Accepted Manuscript

Experimental study on the role of electrical conductivity in pulsating modes of

electrospraying

S. Faraji, B. Sadri, B. Vajdi Hokmabad, N. Jadidoleslam, E. Esmaeilzadeh

PII: S0894-1777(16)30302-8
DOI: http://dx.doi.org/10.1016/j.expthermflusci.2016.10.030
Reference: ETF 8916

To appear in: Experimental Thermal and Fluid Science

Received Date: 4 May 2016

Revised Date: 29 September 2016
Accepted Date: 23 October 2016

Please cite this article as: S. Faraji, B. Sadri, B. Vajdi Hokmabad, N. Jadidoleslam, E. Esmaeilzadeh, Experimental
study on the role of electrical conductivity in pulsating modes of electrospraying, Experimental Thermal and Fluid
Science (2016), doi: http://dx.doi.org/10.1016/j.expthermflusci.2016.10.030

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Experimental study on the role of electrical conductivity in pulsating modes
of electrospraying
S. Faraji a,*, B. Sadrib , B. Vajdi Hokmabadb, N. Jadidoleslamd, E. Esmaeilzadeh*,c,e

a: Department of Chemical Engineering, Istanbul Technical University, Istanbul, Turkey

b: Department of Mechanical Engineering, University of Alberta, Edmonton, Alberta, Canada

T6G 2G6

c: Heat and Fluid Flow Research Laboratory, University of Tabriz, Tabriz, Iran

d: IIHR-Hydroscience & Engineering, The University of Iowa, Iowa City, IA 52242, USA

e: Research branch, Islamic Azad University, Tabriz 51666, Iran

*E-mail: farajis@itu.edu.tr , esmzadeh@tabrizu.ac.ir, Tel: +00985312738137, Fax:

+0984113354153

1
Abstract

In the present experimental study, the effects of electrical conductivity on electrospraying

modes and its produced droplets are investigated. A metallic nozzle with 0.6 mm ID as high

voltage electrode were employed in a point to ring electrode configuration in this work.

Experiments were carried out in still room temperature. Four different aqueous KCl solutions

were sprayed in various high voltages and flow rates. Results confirmed that spraying modes

are more dependent on electrical conductivity rather than flow kinetics. Applied electrical field

required to form a cone shape on the nozzle tip decreases with increasing conductivity.

Moreover, results revealed that electrical conductivity of dispersed solution plays a decisive role

on elongation of the cones in ES procedure. Smaller size of produced droplets was obtained by

increasing conductivity of dispersed liquid while velocity of filaments emanated from liquid jet

decreases at the same time. In this study, we have presented insight to the role of

physicochemical properties on the pulsating modes of spraying.

Keywords: Electrospray, electro-hydrodynamic (EHD), Electrical field, Electrical conductivity,

Taylor cone

1. Introduction

Electrospraying of liquids is a well-established process for producing submicron particles. This

spraying method, also known as electro hydrodynamic atomization (EHDA) is a process in

which high electrical field is employed to disperse a liquid. High voltage is applied to liquid

supplied through an emitter (usually a metallic capillary). In the electrospraying (hereafter ES),

the shear stress, as a result of the electric force applied to the surface of liquid, elongates the

liquid meniscus formed at the tip of a capillary to the shape of a cone and/or a jet which then

2
deforms and disrupts into droplets due to the electrical and mechanical forces. In EHDA, no

additional purely mechanical energy is applied to spray the liquid. Electrohydrodynamic

spraying has wide range of applications ranging from fine resolution electrohydrodynamic

printing [1–3], agriculture [4] polymeric nanofiber and nanoparticle production [5], biomedical

application especially drug delivery system [6] [7] and producing stable emulsions [8] [9].

Early works on the electrified surfaces have been done by Zeleny in 1917[10]. In 1969, Taylor

conducted series of experiments on liquid jets inside electrical field [11]. As a part of these

experiments, conical shape formation on electrified jets is observed which became known as

cone jet mode of spraying. In this respect, Fernandez de la Mora and Loscertales investigated

diameter of droplets and the current emitted from electrosprays in the cone jet mode [12]. They

also studied the effect of physical parameters like electrical conductivity, viscosity, liquid

density, and the feed rate on the ES in the same regime of spraying [13]. Tang and Gomez also

studied cone-jet mode in low conductivity of dispersed liquids in which they found flow kinetics

is primarily effective in the size of produced droplets [14]. Experimental observation of the

effect of dielectric constant in cone jet mode spraying has also been investigated by Chen and

Pui [15]. Moreover, they have introduced scaling laws between producing droplets and

dielectric constants.

For different working feed rates and applied voltages, regimes different from cone jet mode

appears on the tip of nozzle. Smith investigated ES procedure on the different conditions

including different liquid properties (e.g. electrical conductivity, viscosity and etc.). He concluded

that specific conductivity is required for ES procedure, however, there is no higher limit of

conductivity in this process [16]. Cloupeau and Prunet-Foch studied ES modes and presented

the classification based on their observation [17]. They reviewed ES modes and explained the

details of difference between working regimes of ES procedure [18]. Astable modes of spraying,

as a part of EHD spraying modes, attracted growing interest in the recent years [19] [20][21].

These modes of spraying occur in the transition between three axial modes of spraying

3
(Dripping, Pulsating, and cone-jet). Recently, Verdoold et al. introduced electric current as a

convenient tool for controlling different modes of ES process[22]. Besides, Gan et al observed

four types of ES modes including pulsed-jet, cone-jet, skewed cone-jet, and multi-jet as well as

determining jet and spraying regions for the different flow rates and voltages in their most

recent study on the ES of ethanol for using in a small-scale combustor application [23]. Recently,

Pongrac et al. employed time-resolved imaging to understand the effect of electrical conductivity on

the behavior of disintegrated filaments by measuring velocity and size of produced droplets [24].

They reported that lower conductivity of dispersed water resulted in smaller size of droplets and their

higher velocity.

Apart from this, the effect of physical parameters in the ES process has an undeniable role in

manipulation of produced droplets. Viscosity, as one of prominent physical parameters, was

studied by Ku and Kim [25]. They investigated produced droplet diameter and compared their

results with existing scaling laws which demonstrate an evident discrepancy in the size of

produced droplets due to high viscosity of dispersed liquid.

However, the role of electrical conductivity on the ES modes, other than cone jet regime,

remains incomplete or even poorly understood. In fact, other modes of spraying encompass a

large volume of working area of ES that are still obscure in finding their way to become

prominent applications which calls for further investigation.

In the present experimental study, the results are divided to three parts: the first part is the role

of electrical conductivity on the modes of spraying. The second part pertains to the behaviour of

the emerged menisci on the tip of nozzle with different conductivities. The last part of study is

about the diameter of droplets and their emerging velocity in pulsating cone jet mode with

different conductivities. Moreover, velocity of electrosprayed droplets produced by pulsating

functioning modes is studied which may help in producing promising avenue of pulsating ES

into the coating and printing industry [1]. Most of the ES publications to date are related to

droplet diameter in the cone jet mode and disregards to the droplet produced in the other

4
modes of spraying like pulsating modes and the velocity of these drops. In the present study, the

authors strive to present a thorough image for behaviour of produced droplets in pulsating

modes.

2. Materials and methods

An experimental setup, consisting of a metallic nozzle and a ring with 0.6mm and 30mm in

inner diameters, respectively, was developed to study ES process. The ring was fixed at 25mm

below the nozzle tip. A schematic illustration of the experimental apparatus and used nozzle is

presented in

Figure 1. The nozzle is employed as high voltage electrode which was connected to the high

voltage power supply and the ring acts as grounded electrode. The liquid, deemed to be sprayed,

was fed to the nozzle by means of a syringe pump through an insulator tube. Combined effects

of gravity, back pressure in the tube, and the electric forces cause the liquid to discharge

5
vertically downstream through the nozzle toward the ring electrode. Tangential Electric

stresses resulted in spraying of the liquid in different electrosparying modes.

In order to study the effects of electrical conductivity on ES process, KCl was dissolved in

distilled water. Adding KCl changes electrical conductivity of water, dramatically. Electrical

conductivities of water and aqueous KCl solutions were measured by Conductivity-Meter

(EZTECH AZ- 8361) which are reported in Table 1.

Table 1: Electrical and physical properties of dispersed solution.(at 20°C).

Materials Distilled KCl solution KCl solution KCl solution

water
[0.01 Molal] [0.10 Molal] [1.00 Molal]

Electrical 0.042E-3 1.634E-3 11.820E-3 108.620E-3

Conductivity [S/m]

Electrical Permittivity 1.0006 1.0006 1.0006 1.0006

[F/m]
Surface Tension 72.80 72.85 73.30 74.90
[mN/m]

Density [kg/m3] 998.2 998.2 1001.75 1041.48

Viscosity [Pa.s] 8.90E-4 8.90E-4 8.91E-4 9.04E-4

It is worthy to note that the permittivity of water does not change with adding KCl, therefore it

was assumed constant during the experiments this property [26]. The pH of solution for various

electrolyte concentrations was measured to be within the range of 5.6 to 5.8 which confirms the

neutrality of the dispersed liquids. Furthermore, the changes in amount of viscosity [27] and

surface tension [28] are negligible compared to the changes in electrical conductivity.

Imaging of liquid meniscus were performed by a digital single-lens reflex (DSLR) camera (20D

Canon) with 22.5 mm by 15.0 mm CMOS sensor size. This model of camera is selected

specifically due to the crop factor of this camera that makes it capable of within the range of

1000 to 8000 [1/s] shutter speed. In order to achieve better visualization and focus on the

nozzle tip, 500 [mm] macro lens was installed to the camera. The camera was fixed in front of

the nozzle tip and a cooled light supply with 5000-11000 [flash/min] exposure times was

6
employed to achieve the desired type of time-resolved imaging. With aid of systematic imaging,

the droplet size is obtained by image analysis software. Subsequently, droplet velocity is

measured by measuring the distance between two consecutive frames.

7
8
 Figure 1: Schematic illustration of the experimental apparatus and nozzle.

3. Results and discussions

The role of electrical conductivity on the unstable regimes of ES has been divided into three

major parts: prior to liquid ejection from nozzle, at the tip of the nozzle, and after emission from

the nozzle.

3.1 effect of conductivity on ES modes

Effect of liquid conductivity on the ES procedure is studied in this section. Figure 2 shows

different modes of ES for various applied voltages and electrical conductivities. As depicted in

Figure 2, six unsteady modes were observed in this study. The dripping mode was the

preliminary mode of spraying in which the electrical forces on the surface are not strong enough

9
to make a distinctive mode. The main feature of this regime is the increase in dripping

frequency with drop size reduction as a result of augmentation of applied voltage. This regime

promises a high mono-dispersity with rather higher size of droplets. Microdripping regime, on

the other hand, produces mono-disperse droplets with much lower size. In this regime, the

emission takes place droplet by droplet[18]. For rather high applied voltages, oscillating jet

appears on the tip of nozzle in which the swirling of jet front and the vigorous lashing take

place. The unstable cone jet mode, which shows sporadic spraying in cone jet mode, is observed

in 0.1 molal KCl solution for the first time. In the spindle modes of spraying, a filament attached

to the nozzle tip stretches and droplets form by creation of fine jet out of this spindle[18].

Creation of multiple jets out of filament, appeared on the nozzle tip, is the main feature for

multispindle jet mode. The critical voltage, in which the electrified nozzle discharges itself to the

ring as a ground electrode via the air, is defined as discharging voltage. As illustrated in Figure 2,

different modes of spraying are observed simultaneously at the same working condition, i.e.

electrical conductivity and applied voltage which is possibly stem from the electrical field

inconsistencies along the liquid surface that results in bifurcate behavior of spraying [29].

Moreover, these inconsistencies may possibly be associated with point to ring electrode

configuration. Apart from this, discharging voltage diminishes for more conductive solutions

since these solutions provide more charges at the nozzle tip in similar applied voltage. For

instance, the discharging appears in 12kV and 10kV applied voltage for 0.1 and 1 molal KCl

solution, respectively. Interestingly, in spite of the fact that higher liquid conductivity engenders

lower tangential stress on the liquid interface, unstable cone jet mode seemingly appears at

lower applied voltages in higher liquid conductivity. Other than that, presence of at least two ES

functioning modes maybe attributed to electrical field inconsistencies as well as instability of

these modes. In fact, the presence of various ES functioning modes in figure 2 indicates that

electric forces mainly control different modes of spraying due to the presence of various charges

at the tip of nozzle.

10
Apart from this, flow rate, as another important factor on ES process, is studied experimentally.

As illustrated in Figure 3, effect of flow rate on altering the spraying behavior is small compared

to the effect of applied voltage in this specific flow rate range. Regardless of applied electrical

field, functioning modes of spraying remain fairly constant in various flow rates. Without

considering the suction phenomenon throughout spraying process [30], the volume flow rates

are displayed in the figures. As depicted in Figure 2 and 3, it is observed that microdripping

regime and multispindle regime as well as mutispindle and unstable cone jet mode can occur at

the same working condition. The difference in between these two group of functioning modes

lies behind the oscillating movement of filament attached to the nozzle. This oscillating

movement, which generally stems from increase of the flow kinetics in narrower size of

filaments, could happen at the same working condition that stable filament is formed. Besides,

the electrical field inconsistencies, due to electrode geometry, could be the other possible factor

effective in this process.

11
Figure 2: Electrospraying modes for different KCl solution in different applied voltage (the nozzle
inner diameter=0.6 mm).

12
 Figure 3: Modes of spraying with different flow rates and various voltages.

3.2 Effect of conductivity on the cone of the capillary

Exposed menisci on the tip of nozzle undergoes different shapes in various applied electrical

fields which can be explained by determining three parameters as follows[15,31]:

Here, are the liquid density, breakup length, surface tension, and electrical

conductivity of the employed liquid, respectively. The associated forces in ES process requires a

13
systematic definition of timescales to understand the extent of the forces in this process. In this

respect, capillary timescale defines gravitational to surface forces, while, charge relaxation time

shows the rate of diminishing of charge in the volume. Alpha (), as the ratio of capillary to

electric relaxation time, is defined to show the ratio of forces associated with fluid properties to

the forces of electrical properties. Please note that , in Equation 3, is the ratio of capillary

timescale to charge relaxation time. On the other hand, the non-dimensional flow rate is given

by the following equation [28]:

Where flow rate is associated with electrical conductivity and surface tension to bring the

factors effective in ES process altogether. It is worth adding that onset voltage is defined as a

voltage which cone shape mode is observed in this study. The onset voltage fluctuations versus

are depicted in Figure 4. This voltage decreases with rising of conductivity for different KCl

solutions. In fact, dispersed liquid experiences higher rate of normal forces due to higher

amount of charge in the liquid with higher conductivity while tangential forces diminish owing

to smaller drop of electrical field on the interface [24]. On the other hand, onset voltage shows

less sensitivity to working flow rates at the same conductivity of the solution which proves

again predominancy of electrical forces over hydrodynamic forces.

14
 Figure 4: Onset voltage for different values of alpha ().

From theoretical point of view, more conductive liquids obtain charges rapidly. Increase in

conductivity of dispersed phase leads to intensification of electric forces on the capillary due to

more net charge which makes cone form in lower electrical fields on the capillary. For better

understanding on the interaction of these forces on meniscus, Figure 5 is presented. According

to this figure, normal electric stresses are the main reason for forming of liquid cone. At the cone

surface, normal electric stress is balanced by surface tension and viscous forces counterbalance

the tangential electric stress [32]. These normal electric stresses intensify on the capillary with

increasing conductivity of dispersed liquid which leads to form the cone shape in lower

voltages.

15
 Figure 5: Schematic illustration of exerted forces on the meniscus of the capillary.

The EHD body force is expressed as follows [8]:

where are charge density, electrical field, permittivity and liquid density,

respectively. Mentioned force consisted of three terms in which its first term is coulomb force

(electrophoretic) which exerts on positive and negative free charges, the second term is

dielectrophoretic force, mainly depends on electric permittivity gradient, and the third term is

electrostrictive force pertaining to compressible fluids. Here, the dielectrophoretic term can be

neglected because of great amount of electric charge which leads to strengthening

electrophoretic forces. Moreover, the third term is considered negligible due to the properties of

employed liquid.

Owing to the fact that more the conductivity gives rise to more the charge, the electrophoretic

force increases in higher concentration electrolyte in the solution. Therefore, cone exposed to

more electrical forces which cause more vertical extension.

Another important point that could be obtained from Figure 5 is the effect of flow rate on the

cone length. Higher hydrodynamic field leads to more hydrodynamic pressure which elongates

16
the cone menisci in the normal direction. The rate of augmentation of cone length diminishes

with increasing the conductivity of dispersed phase. This behavior was significantly shown in

Figure 6. In Figure 6, the pictures of cone elongation are presented for all solutions in four flow

rates which represent visual comparison between all observed cones.

Figure 6: Illustration of cone elongation on the capillary for different KCl solutions.

Figure 7 shows the cone length variation versus We/Wee that is defined as follows [33,34]:

17
This non-dimensional number illustrates the behavior of hydrodynamic field with respect to the

electrical field. In fact, increasing of electric Reynolds number delineates augmentation of

hydrodynamic forces compared to electrical forces which are the main players in the ES

process. As depicted in Figure 7, cone elongates with rising of electric Reynolds number in which

the slope of variation in cone length diminishes with reduction of electrical field. This behavior

demonstrates the decisive role of electrical field on the behavior of cone. As mentioned before,

since the liquids with higher conductivity experience more exerted electric forces, the maximum

cone elongation take places in the case of 1 molal KCl solution. It is worthy to note that whole

procedure is undertaken in high electrical field compared inertia forces as shown in Figure 7.

Figure 7: Length of the cone variation versus π.

18
3.3 The behavior of emanated droplets and effect of conductivity

The behavior of emanated droplets in the cone-shape jet modes of spraying is very important

for industrial applications. Since polydispersity in radius of droplets and their irregular velocity

result in malfunctioning in highly desired applications of ES process e.g. thin film deposition and

microscale ink jet printing [35], the evolution of droplet during this process needs a detailed

study.

As shown in Figure 8, the droplet velocity initially increases and eventually reaches to a plateau

in higher flow kinetics. Furthermore, velocity of the drops rises with diminishing conductivity

as demonstrated in figure 9. One of the possible implications of this reduction is pertained to the

electrical field strength in various electrolytes of dispersed fluid in which more conductive

liquids require less electrical forces to form cone shape at the tip of nozzle. It is obvious that the

surface charge diminishes due to less conductivity in solutions with lower KCl concentration

[36], [37]. Hence, according to equation [5], two main factors are intensification of electrical

field and reduction of surface charge density. It is worth adding that the results implicate that

intensification of electrical field is the prevailing factor in this process. For instance, the cone-

shape appears in the highest voltage for water, which has the minimum conductivity and

surface charge among employed solutions, therefore, strength of electrical field is maximum in

comparison with other sprayed liquids. As depicted in Figure 8, highest velocity belongs to

water due to maximum value in the strength of electrical field in spite of its minimum surface

charge density.

The effect of electrical field on the velocity of droplets is shown in Table 2. As shown in this

table, electrical Weber number Wee diminishes with conductivity leverage. Electrical Weber

number(Wee) [36] presents the behavior of electric forces with respect to the interfacial forces.

In other words, decreasing in electrical weber number demonstrates shrinking of electrical field

so it is reasonable to deduce that electrical field forces act a main role in motion of droplets. It is

19
interesting that electrical forces are mainly controlling the velocity of droplets in wide range of

dispersed liquid conductivity [38].

Droplets motion is not the only factor important in the coating and printing industry but also

the size of droplets is paramount element for the ES applications. Variation of droplet size

versus applied electrical field is also illustrated in Figure 9. Taking measurements of droplet

diameter in unstable cone jet mode on board, the droplet size increases with flow rate

increment. On one hand, regarding to the constant applied voltage in each concentration,

increasing of droplet size arises from hydrodynamic force intensification which is in good

agreement with [8]. Similar to droplet velocity, size of produced droplets is more dependent on

the electrical conductivity rather than flow rate. This findings is in contrast with the reports on

low conductivity liquids in which flow rate is mainly effective on the size of droplets [14]. The

size distribution of droplets also proves that electrical forces are very important in determining

the range of produced droplets. This information can be found in the supporting information

(Figure S2). It is noteworthy that the diameter of observed droplets is in the range of 150-460

micrometer in all experiments.

On the other hand, raising conductivity leads to diminishing drop sizes that stems from the

presence of more charges in the liquid solution during the process. Regarding to the fact that the

charge of droplet size depends on the magnitude of applied electrical field and electrical

properties of liquid such as conductivity, the interaction between these parameters influences

the size of droplets.

20
 Figure 8: Droplet velocity variation versus flow rate for different dispersed solution.

Table 2: The variation of Electrical Weber number versus Conductivity.

Conductivity 0.0420 E-3 1.634 E-3 11.820 E-3 110.620 E-3

(S/m)

Electrical Weber 453.092 435.195 415.360 373.871

number

21
 Distilled water, V=4.2 kV 0.01 molality of KCl solution, V=4.1 kV

0.1 molality of KCl solution, V=4 kV 1 molality of KCl solution, V=3.8 kV

Figure 9: Droplet size variaton versus flow rate for four different dispersed solutions

(d is droplet size and D is nozzle diameter).

ES functioning modes change from microdripping in low flow rates to pulsating cone jet mode in

higher flow rates. In this range of flow rates, there is no significant increase in droplet size for

distilled water whereas increase in droplet size is observed for KCl electrolyte solutions in

which this process delineates the effect of increasing charge on the augmentation of drops sizes.

22
As shown in Figure 9, salt additives on water rises the sensitivity of the solution to the flow rate

changes. However, this sensitivity slightly diminishes with adding salt.

Conclusion

Pulsating modes of spraying, as the working area between three axial modes of electrospraying,

are studied experimentally in the current work. The two paramount factors, i.e. electrical

conductivity of the dispersed solution and flow rate, are the variables being considered in this

work to observe their possible effects on the pulsating electrospraying. Functioning modes of

spraying are pinpointed in various working conditions, i.e. applied voltage, conductivity of

solution, and flow rate. Results revealed that the stability of spraying functioning is much more

dependent on electrical conductivity rather than flow rate in their employed working range.

Cone shape emerged in lower applied voltages as the conductivity of solution increases which

delineates that force equilibrium reaches at lower applied voltages for higher conductivity of

solution.

Intensifying normal electric force, as a result of increasing solution conductivity, leads to more

cone elongation. The velocity of detached droplets, along with cone elongation, increases with

strengthening of applied electrical field. Velocity of droplet is lower for higher concentration of

salt that shows the decisive role of applied electrical field in accelerating droplets. Not only

velocity of droplets but also their size, as an important aspect of produced droplets, decrease

with augmentation of electrical field and diminishing of flow rate. However, the effect of flow

rate on water droplets, as the least conductive solution in the experiment, is less pronounced

compared to salt concentrated solutions.

23
Nomenclature

Symbol Definition

tc Capillary timescale

 Liquid density

l Length

 Surface tension

te Electrical relaxation time

 permittivity

 Electrical conductivity

 Capillary to charge relaxation time ratio

2 Non-dimensional flow rate

K Electrical conductivity

Q Flow rate

0 Vacuum permittivity

f Charge density

E Electrical field

U Velocity

d Diameter

 Hydrodynamic to electrical field ratio

We Weber number

Wee Electric Weber number

24
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 Highlights

 Effects of electrical conductivity on EHDA modes and produced droplets are studied.
 Different aqueous KCl solutions were sprayed in various high voltages and flow rates.
 Spraying modes depend more on conductivity variation rather than flowrate fluctuations.
 Conductivity of solution acts a main role on forming and elongation of the cones.
 The velocity of detached droplet increases with applied electric field strengthening.

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