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On the Use of an Incremental Casting

Technique To Obtain Color Gradients


In Jewelry Components
By Dr. F.S. Silva, L. Mazare, B. Henriques
& D. Soares, Department of Mechanical
Engineering, University of Minho

©2011 The Bell Group, Inc. All rights reserved.

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On the Use of an Incremental
Casting Technique to Obtain Color
Gradients in Jewelry Components

Dr. F.S. Silva


L. Mazare
B. Henriques
D. Soares
Department of Mechanical Engineering,
University of Minho
Azurem, Portugal

Abstract
The production of colored gold-based components (white, red, pink, blue, green,
purple, yellow, etc.) is widely known but the production of multi-colored pieces
(with two, three or more colors and a smooth gradient in between) in one casting
step (without components soldering) is a totally new manufacturing process. This
process applies to the production of gold artifacts including the jewelry field. Its
main advantage is the ability to develop and produce jewelry pieces with
innovative designs. The basis of the process is the production of gold-based
components with a controlled color gradient. This is obtained with the control of
the alloy chemical composition along the piece. The component’s production will
be based on an incremental process of melting and solidification.
The process is essentially based on a continuous melting of the base materials
by induction heating inside a mold with the addition of new elements or alloys
in order to continuously change the component’s chemical composition. By the
control of the process variables (materials added, melting and solidification rates)
it will be possible to obtain a component with the desired chemical composition
gradients. The chemical composition gradient will be selected considering the
aesthetic of the component and the physical, metallurgical and mechanical
properties of the intermediate phases formed in the component. The end of the
process yields jewelry pieces (polychromatic pieces like rings, pendants, etc.)
with controlled color gradients along the component in both a micro and macro
scale.

1. Introduction
While some recent experiments have been carried out using the Incremental
Melting and Solidification Process (IMSP), it is still a new field of materials
processing for the production of functionally graded materials,1,2,3 and there is
still a substantial lack of information on this process, especially in regards to
different materials.

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The operation principle can be described as follows. The different materials that
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are continuously fed to the mold are melted by induction heating. This procedure
creates a gradual melting at the top of the casting and solidification at the
bottom of the casting. The IMSP proceeds from the bottom to the top of the mold
by changing the relative position between the mold and the heating apparatus.
This process allows the possibility of having locally controlled properties on a
single component. It permits a new concept of materials design that may be used
to respond to tailoring of components that will be exposed to different local
solicitations, either mechanical or environmental, under particular applications. In
the case of jewelry components, which are mainly dependent on aesthetic aspects,
the different properties are mainly physical such as color and brightness, etc.
Furthermore, the IMSP is expected to allow the production of components
with a smooth chemical transition between dissimilar materials. The interface
region might have lengths in the order of hundreds of micrometers to tens of
millimeters, if necessary. The gradual transition allows for a smoother transition
in metallurgical, mechanical and physical properties of the materials and
consequently creates components with a different aesthetic then those with
different colors but obtained with welding processes where sharp color
transitions occur.
Further to the chemical composition transition, this process is able to control
the solidification behavior in any point on the casting in a specific way. This
means that even with a homogeneous alloy it is possible to substantially vary
some metallurgical features such as grain size and grain orientation, thereby
providing different mechanical, wear and physical properties in different parts of
the component.
This paper is concerned with the possibility of producing functionally graded
alloys with an extended transition region between two dissimilar materials as
well as with the control of the metallurgical properties along a homogeneous
material.

2. Materials and Methods


Materials
To test the technology a simple alloy system (Figure 1) was selected. The Ag-Cu
phase diagram is constituted by a eutectic transformation, and the solid solution’s
limits are characterized by a very low solute solubility at room temperature. Two
dissimilar alloys were tested: a silver-rich alloy with a composition of 95Ag5Cu
and a copper-rich alloy with a composition of 80Cu20Ag (Figure 1).
The Cu-Ag system was chosen for these first experiments on the IMSP because
it is a simple system with no intermetallic formations, very similar to the ones
used in jewelry with Au-Ag or Au-Cu. Furthermore and in order to facilitate the
process, the pure metals do not have very different melting temperatures.

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Figure 1 Ag-Cu phase diagram. The pointed lines correspond to
the chemical composition of the Ag-rich and Cu-rich alloys used).4

Methods and Processing


Two different types of experiments were carried out using an induction furnace:
1) In the first tests, castings with a selected homogeneous alloy (Ag-rich and
Cu-rich) that was placed inside the mold in order to fill it when heated
2) Castings with sequential addition of the alloys (from Cu-rich to Ag-rich )
during casting in order to generate a functionally gradient material
The first experiments were performed in order to observe what influence the
mold dislocation rate would have on properties such as chemical composition,
hardness, and grain size along the length of the sample. The second experiments
were performed in order to produce functionally graded materials.
The castings were performed in a fixed induction coil furnace in which the mold
could be moved vertically at a controlled speed as schematically shown in Figure
2. The bottom of the mold was water cooled. This cooling system promotes a
progressive cooling direction essentially from the bottom to the top of the mold.
Six thermocouples were placed in the mold in order to capture the temperature
profile with time at six different points (see Figure 3a) from bottom to top of the
specimen as the casting progressed. The dimensions of the specimen obtained are
shown in Figure 3b.

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Three
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Anot
a com
cooli
meta
exper

Tabl
an
Figure 2 Schematic representation of the IMS Process
Te
N
1
2
3
4
5

b) I
d
A
In th
state
Figure 3 a) position of the thermocouples inside the mold 0.1m
and initial position of coil in relation to the mold; part
b) dimensions of the specimen obtained (mm) the m
stopp
The
a) Incremental cooling with homogeneous alloys for different mold (by S
dislocation rates perce
Phas
These experiments were performed in two steps. First the mold was heated in a
was m
defined position inside the coil (Position 1 in Figure 2) with the material inside the
mold from the beginning of the test; after the mold reached a certain temperature
with the material melted, the mold started to move downwards within the fixed
coil. The mold movement stopped when the mold was out of the coil (see Position 3. R
3 in Figure 2). Throughout the whole process the bottom of the mold was water
a) I
cooled and the heating power remained constant. With this procedure, at a
certain moment the temperature at the lower part of the mold is below the
d
‘solidus’ (the material is solid), while the upper part of the mold is still above the These
liquidus temperature (the alloy is still liquid). Thus progressive solidification is the m
promoted from the bottom to the top of the casting. The thermal cycles for each the ca
test are presented in Figures 4 and 6 for the two alloys and for the different the m
relative mold dislocation rates. for th
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Three different mold dislocation rates were tested (0.1, 0.5 and 1.0mm/second).

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Another test was performed without mold movement. This test was used for
a comparative baseline in order to know what the influence of the directional
cooling in the castings would be. The samples were characterized in terms of
metallurgical and chemical properties in the axial direction of the specimen. The
experimental conditions are presented in Table 1.

Table 1 Experimental conditions used in the castings with homogeneous alloys (1 to 4)


and with a functionally graded material from a Cu-rich alloy to a Ag-rich alloy (5)

Test Frequency Mold speed Power input (V)


Casting Type
Nº (kHz) [mm/s] Ag alloy Cu alloy
1 0
2 0.1
Homogeneous
3 250 0.5 60 %
4 1.0
5 FGM 0.1

b) Incremental melting and cooling with sequential addition of two


different dissimilar materials: from Cu-rich alloy (80Cu20Ag) to
Ag-rich alloy (95Ag5Cu)
In this case 5.532 grams of Cu-rich alloy was introduced into the mold in a solid
state and fully melted. Then the mold started to move downwards at a rate of
0.1mm/second. While the lower part of the alloy was solidified and the upper
part was still liquid, 6.228g of the Ag-rich alloy in a solid state was added into
the mold. The movement proceeded until the mold was out of the coil and then
stopped (see Position 3 in Figure 2).
The samples obtained were characterized in terms of chemical composition
(by SEM/EDS) and microstructure (optical microscope), namely by phase
percentage quantification and grain size quantification along the axial direction.
Phase quantification was obtained using an image analysis technique. Grain size
was measured based on secondary dendrite arm spacing (SDAS).

3. Results and discussion


a) Incremental cooling with homogeneous alloys for different mold
dislocation rates
These first experiments were performed in order to understand what would be
the metallurgical features influencing both physical and mechanical properties of
the castings. Figure 4 presents the solidification curves and the relative position of
the mold in relation to the coil for the Ag-rich alloy. Similar curves were obtained
for the Cu-rich alloy.
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Figure 4 a) Temperature curves for the Ag-rich alloy with coil movement
rate of 0.5mm/s; b) detail of the temperature curves in the solidification range

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The first part of the thermal cycle is the one with the mold and coil fixed. It can be

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seen that, due to the relative position of the coil in relation to the mold but more
importantly due to the proximity of the thermocouple T5 to the cooling system
(Figures 2 and 3a), the temperature at the bottom of the mold is lower than the
temperature in all other positions by about 100ºC (180°F). In the remaining
positions the temperatures are mainly dependent on the position of the mold
relative to the induction coil. There is a difference among the other thermocouples
of less than 30ºC (54°F).
The second part of the thermal cycle is when the mold starts to move downwards.
The main aspect to highlight (Figure 4) is that the movement has a strong
influence on the temperature distribution along the mold axis. Temperatures T3,
T4 and T5 start to decrease but T0, T1 and T2 increase for a certain period. These
profiles are strongly dependent on the dimensions of the coil and the mold used.
In these particular experiments the height of the mold is greater than that of the
coil (see Figure 3). After a few seconds, when T0 reaches the peak temperature, all
the temperatures start to decrease. It is observed that temperatures at this moment
have a difference of about 350ºC (630°F) between the extreme positions, T0 and T5,
and provide a regular step among the different thermocouples between the top
and bottom of the mold.
Figures 5a and 5b show that, during the solidification intervals in both alloys when
there is mold movement, the temperature cooling rates are higher in position T0
and lower for position T5. Thus, although the solidification sequence is from
position T5 to position T0, the solidification rates follow the opposite sequence.

Figure 5a Solidification time for silver-rich alloy

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Figure 5b Solidification time for copper-rich alloy

It can be seen in Figures 5a and 5b that the solidification rates are very different
between mold positions and also substantially differ with mold dislocation rate.
As a comparison, temperature profiles in tests with no movement of the mold are
also provided. Figure 6 presents temperatures profiles obtained in the castings of
the Ag-rich and Cu-rich alloys without mold movement.
The temperature profiles are very different. Part one of the thermal cycle is
similar but after the alloy is fully melted and the induction power is switched off,
the temperature profiles are very different from those in Figure 4. The maximum
temperature difference in the different mold positions at the solidification interval
is less than 100ºC (180°F), which is much lower than that shown in Figure 4, and
the rates of temperature decrease are very similar among the different positions
(Figure 5). The solidification still proceeds from bottom to top but with very
close cooling rates between positions. The bottom part of the mold remains water
cooled during the whole test.

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Figure 6 a) Temperature curves for Ag-rich alloy without mold movement;
b) detail of the temperature curves in the solidification range

b) Incremental melting and cooling with sequential addition of two


different dissimilar materials: from 80Cu20Ag to 95Ag5Cu
In this experiment a gradual chemical transition was promoted by a sequential
addition of the two different alloys. The temperature curves obtained are
presented in Figure 7.
As was done in the previous test, the copper-rich alloy was placed in the mold
and was fully melted. The material filled only half of the mold (the related
temperature reading positions are T5, T4 and T3). The lower temperature is above
980ºC (1796°F), the liquidus temperature of the alloy (Figure 7). After 400 seconds
the mold started to move down at a rate of 0.1mm/s. After some time there is a
partial solidification of the Cu-rich alloy inside the mold. The bottom part of the
alloy (T5) is below its liquidus temperature but the top (T3) is still fully liquid.
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The Ag-rich alloy was then added in the solid state (Figure 7). The added Ag-rich
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Met
alloy mixed with the top part of the liquid Cu-rich alloy. As there is a temperature
profile on the Cu-rich alloy region, the mixing process should provide a gradient a) In
of chemical composition along the component. The sample obtained is expected d
to have a decreasing copper content from the bottom to the top (Figure 13b). The As a
process proceeded at 0.1mm/s until the mold was out of the coil region. Figure 5 the t
shows that the cooling rates are similar to the ones obtained for the homogeneous micro
alloy at the same dislocation rate. The whole temperature profile along the mold speci
during the test is quite similar to the equivalent one for the homogeneous alloy
The f
that had the same mold dislocation speed rate (see Figures 4 and 7). Using this
The
experimental procedure a sample was obtained that exhibited material with
size
several different zones in terms of chemical composition and microstructures.
first
solid
in Fig

These
be se
move
conse
rate i
prop
Figure 7 a) Temperature curves obtained in the IMSP for the experiments
the S
with movment of the coil for graded chemical composition;
b) detail of the temperature curves in the solidification range
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Metallurgical analysis
a) Incremental cooling with homogeneous alloys for different mold
dislocation rates
As an example, Figures 8 and 9 present the microstructure of one series of
the tests (mold rate of 0.1mm/s) for the two tested homogeneous alloys. The
microstructures are representative of the bottom, middle and top regions of the
specimens.
The first aspect to highlight is that there is a gradual variation of microstructure.
The difference in grain size is clear, mainly for the Cu-rich alloy. The grain
size decreases from bottom to top. In fact, although the bottom region is the
first to solidify the solidification rate is lower in that region (see Figure 7). The
solidification rates in Figure 5 are representative of both homogeneous alloys and
in Figure 10 you can see the SDAS along those castings.

Figure 8 Microstructures obtained along the piece for the


Cu-rich alloy with mold speed of 0.1mm/s (mag. 500X)

Figure 9 Microstructures obtained along the piece for the


Ag-rich alloy with mold speed of 0.1mm/s (mag. 500X)

These micro-structural changes can be explained by the solidification rate. It can


be seen that, for example, the Ag-rich alloy (Figures 5a and 10a) with no mold
movement has about the same solidification rate along the whole component and
consequently the same SDAS. For 1mm/s of dislocation rate the solidification
rate increases from the bottom to the top and the SDAS decreases in the same
proportion. The other solidification rates are in between the previous values and
the SDAS is also in between.

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b) In
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An expected result in Figure 5 is that the faster the mold dislocation rate, the
higher the cooling rate. Furthermore, without mold movement and due to the d
water cooling system at the bottom, the cooling rates are higher at the bottom. (9
With mold movement the cooling rates change from lower values at the bottom In th
to higher values at the top. varia
mate
more
trans
will s
eutec
(Figu
of th
evolu
alloy
mate
a lim
alrea
Figure 10 SDAS a) Ag-rich alloy and b) Cu-rich alloy to ob
proce
For e
Regarding the chemical composition, it is observed that although the initial alloy addit
chemical composition was homogeneous along the component, for the lowest
mold rate (0.1mm/s) on the copper-rich alloy, there is a change in the copper
content from 84% in the bottom to 75% in the top. This shift in chemical
composition is attributed to macro-segregation effects.5 This shift also shows that
it is possible to obtain chemical gradients by using very small mold dislocation
rates. However, this procedure is very time consuming.
With the increase in the mold dislocation rates the solidification rate also increases
(Figure 5), and there is no time for the liquid phase to move from the bottom to
the top region of melt (macro-segregation). Thus the distribution of Cu phase and
eutectic constituent is more homogeneous along the sample.
The s
is pre
rates

a) b)
Figure 11 Chemical composition along the sample’s vertical axis for Figur
a) Ag-rich alloy; b) Cu-rich alloy.
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b) Incremental melting and cooling with sequential addition of two

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e, the
o the different dissimilar materials: from Cu-rich (80Cu20Ag) to Ag-rich
ttom. (95Ag5Cu)
ottom In this test a mold dislocation rate of 0.1mm/s was selected. For the test with
variation of chemical composition from Ag-rich to Cu-rich imposed by two
material additions, the solidification characteristics are quite different and much
more complex. Between the initial alloy chemical compositions there is a eutectic
transformation (Figure 2). Thus, chemical composition of the resulting sample
will start with an alloy rich in the Cu phase (Figure 12a) in the bottom region. The
eutectic constituent increases until a certain region in the middle of the sample
(Figure 12b) and from that point on the Ag phase increases until the top region
of the sample (Figure 12c, d and e). The resulting chemical composition
evolution along the sample is shown in Figure 13b. It can be seen that the second
alloy added mixed with the liquid phase in the first alloy added and the liquid
material almost homogenized. The chemical composition variation occurred in
a limited region of about 10-15mm of the sample. This result shows that there is
already a substantial gradient region between initial alloys. However, in order
to obtain smoother transitions there are other possibilities such as using other
processing parameters or adopting a procedure with more additions of material.
For example, after the first addition of a Cu-rich phase there can be two or more
alloy additions of the Ag-rich alloy.
owest
opper
mical
s that
ation

a) b) c) d) e)
eases
om to Figure 12 The microstructure from the bottom a), to the top e) of a casting
e and

The solidification rates along the sample are shown in Figure 7. The SDAS graph
is presented in Figure 13a. This graph shows again that for higher solidification
rates the grain size is smaller.

a) b)
Figure 13 a) Alloy SDAS, b) and mean chemical composition along the sample’s vertical
axis for the experiments with graded chemical composition

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This result shows that this process allows the production of functionally graded
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components. It also shows that even for homogeneous alloys the process may give
rise to different metallurgical properties along the component.
Obviously the process is not easy but with a careful coordination of the
temperature profiles along the piece (by changing the power input along the
casting) with the characteristics of the new materials additions (chemical
composition, addition time, quantity of added material, and temperature of the
added material – solid or liquid state), it will be possible to control the final phase
morphology distribution and respective mechanical properties.
In the case of jewelry components this process allows aesthetic effects like
those shown in the following pictures. Figure 14 shows two components with a
controlled solidification: one with elongated grains and the other with regular
grains. Figure 15 shows a component with changing chemical composition from
left to right and approximately equal grain size from left to right.

Figure 14 Example of a gold-based components with


a) oriented solidification, b) homogeneous solidification

Figure 15 Example of a gold-based specimen with a changing


greenish (left) to reddish color (right) and micro gradients

Figure 16 shows a component where the chemical composition is homogeneous


along the component, but there is a strong difference in the solidification behavior
along the component. On left and right sides of the component the solidification
rates are high while in the middle there is a very low solidification rate. Finally,
Figure 17 shows a component where both chemical composition and solidification
behavior are locally controlled.
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Figure 16 Example of a gold-based specimen with homogeneous
chemical composition and changing solidification behavior

Figure 17 Example of a gold-based specimen with both changing color


(chemical composition) and solidification behavior

This process allows the designer to have tools for enhancing the aesthetics of the
jewelry components and to provide a completely new and unique type of jewelry
component.

4. Conclusions
The main conclusions drawn from this work are as follows:
• The Incremental Melting and Solidification Process allows the production
of materials with controlled gradient chemical compositions.
• The incremental solidification process allows the production of
homogeneous alloys with changing microstructure along the component.
• The incremental solidification process is strongly dependent on the
solidification characteristics of the alloy as imposed by the mold
dislocation rate.
• A smooth, controlled gradient transition is possible with several
material additions.

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References
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1. F.S. Silva, “Process and Equipment for Obtaining Metallic Components


or Metal Matrix Components with Varying Chemical Composition Along
Its Height and Components Thus Obtained,” International Pending Patent
PCT/PT2004/00020 (2004).
2. P. Pinto, L. Mazare, D. Soares, F.S. Silva, “Incremental Melting and
Solidification Process-Metallurgical Characterization,” FGM Congress,
Hawaii (2006).
3. L. Mazare, P. Pinto, D. Soares, F.S. Silva, “Mechanical and Metallurgical
Characterization of Cu-Sn and Cu-Ag Graded Materials Obtained by an
Incremental Melting and Solidification Process,” IV Int. Mat. Symp., Porto
(2007).
4. T. Massalski: ASM CD-ROM, Binary Phase Diagrams, 2nd ed. (Ohio: ASM
International, 1996).
5. C. Beckerman, “Macrosegregation,” Encyclopedia of Materials: Science and
Technology, ISBN: 0-08-0431526 (2001): 4733-4739.

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