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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 Ingenier a Qu mica, Universidad de Antofagasta, Centro de Investigaci on Cient co Tecnol ogico para la Miner a (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 efcient 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 ner 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 ow in a porous media representing the leaching process we refer to Cariaga, Concha, and Sep ulveda (2005). With respect a two-dimensional partial differential equations model in bioleaching we can cite the work of Casas, Mart nez, Moreno, and Vargas (1998). In Cross, Bennett,

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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) supercial bulk ow 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 bulk solution volume fraction b heap void fraction h ore porosity 0 dimensionless ow 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

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 Sarra (2005), unsaturated ow 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 nite difference method giving the distribution of the degree of saturation in the particles and in the bed and the vertical velocity of ow in the bed, as well as the effect of periodic inltration 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 owing-reaction-deformation behaviour with mass transfer in heap-leaching are developed. The model equations are solved using an explicit nite 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 signicant 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 efcient 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 dene the following parameters: s = =
s R 3k s C s , bi DAe 0 bi CA0

p = ,

0 (1 =

p 2 0 )kp Cp R

bi DAe
b 0 (1 h )

0 (1

0 )CE0

and

Croft, McBride, and Gebhardt (2006), a framework was developed for multi-phase ows, 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

3(1 h )DAe Z , us R 2

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

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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 supercial bulk ow 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 together with the initial condition: 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 together with the initial condition: s (0) = 1, 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 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 , (3) (2) (1)

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 ow 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 together with the initial condition: i (x, 0) = 0 and the boundary conditions: i (1, t ) = b , We note that us t . = bZ 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 = z x (5)
(x=1)

(4)

i (0, t ) = 0. x

together with the initial condition: ib (z, 0) = 0 and the boundary condition: ib (0, ) = 0. The balance equation for a strictly aqueous phase reagent in the bulk lixiviant is expressed by means of b b = z x (6)
(x=1)

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

ib (1, t ) dt.

(7)

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Unlike conversion, extraction may be evaluated directly from chemical analysis of the heap efuent 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 rst order (5) and (6) and two equations of second order (3) and (4). We rst concentrate our attention in (1) and (2). Certainly, at a rst 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 rst 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 nd that, and considering reaction order for both equations as equal to the unity: p (x, ) = exp and s (x, ) = exp s 3 . (9) p 3(1 ) (8)

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):
1p v = p 1s and v = s ,

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 nite difference method (Hackbusch, 1992), the nite element method (Brenner & Scott, 1994; Ciarlet, 1978; Hackbusch, 1992; Zienkiewicz & Taylor, 2000), nite 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 nite element method or nite differences is equivalent. Also, as the nite differences are easier to handle as compared with nite elements, we solve these equations with a CrankNicholson fully implicit nite 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 uid elements, nite 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 nd that ib i = 2 x

(x=1)

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 nite number of terms in an innite 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, nite differences. Moreover, it is easier to deal with a numerical method than sum truncation in what concerns error studies of the proposed methodology.

Now, by using the initial and boundary value conditions, we have ib (z, ) = , and ib (z, ) = z, where i = 2 x > z, (11) <z (10)

(x=1)

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By using the same arguments, we nd the analytical solution for (6), this is b (z, ) = , and b (z, ) = 1 z, where = 2 x
(x=1)

3.1. Heap leaching with homogeneous particles sizes Now, we present the algorithm by considering heap leaching with homogeneous particle sizes. The algorithm reads 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 With obtain p through p (x, ) = exp p 3(1 ) .

<z

(12)

> z,

(13)

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 modied 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 modication which allows to deal with distribution of particles just by taking under consideration the corresponding scaling for p , and by means of dening 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.

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 uxes for and i . Compute ib and b through ib (z, ) = and ib (x, t ) = Also b (z, ) = and b (x, t ) = 1 2 x z, > z. 2 x , <z i 2 x z, > z. i 2 x , <z

(x=1)

(x=1)

(x=1)

(x=1)

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.

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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 dene a dimensionless particle radius as = R , R = 2 , w = 2 w

and b (z, ) = 1 2
1 0

(x=1)

m m3 d z,

> z.

Compute and store E( ) =

0

is a reference radius, and making the scaling where R p = 2 p ,

ib (1, t ) dt.

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 With obtain p through p (x, ) = exp p 3(1 ) .

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 nally 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 nished, the extraction (7) must be stored for further study. 4. Numerical experiments 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 efciency 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 s 3 .

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 Compute the corresponding uxes for and i . Compute ib and b through ib (z, ) = and ib (z, ) = Also b (z, ) = 2
1 0

1 0

i x

(x=1)

m m3 d ,

<z

1 0

i x

(x=1)

m m3 d z,

> z.

(x=1)

m m3 d ,

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

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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, supercial bulk ow 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 modication 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 simplications 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, nite volume methods for the differential equations, modication of (5). Also, this numerical approach can be used in others models. Our modication of the numerical solving for this model allows to obtain accurate solutions in an efcient 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 nancial support, through Fondecyt Project 1060342. References
de Andrade Lima, L. R. P. (2004). A mathematical model for isothermal heap and column leaching. Brazilian Journal of Chemical Engineering, 21, 435 447. Bouffard, S. C., & Dixon, D. G. (2001). Investigative study into the hydrodynamics of heap leaching processes. Metallurgical and Material Transactions B, 32B, 763776.

Fig. 4. Behaviour of E against days.

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