Beruflich Dokumente
Kultur Dokumente
REVIEW
Vol.57, No. 6, December 2004, pp. 593-610
ABSTRACT
This review attempts to present the current understanding of the mechanism of pitting corrosion of heat treatable
aluminium alloys and their welds. The role of alloying elements and intermetallic phases on the corrosion
behavior of these alloys has been discussed. Pitting mechanism of aluminium- copper alloys is specifically
discussed. Finally effect of welding on the pitting corrosion of these alloys is also presented.
defect model as a modified or related penetration ion penetration and migration, and stress-induced
model. The point defect model addresses the transport breakdown of passive film. Although these models
of cationic vacancies to the metal/oxide interface obtained some experimental support, no comprehensive
controlling pit initiation instead of anion penetration. or universal model can account for pitting corrosion
The point defect model has been fitted to experimental in all metal/environment systems. This indicates that
data such as pitting potential and induction time for pit initiation is rather complicated and a combination
pitting corrosion of Al and Al alloys in halides. of these models could explain pitting for a certain
However this model cannot explain metastable pitting, metal/environment system.
and some assumptions such as the electrode potential
and vacancy migration in extremely high electric field 2.2 Metastable Pitting
(on the order of 106 to 107 V/cm) are suspicious.
The film-breaking model involves the breakdown and Metastable pits are pits that survive for a very short
repair of the passive film simultaneously. Mechanical lifetime in the order of seconds or less. They can
stresses due to electrostriction and surface tension initiate and grow to the micron size at potentials far
cause the passive film breakdown, which is repaired below the pitting potential and also above the pitting
rapidly. According to this film-breaking model, pits potential during the induction time prior to the onset
initiate as a result of the passive film breakdown of stable pitting. Figure 3 shows typical metastable
only when stable pits grow afterward. pit current transients on stainless steels, in chloride
solution under an applied anodic potential. The current
In summary, these models address important aspects increases corresponding to the growth of metastable
of pit initiation such as aggressive ion adsorption, pit followed by a sharp current decrease due to
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repassivation process. Since metastable pits experience These detailed studies show that the early
initiation, growth, and repassivation, a better development of stable pits appears to be identical to
understanding of these three stages for the stable pit that of metastable pits, and the probability of stable
can be gained through study of metastable pitting. pitting is directly correlated to the intensity of
Metastable pitting phenomenon was first observed in metastable pitting events. Metastable pits repassivate
stainless steel in the early 1970s12. Frankel and probably when the porous cover ruptures and the pit
coworkers used the term of metastable pitting for the electrolyte is diluted. In contrast to a huge amount of
first time13. Over the past 30 years, metastable pitting studies on corrosion of stainless steels, literature on
has been systematically investigated by analyzing pit corrosion of Al or Al alloys is limited. Pride14 et al.
current density for individual metastable pits and studied metastable pitting on pure Al. They found
stochastic approaches to groups of metastable pits. that the number of metastable pits and the current
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(a)
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impedance value (Ohm.cm2), where the phase angle Coarse intermetallic particles play a crucial role in
approaches zero is accurate polarization resistance of the corrosion behavior of Al alloys. The micro
the alloy in a given environment. Recently EIS galvanic coupling between the matrix and the
technique has been recognized as the accurate method intermetallic particles is generally believed to result
of determining the corrosion resistance of aluminium in pitting corrosion and further develop intergranular
alloys in solutions containing aggressive halide ions. cracking (IGC) into the deep structure of Al alloys.
Determining polarization resistance of the alloys In this section, the role of alloying elements in solid
immersed in sodium chloride solution as function of solution and intermetallic particles in pitting corrosion
time and its variation may be criteria for the of Al alloys will be reviewed.
measuring pitting corrosion resistance of aluminium
alloys. Recently Q.Meng et..al 42 studied the 3.1 Alloying Elements
corrosion behaviour of 7xxx alloys with varying
Copper content using immersion tests in aerated Muller and Galvele43 first studied the role of alloying
chloride solutions (Fig.8) and concluded that the elements in pitting corrosion of Al-Zn, Al-Mg, and
polarization resistance decreases as the Cu content Al-Cu binary alloys in dearated 1 M NaCl. Zn, Mg,
increases, which has been attributed to the Cu and Cu as alloying elements have different effects on
enrichment on the surface. the pitting potential of Al alloys (Fig. 9). Pitting
potential decreased greatly with increasing Zn content
up to 3wt% and remained the same with further
increase in Zn content. There was no influence of
Mg on pitting potential. Pitting potential increased
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(S),Al2CuMg (S) and Al20Cu2(Fe Mn)3 52-53. The when exposed in acidic solution or chloride solution.
coarse intermetallics Al3Fe, Al7Cu2Fe, Al2CuMg, and Mg 2Si phase in AA6000 dealloyed in 0.1 M
Mg2Si are found in Al-Zn-Mg-Cu alloys such as phosphoric acid and MgO was found on the Mg2Si
AA7075-T6. The fine precipitates for AA2024-T3 particles. Buchheit and coworkers58,60-62 studied the
and AA7075-T6 are Al2CuMg and Mg (Zn Cu Al)2, electrochemical behavior of S (Al2CuMg) phase in
respectively. As mentioned earlier, intermetallic the form of both synthesized bulk and real phases in
particles play a crucial role in localized corrosion of AA2024-T3. They found that S phase supported rapid
Al alloys. The coarse intermetallic particles mentioned anodic and cathodic reaction kinetics and selective
above can be further divided into two groups: active dissolution of Mg and Al readily occurred under
and noble particles relative to the Al matrix. Al2Cu, anodic and cathodic polarization. Dealloying of active
Al3Fe, Al7Cu2Fe, and Al20Cu2 (Fe Mn)3 are found S phase left Cu-rich remnants, which was cathodic to
to be noble to the matrix, while Al2CuMg and Mg2Si the matrix and therefore caused grooving by alkaline
are active to the matrix. Buchheit 54 compiled the dissolution and then pitting at the dealloyed S phase.
corrosion potentials of various intermetallic phases in They also proposed that decomposition of Cu-rich
Al alloys, showing that the intermetallics exhibit remnants of S phase resulted in Cu release and
different electrochemical properties from the matrix. redistribution, which further accelerated corrosion of
Pits are readily found at the periphery of noble the Al alloys. This hypothesis has been supported by
particles in Al alloys during exposure to chloride RRDE experiments on S particles. The details about
solution. It is generally accepted that noble Fe- or Cu enrichment and redistribution will be reviewed
Cu-containing intermetallic particles act as cathodes below. In summary, alloying addition and various
and support oxygen reduction. As a result, a high pH intermetallic particles play an important role in the
local environment is established at the noble particles, corrosion properties of Al alloys.
which causes grooving of the surrounding Al matrix
by alkaline dissolution. The alkaline attack must then 3.3 Cu Enrichment and Redistribution
somehow switch to acid attack to result in a stable
The critical role of intermetallic particles in localized
pit, which requires an acid environment.
corrosion of Al alloys was described previously. Many
Electrochemical studies have been conducted on Al3Fe studies revealed that Cu-containing intermetallic
and Al2Cu 55-57. Nisancioglu found that near the particles govern the corrosion of high strength Al
open circuit potential in NaOH solution, Al3Fe alloys due to the noble nature of the Cu rich particles.
underwent a preferential dissolution of Al, which In chloride environment, Cu-rich particles,
resulted in an Fe rich surface55. It was suggested that particularly Al2CuMg (S) particles, often lead to Cu
Fe enrichment on the Al3Fe surface is detrimental to enrichment and redistribution, which in turn is
cathodic behavior due to the formation of a protective detrimental to corrosion resistance. Buchheit and
Fe oxide. The presence of Mn and Si in Al3Fe can coworkers58,60-62 attributed Cu enrichment in AA2024
reduce the effect of Fe on both anodic and cathodic to dealloying of S-phase, which accounts to about
rates. Mazurkiewicz and Piotrowski57 found that 60% of total intermetallic particles (Fig. 11). S phase
Al2Cu underwent dissolution to form Al and Cu ions is susceptible to dealloying in acidic solution or
at the open circuit potential and under anodic chloride solution. Selective dissolution of Mg and Al
polarization in sulfate solutions. Cu ion release was leaves behind Cu rich sponge remnants. Buchheit
also found in Rotating Ring-Disk Electrode (RRDE) et..al62 further pointed out that Cu redistribution was
experiments on Al2Cu and Al7Cu2Fe at the OCP and attributed to the formation and re deposition of Cu
under anodic and cathodic polarization in chloride ions although the corrosion potential of AA2024 is
solution . well below the reversible potential for Cu/Cu2+.
There are two possible explanations for this seemingly
The corrosion potentials for Mg2Si (D) and Al2CuMg thermodynamic contradiction. They proposed that the
(S) particles in chloride solution are -1.59 and -0.92 Cu rich sponge remnants undergo physical coarsening,
V SCE, respectively. Both Mg-containing phases are which results in non faradaical liberation of
active to the matrix and act as anode. They are mechanically and electrically isolated metallic Cu
susceptible to active dissolution or Mg dealloying clusters.
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Fig.11 : (a) Optical picture and (b) Schematic representing Cu enrichment redistribution during localized corrosion in
AA2024-T3
Metallic Cu clusters suspended in the solution or view point, the curvature effect is thought to be
isolated in the corrosion product can achieve a responsible for the formation of Cu ions rather than
corrosion potential that is not controlled by the alloy the liberation of metallic Cu clusters. The curvature
potential. In an aerated solution, metallic Cu is of Cu rich clusters on the surface shifts the reduction
oxidized into Cu ions. Dissolved Cu2+ ions can drift potential for Cu in the anodic direction (equation 1),
around by solution convection and redeposit on the dramatically when the radius r is very small.
alloy surface, reducing back to metallic Cu. This
then leads to the localized corrosion in other places. 2γ Cu Ω Cu
E Cu = E Cu − (1)
63-64 nFr
Sieradzki and coworkers proposed a different
viewpoint that Cu ions are formed directly from Cu where E Cu is the potential of the Cu rich remnant,
rich sponge remnants on the alloy surface. In this E Cu is the reversible potential for Cu, n is
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When localized corrosion does occur in aluminum a knife-edge attack parallel to at some distance from
welds, it may take the form of preferential attack of weld.
the weld bead, pitting, intergranular attack or
exfoliation may occur in a HAZ a short distance Gas tungsten arc welding (GTAW) and Gas Metal
from weld bead. Welds in Al-Mg-Si alloys (AA6061) Arc Welding (GMAW) processes are widely used for
generally have a good resistance to atmospheric joining aluminium alloys for various applications like
corrosion, but in specifically corrosive environments aerospace, defence and automotive industries. The
like seawater localized corrosion may occur. Welds resistance to corrosion of aluminium alloy welds is
in Al-Cu alloys (AA2014, AA2219, AA2026), Al- affected by the alloy being welded and by the filler
Zn-Mg-Cu alloys (AA7075) and Al-Zn-Mg alloys alloy and the technique used. Galvanic cells that cause
(7039) have less corrosion resistance, due to corrosion can be created because of the corrosion
metallurgical changes in the HAZ. Reheat treatment potential differences among the base metal, the filler
of the welded part might restore the original corrosion metal and the heat-affected regions where
resistance, but this is rarely possible. microstructural changes have been produced.
Some of the heat treatable alloys particularly those In the Aluminium-copper alloys, the heat-affected
containing substantial amounts of copper and zinc, zone (HAZ) becomes cathodic, where as in aluminum-
may have their resistance to corrosion lowered by the zinc alloys, it becomes anodic to the remainder of
heat of welding. These alloys exhibit grain boundary the weldment The corrosion potentials across the weld
precipitation in the HAZ and of this zone is normally zone for a 5xxx, 2xxx and 7xxx series weldment are
anodic to the remainder of the weldment. In a shown in Fig. 14.These differences in potential can
corrosive environment selective corrosion on the grain lead to localized corrosion as demonstrated by
boundaries may take place and in the presence of corrosion of the alloy 7005 shown in Fig. 15. The
stress this corrosion can proceed more rapidly. Post HAZ in the 5xxx alloy is mildly cathodic, where as
weld heat treatment provides a more homogeneous the 2xxx alloy exihibits a greater cathodic potential.
microstructure and improves the corrosion resistance The 7xxx series HAZ is anodic to the unaffected
of these alloys. Welds in Al-Zn-Mg alloy were seen material and would be of great concern. Selection of
to be attacked preferentially in an area adjacent to proper filler wire is important to avoid cracking during
the weld bead when exposed to a corrosive environment welding and to optimize corrosion resistance. When
in the as welded condition. Post weld aging for a the solution potential of the filler is same as that of
sufficient at a high enough temperature eliminated the base metal (4043 for 6061-T6 alloy), optimum
this preferential attack. Insufficient aging resulted in corrosion resistance is obtained. In some cases,
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Fig. 14 : Effect of the heat of welding on microstructure, hardness and corrosion potential of welds of three aluminium
alloys. (a) Alloy 5456-H3 with 5356 filler (b) Alloy 2219-T87 base metal with 2319 filler (c) Alloy 7039-T6 base
metal with 5183 filler
intermetallic phase formed by the base metal and influence on microstructure has the least chance of
filler wire determines the final corrosion resistance reducing the corrosion resistance of aluminium
of the weld, for example magnesium silicide formed weldments. The alloy with the more negative potential
during welding 5xxx alloy with 4043 filler can be in the weldment will attempt to protect the other
highly anodic to all other parts of the weldment 72. part. Thus if the weld metal is anodic to the base
metal (as 5356 weld in 6061-T6), the small weld can
In general, the welding procedure that has the least be attacked preferentially to protect the larger surface
area of the base metal.
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controlling the welding parameters and selecting proper number of metastable pits and the current spikes
filler wire suitable for the base metal composition increase with increasing applied potential below
and thermal temper. Recent unpublished work of the pitting potential and the chloride concentration.
authors proved that PMZ is a strong function of The potential distribution in pits is considered to
prior thermal temper of the Al-alloy like T-4, T-6 be another important factor to stabilize pit growth
and T-87.Similarly it was also found that width of and a pit must maintain a minimum current
the PMZ is less in pulsed current (PC) GTA welding density for stabilized growth.
compared to that of continuous current (CC) GTA
welding of Al-alloys. Improvement in corrosion 2. Pitting potential ( EP) and Repassivation potential
resistance in Pulsed GTA welds of 2219 and 6061 ( ER) can be used to evaluate the susceptibility
alloys has been attributed to the decrease in segregation to pitting corrosion of aluminium alloys and
and refinement of eutectic network of the weld metal. recently Electrochemical Impedance Spectroscopy
Corrosion studies on Heat Affected Zones with PMZs (EIS) has been recognized as the accurate method
in CC and PC GTA welds of AA2219 (T6 and T87) of determining the corrosion resistance of
and AA6061 (T4 and T6) indicated the significant aluminium alloys in solutions containing
influence of prior welding technique and prior thermal aggressive halide ions.
temper. HAZs of PC GTA welds of 2219-T87 and 3. The role of alloying elements was to mainly
6061-T4 are found be having higher corrosion change the surface over potential and shifting
resistance when compared to that of T-6 temper. the repassivation potential. Intermetallic particles
Corrosion damage is extensive in the PMZ area of weaken the passive film and are sites for pit
the HAZ due to grain boundary eutectic enrichment nucleation. Cathodic intermetallics produce a
and segregation of alloying elements during welding galvanic cell with aluminium matrix and act as
and this is evident from the optical microscopy and cathode for the oxygen reduction.These particles
scanning electron microscopy studies on GTA welds selectively dissolve and remnants from the
of 2219-T6 alloy (Fig. 16). Authors76 recently made particles dissolution- metallic Cu, Fe are still
an attempt to study the effect of prior copper removal more cathodic than the intermetallics. High pH
treatment on the corrosion resistance of the CC GTA local environment is established at these particles,
Welds of 2219-T6 and uniform pitting potential has which causes grooving of the surrounding al-
been achieved in all three zones of the weldment. matrix by alkaline dissolution.
To summarize welding will have a strong influence 4. Copper enrichment and re-distribution is the root
on the pitting corrosion of heat-treatable Al-alloys, cause of pitting in aluminium-copper alloys.
mainly microstructural changes in heat affected zone Chloride ions which accelerate the corrosion
and partially melted zone might lead to non-uniform process may be attributed to oxide film break
pitting potential across the weldment. Proper care down or assisting the anodic reaction.
has to be taken in the selection of welding technique
and the filler wire, depending on the base metal 5. Pitting corrosion resistance of heat-treatable
history of the Al-alloy. aluminium alloy welds depend strongly on
welding technique and the prior thermal temper.
6. CONCLUSIONS Partially melted zone of the Al-alloy welds is
severely damaged by corrosion and is attributed
1. In general, pitting corrosion involves three stages: to the grain boundary eutectic enrichment and
pitting initiation, metastable pitting, and pitting segregation.
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