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Extraction of Melaleuca cajuputi Using Supercritic Fluid Extraction and Solvent Extraction

  • Universiti Kebangsaan Malaysia (UKM), Malaysia

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Extracts of Melaleuca cajuputi were obtained by supercritical (carbon dioxide) extraction and solvent (hexane) extraction methods. This work is aimed at adapting the green technology of using supercritical CO2 (SC-CO2) as solvent in a batch process to extract Melaleuca cajuputi leaves. The plant leaves were collected from Trengganu, Malaysia. Cajuputi extract analyses were performed by GC and GC/MS. The maximum yields obtained were 4.2% and 6.0%, respectively, by supercritical fluid (SFE) and solvent extraction (SE). Several compounds were identified and significant qualitative and quantitative differences were observed under different conditions. The major components of Cajuputi oil consisted of sesquiterpenes (δ-elemene, β-elemene, β-caryophyllene, α-humulene, 9-epi-β-caryophyllene), their oxygenated derivatives (viridiflorol, platyphyllol, β-eudesmol, bulnesol, (Z,Z)-farnesol and (E,E)-farnesal) and polyphenolic ketones (isoeugenitine and three unknown compounds).
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M. cajuputi
Vol. 22, May/June 2010 Journal of Essential Oil Research/1
Received: January 2008
Revised: May 2008
Accepted: August 2008
Extraction of Melaleuca cajuputi Using Supercritical
Fluid Extraction and Solvent Extraction
S.M. Jajaei,* W.R.W. Daud and M. Markom,
Department of Chemical and Process Engineering, Faculty of Engineering, UKM, 43600, Bangi, Selengor Darul
Ehsan, Malaysia
Z. Zakaria,
School of Chemical Sciences & Food Technology, Faculty of Science and Technology, UKM, 43600, Bangi, Selengor Darul
Ehsan, Malaysia
M. Lo Presti, Rosaria Costa and L. Mondello,
Dipartimento Farmaco-chimico, Università di Messina, Viale Annunziata, 98168 Messina, Italy
Extracts of Melaleuca cajuputi were obtained by supercritical (carbon dioxide) extraction and solvent (hexane)
extraction methods. This work is aimed at adapting the green technology of using supercritical CO2 (SC-CO2) as solvent
in a batch process to extract Melaleuca cajuputi leaves. The plant leaves were collected from Trengganu, Malaysia.
Cajuputi extract analyses were performed by GC and GC/MS. The maximum yields obtained were 4.2% and 6.0%,
respectively, by supercritical fluid (SFE) and solvent extraction (SE). Several compounds were identified and significant
qualitative and quantitative differences were observed under different conditions. The major components of Caju-
puti oil consisted of sesquiterpenes (d-elemene, b-elemene, b-caryophyllene, a-humulene, 9-epi-b-caryophyllene),
their oxygenated derivatives (viridiflorol, platyphyllol, b-eudesmol, bulnesol, (Z,Z)-farnesol and (E,E)-farnesal) and
polyphenolic ketones (isoeugenitine and three unknown compounds).
Key Word Index
Melaleuca cajuputi, Myrtaceae, cajuput, supercritical fluid CO2 extract composition, extract composition.
1041-2905/10/0003-01$14.00/0 —© 2010 Allured Business Media
J. Essent. Oil Res., 22 (May/June 2010)
*Address for correspondence
Melaleuca cajuputi (cajuput or white tea tree) is a na-
tive Malaysian plant (Gelam, native name) that has food and
medicinal properties. It is used as a fragrance and freshening
agent in soaps, cosmetics, detergents and perfumes. Cajuput
oil, which has a camphorlike odor, is used as an insect repellent
and as a painkiller for headache, toothache, rheumatism, and
convulsions in the form of applied plaster (1).
In recent years, tea tree oil (ex Melaleuca alternifolia Cheel)
has gained widespread acceptance and it is now incorporated
as the principal antimicrobial or preservative in a range of
pharmaceuticals or cosmetics for external use, such as face
and hand washes, pimple gels, vaginal creams, foot powders,
shampoos, conditioners and veterinary skin care products.
The chemical composition of tea tree oil is well-defined (2)
and previous investigations have identified the oxygenated
terpenoids as the main active components (3,4).
The extraction of volatiles with dense carbon dioxide is an
important application of supercritical fluid technology. As an
alternative approach, supercritical fluid extraction (SFE) has
received increasing attention in the extraction from yarrow (5),
celery seed (6), Salvia officinalis L. (7), orange peel (8), rosehip
seed (9), Hyssopus officinalis L. (10) and parsley seed (11).
Supercritical fluid extraction (SFE) of the monoterpenes
from Australian tea tree (M. alternifolia) leaves was found to
be at optimum conditions with 0.25 g/mL supercritical CO2
density at a chamber temperature of 110°C (12).
Essential oils are high valued products mainly composed of
terpenelike compounds, which mainly range from 10–15 carbon
atoms and are highly soluble in dense CO2 under relatively
high pressure and low temperature conditions. Generally, they
consist of a complex mixture of mono- and sesquiterpenes, and
their oxygenated derivatives. Essential oils can also contain
diterpenes and some specific compounds, which cannot be
classified as belonging to any of the above-mentioned com-
pound families (13).
The comparison of traditional isolation methods, such
as steam or hydrodistillation, and soxhlet extraction suffers
Jajae et al.
2/Journal of Essential Oil Research Vol. 22, May/June 2010
from several limitations: soxhlet extraction usually involves
organic solvents that are flammable, toxic and environmentally
unfriendly; steam distillation frequently calls for the institu-
tion of harsh conditions where some components may be lost
through thermal degradation (14), hydrolysis or volatilization.
The resulting isolate may therefore reflect an incomplete or
altered profile of compounds compared with that of the original
material (15).
Hydrodistillation of cajuput (Melaleuca cajuputi) leaves
collected from six sites in Narathiwat (Korea) gave different
yields of cajuput oils. The maximum oil yield obtained was
0.97% (16).
Leaves and twigs of M.cajuputi from Trengganu (Malaysia)
were distilled separately to yield 0.46% (leaves) and 0.02% (twigs)
of essential oil (17). Christoph et al. (18) divided Melaleuca oil
obtained by steam distillation into three groups: monoterpenes
(monoterpenes and oxygenated monoterpenes), sesquiterpenes
(sesquiterpenes and oxygenated sesquiterpenes) and ketones.
Their study identified three ketones, namely flavesone, lep-
tospermone and isoleptospermone. Also, Sawada et al. (19)
reported the isolation of ten polysubstituted polyphenols
(PSPP), found in methanol and hexane extract of dry leaves of
Cajuput trees harvested in the southern part of Thailand. One
polyphenol, eugenitine, was determined to be an inhibitor of
cell growth in mice affected by T-lymphoma.
This work is aimed at adapting the use of supercritical CO2
(SC-CO2) as solvent in a batch process to extract the volatiles
from Melaleuca cajuputi leaves.
Plant material: Samples of M. cajuputi leaves were
harvested in Trengganu, Malaysia, in April 2005 and dried at
room temperature, under the fan and stored at -12°C. Leaves
were cut in pieces of about 5 mm in length. A voucher speci-
men of M. cajuputi (UKMB .RY-0001) was deposited in the
Herbarium of Universiti Kebangsaan Malaysia, Bangi.
Hexane extraction: Dry test material (5 g) was placed
inside a thimble made from filter paper, which was loaded
into the soxhlet extractor. The extractor was attached to a flask
containing hexane (500 mL) and a condenser, and the solvent
was heated for 8 h. At the end of each extraction, the excess
Table I. SFE and SE experimental conditions and extraction yields of Melaleuca cajuputi
Yield% (g/100 g) in
No. A = T(°C) B = P(MPa) C = Time (min.)
20 40 60 80 100 120
1 43.8 14 0.8 1.4 2 2.4 2.8 3.4
2 50 10 0.6 1 1.2 1.4 1.6 1.8
3 50 18 1 2 2.6 3.2 3.8 4.2
4 65 8.34 0.6 0.8 1 1.2 1.4 1.6
5 65 14 0.8 1.4 1.8 2.2 2.8 3.2
6 65 14 1.2 2.2 2.6 2.8 3.2 3.2
7 65 14 0.8 1.4 2 2.4 2.6 2.8
8 65 19.7 1 1.8 2.2 2.8 3.6 4
9 80 10 0.4 0.8 1 1.4 2 2.2
10 80 18 1 2 2.6 3 3.4 3.8
11 86.2 14 1.2 1.6 2 2.4 2.8 3.4
SE Hexane Extraction 6.00
Table II. Analysis of variance (ANOVA) (Response Surface Quadratic Model)
Source of Sum of Degree of Mean F* value Prob > F
variance square freedom square
Model 58.5 20 2.92 52.0 < 0.0001 *
A 4.9x10-5 1 4.9x10-5 8.73x10-4 0.98
B 18.3 1 18.3 326 < 0.0001 *
C 36.1 5 7.2 128 < 0.0001 *
A2 5.9x10-6 1 5.9x10-6 1.05x10-4 0.99
B2 1.03 1 1.03 18.4 < 0.0001 *
AB 0.06 1 0.06 1.07 0.31
AC 0.03 5 0.006 0.098 0.99
BC 2.86 5 0.57 10.2 < 0.0001 *
Residual 2.53 45 0.056
Lack of Fit 1.27 33 0.04 0.37 0.99
Pure Error 1.26 12 0.11
Cor Total 61.0 65
* The term is signicant at P ≤ 0.01.
M. cajuputi
Vol. 22, May/June 2010 Journal of Essential Oil Research/3
solvent was removed using a rotary evaporator, leaving behind
only the extract (0.3 g).
Supercritical fluid extraction (SFE): The supercritical-
fluid extraction system consisted of a CO2 tank, a pump to
pressurize the gas (Model Jasco, PU 1580, and Japan), an
oven containing the extraction vessel, a restrictor to maintain
a high pressure in the extraction line, and a trapping vessel.
In such a system, analytes are trapped by letting the solute-
containing supercritical fluid to decompress into an empty vial.
Extractions were done in combination mode with 30 min static
time and 120 min dynamic time and samples were collected
every 20 min.
The SFE equipment assembled was tested using samples
of M. cajuputi leaves harvested in Trengganu, Malaysia. Extrac-
tions were carried out in the range of 5080°C, at a pressure
of 10 MPa up to 18 MPa (according to Design-expert 6.0.10
software). Samples containing M. cajuputi leaves (5 g) were
extracted into a 50 mL extractor vessel. The extractions were
repeated at different conditions of temperatures and pressures
according to the Central Composite experimental design. The
best conditions of extraction, in terms of maximum yield per
cent, were determined by using the response surface meth-
Analytical methods: GC-FID analyses were carried out
on a Shimadzu GC-2010 gas chromatograph operated with a
split/splitless injector; a 60 m x 0.25 mm x 0.25 mm film thick-
ness DB-5MS column (J&W Scientific); temperature program:
from 50°C (2 min) to 250°C (10 min) at 3°C/min; injection
temperature: 250°C, injection volume, 1.0 mL. Split ratio: 1:50.
Samples were diluted 1:10 in hexane prior to analysis.
GC/MS analyses were performed with a Shimadzu GCMS-
QP2010 model gas chromatograph-mass spectrometer equipped
Figure 1. GC profile of Melaleuca cajuputi
Figure 2. Effect of factors A (temperature), B (pressure)
and C (time) on yield per cent (Y)
with an AOC-20i auto injector; column was an SLB-5MS (Su-
pelco), 30 m x 0.25 mm x 0.25 mm film thickness; temperature
program was: from 50°C (2 min) to 250°C (10 min.) at 3°C/
min; injection temperature: 300°C; injection volume: 1.0 mL;
inlet pressure: 37.1 kPa; carrier gas: He, at a linear velocity
u) of 32.4 cm/sec; injection mode: split, split ratio: 1:50; MS
parameters: interface and source temperatures were 220°C
and 250°C, respectively; MS mode: EI; detector voltage: 0.9
kV; mass range: 40400 u; scan speed: 769 u/s; interval: 0.50
s (2 Hz).
Experimental design and statistical analysis: The
experimental design of the supercritical fluid extraction was
carried out by a response surface methodology (RSM) using
the central composite initial design, two numerical factors of
A and B (temperature and pressure) and one categorical fac-
Jajae et al.
4/Journal of Essential Oil Research Vol. 22, May/June 2010
Table III. Percentage composition of the extracts of Melaleuca cajuputi
Compound LRI a LRI b Run1 Run2 Run3 Run4 Run5* Run8 Run9 Run10 Run11 SE S.D. C.V.
a-thujene 924 927 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.1 0.0 0.0
a-pinene 931 933 0.0 0.0 - 0.0 0.0 0.0 0.0 0.0 0.0 0.1 0.0 0.0
b-pinene 976 978 - - - - - - - - - 0.1 - -
a-phellandrene 1005 1007 - 0.0 - - - - - - - 0.1 0.0 0.1
a-terpinene 1015 1018 0.0 0.0 0.0 - 0.0 0.0 0.0 0.0 0.2 0.1 0.1
p-cymene 1023 1025 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.3 0.1 0.1
g-terpinene 1056 1058 0.1 0.1 0.0 0.1 0.3 0.0 0.0 0.0 0.0 0.4 0.2 0.1
terpinolene 1084 1086 0.0 0.0 0.0 0.0 0.5 1.1 0.0 0.2 0.0 1.5 0.5 0.3
trans-p-menth-2-en-1-ol 1143 1141 - - - - - - - - - 0.3 - -
terpinen-4-ol 1179 1180 0.3 0.1 0.8 0.0 0.1 0.8 0.1 0.4 0.0 2.8 0.8 0.5
a-terpineol 1194 1195 0.2 0.0 0.6 0.1 0.2 0.3 0.1 0.6 0.1 3.3 1 0.0
trans-piperitol 1208 1209 - - - - - - - - - 0.1 - -
acetate 1222 1231 - - - - - - - - - 0.1 - -
ascaridole 1238 1234 - - - - - - - - - 0.1 - -
carvacrol 1298 1298 0.0 0.0 0.0 0.0 0.0 0.0 - 0.0 0.0 0.2 0.1 0.0
d-elemene 1331 1335 2.0 2 2.8 2 1.0 2.3 2.2 1.7 2.7 1.8 0.5 0.3
eugenol 1351 1357 0.4 1.2 0.9 0.4 0.7 1.1 0.1 0.9 0.4 1.2 0.4 0.2
cyclosativene 1368 1367 0.4 0.2 1 1.7 0.5 1.2 0.3 0.8 0.9 1.3 0.5 0.3
a-copaene 1375 1375 0.3 0.3 0.5 0.3 0.3 0.3 0.3 0.4 0.3 0.6 0.1 0.1
b-elemene 1389 1390 9.7 7.0 7.1 3.9 4.5 5.3 8.4 6.5 4.3 8 1.9 1.2
methyl eugenol 1398 1403 0.2 1.3 0.9 0.4 0.2 0.5 0.2 1.5 0.8 0.9 0.5 0.3
a-gurjunene 1407 1409 0.2 0.4 0.7 0.4 0.3 0.2 0.2 1 0.6 0.5 0.3 0.2
b-caryophyllene 1421 1424 17.2 14.7 16.7 26.3 15.9 16.7 13.5 15.3 17.3 10.0 4.1 2.6
b-gurjunene 1430 1431 0.3 0.3 0.3 0.4 0.2 0.2 0.3 0.5 0.3 0.3 0.1 0.1
aromadendrene 1439 1439 0.1 0.3 0.5 1.1 1.8 0.7 0.2 0.6 0.4 0.4 0.5 0.3
a-humulene 1456 1454 5 4.5 5.7 4.7 6.1 7.3 4.1 4.4 7.1 6.4 1.2 0.7
9-epi-(b)-caryophyllene 1460 1464 3.8 1.5 3.1 3.1 2.0 3.2 3.7 3.5 3.5 3.9 0.8 0.5
selina-4,11-diene 1474 1476 0.1 0.8 1.0 0.4 0.2 0.2 2.1 0.4 0.9 0.3 0.6 0.4
g-muurolene 1481 1478 0.8 1.1 3.8 3.8 3.7 2.8 3.6 1.9 2.4 2.8 1.1 0.7
b-selinene 1489 1492 0.1 0.4 0.7 0.4 1.0 0.2 0.1 0.8 1 0.7 0.3 0.2
a-selinene 1496 1501 0.1 1.5 0.4 1.1 0.4 0.4 0.3 0.8 0.4 0.4 0.4 0.3
germacrene D 1483 1479 1.4 0.5 0.7 0.4 0.7 0.8 0.1 0.5 0.6 0.6 0.3 0.2
eremophilene 1491 1491 0.1 0.9 1 1.4 0.6 0.3 0.1 0.8 0.5 0.5 0.4 0.3
bicyclogermacrene 1496 1497 0.1 0.6 0.6 0.3 1.6 0.9 0.2 0.6 0.6 0.9 0.4 0.3
g-amorphene 1492 1490 0.2 0.9 0.6 0.9 0.2 0.3 1 0.6 0.6 0.3 0.3 0.2
a-bulnesene 1507 1505 0.1 0.7 0.3 0.6 0.8 0.7 0.3 0.5 0.6 0.4 0.2 0.2
g-cadinene 1513 1512 0.1 3.2 0.3 1.0 0.6 0.6 0.6 0.7 0.6 0.5 0.9 0.5
d-cadinene 1519 1518 0.1 0.4 0.3 1.1 3.4 0.6 0.7 0.6 1.8 0.4 1 0.6
zonarene 1523 1528 0.2 0.3 0.4 0.5 1.8 2 0.6 0.4 0.3 0.4 0.7 0.4
a-cadinene 1537 1538 0.8 0.4 0.5 2.2 3.5 1.4 0.7 0.4 1.2 0.6 1.0 0.6
a-elemol 1551 1546 0.8 0.2 0.7 0.6 0.2 0.3 0.4 0.5 0.5 0.4 0.2 0.1
germacrene B 1562 1557 1.1 1.1 0.9 0.3 0.4 1.0 0.4 1.0 0.8 0.3 0.3 0.2
ledol 1571 1574 0.2 0.8 0.5 0.7 0.2 0.4 0.4 0.9 1.3 0.4 0.3 0.2
spathulenol 1578 1576 0.6 0.8 0.3 1 0.4 0.6 1.4 0.6 0.5 0.5 0.3 0.2
guaiol 1599 1603 0.6 1.3 0.6 1.6 1.4 0.9 0.3 1.1 0.3 0.6 0.5 0.3
caryophyllene oxide 1583 1587 0.1 3.4 0.3 0.6 0.7 0.3 0.2 0.6 0.7 1.9 1.0 0.6
globulol 1587 1587 0.1 0.3 0.9 0.4 0.2 0.3 0.1 0.5 0.3 0.5 0.2 0.2
viridiorol 1595 1594 3.6 0.4 0.6 1.0 0.2 0.6 3.2 1 1.1 0.6 1.2 0.7
platyphyllol 1604 1607 12.1 16.4 7.2 11.1 8.3 6.2 8.3 6.2 6.3 13.1 3.5 2.2
humulene epoxide 1611 1613 0.3 0.7 0.4 1.3 0.9 0.6 0.4 0.7 0.5 0.3 0.3 0.2
epi-cubenol 1630 1631 0.9 0.6 1.3 0.3 0.6 0.3 0.7 0.3 1.8 0.3 0.5 0.3
g-eudesmol 1636 1632 0.5 4.6 0.7 0.6 0.2 1.4 0.5 0.3 0.7 0.5 1.3 0.8
epi-a-muurolol 1645 1640 0.2 2.4 3.1 0.2 1.4 0.4 0.5 0.9 2.9 0.3 1.2 0.7
a-muurolol 1648 1651 0.3 0.3 0.3 0.3 0.4 3.0 1.1 0.5 0.5 0.6 0.8 0.5
cadin-4-en-1-ol 1657 1659 1.2 0.5 0.5 0.8 1.6 0.4 0.2 0.8 0.7 0.3 0.4 0.3
b-eudesmol 1659 1656 2.0 0.8 0.5 0.3 0.4 0.3 0.3 0.8 1 0.8 0.5 0.3
a-11-selinen-4-ol 1660 1658 0.6 1.4 0.8 3.9 0.4 3.8 2.3 1.3 1.7 1.1 1.3 0.8
neointermedeol 1661 1658 0.8 2.2 2.5 0.8 2.5 0.8 1.6 1.5 0.9 0.7 0.7 0.5
phloroacetophenone 1666 1667 3.5 0.7 0.7 0.6 2.7 1.5 3.5 3.5 2.1 1.1 1.2 0.8
bulnesol 1669 1673 12.6 5.5 11.5 9.3 12.4 8.7 19.3 11.1 11.9 4.3 4.2 2.6
nerolidol 1701 1706 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.3 0.0 0.2 0.2 0.2
M. cajuputi
Vol. 22, May/June 2010 Journal of Essential Oil Research/5
(Z,Z)-farnesol 1714 1716 6.7 4.1 4.7 2.0 1.8 2.6 5.4 2.5 3 3.9 1.6 1
(E,E)-farnesal 1736 1737 3.0 2.4 2.5 0.4 2 0.3 3 2.6 3.0 1.3 1.1 0.7
bancroftinone 1745 1737 0.1 0.3 0.3 0.3 0.2 1.8 0.4 0.8 0.4 0.3 0.5 0.3
cryptomeridiol 1822 1813 0.1 0.3 0.4 1.0 0.2 0.3 0.2 0.7 1.1 0.7 0.4 0.2
isoeugenitine 1972 1963 0.1 0.2 0.0 0.1 0.4 1.5 0.4 0.6 1.3 1.6 0.6 0.4
unknown (A) 1982 0.1 0.0 0.0 0.1 1.5 2 0.1 1.7 0.5 3.1 1.1 0.7
unknown (B) 1993 0.1 0.0 0.0 0.0 0.5 2.6 0.0 2.6 0.5 1.7 1.1 0.7
unknown (C) 2011 0.1 0.0 2.2 0.3 1.6 2.6 0.1 6.2 0.5 1.3 1.9 1.2
LRI a: linear retention index, calculated using a C7-C40 n-alkanes mixture; LRI; b: linear retention index reported in Adams library (ref. 20); * Run5 is average of Run5, Run6,
Run7; MS spectrum data of the unknown component (A): 220(100), 191(45), 252(40), 202(35), 165(25),235(20); MS spectrum data of the unknown component (B): 220(100),
191(40), 202(25), 161(12), 55(12),43(10), 137(8), 121(8); MS spectrum data of the unknown component (C): 234(100), 220(98), 216(25), 189(14), 151(10), 71(10), 77(10), 55(10),
(43(10), 161(8), 95(8), 136(5), 117(4); correct isomer not identied.
tor of C (time) that was obtained from Design-Expert 6.0.10
software. After entering responses data in the design layout
view, a response was chosen by the corresponding node under
analysis. This was followed by variable transformation, model
choice (RSM/Mix) and analysis of variance (ANOVA).
Results and Discussion
The solvent extraction process has been traditionally used
in the extraction of plant material at a laboratory scale. This
research intended to compare the efficiency of this process
with SFE in relation to the volatile composition of the extracts
from M. cajuputi.
The selected factors of extraction and their correspond-
ing ranges are shown in Table I. The experimental domain of
the 3-factor consisted of 11 runs. Eleven experiments were
performed and the measured responses were defined as the
% (w/w) of extracted oil. Optimization of the method can be
carried out step-by-step or by using an experimental design.
Table I shows different conditions of SFE experiments for
extractions of M. cajuputi according to the RSM experimen-
tal design. The results of the SFE experiments based on the
extraction yields are given, once again, in Table I.
The maximum extract yield obtained was 4.2% at optimum
conditions (50°C and 18 MPa). The volatile compositions of M.
cajuputi obtained through GC analyses have been studied as
well. Identification of the substances was made by comparison
of analytes mass spectra with those recorded in two GC/MS
databases (20,21) and retention indices with literature records.
A total of 88 different compounds were identified and signifi-
cant qualitative and quantitative differences were observed
depending upon different analytical conditions. Rahimah
(17) obtained 0.46% (10 times less than SFE) the oil from M.
cajuputi leaves using a hydrodistillation method. She isolated
the same main components except for polyphenolic contents
and the last four peaks.
Since various parameters potentially affect the extraction
process, optimization of the experimental conditions represents
a critical step in the development of a SFE method. In fact,
pressure and temperature of the fluid and extraction times
have been generally considered as the most important factors
(Figure 2).
Table III. Continued
Compound LRI a LRI b Run1 Run2 Run3 Run4 Run5* Run8 Run9 Run10 Run11 SE S.D. C.V.
Table II shows analysis of variance (ANOVA) results for the
calculated models. It is worthy to note that the obtained data
are valid only for the studied sample. The ANOVA results of this
experiment indicated that the pressure and time of SFE play
an important role in the SFE of M. cajuputi and appear to be
significant for all the analytes. The pressure increase causes an
increase of the fluid density and thus it could have an important
effect on the yield. The solvating power of the supercritical
fluid responsible for quantitative recoveries and the increase
of time causes an increase of solvent contact with sample. The
effects of temperature in the studied range on the extraction
efficiency were not significant (Table II and Figure 2).
Detailed identification and quantification of the com-
pounds found in M. cajuputi extracts, produced by SE and
SFE under different conditions, were performed by GC/MS,
as reported in Figure 1. In addition, the results are shown in
Table III, for comparison. The major components of Cajuput
leaf extract consisted of sesquiterpenes (d-elemene, b-elemene,
b-caryophyllene, a-humulene, 9-epi-b-caryophyllene), their
oxygenated derivatives (viridiflorol, platyphyllol, b-eudesmol,
bulnesol, (Z,Z)-farnesol and (E,E)-farnesal) and polyphenolic
ketones (isoeugenitine and three unknown compounds).
However, the recovery selectivity of components in SFE
was better than in solvent extraction. Besides giving a better
selectivity for compounds of interest, the use of SFE was less
tedious as concerns changing extraction variables and it required
a shorter extraction times.
Table III indicates that the number of components ex-
tracted by SFE (67 components) is lower than those obtained
by hexane extraction (88 components). Therefore, the SFE
procedure is more selective than SE.
In conclusion the supercritical fluid extraction of M. cajuputi
for the yield optimization was studied. Monoterpenes, sesqui-
terpenes and polyphenolic ketones were extracted. The global
extraction yield ranged between 1.6% and 4.2 wt. % depending
on extraction conditions, which are listed in Table I. The ef-
fect of the process parameters was studied in the supercritical
fluid extraction of M. cajuputi. SFE showed different results
in comparison with the SE procedure. In addition, SFE gave
a better selectivity for compounds of interest and it required
a shorter extraction time. The flexibility in the management of
the variables involved in the SFE process allowed optimizing
Jajae et al.
6/Journal of Essential Oil Research Vol. 22, May/June 2010
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... There are several studies that are being conducted to extract oil from Melaleuca cajuputi which are maceration [9], hydrodistillation [12], soxhlet extraction as well as SC-CO 2 extraction [13]. SC-CO 2 extraction employs supercritical CO 2 to extract the active compounds from the plant matrix [14]. ...
... The chemical constituents of the Melaleuca cajuputi extract was analyzed using GC-MS and is shown in Table 3. The chemical compounds present at optimized condition of SC-CO 2 extraction of Melaleuca cajuputi are compared with 4 conditions which are SC-CO 2 extraction at optimized condition but with the addition use of ethyl acetate as co-solvent, Soxhlet extraction of Melaleuca cajuputi using hexane as well as compared with literature by Jajaei et al. [13] and Kim et al. [12]. It is found that the chemical compounds that are present in both the experimental runs and Jajaei et al. [13] are β-caryophyllene, humulene, germacrene D, β-Selinene, humulene epoxide II, spathulenol and neointermedeol which verify the identification of Melaleuca species. ...
... The chemical compounds present at optimized condition of SC-CO 2 extraction of Melaleuca cajuputi are compared with 4 conditions which are SC-CO 2 extraction at optimized condition but with the addition use of ethyl acetate as co-solvent, Soxhlet extraction of Melaleuca cajuputi using hexane as well as compared with literature by Jajaei et al. [13] and Kim et al. [12]. It is found that the chemical compounds that are present in both the experimental runs and Jajaei et al. [13] are β-caryophyllene, humulene, germacrene D, β-Selinene, humulene epoxide II, spathulenol and neointermedeol which verify the identification of Melaleuca species. From the results by Jajaei et al. [13] on SC-CO 2 extraction of Melaleuca cajuputi leaves, − β caryophyllene is also detected as one of the major compounds. ...
Due to the rice production problem, control of paddy weeds with the use of allelopathy as active compounds serve as new alternative for sustainable weeds management. The volatile oil from Melaleuca cajuputi which has possible active allelopathy compound present is extracted and analyzed. Response Surface Methodology (RSM) with central composite rotatable design (CCRD) is used to design the experiment for optimization of supercritical carbon dioxide (SC-CO2) extraction of volatile oil from Melaleuca cajuputi leaves for maximum oil yield. Three factors which included carbon dioxide (CO2) flow rate (4–7 ml/min), temperature (40–55 ℃) and pressure (14–26 MPa) were investigated. The regression model shows a good prediction with coefficient of determination, R² of 0.9607. The optimum condition of SC-CO2 extraction is determined to be at CO2 flow rate of 5.88 ml/min, temperature of 43.10℃ and pressure of 24.91 MPa with the prediction yield of 1.24 wt%. The optimum condition is validated with experimental runs which gives an average yield of 1.26 wt% which indicates good agreement between the measured and predicted value. The chemical composition of the volatile oil at optimized condition is analyzed using Gas Chromatography Mass Spectrometry (GC–MS) and Gas Chromatography with Flame Ionization Detector (GC-FID). Caryophyllene and humulene are the two major sesquiterpenes detected from the optimized condition. Thus, volatile oil extract from the foliage of Melaleuca cajuputi can be considered as potential source for bio-herbicides due to the presence of caryophyllene which has allelopathic effect. Kinetics studies are also studied with modified Reverchon-Sesti Osseo as the model fitting.
... Also, with the same method, the leaf from Cuba yielded oil as much as 0.9% (Pino et al., 2002). The higher results were obtained by applying CO 2 extraction and soxhlet hexane extraction with the value of 4.2% and 6.0%, respectively (Jajaei et al., 2010). The use of microwave in extraction was also investigated. ...
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The essential oil from Melaleuca leucadendra L. leaves has been widely used as a perfume and traditional remedy, cosmetics and pharmaceutical products ingredient since many years ago. The common technology to recover the oil is hydro-distillation and steam-distillation. However, all oil can not be fully extracted from the leaves by this method due to the recalcitrant structure of leaves that hindrance the access of the solvent. Adding a submerged fermentation as a pre-treatment step prior to the extraction process helped to loosen the lignocellulose structure and enhance oil release in the extraction process. In this study, the raw materials were collected from the natural forest in Buru Island, Maluku, Indonesia. The biological agents applied in these processes were Phanerochaete chrysosporium ITBCC136 and Trichoderma viride ITBCC143. The oil extraction process was conducted by method of steam-distillation, the oil was analysed using gas chromatography-mass spectroscopy (GC-MS), and the lignocellulose content in the biomass was measured by the fractionation method. The treatment using T.viride provided the highest increase in yield percentage up to 3.47% as compared with control of 1.45%, with the lowest percentages of the remained cellulose, while the fermentation with the presence of P.chrysosporium did not affect the oil yield even the lignin content was decrease as much as 21%. The percentages of 1,8-cineole in the oil were almost unchanged, which was about 20% of the oil.
... To be specific, essential oil extraction from leaves and twigs of M. cajuputi resulted in yield of 0.46% (leaves) and 0.02% (tree branches) respectively. Jajaei et al. [16] conducted the extraction of essential oil from Melaleuca cajuputi (Trengganu, Malaysia) by the supercritical extraction method (carbon dioxide) and solvent extraction method (hexane). The maximum yield for the two method was 4.2 and 6.0% respectively. ...
The essential oil of Melaleuca cajuputi was obtained by hydrodistillation method. This work aims to adopt water as a solvent in a batch process to extract essential oil from Melaleuca cajuputi fresh leaves. The leaves are collected from Quang Tri Province, Vietnam. Analysis of constituents was performed by GC/MS. The maximum yield ranged from 0.6 to 0.7%. Several compounds have been identified in high quantities and meaningful qualitative and quantitative differences have been observed under different conditions. The main components of the M. cajuputi essential oil included eucalyptol (27.512%), γ-terpinene (8.59%), terpinolene (9.047%), β-eudesmene (3.359%), α- selinene (3.889%), α-terpineol (4.108%), 1R-α-pinene (2.158%), caryophyllene (6.48%) and α-caryophyllene (3.522%). This study has confirmed that the essential oil of M. cajuputi essential oil is a promising bactericidal agent on several Gram-positive and Gram-negative bacteria.
... M. cajuputi tree can be found abundantly along east coast area of Peninsular Malaysia especially Kelantan in swampy land [12]. There have been numerous reports on the essential oil distillation [13][14][15][16] and evaluation of the essential oil as insecticides such as termicide [14], mosquitocide [17,18] and against Tribolium castaneum and Sitophilus zeamais [19]. Studies proved that the leaves of M. cajuputi retain antibacterial [20][21][22], anti-inflammatory and anaesthetic properties and have the potential to repel and kill insects [23]. ...
Treatment of old historical wooden houses with synthetic preservative lined with chemical pesticide were known to cause hazards to human and the environment. Gelam tree crude extract was investigated in this study to explore its potential to repel wood damaging carpenter ants in order to reduce the use of hazardous pesticides and attack on the timber by wood boring insects. The crude extract from Gelam tree stem (Melaleuca cajuputi) was extracted by sequential extraction using hexane, dichloromethane and methanol. The repellent activity was tested at 20% w/v concentration using World Health Organization (WHO) recommended method on ant repellent testing for 3 hrs with 15 min’s interval. All the extracts showed significant repellent activity on the tested Camponotus sp. ants. The toxicity activity on Camponotus sp. was determined by using 10% w/v concentration of crude extract mixed with honey. Toxicity activity of methanol extract (84.3%) showed the high toxicity percentage against Camponotus sp. The LT50 recorded for Camponotus sp. tested with hexane, dichloromethane and methanol crude extract were 19.11 hrs, 11.89 hrs and 9.43 hrs respectively. This study indicated that M. cajuputi stem has potential to be further studied and developed as natural insecticide against carpenter ants for the application on wooden buildings.
... This oil is a complex mixture of volatile components extracted from the leaves and twigs through water-steam distillation. MCO can be divided into two main groups which are monoterpenes (monoterpenes hydrocarbon and oxygenated monoterpenes) and sesquiterpenes (sesquiterpenes hydrocarbon and oxygenated sesquiterpenes) [29]. As previously reported, the major constituent of MCO is 1,8-cineole comprising 30% to 70% of the oil [25,30]. ...
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To reduce the economic impact caused by the fossil fuel crisis and avoid relying on existing biofuels, it is important to seek locally available and renewable biofuel throughout the year. In the present work, a new light biofuel—Melaleuca Cajuputi oil (MCO)—was introduced to blend with refined palm oil (RPO). The physicochemical properties, combustion characteristics, engine performance, and exhaust emissions were comprehensively examined. It was found that the higher the percentage of MCO, the lower the viscosity and density of the blends obtained. Calorific value (CV) was increased with the increase of MCO fraction in the blend. Regression analysis has suggested that the blend of 32% (v/v) of RPO and 68% (v/v) of MCO (RPO32MCO68) is optimal to obtain viscosity and density in accordance with ASTM 6751/EN 14214 standards. The experimental results show that the in-cylinder pressure, brake torque, and brake power of the optimal blend were slightly lower than those of baseline diesel fuel. Brake specific fuel consumption (BSFC), carbon monoxide (CO), and unburnt hydrocarbon (HC) were found to be slightly higher compared to diesel fuel. Notably, nitrogen oxides (NOx) and smoke opacity were found to be decreased over the entire range of the test. Overall, the optimal blend of RPO32MCO68 has shown a decent result which marks it as a potential viable source of biofuel.
Shrimp consumption has increased steadily around the world, as has the emergence of bacterial pathogens, which cause massive economic losses. The incorporation of plant extracts in aquatic animal feeds has been suggested to improve growth performance and resistance against bacterial pathogens. Therefore, the aim of this study was to evaluate the effects of Cajeput Melaleuca cajuputi leaf extract (MCLE) on the growth performance, physiological responses and resistance of Giant freshwater prawn Macrobrachium rosenbergii against Aeromonas hydrophila. The phytochemical composition of the MCLE was analysed using gas chromatography–mass spectrometry (GC‐MS). Thereafter, the MCLE was included in diets (0.0, 5.0, 10.0 and 15.0 g/kg) fed to the M. rosenbergii. The growth was observed after 45 days of the feeding trial, whereas physiological responses and clearance efficiency (%) against A. hydrophila were observed on the 60th day. 2‐Isopropyl‐10‐methylphenanthrene, phenanthrene, 1‐methyl‐7‐(1‐methyl ethyl) and 4H‐1‐Benzopyran‐4‐one, 3‐acetyl‐5, 7‐dihydroxy‐2‐methyl‐ compounds were detected as the major compounds in the MCLE. A significant improvement (p < 0.05) of growth and survival of M. rosenbergii fed with MCLE supplementation at 15.0 g/kg was observed. The total haemocyte count, hyaline cells and granular cells were also increased (p < 0.05) in the M. rosenbergii fed with diets included with MCLE. Upon challenging the primed M. rosenbergii with sub‐lethal doses of A. hydrophila, the highest clearance efficiency (73%) was achieved in the prawn‐fed 15.0 g/kg MCLE based diet (p < 0.05) after 96 h post injection. These findings indicate the potential of MCLE supplementation to improve growth, immune responses of M. rosenbergii and their resistance against A. hydrophila.
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The history of aroma and fragrance dates back through several ages and civilizations. The sagacity of smell plays a remarkable role for human being to recognize right food. Best fruits can be judged when they are ripe and fit for consumption emitting lovely smell or aroma. The same attribute from flowers attract insects leading to cross-pollination. India has enjoyed a paramount place in the fabrication of quality perfumes and aromatics since prehistoric era. The celebrated Chinese voyager Fa-Hien described India as the land of aromatic plants. Visitors, at Nawabi banquets, were welcomed essentially with attar. Indian cities like Delhi, Agra, Kannauj, Lucknow, Jaunpur, Ghazipur, Aligarh, Bharatpur, Mysore, and Hyderabad, emerged as centers of the national and international trade in perfumery and other aromatic compounds, and were known for their quality across Asia, Europe and Africa. Aromatic plants precisely possess odorous volatile substances in root, wood, bark, stem, foliage, flower and fruit. The typical aroma is due to an assortment of composite chemical compounds. At present, information on the chemistry and properties of essential oils of only about 500 aromatic plants species is known in some detail out of a total of about 1500. Of these, about 50 species find use as commercial source of essential oils and aroma chemicals. It is realized now that perfumes are not the essentials of sumptuousness as they were in the past. It has given birth to new streams of medicinal therapy, aromatherapy, involving the use of essential oils and aromatics derived from plants to treat diseases. Essential oils are also reported to be better than antibiotics due to their safety and broad spectrum activity. Natural essential oils are also potentially safe insecticides. The essential oil obtained from Acorus calamus having ß-asarone as an active principle, produces sterility among a variety of insects of either sex. It has, therefore, been found very useful and secure for the storage of food grains. However, there is still very inadequate research for the cultivation of aromatic crops and extraction of essential oils across the globe. This book has been designed to highlight the associated issues of aromatic plants including the aspects of their classification, importance, uses and applications for human wellbeing, botany, agrotechniques, major bioactive constituents, post harvest extraction, chemistry and biochemistry of aroma compounds alongwith an informative modern global research on these plants throughout the world. Hope this book will cater the scholastic services and rewards to diverse professionals and stakeholders and serve as an informative handbook for theoretical as well as practical purposes.
The leaf essential oils from Eugenia luschnathiana Klotzsch ex B.D. Jacks. and Myrciaria tenella (DC.) O. Berg growing in two different locations in southeastern Brazil were obtained by hydrodistillation and analyzed by GC and GC-MS. The oil profiles of individual accesses of E. luschnathiana from each location were characterized by the virtual absence of monoterpenes. The sesquiterpenes were of the caryophyllane (32%), guaiane (27%) and cadinane (19%) types in the São Paulo State access and caryophyllane (43%) and cadinane (28%) types in the Rio de Janeiro access. This is the first report on the composition of E. luschnathiana oil. Monoterpenes were predominant in both accesses of M. tenella (57-65%), and sesquiterpenes were mostly represented by the guaiane-eudesmane (16%) or caryophyllene-guaiane types (17%), respectively, in the São Paulo and Rio de Janeiro accesses. In monoterpene composition, the M. tenella oils qualitatively and quantitatively resembled that from a previous access from southern Brazil, whereas the sesquiterpene accumulation showed no similarity to any previous collection in Brazil regarding any favored skeleton type.
Along more than a decade, R&D on supercritical fluid extraction (SFE) of vegetable matrices has been increasingly reported in the literature. Aiming at portraying the current state of this field and its evolution in terms of raw materials, products, modes of operation, optimization, modeling techniques, and closeness to industrial application, a large compilation of almost 600 essays from 2000 to 2013 has been deeply analyzed in order to unveil those indicators and their trends. Furthermore, strengths and weaknesses are identified, and some remarks that may drive upcoming research are provided. Globally, more than 300 species are reported in the literature, with prevalence of the extraction of seeds (28% of works) and leaves (17%). The main families of extracted compounds, cosolvents and operating conditions adopted are critically examined, being possible to conclude that researchers investigate many times working regions far from the optimum due to practical limitations or absence of experimental optimization. Current phenomenological, statistical and semi-empirical approaches are reviewed, along with scale-up studies, and economic analysis. In the whole, the most comprehensive picture over SFE of vegetable matrices is provided in this review, highlighting pertinent aspects and opportunities that may further consolidate the convincing route of this technology for the next years.
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Detailed GC and GC-MS analyses of oil of Melaleuca have identified several constituents not previously reported from Melaleuca alternifolia and clarified some earlier assignments. The range, mean, and coefficient of variation for the principle constituents in 800 typical samples are presented along with the compositions of several substandard oils. Isolation and storage procedures affecting the chemical composition of the oil are reported. Ethanolic extraction of mature leaves gave solutions suitable for direct injection into a gas chromatograph for the qualitative determination of tea tree oil. Comparison with conventional steam distillation showed that this technique was suitable for preliminary analysis of tea tree oil yield and quality.
Hydrodistillation of cajuput (Melaleuca cajuputi) leaves collected from 6 sites in Narathiwat gave different yields of cajuput oils. The maximum oil yield (0.97%) was obtained from leaves from Ban Koke Kuwae, Thambon Kosit, and Amphur Tak Bai. The oil yields from leaf samples of other sites were 0.84% from Ban Pha Ye and Thambon Sungai Padi in Amphur Sungai Padi; 0.76% from Ban Lubosama, and Thambon Pasemat, in Amphur Sungai Kolok; 0.70% from Ban Tha Se, and Thambon Kosit, in Amphur Tak Bai; 0.66% from Ban Mai, and Thambon Sungai Padi, in Amphur Sungai Padi; and 0.56% from Ban Toh Daeng, and Thambon Phuyoh, in Amphur Sungai Kolok. Cajuput oil densities from the 2 sites of Amphur Sungai Kolok and from Ban Mai, Thambon Sungai Padi, Amphur Sungai Padi were almost the same, but higher than others. Although major components were not different, the minor components varied in terms of both structure and proportion. The major compositions of both cajuput oils from Ban Toh Daeng, Thambon Phuyoh, and Amphur Sungai Kolok consisted of 49.22% monoterpenes and 46.45% sesquiterpenes, and the rest were hydrocarbons and a diterpene. Other cajuput oils obtained composed mainly of monoterpenes (more than 62%), sesquiterpenes, hydrocarbons and some unknown compounds respectively. There was no diterpene present in these oils. Since cajuput oil was locally used as insecticide, termicidal activities of all oils were also investigated.
Supercritical CO2 extraction of essential oil from lavender was performed on a laboratory apparatus as well as in a pilot plant. A two-stage separation procedure was used to induce the fractional separation of the extracts. Detailed CC-MS analysis of the products was performed to assess the best extraction and the best separation conditions. The lavender oil produced by supercritical extraction was compared to the oil obtained by hydrodistillation. The major difference between the two products was reflected in the linalyl acetate content. This compound was found to be 34.7% of the oil produced by supercritical fluid extraction and 12.1% of the hydrodistilled product. This difference can be ascribed to the hydrolysis of part of this compound during hydrodistillation. The oil yield of the extraction process was measured at various extraction lengths. It was modeled using a simple mathematical model.
The essential oil of chamomile flowerheads was extracted by supercritical CO2, producing the fractional separation of the extract to enhance the process selectivity. The extract fractions were analyzed by GC-MS and SFC to assess the presence of undesirable compounds and to obtain the detailed oil composition. The best oil was obtained by extracting at p = 90 bar and T = 40 degrees C and fractionating the product in two separators in series operating at p = 90 bar, T = 0 degrees C, and p = 30 bar, T = -5 degrees C, respectively. All undesired compounds were precipitated in the first separator. The oil did not suffer thermal degradation: matricine was not converted to chamazulene. The other chamomile oil characteristic compounds (bisabolol oxides, alpha-bisabolol, and bisabolone oxide) contributed more than 75% and dicycloethers contributed about 13% to the oil composition. Organoleptic analysis confirmed the high quality of the product.
Hyssopus officinalis L. (hyssop) as a food ingredient has its own importance in flavor industry and also in sauce formulations. Supercritical fluid extraction (SFE) of hyssop, cultivated in Iran, was performed at various pressures, temperatures, extraction (dynamic and static) times and modifier (methanol) concentrations using an orthogonal array design with an OA25(55) matrix conditions. Pressure, temperature and modifier in the SFE system influenced the extraction yield. Also, the composition of the extracted oils was greatly impacted by the operating conditions. Main components of the extracts under different SFE conditions were sabinene (4.2–17.1%, w/w), iso-pinocamphene (0.9–16.5%) and pinocamphene (0.7–13.6%). The extraction of sabinene, for example, was favored at 100 atm, 55 °C, 1.5% (v/v) methanol, 30 min dynamic time and 35 min static time. Use of SFE under different conditions can allow targeting the extraction of different constituents.
The supercritical fluid extraction (SFE) of orange essential oil was studied using dehydrated orange peel (0.0538 kg H2O/kg dm) from naveline cultivars as raw material and CO2 as solvent. The effect of operation conditions was analyzed in a series of experiments at temperatures between 293 and 323 K and pressures between 8 and 28 MPa. The collected extracts were analyzed and the relative composition of the essential oil was determined. Limonene was the principal component extracted, the optimum conditions for limonene extraction were 12.5 MPa and 308 K, in these conditions limonene represents more than 99.5% of the essential oil. Within the operating range conditions, the optimum for extracting linalool was found at 80 bar and 35°C, conditions which coincide, in quite an approximate way, with those in the bibliography (F. Temelli et al., Food Technol. 42 (1988) 1451). Furthermore, the effect of CO2 flow rate and particle size of orange peel was studied in the range of 0.5 to 3.5 kg h−1 and 0.1 to 10 mm, respectively. For a rapid extraction, particle sizes lower than 2 mm are adequate. For particle size of 0.3 mm and any CO2 mass flow, approximately 75% of the total content of essential oil was extracted using a solvent ratio of 6 kg of CO2 per kg of orange peel. A model based on the assumption of plug flow of a solvent through a fixed bed of milled material was applied to analyze the experimental results. The model successfully fitted the kinetic extraction of the essential oil.
Dry sage leaves were extracted with dense carbon dioxide under the following conditions: pressure, 9–12.8 MPa; temperature, 25–50 °C; sage feed, 3–4 g; carbon dioxide flow rate, 0.05–0.35 g/min; solvent-to-feed ratio, 16–21. The oil in finely ground particles was easily accessible to the solvent and its extraction was controlled by phase equilibrium. A part of essential oil dissolved in CO2 almost immediately, the other part was extracted gradually together with cuticular waxes and water. The difference in extraction rate was connected with essential oil fractionation due to the different solubility of oil components and solute–matrix interaction in the second extraction period. Collection efficiency of a cooled glass U-tube at ambient pressure was low for volatile substances but good for sesqui- and diterpenes. The extraction yield of oxygenated monoterpene manool was more than double its yield obtained by hydrodistillation.
Parsley seed oil extraction with supercritical carbon dioxide at pressures of 10 and 15 MPa, temperatures of 308 and 318 K, flow rates of 0.7, 1.1 and 2 kg/h and mean particle sizes of 293 and 495 μm was investigated in a bench-scale apparatus. For the correlation of the experimental data, a mass balance model coupled with various assumptions—including those of the Lack’s plug flow model—was employed. Comparison of the results demonstrated that best fit is obtained when the model takes into account the equilibrium as well as the mass transfer phenomena, that control the extraction process.