Advances in Materials Science and Engineering
Volume 2018 (2018), Article ID 4570120, 16 pages
https://doi.org/10.1155/2018/4570120

Review Article

Low-Temperature Brazing of Titanium Using Al-Based Filler Alloys

A. Muhrat, H. Puga, and J. Barbosa

Centre for Micro-Electro-Mechanical Systems (CMEMS), The University of Minho, Campus of Azurém, 4800-058 Guimarães, Portugal

Correspondence should be addressed to A. Muhrat; eng.abdulsalam.edu@gmail.com

Received 1 December 2017; Accepted 23 January 2018; Published 12 April 2018

Academic Editor: Fantao Kong

Copyright © 2018 A. Muhrat et al. This is an open access article distributed under the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

Abstract.

Brazing of titanium using low melting temperature filler alloys is a preferred choice regarding cost and preserving its mechanical properties. However, brazing titanium at low temperature is still a challenge, especially regarding aluminum-based filler alloys. During the last years, several brazing methods and Al-based fillers were developed to meet industrial requirements; some of them might achieve some of those requirements. The use of ultrasound in brazing has gained increased attention recently, which helps to reduce the time and the necessity for a special brazing environment, subsequently, reducing cost and increasing applicability. Brazing titanium below the transformation temperature, using commercial and experimental Al-based fillers of different compositions, is presented in this review; including the procedures of traditional and ultrasound-assisted brazing methods. Correspondingly, the effects of brazing conditions and alloying elements on the mechanical properties and the intermetallic compounds formation are examined.

1. Introduction

Brazing of titanium at a temperature below transformation temperature has great importance in avoiding undesirable changes in its original microstructures [1, 2]. A low brazing temperature is particularly crucial for thin-wall brazing structures of aerospace components and heat exchangers [3]. The shorter brazing cycle/less brazing temperature helps to prevent the excess interaction between the joint components and growth of the intermetallic compounds at the joint interface [2]. Titanium has a strong chemical attraction of oxygen; therefore, even at room temperature, a passive amorphous oxide layer forms rapidly on its surface [4]. The oxidation of the surface makes titanium joining process challenging from the point of establishing the metal connection; furthermore, titanium should be protected from severe oxidation at temperatures exceeding 650°C [5]. In addition to susceptibility to grain coarsening and affecting strength/ductility of the parent components, high-temperature brazing requires special equipment, conditions, and longer processing time, leading to higher processing cost compared with low-temperature brazing.

Titanium joining has been widely studied [6]. Unlike brazing, welding is not used usually for titanium honeycomb sandwich structures [7–10] which require joining many points without distortion. Moreover, the welding process is not suitable for joining titanium aluminides [11]. A great number of brazing filler alloys were developed and studied for brazing titanium alloys; some of them were commercially used. In 1950s and 1960s, early work was focused upon Ag-, Au-, Cu-, and Pd-based filler alloys for ∼(316–427°C) and Al-based filler alloys for ∼204°C service temperatures. Ti- and Ti–Zr-based alloys were developed later, which showed better metallurgical compatibility with titanium [12] and produced higher joint strength when compared with the other systems of brazing fillers. Table 1 shows some examples of relatively high strength and temperature brazed joints using Ti- and Ti–Zr-based filler alloys. However, low-temperature brazing with more free conditions could find several applications: where the inert atmosphere cannot be applied, the parts to be joined cannot fit within limited and special environments such as the mass production by continuous brazing, the large brazing joints, or for in-place brazing. Furthermore, reducing the joining cost by lowering temperature is important for reducing the total fabrication cost and maintaining titanium share in the total structural weight of aerospace systems [13].

Table 1: Examples of high-temperature brazing of titanium.

Shear strength (MPa)
Conditions
Filler
Parent metal
References

300
Vacuum + argon, 880°C, 60 min

Commercially pure titanium (Grade 2)
[14]

261.7
Vacuum + argon, 870°C, 30 min

Commercially pure titanium (Grade 2)
[15]

540
Argon, 950°C, 30 min

(Grade 5)
[16]

545
Vacuum, 1030°C, 3 min

(Grade 5)/
[17]

According to the main alloying elements, filler alloys for brazing titanium and its alloys can mainly be classified into five groups: titanium-based [1, 14, 16, 18–21], zirconium-based [16, 19, 22, 23], silver-based [24–27], aluminum-based [28–31], and nickel-based [19, 32] filler alloys. Attempts of brazing titanium using Al-based filler alloys and other filler systems started over than 60 years ago [33]. Many Al-based filler alloys have been developed since that time, and many attempts were made in pursuit of achieving suitable brazing conditions. Titanium was brazed to itself and to aluminum alloys by Al-based fillers using an oxyacetylene torch with flux [30, 33], in high-purity argon [10, 33], in vacuum [28–31, 34–36], and in air conditions: in fluxless process assisted by the ultrasonic vibration (USV) [37–39] or by additional pressure [40]. Investigating and improving the mechanical properties of the produced joint through a careful design of the brazing cycle and controlling the intermetallic compound formation/diffusion zone were among the primary explored objectives in brazing titanium and its alloys. Considerable efforts have been made to reduce brazing cycle time while still achieving a suitable strength by employing new techniques and developing new compositions of low-melting filler materials. Although significant work has been done so far, brazing of titanium by Al-based fillers still needs more development to increase its share in the industrial sector.

The developed microstructure and mechanical properties of brazing joints depend on the component compositions, temperature-time cycle, and the joint design. Choosing the right cycle parameters depends, in turn, on the rate and nature of the interaction at parent/filler interface. The short temperature-time brazing cycle protects the parent component from unwanted metallurgical changes, which may occur faster as the temperature increases; for instance, the aging effects which take place in 4 h at 537.8°C (1000°F) in Ti-–6Al-–4V would occur in ∼10 min at 579.4°C (1075°F) [41]. However, brazing time could be increased according to the parent/filler materials' compositions to allow the interface element diffusion to take place for a certain limit which is necessary to achieve the optimal joint strength. The diffusion of some brazing processes, usually in high temperature, may proceed for a relatively long holding time until achieving the microstructure homogenization over all the joint, which is particularly known as diffusion brazing. Matsu et al., Ganjeh et al. and Chang et al. [16, 17, 42] investigated the diffusion brazing of several Ti- and Zr-based fillers, which led to specific microstructures and high shear strengths (Table 1). These processes involve isothermal solidification and homogenization of the joint [43].

In metal casting, the ultrasonic vibration (USV) provides multiple significant effects such as degassing [44–47], refining, and modifying the microstructures [48–51]. Using USV in brazing is an attractive assisting tool [37–39, 52–58]; however, studying the combined effects of USV with the technological parameters of brazing process and developing a joint interface more compatible with the USV have not yet received an adequate attention. The focus in this review will be on the titanium/aluminum interface which includes Al-based filler alloys for brazing titanium/titanium and titanium/aluminum parent (base) components, taking into consideration the technological parameters and procedures.

2. Aluminum-Based Filler Alloys

Various Al-based alloy systems have been tested for brazing titanium/titanium and titanium/aluminum parent components. The alloying additions to the filler materials serve several purposes, such as reducing melting temperature, improving wetting [28, 34], reducing intermetallic thickness [29], improving corrosion resistance [41], and improving static/dynamic strength at work temperature [29].

Lowering the brazing temperature and reducing the contact time of a molten filler alloy with a parent titanium alloy reduce the Ti erosion [26, 42] and increase the reliability of the thin-wall titanium joints [3]. Al-based filler alloys can be a suitable candidate for brazing titanium satisfying the following conditions: the melting temperature considerably below the transformation temperature of titanium alloys, a good metallurgical compatibility with titanium alloys, good wetting and spreading on titanium surface, good corrosion resistance [59], low density, and acceptable strength for a large joining surface [2]. Some commercial Al-based filler alloys of Al–Cu, Al–Mg, and Al–Si systems with addition of Cr and Ti were introduced [3, 19]. However, aluminum leads to fast formation of a brittle intermetallic layer at the joint interface with Ti and provides relatively low strength compared with other filler alloys; the activity of Al with Ti is considered the dominant challenge when designing Al-based fillers and optimizing the brazing process.

2.1. The Developing of Brazing Conditions/Methods in Brazing Ti/Ti and Ti/Al Using Aluminum-Based Fillers

2.1.1. Vacuum, Torch Brazing, and Other Methods

Lewis et al. [33] tested initially many of commercially available brazing fillers using careful sample preparation procedures. The obtained shear strength of the double-lap-brazed joints in a controlled-atmosphere furnace brazing was 73.77–115.69 MPa using 61S (6061) aluminum filler. Further torch-brazing tests were made by covering the specimen surfaces with a commercial titanium flux and using a slightly reducing flame. In general, the strength results were lower 44.82–88.94 MPa when compared with the controlled-atmosphere furnace brazing; the reason was explained by flux entrapment in the joint area or insufficient temperature control and oxidation protection in torch brazing. The use of torch brazing must always be accompanied by specific fluxes, choosing the suitable flux should consider the alloying elements in the molten filler and should be suitable for all joint elements. Fluxes for titanium are primarily mixtures of fluorides and chlorides of the alkali metals, sodium, potassium, and lithium [4].

Takemoto et al. [28] investigated brazing of pure Ti/Al3003 (Al–1Mn) joint in vacuum using three different Al-based filler alloys. Brazing time was short (3–5 min) and brazing temperature did not exceed . Table 2 shows the shear strength results.

Table 2: Results of brazing Ti/Al3003 by Takemoto et al. [28].

Shear strength (MPa)
Brazing conditions
Fillers

38.25
vacuum
Al–10Cu–8Sn

38.25
vacuum
Al–20Ag–10Cu

69.88
vacuum
Al–10Si–0.5Mg

Pure Ti/Ti joints were investigated under the same level of vacuum using pure aluminum and Al–0.8%Si as filler materials at and 3 min holding time [28, 29]. The reported shear strength was for both filler metals; anyway, increasing the holding time leaded to drastic decrement rate of the joint strength of the pure Al filler. It was found that the use of pure Al as a filler metal to braze Ti/Ti in 700°C leaded to self-separation of the joint after holding time of 30 min, and the thickness of the formed intermetallic compound layer () was the greatest, which acts as an initiation site for cracks.

Sohn et al. [34] studied the diffusion between the filler metal and the parent metals of CP-Ti/Al1050 by maintaining the temperature at and changing the holding time in vacuum as it is presented in Figure 1.

Figure 1: Shear strength variation of brazed joints CP-Ti/Al1050 at using Al–10Si–1Mg filler alloy. Reproduced from Sohn et al. [34], copyright 2003, with permission from Elsevier.

The best-achieved shear strength was for the brazing time of 25 min. For longer brazing time, bond strength decreased due to the formation of cavities in Al near Al/intermetallic interface. Shiue et al. [35] investigated a fast heating approach in joining titanium aluminide Ti50–Al50 by infrared brazing using pure aluminum and as filler alloys. Brazing was done in the vacuum using a high-speed infrared source for heating of , and preceded by a preheating for . For the pure aluminum filler, a large formation of the brittle intermetallic phase was found for all holding times, and the bonding strength was very weak. Figure 2 shows the place of the crack through the major phase of in the joint.

Figure 2: The crack location of the brazed joint (). Reproduced from Shiue et al. [35], copyright 2003, with permission from Elsevier.

While for filler alloy which contains Si, it was observed that the intermetallic was prominent at an early stage of infrared brazing. By increasing the time and temperature, the volume fraction of decreased dramatically and replaced by , and then it disappeared. The highest strength was achieved for brazing temperature.

Khorunov et al. [31] investigated Al–Si and Al–Mg filler alloys in brazing OT4 (Ti–3Al–1.5Mn) titanium alloy in vacuum. The resulted strengths using Al–Mg filler alloys were relatively high (82–83 MPa), while the produced joint using Al–Si filler alloy was characterized by inferior quality with a continuous layer of silicide detected along the interface.

Some efforts have been made to simplify brazing process and carry out titanium brazing in normal ambient air conditions. These efforts were focused on developing low-melting brazing fillers and finding a suitable technique to remove the oxide layer on the faying surfaces of the joint. In Germany, Bach et al. (cited in [2]) conducted an early attempt of Ti–6Al–4V brazing in the air by utilizing an alloy of low-melting temperature, which was a thin Al foil coated with copper (33% Cu) for a brazing gap of . The produced joint had a good quality; anyway, the shear strength did not reach more than 25 MPa, which serves in joining large areas only. This showed that the eutectic Al–Cu was active enough to react with titanium in the air. Karfoul and Muhrat [40] investigated Ti/Ti-brazed joint strength in relation to the filler metal compositions and brazing parameters in the air. New brazing filler alloys of Al–Cu–Ni–Ti group were studied to find the effects of the alloying elements, as well as investigating the possibility of brazing in the air. The highest average shear strength achieved was ∼74–73 MPa using Al–8.54Cu–1.35Ni–0.08Ti and Al–6.44Cu–1.96Ni–0.92Ti filler alloys. Removing the oxide layers between the aluminum and titanium is the initiation key of the bonding process. Accordingly, adding pressure will lead, with the help of Ti surface roughness, to break the oxide layer of Al-based filler. Then, buckling proceeds through thickness cracking of the scale, and the stripped Al surface atoms will react with the Ti-oxide layer to reduce it to atomic Ti [40]. Using USV as an assistant tool in brazing, which leads to fast breaking of the oxide layer at the joint interface and makes the joining process possible in air conditions, is summarized in the following.

2.1.2. Ultrasound-Assisted Brazing of Ti by Al-Based Fillers

The sonochemical effects of the USV in liquids have been explored for over 80 years [60]. The interest in ultrasound-assisted brazing started more than 50 years ago. One of the early US patents was an ultrasound-assisted brazing unit using an ultrasonic tip surrounded by local heating flame [61].

Using USV for a short period results in very fast destroying of the oxide layer on the parent material and wetting it by the filler material [52], even it is effective in achieving a good wetting on ceramics by the filler materials in the air [53, 54, 62]. The acoustic cavitation generated in the liquid metal is considered as the most important physical effect of the ultrasonic oscillation propagation [63–66]. The formation of cavities starts with the half period of rarefaction at the weakest points of the melt [63]. Cavities continue to increase in size until they collapse by the compressing stresses during the next compression half period; the results of this collapse include high-intensity pressure pulses, temperature spikes, and high-velocity jets. The important physical and chemical processes due to the ultrasonic cavitation are melt degassing, filtration, wetting of the solid inclusions, and structure modifications. Moreover, the acoustic cavitation results in ultrasound energy adsorption and formation of acoustic streaming. The sound pressure must exceed a certain level to be able to initiate cavitation in the liquid metal, which is called cavitation threshold [63].

Employing USV in brazing results in short processing time, consequently, reducing the cost, and preserving the parent components from further metallurgical changes. The advantages include less specific atmosphere requirements due to the fast-breaking of the oxide layer [39, 52], enhanced spreading of the molten filler [55, 62], and homogenizing the microstructures of the joint [39]. Table 3 summarizes the technological parameters and the shear strength results of the ultrasound-assisted brazing of Ti/Ti and Ti/Al joints using Al-based fillers.

Table 3: Recent studies of ultrasound-assisted brazing of Ti/Ti and Ti/Al joints by Al-based fillers.

Reference
Materials
Heating method and best conditions (all in air)
Shear strength (MPa)

[37]
Parent metal: Ti Grade 5;
filler metal: TiBraze Al-665(Al–2.5Mg–0.3Cr)/100 
Induction brazing, 660°C, (5 sec, 84 W) USV, no holding time
50–60

[39]
Parent metals: Ti Grade 5/Al1060;
filler metal: Al–12Si
(A = 6 , 20 kHz) USV, 620°C, 4 sec USV + holding for 15 or 5 min + 4 or 0 sec USV
∼68

[38]
Parent metal: Ti Grade 2;
filler metal: TiBraze Al-665A (Al–2.5Mg–0.3Cr)/50 
Induction brazing, (25 kHz, 120 W) USV, 670°C, holding for 5 min at 560°C, then heating to 670°C and holding for 3 min, applying USV for 6 s
∼64

[55]
Parent metals: Ti Grade 5/Al6061;
filler metal: Al–9.4Si–10Zn–10Cu–2Ni
(A = 6 , 20 kHz) USV, 560°C, 4 sec USV + holding for 60 min + 4 sec USV
∼43

[55]
Parent metals: Ti Grade 5/Al6061;
filler metal: Al–15Sn–8.2Si–8.5Zn–8.5Cu–1.7Ni
(A = 6 , 20 kHz) USV, 560°C, 4 sec USV + holding for 15 min + 4 sec USV
∼76

Chen et al. [52] explored the instantaneous breakage behavior of the oxide film of Ti–6Al–4V on its interface with the liquid Al–Si alloy and the chemical interactions during the process using 20 kHz frequency and amplitude USV. The samples were heated to then the titanium sonotrode was quickly loaded on the titanium substrate with a constant pressure of 0.2 MPa. The applied time of USV was 2–16 s. Due to the USV effect, a large number of pits were formed on the titanium substrate as it is shown in Figure 3. The formation of the pit started by a small notch on the surface of the Ti oxide film due to “cavitation erosion” [65, 67] (N in Figure 4) which serves as a microchannel and allows direct interaction between the fresh Ti surface and molten Al alloy.

Figure 3: The morphology of Ti–6Al–4V substrate surface: (a) after interaction with the liquid Al–Si alloy for 10 min without ultrasonic treatment and (b) with ultrasonic treatment for 8 s. Reproduced from Chen et al. [52], copyright 2012, with permission from Elsevier.

Figure 4: The microstructure (SEM) of Al–12Si/Ti–6Al–4V interface after: (a) 4 s; (b) 4 s + 5 min; (c) 4 s + 15 min; (d) 4 s + 15 min + 4 s. Reproduced from Chen et al. [39], copyright 2013, with permission from Elsevier.

The suggested pit formation mechanism according to this study was firstly, the formation of a notch at the oxide layer of the titanium substrate and secondly, violent chemical dissolution of the solid phase Ti–6Al–4V into the liquid filler Al–Si, followed by further interfacial chemical reactions.

Chen et al. [39] conducted a further work in ultrasound-assisted brazing of Ti–6Al–4V/Al1060 in the air using Al–12Si filler. In this study, ultrasonic vibration was applied to Ti–6Al–4V plate for 4 s at followed by 0, 5, and 15 min holding time, and then by a second ultrasonic vibration period for 4 s. Applying the first ultrasonic vibration for 4 s caused formation of pits at the surface of the titanium alloy (Figure 4(a)). By applying a holding time of 5 or 15 min, the dissolving continued at Al1060 and Ti sides; consequently, the oxide film detached off the titanium substrate which is called “substrate oxide undermining” (Figures 4(b) and 4(c)). In addition to the pit formation, the cavitation and the stirring action of acoustic streaming caused the following effects during the ultrasound operation:

(i)Accelerating the dissolution process at Ti side once the pits had been formed on the Ti oxide film, as well as along Al1060 side.(ii)During the second 4 s of USV, breaking the floating oxide film of the titanium alloy (Figure 4(d)). Simultaneously, breaking the Al dendrites and causing the Al phases to distribute uniformly in the joint.

Anyway, increasing holding time to 15 min or adding a second USV period did not improve the shear strength of the brazed joints.

Tillmann et al. [37] studied the ultrasound-assisted brazing of Ti–6Al–4V using Al–2.5Mg–0.3Cr filler and induction heating. The studied parameters were the layer thickness (60–200 µm), brazing temperature (660–680°C), and acoustic power (60–96 W), and then the sample of the best ultrasound-assisted brazing parameters was compared to a traditional vacuum brazing one. Increasing temperature over or reducing the thickness to less than 100  resulted in big voids in the brazed area. Increasing the acoustic power up to 70% (84 W) resulted in a considerable reduction of the oxide layer at the interface, and less intensities could not remove the oxide layer, while the highest one of 80% caused a significant cavitation leading to gap formation in the joint (Figure 5). The highest shear strength obtained using the sample of 100 , 660°C, 5 s, 70% did not reach more than 60 MPa and between 30 and 40 MPa for vacuum-brazed samples.

Figure 5: The formed voids and gaps in Ti–6Al–4V/Al–2.5Mg–0.3Cr/Ti–6Al–4V brazed joints by different ultrasound-assisted brazing parameters: (a) 100 , 670°C, 5 s, 60%, (b) 60 , 660°C, 5 s, 50%, and (c) 100 , 660°C, 5 s, 80%. Reproduced from Tillmann et al. [37], copyright 2015, with permission from Springer.

The lower strength values for the samples brazed in the vacuum were attributed to the low heating rate which resulted in an excessive formation of a low-ductility intermetallic at the interface.

Elrefaey et al. [38] conducted a preliminary investigation of the microstructure and the fracture behavior of ultrasound-assisted brazing of Grade 2 titanium using TiBrazreAl-665A filler alloy. The results showed the formation of the thin interaction layer of , and the joint failed mainly at Ti/Al interface due to the brittle nature of the intermetallic. Chen et al. [55] investigated the addition of Sn to in ultrasound-assisted brazing of Ti/Al joint. In a similar way in other works [39, 62, 68], a simple overlap assembly was used with a preset joint clearance of . The addition of Sn caused the widening of the melting range; before reaching the solidus temperature, the residual Sn-rich liquid filled the capillary gaps between the solidified grains which significantly reduced the residual thermal stresses and enhanced the joint strength [55].

To guarantee the efficient transfer of USV to the joint, the fixing rig and the mechanism by which the USV is being transferred should be designed carefully. This includes the consideration of the acoustic properties of the fixing rig components, the applied force on the joining area, and the location of the sonotrode tip [69]. Elrefaey et al. [38] used, for instance, an apparatus where the horn was installed vertically, and the sample which was mounted into a steel holder was under 0.2 MPa pressure as a result of the horn weight (Figure 6). While, Tillmann et al. [37] used overlapped brazing joints with a torque of 8 Nm introduced by a screw connection.

Figure 6: Schematic illustration of an ultrasonic-assisted brazing apparatus used by Elrefaey et al. Reproduced from Elrefaey et al. [38], copyright 2013, with permission from American Welding Society (AWS).

Even though using USV is a valuable way to break up the oxide layer and improve the properties of the joint, the results of ultrasound-assisted brazing of Ti/Ti and Ti/Al confirm that the process needs more control and investigation on the brazing conditions/materials to achieve higher mechanical properties.

2.2. The Intermetallic Compound Formation at the Ti/Al Interface

Several intermetallic phases occur in the Ti–Al system such as , [70]. In fact, only are technically interesting [71]. Since almost all filler metals form intermetallic compounds with titanium [29], therefore, studying and controlling their formation/development at the interface largely determine the mechanical behavior of the brazed joints. The formation and growth of the intermetallic compound at the interface is related basically to the compositions of the filler materials, the parent material, and the temperature-time parameters. Brazing titanium with pure aluminum, for instance, mainly leads to the formation of at the interface; adding Si (≥3%) to the aluminum filler alloy will lead to formation of ; however, adding Cu or Ag will not change the probability of formation [29]. The predicted phase by the effective heat of the formation rule does not necessarily form at the moving reaction interface if it is difficult to nucleate [72]. Many studies showed that would form at the expense of the preexisting or phases in the presence of excess Al. Sujata et al. [73] calculated the free energies of formation of different titanium aluminide compounds in the temperature range ∼(0–1200°C), and they found that the free energy of is less than that of but slightly higher than that of . The preferred formation of as the only product during solid Ti/liquid Al reaction was explained by two factors: the first one is the additional steps in formation which include as one of the starting phases and the second factor is the presence of the excess amount of liquid Al which minimizes the trend of or Ti-rich compound formation. Wöhlert and Bormann [74] investigated the phase selection mechanism of intermetallic compounds in Ti/Al phase reaction. The predeposited layers of and , between Al/Ti elemental layers after annealing for 50 and 20 h at 400°C, respectively, were disappeared and replaced by . Accordingly, the phase selection during the interface reaction was explained by the differences in growth velocities of the competing phases. Similar main phase selection reason was concluded by Michaelsen et al. [75] including the nucleation as a first step in TiAl₃ formation. Analogous results of formation on a -based alloy were reported by Zhang et al. [76] by using hot dip aluminizing (750°C-15 s) followed by interdiffusion treatment (600°C-30 h). It was found that the addition of Si, Mn, or Ag to the pure Al coating improved the thickness uniformity and reduced the formation of the transverse cracks. Further intermediate layers consisting of (TiAl₃ + TiAl₂) and/or TiAl were formed after high-temperture oxidation for all the coatings. Zhang et al. [77] reported in another work using similar aluminizing and interdiffusion procedures the growth of as solid state reaction products at the interface of and substrate after the subsequent oxidation at 700°C and 300h, whereas TiAl₃ + TiAl₂ and Ti₃Al layers were formed at 800°C and 300 h of oxidation in air. The mixed + layer resulted from O₂ reaction with . Xu et al. [78] applied vacuum hot pressing on Ti/Al laminates followed by annealing and found that the next reaction phase after TiAl₃ was TiAl at the Ti/Al interface after consuming Al layer and during a second-stage annealing treatment at higher temperatures. The diffusion at the Al/Ti interface can be accelerated with the amount of cold/hot rolling reduction [78, 79]. In brazing titanium alloy OT4 by Mg-containing aluminum alloys, the formation of between and titanium also could take place [31].

The diffusion of the chemical elements across the interface of the brazing joint is high at the beginning of the brazing process since the diffusion at the beginning is between liquid and solid phases. As soon as the formation of the intermetallic compounds takes place, the diffusion rate is reduced and becomes less and less by increasing the intermetallic layer thickness until the growth of the intermetallic compound is suppressed. Considering, in titanium-rich aluminide, titanium can diffuse faster than Al [80, 81]. The thickness of the intermetallic layer when using pure aluminum as a filler is the largest one, and any addition or impurity elements will suppress—but differently—the growth of the intermetallic layer [29].

Brazing titanium aluminide TiAl at 900°C for 30 s using pure Al filler produced very weak joint, and the primary phase in the joint was the brittle phase [35]. On the other hand, for a different case with longer bonding cycle under pressure and without any additional filler, the “diffusion bonding” of two-phases gamma-based titanium aluminide Ti–45Al (in at.%) produced phase at the bonding interface. It was concluded by Buque and Appel [82] that the unavoidable contamination of the diffusion couple with oxygen leads to the formation of a thin layer of phase. Similar result was found by Herrmann and Appel [83] for various two-phase gamma-based titanium aluminides, even considerably higher vacuum was used.

2.3. Main Aluminum-Based Filler Systems

2.3.1. Pure Aluminum as a Filler Metal

Pure aluminum is highly active with titanium at brazing temperature causing high erosion level, consequently, unreliable brazed joints specially for the thin-wall titanium structures [2]. Takemoto et al. [28, 29] found that the highest thickness of the intermetallic compound was caused by using pure aluminum as a filler. The small additions of alloying elements or impurities to the pure Al filler reduced the intermetallic layer thickness at the brazed interface. It was found that the addition of 0.8%Si greatly reduced the thickness and the growth rate of the intermetallic , and the produced Ti/Ti joints using Al-0.8Si filler maintained higher joint strengths after brazing for relatively higher temperatures and longer holding times comparing with pure Al filler [29]. In the same context, Shiue et al. [35] found that the bonding strength of TiAl/Al/TiAl joint was very weak to be evaluated due to the extensive presence of the stable phase in the joint.

The minor modifications in the alloying elements affect the wetting and spreading behavior and should be designed according to the type of the Ti parent metal. For instance, comparing the fillers Al–4.5Mg–0.4Si–0.1Cr and Al–4Mg–0.5Si–0.4Mn [30], the former with more 0.5%Mg and 0.1Cr instead of 0.4Mn, has a lower contact angle and better spreading on Grade 5 titanium; by contrast, these modifications have a different effect in brazing Grade 2 titanium. Table 4 shows a summary of Ti/Ti–Ti/Al-brazed joints using pure or low-alloyed Al fillers.

Table 4: Ti/Ti–Ti/Al-brazed joints using pure or low-alloyed Al fillers.

References
Materials
Conditions
Bonding
Shear strength (MPa)
Intermetallic compounds at Ti/filler interface

Parent 1
Parent 2
Filler

Type
Thickness/gap width ()
Temperature (°C)
Time (min)

[29]
Pure Ti
Pure Ti
Pure Al
100
Vacuum
680
3
∼92

680
10
∼42

Al–0.8Si
680
3
∼94

680
10
∼75

[31]
OT4 titanium
OT4 titanium
AD1 (Al–0.4Si–0.3Fe)
60
Vacuum
685
3
76

Cited in [2]
Ti Grade 5
Ti Grade 5
Al–0.3Si–0.8Fe–0.2Mg

>660

72

[35]
Ti50–Al50
Ti50–Al50
Pure aluminum
75
Vacuum
900
0.5
Very weak joint

The shear strength values calculated according to Figure 11 in [29]. Infrared brazing , preheating in 400°C for 60 s.

2.3.2. Al–Mg-Type Filler Alloys

Flom [84] reported the disappearing of magnesium from the interface layer between Al–Mg filler alloy and titanium parent alloy during vacuum brazing. Similarly, Khorunov et al. [31] found, after brazing using AMg6 alloy containing 6% of Mg, that only 1.5% of Mg remained in the joint and no Mg remained at the interface; the reduction of Mg was explained by the evaporation of Mg from the filler during the heating and melting in vacuum. The volatility of magnesium in elevated temperatures [85] and the reaction of the magnesium vapor with the oxide surface of aluminum make Mg an excellent wetting promoter [86]. Mg reacts with aluminum oxide forming a complex oxide [87] or reducing it to Al + MgO [34], which forms inclusions and induces bonding to occur; as a result, the content of Mg is reduced in the joint considerably [31]. The improved wetting of Al–Mg filler alloys was also confirmed by Khorunov et al. [31], where Al–Mg filler showed better wetting on titanium alloy OT4 for a temperature less than 700°C comparing with Al–Si. Raising brazing temperature more than 700°C resulted in reducing the contact angle for all the fillers containing Si or Mg. Mg content in the filler and the brazing conditions must be taken together into consideration when designing the brazing alloy, for example, alloy showed a good result of 117 MPa in torch brazing but produced only 61 MPa in vacuum brazing [30]. Another example, the vacuum brazing by Mg-containing filler alloys of 6% and 2.5% Mg showed almost identical strengths which were higher than the one using the Si-containing fillers [31]. Eckardt et al. [30] reported the formation of a variable and discontinuous intermetallic layer of between the Al–Mg fillers and the titanium parent metal. In addition, it was reported that a thicker intermetallic layer was formed on Grade 5 titanium comparing with Grade 2 titanium. The high-Mg alloys did not show better fillet formation properties compared with the average-Mg braze alloy such as TiBraze 665 which contains only 2.5% Mg [30]. Table 5 shows a summary of Ti/Ti–Ti/Al-brazed joints using Al–Mg-type filler alloys.

Table 5: Ti/Ti–Ti/Al-brazed joints using Al–Mg-type filler alloys.

References
Materials
Conditions
Bonding
Shear strength (MPa)
Intermetallic compounds at Ti/filler interface

Parent 1
Parent 2
Filler

Type
Thickness/gap width ()
Temperature (°C)
Time (min)

[33]
Ti
Ti
61S(Al (6061)) (Al–1Mg–0.6Si–0.25Cu–0.25Cr)
76
Argon(furnace)

5
73.8–115.7

Torch with flux

44.8–88.9

[29]
Pure Ti
Pure Ti
Al–1Mg
100
Vacuum of
680
3

[30]
Ti Grade 5, 2
Ti Grade 5, 2
Al–4.5Mg–0.4Si–0.1Cr
800
Vacuum/torch with flux
>638 liquidus temperature

Poor result
,

Al–4Mg–0.5Si–0.4Mn
500
>640 liquidus temperature

61 in vacuum and 117 by the torch

[3]
Ti Grade 5, 2
Ti Grade 5, 2
TiBraze Al-665 (Al–2.5Mg–0.3Cr)
100
Vacuum/torch with flux
680

110.4 G5 97.6 G2

Al–4Mg–0.5Si–0.4Mn
320
650–700

98.8 G5 77.4 G2

[31]
OT4 titanium
OT4 titanium
AMg6 (Al–6Mg–0.6Mn–0.4Si–0.4Fe–0.1Ti)
60
Vacuum
685
3
82

AMg6 (Al–6Mg–0.6Mn–0.4Si–0.4Fe–0.1Ti)
60
720
40

Al–2.5Mg–0.2Si–0.4Fe–0.2Cr
100
685
83

[84]
Ti Grade 2/Grade 12
Ti Grade 2/Grade 12
TiBraze Al-645 (Al–5Mg–0.2Si–0.2Ti)
<25
EB + vacuum
>melting point
0.5–0.75

[37]
Ti Grade 5
Ti Grade 5
TiBraze Al-665 (Al–2.5Mg–0.3Cr)
100
Ultrasound-assisted induction brazing in air
660
5 sec USV
50–60

[38]
Ti Grade 2
Ti Grade 2
TiBraze Al-665A (Al–2.5Mg–0.3Cr)
50
Ultrasound-assisted induction brazing in air
670
5 min in 560°C + 3 min in 670°C + 6 s USV
∼64

A double-lap joint. Considering 1205°F is the liquidus temperature [88].

2.3.3. Al–Si-Type Filler Alloys

Takemoto and Okamoto [29] reported that the small addition of 0.2–0.8%Si is highly effective in suppressing the intermetallic layer growth of . However, further additions of Si increased the intermetallic thickness and promoted the formation of additional intermetallic compounds: at the interface, where was adjacent to the titanium parent side. Using mainly produced and a small quantity of intermetallic compounds. The best result of tensile test was for comparing with the other two filler materials and . It was found that the fracture occurred within the filler metal when using [29]. Under almost similar conditions, but for longer brazing time, Sohn et al. [34] investigated the diffusion brazing of Al/Ti joint by . The bonding at the Ti/filler interface started as soon as the filler had been melted; two intermetallic compounds were observed, the continuous at the titanium side, which increased by the time due to the diffusion of Si into Ti, and the discontinuous one at the filler side and the fracture occurred in Al layer. In ultrasound brazing of titanium, two intermetallic compounds were formed at Ti–6Al–4V/Al–12Si filler interface [39]. The intermetallic IMC-A () formed at the pit edge during the first USV, while IMC-B () at the wall and the bottom of the pit. Applying holding time for 5 min caused the IMC-A () to form at the interface between IMC-B () and Ti–6Al–4V; by increasing the holding time to 15 min, the thickness of IMC-B () increased (Figure 4). Wells [41] reported that the Al–7.5%Si alloy cladded to a core of aluminum alloy 6951, which did not melt during brazing, produced stronger joint than 63Al–32Cu–5Ag–0.01Li for Grade 5 Ti. However, Khorunov et al. [31] found that Mg-containing filler alloys provided higher joint strength than the Si-containing filler alloy (5.3% Si), which was explained by the solidification of the silicide as a continuous strip at the brazing interface. Table 6 shows a summary of Ti/Ti–Ti/Al brazed joints using Al–Si-type filler alloys.

Table 6: Ti/Ti–Ti/Al-brazed joints using Al–Si-type filler alloys.

References
Materials
Conditions
Bonding
Shear strength (MPa)
Intermetallic compounds at Ti/filler interface

Parent 1
Parent 2
Filler

Type
Thickness/gap width ()
Temperature (°C)
Time (min)

[34]
CP-Ti
Al (1050)
Al–10Si–1Mg
100
Vacuum
620
25
84
,

[29]
Pure Ti
Pure Ti
Al–(0.1–10)Si
100
Vacuum
680
3
∼94 for Al–0.8Si
, ,

[28]
Pure Ti
Al (3003)
Al–10Si–0.5Mg
100
Vacuum
600
3
∼70
,

[3]
Ti Grade 5, 2
Ti Grade 5, 2
AWS BAlSi-4 (Al–12Si–0.8Fe)
80
Vacuum/torch with flux
600–620

74.2 G5 69.6 G2

[31]
OT4 titanium
OT4 titanium
Al–5.3Si–0.8Fe–0.3Cu–0.2Ti
100
Vacuum
685
3
56
Continuous silicide

[89]
Ti Grade 5
Al (6060)
Al–8.4Si–20Cu–10Ge–0.1Re
200
Vacuum + argon
530
10/30/60
49/55/48

Al–8.4Si–20Cu–10Ge
530
10/30/60
23/17/20

[35]
Ti50–Al50
Ti50–Al50
BAlSi-4 (Al–(11–13)Si–0.3Cu–0.1Mg–0.2Zn–0.15Mn–0.8Fe)
75
Vacuum
900
3
86.2
 + ( for longer brazing time)

[84]
Ti Grade 2/Grade 12
Tit Grade 2/Grade 12
TiBraze Al-642 (Al–5.3Si–0.8Fe–0.2Ti)
<25
EB + vacuum
>melting point
0.5–0.75

[39]
Ti Grade 5
Al1060
Al–12Si

Ultrasound-assisted brazing in air
620
4 sec USV + holding of 15 or 5 min + 4 or 0 sec USV
∼68
,

Transient liquid phase bonding. For Al–0.1Si/3 min, only was observed. Very weak diffraction line was observed for . Infrared brazing .

2.3.4. Al–Cu- and Al–Ag-Type Filler Alloys

Al–Cu and Al–Ag promoted mainly formation at the brazed interface of titanium. Adding Sn did not change the intermetallic type since Al–10Cu–8Sn filler metal mainly promoted formation in Al(A1100)/Ti joints and very weak diffraction line corresponding to . However, high peak of Sn at the interface was showed by EDX line analysis, and the fracture occurred within the intermetallic compound [29]. In a different manner, the existence of Si in the filler changes the intermetallic type; Chen et al. [55] reported the formation of the intermetallic at the interface between the Grade 5 Ti and each of Al–9.4Si–10Zn–10Cu–2Ni and Al–15Sn–8.2Si–8.5Zn–8.5Cu–1.7Ni fillers; it was concluded that the addition of Sn improved the strength through reducing the residual thermal stress. Eckardt et al. [30] found that the filler alloy TiBraze Al-635 (Al–4.2Cu–1.5Mg–0.5Mn–0.5Si) had the lowest contact angle on Grade 5 Ti and a good one (second-lowest one) on Grade 2 Ti with the highest strength among the other alloys of Al–Ag, Al–Mg, and Ag–Cu–Zn–(Cd–Sn) using vacuum brazing. The interlayer between the parent metal and the filler TiBraze Al-635 consisted of variable and discontinuous layer of . According to Wells [41], the addition of Mg or the small addition of Li to the filler metal improved the flow characteristics of Al–Cu–(5–50)Ag-type alloys; on the other hand, alloying with Mg significantly decreased the corrosion resistance of the joints. Si and/or Sn-containing filler metals formed weaker joints or exhibited flow temperature of ∼587°C (860 K) or higher. It was found that the flow temperature for the Al–Cu–Ag alloys varied with the employed atmosphere; flow temperatures were 111°C higher in the vacuum than in of argon. In brazing damage-tolerant titanium structures, Al–Cu–Ag filler materials prevent the cracks from spreading by delamination in the crack arrest orientation. The behavior in the crack divider orientation was similar to the behavior of the monolithic material [41]. Tables 7 and 8 show a summary of Ti/Ti–Ti/Al-brazed joints using Al–Cu and Al–Ag-type filler alloys, respectively.

Table 7: Ti/Ti–Ti/Al-brazed joints using Al–Cu-type filler alloys.

References
Materials
Conditions
Bonding
Shear strength (MPa)
Intermetallic compounds at Ti/filler interface

Parent 1
Parent 2
Filler

Type
Thickness/gap width ()
Temperature (°C)
Time (min)

[29]
Pure Ti
Pure Ti
Al–1Cu
100
Vacuum
680
3

[28]
Pure Ti
Al (3003)
Al–10Cu–8Sn
100
Vacuum
615
5
∼38

[29]
Pure Ti
Al (3003)
Al–33Cu
100
Vacuum
630
3

[30]
Ti Grade 5, 2
Ti Grade 5, 2
TiBraze Al-635 (Al–4.2Cu–1.5Mg–0.5Si)
300
Vacuum/torch with flux
>638 liquidus temperature

140 in vacuum and 88 by the torch
, larger on Grade 5

[3]
Ti Grade 5, 2
Ti Grade 5, 2
TiBraze Al-635 (Al–4.2Cu–1.5Mg–0.5Si)
200
Vacuum/torch with flux
660–700

140.7 G5 100.8 G2
, larger on Grade 5

Al–25Cu–9Si
100
580–620

88.6 G5 34.1 G2

Ti Grade 2
Ti Grade 2
Al–24Cu–8.6Si–3.5Sn
150
580–620

47.7

(Cited in [2])
Ti6Al4V
Ti6Al4V
Al–33Cu
6–20
Air
550

25

[55]
Ti Grade 5
Al (6061)
Al–9.4Si–10Zn–10Cu–2Ni
∼200
Ultrasound-assisted induction brazing in air
560
4 sec USV + 60 min + 4 sec USV
∼43

Al–15Sn–8.2Si–8.5Zn–8.5Cu–1.7Ni
4 sec USV + 15 min + 4 sec USV
∼76

[40]
Ti-5 (95%)
Ti-5 (95%)
Al–8.54Cu–1.35Ni–0.08Ti
100
By applying pressure/in air
647
13
74.78

Al–6.44Cu–1.96Ni–0.92Ti
648
9
73.66

Very weak diffraction line was observed for .

Table 8: Ti/Ti–Ti/Al-brazed joints using Al–Ag-type filler alloys.

References
Materials
Conditions
Bonding
Shear strength (MPa)
Intermetallic compounds at Ti/filler interface

Parent 1
Parent 2
Filler

Type
Thickness/gap width ()
Temperature (°C)
Time (min)

[28]
Pure Ti
Al (3003)
Al–20Ag–10Cu
100
Vacuum
600
5
∼38

[29]
Pure Ti
Al (3003)
A1–33Ag
100
Vacuum
630
3

[30]
Ti Grade 5, 2
Ti Grade 5, 2
Al–38Ag–7.4Si–0.6Fe
260
Vacuum/torch with flux
>580 liquidus temperature

Poor result

[3]
Ti Grade 2
Ti Grade 2
Al–28Ag
Powder +325/−100 mesh
Vacuum/torch with flux
600–620

70

Al–28.5Ag–21Cu–1.3Mg
260
650–710

67.6

Another undetermined very thin one.

2.3.5. Al–Ni, Al–Mn, and Other Types of Filler Alloys

Nickel addition to the pure aluminum filler had a little effect on the suppression of the intermetallic layer at the Ti/filler interface, whereas Mn addition showed a better result [29]. However, nickel addition to Al–Cu–Ti filler together with a decrease in copper ratio increased the shear strength [40]. Ge improved the corrosion resistance when added to the Al–Cu- and Al–Cu–Ag-type alloys but formed very fragile joints [41]. Table 9 shows a summary of Ti/Ti-brazed joints using Al–Ni- and Al–Mn-type filler alloys.

Table 9: Ti/Ti-brazed joints using Al–Ni- and Al–Mn-type filler alloys.

References
Materials
Conditions
Bonding
Shear strength (MPa)
Intermetallic compounds at Ti/filler interface

Parent 1
Parent 2
Filler

Type
Thickness/gap width ()
Temperature (°C)
Time (min)

[29]
Pure Ti
Pure Ti
Al–1Mn, Al–1Ni
100
Vacuum
680
3

[30]
Ti Grade 5, 2
Ti Grade 5, 2
TiBraze Al-700 (Al–21.5Ni–9Cu–9.6Si–1.3Fe–0.6Mn)
300
Vacuum/torch with flux
≥607

93 in vacuum and poor result by torch
,

[3]
Ti Grade 5, 2
Ti Grade 5, 2
TiBraze Al-700 (Al–21.5Ni–9Cu–9.6Si)
290
Vacuum/torch with flux
700–720

127.3 G5 81.6 G2
,

Cited in [2]
Ti Grade 5
Ti Grade 5
Al–1.2Mn–0.6Si–0.7Fe–0.2Cu

>660

89

3. Conclusions and Future Work

In this review, the aluminum-based filler alloys for brazing titanium and the formation of the intermetallic compounds at the interface of Ti/filler have been analyzed. The proper design of time-temperature cycle and the controlled alloying additions in the aluminum filler are crucial factors for the intermetallic compound formation at the interface. The thickness and type of the intermetallic phases will largely determine the mechanical properties of the brazed joint. In the case of brazing Ti/Al joints, further decrease in brazing temperature, adequate time-temperature cycle, and the compatibility of the brazing filler on the both Ti/Al sides should be considered thoroughly.

Several technological parameters have been examined for ultrasound-assisted brazing of titanium by Al-based filler alloys, including the acoustic power, the USV period, the holding time, the filler thickness, and the brazing temperature; accordingly, the following points should be highlighted:

(i)The holding time after USV is necessary for the diffusion process proceeding at the interface between the filler and the titanium parent metal.(ii)Varying the power of the ultrasound affects the oxide removal at the filler/parent metal interface directly.(iii)The thickness of the filler should be chosen according to USV parameters and time-temperature brazing cycle; considering the accelerated interaction between the liquid filler and the parent metal by the effect of USV.(iv)Brazing and ultrasound parameters/conditions should be considered together in ultrasound-assisted brazing process, for instance, the ultrasonic power/intensity, the coupling method of the ultrasound with the workpiece which insures the excellent delivery of the USV to the joint area, the USV activation time, and other traditional brazing parameters.(v)Studying the USV effects on the microstructure of the brazed joint should be given more attention.

Brazing process has many factors that should be considered to achieve the best possible mechanical properties of the produced joint; the quality of the filler material is one of these factors. Different processes are available for aluminum filler production; the casting process is used as a favorite way to produce new filler aluminum alloys or known ones of lab-scale size for testing purposes. However, the properties and the quality of the cast affect the mechanical properties and the quality of the final brazing joint. The impact of the cast defects and the imperfections varied according to the form of the brazing filler alloy and the brazing process. The filler alloy, as a primary consideration, should have homogeneous chemical composition, with controlled or free of inclusions, and free of porosity. Using USV in the preparation and developing specific, low-melting temperature filler alloys for brazing process from their pure elements would be a great tool in enhancing the filler alloy properties, accelerating the process, and thus, exploring more compatible brazing fillers. Due to the limited works in ultrasound-assisted brazing of Ti by Al-based fillers and the mechanical properties of the produced joints, it is tempting to investigate and seeking to develop further compositions of the Al-based fillers which can be more adequate for ultrasound-assisted brazing of Ti and to conduct deeper studies considering the integration between the USV and the traditional brazing parameters.

Conflicts of Interest

The authors declare that they have no conflicts of interest.

Acknowledgments

This work is supported by Erasmus Mundus through PEACE II Lot 2 Project 2013–2443/001-001-EMA2 and FCT with the reference project UID/EEA/04436/2013, COMPETE 2020, with the code POCI-01-0145-FEDER-006941.

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