Acta Materialia 55 (2007) 3103–3109

www.elsevier.com/locate/actamat

Refining mechanism of the electric current pulse on the

solidification structure of pure aluminum
a,b a,*
Xiliang Liao , Qijie Zhai , Jun Luo a, Wenjie Chen a, Yongyong Gong a

a
School of Materials Science and Engineering, Shanghai University, 149 Yanchang Road, 200072 Shanghai, China
b
School of Mechanical Engineering, Shandong University, Jinan 250061, China

Received 25 September 2006; received in revised form 31 December 2006; accepted 4 January 2007
Available online 7 March 2007

Abstract

The refining mechanism of the electric current pulse (ECP) on the solidification structure of pure aluminum is systematically inves-
tigated by properly designed experiments. The experiment results show that the solidification structure cannot be refined by exerting an
ECP on the high temperature liquid phase, indicating that the ECP has no inoculation effect on the liquid metal. The ECP has also no
obvious influence on the solidification structure when it is applied during crystal growth, showing that the ECP cannot cause melting or
break off the growing crystal. However, the very fine macrostructure is obtained by applying an ECP during the nucleation of the melt.
The reason is that the ECP makes the crystal nuclei formed on the wall of the mould fall off and move freely in the molten metal, pro-
moting the multiplication of crystal nuclei.
 2007 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Keywords: Pure aluminum; Electric current pulse; Solidification structure; Refining mechanism

1. Introduction Sn–15 wt.% Pb hypoeutectic alloy and pointed out that

The effect of an electric current pulse (ECP) on the solid-
ification of alloys or pure metal [1–3], especially on the
grain refinement [4–10], has been confirmed by many inves-
tigations since ECP was firstly applied to the solidification
process of the Sn–15 wt.% Pb hypoeutectic alloy by Nak-
ada et al. in 1990 [11]. Although, many experiments
[12,13] and numerical simulations [14,15] of this process
have been carried out in recent years, the mechanism of
grain refinement is still not clear. Understanding of the
refining mechanism remains limited to phenomena where
solid proof from experiments is absent. Yan et al. [16]
reported that the pulse magnetic pressure caused by ECP
made the dendrites in the molten metal break and fracture,
leading to the grain refinement.
Barnak et al. [4] investigated the influence of high den-
sity current electropulsing on the microstructure of the
*
Corresponding author. Tel.: +86 21 56331218.
E-mail address: qjzhai@staff.shu.edu.cn (Q. Zhai).
the solidification structure transformed from large den-
drites to fine globular crystals by means of pulse electric
discharging with a capacitor bank. They reason that the
pinch effect resulting from the current pulse yields a shock
wave which can break off the dendrites during solidifica-
tion. However, a mechanism explaining how ECP affects
the solidification is lacking, impeding the development of
a refining technique by ECP and making it difficult to
obtain useful technology in practice. Therefore, it is funda-
mentally important to investigate the mechanism of grain
refinement by ECP. In this paper, we support the idea that
crystal rain is the main mechanism of grain refinement,
based on our systematic experiments.
2. Experimental apparatus and procedure
Fig. 1 shows our experimental apparatus which consists
of an electric current pulse generator with a capability of
1500 lF and a temperature measurement system with a
cooling-curve plotter. The pulse power provides a

1359-6454/$30.00  2007 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
doi:10.1016/j.actamat.2007.01.014
3104 X. Liao et al. / Acta Materialia 55 (2007) 3103–3109

Fig. 1. Schematic sketch of experimental setup.

frequency from 100 to 1000 Hz, and the electric voltage
ranges from 12.5 to 3000 V.
Pure Al (99.97%) was used as the starting material. It
was melted in an electric resistance furnace and heated to
1113 K. After holding at 1113 K for 30 min, the molten
metal was poured into two sand moulds at the same time.
Under the same cooling conditions, one specimen was sub-
jected to an ECP while the other was not treated. Both
specimens were u40 · 160 mm in size. A 50-mm piece test
sample was cut from the bottom of the solidified specimen
and sectioned along the center line, and then polished for
metallographic examination. The etching reagent used to
reveal the macrostructure was a mixture of 3 parts nitric
acid: 3 parts hydrofluoric acid: 9 parts hydrochloric acid:
5 parts water.
In order to clarify the refining mechanism of ECP on the
solidification structure of pure aluminum, as shown in
Fig. 2, eight ECP treatment techniques were carried out
according to the cooling curve of the specimen solidified
without ECP. The refining mechanism of the ECP was dis-
cussed based on its effect on different solidification stages.
In these experiments, the peak value of the pulse current
was 2000 A with a pulse frequency of 1000 Hz, the pouring
temperature was 1113 K and the mould was at room
temperature.
3. Results and discussion
Fig. 3 shows the typical solidification structure, i.e. the
columnar crystal, of the specimen solidified without ECP.

Fig. 2. Schematic sketch of solidification stages treated with an ECP. (a) After pouring, apply ECP until the molten metal is cooled down to 938 K. (b)
Apply ECP for a period of 10 s around the maximal nucleation rate. (c) After pouring, apply ECP to the initial stage of crystal growth. (d) After pouring,
apply ECP until nucleation is finished. (e) After nucleation, apply ECP in the first half of the time taken for crystal growth. (f) Apply ECP in the last half of
the time taken for crystal growth. (g) Apply ECP for the whole stage of crystal growth. (h) Apply ECP for the whole stage of solidification.
 X. Liao et al. / Acta Materialia 55 (2007) 3103–3109
Fig. 3. Solidification structure of specimen without ECP treatment.
The solidification structures with an applied ECP on differ-
ent solidification stages are presented in Fig. 4. For com-
parison, only the refining zone is shown in Figs. 3 and 4,
that is, the lower part showing the 50 mm samples.
3.1. Liquid phase stage at high temperature
The solidification structure shown in Fig. 4a is related to
the ECP treatment (a) of Fig. 2. It is obvious that the spec-
imen has almost the same solidification structure, that is a
coarse columnar crystal, as the specimen without ECP
treatment, showing that ECP cannot refine the solidifica-
tion structure of pure aluminum when it is applied to a high
temperature liquid metal. This indicates that ECP has no
inoculation effect on the liquid Al. Our experimental results
are different from the previous report [17] which ascribed
the grain refinement to the inoculation effect of ECP.
3.2. Nucleation stage
Fig. 4b–d correspond to ECP treatments (b), (c) and (d)
of Fig. 2. Fig. 4b shows the solidification structure when
ECP is applied for 10 s around the maximum nucleation
rate, namely the over-cooling valley. Fig. 4c shows the
solidification structure of the specimen to which ECP was
applied from the onset of solidification to the initial stage
of crystal growth. Fig. 4d shows the solidification structure
to which ECP was applied from the onset of solidification
to the end of nucleation. It is obvious that the ECP was
applied during nucleation but before crystal growth for
all three treatments. All the solidification structures are fine
globular crystals and the grain size decreases with the
increase in the ECP treatment time. This indicates that
the solidification structure of pure aluminum can be effec-
tively refined by applying ECP during nucleation. Espe-
cially, ECP is most effective on grain refinement when it
is applied around the over-cooling valley at the maximum
3105
nucleation rate. Our result agrees with the previous report
by Nakada et al. [11].
3.3. Crystal growing stage
Fig. 4e–g relate to the ECP treatments (e), (f) and (g) of
Fig. 2. Fig. 4e shows the solidification structure of the spec-
imen to which ECP was applied in the first half period of
crystal growth after nucleation. Fig. 4f shows the solidifica-
tion structure to which ECP was applied in the latter half
period of crystal growth. Fig. 4g shows the solidification
structure to which ECP was applied during the whole stage
of crystal growth. Their solidification structures remain
mainly columnar crystals. However, compared with the
specimen without ECP, the solidification structures are
slightly refined and have a certain amount of coarse glob-
ular crystals. According to previous reports [11,18,19],
ECP treatment could cause break off, fracture or burn
out to the growing crystal. However, comparing Fig. 4b–
d with Fig. 4e–g, ECP treatment during crystal growth is
not crucial despite having some influence on crystal
growth.
Based on the above experiments, grain refinement by
ECP is mainly achieved during nucleation but not at the
stage of crystal growth or in the high temperature liquid
phase. Fig. 4h shows the extremely fine globular grain pro-
duced by applying ECP during the whole period of solidifi-
cation. Compared with Fig. 4c, the refined macrostructures
are almost identical, which confirms that the grain refine-
ment effect of ECP mainly occurs during nucleation.
3.4. Nucleus multiplication by ECP
The large number of crystal nuclei created by ECP is the
most important reason for the grain refinement of pure alu-
minum. In order to clarify the refinement mechanism of
ECP, it is essential to explain the origin of these crystal
nuclei.
When ECP penetrates the liquid metal, a pulse magnetic
field is induced, which distributes in a gradient over the cyl-
inder specimen. Consequently, the pulse magnetic field,
which is stronger at the wall and weaker in the center,
yields a gradient pressure.
When the melt starts solidifying, the nucleus originates
first on the wall of the mould. As mentioned above, the
pulse magnetic field is induced by the ECP. The pulse mag-
netic pressure originating from the pulse magnetic field has
an oscillatory surge on the molten metal, which results in a
large amount of convection in the liquid metal and an
intensive strike on the mould wall. During nucleation, the
nuclei created on the mould wall are broken off and fall
into the melt under the pulse electromagnetic force. There-
fore, a solidification shell cannot be formed on the mould
wall. The large number of nuclei in the melt leads to crystal
rain. In other words, the nuclei will be dissociated from the
mould wall by the pulse magnetic pressure if a solidifica-
tion shell has not been formed on the mould wall. Once a
3106 X. Liao et al. / Acta Materialia 55 (2007) 3103–3109

Fig. 4. Solidification structures with an applied ECP at different solidification stages. (a) After pouring, apply ECP until the molten metal is cooled down
to 938 K. (b) Apply ECP for a period of 10 s around the maximal nucleation rate. (c) After pouring, apply ECP to the initial stage of crystal growth. (d)
After pouring, apply ECP until the nucleation is finished. (e) After nucleation, apply ECP for the first half of the time taken for crystal growth. (f) Apply
ECP for the last half of the time taken for crystal growth. (g) Apply ECP for the whole stage of crystal growth. (h) Apply ECP for the whole stage of
solidification.
 X. Liao et al. / Acta Materialia 55 (2007) 3103–3109
solidification shell is formed on the mould wall, the solidi-
fication structure can no longer refined by the ECP because
no new crystal nuclei can be dissociated from the mould
wall. This is the reason why the solidification structure
can be refined when ECP is applied during nucleation
and why ECP has almost no effect on the solidification
structure when it is applied after nucleation. In order to
confirm this grain refinement mechanism of ECP, two ser-
ies of experiments were carried out. One was to certify that
the crystal nucleus originates from the mould wall and the
other was to test that the nucleation rate increases by
retarding the formation of the solidification shell.
As shown in Fig. 5, three experiments were designed to
certify that the crystal nucleus originated from the mould
wall. The wire netting was put into each specimen to pro-
tect the nucleus outside the netting from entering the net-
ting. For these three experiments, the pouring condition
was the same and an ECP with the same parameters was
applied, that is, an ECP was applied during the whole
solidification, the peak value of the pulse current was
2000 A with a pulse frequency of 1000 Hz, the pouring
temperature was 1113 K and the mould was at room tem-
perature. For each experiment, the molten metal was simul-
taneously poured into two sand moulds with the same
cylindrical wire netting, but only one of the specimens
was treated with an ECP. For experiment (a), in order to
avoid the nucleus entering the netting from the top and
side, the wire netting was as high as the specimen and the
top of the netting was sealed. For experiment (b), the
height of the netting was the same as the specimen, but
the netting had an open top. Therefore, the nucleus could
enter the netting from the top, but could not enter from
Fig. 5. Experiment to certify that the nuclei dissociate from the mould wall. (a) Net with a closed top: left, untreated; right, treated. (b) Net with an open
top: left, untreated; right, treated. (c) Half-height net with a closed top: left, untreated; right, treated.
3107
the side. For experiment (c), the height of the netting was
only half of that of the specimen and the top was sealed
to protect the crystal nucleus from entering the netting
from the top and side.
Fig. 5a shows that the solidified metal inside the netting
has a similar solidification structure, i.e. coarse columnar
crystal. However, the solidification structure outside the
netting is different. The untreated specimen is mainly made
up of coarse columnar crystals, but the treated specimen it
is mainly fine globular crystals. This indicates that the crys-
tal nuclei fall off from the mould wall and enter the molten
metal continuously via a shock wave resulting from the
pulse magnetic pressure during solidification. The metal
inside the netting solidifies into coarse columnar crystal
because it can only nucleate and grow by itself, indicating
that the ECP cannot promote nucleation of the molten
metal inside the netting and the dendrites cannot be frac-
tured by the pulse magnetic pressure or burnt out by Joule
heating. As shown in Fig. 5a and b, the experimental result
is almost the same and the crystal nucleus dissociating from
the mould wall cannot enter the netting from the top.
Fig. 5c shows, for the untreated specimen, that the macro-
structures both inside and outside the netting are mainly
coarse columnar crystals. However, for the specimen trea-
ted with ECP, fine globular crystals constitute the solidifi-
cation structure outside the netting, especially at the top
of the netting. This indicates that crystal nuclei fall off
the mould wall continuously under the action of ECP,
but they cannot enter the netting because the top of the net-
ting is sealed.
Thus, we confirm that treatment (a) of Fig. 2, namely
applying ECP to the high temperature liquid metal, cannot
3108 X. Liao et al. / Acta Materialia 55 (2007) 3103–3109

be used to refine the solidification structure because the

molten metal does not reach the nucleation temperature
and no crystal nuclei can be formed on the mould wall.
Fig. 6 shows the macrostructure of the longitudinal section
of the specimen after the following treatment: ECP was
applied during the whole solidification, the peak value of
the pulse current was 2000 A with a pulse frequency of
1000 Hz, the pouring temperature was 1113 K and the
mould was at room temperature. Based on the analysis
of the crystalline region of the whole specimen, the bound-
ary between the equiaxed crystal and the columnar crystal
on the upper part of the sample looks like the letter V (the
white line in Fig. 6). Comparing with the macrostructure of
the specimen without ECP, as shown in Fig. 7, we can
explain how the boundary forms in this shape as follows.
First, the pulse magnetic force causes the nuclei to break
off from the mould wall. Then they move towards the cen-
ter and bottom of the mould via the pulse magnetic force
and gravity. However, where the nuclei can move to is
determined by their original positions and the time that Fig. 7. Macrostructure of the specimen without ECP.
they break off from the mould wall. The nearer to the
top and the earlier the nuclei break off from the mould tures: room temperature, 373 K and 673 K. The same ECP
wall, the deeper and nearer to the center of the mould they parameters and pouring temperature were used for these
reach. Instead, the nuclei that form on the lower part of the experiments. The peak value of the pulse current was
lateral wall and those breaking off the mould wall after- 2000 A with a pulse frequency of 200 Hz. The pouring tem-
wards will stay close to the place where they formed. perature was 1113 K and the ECP was applied during the
Finally, the ‘‘V’’ shaped boundary is formed because of entirety of solidification. The experiment results are pre-
the complex transverse and lengthways movement of the sented in Fig. 8. Fig. 8a shows that when the mould is at
nuclei (further investigation of this ‘‘V’’ shaped boundary room temperature, the solidification structures are fine
continues and a detailed analysis will be published equiaxed crystals at the bottom, columnar crystals in the
elsewhere). center of the sample growing along the radial direction
For the experiment to certify that the nucleation rate is and equiaxed crystals at the side of the sample, respec-
increased by retarding the formation of the solidification
shell, the formation of the solidification shell must be con-
trolled by preheating the sand mould to different tempera-

Fig. 8. Effect of the preheated temperature of the mould on the

solidification structure treated with an ECP. (a) Room temperature, (b)
Fig. 6. Boundary between the equiaxed and columnar crystals. 373 K and (c) 673 K.
 X. Liao et al. / Acta Materialia 55 (2007) 3103–3109
tively. Fig. 8b shows the solidification structure at a mould
temperature of 373 K. Fine and coarse equiaxed crystals
are formed at the bottom and in the middle of the sample,
respectively. Fig. 8c shows the solidification structure with
the mould preheated to 673 K, in which the region of the
fine equiaxed crystal increases significantly. This experi-
ment indicates clearly that the formation of the solidifica-
tion shell is delayed by preheating the mould, leading to
an increase in the time to nucleate on the mould wall.
The nucleation rate increases dramatically because more
nuclei are dissociated from the mould wall owing to the
expansion in the time of ECP treatment. It is obvious that
the crystal nuclei dissociate from the mould wall continu-
ously by ECP before the solidification shell is formed on
the mould wall. Once the solidification shell forms on the
mould wall, nucleation is finished and the ECP treatment
cannot refine the solidification structure any more. This is
also solid proof for the experiment results shown in Figs.
4 and 5.
3.5. Influence of the skin effect of ECP on the solidification
structure
ECP is not distributed homogeneously over the cross-
section of the specimen when it penetrates the liquid metal,
which leads to the skin effect. A gradient distribution is pre-
sented for ECP and the current density at the surface is lar-
ger than that in the interior. The skin depth on which the
current density is mainly focused is described in Ref. [4]:
1
d ¼ ðprlf Þ2
where l is the permeability of the molten metal which
approximates to the vacuum permeability, f is the wave fre-
quency of ECP, and r is the electric conductivity of the li-
quid metal.
According to the given parameters of our experiment,
the calculated skin depth based on the above equation is
about 3.5 mm. The maximum current density is mainly
concentrated in the skin depth of the surface of the speci-
men. The skin effect results in two kinds of effects of
ECP on the solidification structure. On one hand, the mag-
netic pressure induced by the ECP has a maximum value
near the mould wall and a shock wave also focuses around
the mould wall, causing the nucleus to fall off and drift into
the liquid metal. This significantly promotes the multiplica-
tion of nuclei, indicating that the skin effect of ECP
enhances the formation of crystal rain. On the other hand,
after a shell layer solidifies on the mould wall, the current
prefers to penetrate it first because the electrical resistivity
of the liquid is greater than that of the solid. In addition,
the current density in front of the solid–liquid interface is
very small owing to the skin effect. Therefore, the magnetic
pressure or shock wave originating from ECP cannot break
off or fracture the columnar crystals of pure aluminum dur-
ing solidification and the solidification structure cannot be
3109
refined. Thus, the solidification structure shown in Fig. 4f
which is related to the ECP treatment (f) of Fig. 2 is a
columnar crystal. For the same reason, all the solidification
structures inside the netting, as shown in Fig. 5, are colum-
nar crystals too.
4. Conclusions
(1) The solidification structure cannot be refined when
ECP is applied to the high temperature liquid metal
or during crystal growth, indicating that ECP has
no inoculation effect on the high temperature melt
and the growing crystal cannot be burnt out, broken
off or fractured by the ECP treatment. The solidifica-
tion structure of pure aluminum can only be dramat-
ically refined by applying ECP during nucleation.
(2) The grain refinement mechanism of ECP occurs when
ECP makes the crystal nucleus on the mould wall fall
off and drift in the liquid, leading to a multiplication
of the crystal nuclei and grain refinement. The skin
effect of ECP particularly enhances this effect.
Acknowledgements
The authors gratefully acknowledge financial support
from the Pre-research Foundation of the National Basic
Research Program (973 Program, Grant No. 2004
CCA07000), the Science and Technology Committee of
Shanghai Municipality (Grant No. 04XD14008) and the
National Natural Science Foundation of China
(50274050, 50374046).
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