Proceedings of the 3rd International Conference on Properties and Applications of Dielectric Materials July 8-12, 1991 Tokyo, Japan

ALL FILM POWER CAPACITORS - DEGRADATION UNDER ALTERNATING ELECTRICAL STRESS OF IMPREGNATED POLYPROPYLENE FILMS EFFECT OF THE EPOXIDE ADDITIVE
E . SEBILLOTTE, S . THEOLEYRE, S. SAID*, B. GOSSE*, J.P. GOSSE*
VARILEC - BP I O 74371 PRINGY FRANCE

* LEMD - CNRS - BP 166X

38042 GRENOBLE CEDEX FRANCE

Abstract The ageing of impregnated PP film was carried out on model capacitors at 8OoC 50 Hz AC electrical Stress under (135 Vrms/pm). The ageing is estimated from the local measurement of breakdown voltage of the PP film. The effects on the ageing of impurities (electrolyte, water, oxygen) and of epoxide additive, added to the impregnating liquid, were observed. Introduction The technology of all film power capacitors using impregnated polypropylene (PP) film and non chlorinated impregnanting liquid has resulted in the increase of the voltage gradient and thus the power per unit capacitor. However, as with previous technologies, these capacitors age in service, limiting their time-life whlch is correlated with a decrease of capacitors elements breakdown voltage [l] [2] probably due to a localised degradation of the insulation with an unknown mechanism [ 3 ] . So, using these new materials which have high performance but under stronger stresses (electrical, thermal) subjecting them to lead us to consider the ageing of power capacitors : why and how does the breakdown voltage decrease, why do epoxide additives increase the time-life ? [ 4 ! . We have chosen to study the ageing of the all film power capacitors on model capacitors with small area electrodes. In this way, it is possible to do many tests and determine where degradation occurs. We have done the tests with plane electrodes to be as near as possible to the conditions encountered in real capacitors. To accelerate the ageing, voltage gradient used was twice the standard one , and impurities like oxygen, electrolyte, water, were added to the impregnant liquid. Each experiment was conducted with or without epoxide additive. Experimental Impreqnantinq licruid
A blend of mono-, di-benzyltoluene (M/DBT) was used without additive (liquid A ) or with epoxide additive (liquid B). After being purified, mains caracteristics are : E = 2.65 ; e = 2.10-'* am ; water content 1.5.10-3 M.

After a vacuum drying at 80C, the film was impregnated with liquid A or B. Impregnation rate was 10% in weight. Model capacitor It was built in PTFE. Two impregnated PP sheets were placed between two indentical electrodes with a pressing force about 2 bars. Then the model capacitor was filled up in vacuum. The electrodes were made in duralumin (fig. 1). Their working surface was carefully polished. The working surface edge was made round (curvature radius about 0.2 mm) and polished in order to eliminate irregularities and field enhancement. Due to polishing, the working surface is not exactly plane but slightly convex. In that way, the liquid layer thickness between electrode and PP film may reach a few microns at the working surface boundary (greater than that due to the PP film roughness).

Figure 1

ELECTRODE PROFILE

radius =

0,Z mm

convexity =

4 pm

Aqeina conditions PP sheets were submitted to an electrical stress of 135 Vrms/pm (4.1 kVrms) at 8OOC. Under this gradient voltage any partial discharge larger than 1 pC (limit of detector's sensibility) was detected (the first 1 pC discharge was detected at 200 Vrms/pm (6 kVrms)). 16 model For each experiment, capacitors were aged simultaneously, 8 with liquid A and 8 with liquid B.

Polvpropvlene film We have used an isotactic (95%) PP film, rough on both sides. Ponderal thickness was 13.6 pm with a space factor about 10%.

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Aqeinq analysis Model capacitors dielectric losses : The dielectric losses of model capacitors mainly depend on the liquid layer (thickness, resistivity) between the electrodes and the PP sheets [ 5 ] . After ageing, dielectric losses were found to be ten times higher than before ageing. This was correlated with the drop of the liquid resistivity ( l o i o Rm after ageing) due to its thermal oxydation in air at 8 0 C . No difference has been observed between liquid A and liquid B. So, the measurements of the model capacitor dielectric losses havent given us any information about those of the impregnated PP films. Measurement of the local breakdown voltaqe of the PP sheet : It was measured between a plane electrode and a ball ($I = 2 mm) in MIDET at 2OOC. A DC voltage ramp ( 5 0 0 V.s-) was applied. On each PP sheet, about 5 0 breakdown voltages were recorded and classified in two groups depending on where the measurement had been performed : in the Electrically Stressed (E.S.) area (under the electrodes during the ageing) or in None Electrically Stressed area (outside the electrodes). For each group data were analysed with WEIBULLs statistic. PP sheets have been observed after ageing with an optical microscope and with a scanning electron microscope. Results Influences of impurities and of epoxide additive Four ageing tests were performed : The impregnating liquids , A and B) were L as pure as possible ( e = 2.10 nm at 2OOC). Ageing stopped after 1 8 0 0 h. M of an electrolyte, TIAP (Triisoamylammonium) were added to the impregnating liquids (A and B ) (e= 7 . 1 0 nm at 2OOC). Ageing stopped after 1 3 6 0 h.

The impregnating liquid (A only) was M) 6 . 1 0 nm satured in water (1.7 at 2 0 C ) . Model capacitors were put into an enclosure full of Nitrogen saturated in water vapor. The model capacitors average time-life was 1 6 0 h. The impregnating liquids (A and B) were as pure as possible but the model capacitors were put into an enclosure full of oxygen. In this case, model capacitors with liquid A had a time-life about 2 5 h, and none of those with liquid B had failed before 1 6 0 h when the test was stopped. Table 1 gives the average values of the local breakdown voltage of the impregnated PP sheets before and after different ageing tests. Each value is the average of about 1 0 0 data. Variation coefficient (6n/m in %) is reported. Some examples of impregnated PP sheets breakdown voltage distribution after ageing are given in figure 2. After 1 8 0 0 hours of ageing under 1 3 5 Vrms/pm at 80OC with pure liquids, we can see that the dielectric strength of impregnated PP sheets is almost unaffected. If the impregnating liquids contain an electrolyte without epoxide additive (liquid A) and after 1 3 6 0 hours of ageing, the dielectric strength seems to decrease about 2 0 % in the E.S. area. With epoxide additive (liquid B) , this decrease is only

(e=

7%.

For both long-time ageing tests, the PP sheets were examined with a scanning electron microscope which showed that the films surface was damaged in the E.S. area. This degradation occurs only on the films side which faces the electrode and was localised in a ring around the periphery of the E.S. area. So this degradation has a close connection with the thickness of the liquid layer between PP sheet and the electrode.In case of liquid E, the observed degradation was clearly less important than with liquid A. Very different results are obtained if the impregnating liquid is saturated in water or in oxygen since without epoxide additive, the time-life of model capacitor was very short.

Table

1 :

Average values (volt) of the local breakdown voltage of impregnated PP sheets - variation coefficient ( % )

I I Before ageing
After ageing Pure liquids ( 1 8 0 0 hours)
~~

LIQUID A
8750 (2%)

I I
8700 2.5% 6950 8.0% 6950 13.0% 6050 4.0% 8050 2.5% 8600 2.0% 8550 2.5%

LIQUID B
8750 (2%)

I
8750 3.5%

None E.S. areaE.S. area None E.S. area E.S. area

8650 2.5% 7750 4.5% 8250 2.0% 8300 2.5%

Liquids + TIAP ( 1 3 6 0 hours) Liquid saturated H 2 0 ( 1 6 0 hours) Liquid saturated O2 (A:25 h B:160 h)

8150 10.5%

8100 3.5%

741

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JA(

IO1

liq A

lol

0 None E . S .

area

U 31

10i

E.S.

area aged

- -- None
10-1

3 9 e
3

None E . S .

area

100

E.S.

area

None a g e d

-]
I
I

I"

. . . . . .,
1o4

10-2

2
Breakdown v o l t a g e
:

103
Breakdown v o l t a g e : V o l t

lo3

Volt

1o4

IB/

lo'

101
Liq A + T I A P
'L

Liq B +

TIAP

0 None E . S . a r e a A E.S. area

0 NOM

E.S.

area

E.S.

area

_ _ _ None

aged
1

. None a g e d
c)

f
A
0

I
1 I

+:
A
I

0 1

1o3
Breakdown v o l t a g e : V o l t

1o4

101
Liq A + 0 2

U 31

10';

None E . S . a r e a
E.S.

area aged

{ j
I

lo'
U 31

&:
I

3 2
1

3 9
3
cq
3

100

. - - - None
10-1 :

A
A

U I
01 0 1
I

1 3

p: f

9 10-I
I

01
I

10-2

1o-2
1o4
Breakdown v o l t a g e
:

Volt

Fiq. 2 :Breakdown different A and A' : B and B 1 : C and C 1 :

voltage distributions of impregnated PP sheets after ageings : pure liquids during 1800 h liquids + TIAP during 1360 h liquid saturated O2 during 25 h or 160 h

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Graph C figure 2 shows that in the E.S. area there are many points which have a low breakdown voltage which is correlated with the short time-life of model capacitors. With epoxide additive (graph Cl) , E.S. area and None E.S. area have the same dielectric strength, showing the epoxide additive's effect in reducing the ageing. However in this case and for both areas, the average breakdown voltage is below that of the none aged impregnated PP sheets. This probably results from the thermal oxydation of PP. Then the local breakdown voltage values was analysed as a function of the distance area. d from the center of the E . S . Considering the E.S. area as a disk having a radius R, the average breakdown voltage was calculated in four concentric rings : d 5 R/3 ; R/3 < d 5 2R/3 ; 2R/3 < d 5 R ; d > R (figure 3). The points of the E . S . area having the lower breakdown voltage are collected in a ring situated between 2R/3 and R. So the drop of dielectric strength occurs when the thickness of the liquid layer between the sheet and the electrode was greater, and moreover, it is in this ring that the model capacitor breakdown occurs during the ageing. It is important to note. that in the (liquids case of short , time ageing saturated in water or in oxygen), no damage of the PP film's surface was observed. This indicates that the drop of dielectric strength is not due to perceptible degradation of the film.

:'ooooi

Liq B

i 1
-

of E.S. from Distance area center

RI3

2FU3

Fiqure 3 : Average breakdown voltage in concentric rings of impregnated PP sheets after ageing with impregnating liquids saturated in oxygen A) liquid A (without epoxide additive) B ) liquid B (with epoxide additive)

Table 2 :

Time-life and breakdown voltage of impregnated PP sheets after ageing.

2 (67) 3100
7000

Voltage conditions (kVrms) (voltage gradient Vrmslpm) Average Time-life (h) Breakdown voltage (V)

3.6 (120)

4.1 (135) 25
6100

5
(167) 12 6400

6 (200) 0.3 8300

85
6800

Table 3 : Time-life and breakdown voltage of impregnated PP sheets after ageing with an hydrostatic pressure of 40 bars. Voltage conditions (kVrms) Time-life (h)
4.1 25 6 11

I Breakdown voltage

(V)

6200

6200

I
- 143 -

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Voltaqe dependence of aqeinq Model capacitors impregnated with liquid A saturated in oxygen were aged under different voltages (i.e. different voltage gradients) . Table 2 indicates the average values of model capacitors time-life and breakdown voltage after different ageings in the ring situated in the E.S. area between 2R/3 and R. For 2 kVrms to 5 kVrms, the time-life is affected by the applied voltage, but not the residual dielectric strength after ageing. This leads us to believe that, when the dielectric strength drops to a certain value, breakdown of model capacitors occurs. On the contrary, ageing performed under 6 kVrms induces a very short time-life but without any marked drop of residual dielectric strength that indicates a change in breakdown process. This is not surprising bearing in mind that partial discharges above 1 pC are detected from 6 kVrms which can quickly induce the breakdown. To confirm this hypothesis, we have performed the same ageing test as mentionned above, but with a hydrostatic pressure (40 bars) on the impregnating liquid. Table 3 gives the results. Applying a hydrostatic pressure does not affect the ageing conducted at 4.1 kVrms but clearly changes the results of the one at 6 kVrms. In this case, the residual dielectric strength reaches the same level as for 4.1 k V r m s , indicating an equivalent ageing process because partial discharges above 1 pC cannot develop. We have clearly shown that epoxide additive is able to markedly reduce (or stop) the electrical ageing of PP but not the thermal oxydation. The exact mechanism which results in the degradation of impregnated PP film under alternating electrical stress and the epoxide additives interaction with it, still have not been determined. References
[l] J. SAMAT, J.J. COURTET, G. BERNARD,

P. JAY, P. BERNARD, Rapport CIGRE, WG 15.06 (1986) [2] G. BERNARD, M. NICOLAS SEE (3 XI1 1987) p. 83
[3]

T. UMEMURA, K . AKIYAMA IEE Trans. on Elect. Insul. EI22, 3 , p. 309 (1987)

[4] N. BERGER, P. JAY Conf. rec. of 1984 IEE Int. Symp. on Elect. Insul., Montreal (1984), p. 319 [5] E. SEBILLOTTE

These de Docteur INPG, Grenoble, 1989

Conclusion We have shown that the ageing of impregnated PP film is greatly amplified by the impurities (electrolyte, water, oxygen) added to the impregnating liquid. Oxygen has the stronger effect. During ageing, points in the film having low breakdown voltage expand which lead to capacitor breakdown and limiting in this way its time-life. The lower residual dielectric strengths have been obtained without any damage observed on the film surface. It seems that there is not correlation between them. Ageing of the PP film occurs especially where the liquid layer between the film and the electrode reaches a few microns in thickness, i.e., larger than that induced by the film roughness. The measurement of partial discharge level and the study of ageing with different voltage and hydrostatic pressure applied, clearly show that the observed ageing is not caused by partial discharges above 1 pC which may develop in the liquid layer. However the ageing mechanism is certainly initiated in the liquid layer between the film and the electrodes where active chemical species may be created and than lead to the PP degradation.

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