Journal of Electrostatics, 8 (1980) 139--152 139

© Elsevier Scientific Publishing Company, Amsterdam -- Printed in The Netherlands

PRELIMINARY OBSERVATIONS ON BULK ELECTROCONVECTION

IN E L E C T R I C A L L Y STRESSED LIQUID INSULANTS

PART I: EXPERIMENTAL INVESTIGATION

J.M.H.P.ETERS
Liverpool Polytechnic, Department of Mathematics, Faculty of Engineering, Liverpool
L69 3BX (Gt. Britain)
J.L. SPROSTON
University of Liverpool, Department of Mechanical Engineering, Liverpool L69 3BX
(Gt. Britain)
and G. WALKER
University of Liverpool, Department of Applied Mathematics and Theoretical Physics,
Liverpool L69 3BX (Gt. Britain)
(Received January 26, 1979; accepted in revised form April 23, 1979)

Summary
Electroconvective motions which occur in the bulk of insulating liquids under electric
stress are considered.
In order to study such motions, an experiment was devised in which a liquid insulant
was electrically stressed in rectangular cells of square cross section with different electrode
configurations. Using a suitable flow visualisation technique, the resulting motions were
found to remain essentially two-dimensional and streakline photographs for the particle
paths were obtained. These suggest that electrical shearing forces acting adjacent to the
boundaries of the liquid are mainly responsible for the bulk motions in the liquid.

1. Introduction

When an insulating liquid, such as kerosene, is electrically stressed by an

externally imposed electric field, convection occurs b o t h in the liquid bulk
and at its free surface. The bulk motions are less p r o n o u n c e d than those at
the surface and their character is determined b y the dielectric, the field
strength and the electrode shape. The surface p h e n o m e n a depend u p o n the
physical properties of the t w o adjacent fluids, the orientation and strength
of the electric field and u p o n the types of disturbance which the surface
may undergo.
Although bulk electroconvection is n o t as p r o n o u n c e d as that at the
surface, it is still readily discernible at high enough field strengths. The
motion is usually cellular in nature with the number and t y p e o f cells at a
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given field strength depending on the electrode configuration. As the field

strength rises, the n u m b e r of cells changes until at very high field strengths the
motion becomes disordered and turbulent.
There appear to be t w o basic driving mechanisms which govern bulk electro-
convection, with some others providing secondary effects. The first dominates
the low-field motion and is most aptly described as electroconvection at the
wall. Here the diffuse charge, which is always present in a layer of liquid
adjacent to a wall, is swept away by the tangential c o m p o n e n t o f the electric
field. A shear stress results which gives rise to circulatory bulk motions. The
second mechanism is manifest at high field strengths and it is caused by the
injection of free charge from the electrodes. This is then acted upon by the
electric field. A highly unstable situation develops and the flow regime be-
comes turbulent. The character of these two mechanisms is summed up by
the statement that, at low field strengths, vorticity is generated at the liquid
boundary whereas, at high field strengths, vorticity is generated in the liquid
bulk.
Interest in bulk electroconvection in liquids grew primarily o u t of a desire
to examine the conduction process in low-conductivity liquids. At first it
was believed that t w o conduction regimes prevailed, namely an ohmic one
at low field strengths and a space-charge limited one at high field strengths.
However, some mobility and viscosity measurements departed significantly
from Walden's rule of inverse relationship. This was later attributed to
electroconvection, a p h e n o m e n o n which had already been hinted at in the
study of electro-osmotic motions induced in uncharged liquids under electric
stress [1--5].
Subsequent investigations into the behaviour of charged liquids in the
presence of electric fields identified t w o flow regimes depending on the
quantity of charge in the liquid and the strength of the applied field.
The first is characterised by laminar flow in which the mean velocity
varies as the square of the field strength and the current varies as its cube.
The second is characterised by turbulent flow with the mean velocity and
current, respectively, varying linearly and quadratically with field strength
[6--8]. In the latter mode, it was also observed that mixing tends to unify
the bulk charge distribution [9]. Rapid streaming away from pointed elec-
trodes was also reported [10] and practical applications of this pumping
mechanism have been considered [11] [12].
The aim of the present Work was to study the characteristics and to
identify the causes of electroconvection in the bulk of insulating liquids
confined within rigid boundaries and stressed b y externally applied electric
fields. The experimental objective, presented in this paper, was to obtain
a visualisation of the flow structure induced b y a given electric field distribu-
tion, whilst the theoretical considerations are presented in Part II.
 141

2. Flow measurement techniques

Various ways of making the flow in liquids visible have been suggested.
The simplest involves the use of particles or dyes which follow the motion
of the liquid. More elaborate arrangements include the optical method of
Schlieren and Toepler and those which utilise the Doppler effect. Here the
observed change in frequency of a monochromatic light beam or an ultra-
sonic sound wave, when it passes through the moving fluid, can be used to
deduce the flow.

3. Direct methods

Gray and Lewis [13] detected electrically induced motion in hexane

using Sudan Black dye. Ostroumov [7] observed rapid motions in electrically
stressed electrolytes containing an unspecified dye. Hoburg and Melcher [14]
used clear and dyed corn oil to study the behaviour of the interface between
electrically stressed liquids of different conductivity in relation to the high-
field mixing process.
Jolly and Melcher [15] injected small air bubbles into corn oil in their
observations of the steady cellular convection at the plane surface of an
insulating liquid layer. Malkus and Veronis [16] used aluminium dust in
paraffin to trace out Streamlines in their study of electroconvection at
curved liquid surfaces. In an experimental analysis of bulk electroconvection
in a mixture of carbon tetrachloride and kerosene, Mackey [17] used neutral-
ly buoyant polyethylene particles, coated with a gold--palladium alloy, to
follow the liquid motion.

4. Indirect methods

4.1. Toepler--Schlieren system

The method was used by Chadband and Wright [18] and Farazmand [19]
in studies of pre-breakdown and breakdown phenomena in liquid dielectrics
respectively, and by Hakim and Higham [20] in an investigation of the excess
pressures produced in dielectrics stressed by electric fields. Finally, Hopfinger
and Gosse [ 21] presented Schlieren photographs of the turbulent flow
caused by injecting charge into nitrobenzene.
A drawback associated with the application of the Schlieren method of
liquid flow is that only very small variations in the refractive index can be
expected under conditions of constant density.

4.2. The laser Doppler velocimeter

The laser Doppler method has been applied to the measurement of elec-
trohydrodynamic velocities in liquid insulants in the presence of charge
142

injection from corona emitters [22] [23]. In the former case, the laser light
was scattered by:
(1) alumina powder in paraffin, which did not affect the conductivity of
the liquid, and
(2) iodine in transformer oil, which increased the conductivity slightly.
In the latter case, light was scattered by naturally occurring contaminants in
hexane.
The drawback associated with the application of the laser Doppler effect
to electrohydrodynamic measurement is that the scattering contaminants
must be electrically inert, which is not necessarily the case.

4.3 Ultrasonic technique

A method which uses the phase shift between an upstream and down-
stream ultrasonic wave has been developed by Kalmus [24]. Unlike the laser
Doppler technique, it does not rely on the presence of impurity particles in
the liquid and thus may prove to be a valuable tool in assessing electrohydro-
dynamic behaviour.

5. Choice of flow visualisation technique

The introduction of dye into the liquid alters its conductivity and, be-
cause of diffusion and electrical mixing, the times allowed for observation
are limited. The drawbacks associated with the laser Doppler technique
have been outlined by Mackey [17], where he pointed out that the method
is incapable of differentiating between particle motions linked directly with
the electric field and those due to liquid convection. The behaviour of im-
purity particles in insulating liquids under electric stress as described by
Mackey has also been reported by Nossier [25]. In addition, Masuda and
Matsumoto [26] have analysed the behaviour of charged impurity particles
in electrically stressed inviscid media. The Schlieren method was rejected
because the deflection of the light beam after its passage through the liquid
would have been difficult to detect under conditions of constant density.
Of the two remaining techniques which have been described, the flow
visualisation particle method was chosen on the grounds of simplicity and
directness.

6. Experimental apparatus

The most convenient way of detecting electroconvective motions in the

bulk of electrically stressed dielectrics was that used by Mackey as described
in [17]. Here, electrically inert polyethylene particles with an average di-
mension of 150/~m were introduced into carbon tetrachloride and kerosene
mixed in such proportions as to make them neutrally buoyant.
In the present case, the liquid was contained in long rectangular cells
 143

designed to facilitate the illumination of those particles suspended in a given

cross section of the liquid. The external electric field was applied by means
of electrodes which constituted part o f the cell boundaries and the m o t i o n
of the illuminated particles could be observed through an inclined mirror
placed above the cell.
The experimental arrangement is illustrated in Fig.1. It consisted of an
external light source with lenses positioned to bring the light to a parallel
beam. This passed through a vertically traversible narrow slit in a shroud
which concealed the electroconvective cell. The slit was 3 m m thick and as
wide as the optically flat glass wall of the cell facing it, so t h a t the light il-
luminated those polyethylene particles suspended in an entire cross section
of the liquid. These showed up as points of light and on application of an
electric field they moved in roughly circular paths which remained in the
illuminated cross section of the cell. An inclined mirror above the cell
reflected this light to a camera which recorded the particle m o t i o n photo-
graphically.

Fig.1. The experimental arrangement: a, air-cooled box; b, light bulb; c, camera; l, lenses;
m, mirror; P, illuminated polyethylene particles; r, reflector; s, shrouds; v, to high-voltage
source.

7. The electroconvective cells

Three electroconvective cells were made. The first of these was a cubical
box, whilst the other two were tall containers with a square cross section.
The glass used in the cells was optically fiat and 4 m m thick. The plane
electrodes were made from stainless-steel strips 0.56 m m thick. Each cell
was provided with a glass lid which recessed into the t o p of the cell so t h a t
when the cells were full of liquid no free surface was present.
The cubical cell shown in Fig. 2, was of interior dimension 6.2 cm and
contained two 6.2 cm × 2.4 cm strip electrodes. These were glued, with
144

Fig.2. S p l i t - e l e c t r o d e s h o r t cell, i n t e r i o r d i m e n s i o n 6.2 c m X 6.2 c m X 6.2 era: e, 2.4 e m

X 6.2 c m stainless steel e l e c t r o d e s ; 1, recessed lid.

\ /\e

\
\

Fig.3. Parallel-electrode l o n g cell w i t h e l e c t r o d e edges o u t s i d e , i n t e r i o r d i m e n s i o n s 5 c m

× 5 c m × 20 c m : e, 10.5 c m x 20 c m stainless steel e l e c t r o d e s ; 1, recessed lid.

Fig.4. S p i n d l e e t e c t r o d e cell, i n t e r i o r d i m e n s i o n 5 c m × 5 c m × 20 c m : e, 1.4 m m dia-

m e t e r spindle e l e c t r o d e s ; 1, recessed lid.
 145

their edges parallel and separated b y a distance of 1.4 cm, to one of the
glass wails of the cell.
The tail cells b o t h had interior dimensions of 20 cm × 5 cm × 5 cm. The
first of these, shown in Fig. 3, had parallel-plate electrodes facing one an-
other. These were 20 cm × 10.5 cm steel plates and t h e y formed opposite
walls of the cell with their edges lying outside it.
More non-uniform fields were provided by the cell shown in Fig.4, where
stainless-steel spindle electrodes of diameter 1.4 mm and length 20 cm were
positioned in diametrically opposite corners of the cell.

8. Experimental m e t h o d

When an electroconvective cell was ready for use, it was filled with the
liquid sample containing polyethylene particles and closed with the recessed
lid so that no free surface of the liquid was present, after which it was placed
in the apparatus described in section 6. When sufficient time had elapsed
for the initial liquid m o t i o n to subside, the particles in a section of the
liquid midway between the t o p and b o t t o m o f the cell were illuminated and
they were visible as stationary points of light suspended in the liquid.
In this state, the liquid was electrically stressed b y means of the external
field. At sufficiently low fields, no motion was observed, b u t as the applied
voltage was increased there came a point at which the particles were seen to
begin to move. There was a time delay of a second or more b e t w e e n the
application of this voltage and the c o m m e n c e m e n t of the motion, which then
developed gradually to a steady state. These features were examined b y
Mackey [17] ; see also [27].
Visual observation revealed that the particles moved round the cell, remain-
ing more or less in the illuminated cross section of the liquid. This indicated
that the motion was essentially two-dimensional.
The way in which the particles moved suggested that they were being
carried round b y convective motions in the liquid rather than b y electric
forces acting directly on them.
Although the polyethylene particles behaved as though they were electric-
ally inert, they did tend to accumulate dielectrophoretically at the electrodes,
especially near their edges where the field was most non-uniform. However,
the speed of this process was negligible compared with that o f the circulating
motions, though it did result in the loss of a significant n u m b e r of flow
visualisation particles from the liquid bulk after long periods of electric
stress.
Because dielectrophoresis is present with b o t h d.c. and a.c. fields, an a.c.
variable-voltage generator, capable of supplying fields oscillating at 50 Hz,
was substituted for the d.c. one. Application o f oscillating fields b y this
means produced no visible motion in any of the electroconvective cells,
even at field strengths as high as 100 kV/m, though the tendency for the
particles to collect at the electrodes, as previously described, persisted.
 146

9. Photographic results

In this section, photographs are described which depict the fully devel-
oped bulk motion of the liquid sample under electrical stress in each of the
electroconvection cells described in section 7. Each photograph represents a
horizontal cross section of a cell in which a glass wall is uppermost in the
picture -- so that the light beam enters from the t o p of the picture and
proceeds downwards -- and is accompanied by a schematic diagram of the
streak pattern it displays. Beneath each diagram is given the magnitude, A ¢,
of the potential differences applied between the electrodes and the time
exposure, exp., of the photograph.

i llll

F i g . 5 . S p l i t - e l e c t r o d e s h o r t cell, ~ = 1 . 5 k V , e x p . = 3 0 s.

F i g . 6 . S p l i t - e l e c t r o d e s h o r t cell, A~ = 2 . 5 k V , e x p . = 3 0 s.
 147

Fig.7. Split-electrode short cell, A~ = 3.5 kV, exp. = 30 s.

The first set of photographs in Figs. 5 to 7 show the flow pattern in the
split-electrode short cell at different values of the applied voltage. The elec-
trodes are on the left wall of the square with the earthed one uppermost.
The single central vortex persisted throughout the voltage range, b u t at
potentials in excess of 3500 V, small vortices appeared in each corner o f the
square.
The flow patterns which occurred in the parallel-electrode long cell with
the electrode edges outside the cell are shown in Figs. 8 to 10. Here, at
applied potentials of less than 2000 V, the particles remained almost
stationary. At 3000 V t w o vortices appeared in the t o p and b o t t o m halves

Fig.8. Parallel-electrode long cell, ~ - 3 kV, exp. 10 s.

148

'It--

"F"-

Fig.9. Parallel-electrode long cell, A ~ = 4 kV, exp. ffi 6 0 s.

Fig.10. Parallel-electrode long cell, A~ = 5 kV, exp. = 60 s.

of the square. At 4000 V a central vortex, together with two or three sub-
sidiary ones situated close to the lower glass wall o f the cavity, developed,
with the liquid in the top comers stationary. This picture persisted with
increasing voltage up to 6000 V.
Figs. 11 to 15 depict the flow behaviour in the spindle electrode cell. The
earthed and high-tension electrodes are, respectively, at the b o t t o m left-
and top tight-hand comers of the cavity. The initial motion at 1000 V was
made up of vortices which changed in number and location with time. At
 149

.jJ--

Fig.11. Spindle electrode cell, A ~ ffi1 kV, exp. = 50 s.

Fig.12. Spindle electrode cell, A ~ = 2 kV, exp. ffi30 s.

Fig.13. Spindle electrode cell, A ~ = 3 k V , exp. = 50 s.

150

applied potentials greater than 2000 V this variable pattern settled down
into one comprising four triangular vortices. This picture remained as the
voltage was raised, until it reached 4000 V, when only two vortices were
evident. These had their centres in diametrically opposite corners of the cross
section. As the voltage was increased to 6000 V, the two vortices persisted
although the streaklines became less ordered.

L ~ v .....

F i g . 1 4 . S p i n d l e e l e c t r o d e cell, A~ = 4 k V , e x p . = 4 0 s.

F i g . 1 5 . S p i n d l e e l e c t r o d e cell, A¢ = 5 k V , e x p . = 50 s.

10. Conclusions

It is probable that the single vortex occurring in the short split-electrode

cell shown in Figs. 5 and 6 was due to a shearing force which acted in the
region between the electrodes where the field was most intense. This shear-
ing force could have arisen because of the action of the field on either the
 151

diffuse charge layer adjacent to the glass wall separating the electrodes, or
any charge which was injected into the liquid from the sharp edges of the
electrodes.
The formation of the four subsidiary vortices which appeared in the comers
of the square at applied potentials in excess of 3500 V, as in Fig.7, may be
explained as follows. Considering for the moment the two right-hand comers
of the square most distant from the electrodes, it is suggested (Greenspan
[28] ) that subsidiary vortices of this form accompany one large central
vortex in cavity flow for which a shearing force occurs at one wall of the
cavity. This phenomenon begins to occur when the wall Reynolds number
based on cell dimensions and a typical maximum fluid velocity is about 50.
The vortices which occurred in the left-hand comers of the square can be
attributed to an additional minor shear associated with charge injection
which, at high field strengths, developed at the edges of the electrodes
adjacent to the top and bottom glass walls of the cross section.
Figure 8 indicates that at 3000 V vorticity was created in the liquid bulk
when it was electrically stressed in the parallel-electrode cell with the
electrode edges outside the cell. This bulk vorticity was again probably
created by charge injection from the centre of the electrode, for the streak-
line picture in Fig. 8 resembles one suggested by Felici [ 29 ], which covers
such a case.
Figures 9 and 10 suggest that, at higher voltages, coupled shearing forces
occurred in the liquid close to the glass walls of the cavity.
The photographs in Figs. 11 to 15 indicate that with the liquid in the
spindle electrode cell, subjected to an applied potential of 1000 V, charge
injection initially created vorticity in the liquid bulk, but at higher potentials
shearing forces operated at the walls of the square. It could be that at applied
potentials between 2000 and 3000 V these shearing forces acted in opposi-
tion to the bulk forces associated with charge injection, to create the four
triangular vortices shown in Figs. 12 and 13. At higher potentials one or
other of these forces could have taken over, to create the two vortices ap-
parent in the remaining photographs of this cell.

Appendix. Physical properties of the liquid

The conductivity of the liquid sample under investigation was measured

using a potential decay method described by Klinkenberg and Van der Minne
[30] and further elaborated by Hignett [31].
The values of density, kinematic viscosity and dielectric constant of the
liquid sample were obtained from Mackey's thesis [17] the justification
being that since the polyethylene particles came from the same source as
those used by Mackey then they would be neutrally buoyant in the same
liquid mixture as that used by him.
The properties are listed in Table 1.
152

TABLE 1

Properties of the liquid investigated (mixture: 63% kerosene + 37% carbon

tetrachloride)

Density Kinematic Dielectric Approximate

viscosity constant conductivity

(kg m -3) (m 2 s-1) (S m "1)

1.07 × 103 9.85 × 10 -7 2.14 6.5 × 10 "12

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