The Modelling of Coalescence Processes in Fluid-Liquid Dispersions: A Review of Current Understanding
The Modelling of Coalescence Processes in Fluid-Liquid Dispersions: A Review of Current Understanding
The Modelling of Coalescence Processes in Fluid-Liquid Dispersions: A Review of Current Understanding
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Chemical Engineering Research and Design
Published: 01/01/1991
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":he re~iew addre~ .curren~ uoderstandin~ of the. p.rocesses of collision and coalescence in pure gas-Iiquid and liquid-liquid
~lsperslOns. Attentton IS restncted to f1ow-dnven collisIons, apart from briefreference to related
gravity-driven pbenomena at free-
mterfaces. Plane-film an~ full numerical solulions of drainage are compared in Ihe immobile, parlialJy-mobile and fully-mobile
cases aod related expressIOns developed for Ihe coalescence probabilily. Fioally, tbe perspeclives and prnblems in"olved in Ihe use
of such expressions are examined, in conjunction with flow simulation codes for the mathematic.al modelling of particle-size
evolution in dispersed f1ows.
with the corresponding values of k are given above lor F-61tpR(YR). (2)
three important flow types (Tabie I). A typical collision duration-the time spent by the
[n realit . ev n at separations comparable with the particles in close proximity-would be expected lo be
particIe iz. particIe trajectories deviate significantly given by
from the streamlines ofthe basic flow. The first reason for
1;-R/(YR)-(Y)-I. (3)
this is that each particIe disturbs the flow in its vicinity. [n
i c u. imple shear for example the streamline which, at Equations (2) and (3) are confirmed by Batchelor and
infinity. is on lin with the centre of a rigid particIe Green's results, which indicate that provided the particles
a tuall. pa se ir at a distance ofsome 15% ofthe particIe are close, F depends only on the inclination of their axes
mdius ( ee. for exarnple. Batchelor and Greens). This and not on their exact separation. This confinns the
mans rhar a maller particle cannot approach c10sely expectation, implicit in the internal/external spli t, thal Fi
unies it radius i at least 15% of that of the larger. [n to the first approximation independent of the details of
\;e\\, of uch powerful h drodynamic interactions. an the internal flow including presumably any interfacial
,tension f equation (I) to the unequal-particle case is of deformation, provided the region concerned is Inueh
litlle value. dded to the preceding effect is the fact that smaller than the particIe radius (a~R: Figure I). The
ani Ie _ do n t perfecti)' folio the flow produced by exact interaction time in a given case depends on the
pani Ie I. a a r uit both of inertial effects (important incidence of the particles.
only if Red = pdc 11 ~ I) and of the pressure generated by The particles of interest in the present context are of
:<pul ion ofthe intervening liquid. The latter effect can be
\'ie\\ed as pan of film drainage. Inertial effects can either
course fluid rather than solid and F and 'j
will then in
addition be a weak function of Pd/JI. No informati n on
in rease or d rea e th colli ion rate, depending on this dependence is currently available, however.
wheth I' th parti I i (respecti ely) more or Ie dense Similar rea oning applied to the ca e of vi caus
than the continuous pha e aod can be een a part of the colli ions in turbulent flow lead 1.0 the replac mem of~1 in
tataI hydrod -namie interaction of the panicle . equations (2) and (3) by Yk, a rate of strain characteri ti
The approximation at present offered by the literature of flow in the smallest eddies:
is to ignore all hydrodynamic interaction. While this
approximation is likely to be reasonable for particles of (4)
similar size (see section 5,1 for corroboration), it is likely
to fail seriously in the low-Reynolds-number, unequal-
particIe case. A number of collision mode Is taking
account of hydrodynamic interaction, developed by the
author in the context of a recently completed BRITE
project·, should appear in the literature shortly.
.
time, ~ (film thickness, h)
inertial regimes correspond respectively to particles much
maller and much larger than the length scale of the
smallest (Kolmogorov) eddies. film ruplure
(h ~ hel
• Partners' '( K), Imperial Colle3e (London). Uni lever Research confluence
~
(the etherland ) Figure I. Conceptual framework ror coalescence modelling.
ters 11) that the equa tions governing (axi-symmetrical) why coalescence is favoured by gentie collisions. The
film drainage between unequal particles are the same as explanation is supplied by equation (15): increase in F
th se between equal particles of equivalent radius, Rcq , increases lhe size of the film while the driving pressure
given by remains Iimited to the order of 2a/R.
11' F is constant, integration of equation (22) yields
Rcq -I =(R 1- 1+R 2- 1)/2. (18)
h- 2 -h - 2-(16n(J2/3).LR 2 F)l
o (23a)
Equation (18) indicates, for example, that provided thè
deformed porlion of the interface is smalI, drainage or
betwen a free interface and a drop of radius R is h 2 _ (3).LR 2F/ 16n(J2)/t, (23b)
equivalent to drainage between equal drops of radius 2R.
The following discussion of drainage between equal if h~ho
partiJ can thus be generalized directly to unequal
panicles, provided estimates of the relevant boundary The onset ofjlaltening
conditions (collision force/velocity and duration) are As initially spherical particles having immobile inter-
available. faces approach each other under the action of a constant
Vari us regimes of drainage may be distinguished, force, the pressure at the centre of the intervening film
depending on the rigidity and mobility of the interfaces. rises, eventually becoming of the order of the pressure,
The onl one permitting an analytic solution is that of 2a/R, required to f1atlen the interfaces. The separation,
rigid immobile interfaces. Important regimes of h ftal at which this occurs can be estimated either from an
deC rmed-particle drainage are those of immobile. par- expression 1'01' the film pressure or from the separation at
tially mobile and fully mobile interfaces. The latter regime which the drainage relations, equations (19) and (22)
splits into t\ 0 sub-regime. depending on whether inertial yield the same thinning rate, - dh/dt:
or viscous forces domina te in the draining film. Analyses
hflal - F/2n(J. (24)
of these regimes are 1.0 be found in the literature the
eartier models approximating the film as parallel-sided
NlIlI1ericaf reslIlrs
while Lat r ones oumerically tackle the full coupled
Recently Yiantsios and Davis' have generaled nurneri-
problem of interfacial deformation and film flow. All
cal solutions of the coupled deformation and film-flow
modeLs supp e simple boundary conditions: either con-
equations for the gravity-driven approach of a drop lo a
tant interaction force or constant approach velocit ; in
free interface, under lhe restriction equation (17). Gravity
realit bath will ary duriog acollision.
J
then plays a role only in supplying the inleraction force,
F= (4/3)nR 3tlpg (25)
3.1. Drainage bem een rigid particles
and lhe result an be tran.lated, via lhe equivalent radiu
FOT a gi en approach velocity (- dh/drY ofthe spheres, principle, to any constant-force collision.
lhe mean radial velocity in the film follows from conti- In the Iimiting case of very high drop viscosities, for
nuity and implies in turn (via the Poiseuille relation for which the interface is immobile, the authors express the
flow between quasi-parallel sUl'faces) a certain pressure governing equations in terms of the dimensionless vari-
variation and hence a certain interaction force: ables,
F= 3n11R2( - dh/dr)/2h. ( 19) 11'=h/h;, r'=r/(h;R)'/2, ('=t/().L/tlpgR), (26)-(28)
For constant F, (19) integrates to resulting in a single dimensionless parameter in their
h=hoexp( -t/leh), (20a) equations, (5:
where the characteristic time. Ich, is given by (29)
leh
2
= 3nR .11j2F. (20b) These equations are then solved 1'01' one value of
(5=0.025*.
Before discussing the resul ts obtained, it is noted that
3.2. Drainage between deformable immobiLe interfaces an alternative transformation of variables,
Parallel-film model h* = h'/0 = ha//1pgR J = h/(3F/4na) (30)
11' the deformed portion of the film is supposed to be 4
parallel-sided a similar approach to the preceding one r*=r'l(51/2=r(a//1pgR )1/2=r/(3FRcq /8n(J)12 (31)
yields (Mackay and Mason l2 ) 1* = (' = t/(n).LR c//3F), (32)
-dh/dl = 2h 3F/3nJ-L Q 4. (21) leads Lo a universal set of equations containing no
Fand a are not independent ofeach other sim;e the excess parameters at all. Expressed in terms of these asterisked
pressure in the film must be of the same order, 2(J/ R, as variables, the solution of Yianlsios and Davis can thus be
that in the drop/bubble (equation (15)). Flimination of a translated into the behaviour in any other case, regardless
with the help of equation (15) leads to of the value of () or of the radius ratio of the particles
I that is to
"*Illin = (4/3) 1/2 (34)
0.02
In view of the distinctly non-plane character of the actual
I' = 29 film in the final stages of drainage, the re emblance of
h' equations (33) and (34) to the corresponding predictions
(23b*) and (15*) of the plane-film model is astoni hing.
0.01
51.5
74 3.3. Drainage betwccn defor-mabJe partially-mobile
intcr-faces
119
The approximation of immobility of the film surfaee i
0 applicable only to systems with extremely high dispersed-
r' 0 0.1 0.2 phase viscosities or to one containing a urfactant
soluble in the continuous phase_ In many pure Iiquid-
liquid systems, drainage is eontrolled predominantly by
the motion of the film surface, the eontribution of the
0.003 additional flow within the film due to the prevailing
(' = 907 pressure gradient being much smaller. This situation is
termed here partial mobility, the term full mobility being
reserved for system in whieh the interface is effeetively
0.002 shear-stress free.
.dh·.
mon /dt . a disjoining pressure, n (the force per unit area of film
10 required 10 compensate van der Waal attraction),
n = -A/6nh 3 , (53)
he - (AR....'Q/8nu)'O. (56)
Equation (56) indicates that the effective. or critical, or
rupture thickness varies from a few hundred Angstroms P'='='CI (3/4)-1/8FI- e2/8, (60)
for large drops/bubbles to a few tens for small ones.
where the flow number Ft is defined as
5. COALESCENCE PROBABILITY Fl=6npyR J/A (61)
The foregoing considerations provide the basis for a and the constants Cl and Cl, of order unity, take account of
pr liminary estimate of the probability of coalescence the approximate character of the various numerical
during the collision of given particles under the action of estimates in the model (for example, the coefficient ory-I
giv n local flow conditions. The starting point is simply in equation 3).
Ihat oalescence--that is. film rupture--will occur if the Equation (60) is compared in Figure 7 with the exact
interaclion lime, tj. exceeds the time. te, required for numerical solution (Schowalter 24 ) for the capture effi-
drainage t the thickness "e. The expressions for Ij ciency (the fraction of the collisions, predicted by equa-
re iewed in seet.ion 2 represent typical values. For given tion (I), leading to coagulation), taking account of all
10 al flm conditions. individual values will ofcourse vary possible incidences and of van der Waals attraction
con iderabl,. depending on the incidence of the colliding throughout the interaction process. The best-fit va lues of
particl s. turbulent fluctuations. etc. Likewise, the ex- Cl and C2 are indeed of order unity, while the q uality ofthe
pre i n- re iewed in section 4 for te depend upon the description provided by the approximate model is very
colLision force/velocit ,which in turn will vary consider- encouraging.
abl. in a gi en location. In reality therefore, even aside
from the shortcomings ofthe indi idual modeIs. the ratio
I 'Ij provides onl)' a first indication ofwhether coalescence
5.2. Deformable, partially-mobile, drops in viscous
\ ill or will not occur in a gi en location. Ihe coalescence simple shear
probabilit.. P, tending to zero lor large alues ofthi ratio Together with equalions (2) and (3), equation (43b)
and to unit. for small ones. Arelalion sali f ing these leads 10 an expression for Ihe film thickness at the end of
characleri ti hich hould pro ide a first indicalion the collision process. hr, given by
(Ro el 01.]223) i
h r/R-(3/4 x O.66)(Pd/l-t)n 312 ,
P= Xp(-/c'tJ (57)
hrlR-(/ld/p)n 3 -, (62)
Equation (S ) will n be u d. in conjunclion wilh the
rel ant xpressions for te and Ij, to explore the coale -
cence behaviour in three illu trati e cases.
2.0
he~(A/72npYR)I/~. (58)
te now follows from equation (20), if an estimate is
0.1
available of ho-the separation at which the drainage law,
equation (19) first applies. Since at large separations the 0.08
h o -R/4. (S,}) fl
Equations (20), (58) and (59) now provide the requirl:d Figure 7. Numerical prcdiction of capture eflkiency. 0<0. for equal
expression for Ic. Togethcr with the expression (3) for tj, spheres in viscous shear (solid line: Schowalter 24 ) with capture probabi-
this then leads 10 lity. p. according 10 equation 60 (dolled Iinc. ('I = 1.17. q= 1.80).
where A typical force per unit volume of film due to gas hear
stress, FG , may now be com pa red with a typical force, F p ,
(63)
due to liquid inertia:
The capillary number, n, is the dimensionless group
controlling drop deformation and break-up in viscous FG = 2Td/h ~ 2IJ.d u/ hl,
shear, drops being nearly spherical for values of n Fp = puau/iJr~ pu 2/1,
considerably smaller"than unity (see, for example Ralli-
FG/Fp~2IJ.d/puh.
50n 25 ). n also determines the magnitude of a/ R, as
combination of equations (3) and (15) shows: The retarding effect of gas shear stre s thus become
a/R~(3n)1/2. (64)
substantial if
number (p V- Reqj(J = 2p V 2R/(J) greater than around 0.5 Given thc local VOllllllC fraction, ex, of the dispersed
are ob erved to bounce one or more times before phase, lhe eorresponding Sauter me;ln particIe diameIer,
coalescing (Kirkpatrick and Lockett 27 . Farooq2~). An dn , follows from thc valuc of S:
extension of the considerations for equal bubbles to this
S = 6ex/ndn- (78)
case (Chesters and Hofman 9) results in
The entire modelling procedure of course requires the
lcjt;-(2H E)I/2 (73)
coupling ofeqllation (76) with numerical Aow simulation.
rather than equation (71). where Additional contributions 10 OSjOt due to particIe break-
up will also have to be modelled in genera\. For eases in
WE=pf -Rcqj(J = 2pV 2 Rj(J, (74)
which the particles follow the eontinllous-phase Aow
impl. ing a critical value of WE of order Ij2. Equation c1osely, a single-phase flow code which takes account of
( 3) is. of course. based on a greally simplified model of the influence of the particles on the effective continuous-
the bouncing process. together with the assumption that phase viscosity will suffice. For bubbles or large drops,
WE I. \ hich is no longer weil satisfied at the Weber however, a two-phase Aow code will in general be
numbers coneerned. Nevertheless. the global agreement required and the flow itself will then be cOllpled with the
with observations is encouraging. The number ofbounees particIe size.
required \ill depend on the initial Weber number.
su ce ive approaches progressi ely redllcing lhe Weber
number due t drag dllring its de cent and re-aseent. 6.2. Transition between regimes
Returning to turbulence-indllced coalescence. if the The preceding discussions have by and large been
bubble are smaller than the size ofthe energy-containing Iimiled to a discussion of collision, film drainage and
eddie a typical relati e approach velocity of adjacent rupture in cerlain weil defined regimes: inerlia or viscous
bubbles may be upp ed to scale with L' (equation (5». collisions, partially or fully mobile interfaces etc. In
E uation ( _ th n become reality, the regime applicable is likely to change smoolhly
from one loealion in lhe Aow to anolher. The simplest
P~e. p[ -c (Wel_)' 2]. (75)
way of coping with th is problem is to apply the model
where c· i another constant of order unity. whieh corresponding 10 lhe regime most c10sely applieable, a
in Iud the ratio I' the fluctuating bubble to conlinous- transilion from one regime to another being indicated
phase velocity. noted in section 2.2, turbulence- wh n, for example, the relation for each regime yield lhe
indu d bubble break-up oc urs at value of f-JI: of order same ailie of lhe quantity being predicted (colli ion rate.
unit)'. Equation (7 ) uggest that under these condition coale-cence probability, 0 lOl, etc.). Thi difficult will
th hance of oale ence i again smalI, though nol as of cour e disappear onee more broadly applicable models
mali a in the ase of panially mobile dr p . become available.
of course the exception rather than the rule. Almost all area ofvariable interfacial ten ion i virtually unexplored.
emulsions involve an aqueous phase containing some A IittJe work has still to be done'
surface-active material, either by accident or design, and
many systems contain surface-active ingredients in both
phases. Likewise. many dispersions are created to permit NOMENCLATURE
effeetive mass transfer of a third component between lhe {/ film radiu (Figur land 2)
phases. Jn such cases, the variation of species concentra- A Hamaker constanl
Cl -c~ eonstants of order unity
tion over the interface engenders a corresponding varia- C parlicle collision rale per unit time and volume
lion in the interfacial tension. d particIc diameter
The variation of interfacial tension produces a net dJ2 Sauter mean particIe diameter
tangential force per unit area, 1"a: J free energy per unit area of film
F interaction force excrted by one particle on another
1"a=grad a. (79) Fe.xt force exerted by the external flow on a particle
Fw radial force per unit volume of film due 10 van der Waals
Like the shear stress exerted on the interface by the force
dispersed phase, this small force per unit area translates radial force per unit volume of film due lo gas shear Iress
into a significant force, Fa. per unit volume of the film, radial force per unit volume offilm due lo continuous-phase
inertia
Fa =21"a/h = 2grada/h, (80) F" radial force per unit volume of film due to interfacial-
tension va ria tion
whieh can radically retard or accelerate film drainage. Ft flow number (equalion (61»
The modelling ofsuch effects requires primarily a modifi- g acceleration due 10 gravity
calion of the film drainage modeis, the basic equations h (minimum) film thickness
ho initial film thiekness
de eribing film drainage being extended to include lhe hj initial film thickness used in lhe compulalion of Vian ios
species diffusion equation, an equation relating bulk to and Davis
interface concentralions and an equation relating the
inl rfacial tension to the interfacial concentration of lhe
"e
hniJl
crilical ruplure thickne
film thickness at the onset of f1all ning
pecie . A recent example in the domain of drop deforma- "rH final film thickness at lhe end of a colli ion
(1/2) In"
tion i provided by Stone and Lea1 30 . k olli ion coefficient (equalion (I»
t length scale haracteristic of radial "ariation offilm proper-
tie
L y tem length scale
7. PERSPECTIVES, CHALLENGES 1/1 actual plu virtual ma of a particl
TI number of particl per unil \olum
From a 'helicopter view', the task of implementing the p film pr ure
eheme portra ed in Figllre I compri e threc a p cts: p probability of coalescenee during a collision
r radial di lanee in th draining film
I. The generation of the separale pieces of the pllzzle- R particle radius
the drainage and collision laws for the various regimes. Rcq cquivalent radius (equation (18»
_. Their incorporation in compact relations which can be Re Reynolds numbcr pril /11
RE Reynolds number pR~ V/II
applied locally wilhin a numerical stimulation of the s surface area of a parlicle or parlicle pair
multiphase flow without requiring excessive computation S specific interfacial area
time. time
3. The development of efficient and robust numerical time required for drainage 10 the critica I ruplure lhickness
mc:thods incorporating both flow and local effects. characterislic time seale
interaction time of colliding particles
Until recenlly, the absence ofvarious key pieces ofthe time scale chara teristic of the exlernal flow (equation (7»
interface velocity
puzzle has prevenled any worthwhile work in areas 2 and vclocity of the dispersed phase
3. aside from considerations of global strategy and t' eharacleristic velocity variation over a distanee d in the
progress towards increasingly effective two-phase flow basic flow
simulations bascd on conslant particIe size. The arrival, in V relative velocity of centres of colliding parlicles
particular. of various key drain;.tge modeIs now makes We. WE Weber numbers. defined by equations (11 b) and (14b)
2R minus the distance between particIe ccntres
serious work on areas ~ and :I bath possible and attraclive
for the pure-fluid case and high-quality experimental G,....k fell""s
validalion of sudden urgency. In addition it enables (J. volume fraetion of the dispersed phase
'back-of-the-envelüpe' calculations to be carried Ollt ft coeflicient of virtual mass (equation (10»
shear rate
which may. on a short term basis. be of greater impür- rale ofslrain in the smallest (Kolmogorov) cddies (equation
tanee la those seeking an immediate. if approximak. (4»
answer. dimensionle s gTOUp öpgRJ/uh,
Understanding and model devclopment in area I is of turbulence energy dis ipalion nHe per unit mas-
eontinuous and disperscd-phase viseosilies (respectiv Iy)
course far from complete. The available slIb-modeis
I'/f'
rcmain approximale: the numerical drainage reslilts do n disjoining prcssurc
not incorporate lhe actllal force/velocity varialion p. Pd eontinuous and dispersed-phas densiti (respecli,cl~)
encountered in real collisions nor are van der Waals u inlerfacial tension
2:[ film lension
farces included. while hydrodynamic inlcractions have shear stn:ss excrted on lhe film b~ th di-persed pha-
yet to he satisfaclorily modelled. In addition. gravily- tangential force per unit int rfacial area due t u-\ n:J1i n
induced collisions have still to bc model led and the enlire n capillary numbcr (equati n (63))