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Computers and Chemical Engineering 32 (2008) 23952402

An analyticalnumerical method for solving a heap leaching problem

of one or more solid reactants from porous pellets
Mario E. Mellado , Luis A. Cisternas
Departamento de Ingeniera Qumica, Universidad de Antofagasta, Centro de Investigacion Cientco Tecnologico
para la Minera (CICITEM), Chile
Received 4 September 2007; received in revised form 26 December 2007; accepted 1 January 2008
Available online 6 January 2008

Abstract
In this paper we present an alternative method based on analytical and numerical solutions for solving the differential equations which describe
heap leaching of one or more solid reactants from porous pellets. We propose to use analytical solutions for the differential equations which describe
rate dissolutions along the pores and the surface of the particles under suitable regularity conditions. Moreover, we propose to use continuous and
discontinuous solutions for the continuity partial differential equations describing balances. We comment on the efficient numerical solving of the
remaining partial differential equations within the proposed numerical scheme. All of this, allows to obtain a numerical algorithm which is fast and
accurate for the heap leaching problem. Also, we include particle size distributions on the proposed numerical methodology. This method applies
to the case where the rate-controlling reagent is a component of the lixiviation solution only and not of the gas phase. The model includes the
effects of particle scales, kinetic factors, heap scales and several operation variables. Finally, numerical experiments are presented.
2008 Elsevier Ltd. All rights reserved.
Keywords: Heap leaching; Differential equations; Discontinuous solutions; Analytical solutions; Numerical methods

1. Introduction
Heap leaching is a hydrometallurgical process which has been
used since a long time which was originally designed for oxides
ores but today have several applications including sulphide ores
and caliche minerals. Heap leaching has been a matter of wide
research and several mathematical models which allows to simulate, analyze, design and optimize these operations. Indeed,
the extractive metallurgy by chemical dissolution is one of the
metal recuperation techniques most used in modern industry.
Nowadays, the main interest to use hydrometallurgical processes
arises from avoiding ambient contamination produced by conventional pyro-metallurgical processes and the treatment of low
grade minerals. Also, heap leaching allows low operational cost
from the energetic and production point of view. The heap leaching can use a pre-treatment of the ore. This operation generally
is based upon the trituration of the ore up to a finer level and

Corresponding author. Tel.: +56 55 637313; fax: +56 55 240152.

E-mail addresses: mmellado@uantof.cl (M.E. Mellado),
lcisternas@uantof.cl (L.A. Cisternas).
0098-1354/$ see front matter 2008 Elsevier Ltd. All rights reserved.
doi:10.1016/j.compchemeng.2008.01.001

its granulation by means of water and concentrated sulphuric

acid. Throughout this process, it is possible to increase the heap
material resistance while keeping good enough permeability.
All of this with the objective of constructing heaps with a suitable height, improve the recuperation and decrease the leaching
time. The solution obtained in heap leaching is sent to recuperation operations, usually solvent extraction. A complete literature
review is outside the objective of this work, but a brief revision
is given hereafter.
In de Andrade Lima (2004), is presented a model to simulate
the transient evolution of the dissolved chemical species in the
heap and column isothermal leaching processes. In Bouffard and
Dixon (2001), a study about the heap leaching planning from a
optimization point of view is presented. In Bouffard and Dixon
(2006), the rates of pore diffusion and cyanide gold dissolution
in coarse, porous gold oxide ore particles are compared. Respect
to the numerical solution of a two dimensional partial differential
equations model for a two-phase flow in a porous media representing the leaching process we refer to Cariaga, Concha, and
Sepulveda (2005). With respect a two-dimensional partial differential equations model in bioleaching we can cite the work of
Casas, Martnez, Moreno, and Vargas (1998). In Cross, Bennett,

2396

M.E. Mellado, L.A. Cisternas / Computers and Chemical Engineering 32 (2008) 23952402

Nomenclature
bi
CA0
CE0
Cp
Cs
DAe
E
kp
ks
R
t
us
x
z
Z

stoichiometric number (mol/mol)

reference reagent concentration
initial extractable grade of solid reactant (mol/g)
is the grade of solid reactant within particle
(mol/g)
is the grade of solid reactant on particle surface
(mol/g)
effective pore diffusivity of reagent (cm3 /(cm s))
extraction
is the rate constant of solid reactant within particle
(mol/(g s))
is the rate constant of solid reactant on particle
surface (mol/(cm2 s))
particle radius (cm)
time (s)
superficial bulk flow velocity (cm3 /(cm2 s))
space coordinate (cm)
space coordinate (cm)
heap depth (cm)

Greek letters

dimensionless concentration of reagent

b
dimensionless concentration of the reagent external to the particle

reagent strength parameter relative to solid reactant

b
bulk solution volume fraction
h
heap void fraction
ore porosity
0

dimensionless flow time

p
Damkohler II number for solid reactant within the
particle
s
Damkohler II number for solid reactant on the
particle surface

surface fraction of solid reactant

0
ore density (g/cm3 )
p
dimensionless grade of solid reactant within the
particle
s
dimensionless grade of solid reactant on the particle surface
p
reaction order for solid reactant within particle
reaction order for solid reactant on the particle
s
surface
i
dimensionless concentration of dissolved species
ib
dimensionless bulk concentration of dissolved
species

Croft, McBride, and Gebhardt (2006), a framework was developed for multi-phase flows, gasliquidsolid, in reactive porous
media, capturing several key chemico-physicalbacterial phenomena and their interactions. In Lizama, Harlamovs, McKay,
and Dai (2005), it is shown that for sphalerite and pyrite heap
bio-leaching kinetics were proportional to the irrigation rate

divided by the height. In Mousavi, Jafari, Yaghmaei, Vossoughi,

and Sarkomaa (2006), is provided a detailed information of
momentum and mass transfer phenomena in a granular bed. In
Sheikhzadeh, Mehrabian, Mansouri, and Sarrafi (2005), unsaturated flow of liquid in a bed of uniform and spherical ore particles
is studied numerically and experimentally. An unsteady and
two-dimensional model is developed on the basis of the mass
conservation equations of liquid phase in the bed and in the particles. The model equations are solved using a fully implicit finite
difference method giving the distribution of the degree of saturation in the particles and in the bed and the vertical velocity of
flow in the bed, as well as the effect of periodic infiltration on the
above distributions. In Sidborn, Casas, Martinez, and Moreno
(2003), a two-dimensional dynamic model for bio-leaching of
secondary copper minerals from a pile has been developed. The
set of partial differential equations is solved using commercial
software. In Wu, Liu, and Tang (2007), the governing equations
for a fully coupled flowing-reaction-deformation behaviour with
mass transfer in heap-leaching are developed. The model equations are solved using an explicit finite difference method
under the conditions of invariable application rate and constant
hydraulic head.
In the work Dixon and Hendrix (1993a, 1993b), is presented
a mathematical model, in dimensionless form, for heap leaching
of one or more solid reactants from nonreactive, porous, spherical ore particles. These contributions are significant to model
the complete heap leaching process (Cross et al., 2006). However, the works of Dixon and collaborators require of expensive
numeric procedures to solve their equations, situation that limits their applicability, for example, in optimization. The main
goal of this work is to develop an efficient analyticalnumerical
scheme for solving differential equations that describe heap
leaching. An outline of the paper is as follows. In Section 2 we
present a mathematical framework already presented in the literature. In Section 3 we show our analyticalnumerical scheme
for the model problem. Some numerical essays are shown in
Section 4. Finally, we conclude with some remarks in Section 5.
2. Mathematical framework
Following Dixon and Hendrix (1993a, 1993b), we present
a system of partial and ordinary differential equations which
describes heap leaching. For further details we refer to Dixon
and Hendrix (1993a, 1993b). First, we define the following
parameters:
s =

3ks Css R
,
bi DAe

0 bi CA0
,
0 (1 0 )CE0

3(1 h )DAe Z
,
us R 2

p =

0 (1 0 )kp Cpp R2
bi DAe
=

b
and
0 (1 h )

where ks is the rate constant of solid reactant on the particle

surface (mol/(cm2 s)), Cs the grade of solid reactant on particle surface (mol/g), s denotes the reaction order for solid

M.E. Mellado, L.A. Cisternas / Computers and Chemical Engineering 32 (2008) 23952402

reactant on particle surface, R the particle radius (cm), bi the

stoichiometric number (mol/mol), DAe the effective pore diffusivity of reagent A (cm3 /(cm s)), 0 the ore density (g/cm3 ),
0 the ore porosity, kp the rate constant of solid reactant within
particle (mol/(g s)), Cp the grade of solid reactant within particle
(mol/g), p stands for the reaction order for solid reactant within
particle, CA0 the reference reagent concentration, CE0 the initial
extractable grade of solid reactant (mol/g), b the bulk solution
volume fraction, h the heap void fraction, us the superficial bulk
flow velocity (cm3 /(cm2 s)) and Z denotes the heap depth (cm).
With this, the ordinary differential equation to compute p ,
the dimensionless grade of solid reactant within the particle, is
given as follows:
dp
p
=
p
dt
(1 ) p

(1)

p (x, 0) = 1,
where t is the time, x the space coordinate, p the Damkohler II
number for solid reactant within the particle, a dimensionless
stoichiometric ratio which indicates reagent strength relative to
the grade of solid reactant, the fraction of solid reactant residing on the particle surfaces initially and is the dimensionless
reagent concentration.
The ordinary differential equation to compute s , the dimensionless grade of solid reactant on the particle surface, is given
by
ds
s s
=
b
dt
s

particle and the other one describes the interaction of all particles
through the heap. Of course, the particle time scale is faster than
the time scale which involves all particles. Therefore, the time
t in all the particular model equations must be replaced with a
dimensionless bulk flow time to solve the equations with a
common time.
Now, we present the partial differential equation to compute
the dimensionless concentration of dissolved species i , this is
3 i
2 i
i
2 i
+
=
=
+ p p

t
x2
x x
i (x, 0) = 0
and the boundary conditions:
i
(0, t) = 0.
x

We note that
us t
.
=
b Z
In the bulk lixiviant of the heap, the partial differential
equation to compute the dimensionless bulk concentration of
dissolved species ib is given by


ib
ib
i
=

(5)

z
x (x=1)
together with the initial condition:

(2)

ib (z, 0) = 0

together with the initial condition:

and the boundary condition:

s (0) = 1,

ib (0, ) = 0.

where s is the Damkohler II number for solid reactant on the particle surface and b stands for the dimensionless concentration
of the reagent in the bulk solution external to the particle. The
differential Eqs. (1) and (2) are complemented with four partial
differential equations to have a model for heap leaching. In fact,
the continuity equation for , the dimensionless concentration
of reagent A, is given by

2 2
= 2 +
p p
t
x
x x

The balance equation for a strictly aqueous phase reagent in

the bulk lixiviant is expressed by means of
 
b
b

(6)

z
x (x=1)
together with the initial condition:
b (z, 0) = 0

(3)

together with the initial condition:

(x, 0) = 0
and the boundary conditions:

(0, t) = 0.
x
It is important to remark that the differential Eqs. (1)(3)
describe the leaching of one particle. It will be clear in the following that our analysis is also applicable to this situation (Dixon
& Hendrix, 1993a).
There exist two time scales involved in this heap leaching
model. One time scale describes the chemical reactions within a
(1, t) = b ,

(4)

together with the initial condition:

i (1, t) = b ,

together with the initial condition:

2397

and the boundary condition:

b (0, ) = 1.
The differential Eqs. (1)(6) complete a partialordinary differential equation model for heap leaching. We use the notion of
extraction of reactant from the heap, which represents the total
fraction of extractable reactant which has issued from the heap at
any given time. Except for very short leaching times or in heaps
with an unusually high holdup, extraction takes approximately
the same value as conversion. Therefore, as a heap performance
index we use the extraction notion, which can be written as

E() =
ib (1, t) dt.
(7)
0

2398

M.E. Mellado, L.A. Cisternas / Computers and Chemical Engineering 32 (2008) 23952402

Unlike conversion, extraction may be evaluated directly from

chemical analysis of the heap effluent and therefore, is far a more
convenient measure of the heap performance.
3. The analyticalnumerical scheme for the model
Now, we discuss in detail the analyticalnumerical aspects for
solving the system (1)(6). First, it is clear that there exist couplings between the differential equations through the unknown
variables and the initial and boundary conditions. Moreover, the
model consists in two ordinary differential Eqs. (1) and (2), two
partial differential equations of first order (5) and (6) and two
equations of second order (3) and (4).
We first concentrate our attention in (1) and (2). Certainly,
at a first glance, these equations cannot be solved analytically
because the term and b . Moreover, we remark that the terms
and b in the right-hand side of both equations are discrete and in
certain sense, the only way to solve these equations is via numerical methods, such as Euler, RungeKutta, among others (Stoer
& Bulirsh, 1996). As we will solve the system of differential
equations in an iterative way, we can assume that the functions
and b are constants through a small enough time step, i.e.,
these functions are considered to have enough regularity. If we
assume the latter, Eqs. (1) and (2) have the structure of a general
first order ordinary differential equation. All of this, have the
obvious consequence of improve the speed and accuracy of the
numerical code.
Certainly, by using ordinary differential equations theory
(Boyce & Di Prima, 1993), we find that, and considering reaction
order for both equations as equal to the unity:


p
p (x, ) = exp
(8)
3(1 )
and

s (x, ) = exp

s
3


.

(9)

It is important to recall that if it is necessary to consider

reactions orders p and s different to the unity, the differential equations can be solved analytically by using the Bernoulli
transformation (Boyce & Di Prima, 1993):
v = p1p

and v = s1s ,

respectively.
Now we describe our approach for the partial differential Eqs.
(3) and (4). These equations are actually the radial part of the
Helmholtz equation written in spherical coordinates. Although
its is possible to solve (3) and (4), under several assumptions, in
an analytical manner, we note that this is quite expensive from the
theoretical and numerical point of view. The analytical solution
of this equation needs to consider a finite number of terms in an
infinite sum of terms and for each term, it is necessary to solve
a nonlinear equation. This procedure is, at least, so expensive
from the computational point of view than using, for instance,
finite differences. Moreover, it is easier to deal with a numerical
method than sum truncation in what concerns error studies of
the proposed methodology.

There exist a number of ways to solve numerically these equations. We note that the number 2 in Eqs. (3) and (4) corresponds
to spherical diffusion and corresponds to the radial part of the
Helmholtz equation in spherical coordinates (see Bouffard &
Dixon, 2001, Eq. (5)).
We can mention the finite difference method (Hackbusch,
1992), the finite element method (Brenner & Scott, 1994; Ciarlet,
1978; Hackbusch, 1992; Zienkiewicz & Taylor, 2000), finite
volume methods, among others. We recall that we use uniform
discretizations for solving Eqs. (3) and (4). In this sense, and
by considering standard versions, the use of the finite element
method or finite differences is equivalent. Also, as the finite
differences are easier to handle as compared with finite elements, we solve these equations with a CrankNicholson fully
implicit finite difference scheme (Hackbusch, 1992). Both equations, after the discretization procedure, require the solving of
a linear tridiagonal system of equations whose entries depends
entirely of the discretization in time and space coordinates. It
is very important to note that the generated matrices are sparse,
non symmetric and stable. Therefore, we have to deal with a
linear system of equations that must be solved in each step of
the iterations either in space or time. The linear systems can be
solved with a number of methods (Stoer & Bulirsh, 1996). We
use here a preconditioned LU solver and we recall other solvers
can be used, specially taking into account the sparse structure of
the matrices. For programming purposes, we note that it is only
necessary to assemble the matrices just once, but update their
respective right-hand sides each iteration. Therefore, there is no
computational effort in assembling the stiffness matrices.
Now we present our approach for the partial differential Eqs.
(5) and (6). First, we note that both equations have exactly the
same structure and they differs just on the initial and boundary conditions. Again, we need to mention that these equations
can be solved numerically by using, for example, the tracking of
fluid elements, finite volume methods or other similar numerical
methods. In despite of that, we solve these equations in an analytical manner. We recall that in the bulk lixiviant of the heap, the
mass balance for dissolved species is given by Eq. (5). To obtain
analytical solutions, we consider the transformation (Kesavan,
1989):
=z

and

= z + .

With this, and after some computations, we find that



ib
i
.
=

2 x (x=1)
Now, by using the initial and boundary value conditions, we
have
ib (z, ) = ,

<z

(10)

> z,

(11)

and
ib (z, ) = z,
where


i
=
.
2 x (x=1)

M.E. Mellado, L.A. Cisternas / Computers and Chemical Engineering 32 (2008) 23952402

By using the same arguments, we find the analytical solution

for (6), this is
b (z, ) = ,

<z

where
=

2 x

> z,

3.1. Heap leaching with homogeneous particles sizes

(12)

Now, we present the algorithm by considering heap leaching with homogeneous particle sizes. The algorithm reads as
follows, for a Z space step, solve:

(13)

Given p and b , obtain by solving

and
b (z, ) = 1 z,

2399


.
(x=1)

We note that (10) and (11) are continuous in R2 while (12)

and (13) is discontinuous when z = . This discontinuity reveals
the important fact that, for b , the partial differential equation
could be modified in order to have a consistent model. This can
be achieved, for instance, by introducing a second order term
which allows to have a continuous solution.
On the other hand, the discontinuity is just when = z which
is a zero measure set in R2 (Kufner, John, & Fucik, 1977), which
suggests the use of this discontinuous solution because the regularizing effect of the sequence of integrations. This fact is proved
via numerical experiments which shows not only good results
in what concerning the agreement with reality but also giving
suitable continuous global solutions.
Now, in what concerning the use of size distribution of particles functions, as the GatesGaudinSchumann distribution,
our analyticalnumerical approach applies without any modification which allows to deal with distribution of particles just by
taking under consideration the corresponding scaling for p ,
and by means of defining a reference particle size (Dixon &
Hendrix, 1993a, 1993b).
Now, we discuss on the algorithmic aspects itself. In fact,
once we know how to solve each differential equation there
exists mainly two approaches to compute the solution of the system, namely, uncoupled and totally coupled. The totally coupled
approach consists on solving a non-linear system of algebraic
equations per iteration which means to deal with nonlinear
solvers, uniqueness of solution studies, non feasible solutions,
the conditions to achieve correct solutions and take care about
the cost of the computational implementation. But, if we follow
this approach correctly, we would have a very accurate solution.
It depends on the application if such accurate solution is needed
or not.
On the other hand, the uncoupled algorithm means that the
solution of the previous equations are introduced as source terms
to the other equations producing a sequence of equations solving. Of course, this method introduces numerical errors if one no
take care about discretizations in time and space. But the implementation cost is lower, the errors can be controlled and with our
approach, one can infer that the errors are not high because we
have analytical solutions. Also, it is much easier to understand
from the engineering and numerical point of view.
Therefore, we solve the model with the uncoupled scheme
and the order of solving Eqs. (1)(6) is within two sweeps of
iterations. The inner loop is in space and the outer loop is in
time.

2 2
= 2 +
p p , (x, 0) = 0,
t
x
x x

(1, t) = b ,
(0, t) = 0.
x
With obtain p through

p (x, ) = exp

p
3(1 )


.

With obtain s through


s (x, ) = exp

s
3


.

Obtain i by solving
2 i
3 i
2 i
+
=
+ kp p ,

x2
x x
i
i (1, t) = b ,
(0, t) = 0.
x

i (x, 0) = 0,

Compute the corresponding fluxes for and i .

Compute ib and b through


i
,
ib (z, ) =
2 x (x=1)

<z

and


i
ib (x, t) =
z,
2 x (x=1)

> z.

Also
b (z, ) =

 

,
2 x (x=1)

<z

and
b (x, t) = 1

 

z,
2 x (x=1)

> z.

Compute and store


E() =
0

ib (1, t) dt.

Do the same up to Z = 1. Then, increase t. Once the desired

simulation time is reached, stop the iterations.

2400

M.E. Mellado, L.A. Cisternas / Computers and Chemical Engineering 32 (2008) 23952402

3.2. Heap leaching with distribution function for different

particles sizes
To deal with heap leaching with a distribution function for different particles sizes, we define a dimensionless particle radius
as
=

R
,

b (z, ) = 1

= 2 ,

w = 2 w

and using the GatesGaudinSchuhmann distribution function

of parameter m, the algorithm is as follows: for a Z space step,
solve:
Given p and b , obtain by solving

2 2
= 2 +
p p , (x, 0) = 0,
t
x
x x

(1, t) = b ,
(0, t) = 0.
x


p
3(1 )

s
3

1  

m m3 d z,


.


.

Obtain i by solving
3 i
2 i
2 i
+
=
+ p p ,
2

x
x x
i
i (x, 0) = 0, i (1, t) = b ,
(0, t) = 0.
x

ib (1, t) dt.

Do the same up to Z = 1. Then, increase t. Once the desired

simulation time is reached, stop the iterations.
We use Gauss quadrature for computing E and recall other
methods can be used (Stoer & Bulirsh, 1996). We finally note
that, even for dense simulations, the only time cost is due to the
numerical solution of the two differential Eqs. (3) and (4). Also,
every time the inner loop is finished, the extraction (7) must be
stored for further study.

Compute the corresponding fluxes for and i .

Compute ib and b through
ib (z, ) =

1 


0

m m3 d ,

<z

m m3 d z,

> z.

(x=1)

and
ib (z, ) =

1 


0

(x=1)

Also
b (z, ) =


0

1  

(x=1)

m m3 d ,

> z.

(x=1)

Before to start with a numerical experimentation of our

approach we need to point out that our approach is able to reproduce the results shown in Dixon and Hendrix (1993a, 1993b),
by considering the operation conditions indicated there for the
cases of one particle, leaching of one particle and leaching of particle distributions. A complete agreement with that simulations
was used to test our computational code. Again, we remark that
our approach generates a simple computational code with time
efficiency because analytical solutions are available and allows
to have a good control of the numerical error. No additional
iterations are needed to solve differential Eqs. (3)(6) which, in
fact, need to be within two sweeping loops which is suitable for
computational purposes. We now present, in Figs. 1 and 2, and
just for the sake of completeness, an abstract result presented
in Dixon and Hendrix (1993a), Figs. 3 and 4, with the design
parameters w = 1, p = 1, = 1, = 1.

With obtain s through

s (x, ) = exp

4. Numerical experiments

With obtain p through

p (x, ) = exp

Compute and store

E() =

is a reference radius, and making the scaling

where R
p = 2 p ,

and

<z
Fig. 1. Behaviour of i against days.

M.E. Mellado, L.A. Cisternas / Computers and Chemical Engineering 32 (2008) 23952402

2401

0 := 0.03, p := 0.000157, grade of solid reactant within particle Cp := 0.000157, particle radius r := 2.5, stoichiometric
number bi := 1.0, effective pore diffusivity of reagent DAe :=
106 , reference reagent concentration CA0 := 0.00333, initial
extractable grade of solid reactant CE0 := 0.000157, bulk solution volume fraction b := 0.03, heap void fraction h := 0.03,
superficial bulk flow velocity us := 0.000333, heap depth Z :=
1000.0.
Figs. 3 and 4 show a qualitative agreement with the standard
copper heap leaching process which validates, in some way, our
approach and allows to conclude this simple modification of
the numerical algorithm for solving (1)(6) can produce good
results at a low computational effort.
5. Conclusions
Fig. 2. Behaviour of E against days.

Fig. 3. Behaviour of i against days.

We now present a simulation, using our numerical scheme,

under similar conditions to standard copper heap leaching process in the north of Chile. We present numerical results for
the following situation: ore density 0 := 1.3, ore porosity

An analyticalnumerical approach method for solving the

heap leaching problem has been developed. The mathematical
theory is consistent and shows the possibility of improvement
the model by including, for instance, a second order term in (5)
in order to get a continuous solution. Also, this methodology
can be applied to obtain totally analytical models by considering the analytical solutions presented together with analytical
solutions for Eqs. (3) and (4), for instance, by some reasonable
simplifications of the differential equations. A qualitative agreement with industry processes validates our method from the
engineering point of view. Further research may be developed
in what concerning the mathematical aspects of the proposed
method, for instance, convergence of the algorithm, order of
convergence, finite volume methods for the differential equations, modification of (5). Also, this numerical approach can
be used in others models. Our modification of the numerical
solving for this model allows to obtain accurate solutions in
an efficient manner from a computational point of view. Moreover, the fact to use analytical solutions reveals several facts in
what leaching process concerns. In fact, there are two kinetics
involved in the process which can be used to develop totally
analytical models. It is possible to use discontinuous solutions
with continuous and good results. The fact that there is an equation which is discontinuous reveals the fact that, in particular,
this model could be corrected. The obtention of analytical solutions would allow to obtain hybrid models suitable for heap
leaching planning and design using techniques as mathematical
programming.
Acknowledgment
Luis A. Cisternas wishes to thank CONICYT for financial
support, through Fondecyt Project 1060342.
References

Fig. 4. Behaviour of E against days.

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2402

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