NanoShuchred

Pergamon

Materials, Vol. 5, Nos. l/8, pp. 793-799.1995

Ekvier Science Ltd
Copyright Q 1995 Acta Metallurgica Inc.
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INVESTIGATION
OF NANOMETER POWDERS PRODUCED
AN ELECTROHYDRODYNAMIC
TECHNIQUE
X.F. Yu*, Z.Q. Hu*, X.

BY

Liu**and Z. Jiang

*State Key Lab of RSA, Institute of Metal Research, Academia Sinica,

Shenyang 110015, Peoples Republic of China
**Northeastern University, Shenyang, llOOOf5,Peoples Republic of China
(Accepted August 1995)
Abstract-Sn-Binanometerpowders
wereproduced by an electrohydrodynamic technique.
The effects of processing variables on the size of Sn-Bi nanometer powders were studied.
Experimental results indicate that with an increase in high voltage and a decrease in diameter of
the capillary nozzle, the size of Sn-Bi nanometer powders decreases. In addition, thefeedpressure
for delivering the molten alloy to the tip of the capillary nozzle is also an important factor in
controlling the size of the nanometer powders.

INTRODUCTION

The electrohydrodynamic (EHD) technique requires an intense electric field to generate

charged liquid droplets from the liquid state, and these droplets are accelerated by the same electric
field to a collector. The use of the EHD technique to produce nanometer-sized particles was
introduced by Perel et al. in 1977 (1,2,3). In recent years, we have also studied EHD processing
of nanoscale powders: sub-micron Sn-Bi-Pb powders were produced.
In this study, we report on the use of a fine quartz capillary tube (CO.1 mm dia) to synthesize
nauosized powders of Sn-Bi alloy.

EXPERIMENTAL

The experimental apparatus employed to produce nanometer powders is shown schematically in Figure 1. Specific experimental parameters are shown in Table 1. The diameter of the
quartz crucible tube is 9.2 - 9.5 mm. One end of this tube is drawn into a capillary. The cathode
and anode are made of stainless steel.
793

794

XF

Yu,ZQ Hu, X LIUANDZ JIANG

TABLE 1
Experimental Parameters
Diameter of the capillary nozzle
Length of the capillary nozzle
Height of the cathode tube
Diameter of the cathode tube
External diameter of the circular anode
Internal diameter of the circular anode
Vacuum in the chamber
Distance between cathode and anode

co.1
10
15
4.2
5
3
10-5
4

:Z;
:ZZ;
:Z;
(Ton.)
(m@

A master ahoy of Sn-60 Wt.% Bi eutectic was prepared by vacuum melting. Small pieces
were placed in a quartz jet tube, sealed up, and placed in the heater. When the vacuum in the
chamber reached 10e5torr, the Sn-Bi alloy was heated to 35OC,andthe molten alloy was delivered
to the tip of the capillary nozzle to which a high voltage was applied. Charged liquid droplets were
formed, which were scattered and accelerated by the electric field onto a collector. The droplets
solidified in flight to produce the nanometer powders.
Powders were observed under a transmission electron microscope, Phillips EM-420. Size
distribution of the nanometer powders was analyzed by an image analyzer.

1. seal plate
2. baseplate shield
3. collector
4. anode
5. stainless steel shell
6. droplet source
7. high voltage wire
8. procelain insulator
9. heat shield
10. emitter
11. high voltage source
12. shield
13. droplet beam
14. sealing ring
15. gas pressure source
16. vacuum set
17. heat power source
Figure 1. Schematic of experimental EHD apparatus.

795

NANOMETER
Powoms PFKWCED BY ELECTROHYDROD~NAMIC
TECHNICWE

30I25
g
w. 20
._
VI
.g I5
=o
e
LZ
8 10
5
0
O
High voltage, kV

10

15

20

High voltage, kV

Figure 2. Relationship between the emitting

frequency of liquid droplets and the high
voltage applied.

Figure 3. Effect of high voltage on the mean

size of the nanometer powders.

EXPERIMENTAL RESULTS AND DISCUSSION

Effects of High Voltage on the Emitting Frequency of Liquid Droplets and the Mean Size of the
Nanometer Powders

Figures 2 and 3 show, under the experimental conditions of Table 1, the relationships
between the emitting frequency of liquid droplets, the mean size of the nanometer powders ,and
the high voltage, respectively. From these results it can be seen that with an increase of the high
voltage, the emitting frequency of liquid droplets increases and the mean size of the nanometer
powders decreases. The relationship between the mean size of the nanometer powders and the high
voltage is given by (4)
6&cGV
r = E(#J-JI -I-2v@J77$7
where, r is the minimum mean size of the nanometer powders: v the surface tension of the liquid
droplet; so the permittivity of free space; p the coefficient related to field strength: G the volumetric
flow rate; V the high voltage; and I the EHD source current.

XF Yu,

796

\a

2m -0.06
$- -0.0s
M
5 -0.10
8
t&
-0.12

ZQ Hu, X LIUANDZ JIANG

3= -0.06

0.2

0.1

(1.3

-0.12 0

Diameter of the capillary nozzle, mm

Figure 4. Relationship between feed pressure
and diameter of the capillary nozzle.

2
4
6
8
10
Length of the capillary nozzle, mm

Figure 5. Relationship between feed pressure

and length of the capillary nozzle.

Effects of Diameter and Length of the Capillary Nozzle on the Feed Pressure for Delivering a
Molten Alloy to the Tip of the Capillary Nozzle

Figures 4 and 5 show the relationships between the feed pressure and the diameter and length
of the capillary nozzle, respectively. It canbe seen that the feed pressure decreases with an increase
in the diameter of the capillary nozzle and a decrease in the length of the capillary nozzle. For a
quartz jet tube with fixed capillary nozzle diameter and length, an appropriate feed pressure is
necessary for emitting stable liquid droplets.
30

._
CA
S
._
Ti
kil
= IO
3
z
g201
0

0
0
-J
0.3
0
0.1
0.2
Diameter of the capillary nozzle, mm

Figure 6. Relationship between mean size of the nanometer

powders and diameter of the capillary nozzle.

NANOMETER
POWDERSPRODUCED
BYELECTFIOHYDROCWNAMIC
TECHNIQUE

797

Effect of Diameter of the Capillary Nozzle on the Mean Size of the Nanometer Powders

The relationship between the mean size of the nanometer powders and the diameter of the
capillary nozzle is shown in Figure 6. The mean size of the nanometer powders increases as the
diameter of the capillary nozzle increases. The size of the liquid cone produced in the capillary
nozzle is determined by the diameter of the capillary nozzle, which affects field strength at the
liquid cone tip and the size of the scattered liquid droplets. With decreasing diameter of the
capillary nozzle, the size of the liquid cone in the capillary nozzle decreases, and the effect of the
high voltage electric field on the scattered liquid droplets increases, so the mean size of the
nanometer powders decreases.
Effect of Feed Pressure on the Mean Size of the Nanometer Powders

There are three kinds of resistance when a liquid-alloy flows through the capillary nozzle and
begins to form a jet.
(i) The pressure drop for a flow in the capillary, Pi. Generally speaking, laminar flow occurs
when the viscous liquid flows through the capillary. It is assumed that the flow of a molten alloy
in a capillary is a stable laminar flow. According to the Darcy-Weisbach equation, the pressure
drop Pl is given by (5)

where f is the friction factor: D the diameter of the capillary: L the length of the capillary: V,, the
average-velocity across the section; and p the mass density of the molten alloy.
(ii) Additional pressure, P2, produced by surface tension of the liquid cone formed at the tip
end of the quartz capillary.
p = 2ocose
2-

where cr is the surface tension of the liquid cone, r the surface curvature radius of the liquid cone,
and 0 the contact angle of the molten alloy and material of the jet nozzle.
(iii) Gas pressure, P3, out of the quartz capillary in the working chamber. In addition, the
static pressure of a molten alloy, P,, affects the molten alloy itself

where p is the mass density of the molten alloy, g the acceleration of gravity,and H the height from
the upper surface between the molten alloy to the lower end of the jet nozzle.
Only when the combined forces of the feed pressure, P, and the static pressure, Pg, are
slightly larger than the total resistance, that is

XFYu,ZQ Hu,X LtuAND Z JIANG

798

Figure 7. TEM microgmph of Sn-Bi nanometer powders.

%
14

12
10
8

6
4
2
0

1.0

1.5 2.0 2.5

3.0
Powders size, nm

3.5

Figure 8. Particle size distribution of Sn-Bi nanometer powders shown in Figure 7.

will the molten alloy begin to form a jet. The feed pressure is the important condition for achieving
a continuous and stable jet. The control for the feed pressure value and its stable state directly
affects the mean size and distribution of the nanometer powders. If the feed pressure value is
unstable, the mean size of the nanometer powders is not uniform. Its specific value must be
determined by experiments.

NAN-R

POWOERS
PRODUCED
BYELE~TR~RODWMC TECHNIQUE

799

Morphology and Size Distribution of the Nanometer Powders

A TEM photomicrogmph of the Sn-Bi nanometer powders is shown in Figure 7, and the
corresponding image analysis in Figure 8. Most of the nanoparticles are < 3 nm in size.
CONCLUSIONS
Sn-Bi nanometer powders can be produced by the elecbohydrodynamic technique. Critical
variables in the powder synthesis are high voltage, shape and size of the cathode and anode,
diameter and length of the quartz capillary nozzle, and the feed pressure.
REFERENCES
1.

J. Perel, J.F. Mahoney, B.E. Kalensher, K.E. Vickers, and R. Mehrabian, Rapid Solidification
Principles and Technologies, eds. R. Mehrabian, B.H. Kear, and M. Cohen, Claitor
Publishing Division, Baton Rouge, LA, p. 258 (1978).
J. Perel, J.F. Mahoney, B.E. Kalensher, and R. Mehrabian, Twenty-fifth Sagamore Army Materials
Conference on: Recent Advances in Metal Processing, Bolton Landiig, New York, p. 79 (1978).
J. Perel, J.F. Mahoney, P. Duwez, and B.E. Kalensher,RapidSolidification
Processing: Principles
and Technologies 2, eds. R. Mehrabian, B.H. Kear, and M. Cohen, Claitor Publishing Division,
Baton Rouge, LA, p. 287 (1980).
H.S. Hu, X. Liu, L. Zou, L.Z. Cheng, G.L. Jia, G.Z. Zhaug , X.Q. Dong , and Z.Q. Hu, 94 Autumn
Materials Investigation and Discussion Conference of the Peoples Republic of China, p. 1475
(1994) (in Chinese).
J.J. Bertin, Engineering Fluid Mechanics, Prentice-Hall, Inc., Englewood Cliffs, New Jersey, p.
224 (1984).
Processing:

2.
3.

4.

5.