(In-Jin Shon)
1*
Copyright © 2018 The Korean Institute of Metals and Materials
Key words(Korean)
wettability, Al4C3, electric current, aluminum, graphite
1. INTRODUCTION
Graphite fibers have been used extensively as reinforcement materials in polymer and
epoxy based composites due to their excellent properties. These properties include
low density and high strength. The unique properties of graphite fibers also attracted
much attention in the area of aluminum based composite. However, one of the major
drawbacks in fabricating graphite reinforced metal matrix composites (MMCs) is aluminum
generally does not wet graphite. Therefore, it is difficult to impregnate the graphite
fiber with molten aluminum. To solve the difficulty, Oh et al. [1] reported that the wettability of molten Al can be remarkably improved by coating
graphite particles with Cu. In addition, the applications of external electric power
have been recently reported as a promising way to improve the wettability [2]. The effect of an electric current on the wettability of molten Al on graphite has
not been investigated. In this communication, we report the effects of electric current,
density and heating time on wettability, thickness of product (Al4C3) and microstructure.
2. EXPERIMENTAL PROCEDURE
In this study, in order to enhance the wettability of the Al melt on graphite, its
wetting behavior on graphite was observed using the sessile drop test, by which its
wetting angle was measured. Graphite plates were polished using diamond paste, and
then cleaned in ethanol using ultra-sonication. Aluminum ingot (99.999% purity) was
used as a liquid drop material. Figure 1 displays a schematic diagram of the device used for the sessile drop test. To observe
the wetting behavior of Al droplets, the graphite substrate was placed on the alumina
crucible horizontally to the CCD camera. The furnace was evacuated under the vacuum
of 10-5 torr and heated to 1050 ºC at a heating rate of 5 ºC/min. When the temperature reached
to 1050 ºC, a droplet of Al was made to fall onto the graphite substrate. After the
molten Al was dropped, the wetting behavior was captured by a high resolution CCD
camera. The captured images were used to evaluate the contact angle. An electric current
(0, 5, 10 and 15 A) was applied through the molten Al bead and graphite substrate.
In this study, we defined the electric current flowing from an Al droplet to CNT substrate
as the positive current (+), otherwise as the negative current (−). Compositional
and microstructural analyses of the products were conducted through optical microscopy
and electron probe micro-analysis (EPMA).
3. RESULTS AND DISCUSSION
Figure 2 displays the variation of the contact angle (θ) with heating time for molten Al on a graphite substrate during isothermal exposure
at 1050 °C. The wettability of molten Al on graphite without an applied current is
initially poor and the contact angle continuously decreases with heating time due
to formation of Al4C3 [3]. Contact angle decreases markedly with increases of applied currents. The droplet
image during isothermal exposure at 1050 °C for molten Al on graphite substrate without
applied current and with an applied of 5A, 10A and 15A are shown in Fig. 3. Contact angle of molten Al on graphite substrate is decreased with applied electric
current. An applied current may accelerate the wetting of molten Al on graphite and
decrease remarkably the contact angle. Figure 4 shows the optical micrograph of a cross-section perpendicular to the interface of
pure Al on graphite after wetting at 1050 °C, for various electric current. It can
be found that the thickness of the product, which was analyzed as Al4C3 using EPMA, increases with applied current.
Variation of contact angle of molten Al on graphite under the different direction
of current (+10A and -10A) is shown in Fig. 5. The contact angle is considerably reduced with heating time in the case of an applied
negative current of -10 A. Evolution of the droplet image during isothermal exposure
at 1050 °C for molten Al on graphite substrate without and with an applied current
of +10 A are shown in Fig. 6. The direct current direction has an obvious influence on the spreading rate and
contact angle of molten Al on graphite substrate. But Xu et al [4] has reported the contact angle of molten Bi on Cu substrate with an applied positive
current of +2 A is smaller than that with an applied negative current of −2 A. This
result is in opposite with our result.
Figure 7 displays the optical micrograph of a crosssection perpendicular to the interface
of pure Al on graphite after wetting at 1050 °C for 2 h under the electric current
of 10 A. It can be found the thickness of a product, which was analyzed as Al4C3 using EPMA increases with applied current. Figure 8 displays the interaction between carbon and aluminum is thermodynamically feasible.
The contact angle of molten Al on graphite depends on an applied current, a direction
of current and a heating t ime, To understand the variation of wettability, two factors
may be considered. One is the effect of surface energy between molten Al and Al4C3 according to formation of Al4C3 during heating. Unfortunately, surface energy between molten Al and Al4C3 was not reported. However, the interface reaction product (Al4C3) promotes wetting in this study. This behavior matches well with another study [3]. From this result, surface energy between molten Al and Al4C3 may be lower than that of molten Al and graphite. The other would be the role of
heat energy produced from the formation of Al4C3 on the wettability. The temperature of molten Al can increase due to the heat energy
(enthalpy change) according to the equation (2). The calculated adiabatic temperature is 2020 ºC.
Where, ΔHf(Tiq)is formation enthalpy change of Al4C3 at 1050 ºC, Tad is adiabatic temperature, Tig is ignition temperature, and CPs(p) is heat capacity of Al4C3. Surface tension of molten Al continuously decreases with heating temperature [5]. This can enhance wettability of molten Al on graphite. The thickness of the interfacial
reaction layer increases remarkably due to the enhanced diffusivity of the atoms.
This could be related to the electromigration effect [6]. Wettability can be enhanced under an electric current which may be related to the
thickness of the interfacial reaction layer. This means that more heat per time can
be produced. Therefore, the temperature of molten Al, when applying an electric current,
may be higher than that of non-electric field, and wettability can be enhanced under
the electric current.
Figure 9 shows the variation of the contact angle (θ) with heating time for molten Al on a graphite substrate with different relative
density measured using Archimedes method during isothermal exposure at 1050 °C. The
wettability of molten Al on graphite with relative density of 70% is better than that
of graphite with relative density of 100%. The reaction site of molten Al and graphite
to form Al4C3 increases with an increase in porosity. This means that more Al4C3 in graphite of lower relative density can be produced at the same heating time. Figure 10 displays the optical micrograph of a cross-section perpendicular to the interface
of pure Al on graphite with different relative density after wetting at 1050 °C for
1 h. It can be found that the thickness of the product, which was analyzed as Al4C3 using EPMA, is thicker in graphite of lower relative density. More heat per time
can be produced. Therefore, the temperature of molten Al, when applying a low relative
density of graphite, may be higher than that of high relative density of graphite
and wettability can be enhanced under the low relative density.
4. CONCLUSION
The wettability of molten Al on graphite without an applied current is poor, and the
contact angle continuously decreases with heating time. Contact angle of molten Al
on graphite substrate is decreased with applied electric current. An applied current
may accelerate the wetting of molten Al on graphite and decrease the contact angle
considerably. Wettability can be enhanced under an electric current which may be related
to the thickness of the interfacial reaction layer (Al4C3). This means that more heat per time can be produced. The wettability of molten Al
on graphite substrate is better under an applied negative current and with lower relative
density.
Acknowledgements
This work was supported by the KIST Institutional Program (Project No. 2E 26980-17-026)
and this research was supported by Basic Science Research Program though the National
Research Foundation of Korea (NRF) funded by the Ministry of Education (2015R1D1A1A01056600)
and this work was supported by the Korea Institute of Energy Technology Evaluation
and Planning (KETEP) and the Ministry of Trade, Industry & Energy (MOTIE) of the Republic
of Korea (No. 20184030202210).
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Figures
Fig. 1.
Schematic representation of the device used for the sessile drop test.
Fig. 2.
The variation of the contact angle (θ) with time for molten Al on graphite substrate during isothermal exposure at 1050
°C under various electric current.
Fig. 3.
The droplet image during isothermal exposure at 1050 °C for molten Al on graphite
substrate with heating time and electric current : (a) 0A, (b) 5A, (c) 10A and (d)
15A.
Fig. 4.
Optical micrograph of cross-section perpendicular to the interface of pure Al on graphite
after wetting at 1050 °C for 120 min with various electric current.
Fig. 5.
The variation of the contact angle (θ) with time for molten Al on graphite substrate during isothermal exposure at 1050
°C under various electric current.
Fig. 6.
The droplet image during isothermal exposure at 1050 °C for molten Al on graphite
substrate with heating time and electric current : (a) 0A, (b) 10A and (c) -10A.
Fig. 7.
Optical micrograph of cross-section perpendicular to the interface of pure Al on graphite
after wetting at 1050 °C for 120 min with various electric current.
Fig. 8.
Temperature dependence of the Gibbs free energy variation by interaction between 4Al
and 3C.
Fig. 9.
The variation of the contact angle (θ) with time for molten Al on graphite substrate during isothermal exposure at 1050
°C under different relative density of graphite.
Fig. 10.
Optical micrograph of cross-section perpendicular to the interface of pure Al on graphite
after wetting at 1050 °C for 60 min under different relative density of graphite.