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filter cakes of very low permeability and hence be able to come into close contact and
low filtration rates. Again, aggregation can give aggregation will be prevented. Such particles
a marked improvement. are said to be colloidally stable, in the sense that
In this chapter we shall review the more they remain dispersed over long times. The
important aspects of coagulation/flocculation most common reason for colloid stability is the
and depth filtration processes. No further fact that most particles in water are charged
discussion of membrane filtration will be and hence repel each other electrically. Similar
given. There is a large and growing body of considerations apply to the attachment of
literature on this subject (see Mallevialle et al., particles to filter media.
1996). If there is only limited repulsion between
The subject of colloid interactions is very particles, or if there is an attraction, then
important in both coagulation and filtration, aggregation can occur when particles collide
since attachment of particles to each other or to and the suspension is said to be unstable.
filter media is essential. The important types of interaction between
particles in water are:
that they only come into play when particles have much higher values. An expression of
are nearly in contact and they have little similar form to equation (1), but with a factor 1/
influence over the transport of particles in 6, applies to the interaction between a spherical
coagulation or filtration processes. particle and a flat surface, which is a reasonable
Furthermore, the magnitude of these inter- model for a colloidal particle approaching the
actions is roughly proportional to the particle surface of a much larger filter grain.
size, which has very important implications in Equation (1) applies only to very close
practice. Other forces, such as gravity and approach, where d ,, a, but the interaction
hydrodynamic drag, have different depen- is often negligible at larger distances. The
dence on particle size. Thus the gravitational negative sign implies, by convention, an
attraction on a particle depends on the mass of attraction. The energy is proportional to par-
the particle and is hence proportional to the ticle size, as mentioned above, and depends
cube of the size. The drag force on a particle in a inversely on separation distance, becoming
flowing fluid is dependent on the square of the very large as particles come into contact.
particle size. It follows that these ‘external’ van der Waals attraction is essential in
forces become very important for larger par- coagulation and filtration, and we have to be
ticles and can be much larger than the aware of its presence. However, there is no
‘colloidal’ interactions listed above. Conver- realistic method by which the attraction can be
sely, colloidal interactions usually predominate significantly altered in practical systems and we
for smaller particles, typically of the order of a shall not go any further into theoretical aspects.
few micrometres or less. This is the reason for
the term ‘colloidal interactions’.
Although all of the interactions 1 –5 above 2.3 Electrical interaction
can be important in practice, we shall here Particles in aqueous suspensions usually carry
concentrate on van der Waals attraction and a surface charge. This may arise for several
electrical repulsion, since these form the basis reasons, including ionization of surface groups
of the DLVO theory of colloid stability, which and adsorption of certain ions. Biological
will be reviewed briefly below. Polymer brid- surfaces are usually charged through acid–
ging will be discussed separately, under the base interactions, such as the ionization of
heading of Polymeric flocculants. carboxylic acid groups and the protonation of
amine groups. Oxide surfaces are charged by
2.2 van der Waals attraction virtue of protonation/deprotonation of surface
hydroxyl groups. In these cases the surface
The universal attractive forces between charge depends greatly on the pH of the
atoms and molecules, originally postulated solution, with positive values at low pH and
by van der Waals, have long been known to negative charge at high pH. There is a
act between all materials (e.g. Israelachvili, characteristic pH value at which the surface
1991). Between equal spherical particles of charge is zero, with equal numbers of positive
radius a, separated by a distance d, the and negative surface groups. This is the
van der Waals interaction energy, VA, is given point of zero charge ( pzc), which is a very
approximately by: important surface characteristic. The charging
of a hypothetical biological surface is shown
Aa
VA ¼ 2 ð1Þ schematically in Fig. 38.2.
12d
Whatever the origin of surface charge, it must
where A is the Hamaker constant, which depends be associated with an appropriate number of
on the properties of the particles and water. For oppositely charged ions (counterions) in sol-
aqueous suspensions, this ranges between ution, so that overall the system has no
about 5 and 100 £ 10221 J. The lower values net charge. A surface charge, together with
are typical of biological particles such as counterions in solution gives an electrical double
bacteria and algae. Dense mineral particles layer, the structure of which is very important in
636 Coagulation and filtration
where
x is the distance from the Stern plane and
k is a parameter which determines the rate
of decrease of potential with distance.
k is known as the Debye-Hückel parameter and
has a great influence on colloid interactions. It
has the dimensions of reciprocal length (m21)
and depends on the valence and concentration
of ions present in solution. For aqueous
solutions at 258C, it is given by:
qffiffiffiffiffiffi
X 2
k ¼ 2:32 £ 109 ci zi ð3Þ
Fig. 38.2 Surface charge development by ionization The distance 1/k, effectively the ‘thickness’
of surface groups. The point of zero charge (pzc) of the double layer, ranges from around 1 to
occurs at a characteristic value. 100 nm in typical salt solutions. In 1024 M NaCl
the value is about 30 nm. In a natural water
with a high level of dissolved salts the distance
governing the interaction between charged can be much lower, for instance in River
particles. A simple model of the double layer Thames water the value is about 4 nm.
is shown in Fig. 38.3. This shows the variation Experimentally, charged particles can be
of electric potential, c, with distance from investigated by a range of electrokinetic tech-
the surface. At the surface the value is c0 (the niques, such as microelectrophoresis, in which
surface potential). For a short distance from the the velocity of a particle in an electric field is
surface (of the order of the size of a hydrated determined. This gives a value of electric
ion), the potential drops quite rapidly to a value potential at the plane of shear, or slipping
cd (the Stern potential). (The region close to the plane, between the particle and the fluid: the
surface is known as the Stern layer.) Further from zeta potential, z. The slipping plane is generally
the surface, the potential decays in an approxi- assumed to be close to the Stern plane, so
mately exponential manner, according to: that the zeta potential can be used instead of
the Stern potential (which is not directly
c ¼ cd expð2kxÞ ð2Þ measurable).
When two charged particles approach each
other their diffuse layers overlap and this leads
to a repulsion or attraction, depending on the
signs of charge. For similar spherical particles,
radius a, there is a repulsion and the interaction
energy is given approximately by:
where
e is the electron charge and
d is the separation distance between the
particles.
The magnitude of the repulsion depends
greatly on the zeta potential, but the range of
interaction is determined by the parameter k.
For the case of a sphere, radius a, approach-
Fig. 38.3 A simple model of the electrical double ing a flat surface (representing a particle and
layer. the surface of a filter grain), the corresponding
2Colloidal interactions and colloid stability 637
expression is: From equations (1) and (4), the total inter-
action energy between similar particles, radius
4peaz1 z2 expð2kdÞ ð5Þ a, separated by a distance d is:
Fig. 38.4 Potential energy diagram for the interaction of spherical colloidal particles, diameter 1 mm and zeta
potential 25 mV. The Hamaker constant is assumed to be 2 kT and the medium is an aqueous solution of 1-1
electrolyte at a concentration of 50 mM.
638 Coagulation and filtration
also plays an important role. The detailed parts of the same polymer chain can adsorb on
mode of action of PAC and similar coagulants different particles, leading to polymer bridging
has yet to be elucidated. as a means of binding particles together. This
Hydrolysing coagulants are also effective in is illustrated schematically in Fig. 38.6a.
removing dissolved organic matter, such as Polymer bridging is now recognized as a
humic substances, from water. The mechanism very important mechanism in practice. It is
may be charge neutralization or adsorption on most effective with linear, high molecular
precipitated hydroxide (Bose and Reckhow, weight (several millions) polymers. Aggrega-
1998). tion brought about in this way is often known
as flocculation, in order to distinguish it from
coagulation caused by salts. However, this
3.2 Polymeric flocculants distinction is not universally used and the
terms are often used interchangeably.
Organic polymers, both natural and synthetic, Many types of polymer are effective as
can adsorb on a wide range of surfaces and flocculants, but only relatively few are used
have a great effect on particle interactions and
commercially. Polymers may be non-ionic,
hence on colloid stability (see Gregory, 1996).
anionic or cationic, and if there are ionic
Polymers may give enhanced stability, for
groups, the products are known as polyelec-
instance by steric stabilization, or may promote
trolytes. By far the most important are those
aggregation of particles. We shall only be
based on polyacrylamide, which can be pro-
concerned with the latter aspect here.
duced with very high molecular weights (20
Extracellular polymers, such as polysacchar-
million or more). Nominally, polyacrylamide is
ides, are produced and exuded by many
non-ionic, but controlled hydrolysis of amide
bacteria and play a large part in bioflocculation,
groups gives carboxylic acid groups, which can
for instance in the activated sludge process
ionize at around neutral pH and higher to give
(Morgan et al., 1990). Also, natural polymers,
anionic sites. Cationic polyelectrolytes can be
extracted from certain plant products
synthesized by copolymerization of acryl-
(especially nuts and seeds) have been found
amide with suitable cationic monomers. This
to act as flocculants (e.g. Muyibi and Evison,
1995). However, most commercial applications is a common route to commercial cationic
use synthetic polymers. polyelectrolytes of high molecular weight.
The most important characteristics of poly-
meric flocculants are the molecular weight and,
3.2.1 Polymer bridging in the case of polyelectrolytes, the charge
Polymers of high molecular weight may density.
adsorb on surfaces from solutions in such a For effective bridging flocculation polymers
way that parts of the polymer chain extend must adsorb on particles to give only partial
into the solution. This gives the possibility that surface coverage, with segments extending
in the formation of aggregates. The fraction of This expression is based on the assumption
successful collisions is known as the collision of spherical particles, radius a, in a laminar
efficiency, a. When there is significant repulsion shear field with a uniform shear rate G. The
between particles the collision efficiency will be particle number concentration is n. These are
very low, but when repulsion has been elimi- highly restrictive conditions, which would not
nated, by suitable chemical treatment, a can apply in practical coagulation processes.
approach unity, so that nearly every collision Nevertheless, this approach leads to a simple
results in attachment. result that gives an idea of the important
Detailed accounts of this subject can be parameters.
found elsewhere (e.g. Elimelech et al., 1995). No practical coagulation processes are car-
Only a brief and selective treatment can be ried out under laminar conditions; turbulent
given here. flow is almost always involved. In this case an
The frequency of collisions between par- effective shear rate can be defined, in terms of
ticles of type i and j depends on the product of the power input to the vessel (such as a stirred
their concentrations, the collision efficiency and tank), P, the volume of suspension, V and the
a rate coefficient, kij, which depends on the mode viscosity, m. The result due to Camp and Stein
of transport of particles (see below): (1943) is:
sffiffiffiffiffiffi
Jij ¼ akij ni nj ð8Þ ¼ P
G ð10Þ
mV
where
Jij is the number of collisions occurring The effective shear rate can then be inserted
between i and j particles and in the appropriate rate expression instead of
ni and nj are their number concentrations. the laminar shear rate. Although this approach
The rate coefficient depends on the particle is undoubtedly oversimplified, it gives a result
sizes and on certain physical factors. Relative which is quite similar to that from a more
motion between particles, leading to collisions, rigorous approach.
may caused by: Equation (9) shows that the rate of coagu-
lation depends on the square of the particle
1. Brownian motion (perikinetic coagulation) concentration, as expected for a second-order
2. Fluid motion (orthokinetic coagulation) rate process. There is also a very strong
3. Differential settling. dependence on particle size, which explains
why orthokinetic coagulation becomes much
Of these, Brownian motion is important only more important for larger particles.
for quite small particles and is not usually able The form of equation (9) is such that a
to produce the large flocs that are required in simple transformation gives the result in terms
most practical applications. Usually, some form of the volume fraction of particles, which is
of agitation, such as in stirred tanks or flow- simply the total volume of particles per unit
through reactors is applied, causing particle volume of suspension. For equal spherical
collisions. With a range of particle sizes, particles this is simply given by:
different settling rates cause relative motion
4
and hence collisions. This can become signifi- f¼ pa3 n ð11Þ
cant as flocs grow quite large. 3
In the most important case of orthokinetic If it is assumed that the volume of particles
collisions, the rate of coagulation can be written remains constant during the coagulation
in terms of the rate of reduction of particle process, and the collision efficiency, a ¼ 1
number concentration, since each successful (i.e. for a fully-destabilized suspension), then
collision results in the net loss of one particle: equations (9) and (11) lead to:
dn 16 2 n 24Gft
2 ¼ an Ga3 ð9Þ ¼ exp ð12Þ
dt 3 n0 p
644 Coagulation and filtration
Although this expression is based on a growth will be faster, but the limiting floc size
number of simplifying assumptions, it is very will be less. There is, as yet, no quantitative
important in showing the main parameters theory of floc strength, but a common empirical
influencing the rate of orthokinetic coagulation. approach is to relate the limiting floc size to the
The term n/n0 represents the loss of particles by effective shear rate (Mühle, 1993):
coagulation and the reciprocal, n0/n can be dmax ¼ CG2g ð13Þ
regarded as the average floc size at time t.
(Effectively, it is the average number of primary where dmax is the maximum floc size for a
particles per floc.) shear rate G and C and g are empirical
Equation (12) shows that the extent of constants. Reported values of g are in the
coagulation increases with the shear rate G, range 0.2 – 0.5.
the volume fraction of particles and the time t. Another factor which greatly affects coagu-
The product Gt is a dimensionless number, lation rate is the solids concentration, or the
sometimes called the Camp number. In water volume fraction, f. Equation (12) shows that
treatment plants, flocculation units are often this parameter is of equal importance to G and
designed to have a Camp number in the region t. In practical units it is of great advantage to
of 30 000 –50 000. In principle, the same degree maintain a zone of high solids concentration to
of coagulation should be attained for any exploit this effect. Recycling of flocs (as in
combination of G and t, provided that the activated sludge units) or establishing a ‘floc
product remains constant. A high shear rate for blanket’ (as in upflow clarifiers) are effective
a short time or a low shear rate for a means of achieving high solids concentrations.
correspondingly longer time should give the The use of hydrolysing coagulants under
same result. However, this ignores the break- ‘sweep floc’ conditions also increases the
effective volume fraction by the formation of
up of flocs, which becomes very important at
a voluminous hydroxide precipitate.
high shear rates. Also, for hydrodynamic
reasons, the effective collision efficiency at
high shear rates can become quite low 3.4 Properties of flocs
(van de Ven and Mason, 1977).
The main purpose of carrying out a coagu-
The growth of flocs, for different shear rates lation process is to achieve more efficient
is shown schematically in Fig. 38.8. At low solid –liquid separation. Certain floc proper-
shear rate, the coagulation rate is low, but the ties, notably floc density, can greatly influence
flocs can eventually reach quite large sizes. By separation processes.
contrast, at high shear rates, the initial floc
3.4.1 Fractal nature of flocs
Aggregates or flocs are now recognized
as self-similar, fractal objects (Meakin, 1988).
Self-similarity simply means that an aggregate
appears to have a similar structure, indepen-
dent of the scale of observation. Fractal
character implies that the mass of an aggregate
(or the number of primary particles within it)
scales as the size raised to some power, dF
(or the fractal dimension).
M / Ld F ð14Þ
Of course, a solid, three-dimensional object
has a mass which depends on the cube of its
Fig. 38.8 Growth of flocs under (a) high shear and size. Aggregates effectively have fractional
(b) low shear conditions. dimensions; hence the term ‘fractal’.
3Coagulation and flocculation 645
3.5 Practical aspects have a smaller size and hence will experience
less fluid drag. This gives more rapid sedi-
Coagulation/flocculation processes are usually mentation and more permeable filter cakes.
carried out in some form of flow-through unit, The addition of small particles to existing
such as stirred tanks or upflow clarifiers. The flocs promotes higher floc density and this
purpose is to encourage particle collision by explains why high floc recirculation or floc
induced fluid motion (i.e. orthokinetic coagu- blanket clarifiers tend to give quite dense
lation). It is necessary to ensure that the flocs. An extreme case is the so-called pellet
particles are adequately destabilized by the flocculation process (e.g. Yusa and Igarishi, C,
addition of suitable coagulants, such as metal 1984) where compact flocs of very high density
salts or polymers. can be produced, without the usual decrease of
Additives need to be thoroughly and density with increasing floc size. (This implies
rapidly mixed throughout the suspension and a fractal dimension close to 3.) The fundamen-
this is achieved by a rapid mix unit at the point tals of this process are not yet fully understood,
of coagulant dosing. Only a short time of rapid but it depends on a zone of high solids content
mix (a few seconds) is needed and the dosed with some mechanical agitation (to promote
suspension then flows to the flocculation unit, restructuring of flocs) and usually involves the
where the agitation is gentler, allowing flocs to use of high molecular weight polymers to give
form. The energy input to the flocculator, or the strong bonding.
effective shear (see equation 12) determines the
rate of flocculation, but too high a value will
result in floc breakage. A compromise between 4 FILTRATION
rapid floc growth and the avoidance of high
shear rates is the process known as taper 4.1 Introduction
flocculation. This involves a series of stirred
tanks or compartments with decreasing power Filtration through granular media has been
input. In the early stages, high shear causes practised since Roman times. It is a physical
rapid growth of small flocs, which are then process to remove suspended particles from
allowed to grow larger in the subsequent water. The suspended particles may be inor-
stages, as the shear rate is reduced. ganic or organic, including microbes. In the
The most important factors influencing the light of problems with Cryptosporidium and the
rate of floc growth are the shear rate and the pressure to improve the bacterial quality of
solids content. A high solids content can be treated water, a great deal of attention has been
achieved by recirculating flocculated material paid to filtration processes, especially optimiz-
or in a form of clarifier, where incoming ation through the correct choice of operational
particles pass through a layer of previously- procedures.
formed flocs (a floc blanket). There are three main types of granular
The density of flocs is an extremely import- media filter used in water treatment:
ant property (Gregory, 1997) which determines
the rate of floc growth. The larger the floc, for a † slow sand filters
given mass, the greater the rate of collision † rapid gravity filters
with other flocs. For similar reasons, the † pressure filters.
capture of flocs by filter grains and by bubbles
in flotation processes is more effective with
flocs of lower density. However, there are other
4.2 Slow sand filters
separation processes, notably sedimentation As the name implies, slow sand filters
and cake filtration (such as in sludge dewater- are operated at low filtration rates, typically
ing), where flocs of high density are preferred. 0.1 – 1 m/h. (Note: filtration rate is usually
For a given mass, a higher density floc will expressed as approach velocity, e.g. m/h, which
4Filtration 647
is equivalent to a volume flow rate per unit low, the sedimentation step can be omitted
area, m3/m2h.) Slow sand filters use rather fine and the process is then known as direct
sand (less than 0.5 mm) and generally give the filtration.
best removal performance of all granular Granular media in rapid filters typically
media filters. This is only partly due to the have grain sizes in the range 0.5 – 2 mm and the
low filtration rate and small filter grains, since pores are of the same order of size. Particles to
in many cases there is significant biological be removed are usually very much smaller
action, restricted to a fairly thin layer at the than the pores and so straining is not a
surface – the Schmutzdecke. Aerobic bacteria in significant removal mechanism. There are two
the top few centimetres of sand produce essential aspects of particle removal in gran-
extracellular polymers which form an adhesive ular filters:
network, giving enhanced removal of fine
particles. It is likely that microbes captured in † Particle transport to filter grains
the schmutzdecke are subject to predation by † Attachment of particles to grain surfaces
other organisms which colonize this layer. In or to existing deposits.
most cases slow sand filters are operated
without prior chemical treatment or coa- These steps together result in particle capture by
gulation. They are cleaned periodically by a filter grain (often called a collector in the
scraping off the top 2 – 3 cm of sand, which is fundamental filtration literature).
washed and returned to the filter. Attachment is governed by colloid inter-
The disadvantages of slow sand filtration actions, which have been discussed earlier. If
include the large land area required to give there is significant repulsion between particles
high volumetric production and the incon- and filter grains then essentially no removal
venient cleaning method. can occur. In most cases coagulant is added
We shall now restrict attention to rapid before filtration, so that particles usually have
filtration methods, which rely predominantly quite a low charge and there would be little
electrical repulsion. In that case practically all
on physical removal mechanisms. There is
encounters between particles and filter grains
no fundamental difference in principle
(or ‘collectors’) would result in attachment and
between the action of rapid gravity and
the collision efficiency would be close to 1. If
pressure filters. The former is operated by
this is not the case, then only a fraction of
gravity flow and the latter under applied
collisions would be effective and the filtration
pressure in closed vessels.
efficiency would be reduced.
In discussing transport mechanisms it is
convenient to assume that there is no repulsion
4.3 Rapid filtration (a ¼ 1). Another important point is that colloid
interactions are of rather short range (typically
Rapid gravity filtration developed from slow below 0.1 mm and hence less than the size of
sand filtration in response to requirements for most particles). This means that the transport of
greater volumetric production from less land a particle from the flowing water in a filter pore
area. By using coarser media than for slow to the surface of a filter grain is almost entirely
sand filters, depth penetration of deposits is unaffected by colloid forces. Although
possible, thereby using the whole bed depth. van der Waals attraction may be vital to ensure
Filtration rates are usually in the range 5– particle attachment, it is of much too short a
30 m/h. In conventional operation rapid fil- range to influence the transport step. A particle
tration is preceded by coagulation/floccula- would have to be practically in contact with
tion and sedimentation, which greatly reduces a grain for the attraction to be felt. This
the load on the filters. However, in cases justifies treating transport and attachment
where the suspended particle concentration is separately.
648 Coagulation and filtration
Cleaning mechanisms. When a filter is being flow rates for a given medium a phenomenon
backwashed, the mechanisms that detach known as collapse-pulsing (Amirtharajah, 1993)
deposits and get the filter grains clean are: is observed. This corresponds to the onset of
three-phase fluidization.
† fluid shear forces What this means in practice is that fluidized
† grain collisions bed conditions are achieved for a much lower
† abrasion between grains water rate – typically less than 0.5 vmf. Flow
† forces associated with the air/water rates when a water only wash is used are
interface. greater than vmf. In addition, during collapse-
pulsing there is a very high degree of bed
Research has shown that water-only backwash agitation, as pockets of air form and collapse
is a weak cleaning process as grain collisions within the media. This ensures that deposits
are minimal. It is more effective to include air are detached from the grain surfaces and can
flow in the cleaning process. be particularly good for removal of biofilms.
to be carefully selected; we need to maximize † increased chemical dosing (e.g. during final
cleaning without causing too much attrition of stage of backwash)
the media. † backwash optimization.
the whole bed depth. However, as discussed fectants at normal dosages, so it is essential that
above, when a filter is backwashed a single they are removed physically in water treatment
graded medium will stratify so that finer grains processes.
are at the top and coarser grains at the bottom The usual method of monitoring filtered
of the bed, i.e. the opposite of what is required water is by measuring turbidity. Current stan-
for a gravity or downward flow filter. dards for drinking water turbidity are around 1
The idea behind dual and triple media filters NTU (a conventional turbidity unit), but more
is that we can achieve a progressively finer stringent standards may be applied – perhaps
filter by having finer, denser media below down to 0.1 NTU. Such low levels are approach-
coarser, heavier media. The difference in ing the limits of detection of commercial
densities of the media should ensure that the turbidity meters, yet may still correspond to
finer material stays at the bottom during and particle concentrations of several hundred per
after backwashing. ml. Furthermore, turbidity is a measure of light
Dual media filters usually consist of a layer scattered by the water sample and this is not a
of coarser anthracite above a layer of finer sand. sensitive measure of particles much larger than
Triple media filters consist of anthracite, sand the light wavelength, such as Cryptosporidium
and then an even finer grained layer of garnet. oocysts.
Other configurations of media have appeared It has become quite common to apply more
around the world, e.g. a triple media filter sensitive techniques, such as particle counting,
consisting of granular activated carbon (GAC) to the monitoring of filtered water quality
above German anthracite with a layer of fine (Gregory, 1998). Typical particle counters can
sand at the bottom. resolve particles down to about 1– 2 mm in size.
These methods can give an earlier indication of
particle breakthrough than conventional tur-
4.5.4 Backwashing of dual and triple bidity monitoring.
media filters Even a simple visual inspection can be
Dual and triple media filters are usually helpful, particularly of the backwash and the
designed so that they remain stratified after filter bed surface where mudballs may be
backwashing. It is relatively easy to maintain evident.
stratification between anthracite and sand, for
the size ranges typically employed, however,
mixing between the sand and fine garnet layers REFERENCES
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This may not actually be detrimental to filter Amirtharajah, A. (1993). Optimum backwashing of filters
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