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Study of Dissolution Process of Solid Cu in Liquid Al

  • Shuying Chen , Yang Wu EMAIL logo , Guowei Chang , Changxu Zhu and Qingchun Li
Published/Copyright: October 21, 2015
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High Temperature Materials and Processes
From the journal High Temperature Materials and Processes Volume 35 Issue 8

Abstract

The dissolution process of solid Cu in liquid Al influences the compound quality directly when fabricating the copper cladding aluminum (CCA) composite castings utilizing the casting aluminum method. Dissolution rate of solid Cu is investigated utilizing the method of quenching rapidly. Effects of liquid Al temperature and the contact time between solid Cu and liquid Al on the dissolution rate of Cu are investigated; meanwhile, the dissolution mechanism of Cu is explored. Subsequently, the influences of processing parameters on the dissolution thickness of Cu are examined. The results indicate that chemical compounds, such as AlCu2, Cu5Al, CuAl2 and Cu2Al3, may form on the contact surface between solid Cu and liquid Al. These chemical compounds are contributed to decompose the solid Cu, Cu5Al exerts the greatest effect. The dissolution of Cu is affected by the contact time between solid Cu and liquid Al, temperature and cooling method of Cu plate. The dissolution of Cu cannot terminate immediately even though the Cu plate is cooled by the spray. The experimental results will provide a reference for controlling the composite layer thickness.

Keywords: Cu/Al composite; dissolution rate; dissolution mechanism; processing parameters

Introduction

Copper cladding aluminum (CCA) composite preparation requires metallurgical bonding between Cu and Al. Preparation methods are divided into two parts to achieve metallurgical bonding: before plastic working and after plastic working.

For realizing the metallurgical bonding before plastic working, Al liquid must contact solid Cu to allow dissolution of the copper surface and formation of copper-aluminum alloy or aluminum-copper alloy between solid Cu and liquid Al, and then the metallurgical bonding is realized after solidification [1–7]. For obtaining the metallurgical bonding after plastic working, first, the Cu is wrapped on the surface of Al to realize the mechanical bonding, and then a transition layer between Cu and Al forms as a result of Cu and Al atoms diffusing during a heat treatment process, and the aim of metallurgical bonding is achieved [8–15].

The preparation methods of the CCA composite are widely explored by the researchers, in the meantime, the formation of the transition layer of CCA composite, the structure composition and the mechanical properties of the composite layer are also researched [1–5, 6–18]. In order to study the composite transition layer specially, the method that liquid Al contacts with solid Cu for a long time is utilized to make Al atoms permeate into solid Cu. The influences of the temperature, time, cooling ways and intensive magnetic field on the transition layer are obtained [16–18]. This lays a solid foundation for controlling Cu and Al composite process.

Past research results indicate that the transition layer thickness of the CCA composite plays a decisive role on the bonding strength [1, 4, 5, 9, 12, 13, 19–21]. The transition layer thickness depends on the temperature and action time between liquid Al and solid Cu for liquid Al and solid Cu composite method. It is important for controlling the transition layer thickness to find out the dissolution rate of Cu in liquid Al. Therefore, the dissolution rate of solid Cu in liquid Al, the influences of related factors, and the dissolution mechanism of Cu are investigated in this study.

Experimental procedures

The solid Al (140 g, 99.99 wt%) is put into the graphite crucible, after the crucible is heated to 1,023 K in the resistance furnace, the liquid Al is degassed and refined with the Cl2C6. The Cu block (26 g, 99.99 wt%) with the dimensions of 25 mm×20 mm×6 mm is shined to remove the oxide skin, then it is put into the liquid Al rapidly for 60 s, 120 s, 180 s and 240 s, respectively. The liquid Al containing the Cu plate is then poured into water to cool. Diluted hydrochloric acid is applied to dissolve the Al remaining on the Cu plate, the partially dissolved Cu block is weighed. The dissolution speed of Cu vw (g.s−1) is then obtained. Supposing the surface of Cu block is dissolved uniformity, the translational speed v (μm.s−1) from the Cu surface to the Cu inner can be calculated according to the dissolved quantity of Cu.

The CCA composite casting is prepared according to the method presented in Figure 1 where the size of the cast cavity is lAl×60×80 mm, lAl is the thickness of Al in the casting, equaling 30 mm, 40 mm and 50 mm, respectively and the casting temperature of Al is 973 K. The cooling fashions of exterior surface of Cu plate include the natural cooling, wind cooling and spray cooling after casting. The inside surface cooling curve of Cu plate is measured by a thermal couple. The vertical section of the casting is polished, and the dissolved thickness of Cu plate is measured in the photograph.

Figure 1: Compounding methods of solid Cu and liquid Al a, covering agent for thermal retardation; b, cooler; c, thermal couple; d, Cu plate; e, sand mold; f, liquid Al; g, covering material; lCu and lAl are the thickness of Cu and Al, respectively.
Figure 1:

Compounding methods of solid Cu and liquid Al a, covering agent for thermal retardation; b, cooler; c, thermal couple; d, Cu plate; e, sand mold; f, liquid Al; g, covering material; lCu and lAl are the thickness of Cu and Al, respectively.

Experimental results

Dissolution rate of Cu in Al liquid

Figure 2 illustrates the influences of the time of solid Cu (~26 g) in the liquid Al (~140 g) and liquid Al temperature on the dissolving speed of solid Cu. In this figure, the dissolved quantity of solid Cu is the measured value and the dissolving speed is the calculated value.

Figure 2: Impacts of time and temperature on the dissolved quantity and the dissolved speed of Cu (a) Temperature of Al is 973 K (b) Contact time of Cu and Al is 120s △w – dissolved quantity of Cu, v – translational speed from the Cu surface to Cu inner, vw – dissolved speed of Cu, t – time, T-temperature.
Figure 2:

Impacts of time and temperature on the dissolved quantity and the dissolved speed of Cu (a) Temperature of Al is 973 K (b) Contact time of Cu and Al is 120s △w – dissolved quantity of Cu, v – translational speed from the Cu surface to Cu inner, vw – dissolved speed of Cu, t – time, T-temperature.

When the temperature of Al T=973 K, the dissolved quantity of Cu increases continuously, while the dissolution rate is fast at first and then slow with extended time (Figure 2(a)). When the time is extended to 180 s, the dissolution speed reaches the maximum value. After that, the speed begins to decline. The average dissolution rate of Cu attains 0.086 g/s within 180 s, indicating the dissolved speed of solid Cu is rapid in liquid Al. In other words, solid Cu rapid dissolution in liquid Al occurs within 200 s.

When the solid Cu is held in liquid Al for 120 s (Figure 2(b)), the dissolution rate of solid Cu accelerates with increasing the temperature of liquid Al, while when the temperature of liquid Al exceeds 1,070 K, the dissolution speed of solid Cu increases sharply from 0.084 g/s to 0.15 g/s. When the temperature exceeds 1,070 K, the dissolution speed of Cu increases linearly with the increase of temperature.

Distribution of the dissolved Cu in Al liquid

The CCA casting is prepared with liquid Al temperature T=973 K, holding time t=120s, and water cooling. The distributions of Cu and Al on two sides of Cu/Al bonding interface are shown in Figure 3. The distribution rules of Cu and Al are in accordance with the results of past research [1, 5, 16] (Figure 3(c)). An aluminum-containing layer is observed within the solid Cu with thickness is δp. Su et al. [5] consider that the formation of δp is the result of Al atoms diffusing into Cu after solidification. Al atoms diffusing into Cu after the solidification is not possible in this study with the accelerated cooling rate, thus δp formation was determined to occur during the process of solid Cu dissolving in liquid Al. Surface atoms of Cu dissolve into liquid Al then allowing Al atoms to dissolve into Cu, affecting the dissolution of Cu. The content of Cu at point A, as indicated in Figure 3(c), is relatively low at approximately 46% (atomic percent) according to EDS point analysis. Analysis suggests that the liquid will flow severely during the process of pouring liquid Al containing Cu into the water, leading the Cu concentration to decrease on the Cu/Al interface.

Figure 3: Distributions of Cu and Al on the two sides of Cu/Al bonding interface a-line scanning results of Al, b-line scanning results of Cu, c-distributions of Cu and Al, δp-thickness of aluminum-containing layer in solid copper.
Figure 3:

Distributions of Cu and Al on the two sides of Cu/Al bonding interface a-line scanning results of Al, b-line scanning results of Cu, c-distributions of Cu and Al, δp-thickness of aluminum-containing layer in solid copper.

Dissolution layer of Cu plate in CCA castings

A adjustment in the copper-aluminum ratio of the CCA castings assumes value of lCu/lAl is 4/30, 4/40, and 4/50, respectively. The casting temperature of Al is 973 K and remains for 100 s after casting, after that the copper plate outside surface is treated with the spray cooling, wind cooling and natural cooling, respectively. The vertical sections of CCA castings photographs are presented in Figure 4.

Figure 4: Vertical section photographs of CCA composite castings a, c, e, lCu/lAl=4/30; b, d, f, lCu/lAl=4/50 a, b: Spray cooling; c, d: Wind cooling; e, f: Natural cooling.
Figure 4:

Vertical section photographs of CCA composite castings a, c, e, lCu/lAl=4/30; b, d, f, lCu/lAl=4/50 a, b: Spray cooling; c, d: Wind cooling; e, f: Natural cooling.

Observing the shapes of Cu/Al bonding interface, as the white imaginary line shown in Figure 4, it is found that the interface shapes turn from a flat interface to flexure plane when the surface of Cu plate is cooled with the spray cooling, wind cooling and natural cooling, respectively, with higher rapid cooling speeds creating more straight interfaces.

The dissolution thickness of the Cu plate is gained by measuring the distance from the black two-dot line to the white imaginary line shown in Figure 4(a) through (f) (Figure (5)). When the cooling fashion is consistent, the smaller the lCu/lAl value, the thicker the dissolved thickness, while when the lCu/lAl value is equal, the faster the cooling rate, the thinner the dissolved thickness.

Figure 5: Average dissolved thickness of copper plate δ0 – initial dissolved thickness; δ1, δ2, δ3 – redissolved thickness after spray cooling, wind cooling and natural cooling.
Figure 5:

Average dissolved thickness of copper plate δ0 – initial dissolved thickness; δ1, δ2, δ3 – redissolved thickness after spray cooling, wind cooling and natural cooling.

The dissolved thickness of Cu δ0 is approximately 0.76 mm by calculating according to Figure 2(a), with the casting temperature of Al of 973 K and remaining for 100 s after casting. Compared with δ0, when the surface of Cu plate is cooled with the spray and the lCu/lAl value is 4/30, 4/40 and 4/50, respectively, the re-dissolved thickness of Cu plate (δ1, δ2, δ3) is 0.17 mm, 0.36 mm and 0.65 mm, respectively an the re-dissolved thickness of Cu plate (δ1, δ2, δ3) cooled with the wind is 0.3 mm, 0.55 mm and 0.71 mm, respectively. These approve that the continued dissolution of Cu plate can be depressed effectively by the forced cooling.

Effects of Cu/Al ratio on contact time between solid Cu and liquid Al

The cooling curves of Cu plate and liquid Al contact positions are presented in Figure 6, where the CCA castings are prepared under the conditions lCu/lAl=4/30, and 4/40, respectively, with the casting temperature of Al T=973 K, and the Cu plate outside surface is naturally cooled. The alloyed states in different periods are given (Figure 6). Thus, for the casting which lCu/lAl=4/30, and 4/40, respectively and the Cu plate surface is natural cooled, the time remaining liquid phase at contact positions of Cu plate and liquid Al is 120 s and 280 s, respectively, the time remaining solid–liquid two-phase is 210 s and 340 s, respectively, and tL/tt is 36.4% and 45.1% respectively.

Figure 6: Cooling curves of contact positions of copper plate and liquid aluminum L – liquid phase; L+S – solid liquid two-phase; S – solid phase; tL – time remaining the single liquid phase; tt – time to the end of solidification.
Figure 6:

Cooling curves of contact positions of copper plate and liquid aluminum L – liquid phase; L+S – solid liquid two-phase; S – solid phase; tL – time remaining the single liquid phase; tt – time to the end of solidification.

Combined with Figure 2(a), the dissolved thickness of the Cu plate contacting with liquid phase is calculated at 0.97 mm and 1.03 mm occupying 72.4% and 68.2% of the total dissolved thickness, respectively.

Discussion

The dissolved process of solid Cu in liquid Al and the reason of fast dissolution are discussed, by analyzing the crystal structure of Cu, extra-nuclear electron configuration of Cu and Al, and contact modes of Cu and Al atoms.

Contact modes between liquid Al atoms and solid Cu surface atoms and dissolved process

The contact patterns of Al and Cu are presented in Figure 7 following contact between liquid Al atoms and solid Cu atoms.

Figure 7: Contact manners between liquid Al atoms and surface atoms of solid Cu (a) Four Cu atoms around an Al atom (b) Three Al atoms around a Cu atom (c) Eight Cu atoms around an Al atom (d) Two Al atoms around a Cu atom.
Figure 7:

Contact manners between liquid Al atoms and surface atoms of solid Cu (a) Four Cu atoms around an Al atom (b) Three Al atoms around a Cu atom (c) Eight Cu atoms around an Al atom (d) Two Al atoms around a Cu atom.

When the solid Cu atoms contact with the liquid Al atoms, the atomic number of Cu in proximity of an Al atom is more than 2 (Figure 7). On account of the configuration of extra-nuclear electron of Cu is 4s1, while that of Al is 3s2 3p1, two random Cu atoms around the Al atom can easily provide 4s1 track electron to Al atom. This can keep the 3p track of Al atoms in a half full state and form two polar covalent bonds. At the meantime, the metallic bonds existed between the two Cu atoms and other Cu atoms disappear. This induces the binding force between the two Cu atoms and solid Cu to equal zero. Therefore, the Al atom takes the two Cu atoms away from the solid Cu, and the Cu is dissolved in Al liquid (Figure 8).

Figure 8: Dissolved process of Cu atoms in Al liquid (a) Liquid Al atom contacting with solid Cu atoms (b) Accomplishing the reconfiguration of extra-nuclear electrons (c) Cu atoms entering into Al liquid with Al atom.
Figure 8:

Dissolved process of Cu atoms in Al liquid (a) Liquid Al atom contacting with solid Cu atoms (b) Accomplishing the reconfiguration of extra-nuclear electrons (c) Cu atoms entering into Al liquid with Al atom.

Potential products when Cu atoms encountering with Al atoms

An Al atom contacting with four Cu atoms

An Al atom contacts with four surrounding Cu atoms (Figure 7(a)). The three sp2 hybrid tracks formed by the Al atom coincidence with 4s tracks of the three Cu atoms, so three covalent bonds and the compound Cu3Al are formed. Because the 4s layer electrons of the three Cu atoms around the Al atom enter into the three sp2 hybrid tracks of Al atom, the metallic bonds maintain between the three Cu atoms and adjacent Cu atoms in the solid copper. The difficulty that the Al atom takes the Cu atoms into Al liquid is greater than AlCu2.

An Al atom contacting with eight Cu atoms

The distortions of lattice of Cu generate after part of the Cu atoms are dissolved or the vacancies appear on the crystal surface of Cu, as a consequence, the Al atom reaches the crystal surface of Cu (see Figure 7(c)). The random five Cu atoms around the Al atom can easily provide 4s1 layer electron to the Al atom, which makes the 3p track of Al atom in a state of full and five ionic bonds form. It can be seen from Figure 7(c) that the spatial location can also easy to meet. Therefore, the compound Cu5Al is formed. At the same time, the metallic bonds between the five Cu atoms and other Cu atoms disappear. Hence an Al atom takes five Cu atoms into Al liquid. This is a kind of way that the dissolution rate of Cu in Al liquid is the fastest.

A Cu atom contacting with two Al atoms

A Cu atom contacts with two Al atoms after there appear the vacancies in Al liquid (Figure 7(d)). The two Al atoms form six sp2 hybrid tracks. A total of six electrons including the 4s track and 3d track of the Cu atom enter into the six hybrid tracks of Al, so the 3d track of Cu atom is in a state of half full and six polar covalent bonds are formed. From the contact way shown in Figure 7(d), the spatial location can be easy to meet. So the compound CuAl2 is formed.

Two Cu atoms contacting with three Al atoms

The contact way that two Cu atoms contact with three Al atoms is the most likely to appear (Figure 7(b)). When two Cu atoms contact with three Al atoms, three Al atoms form nine sp2 hybrid tracks, and Cu atoms form more complex hybrid tracks. Because the hybrid track of Al atom is plane, the contact way shown in Figure 7(b) also meets the requirements in the space. So the compound Cu2Al3 is likely to form.

Mechanism of fast dissolution of Cu in Al liquid

To sum up, these compounds AlCu2, Cu5Al, CuAl2 and Cu2Al3 are likely to form on the contact surface after the Al liquid contacts with the solid Cu, contributing to the dissolution of solid Cu. Fastest dissolution results from Cu5Al as an Al atom absorbs five Cu atoms into Al liquid.

Conclusions

  1. The dissolution rate of Cu exhibits a linearly increasing tendency when the contact time between solid Cu and liquid Al is within 180 s, the temperature of Al is 973 K or and the temperature exceeds 1,070 K.

  2. The dissolution of solid Cu is influenced by the contact time between liquid Al and solid Cu, the temperature and the cooling method of the Cu plate, when the CCA composite casting is fabricated by the casting Al method. Even though the Cu plate is cooled with the spray, the dissolution of solid Cu can not stop immediately, there is still a little solid Cu continuing to dissolve.

  3. The compounds AlCu2, Cu5Al, CuAl2 and Cu2Al3 tend to form on the contact surface after the solid Cu initially contacts with the liquid Al. Cu5Al presence ultimately results in the fast dissolution of Cu in liquid Al.

Funding statement: Funding: The authors gratefully express their appreciation to Project (LJQ2014062) supported by the Growth Plan for Outstanding Young Scholars in Colleges and Universities of Liaoning Province and Project (2007T078) supported by the Outstanding Innovation Team in Colleges and Universities of Education Department of Liaoning Province for sponsoring this work.

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Received: 2015-1-4
Accepted: 2015-9-18
Published Online: 2015-10-21
Published in Print: 2016-9-1

©2016 by De Gruyter

This article is distributed under the terms of the Creative Commons Attribution Non-Commercial License, which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided the original work is properly cited.

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  2. Short Communication
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https://doi.org/10.1515/htmp-2015-0003
Keywords for this article
Cu/Al composite; dissolution rate; dissolution mechanism; processing parameters
Creative Commons
BY-NC-ND 3.0

Articles in the same Issue

  1. Frontmatter
  2. Short Communication
  3. Microscale Interface Synthesis of Ni-B Amorphous Nanoparticles from NiSO4 by Sodium Borohydride Reduction in Microreactor
  4. Research Articles
  5. The Effect of Post-heat Treatment on the Microstructures of Single Crystal DD6 Superalloy
  6. Changes in the Material Properties of Steel 1.4762 Depending on the Temperature
  7. Formation of Ti5Si3 by Combustion Synthesis in a Self-Propagating Mode: Experimental Study and Numerical Simulation
  8. Effect of Processing Parameters on Plasma Jet and In-flight Particles Characters in Supersonic Plasma Spraying
  9. Crystallization Behavior and Growing Process of Rutile Crystals in Ti-Bearing Blast Furnace Slag
  10. Evaluation of Anticorrosion Performance of New Materials for Alternative Superheater Tubes in Biomass Power Plants
  11. Investigation on Burden Particle Softening and Melting Process under High Reduction Potential Condition
  12. Application of response surface methodology for optimization of parameters for microwave heating of rare earth carbonates
  13. Interfacial Evolution of Cement and Steel in CO2 Dissolved Solution Under High Temperature and High Pressure
  14. Study of Dissolution Process of Solid Cu in Liquid Al
  15. The Pin-Loaded Small One-Bar Specimen in Use to Determine Uniaxial and Multiaxial Creep Data
  16. Vertical Compensation Friction Stir Welding of 6061-T6 Aluminum Alloy
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