Eng. & Tech. Journal ,Vol.32, Part (A), No.5, 2014
Effect of some vegetables (Carrots, Onion, Parsley, and Red
radish) on Corrosion Behavior of Amalgam Dental Filling in
Artificial Saliva
Slafa Ismael Ibrahim
Energy and Renewable Energies Technology Center, University of Technology/Baghdad.
Email: chemistsulafa_59@yahoo.com
Received on: 15/9/2013
&
Accepted on: 9/1/2014
ABSTRACT
This work involves study corrosion behavior of amalgam in presence of some
vegetables including (Carrots, Onion, Parsley, and Red radish) which were chosen
because they require mastication process by teeth and taking enough time that make
them in a contact with amalgams filling in artificial saliva.
The corrosion parameters were interpreted in artificial saliva at pH (5.1) and
(37±1oC) by adding (50 ml/l) of vegetable juice to artificial saliva, which involve
corrosion potential (Ecorr), corrosion current density (i corr), Cathodic and anodic Tafel
slopes (bc & ba ) and polarization resistance, the results of (E corr) and (icorr) indicate
that the medium of saliva and (50 ml/l) onion is more corrosive than the other media.
Cathodic and anodic tafel slopes were used to calculate the polarization resistance
(Rp) to know which medium more effective on amalgam of dental filling, this study
shows that the increasing in polarization resistance through the decreasing in
corrosion rate values, the results of (R p) take the sequence:
Rp:( saliva+ parsley) >( saliva+ red radish)> saliva>(saliva+ carrots) >(saliva+ onion).
While corrosion rates (CR ) take the sequence:
CR: (Saliva+Parsley)<(Saliva+Red radish)<Saliva<(Saliva+Carrots)<(Saliva+ Onion)
Keyword: Amalgam, Corrosion in saliva, Potentiostatic measurements.
اﻟﻔﺠﻞ اﻷﺣﻤﺮ( ﻋﻠﻰ اﻟﺴﻠﻮك, اﻟﻤﻌﺪﻧﻮس, اﻟﺒﺼﻞ, ﺗﺄﺛﯿﺮ ﺑﻌﺾ اﻟﺨﻀﺮوات )اﻟﺠﺰر
أﻟﺘﺂﻛﻠﻲ ﻟﻤﻠﻐﻢ ﺣﺸﻮة اﻷﺳﻨﺎن ﻓﻲ اﻟﻠﻌﺎب اﻟﺼﻨﺎﻋﻲ
اﻟﺨﻼﺻﺔ
, اﻟﺒﺼﻞ,ﯾﺘﻀﻤﻦ ھﺬا اﻟﻌﻤﻞ دراﺳﺔ اﻟﺴﻠﻮك اﻟﺘﺎﻛﻠﻲ ﻟﻠﻤﻠﻐﻢ ﺑﻮﺟﻮد ﺑﻌﺾ اﻟﺨﻀﺮوات واﻟﺘﻲ ﺗﺘﻀﻤﻦ )اﻟﺠﺰر
ﺮWﺎ أﻛﺜWﺎ ﯾﺠﻌﻠﮭWﺔ ﻣﻤWﺮة زﻣﻨﯿWﻨﺎن ﻟﻔﺘWﻎ ﺑﺎﻷﺳW واﻟﻔﺠﻞ اﻷﺣﻤﺮ( واﻟﺘﻲ ﺗﻢ اﺧﺘﯿﺎرھﺎ ﻷﻧﮭﺎ ﺗﺘﻄﻠﺐ ﻋﻤﻠﯿﺔ ﻣﻀ,اﻟﻤﻌﺪﻧﻮس
.اﺗﺼﺎﻻ ﻣﻊ ﻣﻠﻐﻢ ﺣﺸﻮات اﻷﺳﻨﺎن ﻓﻲ اﻟﻠﻌﺎب اﻟﺼﻨﺎﻋﻲ
ﺔWW( ﻣﺌﻮﯾ1±37) ﺮارةWWﺔ ﺣWW( و درﺟ5.1) ﯿﺔWWﺔ ﺣﺎﻣﻀWWﺪ داﻟWWﻨﺎﻋﻲ ﻋﻨWWﺎب اﻟﺼWWﻲ اﻟﻠﻌWWﺮت ﻓWWﻞ ﻓﺴWWﺎﻣﻼت اﻟﺘﺂﻛWWﻣﻌ
ﺑﺈﺿﺎﻓﺔ
ﺎرWﺔ ﺗﯿWﻛﺜﺎﻓ, (Ecorr ) ﻞWﺪ اﻟﺘﺂﻛWﻤﻦ ﺟﮭWﺬي ﯾﺘﻀW واﻟ,ﻨﺎﻋﻲWﺎب اﻟﺼWﻰ اﻟﻠﻌWﺮوات إﻟWﯿﺮ اﻟﺨﻀWﻦ ﻋﺼWﺮ( ﻣWﻟﺘ/ ﻣﻞ50)
ﻞWﺎر اﻟﺘﺂﻛWﺔ ﺗﯿWﻞ و ﻛﺜﺎﻓWﺪ اﻟﺘﺂﻛWﺎﺋﺞ ﺟﮭWﯿﺮ ﻧﺘW ﺗﺸ, ﻣﯿﻮل ﺗﺎﻓﻞ اﻟﻜﺎﺛﻮدﯾﺔ واﻻﻧﻮدﯾﺔ وﻣﻘﺎوﻣﺔ اﻻﺳﺘﻘﻄﺎب, (icorr) اﻟﺘﺂﻛﻞ
ﻞWWﻮل ﺗﺎﻓWWﺘﺨﺪام ﻣﯿWWﻢ اﺳWWﺗ, .ﺎطWWﺔ اﻷوﺳWWﻦ ﺑﻘﯿWWﺮ ﻣWWﻞ أﻛﺜWWﻂ آﻛWWﺮ وﺳWWﻞ ﯾﻌﺘﺒWWﺮ( ﺑﺼWWﻟﺘ/ ﻞWWﻣ50)ﺎب وWWﻂ اﻟﻠﻌWWﻰ إن وﺳWWإﻟ
,ﻨﺎنWﻮه اﻷﺳWﻢ ﺣﺸWﻰ ﻣﻠﻐW( ﻟﻤﻌﺮﻓﺔ أي اﻷوﺳﺎط أﻛﺜﺮ ﺗﺄﺛﯿﺮا ﻋﻠRp) اﻟﻜﺎﺛﻮدﯾﺔ واﻻﻧﻮدﯾﺔ ﻟﺤﺴﺎب ﻣﻘﺎوﻣﺔ اﻻﺳﺘﻘﻄﺎب
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Eng. & Tech. Journal ,Vol.32, Part (A), No.5, 2014
Effect of some Vegetables (Carrots, Onion,
Parsley, and Red Radish) on Corrosion
Behavior of Amalgam Dental Filling in
Artificial Saliva
ﺬW( ﺗﺄﺧRp) ﺎﺋﺞW ﻧﺘ, ﻞWﺮﻋﺔ اﻟﺘﺂﻛWﯿﻢ ﺳWﻲ ﻗWﻨﻘﺺ ﻓWﻼل اﻟWﻦ ﺧWﺘﻘﻄﺎب ﻣWﺔ اﻻﺳWﻲ ﻣﻘﺎوﻣWأظﮭﺮت ھﺬه اﻟﺪراﺳﺔ زﯾﺎدة ﻓ
:اﻟﺘﺴﻠﺴﻞ اﻟﺘﺎﻟﻲ
( ﺑﺼﻞ+ ﺟﺰر( < )ﻟﻌﺎب+ ﻓﺠﻞ اﺣﻤﺮ( < ﻟﻌﺎب < )ﻟﻌﺎب+ ﻣﻌﺪﻧﻮس( < )ﻟﻌﺎب+ )ﻟﻌﺎب: Rp
:( ﺗﺄﺧﺬ اﻟﺘﺴﻠﺴﻞ اﻟﺘﺎﻟﻲCR ) ﺑﯿﻨﻤﺎ ﺳﺮﻋﺔ اﻟﺘﺂﻛﻞ
( ﺑﺼﻞ+ ﺟﺰر( > )ﻟﻌﺎب+ ﻓﺠﻞ اﺣﻤﺮ( > ﻟﻌﺎب > )ﻟﻌﺎب+ ﻣﻌﺪﻧﻮس( > )ﻟﻌﺎب+ )ﻟﻌﺎب:CR
INTRODUCTION :
egetables are vital to human body as they contain essential components
needed by the human body such as carbohydrates, proteins, vitamins,
minerals and also trace elements as shown in table (1)[1-3] .
All of the ingredients found in food and drink are capable of becoming incorporated
into saliva .However; most of the foods are ingested before the breakdown into basic
chemicals occurs. Some foods and beverages, though, contain chemicals that are
reactive by themselves without any reductions and may become dissolved in saliva
and affect the tarnish and corrosion of metallic materials [4]. Various studies have
been conducted on Dental filling; Rivera P.C. and coworkers[5] studied the
evaluation of the galvanic corrosion of three high copper dental amalgams by means
of electrochemical techniques, the dental amalgams were: a national Nu Alloy( which
is a dispersed-phase, high-copper-content dental alloy with no zinc content) (New
Stetic) and two imported Contour (Kerr university , USA) and GS-80,(SDI,
Australia) (SDI, is a specialist manufacturer and distributor of dental restorative
materials), (alloy composition Ag 40%,Sn 31.3%, Cu 28.7%,Hg 47.9%). The dental
metallic materials were: Titanium CP(Commercially Pure) , Ti-6Al-4V type COC
(Ceramic-on-Ceramic) , International power system (IPS) design 15 (Ni-Cr-Mo) and
IPS design 91 (Au-Pd). Under the test conditions, they concluded that the home
amalgam has the same tendency to undergo galvanic corrosion as comparison to
imported amalgams. Using statistical analysis of variance (ANOVA) method of a
single via it was corroborated the same electrochemical behavior of dental amalgams
. Alves and coworkers[6] studied electrochemical impedance applied to the corrosion
behavior of dental amalgams in synthetic physiological fluids. This study was done
with Duxalloy and Tytin Plus samples in four different electrolytes: Phosphate buffer
saline, Hank solution, artificial saliva and NaCl 0.9%, they concluded that the passive
film resistance is high at initial immersion times and decreases after 168h. Although
this fact is systematic, the passive film continued to show its semiconductive and
resistive properties even after a period of (168 h.) of immersion, in other words, it
presented protective properties against corrosion and because of this, and the
biomaterial does not produce potential risks to human health. Zhang and coworkers
[7] studied the effect of silver on the corrosion behavior of Ti-Ag alloy in artificial
saliva solutions, they concluded that, addition of Ag was effective in reducing the
corrosion current density and increasing the open circuit potential of titanium in
artificial saliva environment, and addition of fluoride ions in the solution severely
reduced the corrosion resistance if Ti-Ag alloys. Zhang and coworkers [8] studied the
corrosion behavior of Ti-5Ag alloy with and without thermal oxidation in artificial
saliva solution, they concluded that, the corrosion resistance was enhanced by
addition of Ag for titanium and could be further improved by thermal oxidation.
V
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Eng. & Tech. Journal ,Vol.32, Part (A), No.5, 2014
Effect of some Vegetables (Carrots, Onion,
Parsley, and Red Radish) on Corrosion
Behavior of Amalgam Dental Filling in
Artificial Saliva
Experimental
Materials and Chemicals
The used alloy in this study was amalgam; the chemical composition of this
alloy is shown in table (2) which prepared by triturating (0.7g) of powder alloy and
the corresponding weight of mercury by amalgamator type(YDM-Pro) for (15sec.) at
high speed. And then cold mounted using pyrax polymers to obtain only surface area
of cylinder specimen, with (1.5cm) diameter.
The open side was polished mechanically to a mirror finish, rinsed in distilled
water and stored in desiccators. First electrolyte was used as a reference by modified
Fusayama artificial saliva [9], which closely resembles natural saliva, with
composition of (0.4 g/L KCl, 0.4g/L NaCl, 0.906 g/L CaCl 2.2H2O, 0.69 g/L
NaH2PO4.2H2O, 0.005g/L Na2S.9H2O and 1g/L urea), all chemicals are from Thomas
Baker (chemicals) PVT.Limited (India) with purity (98-99.5%) pH of this electrolyte
was (5.1). The vegetables were washed with tap water followed by distilled water to
eliminate attached soil particulates, and dried, then converting it to juice by juice
maker.
50ml/L of each vegetable was added to artificial saliva to study of it on
corrosion behavior of amalgam. The value of pH for artificial saliva after adding
these vegetable was increased up to 5.6 or less depending on the type of vegetable as
shown in table (3).
Corrosion Test
Polarization experiments were performed in WINKING M Lab 200
Potentiostat/Galvanostat from Bank-Elektronik with electrochemical standard cell
with provision for working electrode (amalgam), auxiliary electrode (Pt electrode),
and a Luggin capillary for connection with saturated calomel electrode SCE reference
electrode. Electrochemical measurements were performed with a potentiostat by SCI
electrochemical software at a scan rate of 3 mV.sec-1.
The main results obtained were expressed in terms of the corrosion potentials
(Ecorr) and corrosion current density (i corr) besides measurement of the tafel slops by
tafel extrapolation method.
Results and Discussion
Corrosion Behavior
Figure (1) shows the variation of potential (OCP) with time for amalgam in
saliva and mixture of saliva with some type of vegetable samples including (Carrots,
Onion, Parsley, and Red radish), this behavior indicates that behavior of amalgam in
(saliva & parsley) and (saliva& carrots)solutions more stable than (saliva& Red
radish) and (saliva& Onion) solutions with time. This could be due to the mixed
potential resulting from the ionic constitution of the solutions. The open circuit
potential values take the following sequence for amalgam:
E OCP: saliva & parsley< saliva& carrots<saliva<saliva& Red radish<saliva&
Onion.
The potentiodynamic polarization and cyclic polarization curves are shown in
Fig. (2)and Fig. (3).These figures show the main two behavior of the anodic and
cathodic regions; the lower section represents reduction reaction which includes
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Eng. & Tech. Journal ,Vol.32, Part (A), No.5, 2014
Effect of some Vegetables (Carrots, Onion,
Parsley, and Red Radish) on Corrosion
Behavior of Amalgam Dental Filling in
Artificial Saliva
evolution of hydrogen molecules because acidity of electrolyte (artificial saliva) as
follows:
2H+ + 2e → H2
…..(1)
In addition to reduction of oxygen to water molecules:
O2 + 4H+ + 4e → 2H2O
….(2)
While at anodic sites dissolution of metals in amalgam can occur such as Ag, Sn, and
Cu. Mercury diffuses into the alloy particles and reacts with silver, tin and copper,
forming various compounds. The exact compounds formed depend on the chemical
composition of the powder and on particle shape (which can be spherical or irregular)
but are mainly phases of the systems Sn–Hg, Ag–Hg, with Ag–Cu and Ag–Sn phases
remaining from the reactants. For the currently used, high copper amalgams, the main
reaction is [10]:
γ-Ag3Sn + Ag–Cu + Hg → γ1-Ag2Hg3 + γ2-Sn7Hg + γ-Ag3Sn + Ag–Cu …..(3)
The Sn–Hg phase, which has a relatively low corrosion resistance, then undergoes
further reaction, according to:
γ2-Sn7Hg + Ag–Cu → ή -Cu6Sn5 + γ1-Ag2Hg3
…..(4)
The microstructure of the dental amalgam is complex, consisting of new
microphases, as produced in the reactions above, and the remains of the powder alloy
particles, within the γ1-Ag2Hg3 matrix phase [10]. For this reason, and in order to
understand better the role of the various phases, individual phases have
electrochemical measurements can lead to an improved understanding of the
processes that take place at the amalgam electrode surface as well as the influence of
surface oxide. Hypothesis has also been proposed, that the released mercury may
partly react with Ag3Sn, to produce additional Sn 7Hg, so that the corrosion cycle
can continue. The filling becomes porous and can lose most of its strength.
Absorption of released mercury by Ag3Sn requires the absorbing phase in close
vicinity of the corroding Sn 7Hg-phase; otherwise there is no thermodynamical reason
for mercury to diffuse into the filling with high mercury content. Otherwise, it will
evaporate. The content of Ag3Sn may vary depending on amalgam composition and
working methods of the particular dentist. As the amount and distribution of Ag 3Sn
cannot be controlled, the hypothesis about Ag3Sn as a sink for all mercury released by
corrosion is not substantiated. As reported by Brune [11] silver has been found in the
solution already after a few days exposure to artificial saliva. Though ionized
mercury also has been found among the dissolved corrosion products by radioactive
tracer method [12] the main part is released as metallic mercury, which can be found
as droplets on freshly corroded amalgam surfaces [13].
The corrosion parameters listed in Table (3) show that the sequence of corrosion
potential of amalgam takes the following sequence:
-Ecorr: saliva& Onion> saliva& Red radish> saliva& carrots> saliva & parsley> saliva.
While the corrosion current densities values (i corr) takes the following sequence:
icorr: saliva& Onion> saliva& carrots> saliva> saliva& Red radish> saliva & parsley.
The rate of corrosion (C R mm/y) for amalgam in saliva and mixture of saliva
with some type of vegetable samples including (Carrots, Onion, Parsley, and Red
radish) is directly proportional with its corrosion current density (i corr) in accordance
with the relation [14]:
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Eng. & Tech. Journal ,Vol.32, Part (A), No.5, 2014
C R ( mm / y ) = 3 . 27
e
icorr .
ρ
Effect of some Vegetables (Carrots, Onion,
Parsley, and Red Radish) on Corrosion
Behavior of Amalgam Dental Filling in
Artificial Saliva
.....( 5 )
Where CR(mm/y): corrosion rate in millimeter per year, e: equivalent weight of
alloy (gm), and ρ: density of alloy (gm/cm3).
The polarization resistance (Rp) can be determined from the Tafel slopes and
according to Stern- Geary equation [15]and [16]:
b a bc
dE
Rp =
=
di i = 0 2 .303 (b a + bc )i corr
.......( 6 )
The values of Rp which have been calculated from above equation are taken the
following sequence:
Rp: saliva & parsley> saliva& Red radish>> saliva> saliva& carrots> saliva& Onion.
Cyclic polarization measurements were in a good agreement with
potentiodynamic polarization as shown in Fig. (3).These curves show that forward
scan and reverse scan shift to higher range of current densities for the presence of
carrots and onion in artificial saliva, where these vegetables lead to increase corrosion
rate of amalgam. This result of behavior of vegetables may be due to presence of
various sulfides, sulfenic acids and acetic acid [17].
Cyclic polarization of amalgam in artificial saliva in the presence of parsley and
red radish indicates that reverse scan shift to lower values of current density
compared with forward scan, where these materials led to decrease corrosion rate of
amalgam.
This result of behavior of vegetables may be due to presence of some contents
which behave as inhibitors when it adsorbed on the amalgam surface such as Vitamin
K, 4-methoxy-1H-indole-3-carboxaldehyde) ,and 1H-indole-3-carboxaldehyde, …etc.
These contents may be acted as barrier between saliva and amalgam due to chain of
hydrocarbons and other chemical functionally group work to isolate the metallic
surface from corrosive electrolyte.
CONCLUSION:
Presence of carrots and onion in saliva increases corrosion rate of amalgam
filling while presence of parsley and red radish in saliva decreases corrosion rate of
amalgam filling.
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Eng. & Tech. Journal ,Vol.32, Part (A), No.5, 2014
Effect of some Vegetables (Carrots, Onion,
Parsley, and Red Radish) on Corrosion
Behavior of Amalgam Dental Filling in
Artificial Saliva
Table (1): Some compounds in selected vegetable.
Compounds found in:Carrotsa
p-cymene, limonene, β-myrcene, sabinene, terpinolene, γ -terpinene,
β -caryophylene, (E) - γ -bisabolene, β –bisabolene, α-pinene ,
3-hydroxy- 2-butanone, ethanol, hexanal, acetic acid, and
erythro- and threo-2,3-butanediol.
Oniona
Parsleyb
Red radisha,c
Cysteine sulfoxides, Sulfenic acids, Propanethial-S-oxide,
Thiosulfinates, Propanal, Polysulfides, Thiosulfonates
α-Pinene, β-Myrcene, α-Phellandrene, β-Phellandrene, cis-Ocimene,
Isopropenyl-4-methylbenzene , α-Terpinolene, p-Mentha-1,3,8triene,
α-Copaene, Caryophyllene , β-Farnesene , β-Selinene , γ-Cadinene,
Myristicin , β-Bisabolene, β-Sesquiphellandrene, Apiole .
4-methylthio-butyl isothiocyanate, 5-methylthio-pentyl
isothiocyanate, dimethyl trisulfide, 2-phenylethyl isothiocyanate,
acylated Anthocyanins, 4-methoxy-1H-indole-3-carboxaldehyde) ,
and 1H-indole-3-carboxaldehyde .
a: Ref.[1] , b: Ref.[2], c: Ref. [17,18].
Table (2): Chemical composition of amalgam.
Metal
Wt%
Ag
56.7
Sn
28.6
Cu
14.7
Table (3): Corrosion parameters of amalgam in artificial saliva and in presence
saliva with (of Carrots; Onion; Parsley; and Red radish) at (37±1) oC.
Solution
component
pH
of the
Eoc
solution mV
-Ecorr
mV
Tafel slope
Corrosion
(mV.dec-1)
current
Polarization
density
resistance
-bc
ba
icorr/μA.cm- mV.dec- mV.dec- (Rp/Ω.cm2)
2
1
CR
mm/y
1
Saliva
5.1
488
474.5
1.82
92.0
93.7
11.075
0.0611
Saliva+
5%Carrots
Saliva+
5% Onion
Saliva+
Parsley
Saliva+
5% Red
radish
5.63
485
491.5
2.06
112.5
87.9
10.401
0.0692
5.05
509
545.1
2.08
94.9
94.9
9.905
0.0699
5.23
466
478.8
1.65
110.5
106.0
14.237
0.0554
5.39
490
500.3
1.69
107.7
97.7
13.162
0.0568
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Eng. & Tech. Journal ,Vol.32, Part (A), No.5, 2014
- Saliva only
-In presence of Saliva& Carrots
- In presence of Onion
-In presence of Parsley
-In presence of Red radish
-100
-200
Potential (mV)
Effect of some Vegetables (Carrots, Onion,
Parsley, and Red Radish) on Corrosion
Behavior of Amalgam Dental Filling in
Artificial Saliva
-300
-400
-500
-600
-700
0
200
400
600
Time (Sec.)
800
1000
Figure (1): Variation of potential with time of amalgam in artificial saliva
at (37±1)oC and in presence of Carrots, Onion, Parsley , and Red radish.
-100
- In Saliva only
In presence of Saliva&Carrots
E /mV vs. SCE
-200
-300
- In presence of Saliva &Onion
-In presence of Saliva & Parsley"
In presence of Saliva&Red radish
-400
-500
-600
-700
-800
0.00001
0.0001
0.001
0.01
0.1
1
-2
log i /mA.cm
Figure (2): Linear polarization of amalgam in artificial saliva at (37±1) oC
and in presence of Carrots, Onion, Parsley, and Red radish .
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Eng. & Tech. Journal ,Vol.32, Part (A), No.5, 2014
Effect of some Vegetables (Carrots, Onion,
Parsley, and Red Radish) on Corrosion
Behavior of Amalgam Dental Filling in
Artificial Saliva
Figure (3) to be continued
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Eng. & Tech. Journal ,Vol.32, Part (A), No.5, 2014
Effect of some Vegetables (Carrots, Onion,
Parsley, and Red Radish) on Corrosion
Behavior of Amalgam Dental Filling in
Artificial Saliva
Figure (3) to be continued
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Eng. & Tech. Journal ,Vol.32, Part (A), No.5, 2014
Effect of some Vegetables (Carrots, Onion,
Parsley, and Red Radish) on Corrosion
Behavior of Amalgam Dental Filling in
Artificial Saliva
Figure (3): Cyclic polarization of amalgam in artificial saliva at (37±1) oC
and in the presence of Saliva with (Carrots, Onion, Parsley, and Red radish).
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techniques" , Rev. Fac. Ing. Univ. Antioquia No.( 45) pp:( 77-86). Sep., 2008.
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[7] Zhang B.B. ,Zheng Y.F., Liu Y., "Effect of Ag on the corrosion behavior of Ti-Ag
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Eng. & Tech. Journal ,Vol.32, Part (A), No.5, 2014
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