Ultrasonics - Sonochemistry 68 (2020) 105180

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Ultrasonics - Sonochemistry
journal homepage: www.elsevier.com/locate/ultson

Ultrasound-assisted extraction of phytocompounds from dragon fruit peel: T

Optimization, kinetics and thermodynamic studies
G.V.S. Bhagya Raja, Kshirod K. Dasha,b,
⁎

a
Department of Food Engineering and Technology, Tezpur University, Tezpur, Assam 784028, India
b
Department of Food Processing Technology, GKCIET, Malda, West Bengal 732141, India

ARTICLE INFO ABSTRACT

Keywords: Ultrasound-assisted extraction method (UAE) was applied to recover phytocompounds from dragon fruit peel
Antioxidant activity and the process was modelled and optimized using the combination of artificial neural network (ANN) and
Betacyanin genetic algorithm (GA). The influence of ultrasonic temperature (30–70 °C), solvent to solid ratio
Genetic algorithm (10:1–30:1 mL/g), solvent concentration (30–60%), and ultrasonic treatment time (5–25 min) on total poly-
Artificial neural network
phenolic content (ZT ), antioxidant activity (ZD ) and betacyanin content (ZB ) was investigated. The ANN model
successfully fitted to the experimental data and the output of ANN model was applied for genetic algorithm
optimization. The optimal UAE conditions were obtained at ultrasonic temperature of 60 °C, solvent to solid ratio
25:1 mL/g, solvent concentration 60%, and ultrasonic treatment time of 20 min. The extraction kinetics and
thermodynamic study for phytochemical compounds extracted from dragon fruit peel using UAE process was
carried out at different combinations of temperature and time of extraction. The effective diffusion coefficient for
total polyphenol content, antioxidant activity and betacyanin content were ranged from
2.99 × 10 11 to 4.84 × 10 11m2/s , 1.89 × 10 11 to 4.51 × 10 11 m2/s and 2.55 × 10 11 to 5.40 × 10 11 m2/s respec-
tively and the corresponding mass transfer coefficient were varied between 2.00 × 10 06 2.81 × 10 06 m/s ,
1.53 × 10 06 2.66 × 10 06 m/s and 1.81 × 10 06 3.05 × 10 06 m/s respectively. The obtained information on
effective diffusivity and mass transfer coefficient during extraction would allow the prediction of extraction rate
and for estimation of operation conditions for industrial implementation.

1. Introduction
Dragon fruit identified as pitaya, is one of the tropical fruits, a
member of cactus family, Cactaceae, belongs to genus Hylocereus [1].
Dragon fruits are edible fruits with sweet taste and rich in bioactive
compounds, helps in boosting the human immunity system, and im-
proves physical and mental abilities of individuals [2]. The fruit is
having very high economical value as it comprises glucose, betalains,
proteins, vitamins, different organic acids, soluble dietary fiber, phyto
albumins and minerals like potassium, magnesium and calcium, [3–5].
Dragon fruit species have been classified based on the color of flesh and
the peel, Hylocereus undatus variety has white flesh with pink skin
known as white dragon fruit, flesh of Hylocereus polyrhizus was red in
color with pink skin know n as red pitaya and Hylocereus megalanthus
with white pulp and yellow skin known as yellow pitaya [6,7]. The
peels of dragon fruits (Hylocereus undatus) have the attractive color due
to the water soluble nitrogen comprising pigment betacyanin, and the
chemical compounds in peels are potent inhibitor of cancer cell growth
[8–10]. The major by-product of dragon fruit obtained either by fresh
consumption or processing of fruit is the peel of the fruit, generally
dumped into eco system which leads to environment degradation and
wastage of bioactive compounds present in the peels [11,12]. The peels
of Hylocereus undatus can be utilized in the production of pectin, ex-
traction of phenolic compounds and pigments.
There are many types functions of phyto-chemicals in fruits and
vegetables, and one of these is the phenolic compounds. Phenolic
mixtures are vital in providing anti-oxidant activity among the phyto-
chemicals. Hylocereus undatus are rich in phytocompounds that assist to
prevent deadly diseases such as arthritis, arteriosclerosis, colon cancer,
heart diseases, inflammation, brain dysfunction, and diabetes and
known to regulate the cholesterol level and blood pressure of the body
[13,14]. Betacyanins is among the betalain pigments that imparts red-
violet colour in the peels of dragon fruit. Studies revealed that beta-
cyanins are three times stronger than the red-purple-blue dye produced
by anthocyanins [15]. Sample preparation and extraction techniques
are crucial steps in isolation, identification of phytocompounds in plant

⁎
Corresponding author at: Department of Food Engineering and Technology, Tezpur University, Tezpur, Assam 784028, India.
E-mail address: kshirod@tezu.ernet.in (K.K. Dash).

https://doi.org/10.1016/j.ultsonch.2020.105180
Received 23 March 2020; Received in revised form 5 May 2020; Accepted 17 May 2020
Available online 21 May 2020
1350-4177/ © 2020 Elsevier B.V. All rights reserved.
G.V.S. Bhagya Raj and K.K. Dash
materials and the study of antioxidant activity along with their usage in
food products [16]. Mostly extraction process implemented in food
industries involve the blend of chemical solvent and high temperature
[17]. Usage of high temperatures could affect heat liable bioactive
compounds present in the plant materials and lot of solvent is required
to get maximum extraction of the targeted compound. Among the dif-
ferent extraction methods, UAE is a versatile, cheaper technique and
mostly preferred by many researchers due to its ability of high re-
producibility in shorter time, faster rate of heat and mass transfer, and
low instrumental requirements resulting in enhanced quality of pro-
duct. Additionally, the process had reduced solvent consumption that
favour the use of generally recognized as safe solvents and lower energy
input with higher efficiency for extraction of the target species at
shorter time [18–21]. UAE is based on the principle of cavitation that
includes acoustic cavitation and hydrodynamic cavitation phenomena.
The cavitation phenomenon consists of recurrence of three steps such as
creation, expansion and impulsive collapse of microbubbles which
improves the solvent accessibility of the solid particles [22–25]. Cavi-
tation also causes disruption of cell walls and bring changes in internal
structure of the plant cell and intensifies the mass transfer rates
[26–28]. UAE was a promising method to extract wide range of
bioactive compounds from fruits. UAE was used by many researchers
for extraction of polyphenols from different fruits like olive fruit [29];
cabernet franc [30]; grape seeds [31]; mulberry pulp [32]; Pouteria
campechiana pulp [33]. A number of factors that affect the extraction
can be operated to optimize the process of extraction using ultrasound
such as ultrasonic extraction time, concentration of the solvent, solvent
to solid ratio, ultrasound frequency, ultrasound power and ultrasonic
temperature.
Artificial neural network (ANN) is a computational and mathema-
tical modelling method that has been broadly and effectively applied in
many fields to predict response based on the data trained in the ex-
perimental range and has the ability to study the influence of input
neurons (variables) on investigated outputs through generalization and
predictive modelling [34]. ANN acquire information similar to that of
human brain by learning, analysis, association and adaptation, and is
emulated based on inspiration from the biological brain [35–37]. ANNs
has emerged as alternate technique for modelling and optimization of
non-linear problems and is considered as a powerful tool for modelling
of several biochemical processes because of its adaptivity, general-
ization, model independence, and ability in the flexible fitting of in-
vestigated data with higher accuracy [38–40].
The key objective of extraction process is to maximize yield of
specified component with high purification without affecting the
properties of component to be extracted. Therefore, a novel and green
extraction method was established to improve the efficiency of ex-
tracting bioactive compounds from dragon fruit peel. The study of ki-
netics and thermodynamics of the UAE process is essential for the basic
understanding of the nature of the process and for assessment of its
industrial applicability. Based on this, the objective of this study is to
model and optimize the process parameters of ultrasound assisted ex-
traction process for extraction of phytochemical compounds from
dragon fruit peel (DFP). Additionally, the mass transfer kinetics, ef-
fective diffusivity and thermodynamics of extraction of phyto-
compounds during UAE process was studied.
2. Material and methods
2.1. Sample preparation
Dragon fruits (Hylocereus undatus) were thoroughly cleaned and
peeled in a dirt-free environment to separate peel from pulp. The peels
of dragon fruit were dried in a freeze dryer (Lyolab Freeze Lab,
Lyophilization Systems Inc., USA). Finally, dried peels were ground into
fine powder, passed through 0.25 mm mesh screen, packed in poly-
ethylene bags and stored at 4 °C for further analysis.
2
Ultrasonics - Sonochemistry 68 (2020) 105180
2.2. Ultrasonic assisted extraction (UAE) of DFP
An ultrasonic homogenizer with probe (U500, Takashi, Japan) was
used to perform the extraction of phytocompounds from DFP powder at
a fixed power of 100 W. Ethanol was selected as solvent for the ex-
traction of phytocompounds with varying temperature from 30 to 70 °C
within a maximum error of ± 1 °C. The influence of solvent on the
process of extraction was studied by considering different concentra-
tions of ethanol varying from 30 to 60% and different ratios of solvent
to solid ratio varying from 10:1 to 30:1. Time of extraction (5–25 min)
was considered to study the effect of process parameters on extraction
as well as to evaluate the extraction kinetics and thermodynamic study.
The freeze-dried dragon peel powder was kept in a beaker along with
the solvent and the temperature of the fluid (water) around the beaker
was maintained by means of thermostat control.
2.3. Artificial neural network modelling
ANN consists of simple neurons that operates in parallel. A multi-
layer perceptron (MLP) based on series of feed-forward-type network
models with back-propagation and training algorithm was developed
for modelling of ultrasonic assisted extraction of DFP under different
process conditions. Feed forward neural networks was mostly applied
due to its convenience for function approximation. The established
ANN model was constructed with three layers namely input, a hidden
and an output as illustrated in Fig. 1 and each layers consist of several
neurons. The independent and depend variables of UAE of DFP are the
neurons for input and output layers of the proposed ANN model. For
developing the ANN model, the data of both input and output layer
were coded. The input layer of ANN model had four neurons denoted by
nx = 4 , which are most prevailing elements governing the ultrasound
assisted extraction process and represented the previous independent
variables of CCD design, viz. ultrasonic temperature ( XUT ) in °C, solvent
to solid ratio ( XSr ) in mL/g, ethanol concentration ( XSc ) in % and ul-
trasonic treatment time (XUt ) in min. The output layer had three neu-
rons (nz = 3) that represented the fitness of the output neurons and
consisted of total phenolic content (ZT ) in mg of GAE/g of dry weight,
antioxidant activity (ZD ) in % DPPH and betacyanin content (ZB ) in
mg/ g dry wet basis. The input data set ( XUT , XSr , XSc andXUt ) were
coded between −1 and +1 and the output data (ZT , ZA and ZB ) were
coded between 0 and +1. The ANN analysis included one hidden layer
in between the input and output layers as it is effective for most of the
problems and over-fitting can occur with more hidden layers in the
network [41]. The number of neurons in the hidden layer were eval-
uated based on the number of neurons in the input and output layer.
The process of UAE of DFP was designed using central composite
design (CCD) with 4 independent variables XUT , XSr , XSc and XUt with
real and coded values ( xUT , xSr , xSc and xUt ) are represented in
Table 1, resulted in 30 experiments with various combinations. One
data set can be used at a time among ‘n’ sets of input-output data, to
obtain the corresponding output data. Therefore, a single input dataset
was represented by a row matrix ‘x’ of sizes "nx × 1" (4 × 1) and single
output data series was represented by a row matrix ‘z’ of size
"nz × 1"(3 × 1). Out of total 30 experimental data set, 70% of the ex-
perimental data was chosen for training, 15% for testing and 15% data
was used for validation. The training procedure, using the Levenberg-
Marquardt algorithm, was composed of following three steps: (i) feed-
forward of the input training pattern, (ii) calculation and back propa-
gation of the associated error, and (iii) the adjustment of the calculated
weights. The critical point for the development of a neural network is
the learning procedure. ANN training is an optimization process in
which an error function is minimized by adjusting the ANN weights.
When an input training data set was introduced to the ANN, an output
was evaluated based on the input data. This network output was
compared with the actual output (target) provided by the user. The
difference between the computed output vector and the target vector
G.V.S. Bhagya Raj and K.K. Dash Ultrasonics - Sonochemistry 68 (2020) 105180

Fig. 1. The architecture of ANN model used for modelling of Ultrasound Assisted extraction of Dragon fruit peel.

Table 1 network and they are produced by technique of random number gen-
Evaluated factors, factor notation, and their levels in CCD design. eration. Weights are assigned to neurons between two layers input-
Independent Variables Notation of Levels
hidden (wij ), hidden-output (wjk ) layer and bias values for each hidden
Factor (Tj ) and output (Tk ) layer. The size of these parameters wij , wjk , Tj and Tk
−2 −1 0 +1 +2 is represented by nx × nh = 4 × 11, nh × ny = 11 × 3, nh × 1 = 11 × 1
and 1 × nh = 1 × 11 respectively. Forward and backward calculations
Ultrasonic Temperature (°C) XUT 30 40 50 60 70
were executed repeatedly on all data pairs obtained at input and output
Solvent-Solid ratio (ml/g) XSr 10:1 15:1 20:1 25:1 30:1
Solvent Concentration (%) XSc 30 40 50 60 70 layers for a specific number of times in a cycles. The new weights and
Time (min) XUt 5 10 15 20 25 the threshold values of the network were updated by calculation be-
tween input and output data pairs using the Eqs. (5)–(8).

was used to determine the weights using an optimization procedure in wijnew = x ' × L × e'j + wij (7)
order to minimize the individual sum of squares of the errors.
The calculated output values of neurons presented in both the
wjknew = L × y × e'k + w (8)
hidden and output layer were represented as y and z respectively and
were evaluated using Eqs. (1) and (2).
where L known as the learning rate, value lie in between 0.6 and 0.9.
1 For the determination of new parameter values of network L of value
y=
1 + exp[ (wij' × x ' + T)]
j (1) 0.6 was chosen.
During this process the weights and bias are updated continuously
1 through the process of training, with aim at the determination of the
z=
1 + exp[ (wjk' × y + Tk)] (2) structure and the final parameters of the network. This process was
repeated until the lowest relative deviation is acquired between pre-
where wij is the weight between input and hidden layer, x is the input
dicted values of output neurons and experimental values. The network
values, y is the output value of hidden layer, z is the output values of
established by this process can be able to predict the dependent vari-
output layer Tj is the bias value at hidden layer, wjk is the weight be-
able.
tween hidden and output layer, and Tk is the bias value at output layer.
The relative effect of input parameter on the output parameter is
The errors of back propagation at hidden and output layer were
calculated using Eqs. (9)–(12).
used to update the values of network parameters and are represented by
ej and ek respectively. The computed value of error ek and ej was cal- ( z ) xUT = (z )+1,0,0,0 (z ) 1,0,0,0 (9)
culated using Eqs. (3) and (4)

e k = (y ' z) × z × (1 z) (3) ( z ) xSr = (z ) 0, +1,0,0 (z )0, 1,0,0 (10)

e j = y × (1 y) × (wjk × e k) (4) ( z ) xSc = (z ) 0,0, +1,0 (z ) 0,0, 1,0 (11)

The bias value at the layer Tjnew was determined using the Eq. (5)
and at output layer Tknew is calculated using the Eq. (6).
Tjnew = L × ej + Tj
Tknew = L × e k + Tk
In back propagation method the error calculated at the output layer
by the help of input layer and hidden layer, is reverse transmitted to the
hidden layer and reaches input layer to update the connection weights.
Weights and the threshold values (bias) are the parameters of the
( z ) xUt = (z ) 0,0,0+ 1 (z ) 0,0,0, 1 (12)
(5) where ( z ) xUT is the computed coded output values of response at ul-
(6) trasonic temperature; ( z ) xSr is the computed coded output values of
response at solvent solid ratio; ( z ) xSc is the computed coded output
values of response at solvent concentration; ( z ) xUt is the computed
coded output values of response at ultrasonic time; (z )+1,0,0,0 represents
coded response calculated at xUT of level +1 and the rest of three in-
dependent variables (xSr , xSc and xUt ) at level 0.

3
G.V.S. Bhagya Raj and K.K. Dash Ultrasonics - Sonochemistry 68 (2020) 105180

2.4. Genetic algorithm (GA) 2.7. Determination of betacyanin content

Artificial Neural Networks (ANN) integrated with Genetic ZB of DFP was determined by means of McIlvaine buffer method
Algorithms (GA) was implemented to optimize the multi-objectives of described by Wong (2015) [44]. Buffer was prepared by mixing 30 mL
materials. Genetic algorithms are direct search algorithms that derive of 0.1 M citric acid with 70 mL of 0.2 M sodium phosphate dibasic. A
their behaviour from the principles of biological evolution in natural sample volume of 0.1 mL was added to 3.9 mL of McIlvaine buffer and
genetic system and are used to solve complicated optimization pro- the absorbance was measured at 537 nm using UV–vis Spectro-
blems. GA solutions are based on ‘survival of the fittest’ strategy, where photometer. McIlvaine buffer of 4.0 mL was used for blank and ZB of
in general biological process individuals that better fit the environment DFP was calculated using Eq. (15).
have high chances of extant and send their chromosomes to their off- A × F × MW
spring, compared to individuals with poor fitness that may extinct. Betacyanin content (ZB) = × 1000
(15)
×l
These algorithms maintain and manipulate a population of solutions by
means of selection, reproduction, crossover, and mutation for the op- where A = absorption value at 537 nm, F = dilution factor,
timization process. In the current process, the fitness function was de- MW = betacyanin molecular weight (550 g/mol), = molar extinction
veloped on maximization of all the output neurons i.e., total phenolic coefficient of betacyanin (60,000 L/mol cm), l = path length of the
content (ZT ), antioxidant activity (ZD ) and betacytin content (ZB ) and cuvette (1 cm).
hence the developed fitness function was presented as
F = ZT + ZD + ZB . 2.8. Kinetic modelling of ZT , ZD and ZB extracted from DFP using UAE
New individual was produced by crossover step and mutation step
and element value of every chromosomes was modified according to the The extraction kinetics for DFP extracted by UAE process was in-
mutation probability, which helps in providing new information into vestigated according to pseudo second-order model for extraction of the
the population. This cycle was continued until very low values of the different phytocompounds (ZT , ZD and ZB ). This model is evident in
sum of square of the error between the mean and individual fitness studying extraction kinetics of flavonoids extracted from Terminalia
values were accomplished. The cycle was continued after the mutation bellerica by microwave assisted extraction method [45], glycyrrhizic
and if the desired solution was not achieved, again the obtained po- acid extraction using UAE from licorice root [46], and antioxidants
pulation was used for the reproduction, crossover, and mutation in the from pomegranate marc [47],
next cycle. The extraction rate of phytochemical from DFP was determined
using kinetic model presented in Eq. (16).
2.5. Quantification of total phenolic content dCt
= k (Cs Ct ) 2
dt (16)
Folin–Ciocalteu (FC) reagent and spectrophotometric method was where Ct is the concentration of phytochemical compound in the liquid
used for quantification of ZT extracted from DFP [42]. Galic acid was extract at a given time t , Cs is the saturation concentration of phyto-
selected as a standard equivalent (in mg/g) and ZT was expressed in chemical compound in the liquid extraction and k is the pseudo second
terms of gallic acid equivalent (GAE). 0.5 mL of ethanolic DFP extract order rate constant.
was combined with 10% FC reagent and mixed with 2.5 mL of 7.5% Boundary conditions: Ct = 0 at t = 0 ; Ct = Ct at t = t
NaHCO3. The mixture was incubated for a time of 45 min and the blank The pseudo second-order model presented in Eq. (16) can be
was prepared without the peel extract. After the incubation the absor- transformed into the Eq. (17) under the above mentioned the boundary
bance was recorded at max = 765 nm using spectrophotometer. Each conditions.
experiment was conducted in triplicate for determination of ZT and the
mean absorbance data was recoded. For the standard solution of gallic Cs2 kt
Ct =
acid same procedure was repeated, the calibration line was construed 1 + Cs kt (17)
and the ZT of DFP was calculated using Eq. (13). The Eq. (17) can be simplified into liner form represented in Eq.
c×V (18).
Total phenolic content (ZT ) =
w (13) t 1 t
= +
where c = concentration of gallic acid from standard curve, V = vo- Ct kCs2 Cs (18)
lume of DFP extract and w = Sample weight. t 1 t
= +
Ct h Cs (19)
2.6. Determination of antioxidant activity of DFP
where ‘h ’ is the initial extraction rate when t approaches 0, which is the
product of ‘k ’ and Cs2 .
Antioxidant activity of DFP was determined using DPPH radicals
The extraction rate constant (k ) was corelated with temperature by
scavenging method described by Alara (2018) [43]. In concise, DPPH
Arrhenius equation shown in Eq. (20)
crystalline solid quantity of 0.004 g was dissolved in analytical grade
ethanol (99.95% purity) of 100 mL, to prepare 0.1 mM DPPH solution Ea
k = k 0 exp
and kept at 4 °C. A quantity of 0.2 mL DFP extract was added to 2 mL of RT (20)
ethanol and 2 mL of DPPH solution. The solution left for 30 min at room
where Ea is activation energy, R is the gas constant (8.314 J mol 1 K 1).
temperature in a dark place for incubation. After the incubation, ab-
The Eq. (20) can be expressed in linear form as shown in Eq. (21)
sorbance was recorded at 517 nm using a UV–vis Spectrophotometer.
Ethanol was selected as blank and the ZD of DFP calculated by the Eq. ln(k ) = ln(k 0 )+
Ea 1
(14) R T (21)

Asample
% DPPH antioxident capacity (ZD)= 1 × 100 2.9. Determination of effective diffusion coefficient during extraction
Acontrol (14)

where Acontrol = mixture of ethanol and DPPH solution, Asample = solu- Fick’s second law was used to describe the effective diffusion coef-
tion containing DFP extract and DPPH solution. ficient of phytochemical compounds from DFP. Following assumptions

4
G.V.S. Bhagya Raj and K.K. Dash Ultrasonics - Sonochemistry 68 (2020) 105180

were assumed for studying UAE extraction method: (i) External re- saturation concentration of phytochemical content in the extract and Ct
sistance to mass transfer is considered to be negligible. (ii) The dried is the extractable phytochemical content of DFP at time t.
DFP particles were considered to be spherical in shape (iii) concentra-
tion differences was only relevant in radial direction. The average 2.11. Thermodynamics of UAE
diameter of dried DFP particles was found to be 0.064 mm.
The unsteady state mass transfer in the radial direction of a sphe- In the solid liquid extraction process, dispersion of the solute out of
rical particles with radius ‘r’ is presented in Eq. (22). the solid and into the liquid solvent was the main controlling phase of
C 2C 1 C extraction. Gibbs free energy compute the beneficial work available
= + from a thermodynamic system at a constant temperature and pressure
t r2 r r (22)
and in order to estimate Gibbs energies during the chemical changes the
On substituting u = Cr , Eq. (22) transforms to Eq. (23)
free energies of the distinct components of the extraction needs to be
u 2u identified. Standard free energy of formation can be estimated from the
=D 2
t r (23) standard enthalpy of formation and the standard entropy of the com-
pound as shown in Eq. (30).
Boundary conditions:
G° = H ° T S° (30)
u = 0, x = 0 and t > 0 (24.1)
The thermodynamic study of extraction of solute during extraction
u = aCS , x = r and t > 0 (24.2)
was studied through calculation of G°, H ° and S °. The Gibbs free
u = xf (x ), t = 0 and 0 < x < r (24.3) energy isotherm equation is presented in Eq. (31)

The spherical particles are initially at a uniform concentration Ci G° = RTlnK eq (31)

and the surface concentration is maintained constant at Cs , the solution
of Fick’s second law Eq. (23) with respect to the boundary conditions in Van’t Hoff equation represented in Eq. (32) was used to calculate
Eq. (24) can be presented in Eq. (25) H ° and S ° which was obtained by combining Eqs. (30) and (31).

Ct Ci 2r ( 1)n n x De n2 2t H° S°
lnK e = +
=1+ sin exp RT R (32)
Cs Ci x n= 1
n r r2 (25)
where ‘K e ’ is the equilibrium constant for extraction of the desired
The total quantity of diffusing material inflowing or outflowing the
component and known as the ratio of extracted quantity of phyto-
sphere is given by Eq. (26).
chemical to the remaining quantity of phytochemical unextracted,
Ct 6 1 De n2 2t presented in Eq. (33).
=1 2
exp
Cs n=1
n2 r2 (26) Zs
Ke =
where C is the phytochemical content in DFP (kg/m3 ), r is the radius of Zmax Zs (33)
DFP spherical particle (m ), De is the effective diffusion coefficient of where Zs is the phytochemical compound extracted after 25 min of
phytochemical compound and t is time (s ). ultrasonic extraction time at a temperature T (K) and Zmax is the phy-
The Fick’s second law equation for spherical particle Eq. (26) can be tochemical compound extracted after an exhaustive extraction using
transformed into the Eq. (27) solvent mixture containing ethanol and water.
Cs Ct 6 De 2t
Zr = = exp
Cs 2 r2 (27) 2.12. Statistical analysis

where Zr is the ratio between remained phytochemical content of DFP

Numerous statistical parameters, including the coefficient of de-
and the phytochemical content of DFP at time ‘t’ and saturation re-
termination (R2 ), root mean square error (RMSE), mean square error
spectively, Ct is the extractable phytochemical content of DFP at a
(MSE) and chi-square ( 2 ), were calculated using Eqs. (34)–(37) re-
particular time t, Cs referred as total phytochemical content extracted at
spectively. The ANN-GA model adequacies were validated by estima-
saturation. The effective diffusion coefficient was assessed from the
tion of the relative deviation percentage (R d ) using Eq. (38).
slopes the plot of parameter ‘Zr ’ against time for different process
temperatures. n
i=1
(Zpre Zexp)
R2 = 1 n
i=1
(Zm Zexp) (34)
2.10. Biot number
n
(Zpre Zexp)
The diffusion parameters during extraction was defined by using RMSE = i=1
n (35)
dimensionless Biot number to study the behaviour of mass transfer. The
Biot number is the ratio of internal and external diffusion resistance, n
1
which corelates the relative transport resistances for extraction of solid MSE = (Zpre Zexp ) 2
in liquid phase. The Biot number (Bi ) for extraction of solid–liquid n i=1 (36)
process was calculated from Eq. (28).
n
2 i=1
(Zpre Zexp ) 2
km Dp =
Bi = Zexp (37)
De (28)
where km is mass transfer coefficient (m/s ) and Dp is particle size (m ). 100 n |Zexp Z pre |
The value of ‘km ’ was calculated by Eq. (29) [45,48]. Rd =
n i=1 Zexp (38)
Cs k
ln = mt Where Zpre is the predicted value obtained from ANN, Zexp is the ob-
Cs Ct Lc (29)
served value, Zm is the average value, and n is the number of experi-
where Lc represents characteristic length of the sphere, Cs represents ments.

5
G.V.S. Bhagya Raj and K.K. Dash Ultrasonics - Sonochemistry 68 (2020) 105180

3. Results and discussions
3.1. ANN modelling of UAE of DFP
A feed-forward back propagation neural network with error algo-
rithm (BP-ANN) was used for the modelling of UAE of DFP. The BP-
ANN model was architectured with 3 layers containing 1 input layer
with 4 neurons, 1 hidden layer with 11 neurons (selected based on
lower MSE value) and 1 output layer with 3 neurons and the proposed
ANN topology is represented in Fig. 1. There are two elementary steps
in developing ANN model which include a training step and a testing/
validation step [49]. A central composite design resulted in 30 ex-
perimental data sets out of which 20 experimental data groups were
used for training, 5 data groups for validation and 5 data groups for
testing. The data set were chosen randomly for model fitting. The va-
lues of weights and bias were acquired by random number generation
using trial and error method after the 2000 computational cycles. The
matrix of wij and wjk represented the weights between the input layer
and hidden layer and hidden layer and output layer respectively. The
bias value at hidden layer and output layer is represented by Tj and Tk
respectively. After computational cycles the final matrices of wij with
size of 4 × 11, wjk with size 11 × 4, Tj of size 11 × 1 and Tk of size
1 × 3 was obtained and represented in Table 2. The resulted weights
and biases of the network were used for developing BP-ANN model,
which were again used in GA.
3.2. Influence of UAE process variables on total phenolic content of DFP
Under different combination of independent variables, the ZT of
DFP was varied in the range of 4.509–8.536 mg GAE/g dry weight.
Between the four independent variables, ultrasonic temperature
had highest effect followed by concentration of solvent, solvent to
solid ratio and ultrasonic treatment time (( zT ) xUT >
( zT ) xSc > ( zT ) xSr > ( zT ) xUt ). The ANN model showed that ultra-
sonic temperature had positive effect on the ZT yield(( zT ) xUT = 0.724 )
of DFP (Table 3), i.e. increase of the XUT increased the yield of ZT
(Figs. 2A–2D). Further, the influence of ultrasonic temperature on the
ZT yield was analysed by varying the temperature from 30 to 70 °C (30,
40, 50, 60, and 70 °C) at XSr of 20:1 mL/g and XSc of 50% for an ex-
traction duration of 15 min represented in Fig. 2A. When the ultrasonic
temperature was increased from 30 to 60 °C the yield of ZT was in-
creased from 5.199 to 6.111 mg GAE/g dry matter whereas extraction
at 70 °C caused deterioration of 5% in the yields of ZT . The improved
yield was due to increase in the mass transport at higher ultrasonic
temperature which may increase liquid phase pressure within the plant
cell membrane cause centrifugal flow allow the solute to break out from
cell [50]. Extraction at higher temperature leads to softening of the
plant tissue and weakens the cell wall integrity. This favours the
entrance of ethanol into the phenolic-matrix and increase the diffusivity
of ethanol (solvent) [51–53]. Because extraction at higher temperatures
oxidize the solubilized phenolic compounds and decrease the ZT yield
[54]. Additionally, temperature above 60 °C may cause decrease of
surface tension as well as solvent viscosity. Decrease of solvent viscosity
affects the solvent typical feature of mass transfer intensity during the
diffusion process. Similar trends of decrease in ZT yield was observed
after 54 °C during UAE extraction of rice bran [55].
The relative effect of solvent to solid ratio ( XSr ) on ZT yield was
represented as ( zT ) xSr , and the value calculated by ANN model was
found to be 0.470. The positive sign of ( zT ) xSr value indicated that XSr
had positive effect on ZT yield. The effectiveness of XSr on ZT yield from
DFP was assessed at five levels of solvent solid ratio: 10:1, 15:1, 20:1,
25:1 and 30:1 mL/g using XSc of 50% at XUT of 50 °C for 15 min of XUt .
ZT yield was improved significantly (p < 0.05) with increase of XSr
and presented in Fig. 2B. The value ZT yield was found to be 5.003 mg
GAE/g d.w. at 10:1 mL/g of XSr and at 30:1 mL/g of XSr the ZT yield
was increased by 24%. At higher XSc , concentration difference between
solute and solvent was high and hence the high driving force between
the material matrix and solvent caused better dissolution of phenolic
compounds. The extraction of phenolic compounds from Berberis asia-
tica fruits was conducted at different methanol concentrations
(20–80%), pH (3–8), temperatures (30–80 °C) and extraction time
(30–90 min) [56]. The results exhibited an increase in ZT with increase
of methanol solid ratio from 10:1 to 50:1. This concluded that increase
in solvent volume increased the ZT yield, due to effective dissolution of
phenolic compounds created better ZT yield.
The relative influence of XUt on the yield of ZT from DFP determined
by the ANN model was 0.132 and xUt has positive effect on ZT yield. To
analyse the influence of xUt on yield of ZT from DFP, extraction was
carried out at xUT of 50 °C in xSc of 50% with a xSr of 20:1 mL/g for
different XUt i.e. 5, 10, 15, 20, and 25 min. A sharp increase in ZT yield
from 5.063 to 5.760 mg GAE/g d.w was observed from 5 to 20 min of
XUt and afterwards a decrease of 3% in the yield of ZT was observed at
25 min of treatment (Fig. 2C). The results revealed that prolonged ul-
trasonic extraction time is not favourable for the extraction of plant
phenolic compounds. Higher extraction yields at initial stages can be
supported by Fick’s second law, which states that the rate of extraction
increases till equilibrium state was attained between the concentration
in the plant material (phytocompounds) and surrounding solvent
(ethanol) [57]. Decline in the yields of ZT beyond 20 min may be at-
tributed to reduced diffusion rates due to increase in the diffusion
distance and reduction of diffusion area with longer exposure time
[58]. Extensive exposure of phenolic compounds to sonication and ul-
trasonic temperature may also attribute to the degradation and struc-
tural devastation of phenolic compounds extracted from DFP and incite
the thermal degradation of the extracted phenolic compounds present
in the solvent. As reported in previous research, ZT yield was increased

Table 2
Parameters of BP-ANN model.
wij = 0.863 −3.324 −1.432 −1.090 0.638 3.116 1.090 3.946 4.344 −6.527 −2.067
4.593 0.331 −0.492 −1.148 1.412 1.563 −0.998 4.523 3.923 0.681 4.393
1.011 2.188 9.062 1.607 7.715 0.713 −1.646 3.127 −0.495 0.073 −1.639
1.559 1.224 −0.281 6.584 2.022 −4.639 3.267 2.813 2.812 0.962 −1.212

wjk= 3.171 0.446 −0.390 Tj= −2.451 Tk= −1.938

−4.455 −0.805 0.775 3.003 −4.579
4.691 −3.142 0.119 −1.384 −6.261
3.875 6.018 2.350 2.055
−2.866 3.901 0.269 −0.595
2.710 1.796 1.662 −1.098
1.997 −3.766 −0.324 −1.355
2.098 2.086 5.451 −6.131
0.308 2.014 3.340 2.821
−1.306 −6.415 1.594 −4.628
1.605 3.137 −3.347 −4.935

6
G.V.S. Bhagya Raj and K.K. Dash Ultrasonics - Sonochemistry 68 (2020) 105180

Table 3
Relative influence of the coded values of independent variables on the response total phenolic content, antioxidant activity and betacyanin content from Dragon fruit.
xUT xSr xSc xUt zT Rd zD Rd zB Rd

+1 0 0 0 ( zT ) xUT = 0.724 3.133 ( zD ) xUT = 0.967 3.759 ( zB ) xUT = 0.532 1.162

−1 0 0 0
0 +1 0 0 ( zT ) x Sr = 0.313 ( zD ) x Sr = 0.720 ( zB ) x Sr = 0.430
0 −1 0 0
0 0 +1 0 ( zT ) x Sc = 0.470 ( zD ) x Sc = 0.772 ( zB ) x Sc = 0.504
0 0 −1 0
0 0 0 +1 ( zT ) xUt = 0.132 ( zD ) xUt =0.838 ( zB ) xUt = 0.472
0 0 0 −1

Note: zT , zD and zB represents the coded values of the responses and xUT , xSr , xSc andxUt represents the coded values of independent variables.

initially with increase of time of extraction up to 20 min during ex-
traction of phenolic compounds from olive fruits using UAE treatment,
whereas prolonged treatment of ultrasound after 20 min declined the
yield of ZT [29].
The increase in solvent concentration (( zT ) xSc = 0.313) was po-
sitively associated with ZT yield extracted from DFP which was proved
by the magnitude of relative influence of XSc on ZT extraction showed
in Fig. 2D. The influence of XSc on the ZT yield from DFP during UAE
process was studied at XUT of 50 °C, for XUt of 20 min using solvent
solid concentration of 20:1 mL/g and varying the XSc from 30 to 70%
(30, 40, 50, 60 and 70%). The ZT yield at 30% of XSc was found to be
5.048 mg GAE/g d.w. and the yield was increased 18% with increase of
the XSc from 30 to 70%. The extraction of total monomeric anthocyanin
and ZT from eggplant peel was increased with increase in methanol
solution concentration from 50% to 70% [59].

Fig. 2A. Effect of ultrasonic temperature on total phenolic content (ZT ), antioxidant activity (ZD ) and betacyanin content (ZB ).

Fig. 2B. Effect of solvent solid ratio on total phenolic content (ZT ), antioxidant activity (ZD ) and betacyanin content (ZB ).

7
G.V.S. Bhagya Raj and K.K. Dash
Fig. 2C. Effect of ultrasonic treatment time on total phenolic content (ZT ), antioxidant activity (ZD ) and betacyanin content (ZB ).
3.3. Influence of UAE process variables on antioxidant activity of DFP
The ZD of DFP in terms of percentage DPPH at different experi-
mental conditions was varied in the range of 41.404–74.811%. Out of
all the four independent variables ultrasonic temperature had highest
effect on ZD of DFP followed by ultrasonic treatment time, solvent solid
ratio, and solvent concentration as shown in Table 1
(( zD ) xUT > ( zD ) xUt > ( zD ) xSr > ( zD ) xSc ) . The UAE (frequency of
40 kHz and power of 250 W) of totalphenoliccontent and antioxidants
from Grape (Vitis vinifera) seeds process by considering independent
variables XUT (33–67 °C), XUt (16–34 min), and XSc (33–67%) [60]. The
process parameters showed positive impact on ZT yield and ZD . The
value of ( zD ) xUT representing the relative effect of ultrasonic tem-
perature for ZD of DFP value found to be 0.967 with positive magnitude
showed that XUT had positive effect on ZD .
The UAE was carried out at XSr of 20:1 mL/g with XSc of 50% for a
period of 15 min at five different levels of XUT (30, 40, 50, 60 and
70 °C). The ZD of DFP in terms of percentage DPPH at 30 °C was found
to be 41.404% and with increase of temperature to 60 °C resulted in
84% increase in yield (Fig. 2A). The positive effect of temperature was
due to enhanced diffusivity during the extraction process caused by
variation of different properties such as viscosity, surface tension, and
solubility. The results showed that the maximum ZD extraction was
achieved at 60 °C and extraction above 60 °C caused decrease of ZD due
Fig. 2D. Effect of solvent concentration on total phenolic content (ZT ), antioxidant activity (ZD ) and betacyanin content (ZB ).
8
Ultrasonics - Sonochemistry 68 (2020) 105180
to the degradation of heat liable phenolic compound at higher tem-
perature.
Solvent concentration(( zD ) xSc = 0.720 )) revealed positive effect on
ZD of DFP extract (Table 3). To assess the effect of solvent concentration
on ZD , different XSc ranging from 30 to 70% (5 levels) were used along
with other three independent variables at fixed level i.e. at XUT (50 °C),
for XUt (20 min) using XSr (20:1 mL/g). At 30% of XSc the ZD was found
as 48.239% and with increase of XSc from 30 to 60% the ZD of DFP was
increased to 53% and beyond 60% the effect of XSc on ZD was found to
be insignificant (Fig. 2D). The positive effect of solvent concentration
on ZD was also observed during extraction of bioactive compounds from
wood apple fruit with concentration of ethanol (30–70%), incubation
temperature (37–60%) and XSr (20–40%) [61].
The proposed ANN model predicted a magnitude of 0.838 for re-
lative effect of ultrasonic treatment time on ZD ( zD ) xUt which suggests
that ultrasonic treatment time had positive effect on the ZD . The effect
of XUt was studied by using different levels of time: 5, 10, 15, 20, and
25 min, at a temperature of 50 °C using XSc of 50% and XSr of 20:1 mL/
g. The ZD of DFP extracted using UAE was found to be 43.036%. The
results revealed that XUt had positive effect with 76% increase in the ZD
with increase of time from 5 to 20 min and was given in Fig. 2C, but
decline in the ZD was observed beyond 20 min and the decrease was
found to be 6% at 25 min. This may be due to the degradation of
phenolic compounds with ZD on continuous heating. During the
G.V.S. Bhagya Raj and K.K. Dash
ultrasonic extraction of antioxidants from Chinese sumac (Rhus typhina
l.) fruit the DPPH scavenging activity was increased from 77.10 to
88.38% up to 20 min of extraction period and declined to 82.03% after
20 min [62].
Results from ANN showed that relative effect of XSr on ZD ( zD ) xSr
had positive effect on the ZD of DFP with a positive magnitude value of
0.772 and given in Table 3. Furthermore, the effect of XSr was studied
by conducting the UAE extraction process using 50% of XSc , different
ratios of solvent and solid: 10:1, 15:1, 20:1, 25:1 and 30:1 mL/g at a
temperature of 50 °C for 15 min of XUt and illustrated in Fig. 2B. Results
demonstrated that ZD was increased with increase of solvent solid and
the increase was found to be 48%. Similar trend of increase in ZD with
increase of XSr was reported during microwave assisted extraction of
polyphenols from defatted wheat germ [63].
3.4. Effect of UAE process variables on betacyanin content of DFP
The ZB extracted from DFP was in the range of 1.018–1.602 mg/g
d.w. Out of four independent parameters ultrasonic temperature had
higher effect on the extraction of ZB followed by solvent solid ratio,
ultrasonic treatment time and solvent concentration.
The influence of ultrasonic temperature on the betacyanin yield
( zB ) xUT was found to be positive, confirmed by the value obtained
from ANN model which was found to be 0.532 and shown in Table 3.
The effect of ultrasonic temperature was observed by conducting ex-
periments at different XUT : 30, 40, 50, 60 and 70 °C by using XSc of 50%
and the ratio of XSr of 20:1 for XUt of 15 min and illustrated in Fig. 2A.
The XUT exhibited positive influence on the yield of ZB from DFP. The
ZB extracted was in the range of 1.193–1.562 mg/g of d.w. Maximum
yield was obtained at an XUT of 60 °C but a decline in the yield was
noticed at 70 °C. As the betacyanin is a heat sensitive pigment extrac-
tion beyond 60 °C may caused the degradation of the pigment, resulted
in the lower yield of betacyanin. Previous reports on Basella rubra L.
fruits extraction using UAE also demonstrated increase of betacyanin
yield with increasing temperature from 40 to 55 °C followed by a de-
clining pattern in betacyanin yield beyond 55 °C of temperature [64].
The magnitude calculated by the ANN model for the relative in-
fluence of XSr on the yield of betacyanin ( zB ) xSr was found to be po-
sitive value of 0.504 which demonstrates that XSr had positive effect on
the betacyanin extraction and presented in Table 3. The higher ratio of
solvent to solid create a high concentration difference which favours
mass transfer and enhances the extraction of the targeted compound
into the solvent. To study the effect of solvent solid ratio on the beta-
cyanin, experiments were conducted at XUT of 50 °C using XSc of 50%
with different XSr of 10:1, 15:1, 20:1. 25:1 and 30:1 mL/g for a XUt of
15 min and presented in Fig. 2B. The rate of increase in the betacyanin
yield was rapid with increase of the XSr from 10:1 to 25:1 mg/L beyond
which the rate of increase was very slow (Fig. 2B). The highest beta-
cyanin yield recorded at XSr of 30:1 mL/g was 1.506 mg/g of DW,
which was 37.41% higher than that obtained at XSr of 10:1. Similar
trends of increase of betalain yield from Glasswort (S. fruticosa) with
increase of XSr (1:10–1:20) when other independent parameters time
(10 min) and temperature (25 °C) fixed [65].
The magnitude obtained by the ANN model for the relative effect of
solvent concentration on the yield of betacyanin from DFP ( zB ) xSc was
found to be 0.504 suggests that XSc had positive effect on the yield of
betacyanin and is presented in Table 3. To assess the effectiveness of the
XSc on betacyanin yield from DFP experiments were conducted at XUT
of 50 °C using XSr of 15:1 mL/g with varying XSc : 30, 40, 50, 60 and
70% for 20 min of XUt . The betacyanin yield extracted from DFP during
UAE extraction process at XSc varying between 30 and 70% was in the
range of 1.183–1.557 mg/g d.w (Fig. 2D).
The magnitude for relative effect of ultrasonic treatment time on the
yield of betacyanin ( zB ) xUt obtained from ANN model was found to be
0.430 which suggests that ultrasonic treatment time had positive effect
on the yield of betacyanin and is presented in Table 3. The effect of
9
Ultrasonics - Sonochemistry 68 (2020) 105180
different XUt : 5, 10, 15, 20 and 25 min on the yield of betacyanin from
DFP during UAE process was studied at XUT of 50 °C using XSc of 50%
and XSr of 20:1 mL/g illustrated in Fig. 2C. The increase in XUt from 5 to
20 min showed significant effect (p < 0.05) and was positively asso-
ciated with betacyanin yield, in the range from 1.115 to 1.450 mg/g of
d.w. but a decline in the yield was observed beyond 20 min. A yield of
1.411 mg/g of d.w was observed when the extraction was carried for
25 min, decrease in the yield of betacyanin found to be 3% which was
probably due to attainment of equilibrium point. Similar trends of in-
creasing in the yields of natural pigment from annatto seeds during UAE
was observed at the beginning of the process and started to decline at
the end of the extraction process [66].
3.5. Genetic algorithm optimization of UAE process and validation of GA
The experimental values of ZT , ZD and ZB of DFP extracted using
UAE were used for achieving the optimum UAE process conditions by
application of GA. The three responses ZT , ZD and ZB were maximized
based on the fitness function. The output of ANN model i.e., the para-
meters of the model wij , wjk , Tj and Tk were used as the initial population
for GA optimization. Precision for determining the string lengths of the
Genetic algorithm (GA) series was obtained based on the maximum and
minimum values of independent variables. Based on the highest fitness
function the optimum process parameters were selected and the op-
timum UAE process parameter was found to be 59.96°C ultrasonic
temperature, 25: 1 mL/g solvent to solid ratio, 60% solvent concentra-
tion and 20 min ultrasonic treatment time. Optimum condition resulted
in ZT of 8.366 mg GAE/g d.w., ZD of 80.933% and ZB of 1.609 mg/g
d.w.
Genetic algorithm optimization was validated by conducting the
experiments at the optimal condition and the obtained response values
were compared with the predicted response values. The experiments
were conducted in triplicates and the average response values were
considered for evaluation of relative deviation. The average experi-
mental value at optimal condition were found to be 8.471 mg GAE/g
d.w., 79.300% and 1.586 mg/g d.w. (Table 4) and the relative deviation
(R d ) was calculated using Equation (38). The R d values for experimental
and predicted values of ZT , ZD and ZB was found to be 1.234, 2.059 and
1.431 respectively (Table 4).
3.6. Extraction kinetics of ZT , ZD and ZB of DFP during UAE treatment
The extraction kinetics for the three responses carried out at dif-
ferent combinations of temperature and time of extraction. The tem-
perature was varied from lower level of ultrasonic temperature (30 °C)
to optimum temperature level (60 °C) obtained from integrated ANN-
GA model and the responses were measured at an interval of 5 min i.e.
at 0, 5, 10, 15, 20, and 25 min of sonication time. The other two
parameters solvent/liquid ratio and solvent concentration were kept
under optimized condition obtained from ANN-GA model i.e., 25:1 and
60% respectively throughout the process of extraction for kinetic study.
A pseudo second-order model was used to study the model’s char-
acteristics for ZT , ZD and ZB (Figs. 3–5). All the responses rapidly in-
creased with increase of temperature and time of extraction at the
Table 4
Relative deviation between experimental and predicted values obtained at
optimal condition.
Responses Experimental values Predicted Relative
values deviation
ZT (mg GAE/g d.w.) 8.471 8.366 1.234
ZD (%) 79.300 80.933 2.059
ZB (mg/g d.w.) 1.586 1.609 1.431
Note: ZT , ZD and ZB represents the real values of the responses.
G.V.S. Bhagya Raj and K.K. Dash
Fig. 3. Pseudo second-order kinetic plot for the total phenolic content of
Dragon fruit peel extracted at different ultrasonic temperatures.
Fig. 4. Pseudo second-order kinetic plot for the antioxidant activity of Dragon
fruit peel extracted at different ultrasonic temperatures.
starting stage of UAE process followed by more controlled increase and
becomes stagnant towards the end of extraction process i.e., after
20–25 min and reaches the saturation stage. The pseudo second order
model was found to be the best-fit model with highest average R2
(R2 > 0.998) and lower 2 value ( 2 < 0.07) for all the three re-
sponses (Table 5).
Saturation concentration (Cs ) of phytochemical compound in the
liquid extraction and pseudo second order rate constant (k ) was in-
creased with increase of temperature for all the three responses. The Cs
was in the rage of 9.35–9.62 mg GAE/g of d.w., 80.62–85.21% and
1.69–1.77 mg/g of d.w. for ZT , ZD and ZB respectively. The k value was
found to be in the range of 0.02–0.04 g d. w. /mg GAE min ,
1.43 × 10 3 3.92 × 10 3 min 1 and 0.09–0.26 g d. w. /mg min for ZT ,
ZD and ZB respectively (Table 5). The increase in Cs with increase of XUT
may be associated to unsteady interactions between the solute and
solid. The rate constant also increased with increase of temperature,
which may be because of requirement of large thermal energy for the
10
Ultrasonics - Sonochemistry 68 (2020) 105180
Fig. 5. Pseudo second-order kinetic plot for the betacyanin content of Dragon
fruit peel extracted at different ultrasonic temperatures.
diffusion of solute. Similar trends of increasing saturation concentration
and rate constant were reported during extraction of flavonoids from
Terminalia bellerica using microwave assisted extraction [45] and in the
recovery of paclitaxel from Taxus chinensis using microwave assisted
extraction in the temperature range of 30–45 °C [67]. The activation
energy for ZT , ZD and ZB was calculated using extraction rate constant
(k) from Table 5. The calculated activation energy for ZT , ZD and ZB
from DFP was found to be 17.74, 26.29 and 28.59 kJ/mol respectively
in the temperature range of 30–60 °C.
3.7. Estimation of effective diffusion coefficient, mass transfer coefficient
and Biot number for UAE of DFP
The effective diffusion coefficient, and mass transfer coefficient of
ZT , ZD and ZB , depending on the extraction temperature are summar-
ized in Table 6. The Biot number for ZT , ZD and ZB was varied in the
range of 8.81–10.19, 8.98–12.29 and 8.58–10.81 respectively. The ef-
fective diffusion coefficient was increased with increase of temperature
for all the three responses of UAE of DFP and ranged from
2.99 × 10 11 to 4.84 × 10 11 m2/s , 1.89 × 10 11 to 4.51 × 10 11 m2 /s and
2.55 × 10 11 to 5.40 × 10 11 m2/s for ZT , ZD and ZB respectively. The
mass transfer coefficient of ZT , ZD and ZB was found to be in the range
of 2.00 × 10 06 2.81 × 10 06 m/s , 1.53 × 10 06 2.66 × 10 06 m/s and
1.81 × 10 06 3.05 × 10 06 m/s respectively. When the mass transfer
coefficient was compared with the effective diffusion coefficient, it was
found that the mass transfer coefficient was increased on a considerably
larger scale. The increase of temperature has positive effect on both
effective diffusion coefficient and mass transfer coefficient. This may be
due to increase of the thermal energy with increase of temperature that
in turn increases the diffusion coefficient and mass transfer coefficient.
The increase in mass transfer may also be attributed to decrease in the
solvent viscosity with increase of temperature [27,67]. Similar trends of
increasing effective diffusion coefficient and mass transfer coefficient
was reported in ultrasound assisted extraction of dried passion fruit peel
within the temperature range of 40–70 °C [68]. The diffusion coeffi-
cient was increased from 0.88 × 10 8 to 1.78 × 10 8 m2 /s for the ex-
traction of phenolic compounds from Avogadro seed using ultrasound
assisted continuous extraction with increase of temperature from of 20
to 60 °C respectively [69].
G.V.S. Bhagya Raj and K.K. Dash Ultrasonics - Sonochemistry 68 (2020) 105180

Table 5
The second-order pseudo model parameters for the UAE of phytochemicals from Dragon fruit peel at different temperatures.
Response Temperature (°C) k Cs 2 × 10 2 R2 RMSE

Total phenolic content 30 0.0200 ± 0.0005 9.3549 ± 0.0149 0.0392 0.9995 0.0181
40 0.0266 ± 0.0021 9.4016 ± 0.0400 0.4150 0.9995 0.0588
50 0.0271 ± 0.0044 9.4837 ± 0.0814 1.7720 0.9980 0.1215
60 0.0402 ± 0.0050 9.6154 ± 0.0546 1.2060 0.9988 0.1002

Antioxidant activity 30 0.0014 ± 0.0000 80.6165 ± 0.5885 6.9030 0.9999 0.2398

40 0.0022 ± 0.0000 83.0910 ± 0.2619 2.9790 0.9995 0.1576
50 0.0025 ± 0.0000 83.6877 ± 0.2119 2.2940 0.9996 0.1383
60 0.0039 ± 0.0001 85.2082 ± 0.2322 4.7660 0.9994 0.1993

Betacyanin content 30 0.0907 ± 0.0012 1.6933 ± 0.1478 0.0286 0.9988 0.0154

40 0.1481 ± 0.0021 1.7207 ± 0.1325 0.0465 0.9984 0.0197
50 0.1936 ± 0.0031 1.7380 ± 0.1330 0.0629 0.9980 0.0229
60 0.2573 ± 0.0030 1.7668 ± 0.0883 0.0360 0.9989 0.0173

Note: Unit of second order rate constant (k) for total phenolic content, antioxidant activity, betacyanin content was g d. w. /mg GAE min , min 1 and g d. w. /mg min
respectively. Units of saturation concentration for total phenolic content, antioxidant activity, betacyanin content was mg GAE/g of d.w., %, and mg/g of d.w.
respectively.

Table 6 ordered solid phase to the less ordered liquid phase [70]. The ΔS° values
Effective diffusion coefficient, and mass transfer coefficient during UAE of were found to be 102.171 J/mol K, 66.168 J/mol K and 83.730 J/mol K
dragon fruit. for ZT , ZD and ZB respectively. The value of ΔG° found to be in the range
Response Temperature (°C) De × 10 11 (m2/s) KT × 10 6 (m/s)
of −7.353 to −10.418 kJ/mol, −4.994 to −6.979 kJ/mol and
−6.049 to −8.561 kJ/mol for ZT , ZD and ZB extracted using UAE of
Total phenolic 30 2.9881 ± 0.0150 2.0039 ± 0.0147 DFP. The negative values of change in Gibbs free energy (ΔG°) signify
content 40 3.7425 ± 0.0112 2.3307 ± 0.0103 thermodynamically spontaneous nature of the extraction process. The
50 3.8828 ± 0.0187 2.3915 ± 0.0160
values of ΔG° for the responses found to be increasing with increase of
60 4.8418 ± 0.0203 2.8069 ± 0.0121
temperature showed an indication of increase in feasibility of extraction
Antioxidant 30 1.8888 ± 0.0092 1.5276 ± 0.0090
at higher temperatures.
activity 40 2.9647 ± 0.0126 1.9937 ± 0.0101
50 3.2571 ± 0.0138 2.1179 ± 0.0095
60 4.5085 ± 0.0206 2.6625 ± 0.0115 4. Conclusion
Betacyanin content 30 2.5496 ± 0.0161 1.8139 ± 0.0094
40 3.7951 ± 0.0092 2.3535 ± 0.0111 The ZT , ZD and ZB of DFP extracted by application of UAE process
50 4.5494 ± 0.0203 2.6803 ± 0.0126
was in the range of 4.509–8.536 mg GAE/g of d.w., 41.404–74.811%
60 5.3973 ± 0.0213 3.0476 ± 0.0164
and 1.018–1.602 mg/g d.w. respectively. From the results, it was found
that all the four parameters had positive effect on all the three re-
3.8. Extraction thermodynamics of UAE process sponses. The optimized condition obtained from ANN-GA, in order to
achieve the maximum extraction performance by means of UAE, 60 °C
Extraction thermodynamic parameters of UAE of phytocompounds temperature, 25:1 mL/g liquid to solid ratio, 60% of solvent con-
from DFP are shown in Table 7. The positive value of the change in centration and 20 min of extraction time should be employed as op-
enthalpy (ΔH°) indicated the endothermic nature of the UAE process. timal operating conditions. Saturation concentration (Cs ) and pseudo
The ΔH° value was found to be 23.605 kJ/mol, 15.055 kJ/mol and second order rate constant (k ) of pseudo second order kinetic model
19.321 kJ/mol for ZT , ZD and ZB respectively. The positive value of the found to increase with increase of temperature for all the responses. The
change in entropy ( S ) illustrated the increase in disorder of the so- activation energy was found to be maximum for ZB with 28.58 kJ/mol
lid–liquid extraction system due to the solute transfer from more followed by ZD (17.73 kJ/mol) and ZT (26.29 kJ/mol). The effective
diffusion coefficient and mass transfer coefficient found increasing with
Table 7
increase of temperature. The thermodynamic parameters ΔH° and ΔS°
Thermodynamic parameters for UAE of total phenolic content, antioxidant value was maximum for ZT with value of 23.605 kJ/mol and
activity and betacyanin content from Dragon fruit. 102.171 J/mol K respectively followed by ZB and ZD . The value of ΔG°
found to be in the range of −7.353 to −10.418 kJ/mol, −4.994 to
Response Temperature (°C) H (kJ/mol) S (J/mol K) G (kJ/mol)
−6.979 kJ/mol and −6.049 to −8.561 kJ/mol for ZT , ZD and ZB re-
Total phenolic 30 23.605 102.171 −7.353 spectively extracted using UAE of DFP. Results of this study concluded
content 40 −8.374 that UAE is better for the extraction of betacyanin from DFP with
50 −9.396 minimal degradation to the pigment with higher extraction yields and a
60 −10.418
promising source for natural colorant.
Antioxidant 30 15.055 66.168 −4.994
activity 40 −5.656
50 −6.317 CRediT authorship contribution statement
60 −6.979

Betacyanin 30 19.321 83.730 −6.049 G.V.S. Bhagya Raj: Methodology, Software, Validation, Formal
content 40 −6.887 analysis, Investigation, Resources, Data curation, Writing - original
50 −7.724 draft. Kshirod K. Dash: Conceptualization, Software, Investigation,
60 −8.561
Resources, Data curation, Writing - review & editing, Visualization,
Supervision, Project administration, Funding acquisition.

11
G.V.S. Bhagya Raj and K.K. Dash
Acknowledgements
The authors gratefully acknowledge the DST-FIST, NEQIP-AICTE
and UGC-SAP for providing financial support for infrastructure devel-
opment at the Department of Food Engineering and Technology, Tezpur
University. Authors also gratefully acknowledge the research support
provided by Packaging laboratory in conducting the experiments.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.ultsonch.2020.105180.
References
[1] S. Priatni, A. Pradita, Stability study of betacyanin extract from red dragon fruit
(Hylocereus polyrhizus) peels, Proc. Chem. 16 (2015) 438–444, https://doi.org/10.
1016/j.proche.2015.12.076.
[2] D.H. Tran, C.R. Yen, Y.K.H. Chen, Effects of bagging on fruit characteristics and
physical fruit protection in red pitaya (Hylocereus spp.), Biol. Agric. Hortic. 31 (3)
(2015) 158–166, https://doi.org/10.1080/01448765.2014.991939.
[3] F. Le Bellec, F. Vaillant, E. Imbert, Pitahaya (Hylocereus spp.): a new fruit crop, a
market with a future, Fruits EDP Sciences 61 (40) (2006) 237–250, https://doi.org/
10.1051/fruits: 2006021.
[4] L. Xu, Y. Zhang, L. Wang, Structure characteristics of a water-soluble poly-
saccharide purified from dragon fruit (Hylocereus undatus) pulp, Carbohydr.
Polym. 146 (2016) 224–230, https://doi.org/10.1016/j.carbpol.2016.03.060.
[5] Y.D. Ortiz-Hernández, J.A. Carrillo-Salazar, Pitahaya (Hylocereus spp.): a short
review, Comun. Sci. 3 (4) (2012) 220–237.
[6] G. Barbeau, La pitahaya rouge, un nouveau fruit exotique, Fruits 45 (2) (1990)
141–147.
[7] Hernawati, N.A. Setiawan, R. Shintawati, D. Priyandoko, The role of red dragon
fruit peel (Hylocereus polyrhizus) to improvement blood lipid levels of hyperlipi-
daemia male mice, J. Phys. Conf. Ser. 1013 (1) (2018), https://doi.org/10.1088/
1742-6596/1013/1/012167.
[8] S. Wybraniec, B. Nowak-Wydra, K. Mitka, P. Kowalski, Y. Mizrahi, Minor betalains
in fruits of Hylocereus species, Phytochemistry 68 (2) (2007) 251–259, https://doi.
org/10.1016/j.phytochem.2006.10.002.
[9] L.C. Wu, H.W. Hsu, Y.C. Chen, C.C. Chiu, Y.I. Lin, J.A.A. Ho, Antioxidant and an-
tiproliferative activities of red pitaya, Food Chem. 95 (2) (2006) 319–327, https://
doi.org/10.1016/j.foodchem.2005.01.002.
[10] Wee, Wee, Antioxidant properties of two species of Hylocereus fruits, Adv. Appl.
Sci. Res. 2 (3) (2011) 418–425.
[11] W. Liaotrakoon, P.K. Dewettinck, Characterization of Dragon Fruit (Hylocereus spp.
) Components with Valorization Potential, vol. PhD, 2013.
[12] J. Prakash Maran, K. Swathi, P. Jeevitha, J. Jayalakshmi, G. Ashvini, Multiple re-
sponse analysis and optimization of microwave-assisted extraction of antioxidant
phenolic compounds of waste Mangifera indical Peel, J. Food Process. Preserv. 39
(6) (2015) 2276–2285, https://doi.org/10.1111/jfpp.12473.
[13] E. Susanti, S.B. Utomo, Y. Syukri, T. Redjeki, Phytochemical screening and analysis
polyphenolic antioxidant activity of methanolic extract of white dragon fruit
(Hylocereus undatus), Indones. J. Pharm. 23 (1) (2012) 60–64.
[14] A.M. Som, N. Ahmat, H.A. Abdul Hamid, N.M. Azizuddin, A comparative study on
foliage and peels of Hylocereus undatus (white dragon fruit) regarding their anti-
oxidant activity and phenolic content, Heliyon 5 (2) (2019) e01244, , https://doi.
org/10.1016/j.heliyon.2019.e01244.
[15] C.L. Roriz, L. Barros, M.A. Prieto, P. Morales, I.C.F.R. Ferreira, Floral parts of
Gomphrena globosa L. as a novel alternative source of betacyanins: optimization of
the extraction using response surface methodology, Food Chem. 229 (2017)
223–234, https://doi.org/10.1016/j.foodchem.2017.02.073.
[16] B. Lapornik, M. Prošek, A.G. Wondra, Comparison of extracts prepared from plant
by-products using different solvents and extraction time, J. Food Eng. 71 (2) (2005)
214–222.
[17] F.J. Barba, Z. Zhu, M. Koubaa, A.S. Sant’Ana, V. Orlien, Green alternative methods
for the extraction of antioxidant bioactive compounds from winery wastes and by-
products: a review, Trends Food Sci. Technol. 49 (2016) 96–109, https://doi.org/
10.1016/j.tifs.2016.01.006.
[18] M.H. Ahmad-Qasem, J. Cánovas, E. Barrajón-Catalán, V. Micol, J.A. Cárcel,
J.V. García-Pérez, Kinetic and compositional study of phenolic extraction from olive
leaves (var. Serrana) by using power ultrasound, Innov. Food Sci. Emerg. Technol.
17 (2013) 120–129, https://doi.org/10.1016/j.ifset.2012.11.008.
[19] F. Chemat, N. Rombaut, A.G. Sicaire, A. Meullemiestre, A.S. Fabiano-Tixier,
M. Abert-Vian, Ultrasound assisted extraction of food and natural products.
Mechanisms, techniques, combinations, protocols and applications. A review,
Ultrason. Sonochem. 34 (2017) 540–560, https://doi.org/10.1016/j.ultsonch.2016.
06.035.
[20] F. Chemat, V. Tomao, M. Virot, Ultrasound-assisted extraction in food analysis,
Handbook of Food Analysis Instruments, 2016, pp. 85–103.
[21] C. Wen, et al., Advances in ultrasound assisted extraction of bioactive compounds
from cash crops – a review, Ultrason. Sonochem. 48 (May) (2018) 538–549,
https://doi.org/10.1016/j.ultsonch.2018.07.018.
12
Ultrasonics - Sonochemistry 68 (2020) 105180
[22] F.J. Barba, S. Brianceau, M. Turk, N. Boussetta, E. Vorobiev, Effect of alternative
physical treatments (ultrasounds, pulsed electric fields, and high-voltage electrical
discharges) on selective recovery of bio-compounds from fermented grape pomace,
Food Bioprocess Technol. 8 (5) (2015) 1139–1148, https://doi.org/10.1007/
s11947-015-1482-3.
[23] M.B. Hossain, B.K. Tiwari, N. Gangopadhyay, C.P. O’Donnell, N.P. Brunton,
D.K. Rai, Ultrasonic extraction of steroidal alkaloids from potato peel waste,
Ultrason. Sonochem. 21 (4) (2014) 1470–1476, https://doi.org/10.1016/j.
ultsonch.2014.01.023.
[24] J.M. dos Santos, J.K. de Andrade, F. Galvão, M.L. Felsner, Optimization and vali-
dation of ultrasound-assisted extraction for the determination of micro and macro
minerals in non-centrifugal sugar by F AAS, Food Chem. 292 (2019) 66–74, https://
doi.org/10.1016/j.foodchem.2019.04.037.
[25] C. Mcdonnell, B.K. Tiwari, Ultrasound: A Clean, Green Extraction Technology for
Bioactives and Contaminants vol. 76, Elsevier Ltd, 2017.
[26] A. Trojanowska, et al., Ultrasound-assisted extraction of biologically active com-
pounds and their successive concentration by using membrane processes, Chem.
Eng. Res. Des. 147 (2019) 378–389, https://doi.org/10.1016/j.cherd.2019.05.018.
[27] Y. Tao, Z. Zhang, D.W. Sun, Kinetic modeling of ultrasound-assisted extraction of
phenolic compounds from grape marc: influence of acoustic energy density and
temperature, Ultrason. Sonochem. 21 (4) (2014) 1461–1469, https://doi.org/10.
1016/j.ultsonch.2014.01.029.
[28] K. Duarte, C.I.L. Justino, A.M. Gomes, T. Rocha-Santos, A.C. Duarte, Green analy-
tical methodologies for preparation of extracts and analysis of bioactive com-
pounds, Comprehensive Anal. Chem. 65 (vol. 2014,) 59–78.
[29] T. Jerman, P. Trebše, B. Mozetič Vodopivec, Ultrasound-assisted solid liquid ex-
traction (USLE) of olive fruit (Olea europaea) phenolic compounds, Food Chem. 123
(1) (2010) 175–182, https://doi.org/10.1016/j.foodchem.2010.04.006.
[30] N. El Darra, N. Grimi, R.G. Maroun, N. Louka, E. Vorobiev, Pulsed electric field,
ultrasound, and thermal pretreatments for better phenolic extraction during red
fermentation, Eur. Food Res. Technol. 236 (1) (2013) 47–56, https://doi.org/10.
1007/s00217-012-1858-9.
[31] C. Da Porto, E. Porretto, D. Decorti, Comparison of ultrasound-assisted extraction
with conventional extraction methods of oil and polyphenols from grape (Vitis vi-
nifera L.) seeds, Ultrason. Sonochem. 20 (4) (2013) 1076–1080, https://doi.org/10.
1016/j.ultsonch.2012.12.002.
[32] E. Espada-Bellido, M. Ferreiro-González, C. Carrera, M. Palma, C.G. Barroso,
G.F. Barbero, Optimization of the ultrasound-assisted extraction of anthocyanins
and total phenolic compounds in mulberry (Morus nigra) pulp, Food Chem. 219
(2017) 23–32, https://doi.org/10.1016/j.foodchem.2016.09.122.
[33] N.H. Che Marzuki, M. Abdul Hamid, R. Abdul Wahab, Assessment of fatty acid
composition and response surface optimization of ultrasonic-assisted extraction of
phenolic compounds from Pouteria campechiana pulp, Malaysian J. Fundam. Appl.
Sci. 14 (2) (2018) 269–277, https://doi.org/10.11113/mjfas.v14n2.984.
[34] K.H. Musa, A. Abdullah, A. Al-Haiqi, Determination of DPPH free radical scaven-
ging activity: application of artificial neural networks, Food Chem. 194 (2016)
705–711, https://doi.org/10.1016/j.foodchem.2015.08.038.
[35] B. Aliakbarian, et al., Optimization of spray drying microencapsulation of olive
pomace polyphenols using response surface methodology and artificial neural
network, LWT 93 (2018) 220–228, https://doi.org/10.1016/j.lwt.2018.03.048.
[36] J.A. Sánchez-Mesa, C. Galan, J.A. Martínez-Heras, C. Hervás-Martínez, The use of a
neural network to forecast daily grass pollen concentration in a Mediterranean
region: the southern part of the Iberian Peninsula, Clin. Exp. Allergy 32 (11) (2002)
1606–1612, https://doi.org/10.1046/j.1365-2222.2002.01510.x.
[37] Y. Nagata, K.H. Chu, Optimization of a fermentation medium using neural networks
and genetic algorithms, Biotechnol. Lett. 25 (21) (2003) 1837–1842, https://doi.
org/10.1023/A:1026225526558.
[38] S.M. Huang, C.H. Kuo, C.A. Chen, Y.C. Liu, C.J. Shieh, RSM and ANN modeling-
based optimization approach for the development of ultrasound-assisted liposome
encapsulation of piceid, Ultrason. Sonochem. 36 (2017) 112–122, https://doi.org/
10.1016/j.ultsonch.2016.11.016.
[39] F. Coelho Sampaio, et al., Batch growth of Kluyveromyces lactis cells from depro-
teinized whey: response surface methodology versus artificial neural network-ge-
netic algorithm approach, Biochem. Eng. J. 109 (2016) 305–311, https://doi.org/
10.1016/j.bej.2016.01.026.
[40] K.M. Desai, S.A. Survase, P.S. Saudagar, S.S. Lele, R.S. Singhal, Comparison of ar-
tificial neural network (ANN) and response surface methodology (RSM) in fer-
mentation media optimization: case study of fermentative production of scler-
oglucan, Biochem. Eng. J. 41 (3) (2008) 266–273, https://doi.org/10.1016/j.bej.
2008.05.009.
[41] D. Learning, Ian Goodfellow and Yoshua Bengio and Aaron Courville, MIT Press,
2016.
[42] M.S. Stanković, Total phenolic content, flavonoid concentration and antioxidant
activity of Marrubium peregrinum L. extracts, Kragujev. J. Sci. 33 (January 2011)
(2011) 63–72 doi: 581.19:582.929.4:577.164.3.
[43] O.R. Alara, N.H. Abdurahman, O.A. Olalere, Optimization of microwave-assisted
extraction of flavonoids and antioxidants from Vernonia amygdalina leaf using
response surface methodology, Food Bioprod. Process. 107 (2018) 36–48, https://
doi.org/10.1016/j.fbp.2017.10.007.
[44] Y.M. Wong, L.F. Siow, Effects of heat, pH, antioxidant, agitation and light on be-
tacyanin stability using red-fleshed dragon fruit (Hylocereus polyrhizus) juice and
concentrate as models, J. Food Sci. Technol. 52 (5) (2015) 3086–3092, https://doi.
org/10.1007/s13197-014-1362-2.
[45] R. Yedhu Krishnan, K.S. Rajan, Microwave assisted extraction of flavonoids from
Terminalia bellerica: Study of kinetics and thermodynamics, Sep. Purif. Technol.
157 (2016) 169–178, https://doi.org/10.1016/j.seppur.2015.11.035.
G.V.S. Bhagya Raj and K.K. Dash
[46] T.W. Charpe, V.K. Rathod, Extraction of glycyrrhizic acid from licorice root using
ultrasound: process intensification studies, Chem. Eng. Process. Process Intensif. 54
(2012) 37–41.
[47] W. Qu, Z. Pan, H. Ma, Extraction modeling and activities of antioxidants from po-
megranate marc, J. Food Eng. 99 (1) (2010) 16–23.
[48] G. Berthier, Problèmes théoriques liés à la détermination des coefficients d’auto-
diffusion dans les solides par la méthode des échanges isotopiques hétérogènes, J.
Chim. Phys. 49 (1952) 527–536.
[49] P. Rai, G.C. Majumdar, S. DasGupta, S. De, Prediction of the viscosity of clarified
fruit juice using artificial neural network: a combined effect of concentration and
temperature, J. Food Eng. 68 (4) (2005) 527–533, https://doi.org/10.1016/j.
jfoodeng.2004.07.003.
[50] J. Welti-Chanes, J. Vélez-Ruiz, G.V. Barbosa-Cánovas, Transport phenomena, Food
Process. (2016).
[51] R. Tabaraki, E. Heidarizadi, A. Benvidi, Optimization of ultrasonic-assisted ex-
traction of pomegranate (Punica granatum L.) peel antioxidants by response surface
methodology, Sep. Purif. Technol. 98 (2012) 16–23, https://doi.org/10.1016/j.
seppur.2012.06.038.
[52] J. Wang, B. Sun, Y. Cao, Y. Tian, X. Li, Optimisation of ultrasound-assisted ex-
traction of phenolic compounds from wheat bran, Food Chem. 106 (2) (2008)
804–810.
[53] M. Toma, M. Vinatoru, L. Paniwnyk, T.J. Mason, Investigation of the effects of
ultrasound on vegetal tissues during solvent extraction, Ultrason. Sonochem. 8 (2)
(2001) 137–142, https://doi.org/10.1016/S1350-4177(00)00033-X.
[54] I.G. Moorthy, J.P. Maran, S. Ilakya, S.L. Anitha, S.P. Sabarima, B. Priya, Ultrasound
assisted extraction of pectin from waste Artocarpus heterophyllus fruit peel,
Ultrason. Sonochem. 34 (2017) 525–530, https://doi.org/10.1016/j.ultsonch.2016.
06.015.
[55] E. Karacabey, G. Mazza, Optimisation of antioxidant activity of grape cane extracts
using response surface methodology, Food Chem. 119 (1) (2010) 343–348, https://
doi.org/10.1016/j.foodchem.2009.06.029.
[56] T. Belwal, P. Dhyani, I.D. Bhatt, R.S. Rawal, V. Pande, Optimization extraction
conditions for improving phenolic content and antioxidant activity in Berberis
asiatica fruits using response surface methodology (RSM), Food Chem. 207 (2016)
115–124, https://doi.org/10.1016/j.foodchem.2016.03.081.
[57] R.K. Salar, S.S. Purewal, M.S. Bhatti, Optimization of extraction conditions and
enhancement of phenolic content and antioxidant activity of pearl millet fermented
with Aspergillus awamori MTCC-548, Resour. Technol. 2 (3) (2016) 148–157,
https://doi.org/10.1016/j.reffit.2016.08.002.
[58] S. Zhao, K.C. Kwok, H. Liang, Investigation on ultrasound assisted extraction of
saikosaponins from Radix Bupleuri, Sep. Purif. Technol. 55 (3) (2007) 307–312,
https://doi.org/10.1016/j.seppur.2006.12.002.
[59] F. Dranca, M. Oroian, Optimization of ultrasound-assisted extraction of total
13
Ultrasonics - Sonochemistry 68 (2020) 105180
monomeric anthocyanin (TMA) and total phenolic content (TPC) from eggplant
(Solanum melongena L.) peel, Ultrason. Sonochem. 31 (2016) 637–646, https://
doi.org/10.1016/j.ultsonch.2015.11.008.
[60] K. Ghafoor, Y.H. Choi, J.Y. Jeon, I.H. Jo, Optimization of ultrasound-assisted ex-
traction of phenolic compounds, antioxidants, and anthocyanins from grape (Vitis
vinifera) seeds, J. Agric. Food Chem. 57 (11) (2009) 4988–4994, https://doi.org/
10.1021/jf9001439.
[61] N. Ilaiyaraja, K.R. Likhith, G.R. Sharath Babu, F. Khanum, Optimisation of extrac-
tion of bioactive compounds from Feronia limonia (wood apple) fruit using re-
sponse surface methodology (RSM), Food Chem. 173 (2015) 348–354, https://doi.
org/10.1016/j.foodchem.2014.10.035.
[62] J. Lai, H. Wang, D. Wang, F. Fang, F. Wang, T. Wu, Ultrasonic extraction of anti-
oxidants from chinese sumac (Rhus typhina L.) fruit using response surface meth-
odology and their characterization, Molecules 19 (7) (2014) 9019–9032, https://
doi.org/10.3390/molecules19079019.
[63] N. Teslić, et al., Defatted wheat germ as source of polyphenols—optimization of
microwave-assisted extraction by RSM and ANN approach, Chem. Eng. Process.
Intensif. 143 (2019) 107634.
[64] J.P. Maran, B. Priya, Natural pigments extraction from Basella rubra L. fruits by
ultrasound-assisted extraction combined with Box-Behnken Response surface de-
sign, Sep. Sci. Technol. 50 (10) (2015) 1532–1540, https://doi.org/10.1080/
01496395.2014.980003.
[65] E.E. Ahmed, S. Iwamoto, R. Yamauchi, Optimization of betalain extraction from
Salicornia fruticosa and its encapsulation, no. March, 2018.
[66] M. Yolmeh, M.B. Habibi Najafi, R. Farhoosh, Optimisation of ultrasound-assisted
extraction of natural pigment from annatto seeds by response surface methodology
(RSM), Food Chem. 155 (2014) 319–324, https://doi.org/10.1016/j.foodchem.
2014.01.059.
[67] S.H. Lee, J.H. Kim, Kinetic and thermodynamic characteristics of microwave-as-
sisted extraction for the recovery of paclitaxel from Taxus chinensis, Process
Biochem. 76 (November) (2019) 187–193, https://doi.org/10.1016/j.procbio.
2018.11.010.
[68] E.M.G.C. Do Nascimento, A. Mulet, J.L.R. Ascheri, C.W.P. De Carvalho, J.A. Cárcel,
Effects of high-intensity ultrasound on drying kinetics and antioxidant properties of
passion fruit peel, J. Food Eng. 170 (2015) 108–118, https://doi.org/10.1016/j.
jfoodeng.2015.09.015.
[69] F.J. Segovia, J.J. Corral-Pérez, M.P. Almajano, Avocado seed: modeling extraction
of bioactive compounds, Ind. Crops Prod. (2016), https://doi.org/10.1016/j.
indcrop.2016.03.005.
[70] R.C.A. Amarante, P.M. Oliveira, F.K. Schwantes, J.A. Morón-Villarreyes, Oil ex-
traction from castor cake using ethanol: kinetics and thermodynamics, Ind. Eng.
Chem. Res. 53 (16) (2014) 6824–6829, https://doi.org/10.1021/ie500508n.