Computers and Mathematics with Applications 65 (2013) 1698–1718

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Computers and Mathematics with Applications

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Dynamics of fines/bacterial cells accumulation in trickle-bed

reactors/bioreactors—Multiscale modeling framework
Ion Iliuta, Faical Larachi ∗
Department of Chemical Engineering, Laval University, Québec, G1V 0A6, Canada

article info abstract

Keywords: Modeling the dynamics of fines/bacterial cells accumulation in gas–liquid–solid reactors/
Trickle-bed (bio)reactors
bioreactors is a difficult task which demands an improved understanding and quantifi-
Plugging
cation of the complex fluid dynamics, surface physical and microbiological phenomena
Biological clogging
Mathematical modeling coupled with (bio)chemistry and thermodynamic backgrounds. This contribution is of-
fered as a step in that direction and presents two case studies with reference to modeling
the complex physical and biological plugging/clogging phenomena in trickle-bed reactors/
bioreactors, induced, respectively, by the retention of fine particles and by the formation
of an excessive amount of biomass. The complex gas–liquid flow and space–time evolu-
tion of fines/bacterial cells capture, aggregation, detachment and migration in trickle-bed
reactors/bioreactors were analyzed after a mathematical description was cast in terms of
Euler–Euler two-fluid dynamic models based on the volume-average mass and momentum
equations developed for multiphase systems coupled with species balance equations, solid
deposit/biomass dynamics equations, filtration equations for the fines/bacterial cells and
the aggregates, population balance equations for the fines/bacterial cells agglomeration.
© 2013 Elsevier Ltd. All rights reserved.

1. Introduction

A major drawback limiting the use of co-current gas–liquid downflow packed bed reactors/bioreactors (trickle-bed
reactors/bioreactors) is ascribed to the complex physical/biological clogging phenomena induced, respectively, by the
retention of inert suspended fine particles advected in the liquid influent stream and by the formation of an excessive
amount of biomass which narrow the free interstitial space left to fluid flows. When heavy gas oil suspensions containing
a low concentration of non-filterable fine solid impurities are treated in trickle-bed hydrotreaters clogging develops and
leads to their bed progressive obstruction that is accompanied with a build-up in pressure drop [1–3]. Although the fines
concentration is in the 100-range parts per million, the cumulative effect of several months of refining operation diverts
the catalyst bed from its catalytic function to that of a huge filter where fines accumulation causes the pressure to rise by
restricting the flow. In these conditions the unit must often be shutdown to unload the physically-deactivated catalyst
for replacement with a pristine one. Furthermore, fines attachment can provoke a possible unfavorable impact on the
trickle-bed hydrotreating performance as a result of inter-particle diffusional limitations by the fines deposits. Similarly,
the excessive biomass accumulation in gas–liquid downflow packed bed bioreactors induces biological clogging and leads
to the progressive obstruction of the bed that is accompanied with a rise in two-phase pressure drop and flow channeling
[4–8]. To prevent this problem, it is important to conserve a very thin and active biofilm rather than a thick and less effective
biological fixed film. For maintaining acceptable operating cycles, the units require periodic backwashing and/or shutdowns
for removing excess biomass that has progressively built up across the porous layer.

∗ Corresponding author. Tel.: +1 418 656 3566; fax: +1 418 656 5993.
E-mail addresses: ion.iliuta@gch.ulaval.ca (I. Iliuta), faical.larachi@gch.ulaval.ca (F. Larachi).

0898-1221/$ – see front matter © 2013 Elsevier Ltd. All rights reserved.
doi:10.1016/j.camwa.2013.01.010
 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718 1699

Notation
a effective specific surface area, m2 /m3(bio)p
2  √  √
dp (t )
 
d d
A∆ collector area loss, A∆ = 1
2 2
2 3 d (f t ) − sin 2 3 d (f t )
p p
, m2
ca,k concentration of κ -size fines (cells) aggregate, m /mℓ (kg/mℓ )
3 3 3

cc concentration of cells in liquid phase, kg/m3ℓ

cf fine particles concentration, m3 /m3ℓ
Cj,α concentration of species j in α -phase, kmol/m3
Cj,d concentration of component j in the biofilm when the external surface area of the biocatalyst particle is
completely dry, kg/m3
Cj,w concentration of component j in the biofilm when the external surface area of the biocatalyst particle is
completely wetted, kg/m3
db bioparticle diameter, m
dc bacterial cell diameter, m
df primary fine particle diameter, m
dp particle diameter, m
σ

dp (t ) effective particle diameter at time t , dp (t ) = dop 3 1 + (1−ε )( o , m
d 1−ε )

Dα axial dispersion coefficient in the α -phase, m2 /s

Df fractal dimension
eff
Dj effective diffusivity of component j, m2 /s
2k T
DBM Brownian diffusion coefficient, DBM = 6πµB d
ℓ f
E1 , E2 Ergun constants
Fg ℓ gas–liquid drag force, N/m3
Fgs gas–solid drag force, N/m3
Fℓs liquid–solid drag force, N/m3
g gravity acceleration, m/s2
Gm mean velocity gradient in the liquid phase, s−1
H bed height, m
Ha Hamaker constant, J
Hej Henry constant, m3ℓ /m3g
k particle size class indices, -
kdf specific decay rates for free cells, s−1
kds specific decay rates for captured cells, s−1
kgs gas–solid mass transfer coefficient, m/s
kℓ ag ℓ volumetric liquid-side mass transfer coefficient, s−1
kℓs liquid–solid mass transfer coefficient, m/s
kB Boltzmann’s constant, J/K
kF coefficient of sliding friction, m
Ki inhibition constant, kg/m3
Ks saturation constant of phenol, kg/m3
Kox saturation constant of oxygen, kg/m3
n1 number density of primary bacterial cells
nk number density of κ -size aggregate
Nc number of collectors in grid cell volume v, Nc = 6vo (1 − ε o )
π (dp )
3

6v
Nf number of trapped fines in grid cell volume v, Nf = (ε o − ε) (1 − εd )
π d3f
2
d (t )

∂ Nf number of peripheral fines per collector, ∂ Nf = 4β(1 − εd ) pd
f
P pressure, Pa
Pα pressure of α -fluid, Pa
r radial position within solid particle, m
rdep fines (cells) deposition rate, m3p /m3 s (kg/m3 s)
rdf decay rate for free cells, kgcells /m3 s
rds decay rate for captured cells, kgcells /m3 s
rgf growth rate for free cells, kgcells /m3 s
1700 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718

rgs growth rate for captured cells, kgcells /m3 s

rp radius of catalyst particle, m
rdet fines (cells) detachment rate, m3p /m3 s (kg/m3 s)
R ideal-gas constant
t time, s
T temperature, K
uα average interstitial velocity of α -phase, m/s
ug , i gas interfacial velocity in the bed, m/s
vc volume of a cell, m3
vsα superficial velocity of α -phase, m/s
YX /O2 yield coefficient, kg biomass/kg oxygen
YX /S yield coefficient, kg biomass/kg phenol
z axial coordinate, m

Greek Letters
α fractional collision efficiency
αdet
c
colloidal first-order release or detachment rate coefficient, αrel
c
= DBM /δbl2 , s−1
αdet
h
hydrodynamic release or detachment rate coefficient, kg/N s
βij collision frequency function
ε bed porosity
εd porosity of solid deposit
εp catalyst particle porosity
εα α -phase holdup
δ separation distance between the fine particle (bacterial cell) and the collector plane, δ = 4 × 10−10
δb biofilm thickness, m
1/3
δbl thickness of the boundary layer around a single spherical (bio)particle δbl = 0.5dp 2DBM /uℓ dp

γa,k fraction of the collector surface area not available for detachment of κ -size aggregate, γa,k = τcr ,a,k /τw
γa,k−1 fraction of the collector surface area not available for detachment of the (κ − 1)-size aggregate, γa,k−1 =
τcr ,a,k−1 /τw
ηo single-collector efficiency
ηg effectiveness factor for a completely dry particle
ηe external wetting efficiency
ηℓ effectiveness factor for a fully wetted particle
ηG overall effectiveness factor
λ filter coefficient, m−1
µα α -phase dynamic viscosity, kg/ms
µeα α -phase effective viscosity (combination of bulk and shear terms), kg/m s
ρα density of α -phase, kg/m3
ρb total dry biomass in the biofilm, kg/m3
ρc dry cell mass/cell volume, kg/m3
ρp catalyst particle density, kg/m3
σ volume of captures fines/cells and aggregates in unit volume of reactor, σ = k−2 σa,k + σf ,c
max

σa,k volume of κ -size aggregate in unit volume of reactor, m3 /m3r

σc ,f volume of captured cells/fines in unit volume of reactor, m3c ,f /m3r
σℓ surface tension, N/m
τ shear stress, N/m2
τw shear stress on the collector plan, N/m2
ξ surface-area parameter
ψg ℓ gas–liquid interaction factor

Subscripts
a, k κ -size aggregate
b biofilm
c bacterial cell
d solid deposit
f fine particle
g gas phase
 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718 1701

ℓ liquid phase
in reactor inlet
p catalyst particle
S phenol

Superscripts
in reactor inlet
o clean bed state
∗ on bioparticle surface

Numerous investigators in the past have attempted to model the transient behavior of the fines/cells attachment process,
at the macroscopic and microscopic levels, in the case of single-phase (liquid) flow through porous packed beds [9]. The
macroscopic studies are aimed at the phenomenological description of the attachment process, the prediction of its dynamic
behavior, and the development of a methodology and techniques for design, calculation, and optimization. Microscopic
approaches, known as trajectory theories, are planned to provide information and insight about the mechanisms of particle
attachment, the conditions under which the attachment may be facilitated, and the effect of attachment on the structure of
the packed bed. The phenomenological theory of fines/cells attachment has two limitations: the lack of generality and the
failure to give a fundamental understanding of this mechanism. On the contrary, a trajectory theory explores the attachment
of each particle on the collector as suspension flows through the collector. Even if current trajectory analysis models differ
by their geometrical representation of the granular media and inclusion of surface forces there is a little difference in the
accuracy between them [9]. However, trajectory analysis applies only to the initial stage of the particle attachment process.
To model the attachment process in its entirety, the effect of deposited particles on collector efficiency must be calculated
because the surface interactions between the collecting body and particles to be attached become more complicated. In
the presence of favorable surface interactions the attachment rate increases in time because deposited particles act as
additional attachment sites. If particle–particle interactions are unfavorable the attachment rates may be a fraction of that
under favorable surface interactions, even if all other conditions are the same [9].
In contrast, the literature still remains short about modeling the dynamics of fines/bacterial cells accumulation in
gas–liquid–solid reactors/bioreactors used in petroleum refining industry and in wastewater treatment. The modeling
of physical/biological clogging in gas–liquid–solid reactors/bioreactors necessitates an improved understanding and
quantification of the complex fluid dynamics, surface physical and microbiological phenomena coupled with (bio)chemistry
phenomena and thermodynamics. This contribution is offered as a step in that direction and it is a continuation of our
endeavor [3,10–19] in developing mathematical models for the description of gas–liquid flow and space–time evolution
of clogging in gas–liquid–solid reactors/bioreactors. Two case studies with reference to modeling the complex physical
and biological clogging phenomena in trickle-bed reactors and bioreactors are presented. Two-phase flow and space–time
evolution of clogging in trickle-bed reactors/bioreactors was described via Euler–Euler two-fluid dynamic models based on
the volume-average form of the transport equations developed for multiphase systems coupled with the population balance
equations for the particles agglomeration. Mono-layer and multilayer attachment via deep-bed filtration mechanism was
considered for Brownian fines/bacterial cells and only mono-layer attachment in the case of the detaching aggregates. The
detachment of the fines/bacterial cells or aggregates from the collector surface was assumed to be induced by the colloidal
forces in the case of Brownian fines/cells/aggregates or by the hydrodynamic forces in the case of non-Brownian aggregates.
The generation of the fines/bacterial cell aggregates was considered to take place by collision and subsequent bonding of the
fines/cells transported from the bulk liquid to the surface of the catalyst particle/bioparticle in the liquid approaching the
catalyst particle/bioparticle and by the collision with the associated growth cells. The complex coupling between the liquid
suspension and solids was monitored via the fines/bacterial cells and aggregates filtration rate equations, the fines/bacterial
cells and aggregates detachment rate equations and the interaction drag or momentum exchange force terms. Phenol
biodegradation by Pseudomonas putida as the predominant species immobilized on activated carbon is chosen as a case
study to illustrate the consequences of formation of excessive amounts of biomass in trickle-bed bioreactors.

2. Dynamics of fines accumulation in trickle beds

A co-current downward two-phase trickle flow through a porous fixed bed of uniform initial porosity and single-
sized catalytic particles is considered. Two-phase flow is annular and completely separated and the catalyst particles sur-
face is partially wetted by the liquid film. Two-phase flow is assumed unidirectional and both the flowing phases are
assumed as viscous Newtonian. The liquid is incompressible and the gas phase is ideal. The gas/liquid/Brownian parti-
cles/aggregates/porous medium multiphase system is viewed as a system of three interpenetrated continua: (i) a flowing
gas phase; (ii) a dilute pseudo-homogeneous suspension phase containing the liquid, the seeding single-sized fines (Brownian
particles) and the detached aggregates; (iii) and a stationary pseudo-continuous solid phase made up of the catalyst (collec-
tor) particles and the Brownian particles and the aggregates that get captured/generated onto their surface. The properties of
1702 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718

the pseudo-homogeneous suspension (density, viscosity, holdup) are equal to those of the embracing liquid (influent fines
volume fraction <0.1h). Only the inlet liquid is considered as a source for fine particles without considering fines generated
in the catalyst bed (due to attrition, byproduct build up, etc.). Fines and aggregates attachment occurs via a deep-bed filtra-
tion mechanism [20]. Only the attachment under favorable conditions of surface interactions is considered, i.e., the double
layer force is attractive. The gas–liquid interface is impervious to the Brownian particles and aggregates and the net sink in
the fluid momentum balance due to the mass transfer of Brownian particles and detached aggregates from the fluid to the
collector is negligibly small. The generation of the aggregates is considered to take place by collision and subsequent bond-
ing of primary Brownian particles transported from the bulk liquid to the surface of the collector in the liquid approaching
the collector, i.e., transport to the grain surface is quantified by the collection efficiency. The fine–fine attractive interactions
within the pseudo-homogeneous suspension phase are assumed absent or at least small enough to preclude aggregation.
The fracture of the agglomerates by the disruptive stresses created by the liquid and gas motion is neglected. The release of
colloidal fines or aggregates (df < 2 µm) from the catalyst particle surface is controlled by the colloidal forces, i.e., Brow-
nian diffusion through the hydrodynamic boundary layer in the absence of energy barrier [21,22] and the detachment of
non-Brownian aggregates (df > 2 µm) is induced by hydrodynamic forces [22].
Two-phase flow and space–time evolution of clogging in trickle-bed reactors is described via an Euler–Euler two-fluid
dynamic model based on the volume-average form of the transport equations developed for multiphase systems [23,24]
coupled with the population balance equations for the particles agglomeration [25]. The general model equations consist
of the conservation of volume, the continuity and the Navier–Stokes equations for the gas and the pseudo-homogeneous
suspension phases, the continuity equation for the solid stationary phase and the species balance equation for the Brownian
particles and detached aggregates undergoing migration from the pseudo-homogeneous suspension phase to the solid
phase, filtration equations for the Brownian particles and the aggregates, solid deposit dynamics equation:
Conservation of volume
εg + εℓ = ε. (1)
Continuity equations for the gas, the pseudo-homogeneous suspension and the solid phases
∂ ∂ 
εg ρ g + εg ρg ug = 0
  
(2)
∂t ∂z
∂ ∂ dσ
(εℓ ρℓ ) + (εℓ ρℓ uℓ ) = −ρf (3)
∂t ∂z dt
∂ dσ
(1 − ε )ρp + (1 − εd )(ε − ε)ρf = ρf
o o
.
 
(4)
∂t dt
Species balance equation for the Brownian fines

∂  ∂  ∂2 
εℓ cf + uℓ εℓ cf = Dℓ 2 εℓ cf − rdep,f + rrel
c
,f .
  
(5)
∂t ∂z ∂z
Species balance equation for the κ -size aggregate

∂  ∂  ∂2 
εℓ ca,k + uℓ εℓ ca,k = Dℓ 2 εℓ ca,k − rdep,a,k γa,k + rrel
c
,a,k + rrel,a,k (1 − γa,k ).
h
  
(6)
∂t ∂z ∂z
Momentum balance equations for the gas and continuous pseudo-homogeneous suspension phases

∂  ∂  ∂ 2 ug ∂P
ρg εg ug + ug ρg εg ug = εg µeg 2 − εg + εg ρg g − Fg ℓ − Fgs
 
(7)
∂t ∂z ∂z ∂z
∂ ∂ ∂ 2 uℓ ∂P εηe − εℓ 
(ρℓ εℓ uℓ ) + uℓ (ρℓ εℓ uℓ ) = εℓ µeℓ 2 − εℓ + εℓ ρℓ g + Fg ℓ + Fgs − Fℓs .

(8)
∂t ∂z ∂z ∂z εg
Filtration equation for the Brownian fines

dσf
max
 dnk
= Nf − vf k − rrel
c
(σf ). (9)
dt k=2
dt

Generation and filtration equation for the κ -size aggregate

dσa,k dnk
vf k + rdep,a,k γa,k − rrel
c
,a,k (σa,k ) − rrel,a,k 1 − γa,k .
h
 
= (10)
dt dt
Global filtration equation

dσ dσf dσa,k
max

= + . (11)
dt dt k=2
dt
 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718 1703

Note that in the formulation of the momentum balance equations, the capillary pressure between liquid and gas phases
is neglected. The fraction of the collector surface area not available for the κ -size aggregate particles detachment (γa,k )
corresponds to the regions where the shear stress acting on the collector is lower than the critical shear stress [16]. In the
case of Brownian aggregates the detachment by hydrodynamic mechanism is not possible as critical shear stress is very
high and all the particle surface area is not available for detachment (γa,k = 1); in the case of non-Brownian aggregates
the rate of colloidal aggregates reentrainment is negligible (rdet
c
,a,k = 0). The filtration rate for the κ -size aggregate, which
represents the volume of κ -size aggregate deposited per unit reactor volume and unit of time, is the algebraic sum of the
κ -size aggregate accumulation rate, the attachment rate and the colloidal and hydrodynamic reentrainment rates (Eq. (10)).
The filtration rate for Brownian particles is the algebraic sum of the attachment rate, the aggregates accumulation rate and
the colloidal reentrainment rate (Eq. (9)).
The solution of the dynamic multiphase flow model requires the knowledge of the particles attachment, aggregation and
detachment processes kinetics. The attachment rate determines the degree of collection of fines or detached aggregates. A
simple logarithmic law was used to express the dependence of attachment rate versus fines or the aggregates concentration
and superficial liquid velocity [9]:
rdep,i = λci vsℓ where i = f , i = a, k. (12)
In Eq. (12), λ is filter coefficient which can be thought of as the probability for a fine particle or a detached aggregate to be
captured as it travels a unit distance through the bed [9]. The form of the filter coefficient is dictated by the nature of the
capture phenomena in play, and by the amount of capture as bed clogging proceeds. Mono-layer and multilayer attachment
was considered for Brownian particles and only mono-layer attachment in the case of the detached aggregates. During the
fine-collector capture step, the fines or detached aggregates adhere individually as a mono-layer on the collector surface
via fine/aggregate-collector interaction forces: fluid drag, gravity, van der Waals surface-interactive forces, and Brownian
diffusion force [9]. For mono-layer attachment, Logan et al. [26] describe the attachment of suspended particles as a two-step
process: the transport to the grain surface quantified by the collection efficiency (η0 ) and the frequency at which particles
in the liquid phase come into contact with the collector quantified by the fractional collision efficiency (α):
3 ηo α
λ= (1 − ε o )1/3 . (13)
2 dp
Single-collector efficiency for mono-layer attachment was estimated with the correlation developed by Rajagopalan and
Tien [27], obtained by the combination of the trajectory analysis of a spherical particle in the vicinity of a spherical
collector with the contribution of Brownian diffusion. For fine–fine capture step, attachment becomes driven by the fine–fine
interaction forces yielding a multilayer deposit for which the filter coefficient no longer remains constant in time. The change
of the filter coefficient as a function of the specific deposit was estimated using the correlation developed by Tien et al. [28].
Extra information about trickle bed deep-bed filtration model is given in Iliuta et al. [3], Iliuta and Larachi [10,19].
The detachment or release of the fine particles/aggregates from the collector surface was assumed to be induced
by hydrodynamic forces in the case of non-Brownian particle/aggregates or by colloidal forces in the case of Brownian
particles/aggregates [16]. For non-Brownian aggregates, the rate of hydrodynamic particle reentrainment was considered
to be proportional to the difference between the wall shear stress and the critical shear stress [21]
 1
,a,k = αrel,a,k a(1 − ε)ηe τw − τcr ,a,k for τw > τcr ,a,k
h h

rrel (14)
ρf
h
rrel,a ,k = 0 for τw < τcr ,a,k (15)
where the critical shear stress was estimated for the condition of equilibrium between the forces acting on an attached
particle along the tangential direction [16]:
6(1−ε o ) Ha
kf dop 12δ 2
τcr ,a,k = . (16)
2.551π da,k
For colloidally induced release (Brownian particles/aggregates), in the absence of an energy barrier, the detachment rate is
based on the assumption that the rate-limiting step is the diffusion of detached colloids across the boundary layer between
collector surfaces and liquid bulk [29]:

,i = αrel,i a(1 − ε)ηe di σi

c c
rrel (17)
where α c
designates the Brownian fines detachment (i = f ) or the κ -size aggregate detachment (i = a, k).
rel,i
Particle aggregation was described by the rate at which a certain size aggregate is being formed by smaller aggregates
minus the rate at which the aggregate combines to form a larger aggregate (neglecting aggregate break-up). This is given be
the discrete population balance equations of von Smoluchowski [25]:
max
dnk 1  
= α βij ni nj − nk α βik ni k = 2, 3, . . . , max (18)
dt 2 i+j=k i =1
1704 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718

where α is the fractional collision efficiency, βij is the rate at which particles or aggregates of volume vi and vj collide, ni is
the number density of particles or aggregates with volume vi, i, j, k refer to particles or aggregate size class indices and max
refers to a maximum size class.
In Eq. (18), the first summation is over the sets of sizes that, when added, produce a κ -size aggregate and second sum-
mation reflects the loss of κ -size aggregates as they combine with all other aggregates sizes to form larger aggregates. The
collision between two particles, two aggregates or a particle and an aggregate results in a newly formed particle, depending
on the efficiency of the collision which is a complex function of the surface properties, the structure of the aggregates or
the diameter of the aggregates, hydrodynamic effects, and the prevailing colloidal forces [30]. The collision frequency func-
tion, βij , reflects the physical environment, such as temperature, viscosity, shear stress, and aggregation size. It is generally
accepted that there are three mechanisms which cause particle collision: Brownian motion or perikinetic aggregation, differ-
ential settling and liquid shear or orthokinetic aggregation. The collision frequency function due to Brownian motion is [31]:

2κB T
 
1 1
βij,BR = ri + rj .
 
+ (19)
3µℓ ri rj
Differential settling occurs when larger aggregates settle more rapidly then smaller aggregates and particles. The terminal
velocity of settling particles and aggregates is assumed to follow Stokes law. Considering differential settling rates and the
rectilinear collision model, the rate constant is described by [32]:

π g (ρa − ρℓ )  3
βij,DS = di + dj |di − dj |. (20)
72µℓ
For liquid shear-induced aggregation, the most widely accepted form of the collision frequency function is that based on
a purely rectilinear model which considers that the particle trajectories at some distance from the particle under observa-
tion continue along the same path and are not influenced be the flow field surrounding the observed particle. The collision
frequency function for the rectilinear model is given by [33]:

1 3
βij,SH = di + dj Gm . (21)
6
Because the aggregates comprised of solid particles can be treated using a fractal dimension [30], the radius ra,k of a size
class κ -aggregate can be expressed as [34]:
1
ra,k = r1 (k) Df (22)

where Df is the fractal dimension, which defines the relationship between particle size and density.
The assumption of bed partial wetting entrains that the gas-phase drag has contributions due to effects located at the
gas–liquid (Fg ℓ ) and gas–solid (Fgs ) interfaces. Similarly, the resultant of the forces exerted on the liquid phase involves
two components: (i) the drag force, Fℓs , experienced by the liquid due to the shear stress nearby the liquid–solid boundary,
(ii) and the gas–liquid interfacial drag due to the slip between fluids, Fg ℓ . Assuming trickle flow regime, the double slit model
provides satisfactory approximations for the liquid–solid, gas–solid and gas–liquid drag forces [35]. For the adaptation to
the trickle flow clogging context, these drag equations were recast as a function of local instantaneous values of porosity
and effective specific surface area:
 
a (1 − ε)2 µℓ ηe a(1 − ε)
2
E1 E2 
Fℓs = ηe 2
1 + ψg ℓ Cwi ρℓ |vsℓ | vsℓ εℓ

Cw + (23)
36 εℓ3 6 εℓ3
 
a (1 − ε)2 µg a(1 − ε)
2
E1 E2
Fgs = (1 − ηe ) ρg vsg  vsg ε
2
 
Cw + Cw i (24)
36 ε3 6 ε3
 
1 2 a (1 − ε) µg  a(1 − ε)ρg
vsg − ε − εℓ ug ,i 
2 2

E    
E2 
Fg ℓ = ηe Cwi 1 + ψg ℓ 
 
Cw  2 +
ηe
2
36 ε 6
ε − ηεℓe εg
 
ε − ηℓe εg

 
εℓ
   
× vsg − ε − ug , i ε g . (25)
ηe
The effective surface area is expressed as the summation of surface area of the porous medium and surface area of the
Brownian particles where we considered the specific solid deposit being formed only by Brownian particles [36]:

Nc ξ π d2p (t ) + Nc ∂ Nf ξ π d2f − A∆ (t )
 
a= . (26)
Nc π6 d0p + Nf π6 d3f
 3
 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718 1705

With the evolution of attachment, the solid–liquid surface area gets altered by two opposing phenomena [37]: an increase
in surface area through addition of area of the captured fines, and a loss of area A∆ due to the shadow effect [38]. The latter
effect refers to an exclusion collector area hidden nearby the fine once it gets captured forbidding thereafter access by future
approaching fines.

3. Dynamics of biomass accumulation in trickle-bed bioreactors

A downflow gas–liquid trickle flow through a porous medium of uniform initial porosity and single-sized solid particles is
considered. Two-phase flow is assumed unidirectional and both the flowing phases are assumed as viscous Newtonian. The
liquid is incompressible and the gas phase is ideal. The gas/liquid/biofilm/porous medium multiphase system is viewed as
a system of three interpenetrated continua: (i) a flowing gas phase; (ii) a flowing liquid phase; (iii) and a stationary pseudo-
continuous solid phase made up of the packing particles (activated carbon) constituting the clean porous medium as well as
of the biomass (cells and aggregates) captured onto their surface. The bioparticle surface is assumed partially wetted by the
liquid film and two-phase flow is annular and completely separated. The biofilm thickness increases with the time during
transient state and consequently a moving boundary problem must be solved.
Phenol biodegradation by Pseudomonas putida as the predominant species immobilized on activated carbon is considered.
The bacterial cells seeded in the liquid phase are considered single-sized and the cell aggregates are formed by lumps
of the cells at the surface of bioparticle. Cells attachment occurs via deep-bed filtration mechanism. The generation of
cell aggregates was considered to take place by collision and subsequent bonding of the cells transported from the bulk
liquid to the surface of the bioparticle in the liquid approaching bioparticle and by collision with the associated single-sized
growth cells. The cell–cell attractive interactions within the bulk liquid phase are assumed absent or at least small enough to
preclude aggregation. Cells within the biofilm (including cells associated to aggregates growth process) were individualized
as in the case of individual-based modeling (IbM) theory to describe the cells agglomeration process [39]. The gas–liquid
interface is impervious to bacterial cells and aggregates; cells and aggregates migration to the gas–liquid interface caused by
cells/aggregates surface properties akin to froth flotation has been neglected. The detachment is induced by hydrodynamic
forces (non-Brownian bacterial cells/aggregates) or colloidal forces (Brownian bacterial cells/aggregates). Growth and death
of detached cell aggregates are not possible in this model.
Two-phase flow and space–time evolution of bioclogging in trickle-bed bioreactors was described via an Euler–Euler
two-fluid dynamic model based on the volume-average form of the transport equations developed for multiphase systems
[23,24] coupled with the population balance equations for the bacterial cells agglomeration [25]. The general model
equations consist of the conservation of volume, the continuity and the Navier–Stokes equations for the gas and liquid,
the continuity equation for the solid stationary phase, the unsteady state mass balance equations for planktonic cells and
detached aggregates undergoing migration from the liquid to the solid phase, species balance equations in the liquid and
gas phases, filtration equations for the bacterial cells and aggregates, biomass dynamics equation:
Conservation of volume

εℓ + εg = ε. (27)

Continuity equations for the gas, the liquid and the solid phases

∂  ∂ 
εg ρg + εg ρg ug = 0
 
(28)
∂t ∂z
∂ ∂ max
 max

(εℓ ρℓ ) + (εℓ ρℓ uℓ ) = −rdep,c + rrel
c c h
,a,k 1 − γa,k
 
,c + rrel,a ,k + rrel (29)
∂t ∂z k=2 k=2
 
∂  dσc  dσa,k
max
(1 − ε o )ρp + (ε o − ε)ρb = ρc .

+ (30)
∂t dt k=2
dt

Momentum balance equations for the gas and liquid phases

∂  ∂  ∂ 2 ug ∂P
ρg εg ug + ug ρg εg ug = εg µeg 2 − εg + εg ρg g − Fg ℓ − Fgs
 
(31)
∂t ∂z ∂z ∂z
∂ ∂ ∂ 2 uℓ ∂P εηe − εℓ 
(ρℓ εℓ uℓ ) + uℓ (ρℓ εℓ uℓ ) = εℓ µeℓ 2 − εℓ + εℓ ρ ℓ g + Fg ℓ + Fgs − Fℓs .

(32)
∂t ∂z ∂z ∂z εg
Unsteady-state mass balance equation for planktonic cells (cells freely suspended in aqueous phase)

∂ ∂ ∂2
(εℓ cc ) + uℓ (εℓ cc ) = Dℓ 2 (εℓ cc ) + rgf − rdf + rrel,c − rdep,c .
c
(33)
∂t ∂z ∂z
1706 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718

Unsteady state mass balance equation for κ -size aggregate in the liquid phase (without growth and death of detached cell
aggregates)

∂  ∂  ∂2 
εℓ ca,k + uℓ εℓ ca,k = Dℓ 2 εℓ ca,k + rrel
c
,a,k + rrel,a,k (1 − γa,k ) k = 2, . . . , max.
h
  
(34)
∂t ∂z ∂z
Growth, attachment and detachment equation for the bacterial cells

dσc
max
 dnk
ρc = rgs ηG − rds + rdep,c − vc kρc − rdet
c
,c (σc ). (35)
dt k=2
dt

Generation and filtration equation for the κ -size aggregate

dσa,k dnk
ρc vc kρc − rrel
c
,a,k (σa,k ) − rrel,a,k 1 − γa,k
h
k = 2, . . . , max.
 
= (36)
dt dt
Biomass dynamics equation

dσ dσc dσa,k
max

= + . (37)
dt dt k =2
dt

Species balance in the liquid phase (axial dispersion in the liquid phase)

∂  ∂  ∂2  rgf rgs ηG
CS ,ℓ εℓ + uℓ CS ,ℓ εℓ = Dℓ 2 CS ,ℓ εℓ −
  
− (38)
∂t ∂z ∂z YX /S YX /S

∂  ∂  ∂2  rgf rgs ηG
CO2 ,ℓ εℓ + uℓ CO2 ,ℓ εℓ = Dℓ 2 CO2 ,ℓ εℓ + kℓ ag ℓ O CO2 ,g /HeO2 − CO2 ,ℓ − .
      
− (39)
∂t ∂z ∂z 2 YX /O2 YX /O2
Species balance in the gas phase (no axial dispersion in the gas phase)
∂  ∂  ∂ CO2 ,b 

eff
CO2 ,g εg + ug CO2 ,g εg = − kℓ ag ℓ O CO2 ,g /HeO2 − CO2 ,ℓ − DO2 ,b a(1 − ε) (1 − ηe ) .
     
(40)
∂t ∂z 2 ∂ r r =rb
The overall effectiveness factor defined as a weighted sum of the effectiveness factors for completely dry particle (ηg ) and
fully wetted particle (ηℓ )
ηG = (1 − ηe ) ηg + ηe ηℓ (41)
was obtained solving the mass balance equations for the biofilm and the simultaneous diffusion and adsorption of both
phenol and oxygen within the activated carbon particles (under the assumptions given in Iliuta and Larachi [18]):
∂ Cj,b 1 ∂ ∂ C j ,b µρb
 
eff
εb = 2 r 2
D j ,b − j = O2 , S (42)
∂t r ∂r ∂r YX /j
∂ C S ,p ∂ qS ,p 1 ∂ eff ∂ CS ,p 3825.3CS ,p
 
εp + ρp = 2 r 2 DS ,p qs,p = (43)
∂t ∂t r ∂r ∂r 1 + 25.329cS ,p
∂ CO2 ,p 1 ∂ eff ∂ CO2 ,p
 
εp = 2 r 2 DO2 ,p . (44)
∂t r ∂r ∂r
The corresponding boundary and initial conditions for Eqs. (42)–(44) are given as:
∂ C j ,p
r =0 =0 (45)
∂r
eff ∂ Cj,b  eff ∂ Cj,p 
 
   
r = rp Dj,b = D j ,p Cj,b r = Cj,p r (46)
∂ r r =rp
 ∂ r r =rp p p

r = rb (t ) - external surface area of the bioparticle is completely wetted (to calculate ηℓ )

∂ Cj,w 

eff
= kℓs,j Cj,ℓ − Cj∗,w
 
D j ,b (47)
∂ r r =rb (t )

- external surface area of the bioparticle is completely dry (to calculate ηg )
∂ CO2 ,d 

eff
CS∗,d = kgs,O2 CO2 ,g − CO∗2 ,d HeO2
 
= CS ,ℓ DO2 ,b (48)
∂ r r =rb (t )
t =0 Cj,p(b) (r , 0) = Cjin
,ℓ . (49)
 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718 1707

The biofilm thickness increases with the time during transient state and consequently Eq. (42) is a moving boundary
problem. The average biofilm thickness was estimated at any time by means of the following relationship:

ε o − ε(t )
δb ( t ) = 0
. (50)
a
Because there is no physiological change of microbes when immobilized onto the activated carbon particles, the kinetic
expression of the cell growth obtained from a suspended cell culture can be applied equally well to the immobilized system.
The bacterial growth kinetics for free and captured cells is:
rgf = µεℓ cc (51)
rgs = µρc σ (52)
where µ is the specific growth rate given by the Haldane type equation developed by Tang et al. [40]:
µmax CS CO2
µ= . (53)
Ks + CS + CS /Ki ox + CO2
2
K
Also, the kinetic expression of cell death obtained from a suspended cell culture is applied equally to the immobilized system.
Sen et al. [41] proposed an irreversible first order reaction for death of bacterial cells:
rdf = kdf εℓ cc (54)
rds = kds ρc σ . (55)
Bacterial cells attachment rate was evaluated coupling Eqs. (12) and (13). The transport of the bacterial cell to the bioparticle
surface quantified by the collection efficiency was estimated with the expression developed by Rajagopalan and Tien [27],
obtained by the combination of the trajectory analysis of a spherical particle in the vicinity of a spherical collector with the
contribution of the Brownian diffusion.
Under trickle flow conditions fluid shear stress has no significant influence on the cells detachment rate. However, during
reversible attachment, cells still exhibit Brownian motion and are easily removed by application of mild shear force [42]. So
reversibility implies detachment of adhering cells when conditions become unfavorable and the rate-limiting step in cells
detachment is diffusion of detached cells across the boundary layer between collector surfaces and liquid bulk. The rate of
Brownian cells and aggregates detachment was evaluated using the expression developed by Ryan and Gschwend [29] in
the case of colloids detachment (Eq. (17)). For non-Brownian cell aggregates, the rate of hydrodynamic detachment was
considered to be proportional to the difference between the wall shear stress and the critical shear stress [21]:

,a,k = αrel,a,k a(1 − ε)ηe τw − τcr ,a,k for τw > τcr ,a,k
h h
 
rrel (56)
h
rrel,a ,k = 0 for τw < τcr ,a,k (57)
where critical shear stress was estimated for the condition of equilibrium between the forces acting on the attached
aggregate along the tangential direction, Eq. (16).
The generation of the bacterial cell aggregates was considered to take place by the collision and subsequent bonding
of the cells transported from the bulk liquid to the surface of the bioparticle in the liquid approaching the bioparticle and
by the collision with the associated growth cells (the aggregation process includes the bacterial cells autoaggregation —
attachment of one species to its clonal descendents). Cells within the biofilm were individualized as in the case of IbM
theory [39]. Bacterial cells aggregation rate was described by the rate at which a certain size aggregate is being formed
by smaller aggregates minus the rate at which the aggregate combines to form a larger aggregate (neglecting aggregate
break-up). This is given be the discrete population balance equation of von Smoluchowski [25], Eq. (18). In this equation,
the population balance equation for the primary microbial cells which collide to form aggregates is the following:

rgs ηG
max
dn1 rdep,c  dnk rds
= + − k − . (58)
dt vc ρc vc ρ c k=2
dt vc ρc
Only Brownian motion and differential settling were considered to give particles collision (Eqs. (19) and (20)).
Assuming trickle flow regime, the double slit model provides satisfactory approximations for the liquid–solid, gas–solid
and gas–liquid drag forces [35]. For the adaptation to the biofilm clogging context, these drag equations are recast as
local functions of the local instantaneous values of the porosity and of the effective specific surface area of the bioparticle
(Eqs. (23) and (25)).

4. Numerical implementation

To make the two Euler–Euler models solvable, boundary and initial conditions need to be specified for the system in
trickle flow regime. The inlet velocities are specified in Dirichlet-type boundary conditions. At the outlet, an open boundary
condition is used [24] which implies, except for pressure, zero gradients for all flow variables normal to outflow boundary.
1708 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718

Table 1
Model parameters — clogging in trickle-bed reactors.

Properties of materials
Liquid
Straight run gas oil
Viscosity: 0.24 × 10−3 Pa s
Density: 610 kg/m3
Surface tension: 7.8 × 10−3 N/m
Superficial velocity = 0.005 m/s
Gas
Hydrogen
Superficial velocity = 0.05 m/s
Fine particles
Kaolinite
Average diameter: 1–2 µm
Density: 2000 kg/m3
Porosity of deposit layer: 0.8
Influent concentration: 1.0 g/l
Packing
Spherical catalyst particles
Diameter: 0.003 m
Bed porosity: 0.37
Geometry of fixed bed reactor
Diameter: 0.051 m
Height: 1.0 m
Temperature: 573 K
Pressure: 10 MPa
Coefficient of sliding friction: kf = 3.79 × 10−6 m [44]
Hamaker constant: Ha = 1.4 × 10−20 J
Hydrodynamic release rate coefficient: αdeth
= 1.4 × 10−8 kg/N s

Table 2
Model parameters — bioclogging in trickle-bed bioreactors.

Temperature, °C 25
Pressure, atm 1.0
Reactor diameter, m 0.051
Bed height, m 1.0
Diameter of support particle, m 0.003
Density of support particle, kg/m3 1400
Internal porosity 0.575
External porosity 0.37
Superficial liquid velocity, m/s 0.0015
Superficial gas velocity, m/s 0.03
Dry cell mass/cell volume, g/l [45] 1100
Cells diameter, m [45] 1.6 × 10−6
Total dry biomass in the biofilm/wet biofilm volume, g/l 30–75
Henry’s law constant 30
Hamaker constant, J [46] 1.0 × 10−20
Hydrodynamic detachment rate coefficient, kg/Ns 1.0 × 10−8
Coefficient of sliding friction, m [44] 3.79 × 10−6

The liquid hold-up at the reactor inlet is evaluated assuming ∂ ug /∂ z = ∂ uℓ /∂ z = 0 and fully wetted particles and combining
the momentum balance equations for the gas and liquid phases. Danckwerts boundary conditions are used for unsteady
state mass balance equations for planktonic cells and κ -size aggregates and species balance equations in gas and liquid
phases.
In order to solve the partial differential equations, we discretized in space and solved the resulting set of ordinary
differential equations. The spatial discretization is performed using the standard cell-centered finite difference scheme (at
reactor level) and the method of orthogonal collocation (at solid particle and biofilm levels). The number of collocation points
specified for the biofilm and activated carbon particle was restricted to 5. The GEAR integration method for stiff differential
equations was employed to integrate the time derivatives. The relative error tolerance for the time integration process in
the present simulations is set at 10−6 for each time step. Fortran 77 software on Intel⃝ R
CoreTM 2 Duo Processor E7500 was
used to generate the numerical platform.
The aggregation model stability was examined by the number or mass conservation during aggregation modeling which
can be represented by a mass conservation factor that is the ratio of the total number of primary particles for each aggregate
 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718 1709

Fig. 1. Impact of aggregate fractal dimension on transient behavior of two-phase pressure drop (df = 2 µm, α = 1.0, max = 15).

size class to the initial primary particle number concentration:

max
k (nk )t

k=1
Mass conservation factor = . (59)
(n1 )t =0
To describe the aggregation process a maximum size class of 25 was used. Although it would be desirable to have an unlim-
ited size class such that the aggregate growth would be unbounded, computationally this is not possible. So, this maximum
size class was limited.

5. Results and discussion

Capture, aggregation, detachment and migration of Brownian particles/cells and aggregates in two-phase flow porous
media systems are complex so that flow field imaging of these transient phenomena accompanying two-phase flow is not
trivial and has not yet been experimentally attempted. It is proposed here to test the models potentiality through simulations
of different experimental configurations by solving the transport equations for trickle-bed reactors/ bioreactors experiencing
physical/biological clogging via fines/cells attachment, aggregation and detachment. Biological clogging tests are simulated
for phenol biodegradation by Pseudomonas putida as the predominant species immobilized on spherical activated carbon
particles. The simulated conditions are listed in Tables 1 and 2.

5.1. Plugging in trickle-bed reactors

Pressure drop across the bed is probably the most straightforward criterion to sense plugging in trickle bed reactors. Fig. 1
shows the history of ∆P /∆P o ratio (where ∆P o is the two-phase pressure drop for the clean bed under otherwise identical
conditions) for different values of the fractal dimension for the operating conditions listed in Table 1. Fig. 2 shows that the
primary Brownian fines volume-averaged solid deposit and aggregates volume-averaged specific deposit increases in time
yielding a higher total volume-averaged specific deposit. As a result, the bed porosity decreases and two-phase pressure drop
increases. The major change resulting from fine particles deposition in the bed involves the reduction of bed porosity, and
therefore the increase of two phase pressure drop is the result of the decrease in the available free space. Also, Fig. 2 shows
that with the increase of fractal dimension (which characterizes the aggregation process) the aggregates volume-averaged
specific deposit increases and consequently the primary Brownian fines volume-averaged specific deposit decreases. The
total volume-averaged specific deposit is higher at higher fractal dimension (Fig. 2(c)) due to the lower colloidally induced
release rate of the primary Brownian deposited particles and due to the lower number of non-Brownian aggregates able
to be detached by hydrodynamic forces. On the other hand, a smaller fractal dimension for a given collision efficiency
results in a larger aggregate size and a larger number of non-Brownian aggregates able to be detached by hydrodynamic
forces. It is also to notice that inclusion in the model of the fines/aggregates detachment mechanisms does not eliminate
deposition, but rather tends to stretch it in time. Said otherwise, when accounting for detachment the model predicts that
longer durations are needed to attain the same specific deposit values as if the detachment terms were to be excluded in the
model.
1710 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718

Fig. 2. Effect of aggregate fractal dimension on transient behavior of aggregates, fines and total volume-averaged specific solid deposit (df = 2 µm, α =
1.0, max = 15).

The model is sufficiently sensitive to collision efficiency at the beginning of the plugging process (Fig. 3). There is an
evident decrease in aggregates volume-averaged specific deposit with decreasing collision efficiency that is coherent and
also mirrored by the increased fines volume-averaged specific deposit. At high collision efficiency the rate of Brownian
particle agglomeration is elevated and the aggregates volume-averaged specific deposit increases. If the collision efficiency
is less than 0.001, slow aggregation can be expected. At long term, as plugging is a slow (large time-scale) unsteady-
state phenomenon, the collision efficiency does not influence considerably the aggregation process. Because the collision
efficiency approaches unity when colloidal interactions are dominated by deposition [43], the majority of simulations were
undertaken for these conditions.
 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718 1711

Fig. 3. Impact of collision efficiency on the aggregates and fines volume-averaged specific solid deposit (df = 2 µm, Df = 2.0, max = 15).

With the increase of the maximum size class of the aggregates, for a given fractal dimension and collision efficiency,
the number of non-Brownian aggregates able to be detached by hydrodynamic forces increases (Fig. 4). However, the total
volume-averaged solid deposit and two-phase pressure drop do not change with the value of maximum size class of the
aggregates (results not shown). This is because there is equilibrium between the non-Brownian aggregates deposition and
reentrainment and consequently the aggregates volume-averaged solid deposit is not influenced by the hydrodynamic
detachment.
The effect of primary Brownian fines diameter on the fines and aggregates volume-averaged specific deposit is shown
in Fig. 5. The number of primary Brownian particles transported from the bulk liquid to the surface of the collector and the
number of Brownian particles found in the aggregates are higher for df = 1 µm (Fig. 6). However, this is not reflected in
higher values for the fines and aggregates volume-averaged specific deposits because the majority of the aggregates are
colloidal (Fig. 6) and the rate of colloidally induced release of the aggregates is very high. Also, the deposition rate and the
generation rate of the aggregates are higher in the case df = 2 µm yielding higher fines and aggregates specific deposits
at the same filtration time. As a consequence, the decrease in bed porosity is much higher for df = 2 µm and therefore the
increase of two-phase pressure drop is most significant (Fig. 7).

5.2. Bioclogging in trickle-bed bioreactors

From Figs. 8 and 9, it is clear that biomass is not uniformly distributed along the bed and as a consequence the extent of
biological clogging depends upon axial distance (operating conditions and kinetic parameters are listed in Tables 2 and 3).
There is a noticeable increase in biofilm thickness in the entrance section of the bed that is coherent and also mirrored by
the decrease in local porosity. As time advances, the biological clogging front progressively fills up the bioreactor. However,
biomass accumulation is more confined in the entrance region, even if the overall effectiveness factor is lower, because
the cell growth rate is higher in this region. Towards the outside of the bioreactor, the cell growth rate decreases due to
the decrease in substrate concentration and, as a result, the biomass accumulation is much lower than in the entrance
1712 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718

Fig. 4. Variation of number of aggregates of different dimensions along the axial coordinate (df = 2 µm, α = 1.0, Df = 2.0, t = 172 min): (a) max = 15;
(b) max = 25.

Table 3
Values of kinetic parameters [40]—bioclogging in trickle-bed bioreactors.
Kinetic parameter Value

µmax , h−1
0.365
Ks , mg/L 10.948
Ki , mg/L 113.004
Kox , mg/L 0.1
YX /O2 , mg oxygen/mg phenol 0.354
YX /S , mg cell/mg phenol 0.496
Specific decay rate for free and captured cells, s−1 7 × 10−7 s−1

section. As a consequence, the increase of the biofilm thickness is much lower. The biofilm profiles suggest that progression
of biofilm accumulation exhibits a sigmoidal behavior. Such progression can practically be divided into three zones:
(1) induction with biofilm thickness neighboring ca. 1 µm, (2) exponential or log accumulation, and (3) a plateau or steady
state zone.
 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718 1713

Fig. 5. Impact of primary Brownian particles diameter on fines and aggregates volume-averaged specific solid deposit (Df = 3.0, α = 1.0, max = 15).

Even if a smaller fractal dimension for a given collision efficiency results in a larger number of Brownian aggregates non
detachable by hydrodynamic forces (Fig. 9: surface 1 in the region of lower values of κ -size aggregate), the aggregates
volume-averaged specific deposit is lower in this case because the number of cell aggregates able to be detached by
hydrodynamic forces is most important (Fig. 9: surface 2 in the region of higher values of κ -size aggregate). Additionally, the
rate of colloidally induced detachment of bacterial single cells and Brownian aggregates increases and the result is a lower
total (cells + aggregates) volume-averaged specific deposit and biofilm thickness (Fig. 8).
There is an evident increase in bacterial cells and aggregates volume-averaged specific deposit with the increase of
collision efficiency that is coherent with the increase of biofilm thickness (Fig. 10). The collision efficiency affects both cells
attachment and aggregation processes. At high collision efficiency the rate of bacterial cells attachment is elevated and
the volume-averaged specific deposit of bacterial cells increases. On the other hand, at high collision efficiency the rate of
bacterial cells agglomeration is higher indicating a higher value of the volume-averaged specific deposit of aggregates and
consequently a decrease of the volume-averaged specific deposit of bacterial single cells. Additionally, the rate of colloidally
induced detachment of bacterial single cells decreases and the result is a higher total (cells + aggregates) volume-averaged
specific deposit.
Two-phase pressure drop is probably the most straightforward criterion to sense biological clogging. Fig. 11 shows the
history of ∆P /∆P o ratio for different values of the fractal dimension (Fig. 11(a)) and collision efficiency (Fig. 11(b)). The
cells and aggregates volume-averaged specific deposit increases in time yielding thicker biofilm (Figs. 8, 11). As a result, bed
porosity decreases and two-phase pressure drop increases. Two-phase pressure drop first increases slowly, while later on,
due to severe biomass clogging, the increase turns quasi exponential. It is to notice that inclusion in the model of bacterial
cells/aggregates detachment mechanisms reduces biomass accumulation resulting in delayed pressure drop breakthroughs.
However, in the first period of biofilm growth, only a small number of cells and aggregates detach from the surface indicating
that the process is dominated by growth, attachment and aggregation.
1714 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718

Fig. 6. Variation of number of aggregates of different dimensions along the axial coordinate (α = 1.0, Df = 3.0, max = 15, t = 315 min): (a) df = 1 µm;
(b) df = 2 µm.

6. Conclusion

The complex two-phase flow and space–time evolution of fines/bacterial cells capture, aggregation, detachment and
migration in trickle-bed reactors/bioreactors were modeled via Euler–Euler two-fluid dynamic models based on the
volume-average form of the transport equations developed for multiphase systems coupled with the population balance
equations for the particles agglomeration. Mono-layer and multilayer attachment via deep-bed filtration mechanism was
considered for Brownian fines/bacterial cells and only mono-layer attachment in the case of the detaching aggregates.
Detachment of fines/bacterial cells or aggregates from the collector surface was assumed to be induced by colloidal
forces in the case of Brownian fines/cells/aggregates or by hydrodynamic forces in the case of non-Brownian aggregates.
Generation of the fines/bacterial cell aggregates was considered to take place by the collision and subsequent bonding
of the fines/cells transported from bulk liquid to surface of the catalyst particle/bioparticle in the liquid approaching
the catalyst particle/bioparticle and by the collision with the associated growth cells. The complex coupling between
the liquid suspension and solids was monitored via the fines/bacterial cells and aggregates filtration rate equations, the
fines/bacterial cells and aggregates detachment rate equations and the interaction drag or momentum exchange force
terms.
 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718 1715

Fig. 7. Two-phase pressure drop ratio versus time at different values of primary fine particles diameter (Df = 3.0, α = 1.0, max = 15).

Fig. 8. Biofilm thickness versus time at different values of fractal dimension (CSin,ℓ = 30 mg/l, COin2 ,ℓ = 6 mg/l, COin2 ,g = 275 mg/l, ccin = 0.1 g/l, ρb =
30 g/l, α = 0.5): (a) Df = 1.5; (b) Df = 2.0.

The authors’ goal was to develop a framework to enlighten on how the fines/bacterial cells accumulation alter the
hydrodynamics of trickle-bed reactors/bioreactors. Of course there is room for including more phenomena in the models
and we are aware that the value of these, yet complex, models can be further enhanced. 2-D rather than 1-D models, as
suggested here, can be used to account for the partial fouling or evolving maldistribution of gas and liquid.
1716 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718

Fig. 9. Variation of number of aggregates of different size with the axial distance: (CSin,ℓ = 30 mg/l, COin2 ,ℓ = 6 mg/l, COin2 ,g = 275 mg/l, ccin = 0.1 g/l, ρb =
30 g/l, α = 0.5, time = 2000 min, surface 1 − Df = 1.5, surface 2 − Df = 2.0).

Fig. 10. Cells and aggregates volume-averaged specific deposit and biofilm thickness versus time at different values of collision efficiency (CSin,ℓ =
30 mg/l, COin2 ,ℓ = 6 mg/l, COin2 ,g = 275 mg/l, ccin = 0.1 g/l, ρb = 30 000 mg/l, Df = 2.0).

Acknowledgments

Support from the Canada Research Chair ‘‘Green processes for cleaner and sustainable energy’’ and the FQRNT-funded
‘‘Center in Green Chemistry & Catalysis’’ (CVCC) is gratefully acknowledged.
 I. Iliuta, F. Larachi / Computers and Mathematics with Applications 65 (2013) 1698–1718 1717

Fig. 11. Two-phase pressure drop ratio versus time at different values of fractal dimension (a) and at different values of collision efficiency (b) (CSin,ℓ =
30 mg/l, COin2 ,ℓ = 6 mg/l, COin2 ,g = 275 mg/l, ccin = 0.1 g/l, ρb = 30 g/l): (a) α = 0.5; (b) Df = 2.0.

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