Journal of Food Engineering 218 (2018) 33e43

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Journal of Food Engineering

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

Intensified degumming of crude soybean oil using cavitational

reactors
Nishant S. More, Parag R. Gogate*
Chemical Engineering Department, Institute of Chemical Technology, Matunga, Mumbai, 400 019, India

a r t i c l e i n f o a b s t r a c t

Article history: A novel cavitation assisted degumming approach for the purification of crude soybean oil in terms of the
Received 14 March 2017 removal of the total phospholipid content has been reported in the work with a detailed study into the
Received in revised form effect of operating parameters such as temperature, hydrogen peroxide loading and introduction of
2 August 2017
ozone gas at varying flow rate. Ultrasonic horn, ultrasonic bath and hydrodynamic cavitation reactors
Accepted 31 August 2017
have been used for comparing the efficacy of different types of cavitational reactors. Initially, extent of
Available online 31 August 2017

degumming was quantified at different temperatures and 60 C was established as optimum to give
significant extent of degumming in terms of phospholipids removal. Degumming in the presence of
Keywords:
Degumming
ozone gas gave unsatisfactory results because of the specific physical and chemical properties of crude
Crude soybean oil soybean oil. Combination of ultrasound and hydrogen peroxide resulted in complete phospholipid
Ultrasound degradation at capacity of 250 ml at optimized temperature in 100 min of treatment. Ultrasonic horn and
Hydrodynamic cavitation bath were also used at 1 L operating volume and the extent of degumming was found to be 90.81% and
Hydrogen peroxide 93.50% respectively. For large scale studies, hydrodynamic cavitation was operated at 4 bar pressure
Ozone using slit venturi as the cavitating device which gave 93.65% as the extent of degumming. Overall,
intensified degumming approach for processing of crude soybean oil was demonstrated to yield high
quality oil in terms of the reduced phospholipids content. Cavitation based degumming process can be an
excellent alternative approach to the conventional method with major benefits like reduction in time and
energy requirements as demonstrated in the present work.
© 2017 Elsevier Ltd. All rights reserved.

1. Introduction
Crude soybean oil is obtained by seed pressing or solvent
extraction processes and mainly comprises of free fatty acids, tri-
glycerides, trace elements, heavy metals, sterols, phospholipids and
other minor impurities (Lin et al., 1997; Koris and Vatai, 2002;
Hafidi et al., 2005). Among the different impurities present, con-
centration of phospholipids derivatives is at the top, which is also a
decision making factor for different applications. Substantial pres-
ence of the chemical species may extensively affect the quality of oil
in terms of odour, shelf life and undesirable flavour. An exhaustive
oil refining process is required to get desired product characteris-
tics required for different applications. The different crude oil
refining operations include degumming, neutralization, bleaching,
dewaxing, decolourisation (Manjula and Subramanian, 2009; Yu
et al., 2013). Degumming is the primary step intended to separate
* Corresponding author.
E-mail address: pr.gogate@ictmumbai.edu.in (P.R. Gogate).
phospholipids, lecithin and trace metals from crude oil. Degummed
soybean oil (with significantly lower phospholipid content) is most
widely used for making salad dressings, frozen foods, imitation
dairy products, mayonnaise and commercially baked goods. Soy-
bean oil has good emulsifying ability as compared to other edible
vegetable oils and hence is the first choice in food processing in-
dustries. It is also used as a renewable raw material for the pro-
duction of plasticizers, soy candles, paints and crayons. Another
important application of soybean oil has been reported as a raw
material for biodiesel production due to its low acid value (Li et al.,
2015; Fox and Austic, 2002). For all the above applications, crude
soybean oil needs to be degummed in a controlled manner to give
maximum degumming yield at the same time maintaining the
important properties.
Phospholipids are generally classified into hydratable (HPL) and
nonhydratable (NHPL) form, which need to be removed from oil
using stepwise degumming operation. Crude Soybean oil contains
maximum amount of hydratable phospholipids (HPL) which can be
removed by water based degumming and also some quantum of
non-hydratable phospholipids is removed in the process (Yu et al.,

http://dx.doi.org/10.1016/j.jfoodeng.2017.08.029
0260-8774/© 2017 Elsevier Ltd. All rights reserved.
34 N.S. More, P.R. Gogate / Journal of Food Engineering 218 (2018) 33e43
2013). The phosphatidyl chlorine and phosphatidyl mositol are
completely hydratable whereas phosphatidyl ethanolamine is
partly hydratable and phosphatidic acid is completely non-
hydratable form of phospholipid. Most times, all these derivatives
of phospholipids form salts with divalent cation (calcium and
magnesium). Non-Hydratable phospholipids can be removed by
the addition of phosphoric acid, citric acid or oxalic acid at higher
temperature (Haahr and Jacobsen, 2008). The conventional acid
degumming process is based on the principle of decomposition of
phosphatide/metal complexes by addition of acid or complexing
agent followed by hydration of phospholipids in water. Partial
neutralization of acid is subsequently applied to avoid migration of
phosphatides back to the oil phase (Liu et al., 2012). The overall
process is usually combination of multiple steps based on acid,
complexing agent and water treatments applied in different
sequence depending on the specific oil to be processed. This pro-
cessing approach consumes large amount of chemicals and also
generates plenty of wastewater. In addition, use of high tempera-
ture compromises nutritional factors in the final product.
For avoiding problems of conventional degumming method,
using ultrafiltration membranes for separation of compounds on
the basis of permeability of membrane and molecular weight of
compounds has been applied generally either individually or in
combination with the acid degumming. Liu et al. (2012) studied
acid degumming process combined with ultrafiltration and re-
ported significant reduction in phospholipid concentration. Koris
and Marki (2006) reported that 87% extent of degumming was
achieved using ultrafiltration alone with advantages of lower
effluent production, lower power consumption, no requirements
of additional chemical compounds and higher separation of un-
desirable particles. Another study of degumming of crude vege-
table oil using membrane separation revealed that maximum
rejection of phospholipids was achieved at 300 psi pressure and
temperature of 40
C with feed velocity of 220 L/h (Lin et al.,
1997). There are possibilities of using different types of mem-
branes in the degumming. De Moura et al. (2005) reported that
ultrafiltration using polyethersulphone (PES) membrane resulted
in good permeate flux and reduction in phospholipid concen-
tration. Ochoa et al. (2001) and Pagliero et al. (2007) reported
that degumming of crude vegetable oil using Polyvinyliden-
fluoride (PVDF) membrane gave better efficacy due to small pore
sizes. Degumming of vegetable crude oil using ceramic ultra-Fine
membrane was studied by de Carvalho et al. (2006) and Manjula
and Subramanian (2009) and it was reported that UF membrane
has high potential to remove phosphorus from crude oil miscella
with high flux of permeate and elevated retention of phospho-
lipids. Another commonly reported approach of degumming is
based on the use of enzymes. Jiang et al. (2015) investigated the
enzymatic degumming of crude oil using Pseudomonas fluo-
rescens BIT-18 enzyme and reported that after enzymatic treat-
ment of 5 h at 40
C temperature, phospholipid concentration
was reduced to 5 mg/kg. Lamas et al. (2014) also reported similar
efficacy for phospholipase A1 and acryltransferase at enzyme
dosage of 200 U/kg in 60 min of processing. Yu et al. (2013) re-
ported the use of phospholipase A1 immobilized on magnetic
nanoparticles for degumming of soybean and sunflower seed oil.
In another work, Qu et al. (2016) reported the application of
immobilized phospholipase A2 for giving stable degumming ac-
tivity. Lamas et al. (2016) evaluated phospholipase A1 and
Phospholipase A2 for degumming and reported that 97%
degumming was obtained during 180 min of processing under
optimized conditions.
Analysis of the two more commonly used approaches revealed
that the membrane degumming approach gives better efficiency
but it is expensive and time consuming. The process is also facing
the problem of membrane fouling which enhances the mainte-
nance. In enzymatic degumming, enzyme activity can be affected
by high content of phospholipids and other constituents present in
vegetable oil attributed to the enzyme inhibition. Also, the enzy-
matic processes are significantly slower, giving very high treatment
times. Considering these aspects, the present work has focused on
the use of cavitational reactors for developing an improved
degumming approach with possible intensification benefits such as
reduced time and requirements of chemicals/temperature.
Cavitation has been widely used as an intensifying approach
for different chemical processing applications in different in-
dustrial sectors such as chemical, pharmaceutical, petrochemical,
polymer and textiles. Cavitation is the formation, growth and
subsequent collapse of micro-bubbles occurring within a very
small fraction of time and releasing significant quantum of en-
ergy generating very high local temperatures (in the range
1000e15,000 K) and pressures (in the range 500e5000 bar).
Hydroxyl and many other radicals are also formed due to the
dissipation of high magnitude of energy locally (Gogate, 2008;
Lauterborn and Ohl, 1997). These radicals have the potential to
initiate the reactions at higher rate and also result in oxidation of
many compounds. Use of additional oxidizing agent or activators
can inevitably produce more hydroxyl radicals giving intensified
approach. Various activators like hydrogen peroxide, ozone, hy-
droquinone, sulphites and pyrosulphates etc. can be used
depending on the nature of liquid medium (acidic, basic or
neutral) for different applications (Chakinala et al., 2007;
Niemczewski, 1999). Hydrogen peroxide is a strong oxidizing
agent contributing to the formation of enhanced quantum of
hydroxyl radicals in liquid medium giving high oxidation ca-
pacity and hence has been explored in the present work in
combination with ultrasound. There have been some studies
reporting the intensification of oil processing applications mainly
extraction using ultrasound. Li et al. (2004) studied oil extraction
from soybean seeds using ultrasound at 20 kHz frequency using
mix solvent (Hexane and isopropanol) and reported that 40%
intensification was obtained due to cavitational effect of shock
waves produced by ultrasonic transducer in liquid solvent.
Another ultrasound assisted oil extraction approach was inves-
tigated by Sicaire et al. (2016) with reported benefits as reduced
solvent consumption and maximum productivity based on opti-
mum conditions of ultrasonic intensity (7.7 W/cm2) and solid/
liquid ratio (1/15). Analysis of literature also revealed that there
are no studies related to intensified degumming using ultrasound
and hence the novelty of the current work is established.
Present work has focused on the use of ultrasound for devel-
oping greener intensified degumming approach that can possibly
give considerable economic savings. Cavitation based approach has
been specifically applied for removal of phospholipids present in
crude soybean oil with further intensification studies based on the
use of hydrogen peroxide and ozone gas as an oxidizing agent. The
extent of degumming has been monitored in terms of decrease in
phospholipid concentration of processed soybean oil. Phospholipid
determination was performed using the AOCS Ca 12-55 method
based on sodium molybdate dye reagent (https://www.aocs.org/
info/6th-edition/6th-edition#section-c-commercial-fats-and-oils).
2. Materials and methods
2.1. Materials
Commercially extracted crude soybean oil was obtained from
Maharashtra oil extractions Pvt. Ltd., Dhule, Maharashtra (India)
and stored in dark before use. Hydrogen peroxide (30% W/V) was
procured from Thomas Baker (Chemicals) Pvt. Ltd., Mumbai (India).
 N.S. More, P.R. Gogate / Journal of Food Engineering 218 (2018) 33e43
All the other required analytical grade chemicals such as hydrazine
sulphate, sodium molybdate, potassium dihydrogen orthophos-
phate, potassium hydroxide pellets, zinc oxide and hydrochloric
acid (35.4%, sp. gr. 1.18) were procured from S. D. Fine Chemicals
Pvt. Ltd., Mumbai (India). All the chemicals were used as received
from the supplier unless otherwise started.
2.2. Experimental setup
2.2.1. Ultrasonic horn
Laboratory scale degumming studies were performed using ul-
trasonic horn mostly at 100 W optimized power dissipation level
(based on the calorimetric study in terms of maximum transfer
efficiency, except for the set of understanding the effect of oper-
ating power). A schematic representation of the experimental set
up based on the ultrasonic (US) horn with jacketed reactor has been
shown in Fig. 1. Duty cycle was adjusted at 80% (8 s ON and 2 s OFF)
based on recommendation from supplier. The ultrasonic horn was
obtained from M/s Dakshin, Mumbai (India) and operated at fixed
frequency of 20 kHz with horn tip area of 3.46 cm2 (Prajapat and
Gogate, 2016).
2.2.2. Ultrasonic bath
The indirect sonication was achieved using multiple fre-
quency (25 kHz and 40 kHz) ultrasonic bath supplied by M/s
Dakshin, Mumbai (India). US bath is basically a rectangular
shape stainless steel tank (dimension: 300  150  150 mm)
consisting of five transducers fitted at the bottom of the tank.
Experiments were performed at 25 kHz frequency and 100W
power with 60
C as the controlled temperature (Rao and Rathod,
2015).
2.2.3. Hydrodynamic cavitation
Large scale operation was performed using hydrodynamic
cavitation (HC) setup which consists of 7 L stainless steel (SS) jac-
keted tank (5 L oil was processed in the present work), slit venturi
as a cavitating device and pressure regulating valve provided on
bypass line (Barik and Gogate, 2016; Patil et al., 2014). The on-line
pressure was adjusted at 4 bar throughout the experimentation as
per the optimum observed in earlier studies (Barik and Gogate,
2016).
Fig. 1. Schematic representation of experimental set up for ultrasonic horn with jacketed reactor.
35
2.2.4. Ozone generator
Ozone gas generator was procured from Eltech Engineers,
Mumbai and it was operated over the flow rate range of 200 mg/h
to 400 mg/h. The flow rate calibration study was performed using
iodometric titrations for exact flow rate adjustments (Barik and
Gogate, 2016).
2.3. Experimental methodology
Ultrasound assisted degumming experiments were performed
using 250 ml and 2 L glass reactors. Scale up studies in hydrody-
namic cavitation were performed using SS jacketed reactor of 7 L
volume. Pre-analysis of crude soybean oil was performed in terms
of total phospholipids concentration and all the experiments were
performed with the same oil.
Initially, effect of power dissipation on the efficacy of ultrasonic
degumming process was studied at 80 W, 100 W and 120 W under
ambient conditions. Further, ultrasonic degumming was performed
at different temperatures (40
C, 50
C, 60
C, 70
C and 80
C) using
water bath to establish the effect of temperature. The actual tem-
perature was monitored by immersing thermocouple into the re-
action mixture. Effect of oxidizing agents like hydrogen peroxide
(H2O2) and ozone gas (O3) have been investigated at different
loadings and flow rates respectively. The measured quantity of
crude oil was heated from 35 ± 1
C to the desired temperature
depending on the protocol for experiments. In a typical experi-
mental run, the temperature was observed every minute and
samples were withdrawn for analysis after every 10 min. The
withdrawn samples were centrifuged at 3000 rpm for 10 min, and
clear oil was obtained in supernatant phase. The oil was separated
and stored in amber colour bottle without exposing to sunlight for
further analysis. All the experiments were performed repeatedly (at
least two times) to check the reproducibility of the results and
obtained variation in the data has been depicted in figures with
error bars. In general, it was observed that the variation due to the
experimental errors was within ±2%.
2.4. Phospholipid analysis
Total phosphorus content in processed oil samples was evalu-
ated using standard sodium molybdate method (AOCS Ca12-15)
36 N.S. More, P.R. Gogate / Journal of Food Engineering 218 (2018) 33e43

based on the UV-VIS spectrophotometer (Thermofisher UV 2600)
analysis at 650 nm wavelength (Lin et al., 1997). Following equa-
tions were used to calculate phospholipid content from the ob-
tained phosphorus concentration data.
10  ðA  BÞ
Phosphorus ð%Þ ¼
V W
Phospholipid ð%Þ ¼ Phosphorus  30
ðInitial phospholipid  Final phospholipid Þ
Degumming ð%Þ ¼
Initial phospholipid
 100
where
A ¼ Phosphorus content of sample aliquot (mg)
B ¼ Phosphorus content of blank aliquot (mg)
W ¼ Mass of sample in (g)
V ¼ Volume of aliquot taken (ml)
3. Results and discussion
3.1. Effect of power dissipation on ultrasonic degumming process
Effect of ultrasound on extent of degumming was evaluated at
different powers of 80 W, 100 W and 120 W. The obtained results
are given in Table 1 and graphical representation depicted in Fig. 2.
It was observed that 74.31% phospholipids were removed from oil
at 80 W power within 100 min of treatment whereas very similar
phospholipid separation (80e81%) was achieved at 100 W and
120 W ultrasonic power. Hence, 100 W power was set to be an
optimum value for power dissipation, which gave marginally
higher extent of degumming. The extent of intensification is always
dependent on the cavitational intensity. In the presence of ultra-
sound, hydratable phospholipids get segregated at ambient tem-
perature but non-hydratable phospholipids require more energy
for conversion to hydratable phospholipids for complete degum-
ming. Cavitation effectively works when the solution contains
aqueous matter to form radicals. Crude soybean oil contains
negligible amount of water, which resulted in marginal changes in
extent of degumming. Hence it was thought desirable to consider
modified approaches for getting higher extent of degumming. It is
expected that use of higher temperature could give better efficacy
in terms of complete phospholipids separation. Ultrasound com-
bined with oxidizing agent can also enhance the cavitation effect to
give desired degumming. Considering these aspects, further work
was concentrated on using higher temperatures and additives as
ozone and hydrogen peroxide as oxidizing agents that can provide
significant quantity of hydroxyl radicals.
3.2. Effect of temperature on degumming using ultrasound






Effect of temperature (40 C,50 C, 60 C, 70 C, 80 C) on the
extent of degumming has been investigated for reaction volume of
250 ml and 100 W ultrasonic power using ultrasonic horn. An


additional study using high temperature as 70 C without ultra-
sound has also been performed to elucidate the role of ultrasound.
Higher temperature can enhance the degumming effect based on
conversion of non-hydratable phospholipids to hydratable which
can be easily separated by centrifugation. The results for extent of
degumming obtained from different sets of experiments at varying
temperatures have been depicted in Fig. 3. Extent of degumming
gradually increased (81e83%) over the initial temperature range



(40 C and 50 C) whereas drastic increase in degumming (91e93%


as the actual extent) was observed above 60 C temperature. Mar-
ginal difference in percentage degumming was observed for oper-




ating temperatures of 60 C, 70 C and 80 C. It was also observed


that the extent of degumming obtained at 70 C for only heating
treatment (without ultrasound) was only 72.28% which clearly
establish the role played by cavitational effects.
Kinetic analysis was also performed in the work and the order of
reaction was calculated by plotting graph of required function of
concentration for the second order fitting with respect to time from

Table 1
Comparison of results obtained for different degumming approaches in terms of extent of degumming.

Approach Operating Condition Reaction time Extent of degumming (%)

Only US (Power study, 250 ml) 80 W 100 min 74.31

100 W 100 min 79.74
120 W 100 min 81.12
US Horn at different Temperatures 40
C 100 min 81.91
(250 ml) 50
C 100 min 83
60
C 100 min 90.71
70
C 100 min 91.8
80
C 100 min 92.5
Heating without US 70
C 100 min 72.28
US Horn þ O3 200 mg/h 120 min 89.03
(250 ml) 400 mg/h 120 min 90.9
US Horn þ H2O2 30 PPM 100 min 86.6
(250 ml) 40 PPM 100 min 88.83
50 PPM 100 min 90.01
60 PPM 100 min 93.9
100 PPM 100 min 99.51
Without US (only H2O2) 100 PPM 100 min 86.45
US Horn þ H2O2 (Scale up at 1 L capacity) 100 PPM 120 min 89.8
200 PPM 120 min 90.8
500 PPM 120 min 94.4
US Batch þ H2O2 (Scale up at 1 L capacity) 100 PPM 120 min 93.40
200 PPM 120 min 93.51
500 PPM 120 min 97.5
HC þ H2O2 100 PPM 140 min 93.7
(scale up at 5 L capacity)

US- Ultrasound.
HC- Hydrodynamic cavitation.
 N.S. More, P.R. Gogate / Journal of Food Engineering 218 (2018) 33e43 37

100

90

80
EXTENT OF DEGUMMING (%)

70

60

50

40
80 W
30
100 W
20
120 W
10

0
0 10 20 30 40 50 60 70 80 90 100
TIME (MIN)

Fig. 2. Effect of ultrasonic power dissipation on extent of degumming.

120

100
EXTENT OF DEGUMMING (%)

80

60

40 40C 50C 60C 70C 80C 70C (Without US)

20

0
0 20 40 60 80 100 120
TIME (MIN)

Fig. 3. Effect of temperature on extent of degumming.

the experimental data as depicted in Fig. 4 and Table 2. Second 103 mol.L1.min1 was obtained for higher temperature of 60 C,




order rate constants estimated from the graph were 70 C and 80 C. Considering the obtained results, 60 C was selected



5  104 mol.L1.min1 obtained for 40 C and 50 C. Further, as the optimum temperature and used in further studies. De Moura
significantly increased degumming rate constant as 1.1  et al. (2005) investigated membrane degumming of soybean oil and
38 N.S. More, P.R. Gogate / Journal of Food Engineering 218 (2018) 33e43

0.14

0.12

0.1

0.08
1/ C

40C
0.06
50C

0.04 60C

70C
0.02
80C

0
0 10 20 30 40 50 60 70 80 90 100
TIME (MIN)

Fig. 4. Kinetic analysis of ultrasonic degumming at different temperatures.

Table 2
Comparative results for the effect of temperature and ultrasound on extent of degumming and rate constants.

Temperature
C Extent of degumming (%) Rate constant (mol.L1 min1) R2 Order of reaction
4
40 81.91 5  10 0.9918 2
50 82.96 5  104 0.9849 2
60 90.17 1.1  103 0.9633 2
70 91.76 1.1  103 0.9725 2
80 92.46 1.1  103 0.9554 2

reported that 89% phospholipids were separated at 50 C whereas


97% phospholipids separation was obtained at 60 C using mem-
brane filtration process (Koris and Vatai, 2002). The maximum
degumming yields were obtained at similar temperature in both
the cases of cavitation process in the present work and membrane
filtration process as per majority reports in literature (comparison
with membrane was done as no reports with ultrasound were
available). Generally the reported range of temperature for best
results is 50 to 60
C. De Carvalho et al. (2006) performed ceramic
membrane based degumming at 40
C and reported 70e95%
phospholipid retention. Polyvinylidenfloride (PVDF) Membrane


degumming experiments performed in another study at 50 C also
confirmed 95% phospholipids retention (Pagliero et al., 2007). In
some cases of membrane degumming processes, membrane gets
elongated and loses their properties at elevated temperature and
hence not many studies could be observed related to effect of
temperature above 60
C.
3.3. Effect of ozone addition on ultrasonic degumming
Effect of introducing ozone on ultrasonic degumming process
was investigated at different flowrates (200 mg/h and 400 mg/h)
and the obtained results have been depicted in Fig. 5. It was
observed that use of ozone did not give any significant process
intensification benefits with less than 90% as the extent of
degumming. Crude soybean oil exhibit much higher viscosity
(54.3 cP) and lower density (0.896 g/ml) as compared to water and
hence soybean oil has poor ozone solubility. Also, due to higher
viscosity of the oil, cavitational bubbles does not grow significantly
which suppress the cavitational effects and hence the production of
hydroxyl radicals from ozone might be limited. As the process was
performed at elevated temperature, the solubility of ozone was also
reduced (Jodzis and Patkowski, 2017). Therefore, this experimental
approach did not result in significant improvement in the
degumming yield (81e82% phospholipid removal). Hence, it was
thought desirable to use another oxidizing agent as hydrogen
peroxide.
3.4. Effect of addition of hydrogen peroxide (H2O2) on ultrasonic
degumming
Addition of hydrogen peroxide (H2O2) in ultrasonic degumming
process was investigated using ultrasonic horn at optimized tem-


perature (60 C). Effect of addition of hydrogen peroxide at various
concentrations (30 PPM, 40 PPM, 50 PPM, 60 PPM, 100 PPM, 200
PPM and 500 PPM) was studied at 100 W US power and 100 min as
the treatment time. The obtained results have been given in Fig. 6
from which it is observed that extent of degumming increases
 N.S. More, P.R. Gogate / Journal of Food Engineering 218 (2018) 33e43 39

100

90

80
EXTENT OF DEGUMMING (%)

70

60

50

40

30 UV Horn+ O3 (200 MG/H)

20 UV Horn+ O3 (400 MG/H)

10

0
0 20 40 60 80 100 120
TIME (MIN)

Fig. 5. Effect of addition of ozone on the extent of ultrasonic degumming.

with an increase in hydroxide peroxide concentration. From initial
value of 30 PPM H2O2, the extent of degumming increased gradu-
ally up to 50 PPM. Significant increase in degumming was observed
after 60 PPM H2O2 addition and 99.51% of degumming was ob-
tained at 100 PPM H2O2 concentration. The contribution of ultra-
sound was evaluated by performing degumming process without
ultrasound at 100 PPM H2O2 and 60
C temperature which resulted
in 86.45% phospholipids separation. Comparison of both the studies
(with and without ultrasound) concluded that ultrasound played a
crucial role driving the complete degumming of crude oil. It is ex-
pected that significant quantum of hydroxyl radicals are produced
from hydrogen peroxide in the presence of cavitational effects
(Sivasankar and Moholkar, 2009). Hydroxyl radicals react with
nonhydratable phospholipids derivatives to dissociate the non-
hydratable (e.g. phosphatidic acid) matters into hydratable form
which are further easily removed from the processed oil.

100

90

80
EXTENT OF DEGUMMING (%)

70

60

50 US+30 PPM H2O2

40 US+40 PPM H2O2

30 US+50 PPM H2O2

US+60 PPM H2O2
20
US+100 PPM H2O2
10
Without US (only 100 PPM H2O2)
0
0 10 20 30 40 50 60 70 80 90 100
TIME (MIN)

Fig. 6. Effect of addition of hydrogen peroxide on extent of degumming using ultrasound.

40 N.S. More, P.R. Gogate / Journal of Food Engineering 218 (2018) 33e43

100

90

80
EXTENT OF DEGUMMING (%)

70

60

50

40
US HORN+H2O2(100 PPM)
30
UV HORN+H2O2 (200 PPM)
20 US HORN+H2O2 (500 PPM)

10

0
0 20 40 60 80 100 120
TIME (MIN)

Fig. 7. Effect of combination of ultrasonic horn and hydrogen peroxide on extent of degumming at large scale capacity of 1 L.

Subsequently, scale up studies were also performed using both (90e91%) for 100 PPM and 200 PPM H2O2 concentration and higher
US horn and bath at 1 L operating volume of crude soybean oil at extent of degumming as 94.5% was observed at 500 PPM H2O2
fixed power. Effect of hydrogen peroxide (100 PPM, 200 PPM, 500 concentration. On the other side, US bath treatment resulted in
PPM) on extent of degumming was again investigated and the maximum degumming (97.48%) at 100 PPM H2O2.Generally,
obtained results depicted in Fig. 7 and Fig. 8. It was observed that hydrogen peroxide dissociates to form hydroxyl radicals and the
degumming using US horn resulted in similar degumming quantum is dependent on cavitational activity.US bath resulted in

100

90

80
EXTENT OF DEGUMMING (%)

70

60

50

40

30 UV Bath+H2O2 (100 PPM)

20 US Bath+H2O2 (200 PPM)

10 US Bath+H2O2 (500 PPM)

0
0 20 40 60 80 100 120
TIME (MIN)

Fig. 8. Effect of combination of ultrasonic bath and hydrogen peroxide on extent of degumming at large scale capacity of 1 L.
 N.S. More, P.R. Gogate / Journal of Food Engineering 218 (2018) 33e43 41

100

90

80
EXTENT OF DEGUMMING (%)

70

60

50

40

30

20

10

0
0 20 40 60 80 100 120 140
TIME (MIN)

Fig. 9. Scale up study (5 L) using combined operation of hydrodynamic cavitation and hydrogen peroxide.

higher degumming yield compared to US horn and more impor-
tantly at lower loading of hydrogen peroxide attributed to the fact
that higher number of transducers are available in the case of ul-
trasonic bath which produces cavitational activity over a large
active zone as compared to ultrasonic horn (operated at 1L capac-
ity) giving higher extent of dissociation of H2O2 and hence higher
quantum of free radicals.
3.5. Scale up studies using hydrodynamic cavitation (HC) in
combination with hydrogen peroxide
Pilot scale degumming studies were also performed using hy-
drodynamic cavitation set up under operating conditions of inlet
pressure of 4 bar (optimum established as per earlier studies of
Barik and Gogate (2016), Patil et al. (2014) performed in the same


reactor) and temperature of 54 ± 2 C with the addition of 100 PPM
H2O2 for 140 min of treatment. The obtained results have been
shown in Fig. 9. It can be observed that extent of degumming in-
creases with respect to the time significantly till 100 min (89%) and
further increase to 140 min resulted in marginal increase in the
obtained maximum extent of degumming (93.65%). The crude oil
was continuously circulated through the pipe exposing the same to
cavitating conditions inducing the formation of hydroxyl radicals
(Moholkar et al., 1999; Patil et al., 2014) transforming the remaining
phospholipid derivatives to easily separate from the oil mixture.
The studies with hydrodynamic cavitation also established that
major issues in terms of clogging and chocking due to the precip-
itation of gum inside the pipeline occurred, which means that
closed loop setup is not proper for processing the soybean oil.
Considering these processing problems, further optimization
studies for the hydrodynamic cavitation were not performed.
3.6. Comparative analysis of cavitational yield for ultrasonic bath
and horn
The effectiveness of different degumming approaches in terms
of the extent of degumming, synergistic index (f) and cavitational
yield (described as the extent of phospholipid reduction per unit
energy consumption) have been investigated (Bolton et al., 2001;
Gogate and Bhosale, 2013; Bagal et al., 2013; Capocelli et al.,
2014). The details of calculations for all these parameters
have been given in Appendix 1 and 2. The obtained data has
also been summarized in Table 3. It has been observed that com-
bined approach of ultrasound and H2O2 resulted in maximum

Table 3
Comparison of extent of degumming, synergistic index and cavitational yield for different approaches.

Scheme Extent of degumming Synergistic index (F) Cavitational Yield

(%) (Including power required for heating
and stirring) (mg/J)

Only Ultrasonic(US) Horn 81.12 e 4.33  106

US Horn þ Temperature Study 92.5 e 2.51  106
US Horn þ Ozone 90.9 1.15 3.46  106
US Horn þ H2O2 (250 ml) 99.51 3.85 5.18  106
US Horn þ H2O2 (1L) 94.4 1.65 6.81  106
US Bath þ H2O2 (1L) 97.5 2.15 1.11  105
Hydrodynamic cavitation þ H2O2 93.7 1.85 3.75  105
42 N.S. More, P.R. Gogate / Journal of Food Engineering 218 (2018) 33e43

cavitational yield (5.18  106 mg/J with synergistic index as 3.85 phospholipid removal during pilot scale studies performed at 5 L
for the case of ultrasonic horn) in comparison with only ultrasound batch volume though the closed loop setup did show processing
(4.33  106 mg/J), ultrasound combined with heating treatment problems. Overall, it has been established that cavitation based
(2.51  106 mg/J) and ultrasound combined with ozone degumming approach results in intensified processing of crude
(3.46  106 mg/J with synergistic index as 1.15). For the large scale soybean oil with significant reduction in phospholipid concentra-
operation, combination approach of ultrasonic bath and H2O2 tion in less treatment time.
resulted in maximum cavitational yield as 1.11  105 mg/J and
synergistic index of 2.15 giving 97.5% as the extent of degumming. Acknowledgement
The obtained values were significantly higher than the cavitational
yield obtained using ultrasonic horn (6.81  106 mg/J), which Authors would like to acknowledge the University Grant Com-
confirmed better cavitational activity for the ultrasonic bath at mission- Basic Scientific Research (UGC-BSR) Government of India,
larger scale of operation due to higher number of transducers. The New Delhi, India for providing research funding for fellowship to
approach of using hydrodynamic cavitation (HC) resulted in sub- NSM and Maharashtra Oil Extractions Pvt. Ltd., Dhule, Maharashtra
stantially lower reduction in the phospholipid concentration of (India) for coordination in research work.
about 93.7% for 5 L operating volume giving 3.75  105 mg/J as the
cavitational yield. Hydrodynamic cavitation also results in effects
Appendix 1. Cavitational yield
similar to the ultrasound such as significant local release of energy
and production of the free radicals (Moholkar and Pandit, 1997;
1.1. Ultrasonic horn
Rajoriya et al., 2016) though these were not found to be very
effective as compared to ultrasound in the present case of
Reaction time: 100 min
degumming.
Batch volume: 250 ml
US power dissipation: 120 W
4. Conclusions Centrifuge power: 350 W
Magnetic Stirrer: 300 W
A novel cavitation assisted degumming approach was demon- Total Power dissipation: 770 W

Degradation Obtained ¼ ðExtent of degumming  Initial phospholipid concentrationÞ= 100

¼ ð81:12  98:75Þ = 100 ¼ 80:106 mg=L

Power Density ¼ ðTotal power dissipation  Treatment time in secondsÞ = Batch volume in L
¼ ð770  100  60Þ = 0:25 ¼ 18480000 J=L`
Cavitational Yield ¼ Degradation Obtained = Power Density
¼ 80:1 = 18480000 ¼ 4:33  106 mg=J

strated for the efficient phospholipid removal giving better yield 1.2. Ultrasonic bath
and efficacy as compared to the conventional degumming pro-
cesses. The optimized protocol for maximum benefits was based on Reaction time: 120 min
combination of ultrasound and hydrogen peroxide at elevated Batch volume: 1 L
temperature. Hydrogen peroxide played a vital role in the desired US Power dissipation: 120 W
formation of hydroxyl radicals which resulted in enhanced Water bath power (for temperature control): 750 W
degumming quantified in terms of total phospholipid removal. Centrifuge power: 350
Combination of ultrasonic horn and hydrogen peroxide (100 PPM) Total power dissipation: 1220 W

Degradation Obtained ¼ ðExtent of degumming  Initial phospholipid concentrationÞ= 100

¼ ð97:5  98:75Þ = 100 ¼ 96:28 mg=L
Power Density ¼ ðTotal power dissipation  Treatment time in secondsÞ = Batch volume in L
¼ ð1220  120  60Þ = 1 ¼ 8784000 J=L`
Cavitational Yield ¼ Degradation Obtained = Power Density
¼ 80:1 = 8784000 ¼ 1:1  105 mg=J

resulted in complete phospholipid degradation under lab scale 1.3. Hydrodynamic cavitation
studies. Satisfactory degumming results (93.5%) were also obtained
during scale up studies using ultrasonic bath and hydrogen Reaction time: 140 min
peroxide at 1 L operating volume. Hydrodynamic cavitation in Batch volume: 5 L
combination with hydrogen peroxide also resulted in 93.65% Pump power dissipation: 1120 W
 N.S. More, P.R. Gogate / Journal of Food Engineering 218 (2018) 33e43
Centrifuge power: 350 W
Total power dissipation: 1470 W
Degradation Obtained ¼ ðExtent of degumming  Initial phospholipid concentrationÞ= 100
¼ ð93:67  98:75Þ = 100 ¼ 92:52 mg=L
Power Density ¼ ðTotal power dissipation  Treatment time in secondsÞ = Batch volume in L
¼ ð1470  140  60Þ = 5 ¼ 2469600 J=L`
Cavitational Yield ¼ Degradation Obtained = Power Density
¼ 92:52 = 2469600 ¼ 3:74  105 mg=J
Appendix 2. Synergistic index (f)
2.1. combination of Ultrasonic (US) horn and hydrogen peroxide
(H2O2)
Rate constant for ultrasonic horn at optimized ultrasonic power
(kUS) ¼ 0.0005 min1
Rate constant for only H2O2 ¼ 0.0008 min1
Rate constant for the combined scheme i.e. US horn and H2O2
(kUS/H2O2) ¼ 0.005 min1
Synergistic Index ð f Þ for US horn and H2 O2 combined approach
. technol. Bioprocess Eng. 20, 965e970.
¼ kUS=H2 O2 kUS þ kH2 O2 ¼ 0:005= ð0:0005 þ 0:0008Þ ¼ 3:846
References
Bagal, M.V., Lele, B.J., Gogate, P.R., 2013. Removal of 2,4-dinitrophenol using hybrid
methods based on ultrasound at an operating capacity of 7 L. Ultrason. Sono-
chemistry 20, 1217e1225.
Barik, A.J., Gogate, P.R., 2016. Ultrasonics Sonochemistry Degradation of 4-chloro 2-
aminophenol using a novel combined process based on hydrodynamic cavita-
tion, UV photolysis and ozone. Ultrason. Sonochemistry 30, 70e78.
Bolton, J.R., Bircher, K.G., Tumas, W., Tolman, C.A., 2001. Figures-of-merit for the
technical development and application of advanced oxidation technologies for
both electric- and solar-driven systems. Pure Appl. Chem. 73, 627e637.
Capocelli, M., Musmarra, D., Prisciandaro, M., Industriale, I., 2014. Chemical effect of
hydrodynamic Cavitation : simulation and experimental comparison. AIChE J.
60, 2566e2572.
Chakinala, A.G., Gogate, P.R., Burgess, A.E., Bremner, D.H., 2007. Intensification of
hydroxyl radical production in sonochemical reactors. Ultrason. Sonochem 14,
509e514.
de Carvalho, C.C., de Souza, M.P., da Silva, T.D., Gonalves, L.A.G., Viotto, L.A., 2006.
Soybeans crude oil miscella degumming utilizing ceramic membranes: trans-
membrane pressure and velocity effects. Desalination 200, 543e545.
De Moura, J.M.L.N., Gonçalves, L.A.G., Petrus, J.C.C., Viotto, L.A., 2005. Degumming of
vegetable oil by microporous membrane. J. Food Eng. 70, 473e478.
Fox, N., Austic, G., 2002. Small scale degumming techniques for oil entering the
biodiesel market. Piedmont Biofuels LLC 5, 13e18.
Gogate, P.R., 2008. Cavitational reactors for process intensification of chemical
processing applications : a critical review. Chem. Engg. Process. 47 (2016),
515e527.
Gogate, P.R., Bhosale, G.S., 2013. Comparison of effectiveness of acoustic and hy-
drodynamic cavitation in combined treatment schemes for degradation of dye
wastewaters. Chem. Engg. Process. 71, 59e69.
Haahr, A., Jacobsen, C., 2008. Emulsifier type, metal chelation and pH affect
oxidative stability of n -3-enriched emulsions. Eur. J. Lipid Sci. Technol. 110
(110), 949e961.
Hafidi, A., Pioch, D., Ajana, H., 2005. Membrane-based simultaneous degumming
and deacidification of vegetable oils. Innov. Food Sci. Emerg. Technol. 6,
203e212.
Jiang, X., Chang, M., Jin, Q., Wang, X., 2015. Application of phospholipase A1 and
phospholipase C in the degumming process of different kinds of crude oils.
Process Biochem. 50, 432e437.
Jodzis, S., Patkowski, W., 2017. Macrokinetic study on ozone boundary
43
concentration. Effect of temperature. J. Electrostat 85, 43e51.
Koris, A., Marki, E., 2006. Ceramic ultrafiltration membranes for non-solvent
vegetable oil degumming (phospholipid removal). Desalination 200,
537e539.
Koris, A., Vatai, G., 2002. Dry degumming of vegetable oils by membrane filtration.
Desalination 148, 149e153.
Lamas, D.L., Constenla, D.T., Raab, D., 2016. Effect of degumming process on
physicochemical properties of sunflower oil. Biocatal. Agric. Biotechnol. 6,
138e143.
Lamas, D.L., Crapiste, G.H., Constenla, D.T., 2014. Changes in quality and composition
of sunflower oil during enzymatic degumming process. LWT - Food Sci. Technol.
58, 71e76.
Lauterborn, W., Ohl, C.D., 1997. Cavitation bubble dynamics. Ultrason. Sonochem-
istry 4, 65e75.
Li, H., Pordesimo, L., Weiss, J., 2004. High intensity ultrasound-assisted extraction of
oil from soybeans. Food Res. Int. 37, 731e738.
Li, Y., Huang, Y., Du, W., Dai, L., Liu, D., 2015. Combined phospholipase and lipase
catalysis for biodiesel production from phospholipids-containing oil. Bio-
Lin, L., Rhee, K.C., Koseoglu, S.S., 1997. Bench-scale membrane degumming of crude
vegetable oil: process optimization. J. Memb. Sci. 134, 101e108.
Liu, K.T., Gao, S., Chung, T.W., Huang, ming, C., Lin, Sen, Y., 2012. Effect of process
conditions on the removal of phospholipids from Jatropha curcas oil during the
degumming process. Chem. Eng. Res. Des. 90, 1381e1386.
Manjula, S., Subramanian, R., 2009. Simultaneous degumming, dewaxing and
decolorizing crude rice bran oil using nonporous membranes. Sep. Purif.
Technol. 66, 223e228.
Moholkar, V.S., Kumar, P.S., Pandit, A.B., 1999. Hydrodynamic cavitation for sono-
chemical effects. Ultrason. Sonochem 6, 53e65.
Moholkar, V.S., Pandit, A.B., 1997. Bubble behavior in hydrodynamic Cavitation . Eff.
Turbul. AIChE J. 43 (1997), 1641e1648.
Niemczewski, B., 1999. Chemical activation of ultrasonic cavitation. Ultrason.
Sonochem 6, 211e216.
Ochoa, N., Pagliero, C., Marchese, J., Mattea, M., 2001. Ultrafiltration of vegetable
oils degumming by polymeric membranes. Sep. Purif. Technol. 22e23,
417e422.
Pagliero, C., Mattea, M., Ochoa, N., Marchese, J., 2007. Fouling of polymeric mem-
branes during degumming of crude sunflower and soybean oil. J. Food Eng. 78,
194e197.
Patil, P.N., Bote, S.D., Gogate, P.R., 2014. Degradation of imidacloprid using combined
advanced oxidation processes based on hydrodynamic cavitation. Ultrason. -
Sonochemistry 21, 1770e1777.
Prajapat, A.L., Gogate, P.R., 2016. Intensification of depolymerization of polyacrylic
acid solution using different approaches based on ultrasound and solar irradi-
ation with intensification studies. Ultrason. Sonochem 32, 290e299.
Qu, Y., Sun, L., Li, X., Zhou, S., Zhang, Q., Sun, L., Yu, D., Jiang, L., Tian, B., 2016.
Enzymatic degumming of soybean oil with magnetic immobilized phospholi-
pase A2. LWT - Food Sci. Technol. 73, 290e295.
Rajoriya, S., Carpenter, J., Saharan, V.K., Pandit, A.B., 2016. Hydrodynamic cavitation :
an advanced oxidation process for the degradation of bio-refractory pollutants.
Rev. Chem. Eng. 32 (4), 379e411.
Rao, P.R., Rathod, V.K., 2015. Mapping study of an ultrasonic bath for the extraction
of andrographolide from Andrographis paniculata using ultrasound. Ind. Crops
Prod. 66, 312e318.
Sicaire, A.G., Vian, M.A., Fine, F., Carre , P., Tostain, S., Chemat, F., 2016. Ultrasound
induced green solvent extraction of oil from oleaginous seeds. Ultrason.
Sonochem 31, 319e329.
Sivasankar, T., Moholkar, V.S., 2009. Physical insights into the sonochemical
degradation of recalcitrant organic pollutants with cavitation bubble dynamics.
Ultrason. Sonochemistry 16, 769e781.
Yu, D., Ma, Y., Xue, S.J., Jiang, L., Shi, J., 2013. Characterization of immobilized
phospholipase A1 on magnetic nanoparticles for oil degumming application.
LWT - Food Sci. Technol. 50, 519e525.