metals

Article
Experimental Investigation of Solidification in the
Cast Mold with a Consumable Cooler
Introduced Inside
Ran Niu 1 , Baokuan Li 1, *, Zhongqiu Liu 1 , Lifu Bu 1 , Xianglong Li 1 , Xiao Yang 2 and
Fumitaka Tsukihashi 2
1 School of Metallurgy, Northeastern University, Shenyang 110819, China; [email protected] (R.N.);
[email protected] (Z.L.); [email protected] (L.B.); [email protected] (X.L.)
2 Graduate School of Frontier Science, The University of Tokyo, Kashiwanoha 5-1-5, Kashiwa 2778561, Japan;
[email protected] (X.Y.); [email protected] (F.T.)
* Correspondence: [email protected]; Tel.: +86-24-83672216




Received: 6 December 2018; Accepted: 7 January 2019; Published: 9 January 2019


Abstract: The microstructure is of great significance for the stability and mechanical performance
of the cast slab. Recently, an innovative technology of feeding a consumable cooler into the mold
has been proposed to improve the internal quality of castings. But the mechanism is not clear. In the
present work, a water-cooled transparent laboratory equipment was set up and solidification of
NH4 Cl-70%H2 O solution was studied to observe the in-situ growth and sedimentation of crystals.
The experiments were conducted with and without adding a consumable cooler. Morphology
variation of the solidification structure was visualized and temperature distribution during the
process was recorded. Results show that introduction of the consumable cooler significantly reduces
the temperature of the central zone. Melting of the consumable cooler can supply a large quantity of
equiaxed crystals, which prevent the growth of columnar dendrites and thereby promote columnar
to equiaxed transition (CET). Moreover, the enhanced convection shows an effect of grain refinement.

Keywords: NH4 Cl-H2 O solution; solidification; crystallization; dendrite growth; CET

1. Introduction
Quality and reliability of the castings are heavily dependent on the crystal structure and their
homogeneity. Internal central segregation and porosity are common defects in the continuous casting
(CC) slab and these defects affect the internal quality of the final rolled plate. Reducing the defects is
essential for achieving satisfactory properties in the products [1]. Many methods including the low
superheat pouring technique [2], the Electromagnetic Stirring (EMS) [3] and the ultrasonic vibration [4]
have been implemented to reduce the defects. All these methods tend to improve the homogeneity
and the amount of equiaxed crystals in the cast slab [5]. Nevertheless, the efficiency of these techniques
is limited by different reasons, such as submerged entry nozzle (SEN) clogging, the size and shape of
the slab [6], etc. Generally, the slab quality can be improved by generating a large amount of equiaxed
grains and promoting a columnar to equiaxed transition (CET). Recently, an innovative method of
feeding a consumable steel strip to the mold has been proposed by the Azovstal’ Metallurgical Combine
in Ukraine and the Kawasaki Steel Corporation in Japan, which can alleviate the central segregation
and porosity defects of CC slab [7–10]. For the new technology, a thin consumable strip is continuously
fed into the CC mold through a strip “feeder” at a desired feeding speed. The melt superheat in the
central zone of the mold is decreased by the phase change decalescence of the cold strip. Melting of
the cold strip can promote the formation of equiaxed grains while hindering the growth of columnar
dendrites. A new pattern of solidification proceeding simultaneously at the outside and inside of

Metals 2019, 9, 55; doi:10.3390/met9010055 www.mdpi.com/journal/metals

Metals 2019, 9, 55 2 of 11

the slab eliminates the centerline segregation and improves the internal consistency. However, the
mechanism underlying the improvement of internal defects by this technology is not clear because of
the opaque mold as well as the harsh casting environment.
In 1965, Jackson tested several transparent compounds showing a similar pattern to metals
during solidification [11]. From then on, NH4 Cl-H2 O solution has been widely adopted for
experimental studies of the fluid motions associated with crystallization and solidification processes.
Christenson et al. [12] studied the solidification of NH4 Cl-H2 O solution in a rectangular cavity with
varying initial concentrations and cooling conditions. Tatsuo et al. [13] studied the detailed information
of double-diffusive convection during solidification by performing the experiment of solidification
of NH4 Cl-H2 O solution in a rectangular chamber with lateral cooling. Beckermann and Wang [14]
experimentally studied the flow field during equiaxed dendritic solidification of NH4 Cl-H2 O solution.
Shigeo et al. [15] used a potassium permanganate dye to trace fluid motion within the sidewall mushy
region during a two sides chilling solidification. Kharicha et al. [16] used the PIV technique to study
the flow pattern and the equiaxed crystal motion during an equiaxed/columnar solidification process.
Zhong et al. [17] investigated the effect of crystal rain produced from the free surface on columnar to
equiaxed transition. Nevertheless, investigation of the solidification process with a consumable cooler
is still absent.
In the present work, solidification process of NH4 Cl-H2 O solution in a cavity cooled from two
sidewalls was experimentally investigated. The columnar dendrites growth from two cooling sidewalls
and the equiaxed crystals motion were studied. The influences of the crystals generated from the solid
consumable cooler on the solid structure and the occurrence of the CET were investigated. Related
mechanisms are herein discussed.

2. Experimental Procedure
A solution of NH4 Cl-70%H2 O was used in the transparent experimental study of solidification
and crystallization. The thermophysical properties of NH4 Cl-70%H2 O solution is shown in Table 1.
The experiments were performed in a cavity made of acrylic with two 1-mm-thick cooper plates as two
side vertical walls. Two cooling water tanks were set immediately adjacent to the two side walls. Three
thermocouples with diameter 5 mm were positioned in the Y-Z median plane of the cavity at positions
2.5 mm (T3), 12.5 mm (T2) and 22.5 mm (T1) relative to the left cooling plate and were directly in
contact with the NH4 Cl-H2 O solution. The schematic diagram of the experiment set up is shown in
Figure 1. During the solidification process, the two sidewalls of the cavity were rendered towards
cooling by pumping the cold water into the tank at a given rate. The cooling water was supplied by a
thermostat water bath with a mixture of ice and water. The top, front, back and bottom walls of the
cavity were well insulated, leaving a slit for the light sheet and cooler adding in the top plate. A double
cavity Nd-YAG laser was used as the light source. A camera monitoring system was also set up to
visualize the crystallization process from the front plate. The output data of the thermocouples were
displayed on a computer. The schematic diagram of the experimental system is shown in Figure 2.

Table 1. Thermophysical properties data for NH4 Cl-70% H2 O [14].

Property Value
(kg/m3 )
Density of the liquid phase, ρf 1078
Density of the solid ammonium chloride, ρs (kg/m3 ) 1527.4
Dynamic viscosity of the liquid phase, µf (N s/m2 ) 0.0013
Thermal conductivity of the liquid phase, kf (W/m K) 0.468
Thermal conductivity of the solid phase, kfs (W/m K) 2.7
Specific heat of the liquid phase, cf (J/kg K) 3249
Specific heat of the solid phase, cs (J/kg K) 1827
Thermal expansion coefficient, βT (1/K) 3.832 × 10−4
Latent heat of fusion at TE , ∆h (J/kg) 3.138 × 105
Eutectic temperature, TE (K) 259.2
Liquidus temperature, TL (K) 310.2
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Eutectic temperature, TE (K) 259.2

Eutectic temperature, TE (K) 259.2
Metals 2019, 9, 55 Liquidus temperature, TL (K) 310.2 3 of 11
Liquidus temperature, TL (K) 310.2

Figure 1. The schematic diagram of the experiment set up.

Figure 1. The
Figure 1. The schematic
schematic diagram
diagram of
of the
the experiment
experiment set
set up.
up.

Theschematic
Figure2.2.The
Figure schematicdiagram
diagramof
ofthe
theexperimental
experimentalsystem.
system.
Figure 2. The schematic diagram of the experimental system.
Detailsabout
Details aboutthe theexperimental
experimental procedure
procedure are
are as
as follows.
follows. TheThe solution
solution of of NH
NH44Cl-H
Cl-H22OOwas washeated
heated
to85 Details
85°C.◦ C.After about
Aftercomplete the experimental
completemelting,
melting,the procedure
thesolution
solutionwas are as
waspoured follows.
pouredinto The solution
intoaacavity of
cavitypreheated NH
preheated to 4Cl-H2O
to 85 ◦ was
85 °CCto heated
tomake
make
to aa
to
70 85 °C.
mm-deep After complete
bath. Later, melting,
cooling the
water solution
was was
pumped poured
to the into
tanks atocavity
triggerpreheated
the to 85
solidification.°C to
At make
every a
70 mm-deep bath. Later, cooling water was pumped to the tanks to trigger the solidification. At every
70 mm-deep
100 ss interval, bath. Later, cooling water was pumped to the tanks to trigger the solidification. At every
100 interval,thethe insulation
insulationof the
of front
the plate
front was
plateremoved to photograph
was removed the progressthe
to photograph of solidification.
progress of
100 s interval,
Solidification with the insulation
a consumable of the front plate was removed to photograph the progress of
solidification. Solidification with cooler was also investigated.
a consumable cooler was also By the time the solidification
investigated. By the time started,
the
solidification.
a laboratory consumable Solidification with a consumable
cooler wasconsumable
immersed into cooler
the was was
solution also investigated.
bath center withsolutionBy the
an immersed time the
length
solidification started, a laboratory cooler immersed into the bath center
solidification
of 30 mm. The started,
consumable a laboratory
cooler wasconsumable
prepared bycooler
cooling wastheimmersed
NH Cl-H into
O the solution
solution in a bath center
cuboid shape
with an immersed length of 30 mm. The consumable cooler was prepared 4 2 by cooling the NH4Cl-H 2O
with
mold an
in immersed
a freezer. length
Three of 30
coolers mm.
with The consumable
different sizes cooler
(cross was
section:prepared
3 × 10 by
mm cooling
2 , 5 × 10themmNH2 4Cl-H2O
and 7 ×
solution in a cuboid shape mold in a freezer. Three coolers with different sizes (cross section: 3 × 10
solution
10 mm in a cuboid
2 ) were prepared shapeto mold in a freezer.
investigate the Threeof
influence coolers
cooling with different
efficiency on sizes
the (cross section:
solidification 3 × 10
process.
mm ,2 5 × 10 mm 2and 7 × 10 mm )2 were prepared to investigate the influence of cooling efficiency on
2 2 2
mmtemperature
The , 5 × 10 mm and 7 × 10experiments mm ) were prepared to investigate the from
influenceobservation
of cooling efficiency on
the solidification measuring
process. The temperature were conducted
measuring separately
experiments were theconducted separately experiments
from
theensure
to solidification
that there process.
was noThe temperature
interference withmeasuring
the morphologyexperiments were conducted
of the solidification separately from
front.
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the observation experiments to ensure that there was no interference with the morphology of the
solidification front.
Metals 2019, 9, 55 4 of 11

3. Results and Discussion

3. Results and Discussion
3.1. Dendrite Growth during Solidification
3.1. Dendrite Growth during
The solidification Solidification
morphology in the cavity at selected moments is shown in Figure 3. In the
initial stage, after cooling for 300
The solidification morphology in the s, in Figure
cavity3a,at the frozenmoments
selected thicknessisgrown
shownfrom the mold
in Figure 3. Inwalls, and
the initial
the bottom corner towards the inside can be seen. The frozen area was
stage, after cooling for 300 s, in Figure 3a, the frozen thickness grown from the mold walls, and the made up with columnar
dendrites
bottom which
corner werethe
towards notinside
completely perpendicular
can be seen. The frozen to area thewascooling
made up plate
withbut insteaddendrites
columnar inclined
which were not completely perpendicular to the cooling plate but instead inclined upwardlyphase.
upwardly at an angle, indicating an upward liquid flow in the columnar front in the liquid at an
With the
angle, proceeding
indicating of solidification,
an upward liquid flowa infewthesmall equiaxed
columnar frontgrains
in theappeared (see With
liquid phase. Figure the3b). This can
proceeding
be solidification,
of understood asathe fewNH 4Cl crystals
small equiaxed “breaking off” at the(see
grains appeared dendritic
Figuremushy region,
3b). This can which had little
be understood
as the NH4 Cl crystals “breaking off” at the dendritic mushy region, which had little effectcrystals
effect on the growth of columnar dendrites. In the third stage, numerous larger equiaxed on the
presented
growth in the lower
of columnar part of the
dendrites. cavity,
In the thirdwhich
stage, indicated
numerousthe occurrence
larger equiaxedofcrystals
crystal presented
rain (see Figure
in the
3c). Some of these equiaxed grains were generated from the initial cooling
lower part of the cavity, which indicated the occurrence of crystal rain (see Figure 3c). Some of these wall and driven to the
central zone by thermal convection. Others were generated from the columnar
equiaxed grains were generated from the initial cooling wall and driven to the central zone by thermal dendrite fragments
[18] and transported
convection. Others were by the fluid flow
generated fromor the
carried downdendrite
columnar by gravity. The equiaxed
fragments [18] and crystals settledby
transported at
the bottom of the cavity or were captured by the columnar dendrites in the
the fluid flow or carried down by gravity. The equiaxed crystals settled at the bottom of the cavity lower part of the cavity.
In were
or the following
captured stage
by theofcolumnar
solidification, as shown
dendrites in the in Figure
lower part3d, the cavity.
of the equiaxed crystals
In the followingahead of the
stage of
columnar front continued to grow towards the melt. The CET occurred
solidification, as shown in Figure 3d, the equiaxed crystals ahead of the columnar front continued when the equiaxed crystals
sediment
to bed grew
grow towards thetomelt.
the height
The CET corresponding
occurred when to thethe
location.
equiaxed Solidification ended after
crystals sediment bed 1400
grews to
when
the
the frozen
height area covered
corresponding to about 60% of Solidification
the location. the domain (including
ended after the1400
mushy zone).
s when theThe V shape’s
frozen frozen
area covered
thickness
about 60%consisted
of the domain of both the columnar
(including the mushydendrites
zone).grown
The V fromshape’sthefrozen
two cooling
thickness plates and the
consisted of
equiaxed crystals aggregated in the bottom regions. The liquid in the center
both the columnar dendrites grown from the two cooling plates and the equiaxed crystals aggregated region was mostly water.
The
in theschematic diagram
bottom regions. Theof liquid
the development
in the centerofregion
various wasmicroscopic
mostly water. structural zones indiagram
The schematic a cast mold
of theis
shown in Figure 4.
development of various microscopic structural zones in a cast mold is shown in Figure 4.

Figure 3. Solidification morphology in the melt at selected times.

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Metals 2019, 9, 55 5 of 11
Figure 3.
Figure 3. Solidification
Solidification morphology
morphology in
in the
the melt
melt at
at selected
selected times.
times.

Figure4.
Figure 4. The
The schematic
schematic diagram
diagram of
of the
the development
development of of various
various microscopic
microscopicstructural
structuralzones
structural zonesin
zones inaacast
cast
mold(a)
mold (a)initial
initialstage;
stage; (b)
(b) mediate
mediate stage;
stage; (c)
(c) final
final stage.
stage.
stage; (b) mediate stage; (c) final stage.

Toinvestigate
To
To investigatethe
investigate themotion
the motionof
motion ofthe
of thefree
the freecrystals,
free crystals,which
crystals, whichfurther
which furtherpromote
further promotethe
promote theCET,
the CET,an
CET, anisolated
an isolatedNH
isolated NH444Cl
NH Cl
Cl
crystal was
crystal
crystal was traced.
was traced. With
traced. With the
With the progress
the progress of
progress ofof solidification,
solidification, natural
solidification, natural convection
natural convection within
convection within the
within thethe section
section around
section around
around a
aa plume
plume
plume waswas was
induced induced
by theby
induced by the thermo-solutal
thermo-solutal
thermo-solutal
the buoyancy. buoyancy.
Thus, an upward
buoyancy. Thus, an
Thus, an
flow upward
within the
upward flow
flow within the
interdendritic
within the
interdendritic
liquid is formed liquid
which is formed
spews manywhich spews
dendrite many
fragmentsdendrite
into fragments
the bulk
interdendritic liquid is formed which spews many dendrite fragments into the bulk liquid [19]. Some liquidinto the
[19]. bulk
Some liquid
of the [19]. Some
fragments
of the
of the fragments
dissolvedfragments
when they dissolved
met thewhen
dissolved when
melt at they
they met thethe melt
a temperature
met melt at aa temperature
above
at temperature
the liquidus. above above
The otherthe fragments
the liquidus. The
liquidus. The other
survived
other
fragments
as the sources survived
of the as
equiaxedthe sources
grains of
when the
they equiaxed
reached grains
the liquid
fragments survived as the sources of the equiaxed grains when they reached the liquid at when
at a they
temperaturereached belowthe liquid
the at aa
liquidus.
temperature
The equiaxed below
grains the liquidus.
rejected from The
the equiaxed
sidewalls grains
began rejected
to grow from
until
temperature below the liquidus. The equiaxed grains rejected from the sidewalls began to grow until the
they sidewalls
reached abegan
size to
when grow until
gravity
they reached
they reached
dominated overaa size
size when
other
when gravity
forces, dominated
thendominated
gravity they started over other forces,
to other
over sink. forces,of
Some then they
thethey
then started
equiaxed
started to sink.
sink.
crystals
to Someto
settled
Some ofthe
of the
the
equiaxed
bottom of crystals
the cavity.settled
During to the
the bottom
settling, ofa the cavity.
coalescence During
could the
have
equiaxed crystals settled to the bottom of the cavity. During the settling, a coalescence could havesettling,
occurred a coalescence
between the could
two have
small
occurredafter
crystals
occurred between
betweenthey thethe two
two small
collided, small
which crystals after
couldafter
crystals they
havethey collided,
promoted
collided, which
thewhich
settling. could
could The have promoted
coalescence
have promoted the settling.
between
the settling.
two
The coalescence
crystals during between
sinking is two
shown crystals
in during
Figure 5. sinking
These is
settled shown
crystals
The coalescence between two crystals during sinking is shown in Figure 5. These settled crystals in Figure
formed 5.
a These
sediment settled
bed. crystals
There
formed
also
formedwere aa sediment
sediment
some bed. There
equiaxed
bed. There
crystals also
also thatwere
were some equiaxed
followed
some equiaxed crystals that
the convectional
crystals that followed
flow followed
and interactedthe convectional
the convectional
with columnar flow
flow
and interacted
and interacted
dendrites with columnar
front with
where columnar
they were dendrites
captured.
dendrites front where they
As shown
front where they
in were6,captured.
Figure
were captured.
the position As shown
As shown in
variation in of
Figure 6, the
the traced
Figure 6, the
position
crystal has variation
been of
marked the traced
with a crystal
circle. Whenhas been
the marked
captured with
crystals a circle.
as well
position variation of the traced crystal has been marked with a circle. When the captured crystals as When
as the the captured
sediment bed crystals
increased as
well
to the as the
height sediment
corresponding bed increased
to the to the
location, height
the corresponding
growth of the to
columnar
well as the sediment bed increased to the height corresponding to the location, the growth of the the location,
dendrite the
front growth
was of
blocked the
columnar
there dendrite front
[20]. dendrite
columnar Afterwards, front thewas
wasCET blocked
occured.
blocked there [20].
there [20]. Afterwards,
Afterwards, the the CET
CET occured.
occured.

Figure
Figure 5. The
Figure5.
5. The coalescence
The coalescence between
coalescence betweentwo
between twocrystals
two crystalsduring
crystals duringsinking.
during sinking.
sinking.
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Figure6.6. Illustration
Figure Illustrationof
of the
the process
process of
of aa downward
downward moving
movingequiaxed
equiaxedcrystal
crystalcaptured
capturedby
bythe
thesolidified
solidified
side wall.
side wall.

3.2. Effect of Cooler on the Solidification Morphology

3.2. Effect of Cooler on the Solidification Morphology
After the solution was poured into the cavity, the cooler was equipped to the top surface center
After the solution was poured into the cavity, the cooler was equipped to the top surface center
and immersed into the solution. The solidification morphology in the cavity at selected moments with a
and immersed into the solution. The solidification morphology in the cavity at selected moments
cooler is shown in Figure 7. After the immersion of the cooler, the degree of supercooling was sufficient
with a cooler is shown in Figure 7. After the immersion of the cooler, the degree of supercooling was
in the center to generate the nucleation. Thus, a large amount of nucleation generated around the
sufficient in the center to generate the nucleation. Thus, a large amount of nucleation generated
cooler and developed into equiaxed grains. The equiaxed grains attached to the cooler surface resulted
around the cooler and developed into equiaxed grains. The equiaxed grains attached to the cooler
in the increase of cooler thickness. Afterwards, the attached grains grew to equiaxed crystals and sank
surface resulted in the increase of cooler thickness. Afterwards, the attached grains grew to equiaxed
into the bulk liquid. After 200 s, the cooler began to melt. It can be observed that the dendrites that
crystals and sank into the bulk liquid. After 200 s, the cooler began to melt. It can be observed that
split off from the cooler remarkably increased the amount of free equiaxed crystals. As the movement
the dendrites that split off from the cooler remarkably increased the amount of free equiaxed crystals.
of free crystals is driven by the density difference between solid and liquid, the natural convection in
As the movement of free crystals is driven by the density difference between solid and liquid, the
the cooler adding zone was enhanced. Thus, the crystal rain introduced by the cooler expanded from
natural convection in the cooler adding zone was enhanced. Thus, the crystal rain introduced by the
the central zone to the whole domain. The overall freezing method simultaneously was altered both
cooler expanded from the central zone to the whole domain. The overall freezing method
internally and externally. The acceleration of the sediment bed growth also promoted the occurrence
simultaneously was altered both internally and externally. The acceleration of the sediment bed
of CET. Moreover, the size of the equiaxed crystals introduced by the cooler was smaller than those
growth also promoted the occurrence of CET. Moreover, the size of the equiaxed crystals introduced
grown from the free crystal rain. This is because with the continuous changes in temperature and
by the cooler was smaller than those grown from the free crystal rain. This is because with the
solute concentration, the convection is enhanced, and the moving crystal grains in the solution will
continuous changes in temperature and solute concentration, the convection is enhanced, and the
repeatedly undergo local dissolution and growth, which will cause the refinement of crystals [21].
moving crystal grains in the solution will repeatedly undergo local dissolution and growth, which
The schematic diagram of the mechanism of the grain refinement is depicted in Figure 8. In addition,
will cause the refinement of crystals [21]. The schematic diagram of the mechanism of the grain
it can be found that the freezing process accelerates with an increase of heat loss rate. The amount of
refinement is depicted in Figure 8. In addition, it can be found that the freezing process accelerates
introduced free crystals increases and the size of the crystals decreases with the increase of the cooler
with an increase of heat loss rate. The amount of introduced free crystals increases and the size of the
thickness. This is because when a thicker cooler is employed, more surrounding solution could be
crystals decreases with the increase of the cooler thickness. This is because when a thicker cooler is
cooled to promote the formation of nucleation. At the same time, more dendrites split off from the
employed, more surrounding solution could be cooled to promote the formation of nucleation. At
cooler are potential nuclei for new grains, promoting the widening of the equiaxed zone.
the same time, more dendrites split off from the cooler are potential nuclei for new grains, promoting
the widening of the equiaxed zone.
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Figure 7. Solidification evolution in the cavity with a consumable cooler introduced inside.
Figure 7. Solidification evolution in the cavity with aa consumable
consumable cooler
cooler introduced
introduced inside.
inside.

Figure 8. Schematic diagram of the mechanism of the grain refinement.

Figure 8. Schematic diagram of the mechanism of the grain refinement.
3.3. Effect of Adding Cooler8.on
Figure Schematic diagramProfile
the Temperature of the mechanism of the grain refinement.
3.3. Effect of Adding Cooler on the Temperature Profile
The measured
3.3. Effect of Adding temperature
Cooler on the variation
Temperature at different
Profile horizontal positions, with and without a cooler,
The measured
was plotted in Figuretemperature
9. The solutionvariation at different
in all cases horizontal
were heated to 85 positions, withof
◦ C. Zero point and
timewithout a cooler,
is the moment
The measured temperature variation at different horizontal positions, with and without a cooler,
when sidewall chilling started. In the reference experiment (without cooler), a relatively rapid is
was plotted in Figure 9. The solution in all cases were heated to 85 °C. Zero point of time the
drop
was plotted
moment when in Figure
sidewall 9. chilling
The solution in In
started. all the
cases were heated
reference to 85 °C.
experiment Zero point
(without of atime
cooler), is the
relatively
in temperature at position T3 occurred in the initial stage because of the large temperature gradient
moment
rapid drop whentemperature
sidewall chilling started. In the reference experiment (without cooler), a relatively
imposed byin the cooling wall. at position T3 occurred
During this period, the in the initial
temperature stage because
at the of the
central large of
position temperature
the cavity
rapid drop
gradient in
imposedtemperature
by the at position
coolingAfter T3 occurred
wall. about
During thisin the initial
period, stage because
the temperature of the large temperature
at the central followed
position of
(T1 and T2) decreased gradually. 200 s, the decrease of the three temperatures a
gradient
the cavity imposed by
T2)the
(T1 andAlso, cooling gradually.
decreased wall. During thisabout
After period,200the temperature of
s, the at the
the three
central position of
similar tendency. the temperature distribution between the decrease
three measuring temperatures
points exhibited
the cavitya(T1
followed and T2)
similar decreased
tendency. gradually.
Also, the solutionAfter about
temperature 200 s, thebetween
distribution decreasetheof three
the three temperatures
horizontal thermal stratification as the was cooled from the sidewalls to themeasuring
center. points
followed
exhibitedahorizontal
similar tendency.
thermal Also, the temperature
stratification distribution
as the solution was cooledbetween
fromthe
thethree measuring
sidewalls points
to the center.
exhibited horizontal thermal stratification as the solution was cooled from the sidewalls to the center.
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Figure
Figure 9. Themeasured
9. The measuredtemperature
temperaturevariation
variation
at at different
different horizontal
horizontal positions
positions (a) (a) position
position T3; T3;
(b)
(b) position T2; (c) position
position T2; (c) position T1. T1.

In
In the
the experiments
experiments with
with aa cooler,
cooler, in
in the
the initial
initial stage,
stage, the
the temperature
temperature atat position
position T1
T1 dropped
dropped
quickly due to the solid cooler. At the same time, the temperature at position T2 decreased
quickly due to the solid cooler. At the same time, the temperature at position T2 decreased because of
because
of the cooling diffusion. The region near the cavity center was cooler than other locations. This
Metals 2019, 9, 55 9 of 11
Metals 2018, 11, x FOR PEER REVIEW 9 of 14

the cooling
situation is diffusion.
different fromThe region near the
the reference cavity
case center was
of cooling fromcooler
externalthan to other
internal.locations.
Under This situation
the combined
is different
cooling effect offrom the reference case of cooling from external to internal.
internal cold source and external cooling, the overall heat dissipation rate Under the combined cooling
of the
effect
cavityofwas thesignificantly
internal coldaccelerated.
source andAs external
a result, cooling, the overall
the decrease of theheat dissipationatrate
temperatures of the T2
positions cavity
and
was significantly accelerated. As a result, the decrease of the temperatures
T3 was accelerated. In addition, the cooling effect of the cooler increases with the cooler thickness. A at positions T2 and T3 was
accelerated.
thicker cooler Inled
addition,
a lowerthe cooling effect
temperature. of the
It can be seencooler thatincreases
for T2, itwith
takes the140cooler
s lessthickness.
for the 7 mm A thicker
cooler
cooler
to drop ledtoa25 lower temperature.
degrees comparedIt with can bethe seen
3 mm thatcooler.
for T2,The it takes
final140 s less for the
temperature in 7the
mm cooler
cavity to drop
center for
to 25 degrees compared with the 3 mm cooler. The final
the 7 mm cooler is also seven degrees lower than that for the 3 mm one. Studies show thattemperature in the cavity center for the 7 mm
larger
cooler
cooling is rate
also will
seven degreesthe
promote lower than that
formation offor
finerthegrains,
3 mm one. thusStudies
the amount show of that the larger
refined cooling
equiaxed rate
grains
will
in thepromote the formation
mold increases with the of finer grains,
increase thus the
of cooler amount
thickness of refined equiaxed grains in the mold
[22,23].
increases
The with the increase
temperature of cooler
gradients thickness
among the three [22,23].points with and without the cooler are plotted in
Figure The 10.temperature
The temperature gradients gradientamong the three
is defined as thepoints with and difference
temperature without the coolerby
divided aretheplotted
distance in
Figure 10. The temperature gradient is defined as the temperature
between the two thermocouples, as T1-T2 and T2-T3 (°C/cm). In all cases, variation of the temperature difference divided by the distance
between
gradientsthe cantwobethermocouples,
divided into three as T1-T2
periods: andfirst
T2-T3 (◦ C/cm).then
increasing, In alldecreasing
cases, variation of the increasing
and finally temperature to
gradients
a stabilized canvalue.
be divided
In the into
initial three periods:
stage, first increasing,
the temperature gradient thenincreased
decreasing and because
firstly finally increasing
the initial
to a stabilized
period is dominated value. by Incooling
the initial stage, theLater,
conduction. temperature
with thegradientprogressincreased firstly because
of solidification in the solid- the
initial
liquid period
interface is dominated
and under the by cooling
effect ofconduction.
latent heat release Later, with and thethe double-diffusive
progress of solidification convection, in thethe
solid-liquid
temperatureinterface gradientand under
drops. the effect
Finally, the of latent heat release
temperature gradient and the double-diffusive
magnitude returns to aconvection,
stabilized
the
valuetemperature gradient drops.
after the solid-liquid interfaceFinally, the temperature
has passed through that gradient
location.magnitude
With a cooler,returnsthe totemperature
a stabilized
value
gradientafter the solid-liquid
between T1 and T2 interface has passed
turned negative, butthrough
the absolutethat location.
magnitude Withofathe cooler, the temperature
difference increased.
gradient between T1 and T2 turned negative, but the absolute
The temperature gradient between T2 and T3 decreased as temperature at T2 dropped faster magnitude of the difference increased.
under
The temperature
the effect gradient
of enhanced between
cooling. It is T2 and T3that
observed decreased
while the as temperature
wall temperature at T2 dropped
reached afasterlowerunderlimit,
the
the effect of enhanced
temperature gradientcooling.
between It isT2
observed
and T3 that while the
decreased wall temperature
gradually in the later reached a lower limit,
stage of solidification.
the
It istemperature
observed in gradient between
the reference T2 and that
experiment T3 decreased
the CET occurs gradually afterinthethesolid-liquid
later stage of solidification.
interface moved
It is observed
over T2, whereincolumnar
the reference experiment
and equiaxed that the
crystals CET occurs
co-exist. The CET after the solid-liquid
occurs in the presence interface moved
of a relatively
over T2, where columnar
low temperature gradientand (aboutequiaxed
2.8 °C).crystals
With aco-exist.
cooler, the TheCETCEToccurs
occursafter in the thepresence of a relatively
solid-liquid interface
low temperature gradient (about 2.8 ◦ C). With a cooler, the CET occurs after the solid-liquid interface
developed over the T3 (between T3 and T2). The achieved temperature gradient (as high as 6.2 °C)
developed ◦ C)
during the over the T3 (between
CET period is much larger T3 and thanT2).that Theof achieved
the reference temperature
experiment. gradient (as high that
This indicates as 6.2 while
during
under the the solution
CET period at aishigh
much larger thangradient,
temperature that of the reference
when a large experiment.
number of This indicates
nucleation that while
is introduced
under
into the thebulksolution at a high
solution, temperature
the triggered gradient,
equiaxed crystalwhen raina large number
can also of nucleation
promote the CET issignificantly.
introduced
into
Withthe thebulk solution,
increase the triggered
of cooler thickness, equiaxed crystal raingradient
the temperature can also increased
promote the CETearly
in the significantly.
stages, whichWith
the increase of cooler thickness, the temperature gradient increased
depresses the growing rate of crystal [24,25]. As such, a thicker cooler will promote the refinement of in the early stages, which depresses
the
the growing
crystals. rate of crystal [24,25]. As such, a thicker cooler will promote the refinement of the crystals.

Figure 10. The temperature gradients between

between the
the three
three points
points with
with and
and without
without adding
adding cooler.
cooler.

4. Conclusions
Metals 2019, 9, 55 10 of 11

4. Conclusions
Experiments were conducted to study the solidification of NH4 Cl-70%H2 O solution in a cavity
with two cooled side walls. The effect of adding a consumable cooler with different thickness into the
cavity was studied. The morphology variation of the crystals and the temperature distribution during
the process were recorded. The main conclusions are as follows:

(1) The solidification process can be divided into three periods: pure columnar dendrites growth,
equiaxed crystal rain occurrence, equiaxed crystal block the columnar growth to a steady state.
(2) Introduction of the consumable cooler can significantly reduce the temperature of the central
zone of mold. Melting of the consumable cooler can supply large quantity of equiaxed grains
and refine the crystal size. The introduced equiaxed crystals can block the growth of columnar
dendrites, thereby promoting the CET.
(3) In the reference experiment without a cooler, CET occurs when the temperature gradient
decreased to 2.8 ◦ C. In the experiment with a consumable cooler included, the CET occurs
even if the temperature gradient is as high as 6.2 ◦ C.
(4) The consumable cooler with a larger thickness can introduce more equiaxed crystals with smaller
sizes. Thus, the solidification rate and the compactness of the solidified structure increased.

Author Contributions: R.N. and B.L. designed the experiments; R.N., Z.L. and L.B. analyzed the results; X.L., X.Y.
and F.T. assisted in data analysis and revised manuscript.
Funding: The authors’ gratitude goes to National Natural Science Foundation of China (51574068 and 51604070)
and Young Elite Scientists Sponsorship Program by China Association for Science and Technology (CAST).
Conflicts of Interest: The authors declare no conflict of interest.

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