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energies Article Dielectric Properties of Electrical Insulating Liquids for High Voltage Electric Devices in a Time-Varying Electric Field Peter Havran , Roman Cimbala * , Juraj Kurimský , Bystrík Dolník , Iraida Kolcunová, Dušan Medved’ , Jozef Király, Vladimír Kohan and L’uboš Šárpataky Department of Electric Power Engineering, Faculty of Electrical Engineering and Informatics, Technical University of Košice, Letná 9, 04200 Košice, Slovakia; [email protected] (P.H.); [email protected] (J.K.); [email protected] (B.D.); [email protected] (I.K.); [email protected] (D.M.); [email protected] (J.K.); [email protected] (V.K.); [email protected] (L’.Š.) * Correspondence: [email protected]; Tel.: +421-55-602-3557 Citation: Havran, P.; Cimbala, R.; Abstract: The motivation to improve components in electric power equipment brings new proposals Kurimský, J.; Dolník, B.; Kolcunová, from world-renowned scientists to strengthen them in operation. An essential part of every electric I.; Medved’, D.; Király, J.; Kohan, V.; power equipment is its insulation system, which must have the best possible parameters. The current Šárpataky, L’. Dielectric Properties of problem with mineral oil replacement is investigating and testing other alternative electrical insulating Electrical Insulating Liquids for High liquids. In this paper, we present a comparison of mineral and hydrocarbon oil (liquefied gas) in Voltage Electric Devices in a terms of conductivity and relaxation mechanisms in the complex plane of the Cole-Cole diagram and Time-Varying Electric Field. Energies dielectric losses. We perform the comparison using the method of dielectric relaxation spectroscopy 2022, 15, 391. https://doi.org/ in the frequency domain at different intensities of the time-varying electric field 0.5 kV/m, 5 kV/m, 10.3390/en15010391 and 50 kV/m. With the increasing intensity of the time-varying electric field, there is a better approximation of the Debye behavior in all captured polarization processes of the investigated oils. By comparing the distribution of relaxation times, mineral oil shows closer characteristics to Debye relaxation. From the point of view of dielectric losses at the main frequency, hydrocarbon oil achieves better dielectric properties at all applied intensities of the time-varying electric field, which is very important for practical use. Keywords: dielectric polarization; conductivity; oil insulation; electric field effects; complex electric modulus; frequency domain analysis Academic Editor: Gabriel Vélu 1. Introduction Received: 10 November 2021 The problems of the constant increase of electricity consumption and its supply to the Accepted: 31 December 2021 end customer in the required quality and with high reliability correspond to the state of Published: 5 January 2022 electrical equipment that participates in the whole process. The fundamental component in this system is the insulation of electrical equipment, which is required to operate as Publisher’s Note: MDPI stays neutral efficiently as possible [1–5]. The condition of the insulation system is an essential indicator with regard to jurisdictional claims in of the operational reliability of power transformers and other high voltage equipment published maps and institutional affil- in the power system. The transformer is included as one of the main components in the iations. transmission and distribution network, and its service life depends on the condition of the insulation system. Said system continuously withstands thermal, chemical, and electrical Copyright: © 2022 by the authors. stresses during its operation. Insulation and cooling effects are the basic properties of fluids Licensee MDPI, Basel, Switzerland. used in transformers [6–13]. This article is an open access article distributed under the terms and The development of materials is advancing, which also applies to liquid insulating conditions of the Creative Commons materials. Mineral oil produced based on non-renewable petroleum products has long been Attribution (CC BY) license (https:// used in power transformers due to its low cost and relatively high rate of heat dissipation. creativecommons.org/licenses/by/ Therefore, based on its biodegradability, global researchers are focusing on alternative, 4.0/). electrical insulating liquids [10,14–16]. In researching new materials, it is possible to draw on the knowledge currently acquired during the research or by monitoring the materials Energies 2022, 15, 391. https://doi.org/10.3390/en15010391 https://www.mdpi.com/journal/energies

Energies 2022, 15, 391 2 of 21 after commissioning [6]. In recent years, it is possible to register the development of hydrocarbon transformer oil, produced based on GTL (Gas to Liquid) technology, which is obtained by converting natural gas into liquid waxy hydrocarbons using the Fischer- Tropsch process. These hydrocarbons are finally transformed using a unique technology that includes new catalysts and subsequently distilled into a wide range of products, including electrical insulating oils and other raw materials for the chemical industry. The difference is that the products do not contain inorganic substances such as sulfur, but only pure hydrocarbons, ensuring sufficient paraffin saturation. The absence of sulfur and the negligible amount of aromatic and unsaturated hydrocarbons, significantly present in conventional mineral oils, provide GTL with excellent properties compared to the mineral oils used in operation [17–19]. 2. Motivation of the Experiment The publication [20] contains, among other things, a comparison of mineral oil and hydrocarbon oil (liquefied gas) in terms of dielectric losses at different intensities of time- varying electric field (100 kV/m –900 kV/m) at a mains frequency of 50 Hz. Through comparing dielectric losses, it was found that hydrocarbon oil has better insulating prop- erties than conventional mineral oil at all applied electric field intensities. However, the contribution does not include the dielectric behavior of the compared oils in the frequency spectrum but only at the frequency of the network. The reason is that the authors focused their research on the response of the investigated samples only when applying relatively high intensities of the electric field with an industrial frequency. Dielectric behavior in a specific frequency spectrum characterizes the method of dielectric relaxation spectroscopy, which includes measurements of dielectric parameters when applying lower electric field intensities, as mentioned above in [20]. Therefore, our paper will deal with comparing mineral and hydrocarbon oil at lower electric field intensities (E ≤ 50 kV/m), the method of dielectric relaxation spectroscopy in the frequency domain to describe the dielectric in more detail phenomena occurring in the material. The paper [21] presents frequency-dependent dielectric relaxation spectroscopy of a weakly polar ferrofluid based on mineral oil Mogul TRAFO CZ-A with a nanoparticle concentration of 6.6% at a time-varying electric field intensity of 20 kV/m. Spectroscopic measurements of complex permittivity showed that the investigated sample showed a polarization process close to Debye relaxation in the measured frequency spectrum of 20 Hz–100 kHz. Said process is shown in Figure 1. Figure 1. Dielectric behavior of weakly polar ferrofluid based on mineral oil Mogul TRAFO CZ-A in the complex plane. Adapted from [21].

Energies 2022, 15, 391 3 of 21 Therefore, another goal of our paper is to examine only the carrier medium (i.e., min- eral oil Mogul TRAFO CZ-A), supplemented with a comparison with the hydrocarbon oil Shell DIALA S4 ZX-1, produced based on GTL technology. Compared to the contribu- tion [21], we introduce a different experimental study, where dielectric measurements and analyses were conducted at different intensities of the time-varying electric field (lower and higher than 20 kV/m), and also the dielectric processes monitored in the lower frequency band (0.1 mHz–3 kHz). To investigate dielectric processes, it is necessary to study dynamic polarization spectra, extended by the analysis of conductivity characteristics. Impedance analysis of Cole-Cole formalism in dielectric spectroscopy is a suitable method for studying the con- ductivity of a material. The paper [22] generally explains the processes of ionic hopping and relaxation in disordered rigid structures through complex plane impedance and frequency- dependent electrical conductivity. The mentioned conductivity performance analysis will be used in our study to describe the conductivity characteristics of electrical insulating oils in the applied time-varying electric field. As only data for sulfur-containing naphthenic mineral oil—Mogul TRAFO CZ-A are known, our goal is to compare these data with a unique type of transformer oil, which has a minimum sulfur content and was produced by liquefaction of natural gas. Dielectric spectroscopy is one of the diagnostic tools that examine the quality of the insulation system. However, comparative data at different electric field intensities and test voltage frequencies are not available, so that we will address this in this paper. In power engineering, the dielectric properties of electrical insulating liquids are critical, therefore a complex experimental investigation is required at lower and higher electric field intensities, together with the coverage of the most comprehensive possible frequency spectrum. Dielectric spectroscopy in the frequency domain is a useful method for general insulation testing in diagnostics. Dielectric spectroscopy has many advantages over standard dielectric power loss tests at 50 and 60 Hz. One of the main advantages is the testing of the material in a wide range of frequencies, which makes it possible to selectively distinguish the properties of the insulation system [21,23]. 3. Dielectric Relaxation Spectroscopy Using a Complex Electric Modulus Complex electric modulus M* is defined as the inverse of the complex permittivity ε*. The complex permittivity is given by the relation ε*(ω) = ε (ω) – iε (ω), where ε (ω) is the real part of the complex permittivity (relative permittivity) and ε (ω) is the imaginary part of the complex permittivity, representing the factor of dielectric losses and ω is the angular velocity. It follows that M* is expressed according to the equation: M* = 1/ε* = (ε /ε 2 + ε 2) + i(ε /ε 2 + ε 2) = M + iM (1) The complex electric modulus was first used by Macedo et al. to research relaxation processes in glassy ionic conductors. It has also been used to provide information on electric charge dynamics and dielectric polarization in polymer electrolytes. It has rarely been used to describe the dielectric behavior of insulating materials [24–30]. The Cole-Cole dielectric relaxation is given by the complex permittivity ε*: ε*(ω) = ε∞ + (εs − ε∞/1 + (iωτ)1−α) (2) where ε∞ is the optical permittivity, εs is the static permittivity, and τ is the relaxation time within the complex permittivity, where β (0 < β < 1) is a parameter of the semicircle shape in the complex plane of the Cole-Cole diagram and β = 1 − α holds. Based on Equation (2), a complex electric modulus can be defined as: M*(ω) = 1/ε* = 1/(ε∞ + (εs − ε∞/1 + (iωτ)β)) = M∞ − (M∞ − Ms/1 + (iωτM)β) (3)

Energies 2022, 15, 391 4 of 21 In this case, M∞ = 1/ε∞ is the optical electric modulus, and Ms = 1/εs is the static electric modulus. Then for the real and imaginary part of the complex electric modulus: M (ω) = M∞ + (Ms − M∞/1 + (ωτM)2) (4) M (ω) = (Ms − M∞) ωτM/1 + (ωτM)2 (5) where τM is the relaxation time for M* equal to: (6) τM = τ(ε∞/εs)1/β In general, εs is greater than ε∞, so τM is less than τ. It causes relaxation processes at higher frequencies within the complex electric modulus M*, in contrast to the low-frequency relaxation processes described by the complex permittivity ε*. The position ε and ε in the denominator of Equation (1) causes low values of M and M under the condition of higher values of ε and ε . The relaxation peaks are completely bounded in the frequency spectra of M and M . The shape of the curve in the complex plane does not change during the transformation from ε* to M* and thus not even β, as expressed in Equation (3). In other words, for complex permittivity and complex electric modulus in the complex plane, a lower value of β is related to a larger distribution of relaxation times τ or τM in each respective center of the semicircle [24,25,31]. The degree of Cole-Cole relaxation time distribution between M* and ε* does not change through the parameters α and β. The difference is that the position of their loss peaks Mmax and εmax will be different. Mmax is shifted to higher frequencies at position (ωτ)Mmax α = εs/ε∞, while εmax is located at position (ωτ)εmax = 1. This is because M converts the low-frequency increase ε , caused by the ion distribution, into a conductive peak characterizing the ohmic relaxation time. Thus, it is clear that complex electric modulus analysis offers better separation between dipole relaxations and losses with significant ionic distribution than complex permittivity analysis. Simply put, in the low- frequency spectrum, the complex permittivity and the dielectric dissipation factor are significantly affected by the effect of electrode polarization and conductivity. The reduction of the influence of these factors is caused by M*(ω), therefore it is understood as a valuable tool for highlighting the details of relaxation information registered in insulation materials in the low-frequency band [31,32]. 4. Experiment 4.1. Examined Samples We performed experimental measurements on two new, ageless samples of electrical insulating liquids: • Mogul TRAFO CZ-A, hereinafter referred to as MO; • Shell DIALA S4 ZX-1, hereinafter referred to as SD. MO is an inhibited mineral oil with an oxidation inhibitor, which meets all the re- quirements placed on its use properties. It is used as an insulating and cooling liquid for transformers of all voltage levels and other power equipment. It has low density, high surface tension, excellent electrical insulating properties, high oxidative stability, and long life. It is made from high-quality hydrocracked deep-refined base oil obtained from paraffin oil using state-of-the-art technology. Its characteristic parameters are given in Table 1 [33]. SD is a hydrocarbon oil produced based on GTL technology with long service life, negligible sulfur content, and low content of aromatic and unsaturated substances. The service life is an inhibited oil with good oxidizing properties. The negligible sulfur content does not cause corrosion of copper. It does not contain polychlorinated biphenyls (PCBs) and reacts positively to antioxidants. It has excellent viscous properties at low temperatures, which causes efficient heat transfer in the transformer. The characteristic parameters are given in Table 2 [17,18].