Nat. Volatiles & Essent.

Oils, 2021; 8(6): 1575-1588

Solid-State Fermentation Of Cinnamon Bark Using Aspergillus

Awamori To Increase Cinnamon Oil Yield Extracted Using
Hydrodistillation, Maceration, And Soxhlet Extraction
Muhammad Yusuf Abduh 1, 2 , RavelianYulianto1 , Dennis Avima1 , Abednego Kurio
Widianto1 , Rika Alfianny1

1
School of Life Sciences and Technology, InstitutTeknlogiBandung, Jalan Ganesha No. 10 Bandung
40132, Indonesia

2
University Center of Excellence for Nutraceuticals, Bioscience and Biotechnology Research Center,
InstitutTeknlogi Bandung, Jalan Ganesha No. 10 Bandung 40132, Indonesia

Abstract

This research was conducted to determine the optimum fermentation time ofcinnamon (Cinnamomum burmannii)
bark usingAspergillus awamori to degrade lignocellulose content in the cinnamon bark. Aspergillus
awamoriinoculum, 108 cells/g, was added to the substrate and the fermentation was carried out at 25-30°C, ~0
W/cm2 light intensity and ~99% humidity for 0, 3, 6, and 9 days. Before the fermentation, the cellulose,
hemicellulose, and lignin content in the cinnamon bark substrate were 15.37%, 27.83%, and 48.04%, respectively.
The biggest decrease of cellulose, hemicellulose, and lignin occurred after 9 days of fermentation: 12.37%, 16.55%,
and 39.95%, respectively. Cinnamon oil extraction was carried out using hydrodistillation, maceration and Soxhlet
methods. The yield of cinnamon oil after 9 days of fermentation using the hydrodistillation, maceration and
Soxhlet methods were 2.09%, 2.47%, and 3.01%, respectively. Composition of the cinnamon oilwas analysed using
Gas Chromatography - Mass Spectrometry. The cinnamon oil primarily composed of cinnamaldehyde, and the
concentration varies with fermentation time and extraction methods. A mathematical model was also developed
to determine the diffusion coefficient of cinnamon oil during the extraction process that can be used predict the
cinnamon oil yield. The results indicate that a higher diffusion coefficient of 2.36 x 10 -11 m2/s was obtained for the
hdyrodistillation method, followed by Soxhlet (1.44 x 10-11 m2/s) and maceration (1.42 x 10-12 m2/s). The
mathematical model can predict the cinnamon oil yield for all extraction methods reasonably well.

Keywords: Aspergillus awamori,Cinnamon oil, Cinnamaldehyde, Extraction,Lignocellulose

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1. Introduction
Cinnamon is a type of spice obtained from the bark of plants within the genus Cinnamomum and
belongs to the Lauraceae family [1]. There are several species of cinnamon available in the market;
among them are Cinnamomum zeylanicum, Cinnamomum burmannii, and Cinnamomum cassia [2].
Cinnamon plants have a lot of applications in different areas. Cinnamon leaves can be used as pesticides,
its wood can be used as building materials and to make particle board, meanwhile its bark, which is
most widely avialable, can be used as flavor, perfume base, and as an ingredient in pharmaceutical
products [3].

Indonesia, China, Sri Lanka, and Vietnam are the main suppliers of cinnamon in the global market. All
four countries supply up to 99% of the world's demand for cinnamon. Indonesia is the world's largest
supplier of cinnamon with a total production of 87,130 tons in 2017 [4]. Cinnamon plantations in
Indonesia are centered in West Sumatra Province, especially in Kerinci Regency, and are also present in
Aceh, North Sumatra, Bengkulu, West Java, and East Java. Nevertheless, most of the cinnamon
production in Indonesia is still at the upstream level. This is a problem because the export price of
cinnamon has decreased every year, reaching USD 0.17/kg in 2008 due to excessive availability [3]. One
of the efforts that can be made to overcome the excess supply of cinnamon is by processing cinnamon
into its derivative products, such as cinnamon oi that causes the fragrant aroma of cinnamon [6].

Essential oils have many beneficial properties, including antiseptic, antispasmodic, and other health
benefits. In addition, essential oils are also widely used in food and cosmetics, especially in the
production of perfume [7]. Cinnamon oil is widely produced throughout the world with the largest
producer being Sri Lanka [8]. The market price of cinnamon oil is relatively high compared to barley
cinnamon, around USD 29-34/kg [9]. This high price can provide added values for the excess stock of
cinnamon in Indonesia.

Essential oils can be extracted through variousextraction methods such as supercritical extraction and
solvent extractionas well as distillation [10]. A typical issue in the extraction of essential oil is its
relatively low yield. Extraction of essential oils using asteam distillation method produces a yield of 1.23-
2.95% [1,9] whereasahydrodistylation method produces a yield of 1.7-3.1% [11,12], while the yield for
Soxhlet extraction and maceration have been reported as 3,83% [1] and 2.28% [13], respectively. A
higher yield of cinnamon oil can be achieved by optimizing the operating conditions of the extraction
process or through initial treatment/pre-treatmentof the substrate.

Pre-treatment of the substrate can be carried out in the form of drying or degradation of components
within the cell wall of the substrate [14]. Plant cell walls are composed of lignin, cellulose, and
hemicellulose[15]. Degradation of these compounds can facilitate better contact between solvent and
essential oil components present in the cell. Enzymes can be used to degrade compounds of thecell
walls. Aspergillus awamori is one type of microorganisms capable of producing enzymes that can
degrade lignocellulosic compounds or delignify cell walls [16]. Aspergillus sp. can reduce the

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lignocellulose content of a biomass up to 22.6% for lignin, 38.3% for cellulose, and 18.9% for
hemicellulose [17].

Pre-treatment in the form of degradation of lignocellulosic compounds by Aspergillus awamori can

degrade the lignocellulosic content of cinnamon bark to increase the yield of cinnamon oil. Hence, this
study was conducted to determine the effect of biodegradation of cinnamon bark by Aspergillus
awamori on the yield and composition of cinnamon oil. In addition, mathematical modeling of cinnamon
oil extraction was also carried out to determine the diffusion coefficient and predict the cinnamon oil
yield extracted using different methods particularly hydrodistillation, maceration and Soxhlet extraction
methods.

2. Materials and Methods

2.1Materials
Cinnamomum burmannii bark samples were obtained from Gambung Tea and Tea Plantation Center
(PPTK), Bandung Regency, West Java whereas Aspergillus awamori, potato dextrose agar, sodium
chloride, n-hexane, sulphuric acid, dichloromethane, distilled water and aquades were obtained School
of Life Sciences,InstitutTeknologi Bandung, West Java, Indonesia.

2.2 Preparation of Cinnamon Bark

Fresh cinnamon bark was cleaned of its outer skin and vegetation. Cinnamon bark was then cut to about
3 x 3 cm and sterilized using ultraviolet light for 30 minutes [18].

2.3 Preparation of Aspergillus awamori Inoculum

Pure culture of Aspergillus awamoriwere subcultured to a potato dextrose agar (PDA) medium in
reaction tubes using inoculation needles aseptically. The cultures were incubated at room temperature
(25°C) for 7 days. After 7 days, 5 ml of NaCl solution was added into the reaction tubes to harvest
Aspergillus awamori before being transferred to a chemical glass. Determination of the number of cells
was done using ahemocytometer method [19].

2.4 Solid State Fermentation of Cinnamon Bark

Approximately 100 g of Cinnamon bark was placed in a fermentation tray. Each tray was given a solution
of 108 Aspergillus spores/g of cinnamon bark substrate. After that, aquadeswas added with a 1:1 ratio
with respect to the cinnamon bark.Small holes were provided at the bottom of the tray for drainage.
The fermentation tray was covered with a plastic to maintain a low light intensity (~0 W/m2). The
fermentation was performed at room temperature (25–27°C) for 0, 3, 6, and 9 days [17].

2.5 Measurement of Lignocellulose Content

Measurement of lignocellulose content in the cinnamon bark was carried out using a Chesson-Datta
method [20]. Approximately 1 g of cinnamon bark was weighed (a). A total of 150 ml of distilled water

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was added to the sample and heated using a water bath at 90-100°C for 1 hr. The mixture was filtered,
and the residue was rinsed with 300 mlof distilled water. The sample was then dried with an oven until a
constant was obtained (b). The dry residue was mixed with 150 ml of H2SO4 1 N while heated using a
water bath at 90-100°C for 1 hour. The mixture was given the same treatment as in the previous mixture
until a constant weight was obtained (c). The dried residue was then mixed with 10 ml of 72% H2SO4 for
4 hr at room temperature(25–27°C). The mixture was then mixed with 150 ml H2SO4(1 N) and refluxed
for 1 hr. After that, the solid compound obtained was rinsed with 300 ml of distilled water then dried
using an oven at 105°C until a constant weight was attained (d). The solid was then heated in a furnace
until it became ash and was weighed (e). The composition of lignocellulose was then calculated using
equation (1), (2), and (3).

(c) (g) −(d) (g)

% cellulose = (a) (g)
× 100%........................(1)
(d) (g) −(e) (g)
% lignin = (a) (g)
× 100%..........................(2)
(b) (g) −(c) (g)
% hemicellulose = (a) (g)
× 100%...............(3)

2.6 Drying of Cinnamon Bark

Fresh cinnamon bark that had been removed from the stalk was dried using an oven until it reached a
moisture content of 35-45% for extraction of cinnamon oil [9]. The water content of cinnamon bark was
calculated using equation (4).

cinnamon bark mass (g)

Moisture content (%) = fresh cinnamon bark mass (g)
× 100%........(4)

2.7 Extractionof Cinnamon Oil

Extraction of cinnamon oil was carried out using four different methods particularly steam distillation,
hydrodistillation, maceration and Soxhlet extraction. For steam and hydrodistillation, approximately 40
g of cinnamon bark wasused, and the steam distillation was carried out at 90-100°Cfor 4 hr. After that,
the distillate was separated using a separatory funnel and mixed with 30 ml of dichloromethane (DCM)
and shaken for 1 min followed by separation of the organic phase at the bottom part of the funnel. The
processes were repeated 3 times until all the essential oil in the distillate had been dissolved in the DCM
followed by evaporation using a rotary vacuum evaporator to evaporate the DCM[12].

As for maceration, approximately 30 g of cinnamon bark was immersed in a glass chamber containing
180 ml of n-hexane and stirred using a shaker at 150 rpm for 24 hr. After that, the mixture was filtered,
and the n-hexane was evaporated using a rotary evaporator at 60°C. The remaining semi-solid
compound (concrete) was reconstituted with 20 ml of n-hexane. The solution was heated at 75°C and
simultaneously stirred for 5 min and then filtered. The solution was stored at -18°C to -35°C and then
filtered by a cold filtration method. The n-hexane was evaporated again with a rotary evaporator and
the remaining solution was allowed to evaporate at room temperature (25–27°C) until the remaining n-
hexane evaporated.

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As for Soxhlet extraction, approximately 30 g of cinnamon bark was extracted using 150 ml of n-
hexanefor 3 hr followed by evaporation using a rotary vacuum evaporator, resulting in a semi-solid
(concrete) solution. The concrete was then dissolved in 10 ml of ethanol until it was completely
dissolved and then heated at 50ºC using an electric stove. The concrete was stored in a freezer at -20ºC
until the wax solidified. After that, the concrete was filtered to separate the waxy substance and the
mixture of cinnamon oil and ethanol. The filtered product was then evaporated at 40°C until all the
ethanol has evaporated [1,6]. All the extracted cinnamon oil was stored in a dark botlle for further
analysis. Cinnamon oil yield was determined using equation (5).

mass of cinnamon oil (g)

Yield (%) = mass of cinnamon bark (g)x(100−moisture content)
× 100%........(5)

2.8 Cinnamon Oil Composition Analysis

The composition of cinnamon oil was analyzed using a Gas Chromatography - Mass Spectrometry (GC-
MS) method at the Central Forensic Laboratory, Police of the Republic of Indonesia. The GC-MS
equipment consists of an oven, back inlet, and capillary column. The oven was operated at 80 ° C for 30
min. The back inlet was operated using a split method with a split ratio of 30:1. The capillary column
contains 5% phenyl methyl silox. The capillary column has a length of 30 m, a diameter of 0.25 mm, and
a thickness of 0.25 µm. The analysis of the composition of cinnamon oil was carried out based on the
database of National Institute of Standards and Technology.

2.9 Determination of Diffusion Coefficient for Extraction of Cinnamon Oil

A mathematical model was developed out to determine the diffusion coefficient for extraction of
cinnamon oil using a second Fick's law of diffusion[22] as shown in equation (6).

dφ g cm2 d2 φ g
(
dt cm3 s
) = D(s
) d2 x (cm5 ) .................................(6)

whereD is the diffusion coefficient (cm2/s), φ is the concentration (g/cm3), and x is the position
(cm).Relevant assumptions used in constructing the model to determine the diffusion coefficient for
extraction of cinnamon oil are as follows:
1. The value of Dis constant
2. There is no diffusion resistance in the solution around the particles
3. There is no oil concentration on the particle surface due to washing by solvent
4. The concentration of oil in the particles is uniform
5. The geometry of the plate-shaped particles is uniform with a thickness of L
6. The diffusion process occurs in 1 dimension
Equation (6) can be derived using the number of exponential decays to yield equation (7)to compare the
experimental values with those based on the model. This model is valid for the acquisition value when t
is greater than 0.

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Mt (%) −1 ) x t(s))
M∞ (%)
= 1 − Ae(−B(s ...................................(7)

whereMt is the yield at time t, M∞ is the yield at steady state, A is the model constant (A = 8/π2 for plate
geometry), t is time, and B is the diffusion rate constant. Equation (7) can be simplified to equation (8)
by changing the yield fraction of cinnamon oil to a constant E [23].

Mt (%) −1
E=1− = Ae(−B(s ) x t(s))
M∞ (%)
−1 )
ln E = ln A − B(s x t (s) ....................................(8)

Parameter Bwas determined using a curve fitting feature on MATLAB® based on equation (8). The value
of parameter Bwas used to determine the value of D, the diffusion rate coefficient that can be
determined using equation (9), where L is the particle width used in this study (1.25 x 10-3 m)[24].

cm2 B(s−1 ) x L(cm)2

D( s
) = π2
.........................................(9)

3. Results and Discussion

3.1 Effect of Different Extraction Methods on Cinnamon Oil Yield

Essential oil is typically produced using a steam distillation method. In this study, different extraction
methods were used to extract essential oil from unfermented cinnamon bark and the results are shown
in Table 1. Extraction of cinnamon oil using the steam distillation method produces a cinnamon oil yield
of 1.17%, which is lower than previously reported cinnamon oil yield of 3.2% (dry weight) [9]. This
difference can be due to the smaller particle size of the cinnamon bark used in the previous study.
Smaller particle sizes will have a larger surface area so that the diffusion rate is higher and consequently
lead to a higher yield [25]. From Table 1, it can be observed that cinnamon oil yield of the
hydrodistillation method (1.37%, dry weight) is higher than the steam distillation method. This is
because in the hydrodistillation method, the substrate was immersed in water and consequently has a
better contact with the solvent as compared to the steam distillation method. It has been reported that
increasing the contact time between the substrate and the solvent will increase the yield [26].

Table 1 Cinnamon oil yield for diffrent extraction methods

Method Yield (% dry weight)
Steam distillation 1.17 ± 0.22
Hydrodistillation 1.37 ± 0.31
Maceration 0.94 ± 0.35
Soxhlet 1.96 ± 0.13

A lower cinnamon oil yield 0.94% (dry weight) was obtained from the maceration method. Two– stage
maceration with ethanol as a solvent may further increased the cinnamon oil yield as reported in

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another study [13]. Hoewever, the use of ethanol as a solvent may extact other non-volatile ompounds
together with the volatile compounds, thereby reducing the quality of the extracted oil [21].Cinnamon
oil extracted by the Soxhlet extraction method using n-hexane as the solvent produced a higher yield
than the distillation method. The results resemble the findings in previous studies that extraction of
cinnamon oil using Soxhlet extraction produces a higher yield as compared to the steam distillation
method [1,6]. As such is due to the much greater solubility of cinnamon oil in n-hexane as compared to
water [24].

3.2 Effect of Fermentation on Lignocellulose Content of Cinnamon Bark and Cinnamon Oil Yield
The effect of solid-state fermentation of cinnamon bark with Aspergillus awamori on lignocellulose
content of cinnamon bark and cinnamon oil yield are shown in Figure 1-2. From Figure 1, it can be
observed that thelignocellulosic contentof the cinnamon bark shows a decreasing profule with
increasing fermentation time. As such demonstrates that the Aspergillus awamori able to degrade
lignocellulose in the cinnamon bark into simpler compounds. Initially, the lignin content in the
unfermented cinnamon bark was 51.14% gradually decreased to 39.95% after 9 days of fermentation.
The highest decrease of lignin was observed between day 3 and 6, most probably due to the presence of
laccase enzyme secreted by Aspergillus awamori. that typically reaches it highest activity after
fermentation for 6 days [27,28].

Prior to fermentation, hemicellulose content in the cinnamon bark was 27.83%. The value gradually
dereased to 16.55% after fermentation for 9 days with the highest decreased occurred between day 3
and day 6. As such is most probably due to the presence of xylanase enzyme secreted by Aspergillus
awamori that typically reaches it highest activity after fermentation for 5 days [29,30]. The reduction in
hemicellulose content was greater than that of other lignocellulosic compounds. This happened because
Aspergillus awamori is a soft rot fungus that can attack carbohydrates in wood more effectively by
forming holes in the secondary cell walls and causing erosion of the entire secondary cell wall [31].In
contrast to ligin and hemicellulose, cellulose content in the cinnamon bark only slightly decreased from
15.37% to 13.20% after fermentation for 3 days and became stagnant at 12.37-12.67% after
fermentation for 9 days wnich may be due to the limited amount of of cellulose degrading enzyme
secreted by Aspergillus awamori during the fermentation process [32,33].

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60
Cellulose
Hemicellulose
50 Lignin
Lignocellulose fraction(%)

40

30

20

10

0
-1 0 1 2 3 4 5 6 7 8 9 10
Fermentation time (days)

Figure 1 Effect of fermentation time by Aspergillus awamori on lignocellulose content in cinnamon bark

Figure 2 shows that the yield of cinnamon oil continues to increase along with an increasing
fermentation time for all extraction methods, reaching a maximum yield of 3.01%, 2.09%, and 2.47% dry
weight after 9 days of fermentation for extraction of cinnamon oil using Soxhlet, hydrodistillation, and
maceration, respectively. As such indicates that solid-state fermentation of the cinnamon bark with
Aspergillus awamori able to degrade the lignocellulosic components of the cell wall and facilitate better
mass transfer for the extraction of cinnamon oil [34].A higher cinnamon oil yield obtained by the Soxhlet
extraction may be due to the reflux of solvent casusing the solvent not to be saturated with the
dissolved material. Unsaturated solvents can extract more dissolved material because there is a larger
concentration gradient that can increase the mass transfer rate between the solvent and the dissolved
material [35]. Figure 2 also shows that the maceration method produces a higher yield than the
hydrodistillation method. As such may be due to the use of non-polar organic solvent particularly n-
hexane. Cinnamon oil is non-polar so its solubility in n-hexane is higher than in water [36].

4.0

3.5
Yield (% dry weight)

3.0

2.5

2.0

1.5

1.0
Hydrodistillation
Maceration
0.5
Soxhlet
0.0
-1 0 1 2 3 4 5 6 7 8 9 10
Fermentation time (days)

Figure2 Effect of fermentation with Aspergillus awamori on cinnamon oil yield for different extraction
methods

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3.3 Characterization of Cinnamon Oil

Relevant properties of cinnamon oil were characterized and compared with the Indonesian
NastionalStandard (SNI) and the results are shown in Table 2. The color and aroma of cinnamon oil
obtained in this study are already in accordance with the SNI 06-3734-2006 however the density is
slightly larger. The cinnameldehyde content also satifies a minimum requirement of 50%. Table 3
presents the effect of fermentation of cinnamon bark with Aspergillus awamori on the cinnamaldehyde
content in cinnamon oil extracted using different methods. In general, the cinnamaldehyde content
varies for different extraction methods and tend to decrease upon fermentation. Nevertheless, the
cinnamaldehyde content still lies in the range 42.23-96.01% as reported in previous studies
[1,37,38].The lower cinnamaldahydecontent for fermented samples could have been caused by the
presence of other compounds that are also extracted due to the degradation of the lignocellulosic
compounds in the sample causing more compounds to be extracted. The number of identified
compounds also varies with an increasing fermentation time as shown in Table 3. As such because the
composition of essential oil is highly influenced by various factors including internal and external factors
that can cause the composition of cinnamon oil to vary even though the substrate of cinnamon comes
from the same source [39].

Table 2 Physical dan chemical properties of cinnamon oil

Property Experiment Result SNI 06-3734-2006
Color Dark yellow Pale yellow
Aroma Cinnamon Cinnamon
Density (g/mL) 1.032-1.063 1.008-1.030
Cinnamaldehyde content 53.63-93.19% Minimuml 50%
(%)

From Table 3, it can also be observed that cinnamon oil extracted via the hydrodistillation method
contains more ketones and carboxylic acidswhereras cinnamon oil extracted via the Soxhlet method
contains more alcoholic compounds. Meanwhile, cinnamon oil extracted via the maceration method
contains more sesquiterpene compounds. These differencesmay be caused by the different solvent used
in the respective methods. Carboxylic acids and ketones are are easily soluble in water, hence they can
be extracted well using the hydrodistillation method. The sesquiterpene compoundsare practically
insoluble in water and consequentlymore available when extracted using n-hexane via the maceration
and Soxhlet extraction.

Table 3 Effect of fermentation with Aspergillus awamori on the composition of cinnamon oil for
different extraction methods

Fermentation time (day)

Compound 0 3 6 9
1
HD S2 M 3
HD 1
S 2
M 3
HD 1
S2 M 3
HD 1
S2 M3
Cinnamaldeh 80, 93, 73, 60, 74, 68, 53, 73, 63, 76, 79, 73,

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yde 73 19 74 78 11 75 63 38 27 05 68 5
trans- 33, 4,8 30, 18,
Cinnamic acid n.d n.d n.d 19 n.d 9 48 n.d n.d 64 n.d n.d
Benzaldehyde 0,5 1,9 1,3 4,6 1,8 1,1
6 n.d n.d 5 n.d 7 2 n.d 2 1 n.d n.d
3-
Phenylprop- 15, 16, 0,1 1,6
2-enoic acid 44 n.d n.d n.d n.d n.d n.d n.d 32 9 2 n.d
Benzenacetal 0,9 1,5 1,2 0,8
dehyde 0,6 n.d n.d 1 n.d n.d 7 n.d 5 1 n.d n.d
Acetophenon 0,5
e n.d n.d n.d n.d n.d n.d 1 n.d n.d n.d n.d n.d
3- 1,1
Phenylfuran n.d n.d n.d n.d n.d n.d 1 n.d n.d n.d n.d n.d
Chalcone 0,2
n.d n.d n.d n.d n.d n.d 3 n.d n.d n.d n.d n.d
1,4-diphenyl-
1,4- 2,6
Butanedione n.d n.d n.d n.d n.d n.d 9 n.d n.d n.d n.d n.d
α-Cubebene 0,5
n.d n.d n.d n.d n.d n.d n.d n.d n.d n.d n.d 5
δ-Cadinene 0,3
n.d n.d n.d n.d n.d n.d n.d n.d n.d n.d n.d 8
Cinnamaldeh
yde dimethyl 21, 20, 12, 24, 5,4 13, 23,
acetal n.d n.d 6 n.d 94 81 n.d 95 8 n.d 59 0
Caryophyllen 0,1 0,2 0,2
e oxide n.d n.d n.d n.d n.d n.d n.d 1 n.d n.d 2 5
Benzaldehyd
e dimethyl 3,1 3,2
acetate n.d n.d 2 n.d n.d 3,6 n.d n.d 7 n.d n.d n.d
Benzeneprop
anol n.d n.d n.d n.d 0,5 n.d n.d n.d n.d n.d n.d n.d
3-Phenyl-2- 0,3
propen-1-ol n.d n.d n.d n.d 7 n.d n.d n.d n.d n.d n.d n.d
α -Terpineol n.d n.d n.d n.d n.d n.d n.d 0,2 n.d n.d n.d n.d
Others 2,6 6,8 1,5 3,1 4,0 8,5 5,1 1,3 8,5 4,8 2,3
7 1 4 7 8 8 6 6 9 3,2 9 2
1 2 3
Note: Hydrodistillation Soxhlet; Masceration; n.d : not detected

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3.4 Estimation of Cinnamon Oil using a Mathematical Model

Extraction of cinnamon oilis highly influenced by the diffusion rate caused by a concentration gradient.
In this study, thediffusion rate constant and diffusion coeffiecient for different extraction methods were
determined using Fick's Second Law and the results are shown in Table 4. The diffusion rate constant
varies from 9 x 10-6 s-1to 1.49 x 10-4 s-1 whereas the diffusion coefficient varies from 1.42 x 10-12m2s-1to
2.26 x 10-11m2s-1. The results show that the diffusivity rate of the hydrodistillation and Soxhlet methods
are greater than the maceration method. This could have been caused by the application of heat for the
hydrodistillation and Soxhlet methods, while the maceration method was operated at room
temperature. In general, the rate of diffusion is influenced by the movement of molecules. Hence,
application of heat will increase the movement of the molecules, thus increasing the diffusion rate
[40].The diffusion rate constant and diffusion coefficient can be used to develop a model to estimate the
cinnamon oil yield and the results are shown in Figure 3. The figure illustrates that at any time greater
than 0, the model can predict the cinnamon oil yield reasonably well for hydrodistillation, Soxhlet and
maceration.

Table 4 Diffusion rate constant and diffusion coeficientfor extraction of cinnamon oil using different
methods
Method Diffusion rate constant (s-1) Diffusion coefficient (m2s-1)
Hydrodistillation 1.49 x 10-4 2.36 x 10-11
Maceration 9.00 x 10-6 1.42 x 10-12
Soxhlet 9.15 x 10-5 1.44 x 10-11

Extraction time for maceration (hours)

0 6 12 18 24 30
3.5
Hydrodistillation
(Data)
3.0
Hydrodistillation
2.5 (Model)
Yield (% dry weight)

Soxhlet
2.0 (Data)
Soxhlet
1.5 (Model)

1.0 Maceration
(Data)
0.5 Maceration
(Model)
0.0
0 1 2 3 4 5
Extraction time for hydrodistillation and soxhlet (hours)

Figure 3 Comparison of experimental and modelled cinnamon oil yield over time

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Conclusion
Solid-state fermentation of cinnamon bark using Aspergillus awamori able to decrease the lignocellulose
content and increased the cinnamon oil yield. The biggest decrease of cellulose, hemicellulose, and
lignin occurred after 9 days of fermentation: 12.37%, 16.55%, and 39.95%, respectively. The yield of
cinnamon oil after 9 days of fermentation using the hydrodistillation, maceration and Soxhlet methods
were 2.09%, 2.47%, and 3.01%, respectively. The cinnamon oil primarily composed of cinnamaldehyde,
and the concentration varies with fermentation time and extraction methods. A mathematical model
has been successfully to determine the diffusion coefficient of cinnamon oil during the extraction
process and can be used predict the cinnamon oil yield. The results indicate that a higher diffusion
coefficient of 2.36 x 10-11 m2/s was obtained for the hdyrodistillation method, followed by Soxhlet (1.44
x 10-11 m2/s) and maceration (1.42 x 10-12 m2/s). The mathematical model also can predict the cinnamon
oil yield for all extraction methods reasonably well.

Acknowledgement
The authors would like to thank the Central Tea Plantation and Kina Gambung for providing the
cinnamon bark necessary for this research. The authors would also like to thank PPM KK ATB-ITB for
financing this study.

References

[1] Wong, Y. C., Ahmad-Mudzaqqir, M. Y., & Wan-Nurdiyana, W. A., 2014,"Extraction of essential oil
from cinnamon (Cinnamomum zeylanicum), “Oriental journal of chemistry.,30(1), 37-47.
[2] Chen, P., Sun, J., & Ford, P., 2014,“Differentiation of the four major species of cinnamons (C.
burmannii, C. verum, C. cassia, and C. loureiroi) using a flow injection mass spectrometric (FIMS)
fingerprinting method, “Journal of agricultural and food chemistry., 62(12), pp. 2516-2521.
[3] Ferry, Y., 2013, “Prospekpengembangankayumanis (Cinnamomum burmannii L) di Indonesia,
“BalaiPenelitianTanamanIndustri dan Penyegar. Sukabumi.
[4] Food and Agriculture Organization. 2019. FAOSTAT. Retrieved on 31 October 2021 from
http://www.fao.org/faostat/en/
[5] Dirjenbun., 2008, “Kebijakan Pembangunan Komoditi Kayu Manis,“Seminar AgribisnisKayumanis
Nasional 27/03 di Auditorium Deptan, Jakarta. DirektoratJenderal Perkebunan
DepartemenPertanian
[6] Paranagama, P. A., Wimalasena, S., Jayatilake, G. S., Jayawardena, A. L.Senanayake, U. M., &
Mubarak, A. M., 2001, “A comparison of essential oil constituents of bark, leaf, root and fruit of
cinnamon (Cinnamomum zeylanicum Blum) grown in Sri Lanka,“Journal of the National Science
Foundation of Sri Lanka., 29(3&4), pp. 147-153
[7] Rao, V. P., & Pandey, D., 2007, “Extraction of essential oil and its applications, “Biotechnology
thesis., National Institute of TechnologyRourkela., Rourkela, India.
[8] Haddi, K., Faroni, L. R., & Oliveira, E. E., 2017, “Cinnamon oil, “Green Pesticides Handbook: Essential
Oils for Pest Control., pp. 118-150.
[9] Fajar, A., Ammar, G. A., Hamzah, M., Manurung, R., & Abduh, M. Y., 2019, “Effect of tree age on the
yield, productivity, and chemical composition of essential oil from Cinnamomum burmannii,

1586
Nat. Volatiles & Essent. Oils, 2021; 8(6): 1575-1588

“Current Research on Biosciences and Biotechnology., 1(1), pp. 17-22

[10]Younis, A., Mehdi, A., & Riaz, A., 2011, “Supercritical carbon dioxide extraction and gas
chromatography analysis of Jasminum sambac essential oil,“Pakistan Journal of Botany., 43, pp.163-
168.
[11]Jeyaratnam, N., Nour, A. H., Kanthasamy, R., Nour, A. H., Yuvaraj, A. R., &Akindoyo, J. O., 2016,”
Essential oil from Cinnamomum cassia bark through hydrodistillation and advanced microwave
assisted hydrodistillation,”Industrial Crops and Products., 92, pp. 57-66.
[12]Geng, S., Cui, Z., Huang, X., Chen, Y., Xu, D., &Xiong, P., 2011, “Variations in essential oil yield and
composition during Cinnamomum cassia bark growth, “Industrial Crops and Products., 33(1), pp.
248-252.
[13]Setyowati, F. P., Utami, R., Khasanah, L. U., &Manuhara, G. J., 2018,” Optimization of two-stage
cinnamon bark (Cinnamomum burmanii) oleoresin maceration extraction process with ethanol
solvent using response surface methodology (RSM),”AIP Conference Proceedings., 2014(1), 20072,
pp. 1- 8
[14]Baydar, H., Schulz, H., Krüger, H., Erbas, S., &Kineci, S., 2008, “Influences of fermentation time,
hydro-distillation time and fractions on essential oil composition of Damask Rose (Rosa damascena
Mill.), “Journal of Essential Oil Bearing Plants., 11(3), pp. 224-232.
[15]Campbell, N., Reece, J., & Mitchell, L., 2005, “A tour of the cell, “Biology., pp. 1-1390.
[16]Rahardjo, Y. S., Weber, F. J., Le Comte, E. P., Tramper, J., &Rinzema, A.,2002, “Contribution of aerial
hyphae of Aspergillus oryzae to respiration in a model solid‐state fermentation system,
“Biotechnology and Bioengineering., 78(5), pp. 539-544.
[17]Su, Y., Yu, X., Sun, Y., Wang, G., Chen, H., & Chen, G. ,2018, “Evaluation of screened lignin-degrading
fungi for the biological pretreatment of corn stover, “Scientific reports., 8(1), pp. 1-11.
[18]Katara, G., Hemvani, N., Chitnis, S., Chitnis, V., &Chitnis, D. S., 2008, “Surface disinfection by
exposure to germicidal UV light, “Indian journal of medical microbiology., 26(3), 241-242.
[19]Sautour, M., Dantigny, P., Guilhem, M. C., &Bensoussan, M., 2003, “Influence of inoculum
preparation on the growth of Penicillium chrysogenum,“Journal of applied microbiology., 95(5),
pp.1034-1038.
[20]Mayhati, A., Patong, R., Djide, M. N., &Taba, D., 2013, “Biodegradation of lignin from corn cob by
using a mixture of Phanerochaetechrysosporium, Lentinus edodes and
Pleurotusostreatus,“International Journal of Scientific & Technology Research., 11, pp. 79-82.
[21]Geng, S., Zhou, W., Yuan, Q., Cai, D., & Zeng, Y., 2011,” EEG non-linear feature extraction using
correlation dimension and Hurst exponent,” Neurological research., 33(9), pp. 908-912.
[22]Cassel, E., Vargas, R. M. F., Martinez, N., Lorenzo, D., &Dellacassa, E., 2009, “Steam distillation
modeling for essential oil extraction process, “Industrial crops and products., 29(1), pp. 171-176.
[23]Katiyar, R., 2017, “Modeling and simulation of Mentha arvensis L. essential oil extraction by water-
steam distillation process, “International Research Journal of Engineering and Technology., 4(6), pp.
2793-2798.
[24]Chan, C. H., Yusoff, R., &Ngoh, G. C., 2014, “Modeling and kinetics study of conventional and
assisted batch solvent extraction, “Chemical engineering research and design, 92(6),pp. 1169-1186.
[25]Jahongir, H., Miansong, Z., Amankeldi, I., Yu, Z., &Changheng, L., 2019, “The influence of particle size
on supercritical extraction of dog rose (Rosa canina) seed oil,“ Journal of King Saud University-

1587
Nat. Volatiles & Essent. Oils, 2021; 8(6): 1575-1588

Engineering Sciences., 31(2), pp.140-143.

[26]Paibon, W., Yimnoi, C. A., Tembab, N., Boonlue, W., Jampachaisri, K., Nuengchamnong, N.,
&Ingkaninan, K., 2011, “Comparison and evaluation of volatile oils from three different extraction
methods for some Thai fragrant flowers, “International journal of cosmetic science., 33(2), pp. 150-
156
[27]Stoilova, I., Krastanov, A., & Bui, H., 2008, “Biodegradation of mixed phenolic compounds by a
microbial association of Aspergillus awamori and Thermoascusaurantiacus,“ Electron. J. Environ.
Agric. Food Chem., 7, pp. 2625-2633.
[28]El Monssef, R. A. A., Hassan, E. A., & Ramadan, E. M., 2016, “Production of laccase enzyme for their
potential application to decolorize fungal pigments on aging paper and parchment, “Annals of
Agricultural Sciences., 61(1), pp. 145-154.
[29]Umsza-Guez, M. A., Díaz, A. B., Ory, I. D., Blandino, A., Gomes, E., & Caro, I., 2011, “Xylanase
production by Aspergillus awamori under solid state fermentation conditions on tomato pomace,
“Brazilian Journal of Microbiology., 42(4), pp. 1585-1597.
[30]Ajijolakewu, A. K., Leh, C. P., Abdullah, W. N. W., & Lee, C.. 2017, “Optimization of production
conditions for xylanase production by newly isolated strain Aspergillus niger through solid state
fermentation of oil palm EFB, “Biocatalysis and AgriculturalBiotechnology, 11, pp. 239-247.
[31]Eaton, R. A., & Hale, M. D., 1993, “Wood: decay, pests and protection, “Chapman and Hall Ltd.
[32]Muhammad, B. A. O. A. A., &Okiki, P. A., 2016, “Cellulase Production by Fungi Isolated from
OdoAremuDumpsite in Ado-Ekiti, Nigeria“Advances in Life Science and Technology., 46, pp.46-51.
[33]Malherbe, S., & Cloete, T. E., 2002, “Lignocellulose biodegradation: fundamentals and application,
“Reviews in Environmental Science and Biotechnology., 1(2), pp. 105-114
[34]Chávez-González, M. L., López-López, L. I., Rodríguez-Herrera, R., Contreras-Esquivel, J. C., & Aguilar,
C. N., 2016, “Enzyme-assisted extraction of citrus essential oil, “Chemical Papers., 70(4), pp. 412-
417.
[35]De Castro, M. L., &Garcıa-Ayuso, L. E., 1998, “Soxhlet extraction of solid materials: an outdated
technique with a promising innovative future, “Analyticachimica acta., 369(1-2), pp. 1-10.
[36]Patel, P. N., Patel, K. M., Chaudhary, D. S., Parmar, K. G., Patel, H. A.,Kansagra, C. D., & Sen, D. J.,
2011, “Extraction of herbal aroma oils from solid surface, “International Journal of Comprehensive
Pharmacy., 9(2), pp. 1-10.
[37]Suryani, E., Nurmansyah, N. F. N., Purwiyanti, S., &Rostiana, O., 2018, “The Growth, Productivity and
Quality of Fifteen Accessions of Ceylon Cinnamon at Medium Elevation of Solok, West Sumatera,
“BuletinPenelitianTanamanRempah dan Obat., 28(2), pp. 105-112.
[38]Parthasarathy, V., Chempakam, B., & Zachariah, T., 2008, “Chemistry of spices, “Wallingford, UK:
CABI Pub
[39]Moghaddam, M., &Mehdizadeh, L., 2017,” Chemistry of Essential Oils and Factors InfluencingTheir
Constituents,” Soft Chemistry and Food Fermentation., pp. 379–419.
[40]Jones, H. G., 2013, “Plants and microclimate: a quantitative approach to environmental plant
physiology, “Cambridge university press

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