Hydrometallurgy 81 (2006) 45 51

www.elsevier.com/locate/hydromet

Dissolution kinetics of chalcopyrite in acidic potassium

dichromate solution
S. Aydogan a , G. Ucar a , M. Canbazoglu b,
b

a
Department of Mining Engineering, Selcuk University, Konya, Turkey
Department of Mining Engineering, Cumhuriyet University, Sivas, Turkey

Received 1 July 2005; received in revised form 10 October 2005; accepted 20 October 2005

Abstract
The dissolution of chalcopyrite in acidic potassium dichromate solution has been investigated with respect to the effects of
sulphuric acid and potassium dichromate concentrations, by changing stirring speed, leaching temperature and particle size. It was
determined that dissolution rate increased with increasing sulphuric acid concentration, potassium dichromate concentration and
temperature. A particle size below 75 m was required to leach N 80% copper in 150 min at 90 C. The kinetic study showed that
the dissolution of chalcopyrite is represented by shrinking core model with diffusion through a porous product layer of sulphur. The
activation energy (Ea) for the dissolution reaction was calculated as 24 kJ/mol. Pyrite dissolution from the concentrate was
significant in potassium dichromate solutions because of its high oxidation potential.
2005 Elsevier B.V. All rights reserved.
Keywords: Chalcopyrite; Potassium dichromate; Leaching; Kinetic model; Diffusion

1. Introduction
Chalcopyrite is the most important copper sulphide
mineral. It is generally associated with other sulphide
minerals, such as galena (PbS), sphalerite (ZnS) and
pyrite (FeS2). These minerals are generally separated
from each other by flotation and treated by conventional
pyrometallurgical processes. About 8085% of the
world's copper production is carried out using pyrometallurgical processes with SO2 off-gases captured and
converted to sulphuric acid (Antonijevi et al., 2004).
In recent years, there has been a heightened interest in
the possible application of various reagents in the hy Corresponding author. Tel.: +90 346 2191010/1331; fax: +90 346
2191173.
E-mail address: mcanbaz@cumhuriyet.edu.tr (M. Canbazoglu).
0304-386X/$ - see front matter 2005 Elsevier B.V. All rights reserved.
doi:10.1016/j.hydromet.2005.10.003

drometallurgical processing of sulphide concentrates

especially chalcopyrite concentrates. Ferric and cupric
ions, oxygen and bacteria have been used as oxidative
leaching agents of chalcopyrite in sulphate and chloride media, under atmospheric or pressure conditions.
Leaching investigations of chalcopyrite show that this
mineral is hardly reactive at moderate temperatures
around 60 C (Dutrizac et al., 1969; Dutrizac, 1981;
Dutrizac and MacDonald, 1974; Charles and Han,
1997; Beckstead and Miller, 1977; Ammou-chokroom
et al., 1977a,b; Bonan et al., 1981; Rath et al., 1988;
Ngoc et al., 1990; Saxena and Mandre, 1992; Akcil
and Ciftci, 2003).
On the other hand, dichromate ion (Cr2O72) and
hydrogen peroxide (H2O2) have been used recently to
dissolve chalcopyrite in acidic medium because of
their higher oxidation potential compared with other

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S. Aydogan et al. / Hydrometallurgy 81 (2006) 4551

oxidising leaching reagents (Antonijevi et al., 1994,

2004). In this context, there has not been any proper
study with Cr2O72 ion, except for the studies of
Shantz and Morris (1974), Murr and Hiskey (1981)
and Antonijevi et al. (1994). However, Ruiz and
Padilla (1998) studied copper removal from molybdenite concentrate in acidic dichromate solution.
Oxidative dissolution of chalcopyrite by dichromate
ion in sulphuric acid produces elemental sulphur or
sulphate by the two reactions given as follows:

2
6CuFeS2 5Cr2 O2
6Fe3 12S0
7 70H 6Cu

10Cr3 35H2 O

2
6CuFeS2 17Cr2 O2
6Fe3
7 142H 6Cu
3
12SO2
71H2 O
4 34Cr

The reduction of dichromate ion in acidic solutions is

given by Jackson (1986) as:

3
7H2 O E 0 1:33V
Cr2 O2
7 14H 6e 2Cr

3
This potential value (1.33 V) is adequate to oxidise
almost all metal sulphides.
The activation energies and the kinetic models
explaining the oxidative dissolution of chalcopyrite by
various authors are summarised in Table 1. Accordingly, the dissolution mechanism of chalcopyrite is based
on three main kinetic models. These kinetic models are
diffusion, surface reaction and a mixed kinetic model
containing diffusion and surface reactions, which simultaneously take place. However, diffusion may occur

Table 2
Chemical compositions of chalcopyrite concentrate for different
particle size
Particle
size (m)

Element (%)
Cu

Fe

Zn

Pb

212 + 106
106 + 75
75 + 45
45 + 38
38

23.8
29.2
27.2
24.6
21.5

27.7
31.6
27.2
23.6
18.7

1.2
2.8
3.8
4.1
1.8

2.6
2.5
2.6
5.3
0.3

through an elemental sulphur layer or a different intermediate product on the chalcopyrite surface.
In this study, the reaction kinetics of chalcopyrite
with potassium dichromate was determined to understand the effect of strongly oxidising conditions where
both sulphur or sulphate may be formed. For this purpose, the effects of variables such as stirring speed, acid
and dichromate concentration, temperature, solid/liquid
ratio and particle size on the reaction rate were investigated. The reactivity of pyrite that is present in the
concentrate was also determined since this is usually
refractory under normal leaching conditions.
2. Experimental study
2.1. Materials
Chalcopyrite concentrate enriched through flotation
of a CuFeS2PbSZnS complex ore in the Menka
flotation plant (Sivas, Turkey) was used in this study.
Particle size fractions 212 + 106, 106 + 75, 75 + 45,
45 + 38 and 38 m were obtained by wet sieving.

Table 1
Reported kinetic models and activation energies for leaching of chalcopyrite with different leaching media
Leaching medium

Kinetic model
a

Fe2(SO4)3 + H2SO4

Diffusion

FeCl3 + HCl

Diffusionb
Mixed control modelc
Surface reaction
Diffusiona

CuCl2 + NaCl + HCl

FeCl3 + HCl + CuCl2 + NaCl
H2O2 + H2SO4
K2Cr2O7 + H2SO4
O2 + NH3
I2 + NH4
a
b
c

Surface reaction
Surface reaction
Surface reaction
Surface reaction
Surface reaction
Diffusionb

Through product layer.

Through constantly thickening product layer.
Surface reaction + diffusion.

Activation energy (kJ/mol)

Reference

71 12.5 (5094 C)
75 (45100 C)
125 12.5 (25100 C)
15.98 (3090 C)
92.8 (70100 C)
71 (above 85 C)
335 (under 85 C)

60 (2550 C)
49 (3080 C)
50 (2560 C)

50 (1635 C)
30.3 (3560 C)

Dutrizac et al. (1969)

Dutrizac (1981)
Ammou-chokroom et al. (1977a,b)
Saxena and Mandre (1992)
Rath et al. (1988)
Bonan et al. (1981)
Ngoc et al. (1990)
Antonijevi et al. (2004)
Antonijevi et al. (1994)
Murr and Hiskey (1981)
Beckstead and Miller (1977)
Charles and Han (1997)

S. Aydogan et al. / Hydrometallurgy 81 (2006) 4551

2.2. Experimental procedure

90
H2SO4 Concentration, mol/L

80

0.1

70

Cu Extraction, (%)

Chemical analysis of copper, iron, zinc and lead of each

size fraction was done by AAS (Unicam model 929)
and is listed in Table 2. Distilled water and reagentgrade chemicals were used to make up all required
solutions.

47

0.2
0.3

60

0.4
0.5

50
40

A 1-L glass leach reactor was equilibrated to a temperature of 50 to 97 C (boiling temperature) in a water
bath thermostatically controlled with 0.2 C sensitivity. Stirring was provided in the range of 250700 rpm.
The H2SO4 and K2Cr2O7 concentration was in the range
of 0.10.5 mol/L and 0.010.15 mol/L, respectively;
whilst the particle size fractions were 212 + 106, 106
+ 75, 75 + 45, 45 + 38 and 38 m. The liquid volume was kept constant during the experiments carried
out at various solid/liquid ratios. Analysis of copper and
iron in the leach solution were determined at various
times by AAS.

Fig. 2. Effect of H2SO4 concentration on copper extraction

([K2Cr2O7], 0.1 mol/L; stirring speed, 400 rpm; temperature, 50 C;
solid/liquid ratio, 10 g/L; particle size, 75 + 45 m).

3. Results and discussion

3.2. Effect of H2SO4 concentration

3.1. Effect of stirring speed

The effect of sulphuric acid concentration on chalcopyrite dissolution (Fig. 2) shows increasing copper
extraction with increasing sulphuric acid concentration. The copper leached after 150 min at 50 C with
0.1 mol/L and 0.4 mol/L H2SO4 was 20% and 54%,
respectively. It is well known, by applying the Nernst
equation to Eq. (3), that increasing the hydrogen ion
concentration increases the reduction potential of dichromate ion.

The effect of stirring speed on the dissolution of

chalcopyrite was investigated in the range of 250700
rpm. The results in Fig. 1 show no significant difference
in copper extraction in this range. In investigations of
the effect of other parameters, 400 rpm was selected as
the optimum operating stirring speed.

30
20
10
0
0

30

60

90

120

150

Leaching Time, (min.)

90

3.3. Effect of K2Cr2O7 concentration

Stirring Speed, rpm

80

250

Cu Extraction, (%)

70

300
400

60

600

50

700

40
30
20
10
0
0

30

60

90

120

150

Leaching Time, (min)

Fig. 1. Effect of stirring speed on copper extraction ([K2Cr2O7], 0.1
mol/L; [H2SO4], 0.4 mol/L; temperature, 50 C; solid/liquid ratio, 10
g/L; particle size, 75 + 45 m).

The effect of K2Cr2O7 concentration on the copper

extraction from chalcopyrite using a pulp density of 10
g/L is given in Fig. 3. The copper recovery increased
from 7% to 58% after 150 min when the concentration of
K2Cr2O7 was increased from 0.01 mol/L to 0.15 mol/L,
respectively. According to the stoichiometry of Eqs. (1)
and (2) and the composition of the concentrate, a minimum concentration of about 0.04 mol/L dichromate is
required to extract all the copper when sulphur is
formed; whilst about 0.12 mol/L dichromate is required
when sulphate is formed at this pulp density. No significant difference was observed with increasing the
K2Cr2O7 concentration from 0.1 mol/L to 0.15 mol/L;
therefore, a value of 0.1 mol/L was chosen for further
investigations at a pulp density of 10 g/L. It was assumed that sulphur is the main product of reaction as it
was not possible to measure sulphate ion formation in

48

S. Aydogan et al. / Hydrometallurgy 81 (2006) 4551

100

90
K2Cr2O7 Concentration, mol/L

80

90

0.01

80

0.02

70
60

Cu Extraction, (%)

Cu Extraction, (%)

0.04
0.06
0.1

50

0.15

40
30

70
60
50
40
Particle Size, m

30

-38

20

-45 +38

20

-75 +45

10

10

0
0

30

60

90

120

150

Leaching Time, (min.)

-106 +75
-212 +106

0
0

30

60

90

120

150

Leaching Time, (min.)

Fig. 3. Effect of K2Cr2O7 concentration on copper extraction

([H2SO4], 0.4 mol/L; stirring speed, 400 rpm; temperature, 50 C;
solid/liquid ratio, 10 g/L; particle size, 75 + 45 m).

the presence of sulphuric acid. With higher pulp densities, there was a deficiency in dichromate ion at the
chosen concentration of 0.1 mol/L and copper extraction
decreased.

Fig. 5. Effect of particle size on copper extraction ([H2SO4], 0.4 mol/

L; [K2Cr2O7], 0.1 mol/L; stirring speed, 400 rpm; solid/liquid ratio, 10
g/L; temperature, 90 C).

after 150 min, increasing to 82% at the boiling

temperature of 97 C. To investigate the other leaching parameters, 90 C was chosen for the leaching
temperature.

3.4. Effect of temperature

3.5. Effect of particle size
The effect of temperature on copper extraction is
given in Fig. 4. At 50 C, 54% copper was extracted
Temperature, C

100

50

Cu Extraction, (%)

90

60

80

70

70

97

90

As shown in Fig. 5, the copper extraction increases

with decreasing particle size. Copper extraction
reached 40% and 92% after 150 minutes leaching for
212 + 106 and 38 m particle sizes, respectively. It
appears necessary to grind the chalcopyrite to below
75 m to achieve good copper extraction in a reasonable time.
3.6. Kinetic analysis

60
50

The dissolution of chalcopyrite can be explained by

a shrinking core model (Ghosh and Ray, 1991) which
can be expressed as follows:

40
30
20

aAfluid bBparticle Product

10
0
0

30

60

90

120

150

Leaching Time, (min.)

Fig. 4. Effect of temperature on copper extraction ([H2SO4], 0.4 mol/
L; [K2Cr2O7], 0.1 mol/L; stirring speed, 400 rpm; solid/liquid ratio, 10
g/L; particle size, 75 + 45 m).

If the reaction rate is controlled by diffusion through

a product layer, the integrated rate equation is as follows
(Sohn and Wadsworth, 1979):
2
2MB DCA
1 X 1X 2=3
t kd t
3
qB ar02

S. Aydogan et al. / Hydrometallurgy 81 (2006) 4551

0.14

If reaction is controlled by a surface reaction, Eq. (4)

is transformed to Eq. (6) (Levenspiel, 1972).

Temperature, C

0.12

1-2/3X-(1-X)2/3

where X is the fraction reacted, kc is the kinetic constant,

MB is the molecular weight of the solid, CA is the
concentration of the dissolved lixiviant A in the bulk
of the solution, a is the stoichiometric coefficient of the
reagent in the leaching reaction, r0 is the initial radius of
the solid particle, t is the reaction time, D is the diffusion coefficient in the porous product layer, B density
of the solid and kd and kr are the rate constants, respectively, which are calculated from Eqs. (5) and (6),
respectively.
Eq. (5) reveals that if the diffusion through the product layer controls the leaching rate, there must be a
linear relationship between the left side of equation
and time. The slope of the line is the apparent rate
constant kd, which is directly proportional to 1/r02. If
the surface reaction controls the rate, the relation between the left side of Eq. (6) and time must be linear.
The slope of this line is called the apparent rate constant
kr and is directly proportional to 1/r0.
The apparent rate constants (kr, kd) obtained for both
equations and the correlation coefficients were calculated from the plots at each temperature in Fig. 4. The
results are given in Table 3 which shows that the dissolution of chalcopyrite in the temperature range of 5097
C fitted the diffusion model given in Eq. (5). The
results obtained by the application of Eq. (5) to the
values given in Fig. 4 are shown in Fig. 6. As it is
known that a porous elemental sulphur layer occurs on
the chalcopyrite surface during oxidative dissolution
with Fe(III) and with Cu(II) in chloride media (Dutrizac, 1981; Ngoc et al., 1990; Hiroyoshi et al., 2001;
O'Malley and Liddell, 1987; Rath et al., 1988; Dutrizac
et al., 1969; Ammou-chokroom et al., 1977a,b; Hiroyoshi et al., 2004; Dutrizac and MacDonald, 1978,
1974), a similar situation must be valid for oxidative

50
60

70

0.10

90
97

0.08
0.06
0.04
0.02
0.00
0

30

60

90

120

150

Time, min.
Fig. 6. Plot of Eq. (5) vs. t for different temperatures.

of chalcopyrite with dichromate ions. In other words,

the copper extraction is controlled by diffusion of dichromate ion through this layer to the mineral surface or
by the diffusion of dissolved ions into the solution.
Using the apparent rate constants (kd) obtained by
the application of Eq. (5), the Arrhenius plot was
obtained (Fig. 7). The activation energy was calculated
as 24 kJ/mol. This value clearly confirms that this
process was controlled by diffusion (Habashi, 1999).
On the other hand, Antonijevi et al. (1994, 2004) and
Murr and Hiskey (1981) reported that copper extraction
in dichromate solution conformed to a surface reactioncontrolled shrinking sphere model expressed by Eq. (6)
-6.8

-7.2
Ea= 24 kJ/mol

ln kd

11X 1=3

kc M B C A

t kr t
qB ar0

49

-7.6

Table 3
The kr, kd values and correlation coefficients for each temperature
Temperature
(C)

kr
(10 3 min 1)

R2

kd 10 3
(10 3 min 1)

R2

-8.0

50
60
70
90
97

1.75
2.09
2.56
3.04
3.32

0.894
0.844
0.765
0.882
0.862

0.30
0.41
0.49
0.78
0.93

0.999
0.997
0.997
0.999
0.997

-8.4

([H2SO4], 0.4 mol/L; [K2Cr2O7], 0.1 mol/L; stirring speed, 400 rpm;
solid/liquid ratio, 10 g/L; particle size, 75 + 45 m).

2.7

2.8

2.9

1000/T

3.0

(K-1)

Fig. 7. Arrhenius plot for chalcopyrite oxidation.

3.1

50

S. Aydogan et al. / Hydrometallurgy 81 (2006) 4551

Table 4
Effect of temperature on iron extraction and pyrite dissolution
Leaching
time
(min)
5
10
30
60
90
120
150

Leaching temperature
50 C

97 C

Fe (%)

FeS2 (%)

Fe (%)

FeS2 (%)

6.1
12.8
25.8
37.7
45.1
50.2
55.5

6.9
16.8
25.3
40.9
50.1
56.7
65.4

15.8
25.7
46.9
65.4
71.9
78.1
82.4

18.9
32.2
53.0
73.8
79.6
82.8
85.6

([H2SO4], 0.4 mol/L; [K2Cr2O7], 0.1 mol/L; stirring speed, 400 rpm;
solid/liquid ratio, 10 g/L; particle size, 75 + 45 m).

and the activation energy was found to be approximately 50 kJ/mol.

3.7. Pyrite dissolution
The dissolution of other sulphide minerals such as
pyrite, sphalerite and galena during the oxidative leaching of chalcopyrite concentrate is very important to
understand the leach selectivity. It is well known that
the oxidative dissolution of galena produces insoluble
PbSO4 in sulphuric acid leaching medium whilst the
oxidation of sphalerite occurs more easily than chalcopyrite (Dutrizac and MacDonald, 1974, 1978). On the
other hand, pyrite is more refractory and dissolves only
through oxidation of sulphide to sulphate according to
Eq. (7) (Antonijevi et al., 1993).

3
3
2FeS2 5Cr2 O2
4SO2
7 38H 2Fe
4 10Cr
19H2 O
7

The mineralogical composition of the 75 + 45 m

fraction of chalcopyrite concentrate studied in this work
can be calculated, using the values of Table 2, as 79%
CuFeS2, 7% FeS2, 6% ZnS, 3% PbS and 5% unaccounted for by XRD analyses (quartz and other minerals).
This mineralogy seems to be typical compositions of
many chalcopyrite concentrates.
The iron ions in the leaching solution were also
analysed. This occurs from both chalcopyrite and pyrite
according to reactions (1), (2) and (7). Thus, the pyrite
dissolution can be calculated by considering the total
iron in solution, the iron coming from chalcopyrite and
the iron content of the sample. The total iron extraction
and calculated pyrite dissolution at different leaching
temperatures are given in Table 4.
Table 4 shows that pyrite was also oxidized with
dichromate ions during chalcopyrite concentrate leach-

ing. The dissolution of pyrite increases with time and

temperature and reached 85% at 97 C after 150 min
of leaching. This pyrite dissolution kinetics seems to
be faster than the chalcopyrite dissolution and faster
than leaching with Fe(III) or Cu(II)/Cl. Therefore,
when the chalcopyrite concentrate is impure, dichromate leaching of chalcopyrite concentrate does not
give good selectivity.
4. Conclusion
In this study the dissolution kinetics of chalcopyrite
concentrate in acidic potassium dichromate solutions
was studied. It was determined that the reaction rate
increased with increasing sulphuric acid and potassium
dichromate concentrations and temperature, and with
decreasing particle size. The optimum leaching conditions with a 10 g/L solid/liquid ratio were determined
as: 0.4 mol/L H2SO4, 0.1 mol/L K2Cr2O7, 97 C, 400
rpm. With a particle size of 75 + 45 m, 82% copper
was extracted after 150 min with further extraction
taking place over extended time.
The chalcopyrite dissolution in dichromate solutions
seems to be faster than other oxidative leaching reagents
such as ferric and cupric ions. Pyrite dissolution also
seems to be faster and its oxidation more effective.
A shrinking core model can be used to describe the
dissolution kinetics of chalcopyrite in acidic potassium
dichromate solutions above 50 C. The dissolution process was found to be controlled by diffusion through a
porous product layer. The activation energy of the dissolution process was found to be 24 kJ/mol, which was
lower than the activation energy found by Murr and
Hiskey (1981) and by Antonijevi et al. (1994) who
considered that the reaction was described by a surface
reaction shrinking sphere model.
Acknowledgements
This study was supported by The Research Foundation of Selcuk University under Project No. BAP-2004/
088.
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