22nd International Symposium on Plasma Chemistry July 5-10, 2015; Antwerp, Belgium Two modes of optical emission in partial discharges S.A. Shcherbanev1, I.U. Nadinov1, P. Auvray1, S.M. Starikovskaia1, L.G. Herrmann2 and S. Pancheshnyi2 1 Laboratory of Plasma Physics (CNRS, Ecole Polytechnique, Sorbonne Universities, UPMC Univ. Paris 06, University Paris-Sud), Palaiseau, France 2 ABB Corporate Research, Segelhofstrasse 1K, CH-5405 Baden-Dättwil, Switzerland Abstract: Aging of polymer insulators is a complex physical and chemical process taking typically tens of years in real conditions of high-voltage engineering devices. One of the critical aging mechanisms can be modelled experimentally in laboratory conditions using partial discharges. Emission optical spectroscopy was used to characterize the accelerated aging of the voids in epoxy test samples including an air-filled cavity aged under 50 Hz AC voltage at room temperature. Keywords: partial discharge, emission spectroscopy 1. Introduction One of the most serious technical problems arising in high-voltage engineering is aging of dielectric materials, a process which is typically characterized by a long time scale – tens of years. According to the “standard” scenario, the aging proceeds via creation of micro-cavities (voids) in a dielectric material, with following electrical discharge originating in the cavity and leading finally to the breakdown of the dielectric. An artificial aging of dielectric materials at the late stage before breakdown can be achieved via applying high voltage to a sample, containing already a small cavity (void). In this case, the life time of the sample can be as small as a few weeks that becomes suitable for laboratory studies. Typically, 50 Hz sinusoidal AC signal is used in the experiments. The discharge, igniting in the dielectric in this case, is called a partial discharge (PD). The physics of PDs is not well understood yet [1]. The discharge is often considered as a barrier discharge, DBD [2] as far as the electrodes and gas in the cavity are separated by a dielectric layer. The difference between the PDs and the DBDs is that (i) for PDs, the thickness of the dielectric layer is much higher than the size of the void, that is of the gas gap; (ii) the ratio “surface-tovolume” in partial discharge is much higher than in DBDs, and (iii) encompassed in a bulk material, electric current can flow around the void. These features cause physical peculiarities of the PDs, as, for example, a strong interaction between surface of the dielectric and gas in the void, or limitations, at certain values of gas pressure, to the electron multiplication on the typical size of the voids. No study of the PDs spectra were reported at the moment, and no systematic study of time-resolved emission were made. The aim of the present work is to study spectrum and time-resolved optical emission from the partial discharge; to find, by means of spectroscopic measurements, some specific parameter(s) which can be used as indicator(s) for the aging process. P-II-4-13 2. Experimental setup ant methods A general scheme of the experimental setup is presented in Fig. 1. The sinusoidal high voltage (50 Hz, up to 21 kV) is applied to the electrodes of the sample. Two different methods to analyze the optical emission from the discharge in the 300 - 800 nm spectral range were used. Time integrated spectra were measured by spectrometer Aston SP 2500 (Princeton Instruments) with 1200 l/mm grating connected to the PI-Max 4 1024i ICCD camera (Princeton Instruments). The light was collected by optical cable LG-455-020. Time-resolved emission signal, selected by the narrow band wavelength filter, was recorded by the photomultiplier H6610 (Hamamatsu), connected to the 50 Ohm input of the LeCroy WaveRunner 600MHz oscilloscope. Triggering generator was used to synchronize the time of the collecting of the emission spectra with the voltage waveform. Fig. 1. Scheme of the experimental setup: 1) sample, 2) photomultiplier, 3) oscilloscope, 4) triggering generator, 5) high-voltage generator, 6) optical cable, 7) adapter of optical cable, 8) spectrometer, 9) ICCD camera, 10) computer. The partial discharge was initiated in a nearly spherical gas cavity encapsulated into a specially designed sample, schematically presented in Fig. 2. The sample is made of unfilled epoxy. Two cylindrical electrodes with rounded 1 edges are mounted into the sample. The electric field between the electrodes is close to the field of a parallel‐ plate capacitor, the edge effects are minimized. The distance between the end plates of the electrodes is equal to 2.5 ‐ 3 mm. The cavity (void), 1 - 2 mm in diameter, is situated in the gap between the electrodes at approximately equal distance from each end plate. Preliminary cured epoxy cube with a single air void is immersed into the bulk epoxy between the electrodes. Fig. 2. Scheme of the sample with a single void. Four similar samples with a void diameter between 1.3 and 2.0 mm were used in the experiments. Typically, a few hours of operating under the high voltage at amplitude 21 kV were enough to ignite the discharge in the void without any additional ionization source. After the ignition, the samples were tested either up to their breakdown or until PD activity stops. The radiation intensity of partial discharges was low; all the experiments were made in the dark room. Significant number of accumulations of the signal was used to obtain a proper signal-to-noise ratio when working with ICCD camera. When working with PMT, a voltage close to the limit value (2200 V at limit voltage of 2500 V) was used for PMT power supply. The photo of the discharge is presented in Fig. 3. A diffuse character of the optical emission coming from the void is clearly seen. emission is due to excitation of molecular nitrogen. The emission system is known as the second positive emission system of molecular nitrogen. Finally, a range of 400 - 440 nm was selected for day-by-day spectra recording. It was found that two distinctive time-resolved emission signals co-exist in the system (see Fig. 4). We will further designate them as signal A and signal B. The A signals are small in amplitude, typically a few tens of mV, and very short in amplitude, less than 5 ns. The amplitude of the B signals is high, typically a few volts, and their duration can be up to a few tens of nanoseconds. Signals A do not change during the sample life time, while the signals B modify significantly. Signals A are repeated with a very high frequency, tens-hundreds of spikes are observed during one high-voltage period. Signals B is a rare event, one time per a few periods, with pronounced decrease of the frequency of the appearance on a long-scale period. The spectra obtained experimentally result of integrating of the signals A, the input of the signals B is too low because of the low frequency of the signals. At the highest voltage amplitude, signals A appear in the places of maximum voltage derivative; as voltage amplitude decreases, the signals A move to the maximum of the voltage signal. Signals B are scattered and do not demonstrate a correlation with the high voltage signal. Fig. 4. Two types of optical signals detected in the system (see the text for details). Fig. 3. Photo of the emission from the partial discharge. To obtain the discharge spectra, the emission was collected during 1 s by accumulating 1000 shots of ICCD camera 1 ms each. Wavelength range of 300 - 800 nm was tested; it was found that (i) the transmission of the epoxy is close to zero below 350 nm, increasing gradually to a constant value at about 550 nm; and (ii) the main 2 3. Emission spectra and aging Integrated in time spectra in the wavelength range of 400 - 440 nm were taken nearly every day during the discharge operation. Life time of the samples was between 70 and 300 hours. Analysis of the emission intensity vs cumulative work time allowed finding out the regularities in behaviour of 4 different samples. Fig. 5 presents a summary plot of the emission intensity as a function of time; the amplitude of the emission signal at 427 nm was taken as a reference value. The emission intensity was firstly found monotonically decreasing with a half-decay time of approximately 150 hours. This probably was due to the decrease of frequency of PD pulses of the type A with aging time. At later phases, approximately after 150 - 190 hours, two different scenarios of the discharge development were observed: For two of the samples, the discharge has stopped without breaking up the sample, no short-circuit was observed. No evidences of discharge activity, including P-II-4-13 6 5 2+, 0-3 6 2+, 1-5 2+, 0-4 2+, 2-6 a) 2+, 3-8 2+, 2-7 4 2+, 1-6 2 40 hours 2+, 4-10 2+ system: N2(C3Πu-B3Πg) 0 375 6 b) 400 425 450 475 500 + + 2 , 2-6 2 , 0-3 4 525 200 hours 2+, 1-5 2+, 0-4 2 0 375 6 2+ system: N2(C3Πu-B3Πg) 400 425 450 c) 4 475 500 525 224 hours CO(A), 0-0 CO(A), 1-1 CO(A), 0-1 2 CO(A): CO Angstrom 0 375 400 425 450 475 500 525 Wavelength, nm 4 Fig. 6. Evolution of emission spectra: a) initial spectrum, b) spectrum 2 days before, and c) 1 day before breakdown. Molecular bands are marked in the figure. Sample 1. 3 2 1 PD stops change of the spectra; then breakdown 0 0 24 48 72 96 120 144 168 192 216 240 Cumulative work time (hour) Fig. 5. Evolution of emission in 400 - 440 nm spectral range with aging time. For one of the samples, the breakdown of the sample occurs. The short-circuit event was registered at the end of the operation of the sample. The taken photos clearly demonstrate a presence of two channels of different diameters, connecting the void with the electrodes. The void changes the colour: instead of the transparent cavity, the void and the channels of deep brown colour are monitored after the breakdown. The changes are localized in the vicinity of the void. Significant (500%) emission intensity increase in the considered spectral range was detected two days before the failure with the following intensity drop to a value of about 1/20 of the initial emission. This behaviour correlates with the behaviour of the spectra. For the principal descending part of the amplitude of emission (0 - 180 hours in Fig. 5) the spectrum corresponds mainly to a spectrum of the second positive system of molecular nitrogen. This fact is illustrated by Fig. 6a. If the discharge in void stops by a breakdown of the void, the intensity of emission increases dramatically two days before the failure but no change of the spectrum is observed (Fig. 6b). The last day, severe difference in emission composition is observed. Nitrogen emission disappears completely. Simultaneously, three transitions of CO (Ångstrom system) and one undefined molecular band (apparently, the band of the molecule containing some composition of C-H-O-N atoms) become dominating over all the investigated, 440 - 520 nm, spectral range (Fig. 6c). P-II-4-13 Intensity (a.u.) λ = 405.9 nm Sample 1 (breakdown) Sample 2 (PD stop) Sample 3 (PD stop) 4. Time-resolved emission Time-resolved emission of the signal of type B was used to evaluate gas pressure in the void during the sample aging. The emission of the second positive system of molecular nitrogen, in a semi-logarithmic scale, is plotted in Fig. 7 as a function of time in nanoseconds; the day of measurements is used as a parameter. It is seen from the figure that (i) the decay is close to a monoexponential for majority of the data; (ii) the decay time increases with aging time. 0.0 -0.5 ln(I) Emission intensity (ab. un.) 7 Intensity (a.u.) 8 Intensity (a.u.) light emission, were detected. No visible damage of dielectric was observed. The last registered spectral intensity was about 1/3 of the initial emission in the virgin void. Likely, surface conductivity increases [3] that leads to full or partial shielding of the electric field in the void is the most probable explanation for the discharge stop. It was not possible to re-ignite the sample by the constant heating to 70oC during a few days or/and by keeping the sample during a few days under the maximum voltage 21 kV. -1.0 1st day 2nd day 3rd day 4th day 5th day 6th day 7th day 8th day 9th day 10th day -1.5 -2.0 0.0 2.5x10-9 5.0x10-9 7.5x10-9 1.0x10-8 1.3x10-8 1.5x10-8 Time, s Fig. 7. Decay of the PMT signal for different days of the operation of the sample. Sample 4. The following assumptions were made when treating the emission data: 1) The main excitation process is direct excitation of the N 2 (C3Π u ) state by electron impact, and the excitation time scale is much shorter than the quenching decay; 2) The main depopulation processes are spontaneous emission and collisional quenching; 3) The main quenchers are N 2 and O 2 molecules. 3 In this case, if the decay of emission is long comparing to excitation in the short-time discharge, the reverse efficient radiative time can be written as 𝟏 𝟏 𝑵 𝑶 = + 𝒌𝒒 𝟐 [𝐍𝟐 ] + 𝒌𝒒 𝟐 [𝐎𝟐 ] 𝝉𝟎 𝝉 In this case, at known radiative lifetime τ, quenching rate constants k O2 , k N2 and known gas composition, a gas pressure can be calculated. It was further assumed that gas temperature in the void is equal to the ambient temperature. Gas pressure was calculated in two different assumptions: (a) the gas inside the void is molecular nitrogen; (b) the gas inside the void is a dry air (N 2 :O 2 =4:1 mixture). The results are given by Fig. 8. Although the absolute values of pressure are different, the decay by a factor of 1.6 is observed during 250 hours. This result is in a good correlation with the direct measurements of pressure in partial discharges [4, 5]. Still, additional measurements are necessary to make a conclusion about percentage of molecular oxygen in the void during a stable phase with gradual decrease of emission intensity. 0.7 N2 dry air (N2-O2 80:20) 0.6 Pressure (bar) 0.5 0.4 0.3 0.2 the second positive system of molecular nitrogen was observed in near UV and visible region (350 - 500 nm). In the case of dielectric breakdown, a sharp (500%) increase of N 2 emission was observed 2 days before breakdown; the last day a spectrum of CO and some other C-N-O-H containing molecules was observed instead of the spectrum of nitrogen. This fact suggests that it is possible, analyzing the broad emission spectra, to predict a breakdown at least a few hours before it happens. Measurements of the emission of the 0 - 4 and 1 - 5 vibrational transitions of the 2+ system of N 2 at (430 ± 10) nm with nanosecond resolution demonstrated the coexisting of two well distinguished signals with different duration and amplitude: A. Fairly small optical signals of less than 2 - 3 ns in duration and a few tens mV in amplitude were observed continuously in the vicinity of the voltage maxima and minima. The observed emission spectra are mainly determined by these small optical pulses. Based on their short excitation and decay times, these pulses can be short surface discharges inside the void. B. The optical signals of about 40 ns in duration and up to a few volts in amplitude were observed stochastically during the period with a frequency, small comparing to the signals of the type A. The amplitude of these signals was found to be decreasing with the aging time. These pulses are probably originated in the bulk of gaseous voids. It was shown that the modification of the emission decay time during the operation period can be used for analysis of the gas pressure in the void. Pressure decay by a factor of 1.6 was observed during 250 hours. 0.1 0.0 0 50 100 150 200 250 Cumulative work time (hour) Fig. 8. Evaluated gas pressure (at room temperature) variation with aging time. Sample 4. 5. Сonclusions Emission optical spectroscopy was used as a technique to study the partial discharges in a dielectric. Four different samples were subjected for aging process which has taken between 70 and 300 hours before the stop of the discharge operation at voltage amplitude about 20 kV. Two scenarios of the discharge failure were observed: stop of the discharge activity without break of the dielectric and without a short circuit event, or the sharp local disruption of the dielectric with formation of two conductive channels connecting the void with the electrodes and producing a short circuit. It was shown that, with the help of emission spectroscopy, it is possible to follow, in non-intrusive manner, the changes of gas mixture composition during the aging process. For both scenarios, a stable initial phase with gradual decrease of emission intensity from the discharge was typical for a few hundreds of hours of non-stop discharge operation. At this stage, a spectrum of 4 6. References [1] L. Niemeyer. IEEE Trans. Dielectr. Electr. Insul., 2, 510-528 (1995) [2] U. Kogelschatz. Plasma Chem. Plasma Process., 23, 1-46 (2003) [3] C. Hudon, R. Bartnikas and M.R. Wertheimer. in: IEEE Int. Symp. on Electrical Insulation. 153-155 (1990). [4] A.C. Gjaerde. IEEE Trans. Dielectr. Electr. Insul., 4, 674-680 (1997) [5] A.C. Gjaerde. IEEE Trans. Dielectr. Electr. Lnsul., 5, 463-465 (1998) P-II-4-13
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