Chapter 2.

Population Balance Model Theory

This chapter presents an overview of the theory and the governing equations for the
methods used in FLUENT to predict particle growth and nucleation.
Section 2.1: The Particle State Vector
Section 2.2: The Population Balance Equation (PBE)
Section 2.3: Solution Methods
Section 2.4: Reconstructing the Particle Size Distribution from Moments
2.1 The Particle State Vector
The particle state vector is characterized by a set of external coordinates (x), which
denote the spatial position of the particle, and internal coordinates (), which could
include particle size, composition, and temperature. From these coordinates, a number
density function n(x, , t) can be postulated where

, x
x
. Therefore, the
average number of particles in the innitesimal volume dV
x
dV

is n(x, , t)dV
x
dV

. In
contrast, the continuous phase state vector is given by

Y [Y
1
(x, t), Y
2
(x, t), . . . , Y
c
(x, t)]
The total number of particles in the entire system is then

x
n dV
x
dV

(2.1-1)
The local average number density in physical space (i.e., the total number of particles
per unit volume) is given by
N(x, t) =

n dV

(2.1-2)
The total volume fraction of all particles is given by
(x, t) =

n V ()dV

(2.1-3)
where V () is the volume of a particle in state .
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Population Balance Model Theory
2.2 The Population Balance Equation (PBE)
Assuming that is the particle volume, the transport equation for the number density
function is given as

t
[n(V, t)] + [un(V, t)] +
v
[G
v
n(V, t)]
. .. .
Growth term
=
1
2

V
0
a(V V

, V

)n(V V

, t)n(V

, t)dV

. .. .
Birth due to Aggregation

0
a(V, V

)n(V, t)n(V

, t)dV

. .. .
Death due to Aggregation
+

v
g(V

)(V | V

)n(V

, t)dV

. .. .
Birth due to Breakage
g(V )n(V, t)
. .. .
Death due to Breakage
(2.2-1)
The boundary and initial conditions are given by
n(V, t = 0) = n
v
; n(V = 0, t)G
v
= n
0
(2.2-2)
where n
0
is the nucleation rate in particles/m
3
-s.
2.2.1 Particle Growth and Dissolution
The growth rate based on particle volume, G
v
, (m
3
/s) is dened as
G
v
=
V
t
(2.2-3)
The growth rate based on particle diameter (or length) is dened as
G =
L
t
(2.2-4)
The volume of a single particle V is dened as K
v
L
3
, and therefore the relationship
between G
v
and G is
G
v
= 3K
v
L
2
G (2.2-5)
The surface area of a single particle, A, is dened as K
a
L
2
. Thus for a cube or a sphere,
K
a
= 6K
v
.
i
Dissolution of particles can be represented as negative growth.
2-2 c Fluent Inc. July 19, 2006
2.2 The Population Balance Equation (PBE)
2.2.2 Particle Birth and Death Due to Breakage and Aggregation
The birth and death of particles occur due to breakage and aggregation processes. Exam-
ples of breakage processes include crystal fracture in crystallizers and bubble breakage
due to liquid turbulence in a bubble column. Similarly, aggregation can occur due to
particle agglomeration in crystallizers and bubble coalescence in bubble column reactors.
Breakage
The breakage rate expression, or kernel [7], is expressed as
g(V

)(V | V

)
where
g(V

) = breakage frequency; i.e., the fraction of particles of volume V

breaking
per unit time (m
3
s
1
)
(V | V

) = probability density function (PDF) of particles breaking from volume

V

to a particle of volume V
The birth rate of particles of volume V due to breakage is given by
B
br
=

v
g(V

)(V | V

)n(V

)dV

(2.2-6)
where g(V

)n(V

)dV

particles of volume V

break per unit time, producing g(V

)n(V

)dV

particles, of which a fraction (V | V

)dV represents particles of volume V . is the num-

ber of child particles produced per parent (e.g., two particles for binary breakage).
The death rate of particles of volume V due to breakage is given by
D
br
= g(V )n(V ) (2.2-7)
The PDF (V | V

) is also known as the particle fragmentation distribution function,

or daughter size distribution. Several functional forms of the fragmentation distribution
function have been proposed, though the following physical constraints must be met:
the masses of the fragments must sum to the original particle mass, and the number of
fragments formed has to be correctly represented.
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Population Balance Model Theory
Mathematically, these constraints can be written as follows:
For conservation of mass

V

0
(V | V

)dV = 1 (2.2-8)
For binary breakage, is symmetric about V/V

= 0.5; i.e.,
(V

V | V

) = (V | V

) (2.2-9)
Aggregation
The aggregation kernel [7] is expressed as
a(V, V

)
The aggregation kernel has units of m
3
/s, and is sometimes dened as a product of two
quantities:
the frequency of collisions between particles of volume V and particles of volume
V

the eciency of aggregation (i.e., the probability of particles of volume V coa-

lescing with particles of volume V

).
The birth rate of particles of volume V due to aggregation is given by
B
ag
=
1
2

V
0
a(V V

, V

)n(V V

)n(V

)dV

(2.2-10)
where particles of volume V V

aggregate with particles of volume V

to form particles
of volume V . The factor 1/2 is included to avoid accounting for each collision event
twice.
The death rate of particles of volume V due to aggregation is given by
D
ag
=

0
a(V, V

)n(V )n(V

)dV

(2.2-11)
i
The breakage and aggregation kernels depend on the nature of the physical
application. For example, in gas-liquid dispersion, the kernels are functions
of the local liquid-phase turbulent dissipation.
2-4 c Fluent Inc. July 19, 2006
2.3 Solution Methods
2.2.3 Particle Birth by Nucleation
Depending on the application, spontaneous nucleation of particles can occur due to the
transfer of molecules from the primary phase. For example, in crystallization from so-
lution, the rst step is the phase separation or birth of new crystals. In boiling ap-
plications, the creation of the rst vapor bubbles is a nucleation process referred to as
nucleate boiling.
The nucleation rate is dened through a boundary condition as shown in Equation 2.2-2.
2.3 Solution Methods
As discussed in Chapter 1: Introduction, the population balance equation can be solved
by three dierent methods in FLUENT: the discrete method, the standard method of
moments (SMM), and the quadrature method of moments (QMOM). For each method,
the FLUENT implementation is limited to a single internal coordinate corresponding
to particle size. The following subsections describe the theoretical background of each
method and list their advantages and disadvantages.
2.3.1 The Discrete Method
The discrete method (also known as the classes or sectional method) was developed by
Hounslow [5], Litster [6], and Ramkrishna [12]. It is based on representing the continuous
particle size distribution (PSD) in terms of a set of discrete size classes or bins, as
illustrated in Figure 2.3.1. The advantages of this method are its robust numerics and
that it gives the PSD directly. The disadvantages are that the bins must be dened a
priori and that a large number of classes may be required.
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Population Balance Model Theory
i+1 i
n(V)
V
Figure 2.3.1: A Particle Size Distribution as Represented by the Discrete
Method
Numerical Method
In FLUENT, the PBE is written in terms of volume fraction of particle size i:

t
(
s

i
) + (
s
u
i

i
) +

V

G
v

i
V

=
s
V
i
(B
ag,i
D
ag,i
+ B
br,i
D
br,i
) + 0
i

s
V
0
n
0
(2.3-1)
where
s
is the density of the secondary phase and
i
is the volume fraction of particle
size i, dened as

i
= N
i
V
i
i = 0, 1, , N 1 (2.3-2)
where
N
i
(t) =

V
i+1
V
i
n(V, t)dV (2.3-3)
and V
i
is the volume of the particle size i. In FLUENT, a fraction of , called f
i
, is
introduced as the solution variable. This fraction is dened as
f
i
=

i

(2.3-4)
where is the total volume fraction of the secondary phase.
2-6 c Fluent Inc. July 19, 2006
2.3 Solution Methods
The nucleation rate n
0
appears in the discretized equation for the volume fraction of the
smallest size V
0
. The notation 0
i
signies that this particular term, in this case
s
V
0
n
0
,
appears in Equation 2.3-1 only in the case of the smallest particle size.
The growth rate in Equation 2.3-1 is discretized as follows [5]:

G
v

i
V

=
s
V
i

G
v,i1
N
i1
V
i
V
i1

G
v,i
N
i
V
i+1
V
i

(2.3-5)
The volume coordinate is discretized as [5] V
i+1
/V
i
= 2
q
where q = 1, 2, . . . and is referred
to as the ratio factor.
The particle birth and death rates are dened as follows:
B
ag,i
=
N

k=1
N

j=1
a
kj
N
k
N
j
x
kj

kj
(2.3-6)
D
ag,i
=
N

j=1
a
ij
N
i
N
j
(2.3-7)
B
br,i
=
N

j=i+1

j
N
j
(V
i
| V
j
) (2.3-8)
D
br,i
=
i
N
i
(2.3-9)
where a
ij
= a(V
i
, V
j
) and

kj
=

1 for V
i
< V
ag
< V
i+1
, where i N 1
0 otherwise
(2.3-10)
V
ag
is the particle volume resulting from the aggregation of particles k and j, and is
dened as
V
ag
= [x
kj
V
i
+ (1 x
kj
)V
i+1
] (2.3-11)
where
x
kj
=
V
ag
V
i+1
V
i
V
i+1
(2.3-12)
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Population Balance Model Theory
If V
ag
is greater than or equal to the largest particle size V
N
, then the contribution to
class N 1 is
x
kj
=
V
ag
V
N
(2.3-13)
i
Note that there is no breakage for the smallest particle class.
2.3.2 The Standard Method of Moments (SMM)
The SMM, proposed by Randolph and Larson [13] is an alternative method for solving
the PBE. Its advantages are that it reduces the dimensionality of the problem and that
it is relatively simple to solve transport equations for lower-order moments. The disad-
vantages are that exact closure of the right-hand side is possible only in cases of constant
aggregation and size-independent growth, and that breakage modeling is not possible.
The closure constraint is overcome, however, through QMOM (see Section 2.3.3: The
Quadrature Method of Moments (QMOM)).
Numerical Method
The SMM approach is based on taking moments of the PBE with respect to the internal
coordinate (in this case, the particle size L).
Dening the kth moment as
m
k
(x, t) =

0
n(L; x, t)L
k
dL k = 0, 1, , N 1 (2.3-14)
and assuming constant particle growth, its transport equation can be written as

t
(m
k
) + (um
k
) = (B
ag,k
D
ag,k
+ B
br,k
D
br,k
) + 0
k
n
0
+ Growth (2.3-15)
where
B
ag,k
=
1
2

0
n()

0
a(u, )(u, )(u
3
+
3
)
k/3
n(u)dud (2.3-16)
D
ag,k
=

0
L
k
n(L)

0
a(L, )n()ddL (2.3-17)
B
br,k
=

0
L
k

0
g()(L | )n()ddL (2.3-18)
D
br,k
=

k
0
L
k
g(L)n(L)dL (2.3-19)
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2.3 Solution Methods
N is the specied number of moments and n
0
is the nucleation rate. The growth term is
dened as
Growth

0
kL
k1
G(L)n(L, t)dL (2.3-20)
and for constant growth is represented as
kGm
k1
(2.3-21)
Equation 2.3-16 can be derived by using
u
3
= L
3

3
; dL =
u
2
L
2
du
and reversing the order of integration. From these moments, the parameters describing
the gross properties of particle population can be derived as
N
total
= m
0
(2.3-22)
L
total
= m
1
(2.3-23)
A
total
= K
a
m
2
(2.3-24)
V
total
= K
v
m
3
(2.3-25)
d
32
=
m
3
m
2
(2.3-26)
These properties are related to the total number, length, area, and volume of solid
particles per unit volume of mixture suspension. The Sauter mean diameter, d
32
, is
usually used as the mean particle size.
To close Equation 2.3-15, the quantities represented in Equations 2.3-162.3-19 need to
be expressed in terms of the moments being solved. To do this, one approach is to assume
size-independent kernels for breakage and aggregation, in addition to other simplications
such as the Taylor series expansion of the term (u
3
+
3
)
k/3
. Alternatively, a prole of the
PSD could be assumed so that Equations 2.3-162.3-19 can be integrated and expressed
in terms of the moments being solved.
In FLUENT, an exact closure is implemented by restricting the application of the SMM
to cases with size-independent growth and a constant aggregation kernel.
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Population Balance Model Theory
2.3.3 The Quadrature Method of Moments (QMOM)
The quadrature method of moments (QMOM) was rst proposed by McGraw [9] for
modeling aerosol evolution and coagulation problems. Its applications by Marchisio et
al. [8] have shown that the method requires a relatively small number of scalar equations
to track the moments of population with small errors.
The QMOM provides an attractive alternative to the discrete method when aggregation
quantities, rather than an exact PSD, are desired. Its advantages are fewer variables
(typically only six or eight moments) and a dynamic calculation of the size bins. The
disadvantages are that the number of abscissas may not be adequate to describe the PSD
and that solving the Product-Dierence algorithm may be time consuming.
Numerical Method
The quadrature approximation is based on determining a sequence of polynomials or-
thogonal to n(L) (i.e., the particle size distribution). If the abscissas of the quadrature
approximation are the nodes of the polynomial of order N, then the quadrature approx-
imation

0
f(L)n(L)dL
N

i=1
f(L
i
)w
i
, (2.3-27)
is exact if f(L) is a polynomial of order N or smaller [2]. In all other cases, the closer
f(L) is to a polynomial, the more accurate the approximation.
A direct way to calculate the quadrature approximation is by means of its denition
through the moments:
m
k
=
N

i=1
w
i
L
k
i
. (2.3-28)
The quadrature approximation of order N is dened by its N weights w
i
and N abscissas
L
i
and can be calculated by its rst 2N moments m
0
, . . . , m
2N1
by writing the recursive
relationship for the polynomials in terms of the moments m
k
. Once this relationship is
written in matrix form, it is easy to show that the roots of the polynomials correspond
to the eigenvalues of the Jacobi matrix [11]. This procedure is known as the Product-
Dierence algorithm [3]. Once the weights and abscissas are known, the source terms
due to coalescence and breakage can be calculated and therefore the transport equations
for the moments can be solved.
2-10 c Fluent Inc. July 19, 2006
2.4 Reconstructing the Particle Size Distribution from Moments
Applying Equations 2.3-27 and 2.3-28, the birth and death terms in Equation 2.3-15 can
be rewritten as
B
ag,k
=
1
2
N

i=1
w
i
N

j=1
w
j
(L
3
i
+ L
3
j
)
k/3
a(L
i
, L
j
) (2.3-29)
D
ag,k
=
N

i=1
L
k
i
w
i
N

j=1
w
j
a(L
i
, L
j
) (2.3-30)
B
br,k
=
N

i=1
w
i

0
L
k
g(L
i
)(L | L
i
)dL (2.3-31)
D
br,k
=
N

i=1
w
i
L
k
i
g(L
i
) (2.3-32)
Theoretically, there is no limitation on the expression of breakage and aggregation kernels
when using QMOM.
The nucleation rate is dened in the same way as for the SMM. The growth rate for
QMOM is dened by Equation 2.3-20 and represented as
N

i=1
w
i
L
k1
i
G(L
i
) (2.3-33)
to allow for a size-dependent growth rate.
2.4 Reconstructing the Particle Size Distribution from Moments
Given a set of moments, the most likely PSD can be obtained based on the statistically
most probable distribution for turbulent ames [10], which was adapted for crystalliza-
tion problems by Baldyga and Orciuch [1].
The number density function n(L) is expressed as
n(L) = exp

N1

i=0
A
i
L
i

(2.4-1)
The equation for the kth moment is now written as
m
k
=

0
L
k
exp

N1

i=0
A
i
L
i

dL k = 0, 1, , N 1 (2.4-2)
Given N moments, the coecients A
i
can be found by a globally convergent Newton-
Raphson method to reconstruct the particle size distribution (e.g., Figure 2.4.1).
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Population Balance Model Theory
0 0.0005 0.001 0.0015
Length(m)
0
2e+13
4e+13
6e+13
8e+13
N
u
m
b
e
r

D
e
n
s
i
t
y

(
#
/
m
3

m
)
Original PSD
Reconstructed PSD
Figure 2.4.1: Reconstruction of a Particle Size Distribution
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