The minimum flow rate scaling of Taylor cone-jets issued from a nozzle

William J. Scheideler, and Chuan-Hua Chen

Citation: Appl. Phys. Lett. 104, 024103 (2014);

View online: https://doi.org/10.1063/1.4862263
View Table of Contents: http://aip.scitation.org/toc/apl/104/2
Published by the American Institute of Physics

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 APPLIED PHYSICS LETTERS 104, 024103 (2014)

The minimum flow rate scaling of Taylor cone-jets issued from a nozzle
William J. Scheideler and Chuan-Hua Chena)
Department of Mechanical Engineering and Materials Science, Duke University, Durham,
North Carolina 27708, USA

(Received 13 July 2013; accepted 30 December 2013; published online 15 January 2014)
A minimum flow rate is required to maintain steady Taylor cone-jets issued from an electrified
nozzle. This letter reports that the well-known scaling law proportional to the charge relaxation
time and independent of the nozzle diameter is only applicable to lowly viscous systems. For
highly viscous systems with rapid viscous diffusion, the cone-jet transitional region spans a length
scale comparable to the nozzle diameter; the minimum flow rate appears to be proportional to the
capillary-viscous velocity and the cross-sectional area of the nozzle, but independent of the liquid
C 2014 AIP Publishing LLC. [http://dx.doi.org/10.1063/1.4862263]
conductivity. V

The electrohydrodynamic Taylor cone-jet1–4 is funda-
mental to a variety of applications including electrostatic
spraying, spinning, and printing. In the most common setup, a
working fluid is pumped at a flow rate Q through a round noz-
zle, which is electrified at a voltage V with respect to a coun-
ter electrode plate using air as the surrounding medium.
Steady cone-jets are known to exist only for a limited stability
window in the voltage-flow rate (V – Q) operating diagram,
where the applied voltage is around the threshold giving rise
to the Taylor cone2 and the imposed flow rate is above a mini-
mum threshold necessary to sustain a steady jet.3 Although
the applied voltage (field) can be rationalized by balancing
the Maxwell and capillary stresses as in the case of the hydro-
static Taylor cone,2,5–7 the minimum flow rate required to sus-
tain a steady jet is much less well-understood.4,8–13 In
electrospraying systems with the common setup of a working
fluid pumped through an electrified nozzle, the minimum flow
rate (Qm) is known to scale as4,14–16
ec
Qm  ; (1)
rq
where e, c, r, and q are, respectively, the permittivity, surface
tension, electrical conductivity, and density of the working
fluid. This scaling law works well for the electrospraying of
liquids in the “high-conductivity” limit ðrⲏ1 lS=cmÞ,4 and
can be justified on dimensional grounds as long as the liquid
viscosity (l) drops out of the picture. Note that the length
scales of the overall system such as the nozzle diameter do
not enter the scaling law in Eq. (1), because the jet diameter
in the high-conductivity limit is typically orders of magnitude
smaller than the nozzle diameter for high-conductivity
liquids. The requirement of a minimum flow rate is believed
to give rise to pulsating cone-jets when the supplied flow rate
is smaller than this minimum value.17–20 In this sense, the
minimum flow rate scaling is relevant to the transient (quasi-
steady) cone-jets issued from solid nozzles18,19,21–27 as well
as liquid drops17,28–31 and films/pools.32–34
The absence of liquid viscosity in the minimum flow
rate scaling Eq. (1) lacks a rigorous justification, which poses
a severe limitation considering that highly viscous cone-jet
a)
Electronic mail: chuanhua.chen@duke.edu
systems are critical for many practical situations. In nanoe-
lectrospray, nozzles of micrometric or sub-micron diameter
are routinely used;23,35–37 In electrospinning, viscoelastic
polymeric fluids are typically employed;7,9,38,39 In electrohy-
drodynamic printing, fine nozzles are often used, sometimes
in combination with viscous working fluids.40–44 Despite the
practical relevance, systematic studies of the effects of vis-
cosity on Newtonian cone-jets are scarce, and the few avail-
able studies have not focused on the minimum flow
rate.34,45,46 Here, we study the role of viscosity (l) in deter-
mining the minimum flow rate (Qm) for Taylor cone-jets
issued from an electrified nozzle. We show that the conven-
tional Qm scaling Eq. (1) breaks down for cone-jets of highly
viscous working fluids, and that the Qm at high viscosity can
be a strong function of the nozzle diameter (D) instead of the
liquid conductivity (r).
Among the intrinsic properties of the working fluids (l,
q, c, e, and r), only viscosity and conductivity can be varied
by a few orders of magnitude without significantly affecting
other fluid properties. These properties and the nozzle diame-
ter were systematically varied and the corresponding mini-
mum flow rates measured. (Note that permittivity can be
changed by about an order of magnitude within the polar-
liquid limit,14,47,48 but is not systematically varied here.) As
shown in Table I, the working fluids were ethanol, ethylene
glycol or glycerol. These Newtonian working fluids spanned
three orders of magnitude in terms of viscosity. The liquids
were doped with potassium chloride to a desired range of
conductivities and confirmed with a conductivity meter
(Oakton 510). The conductivity was kept above the empirical
threshold of 1 lS/cm for high-conductivity fluids.4 To pre-
vent subconscious bias, the exact conductivity in most
experiments was measured immediately after the measure-
ments of the minimum flow rate (see Table S149). Note that
all three working fluids are commonly used for mechanistic
studies of cone-jets.50
To test the scaling laws, we focused on Taylor cone-jets
issued from a nozzle electrified with respect to a conducting
plate, where the working fluid was supplied at a constant
flow rate by a syringe pump (Legato 180). In addition to its
widespread adoption, the nozzle-to-plate configuration was
the easiest for accurate Qm measurements. Cone-jets were
produced on glass nozzles with outer diameters (D) ranging

0003-6951/2014/104(2)/024103/4/$30.00 104, 024103-1 C 2014 AIP Publishing LLC

V
024103-2 W. J. Scheideler and C.-H. Chen
TABLE I. Material properties of the working fluids based on literature val-
ues at 20  C. The concentration of the glycerol-water mixtures is by weight.
Working fluid l ½103 Pa  s q ½103 kg=m3  c ½103 N=m e=e0 [–]
Ethanol 1.2 0.79 22 25
Ethylene glycol 21 1.11 48 41
90% glycerol 220 1.24 65 47
96% glycerol 620 1.25 64 44
Glycerol 1400 1.26 63 41
from 125 lm to 840 lm at the nozzle exit. For smaller diam-
eters, tapered fused-silica nozzles (New Objective PicoTips)
were used with outer/inner diameters of 125/75 lm,
150/100 lm, and 210/150 lm, respectively. For larger diame-
ters, borosilicate capillaries (Vitrocom Vitrotubes) were used
with outer/inner diameters of 250/150 lm, 330/200 lm,
550/400 lm, and 840/600 lm, respectively. To assess the
potential effects of nozzle conductance, 460/260 lm stainless
steel capillaries (Hamilton 91026) were also used as
received. All glass nozzles were cut to a uniform length of
20 mm and fixed via plastic tubing sleeves to a metallic
union, through which the nozzle was grounded. The counter
electrode was negatively electrified (Trek 610E) and located
at a fixed distance of 1.5 mm from the nozzle tip. A textured
silicon substrate was used as the counter electrode to prevent
accumulation of the working fluid.51 All nozzles were ori-
ented horizontally so that potential gravitational effects were
discernable by an asymmetric cone.
Our experimental procedures to extract the minimum
flow rate followed the methodologies in Refs. 3, 18, and 52,
and were detailed in a prior publication.19 The minimum
flow rate (Qm) required to sustain a steady jet was extracted
as the lowest flow rate bounding the V– Q stability window;
see details in supplemental Fig. S1.49 For highly viscous
working fluids containing glycerol, extra care was taken to
thoroughly flush the electrohydrodynamic systems to avoid
trapping air bubbles, and short plastic tubing connection
between the nozzle and the pump was adopted to minimize
flow capacitances. The uncertainty in the Qm measurements
was typically within 630%, as shown below in Fig. 3 for
selected conditions. All error bars were based on 95% confi-
dence intervals.
Representative images of steady cone-jets of ethylene
glycol and glycerol are shown in Fig. 1. The steady cone-jet
of ethanol was similar to that of ethylene glycol. The main
qualitative difference between the ethylene glycol cone-jet
in Fig. 1(a) and glycerol cone-jet in Fig. 1(b) was in the
FIG. 1. Electrohydrodynamic cone-jets for (a) ethylene glycol and (b) glyc-
erol, each at 10 lS/cm with an outer diameter of 150 lm at the exit of the
tapered glass nozzle. The cone-jet transition was localized around the coni-
cal apex for ethylene glycol with a relatively low viscosity, but spanned the
entire cone for glycerol with a relatively high viscosity.
Appl. Phys. Lett. 104, 024103 (2014)
transitional region, which bridged the Taylor cone of a
dimension dictated by the nozzle diameter with a much thin-
ner jet (that accelerated further downstream). In the ethylene
glycol case with relatively low viscosity, the cone-jet transi-
tion was localized to within a few jet diameters; In the glyc-
erol case with relatively high viscosity, the transition region
extends much wider with a size comparable to the nozzle
diameter.
The minimum flow rates were measured for three sets of
working fluids with wide-ranging viscosities. In Fig. 2(a),
the nozzle diameter was fixed at 150 lm and the conductivity
was varied from 1 lS/cm to 25 lS/cm for each liquid. The
minimum flow rate was a strong function of conductivity for
ethanol and ethylene glycol, but independent of conductivity
for glycerol. In Fig. 2(b), the conductivity was fixed at
5 lS/cm, and the nozzle diameter was varied from 150 lm to
550 lm. The minimum flow rate was essentially independent
of nozzle diameter at low viscosities, but became a strong
function of diameter for highly viscous glycerol.
The minimum flow rate of ethanol and ethylene glycol
in Fig. 2 exhibited trends consistent with the conventional
scaling Eq. (1). However, the parametric dependence of
glycerol contradicted Eq. (1), with the minimum flow rate in-
dependent of the electrical conductivity but dependent on the
nozzle diameter. The diameter-dependence for glycerol was
consistent with the qualitative observation in Fig. 1(b),
where the length scale of the cone-jet transitional region was
comparable to the nozzle diameter. To better understand
these scaling trends, the quantitative dependence on conduc-
tivity and nozzle diameter was evaluated in Figs. 3 and 4.
FIG. 2. The minimum flow rate (Qm) at increasing viscosity (l). (a) With a
given nozzle outer diameter of 150 lm, the Qm was dependent on conductiv-
ity for ethanol and ethylene glycol with relatively low viscosities, but not de-
pendent on conductivity for glycerol with a much higher viscosity. (b) With
a given conductivity of 5 lS/cm, the Qm did not depend on the nozzle diame-
ter (D) at low viscosities but exhibited a strong dependence for highly vis-
cous glycerol.
024103-3 W. J. Scheideler and C.-H. Chen
FIG. 3. In the low-viscosity limit, the minimum flow rate (Qm) was strongly
dependent on the liquid conductivity (r) and nearly independent of the
outer diameter of the nozzle (D). The dashed line was a power law fit with
Qm  r0:5660:07 for all ethylene glycol data.
In Fig. 3, the conductivity of ethylene glycol was varied
by two orders of magnitude, and the resulting minimum flow
rate followed the scaling trend in Eq. (1). However, the
power-law dependence for ethylene glycol was notably
weaker with Qm  r0:5660:07 , consistent with the observa-
tion in Ref. 19. Interestingly, ethanol followed a similar
trend as ethylene glycol, with an arguably larger power law
coefficient. In contrast to the strong dependence on liquid
conductivity, the minimum flow rate did not show any
obvious dependence on the nozzle diameter (Fig. 3 inset).
The measurement was also insensitive to the choice of con-
ducting versus insulating nozzles. The qualitative trend of
decreasing minimum flow rate at increasing conductivity is
consistent with prior reports.4,14–16
In sharp contrast to the low-viscosity cases in Fig. 3, the
minimum flow rate of glycerol in Fig. 4 was essentially inde-
pendent of the liquid conductivity, but depended strongly on
the nozzle diameter. For glycerol with the outer diameter
ranging from 125 lm to 550 lm, the power law was extracted
as Qm  D1:4560:18 . Because of experimental limits, the noz-
zle diameter could be neither much smaller nor much larger.
For smaller nozzles with a diameter well below 100 lm, it
was extremely difficult to consistently pump a highly viscous
liquid like glycerol through the nozzle. For larger nozzles
with a diameter well over 500 lm, gravitational effects could
no longer be neglected; In addition, a larger nozzle diameter
could interfere with the constant nozzle-to-plate separation of
1.5 mm. With the limited range of nozzle diameters, it was
difficult to test if the Qm measurements correlated more
strongly with the inner or outer diameter, and the wetted di-
ameter (outer diameter here) was adopted in all data analysis
to be consistent with prior studies.20,24,25 Similar to pure glyc-
erol, the minimum flow rate of 96% glycerol exhibited a
strong dependence on nozzle diameter (Fig. 4) but nearly no
dependence on liquid conductivity (Fig. 4 inset).
The drastically different scaling regimes of the mini-
mum flow rate in Figs. 3 and 4 are directly related to differ-
ing liquid viscosities, consistent with the effects of viscosity
observed in Fig. 2. The different scaling regimes can be ten-
tatively rationalized with the following analysis on the
Appl. Phys. Lett. 104, 024103 (2014)
FIG. 4. In the high-viscosity limit, the minimum flow rate (Qm) was strongly
dependent on the nozzle diameter (D) but nearly independent of the liquid
conductivity (r). The dashed line was a power law fit with Qm  D1:4560:18
for all glycerol data except the 840 lm cases.
governing time scales. The flow rate scaling in Eq. (1) is pro-
portional to the charge relaxation time, te ¼ e=r, indicating
that te governs the electrohydrodynamic processes at low vis-
cosities. With increasing viscosity, the viscous diffusion
time which scales as tv ¼ qD2 =l may become comparable or
smaller than the charge relaxation time. When the rapid vis-
cous diffusion process dominates over the charge relaxation
process, the minimum flow rate scaling will adopt an alterna-
tive form
cD2
Qm  ; (2)
l
which can be obtained by replacing te with tv in Eq. (1). Note
that with the parametric space explored here for pure glycerol
as well as glycerol mixtures (see supplemental Table
pffiffiffiffiffiffiffiffi
ffi S149),
the Ohnesorge number defined as Oh ¼ l= qcD is consis-
tently greater than 1, which indicates that viscous effects will
dominate over inertial effects and the liquid density (q) drops
out of the scaling. The scaling law in Eq. (2) can also be
viewed as the capillary-viscous velocity ðc=lÞ multiplied by
a characteristic cross-sectional area, which scales as D2 but is
likely smaller in magnitude as in Fig. 1(b).
With the caveat of the somewhat limited parametric
range, particularly the narrow range of nozzle diameters, our
existing experimental data on highly viscous working fluids
were consistent with the capillary-viscous scaling Eq. (2).
The power law dependence on the nozzle diameter extracted
from Fig. 4 appeared to be close to the Qm  D2 scaling.
The independence on conductivity was observed for pure
glycerol as well as 96% glycerol. The scaling dependence on
viscosity was harder to test, given the difficulty in obtaining
Newtonian liquids with a viscosity higher than that of glyc-
erol. Although binary mixtures were not ideal working fluids
with potential complications such as demixing at high elec-
tric fields53,54 and preferential solvent evaporation, prelimi-
nary tests with 100%, 96%, and 90% glycerol did indicate
increasing minimum flow rate with decreasing viscosity,
albeit much weaker than the l1 power law; see
for example, the three cases with 10 lS/cm and 150 lm in
024103-4 W. J. Scheideler and C.-H. Chen Appl. Phys. Lett. 104, 024103 (2014)

Table S1.49 It should be noted that the minimum flow rate of

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