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Mechanisms responsible for sub-micron particle deposition ina laminar wall-jet
Anders Goransson, Christian Tragardh *
Food Engineering Center for Chemistry and Chemical Engineering, Lund University, P.O. Box 124, Lund SE-22100, Sweden
Received 4 December 2001; accepted 2 May 2002
Abstract
An experimental study was performed to investigate the dependency of particle size on the deposition rate.
Polystyrene latex particles of two radii (0.23 and 0.38 mm) were deposited onto a glass surface covered with indium-tin
oxide. Reduced deposition efficiency was observed for the larger particles, although an increase in the deposition
efficiency was seen as that the diffusion boundary layer became thicker. A critical degree of surface coverage, ucrit, was
defined as the fraction of surface coverage at which the linear variation of flux with time ended. When the two particle
sizes were compared, it was found that the value of ucrit depended only on the wall shear stress. This result indicates that
surface shielding is an important factor in the decline in particle flux. The deposition process was divided into two
separate processes, described by a mass-transfer coefficient and an adhesion rate coefficient. It was found that the
process was governed by mass-transfer during the initial period, but for higher degrees of surface coverage adhesion
became the rate-determining factor.
# 2002 Elsevier Science B.V. All rights reserved.
Keywords: Wall-jet; Particle deposition; Deposition efficiency; Shielding
1. Introduction
It is important to have knowledge about the
steps governing deposition in a wide range of
different types of processes, e.g. in applications
where proteins bind to surfaces, or in adhesion of
bacterial spores in the food and pharmaceutical
industries [1�/5]. The process of deposition of
colloidal particles can be described schematically
in three steps: the first step consists of convective-
diffusive transport of particles from the bulk
solution to the surface; the second step involves
the adhesion of the particles to the surface under
favourable conditions; and finally, the third step
consists of detachment, which occurs if the re-
moval forces are sufficiently strong to overcome
the adhesion forces. At the beginning of the
deposition process, when the surface still offers a
large number of energetically favourable sites, the
attachment of particles is a linear process with
time. As the number of available sites becomes
fewer, the deposition rate declines. The critical
* Corresponding author. Tel.: �/46-46-222-9807; fax: �/46-
46-222-4622
E-mail address: [email protected] (C.
Tragardh).
Colloids and Surfaces A: Physicochem. Eng. Aspects 211 (2002) 133�/144
www.elsevier.com/locate/colsurfa
0927-7757/02/$ - see front matter # 2002 Elsevier Science B.V. All rights reserved.
PII: S 0 9 2 7 - 7 7 5 7 ( 0 2 ) 0 0 2 5 9 - 5
point at which this non-linear period commences isstrongly flow-dependent, as was shown by Gor-
ansson and Tragardh [6].
The deposition of colloidal particles has been
investigated with different methods. Marshall and
Kitchener [7] employed a rotating-disc apparatus
to investigate the deposition of carbon black
particles under different electrostatic interactions
between particles and surface. In other investiga-tions, parallel-plate channels have been used
[5,8,9]. The stagnation-point flow collector was
developed by Dabros and van de Ven [10], with the
intention of observing particle deposition in situ.
Albery et al. [11] employed a system using a wall-
jet, originally used in the field of electrochemistry.
In both these latter systems, the deposition process
can be monitored without disassembling the appa-ratus. Another advantage of the two systems is
that analytical expressions can be used to calculate
the theoretical flux, flow velocities close to the
surface and the thickness of the diffusion bound-
ary layer, for example. In a study by Albery [12] an
analytical expression for the initial mass-transfer-
controlled deposition flux in a wall-jet was given
as:
j0�0:165D2=3V3=4
f n�5=12a�1=2r�5=4cb; (1)
where D is the diffusion coefficient in the bulk
solution, Vf the volumetric flow rate, n the
kinematic viscosity, a the diameter of the outlet
of the jet, r the radial position and cb the bulk
particle concentration. The validity of Eq. (1) has
been demonstrated in earlier studies [6,11,13,14]for particles with a diameter of about half a
micrometre.
As the deposition process enters the non-linear
phase, different mechanisms control the process
and contribute to the decrease in deposition rate.
One of these mechanisms is the phenomenon of
blocking, in which part of the free surface is no
longer available for nondeposited free-flowingparticles [5,10,14]. The deposited particles occupy
an area that is larger than their cross-sectional
area. Another factor contributing to the fall in
particle flux and which is responsible for the non-
linear temporal behaviour is the detachment of
deposited particles.
The aim of the present work was to determinethe deposition of sub-micron-sized polystyrene
latex particles which is governed by different
flow-related mechanisms. The effect of particle
size on deposition rate was also investigated, since
it is known that the bulk diffusion coefficient
decreases at short distances from a surface.
2. Theory
The phases of the particle deposition processhave been extensively described in the literature for
a range of different conditions. The presence of a
surface will change the conditions for particle
transport. As a particle reaches the vicinity of the
wall, it is affected by the surrounding fluid, and at
nanometre distances electrostatic interactions have
an influence on whether or not the particle will
adhere to the surface. When the particle hasadhered to the surface, the balance of force
between FH (the sum of the hydrodynamic inter-
actions) and FA (the sum of the colloidal interac-
tions) determines whether the deposited particle
will remain on the surface or detach [15]. If FH5/
FA no detachment will occur, but if FH�/FA the
hydrodynamic interactions will force the particle
to become detached from the surface. A briefsummary of the hydrodynamic forces that affect a
free-flowing particle close to a surface and a
deposited particle on a collector surface follows.
2.1. Hydrodynamic forces acting on a free-flowing
particle
A particle translating in a viscous fluid close to a
wall is affected by the surrounding liquid. In the
presence of a shear flow an inertial lift force will
affect the particle according to Saffman [16]:
Flift�6:46n1=2r(ur�up)r2pj dur
dz j1=2
; (2)
where r is the density of the fluid, ur and up the
velocity of the fluid in the radial direction and
particle velocity, respectively, rp is the particle
radius and z is the distance from the wall. The lift
force is proportional to r2p; implying a greater lift
A. Goransson, C. Tragardh / Colloids and Surfaces A: Physicochem. Eng. Aspects 211 (2002) 133�/144134
force for larger particles. The resistance to movingcloser to the wall increases in the direction normal
to the wall, as described by Brenner [17]:
F zdrag�6plmr2
p
duz
dz; (3)
where uz is the particle velocity normal to the walland l is a resistance coefficient expressed by
Dahneke [18] as a function of particle radius and
gap width:
l(rp; h)�1�rp
h; (4)
where h is the gap between particle and wall. The
resistance coefficient describes the increase in
resistance experienced by a particle when moving
towards a wall, due to the presence of the
molecules of the surrounding medium that must
be displaced. For large gaps the function ap-
proaches unity. In an experimental investigation
by Adamczyk et al. [19] the resistance coefficientfor a solid sphere moving towards a surface was
presented.
2.2. Hydrodynamic forces acting on a deposited
particle
A particle in creeping flow (RepB/1) in contact
with a wall is exposed to forces of various natures.One of the hydrodynamic forces involved in the
process is the viscous drag force parallel to the
surface, expressed as Stokes’ drag force
F rdrag�6pf mr2
p
dur
dzjy�rp
�6pf twr2p; (5)
with a factor f which compensates for wall effects
given as 1.7009 according to O’Neill [20]. The
torque acting on the deposited particle at the point
of contact is expressed by Sharma et al. [21] as
Tcontact�1:399F rdragrp�44:85twr3
p; (6)
with the drag force acting at a distance of 1.399
particle radii from the wall [20]. The torque is thus
proportional to twr3p: The lift force acting on a
stationary particle deposited on the wall was
expressed by Hubbe [22] as:
Flift�81:2m�1=2n�1=2t3=2w r3
p; (7)
where the inertial lift force is proportional to
t3=2w r3
p: In the case of particle Reynolds’ numbers
much smaller than unity, as in our case, the effect
of the inertial lift force on a deposited particle is
negligible [22].
Apart from the above-mentioned hydrodynamic
forces, there are also colloidal interactions of
various strengths and ranges, which act both onfree-flowing particles in the vicinity of the surface
and on deposited particles. The attractive
London�/van der Waals’ interaction energy and
the repulsive electrical double-layer energy are
both proportional to the particle radius.
3. Materials and methods
Particle deposition was studied in a wall-jet cell,
originally developed by Albery et al. [11]. The
experimental set-up is described in detail by
Goransson and Tragardh [6]. The flow cell, made
of Perspex, is shown schematically in Fig. 1. Fluid
was pumped, by self-pressure to avoid a pulsating
flow, perpendicular to a glass surface covered with
Fig. 1. Schematic illustration of the wall-jet cell (r , radial
position from stagnation point; a , the diameter of the jet
outlet).
A. Goransson, C. Tragardh / Colloids and Surfaces A: Physicochem. Eng. Aspects 211 (2002) 133�/144 135
indium-tin oxide (Donnelly Applied Films Cor-poration, Boulder, CO, USA). The cell was
mounted on two x -translator stages, which made
it possible to observe the particle deposition at
several positions, exposed to different wall shear
stresses, in one single experiment. The deposition
kinetics was analysed using total internal reflection
microscopy (TIRM). A 5 mW linearly polarized,
He�/Ne laser (Melles-Griot, Irvine, CA, USA) wasused to create the evanescent wave, directed at a
right angle towards a 708, right-angled prism
(BK7, n�/1.5151 at l�/632.8 nm). A head-on
photomultiplier tube (Hamamatsu R1104, Hama-
matsu, Japan), mounted on top of a light micro-
scope (Jena, Jena, Germany), equipped with an
object lens (Leica EF 32/0.40, Wetzlar, Germany)
with a long working distance (total magnification200�/) was used to measure the light intensity
from the deposited particles. The sampled data
were digitalized and transferred to a computer.
Using a calibration procedure, described pre-
viously [6], the intensity was transformed to the
number of particles per surface unit area.
Polystyrene latex particles of two radii, 0.23
(Sigma Latex Beads, Lot 57H1207, Sigma-AldrichCorp., St. Louis, MO, USA) and 0.38 mm (Sigma
Latex Beads, Lot 067H0291, Sigma-Aldrich Corp.,
St. Louis, MO, USA) were used in the deposition
experiments. The bulk particle concentrations
were 4�/109 cm�3 for the 0.23 mm particles and
8.7�/108 cm�3 for the 0.38 mm particles. These
concentrations were chosen to obtain the same
volume fraction in both cases. During an experi-mental run the bulk particle concentration was
determined by measuring the turbidity of the feed
at 700 nm, and the concentration was frequently
adjusted by adding fresh colloid solution to the
feed. The feed vessel was continuously stirred
throughout the whole experiment. All colloid
solutions were prepared with deionized, double-
distilled water (DDDW) from a Milli-Q plant(Millipore Co., Bedford, MA, USA). The electro-
lyte concentration was 50 mM KNO3, and a
citrate�/phosphate buffer solution was used to-
gether with HNO3 and KOH to set the pH to 5.5.
The volumetric flow rates were chosen so as to
obtain the same hydrodynamic drag forces for the
two particle sizes at corresponding radial positions
from the stagnation point. For the smaller parti-cles the flow rates were set to 0.12 and 0.20 cm3
s�1, corresponding to Reynolds’ numbers of 154
and 253 (Re�/ua /(2n ), where u is the velocity of
the fluid in the jet nozzle, a the diameter of the
nozzle and n the kinematic viscosity). For the
larger particles, the flow rates were chosen to be
0.07 and 0.12 cm3 s�1, with Reynolds’ numbers
equal to 94 and 156. All experiments were carriedout at a temperature of 219/1 8C.
4. Results and discussion
4.1. Mass-transport-controlled particle deposition
In Fig. 2(a),(b) the initial particle flux, linearlyincreasing with time, is shown as a function of
r�5/4 for the 0.38 and 0.23 mm-sized particles,
respectively. For the larger particles the volumetric
flow rate was 0.07 cm3 s�1 and for the smaller
particles it was 0.12 cm3 s�1. In both cases the
initial flux followed the r�5/4 dependency accord-
ing to Eq. (1). From the slope of the regression
lines fitted to the data points it is possible tocalculate the particle diffusion coefficients by
employing Eq. (1). The experimentally calculated
diffusion coefficient for the 0.23 mm-sized particles
was found to be 8.6�/10�9 cm2 s�1, based on the
data in Fig. 2(b). This is in good agreement with
the diffusion coefficient according to the Stokes�/
Einstein relation, which is 9.3�/10�9 cm2 s�1.
However, for particles with a radius of 0.38 mm theexperimentally calculated diffusion coefficient was
found to be only 27% of the theoretical diffusion
coefficient, which is calculated to be 5.6�/10�9
cm2 s�1. It can thus be concluded that Eq. (1) does
not describe the particle flux for the larger
particles under the prevailing conditions.
The particle flux onto a flat surface was shown
by Levich to be proportional to the cubic root ofthe wall shear stress. In Fig. 3 the initial flux of the
small particles is shown as a function of the cubic
root of the wall shear stress, t1=3w ; for the two
volumetric flow rates, 0.20 and 0.12 cm3 s�1. It
can be seen that, for both cases, good correlation
was obtained. Similar behaviour was seen by
A. Goransson, C. Tragardh / Colloids and Surfaces A: Physicochem. Eng. Aspects 211 (2002) 133�/144136
Parsons et al. [23] when studying the initial flux of
polystyrene particles of 0.13 mm radius.
The initial experimental flux, j0,exp, of the
particles with a 0.38 mm radius is shown as a
Fig. 2. The initial particle flux, linear with time, j0,exp, as a function of r�5/4 with r being the radial distance from the stagnation point.
(a) The flux of 0.38 mm particles, with a bulk particle concentration of 8.7�/108 cm�3 and volumetric flow rate of 0.07 cm3 s�1. (b)
Particle radius of 0.23 mm, with a bulk particle concentration of 4�/109 cm�3 and volumetric flow rate of 0.12 cm3 s�1.
A. Goransson, C. Tragardh / Colloids and Surfaces A: Physicochem. Eng. Aspects 211 (2002) 133�/144 137
function of wall shear stress, tw, for a volumetric
flow rate of 0.12 cm3 s�1 in Fig. 4(a). The
theoretical flux, j0,theo, calculated from Eq. (1), is
also included and it can be seen that the experi-
mental flux was considerably lower than that
predicted by theory. By introducing the deposition
efficiency, x , defined as the ratio of the experi-
mental initial flux to the theoretical initial flux
(x�/j0,exp/j0,theo), the reduction in the initial parti-
cle flux can clearly be seen. The reason for this
discrepancy between theory and experiment is that
the initial particle flux equation, Eq. (1), is based
on Smoluchovski�/Levich approximation, i.e. the
reduced hydrodynamic mobility of a particle
approaching a surface, as shown by Brenner in
Eq. (3), is assumed to be balanced by attractive
van der Waals’ forces. As was shown in Fig. 2(b),
the Smoluchovski�/Levich approximation is valid
for the smaller particles, but not for the larger
particles. According to Eq. (3) the hydrodynamic
drag force is proportional to the square of the
particle radius. The van der Waals’ interaction, on
the other hand, shows a linear relation to the
particle radius. It thus follows that for larger
particles the hydrodynamic resistance dominates
over the attractive forces, resulting in a reduction
in the particle flux to the deposition surface. The
deposition efficiency is strongly dependent on the
wall shear stress, which can be clearly seen in Fig.4(a), as well as the particle size. The deposition
efficiency in Fig. 4(a) increased with decreasing
wall shear stress, as described by a power-law fit:
x(tw)�0:29t�0:21w : (8)
The deposition efficiency is proportional to t�0:21w ;
which resembles the results of van de Ven andMason [24], who investigated the coagulation
efficiency of spheres exposed to a shear flow. The
coagulation efficiency was proportional to/g�0:18 (/g
being the wall shear rate). This trend was also
found in an investigation by Sjollema and
Busscher [5], in which the predicted deposition
efficiency increased at lower Peclet numbers (low
wall shear stresses). However, they were not ableto see the increase in deposition efficiency in their
experiments at low Re numbers, since the diffusion
boundary layer was too thick (10 mm). In Fig. 4(b)
the deposition efficiency is shown as a function of
the thickness of the diffusion boundary layer for
the data in Fig. 4(a). The diffusion boundary layer
Fig. 3. The initial particle flux, j0,exp, as a function of the cubic root of the wall shear stress, t1=3w ; for the smaller particles at volumetric
flow rates of 0.20 cm3 s�1 (m) and 0.12 cm3 s�1 (j).
A. Goransson, C. Tragardh / Colloids and Surfaces A: Physicochem. Eng. Aspects 211 (2002) 133�/144138
thickness, which is defined as a region close to the
collector surface where a sudden change in the
concentration profile occurs, has been defined for
a wall-jet [25] according to:
ddbl�5:8sp3=4D1=3a1=2n5=12r5=4V�3=4
f ; (9)
where the constant s equals 0.17, and was
experimentally determined by Yamada and Mat-
suda [26]. By adopting Eq. (9) the diffusion
boundary layer thickness was estimated to vary
from 1 to 3 mm. The deposition efficiency in-
creased linearly as the diffusion boundary layer
Fig. 4. (a) The initial particle flux, j0,exp, as a function of wall shear stress. (m) Data from an experiment carried out at a volumetric
flow rate of 0.12 cm3 s�1, a bulk particle concentration of 8.7�/108 cm�3 and a particle size of 0.38 mm; (j) theoretical particle flux
calculated from Eq. (1); (') the deposition efficiency; and the dashed line represents the linear fit to the deposition efficiency data. (b)
The deposition efficiency versus the diffusion boundary layer thickness at a volumetric flow rate of 0.12 cm3 s�1. The particle radius
was 0.38 mm.
A. Goransson, C. Tragardh / Colloids and Surfaces A: Physicochem. Eng. Aspects 211 (2002) 133�/144 139
became thicker. This behaviour can be explainedby the fact that when the convective contribution
is greater, i.e. the boundary layer is thin, the
particles do not have time to establish contact on
the collector surface, but are dragged away by the
fluid flow. On the other hand, in the case of an
increasing diffusive contribution in particle trans-
port, the free-flowing particles can more easily
reach the collector surface undisturbed by thesurrounding fluid.
4.2. Particle deposition controlled by adhesion
Fig. 5(a) shows typical deposition with time data
for an experiment carried out with particles of 0.38
mm radius, and a volumetric flow rate of 0.12 cm3
s�1 at a radial position 4.00 mm from the
stagnation point. Particle deposition was moni-
tored for 10 h, reaching a degree of surface
coverage of approximately 0.46, which corre-sponds to a particle wall concentration of 1.0�/
108 cm�2. The linear deposition step discussed in
the previous section, prevailed up to a certain
degree of surface coverage, ucrit (the degree of
coverage is defined as cwp2p; where cw is the particle
wall concentration). This critical degree of cover-
age is typical for the flow conditions at the specific
position shown in the figure, which in this case wasapproximately 0.2. The mass-transfer-controlled
step is followed by a deposition phase that is non-
linear with time. The reason for the fall in the
particle deposition flux may be, for example, that
particles on the surface occupy a given area, thus
preventing free-flowing particles from reaching the
surface. The phenomenon is referred to in the
literature as shielding and is strongly flow-depen-
dent, as was demonstrated by Goransson and
Tragardh [14]. The critical degree of surface
coverage, ucrit, can be interpreted as the degree
of surface coverage by deposited particles and
their ‘‘shadows’’ when the non-linear deposition
phase begins. It is then possible to estimate the
magnitude of the area shadowed by a deposited
particle. In Fig. 5(b) the ratio of the excluded area,
Aexcl, to the particle cross-sectional area, ap, is
shown for a range of wall shear stresses for both
particle radii. The experimentally determined ex-
cluded area ratio increased with increasing wall
shear stress. For the flow conditions prevailing in
Fig. 5(a), with a wall shear stress of 0.08 Nm�2,
the excluded area can be estimated to be seven
cross-sectional areas. For higher wall shear stres-
ses, 0.5�/0.9 Nm�2, the size of the excluded area
for the smaller particles reached as high as 25�/30
particle radii. As the deposition process proceeds
the shielded areas will, to some extent, become
occupied by particles, due to factors such as
Brownian diffusion and collisions between free-
Fig. 5. (a) Experimental data for 0.38 mm particles at a radial distance from the stagnation point of 4.00 mm. The wall shear stress at
this distance is 0.08 Nm�2. The volumetric flow rate was 0.12 cm3 s�1 and the bulk particle concentration was 8.7�/108 cm�3. The
degree of coverage at the onset of non-linear particle flux, ucrit, is indicated in the figure. (b) An experimental estimate of the excluded
area is shown as a function of wall shear stress for both particle sizes, (m) 0.23 mm, (k) 0.38 mm.
A. Goransson, C. Tragardh / Colloids and Surfaces A: Physicochem. Eng. Aspects 211 (2002) 133�/144140
flowing particles, and thus the particle wall con-
centration will continuously increase.
Shielding is not the only phenomenon believed
to be responsible for the decline in particle flux.
Another reason for the flux decrease is the
detachment of deposited particles. This detach-
ment may be caused by free-flowing particles
colliding with deposited ones, or removal by the
shear flow acting on the deposited particles,
according to Eq. (5). In Section 2.2 the various
forces affecting particles deposited on a flat sur-
face were presented. By plotting the critical degree
of coverage, ucrit, against twr2p (drag force), twr3
p
(torque), t3=2w r3
p (lift force) and tw (wall shear stress)
the dependency of ucrit was investigated for both
particle sizes (Fig. 6(a�/d)).
Fig. 6(a) shows the critical degree of coverage,
ucrit, as a function of twr2p; i.e. the hydrodynamic
drag force acting parallel to the collector surface
on the deposited particle, according to Eq. (5). The
data shown in the figure are the mean values of
three experiments each at volumetric flow rates of
0.20 cm3 s�1 (rp�/0.23 mm) and 0.12 cm3 s�1
(rp�/0.38 mm). A mutual linear regression fit to
the data for the two particle sizes resulted in a
correlation coefficient of �/0.84. It can be seen that
Fig. 6. The dependency of the end of the initial period of linear flux with time, ucrit, on different phenomena is shown. Mean values are
given for three experiments each, carried out at volumetric flow rates of 0.20 cm3 s�1 (0.23 mm) and 0.12 cm3 s�1 (0.38 mm). (a) ucrit
versus twr2p (drag force), (m) 0.23 mm; (j) 0.38 mm. (b) ucrit versus twr3
p (torque), (m) 0.23 mm; (j) 0.38 mm. (c) ucrit versus twr3=2p (lift
force), (m) 0.23 mm; (j) 0.38 mm. (d) ucrit versus tw (wall shear stress), (m) 0.23 mm; (j) 0.38 mm.
A. Goransson, C. Tragardh / Colloids and Surfaces A: Physicochem. Eng. Aspects 211 (2002) 133�/144 141
the data for the two particle sizes converge as thedrag force increases. Fig. 6(b) shows the signifi-
cance of the torque on ucrit. The mutual regression
line resulted in a correlation coefficient of �/0.63.
In Fig. 6(c), ucrit is plotted against the lift force,
with a correlation coefficient of �/0.84. The
dependencies of ucrit on the lift force and drag
force are thus higher than that on the torque
acting on the deposited particles. In Fig. 6(d), ucrit
is plotted against the wall shear stress. The data
for both particle sizes are gathered on one line,
suggesting that ucrit is solely dependent on the wall
shear stress. The correlation coefficient was �/
0.97. It also follows that the degree of coverage
when the process becomes non-linear with time
does not depend on the particle size. It might also
indicate that the hydrodynamic forces discussed inSection 2.2 do not play significant roles in the
onset of non-linear deposition phase. Instead, it is
indicated that the shielding phenomenon plays an
important role, being responsible for the decrease
in the particle deposition flux, confirming earlier
works in the area such as Sjollema and Busscher
[5], Dabros and van de Ven [10], Adamczyk et al.
[27], among others.The introduction of a dimensionless particle
wall concentration, cw;crit� ; makes it possible to
compare the four different experimental cases
with volumetric flow rates ranging from 0.07 to
0.20 cm3 s�1. The dimensionless concentration is
expressed with the aid of the bulk particle con-
centration, the bulk particle diffusion coefficient
and the volumetric flow rate:
c+w;crit�cw;critD
cbVf
: (10)
In Fig. 7 the dimensionless particle wall concen-
tration at the end of the linear deposition period is
shown as a function of the wall shear stress for the
experimental conditions studied. From the relation
that describes the wall shear stress dependency,expressed as a logarithmic expression:
log c+w;crit� (�9:86�0:85)log tw; (11)
it is possible to estimate the particle wall concen-
tration at which non-linear deposition commences
for a wide range of wall shear stresses.
4.3. The overall deposition process
The overall deposition rate constant, k , can be
divided into two separate processes, which are
governed by a mass-transfer rate coefficient, kmass,
and an adhesion rate coefficient, katt, expressed as:
1
k�
1
kmass
�1
katt
: (12)
The mass-transfer rate coefficient for the wall-jet is
Fig. 7. The dimensionless particle wall concentration (cw,critD /
(cbVf)) as a function of the wall shear stress*/(m) 0.23 mm,
Vf�/0.20 cm3 s�1; (k) 0.38 mm, Vf�/0.12 cm3 s�1; (j) 0.23
mm, Vf�/0.12 cm3 s�1; (I) 0.38 mm, Vf�/0.07 cm3 s�1.
Fig. 8. Rate coefficients from an experiment carried out with
the smaller particles at a volumetric flow rate of 0.20 cm3 s�1 at
3.50 mm from the stagnation point. The overall rate coefficient,
k , (m), the adhesion rate coefficient, katt, (k) and the mass-
transfer coefficient, kmass (dashed line).
A. Goransson, C. Tragardh / Colloids and Surfaces A: Physicochem. Eng. Aspects 211 (2002) 133�/144142
expressed by Eq. (1). In Fig. 8 the three rate
constants are given as a function of the degree of
coverage from an experiment carried out at a
volumetric flow rate of 0.20 cm3 s�1, with a
particle radius of 0.23 mm. The radial position
was 3.50 mm from the stagnation point. It can be
seen that at the beginning of the deposition process
the rate-determining factor is the mass-transfer
rate, but as the particle surface coverage exceeds a
critical level, adhesion becomes the rate-determin-
ing factor.
Fig. 9(a) shows a first-order kinetics plot for the
data shown in Fig. 8. It can be seen that particle
deposition starts to follow first-order kinetics after
approximately 4 h of deposition, at which time the
degree of coverage has reached 0.26. It then
continues until the end of the experiment. Thegradient can be interpreted as the transfer coeffi-
cient in Eq. (13):
du
dt�k(1�u): (13)
Fig. 9. (a) A first-order kinetics plot for the particles of rp�/0.23 mm at a radial distance of 3.50 mm and wall shear stress�/0.34
Nm�2. The first-order period did not commence until approximately 4 h after the start of the experiment and lasted to the end of the
experiment. (b) A first-order kinetics plot of the data shown in Fig. 5(a) at a radial distance of 4.00 mm from the stagnation point and a
wall shear stress of 0.08 Nm�2. The first-order kinetics period lasted for approximately 5.5 h. (c) The dependence of the degree of
coverage at which the first-order kinetics period ends on the wall shear stress for 0.38 mm particles. Experimental conditions are given
in Fig. 5(a).
A. Goransson, C. Tragardh / Colloids and Surfaces A: Physicochem. Eng. Aspects 211 (2002) 133�/144 143
In Goransson and Tragardh [6] it was shown thatk decreases with increased Peclet number (convec-
tion/diffusion ratio).
A first-order kinetics plot for the larger particles
(Fig. 9(b)) shows different behaviour from that of
the smaller particles. The first-order kinetics of the
experimental data presented in Fig. 5(a) is shown.
It can be seen that the deposition process began
with first-order deposition kinetics and lasted forapproximately 5.5 h. The degree of coverage at
which first-order kinetics ceases to control the
deposition is shown in Fig. 9(c) as a function of
wall shear stress for the same experiment. The
period of first-order kinetics lasts longer for those
parts of the surface that are exposed to lower wall
shear stresses.
5. Conclusions
It was demonstrated in this study that the
deposition efficiency was strongly dependent on
wall shear stress and particle size. It was concluded
that hydrodynamic resistance dominates over
attractive forces, resulting in a reduction in mass-transfer for the larger particles.
A critical degree of surface coverage at which
the linear variation in flux with time ended, ucrit,
was introduced. The reason for the change from
linear to non-linear flux was investigated by
studying the effects of different hydrodynamic
forces on the onset of the non-linear flux phase.
It was concluded that ucrit was strongly dependenton wall shear stress, but not on the hydrodynamic
forces investigated, which may indicate that sur-
face shielding plays an important role in the
decline in particle flux.
By introducing a dimensionless particle concen-
tration it was possible to estimate the particle wall
concentration at which the non-linear deposition
commences for a wide range of wall shear stresses.By separating the deposition process into two
consecutive steps, a mass-transfer step and an
adhesion step, it was possible to demonstrate
how the process changed from being governed by
mass-transfer to becoming controlled by the
adhesion rate.
Acknowledgements
The Swedish Research Council for Engineering
Sciences has gratefully provided funding for this
research.
References
[1] R.B. Dickinson, S.L. Cooper, AIChE J. 41 (9) (1995) 2160.
[2] D. Kim, W. Cha, R.L. Beissinger, J. Colloid Interface Sci.
159 (1993) 1.
[3] C.A.-C. Karlsson, M.C. Wahlgren, A.C. Tragardh, J.
Food Eng. 30 (1996) 43.
[4] R.B. Dickinson, J. Colloid Interface Sci. 190 (1997) 142.
[5] J. Sjollema, H.J. Busscher, J. Colloid Interface Sci. 132 (2)
(1989) 382.
[6] A. Goransson, C. Tragardh, J. Colloid Interface Sci. 231
(2000) 228.
[7] J.K. Marshall, J.A. Kitchener, J. Colloid Interface Sci. 22
(1966) 342.
[8] F. Vasak, B.D. Bowen, C.Y. Chen, F. Kastanek, N.
Epstein, Can. J. Chem. Eng. 73 (1995) 785.
[9] Z. Adamczyk, T.G.M. van de Ven, J. Colloid Interface Sci.
80 (2) (1981) 340.
[10] T. Dabros, T.G.M. van de Ven, Colloid Polym. Sci. 261
(1983) 694.
[11] W.J. Albery, G.R. Kneebone, A.W. Foulds, J. Colloid
Interface Sci. 108 (1985) 193.
[12] W.J. Albery, J. Electroanal. Chem. 191 (1985) 1.
[13] S. Joscelyne, C. Tragardh, J. Colloid Interface Sci. 192
(1997) 294.
[14] A. Goransson, C. Tragardh, Colloid Surf. A (submitted
for publication).
[15] J. Visser, J. Colloid Interface Sci. 55 (3) (1976) 664.
[16] P.G. Saffman, J. Fluid Mech. 22 (2) (1965) 385.
[17] H. Brenner, Chem. Eng. Sci. 16 (1961) 242.
[18] B. Dahneke, J. Colloid Interface Sci. 48 (1974) 520.
[19] Z. Adamczyk, M. Adamczyk, T.G.M. van de Ven, J.
Colloid Interface Sci. 96 (1) (1983) 204.
[20] M.E. O’Neill, Chem. Eng. Sci. 23 (1968) 1293.
[21] M.M. Sharma, H. Chamoun, D.S.H.S.R. Sarma, R.S.
Schechter, J. Colloid Interface Sci. 149 (1) (1992) 121.
[22] M.A. Hubbe, Colloids Surf. 12 (1984) 151.
[23] D. Parsons, T. Harrop, E.G. Mahers, Colloids Surf. 64
(1992) 151.
[24] T.G.M. van de Ven, S.G. Mason, Colloid Polym. Sci. 255
(1977) 468.
[25] H. Gunasingham, B. Fleet, Anal. Chem. 55 (8) (1983)
1409.
[26] J. Yamada, H. Matsuda, J. Electroanal. Chem. 44 (1973)
189.
[27] Z. Adamczyk, B. Siwek, L. Szyk, J. Colloid Interface Sci.
174 (1995) 130.
A. Goransson, C. Tragardh / Colloids and Surfaces A: Physicochem. Eng. Aspects 211 (2002) 133�/144144