Journal of Science and Arts Year 20, No. 3(52), pp.

739 -748, 2020

ORIGINAL PAPER
OCCURRENCE, COMPOSITION PROFILES AND POTENTIAL RISK
ASSESSMENT OF POLYCHLORINATED BIPHENYLS (PCBs) IN
TRANSFORMER OILS
CRISTIANA RADULESCU1,2, IOANA DANIELA DULAMA2*,
IOAN ALIN BUCURICA2*, SORINA GEANINA STANESCU2*, ION VASILE2
_________________________________________________
Manuscript received: 15.04.2020; Accepted paper: 27.07.2020;
Published online: 30.09.2020.

Abstract. One of the most common problems encountered in everyday life is the
pollution of the environment. Therefore, regardless of the nature of the daily activities of the
population, this destructive effect of the natural balance finds its origin perhaps in the lack of
capacity over time to treat the problem of waste (industrial and domestic) as it should.
Although important steps have been taken in this regard, and prevention and control rules
have been imposed in most countries of the world, these steps must be supported by all socio-
economic / political components through clear measures, anchored to global developments.
There are among these generic sources of pollution, which are referred to above, processes
that requires high power equipment (generators, transformers, etc.) or hydraulic who which
also requires thermal insulation fluids. The aim of this study is to investigate the
polychlorinated biphenyls (PCBs) presence in the dielectric oil of power transformers. In this
matter, fifteen samples were collected from transformer oils, in the summer of the year 2017,
and analyzed from a physicochemical point of view. A more specific aim was to corroborate
the findings regarding the amount of chlorine in oil samples with the age of the power
transformer using statistical methods. The cluster's analysis indicated that the investigated
samples are clustered into four major groups, providing useful information for further studies
on PCBs mobility in the environment.
Keywords: transformer oil; PCB; viscosity; chlorine content; statistical analysis.

1. INTRODUCTION

Polychlorinated biphenyls (PCBs) are an important group of pollutants, similar in

many aspects to dioxins [1, 2]. Polychlorinated biphenyls belong to a broad class of
chlorinated aromatic hydrocarbons with a biphenyl structure (i.e., two phenyl rings (C6H5)2
and general formula C12H(10-n)Cln) and at least one hydrogen atom substituted by a chlorine
atom (Fig. 1) [3]. Molecules with the same degree of chlorination are isomers; therefore, ten
possible isomer groups of PCBs are revealed (Table 1) [1]. Depending on the position and the
number of chlorine atoms that replace the hydrogen atoms in the structure, the molecule may
have different chemical properties, with a huge chemical stability [1] as well. In this respect,
there are 209 different molecules (Table 1), called congeners, of which only about 130 may be
found in commercial products [4].

1
Valahia University of Targoviste, Faculty of Sciences and Arts, 130004 Targoviste, Romania.
E-mail: radulescucristiana@yahoo.com.
2
Valahia University of Targoviste, Institute of Multidisciplinary Research for Science and Technology, 130004
Targoviste, Romania. E-mail: vasileion20041966@yahoo.com.
*
Corresponding authors: dulama_id@yahoo.com; bucurica_alin@yahoo.com; geaninastanescu@yahoo.com.

https://doi.org/10.46939/J.Sci.Arts-20.3-b05 Chemistry Section

740 Occurrence, composition profiles and … Cristiana Radulescu et al.

Figure 1. Chemical structure of PCBs.

PCBs were discovered in a wide application field such in the hydraulic and thermal
insulation fluids used for electrical transformers and capacitors [5]. PCBs do not easily
degrade in the environment, being lipophilic, and tend to bioaccumulate in adipose tissue of
humans. Thus, PCBs have been demonstrated as being human carcinogens [6], and causing
also a variety of noncancer health effects such as diseases on the reproductive function [7],
immune system [8, 9], nervous system [10-12], endocrine system [13-15], or even loss of
biological diversity [5].
Table 1. Composition of PCB isomer groups.
PCB isomer group Chemical Molecular Chlorine Isomers
formula weight percent numbers
Monochlorobiphenyl C12H9Cl 188.65 18.79 3
Dichlorobiphenyl C12H8Cl2 233.10 31.77 12
Trichlorobiphenyl C12H7Cl3 257.54 41.30 24
Tetrachlorobiphenyl C12H6Cl4 291.99 48.65 42
Pentachlorobiphenyl C12H5Cl5 326.43 54.30 46
Hexachlorobiphenyl C12H4Cl6 360.88 58.93 42
Heptachlorobiphenyl C12H3Cl7 395.32 62.77 24
Octachlorobiphenyl C12H2Cl8 429.77 65.98 12
Nonachlorobiphenyl C12HCl9 464.21 68.73 3
Decachlorobiphenyl C12Cl10 498.66 71.10 1
Total isomers 209

The Stockholm Convention stipulates that all existing PCBs stock/waste and all PCB-
contaminated equipment to be disposed of in an environmentally safe manner (without danger
to human health and the environment) by the year of 2025 [16]. The most important
categories of waste are used substances or articles which either contain or are contaminated
with PCBs (polychlorinated biphenyls) and/or PCTs (polychlorinated terphenyls) and/or
PBBs (polybrominated diphenyls), and heavy metal compounds. Regarding these RoHS
(Restriction of Hazardous Substances), Directive 2002/95/EC (known as RoHS-Recast)
restrict the use of six hazardous materials found in electrical/electronic transformers/products
(Table 2) [17, 18]. Even though PCBs are no longer manufactured or used in industrial
activities, they continue to be encountered as contaminants of concern at hazardous waste
sites and in the environment.
In Romania, the oil from transformers containing PCBs at concentrations of 50 parts
per million (ppm) or greater (≥ 50 ppm) is regulated for disposal under the Decision no.
173/2000 for the regulation [19] of the special arrangements for the management and control
of polychlorinated biphenyls and other similar compounds (Table 1). Despite that, according
to Romanian regulations, it is still authorized the use of intact and non-leaking PCB-
containing dielectrics in transformers in order to ensure the useful life of the types of
equipment.

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Occurrence, composition profiles and … Cristiana Radulescu et al. 741

Table 2. Admitted concentrations of RoHS [17, 19].

Substances Allowed Limit [% weight]
Pb < 0.1 (1000 ppm)
Hg < 0.1 (1000 ppm)
Cd < 0.01 (100 ppm)
Cr(VI) < 0.1 (1000 ppm)
Polybrominated diphenyls (PBBs) < 0.1 (1000 ppm)
Polybrominated diphenyl ethers (PBDEs) < 0.1 (1000 ppm)
Polychlorinated biphenyls (PCBs) Amount < 50 ppm (according to HGR 173/2000)

To overcome these problems through PCBs use, it is very important to shift the world
attention towards eco-friendly alternatives, which not only increase the performances of
electrical transformers sustainably but also protect human health and the environment [20]. In
this respect, the current investigations were performed in order to highlight the amount of
chlorine, as well as to establish the physicochemical properties of lubricants as conditions for
environment and life quality. Statistical analysis revealed that is a strong relationship between
chlorine content in PCBs and the age of power transformers, providing useful information
about emission sources and PCBs mobility in the environment.

2. MATERIALS AND METHODS

2.1. MATERIALS. SAMPLING

All chemicals and reagents were purchased from commercial suppliers and were of the
highest available purity. Dielectric oil samples were collected from fifteen power
transformers, in the summer of the year 2017, establishing in the reporting sheet a series of
characteristics (Table 3) related to transformer performance (i.e., age, total weight, rated
power, cooling type, cooling medium, oil weight).
Table 3. The characteristics of power transformers.
Total weight Oil weight Rated power
Code Year Cooling type* Cooling medium
[kg] [kg] [kVA]
S1 1985 1500/Al 405 400 ONAN Air
S2 1985 1650/Al 384 400 ONAN Air
S3 1978 1780/Al 434 400 ONAN Air
S4 1988 1700/Al 434 400 ONAN Air
S5 1982 1650/Al 384 400 ONAN Air
S6 1986 1780/Al 434 400 ONAN Air
S7 1986 1780/Al 434 400 ONAN Air
S8 2000 760/Al 170 400 ONAN Air
S9 1989 1430 434 400 ONAN Air
S10 1986 1780/Al 434 400 ONAN Air
S11 1985 2500/Al 365 400 ONAN Air
S12 1988 1780/Al 404 400 ONAN Air
S13 1982 1780Al 434 400 ONAN Air
S14 1982 1780Al 434 400 ONAN Air
S15 1983 1780/Al 431 400 ONAN Air
*
ONAN (previous designations OA) - Oil Natural Air Natural

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The samples were collected with the consent of the economic agent, according to
practical guide published by Wells and Hess [21]. This was achieved to provide a better
understanding of the management of PCBs in the old transformer’s oils.

2.2. METHODS

The analysis of PCBs and other chlorinated organic compounds in the matrices of
transformer oil samples was performed by non-specific tests using L2000DXT PCB/Chloride
analyzer (Dexsil, Hamden, CT, USA). This device is a versatile and easy-to-use for analyzing
samples of dielectric oil, water, soil, and contaminated dust. The range of measured values is
2 - 2000 mg/kg, for oil samples. The L2000DX analyzer is programmed with conversion
factors for the main PCBs and most chlorinated substances. The method can apply results
correction factors, taking into account the extraction efficiency, the degree of dilution and the
control sample. The analysis of each oil sample is done very quickly in about 5 minutes. After
calibration, a blank test was performed in order to determine the background level, which is
important for the accuracy of the measurements in the range of low concentrations. The
preparation steps involve the extraction of the chlorinated organic substances from the oil
samples and its treatment with a sodium-based reagent, in order to convert the chlorinated
organic substances into chlorides. Subsequently, the chloride level was measured by the
electrochemical method [22, 23].
The lower and upper limit of oil samples inflammability were performed using an
automates closed cup flash point test system from Tanaka Scientific Limited Corporation,
Japan (i.e., APM-7 automated Pensky-Martens Closed Cup tester, PMCC) [24].
Water content determination from oil samples were performed with Karl Fischer
coulometric titrator (Mettler-Toledo Ltd., Melbourne, Australia). Engler viscometer
(Globecore GmbH, Oldenburg-Eversten, Deutschland) was used for measuring the viscosity
of oil samples.
Statistical Package for the Social Science (SPSS) version 20.0 software for MS
Windows [25-29] was used to interpretation the analytical results and to investigate the
correlations between parameters.

3. RESULTS AND DISCUSSION

The measurements performed on the provided samples have led to the results
systematized in Table 4. The analysis of the results presented in Table 4 shows that the
density of oils varies between 0.8700 and 0.9082 g/cm3, and the viscosity of samples varies
from 1.14 to 1.29 °E. Non-specific tests were standardized for Arochlor 1242 (i.e., PCB blank
sample), with a chlorine content of 42%. Consequently, analysis of samples with more
chlorinated PCB isomers (for example, Arochlor 1260, with a chlorine content of 60%) shows
a higher result than the actual PCB concentration. Non-specific tests are designed to indicate
the presence of chlorine without error.
The density of the oil samples, determined at 20°C, shows values in the range of 0.870
g/cm (S8) and 0.908 g/cm3 (S10), with an average value of 0.884 g/cm3 and standard
3

deviation of 0.011 g/cm3. The recorded values for flash point are similar for all samples: 137-
141°C, with an average value of 138.667±1.543°C. Regarding the viscosity of the samples,
two parameters were reported: oil viscosity (expressed in °E) and viscosity index. The oil

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Occurrence, composition profiles and … Cristiana Radulescu et al. 743

viscosity ranged from 1.17°E (S7) to 1.34°E (S1), with the median value of 1.23±0.05°E. The
total PCB concentration in oil samples ranged from 1.17 mg/kg (S8) to 10.30 mg/kg (S2) with
an average value of 4.501 ppm and standard deviation of 2.557 ppm.

Table 4. Analysis values for transformers which operated after 1975 and worked in the normal
parameters.
Density Oil viscosity PCBs concentration
Flash Water
Aspect/Color/ at [°E] / depending on
Code point content
Impurities 20°C Viscosity chlorine content
[°C] [g]
[g/cm3] Index (V.I.) [ppm]
Clear/Orange/
S1 0.8934 137 17.67 1.34 / 111 6.45
Lack of coal
Clear/Orange/
S2 0.8812 139 10.38 1.28 / 98 5.15
Lack of coal
Clear/Orange/
S3 0.8845 137 12.16 1.21 / 99 10.3
Lack of coal
Clear/Yellow -
S4 citron/Lack of 0.8700 140 8.820 1.19 / 87 2.97
coal
Clear/Orange/
S5 0.8801 139 14.38 1.23 / 96 6.02
Lack of coal
Clear/Orange/
S6 0.8800 137 15.15 1.22 / 99 5.71
Lack of coal
Clear/Orange/
S7 0.8819 138 14.22 1.17 / 101 3.30
Lack of coal
Clear/Yellow -
S8 citron/Lack of 0.8700 141 8.563 1.19 / 87 1.17
coal
Clear/Yellow -
S9 citron/Lack of 0.8723 141 8.614 1.20 / 88 1.37
coal
Clear/Orange/
S10 0.9082 137 16.23 1.28 / 99 6.65
Lack of coal
Clear/Orange/
S11 0.8912 139 10.38 1.32 / 95 6.90
Lack of coal
Clear/Yellow -
S12 citron/Lack of 0.8726 141 8.609 1.21 / 88 1.22
coal
Clear/Orange/
S13 0.8893 138 15.45 1.26 / 103 4.70
Lack of coal
Clear/Orange/
S14 0.8934 139 12.34 1.28 / 97 3.39
Lack of coal
Clear/Orange/
S15 0.8914 137 14.87 1.26 / 98 4.17
Lack of coal

The obtained results highlight that all samples have PCBs content higher than the
reference dose (RfD) established for oral exposure to Aroclor 1016 (7·10-5 mg/kg/day) and
Aroclor 1254 (2·10-5 mg/kg/day) [30, 31]. The oral RfD is based on several studies led on
PCBs effects on monkey: hairline hyperpigmentation, nail changes (prominent beds, elevated
nails), decreased birth weight, possible neurologic impairment (deficits in discrimination-
reversal learning and delayed spatial alternation), reduction of IgG and IgM antibodies, and
human infants: deficits in visual recognition and short-term memory [30, 31].

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However, the Integrated Risk Information System (IRIS) of U.S. Environmental

Protection Agency, National Center for Environmental Assessment, does not offer the
reference concentration (RfC) for inhalation exposure to PCBs [32]. The inhalation exposure
is more probable than swallowing.
PCB concentrations were highest in older transformers and decreased as transformers
were installed earlier (Fig. 2).

12
PCBs concentration depending on chlorine

10 10.3

8
content [ppm]

2
1.17
0
1975 1980 1985 1990 1995 2000 2005
-2
Year

Figure 2. Dynamic analysis of PCBs concentration determined in transformers.

Analysis of variance was used to assess the difference in contamination levels between
the studied transformers, while the Pearson correlation, and Sperman`s indicators were used
to establish relationships among the PCB content identified and with other oil properties. All
statistical analyses were carried out at a significance level of p = 0.05.
Table 5. Pearson correlations of the analysed variables.
Water Oil PCBs
Density Flash point
content viscosity concentration
** ** **
Pearson Correlation 1 -.721 .718 .723 .560*
Density
Sig. (2-tailed) .002 .003 .002 .030
** **
Pearson Correlation -.721 1 -.871 -.409 -.753**
Flash point
Sig. (2-tailed) .002 .000 .130 .001
** **
Pearson Correlation .718 -.871 1 .444 .520*
Water content
Sig. (2-tailed) .003 .000 .097 .047
**
Pearson Correlation .723 -.409 .444 1 .441
Oil viscosity
Sig. (2-tailed) .002 .130 .097 .100
* ** *
Pearson Correlation .560 -.753 .520 .441 1
PCBs concentration Sig. (2-tailed) .030 .001 .047 .100
N 15 15 15 15 15
**. Correlation is significant at the 0.01 level (2-tailed).
*. Correlation is significant at the 0.05 level (2-tailed).

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A moderate correlation relationship can be observed between PCBs concentration and

density, water content and oil viscosity and Sig. <0.05, demonstrates a directly proportional
relationship. Between the density and water content, or between oil viscosity and density it
can be observed a high dependency relationship, sustained by the fact that the value of the
Person coefficient is higher than 0.7. The flash point variable is the only characteristic about
doesn't affirmed it is in a relation of correlation with other analyzed variables.This can be
explained by the fact that the values of this indicator do not depend on the dynamics of the
other variables or their evolution. Applying statistical tests on the data collected is a reliable
way to characterize the statistical population. Based on the information presented in Table 5,
is observed the existence of a moderate or high connection between the analyzed variables.
Sperman’s rank correlations also validate the information obtained through the
Pearson coefficient as it can see from the information presented in Table 6.
Table 6. Sperman’s correlations of the analysed variables.
Flash Water PCBs
Density Oil viscosity
point content concentration
** ** **
Correlation Coefficient 1.000 -.688 .720 .769 .624*
Density
Sig. (2-tailed) . .005 .002 .001 .013
** **
Correlation Coefficient -.688 1.000 -.858 -.407 -.710**
Flash point
Sig. (2-tailed) .005 . .000 .132 .003
** ** *
Correlation Coefficient .720 -.858 1.000 .529 .599*
Water content
Sig. (2-tailed) .002 .000 . .043 .018
** *
Correlation Coefficient .769 -.407 .529 1.000 .631*
Oil viscosity
Sig. (2-tailed) .001 .132 .043 . .012
* ** * *
Correlation Coefficient .624 -.710 .599 .631 1.000
PCBs
Sig. (2-tailed) .013 .003 .018 .012 .
concentration
N 15 15 15 15 15
Correlation is significant at the 0.01 level (2-tailed).**
Correlation is significant at the 0.05 level (2-tailed).*

The value of correlation coefficient ranges between − 1 (indicating perfectly negative

correlation) and + 1 (indicating perfectly positive correlation). The sign indicates the direction
of the trend (i.e., positive or negative), and the absolute value quantifies the strength of the
relationship [33]. Thus, in our case it can observe a strong positive relationship between four
of the analyzed variables (PCBs concentration, density, water content and oil viscosity) and a
strong negative correlation between flash point and the other analyzed variables.
Hierarchical cluster analysis was used to classify the variations in Ʃ15 PCB
concentrations of the investigated samples by using the rescaled distance cluster combine and
average linkage methods. The clustering of the sampling is summarized in the dendrogram
presented in Figs. 3-4.
The cluster analysis indicated that the investigated samples are clustered into four
major groups. The first group of samples (S8, S9 and S12), are characterized by a very low
levels of PCBs (1.17–1.37 ppm). For the second group (S1, S5, S6, S10, and S11) the PCBs
concentrations are the highest and ranges from 5.71 to 6.90 ppm. The third group (S4, S7, and
S14), reached values of PCBs concentration between 2.97 and 3.39 ppm, while, the last group
(S2, S13, and S15) showed values between 4.17 and 5.15 ppm. The sample S3 does not fit
into any groups, reaching the highest value of the concentration of PCBs (10.3 ppm).

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Figure 3. Hierarchical cluster analysis showing the dendrogram of 15 oil samples.

Figure 4. Samples classification about PCBs concentration.

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As it may be seen in Fig. 4, apart from the major classes resulting from the
dendrogram, a single sample S110 has a much higher concentration of PCB, which cannot be
included in any of the groups presented above.

4. CONCLUSIONS

The oil used as dielectric for transformers losing the physicochemical properties
during operation. In this study, fifteen oil samples collected from power transformers were
analyzed from several point of view, such as aspect (all samples were clear), color (from
yellow to orange), impurities (all samples present lack of coal), density at 20°C (values
ranged from 0.870 to 0.903 g/cm3); flash point (137-141°C), water content (8.563-17.670
g/L), oil viscosity (1.17-1.34°E) and PCBs concentration depending on chlorine content
(1.17-10.30 ppm).
The PCBs content is proportional with the age of the power transformer and the
cluster analysis indicated that the investigated samples are clustered into four major groups.

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