Journal of Food Engineering 296 (2021) 110437

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Journal of Food Engineering

journal homepage: http://www.elsevier.com/locate/jfoodeng

Intensified DES mediated ultrasound extraction of tannic acid from

onion peel
N.F. Sukor, V. Panner Selvam, R. Jusoh *, N.S. Kamarudin, S. Abd Rahim
Faculty of Chemical and Process Engineering Technology, College of Engineering Technology, Universiti Malaysia Pahang, Gambang, Kuantan, Pahang, 26300, Malaysia

A R T I C L E I N F O A B S T R A C T

Keywords: Ultrasound–assisted extraction using deep eutectic solvent (DES) was performed to extract tannic acid from
Deep eutectic solvent onion peel. Notably, DES is an excellent extraction agent, which yielded 641.16 ± 0.01 μg/g of tannic acid
Ultrasound–assisted extraction compared to the extraction using a conventional solvent (368.99 ± 0.02 μg/g). Subsequently, the research was
Tannic acid
conducted based on several exploited parameters and achieved the highest extraction yield (1705.79 ± 0.01 μg/
Onion peel
Antioxidant analysis
g) at the DES ratio of 1:1 (mass ratio of choline chloride to urea), solid to solvent ratio of 1:10 and duty cycle of
Kinetics 10%. The onion sample exhibited higher antioxidant capacity than standard ascorbic acid, which was expressed
in the lower values of the half-maximal inhibitory concentration (IC50) at 7.70 ± 1.12 and 10.14 ± 0.11 mg/ml,
respectively. Moreover, the Fick’s model successfully forecasted that diffusivity is the controlling factor in the
extraction of tannic acid via the DES mediated ultrasound–assisted extraction method.

1. Introduction 2016). In addition, a previous study by Galo et al. (2020) successfully

Onion (Allium cepa L.) is a versatile vegetable from the Liliaceae
family that is appreciated worldwide, not only for its taste but also as a
valuable source due to its functional properties of various phenolic
compounds in every part of the onion. Global onion production was
estimated at 400,000 tonnes harvested from 2.40 million ha of land area
(Sagar et al., 2020). On top of that, Munir et al. (2018) previously re­
ported increased of onion production of more than 25% over the past
decade and this consequently increased the production of the waste. It is
reported that more than 550,000 tonnes of onion waste are produced
annually, mainly generated by human consumption and food processing
industries (Gosi Ruivo de Silva et al., 2020).
Fortunately, researchers have been aware of the strategy of using
waste as a rich source of natural extracts. Some studies have highlighted
that the tannins from onion peel may be considered as a good source in
various applications. Hydrolysed tannin has particularly received much
interest as the major polyphenol compound dominating the onion peel
(Nnaji et al., 2013; Verma et al., 2018), including gallic acid, tannic acid,
vanillic acid, ferulic acid and epigallocatechin (Burri et al., 2017). The
presence of tannin compounds located primarily in the peel also
demonstrated satisfactory results in biological effects, including anti­
oxidant, antimicrobial and enzyme inhibitory activities (Eldin Hussein
Elgailani and Yacoub Ishak, 2016; Fuentes et al., 2020; Patra et al.,
determined 59.29% of tannic acid from the onion peel. However, to use
onion peel by products as a source that inhibits oxidation, suitable
extraction methods must be developed to reduce time, cost and envi­
ronmental pollution.
Ultrasound–assisted extraction is considered as an outstanding
alternative to conventional methods, as it is equipped with ultrasound
energy that focuses on the tip of a probe. The corresponding energy
conveys acoustic cavitation to disrupt plant tissues, break down cell
membrane and reduce mass transfer limitations (Sukor et al., 2019). The
extraction method has also been recognised as an important approach in
reducing extraction time, extraction temperature, energy input, con­
sumption of organic solvents, and eventually enhancing the chemical
kinetics, solubility and experimental reproducibility (Katsampa et al.,
2015). In the past few years, the extensive use of conventional organic
solvents such as chloroform, glycerol, hexane and ethyl acetate, has
restricted the implementation of green chemistry in the field of chemical
research. Owing to certain toxicity, volatility and non-degradability,
conventional organic solvents are not in line with the notion of green
chemistry (Gao et al., 2020). To overcome these drawbacks, deep
eutectic solvent (DES) has been evolving as a novel class of green sol­
vents. DES was introduced by Abbott et al. (2003) by mixing solid
quaternary ammonium salts and solid urea to produce eutectics that
were liquid at ambient temperature with unusual solvent properties.

* Corresponding author.
E-mail address: rohayu@ump.edu.my (R. Jusoh).

https://doi.org/10.1016/j.jfoodeng.2020.110437
Received 25 June 2020; Received in revised form 6 October 2020; Accepted 2 December 2020
Available online 5 December 2020
0260-8774/© 2020 Elsevier Ltd. All rights reserved.
N.F. Sukor et al.
DES has superior properties, such as low vapour pressure, high thermal
stability and tunable solubility (Kalhor and Ghandi, 2019), which
enabled DES to show extraordinary application values in various fields
(Barbieri et al., 2020; Oktaviyanti et al., 2019; Zhao et al., 2019) and has
received widespread attention in the extraction of various non-polar and
polar bioactive compounds from plant materials. The synergistic rela­
tionship between sonication and DES in facilitating the release of
phenolic compounds leads to an efficient mass transfer coefficient.
Several kinetic models have been postulated in search of the de­
pendency of the extraction process towards effective component diffu­
sion. In engineering, kinetic modelling provides valuable information on
extraction behaviour. Numerous extraction kinetics, such as rate law,
Peleg’s and Fick’s models, have been previously reported (Chiang et al.,
2017; Gomaa et al., 2018). Nevertheless, the data on the comprehensive
analysis between the kinetic models and the extraction by ultra­
sound–assisted extraction for onion peel extract are scarce.
Although there are previous findings on extracting phenolic com­
pounds via various methods, the study that emphasizes the extraction of
tannic acid from onion peel via ultrasound–assisted extraction with the
implementation of DES as a medium has never been reported so far. Past
studies utilised conventional organic solvents as the extraction media in
obtaining the target compounds. However, these solvents are harmful to
the environment and do not indicate research priorities for the devel­
opment of green chemistry technologies. Based on the discussion, in the
present study, a green and integrated strategy for enhanced tannic acid
extraction from onion peel was developed via DES mediated ultra­
sound–assisted extraction. The antioxidant activity was also studied to
examine the relationship between the optimum operating conditions.
Moreover, this study also aimed to evaluate several mathematical
models to find the controlling factor related to the extraction kinetics.
2. Materials and methods
2.1. Materials and chemicals
Fresh onion (Allium Cepa L.) peel was obtained from shops and res­
taurants. In the preparation of onion peel powder through extraction,
fresh onion peels were first cleaned, washed, and dried in an oven at
40 ◦ C until the peels were completely dried, achieving moisture content
at 0.1 kg water/kg dry onion peel. Then, the sample was pulverised in a
domestic blender until the sample turned into fine powder (0.50 mm)
before further use in extraction. Different extraction media were tested,
namely methanol (Sigma–Aldrich, Germany) and the DES obtained from
the mixing of choline chloride (Sigma–Aldrich, Germany) and urea
(Merck, Germany). Tannic acid (Merck, Germany) was used as a stan­
dard for the quatification of phenolic acids. Acetonitrile (Merck, Ger­
many) and orthophosphoric acids, 85% (Fisher Science, UK) were used
as the mobile phase for high performance liquid chromatography
(HPLC) analysis, whereas 2,2-diphenyl-1-picryl-hidrazil (DPPH) reagent
(Sigma–Aldrich, Germany) was used for scavenging analysis. All re­
agents and standards were purchased from Nano Life Quest Sdn. Bhd.
2.2. Preparation of deep eutectic solvent
Choline chloride is an economical and non-toxic quaternary ammo­
nium salt that is commonly utilised as a hydrogen bond acceptor (HBA),
which can form homogeneous and stable eutectic solvents with
hydrogen bond donors (HBDs), such as organic acids or polyalcohols.
The preparation of DES was adapted and modified from Isaifan and
Anhamed (2018), which consisted of a mixture of choline chloride and
urea at different ratios (1:2, 1:1 and 2:1). The DES ratio of 1:2 (choline
chloride:urea) was prepared by fixing a total amount of 25 ml of mixed
DES solution. The DES ratio of 1:2 (choline chloride:urea) representing
8.33 g of choline chloride and 16.67 g of urea was mixed, stirred and
heated at 80 ◦ C until a colourless liquid (a total of 25 ml) was formed.
Then, 75 ml of distilled water was mixed with previously prepared
2
Journal of Food Engineering 296 (2021) 110437
choline chloride:urea DES solution (Saha et al., 2019), until the mixture
became homogeneous before the extraction process. The DES/water
mixture (aqueous DES) has favourable physicochemical properties, such
as lower viscosity. Despite the high level of water mixed into DES so­
lution, the DES nanostructure is retained due to the solvophobic
sequestration of water into nanostructured domains around cholinium
cations (Alonso et al., 2016; Hammond et al., 2017). Moreover, the
choline–urea hydrogen bonding interaction (OH—NH2) will be
strengthened. Interestingly, the presence of water did not affect the yield
or selectivity of the process but reduced the viscosity of DES, hence
allowing an effective stirring of the reaction (Saha et al., 2019). Thus, it
can be assumed that the effect of water is insignificant to the extraction
performance of tannic acid. The preparation of other DES ratios followed
the same procedures, but the mass of choline chloride and urea was
varied based on the required ratios. For instance, the DES ratio of 1:1
was prepared by mixing 12.50 g of choline chloride and 12.50 g of urea,
whereas the 2:1 ratio consisted of 16.67 g of choline chloride and 8.22 g
of urea.
2.3. Ultrasound–assisted extraction
The experiment with ultrasound application was first carried out in
diluted DES at different DES ratios by fixing other parameters (i.e., solid
to solvent ratio of 1:10, duty cycle of 10%, 3 h of extraction time, 60 ◦ C
of extraction temperature). The extraction was conducted using a high-
intensity processor model Q700 (700 W, 20 kHz) from QSonica, New­
town, USA (Figure S1), with a replaceable flat-tip ultrasonic probe
(sonotrode). The probe of the ultrasound–assisted extraction equipment
was equipped with the amplitude setting to fix the temperature and
reflect the power level. During sonication, the amplitude was set to 13 to
obtain a fixed temperature of 60 ◦ C, reflecting power of 26 W and
sonication intensity of 20.47 W/cm2, whereas the cumulative average
ultrasound dose was varied by adjusting the duty cycle (Sukor et al.,
2019).
Duty cycle is the fraction of one period in which a signal or system is
active, commonly expressed as a percentage or ratio. A period is the time
required for a signal to complete an on-and-off cycle. In this context,
ultrasound–assisted extraction works in a pulsating mode. For example,
10% duty cycle represents a sonication period of 1 s, followed by the rest
period of 9 s. Meanwhile, 20% duty cycle represents sonicating period
for 2 s, followed by rest period of 8 s, while 30% duty cycle represents a
sonication period of 3s, followed by the rest period of 7 s. Throughout
the experiments, the solid to solvent ratio was examined at 1:8, 1:15 and
1:20, whereas the duty cycles was further studied at 20% and 30%.
2.4. Liquid chromatography quadrapole time–of–flight mass spectrometry
(LC-QTOF/MS) analysis
The phenolic compounds in the onion peel were identified using the
method of Tang et al. (2019) with some modifications. The identifica­
tion of the compounds was performed via Agilent 1200 Series (HPLC)
equipped with an Agilent 6520 Accurate-Mass quadrapole time-of-flight
liquid chromatography/mass spectrometry (Q-TOF LC/MS) using C18
column. Gradient elution was performed by varying the proportion of
solvent A (water/acetic acid at the ratio 98:2, v/v) to solvent B (aceto­
nitrile/water/acetic acid at the ratio 100:1:99, v/v/v), in the following
programme: 0–20 min, 10% B; 20–30 min, 25% B; 30–40 min, 35% B;
40–70 min, 40% B; 70–75 min, 55% B; 75–77 min, 80% B; 77–79 min,
100% B; 79–82 min, 100% B; 82–85 min, 10% B. Each sample was
filtered with a nylon syringe filter (pore size 0.22 μm) and subsequently
transferred into a 2 ml vial. The separation was achieved by fixing the
flow rate of 0.8 ml/min and the injection volume was set at 6 μl.
Mass spectra acquisition was performed in the m/z range of 50–1300
Da, drying gas (nitrogen) temperature of 300 ◦ C (flow rate: 5 L/min),
sheath gas temperature of 250 ◦ C (flow rate = 11 L/min), capillary
voltage of 3500 V, nebuliser gas pressure of 45 psi and nozzle voltage of
N.F. Sukor et al. Journal of Food Engineering 296 (2021) 110437

500 V. The identified compounds present in the samples from the (Kaderides et al., 2019). The basis for the model can be written as:
METLIN database with more than 30 library identification score were
dc
further selected for characterisation and m/z verification. = k(c − c∞ )2 (3)
dt

2.5. High performance liquid chromatography analysis where, k is the second-order extraction rate constant (g/μg.min), c∞ is
the extraction capacity (μg/g) and c is the concentration of sample
The identification of tannic acid from onion peel extract with DES as constituent in the solution (μg/g) at any time t (h). The integrated rate
solvent was performed according to Md Zain and Ya’akob (2019) with law can be obtained under the boundary conditions of t = 0 to t and c =
some modifications using a reversed–phase HPLC equipped with a 0 to c, as expressed below:
photodiode array (PDA) detector using C18 column via binary gradient
elution. Gradient elution was performed by varying the proportion of c2 kt
c= (4)
solvent A (100% acetonitrile, 10%) to solvent B (3.0% phosphoric acid, 1 + c∞ kt
90%) in an isocratic programme and pumped at a flow rate of 1 ml/min. Eq. (4) is reorganised in its linear form into:
The gradient started with 95% solution A and ended with 5% solution B.
c 1
The column temperature was maintained at 30 ◦ C, with the injection =( ) ( ) (5)
t
volume of 10 μl. The sample peaks were identified by comparing with 1
+ t
kc2∞ c∞
the standard solution of tannic acid at 280 nm (retention time = 4.40
min). A tannic acid standard curve was prepared at concentration
c/t in Eq. (5) signifies the initial extraction rate, which can also be
ranging from 10 to 60 ppm in ultrapure water (Figure S2). Each sample
denoted by h (μg/g.min). As defined by Eq. (6) when the extraction time,
and standard were filtered with a nylon syringe filter (pore size = 0.22
t approaches zero:
μm). The extraction yields were expressed as micrograms per grams of
sample (μg/g) and calculated as follows: h = kc2∞ (6)
(x)(DF)(V) In this study, k and c∞ can be obtained from the gradient and
ExtractionYield = (1)
(W) intercept values, respectively, by plotting a linear curve of c/t vs. 1/t and
the h values can be subsequently computed. Thus, the final equation
where x is the concentration of tannic acid (μg/L), DF is the dilution describing the concentration of the solute in the onion peel at any time
factor, V is the volume of DES (L) and W is the mass of the solid sample can be written as:
(g).
t
c=( ) ( ) (7)
2.6. Scanning electron microscopy 1
h
+ t
c∞

The cellular microstructure of onion peel sample particles before and

after extraction via different extraction methods was examined using a
scanning electron microscope (Quanta 450). Upon analysis, the samples
were coated with a thin layer of platinum at room temperature and the
images were obtained at 90 V with 3000 × magnification.
2.7. Antioxidant activity determination using DPPH radical scavenging
assay
This assay was produced according to the method of Oussaid et al.
(2017) with some modification. 2,2–diphenyl–1–picrylhydrazyl (DPPH)
was dissolved in methanol to the concentration (of 1 mM, 100 ml), using
39.4 mg of DPPH, forming a purple solution. This antioxidant compo­
nent can scavenge free radicals, thereby bleaching the purple colour
(colourless). Then, 1 ml of extract was added to 1 ml of DPPH meth­
anolic solution and allowed to stand in the dark for 30 min at room
temperature. After that, the absorbance was measured at 517 nm using a
ultraviolet–visible (UV–Vis) spectrophotometer. The free radical scav­
enging activity of the sample extract was determined based on the
equation as follows:
Acontrol − Asample
Scavengingrate(%) = x100%
Acontrol
where Asample is the absorbance of DPPH with a sample at 517 nm and
Acontrol refers to the absorbance of DPPH without the sample at 517 nm.
2.8. Experimental set–up for kinetic analysis
2.8.1. Rate law
Prominently, the second–order rate law is often employed in the
solid–liquid extraction modelling due to its compatibility in represent­
ing a process. These concentration-dependent kinetics were previously
utilised in examining the phenolic content from Hibiscus sabdariffa
calyces (Oluwaseun and Nour Hamid, 2019) and pomegranate peels
2.8.2. Peleg’s model
An established capacity-dependent kinetic of the Peleg’s model has
been extensively enforced to describe the extraction of polyphenols from
spent coffee grounds (Pettinato et al., 2019), stevioside from Stevia
rebaudiana (Rouhani, 2019), and phenolic acids from oak galls (Sukor
et al., 2019). The Peleg’s model equation is expressed as follows:
t
Ct = C0 + (8)
K1 + K2 t
where Ct signifies the concentration of the sample constituent in solution
at any time, t (μg/g), and K1 and K2 are the Peleg’s rate constant (min.g/
μg) and Peleg’s capacity constant (g/μg), respectively. Co is the primary
concentration of sample constituent, which is zero due to the use of a
fresh solvent. The Peleg’s model was modified as extraction typically
occurs in two stages; the first-order trend in the initial stage and the
zero-order trend in the later stage, as presented below:
t
Ct = (9)
K1 + K2 t
where the K1 and K2 values can be obtained from the slope and intercept
(2) of the 1/Ct vs 1/t graph, respectively. Moreover, the Ct value can be
further calculated using Eq. (9) at different time points to examine the
fitting of this model on the extraction of onion peel.
2.8.3. Fick’s model
According to the Fick’s second law of extraction kinetics, it is
assumed that the extraction occurs in two phase; a rapid phase known as
“washing” and a slow diffusion phase, where the concentration of solute
remains in effective diffusion and the external mass transfer resistance is
negligible. This excellent model has been used to perfectly discuss the
nature of the extraction of Glycyrrhiza (Wang et al., 2019), Chinese dark
tea (Cai et al., 2019), and Eucalyptus nitens and Eucalyptus globulus
(González et al., 2017). The model can be described as follows:

3
N.F. Sukor et al.
[( ) ( )]
c∞ − c 6 π 2 D1 t π 2 D2 t
= 2 f1 exp − + f exp − (10)
c∞ π r2
2
r2
where f1 and f2 represent the fractions of the solute, extracted from the
washing or fast and slow diffusion stages, respectively, along with the
diffusion coefficients, D1 and D2. C∞ is the concentration in equilibrium,
C is the concentration in time t and r is the particle radius.
The equation above was applied upon considering several estab­
lished conditions by Shafaei et al. (2016). In this study, the onion peel
sample powder was assumed to be spherical with 0.25 mm radius. In the
later stages of extraction, only the second term on the right-hand side of
Eq. (8) remained significant. The parameters of diffusion, D and fraction
[ ]
of solute, f can be obtained from the slope and the intercept of ln C∞C∞− C
vs. time graph, respectively.
2.9. Statistical analysis
The mean values and standard deviations of all replicates were
calculated using Microsoft Excel. The values were displayed as mean ±
standard deviation (SD) while P < 0.05 was considered statistically
significant. All determinations were measured in triplicate and the
confidence interval is represented by an error bar.
3. Results and discussion
3.1. Identification of phenolic compounds in the sample using LC–QTOF/
MS
A full–spectrum analysis of onion peel extract was performed using
LC–QTOF/MS as illustrated in Fig. 1. Meanwhile, Table 1 shows the
theoretical and observed m/z based on one plant sample for each
phenolic compound with mass errors within ±5 ppm. A total of 34
different phenolic compounds were identified in the onion peel extract
sample based on the records from the METLIN database, including 22
flavonoids, nine phenolic acids, one stilbenes and two polyphenols.
Phenolic compounds, namely, tellimagrandin, nobergenin, 3,4,5-O-tri­
caffeoyl-quinic acid, pedunculagin and tannic acid revealed higher
peaks, detected at the retention time of 0.47, 2.45, 16.54, 16.64 and
15.56 min, respectively. These compounds are a form of tannins, which
are widely found in the onion peel as previously reported by Burri et al.
(2017) and Rodrigues et al. (2017). Firstly, the LC–QTOF/MS analysis
was conducted in this study to confirm the availability of these tannin
compounds on MS basis. Upon the confirmation, HPLC analysis was
used, combined with a diode array detector (DAD) and the
Fig. 1. LC–QTOF/MS chromatogram showing main phenolic compounds in the onion peel extract.
4
Journal of Food Engineering 296 (2021) 110437
quantification by the UV spectrometry, and the results revealed that
tannic acid occupied the highest yield in the sample. Hence, tannic acid
quantification was highlighted in this study and further investigation on
several extraction parameters was conducted using HPLC to evaluate the
process intensification of the amount of extraction yield from the onion
peel.
3.2. Effect of different operating conditions
3.2.1. Effect of solvent
In this study, aqueous DES was used to extract tannic acid from onion
peel, and methanol was used for comparison purposes. Fig. 2A indicates
that DES yielded a higher amount of tannic acid at 641.16 ± 0.01 μg/g
compared to methanol at 368.88 ± 0.02 μg/g. An almost two-fold
greater extraction efficiency of DES-based extraction suggests that the
polyalcohol DES implemented in this study is easy to synthesise and
possesses low viscosity, hence offerring better ability to dissolve the
sample matrix and generate a higher yield (Shafie et al., 2019). Besides,
the polarity of DES is close to those of the target compounds in the onion
peel, which is in favour of extracting the target phenolics (Skarpalezos
and Detsi, 2019).
This is in agreement with a previous study by Barbieri et al. (2020) in
the extraction of rosemary (Rosmarinus officinalis L.), which obtained a
higher total phenolic compound using choline chloride derivative-based
DES with propanediol compared to ethanol at 62.21 mg/g and 49.14
mg/g, respectively. Another finding by Alanon et al. (2020) also
confirmed that choline chloride derivative–based DES was an excellent
solvent for the extraction of phenolic compounds from olive leaf.
Accordingly, DES was selected for further intensification of the extrac­
tion of onion peel extract.
3.2.2. Effect of DES choline chloride:urea ratio
As shown Fig. 2B, different DES ratios of choline chloride:urea at 1:1,
1:2 and 2:1 were applied in evaluating its reliance towards the extrac­
tion yield of tannic acid from the onion peel extract. The 1:1 ratio of
choline chloride:urea demonstrated a significant increase in the
extraction yield of 1705.79 ± 0.01 μg/g of tannic acid compared to the
ratios of 1:2 and 2:1 with the yields of tannic acid of 516.91 ± 0.02 and
422.15 ± 0.04 μg/g, respectively. The same type of DES with different
HBD/HBA ratios showed a great difference in extraction yield due to its
different viscosity, surface tension and polarity.
The increasing amount of HBA (choline chloride) ratio in DES might
increase the surface tension, whereas excess HBD (urea) may result in
stronger steric hindrance that weakens the interactions between the
target compounds and chloride anion (Gao et al., 2020). The appropriate
N.F. Sukor et al. Journal of Food Engineering 296 (2021) 110437

Table 1
Qualitative characterization of phenolic compounds in onion peel extract by LC–QTOF/MS.
Proposed compounds Molecular Mass error Retention time Molecular Theoretical (m/ Observed (m/ Mode of
formula (ppm) (min) weight z) z) ionization

Flavonoids
Pedunculagin C34H24O22 − 4.1 16.64 784.08 785.07 785.08 [M+H]+
Casuarictin C41H28O26 5.2 16.33 936.09 937.08 937.09 [M+H]+
Norbergenin C13H14O9 − 4.0 2.45 314.06 353.06 353.03 [M+K]+
1,2,3,4,6-Penta-O-galloyl-β-D- C41H32O26 − 1.4 16.53 940.12 963.13 963.11 [M+Na]+
glucopyranoside
Arecatannin B1 C45H38O18 − 0.6 16.61 866.21 867.21 867.21 [M+H]+
Laevigatin A C34H26O23 2.8 16.52 802.09 825.09 825.08 [M+Na]+
Phenolic acids
Corilagin 1 C27H22O18 5.4 16.64 634.08 657.08 657.07 [M+Na]+
6′ -O-Galloyl-homoarbutin C20H22O11 − 0.2 5.64 438.12 439.12 439.12 [M+H]+
3,4,5-O-Tricaffeoyl-quinic acid C34H30O15 − 0.9 16.54 678.16 679.13 679.17 [M+K]+
1,3,6-Trigalloyl-β-D-glucose C27H24O18 5.3 16.55 636.10 675.10 675.06 [M+K]+
1-O-Galloylpedun-culagin C41H28O26 5.2 16.55 936.09 937.09 937.10 [M+H]+
Polyphenols
Tellimagrandin II C41H30O26 3.0 0.47 938.10 961.11 961.10 [M+K]+
Stilbenes
4,4′ ,5,6-Tetrahydroxystilbene C14H12O4 − 9.1 16.34 244.07 245.07 245.08 [M+H]+

Fig. 2. Extraction yield of tannic acid under different (A) type of solvents and (B) DES ratio.

ratios of HBD/HBA should be carefully examined in reducing the vis­
cosity and surface tension of DES for accelerating the diffusion and mass
transfer of the reaction system, hence leading to a higher extraction
yield (Isaifan and Amhamed, 2018). Pal and Jadeja (2019) previously
discussed similar results for the extraction of onion peel-mediated DES
(choline chloride:urea) with varied ratios from 1:1 to 1:3, and the
highest total phenolic content of 222.97 mg/g was obtained (at the ratio
of 1:2) compared to other ratios of DES. Therefore, the DES ratio of 1:1
with suitable physio–chemical properties and polarity was selected for
the subsequent experiments.
3.2.3. Effect of solid to solvent ratio
The effect of solid-to-solvent ratio of 1:8, 1:10, 1:15 and 1:20 was
investigated, as demonstrated in Fig. 3A. The extraction yield increased
from 1001.15 ± 0.01 to 1705.79 ± 0.01 μg/g as the solid-to-solvent ratio
increased from 1:8 to 1:10. An increase in the DES volume fraction
positively influenced the extraction efficiency and the yield of tannic
acid that was maximised at 1:10. Nonetheless, with a further increase of
DES volume, the extraction yields insignificantly dropped to 1623.05 ±
0.03 and 1523.76 ± 0.02 μg/g at 1:15 and 1:20, respectively. The slight
decrease in the extraction yield beyond the critical ratio may be
attributed to the formation of liquid film at the interfacial surface of the
sample. These phenomena will hinder the mobility of solvent molecules
into the interior pores, promoting resistance to the diffusion mass
transfer of the solute particles (Anbalagan et al., 2019). This may be due
to the inadequate solvent concentration to extract from the substance
matrix. However, no significant difference was observed, the best con­
dition for the solid-to-solvent ratio is 1:10, which was used to study
another effect in enhancing the extraction yield of tannic acid.
A past study by Kankara et al. (2014) stated that 1:10 appeared to be
the best solid-to-solvent ratio using hot water extraction for extracting
phenolic antioxidants from Guirea senegalensis (Combratecae) leaves.
Another successful finding by Durdun et al. (2016) also suggested
solid-to-solvent ratio of 1:10 positively influenced the total phenolic and
flavonoid contents of the dried fruits of dog-rose, sea buckthorn and
hawthorn via ultrasound–assisted extraction using ethanol as a solvent.
3.2.4. Effect of duty cycle
The duty cycle of ultrasound–assisted extraction is another critical
parameter for an efficient extraction process that will maximise the

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N.F. Sukor et al. Journal of Food Engineering 296 (2021) 110437

Fig. 3. Extraction yield of tannic acid under different (A) solid to solvent ratio and (B) duty cycles.

amount of target compounds. The experimental results of the effect of
duty cycle ranging from 10% to 30% are presented in Fig. 3B. The 10%
duty cycle yielded the highest amount of tannic acid of 1705.79 ± 0.01
μg/g, compared to 20% and 30% duty cycles that obtained 935.37 ±
0.01 μg/g and 431.83 ± 0.01 μg/g of tannic acid, respectively. The in­
tensity level provided by the duty cycle adjuster creates ultrasonic
waves, which generate stable bubbles in the solvent through diffusion
(Mahindrakar and Rathod, 2020). The adequate intensity level at 10%
duty cycle facilitates the disruption of the plant cell wall of the onion
peel and consequently enhances the release rate of target components
from the sample matrix to the solvent. However, the higher intensity
supplied up to 20% and 30% duty cycle may damage the target phenolic
compounds, minimizing the amount of extraction yield (Sulaiman et al.,
2011).
Table 2 tabulates previous findings on the extraction of onion peel
and other plant sources for comparing the extraction methods, operating
conditions and extraction yields. Similar observations by Mohd Abdul
Alim et al. (2016) declared that 10% duty cycle appeared to be the ideal
condition to extract vitexin from Ficus deltoidea leaves. Moreover, Sukor
et al. (2019) also maintained 10% duty cycle in the entire process of
ultrasound–assisted extraction for extracting gallic acid and tannic acid
from oak galls. The extraction of phenolic compounds from the onion
peel has been done in the past studies; however no effort has been use
the greener solvent of DES as the extraction medium along with ultra­
sound–assisted extraction (Chia et al., 2019; de et al., 2017; Katsampa
et al., 2015). The onion peel was previously extracted either by using
conventional organic solvents (i.e., ethanol, glycerol) or water. In this
study, the optimum condition of ultrasound–assisted extraction for
onion peel was achieved under the utilisation of DES as the medium at
the DES ratio of 1:1, solid-to-solvent ratio of 1:10 and duty cycle of 10%.

Table 2
Table of comparison on the various extraction method, operating condition and extraction yield from several plants.
Source Active compounds Extraction method Operating condition Extraction References
yield
Solvent Duty
cycle
(%)

Onion peel Tannic acid Ultrasound–assisted DES (Choline chloride:Urea) 10 1705.80 μg/g This study
extraction
Oak galls Gallic acid (GA) and tannic Ultrasound–assisted Ionic liquid, 1-Butyl-3-methylimidazolium bis 10 497.34 mg/g [6]
acid (TA) extraction (trifluoromethylsulfonyl)imide, [Bmim][Tf2N] (GA)
2430.48 mg/g
(TA)
Mulberry Phenolic compounds Microwave assisted DES (Choline chloride:Glycerol) N/A 8.35 mg/g [8]
(Morus alba extraction
L.)
Quercus Gallic acid (GA) and tannic Ultrasound–assisted Hexadecyltrimethylammonium bromide, CTAB 40 2155.77 mg/ [18]
infectoria acid (TA) extraction kg (GA)
galls 15236.83 mg/
kg (TA)
Ficus deltoidei Vitexin Ultrasound–assisted Water 10 0.74% w/w [41]
leaves extraction
Red onion skin Phenolic compound Aqueous extraction 80% ethanol N/A 757.38 mg/g [42]
Onion solid Polyphenols and pigments Ultrasonic bath Glycerol N/A 490 μmol/g [43]
wastes
Onion peel Bisindolylmenthanes Aqueous extraction Water N/A 90% [44]
Waste onion Quercetin Aqueous extraction DES (Choline chloride:Urea) N/A 2.80 mg/ml [45]
Ginger Gingerols Ultrasonic bath alcohol–based DES N/A 3.82 mg/g [67]
Ethanol (L–cartinine:1,3–butanediol)

6
N.F. Sukor et al. Journal of Food Engineering 296 (2021) 110437

3.3. Microscopic observation using SEM

At the desired operating condition, the scanning electron microscopy

(SEM) images of the outer surface of the onion peel powder sample were
captured and compared before and after extraction, as depicted in
Fig. 4A and B, respectively, at 3000 × magnification. From the micro­
scopic morphology, it is determined that the intensity of the cell wall
integrity depends on the sonication treatment. The obtained results
illustrated that the ultrasound–assisted extraction procedures damaged
cell tissues, as exemplified in Fig. 4B. Meanwhile, a smoother surface
could be observed on the exterior side in Fig. 4A (control). This profile
may support the previous results in attaining a high extraction yield of
tannic acid upon sonication. The damaged cell walls subsequently in­
crease the solvent penetration into the plant sample, thus encourages the
diffusivity of the target compounds from the onion peel matrix sample.
Fonteles et al. (2016) also previously claimed that sonication promotes
diffusivity as many bioactive compounds were obtained from cashew
apple bagasse puree.

3.4. Antioxidant analysis

The antioxidant activity of the onion peel extract was measured to

identify its ability to trap an unpaired electron of the DPPH radical,
which was expressed as the percentage of inhibition of DPPH in the
solution. In Fig. 5, it can be observed that the onion peel sample
exhibited better performance in scavenging the DPPH radical than the
standard ascorbic acid. The onion peel sample displayed 97.51 ± 1.12%
antioxidant activity compared to standard ascorbic acid (94.476 ±
0.11%). The highest scavenging activity is reflected by a smaller value of
the IC50, which indicates how much of a specific pharmacologic agent is
required to inhibit a given biological activity by half. The onion peel
sample extract exhibited a lower IC50 value at 7.70 ± 1.12 mg ascorbic
acid/ml than standard ascorbic acid (10.14 ± 0.11 mg ascorbic acid/
ml).
Tannic acid is a potent antioxidant that donates two hydrogen atoms
to DPPH radical, which transforms it into a quinone intermediate
(Ghatak and Iyyaswami, 2019). Apak et al. (2016) also declared that
tannic acid has the highest antioxidant capacity than other antioxidant
compounds. These statements supported the obtained results in this
study, which agreed that tannic acid possesses high antioxidant activity.
Also, Lee et al. (2014) reported a comparable result of the antioxidant
activity from the onion peel extract of 89.72%. A study by Razavi and
Fig. 5. Antioxidant activity of onion peel extract.
Kenari (2016) for the extraction of onion peel obtained 61.11%–84.68%
inhibition via various extraction methods.
3.5. Kinetic analysis
The results of experimental data, calculated data, coefficient of
determination (R2) and percentage error (%) at the optimum condition
of DES as a solvent, the DES ratio of 1:1, solid-to-solvent ratio of 1:10
and varied duty cycles (10%–30%) were analysed to evaluate different
kinetic models (rate law, Peleg’s model and Fick’s model) in explaining
the extraction nature of onion peel. R2 is a statistical measure that sig­
nifies the goodness-of-fit of a model, whereas the percentage error is the
difference between the experimental and calculated values, divided by
the calculated value and multiplied by 100%. The value of R2 near to 1

Fig. 4. SEM microscopic observation (magnitude 3000 × ) of onion peel surface (control), (B) after ultrasound–assisted extraction method.

7
N.F. Sukor et al.
and a small percentage error show a good correlation between the
experimental and calculated data. In this study, three kinetic models
were compared and evaluated in determining the best kinetic curve that
can best explain the extraction of onion peel.
3.5.1. Rate law
The model parameters of extraction rate constant, k1, initial extrac­
tion rate, h, R2 and percentage error were determined numerically using
the rate law nonlinear regression algorithm at different duty cycles, as
tabulated in Table 3. At the optimum extraction condition using DES as a
solvent, the DES ratio of 1:1 and solid-to-solvent ratio of 1:10, the duty
cycle of 10% recorded the highest k1 value at 6.36 ± 0.03 g/μg min and
subsequently dropped to 3.07 ± 0.06 and 1.70 ± 0.01 g/μg min at 20%
and 30% duty cycles, respectively. High k1 indicates a relatively faster
reaction in extracting the target compounds. The result shows a good
correlation between the optimum condition of 10% duty cycle, resulting
in the maximum yield with the highest k1 value compared to other duty
cycles (“The Rate Law: Concentration and Time | Boundless Chemistry,”
2020). A similar trend was observed on the initial extraction rate values
with the highest h of 26.32 ± 0.04 ( × 105) μg/g min for 10% duty cycle.
As the duty cycle was further intensified to 20% and 30%, the h value
abruptly reduced to 4.71 ± 0.01 ( × 105) and 1.09 ± 0.06 ( × 105) μg/g
min, respectively. Even though the rate law kinetics showed high R2,
values ranging from 0.95 ± 0.01 to 0.99 ± 0.01, the findings contra­
dicted with the high percentage errors between the experimental and
calculated values of 28.83 ± 0.03%, 33.37 ± 0.01% and 11.28 ± 0.01%
at the duty cycles of 10%, 20% and 30%, respectively.
Fig. 6A shows an imprecise fit of the experimental and calculated
data, hence explaining a disagreeable kinetic curve of the rate law model
of onion peel. Furthermore, the underestimation of the calculated
extraction yield and the high value of percentage error imply the in­
efficiency of this concentration-dependent kinetic model as proposed by
the rate law for the extraction of tannic acid from onion peel via DES
mediated ultrasound–assisted extraction. This is in accordance with
previous study by Chua et al. (2018), which argued that the rate law
could not justify the extraction of pectin from dragon fruit peels.
Another finding by Abugabr Elhag et al. (2019) also agreed with this
study that the kinetic modelling of rate law was less successful repre­
senting the extraction behaviour of proteins from the root extracts of
Tongkat Ali (Eurycoma apiculata).
3.5.2. Peleg’s model
Table 4 presents the Peleg’s model parameters, including the rate
constant, K1; capacity constant, K2; R2 and percentage error of the tannic
acid extraction yield from onion peel at various duty cycles. At the op­
timum extraction condition using DES as a solvent, the DES ratio of 1:1
and solid-to-solvent ratio of 1:10, the K1 values increased with elevated
duty cycle, which obtained 1.84 ± 0.07 ( × 10− 2), 3.87 ± 0.02 ( × 10− 2)
and 4.64 ± 0.02 ( × 10− 2) min g/μg for 10%, 20% and 30% duty cycles,
respectively. This gradually increasing pattern with elevated duty cycle
was also observed on the K2 values that attained 0.05 ± 0.05 ( × 10− 2)
g/μg at 10% duty cycles, followed by 0.07 ± 0.01 ( × 10− 2) and 0.21 ±
0.01 ( × 10− 2) g/μg for 20% and 30% duty cycles, respectively. Both K1
and K2 that refer to the rate of mass transfer and the maximum con­
centration of the desired compound during extraction, respectively, are
in concordance with a past study by Anbalagan et al. (2019), which
stated that lower values of K1 and K2 ascertained the accuracy of the
Table 3
The kinetic parameters of Rate law at different duty cycles [Extraction temperature 60 ◦ C; solvent DES; DES ratio 1:1; solid to solvent ratio 1:10].
Condition Experimental (μg/g) k1 (g/μg min)
Duty cycle (%) 10 1705.79 ± 0.02 3.07 ± 0.06
20 935.35 ± 0.03 6.36 ± 0.03
30 431.84 ± 0.03 1.70 ± 0.01
h (x105).
8
Journal of Food Engineering 296 (2021) 110437
Peleg’s model in describing the solid-liquid extraction of mangiferin
from Mangifera indica leaves.
The slope of the curve in Fig. 6B proposed a less scattered experi­
mental data than the previous rate law model; nevertheless, the tabu­
lated data of the high percentage error (1.41 ± 0.01% - 7.36 ± 0.02%)
seemed unfit to elucidate the extraction process. Although satisfactory
R2 between 0.88 ± 0.03 and 0.99 ± 0.01 were obtained at all duty cy­
cles, it is still insufficient to fully describe the nature of the extraction of
onion peel extract. This is in agreement with past findings by Segovia
et al. (2016) and Balyan and Sarkar (2017) which revealed that the
Peleg’s model could not justify the avocado and Syzygium cumini L. seed
extraction, respectively. Therefore, another kinetic model was further
established to adequately fit the experimental data with lower per­
centage error values.
3.5.3. Fick’s model
The diffusivity elements promoted by the Fick’s model are tabulated
in Table 5, comprising the diffusion coefficients, D1 and D2; fraction of
solutes, f1 and f2; R2; and percentage error between the experimental and
calculated data among different duty cycles. The extraction of onion
peel employed under 10% duty cycle (optimum extraction condition
using DES as a solvent, the DES ratio of 1:1 and solid-to-solvent ratio of
1:10) revealed 2.19 ± 0.01 ( × 10− 2) m2/min and 22.34 ± 0.01 ( × 10− 2)
m2/min of D1 and D2, respectively. A further increment in the duty cycle
intensity to 20% and 30% significantly produced lower diffusion co­
efficients of D1 and D2. As 10% duty cycle recorded the highest D1 and D2
coefficients, this finding suggests a rapid initial mass transfer from onion
peel extract. The acoustic cavitation from ultrasound–assisted extraction
provides sufficient disruption towards the plant tissues to easily diffuse
out tannic acid from the sample (Ghitescu et al., 2015; Rashed et al.,
2016). Nonetheless, prolonged and intense duty cycles up to 20% and
30% may eventually damage the plant cells, which leads to a slow
diffusion process.
Fig. 6C shows the precisely adjusted calculated data to the experi­
mental data curve corresponding to the diffusivity factor in explaining
the extraction process. This finding was further supported by the high,
R2 (>0.99 ± 0.05) and low percentage error values (<0.05) obtained at
all duty cycles. The difference between the calculated and experimental
values of the model is significant; therefore, it is suitable to consider the
Fick’s model as the prominent kinetics in describing this diffusion-
dependent extraction of onion peel extract. The applicability of this
model in explaining extraction behaviour was supported by other pre­
vious findings from Oluwaseun and Nour Hamid (2019), Louati et al.
(2019) and Setford et al. (2017) for extracting phenolic compounds from
Hibiscus sabdariffa calyces, Citrus sinensis L. and red grapes, respectively.
A perfectly fit curve of the Fick’s model obtained from previous studies,
and with high R2 (0.99) are the evidences that diffusivity magnitude is
the factor in controlling the process. Thus, it can be concluded that the
diffusivity factor is the core value in the extraction of tannic acid from
the onion peel via synergistic DES mediated ultrasound–assisted
extraction.
4. Conclusion
This study was carried out to determine the performance of the DES
mediated ultrasound–assisted extraction in extracting tannic acid from
onion peel. The extraction using DES significantly yielded higher tannic
h (μg/g min) Calculated (μg/g) R2 % Error
26.32 ± 0.04 1323.31 ± 0.06 0.99 ± 0.01 28.83 ± 0.03
4.71 ± 0.01 701.30 ± 0.06 0.95 ± 0.01 33.37 ± 0.01
1.09 ± 0.06 388.06 ± 0.02 0.99 ± 0.01 11.28 ± 0.01
N.F. Sukor et al. Journal of Food Engineering 296 (2021) 110437

Fig. 6. Extraction kinetics of (A) Rate law, (B) Peleg’s model and (C) Fick’s model at different duty cycles.

Table 4
The kinetic parameters of Peleg’s model at different duty cycles [Extraction temperature 60 ◦ C; solvent DES; DES ratio 1:1; solid to solvent ratio 1:10].
Condition Experimental (μg/g) K1 (min g/μg) K2 (g/μg) Calculated (μg/g) R2 % Error

Duty cycle (%) 10 1705.79 ± 0.02 1.84 ± 0.07 0.05 ± 0.05 1840.49 ± 0.02 0.98 ± 0.03 7.36 ± 0.02
20 935.35 ± 0.03 4.64 ± 0.02 0.07 ± 0.01 922.37 ± 0.01 0.99 ± 0.01 1.41 ± 0.01
30 431.84 ± 0.03 3.87 ± 0.02 0.21 ± 0.01 412.93 ± 0.04 0.88 ± 0.03 4.57 ± 0.01

K1 (x10− 2); K2 (x10− 2).

Table 5
The kinetic parameters of Fick’s model at different duty cycles [Extraction temperature 60 ◦ C; solvent DES; DES ratio 1:1; solid to solvent ratio 1:10].
Condition Experimental (μg/g) D1 (m2/min) D2 (m2/min) f1 f2 Calculated (μg/g) R2 % Error

Duty cycle (%) 10 1705.79 ± 0.02 2.19 ± 0.01 22.34 ± 0.01 30.77 ± 0.06 1746.43 ± 0.03 1705.80 ± 0.02 0.99 ± 0.05 <0.05
20 935.35 ± 0.03 1.97 ± 0.06 23.01 ± 0.01 3.93 ± 0.01 1716.73 ± 0.03 935.36 ± 0.03 0.99 ± 0.05 <0.05
30 431.84 ± 0.03 0.27 ± 0.02 0.32 ± 0.01 0.56 ± 0.01 4.33 ± 0.002 431.85 ± 0.03 0.99 ± 0.05 <0.05

D1 (x10− 2); D2 (x10− 2); f1 (x10− 2); f2 (x10− 2).

9
N.F. Sukor et al.
acid (641.16 ± 0.01 μg/g) than methanol (368.99 ± 0.02 μg/g).
Moreover, the extraction intensification process successfully verified
that the DES ratio of 1:1, solid-to-solvent ratio of 1:10 and duty cycle of
10% attained the maximum amount of extraction yield (1705.79 ± 0.01
μg/g). Meanwhile, microscopic analysis using SEM confirmed that suf­
ficient intensity from sonication positively contributed in extracting the
phenolic compounds from the sample. Besides, the onion peel extract
reflected a very strong antioxidant activity at 97.51 ± 1.12% compared
to standard ascorbic acid. Additionally, diffusivity perfectly explained
the behaviour of the tannic acid extraction from onion peel, as claimed
by the Fick’s model. In conclusion, this DES mediated ultra­
sound–assisted extraction may contribute to the future development of
extraction technology.
CRediT author statement
Nuramira Fateha Sukor: Conceptualization, Methodology, Valida­
tion, Writing–Review & Editing, Vinnoth Panner Selvam: Wri­
ting–Original Draft, Investigation, Resources. Rohayu Jusoh:
Supervision. Nur Syahirah Kamarudin: Formal analysis, Software.
Syarifah Abd. Rahim: Funding acquisition, Supervision.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgement
The authors are grateful for the support from Jabatan Pertanian
Negeri and the internal university grant by Universiti Malaysia Pahang
(Grant No. RDU180353 and RDU190182).
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.jfoodeng.2020.110437.
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