energies

Article
Physiochemical and Electrical Properties of Refined,
Bleached and Deodorized Palm Oil under High
Temperature Ageing for Application in Transformers
Nur Aqilah Mohamad 1 , Norhafiz Azis 1,2, *, Jasronita Jasni 1 , Mohd Zainal Abidin Ab Kadir 1,3 ID
,
Robiah Yunus 4 and Zaini Yaakub 5
1 Centre for Electromagnetic and Lightning Protection Research (CELP), Department of Electrical and
Electronic Engineering, Universiti Putra Malaysia, 43400 Serdang, Selangor, Malaysia;
qieylaqilah@gmail.com (N.A.M.); jas@upm.edu.my (J.J.); mzk@upm.edu.my (M.Z.A.A.K.)
2 Institute of Advanced Technology (ITMA), Universiti Putra Malaysia, 43400 Serdang, Selangor, Malaysia
3 Institute of Power Engineering (IPE), Universiti Tenaga Nasional, 43000 Kajang, Selangor, Malaysia
4 Department of Chemical and Environmental Engineering, Faculty of Engineering, Universiti Putra Malaysia,
43400 Serdang, Selangor, Malaysia; robiah@upm.edu.my
5 Hyrax Oil Sdn. Bhd, Lot 4937 Batu 5 1/2, Jalan Meru, Mukim Kapar, 41050 Klang, Selangor, Malaysia;
zaini@hyraxoil.com
* Correspondence: norhafiz@upm.edu.my; Tel.: +60-3-8946-4373




Received: 15 May 2018; Accepted: 5 June 2018; Published: 16 June 2018


Abstract: This paper presents a high temperature ageing study of refined, bleached, and deodorized
palm oil (RBDPO) olein at 170 ◦ C in the presence of air. In total, two types of RBDPO were examined.
The physiochemical and dielectric properties of RBDPO were measured and analysed. We found
that the moisture and viscosities for both RBDPO increased as the ageing progressed, whereas the
acidities fluctuated at very low levels at less than 0.005 mg KOH/g. The ageing on the AC breakdown
voltages of both RBDPO were not affected throughout the ageing processes. The dielectric dissipation
factors and relative permittivities for both RBDPO increased as the resistivities decreased with the
ageing time.

Keywords: high temperature thermal ageing; open condition; refined, bleached and deodorized
palm oil; physiochemical and electrical properties

1. Introduction
Palm oil (PO) has been identified as possible insulating fluid for transformer applications. PO is
included in the natural ester group and has almost the same characteristics as other types of vegetable oils,
such as having high flash and fire points, and being biodegradable and environmentally friendly [1,2].
Previous studies revealed that the electrical and physiochemical properties of new PO are close to other
types of natural esters and mineral oil (MO) [3–6]. The majority of these properties are comparable
to other types of vegetable oils under ageing at temperatures ranging from 85 to 150 ◦ C, which are
maintained at acceptable levels according to standards [7–11]. Currently, the high temperature ageing
performance of PO has not been well established and requires further investigation.
One of the main purposes of high temperature ageing is to examine the performance of vegetable
oils under extreme conditions where the influences of oxygen and moisture are also considered [12,13].
Previous high temperature ageing studies on vegetable oils examined acidity, viscosity, AC breakdown
voltage, and dielectric properties [12–18]. Several ageing studies at high temperatures ranging from
140 to 170 ◦ C showed that acidity and viscosity of natural ester can be affected by oxygen [14,17].
Natural ester showed a large increase in acidity and viscosity when aged under open conditions

Energies 2018, 11, 1583; doi:10.3390/en11061583 www.mdpi.com/journal/energies

Energies 2018, 11, 1583 2 of 13

at temperatures between 140 and 160 ◦ C [14,19]. In addition, natural ester can start to gel after
subjected to high temperature ageing at 170 ◦ C [15]. The AC breakdown voltage of natural ester is
maintained at an acceptable level regardless of the ageing conditions [16,18]. However, the dielectric
dissipation factor of natural ester can be affected by ageing at high temperatures ranging from 140 to
170 ◦ C [14,18]. A previous ageing study at 170 ◦ C showed that the dielectric dissipation factor of
natural ester increased by five- and eight-fold than the initial value when tested at 25 and 100 ◦ C,
respectively [18]. The ageing of natural ester at temperatures between 140 and 160 ◦ C has been reported
to cause a three- to six-fold increase in the power factor [14]. The impacts of high temperature ageing
on moisture and dissolved gases generation of natural ester vegetable oils are not clear since the trends
fluctuate as ageing progresses [12,18].
Oxidation is one of the main degradation mechanisms for natural ester. The rate of oxidation is
governed by temperature, which can be accelerated by oxygen and metal catalysts [20]. The process
begins with the initiation stage where free radicals are created as a result of the dissociation of
the hydrogen atom from the C-H bond in the fatty acid triglyceride [21,22]. Interaction between
oxygen and the free radicals initiates the propagation stage, which leads to the formation of peroxides.
These peroxides interact with the C-H bond to create hydroperoxides [22]. With the initiation of
the chain scission stage, the hydroperoxides dissociate and the interaction with oxygen promotes
further generation of radicals and peroxides [22]. The final products of oxidation, as a result of
the decomposition of hydroperoxides, are ketones, alcohols, aldehydes, and high molecular weight
polymers [20,22–24]. The secondary non-volatile compounds formed via oxidation are subjected to
cyclisation and polymerization processes. As a result, high molecular weight compounds, such as
gel and lacquer, are formed at high temperatures and pressures [22]. Apart from oxidation, natural
ester can also be subjected to the hydrolysis degradation mechanism. The process has three stages that
begin with the formation of diglyceride as result of the interaction between triglyceride and water [25].
Further interactions between diglyceride and water lead to the formation of monoglyceride [25].
Glycerol is produced as a final product from the interaction between monoglyceride and water [25].
All stages in the hydrolysis of natural ester are reversible and fatty acids are produced at each of
the stages [25].
In this paper, a high temperature ageing study, in the presence of air at 170 ◦ C for 28 days,
was completed on refined, bleached, and deodorized palm oil (RBDPO). Multiple physiochemical and
electrical properties measurements were recorded and analysed.

2. Materials and Methods

2.1. Thermal Ageing Procedure

Two different RBDPO were tested as shown in Table 1. Both RBDPO were olein types from
cooking products on the market. The fatty acid composition for both RBDPO were determined
via gas chromatography analysis according to the Malaysian palm oil board (MPOB) test methods
p3.4:2004 and p3.5:2204, as shown in Table 1 [26]. Both RBDPO had almost balanced compositions of
fatty acids dominated by palmitic and oleic acids.
The oil was first filtered through a membrane filter and was dried in the oven for 48 h at 85 ◦ C.
The final moisture contents for both RBDPO were less than 120 ppm. Next, both RBDPO were sealed
and left at room temperature for 24 h before being placed inside an air circulating oven at 170 ◦ C.
Each RBDPO was aged individually in a separate borosilicate glass bottle. The oil samples were aged
under open conditions for 7, 14, 21 and 28 days.
Energies 2018, 11, 1583 3 of 13

Table 1. Fatty acid compositions of all samples.

Sample (%)
Types of Fats Types of Fatty Acids
RBDPO A RBDPO B
C6: Caproic - -
C8: Caprylic - -
C10: Capric - -
Saturated C12: Lauric 0.3 0.3
C14: Myristic 1.1 0.9
C16: Palmitic 37.7 39.0
C18: Stearic 3.9 4.2
Mono-unsaturated C18: Oleic 42.3 43.0
C18: Linoleic 12.4 10.4
Poly-unsaturated
C18: Linolenic 0.3 0.2
Others 0.1 0.1

2.2. Measurement of Properties

2.2.1. Moisture Content

A Metrohm 831 Karl Fischer (KF) Coulometer was used to measure moisture based on ASTM
D 6304 [27]. In total, 1 g of RBDPO was used for each of the measurements. For each of the samples,
two measurements were carried out in order to obtain the mean value.

2.2.2. Acidity
The measurement of acidity was performed according to ASTM D 974 with a Metrohm SM Titrino
702 [28]. For each of the measurements, 10 g of RBDPO were used where only one measurement was
performed for each of the samples.

2.2.3. Viscosity
The viscosity was determined based on ASTM D 445 using a SVM 3000 Stabinger viscometer [29].
In total, 5 mL of RBDPO were used for the measurement. In this study, only one measurement at 40 ◦ C
was recorded for each of the RBDPO.

2.2.4. AC breakdown Voltage

A BAUR DPA 75C was used to determine AC breakdown voltage according to ASTM D 1816 [30].
The measurement was obtained based on two VDE electrodes (diameter = 36 mm) where the distance
between these electrodes was set to 1 mm. These electrodes were fully immersed in 400 mL of
RBDPO used for the test. The voltage increased at rate of 0.5 kV/s with a 5 min interval between each
breakdown. To obtain the mean value, 50 measurements of AC breakdown voltages were recorded for
each of the samples.

2.2.5. Dielectric Dissipation Factor, Relative Permittivity and Resistivity

Dielectric properties of RBDPO was measured using a BAUR DTL C oil tester according to IEC
60247 [31]. In total, 45 mL of RBDPO were used for the measurement and only one measurement at
90 ◦ C and 50 Hz was recorded for each of the RBDPO. The applied voltages for dielectric dissipation
factor, relative permittivity, and resistivity measurement were 1999 V (AC) and 500 V (DC), respectively.
Energies 2018, 11, 1583 4 of 13

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3. Results
3. Results
Energies 2018, 11, x FOR PEER REVIEW 4 of 13
3.1. Physicochemical Properties
3.1. Physicochemical Properties
3. Results
3.1.1. Moisture
3.1.1. Moisture
3.1. Physicochemical Properties
Overall, both RBDPO A and RBDPO B had almost the same increasing trend in moisture as
in Overall,
shown3.1.1.
Figure 1.both RBDPO A and RBDPO B had almost the same increasing trend in moisture as
The moisture for both RBDPO slightly decreased with ageing up to 14 days
shownMoisture
in Figure 1. The moisture for both RBDPO slightly decreased with ageing up to 14 days and
and subsequently increased as the ageing progressed. After 28 days of ageing, the moisture for
subsequently
Overall, increased
both RBDPO as the ageing
A and progressed.
RBDPO B had After
almost28the
days of ageing,
same the trend
increasing moisture for RBDPO
in moisture as
RBDPOA A and
and
shown
RBDPO
RBDPO B were
in Figure
B were
1. The254
254and
ppm
moisture
ppm and
for225
225
ppm,
both
ppm, respectively.
respectively.
RBDPO slightly decreased with ageing up to 14 days and
subsequently increased as the ageing progressed. After 28 days of ageing, the moisture for RBDPO
A and RBDPO B were 254 ppm and 225 ppm, respectively.

Figure 1. Moisture of refined, bleached, and deodorized palm oil (RBDPO) aged at 170 °C under open
Figure 1. Moisture of refined, bleached, and deodorized palm oil (RBDPO) aged at 170 ◦ C under
conditions.
open conditions.
Figure 1. Moisture of refined, bleached, and deodorized palm oil (RBDPO) aged at 170 °C under open
3.1.2. conditions.
Acidity
3.1.2. Acidity
3.1.2.No clear trend was observed in the acidities for either RBDPO as shown in Figure 2. The acidity
Acidity
Noof clear
RBDPO A slightly
trend decreased
was observed in after 7 days offor
the acidities ageing
eitherand increased
RBDPO after 14indays.
as shown However,
Figure the
2. The acidity of
Noofclear
acidity trendB was
RBDPO observed
fluctuated in the acidities
between 0.0015 mgforKOH/g
either RBDPO
and as shown
0.0029 mg in Figure
KOH/g. Both2.RBDPO
The acidity
had
RBDPO A slightly decreased after 7 days of ageing and increased after 14 days. However, the acidity
of RBDPO
very A slightly
low acidities evendecreased afterof7ageing.
after 28 days days of ageing and increased after 14 days. However, the
of RBDPO B of
acidity fluctuated
RBDPO B between
fluctuated0.0015
between mg KOH/g
0.0015 and 0.0029
mg KOH/g mg mg
and 0.0029 KOH/g.
KOH/g.Both
Both RBDPO
RBDPO hadhad very
low acidities even after 28 days of ageing.
very low acidities even after 28 days of ageing.

Figure 2. Acidity of RBDPO aged at 170 °C under open condition.

Figure 2. Acidity of RBDPO aged at 170 °C under open condition.

Figure 2. Acidity of RBDPO aged at 170 ◦ C under open condition.
Energies 2018, 11, 1583 5 of 13
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3.1.3. Viscosity
3.1.3. Viscosity
The viscosity
The viscosity of
of RBDPO
RBDPO A A remained
remained almost
almost unchanged
unchanged during
during thethe first
first 14
14 days
days of
of ageing
ageing as
as
shown in Figure 3. After 14 days of ageing, the viscosity of RBDPO A increased and
shown in Figure 3. After 14 days of ageing, the viscosity of RBDPO A increased and remains almost remains almost
unchanged from 21 to 28 days.
unchanged days. The
The viscosity
viscosityofofRBDPO
RBDPOBBslightly
slightlydecreased
decreasedduring
duringthethefirst 7 days
first of
7 days
ageing
of andand
ageing then increased
then exponentially
increased as the
exponentially asageing progresses.
the ageing After After
progresses. 28 days28ofdays
ageing, the highest
of ageing, the
viscosities
highest for RBDPO
viscosities A and RBDPO
for RBDPO B were 50.8
A and RBDPO cSt 50.8
B were and cSt
70.9and
cSt,70.9
respectively.
cSt, respectively.

Figure
Figure 3.
3. Viscosity
Viscosity of
of RBDPO
RBDPO aged
aged at
at 170 ◦ Cunder
170 °C under open
open conditions.
conditions.

3.2.
3.2. Electrical
ElectricalProperties
Properties

3.2.1.
3.2.1. AC
ACBreakdown
Breakdown Voltage
Voltage
RBDPO
RBDPO BB had had aa higher
higher AC
AC breakdown
breakdown voltage voltage than
than RBDPO
RBDPO A A throughout
throughout the the ageing
ageing period
period
with
with differences
differences inin percentages
percentages between
between 9.3% 9.3% and
and 40.9%,
40.9%, as as shown
shown in in Figure
Figure 4.4. The
The AC
AC breakdown
breakdown
voltage
voltage ofof RBDPO
RBDPO A A slightly
slightlydecreased
decreasedduring duringthe thefirst
first77days
daysof ofageing
ageingand andincreased
increasedafter
after14
14days.
days.
For
For RBDPO
RBDPO B, B, the
the AC
AC breakdown
breakdown voltage
voltage fluctuated
fluctuated between
between 41.3 41.3 kV
kV and
and 55.2
55.2 kV
kV throughout
throughout the the
ageing
ageing period.
period.
The
The AC
AC breakdown
breakdown voltages
voltages for
for both
both RBDPO
RBDPO were were analysed
analysed based based onon cumulative
cumulative normal
normal andand
Weibull distributions. Equation (1) shows the cumulative normal distribution
Weibull distributions. Equation (1) shows the cumulative normal distribution where µ is the mean where µ is the mean of
the breakdown
of the breakdown voltage
voltagedata
dataand
and σσ is isthe
thestandard
standarddeviation.
deviation.EquationEquation(2) (2)shows
shows the
the cumulative
cumulative
Weibull,
Weibull, where α, α, ββ and
and xx are
are the
the scale
scale and
and shape
shape parameters
parameters and and breakdown
breakdown voltages
voltages for
for each
each of
of the
the
samples,
samples, respectively.
respectively.
1 w x −( t − µ )2
F ( x |µ, σ ) = √ 1 e ( 2σ2) dt (1)
( | , )= σ
2π −∞ (1)
√2
t β
F ( x |α, β) = 1 − e−( α ) (2)
( | , )= 1− (2)
The breakdown voltage of RBDPO A is well-represented by normal distribution compared to
The breakdown voltage of RBDPO A is well-represented by normal distribution compared to
the Weibull distribution, as shown in Figure 5. Conversely, Weibull distribution better represents
the Weibull distribution, as shown in Figure 5. Conversely, Weibull distribution better represents the
the breakdown voltage of RBDPO B. For all ageing times, we found that the breakdown voltage
breakdown voltage of RBDPO B. For all ageing times, we found that the breakdown voltage of both
of both RBDPO at 1% probability for normal distribution was higher than Weibull distribution,
RBDPO at 1% probability for normal distribution was higher than Weibull distribution, as shown in
as shown in Table 2. At 50% probability, the majority of the breakdown voltage of both RBDPO for
Weibull distribution was higher than normal distribution. For normal distribution and 1% probability,
the lowest breakdown voltages for RBDPO A and B were 21.94 kV and 26.23 kV, whereas they were
19.95 kV and 19.8 kV for Weibull distribution, respectively.
Energies
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2018, 11,
11, xx FOR
FOR PEER
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Table
Table 2. 2. At
At 50%
50% probability,
probability, the
the majority
majority of
of the
the breakdown
breakdown voltage
voltage of
of both
both RBDPO
RBDPO for
for Weibull
Weibull
distribution
distribution was higher than normal distribution. For normal distribution and 1% probability, the
was higher than normal distribution. For normal distribution and 1% probability, the
lowest
lowest breakdown
breakdown
Energies 2018,
voltages for RBDPO A and B were 21.94 kV and 26.23 kV, whereas they were 19.95
11, 1583 voltages for RBDPO A and B were 21.94 kV and 26.23 kV, whereas they were 19.95
6 of 13
kV
kV and
and 19.8
19.8 kV
kV for
for Weibull
Weibull distribution,
distribution, respectively.
respectively.

Figure
Figure 4.
Figure 4. AC
4. ACbreakdown
AC breakdown voltage
breakdown voltage of
voltage of RBDPO
of RBDPO aged
RBDPO aged at
aged at 170
at 170 °C
170
◦ Cunder
°C underopen
under open conditions.
open conditions.
conditions.

(a)
(a)

(b)
(b)
Figure
Figure 5. Probability plot of RBDPO aged at 170 °C under open conditions: (a) normal distribution
Figure 5.
5. Probability
Probability plot
plot of
of RBDPO
RBDPO aged
aged at
at 170
170 °C
◦ C under
under open
open conditions:
conditions: (a)
(a) normal
normal distribution
distribution
and
and (b) Weibull distribution.
and (b)
(b) Weibull
Weibull distribution.
distribution.
Energies 2018,
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Table 2. Withstand voltage based on normal and Weibull distribution at 1% and 50% probability.
Table 2. Withstand voltage based on normal and Weibull distribution at 1% and 50% probability.
Normal Distribution Weibull Distribution
Samples Ageing Time (Days) Normal
Samples Ageing Time (Days) 1% Distribution
50% Weibull
1% Distribution
50%
0 1%
23.56 50%
39.37 1%
21.6 50%
39.97
70 21.94
23.56 35.84
39.37 19.95
21.6 36.41
39.97
RBDPO A 147 21.94
24.18 35.84
36.43 19.95
22.22 36.41
36.98
RBDPO A 2114 24.18
23.8 36.43
41.02 22.22
22.35 36.98
41.71
21 23.8 41.02 22.35 41.71
2828 28.23
28.23
43.96
43.96
25.86
25.86
44.63
44.63
0 29.2 41.27 19.80 40.9
0 29.2 41.27 19.80 40.9
77 37.38
37.38 52.71
52.71 37.14
37.14 53.51
53.51
RBDPO
RBDPOBB 1414 37.4
37.4 55.22
55.22 35.86
35.86 56.08
56.08
2121 26.23
26.23 45.19
45.19 23.90
23.90 45.86
45.86
2828 35.06
35.06 51.74
51.74 32.29
32.29 52.5
52.5

3.2.2. Dielectric
3.2.2. Dielectric Dissipation
Dissipation Factor
Factor
Figure 66 shows
Figure shows that
that the
the trends
trends in
in the
the dielectric
dielectric dissipation
dissipation factors
factors for
for both
both RBDPO
RBDPO areare the
the same
same
as for viscosity. The dielectric dissipation factor for RBDPO A increased steadily initially,
as for viscosity. The dielectric dissipation factor for RBDPO A increased steadily initially, and then and then
slightly decreased
slightly decreased after
after 21
21 days
days of ageing. The The dielectric
dielectric dissipation
dissipation factor
factor of
of RBDPO
RBDPO BB increased
increased
exponentially throughout
exponentially throughout the ageing time.

Figure
Figure 6.
6. Dielectric
Dielectric dissipation
dissipation factor
factor of
of RBDPO
RBDPO aged
aged at
at 170 ◦ C under
170 °C under open
open conditions.
conditions.

3.2.3.
3.2.3. Resistivity
Resistivity
The
The resistivities for both
resistivities for both RBDPO
RBDPOshowed
showedclear
cleardecreasing
decreasingtrends
trendsasasshown
shownininFigure
Figure 7. 7. RBDPO
RBDPO A
A experienced a steady reduction in resistivity until 21 days of ageing. The resistivity of RBDPO
experienced a steady reduction in resistivity until 21 days of ageing. The resistivity of RBDPO A remained A
remained almost unchanged
almost unchanged between 21 between
and 2821 andof
days 28ageing.
days of ageing. The resistivity
The resistivity of RBDPO of RBDPO B decreased
B decreased almost
almost linearly as the ageing progressed. The resistivity of RBDPO A was slightly higher
linearly as the ageing progressed. The resistivity of RBDPO A was slightly higher than RBDPO B at all than RBDPO
Bageing
at all times.
ageingRBDPO
times. RBDPO A and RBDPO
A and RBDPO B suffered
B suffered 86.6%and86.6%and 93.7% reductions
93.7% reductions in resistivities
in resistivities at the end at
of
the end of the ageing time,
the ageing time, respectively. respectively.
Energies 2018, 11, 1583 8 of 13
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Figure 7. Resistivity of RBDPO aged

Figure 7. aged at 170 ◦°C
at 170 C under open conditions.

3.2.4. Relative Permittivity

Figure 88 shows
showsthe
theslightly
slightlyincreasing
increasingtrend of of
trend thethe
relative permittivity
relative for both
permittivity RBDPO.
for both The
RBDPO.
relative
The permittivity
relative of RBDPO
permittivity of RBDPO A was almost
A was almostunchanged
unchangedafter
after2121days
daysof
of ageing.
ageing. The
The relative
relative
permittivity of RBDPO B increased almost linearly throughout the ageing period. After 28 of ageing,
permittivity
the relative permittivity of RBDPO A and RBDPO B increased by 7.8% and 12.9% as compared to the
respectively.
initial values, respectively.

Figure 8. Relative permittivity of RBDPO aged at 170 ◦°C

C under open conditions.

4. Discussion
A previous study
study [8] revealed that there is no apparent effect of the ageing on the physiochemical
that there physiochemical
electrical properties
and electrical RBDPO at
properties RBDPO 115 ◦°C
at 115 C under open conditions. However,
However, the current study shows
that several physicochemical and electrical properties
properties of both RBDPO were affected by an ageingageing
temperature of
temperature of 170 ◦
170 °C conditions.
C under open conditions.
Apparent moisture increases were observed for both RBDPO (Figure 1). Apart from ageing,
possible moisture ingression may have occurred from the exterior, since the experiment was
Energies 2018, 11, 1583 9 of 13

Apparent
Energies moisture
2018, 11, x FOR increases
PEER REVIEW were observed for both RBDPO (Figure 1). Apart from ageing, 9 of 13
possible moisture ingression may have occurred from the exterior, since the experiment was performed
under open under
performed conditions.
openInconditions.
natural ester,In the triglycerides
natural ester, thewill interact withwill
triglycerides moisture
interactduring
withhydrolysis
moisture
to generate
during fatty acids
hydrolysis [32]. However,
to generate the presence
fatty acids of moisture
[32]. However, the had no apparent
presence effect had
of moisture on thenohydrolysis
apparent
of RBDPO,
effect on thesince the acidity
hydrolysis remained
of RBDPO, sincelowthe(Figure
acidity 2). The acidities
remained of both
low (Figure 2).RBDPO in thisofstudy
The acidities both
RBDPO
remainedinlowerthis study remained
than 0.005 mg KOH/glower at than 0.005 mg
all ageing KOH/g
times. at all ageing
Meanwhile, times. in
the increase Meanwhile,
the viscositiesthe
increase in the viscosities
of both RBDPO (Figure 3)ofwerebothexpected
RBDPO and (Figure 3) were
in line withexpected
previous and in line
studies with The
[14,20]. previous studies
triglycerides
[14,20].
moleculesThewere
triglycerides
exposedmolecules were in
to air, which exposed to air, which
turn initiated in turnscission
the chain initiatedandthe chain
cross scission
linking and[33].
cross
Large linking
molecules [33]. Large
were molecules
generated that were
change generated that change
the molecular weight andthe molecular weight
lead to changes andviscosity
in the lead to
changes
of naturalinester
the viscosity
[33]. of natural ester [33].
The
The effect
effect ofofthethecurrent
currentageing
ageingstudy
studyonon thethe
ACAC breakdown
breakdown voltages
voltagesof both RBDPO
of both RBDPO was wasnot
apparent, as shown
not apparent, in Figure
as shown 4. Furthermore,
in Figure Figure Figure
4. Furthermore, 9 shows9 thatshowsno clear relationship
that no exists between
clear relationship exists
moisture and AC breakdown
between moisture voltages ofvoltages
and AC breakdown both RBDPO.
of bothSince
RBDPO. the moisture
Since thesaturation
moisture limit of RBDPO
saturation limit
was not available,
of RBDPO was notthe effect ofthe
available, moisture
effect ofonmoisture
the AC on breakdown voltage could
the AC breakdown not be
voltage couldexamined
not be
extensively. The increases
examined extensively. in the dielectric
The increases dissipation
in the dielectric factorsfactors
dissipation of both RBDPO
of both RBDPOwerewere similar
similarto
viscosities (Figures
to viscosities (Figures6 and 10). 10).
6 and The dielectric dissipation
The dielectric factorfactor
dissipation is known as an indicator
is known of the degree
as an indicator of the
of contamination
degree of contaminationand moisture in dielectric
and moisture insulating
in dielectric fluids fluids
insulating [34]. Apart from moisture,
[34]. Apart from moisture,large
molecules generated
large molecules as a result
generated as aofresult
thermal polymerization
of thermal are suspected
polymerization to also affect
are suspected the affect
to also dielectric
the
dissipation factors andfactors
dielectric dissipation viscosities of both RBDPO,
and viscosities of bothasRBDPO,
shown as in shown
Figuresin 10Figures
and 11 10 [35].
andFor11 both
[35].
RBDPO,
For both the
RBDPO,decrease
the in the resistivities
decrease in Figuresin
in the resistivities 7 and
Figures12 are in line
7 and with
12 are inthe
lineincrease
with theinincrease
moisture. in
The slight increase in the relative permittivity in Figures 8 and 13 are consistent
moisture. The slight increase in the relative permittivity in Figures 8 and 13 are consistent with the with the increases in
viscosities,
increases inwhich indicate
viscosities, changes
which in the
indicate chemical
changes structures
in the chemicalofstructures
both RBDPO. of both RBDPO.

Figure 9.
9. Relationship
Relationship between
between AC
AC breakdown ◦ C under
breakdown voltage and moisture of RBDPO aged at 170 °C under
open conditions.
 Energies2018,
Energies
Energies 11,xx1583
2018,11,
2018, 11, FOR PEER
FOR PEER REVIEW
REVIEW 10of
10
10 of13
of 13
13

Figure 10.
Figure10.
Figure Relationship between
Relationshipbetween
10.Relationship dielectric
betweendielectric dissipation
dielectricdissipation factor
dissipationfactor and
factorand viscosity
andviscosity of
viscosityof RBDPO
ofRBDPO aged
RBDPOaged at
agedat 170
at170 ◦C
°C
170°C
under open
underopen
under conditions.
openconditions.
conditions.

Figure 11.
Figure11. Relationship between
Relationshipbetween
11.Relationship dielectric
betweendielectric dissipation
dielectricdissipation factor
dissipationfactor and
factorand moisture
andmoisture of
moistureof RBDPO
ofRBDPO aged
RBDPOaged at
agedat 170
at170 ◦C
°C
170°C
Figure
under open
underopen
under conditions.
openconditions.
conditions.
 Energies 2018, 11, 1583 11 of 13
Energies 2018,
Energies 2018, 11,11, x FOR
x FOR PEER
PEER REVIEW
REVIEW 11 ofof
11 1313

Figure
Figure 12.
Figure12. Relationship
12.Relationship between
between
Relationship resistivity
resistivity
between andmoisture
and
resistivity moisture
and ofofRBDPO
moisture RBDPO agedat
aged
of RBDPO at170
aged 170 °C°C
at under
under
170 open
◦ C open
under
conditions.
open conditions.
conditions.

Figure13.
13.Relationship
Relationship between relative permittivity and moisture ◦ C under
Figure Relationship between
between relative
relative permittivity
permittivity and
and moisture ofof
moisture of RBDPO
RBDPO
RBDPO aged
agedatat170
aged 170°C°Cunder
open conditions.
open conditions.

5.5. Conclusions
5.Conclusions
Conclusions

InIn this
Inthis
this study,
study,the
study, the physiochemical
thephysiochemical
physiochemicaland and electrical
andelectrical properties
propertiesofof
electricalproperties RBDPO
ofRBDPO
RBDPOwere were affected
wereaffected
affectedbyby the
bythe ageing
theageing
ageing
scheme at
schemeatat170
scheme 170 °C
◦
170°CCand and in
andininthethe presence
thepresence
presenceof of air.
of air. The moisture and viscosities
air. The moisture and viscosities
viscosities of of both
ofboth RBDPO
bothRBDPO increased
RBDPOincreased
increasedas
asas
thethe
the ageing
ageing
ageing time time
time increased.
increased.
increased. Theacidities
TheThe acidities
acidities ofofboth
of both bothRBDPO
RBDPO RBDPO
were notwere
were notaffected
affected
not affectedbybythe
by the ageing theand
ageing and
remained
ageing and
remained
low throughout
remained lowthroughout
low throughout
the ageing the
the ageingprocess.
process.
ageing process.
The AC breakdown
The AC breakdown voltages of bothvoltages of bothRBDPO
RBDPOwere werenotnotsignificantly
significantlyaffected
affectedasasthetheageing
ageing
progressed.The
progressed. Thedielectric
dielectricdissipation
dissipationfactors,
factors,resistivities,
resistivities,and
andrelative
relativepermittivities
permittivitiesofofRBDPO
RBDPOwere were
affected by the ageing, where correlations between these parameters and moisture
affected by the ageing, where correlations between these parameters and moisture and viscosity were and viscosity were
Energies 2018, 11, 1583 12 of 13

The AC breakdown voltages of both RBDPO were not significantly affected as the ageing
progressed. The dielectric dissipation factors, resistivities, and relative permittivities of RBDPO were
affected by the ageing, where correlations between these parameters and moisture and viscosity were
observed. Further study is required in the future to comprehensively examine the effect of high
temperature ageing on RBDPO in the presence of insulation paper, pressboard, and metal catalyst.

Author Contributions: The research study was successfully completed with contribution from all authors.
The main research idea, experimental works, and manuscript preparation were contributed by N.A.M. N.A.
contributed to the manuscript preparation and research idea. J.J., M.Z.A.A.K. And R.Y. assisted with finalizing the
research work and manuscript. Z.Y. provided several suggestions from an industrial perspective. All authors
revised and approved the publication of the paper.
Acknowledgments: The authors would like to thank the Ministry of Education and Universiti Putra Malaysia for
the funding provided for this study under the FRGS scheme (03-02-13-1280FR) and PUTRA Berimpak and IPS
schemes (GPB/2017/9570300) and (GP-IPS/2016/9498800, GP-IPS/2018/9605500).
Conflicts of Interest: The authors declare no conflict of interest.

References
1. Abdullahi, U.U.; Bashi, S.M.; Yunus, R.; Mohibullah; Nurdin, H.A. The Potentials of Palm Oil as a Dielectric
Fluid. In Proceedings of the IEEE International Conference on National Power and Energy (PECon),
Kuala Lumpur, Malaysia, 29–30 November 2004; pp. 224–228.
2. Azis, N.; Jasni, J.; Kadir, M.Z.A.A.; Mohtar, M.N. Suitability of Palm Based Oil as Dielectric Insulating Fluid
in Transformers. J. Electr. Eng. Technol. 2014, 9, 662–669. [CrossRef]
3. Azmi, K.; Ahmad, A.; Kamarol, M. Study of Dielectric Properties of a Potential RBD Palm Oil and RBD
Soybean Oil Mixture as Insulating Liquid in Transformer. J. Electr. Eng. Technol. 2015, 10, 709–718. [CrossRef]
4. Thien, Y.V.; Azis, N.; Jasni, J.; Kadir, M.Z.A.A.; Yunus, R.; Ishak, M.T.; Yaakub, Z. The Effect of Polarity on the
Lightning Breakdown Voltages of Palm Oil and Coconut Oil under a Non-uniform Field for Transformers
Application. Ind. Crops Prod. 2016, 89, 250–256. [CrossRef]
5. Raof, N.A.; Rashid, U.; Yunus, R.; Azis, N.; Yaakub, Z. Development of Palm-based Neopentyl Glycol Diester
as Dielectric Fluid and Its Thermal Aging Performance. IEEE Trans. Dielectr. Electr. Insul. 2016, 23, 2051–2058.
[CrossRef]
6. Jonathan, O.O.; Agber, D.J.U. Palm Oil as an Alternative Dielectric Transformer Coolant. Int. J. Res. Eng. Sci.
2014, 2, 8–13.
7. Munajad, A.; Subroto, C.; Suwarno. Study on the effects of thermal aging on insulating paper for high voltage
transformer composite with natural ester from palm oil using fourier transform infrared spectroscopy (FTIR)
and energy dispersive X-ray spectroscopy (EDS). Energies 2017, 10, 1857. [CrossRef]
8. Mohamad, N.A.; Azis, N.; Jasni, J.; Kadir, M.Z.A.A.; Yunus, R.; Ishak, M.T.; Yaakub, Z. Investigation on the
dielectric, physical and chemical properties of palm oil and coconut oil under open thermal ageing condition.
J. Electr. Eng. Technol. 2016, 11, 690–698. [CrossRef]
9. Senthilkumar, S.; Karthik, B.; Chandrasekar, S. Investigations on PD Characteristics of Thermal Aged Palm
and Corn Oil for Power Transfomers Insulation Application. J. Electr. Eng. Technol. 2014, 9, 742–751.
[CrossRef]
10. Suwarno, S.A. Investigation on thermal aging of ester from palm oil and kraft paper composite insulation
system for high voltage transformer. WSEAS Trans. Environ. Dev. 2017, 13, 75–84.
11. Suwarno, S.A. Thermal aging of ester from palm oil and kraft paper composite insulation. Int. J. Appl. Phys.
2016, 1, 77–84.
12. Carcedo, J.; Fernandez, I.; Ortiz, A.; Delgado, F.; Renedo, C.J.; Pesquera, C. Aging assessment of dielectric
vegetable oils. IEEE Electr. Insul. Mag. 2015, 31, 13–21. [CrossRef]
13. Bandara, K.; Ekanayake, C.; Saha, T.; Ma, H. Performance of natural ester as a transformer oil in moisture-rich
environments. Energies 2016, 9, 258. [CrossRef]
14. Duart, J.-C.; Bates, L.C. Aging of high temperature insulation systems with alternative fluids. In Proceedings of
the IEEE International Symposium on Electrical Insulation (ISEI), San Diego, CA, USA, 6–9 June 2010; pp. 1–5.
15. Azis, N.; Wang, Z.D. Acid generation study of natural ester. In Proceedings of the XVII International
Symposium on High Voltage Engineering, Hannover, Germany, 22–26 August 2011; pp. 1–6.
Energies 2018, 11, 1583 13 of 13

16. Borsi, H. Dielectric behavior of silicone and ester fluids for use in distribution transformers. IEEE Trans.
Dielectr. Electr. Insul. 1991, 26, 755–762. [CrossRef]
17. Perrier, C.; Beroual, A. Experimental investigation on insulating liquids for power transformer: Mineral, ester
and silicone oils. IEEE Electr. Insul. Mag. 2009, 25, 6–13. [CrossRef]
18. Liao, R.; Guo, C.; Wang, K.; Yang, L. Investigation on thermal aging characteristics of vegetable oil-paper
insulation with flowing dry air. IEEE Trans. Dielectr. Electr. Insul. 2013, 20, 1649–1658. [CrossRef]
19. International Electrotechnical Commission. Specific Standard for Unused Natural Esters Liquids for Transformers and
Similar Electrical Equipment; IEC 62770; International Electrotechnical Commission: Geneva, Switzerland, 2013.
20. Wilhelm, H.M.; Tulio, L.; Jasinski, R.; Almeida, G. Aging markers for in-service natural ester-based insulating
fluids. IEEE Trans. Dielectr. Electr. Insul. 2011, 18, 714–719. [CrossRef]
21. Sherwin, E.R. Oxidation and antioxidants in fat and oil processing. J. Am. Oil Chem. Soc. 1978, 55, 809–814.
[CrossRef]
22. Fox, N.J.; Stachowiak, G.W. Vegetable oil-based lubricants—A review of oxidation. Tribol. Int. 2007,
40, 1035–1046. [CrossRef]
23. Snyder, J.M.; Frankel, E.N.; Selke, E. Capillary gas chromatographic analyses of headspace volatiles from
vegetable oils. J. Am. Oil Chem. Soc. 1985, 62, 1675–1679. [CrossRef]
24. Neff, W.E.; El-Agaimy, M.A.; Mounts, T.L. Oxidative stability of blends and interesterified blends of soybean
oil and palm olein. J. Am. Oil Chem. Soc. 1994, 71, 1111–1116. [CrossRef]
25. Rooney, D.; Weatherley, L.R. The effect of reaction conditions upon lipase catalysed hydrolysis of high oleate
sunflower oil in a stirred liquid—Liquid reactor. Process Biochem. 2001, 36, 947–953. [CrossRef]
26. ISO 5508:1990. Animal and Vegetable Fats and Oils—Analysis by Gas Chromatography (GC) of Methyl-Esters of
Fatty Acids; International Organization for Standardization: Geneva, Switzerland, 1990.
27. ASTM D6304. Standard Test Method for Determination of Water in Petroleum Products, Lubricating Oils and
Additives by Coulometric Karl Fischer Titration; ASTM International: West Conshohocken, PA, USA, 2016.
28. ASTM D974. Standard Test Method for Acid and Base Number by Color-Indicator Titration; ASTM International:
West Conshohocken, PA, USA, 2014.
29. ASTM D445. Standard Method of Test for Viscosity of Transparent and Opaque Liquids (Kinematic and Dynamic
Viscosities); ASTM International: West Conshohocken, PA, USA, 2017.
30. ASTM D1816. Standard Test Method for Dielectric Breakdown Voltage of Insulating Liquids Using VDE Electrodes;
ASTM International: West Conshohocken, PA, USA, 2012.
31. IEC 60247. Measurement of Relative Permittivity, Dielectric Dissipation Factor and D.C. Resistivity of Insulating
Liquids; International Electrotechnical Commission: Geneva, Switzerland, 2004.
32. Rapp, K.J.; McShane, C.P.; Luksich, J. Interaction mechanisms of natural ester dielectric fluid and kraft
paper. In Proceedings of the IEEE International Conference on Dielectric Liquids (ICDL), Coimbra, Portugal,
26 June–1 July 2005; pp. 393–396.
33. Viertel, J.; Ohlsson, K.; Singha, S. Thermal aging and degradation of thin films of natural ester
dielectric liquids. In Proceedings of the IEEE International Conference on Dielectric Liquids (ICDL),
Trondheim, Norway, 26–30 June 2011; pp. 1–4.
34. IEEE Power and Energy Society. IEEE Guide for Acceptance of Silicone Insulating Fluid and Its Maintenance in
Transformers; IEEE: Piscataway, NJ, USA, 1989.
35. Xu, Y.; Qian, S.; Liu, Q.; Wang, Z.D. Oxidation stability assessment of a vegetable transformer oil under
thermal aging. IEEE Trans. Dielectr. Electr. Insul. 2014, 21, 683–692. [CrossRef]

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