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Corrosion Science 50 (2008) 1498–1504

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Natural honey and black radish juice as tin corrosion inhibitors

I. Radojčić a, K. Berković a, S. Kovač b,*, J. Vorkapić-Furač a
a
Faculty of Food Technology and Biotechnology, University of Zagreb, Pierottijeva 6, 10000 Zagreb, Croatia
b
Faculty of Food Technology, University J.J. Strossmayer in Osijek, Kuhačeva 18, 31000 Osijek, Croatia

Received 30 January 2008; accepted 30 January 2008

Available online 16 February 2008

Abstract

The influence of natural honey (chestnut and acacia) and natural honey with black radish juice, on corrosion of tin in aqueous and
sodium chloride solutions was studied using weight loss and polarization techniques. The inhibition efficiency of acacia honey was lower
than that of chestnut honey, while the addition of black radish juice increased the inhibition efficiency of both honey varieties. The pro-
cess of inhibition was attributed to the formation of multilayer adsorbed film on the tin surface. The adsorption of natural honey and
honey with black radish on tin was found to follow the Langmuir adsorption isotherm.
Ó 2008 Elsevier Ltd. All rights reserved.

Keywords: Natural honey; Black radish juice; Corrosion; Inhibition; Tin

1. Introduction an increased interest in employing naturally occurring sub-

Food industry usually employs a tin plate as an amba-
lage material for making tin cans, which upon exposing
to food components undergo corrosion process [1]. One
of the most effective alternatives for the protection of
metallic surfaces against corrosion is the use of corrosion
inhibitors (inorganic or organic). The inorganic inhibitors
act as anodic inhibitors while the organic inhibitors form
protective film through the adsorption of their molecules
on the metal surface being responsible for the corrosion
resistance [2,3]. Usually, organic compounds that exert a
significant influence on the extent of adsorption on the
metal surface and therefore can be used as effective corro-
sion inhibitors possess hetero atoms such as nitrogen, sul-
phur or oxygen, and an aromatic ring in their molecules
[4]. Their synthesis is very often expensive, and they are
toxic and hazardous for human beings and the environ-
ment. Therefore, the development of non-toxic, ecologi-
cally harmless, green corrosion inhibitors is regarded as
very important and always actual. Recently, there has been
*
Corresponding author. Tel.: +385 31 224 327; fax: +385 31 203 485.
E-mail address: spomenka.kovac@ptfos.hr (S. Kovač).
stances and extracts which fulfil the requirements to be
used as effective corrosion inhibitors. Two papers appeared
dealing with natural honey as corrosion inhibitor for coo-
per in neutral aqueous solution and C-steel in high saline
water. The results obtained confirmed that honey was effec-
tive as an inhibitor of corrosion [5,6]. Also, at the Univer-
sity of Manchester Institute of Science Yin Jin Yee
submitted a thesis in which he examined honey enriched
with extract of herb rosemary (Rosmarinus officinalis L.)
as corrosion inhibitor [7]. Studying usage of natural com-
pounds as corrosion inhibitors our group tested inhibition
efficiency of cabbage glucosinolates extracts and cocoa
liquor polyphenols on tin, and polyphenols (rutin and
quercetin) on aluminium [8–10]. In an ongoing research
project on development of eco-friendly corrosion inhibitors
for tin we evaluated the inhibition efficiency of two varie-
ties of natural honey (acacia and chestnut) in aqueous
and sodium chloride solutions in the absence and presence
of black radish juice. Honey is an easily digestible foodstuff
containing a range of nutritiously important complemen-
tary elements: saccharides, organic acids, amino acids,
polyphenols, mineral matter, colours, aromatic substances,
trace amounts of fat, and some valuable but unstable
compounds such as enzymes, substances of hormonal

0010-938X/$ - see front matter Ó 2008 Elsevier Ltd. All rights reserved.
doi:10.1016/j.corsci.2008.01.013
 I. Radojčić et al. / Corrosion Science 50 (2008) 1498–1504
character, some vitamins and a few minor compounds. It is
considered as part of traditional medicine being effective in
gastrointestinal disorders, in healing of wounds and burns,
and as an antimicrobial agent [11]. Black radish (Raphanus
sativus L. var. niger) is a root plant belonging to Cruciferae
family. It contains a mixture of various inorganic and
organic compounds (minerals, lipids, proteins, carbohy-
drates, dietary fibres and vitamins) as well as polyphenols
and sulphur containing organic compounds such as gluco-
sinolates, having different biological properties (anticancer,
antimicrobial and antiviral) [12].
2. Experimental method
Before the weight loss measurements, the tin samples
were polished using emery paper with different grits, fol-
lowed by washing in ethanol and double distilled water.
Potentiostatic polarization studies were carried out
using EG&G model 173 Potentiostat/Galvanostat. Electro-
chemical measurements were conducted in a conventional
three-electrode electrolytic cell, capacity 150 mL, with
99.95% tin rod working electrode, a platinum counter elec-
trode, and a saturated calomel electrode as the reference
one. The tin electrode was isolated with polyethylene, hav-
ing a free surface area of 0.56 cm2. For electrochemical
measurements the exposed surface was ground with abra-
sive paper up to 600 grit, degreased with ethyl alcohol,
and rinsed by redistilled water. To avoid the influence of
oxygen, during electrochemical measurements, the electro-
lyte was thoroughly deaerated with nitrogen at 25 ± 0.1 °C
for 30 min.
The pH and conductivity values were determined with
EA 940 ‘‘ORION” Expandable Analyser, electrode model
91-02 and LF 320/SET, respectively.
Two monofloral honey types used in experiments and
obtained from the local market were: dark-coloured chest-
nut and light-coloured acacia honey, collected during
2003 in Slavonia (the eastern part of Croatia). The analysis
of polyphenols in these two honey samples was carried out
by RP-HPLC. Total content of flavonoids in acacia honey
was 286.0 lg/100 g, and in chestnut honey 231.0 lg/100 g,
respectively [13]. Both honey samples have similar flavonoid
profile (quercetin, luteolin, kaempferol, apigenin, chrysin
and galangin) with one difference. Namely, flavonoid
myricetin was found in chestnut honey in significant quan-
tities, while in acacia honey samples myricetin was not pres-
ent at all [14]. Black radish (Raphanus sativus L. var. niger),
a cruciferous plant rich in polyphenols and glucosinolates
(sulphur-containing compounds) was of Croatian domestic
production. The total polyphenol content of the juice from
squeezed black radish root was determined by the Folin–
Ciocalteu method described in AOAC [15]. In 100 g of
black radish juice the total polyphenol content was
37.5 mg, with quercetin as the predominant compound.
The total glucosinolate content was determined by HPLC
method being 22.5 mg, with minor quantities of progoitrin,
4-hydroxyglucobrassicin, glucobrassicin, and gluconastur-
1499
tin, and methylthiobutenyl glucosinolate as the predomi-
nant one [16]. The honey solutions were prepared in
concentrations 200, 400, 600, 800, and 1000 ppm by dissolv-
ing 20, 40, 60, 80 and 100 mg of honey in 100 g of water or
3% NaCl solution, respectively. The black radish juice,
obtained by squeezing black radish root, was mixed with
honey in equal quantities (1:1; w/w). After 24 h 20, 40, 60,
80 and 100 mg of this mixture was dissolved in 100 g of
water or 3% NaCl solution, respectively, to prepare solu-
tions in concentrations 200, 400, 600, 800, and 1000 ppm.
3. Results and discussion
The mean values of pH and ion conductivity of all solu-
tions under examination (aqueous and sodium chloride
honey solutions without and with the addition of black
radish juice) are given in Table 1.
The pH values of both honey varieties (acacia and chest-
nut) aqueous solutions are lower than that obtained for the
same solutions with black radish juice added. The same
relations are evident for honey sodium chloride solutions
with pH values being higher. Also, the higher pH values
were obtained for acacia honey in aqueous as well as
sodium chloride solutions in comparison with those
obtained for chestnut honey.
The ion conductivity of both honey varieties in aqueous
solutions is lower than in those with black radish juice
added, while the ion conductivity in sodium chloride solu-
tions in all combinations (acacia honey without and with
addition of black radish juice, as well as chestnut honey
without and with addition of black radish juice) is higher,
being in the range of the values obtained for 3% NaCl solu-
tion alone.
The values of tin corrosion rate (w), surface coverage
(H), and inhibition efficiency (IE) obtained by weight loss
measurements for 3% NaCl solutions with acacia and
chestnut honey in the absence and presence of black radish
juice are given in Table 2.
The corrosion rate of tin was determined by using the
relation:
w ¼ Dm=St
where Dm is the mass loss, S is the area and t is the immer-
sion period.
The inspection of Table 2 reveals that tin corrosion rates
decrease following an increase of the acacia and chestnut
honey concentrations. The same correlation is evident in
solutions with black radish juice added.
The degree of surface coverage (H), which represents the
fraction of the metal surface covered by inhibitor mole-
cules, was calculated using the following equation:
H ¼ 1  w=w0
where w and w0 are the corrosion rates of tin in solutions
with and without inhibitor, respectively, while the percent-
age inhibition efficiency (IE) was obtained by multiplying
H with 100.
1500 I. Radojčić et al. / Corrosion Science 50 (2008) 1498–1504

Table 1
The pH and ion conductivity values of aqueous and sodium chloride solutions of chestnut and acacia honey alone and with addition of black radish juice
(Raphanus sativus L. var. niger) measured at (20.5 ± 0.4) °C
Solution choney pH Ion Solution choney pH Ion
(ppm) conductivity (ppm) conductivity
(j/mS cm1) (j/mS cm1)
Aqueous solutions of chestnut honey 200 4.19 21.60  103 3% NaCl – 5.25 41.10
(CHaq) 200 4.95 41.70
400 4.25 32.75  103 3% NaCl solutions of chestnut honey 400 5.05 40.70
600 5.08 27.00  103 (CHNaCl) 600 5.33 40.15
800 5.13 11.50  103 800 5.30 40.95
1000 5.30 11.40  103 1000 5.38 41.00
Aqueous solutions of chestnut honey 200 4.23 22.30  103 3% NaCl solutions of chestnut honey 200 5.01 40.08
with addition of black radish juice 400 4.28 32.65  103 with addition of black radish juice 400 5.02 41.02
(CHBRaq) 600 4.92 27.51  103 (CHBRNaCl) 600 5.31 40.08
800 4.90 13.60  103 800 5.29 41.12
1000 5.25 12.85  103 1000 5.40 41.05
Aqueous solutions of acacia honey 200 5.60 29.70  103 200 5.68 40.60
(AHaq) 400 5.20 25.50  103 3% NaCl solutions of acacia honey 400 5.90 41.20
600 5.19 21.7  103 (AHNaCl) 600 5.70 41.10
800 5.52 28.30  103 800 6.15 40.70
1000 5.45 24.40  103 1000 6.20 40.90
Aqueous solutions of acacia honey 200 5.62 30.01  103 3% NaCl solutions of acacia honey with 200 5.63 41.02
with addition of black radish juice 400 5.23 26.70  103 addition of black radish juice (AHBRNaCl) 400 42.05 42.05
(AHBRaq) 600 5.21 22.90  103 600 5.75 42.30
800 5.60 29.10  103 800 6.12 41.80
1000 5.48 25.80  103 1000 6.08 41.05

Table 2 molecules of honey followed the increase of solution con-

The values of tin corrosion rate (w), surface coverage (H), and inhibition centration. Due to the fact that honey is a mixture of
efficiency (IE) in 3% NaCl solutions of chestnut and acacia honey alone
various compounds containing oxygen (polyphenols) as
and with addition of black radish juice (Raphanus sativus L. var. niger)
well as nitrogen and sulphur (glucosinolates) which all
Solution choney w H IE
can be adsorbed on the corroded metal it is hard to
(ppm) (g cm2 h1) (%)
decide which of these components is responsible for this
3% NaCl solutions of chestnut honey 200 1.35  103 0.40 40
inhibition. According to the differences in their nature
(CHNaCl) 400 0.87  103 0.61 61
600 0.66  103 0.71 71 and electronic structure some conclusions could be made.
800 0.39  103 0.83 83 The flavonoid compound, found in chestnut honey, but
1000 0.23  103 0.90 90 not in acacia honey is myricetin having six electron-
3% NaCl solutions of chestnut honey 200 1.20  103 0.47 47 donating hydroxyl groups substituted on phenyl ring
with addition of black radish juice 400 0.49  103 0.78 78
which tend to increase the inhibiting effect by forming
(CHBRNaCl) 600 0.38  103 0.83 83
800 0.35  103 0.84 84 chelates with metallic cations. Also, due to the presence
1000 0.19  103 0.92 92 of compound having sulphur, nitrogen and double bond
3% NaCl solutions of acacia honey 200 1.23  103 0.45 45 in the molecule (methylthiobutenyl glucosinolate in
(AHNaCl) 400 1.03  103 0.54 54 squeezed black radish juice) the inhibition efficiency of
600 9.80  104 0.56 56
chestnut honey with black radish juice added was more
800 6.42  104 0.72 72
1000 3.78  104 0.83 83 pronounced. It is, probably, a consequence of the pres-
3% NaCl solutions of acacia honey 200 8.95  104 0.60 60 ence of various adsorption active centres being able to
with addition of black radish juice 400 5.20  104 0.77 77 act synergistically to form a polymeric complex.
(AHBRNaCl) 600 4.95  104 0.78 78 A relationship of corrosion rate and exposure time of tin
800 4.15  104 0.82 82
to aqueous solutions of acacia and chestnut honey at two
1000 1.63  104 0.93 93
concentrations (200 ppm and 1000 ppm) is presented in
Fig. 1.
According to the shape of curves it is obvious that the
It was found that better surface coverage (H) and greatest change of corrosion rate happened in the first
higher inhibition efficiency (IE) were obtained for chest- 24 h at all the concentrations examined, while during fur-
nut honey solutions in comparison with solutions of aca- ther exposure of tin specimen to the aggressive medium
cia honey, especially when black radish juice was added. the corrosion rates decreased. The corrosion rates of tin
The increase of the surface area covered by the adsorbed are smaller for higher honey concentrations.
 I. Radojčić et al. / Corrosion Science 50 (2008) 1498–1504 1501

0.0025 0.0025
AHaq
CHaq 200 ppm
AHBRaq
CHaq 1000 ppm 0.002 AHNaCl

w /g cm-2 h-1
0.002 AHaq 200 ppm AHBRNaCl
3% NaCl
AHaq 1000 ppm 0.0015
w/g cm-2 h-1

0.0015
0.001

0.001 0.0005

0
0.0005 0 200 400 600 800 1000
c / ppm

0 Fig. 3. The values of tin corrosion rates after 24 h of exposure to 3% NaCl

0 24 48 72
time exposure / h
Fig. 1. Dependence of tin corrosion rate on exposure time of tin in
aqueous solutions of different concentration of chestnut (CHaq) and
acacia honey (AHaq).
The comparison of the values of tin corrosion rates after
24 h exposure time in 3% NaCl solution alone, and aque-
ous and sodium chloride solutions of chestnut and acacia
honey without and with addition of black radish juice at
all the concentrations used is shown in Figs. 2 and 3.
It is obvious that corrosion rates in experiments with
both honey varieties in all the solutions examined
decreased following an increase in concentrations of honey,
but the decrease of corrosion rate values was more pro-
nounced in sodium chloride solutions.
The potentiostatic polarization curves of tin in 3% NaCl
and 3% NaCl with chestnut honey in the absence and pres-
ence of black radish juice are shown in Fig. 4.
Addition of honey and honey with black radish juice
into 3% NaCl exerted a greater influence on cathodic than
on anodic polarization curves.
0.0025
0.002
w/g cm-2 h-1
96 120 alone and to aqueous and sodium chloride solutions of acacia honey
(AHaq and AHNaCl) without and with the addition of black radish juice
(AHBRaq and AHBRNaCl).
It is also evident that the values of corrosion potential
are shifted to the area of negative values of potential.
The potentiostatic polarization curves of tin in 3% NaCl
and in all the examined solutions of acacia honey in 3%
NaCl are similar to that of chesnut honey and therefore
are not given.
The electrochemical parameters (ba, bk, Ecorr, icorr)
obtained by potentiostatic polarization method of tin in
3% NaCl solutions without and with addition of inhibitors
at different concentrations, as well as the values of surface
coverage (H) and inhibition efficiency (IE) are given in
Table 3.
The H values are calculated according to the equation:
H ¼ ði0  iÞ=i0
where i0 is corrosion current of tin in solutions without
inhibitors, while i is corrosion current of tin in solutions
with inhibitors. Inhibition efficiency value IE is obtained
by multiplying the H value by 100.
The values of corrosion current of tin in the sodium
chloride solutions of both kinds of honey decrease, while
CHaq
CHBRaq
CHNaCl
CHBRNaCl
3% NaCl

0.0015

0.001

0.0005

0
0 200 400 600 800 1000
c / ppm

Fig. 2. The values of tin corrosion rates after 24 h of exposure to 3% NaCl

alone and to aqueous and sodium chloride solutions of chestnut honey Fig. 4. Tafel polarization curves for tin in solutions: (1) 3% NaCl; (2) 3%
(CHaq and CHNaCl) without and with the addition of black radish juice NaCl with 800 ppm acacia honey (AHNaCl); (3) 3% NaCl with 800 ppm
(CHBRaq and CHBRNaCl). acacia honey and black radish juice (AHBRNaCl).
1502 I. Radojčić et al. / Corrosion Science 50 (2008) 1498–1504

Table 3
Corrosion parameters obtained by the Tafel-extrapolation for tin in 3% NaCl without and with the addition of inhibitors at different concentrations at
(20.5 ± 0.4) °C
Potentiostatic polarization method
Solution choney ba bc Ecorr icorr H IE
(ppm) (mV/d) (mV/d) (mV) (mA cm2) (%)
3% NaCl – 49 108 320 1.75  103 –
3
3% NaCl solutions of chestnut honey (CHNaCl) 200 48 102 380 1.09  10 0.38 38
400 69 211 381 0.89  103 0.49 49
600 68 307 378 0.77  103 0.56 56
800 69 199 345 0.58  103 0.67 67
1000 48 114 383 0.26  103 0.85 85
3% NaCl solutions of chestnut honey with addition of black radish juice (CHBRNaCl) 200 68 191 371 1.05  103 0.40 40
400 71 164 368 0.86  103 0.51 51
600 66 168 372 0.54  103 0.69 69
800 32 33 383 0.47  103 0.73 73
1000 31 250 397 0.18  103 0.90 90
3% NaCl solutions of acacia honey (AHNaCl) 200 67 201 283 1.03  103 0.41 41
400 43 95 280 0.84  103 0.52 52
600 41 54 281 0.75  103 0.57 57
800 44 58 265 0.46  103 0.74 74
1000 31 32 273 0.39  103 0.78 78
3% NaCl solutions of acacia honey with addition of black radish juice (AHBRNaCl) 200 42 43 282 0.98  103 0.44 44
400 46 45 283 0.74  103 0.58 58
600 67 240 267 0.70  103 0.60 60
800 31 131 268 0.37  103 0.79 79
1000 37 104 273 0.23  103 0.87 87

those of surface coverage and inhibition efficiency increase 1200

following the increase of honey concentrations. The same 1000
trend, but with more pronounced values, is evident in
800
honey sodium chloride solutions with black radish juice
c/Θ

600
added. This is the consequence of the fact that honey and
black radish juice are multicomponent systems, consisting 400 CHNaCl
CHBRNaCl
of various compounds able to form protective layer on 200
tin surface, interact mutually or with protective layer. 0
The H values obtained by corrosion rate and corrosion 0 200 400 600 800 1000
current data fit into the Langmuir isotherm, and are related c / ppm
to the equilibrium constant K and c via equation Fig. 5. The relationship between c/H and concentrations of chestnut
honey alone (CHNaCl) and with addition of black radish juice (CHBRNaCl)
K  c ¼ H=ð1  HÞ in 3% NaCl solutions.

The linear dependence of c/H versus c of chestnut and

acacia honey in 3% NaCl solution in absence and presence
of black radish juice is used to determine the adsorption
equilibrium constant K as intercept on ordinate for c = 0 1400
(Figs. 5 and 6). 1200
The equilibrium constant (K) is related to the standard 1000
free energy of adsorption by the relationship: 800
c/Θ

600
K ¼ 1=55:5 expðDG0ads =RT Þ 400
AHNaCl
AHBRNaCl

200
where R is universal gas constant, and the value 55.5 is the 0
concentration of water in the solution, expressed in moles 0 200 400 600 800 1000
per dm3. c / ppm
The values of adsorption constants (K), and Gibbs free Fig. 6. The relationship between c/H and concentrations of acacia honey
energy (DG0ads ), calculated on the basis of H values (Table alone (AHNaCl) and with addition of black radish juice (AHBRNaCl) in 3%
2 and 3) for 3% NaCl solutions of acacia and chestnut NaCl solutions.
 I. Radojčić et al. / Corrosion Science 50 (2008) 1498–1504 1503

Table 4
The values of adsorption constant (K) and the adsorption Gibbs free energy changes (DG0ads ) for 3% NaCl solutions of chestnut and acacia honey alone and
with addition of black radish juice (Raphanus sativus L. var. niger) at 25 °C
Inhibitors c (ppm) Obtained from corrosion rate Obtained from corrosion current
K  103 (dm3) DG0ads (kJ mol1) K  103 (dm3) DG0ads (kJ mol1)
Chestnut honey (CHNaCl) 200
400
600 2.51 19.13 ± 0.01 3.18 19.70 ± 0.02
800
1000
Chestnut honey with black radish juice (CHBR NaCl) 200
400
600 9.52 22.38 ± 0.01 4.37 21.18 ± 0.11
800
1000
Acacia honey (AHNaCl) 200
400
600 4.55 19.10 ± 0.02 5.21 20.01 ± 0.12
800
1000
Acacia honey with radish juice (AHBRNaCl) 200
400
600 6.67 21.50 ± 0.01 5.18 20.28 ± 0.01
800
1000

honey without and with black radish juice added are listed
in Table 4.
Table 4 shows the thermodynamic data obtained from
the Langmuir adsorption isotherm for both honey varieties
without and with addition of black radish juice. The stan-
dard free energy of adsorption calculated from the surface
coverage values, obtained on the basis of corrosion rate,
vary in the range of 19.10 ± 0.02 to 21.50 ± 0.02 kJ/
mol for acacia honey and acacia honey with black radish
juice added, and from 19.13 ± 0.01 to 22.38 ± 0.01
kJ/mol for chestnut honey without and with black radish
juice added, respectively.
The data for DG0ads support a physisorption based mech-
anism for corrosion inhibition by compounds present in
honey and honey with black radish juice.
4. Conclusions
The following conclusions can be made on the basis of
the results obtained:
 Natural honey (chestnut and acacia) in 3% NaCl solu-
tion as well as their solutions with black radish juice
added act as corrosion inhibitors of tin.
 The inhibition efficiency (IE) of all the inhibitors exam-
ined obtained by both methods used decrease in the
order: chestnut honey with black radish juice > acacia
honey with black radish juice > chestnut honey > acacia
honey.
 The inhibition efficiency of honey and honey with black
radish juice increase with the increase of their
concentrations.
 The corrosion inhibition of tin in 3% NaCl solutions of
both honey varieties in the absence and presence of
black radish juice takes place via adsorption on the tin
surface following Langmuir adsorption isotherm.
Acknowledgement
The financial support of the Ministry of Science, Tech-
nology and Sport of Republic of Croatia (Grant No.
058-0582261-2256) is gratefully acknowledged.
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