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GRAIN REFINEMENT OF PERMANENT MOLD CAST COPPER BASE ALLOYS

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Grain Refinement of Permanent Mold Cast Copper-Base Alloys

M. Sadayappan
Materials Technology Laboratory (CANMET), Ottawa, Ontario, Canada

D. Cousineau, R. Zavadil, M. Sahoo and H. Michels*


Materials Technology Laboratory (CANMET), Ottawa, Ontario, Canada
* Copper Development Association, New York, USA.

Copyright 2002 American Foundry Society

ABSTRACT

The grain refinement behaviour of Cu-Zn alloy as influenced by various alloy additions such as tin, aluminum and lead was
evaluated. Tin reduces the amount of grain refiner required for effective grain refinement. On the other hand, aluminum, lead
and bismuth act as grain refiners to some extent. In the second phase of this investigation, grain refinement of four different
copper alloys, leaded yellow brass, Bi/Se modified yellow brass (EnviroBrass III), silicon brass and silicon bronze was
investigated in permanent mold casting conditions. Five different grain refiners Cu-B, FKM 2000, Desofin, Cu-Zr and Cu-Zr-
Mg, were tested for their potency. It was found that boron refined both the yellow brasses whereas zirconium was found to
be effective for all four copper alloys.

INTRODUCTION

Grain refinement is a known and well-established process for many alloys, especially aluminum, which results in enhanced
casting characteristics and improved mechanical properties. Grain refinement of copper-base alloys in permanent mold
casting process is fairly new and is aimed at improving the hot tearing resistance and pressure tightness of plumbing
components.

Preliminary research at MTL has shown that the mechanism of grain refinement in copper-base alloys is not well understood
including the interaction between the grain refiner and minor alloy additions such as Sn, Al, Bi, Se and Pb (Fasoyinu 1997,
Sadayappan 1999). The interaction of various alloy additions is important in the selection of the appropriate grain refiner for
different alloys. For example, European work suggests that for yellow brass, both leaded and Bi/Se modified, boron is
effective only at tin levels less than 0.4%. Zirconium should be added to refine the grain structure when the tin content
exceeds 0.4%. Usually, copper alloys intended for permanent mold casting process contain 0.3 to 0.5% aluminum which is
added to improve casting fluidity in permanent mold casting. However, its effect on the grain refinement is not well
established. Another variable is the effect of cooling rate on grain refinement. Sand castings require relatively more grain
refiners than permanent mold castings. Furthermore, different section sizes may reveal different grain sizes after grain
refinement. This effect would be important in a casting with varying section sizes where the cooling rates differ from section
to section.

Other important issues to be resolved are the fading, loss of grain refinement over prolonged holding or remelting, hard spot
formation and corrosion resistance of grain refined copper alloys (Sahoo, 1997). To understand the grain refinement
mechanism of various copper alloys used in permanent mold casting, a three year study was undertaken at the Materials
Technology Laboratory (CANMET) along with various industry partners, AFS, CDA and US Department of Energy. The
objectives of Year I are given below. This report presents the results from the grain refinement part of the investigation.
1. Effect of minor alloy additions such as tin, aluminum and lead on the grain refinement of base Cu-36% Zn yellow brass.
2. Effectiveness of different commercial grain refiners on four copper alloys namely leaded yellow brass (C85800), Bi/Se
modified yellow brass (EnviroBrass III, C89550), silicon brass (C87500) and silicon bronze (C87600).
3. Investigate the hard spot formation in base and grain refined copper alloy in the presence of impurity elements.
4. Develop an effective experimental method to evaluate grain refinement in copper alloys.

EXPERIMENTAL DETAILS

EFFECT OF MINOR ALLOY ADDITIONS


250 kg of base alloy with a composition of Cu-36% Zn was prepared in an induction furnace and cast into ingots. Three
samples from the melt as well drillings from ingots were sent for wet chemical analysis.

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Two permanent molds were used in this investigation, a shrink bar and a stepped plate. This plate has five section sizes 25,
19, 12.5, 6.25 and 3.2mm (1, 0.75, 0.5, 0.25 and 0.125 in.) and was selected to assess the effect of section size on grain
refinement. The plate mold was mounted on the IMR C-40 gravity permanent mold casting machine. The shrink bar casting
is 125 mm long x 19 mm diameter. Both the molds were preheated to 200C and coated with insulating wash before
commencing the casting.

The Cu-36% Zn alloy ingots were melted in a clay graphite crucible using a push up type induction furnace. The initial
charge was 25kg. After meltdown, castings were poured into the shrink bar and step plate molds. Then selected amount of
alloying element (Sn, Al or Pb ) was added and castings were produced. Boron was added as grain refiner either before or
after the minor alloy addition. In case of Bi/Se modified yellow brass, initially the effect of adding Bi, Se and Ni on grain
refinement was estimated. This was followed by evaluating the effect of Sn and Al in an alloy containing Bi, Se and Ni using
zirconium as the refiner.

The step plate casting was sectioned in the middle and polished. Two half inch specimens were obtained from the bottom of
the shrink bar for macro and micro examination. The macrostructure was revealed by a 50% nitric acid – alcohol solution.
The micro examination was carried out using ferric chloride etch.

EFFECT OF GRAIN REFINERS


In the second part of the investigation, the effect of various grain refiners in four different copper alloys was investigated. The
selected alloys and their composition are listed in Table 1. Of these, three alloys (400 kg each) were prepared at MTL. H.
Kramer supplied the silicon brass ingots. These ingots were used subsequently for the grain refinement work. The melting
and casting procedures followed were explained in the previous section.

Table 1. Compositions of the base alloys prepared

Element Yellow EnviroBrass III Silicon Silicon


Brass Brass Bronze
Zn 36.5 36.5 14 5
Sn 0.3 0.3 - -
Pb 1.5 - - -
Bi - 0.9 - -
Si - - 4.5 4.5
Al 0.4 0.4 - -
Others - 0.04 Se; 0.5 Ni - -

The first casting was obtained before any grain refiner addition and then the grain refiner was added progressively in four
steps. Two grain refining elements, boron and zirconium, were used in this study. Boron was added in three different forms
(Cu-B, FKM 2000 and Desofin) whereas Cu-Zr and Cu-Zr-Mg master alloys were used to add zirconium. The five different
grain refiners and their level of addition are listed in Table 2. After each addition, one step bar and one shrink bar casting
were poured along with the specimen for chemical analysis. Specimens were obtained from the bottom of the shrink bar.
Also, the step plate was sectioned for macro examination.

RESULTS

MACROSTRUCTURAL STUDIES

Grain size evaluation


To-date there are no standards for grain size measurement of cast copper alloys. The existing ASTM standard for grain size
is restricted to wrought copper alloys which are predominantly single phase materials. The grain size of multi-phase cast
alloys will be coarser than wrought alloys. Hence, it was decided to develop some internal standards to assess the grain size
of the cast copper alloys. Two approaches were taken using macro and micro structural studies. The macrostructure were
used as an initial screening test which could be confirmed by microstructural analysis if necessary.

Macrostructures from the step plates were analyzed visually and arranged from very coarse to very fine. From these
macrostructures, a scale containing eight macrostructures was constructed. All the castings could be rated using this scale.
The coarse structure was given a rating of 1C and the finest structure was rated as 8C. The ‘C’ in the rating indicates that
this is for cast alloys. The relative sizes of the grains vary from 3mm in the case of rating 1C to close to 100 microns for the

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rating 8C. (It should be noted that this scale should not be confused with the scale recommended by ASTM for wrought
alloys; ASTM scale is much finer than the current one which vary from 200 microns to 10 microns). The grains were visible
to naked eye till a rating of 6 beyond which the grains were very fine.

Table 2. Composition and levels of additions for the grain refiners used

Refiner Mode of Composition Max. Level of addition, %


addition
Boron Cu-B 2% boron 0.001, 0.005, 0.01 & 0.025
Zirconium Cu-Zr 50% Zirconium 0.001, 0.01, 0.03 & 0.06
Zirconium Cu-Zr-Mg 9% Zirconium 0.001, 0.005, 0.01 & 0.025
9% Magnesium
FKM 2000 Powder Fluoride salts 0.05, 0.1, 0.15 & 0.2
(Proprietary)
Desofin Powder Fluoride salts 0.05, 0.1, 0.15 & 0.2
(Proprietary)

The scale with eight macrostructures is presented in Figure 1. The actual size of the casting is 19mm (0.75 in) thick and the
full casting is shown in the macro photograph. It is evident from the images (a) and (b) that the structure consists of columnar
grains near the wall which changes to equiaxed structure towards the centre of the casting. The evidence of grain refinement
was always the gradual disappearance of the columnar structure which could be used as a visual aid in the evaluation process.

(a) Rating 1C (b) Rating 2C (c) Rating 3C (d) Rating 4C

(e) Rating 5C (f) Rating 6C (g) Rating 7C (h) Rating 8C

Figure 1. Macrographs of the Cu-Zn alloy indicating coarse to fine grain structure

The castings were rated using the above scale by three different operators and averaged. The average may be in the fractions
also. The rating for one melt of base Cu-Zn alloy is shown in Table 3. The first rating of 1.3 indicates that the grain size is
between rating 1C and 2C (The letter ‘C’ is not added in all columns to reduce confusion). Casting #5 has the fine size with a
rating of 6.2C which will be between rating 6C and 7C. The macrostructure of these plate castings are shown in Figure 2.
The total length of the plate is 150 mm (6 in.) and the thickest section is 25mm (1 in.). The results from the table and figure
indicate that the grain size did not change much till 50 ppm of boron was added (casting #4) and full refinement was achieved
only after the addition of 260 ppm boron. Another aspect to be noted is the uniform grain structure in all the section sizes of
the step plate. As mentioned earlier the section size varies from 25 to 3.2 mm. This indicates that the effect of variable
cooling rate is not a factor for grain refinement of permanent mold cast copper alloys.

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Table.3 Rating of one melt for grain size of Cu-36% Zn alloy

Melt Casting # Addition Zn B, % Grain size rating

Op1 Op2 Op3 Aver


N0017 1 Base 35.3 0 1 1 2 1.3C
2 50 gm Cu-B 35.1 0.002 2 2 2.5 2.2C
3 25 gm Cu-B 34.2 0.003 2 1.5 2 1.8C
4 50 gm Cu-B 31.7 0.005 3 3 3 3.0C
5 400 gm Cu-B 33.9 0.026 6 6 6.5 6.2C

Figure 2. Macrographs of step plate casting


Rating from top to bottom 1.3, 2.2, 1.8, 3.0 and 6.2

Effect of minor alloy additions

Leaded yellow brass


The effect of various alloy additions such as tin, aluminum and lead to the base Cu-Zn alloy was investigated after
developing the macro scale for grain size evaluation. Table 4 presents the result of two melts carried out to evaluate the
effect of tin. In the first melt (N0022) 30 ppm of born was added to the base alloy. Then 0.24% tin was added to the alloy.
This resulted in a reduction of the grain size from a rating of 2.3C to 6.0C showing the effect of tin on grain refinement. The
tin content was increased gradually in steps to 1.35% and the grain size varied between 6.2C and 6.5C. In the second melt
(N0029) 0.4% tin was added to the base alloy and the amount of boron was increased slowly. The fine grain size was
achieved with only 40 ppm of boron. This grain size is equivalent to that of the base alloy with 260 ppm of boron.

Similar experiments were conducted to study the effect of aluminum and lead on grain refinement. Some combinations of
these three elements were also evaluated. The results are presented in Table 5. Some salient observations are as follows:
• Tin reduces the amount of boron required for grain refinement. With 0.3% tin, the boron required for grain refinement
reduces from 260 ppm to 30 ppm.
• Aluminum has a significant effect on grain size. When 0.25% aluminum was added to the Cu-Zn-Sn alloy (free of boron)
the grain size rating increased from 2C to 4.5C.
• Lead refines the structure quite effectively even before boron addition. The rating for the alloy with 1% lead is 6.5C.
• The refinement of the alloy with all three elements could be achieved only with 10 ppm boron. The structure got finer as
the boron content was increased from 10 ppm to 90 ppm and a rating of 8C could be achieved.

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Table 4. Effect of tin and zinc on the grain refinement of Cu - 36% Zn alloy

Melt Casting Zn Sn B, % Grain size rating


# Op1 Op2 Op3 Aver.
N0022 1 35.2 0 0.003 2 2 3 2.3C
2 35.2 0.24 0.003 6 6 6 6.0C
3 35.0 0.55 0.003 6 6.5 6.5 6.3C
4 35.9 1.35 0.002 6 6 6.5 6.2C
5 34.6 1.29 0.010 6.5 6.5 6.5 6.5C
N0029 1 35.6 0.41 2 2.5 2.5 2.3C
2 35.6 0.41 0.002 4 4.5 4.5 4.3C
3 35.2 0.41 0.003 5 4.5 5 4.8C
4 35.2 0.41 0.004 6.5 6.5 6.5 6.5C

Table 5. Effect of various minor alloy additions on the grain refinement of Cu-36% Zn alloy

No Composition, % Boron Grain size


Zn Sn Pb Al % Ppm Rating
1 35 - - - - 1.3
2 34 - - - 0.026 260 6.2
3 35.2 - - - 0.003 30 2.3
4 35.2 0.02 - - 0.003 30 6.0
5 35 0.5 - - 0.003 30 6.3
6 35.2 0.4 - - 0.004 40 6.5
7 35.9 1.35 0.002 20 6.2
8 36.5 0.35 0.25 - - 4.5
9 36.5 0.34 - 0.25 0.0029 29 5.8
10 37 0.33 0.24 0.017 170 6.7
11 34 - 1.0 - - 6.5
12 33 - 1.0 - 0.016 160 6.5
13 35 0.4 1.2 0.36 - - 5.5
14 34.2 0.4 1.2 0.36 <0.001 <10 6.3
15 34 0.4 1.2 0.36 0.0015 15 6.5
16 34.5 0.4 1.2 0.36 0.009 90 8

Bi/Se modified yellow brass


The effect of tin and aluminum was also investigated for the Bi/Se modified EnviroBrass III. However, based on our previous
work zirconium was used to refine this alloy and added as zirconium sponge. The results from this investigation are listed in
Table 6. Initially, Bi and Se were added to Cu-Zn alloy to examine their effect on grain size. Another element present in the
alloy, 0.5% nickel was added assuming that it will not have any impact on the grain size. Similar to the observations for lead
in yellow brass, bismuth reduced the grain size of the base Cu-Zn alloy. Tin alone had no effect on grain refinement.
However, it reduced the amount of zirconium required to grain refine the base alloy. Aluminum, on its own, had reduced the
grain size of the base alloy. Similar to leaded yellow brass, EnviroBrass III with bismuth, tin and aluminum has a fine grain
size even before the addition any grain refiner.

Effect of grain refiners on commercial alloys


Four copper alloys were prepared as explained in the experimental section. The compositions for leaded yellow brass and
EnviroBrass III were selected based upon the results from the investigation on the effect of minor alloy elements on grain
refinement. The compositions are reported in Table 1. Five different grain refiners were tested as shown in Table 2. The
macrostructures revealed by 50% nital etch were evaluated by three operators and averaged. Summary of results is presented
in Table 7. The observations are:
• The grain size of yellow brass, EnviroBrass III and silicon bronze is very fine even in the unrefined condition (base
alloy). Only silicon brass has a coarse grain structure.

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Table 6. Effect of various minor alloy additions on the grain refinement of EnviroBrass III

No Composition Zirconium Grain size


Zn Bi Sn Al Others % Ppm rating
1 35.3 - - - - - - 1.3C
2 35.3 0.9 - - 0.6 Ni, 0.03 Se - - 4.3C
3 35.3 0.9 - - 0.6 Ni, 0.03 Se 0.1 1000 7.0C
4 35.1 0.9 0.2 - 0.6 Ni, 0.03 Se 0.03 300 7.0C
5 34.1 0.9 0.55 - 0.6 Ni, 0.03 Se - - 4.2C
6 34.2 0.9 0.55 0.5 0.6 Ni, 0.03 Se - - 6.3C
7 34.1 0.9 0.55 0.5 0.6 Ni, 0.03 Se 0.03 300 6.8C

• Boron when added as Cu-B master alloy refined yellow brass, EnviroBrass and silicon bronze. It is much more effective
for yellow brass and EnviroBrass III than for silicon bronze.
• FKM 2000, a commercial refiner for yellow brass consisting of fluoride salts of boron and other elements, refined yellow
brass and EnviroBrass III. Interestingly this refiner also had some refining effect on silicon bronze.
• Another commercial refiner, Desofin, in the form of salts, had minimum effect on EnviroBrass III and silicon brass. No
change was observed for yellow brass and silicon bronze.
• The two master alloys containing zirconium were found to be effective only for silicon brass.

Table 7. Effect of various refiners on the macrostructure of different copper alloys

Refiner Yellow EnviroBrass Silicon Silicon


brass III Brass bronze
Base alloy 6C 6.5C 3.5C 7C
Cu-2%B 8C 8C No change 7.5C
FKM 2000 7.5C 8C No change 7.5C
Desofin No change 7.2C 4.5C No change
Cu-50% Zr No change No change 6.8C No change
Cu-9% Zr-9% Mg No Change No change 4.5C No change

From the earlier work with various alloys and grain refiners it is well known that boron refines the yellow brass, boron or
zirconium refines EnviroBrass III depending upon the tin content, and zirconium (added as sponge zirconium) refines the
copper alloys containing silicon (Sadayappan, 1999a). However, it is interesting to note that zirconium when added as master
alloys did not have any effect on EnviroBrass III or silicon bronze. It should be noted that these alloys have very fine grain
structure even before any refiner addition. Another interesting observation is the change in grain size of silicon bronze when
boron was added. All these findings indicate that the macrostructure analysis could not be the final say in the study of grain
refinement and further analysis is needed before coming to a conclusion on the effectiveness of various grain refiners. Hence,
it was decided to do the microstructural analysis to study the grain refinement.

MICROSTRUCTURAL EVALUATION
The microstructure of all the alloys, both in unrefined and grain refined conditions, was analyzed using conventional
metallography techniques. The discussions will be restricted to leaded yellow brass in this paper.

Effect of minor alloy addition


In the first part, the effect of various alloy additions was evaluated followed by the grain refiner addition. The base alloy was
melted in the crucible. Two shrink bar samples were poured. This was followed by addition of 0.3% tin and casting of two
more shrink bar castings. Subsequently, Al and Pb were added. The refiner boron, added as Cu-B master alloy, was added in
steps. Samples were obtained from the bars for macro and micro structural evaluation.

The macro and microstructures obtained from the above experiment on Cu-Zn alloy are shown in figure 3. The
macrostructure is presented in the left column while the corresponding microstructure is shown in the right side. The
macrophotograph shows the cross section of a 19mm round bar. The microstructure is taken at 50 times magnification. The
discussion about each set is given below:

The structures of the base Cu-36% Zn alloy is shown in Figure 3a. The macrostructure reveals a grain size rating between
2C and 3C. The microstructure contains long primary α interconnected dendrites with inter-dendritic mixture of α + β. Both

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macro and micro structures of Cu-Zn alloy were not changed by the tin addition as shown in Figure 3b. The ratings remained
same as well the long dendritic structure.

(a)
Cu-36% Zn

(b)
0.36% Sn

(c)
0.35% Al

(d)
1.4% Pb

Macrostructure (19 mm ∅ bar) Microstructure (50 X)


Figure 3. Macro- and micro- photographs of Cu-Zn alloy modified by various alloy additions

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The effect of aluminum addition is shown in figure 3c. Aluminum reduces the grain size marginally. The macrostructure
reveals a grain size rating between 4C and 5C. The microstructure also modified from a interlocking dendritic structure to a
fine feathery structure.

Lead had a very significant effect on the grain size compared to other minor alloy additions. The grain size rating is between
6C and 7C and the microstructure reveals the very fine feathery structure (Figure 3d). Boron refined this structure further and
much finer structure was obtained with just 40 ppm of boron addition (Figures 3e and 3f). The structure shown in Figure 3f
will have a grain size rating close to 8C. Boron addition beyond this level was found to be detrimental. The macrostructure
did not reveal much when 100 ppm of boron was added but the microstructure revealed some dendrites reappearing in the
midst of fine grain structure as shown in Figure 3g. This aspect of grain coarsening had been already reported in earlier
studies (Sadayappan, 2001).

It is possible to identify the effect of grain refiner quite clearly following microstructural examination. Comparing figures 3d
and 3f the effect of boron could be identified. It was then decided to study the other samples of the leaded yellow brass
refined with zirconium in the second part.

(e)
10 ppm B

(f)
30 ppm B
(total 40 ppm B)

(g)
60 ppm B
(total 100 ppm B)

Macrostructure (19 mm ∅ bar) Microstructure (50 X)


Figure 3. Contd.

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Effect of zirconium
The effect of zirconium addition on the macrostructure of leaded yellow brass, when added as Cu-9Zr-9Mg master alloy, is
presented in Table 8. It should be noted that the zirconium is reported as the level of addition. Also, the levels are cumulative,
not absolute i.e., for the last casting (N1057-5) the addition is 0.006% making the total zirconium as 0.019%. The final
residual zirconium will be lower than these values.

Table 8. Grain size rating of yellow brass refined with zirconium

Specimen # N1057-1 N1057-2 N1057-3 N1057-4 N1057-5


Zr Content, % (addition) 0 0.004 0.008 0.013 0.019
Grain size rating 6C 5.7C 4C 5.8C 6.5C

As shown in this table, the macrostructure did not reveal significant increase in the grain rating indicating no grain refinement
had been achieved with zirconium addition to yellow brass. As before, the microstructures of these alloys were analyzed
(Figure 4).

(a) Base alloy (b) 0.004% Zr addition

(c) 0.013% Zr addition (d) 0.019% Zr addition


Figure 4. Microstructures of zirconium added yellow brass (Cu-36% Zn – 1.5% Pb – 0.3% Sn – 0.4% Al)

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As it can be seen from the microstructures, the grain size of the yellow bras had been reduced even with 0.004% (40 ppm) of
zirconium. This was not evident from the macrostructure. This aspect has not been reported earlier. Further analysis is
required to confirm these results. However, the results from the preliminary evaluation of microstructures are listed in Table
9. The findings are as follows:
• Cu-B has refined yellow brass and EnviroBrass III. The microstructure of silicon brass and silicon bronze did not change
with the addition of Cu-B.
• Zirconium refined all the four alloys, even though the relative effect vary with alloys.
• The microstructures of alloys refined with the commercial refiners FKM 2000 and Desofin are still being analyzed.

Table 9. Grain refinement as evaluated by microstructure

Refiner Yellow EnviroBrass Silicon Silicon


brass III Brass bronze
Cu-2%B Refined Refined Not refined Not refined
Cu-50% Zr Refined Refined Refined Refined
Cu-9% Zr-9% Mg Refined Refined Refined Refined

SUMMARY

1. A scale to measure the grain size of Cu-36% Zn alloy castings has been developed using their macrostructures.
2. Minor alloy additions such as tin, aluminum, lead and bismuth have profound effect on the grain size of Cu-36% Zn
alloy.
3. Aluminum, lead and bismuth reduce the grain size of Cu-Zn alloy. Lead has the most significant effect followed by
bismuth and aluminum.
4. Tin reduces the amount of grain refiner (boron or zirconium) required for the effective grain refinement.
5. Boron refined yellow brass and EnviroBrass III. It was not effective for silicon brass and silicon bronze.
6. Zirconium was fund to be an effective refiners for all the four alloys investigated in this work.

ACKNOWLEDGMENTS

This project was funded by the US Department of Energy under Cast Metal Coalition. The authors are thankful to the
following: American Foundry Society, H. Kramer for silicon brass ingots, Afflips of Belgium for Cu-B and Cu-Zr refiners,
Aula Chemie of Germany for FKM 2000, Staff at Experimental Casting Lab at MTL for melting and casting; and Alan
Powell and J. Thomson for metallography.

REFERENCES
Fasoyinu, F.A., Sadayappan, M., Zavadil, R. and Sahoo, M., "Grain Refinement Of Permanent Mold Cast Yellow Brass",
Proc.Conf., 4th Decennial International Conference on "Solidification Processing - 97", 7-10 July, 1997, Sheffield. UK,
(1997).
Sadayappan, M., Fasoyinu, F.A., and Sahoo, M., “Grain Refinement of Copper Base Alloys”, Presented at Copper-99 -
fourth International Conference, Phoenix, USA, October 10-13, (1999)
Sadayappan, M., Whiting, L.V., Thomson, J., Zavadil, R. and Sahoo, M., “Fading of Grain Refinement in Leaded Yellow
Brass (C85800) and SeBiLOY III (C89550, EnviroBrass III)”, Presented at 105th AFS Casting Congress, Dallas, USA,
(2001)
Sahoo, M., and Davis, K.G., “Grain Refinement in copper-Base alloys- A Literature Review”, MTL Internal Report, MTL-
97-10 (TR-R), (1997)

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