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THE EFFECT OF HEAVY METAL IONS ON THE
LOCALIZED CORROSION BEHAVIOR OF STEELS1
Anees U. Malik, Mohammad Mobin, Ismail Andijani,
Fahd Al-Muaili and Mohammad Al-Hajri
Saline Water Desalination Research Institute
Saline Water Conversion Corporation (SWCC)P.O.Box 8328, Al-Jubail 31951, Saudi Arabia.
E-mail: [email protected]
SUMMARY
The localized corrosion is the most serious problem encountered in a processing plant
such as desalination and power plants. The carryover of metal ions by the liquid,
aerosol and vapors appears to be the primary cause of corrosion in evaporators,
distillate system, boiler tubes, turbines, distillate pipelines and other systems of
desalination and power plants. The deposition of carryover heavy metals/oxides on
steel components in MSF desalination or power plants is a common problem and
reported by many authors. The deposits may initiate localized attack in the form of
pitting or crevice corrosion. The pits act as initiators of stress corrosion in the form of
stress corrosion cracking, corrosion fatigue or intergranular corrosion and result in
the failure of components. However, this aspect has been given little attention and is
least understood yet has great relevance to seawater desalination and power plants.
Keeping in view the above facts, a research project entitled, “The effect of heavy metal
ion on the localized corrosion behavior of steels” was formulated by the Corrosion
Department of R&D Center Al-Jubail.
The project contains the results of an investigation concerning with the effect of heavy
metal ions, e.g., Cu, Ni and Zn on the localized corrosion behavior of carbon steel and 316L under different experimental conditions. The work of the project was divided into
five major tasks, namely, literature survey; material and equipment acquisition;
immersion test under static condition; immersion test under dynamic condition; and
electrochemical studies.
Immersion tests of 1, 6 and 12 months duration were carried out to determine the
effect of metal ions on the corrosion rate of steels. The effect of Si a light non-metallic
1Issued as Technical Report: TR. 3804/APP 96010 in March, 2005.
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element has been specifically studied. The important experimental conditions, which
include the nature of aqueous medium, metal ion concentration, temperature, pH and
flow condition, have been taken into account. In general, there is a negligible effect of
metal ions on the corrosion rate of 316L in presence of 50 ppb, 1 ppm and 100 ppm
concentration in either seawater or distillate water under different experimental
conditions. The effect of metal ions on the corrosion rate of carbon steel is quite
pronounced and follows interesting trends. The results from immersion tests show a
decrease in the corrosion rates of carbon steel in distillate water containing higher
concentration of Cu and Ni under both static and dynamic conditions. In seawater, a
higher concentration of Cu is detrimental under dynamic condition. The presence of Zn
in the aqueous medium influences the corrosion behavior of steel differently than that
of Cu and Ni. A higher concentration of Si in seawater, under dynamic condition,
effectively decreases the corrosion rate.
Electrochemical techniques like free corrosion potential, potentiodynamic polarization
and polarization resistance measurements and AC impedance have been used to
investigate the role of heavy metal ions on the corrosion behavior of carbon steel and
SS 316L. The instantaneous corrosion parameters as obtained by electrochemical
techniques show an increase in corrosion rates with increasing metal ion
concentrations. Under controlled laboratory conditions, there is no evidence of
localized attack in presence of different concentrations of metal ions.
1. INTRODUCTION
Corrosion is the major cause of component or material failure in desalination and
power plants. Though one or more forms of corrosion are involved during corrosionfailure in desalination plants general and pitting corrosion are more common modes of
failures [1]. In seawater processing systems, if dissolved oxygen and pH are under
control, general corrosion is the predominant mode of attack on conventional
construction materials such as carbon steel. This form of corrosion is easily
controllable and is desirable in the sense that it permits predictive estimates of service
life. Pitting, the most detrimental form of attack, is often responsible for the corrosion
failures of components in desalination and power plants. In process plants, it accounts
at least 90% of metal damage by corrosion [2]. Though there are several causes of
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pitting, the attack of certain aggressive anions on the protective oxide film on the metal
appears to be most widely referred to in the corrosion literature [3,4]. Stainless steels
particularly austenitic lose their protectivity in presence of chloride ions and undergo
pitting. Steels invariably undergo pitting under stagnant or low fluid velocity
conditions [5, 6, 7]. Contact with heavy metal ions such as copper is another cause
which has been attributed to pitting of steels [8]. This aspect has been given little
attention and is least understood yet has great relevance to seawater desalination and
power plants [9]. A number of cases have been reported regarding the copper induced
pitting corrosion of iron and galvanized pipes and tanks in recirculating hot water
system [10-13]. A copper concentration of 0.1 mg/l was found to be sufficient to cause
accelerated attack.
In multistage flash (MSF) desalination plants, as a result of condenser tube corrosion,
the re-circulating brine has high copper content. This can deposit in the flash chambers
and accelerate the corrosion of steel due to high Cu/Fe local cell action [14]. In a AISI
316L distillate line from an MSF desalination plant, green deposits of copper rich oxide
were found, on removing the deposits, deep pits were observed. The pitting was
attributed to carryover copper from the heat exchanger by the distillate [15].
The frequent deposition of copper oxide in the distillate system has been reported in the
MSF desalination plants of Abu Dhabi [16]. The presence of high concentration of
copper in the distillate was due to the deterioration of protective copper oxide during
the start up following outage.
In steam turbines, the deposits along the steam path resulting from boiler carryover are
most problematic. These deposits are detrimental to efficiency, and can have a drastic
effect on turbine reliability because of increased thrust loading and possibility of stress
corrosion cracking of steam path components from high levels of salts/metal oxide
carryover. A study of the corrosion related problems in steam generating equipment
indicates that while 26% of the failures are attributed to pitting, 57% are caused by the
deposition blades [17]. These deposits are formed from high dissolved and suspended
slit carry over of steam.
Besides copper, silicon compounds like SiO2 or Na2SiO3 form important constituent of
turbine deposits. As SiO2, it is non-aggressive but may possibly act synergistically to
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enhance the corrosion effect of other elements or compounds. Na2SiO3 has been found
very effective in controlling corrosion of carbon steel by many investigators and the
optimum quantity of Na2SiO3 required to suppress the corrosion has been cited as less
than 10 ppm [18]. In unbuffered solutions, Na2SiO3 is effective as corrosion inhibitor
for iron by inhibiting anodic dissolution of the metal [19]. The compound Na2SiO3
dissociates in water solution to form SiO2 and NaOH and could be very aggressive to
some material such as Ti alloys and steam rotor alloys [20].
The present investigation concern with the effect of heavy metal ions such as Cu, Ni
and Zn on the localized corrosion behavior of carbon steel and AISI 316L under
different experimental conditions. The effect of silicon a light non-metallic element
has been specifically studied. The important experimental conditions which include
the nature of aqueous medium, metal ion concentration, pH and flow conditions have
been taken into account. Immersion tests and electrochemical techniques have been
employed to study the effect of heavy metal ions on the corrosion behavior of steels.
The results of the study shall provide important information about the role of heavy
metal carryover on the failure of desalination and power plant components.
2. EXPERIMENTAL DETAILS
The corrosion behavior of steels in presence of heavy metal ions were studied by
carrying out experiments under different sets of conditions. The conditions are as
follows:
Steels used for testing : Carbon steel, AISI 316L
Aqueous test media : Distillate water, filtered raw seawater
Heavy metal ions : Cu, Ni, Zn (effect of Si, a light non-metallicelement was specifically studied)
Metal ion concentration in : 100 ppm, 1 ppm, 50 ppb
the test media
pH of the test media : 4 (moderately acidic), 6.5 (neutral) and 8.5
(basic)
Temperature : 25 oC
Flow condition : Static, dynamic
Duration of immersion test : 1, 6 and 12 months
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under static condition
Duration of immersion test : 1 month
under dynamic condition
Both immersion (weight loss measurements) and electrochemical techniques were used
to determine the effect of heavy metal ion on the corrosion behavior of steels.
2.1 Immersion Tests
2.1.1 Preparation of Specimens
Commercially available carbon steel and 316L were used for immersion tests.
Coupons of dimension 2.4 x 2.4 x 0.3 cm were cut from the sheet. The coupons were
machined and abraded on 180 grit SiC paper to simulate the near service condition. To
hold the specimens, a hole of 1.5 mm dia. was made near the edge. The abraded
coupons were washed, degreased with ethyl alcohol and dried up. The composition of
steels as analyzed by optical emission spectrometer is given in Table 1.
2.1.2 Preparation of Test Solution
The test solutions were made up with distillate water and filtered raw seawater. The
composition of Arabian Gulf seawater is given in Table 2 [21]. The solutions
containing 100 ppm, 1 ppm and 50 ppb of Cu, Ni, Zn and Si, respectively were
prepared in distillate water and filtered raw seawater using Analar grade BDH
chemicals. The pH of the solutions was adjusted using NH4OH and CH3COOH. For the
test solutions made up with distillate water a pH of 4, 6.5 and 8.5 was maintained
whereas for the test solutions made up with seawater a pH of 8.5 was maintained. The
test solutions containing Si was prepared using Na2SiO3 and stored in plastic
containers. In case of Si the test solution pH was not maintained to 6.5 to avoid theprecipitation at higher concentration.
2.1.3 Immersion Test Procedures
Immersion tests were conducted in accordance with ASTM designation G31-72
(Reapproved 1990) which entitled, “Laboratory Immersion Corrosion Testing of
Metals”. After taking the initial weight and dimensions, the coupons were hanged in
the test solution containing varying concentration of metal ions with the help of nylon
thread. A blank experiment, in absence of heavy metal ions, was also carried out for
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comparison purpose. In order to avoid galvanic and crevice corrosion, the coupons
were loosely tied with the nylon threads. The immersion tests were carried out under
both static and dynamic conditions. Under static condition, the test runs were of 1, 6
and 12 months duration whereas under dynamic condition the runs were of 1 month
duration. After completion of the immersion test, the specimens were taken out and
cleaned following ASTM designation G1-90 which entitled, “Standard Practice for
Preparing, Cleaning and Evaluating Corrosion Test Specimens” and observed for any
localized attack. The average corrosion rate was determined by the following
relationship:
Where K = Constant, 3.45 x 106 for mpy
W = Mass loss in g, to nearest 1 mg
A = Area in cm2 to the nearest 0.01 cm2
T = Time of exposure in hours to the nearest 0.01 h
D = Density in g/cm3
2.2 Electrochemical Tests
The electrochemical tests like free corrosion potential, potentiodynamic and
polarization resistance measurements and electrochemical impedance were carried out
to investigate the effect of heavy metal ions on the corrosion behavior of steel. The
electrochemical tests were carried out on Solartron AC Impedance System which
comprised of 1250 B frequency response analyzer with blank front panel and 1287
electrochemical interface unit. The experiments were carried out using a corrosion cell
from EG & G model K0047 with saturated calomel electrode (SCE) as reference and
graphite rod as counter electrode.
2.2.1 Preparation of Specimens
Circular specimens with 1.5 cm diameter were punched from 3 mm thick carbon steel
and 316 L sheets. A nichrome wire was soldered to one face of the specimens for the
electrical connection and the specimens were then mounted in epoxy resin to provide
crevice free mount. The exposed circular face was ground to 180 grit SiC paper. The
ground specimens were washed, degreased and dried up.
2.2.2 Preparation of Test Solution
DxT xA
xW K rateCorrosion =
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The procedure for the preparation of test solutions for electrochemical tests was similar
to that adopted for immersion tests.
2.3 Free Corrosion Potential Measurements
The free corrosion potential measurements of carbon steel and SS 316L were carried
out in both distillate water and filtered raw seawater for a period of 1 month. The
measurements were carried out in presence and absence of metal ions at room
temperature under static condition. The change in voltage against SCE used as
reference electrode, was plotted vs time.
2.4 Potentiodynamic Polarization Measurements
Potentiodynamic polarization measurements were carried out using a scan rate of 0.166
mV/s commencing at a potential above 250 mV more active than stable open circuit
potential. To observe the effect of a particular metal ion in a given medium,
potentiodynamic curves were obtained using the same specimen under similar
experimental condition except a periodic change in metal ion concentration. However,
before starting the polarization scan at each concentration, the specimen was stabilized
for about 1 hour for attaining a steady state which was shown by a constant potential.
2.5 Polarization Resistance Measurements
Polarization resistance measurements were conducted at a scan rate of 0.166 mV/s with
starting and final potential corresponding to -15 mV to + 15 mV vs open circuit
potential, respectively. The maximum current range was 0.1µ A. All the
measurements were completed on the same day with the same specimen. However,
metal ion concentration was periodically changed and before starting the measurements
at each concentration, the specimen was left for about 1 hr for attaining a steady state
which was indicated by a constant potential.
2.6 AC Impedance Measurements
The electrochemical impedance measurements were performed under potentiostatic
conditions at the free corrosion potential. Amplitude sine wave signal was 10 mV over
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the frequency range of 1 KHz to 1 mHz with five points per decade. All the ac
impedance measurements were performed before polarization resistance
measurements. However, before each measurement the specimen was left to attain a
constant potential.
3. RESULTS
3.1 Immersion Tests (weight loss measurements)
The corrosion rates of carbon steel and 316 L in presence and absence of metal ions
under different experimental conditions, as obtained by weight loss measurement
technique are given in Tables 3-10. The results for carbon steel and SS 316L are
summarized separately.
3.1.1 Carbon Steel
Tables 3-6 show the effect of metal ions on the corrosion rate of carbon steel in both
distillate and filtered raw seawater at different pH at 25 oC. In absence of metal ions,
the corrosion rate of carbon steel in distillate water (under both static and dynamic
conditions) and filtered raw seawater (under static condition) are almost the same.
However, in filtered raw seawater, under dynamic condition, there is a large increase in
the corrosion rate of carbon steel. The effect of different metal ions on corrosion rate of
carbon steel is described as follows:
(1) Effect of Copper
In distillate water, under static condition, the presence of 50 ppb and 1 ppm of copper
at both pH 6.5 and 8.5, appears to have negligible effect on the corrosion rate of carbon
steel. However, under dynamic condition there is a large increase in corrosion rate in
presence of 50 ppb and 1 ppm of copper. The highest corrosion rate of 28 mpy is
noticed in presence of 1 ppm of copper. A lowering in the corrosion rate is noticed at
100 ppm of copper concentration under both static and dynamic conditions. In filtered
raw seawater, under static condition, the corrosion rate increases slightly with
increasing copper ion concentration. However, under dynamic condition a large
increase in corrosion rate is observed only in presence of 100 ppm of copper, at other
concentrations, there is no appreciable change in the corrosion rates.
(2) Effect of Nickel
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The presence of nickel in both distillate water and seawater has almost similar effect to
that of copper on the corrosion rate of carbon steel. In distillate water, the highest
corrosion rate of 33 mpy is observed in presence of 50 ppb of nickel under dynamic
condition, this is followed by a corrosion rate of 21 mpy in presence of 1 ppm of
nickel. Both under static and dynamic conditions, a lowering in corrosion rate is
observed only in presence of 100 ppm of nickel. In seawater, under static condition
though there is a slight increase in corrosion rate with increasing metal ion
concentration, there is no significant effect under dynamic condition.
(3) Effect of Zinc
In distillate water, under static condition, except for 100 ppm of zinc ion concentrationwhich indicated an increase in the corrosion rate, there is no appreciable effect of zinc
on the corrosion rate of carbon steel. Under dynamic condition, corrosion rate is
almost unaffected in presence of all the three concentration of zinc. In seawater, under
static condition, the presence of zinc has no significant effect on the corrosion rate of
carbon steel. However, under dynamic condition there is a decrease in the corrosion
rate in presence of zinc at all the three selected concentrations.
(4) Effect of Silicon
The effect of silicon, a light non-metallic element, on the corrosion rate of carbon steel
was specifically studied. The silicon solution in distillate water and seawater were
specially made and kept in plastic containers. The immersion tests were also carried
out in plastic vessels. In both distillate and seawater, under static condition, presence
of silicon appears to have no significant effect on the corrosion rate of carbon steel.
However, under dynamic condition, the corrosion rates appear to decrease with
increasing Si concentration.
3.1.2 SS 316L
Tables 7-10 show the effect of metal ions on the corrosion rate of SS 316L in both
distilled water and filtered raw seawater at different pH at 25 oC. The results are
obtained under static condition. SS 316L is unaffected in distilled water (pH 6.5) and
seawater (pH 8.5) for an immersion period of 1, 6 and 12 months duration. The effect
of different metal ions on the corrosion behavior of 316L is summarized as follows:
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(1) Effect of Copper, Nickel, Zinc and Silicon
In general, there is negligible effect of metal ions on the corrosion rate of 316L in
presence of 50 ppb, 1 ppm or 100 ppm concentration at pH 4, 6.5 or 8.5 for an
immersion period of 1, 6 or 12 months duration in both distilled water and seawater.
3.2 Electrochemical Studies
3.2.1 Free Corrosion Potential (E corr ) Measurements
Figures 1 to 9 show time vs free corrosion potential plots for carbon steel and SS 316L
immersed in distilled water (pH 6.5) and filtered raw seawater (pH 8.5) in presence and
absence of heavy metal ions under static condition. The results for carbon steel and SS
316L are summarized separately.
3.2.1.1 Carbon Steel
The free corrosion potential of carbon steel in distilled water, in absence of metal ions,
for the first 2 hrs is about -550 mV vs SCE; this is followed by an increase in potential
till a stable potential range of -650 to -750 mV is reached. However, in seawater
without metal ions, a potential of -650 mV is reached during the first 2 hrs, this is
followed by an increase in potential till a stable potential range of -700 to -800 mV is
reached. The results of the effect of heavy metal ions on the free corrosion potential of
carbon steel in both distilled water and seawater are summarized as follows:
(1) Effect of Copper
Figures 1 and 2 show potential vs time plots for carbon steel in distilled water and
seawater containing 0, 1 and 100 ppm copper. In distillate water containing 1 ppm Cu,
a positive shift in Ecorr is noticed for the first 24 hours only whereas in presence of 100ppm Cu, a pronounced positive shift in Ecorr is noticed for a time period extending 17
days. In seawater, though, there is no significant effect of the presence of 1 ppm Cu
on the Ecorr of carbon steel, the presence of 100 ppm Cu slightly shifted the E corr in
noble direction and a potential below-650 mV is maintained for the time period
extending 17 days.
(2) Effect of Nickel
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In distillate water a significant ennoblement in Ecorr is observed in presence of both 1
and 100 ppm nickel (Figure 3). An initial decrease in negative potential was observed
in presence of both 1 and 100 ppm nickel, this is followed by a constant noble
potential. However, in presence of 1 ppm Ni after a time period extending 16 to 17
days, an increase in negative potential is observed till a potential equal to the potential
of carbon steel in absence of nickel is reached. In seawater, the effect of nickel on the
potential of steel is not much pronounced. In presence of both 1 and 100 ppm nickel
the potential is reached to above - 600 mV on the first day of immersion (Figure 4).
(3) Effect of Zinc
The Ecorr vs time plots for carbon steel in distilled water and seawater containing 0, 1
and 100 ppm zinc is shown in figures 5 and 6. In distillate water, though the potential
of carbon steel in presence of 100 ppm zinc is slightly below the potentials of carbon
steel, there is no significant effect of zinc on the Ecorr of carbon steel in both distilled
water and seawater.
(4) Effect of Silicon
Figure 7 shows the potential vs time plots for carbon steel in seawater containing 0, 1
and 100 ppm silicon. Though, there is no effect of presence of 1 ppm silicon on theEcorr of carbon steel, a major positive shift in Ecorr is observed in presence of 100 ppm
of silicon.
3.2.1.2 SS 316L
(1) Effect of Copper
Figure 8 shows the potential vs time plots for SS 316L in distillate water containing 1
and 100 ppm copper. An increase in copper ion concentration shifts the Ecorr of 316L in
more noble direction.
(2) Effect of Nickel
Figure 9 shows the potential vs time plots for SS 316L in distillate water containing 1
and 100 ppm nickel. After an initial negative shift in Ecorr , the increasing nickel ion
concentration appears to shifts the Ecorr of 316L in more noble direction.
3.2.2 Potentiodynamic Polarization Measurements
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Figures 10 to 15 show potentiodynamic curves for carbon steel in distilled water and
seawater containing different concentrations of metal ions. The values of corrosion
potential, Ecorr and corrosion current, Icorr for carbon steel in distilled water and
seawater in presence of 0, 50 ppb, 1 ppm and 100 ppm metal ions, as computed from
potentiodynamic curves, are given in Table 11. In general, though there is no
significant effect of the presence of 50 ppb and 1 ppm of metal ions on the E corr and Icorr
values, the presence of 100 ppm of metal ions in both distillate water and seawater has
pronounced effect on the Ecorr and Icorr values. In presence of 100 ppm of Cu and Ni an
increase in Icorr values is observed whereas in presence of 100 ppm Zn a reverse trend is
observed.
3.2.3 Polarization Resistance Measurements
The polarization resistance measurements were carried out on carbon steel immersed in
distilled water containing 0, 50 ppb, 1 ppm and 100 ppm of copper and nickel,
respectively. The measurements were carried out on duplicate samples. Typical
polarization resistance plots are shown in figures 16 to 19. Table 12 lists the
polarization resistance values, R p computed from linear polarization plots. The results
from the polarization measurements show a negative shift in Ecorr and lowering in R p
values with increasing copper and nickel ion concentration in the distilled water.
3.2.4 AC Impedance Studies
The effect of heavy metal ions on the corrosion behavior of carbon steel in distilled
water was studied by electrochemical impedance spectroscopy (EIS). The technique is
unique as it allows the quantitative study of corrosion behavior of low corroding
systems which is not entirely possible by conventional dc techniques. Parameters such
as solution resistance, R S, polarization resistance, R P and interfacial capacitance, C
evaluated from EIS proved to be useful in studying corrosion kinetics and associated
interfacial phenomenon.
Nyquist curves were obtained to study the effect of heavy metal ions on the corrosion
behavior of carbon steel. Nyquist plot is obtained by plotting the imaginary impedance
(Z”) against real impedance (Z’) at each excitation frequency. At high frequency, the
impedance is almost entirely created by solution resistance (R P +R S). The R P
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(inversely proportional to the corrosion rate of exposed metal surface) is the difference
between low frequency limit and high frequency limit.
Figures 20 to 23 show Nyquist plots for carbon steel in distilled water containing
varying concentration of heavy metal ions. The results obtained from Nyquist plots are
listed in Table 13. Though a well defined semicircle characteristics of Nyquist plot is
lacking, the computed values of R P show a decreasing trend with increasing metal ion
concentration. The result is in conformity with the values of R P obtained from dc
experiment (linear polarization resistance measurements).
To observe the effect of metal ion concentration with time, the ac impedance
measurement of carbon steel in distilled water containing 100 ppm nickel was extended
for 1 month. The results are summarized in Table 14.
4. DISCUSSION
The effect of heavy metals like Cu, Ni and Zn and a non-metal Si on the corrosion
behavior of carbon steel and 316L was studied in the pH range of 4 to 8.5 at room
temperature under both static and dynamic conditions. Carbon steel shows a complex
dependence of corrosion rate on pH. In near neutral pH range (5 <pH<9), pH no more
plays a direct role in corrosion [22]. The major reaction governing corrosion in most
practical application in this pH range is the reduction of oxygen present in the solution.
Therefore, under static condition, the pH range under study is not expected to play a
significant role in corrosion and any change in the corrosion behavior of steel may be
expected to be brought about by presence of metal ions in the solution. However,
under dynamic condition in addition to the presence of metal ions the agitation of
solution and presence of solids in the solution may also affect the corrosion rate. The
changes in seawater chemistry and that of biological activities in the test solution with
time and addition of heavy metal ions were not monitored, as these parameters under
the experimental conditions designed for this study are not expected to affect the
corrosion behavior significantly. Further, the monitoring of these parameters were
beyond the scope of project objectives as the main aim of this study was to establish a
baseline data considering the effect of heavy metal ions on the localized corrosion
behavior of steel, if present in test solution. The important parameters affecting
corrosion rate under experimental conditions of this study are well documented and
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supported by relevant reference [22]. In case of steel, in presence of dissolved oxygen,
the corrosion process is controlled by cathodic diffusion and solution agitation is
expected to cause an increase the corrosion rate. The presence of fine suspended solid
particles in the solutions may also cause an increase in corrosion rate due to their
movement over the steel surface. This is evident from the results of immersion studies
for carbon steel, in absence of metal ions, in pH range of 6.5 to 8.5 under dynamic
condition. The corrosion rate in distillate water is unchanged whereas in seawater there
is a large increase in corrosion rate.
Considering the results of immersion test for 316L there is negligible or no effect of the
presence of metal ions on the corrosion rate in both distilled water and seawater in the
pH range of 4 to 8.5. However, the effect of metal ions on the corrosion rate of carbon
steel is quite pronounced and follows interesting trends. Under experimental
conditions the presence of Cu and Ni in both distillate water and seawater has similar
effect on the corrosion rates. In distillate water, a higher concentration of Cu and Ni
result in a decrease in corrosion rate under both static and dynamic conditions whereas
a lower concentration of Cu and Ni considerably increases the corrosion rate under
dynamic condition. In seawater, a higher concentration of Cu is detrimental under
dynamic condition.
An increase in corrosion rate of carbon steel in presence of Cu and Ni can be explained
on the basis of occurrence of two cathodic reactions whereas a lowering in corrosion
rate may be explained on the basis of formation of a stable protective barrier over the
steel surface by the deposited metal. In presence of dissolved oxygen and metal ions
the anodic and cathodic reaction may be written as follows:
Anodic reaction: Fe→ Fe2+ + 2 ē (1)
Cathodic reaction: (Cathodic reactions in pH range of 6.5 to 8.5 are reduction of O 2 and
the metal ions)
½ O2 + H2O + 2 ē → 2OH- (2)
M++ + 2 ē → M (3)
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Since during metallic corrosion, the total rate of oxidation equals to total rates of
reduction, the dissolution rate of steel equals to the reduction rates of O2 and metal ions
and hence the initial corrosion rate of carbon steel in presence of metal ions is expected
to increase. After reduction of the metal ions the resulting metal get deposited over the
steel surface and form a barrier which is likely to protect the steel from further
corrosion. The extent of protection offered to the steel shall depend upon the ability of
the deposited metal to form a stable protective barrier and nature of protection offered
to steel surface. The deposited Cu and Ni protect the steel cathodically. In aqueous
medium containing high concentration of Cu and Ni a stable protective barrier is more
likely to be formed and hence a lowering in corrosion rate is observed. In presence of
lower concentration of metal ions the observed increase in corrosion rate is due to
absence of a stable protective barrier. In seawater the observed increase in corrosion
rate in presence of 100 ppm Cu under dynamic condition is due to erosive action of
fine suspended solid particles on the barrier film.
In presence of Zn, the corrosion rate of carbon steel in distillate water under both static
and dynamic conditions is unaffected except at higher concentration of metal. Since
Zn is anodic to steel, under the given experimental conditions, it is unlikely to get
reduced and deposit over steel surface and thus decrease the subsequent rate of
corrosion. However, it may remain in the solution in the ionic form affecting the
conductivity of the test solution. The observed increase in corrosion rate in presence of
100 ppm of Zn may be accounted due to the increase in the conductivity of the
solution. In seawater, with increasing metal ion concentration a lowering in corrosion
rate under dynamic condition is probably due to limited transfer of dissolved O2 from
bulk solution to the surface. The presence of higher concentration of Si in the aqueous
medium appears to be effective in lowering down in the corrosion rate of carbon steelunder dynamic condition. The effectiveness of Na2SiO3, under dynamic condition, in
lowering down the corrosion rate of carbon steel has already been established [18].
The results of immersion tests find support from free corrosion potential
measurements. The Ecorr of carbon steel in distillate water and seawater is in the range
of -650 to -750 mV and -700 to -800 mV vs SCE, respectively. In distillate water
containing 100 ppm of Cu and Ni a positive shift is E corr is noticed which is maintained
for a considerable period of time. A positive shift in Ecorr is indicative of the protection
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offered to steel surface. In seawater containing 100 ppm of Cu and Ni the shift is not
much significant. The presence of Zn in the aqueous medium does not affect the Ecorr
significantly whereas the presence of 100 ppm Si in seawater shifts the Ecorr
considerably in noble direction. For 316L also an increasing concentration of metal
ions in the aqueous medium appears to shift the Ecorr in noble direction.
The corrosion parameters obtained from potentiodynamic and linear polarization
measurements show an increase in Icorr and lowering in R p values, respectively with
increasing Cu and Ni ion concentrations indicating an increase in corrosion rate of
carbon steel with increasing metal ion concentration in the aqueous medium. The
parameters measured by the above techniques are instantaneous and the increase in
instantaneous corrosion rate with increasing metal ions concentration is expected and
can be explained on the basis of occurrence of two cathodic reactions (Equ. 2 and 3).
5. CONCLUSIONS
(1) Under controlled laboratory conditions the results from immersion and
electrochemical tests show no evidence of localized attack on carbon steel and
316L in presence of different concentration of heavy metal ions.
(2) The results from immersion tests in the pH range 4 to 8.5 at room temperature
show no effect of metal ions on the corrosion rate of 316L.
(3) The effect of metal ions on the corrosion rate of carbon steel in the pH range of
6.5 to 8.5 at room temperature is quite pronounced and follows interesting
trends.
(4) The presence of Cu and Ni in the aqueous medium produces almost similar
effect on the corrosion behavior of carbon steel.
(5) The corrosion rate of carbon steel in distilled water containing higher concentration of Cu and Ni decreases under both static and dynamic conditions.
In seawater, however, a higher concentration of Cu is detrimental under
dynamic condition.
(6) The presence of Zn in the aqueous medium influences the corrosion behavior of
steel differently than that of Cu and Ni.
(7) A higher concentration of Si in seawater, under dynamic condition, effectively
decreases the corrosion rate of carbon steel.
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Table 3. Effect of Copper on the Corrosion Rate of Carbon Steel at Different pH
Under Static and Dynamic Condition at 25oC
Corrosion Rate (mpy)Aqueous Test
Medium
pH Flow
Condition
Ion
Concentration 1 Month 6 Month 12 Month
Distillate Water 6.5 Static Nil 2.669 2.305 2.309" 6.5 Static 50 ppb 2.776 2.416 2.306
" 6.5 Static 1ppm 3.324 0.092 2.012
" 6.5 Static 100ppm 0.724 0.049 0.032
" 8.5 Static 50 ppb 2.838 3.043 2.738
" 8.5 Static 1ppm 0.771 3.006 3.246
" 8.5 Static 100ppm 0.890 0.102 1.212
" 6.5 Dynamic Nil 2.088
" 6.5 Dynamic 50ppb 13.523
" 6.5 Dynamic 1ppm 28.059
" 6.5 Dynamic 100ppm 0.478Filtered Raw
Seawater
8.5 Static Nil 2.668 1.757 1.836
" 8.5 Static 50ppb 2.811 2.392 1.907
" 8.5 Static 1ppm 2.623 2.375 2.208
" 8.5 Static 100ppm 3.366 4.574 4.499
" 8.5 Dynamic Nil 18.917
" 8.5 Dynamic 50ppb 17.819
" 8.5 Dynamic 1ppm 15.822
" 8.5 Dynamic 100ppm 27.527
Table 4. Effect of Nickel on the Corrosion Rate of Carbon Steel at Different pHUnder Static and Dynamic Condition at 25
oC
Corrosion Rate (mpy)Aqueous Test Medium pH
Flow
ConditionIon Conc.
1 Month 6 Month 12 Month
Distillate Water 6.5 Static Nil 2.669 2.305 2.309
" 6.5 Static 50 ppb 2.636 2.421 2.763
" 6.5 Static 1ppm 3.035 3.007 3.274
" 6.5 Static 100ppm 0.110 0.039 0.006
" 8.5 Static 50 ppb 3.311 2.654 2.691
" 8.5 Static 1ppm 3.429 0.085 2.656
" 8.5 Static 100ppm 1.328 0.050 0.028" 6.5 Dynamic Nil 2.088
" 6.5 Dynamic 50ppb 32.9822
" 6.5 Dynamic 1ppm 21.0646
" 6.5 Dynamic 100ppm 1.2971
Filtered Raw Seawater 8.5 Static Nil 2.668 1.757 1.836
" 8.5 Static 50ppb 2.638 1.889 1.719
" 8.5 Static 1ppm 2.851 2.032 1.772
" 8.5 Static 100ppm 4.181 2.840 2.933
" 8.5 Dynamic Nil 18.917 - -
" 8.5 Dynamic 50ppb 16.273
" 8.5 Dynamic 1ppm 18.179" 8.5 Dynamic 100ppm 18.450
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Table 5. Effect of Zinc on the Corrosion Rate of Carbon Steel at Different pH Under
Static and Dynamic Condition at 25oC
Corrosion Rate (mpy)Aqueous Test Medium pH
Flow
ConditionIon Conc.
1 Month 6 Month 12 Month
Distillate Water 6.5 Static Nil 2.669 2.305 2.309" 6.5 Static 50 ppb 2.514 2.069 1.999
" 6.5 Static 1ppm 2.552 2.129 1.973
" 6.5 Static 100ppm 4.980 7.518 4.746
" 8.5 Static 50 ppb 2.971 2.565 2.237
" 8.5 Static 1ppm 2.455 2.958 2.324
" 8.5 Static 100ppm 3.864 3.012 0.052
" 6.5 Dynamic Nil 2.088
" 6.5 Dynamic 50ppb 0.737
" 6.5 Dynamic 1ppm 2.668
" 6.5 Dynamic 100ppm 2.043
Filtered Raw Seawater 8.5 Static Nil 2.668 1.757 1.836" 8.5 Static 50ppb 2.126 2.062 2.050
" 8.5 Static 1ppm 2.387 1.917 1.639
" 8.5 Static 100ppm 2.135 2.185 2.435
" 8.5 Dynamic Nil 18.917
" 8.5 Dynamic 50ppb 12.584
" 8.5 Dynamic 1ppm 9.927
" 8.5 Dynamic 100ppm 10.615
Table 6. Effect of Silicon on the Corrosion Rate of Carbon Steel at Different pH
Under Static and Dynamic Condition at 25oC
Corrosion Rate (mpy)Aqueous Test
MediumpH
Flow
Condition
Ion
Concentration 1 Month 6 Month 12 Month
Distillate Water 6.5 Static Nil 2.669 2.305 2.309
" 8.5 Static 50 ppb 2.789 2.842 3.099
" 8.5 Static 1ppm 2.790 2.216 2.748
" 8.5 Static 100ppm 3.583 2.653 3.030
" 6.5 Dynamic Nil 2.088
" 6.81 Dynamic 50ppb 3.412
" 7.10 Dynamic 1ppm 0.715
" 8.19 Dynamic 100ppm 1.377Filtered Raw
Seawater
8.5 Static Nil 2.668 1.757 1.836
" 8.5 Static 50ppb 3.721 1.975 1.844
" 8.5 Static 1ppm 2.259 1.918 1.608
" 8.5 Static 100ppm 1.817 1.591 1.854
" 8.5 Dynamic Nil 18.917
" 7.94 Dynamic 50ppb 16.937
" 8.10 Dynamic 1ppm 17.289
" 8.64 Dynamic 100ppm 10.158
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Table 7. Effect of Copper on the Corrosion Rate of 316L at Different pH Under Static
Condition at 25oC
Corrosion Rate (mpy)Aqueous Test
Medium
pHFlow
Condition
Ion Concentration
1 Month 6 Month 12 MonthDistillate Water 6.5 Static Nil - - -
" 6.5 Static 50 ppb - .0006 .0016
" 6.5 Static 1ppm .0039 - .00175
" 6.5 Static 100ppm - - .0003
" 8.5 Static 50 ppb - - -
" 8.5 Static 1ppm - .0059 .0009
" 8.5 Static 100ppm - .00198 -
" 4 Static Nil - - -
" 4 Static 50ppb - .00385 -
" 4 Static 1ppm - .00286 -
" 4 Static 100ppm - .00393 -Filtered raw
seawater 8.5 Static Nil 0.0059 .00132 .00165
" 8.5 Static 50ppb .0318 .0023 .00067
" 8.5 Static 1ppm - .0016 .00032
" 8.5 Static 100ppm .0155 .003 .00066
Table 8. Effect of Nickel on the Corrosion Rate of 316L at Different pH Under
Static Condition at 25oC
Corrosion Rate (mpy)Aqueous Test
Medium pHFlow
Condition
Ion
Concentration 1 Month 6 Month 12 Month
Distillate Water 6.5 Static Nil - - -
" 6.5 Static 50 ppb - .0066 .00255
" 6.5 Static 1ppm - .00745 .0009
" 6.5 Static 100ppm .00410 .0067 .0003
" 8.5 Static 50 ppb .01563 .00391 .0003
" 8.5 Static 1ppm .00421 .00537 -
" 8.5 Static 100ppm .00835 .00535 .0003
" 4 Static Nil - - -
" 4 Static 50ppb .00784 .00599
" 4 Static 1ppm - .00469 -
" 4 Static 100ppm .011995 .00644 .0009
Filtered raw
seawater 8.5 Static Nil 0.0059 .00132 .00165
" 8.5 Static 50ppb .0099 .00096 .0003
" 8.5 Static 1ppm .006 - .0003
" 8.5 Static 100ppm .006 .0006 .0003
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Table 9. Effect of Zinc on the Corrosion Rate of 316L at Different pH Under Static
Condition at 25oC
Corrosion Rate (mpy)Aqueous Test
MediumpH
Flow
Condition
Ion
Concentration1 Month 6 Month 12 Month
Distillate Water 6.5 Static Nil - - -
" 6.5 Static 50 ppb .00766 .00639 -
" 6.5 Static 1ppm .00171 .00589 .0006
" 6.5 Static 100ppm .0222 .00635 .0029
" 8.5 Static 50 ppb - .00303 -
" 8.5 Static 1ppm .01519 .00435 .0003
" 8.5 Static 100ppm .02005 .00358 -
" 4 Static Nil - - -
" 4 Static 50ppb .00638 .00486 -
" 4 Static 1ppm .0125 .00466 -" 4 Static 100ppm .01945 .00504 -
Table 10. Effect of Silicon on the Corrosion Rate of 316L at Different pH Under Static
Condition at 25oC
Corrosion Rate (mpy)Aqueous Test
MediumpH
Flow
Condition
Ion
Concentr
ation. 1 Month 6 Month 12 Month
Distillate Water 6.5 Static Nil - - -
" 5.3 Static 50 ppb - .0032 -
" 6.0 Static 1ppm - .0032 .0003
" 9.5 Static 100ppm .00797 .00197 .0003
Filtered Raw
Seawater
8.5 Static Nil 0.0059 .00132 .00165
" 8.1 Static 50ppb - .0006 .00172
" 8.1 Static 1ppm - .0006 .0006
" 8.6 Static 100ppm - .0014 .0010
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Table 11. Values of Ecorr and Icorr for carbon steel in distillate water and seawater as obtained
by potentiodynamic polarization curves at room temperature
Alloy Medium Heavy Metal
ion
Metal in
Concentration
pH Ecorr (V) ICorr (Amp/cm2)
Carbon
steel
Distilled
water
Copper Nil 6.5 -0.453 6.788 x 10-6
” ” ” 50 ppb ” -0.469 8.528 x 10-6
” ” ” 1 ppm ” -0.471 7.371 x 10-6
” ” ” 100 ppm ” -0.002 2.046 x 10-5
” Seawater ” Nil 8.5 - -
” ” ” 50 ppb ” -0.756 8.360 x 10-6
” ” ” 1 ppm ” -0.751 5.529 x 10-6
” ” ” 100 ppm ” -0.750 4.891 x 10-5
” Distilled
water
Nickel Nil 6.5 -0.310 5.585 x 10-6
” ” ” 50 ppb ” -0.375 7.390 x 10-6
” ” ” 1 ppm ” -0.406 9.333 x 10-6 ” ” ” 100 ppm ” -0.659 2.817 x 10
-4
” Seawater ” Nil 8.5 - -
” ” ” 50 ppb ” -0.729 1.274 x 10-5
” ” ” 1 ppm ” -0.740 8.204 x 10-6
” ” ” 100 ppm ” -0.547 9.427 x 10-6
” Distilled
water
Zinc Nil 6.5 -0.466 8.022 x 10-6
” ” ” 50 ppb ” -0.478 7.765 x 10-6
” ” ” 1 ppm ” -0.494 1.134 x 10-5
” ” ” 100 ppm ” -0.488 5.146 x 10-6
” Seawater ” Nil 8.5 -0.718 1.142 x 10-5
” ” ” 50 ppb ” -0.767 7.222 x 10
-6
” ” ” 1 ppm ” -0.772 2.377 x 10-6
” ” ” 100 ppm ” -0.733 4.502 x 10-7
Table 12. Values of corrosion potential, Ecorr and polarization resistance, RP as computed by
linear polarization resistance at room temperature and pH 6.5
Results
Sample -I Sample -IIAlloy Medium Heavy
Metal ion
Metal ion
concentration Ecorr (V) RP (ohm-cm2) Ecorr (V) RP (ohm-cm2)
Carbon
steel
Distilled
water
Copper Nil -0.505 3.14 x 104
-0.431 7.46 x 104
” ” ” 50 ppb -0.528 2.57 x 104
-0.472 2.79 x 104
” ” ” 1 ppm -0.675 7012 -0.476 1.09 x 104
” ” ” 100 ppm -0.737 666 -0.735 1141
” ” Nickel Nil -0.473 4.17 x 104
-0.464 5.84 x 104
” ” ” 50 ppb -0.485 4.18 x 104
-0.483 5.08 x 104
” ” ” 1 ppm -0.547 1.91 x 104
-0.510 2.04 x 104
” ” ” 100 ppm -0.655 780 -0.656 881
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Table 13. AC impedance results for carbon steel and SS 316L in distilled water (pH 6.5) containing
varying concentration of heavy metal ions
Results
Sample -I Sample -IIAlloy Medium
Heavy
Metalion
Metal ion
concentration
RP (ohm-cm2)
Ecorr (V) RS(ohm-cm2)
RP (ohm-cm2
Ecorr (V) RS(ohm-cm2)
Carbonsteel
Distilledwater
Copper Nil 4641 -0.513 - 6014 -0.437 -
” ” ” 50 ppb 2895 -0.550 - 5305 -0.473 -
” ” ” 1 ppm 2462 -0.691 - 2999 -0.501 -
” ” ” 100 ppm 285 -0.738 - 602 -0.736 -
” ” Nickel Nil 4741 -0.473-
4460 -0.468-
” ” ” 50 ppb 4557 -0.491 - 4286 -0.487 -
” ” ” 1 ppm 2191 -0.560 - 3532 -0.515 -
” ” ” 100 ppm 328 -0.655 - 410 -0.658 -
316 L ” Copper Nil 2.85 x 106
-0.0276- -
” ” ” 50 ppb 4.76 x 10
6
-0.0609 - -” ” ” 1 ppm 1.25 x 106 -0.0469 - -
” ” ” 100 ppm 2.37 x 106 -0.1266 -
Table 14. The Values of Ecorr and Rp with time as obtained by ac impedance
Results
Sample -IAlloy Medium Time (days)
Ecorr (V) Rp (ohm-cm2)
Carbon steel Distilled water
containing 100 ppm Ni
1 (immediately) -0.081 1.79 x 106
1 (after 3 hours) -0.069 8230
2 -0.155 7473
6 -0.485 4477
7 -0.231 12542
9 -0.207 14971
10 -0.258 21883
14 -0.116 84134
15 -0.119 38111
16 -0.154 31027
17 -0.330 9766
20 -0.495 257922 -0.378 9843
23 -0.345 36429
27 -0.369 15265
28 -0.372 10638
29 -0.378 49667
30 -0.388 2222
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Figure 1. Ecorr vs time plot for carbon steel immersed in
distillate water (pH = 6.5) containing different
concentration of copper
Figure 2. Ecorr vs time plot for carbon steel immersed in
seawater (pH = 8.5) containing different
concentration of copper
-900
-800
-700
-600
-500
-400
-300
-200
-100
0
100
200
0 5 10 15 20 25 30 35 40
Time (Days)
Potential (mv) vs SCE
1 ppm Cu
100 ppm Cu
0 ppm Cu
-900
-800
-700
-600
-500
-400
-300
-200
-100
0
0 10 20 30 40 50 60
Time (Days)
Potential (mv) vs SCE
1 ppm Cu100 ppm Cu0 ppm Cu
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Figure 3. Ecorr vs time plot for carbon steel immersed in
distilled water (pH =6.5) containing different
concentration of nickel
Figure 4 Ecorr vs time plot for carbon steel immersed in
seawater (pH = 8.5) containing different
concentration of nickel
-900
-800
-700
-600
-500
-400
-300
-200
-100
0
100
0 5 10 15 20 25 30 35
Time (Days)
Potential (mv) vs SCE
100 ppm Ni1 ppm Ni0 ppm Ni
-900
-800
-700
-600
-500
-400
-300
-200
-100
0
0 10 20 30 40
Time (Days)
Potential (mv) vs SCE
100 ppm Ni1 ppm Ni0 ppm Ni
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Figure 5. Ecorr vs time plot for carbon steel immersed in
distilled water (pH = 6.5) containing different
concentration of zinc
Figure 6. Ecorr vs time plot for carbon steel immersed in
seawater (pH = 8.5) containing different
concentration of zinc
-900
-800
-700
-600
-500
-400
-300
-200
-100
00 5 10 15 20 25 30 35
Time (Days)
Potential (mv) vs SCE
1 ppm Zn100 ppm Zn0 ppm zn
-900
-800
-700
-600
-500
-400
-300
-200
-100
0
0 10 20 30 40
Time(Days)
Potential (mv) vs SCE
100 ppm Zn1 ppm Zn0 ppm Zn
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Figure 7. Ecorr vs time plot for carbon steel immersed in
seawater (pH = 8.5) containing different
concentration of silicon
Figure 8. Ecorr vs time plot for 316L immersed in distilled
water (pH = 6.5) containing different concentrationof copper
-900
-800
-700
-600
-500
-400
-300
-200
-100
0
100
0 10 20 30 40
Time (Days)
Potential (mv) vs SCE
1 ppm Si100 ppm Si0 ppm Si
0
50
100
150
200
250
0 10 20 30 40 50 60
Time (Days)
Potential (mv) vs SCE
100 ppm Cu1 ppm Cu
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Figure 9. Ecorr vs time plot for 316L immersed in distilled
water (pH = 6.5) containing different concentration
of nickel
Figure 10. Potentiodyanmic curves for carbon steel in distilled water
(pH=6.5) in presence of Cu
-180
-160
-140
-120
-100
-80
-60
-40
-20
0
20
0 10 20 30 40
Time (Days)
Potential (mv) vs SCE
1 ppm Ni
100 ppm Ni
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Figure 11. Potentiodyanmic curves for carbon steel in seawater (pH=8.5)
in presence of Cu
Figure 12. Potentiodyanmic curves for carbon steel in distilled water
(pH=6.5) in presence of Ni
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Figure 13. Potentiodyanmic curves for carbon steel in seawater (pH=8.5)
in presence of Ni
Figure 14. Potentiodyanmic curves for carbon steel in distilled water
(pH=6.5) in presence of Zn
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Figure 15. Potentiodyanmic curves for carbon steel in seawater
(pH=8.5) in presence of Zn
Figure 16. Polarization resistance curves for carbon steel in distilled water
(pH=6.5) containing different concentration of Cu
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Figure 17. Polarization resistance curves for carbon steel (sample II) in
distilled water (pH=6.5) containing different concentration of
Cu
Figure 18. Polarization resistance curves for carbon steel (sample II) in
distilled water (pH=6.5) containing Ni
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Figure 19. Polarization resistance curves for carbon steel in distilled
water containing Ni
Figure 20. Nyquist plot for carbon steel in distilled water (pH 6.5)
containing different concentration of Cu
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Figure 21. Nyquist plot for carbon steel (Sample II) in distilled water (pH
6.5) containing different concentration of Cu
Figure 22. Nyquist plot for carbon steel in distilled water (pH 6.5)
containing different concentration of Ni
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Figure 23. Nyquist plot for carbon steel (sample II) in distilled water (pH
6.5) containing different concentration of Ni
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Performance and Failure Evaluation in SWCC MSF Plants, Desalination, 97, 171.
2. Asphahani, A.I. and Silence, W.L., (1987), Metal Hand Book: ASME Publication.
Vol. 13., p. 113.
3. Szklarska-Smialowska, Z., (1986), Pitting Corrosion of Metals, NACE, Houston.
4. Uhlig, H.H. and Revie, R.W., (1985), Corrosion Control - An Introduction to
Corrosion Science and Engineering, John Wiley & Sons, 3rd Edi., New York.
5. Sandricks, A.J., (1979), Corrosion of Stainless Steels, John Wiley & Sons, 3rd
Edi., New York.
6. Szklarska-Smialowska, Z., (1987), Industrial Problems Treatment and Control
Techniques, Pergmon Press, Oxform.
7. Malik, A.U., Kutty, P.C.M., Andijani, I.N. and Ahmed, S., (1992), The Influence
of pH and Chloride Concentration on the Corrosion Behavior of AISI 316 L Steel
in Aqueous Solution, Corrosion Science, 33, 1809.
8. Internal Corrosion of Water Distribution System: Cooperative Research Report,American Water Work Association and DVGW-for Schungsteus, (1985), USA, p.
191.
9. Schrieber, C.F., (1986), Measurement and Control Related Corrosion and Scales
in Water Desalination Installation in “Measurement of Control in Water
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22 Metal Handbook (1987) ASM International Vol 13, Corrosion 9th Edition P