant materials at
through evaporation. As steam and essential oil vapours are the laboratory and industrial scales. In this relatively simple meth-
condensed, both are collected and separated in a vessel od, the plant material is directly placed in a microwave reactor
traditionally called the Florentine ask (Guenther, 1948; Dugo without any added solvent or water. The internal heating of the
and Di Giacomo, 2002). in situ water within the plant material distends the plant cells and
The development of new separation techniques for the chemi- leads to rupture of the glands and cell receptacles. Heating under
cal, food and pharmaceutical industries has lately received a lot microwaves thus frees molecules of interest together with in situ
water. This physical phenomenon, known as hydro-diffusion, al-
lows the extract to diffuse outside the plant material and drop by
* Corresponding author. earth gravity out of the microwave reactor through the perforated
E-mail address: farid.chemat@univ-avignon.fr (F. Chemat). Pyrex disc. A heat exchanger outside the microwave oven cools
0260-8774/$ - see front matter 2008 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jfoodeng.2008.06.034
410 N. Bousbia et al. / Journal of Food Engineering 90 (2009) 409413
2. Experimental
In this study, citrus fruits were gathered from the same exper-
imental plantation Institut Technique de lArboriculture Fruitire
(I.T.A.F.), located in the Mitidja region 40 km south of Algiers (Bou-
farik, Algeria). The citrus fruits are: Eureka (Citrus limon L.), Villa
Frana (Citrus limon L.), lime (Citrus aurantifolia (Chrism.) Swing),
Marsh Seedless (Citrus paradisi L.), Tarocco (Citrus sinensis L.),
Valencia late (Citrus sinensis L.), Washington Naval (Citrus sinensis
L.), Tengelo Seminole (Citrus paradisi Macf.). Citrus fruits were
peeled to separate the external part of the lemon (avedo), giving
a yield of 20% (w/w) of the peel with respect to the whole fruit.
Fresh plant material was employed in all extractions.
The statistical analyses were carried out using the Microsoft ondary metabolites is found in the essential oil isolated by MHG,
Exel software package (Microsoft Corp.) and XLSTAT add-on HD or CP, with relatively similar percentages. Limonene, a mono-
(addinsoft). Canonical discriminant analysis (CDA) was performed terpene hydrocarbon, is the main abundant component in the
with extraction methods (CP, HD and MHG) as dependent variable, essential oil extracted from lime with equivalent relative amounts
concentrations of a-pinene, limonene, b-myrcene, linalool, terpin- for both extraction methods: 70.9%, 71.22% and 71.86%, respec-
4-ol, citronellal, neral, a-terpineol, E-caryophellene, n-nonanal as tively for MHG, HD and CP. Geranial, an oxygenated monoterpene,
explanatory variables. is present at 1.37%, 0.85%, and 1.82%, respectively for MHG, HD and
CP. In this application, microwave irradiation highly accelerated
3. Results and discussion the extraction process, but without causing considerable changes
in the volatile oil composition, a phenomenon which was already
An appropriate microwave irradiation power is important to en- described (Pare and Belanger, 1997; Chen and Spiro, 1995).
sure the essential oil is extracted quickly. However, the power The organoleptic properties of essential oils extracted by MHG,
should not be too high otherwise loss of volatile compounds would HD and CP have been done according to sensory evaluation con-
result. Fig. 2 represents the total extraction time (it was until no ducted by twelve trained panelists who were graduate students
more essential oil was obtained) in relation with the microwave and staff members in the laboratory of the University of Avignon.
irradiation power. A microwave irradiation power of 500 W for Randomly coded samples were individually served to panelists.
500 g of plant material was chosen as an optimum and permits For MHG and CP, the extracted essential oils have the same odour
in only 15 min to extract the essential oil completely. of terpenes hydrocarbons with fresh, light, ora woody and sweet
As shown in Fig. 3, MHG is clearly quicker than conventional citrusy odour. For HD, the essential oil has an odour of terpenes
HD, an extraction time of 15 min with MHG provides yields com- hydrocarbons fresh, pungent but different from fresh fruit and with
parable to those obtained after 180 min by means of HD, which a persistent boiled odour. MHG method offers the possibility for a
is the one of the reference methods in essential oil extraction. better reproduction of natural aroma of the fruit essential oil com-
The overall yield of essential oil obtained from lime peels was parable to CP but more than the hydro-distilled essential oil. MHG
1.0 0.1% and 1.1 0.1% by MHG and HD, respectively. The yield could be a good alternative for the isolation of essential oils from
is expressed as g EO/g citrus fruit. citrus fruits.
The essential oils of lime peels extracted either by MHG, HD or This sensory evaluation has been conrmed by the statistical
CP are rather similar in their composition and contains the same analysis done on 8 varieties of citrus extracted by MHG, HD and
dominant components (Table 1). The same number of volatile sec- CP. Canonical discriminant analysis (CDA) was measured on eight
different citrus fruits considering MHG, HD and CP in order to eval-
uate the inuence of each method on the variety. As shown on
45.00 Fig. 4 and Table 1, extraction procedures are presented on factorial
axis. Canonical discriminant analysis (CDA) was performed with
40.00
extraction methods (CP, HD and MHG) as dependent variable,
Total extraction time (min)
Table 1
Chemical compositions of essential oils obtained by SFME, HD, and CP extraction from citrus peels
No. Compoundsa R.I.b R.I.c Eureka Villa Frana Lime Marsh Seedless
MHG HD CP MHG HD CP MHG HD CP MHG HD CP
Monoterpenes 92.10 92.76 93.73 89.68 88.39 93.60 88.70 92.50 95.80 97.93 97.03 97.27
1 Pinene<Alpha-> 926 1023 1.60 1.75 1.62 1.53 1.18 1.02 1.86 1.94 1.62 0.41 0.45 0.27
2 Pinene<Beta-> 974 1109 10.20 15.35 14.00 6.99 7.08 9.24 11.60 13.09 14.00
3 Myrcene<Beta-> 988 1165 1.57 1.33 1.42 1.51 1.52 1.55 1.40 1.46 1.42 1.73 1.81 1.55
4 Carene<Delta-3-> 1101 1290 0.11 0.20 0.15 0.16 0.15 0.15
5 Limonene 1030 1206 69.65 65.25 68.81 70.92 71.22 71.86 60.56 63.44 68.81 95.05 94.21 94.54
6 Terpinene<Gamma-> 1103 1285 8.25 8.08 7.04 7.70 6.58 8.90 11.91 11.17 8.90 0.01 0.03 0.01
Oxygenated Monoterpenes 3.01 3.89 2.65 3.72 3.75 3.65 5.11 4.91 3.71 0.45 0.51 0.36
7 Linalool 1125 1538 0.20 0.18 0.10 0.20 0.35 0.22 0.25 0.36 0.22 0.17 0.18 0.07
8 Citron ellal 1167 1478 0.1 0.05 0.08 0.09 0.06 0.07 0.05 0.05 0.08 0.05 0.02 0.03
9 Terpin-4-ol 1191 1590 0.08 0.42 0.03 0.09 0.37 0.02 0.08 0.19 0.03 0.02 0.09 0.02
10 Terpineol<Alpha-> 1203 1677 0.21 0.56 0.22 0.29 0.53 0.23 0.38 0.37 0.23 0.06 0.08 0.05
11 Nerol 1237 1781 0.26 0.49 0.30 0.44 0.09 0.20 0.13 0.09
12 Neral 1268 1670 0.76 0.68 0.77 0.94 0.53 1.06 1.66 1.55 1.06 0.04 0.03
13 Geraniol 1271 1828 0.24 0.60 0.32 0.56 0.07 0.12 0.07 0.07 0.02 0.02
14 Geranial 1284 1714 1.08 0.89 1.30 1.37 0.85 1.82 2.23 2.05 1.82 0.03 0.04 0.04
Sesquiterpenes 0.85 1.06 1.65 0.99 0.88 2.12 3.56 1.92 1.98 0.49 0.50 1.88
15 Elemene<Beta-> 1373 1583 0.06 0.04 0.08
16 Caryophellene<E-> 1391 1594 0.13 0.18 0.24 0.17 0.16 0.35 0.56 0.31 0.35 0.17 0.20 0.72
17 Bergamotene<Alpha-Trans-> 1437 1577 0.26 0.28 0.50 0.29 0.20 0.58 1.00 0.54 0.58
18 Humulene<Alpha-> 1450 1657 0.03 0.04 0.06 0.03 0.05 0.09 0.13 0.06 0.09 0.04 0.04 0.17
19 Farnesene<(E)-Beta-> 1453 1650 0.01 0.02 0.02 0.01 0.02 0.03 0.06 0.02 0.03
20 Germacrene D 1477 1696 0.05
21 Valencene 1488 1705 0.04 0.01 0.07 0.11
22 Bisabolene<(Z)-Alpha-> 1498 1761 0.02 0.03 0.05 0.03 0.02 0.07 0.10 0.05 0.07
23 Bisabolene(Beta-) 1508 1718 0.38 0.44 0.75 0.43 0.31 0.87 1.51 0.81 0.87
Oxygenated Sesquiterpenes 0.02 0.03 0.03 0.1 0.24 0.04 0.02 0.02 0.03 0.10 0.16 0.26
24 Elemol 1540 1381 0.01 0.01 0.04
25 Nerolidol<E-> 1555 2026 0.01 0.01 0.02
26 Bisabolol<Alpha-> 1684 2212 0.01 0.03 0.03 0.09 0.15 0.04 0.02 0.02 0.03
27 Nootkatone 1799 2250 0.07 0.13 0.15
Other oxygenated compounds 0.95 0.86 0.65 0.75 0.71 0.69 1.19 0.82 0.59 0.52 0.74 0.38
28 Nonanal<N-> 1126 1400 0.08 0.09 0.06 0.10 0.02 0.08 0.04 0.04
29 Citronellyl Acetate 1342 1645 0.02 0.03 0.04 0.02 0.02 0.04 0.04 0.02 0.04 0.01 0.01 0.05
30 Neryl Acetate 1351 1706 0.30 0.26 0.19 0.34 0.36 0.32 0.87 0.60 0.19 0.01 0.01 0.05
Extraction time (min) 15 180 60 15 180 60 15 180 60 15 180 60
Yield (%) 0.7 0.8 0.1 1.6 1.7 0.2 0.8 0.8 0.2 1.0 1.1 0.2
Toal oxygenated compunds (%) 3.98 4.78 3.33 4.57 4.70 4.38 6.32 5.75 4.33 1.07 1.41 1.00
Total non oxygenated compounds (%) 92.95 93.82 95.38 90.57 89.27 95.72 92.26 94.42 97.78 98.42 97.53 99.15
Table 1 (continued)
Tarocco Valencia late Washington Naval Tengelo Seminole
MHG HD CP MHG HD CP MHG HD CP MHG HD CP
Other oxygenated compounds 0.23 0.24 0.30 0.33 0.26 0.38 0.43 0.31 0.18 0.06 0.07 0.03
28 Nonanal<N-> 1126 1400 0.06 0.02 0.05 0.01 0.03 0.05 0.06 0.04 0.02
29 Citronellyl Acetate 1342 1645 0.01 0.01 0.01
30 Neryl Acetate 1351 1706 0.01 0.01 0.03 0.01
4. Conclusion
Observations (axes F1 et F2 : 100.00 %)
3
This is the rst time that microwave heating has been used in
combination with earth gravity to devise a fast and efcient extrac-
2
tion technique. Both the re-design of the glassware and the appli-
cation of microwaves afford a development of a method that serves
F2 (12.47 %)
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