2. similarities between Mg2Si and Si, and between Al–Mg2Si and Al–Si systems from point of
view of properties and solidification behaviour. Figure 1 depicts the equilibrium phase
diagram of Al–Mg2Si [6]. According to Figure 1, during solidification of Al–15%Mg2Si
compound, Mg2Si intermetallic is created as the initial phase. Then, α-Al and secondary
Mg2Si phases simultaneously form from the liquid phase in the ternary phase region. This
pseudo-eutectic reaction is completed at 583.5°C.
The whole reactions from one-phase region of melt to ambient temperature are as
follows:
L ! L1þMg2SiP ! Mg2SiPþ Al þ Mg2Si
E
(1)
where E denotes a eutectic, P refers to a primary and L1 represents a liquid in a two-phase
area.
Some benefits are enumerated for in situ process of production of MMCs, such as
uniform dispersion of second phase, well reinforcement matrix, thermodynamically
stable condition and much lower prices of fabrication compared with their parts from
ex situ processes [7]. Due to coarse primary Mg2Si phase, MMCs reinforced by Mg2Si
usually have weak mechanical properties. It is therefore critical to refine Mg2Si by adding
alloying elements like Sc [8], Ce [9] and Gd [10]. The goal of this research is fabrication of
Al–15%Mg2Si–3%Cu in situ composite and investigation of Cu on the microstructural
and hardness properties.
Figure 1. Pseudo-binary phase diagram of Al–Mg2Si [6].
2 H. RAMEZANALIZADEH AND S. R. IYZI
3. 2. Experimental procedure
The Al–15% Mg2Si–3%Cu composite ingot was produced by using industrially pure
metals (Al, Mg, Si and Cu) as starting materials. All materials were heated in an electrical
resistance furnace using a 6 kg SiC crucible. Due to the importance of elemental loss
during the preparation of the melt, amount of weight loss was selected to be 5, 5, 10 and
15% for Al, Cu, Si and Mg, respectively. Note that the amount of weight loss for Mg
(15%) was due to the high amount of oxidation of this element in the temperature
range used for preparation of the melt. First, pure Al (~2 kg) was melted at 750ƕ
C in
crucible. Then, Si was added to the melt to try to submerge its pieces. After 10 min, Mg
was added to the melt and the solution was hand stirred with a graphite rod for about
1 min to ensure complete mixing. After stirring and cleaning off the dross, molten
MMCs were poured into the cast iron mould (45 mm diameter and 70 mm height,
Figure 2) and left to cool in the air. This sample was considered as base MMC (Cu-free)
sample.
For preparation of Al–15% Mg2Si–3%Cu, after doing the mentioned steps and before
casting, pure Cu (99.99%) was added in small increments to the melt. In addition, 10 min
after Cu addition (3.0 wt.%) the molten MMC was hand stirred for 1 min and finally
poured to mould. For achieving near full density, the cast samples were then subjected to
extrusion procedure in 500ƕ
C and 6:1 ratio. Table 1 shows the chemical composition of
hypereutectic Al–15% Mg2Si-3%Cu in situ (MMCs).
Figure 2. Schematic drawing of cylindrical cast iron mould.
Table 1. Chemical composition of Al–15% Mg2Si–3%Cu (wt.%).
Materials Si Mg Fe Ni Zn Mn Cu Ti Cr
Al–15%Mg2Si 5.71 9.85 0.14 0.01 0.01 0.01 3.1 0.01 0.01
ADVANCES IN MATERIALS AND PROCESSING TECHNOLOGIES 3
4. The sample surfaces from perpendicular section to extrusion direction were selected
for microstructural studies. The cut sections were polished and then etched by HF (1%)
to study the structure. Quantitative data on the microstructures were determined using
an optical microscope equipped with an image analysis system (Clemex Vision Pro.
Ver.3.5.025). Additional microstructural characteristics of the specimens were examined
by scanning electron microscope (SEM) equipped with the energy-dispersive X-ray
analysis (EDX) accessory. Phase composition of samples was also evaluated by X-ray
diffractometer (XRD) (Philips PW-1730) using Cu-Kα radiation.
3. Results and discussion
3.1. Microstructural characterisation
The typical as-cast microstructure of Al–15% Mg2Si composite is shown in Figure 3. It is
clear from the phase diagram (Figure 1) that the composition of the sample is located in
the hyper section of the diagram. This means that the microstructure consisted of
primary Mg2Si particles in a matrix of α-Al and pseudo-eutectic cells (Figure 3). In
addition, according to the quantitative investigations from many pictures like Figure 3,
the size of primary Mg2Si particles was estimated to be almost 20 μm.
Figure 4 shows a SEM picture from microstructure of Al–15% Mg2Si composite. As
seen clearly from this figure, there are three discriminate parts on the base of colour:
dark, grey and bright. As mentioned before, the microstructure of Al–15% Mg2Si
composite consists of primary Mg2Si, α-Al grains in a matrix of Al–Mg2Si eutectic
cells. On the other hand, primary Mg2Si particles will act naturally as heterogeneous
sites for the nucleation of α-Al in order to decrease the interfacial energy [5]. Therefore, it
Figure 3. Optical image of Al–15% Mg2Si composite.
4 H. RAMEZANALIZADEH AND S. R. IYZI
5. could be concluded that the dark faceted particles are primary Mg2Si which is sur-
rounded by a layer of bright α-Al and the grey part is a matrix of Al–Mg2Si eutectic cells.
Figure 5 shows the XRD pattern of the as-cast Al–Mg2Si–Cu composite. The result
reveals that the components of the composite consist of Al, Mg2Si and MgO phases, as
expected. The lack of Cu phases in XRD graph is due to the small amount that XRD
method is unable to characterise them in this condition [11,12].
Figure 4. A backscatter SEM image of Al–15% Mg2Si composite.
Figure 5. XRD pattern of as-cast Al–Mg2Si–Cu composite.
ADVANCES IN MATERIALS AND PROCESSING TECHNOLOGIES 5
6. Figure 6 is a SEM image of MMC containing 3 wt.% Cu. As is clear from this figure,
with the addition of Cu, the microstructural changes were found to be associated with the
formation of new intermetallic phase. To recognise this intermetallic, EDX analysis of the
sample containing 3% Cu was redirected (Figure 6(b)).
Qin et al. [13] have also reported that Cu may have an effect on the relative content of
Mg2Si due to a change in the synchronise equilibrium phase fields. Copper is now used as
a vital alloying element in Al alloys, depending on its amount, and many intermetallic
phases have been reported in the Al–Mg–Si–Cu alloy systems [14]. In addition, Q phase
is the quaternary intermediate phase, which has been given different descriptions and
forms with different stoichiometries [14,15]. Moreover, as shown in Figure 7, it exists in
all three tetrahedrons phase fields. The structure of Q phase is hexagonal type with lattice
parameters of c = 0.405 nm and a = 1.04 nm and 21 atoms in a unit cell [14]. The exact
syntax of Q phase is uncertain. However, it has been defined as Al5Cu2Mg8Si6, Al4CuMg5
Si4, Al4Cu2Mg8Si7 and Al3Cu2Mg9Si7 [14]. Q phase, which formed during solidification,
has a complex honeycomb-type morphology as shown in the backscattered electron SEM
image for a 2014 alloy (Figure 8). It is great to mention that the introduction of Cu to Al–
Mg–Si alloys not only creates the Q phase, but it also develops θ phase (Al2Cu) with
body-centred tetragonal (BCT) structures [14].
3.2. Hardness properties
To study the mechanical properties of Al–15%Mg2Si with addition of 3 wt.% Cu, the
Brinell hardness test was done and measurements showed an 85 HBN amount for
Al–15%Mg2Si–3%Cu, which was more than a 70 HBN level for Al–15%Mg2Si
without Cu. The formation of intermetallics (Q and θ phases) in the microstructure
and its refining is recognised to be an important factor on hardness enhancement. It
should be mentioned that these phases have high hardness and high elastic modulus
values. Therefore, these intermetallics are assumed to be strong reinforcements in
the composite [16–18]. As mentioned earlier, the size of primary Mg2Si particles
decreases by addition of Cu. Lowering the reinforcing particle size at a constant
Figure 6. A backscatter SEM image of Al–15% Mg2Si–3% Cu composite, showing Cu intermetallic
(white colour phase) and (b) corresponding EDX analysis of Cu-containing intermetallic.
6 H. RAMEZANALIZADEH AND S. R. IYZI
7. amount decreases the distance between them. This behaviour is described by
Equation (2). According to this equation, as the reinforcement particle size
decreases, the distance between the particles will also decrease [18].
Figure 7. Line diagram of stable equilibrium phase fields in Al–Mg–Si–Cu system at room temperature
[14].
Figure 8. SEM backscattered electron images of 2014 ingot sample showing the honeycomb-type
structure of the Q phase [14].
ADVANCES IN MATERIALS AND PROCESSING TECHNOLOGIES 7
8. λ ¼
4ð1 f Þr
3f
(2)
where λ is the distance between the reinforcement particles, f is the particle volume
fraction and r is the particle radius, assuming them spherical. In other words, according
to Equation (3) decreasing the distance between the Mg2Si particles will increase the
required tension for dislocations movement between them, leading to an increase in the
composite strength.
τ0 ¼
Gb
λ
(3)
where τ0 is the required tension for forcing dislocations to move among reinforcement
particles, G is the material’s elastic modulus and b is the Berger’s vector [18].
This phenomenon is also explained by the Halle–Petch relationship.
σ0¼σiþKD1=2
(4)
where σo is the flow stress, σi is the stress opposing the movement of dislocations, K is
constant and D is the grain size. According to Equation (4), as the grain size becomes
smaller, flow stress also increases, leading to high strength in the composite [18]. It
should be mentioned that there is a direct relationship between strength and hardness of
a material.
4. Conclusion
Ɣ An Al-based composite containing 15%Mg2Si was fabricated in an in situ manner.
Ɣ The initial microstructures consisted of coarse primary Mg2Si particles (~20 μm)
surrounded by α-Al and pseudo-eutectic cells.
Ɣ Addition of 3 wt.% Cu resulted in Cu-rich intermetallics which could reduce the size
of primary Mg2Si to ~7 μm.
Ɣ The hardness of composite could be improved by addition of Cu.
Disclosure statement
No potential conflict of interest was reported by the author(s).
References
[1] Kumar S, Singh R, Hashmi MSJ. Metal matrix composite: a methodological review. Adv
Mater Proc Technol. 2020;6(1):13–24
[2] Ramezanalizadeh H. On the role of mechanical milling on structural and morphological
features of nano-sized Al3Mg2 powder. Adv Mater Proc Technol. DOI:10.1080/
2374068X.2020.1794229
[3] Ramezanalizadeh H. Effect of milling process on microstructural and properties of a
ball-milled Al-based nanocomposite powder. Adv Mater Proc Technol. DOI:10.1080/
2374068X.2021.1896862
[4] Ramezanalizadeh H. Fabrication and characterization of an Al-based nanocomposite with
high specific strength and good elongation using large amount CMA nanoparticles. J Alloys
Compd. 2020;822:153667.
8 H. RAMEZANALIZADEH AND S. R. IYZI
9. [5] Seth PP, Parkash O, Kumar D. Structure and mechanical behavior of in situ developed Mg2
Si phase in magnesium and aluminum alloys – a review. RSC Adv. 2020;10:37327.
[6] Okamoto H, Schlesinger ME, Mueller EM, editors. ASM handbook volume 3: alloy phase
diagrams. ASM International; 2016.
[7] Wu X-F, Zhang G-G, Wu F-F. Microstructure and dry sliding wear behavior of cast Al–Mg2
Si in-situ metal matrix composite modified by Nd. Rare Met. 2013;32(3):284–289.
[8] Wu X-F, Wang K-Y, Wu F-F, et al. Simultaneous grain refinement and eutectic Mg2Si
modification in hypoeutectic Al-11Mg2Si alloys by Sc addition. J Alloys Compd.
2019;791:402–410.
[9] Shin HC, Son J, Min BK, et al. The effect of Ce on the modification of Mg2Si phases of as-cast
eutectic Mg-Si alloys. J Alloys Compd. 2019;792:59–68.
[10] Wang K-Y, Zhao R-D, Wu F-F, et al. Improving microstructure and mechanical properties
of hypoeutectic Al-Mg2Si alloy by Gd addition. J Alloys Compd. 2020;813:152178.
[11] Cullity BD. Elements of X-ray diffraction. 2nd ed. Addison-esley Publishing; 1977.
[12] Ramezanalizadeh H, Heshmati-Manesh S. Preparation of MoSi2-Al2O3 nano-composite via
MASHS route. Int J Refract Met Hard Mater. 2012;31:210–217.
[13] Qin QD, Zhao YG, Zhou W, et al. Effect of phosphorus on microstructure and growth
manner of primary Mg2Si crystal in Mg2Si/Al composite. Mater Sci Eng A.
2007;447:186–191.
[14] Chakrabarti DJ, Laughlin DE. Phase relations and precipitation in Al–Mg–Si alloys with Cu
additions. Prog Mater Sci. 2004;49:389–410.
[15] Bobel A, Kim K, Wolverton C, et al. Equilibrium composition variation of Q-phase
precipitates in aluminum alloys. Acta Mater. 2017;138:150–160.
[16] Ramezanalizadeh H, Emamy M, Shokouhimehr M. Wear behavior of Al/CMA-type
Al3Mg2 nanocomposites fabricated by mechanical milling and hot extrusion. Tribol
Trans. 2016;59(2):219–228
[17] Ramezanalizadeh H, Emamy M, Shokouhimehr M. A novel aluminum based nanocompo-
site with high strength and good ductility. J Alloys Compd. 2015;649:461–473.
[18] Ramezanalizadeh H, Emamy M. The microstructural revolution of Al-10%Al3Mg2 nano-
composite during mechanical milling. Adv Mater Proc Technol. 2016;2(1):152–164.
ADVANCES IN MATERIALS AND PROCESSING TECHNOLOGIES 9