Volume 8, Issue 6, June – 2023 International Journal of Innovative Science and Research Technology

ISSN No:-2456-2165

Concentration-Concentration Fluctuations and

Chemical Ordering in Liquid Ti-Al Alloy at
Different Temperatures
1* 2
Oreoluwa E. Alade and Temitope E. Ajetomobi
1*
Corresponding Author: Oreoluwa E. Alade

Abstract:- The concentration-concentration fluctuation (having a single phase), heterogeneous (comprising two or
and chemical ordering in liquid Ti-Al at 1773 K, 1873 K, more phases), or intermetallic (characterized by an absence
1973 K, 2073 K, 2173 K, and 2273 K has been of clear phase boundaries) (Abbott, 1980). The process of
investigated using the quasi-chemical approximation alloying involves merging a metal with one or more other
model (QCAM). This analysis shows that chemical elements, either metallic or non-metallic, which typically
ordering leading to complex formation exists in the alloy serves to augment its properties. For instance, steel,
across the whole concentration range. primarily composed of iron, is inherently stronger. While an
alloy's physical properties like density, reactivity, and
I. INTRODUCTION conductivity may not markedly differ from its component
elements, its engineering properties, such as tensile and
Alloys represent combinations of one metal with one shear strength, can vary significantly. Unlike pure metals,
or more additional elements, which could be either metallic most alloys lack a single defined melting point. Instead, they
or non-metallic in nature. Essentially, an alloy emerges exhibit a melting range where the substance transitions
when two or more elements, one of them being metallic, are between solid and liquid states. For most alloys, there exists
melted and fused together. Upon cooling, this blend a specific constituent ratio, referred to as the "eutectic
solidifies into a solid solution, mixture, or an intermetallic mixture," where the alloy exhibits a distinct melting point
compound. Physically disassembling the components of an (Abbott, 1980).
alloy is impossible. Despite potentially containing non-
metals or metalloids, an alloy remains homogeneous and To analyze the alloying behavior of liquid binary
preserves the characteristics of metals. Unalloyed, pure alloys, various compound formation models have been
metals may exhibit certain useful traits, like superior proposed (Singh and March 1995). These models encompass
electrical conductivity, resistance to heat and corrosion, or the Quasi-Chemical Approximation Model (QCAM), Self-
impressive strength and hardness. Association Model (SAM), and Complex Formation Model
(CFM). The selection of Aluminum-Titanium (Al-Ti) as the
Additionally, it's been noted that unalloyed metals focus of our study is spurred by recent predictions of
contain a uniform crystalline structure at the atomic level, thermodynamic data for liquid Al-Ti at varying
stacking layer after layer of identical atoms. However, these temperatures, using the FactSage thermochemical software
layers tend to slide past each other with ease, often making and database. The FactSage suite comprises several
the metal too malleable for practical applications. Take pure informational, database, computational, and manipulative
gold, for example, it's seldom used in jewelry since it's too modules, enabling access and manipulation of pure
delicate to endure much wear and tear. Nevertheless, substances and solution databases as developed by Kostov
introducing an element with a distinct atomic size can and team (2006).
disrupt the layers at random, reducing their propensity to
slide and resulting in a harder alloy. Furthermore, the For this project, we've chosen the Quasi-Chemical
judicious selection of compounds permits metallurgists to Approximation Model (QCAM) to investigate the energetics
custom design other attributes like resistance to corrosion of chemical ordering and temperature effects on Titanium-
and the melting point (Bell, 2019; Lim, 2016). Aluminium (Ti-Al) liquid alloys at various temperatures for
which we have experimental data. Both aluminum and
Alloys are commonly categorized as either titanium have a multitude of significant industrial
substitutional or interstitial, a classification dependent on applications. Aluminium is integrated into a vast array of
their atomic arrangements. In substitutional alloys, the products, including cans, foils, kitchenware, window frames,
atoms from each element can substitute for their counterpart and components of doors and airplanes. Titanium, another
in the crystal lattice, whereas, in interstitial alloys, these well-known metal, finds its use in products such as jewelry,
atoms fill the spaces between the atoms of the host metal. tennis rackets, goalkeeper masks, scissors, bicycle frames,
Further classifications of alloys can include homogeneous surgical tools, and mobile phones. The Ti-Al liquid binary

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Volume 8, Issue 6, June – 2023 International Journal of Innovative Science and Research Technology
ISSN No:-2456-2165
alloy possesses extensive applications in science and II. METHODOLOGY
engineering fields. Particularly, Ti-Al alloys exhibit
potential for supplanting heavier materials in high-  Description of Quasi-Chemical Approximation
temperature structural applications, such as automotive and The Quasi-Chemical Approximation provides a
aerospace engine components (Kassner, 2015). simplified framework for examining liquid alloys. It
predicates on the assumption of like-atom pairing at
The primary objectives of this project are twofold. equivalent sites that have short-ranged interactions between
Firstly, we aim to ascertain the concentration-concentration nearest neighbors. Such pairing engenders the formation of
fluctuations and chemical ordering in liquid Titanium- self-associates within the alloys. A liquid binary A-B alloy
Aluminum (Ti-Al) alloys at varying temperatures and comprises 𝑁𝐴 atoms of element A and 𝑁𝐵 atoms of element
compare the derived results with corresponding B, which collectively form like-atom clusters or self-
experimental data. The activity of Al and Ti as a function of associates of type μA and υB. Here, μ and υ represent the
titanium concentration was calculated in the temperature number of atoms in the clusters within type A and B
range between 1773 K and 2273 K. Secondly, we intend to matrices, respectively. Leveraging this assumption,
employ the Quasi-Chemical Approximation Model (QCAM) expressions for thermodynamic and microscopic functions
to compute the thermodynamic activities of these binary are derived for binary liquid alloys (Koirala et al, 2013).
alloys. The effectiveness of the model will be further
evaluated by juxtaposing the calculated outcomes with The grand partition function, Ξ of a binary molten
experimental data. alloys AB, which consist of NA = 𝑁𝑐 and NB = 𝑁(1 − 𝑐)
atoms of elements A and B, respectively where the total
number of atoms N can be expressed as

Ξ =∑E(qA (T)NA (𝑞𝐵 (𝑇))𝑁𝐵 𝑒𝑥𝑝⦋ 𝜇𝐴 𝑁𝐴 + 𝜇𝐵 𝑁𝐵 − 𝐸⦌/𝐾𝐵 T ……………………………………………………………..……...(1)

where qNi (𝑇)𝑎𝑛𝑑 𝜇𝑖 are atomic partion function and chemical of ith component (i=A,B), 𝐾𝐵 is the Boltzmann’s constant, T
is the absolute temperature and 𝐸 is the configurational energy of all alloy.

After some little algbera, (Prasad et al, 1998), the solution of (1) is given as the ratio of the activity coefficient γ (γ = γA/γB);
γA and γsB are activity coefficients of A and B atoms, respectively for the compound (Aμ Bμ ) forming alloys such as

z(1−C) β+2c−1
ln γ = 2C
.β−2C+1 ………………………………………………………………………………………......……………………(2)

with
1⁄
β = [1 + 4C(1 − C)(η2 − 1)] 2 …………………………………………………………………………………………..………..(3)

2𝜔
η2 = exp (2𝑘 𝑇) exp(2PAB ∆εAB - PAA ∆εAA - PBB ∆εBB/ 𝐾𝐵 𝑇) ……………………………………………………………..……..(4)
𝐵

and the interchange or ordered energy, ω is expressed as

1
ω = Z⦋∆εAE - 2( ∆εAA + ∆εBB )⦌……………………………………………………………………………………………………(5)

∆εAB, ∆εAA and ∆εBB are the interaction parameter and ∆εij is the change in the energy of ij bond in the complex Aμ , Bv , Pij
is the probability that ij bond is apart of the complex.

Pij may be expressed as

PAB = Cµ-1(1 – c )ν-1[2 - Cµ-1( 1 – c )v-1] ……………………………………………………………………………………………..(6)

PAA = Cµ-2(1 – c)ν[2 - Cµ-2(1 – c )ν ], µ ≥ 2 ………………………………………………………………………………………….(7)

PBB = Cµ(1 – c )ν-2[2 - Cµ(1 – c )ν-2], ν ≥ 2 ………………………………………………………………………...........…………..(8)

xs
From which we can get an expression for the excess Gibbs free energy of mixing GM defined by
xs
GM = Gm - RT [c lnc + (1 – c )ln(1 – c )] …………………………………………………………………………………..………(9)

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Volume 8, Issue 6, June – 2023 International Journal of Innovative Science and Research Technology
ISSN No:-2456-2165
xs
Gm being the free energy of mixing. GM can be obtained from (2) by using the thermodynamic relationship Bhatia et al,(1982).
x
GMS 𝑐
RT
=Z∫0 ⦋In σ + (2𝐾𝐵 𝑇) − 1 ( PAA∆εAA − PBB ∆εBB)⦌dx+𝛷 …………………………………………………………..…….(10)

Here, Z is the coordination number, c is the concentration of atom A and R is the universal gas constant and

1 (1−C)(β+2c−1)
In σ = 2 In C(β−2c+1)
…………………………………………………………………………………………………………...(11)

xs
The constant 𝛷 in Eq (10) is determined from the requirement that GM = 0 at c =0 and 1

 Concentration Fluctuation and Chemical Short Range Order

The concentration-concentration fluctuations in the long wavelength limit scc (0) alongside the Warren-Cowley short-range
order parameter (α1 ) are instrumental properties that provide valuable insights into the structural characteristics of molten alloys.
Scc(0) indicates nature of chemical ordering and α1 represents the degree of ordering in the melt. The standard relation for
concentration fluctuation in long wavelength limit (scc (0)) for binary liquid alloys(Zhang et al, 2001).
−1
𝜕 2 𝐺𝑀 ∂aA −1
scc (0) = 𝑅𝑇 ( 2
) = CB aA( ) = CAaB[ ∂a B/ ∂(1-CA)]−1
T⋅P⋅N ………………………………………………………….(12)
𝜕𝐶ᴀ 𝑇⋅𝑃⋅𝑁 ∂CA T⋅p⋅N

For ideal mixing the energy parameters, ω given in (5) is equal to zero and (12) becomes

id (0)
scc = CACB …………….…………………………………………………………………………………......……………..(13)

C(1−C)
scc (0) = 1 ………………………………………………………………………………………...………………………(14)
1+z∕2( −1)
B

(12) is usually utilized to obtain the experimental values of scc (0) from the measured activity or free energy of mixing data.
id (0)
The moxing behaviour of liquid binary alloys can be inferred from the deviation of scc (0) from scc . The presence of chemical
id id
order is indicated by scc (0) < scc (0); on the contray, if scc (0) > scc (0), the segregation and demixing in liquid alloys take
place. The Warren-Cowley short-range order parameter, denoted as α1 , can further provide insights into the local arrangement of
atoms in molten alloys. This parameter, α1 , can be expressed in terms of the β-function (3), allowing a deeper understanding of
the atomic organization within these alloys.

The chemical short-range order parameter is given as

β−1
α1 = …………………………………………………………………………………………………………………….………(15)
β+I

The diffusion coefficient is another valuable tool leveraged by both theoreticians and experimentalists to extract information
about the composition and characteristics of liquid alloys. The interdiffusion coefficient (DM) of binary alloys can be expressed in
terms of activity (ai) and self-diffusion coefficient (Di) of pure component with the help of Darken’s equation:
𝜕𝐼𝑛𝑎𝐴
DM = Ds 𝜕𝑐
…………………………………………………………………………………………...………………………....(16)

With
…...
Ds = ∑CiDi ………………………………………………………………………………………………………………………...(17)

If we apply Eq. (12) in Eq. (16), we obtain an expression for DM in terms of Scc(0), i.e.
Dm C C
Ds
= s A (0)
B
CC

id (0), id (0),
For ideal mixing, sCC (0) ⟶ scc i.e Dm⟶ Ds ; for odered alloys, sCC (0) < scc i.e DM > Ds and similarily for
segregation, DM < Ds .

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Volume 8, Issue 6, June – 2023 International Journal of Innovative Science and Research Technology
ISSN No:-2456-2165
III. RESULTS AND DISCUSSION

The quasi-chemical approximation model was applied to calculate Gibbs free energy of mixing Gm, concentration–
concentration fluctuation scc (0), calculated activity Ca, diffusion co-efficient DM , chemical short range order parameter α1 .
Experimental data were taken from (Kostov et al, 2006). The two alloy and their working temperature present in Table 1

Table 1 Activity of Ti And Al in the Temperature Range from 1773 K to 2273 K

1773 K 18873 K 1973 K
𝐗 𝐓𝐢 𝐚𝐓𝐢 𝐚𝐀 𝐥 𝐚𝐓𝐢 𝐚𝐀 𝐥 𝐚𝐓𝐢 𝐚𝐀 𝐥

0 0 1 0 1 0 1
0.1 0.015141 0.91191 0.020727 0.91426 0.027485 0.91637
0.2 0.032151 0.79919 0.041609 0.80936 0.052499 0.81860
0.3 0.064489 0.63285 0.078649 0.65378 0.094007 0.67319
0.4 0.12757 0.43767 0.14703 0.46617 0.16703 0.49335
0.5 0.23813 0.26243 0.26123 0.29103 0.28389 0.31938
0.6 0.40118 0.13875 0.42316 0.16141 0.44393 0.18492
0.7 0.59423 0.066993 0.60958 0.082052 0.62371 0.098450
0.8 0.77232 0.030590 0.77915 0.039369 0.78535 0.049389
0.9 0.90274 0.012534 0.90404 0.016800 0.90521 0.021859
1 1 0 0 0 1 0

2073K 2173K 2273K

𝐗 𝐓𝐢 𝐚𝐓𝐢 𝐚𝐀 𝐥 𝐚𝐓𝐢 𝐚𝐀 𝐥 𝐚𝐓𝐢 𝐚𝐀 𝐥

0 0 1 0 1 0 1
0.1 0.0355467 0.91829 0.044707 0.92003 0.055217 0.92163
0.2 0.064677 0.82705 0.078218 0.83479 0.093026 0.84191
0.3 0.11045 0.69121 0.12785 0.70800 0.14610 0.72366
0.4 0.18743 0.51928 0.20810 0.5400 0.22893 0.56756
0.5 0.30605 0.34737 0.32767 0.37489 0.34872 0.40190
0.6 0.46358 0.20910 0.48218 0.23377 0.49978 0.25880
0.7 0.63676 0.11607 0.64885 0.13478 0.66007 0.15446
0.8 0.79099 0.060617 0.79615 0.073008 0.80088 0.086505
0.9 0.90627 0.027728 0.90724 0.034412 0.90812 0.041902
1 1 0 1 0 1 0

 Gibbs Free Energy Of Mixing 𝐺𝑚

Using equation (9) we calculated the Gibbs free energy
of mixing for Ti-Al liquid alloy at temperatures of 1773 K,
1873 K, 1973 K, 2073 K, 2173 K, 2273 K respectively.
Figures 1.1-1.6 shows the plots of the concentration
dependence of free energy of mixing at different
temperatures. These figures show that our interaction
parameters give a good representation of the calculated
values of free energy of mixing for Ti-Al alloys at
respectively temperatures.

Fig 1 Gibbs Free Energy of Mixing GM, Versus

Concentration of Ti-Al At 1773 K. The Solid Line
Represents Calculated Values for Ti-Al Alloy. CAl Is the Al
Concentration in the Alloy.

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Volume 8, Issue 6, June – 2023 International Journal of Innovative Science and Research Technology
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Fig 2 Gibbs Free Energy of Mixing GM Versus Fig 5 Gibbs Free Energy of Mixing GM Verse
Concentration of Ti-Al At 1873 K. The Solid Line Concentration of Ti-Al At 2173 K. The Solid Line
Represents Calculated Values. CAl Is Concentration in the Represents Calculated Values. CAl Is Concentration in the
Alloy. Alloy.

Fig 3 Gibbs Free Energy of Mixing GM Versus

Concentration of Ti-Al At 1973 K. The Solid Line
Represents Calculated Values. CAl Is Concentration In The Fig 6 Gibbs Free Energy of Mixing GM Verse Concentration
Alloy. of Ti-Al At 2273 K. The Solid Line Represents Calculated
Values. CAl Is Concentration in the Alloy.

 Concentration-Concentration Fluctuations, 𝑠𝐶𝐶 (0)

From accurate analysis of the nature of ordering in Ti-
Al liquid alloys, the first quantity investigated is the
concentration- concentration fluctuation in the long
wavelength limit sCC (0). The deviation of the sCC (0) from
id (0)
the ideal sCC is an essential parameters in order to
visualize the nature of ordering in liquid alloy. The results
are shown in figures 1.7- 1.12. From the figure, it is clear
id (0)
that calculated sCC (0) < sCC at the six temperatures
investigated. This implies there is tendency for unlike atoms
in the liquid Ti-Al alloys to come together and form
chemical compounds. That’s Ti-Al alloy is a compound
forming alloys. The degree of compound forming in the
liquid Ti-Al alloys does not change much with increasing
temperature from 1773 K to 2273 K. However, the Gm
suggest that the degree of interaction between the
component atoms of the decrease with increase in
Fig 4 Gibbs Free Energy of Mixing GM Verse Concentration temperature. That’s Ti-Al alloys at 1773 K is more
Ti-Al At 2073 K. The Solid Line Represents Calculated interacting than at 1873 K and in that order.
Values. CAl Is Concentration in the Alloy.

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Volume 8, Issue 6, June – 2023 International Journal of Innovative Science and Research Technology
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Fig 7 Concentration-Concentration Fluctuation SCC (0)

Fig 10 Concentration-Concentration Fluctuation SCC (0)
Versus Concentration at 1773 K, for Liquid Ti-Al Alloy.
Versus Concentration At 2073 K, for Liquid Ti-Al Alloy.
The Red Line Represents Ideal Values, the Blue Line
The Red Line Represents Ideal Values, the Blue Line
Represents Theoretical Values and the Circle Represents
Represents Theoretical Values and the Circle Represents
Experimental Values.
Experimental Values.

Fig 8 Concentration-Concentration Fluctuation SCC (0) Fig 11 Concentration-Concentration Fluctuation SCC (0)
Versus Concentration at 1873 K, for Liquid Ti-Al Alloy. Versus Concentration at 2173 K, for Liquid Ti-Al Alloy.
The Red Line Represents Ideal Values, the Blue Line The Red Line Represents Ideal Values,tThe Blue Line
Represents Theoretical Values and the Circle Represents Represents Theoretical Values and the Circle Represents
Experimental Values. Experimental Values.

Fig 9 Concentration-Concentration Fluctuation SCC (0) Fig 12 Concentration-Concentration Fluctuation SCC (0)
Versus Concentration at 1973 K, for Liquid Ti-Al Alloy. Versus Concentration at 2273 K, for Liquid Ti-Al Alloy.
The Red Line Represents Ideal Values, the Blue Line The Red Line Represents Ideal Values, the Blue Line
Represents Theoretical Values and the Circle Represents Represents Theoretical Values and the Circle Represents
Experimental Values. Experimental Values.

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Volume 8, Issue 6, June – 2023 International Journal of Innovative Science and Research Technology
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 Activity Coefficient (Ln Γ)
Using equation (2) we calculated the activity
coefficient for liquid Ti-Al alloys at temperatures of 1773 K
– 2273 K. The aluminium activity shows a negative
deviation from Raoult’s law while the titanium shows a
positive deviation from Raoult’s law. At 0.2 from the
negative side of the concentration, there was a positive shift,
and at 0.8 from the positive side of the concentration, there
was a positive shift.

Fig 16 Calculated Activities of Compounds in Lliquid Ti-Al

Alloys at 2073 K Verse the Concentration of Al.

Fig 13 Calculated Activities of Compounds in Liquid Ti-Al

Alloys at 1773 K Verse the Concentration of Al

Fig 17 Calculated Activities of Compounds in Liquid Ti-Al

Alloys at 2173 K Verse the Concentration Of Al.

Fig 14 Calculated Activities of Compounds in Liquid Ti-Al

Alloys at 1873 K Verse the Concentration of Al

aAl aAl

Fig 18 Calculated Activities of Compounds in Liquid Ti-Al

Fig 15 Calculated Activities of Compounds in Liquid Ti-Al
Alloys at 2273 K Verse the Concentration of Al.
Alloys at 1973 K Verse the Concentration of Al.

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Volume 8, Issue 6, June – 2023 International Journal of Innovative Science and Research Technology
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 Diffusion Coefficient 𝐷𝑀
Using equation (16) we calculated the diffusion
coefficient for liquid Ti-Al alloys at temperatures of 1773
K- 2273 K respectively. The result are shown in Fig. 1.13 to
Fig. 1.18. It can be deduced from the figure that the
diffusion coefficient of liquid Ti-Al alloys are greater than
unity ˃ 1, which suggests the presence of compound
formation in the liquid Ti-Al alloys.

D
Fig 22 Diffusion Coefficient DM Verse Concentration at
Id
2073 K. The Blue Line Represents Calculated Values. CAl Is
Concentration in the Alloy.

D
Fig 19 Diffusion Coefficient DM Verse Concentration at
Id
1773 K. The Solid Line Represents Calculated Values. CAl
Is Concentration in the Alloy.

D
Fig 23 Diffusion Coefficient DM Verse Concentration at
Id
2173 K. The Blue Line Represents Calculated Values. CAl Is
Concentration in the Alloy.
D
Fig 20 Diffusion Coefficient DM Verse Concentration at
Id
1873 K. The Blue Line Represents Experimental Values. CAl
Is Concentration in the Alloy.

D
Fig 21 Diffusion Coefficient DM Verse Concentration at DM
Id Fig 24 Diffusion Coefficient Verse Concentration at
DId
1973 K. The Blue Line Represents Calculated Values. CAl Is
Concentration in the Alloy. 2273 K. The Blue Line Represent Calculated Values. CAl Is
Concentration in the Alloy.

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Volume 8, Issue 6, June – 2023 International Journal of Innovative Science and Research Technology
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 Chemical Short-Range-Order Parameter 𝛼1
Equation (15) was used to obtained the Warren-
Cowley chemical short-range order parameter (α1 ). The plot
of this parameter versus concentration are presented in
figure 4.19-4.24. The negative values of α1 over the whole
concentration range indicates the degree of ordering in Ti-Al
alloys. Chemical short-range order α1 is much less than 1 in
Ti-Al alloys at respective temperatures.

Fig 28 Chemical Short-Range Order 𝛼1 Parameter Versus

Concentration for Liquid Ti-Al Alloys at 2073 K

Fig 25 Chemical Short-Range Order Parameter Versus

Concentration for Liquid Ti-Al Alloys at 1773 K

Fig 29 Chemical Short-Range Order Parameter Versus

Concentration for Liquid Ti-Al Alloys at 2173 K
Fig 26 Chemical Short-Range Order Parameter Versus
Concentration for Liquid Ti-Al Alloys at 1873 K.

Fig 27 Chemical Short-Range Order Parameter Versus

Concentration for Liquid Ti-Al Alloys at 1973 K Fig 30 Chemical Short-Range Order Parameter Versus
Concentration for Liquid Ti-Al Alloys at 2273 K

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Volume 8, Issue 6, June – 2023 International Journal of Innovative Science and Research Technology
ISSN No:-2456-2165
IV. CONCLUSION [9]. Chemistry of Liquids : An International
Thermodynamic Properties of Compound Forming
This is a theoretical approach for the determination of Bhatia, A. B., & Singh, R. N. (n.d.) (1982). Physics
the concentration – concentration fluctuation and chemical and Molten Alloys in a Weak Interaction
ordering in Ti-Al alloy at 1773 K, 1873 K, 1973 K, 2073 K, Approximation. January 2015, 37–41.
2173 K, and 2273 K. The quasi-chemical model (QCAM) https://doi.org/10.1080/00319108208080755
was used for the prediction of this work at the temperatures [10]. Bell, T. (2019), Metal Alloys Explained. Retrieved
listed above with special emphasis on Gibbs free energy of November 1, 2019, from The balance
mixing Gm, concentration- concentration fluctuation in the https://www.thebalance.com/metals-alloys-2340254
long-wavelength and scc (0) , chemical short-range order [11]. Lim, X. (2016). Metal Mixology, Nature, 533,306-307.
parameter α1 , diffusion co-efficient DM and activity [12]. Odusote, Y. A. (2007). Bulk and dynamic properties in
coefficient (ln γ). Al – Zn and Bi – In liquid alloys using a theoretical
model. 353, 1167–1171.
The negative deviation from Raoult’s law is noticed https://doi.org/10.1016/j.jnoncrysol.2006.12.023
which indicates a noticeable tendency for chemical ordering
in Ti-Al liquid alloys across the whole concentration range.

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