o55-thermodynamics and thermophysical properties of liquid...
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Thermodynamics Thermodynamics and and thermophysicalthermophysicalproperties of liquid Bi properties of liquid Bi -- SnSn alloysalloys
Rada NovakovicRada NovakovicDonatella GiurannoDonatella GiurannoEnrica RicciEnrica Ricci
National ResearchCouncil (CNR) – IENIGenoa, Italy
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What kind of input data are necessary for modelling?
1. Phase diagram information
2. Thermodynamic data
3. Thermophysical data
4. Structural data
5. Experimental property data for a comparison with theoretical results
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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1. The Bi-Sn phase diagram
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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Results of calculations
GM/RT≈≈≈≈ 0.6
Bi-Sn is segregating alloy systemalloy system
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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Results of calculations
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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Surface tension measurementsIENI-HTTLabs Equipments
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Surface Tension MeasurementsSurface Tension Measurements
� Measurements by Large drop method
�High purity Tin and Bi (99.9998%)�Ptot ≤ 10-2 Pa + Ta-getter�Alloy sample of about 2.5÷3 g�Check of alloy composition by EDS�Etching + chemical
Preparation of samples
Experimental procedure
� Measurements by Large drop method
� Sapphire crucible
� Atmosphere: Ar-5%H2 Flow rate = 0.25 l/m
� Temperature range : 573-1123 K step 50°
� PO2 ≤10-20 (“oxygen free”) Pa average value in the temperature range
�Real time acquisition of the drop profile by ASTRAview
�10/15 min after the temperature stabilization ( ~ 800 acq /T )
�SEM/EDS analyses on the surface of solidified drop
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Surface tension experimental data
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Effect of temperature on surface tension of Bi, Sn and some of their alloys; the symbols (□)refer to the experimental data of the present work (T = 773, 873, 973, 1073 and 1173 K).
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Table 1 Surface tension together with the corresponding temperature coefficients of binary liquid alloys of the Bi-Sn system. The own surface tension experimental data of liquid Bi and Sn are taken as the reference data.
Composition [at.%]
Bi Sn
Melting temp. [K]
Surface tension at
[mN ⋅⋅⋅⋅m-1]
Surface tension temp. coeff. [mN ⋅⋅⋅⋅m-1⋅⋅⋅⋅K-1]
100 - 544 379.82 -0.083
85 15 510 393.69 -0.073
70 30 475 400.25 -0.061
0σ MTMT
dTdσ
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70 30 475 400.25 -0.061
55 45 440 422.42 -0.061
43 57 412 429.16 -0.060
30 70 440 439.54 -0.046
20 80 461 467.63 -0.044
10 90 482 495.00 -0.043
5 95 494 522.23 -0.045
- 100 505 560.77 -0.063
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Butler(1932):
gives the relation between the surface tension and
bi
si
i
Bi
a
aTkln
ασσ +=
Surface properties of liquid binary alloys: surface tension & surface segregation
gives the relation between the surface tension and thermodynamics of liquids in which the bulk and surface phases are in equilibrium.
& Different solution model
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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Surface tension reference data of Bi
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Surface tension reference data of Sn
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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Results of calculations
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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Results of calculations
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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Microscopic functions (B -T) & Thermodynamics
For ideal solution the S CC(0) becomes
BAidCC ccS =)0(
1
,,
1
,,
1
,,
2
2
)0(−−−
∂∂
=
∂∂
=
∂∂
=NPTB
BBA
NPTA
AAB
NPTA
Mcc C
aaC
C
aaC
C
GRTS
The CSRO parameter and SCC(0) are related to each other by
where Z is the coordination number.
BACC
1
1
)1(1
1)0(
αα−−
+=
Zcc
S
BA
cc
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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Results of calculations
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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The interdiffusion coefficient (Dm) can be given in terms of the S CC(0) by
For “ideal” alloys, S CC(0)= SCC(0,id)= c AcB, then
and finally combining the last two eqs. it is obtai ned,
)0(
)0()( **
CC
idCC
ABBAm S
SDcDcD +=
idABBAABBAm DDcDcDcDcD =+=+= )( **
The criteria for mixing behaviour:SCC(0) > SCC (0, id) segregation ⇒⇒⇒⇒ Dm < Did
SCC(0) < SCC (0, id) presence of chem. order ⇒⇒⇒⇒ Dm > Did
)0(
)0(
CC
idCC
id
m
S
S
D
D=
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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Results of calculations
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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Work in progress
Calculation of the viscosity and electrical resistivity of Bi -Sn melts and resistivity of Bi -Sn melts and comparison with literature data ([0Ple]
*****
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)
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Thank you for your attention!
TOFA 2010 TOFA 2010 -- DISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSDISCUSSION MEETING ON THERMODYNAMICS OF ALLOYSSEPTEMBER 12SEPTEMBER 12--16, 2010 PORTO (PORTUGAL)16, 2010 PORTO (PORTUGAL)