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Water as a green solvent combined with different techniquesfor extraction of essential oil from lavender flowers
Aurore Filly a, Anne Sylvie Fabiano-Tixier a, *, C�eline Louis c, Xavier Fernandez b,Farid Chemat a
a Universit�e d'Avignon et des pays de Vaucluse, INRA, UMR408, GREEN Extraction Team, 84000 Avignon, Franceb Universit�e Nice Sophia Antipolis, UMR 7272 CNRS, Institut de chimie de Nice, Parc Valrose, 06108 Nice, Francec Naturex SA, 250, rue Pierre-Bayle, BP 81218, 84911 Avignon cedex 9, France
a r t i c l e i n f o
Article history:Received 6 October 2015Accepted 28 January 2016Available online 1 April 2016
The traditional way of isolating volatile compounds asessential oils from lavender flowers (Lavandula hybribia L.)is distillation. During distillation, fragrant plants areexposed to boiling water or steam, releasing their essential
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oils. The recovery of the essential oil is facilitated by thedensity difference of water and essential oil at ambienttemperature. Distillation is frequently done by prolongedheating for several minutes to hours, which can causedegradation of the thermo labile compounds present in thestarting plant material and therefore odor deterioration.This conventional method has high consumption of energy(70% of total process energy) and time. Due to increasingenergy prices and the drive to reduce CO2 emissions, aca-demic and industrial scientists are challenged to find
s sciences. This is an open access article under the CC BY-NC-ND license
A. Filly et al. / C. R. Chimie 19 (2016) 707e717708
innovative technologies (Fig. 1) which can reduce energyconsumption, achieve cost reduction and increased quality.Much attention has been devoted to the innovative pro-cesses such as the instant controlled pressure drop (DIC)technology, supercritical fluid extraction (SFE), ultrasoundassisted extraction, microwave extraction, enzyme-assistedextraction, alternative solvents, for isolation essential oilfrom fragrant plants [1e13].
Besides, the use of water as a solvent has tremendousbenefits as a green extraction solvent because water is notonly inexpensive and environmentally benign; but it is alsonon-flammable, nontoxic, providing opportunities forclean processing and pollution prevention.
In addition to the environmental advantages of usingwater instead of organic solvents, purification of products isnormally facilitated because, once cooled, the organic prod-ucts are not soluble at ambient temperature water, whichfaster start-up, and simplification of process steps. However,thewater is a polar solvent, with a density, a viscosity, and anactivity which can impair solubility, the transfer or the con-tact with the matrix. Changing parameters and physicalconditions of extraction, can overcome this problem.
The higher temperature of extraction can increasesolvent-matrix interaction, but also transfer, solubility anddiffusion. The macroscopic dielectric constant of a solvent(εr) characterizes the polarity of the medium and controlsthe ionic dissociation of salts. The dielectric constant ofwater decreases at high temperatures and pressures, whichincreases water diffusivity. Under these conditions, water isable to solubilize more non polar molecules [10].
Fig. 1. Processes for isolating essenti
Under soft conditions, it is possible to use water addi-tives to assist extraction of the natural product. Anotheralternative approach to intensify essential oil release is thepartial or complete hydrolysis of the cell walls by means ofenzymes [14e16]. Surfactant molecules allow solubilityenhancement of more hydrophobic molecules inwater [17]and finally salt may be employed to enhance the concen-tration of certain components in the essential oil [18,19].
This present study has been planned with the aim todesign and optimize a new and green technique for theextraction of essential oils from lavender (L. hybribia L.)flowers and possible improvement of its yield. Compari-sons were investigated between nine extraction techniquesand conventional HD as well as in terms of extraction time,yield, aromatic composition, energy used and environ-mental impact of the process. Finally, using COSMO-RSsoftware was proposed to understand the extractionmechanism.
2. Materials and methods
2.1. Plant and chemical material
The lavender (L. hybribia L.) flowers used were collectedfrom the south of France in July 2013 (Alp'erbo SARL, Man-osque, France). Analytical grade anhydrous sodium sulfateand Tween 40 were purchased from Fisher Scientific (Lei-cestershire, UK). Cellulase from Aspergillus aqueous solutionwas purchased from Sigma Aldrich (Steinheim, Germany).
al oils from the plant material.
A. Filly et al. / C. R. Chimie 19 (2016) 707e717 709
2.2. Extraction procedures
Hydro-distillation is the fundamental method forextraction of the lavender essential oil. This present studyhas been planned with the aim to design and optimize anew and green technique for the extraction of essential oilsfrom lavender (L. hybribia L.) flowers and possibleimprovement of its yield.
The extraction of the essential oils from lavender wasperformed using ten different methods; hydro-distillation(HD), steam distillation (SD), turbo hydro-distillation (THD),pre-treatment with salt (Salt-HD), enzyme (Enzyme-HD),micelle (Micelle-HD), ultrasound (US-HD) or supercriticalwater (WS-HD) followed by conventional hydro-distillationand finishing with microwave assisted extraction tech-niques suchas solvent-freemicrowaveextraction (SFME) andmicrowave steam distillation (MSD) (Fig. 2).
The appropriate experimental variables (amount ofenzyme, surfactant, salt, and microwave power) for eachprocess were optimized in order to maximize the essentialoil yield.
2.2.1. Hydro-distillation (HD)Two hundred fifty gram of lavender weremixedwith 3 L
of water. The mixture was submitted to hydro-distillationusing a Clevenger-type apparatus [20] according to theEuropean Pharmacopoeia for 2 h (until no more essential
Fig. 2. Extraction
oil was obtained). The essential oil was collected, weighed,dried under anhydrous sodium sulfate and stored at 4 �Cbefore analysis. Each extraction was performed at leastthree times.
2.2.2. Steam distillation (SD)To facilitate rigorous comparison, the same glassware
and the same operating conditions were used for conven-tional steam distillation. The specific glassware contained3 L of distilled water and 250 g of lavender on a rack, so thatthere is no contact between water and lavender. The waterwas heated, the steam passed through the sample, evapo-rating and carrying the essential oil, and directed it towardthe condenser and the Florentine flask. The oils obtainedwere recovered, weighed, dried over anhydrous sodiumsulfate (Na2SO4) and stored in amber vials at 4 �C untilrequired. Each extraction was performed at least threetimes.
2.2.3. Turbohydro-distillation (THD)In this method, the same glassware and same conditions
were used as that for hydro-distillation. The mixture wascontinuously agitated with a stainless steel stirrer at100 rpm, for 2 h. The oils obtained were recovered,weighed, dried over anhydrous sodium sulfate (Na2SO4)and stored in amber vials at 4 �C until required. Eachextraction was performed at least three times
processes.
A. Filly et al. / C. R. Chimie 19 (2016) 707e717710
2.2.4. Salt-assisted extraction followed by conventional hydro-distillation (Salt-HD)
Two hundredfifty gramof lavenderweremixedwith 3 L-distilled water containing 150 g of NaCl (values determinedafter optimization). The mixtures were subjected to hydro-distillation for essential oil isolation. To facilitate rigorouscomparison, the same glassware and the same operatingconditions were employed. The oils obtained were recov-ered, weighed, dried over anhydrous sodium sulfate(Na2SO4) and stored in amber vials at 4 �C until required.Each extraction was performed at least three times.
2.2.5. Enzyme-assisted extraction followed by conventionalhydro-distillation (Enzyme-HD)
Two hundred fifty gram of lavender were mixed with3 L-distilled water containing 12 g of cellulase fromAspergillus aqueous solution (SigmaeAldrich) [21e25]. Themixtures were stirred for 60 min at 40 �C and then sub-jected to hydro-distillation for essential oil isolation. Tofacilitate rigorous comparison, the same glassware and thesame operating conditions were employed. The oils ob-tained were recovered, weighed, dried over anhydroussodium sulfate (Na2SO4) and stored in amber vials at 4 �Cuntil required. Each extractionwas performed at least threetimes.
2.2.6. Micelle-mediated extraction followed by conventionalhydro-distillation (Micelle-HD)
Two hundred fifty gram of lavender weremixed with anaqueous surfactant solution containing 10% Tween 40. Tofacilitate rigorous comparison, the same glassware and thesame operating conditions were employed. The oils ob-tained were recovered, weighed, dried over anhydroussodium sulfate (Na2SO4) and stored in amber vials at 4 �Cuntil required. Each extractionwas performed at least threetimes.
2.2.7. Ultrasound assisted extraction followed by hydro-distillation (US-SD)
The ultrasound-assisted extraction was performedusing an ultrasound extraction reactor (BS2d34, HielscherUIP 1000hd). Lavender was extracted with 3 L of distilledwater with an ultrasound of 700 W. The extractor andwater were regulated at 25 �C during sonication. After thepre-treatment of 1800 s, conventional hydro-distillationwas performed to extract the essential oil with the sameglassware. The oils obtained were recovered, weighed,dried over anhydrous sodium sulfate (Na2SO4) and storedin amber vials at 4 �C until required. Each extraction wasperformed at least three times
2.2.8. Subcritical water extraction followed by conventionalhydro-distillation (WS-HD)
Ultraclave is a device of Milestone Company. This is a2.45 GHz multimode microwave reactor with a maximumpower of 1200 W delivered in 10 W increments. Duringexperiments, the time, temperature, and power deliveredby microwave and internal pressure were controlled bythe software. A compressor connected to a nitrogen cyl-inder conditioned initial pressure. The ultraclave supportsa maximum pressure of 200 bar and a temperature of
220�. A cooling system is coupled to the cavity. Theopening system may be at atmospheric pressure with atemperature below 80 �C. The vessel containing 250 glavender mixed with 3 L of water, after having beendegassed by ultrasound, was placed in the cavity. Theinitial working pressure of nitrogen was 30 bar. Theworking temperature of 125 �C is reached with a heatingpower of 1000 W. The temperature increase is achieved in15 min, and then it is regulated for 30 min. The pretreatedlavender was subjected to conventional hydro-distillationto extract essential oils with the same glassware. The oilsobtained were recovered, weighed, dried over anhydroussodium sulfate (Na2SO4) and stored in amber vials at 4 �Cuntil required. Each extraction was performed at leastthree times.
2.2.9. Solvent-free microwave extraction (SFME)SFME was performed in a NEOS (Milestone, Italy)
microwave laboratory oven. This is a 2.45 GHz multi-mode microwave reactor with a maximum power of900 W delivered in 10 W increments. The time andpower of microwaves are selected. The experimentalSFME variables were optimized in order to maximize theessential oil yield. This procedure was performed at at-mospheric pressure. A condenser placed outside a mi-crowave was connected to specific glassware thatcontained 125 g of lavender after having been soaked in500 mL of distilled water for 10 min. Lavender washeated using a fixed power of 500 W for 45 min.Condensed water was refluxed to the extraction vessel inorder to provide uniform conditions of temperature andhumidity for the extraction. Essential oil and aromaticwater were simply separated by decantation in a Flor-entine flask. The oils obtained were recovered, weighed,dried over anhydrous sodium sulfate (Na2SO4) and storedin amber vials at 4 �C until required. Each extraction wasperformed at least three times.
2.2.10. Microwave steam distillation (MSD)To facilitate rigorous comparison, the same equipment
and the same conditions: time and power were used. Theprocess is based on the conventional steam distillationprinciple in which microwave radiation is only applied onthe extraction reactor. The use of water steam generatedwithin the vessel requires that the lavender (125 g) besupported above some boiling water by a grid. The waterwas heated, the steam passed through the sample, evapo-rating and carrying the essential oil, and directed it towardthe condenser and a Florentine flask. The essential oil wascollected, weighed, dried under anhydrous sodium sulfateand stored at 4 �C until used. Each extraction was per-formed at least three times.
2.3. Computational methods: COSMO-RS software
The Conductor-like Screening Model for Real Solvents(COSMO-RS) developed by Klamt and co-workers is knownas a powerful method for molecular description based on aquantum-chemical approach. COSMO-RS combines quan-tum chemical considerations (COSMO) and statisticalthermodynamics (RS) to determine and predict
A. Filly et al. / C. R. Chimie 19 (2016) 707e717 711
thermodynamic properties without experimental data.COSMO-RS is a relatively new prediction method for solu-bility and other physicalechemical properties. The theoryCOSMO-RS is previously given in several papers [21e25]. Abrief sketch of the practical course of a COSMO-RS isconsidered here. The calculation has been investigated forthree molecules of interest (linalyl acetate, linalool, and 4-terpineol), using the cosmotherm program, (Version C30Release 13.01). The COSMO model is applied to simulate avirtual conductor environment for the molecule of interest.In such an environment the molecule induces a polariza-tion charge density s on the interface between the mole-cules and the conductor, i.e. on the molecular surface. Thus,during the quantum calculation self-consistency algorithmthe solute molecule is converged to its energeticallyoptimal state in the conductor with respect to electrondensity and geometry. The standard quantum chemicalmethod for COSMO-RS is density functional theory (DFT),which is used throughout this study. The output of a DFT/COSMO calculation is a file providing this optimized ge-ometry of the molecule, the total energy of the molecule inits conductor environments, and complete three-dimensional information about the polarization chargedensity: s-surface. These calculations act as molecular in-formation input for used the model to real solvents. The s-surface of each molecule X is converted into a distributionfunction (s-profile). The full equations are given in Klamt[22,23]. Finally, the chemical potential of compound X insystem S is calculated by integration, which gives histo-gram s-potential. The chemical potential can now be usedto calculate a wide variety of thermodynamic properties,such as the solubility and energy of the reaction. The sol-ubility option allows for the automatic computation of thesolubility of a liquid or solid compound j in a solvent i.Within the calculation all compounds are also consideredsolutes. This approach is optimized for the calculation ofmany solutes in a limited number of solvents, at a specifictemperature or in a temperature range. Here, the values ofthe solubility of each interest molecules have been calcu-lated in water in the temperature range: 25e150 �C (Fig. 6).It is important to note that the values obtained are relative,not absolute. The reaction panel basically allows calculatingthe equilibrium constant (Kreac) and the free energy (DGreac)of a given reaction in an arbitrary solvent. The Gibbs freeenergy of reaction is defined as difference of the total freeenergies of the product compounds and the reactantcompounds.
For an example of reaction: linalool / 4-terpineol, thefree energy is defined as:
DGreac ¼ Gð4terpineolÞ � GðlinaloolÞThe equilibrium constant of the reaction can be
computed from the Gibbs free energy of the reaction:
Kreac ¼ e
��DGreac
RT
�
In each calculation, the solvent, the temperature andboth sides of the reaction have to be specified. The stan-dard approach gives a prediction relative to a reactionenergy.
2.4. GC and GCeMS identification
2.4.1. Gas chromatography by using a flame ionic detector (FID)GC analysis was carried out using an Agilent 6850 gas
chromatograph, under the following operation condi-tions: vector gas, helium; injector and detector temper-atures, 250 �C; injected volume, 1 ml; split ration 1/100;HP1 column (J&W Scientific), polydimethylsiloxane(10 m � 1 mm i.d., film thickness � 0.4 mm; constant flow0.3 mL/min). Temperature program 60e250 �C at 4 �C/min and 250 �C for 80 min. Retention indices weredetermined with C6 to C27 alkane standards as refer-ences. Relative amounts of individual components arebased on peak areas obtained without FID response fac-tor correction. Three replicates were performed for eachsample. The average of these three values and the stan-dard deviation were determined for each componentidentified.
2.4.2. Gas chromatography-mass spectrometry analysisGCeMS analysis was carried out using an Agilent
6890N coupled to an Agilent 5973 MS (Agilent, Massy,France). Each sample has been diluted at 10% indichloromethane. Samples were analyzed on a fused-silica capillary column HP-1MS™ (polydimethylsiloxane,50 m � 0.25 mm i.d. � film thickness 0.25 mm; Interchim,Montluçon, France) and INNOWAX (polyethyleneglycol,50 m � 0.20 mm i.d. � film thickness 0.4 mm; Interchim,Montluçon, France). Operation conditions: carrier gas,helium; constant flow 1 mL min�1; injector temperature,250 �C; split ratio, 1:150; temperature program,45 �Ce250 �C or 230 �C, at 2 �C/min then held isothermal(20 min) at 250 �C (apolar column) or 230 �C (polarcolumn); ion source temperature, 230 �C; transfer linetemperature, 250 �C (apolar column) or 230 �C (polarcolumn); ionization energy, 70 eV; electron ionizationmass spectra were acquired over the mass range of35e400 amu.
2.4.3. Identification of the componentsIdentification of the components was based on com-
puter matching against commercial libraries (Wiley,MassFinder 2.1 Library, NIST98), laboratory mass spectralibraries built up from pure substances, and MS literaturedata [8,26,27] combined with a comparison of GC retentionindices (RI) on apolar and polar columns reported in theliterature. RIs were calculated with the help of a series oflinear alkanes C6eC27 on apolar and polar columns (HP-1MS™ and HP-INNOWAX). Compounds available in thelaboratory were confirmed by external standard compoundco-injection.
2.5. Sensory analysis
Sensory evaluation was used to discriminate the in-tensities of the main aromatic characteristics of lavendersamples. Each essential oil was evaluated olfactorically byC. Louis (Perfurmer from Naturex, France). Ten differentcoded samples of essential oil of lavender obtained bydifferent techniques have been classified in 12 odor attri-butes: floral lavender, herbaceous, camphoraceous, woody,
A. Filly et al. / C. R. Chimie 19 (2016) 707e717712
spicy pepper, fruity, fatty/aldehydic, sweet/“candy”, soapy,off-note, intensity and persistence. Sample HD were usedas standards. The individual products were scored for theintensity of different aroma attributes on a scale of 0e3,where:
0: not present1: slight intensity2: average intensity3: high intensity
-1
0
1
2
3
4
5
6
7
-20 0 20 40 60
Yiel
d (%
)
Time (min)
-1
0
1
2
3
4
5
6
-20 0 20 40 60
Yiel
d (%
)
Time (min)
a
b
Fig. 3. Yield profile of essential oil obtained via various extraction methods using wwater (b).
The essential oil of lavender has been prepared with 10%of ethanol, in plastic beakers with lids, which stood at roomtemperature for 30 min prior to analysis.
3. Results and discussion
3.1. Kinetics
Fig. 3 shows the variation in extraction yield according toextraction time. The yield is defined as the percentage of
80 100 120 140
HD
SD
THD
US-HD
SFME
MSD
SW-HD
80 100 120 140
HD
Salt-HD
Enzyme-HD
Micellar-HD
ater under different physical states (a) extraction methods with additivated
A. Filly et al. / C. R. Chimie 19 (2016) 707e717 713
weight of the essential oil extracted from the initial mass oflavender flowers used. Hydro-distillation (4.55 ± 0.16%) wasthe reference method in essential oil isolation. The yieldsobtained from steam distillation (4.49 ± 0.06) and enzyme-HD (4.58 ± 0.14) were of the same order of magnitude asthat of conventional hydro-distillation. Turbo-distillation(THD) and supercritical water pre-treatment (SW-HD) donot have a positive effect on extraction kinetics and give amaximumyield of 4.2 ± 0.36% and 3.89± 0.07% respectively,versus 4.55 ± 0.16% by HD. An increase of the extractiontemperature to 100 �C at 125 �C by the SW-HD methodshows a decrease of the extraction efficiency. Thus, a
Table 1Chemical composition of lavender essential oils obtained by different techniques
* Compounds know in the rosemary.a Essential oil compounds sorted by chemical families.b Retention indices relative to C6eC27 n-alkanes calculated on non-polar HP1
prolonged exposure time to each heating temperature ap-pears to decrease terpene stability [28].
Otherwise, it is interesting to note that ultrasound pre-treatment of added salt or Tween 40 at hydro-distillationshows an improvement of the extraction. Indeed, US-HD,Salt-HD and Micelle-HD provide yields of 5.01 ± 0.45%,5.06 ± 0.35% and 4.88 ± 0.07%, respectively, against4.55 ± 0.16% by the conventional method. The cavitationprocess that occurs during sonication causes the rupture ofcell walls, which enhances extraction essential oil. The useof salt in water allows improving the recovery of somevolatile constituents from floral waters.
A. Filly et al. / C. R. Chimie 19 (2016) 707e717714
The presence of surfactant micelles of Tween 40 inwater reduced the surface of tension between oil on theflowers and the distillationwater; this explains the increasein the extraction yield.
One of the advantages of the extraction assisted bymicrowave is rapidity. The extraction process bymicrowaveallows having 80% of final yield in 20 min. The end of theextraction process is reached after 30 min for the micro-wave process and 90 min using HD. Furthermore, thevalues obtained for essential oil yield are 3.9 ± 0.3% and5.4 ± 0.5% for SFME and MSD respectively, versus4.5 ± 0.2%. Based on these initial results, the MSD extrac-tion appears to be promising.
3.2. Composition of essential oil
A total of 47 major compounds (in agreement with theliterature) were identified in the lavender essential oil(Table 1). The lavender flower essential oils extracted using
Fig. 5. Formation of linalo
the different methods are all rather similar in their flavorprofile. The principal volatile compounds are linalool andlinalyl acetate followed by minor amounts of camphor,borneol, 1.8 cineole, lavandulyl acetate, 4-terpineol and a-terpineol; however, their proportions depend on theisolation technique used.
As Table 1 shows, even if these samples seem to be quitesimilar, they are different considering only their mean insome oxygenated compounds such as linalyl acetate,linalool and 4-terpineol. The mean percentage of linalylacetate is slightly higher than that of linalool for theextraction assisted bymicrowave and steam distillation butthe contrary is significantly observed in all other tech-niques (Fig. 4). These differences are probably due to thedegradation of linalyl acetate (when in contact with water)into linalool (Fig. 5). In SD, SFME and MSD, lavender is notdirectly in contact with water like in HD, consequently, thedegradation of linalyl acetate is less marked than in HD[29]. The essential oil obtained by microwave shows higher
ol and 4-terpineol.
0
0.0005
0.001
0.0015
0.002
0.0025
0.003
0.0035
0.004
0.0045
0 50 100 150 200
mas
s sol
ubili
ty: w
_sol
ub (g
/g)
Temperature (°C)
Linalyl acetate
Linalool
4-terpineol
Fig. 6. Solubility as a function of water temperature.
00.5
11.5
22.5
3Floral lavender
Herbaceous
Camphoraceous
Woody
Spicy pepper
FruityCitrus/BergamotFa y/aldehydic
Sweet/"Candy"
Soapy
Intensity
Persistance
HD
THD
SD
US-HD
SW-HD
00.5
11.5
22.5
3Floral lavender
Herbaceous
Camphoraceous
Woody
Spicy pepper
FruityCitrus/BergamotFa y/aldehydic
Sweet/"Candy"
Soapy
Intensity
Persistance
HD
SFME
MSD
00.5
11.5
22.5
3Floral lavender
Herbaceous
Camphoraceous
Woody
Spicy pepper
Fruity
Sweet/"Candy"
Soapy
Intensity
Persistance
HD
NaCl-HD
Enzyme-HD
Micelle-HD
A. Filly et al. / C. R. Chimie 19 (2016) 707e717 715
values of linalyl acetate and lower values than by steamdistillation of linalool.
For extraction Micelle-HD the mean percentage oflinalool was high and the percentage to 4-terpineol wasslightly above the hydro-distillation. The linalool moleculeis unstable and it can transformed into 4-terpineol (Fig. 5).The calculation of the free enthalpy (Greac) and the constant(Kreac) of the reaction has been performed at 100 �C withCOSMOtherm program. As shown in Fig. 4b, linalool rear-rangement of 4-terpineol presents a negative value of Greacand a greater value of Kreac. At 100 �C, the reaction isspontaneous and total. Theory data confirm rearrangementhypothesis.
The same observations can be made for results foundwith THD, enzyme-HD and US-HD.
Furthermore, SW-HD shows a mean percentage oflinalool higher than linalyl acetate, which can be due to thedegradation, as seen previously. This extract presented alsoa significant amount of 4-terpineol. This percentage may beexplained by the rearrangement of linalool in 4-terpineolbut also by the increase extraction temperature. Indeed,calculation of solubilities with Cosmotherm program, of
Conven onal (HD, SD)
Salt-HD
Micellar-HD
Microwave (SFME,MSD)
US-HD
Enzyme-SD
SW-HD
0 0,5 1 1,5 2 2,5 3 3,5 4 4,5 5
Environmental impact
Time (H)
Totale Energy consump on (kW / h)
kg de co2
Fig. 7. Environmental analysis.
Citrus/BergamotFa y/aldehydic
Fig. 8. Sensorial analysis.
A. Filly et al. / C. R. Chimie 19 (2016) 707e717716
three interest molecules, at temperatures ranging from 25to 150 �C (in step of 25 �C) shows a better solubilization(Fig. 6). The influence of the temperature on aqueous so-lution solubility has a significant effect on 4-terpineol,followed by linalool and a less effect on linalyl acetate. Thismay also explain the levels of these molecules in the ex-tracts of SW-HD.
3.3. Environment impact, cost and upscaling
Extractions assisted by microwave are clearly advanta-geous in terms of time and energy (Fig. 7). The energyrequired to perform the two extraction methods are3.452 kW h�1 per gram of essential oil for HD and0.298 kW h�1 per gram of essential oil for microwave. Thepower consumptionwas determined with aWattmeter at amicrowave generator entrance and an electrical heaterpower supply. Hydro-distillation requires an extractiontime of 120 min to heat the water and plant material to theextraction temperature, while the microwave methodsrequire only 30min of lavender flower heating (SFME) or toheat the water (MSD).
Regarding environmental impact, the calculated quan-tity of carbon dioxide released into the atmosphere isdramatically higher in HD (2762 g CO2/g of essential oil)than by microwave extraction (238 g CO2/g of essential oil).These calculations have been made accordingly to obtain1 kWh from coal or fuel, 800 g of CO2 will be rejected in theatmosphere during combustion of fossil fuel [30].
For the extraction, US-HD and SW-HD add an energyconsumption at HD of 0.16 kW h and 1.28 kW h,
Table 2Summarized advantages and drawbacks of using water as a solvent with variabl
TechnicalEssential oil
yield
Extraction
Time
HD Reference Reference
SD = =
THD - =
US + +
SW - +
Salt + =
Enzyme = +
Micelle + =
SFME = -
MSD + -
Sign + corresponding at a value higher than the referenSign – corresponding at a value lower than the referenRed color describe a negative effectGreen color describe a positive effect
Nega ve effect Re
respectively. In other terms, ultrasound rejected 128 g ofCO2, ultraclave pre-treatment rejected 1024 g of CO2. Theuse of the enzyme or surfactant decreases energy con-sumption of 5.05% and 13.05%, respectively, versus theconventional method.
Microwave extraction is a very clean method, which al-lows essential oil extraction without being followed byhydro-distillation. SFME or MSD generate fresh aromaticflower “without essential oil”which couldbeused as food forruminants. The SFME method has an additional advantageversus MSD: step of wastewater treatment is not needful.
Furthermore, microwave and ultrasound becomemature and accepted technologies for industrial applica-tions. Microwave and ultrasound extractions could be usedto produce larger quantities of essential oils by usingexisting large-scale extraction reactors treating for10e100 kg of aromatic herbs and spices [31e37].
3.4. Sensory analysis
The sensory analysis results are presented in Fig. 8. Themain notes of aromatic lavender namely “floral lavender”,“herbaceous”, “camphoraceous”, “fruity citrus/bergamot”are generallywell represented in all samples. It is interestingto note that SW-HD, SFME, MSD and Micelle-HD essentialoils give the most typical profiles: “fruity citrus/bergamot”with sides “fatty/aldehyde” and “sweet/candy” that can tobe associated at linalyl acetate amount. Besides, theextractionmicrowave technology offers a similar odor of theplant. SW-HD sample gives a special typical “peppery spicy”& “citrus bergamot” interesting, that are characteristic notes
e geometry have been compared to the hydro-distillation.
DegradationEnvironmental
friendlyCost
Reference Reference Reference
- = =
+ = +
+ + +
+ + +
- = =
= - +
+ - +
- - +
- - +
ce valuece
ference Posi ve effect
A. Filly et al. / C. R. Chimie 19 (2016) 707e717 717
of 4-terpineol and linalool [38], respectively. Besides, it isobserved that the pre-treatment of the material by grinding(THD) or ultrasound (US-HD) before the hydro-distillationincreases typicities “herbaceous” and “camphoraceous”while maintaining the “floral lavender” side. The pre-treatment with the salt (NaCl-HD) or enzyme (enzyme-HD) presented atypical off-notes. Besides, these extractsgive lower intensity and persistence products. In conclusion,pre-treatment of the material with grinding (THD), ultra-sound (US-HD), micelle-mediated (Micelle-HD) beforehydro-distillation conventional and extraction by micro-wave technology (SFME and MSD) provides an excellentalternative to the traditional technologies such as hydro-distillation or steam distillation.
4. Conclusion
Using water as an alternative solvent for extraction in-cludes: reduced environmental impact, selective extrac-tion, use of simple equipment, no hazards, faster start-up,and simplification of process steps. Advantages and draw-backs of using water as a solvent with variable geometryhave been compared to the hydro-distillation (Table 2).
The values extraction time, extraction yield, degrada-tion, environmental impact of Hydro-distillation areconsidered as the reference. A better extraction yield,shorter extraction time compared to reference, gives posi-tive impact (green). In contrast, longer extraction times,lower extraction efficiency, greater degradation of aromasor a significant environmental impact assessment will beconsidered as negative effects (red).
The results identified the optimal extraction techniqueas being the steam distillation assisted by microwave(MSD). Indeed, MSD offers important advantages overtraditional hydro-distillation. It gave a yield of 5.4% in30 min, versus 4.6% in 120 min for hydro-distillation andconsumed 0.298 kWh against 3.452 kWh by the conven-tional method. The essential oil obtained was of excellentquality (linalyl acetate amount and a similar odor of theplant). MSD is a promising tool for the extraction ofessential oil from lavender flowers.
Acknowledgments
Aurore Filly thanks “R�egion PACA” (ProvenceeAlpeseCote d'Azur) and competitivity cluster PASS (Pole AromesSenteurs et Saveurs) for her doctoral grant.
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