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Abstract
Microfiltration is the oldest membrane process and shows up to now the largest market for technical membranes
and membrane modules. In technical applications crossflow microfiltration is an established process for the separation
of microparticles, bacteria and emulsion droplets. The following article describes the development and the state of the
art. It makes a contribution to understand the mechanisms of crossflow filtration. © 2002 Elsevier Science BV All rights
reserved.
1383-5866/02/$ - see front matter © 2002 Elsevier Science BV All rights reserved.
PII: S 1 3 8 3 - 5 8 6 6 ( 0 1 ) 0 0 1 1 3 - 7
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S. Ripperger, J. Altmann / Separation/ Purification Technology 26 (2002) 19–31
A market research gives a rough idea about sales Fig. 2. Principle of a laser triangulometer.
volumes, market potentials and technical importance
of a technology. This is even truer when dealing
with an expanding business like membranes. The
membrane market, defined by membrane and
module sales, had estimated sales of over US$1.5
billion in the year 1999.
According to different market research results, the
average annual growth rate is about 10%. The
largest market for membranes and membrane units
(membrane cartridges and membrane mod ules) is
still in MF. This area is responsible for approximately
40% of the current sales, and is growing at an
annual growth rate of 8–10%. It can be estimated
that 70–80% of these sales are membranes and
membrane units for dead-end filtration. The market
for membrane modules for CMF has a size in the
range of about US$150 million worldwide. The
annual growth rate of this part of the market is Fig. 3. Filtration curve of diatomaceous earth at constant
expected to be over 10%. transmembrane pressure.
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S. Ripperger, J. Altmann / Separation/ Purification Technology 26 (2002) 19–31 twenty-one
Table 1
Equations of the calculation of the diffusion coefficient D of particles
in the crossflow filtration
kBT
D=
3x
two
eckstein w
=0,…,0.2 D=0.1x
two two
w
=0.2,…,0.5 D0.025x
two
w
D=0.5
assets
x
two two
=0.2,…,0.5 w
D0.335 (1
two
+0.5 exp(8.8))
two
Geissler w
D=x (A exp(ÿB)+C)
(0.005) two
Fig. 8. Estimation of the lift force and the drag of the filtrate flow. 2. New methods for the investigation of the layer
formation in crossflow microfiltration
3 .1 . Macroscopic models
two
w
FL=0.358 .
Fig. 15. Flux of Titan(IV) oxide suspension vs. the-potential.
(3.2)
Fig. 16. Layer structure at the filtration of a stabilized Titan(IV)oxide suspension (a) and an agglomerated suspension (b) at the same magnification.
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26 S. Ripperger, J. Altmann / Separation/ Purification Technology 26 (2002) 19–31
Fig. 17. Layer structure at the filtration of a stabilized Geltech 500 (monodisperse) suspension (a) and an agglomerated suspension (b) at the
same magnification.
dm
=m tÿm backÿm p. (3.4)
dt
Fig. 20. Comparison of lift force and attractive force of a deposited
particle. The penetrating mass flow depends on pthe characteristics of
the membrane and of the particle system. The mass flow
towards the membrane can be calculated as a convective
be determined by the particles in this size range. mt transport of the filtrate flow (Fig. 10). For the estimation of
In the shown calculation this filtration rate is caused by
the back transport from the membrane m back different model
particles of about 200 nm and amount to about 20 l/(m2 h).
assumptions can be found in the literature. Ripperger [13] used
an empirical model with the assumption that the back transport
from the membrane is proportional to the wall shear stress at
3 .3 . Modeling unsteady filtration behavior
the membrane and proportional to the height of the cake layer.
The models from Geißler [12], Sethi and Wiesner [18], Lee
The starting point of modeling the unsteady filtration and Clark [19] based on the macroscopic shear-induced
behavior is in all known models the mass balance of the
diffusion models.
particles on the membrane.
The differential change of dm/dt is equal to the difference of
the mass flow to the membrane (m t ) and the mass flow from
the membrane (m p+ m back) Unsteady state models, which use microscopic consideration
of particle deposition were intro
Fig. 21. Filtration of 1.5 m monodisperse particles (crossflow velocity 2 m/s (w=15 Pa), pH 10.5, 270 s/cm).
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28 S. Ripperger, J. Altmann / Separation/ Purification Technology 26 (2002) 19–31
duced by Chang and Hwang [20], and Altmann and excludes the possibility of the deposition of fine particles
Ripperger [21]. According to Ref. [21], Fig. 11 shows into an existing particle structure.
the scheme of the calculation of the layer growth for the The asymmetrical layer structure at a filtration at
case of a filtration at with constant transmembrane constant transmembrane pressure could be proved by
pressure. electron microscopical images. Fig. 14(a) shows a cross-
At the beginning of the process the filtration is section of a layer of glass spheres.
rate sure
F determined
p and the membrane
by the transmembrane
resistance RM.pressure
The
filtrate flow causes a convective particle transport to the According to this theory, it is possible to generate
membrane. Because of the particle transport and the ate specific layer structures by varying the operating
particle deposition the layer grows. parameters during the filtration. The introduced model
can be applied for the prediction of such specific
In addition the layer resistance increases and the structures. Fig. 14(b) shows, as the result of an
filtration rate declines. The smaller filter flow has two
experiment, a double asymmetric ric structure. Near the
effects: first, the particle transport to the layer decreases membrane the layer with systems of fine particles, in
and second, the specific cake resistance RL increases middle layers of very large particles and on the top
because of the deposition of finer particles. This cycle again of fine particles.
continues until the filtration rate is so small, that the
This structure was generated by an alternating low–
particle transport to the layer becomes zero.
high–low filtration rate.
Fig. 13 points to a strong asymmetrical layer structure. Agglomeration of a particle system occurs when the
The bottom layer near the membrane shows a low repulsive forces become small in comparison with the
resistance while the uppermost layer at the surface of attractive forces. An electrolytic agglomeration can be
the layer has a very high resistance. This high resistance realized by changing the -potential through the pH-
is caused by the fine particles in the upper layers. value. The agglomeration state has a direct influence
on the filtration rate.
The calculation describes the asymmetrical layer Fig. 15 shows the variation of the stationary filtration
structure with a good correspondence. The experimental rate of a crossflow filtration of Ti tan(IV)oxide (crossflow
values show a higher increase of the cake resistance in velocity – 1.5 m/s, solid concentration – 0.3 vol.%,
the upper layers than the calculation. The reason for hydraulic diameter of the filtration channel – 5.7 mm)
that is the assumption of a constant porosity in the vs. . the-potential.
layer. This assumption
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S. Ripperger, J. Altmann / Separation/ Purification Technology 26 (2002) 19–31 29
It can be seen that the agglomeration of the The irreversibility of the particle deposition could be
Titan(IV)oxide suspension causes a rapid increase of the observed in experiments with monodisperse silica
filtration rate at a -potential of about 25 mV because of particles. The particles were filtered at variable
the enlargement of the effective agglomerate size. The transmembrane pressures.
change in the particle system causes a change in the First, the transmembrane pressure was slowly in creased
cake layer structure. up to 3 bar and after that decreased back to zero. The
Fig. 16(a) shows the layer structure of a stable suspension changing of the transmembrane pressure sure was so
with a porosity of =0.45 and Fig. 16(b) shows the structure slow, that at any time a quasi-station ary layer height and
of an agglomerated system. The layer of the agglomerated filter flow was ensured. Fig. 21 shows the dependencies
suspension shows =0.74 a several times higher porosity. of the layer height and filtrate flow on the transmembrane
pressure.
The same behavior could also be observed with other The filtrate flow increased at low transmembrane
particle systems. Fig. 17 shows the structure of a layer pressures according to the membrane resistance. At
from a monodisperse silica suspension. higher transmembrane pressures only a very small
The steady state flux of an agglomerated parti cle increase of the filtrate flow could be observed, while the
system multiple higher than in the stabilized state. Fig. layer height increased linearly with the transmembrane
18 shows for several investigated parti cle systems a pressure. During the crease of the pressure, the layer
strong increase in the flux due to agglomeration.
height did not change significantly, the filtration rate
declined linearly to the transmembrane pressure. This
indicates that the layer structure and resistance was not
4 .2 . Influence of the interaction forces at
influenced by the decreasing pressure. Because of the
stabilized suspensions
irreversible attached particles a particle transport away
from the layer did not take place.
In suspensions with a high-potential the repulsive
forces between the particles dominate the particle
Other tests with monodisperse or narrow distributed
interaction and cause the stabilization of the suspension.
particle systems with a size of 1.0, 0.5 and 0.24 m also
Furthermore, the repulsion reduces the particle deposition
showed this behaviour.
on the layer, because the repulsive forces act opposite to
The force estimation has shown that particle attachment
the drag of the filtrate flow. Therefore, the stationary
to the layer is mostly an irreversible process. Adhesive
filtration rate in creases with the increasing -potential of
forces are dominating on a deposited particle. This effect
the par ticles. This effect is demonstrated by experiments
can be concluded from the experiments. The build-up of
in Ref. [22]. Fig. 19 shows the described behaviour.
the layer is a continuous process, while the removal of
the layer only takes place by removing large agglom
erates or large layer fragments as shown in Fig.
4 .3 . Reersibility of the layer formation
22. A removal of the layer in the form of a reverse
Particle interaction forces strongly influence the transport from single particles could not be observed.
reversibility of the layer formation. For example, the
calculation of the lift force and the attractive force
according to the DLVO theory of a de posited particle in
Fig. 20 shows that fine particles are irreversibly deposited 5. Applications of crossflow microfiltration
on the layer. The calculations based on the following
parameters: particle size – 600 nm, fluid – water at 20°C, CMF is widely used in different industries. The following
-potential – 40 mV, ion strength – 0.001 mol/l, Hammaker– overview demonstrates the scope of this separation
van-der-Waals-constant – 0.5× 10ÿ20 J, membrane- technique for fine particles, droplets and macromolecular
tube diameter – 5 mm, crossflow velocity – 2 m/s. substances:
clarification of fruit juice, wine, cider and vinegar;
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30 S. Ripperger, J. Altmann / Separation/ Purification Technology 26 (2002) 19–31
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fermentation
upgrading
broths; load);
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of solid matter).
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shear flows, J. Fluid Mech. (1993) 249–265.
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