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Chemical Engineering Science 56 (2001) 47254736

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Sedimentation of polydispersed particles from


a turbulent plume
Silvana S. S. Cardoso , Mehran
Zarrebini
Department of Chemical Engineering, University of Cambridge Pembroke Street, Cambridge CB2 3RA, UK
Received 30 June 2000; received in revised form 12 April 2001; accepted 17 April 2001

Abstract
Particle-laden plumes are ubiquitous in many industrial environments, including cement manufacturing, metallurgical processes
and fossil-fuel-based power plants. Once a plume is emitted into the atmosphere, the size of the particles plays a crucial role on
their sedimentation patterns and on the risk they pose to terrestrial ecosystems and to humans. It is therefore of great interest to
consider and compare the behaviour of particles of di5erent sizes emitted from an industrial chimney. In this paper, we present a
model that describes the dynamics and deposition pattern from gravity currents generated by axisymmetric particle-laden plumes
composed of polydispersed particles. Predictions of the deposition patterns of particles of di5erent sizes are successfully compared
with new laboratory measurements. We also present experimental and theoretical predictions for the mean particle diameter in the
deposit at the 8oor as a function of radial position. We consider environments of both in9nite and 9nite lateral extent. Finally,
we illustrate and discuss the application of the model to the emission of chromium particles from a commercial chromium plating
plant. ? 2001 Elsevier Science Ltd. All rights reserved.
Keywords: Particles; Plume; Fluid mechanics; Sedimentation; Pollution; Environment

1. Introduction
Air pollution caused by dust emissions is currently being given great attention by industry and legislation (US
EPA, 1997; World Bank, 1999; WHO, 1999). Particulate matters are emitted from various industrial sources,
including coal-9red thermal power plants, roasters and
smelters for the production of various metals, petroleum
re9neries, 8uidised-bed catalytic cracking units, cement
and fertiliser plants. The e5ects of particulate emissions
on human health and terrestrial ecosystems can be very
severe, more so when noxious chemicals have been adsorbed on the surface of these particles. Small particles,
of diameter of 10 m or less, remain suspended in the
atmosphere for long periods of time. These particles,
when inhaled, can pass through the natural protective
mechanism of the human respiratory system, causing

Corresponding author. Tel.: +44-1223-31863; fax: +44-1223334796.


E-mail address: silvana cardoso@cheng.cam.ac.uk
(S. S. S. Cardoso).

irritation, asphyxia, central nervous system depression,


gastric intestinal track irregularities and pulmonary 9brosis (Schwartz, 1993; Kane, 1994; US EPA, 1996). In
particular, the smaller particles, of 2 m or less, are responsible for most of the excess mortality and morbidity associated with high levels of exposure to particulates
(World Bank, 1999). Furthermore, deposition of particulates on vegetation may result in the reduction of plant
growth and yields. Particulate air pollution also plays an
important role on the corrosion, erosion and soiling of
any exposed surfaces, such as buildings and cars (World
Bank, 1999).
In view of the greater risk to health posed by smaller
particulates in comparison to the larger ones (World
Bank, 1999), it is important to determine and compare
the behaviour in the atmosphere of particles of di5erent
sizes emitted from an industrial chimney. In particular, it
is important to predict the concentrations of each particle
size in the air in the vicinity of the source of pollution,
as well as their deposition rate on the ground.
In a recent paper, Zarrebini and Cardoso (2000) examined the dynamics of and the deposition pattern arising

0009-2509/01/$ - see front matter ? 2001 Elsevier Science Ltd. All rights reserved.
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S. S. S. Cardoso, M. Zarrebini / Chemical Engineering Science 56 (2001) 47254736

laboratory measurements. We also present experimental


and theoretical predictions for the mean particle diameter
in the deposit at the 8oor as a function of radial position.
We consider environments of both 9nite and in9nite lateral extent. Finally, we illustrate and discuss the application of the model to the emission of chromium particles
from a commercial plating plant.

2. Experimental equipment and methods


2.1. Experimental procedure
Fig. 1. Schematic of the experimental apparatus.

from axisymmetric particle-laden plumes. A turbulent


plume was released into an environment of 9nite vertical extent (Fig. 1). Upon reaching the maximum height,
the plume spreads out radially, forming a current. The
sediment is suspended in the current by turbulence, but
particles continuously settle out of the lower boundary
of the current. As the sediment settles out, it is drawn
back towards the plume by a net in8ow driven by the
entrainment of ambient 8uid at the plume margins. As a
result, a fraction of the settling particles are re-entrained
into the rising plume. It was found experimentally that
such interaction between the particles in the environment
and the continuing plume plays a central role on the dynamics of the plume and on the sedimentation patterns
on the surrounding 8oor. Zarrebini and Cardoso (2000)
used these experimental observations to develop a theoretical description of the concentration of particles in the
plume, in the gravity current and in the surrounding environment, as well as the rate of settling on the 8oor. The
theoretical predictions were successfully compared with
data from the laboratory experiments.
The work of Zarrebini and Cardoso (2000) addressed
the simpli9ed case of uniformly sized particles. However, in most industrial processes involving particle-laden
8ows, as the examples described above, a range of particle sizes is present. Such polydispersivity of particle sizes
will have important e5ects on the patterns of sedimentation from the gravity current and on the re-entrainment
of particles into the plume, and thereby on the dynamics
of the continuing plume. Therefore, the concentrations of
the particles in the environment surrounding the plume,
as well as density of the deposit on the 8oor, will depend
on the particle size distribution.
In this paper, we present a model that describes the
dynamics and deposition pattern of radially spreading
gravity currents generated by a particle-laden plume composed of polydispersed particles. Predictions of the deposition patterns are successfully compared with new

The experiments were conducted in a tank of cross


section 75 cm 75 cm and height 75 cm. The tank was
9lled to a depth of 30 cm with NaCl aqueous solution,
with a concentration of approximately 3% (w : w). The
accurate concentration of this solution was measured by
refractometry. A mixture of fresh water and particles was
stirred continuously in a bucket of volume 10 l. The particle concentration in this suspension was 6:00 g=l. The
suspension was pumped continuously through a nozzle
of diameter 7 mm positioned at the centre of the base of
the tank (Fig. 1). The 8ow rate into the tank was controlled by a 8ow diverter; the remainder of the 8ow was
recycled back into the bucket, aiding mixing of the suspension in the bucket. The 8ow rate was measured by
timing the decrease in the level of the suspension in the
bucket. The 8ow rate used was approximately 13 cm3 =s;
this is suIciently small for the 8ow to approximate that
of a pure plume at a short distance above the source. The
volume of suspension injected into the tank during each
experiment resulted in an increase of approximately 3%
in the level of liquid in the tank. The e5ect of this change
on the 8ow in the plume and surroundings is suIciently
small to be neglected in our modelling in Section 3. The
experimental conditions for two nearly identical runs are
summarised in Table 1.
A number of trays were positioned radially away from
the nozzle on the 8oor of the tank in order to collect the
sedimenting particles. Each tray had a cross section of
1:9 cm 1:9 cm. At the end of an experiment, the particles were extracted from each tray using a syringe and
placed in vials for analysis. The diameter of the sampling
syringe was 0:15 cm. The concentration of particles was
determined using a Coulter counter, which works on the
electrical sensing zone method (Allen, 1997).
2.2. Particles
The particles used in all experiments were sieved fractions of ballotini. These glass beads are nearly spherical
and suIciently small to settle at low Reynolds number in
water. The Stokes settling velocity of an isolated particle

S. S. S. Cardoso, M. Zarrebini / Chemical Engineering Science 56 (2001) 47254736

4727

Table 1
The experimental conditions
Experiment

Flow rate
Q0 (cm3 =s)

Buoyancy 8ux
B0 (cm4 =s3 )

Particle diameter
dp (m)

Duration of
experiment (s)

Ambient density
e (g=cm3 )

Particle concentration
at source C0 (g=l)

12a
16

13.24
12.86

203.4
215.8

74.38
73.03

506
476

1.0203
1.0218

6.00
6.00

Fig. 2. The distribution of particle sizes in the source suspension.

Fig. 3. Schematic showing the trajectories of particles settling from


the surface current.

was calculated for each diameter di by


ui =

d2i g
(p e );
18

(1)

where and e are the viscosity and density of water,


respectively, p is the density of the particle and g is
the acceleration of gravity. The local concentrations of
particles in the tank were typically smaller than 0.03%
(v : v); these are suIciently small for hindered settling
e5ects to be neglected (Batchelor, 1982; Huppert, Kerr,
Lister, & Turner, 1991). The mean particle density is
2:47 g=cm3 . The particle-size distribution in each fraction was determined using the Coulter counter. The distribution of particle sizes (by mass fraction) is shown in
Fig. 2. The distribution is bimodal, with particle diameters
ranging from 38 to 115 m. Such distribution was used
to allow us to distinguish easily the behaviour of smaller
and larger particles in the system. The root mean square
particle diameter for each experimental run is given in
Table 1.

3. Model
Zarrebini and Cardoso (2000) have developed a rigorous model for the dynamics and deposition pattern from
axisymmetric particle-laden plumes, composed of dense
particles of one size. Here we extend the model to account
for the dispersion of sizes of the suspended particles.

3.1. Environment of in4nite lateral extent


Consider a turbulent, axisymmetric plume created by
the release of a buoyant suspension into a body of denser
liquid of depth H . In general, the suspended particles
will be polydisperse with a range of settling velocities.
We shall consider a discrete distribution of particle sizes,
with a mass fraction fi of particles of Stokes settling
velocity ui for i = 1; : : : ; n. The concentration of particles
of type i in the suspension released at the source is then
C0i = C0 fi , where C0 is the concentration of particles at
the source; here the concentrations are expressed in mass
per unit volume of mixture.
The plume rises to the surface of the liquid and spreads
out radially producing a turbulent surface current, as illustrated in Fig. 3. The 8ow is suIciently vigorous to
maintain a vertically uniform particle concentration in
the current. However, the particles of type i in suspension, sediment across the bottom boundary of the surface
current with their Stokes velocity ui (Martin & Nokes,
1988; Sparks, Carey, & Sigurdson, 1991). The equation
describing the transport of each type of particle in the
current is thus
Qs dCi (rs ) = 2rs drs Ci (rs )ui ;

(2)

where rs denotes the radial position along the surface


current, Qs is the volumetric 8ow rate of the plume at the
free surface and Ci (rs ) is the concentration of particles of

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S. S. S. Cardoso, M. Zarrebini / Chemical Engineering Science 56 (2001) 47254736

type i at rs . Here, we have assumed that the volumetric


8ow lost by sedimentation from the surface current is
negligible. Integration of Eq. (2) gives the concentration
of particles of type i along the surface current


ui
2
2
(3)
Ci (rs ) = Csi exp (rs bs ) ;
Qs

The result in Eq. (8) simply states that the ratio of the
concentrations of di5erent particles entering the plume
is equal to that leaving the surface current. But, from
Eqs. (3) and (5)


(uj ui )
Ci (rsi )
Cs
= i exp (b2 b2s )
 :
(9)
Cj (rsj ) Csj
Qs

where bs is the radius of the plume at the free surface and


Csi is the concentration of particles of type i in the plume
at bs .
The path of a particular particle depends on its Stokes
velocity, as well as on the radial position at which it leaves
the surface current. Particles with large Stokes velocity
or falling out of the current at small radii tend to be
re-entrained into the plume, whilst particles with small
Stokes velocities or falling out at large radial positions
settle on the ground. In general, the trajectory of a particle
of type i is described by

Now, the velocity in the plume at the spreading level,


ws = Qs =(b2s ), is much greater than the Stokes velocities
of the particles, ui (i = 1; : : : ; n), so

ui r
ui
dz
= =
;
dr
ue bw

(4)

where ue is the radial inward velocity of the environmental 8uid (Zarrebini & Cardoso, 2000), b and w are the
radius and velocity of the plume at height z, respectively,
and  = 0:125 is the entrainment constant (List, 1982;
Turner, 1986).
Consider now two particles of types i and j. Particle
i leaves the current at radius rsi , while particle j leaves
the current at radius rsj . Both particles are re-entrained
into the plume at height zf . Then, using Eq. (4), we may
show that
ui rsi drsi = uj rsj drsj :

(5)

Conservation of particles of type i between the surface


current and the edge of the plume requires that (see the
appendix)
Ci (rsi )ui rsi
drs
cos2 i i ;
Ci (zf ) =
bw
d zf

(6)

where i = arctan(ui =(w)). The radial inward velocity


at the edge of the plume, ue = w, is much greater than
the Stokes velocities of the particles, ui (i = 1; : : : ; n), so
i 0 (i = 1; : : : ; n). Hence,
Cj (rsj )uj rsj
Ci (rsi )ui rsi
drsi =
drsj
Ci (zf )
Cj (zf )
= bue d zf :

(7a)
(7b)

Combining Eqs. (5) and (7a) leads to


Cj (zf ) Cj (rsj )
:
=
Ci (rsi )
Ci (zf )

(8)

(b2 b2s )

(uj ui )
 1
Qs

(10)

and hence
Cs
Ci (rsi )
i
Cj (rsj ) Csj
for particles i and j entering the plume at zf :

(11)

Combining Eqs. (8) and (11), gives


Ci (zf ) Csi
=
:
Cj (zf ) Csj

(12)

Eq. (12) shows that at each height zf , the ratio of the


concentrations of particles of types i and j entering the
plume is equal to the ratio of the concentrations of the
same particle types in the plume at the spreading level.
We may de9ne a critical radius rci for each particle
type i, separating the region of re-entrainment from the
region of settling on the 8oor (Sparks et al., 1991). A
particle i settling from the current at rci has a trajectory
which brings it back to the source of the plume, so that it
is re-entrained (see Fig. 3). In steady state, the 8ow rate
of particles i in the surface current at the critical radius
rci is equal to the 8ow rate of that type of particles at the
plume source
Q0 C0i = Qs Ci (rci );

(13)

where Q0 is the volumetric 8ow rate of suspension at the


source. And, combining Eqs. (11) and (13), we have
C0i
Cs i
=
:
Cs j
C0 j

(14)

Eqs. (12) and (14) show that at each height zf , the ratio
of the concentrations of particles of types i and j entering
the plume is equal to the ratio of the concentrations of
the same particle types in the plume at the source level.
Therefore, the ratio of concentrations of particle types i
and j is constant in the plume.
Conservation of the mass of particles of type i, between
the surface current and the 8oor leads to
Ci (rf ) =

Ci (rsi )rsi drsi


:
rf
drf

(15)

S. S. S. Cardoso, M. Zarrebini / Chemical Engineering Science 56 (2001) 47254736

where

Hence, using Eq. (5),


Cj (rsj )uj rsj drsj
Ci (rsi )ui rsi drsi
=
Ci (rf )
Cj (rf )

(16)

and
Ci (rf )
Ci (rsi )
=
:
Cj (rf ) Cj (rsj )

Q 0 C0 i
exp(1)
Qs

(25)

Qs = 65 ( 109 B0 )1=3 H 5=3 ;

(26)

Csi =
and

(17)

This is a very powerful result in that it allows us to calculate the sedimentation pro9le on the 8oor for each particle type j, given the pro9le for particle type i. Indeed,
combining Eqs. (3), (14) and (17) yields


Ci (rf ) C0i
2
2 uj ui
=
exp (rf bs )
 :
(18)
Cj (rf ) C0j
Qs

where B0 is the buoyancy 8ux of the plume at the source.


Using Eq. (22), the total mass 8ow of particles depositing
on the 8oor per unit radial distance for a dilute plume is
thus
F(rf ) = 2rf

The mass 8ow rate of particles of type j depositing on


the 8oor per unit radial distance is
Fj (rf ) = 2rf Cj (rf )uj :

(19)

Substituting Eq. (18) into Eq. (19) gives




C0j
2
2 ui uj
exp (rf bs )

Fj (rf ) = 2rf uj Ci (rf )
C0 i
Qs
(20)
or
Fj (rf ) = Fi (rf )



C0j uj
ui uj
exp (rf2 b2s )
 :
C0i ui
Qs

(21)

The total mass 8ow rate of particles depositing on the


8oor per unit radial distance is therefore


n

C0j uj
2
2 ui uj
exp (rf bs )
 :
F(rf ) = Fi (rf )
C0i ui
Qs
j=1
(22)
3.2. Dilute plumes in an in4nite environment
Zarrebini and Cardoso (2000) showed that if the concentration of particles in the source suspension is small,
such that
H de
1;
r 0 d z

4729

(23)

then the motion of the plume is controlled by the buoyancy due to salinity de9cit; here r is the reference density taken to be equal to the initial ambient density. In
this case, the mass 8ux of particles of type i depositing
on the 8oor is given by



Qs
ui
;
Fi (rf ) = 2rf ui Csi exp  rf2 b2s +
Qs
ui
(24)



uj
Csj uj exp (rf2 b2s )  1 :
Qs
j=1

n


(27)
3.3. Environment of 4nite lateral extent
In an environment of 9nite lateral extent, the entrainment into the plume causes the environmental liquid surrounding the plume to move downward with an approximately horizontally uniform velocity U (z). At the bottom
of the radially spreading surface current, the liquid moves
downward with velocity Us and hence particles of type i
settle from the current with vertical velocity Us + ui . A
mass balance of particles i in the surface current, taking
into account the radial decrease of volumetric 8ow rate,
yields


Ci = Csi

ui =Us
 2
u =U
Us
R r2 i s
2
2
1 (r bs )
= Csi 2
:
Qs
R b2s

(28)
The trajectory of a particle i leaving the surface current
is now described by
(ui + U )r
ui + U
dz
=
:
=
dr
ue
bw

(29)

Using Eq. (29), we may show that for two particles of


types i and j, leaving the surface current at radial positions
rsi and rsj , respectively, and entering the plume at the
same level zf or settling on the 8oor at radial position rf ,
the following relation holds:
(ui + Us )rsi drsi = (uj + Us )rsj drsj :

(30)

Then, conservation of the mass of particles i between the


surface current and the edge of the plume yields
Ci (zf )
Ci (rsi )
=
Cj (zf ) Cj (rsj )

(31)

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S. S. S. Cardoso, M. Zarrebini / Chemical Engineering Science 56 (2001) 47254736

Ci =Cj (rf ). The problem was therefore solved numerically using Eqs. (31) and (32) in the code developed by
Zarrebini and Cardoso (2000), with new loops to account
for a sequence of particle sizes.
In the next section, we present and compare experimental results with the theoretical predictions considered
above.
4. Results and discussion

Fig. 4. Theoretical predictions for the rate of deposition of sediment


in an environment of in9nite lateral extent.

and conservation of the mass of particles i between the


surface current and the 8oor leads to
Ci (rf )
Ci (rsi )
=
:
(32)
Cj (rf ) Cj (rsj )
Eqs. (31) and (32) show that the ratio of the concentrations of di5erent particles entering the plume, or
settling on the 8oor, is equal to that leaving the surface current. However, it is no longer possible to 9nd
an analytical relation for the particle trajectories, and
hence obtain analytical expressions for Ci =Cj (zf ) and

In this section, we present experimental and theoretical


results obtained using particles with the size distribution
shown in Fig. 2. The new experimental results illustrate
the e5ect of particle size on the deposition pattern. The
e5ects of buoyancy 8ux, particle concentration and tank
size on the sedimentation pattern from turbulent plumes
have been considered elsewhere (Zarrebini & Cardoso,
2000; Cardoso & Zarrebini, 2001).
Fig. 4 shows the theoretical predictions for the rate of
accumulation of sediment on the tank 8oor as a function
of radial distance, for an environment of in9nite lateral
extent. Each solid curve shown corresponds to a speci9c particle size. The larger particles deposit on the 8oor
closer to the plume source, whilst the settling of smaller
particles extends from the source to larger radial positions. As a result, the rates of deposition of large particles

Fig. 5. Particle 8ux at ground level as a function of particle diameter (in9nite environment), at (a) r = 3:4 cm, (b) r = 9:5 cm, (c) r = 17:6 cm
and (d) r = 29:8 cm.

S. S. S. Cardoso, M. Zarrebini / Chemical Engineering Science 56 (2001) 47254736

Fig. 6. Root mean square particle diameter in the deposit as a function


of radial position (in9nite environment).

present well de9ned maxima at relatively small radial


positions, whilst the rates of settling of small particles
are more uniform throughout the tank 8oor. The dashed
curve shows the total rate of accumulation of sediment
on the 8oor.
Fig. 5(a) (d) shows the theoretical predictions and
experimental results for the rate of sedimentation of particles of di5erent sizes at given radial positions. The agreement between the experimental results and the theoretical
predictions is excellent. At small radial positions, r = 3:4
and 9:5 cm, the 8ux of larger particles predominates over
the 8ux of smaller particles. However, further away from
the plume source, the rate of sedimentation of smaller
particles becomes more signi9cant. At r = 29:8 cm, the
8ux of smaller particles is larger than that of larger particles. Experimentally, we 9nd that no large particles are
present at this radial position, possibly owing to the low
accuracy of the measurements of very low particle concentrations with the Coulter counter.
Fig. 6 shows the root mean square particle diameter in
the deposit as a function of radial position. The root mean
square diameter was chosen because the Stokes settling
velocity of each particle is proportional to the square of
the diameter of the particle. As expected, there is a steady
decrease in the root mean square particle diameter with
increasing radial position. The agreement between the
theoretical prediction (solid line) and the experimental
measurements is good, except at positions further away
from the plume, where the concentration of particles is
very low. At such low particle concentrations, the measurements are not accurate.
Fig. 7 presents the total rate of deposition in an in9nite
environment as a function of radial distance. The solid
line represents the theoretical prediction taking into account the polydispersivity of particles. The dashed line
corresponds to the theoretical prediction for a monodisperse particle fraction with root mean square particle diameter equal to that of the polydispersed particles. The

4731

Fig. 7. E5ect of the polydispersivity of particle sizes on the total rate


of deposition in an environment of in9nite lateral extent.

Fig. 8. Comparison of the deposition patterns in environments of


9nite and in9nite lateral extents.

new model including the polydispersion of particles is


in better agreement with the experimental measurements.
This 9gure illustrates that the polydispersivity of particles
has a signi9cant e5ect on the total deposition pattern, particularly at larger radial positions. We note that at large
radial positions there is a noticeable di5erence between
the experimental results for our two nearly identical runs;
this di5erence is attributed to the low accuracy of the concentration measurements at low particle concentrations.
In Fig. 8, we show the e5ect of the lateral extent of the
tank on the rate of settling of particles of di5erent sizes.
In a 9nite environment, the downward advection of the
ambient 8uid increases the particle 8ux and the maximum
in the deposition rate lies closer to the source. This e5ect
is more pronounced for the smaller particles sizes. The
e5ect of the 9nite size of the tank on the total rate of
deposition is also shown. This e5ect, although already
signi9cant for the experimental conditions studied, will
be even more pronounced for larger buoyancy 8uxes at
the source of the plume (Zarrebini & Cardoso, 2000).
Fig. 9 presents the total rate of deposition in a 9nite environment as a function of radial distance. The solid line
represents the theoretical prediction taking into account

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S. S. S. Cardoso, M. Zarrebini / Chemical Engineering Science 56 (2001) 47254736


Table 2
Typical data for hexavalent chromium emissions from an exhaust
stack (Bonin et al., 1995; Bonin, 2000)
Exhaust stack
Height (m)
Diameter (m)
Exit velocity (m=s)
Exit temperature (K)
Particulate emission rate (mg=s)

Fig. 9. E5ect of the polydispersivity of particle sizes on the total rate


of deposition in an environment of 9nite lateral extent.

the polydispersivity of the particles. The dashed line corresponds to the theoretical prediction for a monodisperse
particle fraction with equivalent root mean square particle diameter. The predictions of the new model are in
good agreement with the experimental results. The simple
approach considering an average particle diameter overpredicts the particle 8ux just after the peak of deposition
and underpredicts it at larger radial positions.
5. Application of the model to the emission of
chromium particles from a commercial plating plant
We shall now consider the application of the model
developed in this paper to the discharge into the atmosphere of polydispersed chromium particles from an exhaust stack at a chromium plating plant.
Electroplating is the process of applying a metallic
coating to an object by passing an electric current through
an electrolyte. Hexavalent chromium baths are widely
used in industry to deposit chromium on metal objects.
The baths consist of chromic acid, sulphuric acid and
water. The chromic acid is the source of the hexavalent
chromium that deposits on the metal. The process evolves
hydrogen and oxygen gases that bubble to the surface of
the electrolyte. This results in the formation of a chromic
mist, which is exhausted through an abatement process,
including a cyclone separator and mesh pads, and then
released into the atmosphere.
Hexavalent chromium is a known carcinogen which,
when inhaled, can cause several adverse health e5ects including runny noses, nose bleeds, ulcers, abdominal pain
and vomiting (US EPA, 1998a,b). More details on the
health risks arising from exposure to chromium in the environment are given on the US EPAs integrated risk information system (IRIS). Reference concentration (RfC)
for chronic inhalation exposure for chromium particulates
and chromic acid mist are included. They are estimates
of the daily inhalation exposure of the human population
that is likely to be without an appreciable risk of harm-

15
0.5
2.5
301
1:8 102

ful e5ects during a lifetime. The RfCs for chromic acid


mists and hexavalent chromium particles are 8 106
and 1 104 mg=m3 , respectively (US EPA, 1998a).
Although the exhaust gases from a chromium plating
plant pass through an abatement process before being released into the atmosphere, particles less than 1 m in
diameter, are emitted at a typical concentration of 3:5
102 mg=m3 ; this concentration is much larger than the
RfCs indicated above. It is therefore important to have
a simple and easy to run model capable of predicting the
concentration levels of chromium particulates surrounding the industrial source. The concentration pro9les of
the di5erent particle sizes at ground level will indicate
which sizes are present in high proportions at given radial
positions. These are not necessarily the sizes present in
high proportions at the source, for we have seen that size
plays a role in the ultimate deposition pattern. Our analysis will indicate which particle sizes should be further
removed by an enhanced abatement process.
Bonin, Flower, Renzi, and Peng (1995) presented measurements of the size and concentration of chromium particles released from an electroplating facility in the United
States. Particle samples were taken at three locations in
the exhaust stream: electroplating bath surface, exit of the
cyclone separator and in the exhaust stack. Particle size
measurements were made with an Insitec particle counter,
sizer, and velocimeter, capable of measuring particles diameters from 0:3 to 25 m. In this paper, we use the data
of Bonin et al. (1995) to predict the deposition patterns
of chromium particles released into the atmosphere from
the exhaust stack (downstream of the abatement devices).
The emission data used are presented in Table 2.
Our model is directly applicable to incompressible 8uids. In the example above, the vertical extent of motion in
the atmosphere will be such that it is not possible to treat
air as an incompressible gas. However, the analysis may
still be applied to the atmosphere by replacing absolute
temperatures and densities for potential temperatures and
potential densities (Tritton, 1988). In a density strati9ed
environment, such as the atmosphere, the buoyancy 8ux
in the plume decreases with height and the plume eventually spreads out at the level at which the density in the
plume equals that in the atmosphere (the level of neutral
buoyancy). An equation for the height of rise of a plume
in a linearly strati9ed environment was originally derived

S. S. S. Cardoso, M. Zarrebini / Chemical Engineering Science 56 (2001) 47254736

Fig. 10. The distribution of particle sizes of chromium in the exhaust


stack.

4733

Fig. 11. Theoretical predictions for the total 8ux and concentration
of particles at ground level for a typical stack emission of chromium
particles from a plating plant.

by Morton, Taylor, and Turner (1956) from a momentum, buoyancy and mass balance; uncertainties about the
multiplying constant were later removed by direct experiment (Briggs, 1969). We con9ne our approach to a still
atmosphere, with a positive, constant gradient of potential
temperature in the vertical direction. The particle-laden
gas will rise to a 9nite height H given by (Turner, 1979)
H = 3:76B01=4 N 3=4 :

(33)

Here N is the buoyancy frequency, a measure of the


strength of the strati9cation, de9ned as

1=2 

1=2
1 d
dT=d z
N = g
= g
1+
;
(34)
 dz
Tr
where Tr is the absolute temperature at the source level
and is the adiabatic temperature gradient.
We shall consider a standard atmosphere, for which
Tr =288 K; =9:8 K=km and the rate of decrease of temperature with height is 6:5 K=km (Morton et al., 1956).
Thus, N = 0:02=s. We shall see that in the example under study, the buoyancy 8ux at the source is mainly due
to the di5erence between the source temperature and the
atmospheric temperature, as the particle concentration is
so small that its contribution to the density of the plume
is negligible. Hence,
B0 = g(T0 Tr )Q0 ;

(35)

where T0 is the source temperature and  = 1=Tr is the


thermal expansion coeIcient of air. Once the height of
rise in the atmosphere is calculated from Eq. (33), we
shall use the simpli9ed model in Section 3.2 and thus
neglect the e5ect of strati9cation on the plume behaviour.
This simple analysis will suIce to illustrate the behaviour
of the release in a still atmosphere.
Fig. 10 shows the particle size distribution of hexavalent chromium present in the exhaust stack investigated
by Bonin et al. (1995). The smallest particle size is 0:3 m
in diameter (the lower measurable limit of the probe used
by those authors) and the largest is 0:8 m. Particles with
diameters greater than 0:8 m are only present upstream
of the abatement devices.

Fig. 12. Deposition rates for di5erent particle sizes for a typical
chromium stack emission.

Eq. (33) predicts that the exhaust will rise to about


44 m above the source. At this level the 8ow rate in the
plume is approximately 31 m3 =s and the plume spreads
out radially forming a gravity current. Fig. 11 shows the
total rate of deposition and the concentration of chromium
particles at the ground level. There is a pronounced maximum in the rate of accumulation per unit radial distance
at approximately 800 m from the source. The maximum
concentration occurs near the source and is just below
6 104 mg=m3 . This value exceeds the RfC indicated
above and hence further abatement measures might be
considered. However, what is particle size range responsible for this relatively high concentration near the source?
We answer this question below.
Fig. 12 shows the deposition rates for the di5erent sizes
of chromium particles. The larger particles deposit on the
ground closer to the plume source, up to radial positions
of 1500 m, whilst the settling of smaller particles extends
from the source to radii of 4000 m. As expected, the
rates of deposition of large particles exhibit well de9ned
maxima at positions less than 600 m from the source.
Fig. 13 shows the concentration pro9le of each particle
size at ground level. Near the source, particles of diameter

4734

S. S. S. Cardoso, M. Zarrebini / Chemical Engineering Science 56 (2001) 47254736

Fig. 13. Ground concentration pro9les for di5erent particle sizes for
a typical chromium stack emission.

motion. This assumption is not very restrictive and will


be valid in many problems involving industrial stack
emissions (Zarrebini & Cardoso, 2000). On the other
hand, the e5ect of wind on the dispersal of particles can
be important (Woods et al., 1995); in the presence of
strong wind, the plume will be carried away and will
have su5ered more entrainment by the time a given
height is reached (Morton et al., 1956). We may expect
the transport of particles by wind to become signi9cant
when the wind speed is of the same order or larger
than the radial in8ow driven by entrainment into the
turbulent plume. In our chromium emission example,
the entrainment velocity at the edge of the plume, near
the spreading level, is approximately 0:3 m=s. Therefore, the results presented above are only valid for an
atmosphere with very small wind speeds. This assumption becomes less restrictive as the buoyancy 8ux of the
plume increases due to a temperature increase and=or a
8ow rate increase (see Eq. (35)).
6. Conclusions

Fig. 14. Cumulative distribution of particle sizes at ground level, near


the source, for a typical chromium stack emission.

0:41 m are present in larger concentrations than any


other size, but at larger radial positions the concentration
of smaller particles becomes signi9cant.
Fig. 14 illustrates the cumulative distribution of particle
sizes at ground level, near the source. We may conclude
that to reduce the total concentration at this radial position
to the RfC of 1 104 mg=m3 indicated above, particles
of diameter greater than 0:40 m should be removed by
further abatement processes upstream from the exhaust.
This removal will ensure that the total concentration of
chromium is below the RfC at all other radial positions.
As mentioned before, our experiments and model ignore the e5ects of both particleparticle interactions and
wind on the particle sedimentation patterns. As a 9nal
note, it is instructive to discuss here the conditions under
which our simpli9ed analysis is valid. Particleparticle
interactions become important for particle concentrations larger than approximately 0:03% (v : v) (Batchelor,
1982; Huppert et al., 1991). In the chromium emission
example given above, the particle concentration at the
plume spreading level is approximately 1011 % (v : v)
and hence a given particle is so distant from its neighbours that its motion is determined solely by the 8uid

We have presented analytical and numerical models for


the dynamics and deposition patterns of radially spreading gravity currents generated by axisymmetric turbulent
plumes. Our models take into account the settling of particles of di5erent sizes and=or densities. For simplicity,
we describe here the particles with large Stokes settling
velocities as large particles and the particles with smaller
Stokes velocities as small particles.
A hierarchy of models was developed for increasingly
complex situations. In the limit of dilute plumes, a simple analytical expression for the sedimentation pro9le on
the ground for each particle size was derived. In the case
of sedimentation in an environment of in9nite lateral extent, we show that we can calculate the sedimentation
pro9le on the 8oor for any particle type j, given the pro9le for particle type i. This analytical 9nding was then
used in the numerical code to model the settling of polydispersed particles. Finally, we considered the sedimentation of polydispersed particles in a 9nite environment.
This situation is more complex and we showed that it
requires full numerical solution.
Our theoretical predictions for the deposition patterns
on the 8oor were successfully compared with data from
laboratory experiments. The large particles deposit on
the 8oor closer to the plume source, whilst the settling
of small particles extends from the source to larger radial positions. At small radial positions, the 8ux of large
particles predominates over the 8ux of smaller particles.
However, further away from the plume source, the rate
of sedimentation of smaller particles becomes more signi9cant. At suIciently large radial positions, the 8ux of
smaller particles is larger than that of larger particles.
We 9nd that the root mean square particle diameter in

S. S. S. Cardoso, M. Zarrebini / Chemical Engineering Science 56 (2001) 47254736

the deposit decreases steadily with increasing radial position.


We show that the e5ect of the polydispersivity of particles on the total deposition pattern is signi9cant, particularly at larger radial positions. The simple approach
considering an equivalent root mean square particle diameter overpredicts the particle 8ux just after the peak of
deposition and underpredicts it at larger radial positions.
In a 9nite environment, the downward advection of the
ambient 8uid increases the particle 8ux and the maximum in the deposition rate lies closer to the source. We
show that this e5ect is more pronounced for the smaller
particles sizes. The e5ect of the 9nite size of the tank on
the total rate of deposition is also more pronounced for
larger buoyancy 8uxes at the source of the plume.
We applied our new model to estimate the deposition
patterns of chromium particles exhausted from a stack at a
chromium plating plant in a still atmosphere. It was found
that chromium particles with diameters less than 0:40 m
are transported to distances up to 4000 m from the source,
at ground level. The maximum ground concentration of
chromium particles for an emission with total particulate
concentration 3:5 102 mg=m3 is approximately 6
104 mg=m3 and occurs near the source. To reduce this
concentration to a magnitude below the RfC indicated by
the US EPA, we showed that particles of diameter greater
than 0:40 m should be removed by further abatement
processes upstream from the exhaust.
Notation
b
bs
B0
C0
C0i
Ci (r)
Ci (zf )
Cs i
di
fi
Fi (rf )
g
H
N
Q0

radius of the plume at height z; cm


radius of the plume at the free surface, cm
buoyancy 8ux in the plume at the source (at
z = 0); cm4 =s3
concentration of particles at the source (at
z = 0); g=cm3
concentration of particles of type i at the
source (at z = 0); g=cm3
concentration of particles of type i at radial
position r; g=cm3
concentration of particles of type i at the edge
of the plume at height zf ; g=cm3
concentration of particles of type i in the
plume at bs ; g=cm3
diameter of particle type i; m
mass fraction of particles of type i
mass 8ow rate of particles of type i depositing
along the 8oor at rf per unit radial distance,
g=cm s
gravitational acceleration, cm=s2
depth of environmental 8uid, cm
buoyancy frequency, s1
volumetric 8ow rate of suspension at the
source, cm3 =s

Qs
r ci
rf
rs
R
T0
Tr
ui
ue
Us
U (z)
w
z; zf

4735

volumetric 8ow rate of the plume at the free


surface, cm3 =s
critical radius for particle of type i, cm
radial position along the 8oor, cm
radial position along the surface current, cm
equivalent radius of the environment, cm
source temperature, K
temperature in the environment at the source
level, K
Stokes velocity of an isolated particle of type
i, cm=s
radial inward velocity of the environmental
8uid, cm=s
downward velocity in the environment at the
bottom of the surface current, cm=s
downward velocity in the environment,
cm=s
velocity of the plume at height z, cm=s
height above the source, cm

Greek letters



0
e
p
r

entrainment constant
thermal expansion coeIcient of air, 1=K
viscosity of water, g=cm s
density of the suspension, g=cm3
density of water, g=cm3
particle density, g=cm3
reference density taken to be equal to the
initial ambient density, g=cm3
adiabatic temperature gradient, K=km

Appendix Conservation of particles between the surface


current and the edge of the plume
In this appendix we derive Eq. (6). Consider the
schematic in Fig. 15. A particle of type i leaves the
surface current with vertical velocity ui and is drawn
towards the plume with radial velocity ue . At the edge

Fig. 15. Sketch of particle motion below the surface current.

4736

S. S. S. Cardoso, M. Zarrebini / Chemical Engineering Science 56 (2001) 47254736

of the plume, the velocity of the particle is therefore u =


u i + u e .
Consider now an annulus of width drsi at the lower
boundary of the surface current. All particles settling
within this annulus will, at the edge of the plume, move
with velocity u through an annulus of width ds. Hence,
conservation of particles of type i between the surface
current and the edge of the plume is given by
Ci (rsi )ui 2rsi drsi = Ci (zf )u2b ds:
From geometrical considerations (see Fig. 15)
ue
u=
cos i

(A.1)
(A.2)

and
ds =

d zf
;
cos i

(A.3)

where i = arctan (ui =ue ). Substituting Eqs. (A.2) and


(A.3) into Eq. (A.1), leads to
Ci (rsi ) ui rsi
drsi
cos2 i
:
(A.4)
Ci (zf ) =
ue b
d zf
But from Eq. (4), at the edge of the plume,
bw
:
(A.5)
ue =
b
Hence the concentration of particles of type i at the edge
of the plume at height zf is given by
Ci (rsi ) ui rsi
drs
cos2 i i :
(A.6)
Ci (zf ) =
bw
d zf
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