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J. of Thermal Science Vol.1, No.

1 Journal of Thermal Science


Science Press 1992

Theoretical A s p e c t s of N u c l e a t e P o o l Boiling w i t h
Dielectric Liquids

Avram Bar-Cohen Wei T o n g Terrence W. Simon


Department of Mechanical Engineering University of Minnesota, Minneapolis, MN55455, U.S.A.

Direct cooling with inert, dielectric liquids may well become the technique of choice for the thermal manage-
ment of future electronic systems. Due to the efficiency of phase-change processes and the simplicity of natural
circulation, nucleate pool boiling is of great interest for this application. This paper examines the characteristics
of vapor bubbles and nucleate pool boiling of the dielectric liquids. The results provide a theoretical foundation
for understanding and interpreting the often complex empirical results reported in the literature.
K e y w o r d s : n u c l e a t e p o o l b o i l i n g , d i e l e c t r i c l i q u i d s , t h e r m o - f l u i d p r o p e r t i e s , d i s s o l v e d gas, c o n t a c t
a n g l e , h y s t e r e s e s , e m b r y o f o r m a t i o n , b o i l i n g i n c i p i e n c e , b u b b l e - v a p o r flow r e g i m e , w a k e - p u m p i n g
effect.

INTRODUCTION and provides, for the first time, a comprehensive the-


oretical treatment of nucleate boiling in dielectric liq-
The incessant drive towards higher heat flux and uids.
power density in nearly all categories of electronic
equipment has turned attention to the use of liquid
coolants for the thermal control of electronic compo- FLUID PROPERTIES
nents. Recent developments in the microelectronic
industry, including the introduction of the immer- The fluorocarbon fluids, represented by the perflu-
sion cooled Cray-2 and ETA-10, have opened the orinated Fluorinerts, or "FC" series, of the 3M Com-
way for more widespread implementation of direct pany, and the Chloro-Fluorocarbons, represented by
liquid cooling in electronic systems. Among the di- the Freon refrigerant series of the Du Pont Company,
rect liquid cooling techniques, boiling has proven are widely used dielectric fluids in the microelectronic
to be an efficient heat transfer mode for remov- industry because of their excellent characteristics in-
ing very high heat fluxes and accommodating large cluding thermal stability; electrical properties (high
increases in local heat flux with only modest in- dielectric strength, low dielectric constant, and high
creases in surface temperature. Unfortunately, the volume resistivity); lack of flammability; and low tox-
prime candidate immersion cooling liquids, such as icity. However, in contrast to water and other conven-
the per fluorinated-Fluorocarbons (Fluorinerts) and tional coolants, these dielectric liquids possess rela-
the Chloro-Fluorocarbons (Freons), possess thermo- tively low thermal conductivities and boiling points
fluid properties which are substantially different from and small latent heats of vaporization. They are
those of conventional liquids. This is of particular also characterized by very low surface tension and
concern in ebullient heat transfer, since the success- demonstrate high wettability on all commercial sur-
ful exploitation of this heat transfer mode requires a faces. Fluorinert (FC) liquids are inert and demon-
clear understanding of the many distinct phenomena strate chemical compatibility with circuit package ma-
encountered in pool boiling. A cursory examination terials while Freons often serve as solvents and de-
of the thermo-fluid properties suggests that FC bub- greasers and show high chemical reactivity with many
ble properties, in particular, may differ substantially materials. These characteristics, as well as their un-
from water and lead to a realignment in the impor- usually high gas solubility, have been used to explain
tance of specific bubble growth and thermal transport anomalies associated with some aspects of nucleate
mechanisms. boiling of these liquids.
The theoretical nucleate boiling characteristics of In single-phase heat transfer, it has been shown that
the perfluorinated liquids have been the subject of a the fluids are generally ordered by the combination of
series of publications by the authors. These studies their thermal conductivity and viscosity values. If nu-
have helped to create a theoretical foundation for un- cleate boiling heat transfer becomes the cooling mode
derstanding these phenomena and for interpreting the of choice, the selection of cooling liquids will depend
often complex empirical results reported in the liter- on parameters which affect the incipience superheat
ature. This paper summarizes these previous studies and the critical heat flux. The comparison of proper-
ties between highly-wetting liquids and water is given
* Received July 1991. in Table 1.
Avram Bar-Cohen Theoretical Aspects of Nucleate Pool Boiling with Dielectric Liquids 47

Nomenclature ~d dynamic contact angle


A area, m 2 #Sd,A dynamic advancing contact angle
a thermal diffusivity, m 2 / s ~d,/z dynamic receding contact angle
C specific heat. J(kg . K) fl, static equilibrium contact angle
Db bubble departure diameter, m ~,,A static advancing contact angle
f frequency, s - l /9,, R static receding contact angle
g acceleration of gravity, m / s 2 A~d dynamic contact angle hysteresis,
H Henry's parameter, moles/{mole atm) - ~ d , A -- ~d,R
hi# latent heat of vaporization, J / k g A~, static contact angle hysteresis,
Kin! influenced area ratio --~,,A -- fl,,R
l length, m $ thickness of superheat layer, m
M molar mass, kg/kgmol 2~b cavity angle
N n u m b e r of active bubble sites # dynamic viecosity, Pa.s
Ng mole fraction p density, k g / m 3
Nuc nucleation n u m b e r defined in Eq.(17) a surface tension, N / m
P pressure, Pa; or arm in Henry's law
[P] parachor, mS.kgl/4/(sl/2-mol) Subscript
q heat flow per bubble site, W / s i t e
qU heat flux, W / m 2 b bubble
R radius, m C critical
Ro cavity radius, m g gas
R~ universal gas constant L latent heat
T temperature, K l liquid
Tb boiling point, K m mixture
AT~ wall superheat,--=T,o - T,, K melt melting
U velocity,m/s ne natural convection
V volume,m s s saturated property
tr transition
Greek s y m b o l s v vapor
W wake
j9 contact angle ~ wall

There are several correlations for calculating am for


EFFECT OF DISSOLVED GAS ON THER-
nonaqueous mixtures. Among these is the Macleod-
MO-FLUID PROPERTIES
Sugden model, which is based on empirical relations
for pure liquids, and can be used for a gas-liquid sys-
Gas Solubility
tem (Reid et al., 1987),
Dielectric liquids possess unusually high gas solu-
bility. For example, the solubility of air in FC-72 is n

25 times higher than in water at standard conditions


(3M,1987). Thus, it appears that the dissolved gas i=i
may influence both the liquid properties and the boil-
ing process. where [Pi] is the parachor of the i ~h component; P,,I
The content of dissolved gas (in mole fraction) in and ping, Mini and Mmg, are the densities and molar
liquid can be predicted by Henry's law (Reid et al., masses, of the liquid-gas and vapor-gas mixtures, re-
1987) spectively, and Xi and Y~ are mole fractions of the ith
Ng = H ( T ) P g (1) component in the liquid and gas phases, respectively.
At low pressures, the gas density is much lower than
where Pg is the equilibrium pressure of the gas above the liquid density and the second term of equation (2)
a flat interface separating the liquid and gas. Henry's can be neglected.
parameter, H ( T ) , is determined experimentally as a For the binary mixtures of dissolved air in FC liq-
function of temperature. uids, equation (2) becomes

E f f e c t of D i s s o l v e d G a s o n S u r f a c e T e n s i o n am = {-~mll/Pry(1 -- N~,r) + P~irN~,r]}' (3)


For binary liquid mixtures such as an organic liquid
in water, surface tension varies with the mole frac- where M, nt is the apparent molar mass of the mixture
tion of the solute, always lying between the two pure- in the liquid phase
component values. Usually, dissolved gas merely re-
duces the surface tension of the dissolving liquid. For Mini = (i -- N a i r ) M F c + NairMair (4)
highly-wetting liquids, surface tension is much lower
than for conventional liquids; therefore, even a small Since there is no chemical reaction during the gas
variation in surface tension may cause a large relative dissovling process in this case, the molecules of dis-
change. solved gas lie between the molecules of the liquid; the
48 Journal of Thermal Science, Vol. 1, No.l, 1992

molecular structure of the liquid is unaltered and the correspondingly, the boiling point rises from Tb to T~
molecular spacing is essentially unchanged, hence, the and the melting point lowers from Tmelt to T~e u. The
change of the liquid density with addition of dissolved change in elevation of the boiling point can be pre-
gas is negligible. Assuming P,~t = PEG, equation (3) dicted from
was used to compute the surface tension versus dis-
solved air relationship for FC-72, as plotted in Fig.1. ATb = Z~ - T, = R~'T~ Na
At 1 a t m the saturated mole fraction with air in FC- Mm,(Na)hza(Tb) (S)
72 is 0.006, yielding a 1.5~0 change in surface tension.
The comparison of ATb versus N# between highly-
However, as the saturated mole fraction increases to wetting liquids and water is shown in Fig.3. It m a y
0.06 at 10 a t m .pressure, the change of surface tension
be seen that ATb always increases linearly with an
approaches 20%. increase of Ng. The slope of the curve for water is
lower than that for the highly-wetting liquids. The
8.0 - I F am
curves for the two highly-wetting liquids almost coin-
T = 335 K ] cide. The increase of the boiling point is usually less
7.0 than 0.5K for most candidate cooling liquids at low
pressures.
a 6.0 ~ 2.0
T=345 K
(dyn/cm)
---- FC-72
5.0 ¸ --- RII3 .~¢~.r., '~'"
1.5 ......... Water .,~.o.r.*"
• ~" sd , ." ee
4.0 | • u
ATb 1.0 , .o" °4"'''¢" "
0.00 0.02 0.04 0,06
Nw (moles/mole) (K) o. r

0.5 ¸
Fig.l Effectof dissolved air on surface tensionfor FC-72
(Tong, et al., 1990c)
0.0 ! !

0.00 C.02 0.04 0.06


Nsi r (moles/mole)

Fig.3 Comparison of effect of dissolved air on boiling point


between highly-wetting liquids and water

EFFECT OF CONTACT ANGLE AND ITS


HYSTERESES ON EMBRYO FORMATION
AND BUBBLE GROWTH

Contact Angle a n d its Hystereses


W h e n a drop of a liquid is brought into contact
with a solid surface, a contact angle (wetting angle)
is formed between the liquid/solid interface and the
tangential plane of the liquid/vapor interface at the
contact line. If the drop spreads completely over the
T~cu T ~ Tb T~ solid and forms a thin liquid film, the contact angle
Tcmpcratur¢(T) is zero and such a liquid is defined as a completely-
wetting liquid. By contrast, if the drop contacts with
Fig.2 Effect of dissolved gas on the boiling and the solid at only one point, the contact angle is 180 °
melting point of the liquid and the liquid is defined as a non-wetting liquid. For
all liquid-solid systems, the contact angles lie between
Effect of Dissolved Gas on Boiling Point zero and 180 ° .
It has been found t h a t a nonvolatile solute can According to the state of motion of the liquid-solid-
lower the chemical potential of the liquid solvent; con- vapor boundary line, the contact angle can be defined
sequently raising the boiling point and lowering the as a static or a dynamic contact angle. Measurements
melting point (Murrell and Bouncher, 1982). The ef- of contact angle have shown the existence of the con-
fect of dissolved gas on boiling and melting points of tact hystereses for both kinds of contact angles. A
a solution is shown in Fig.2. The chemical potential measured contact angle value always lies in a range
of a pure liquid is indicated as p~. As dissolved gas is bounded by the m i n i m u m [static (or dynamic) reced-
added, the chemical potential shifts down to ml and, ing contact angle,/~,,R (or/~d,R)] and m a x i m u m values
Avram Bar-Cohen Theoretical Aspects of Nucleate Pool Boiling with Dielectric Liquids 49

[static (or dynamic) advancing contact angle, /3.,A(or cavity radius, Ro, can be found as
/3d,A)]. The differences between the two angles, i.e., RI
/3,,4-/3,,R and /3d,A --/3d,R,axe defined as the static
and dynamic contact angle hysteresis, respectively.
sin(/3d -- 2~)
The dynamic contact angle is of special importance
for highly-wetting liquids. Generally, the dynamic sin(/3d -- ~b)Sin
contact angle is a complex function of the interface cos(/3.- ,) -F [2 - 3 sin(/3. - ~b) -i-sin3 (/3. - ~b)]
velocity and viscosity. For a highly-wetting liquid, ~, tan~
though its static contact angle is small, its dynamic tan~ 112 l l / s
value could be very large at high interface velocities. tan(/3d -- ~b) -- ]
For instance, for a stainless steel-hexadecane system,
the static equilibrium contact angle is observed to [,
"-"---~an2~--~3/° ""
I (7)
be near sero, but the dynamic contact angle is as
high as 75 ° when the liquid velocity is about 9.7cm/s For the highly-wetting liquids, of primary interest in
(Schwartz and Tejada,1972). the present study, equation (7) can be approximately
simplified as
Vapor Trapping Process
In heterogeneous nucleate boiling, a vapor bubble ~1 (1- 2~) 1/2
grows from a vapor nucleus which is formed by the ~ /3d
trapped vapor in a microcavity on the heated surface. Ro -- {i -F- ~b[2 - 3(/3, - ~b) -t- (/3. - ~)31)1/3 (8)
As a result, the existence of such vapor nuclei (bubble
embryo) is the necessary condition for the initiation Bubble Growth Process
of boiling. The formation of a vapor/gas embryo in a sur-
face cavity creates a void into which superheated
liquid can evaporate. This evaporation increases
the volume of the gaseous mixture and contin-
ues until the bubble reaches the equilibrium con-
dition. This behavior and the change of the
bubble radius through the four distinct stages of
bubble growth will be examined in the following.

2#

~ ~ - - " __ . ._.

(a) (b)

Fig.4 Vapor/gas-trapping process


(a) (b) (c) (d)

The vapor trapping process can be envisaged to be-


gin with the flow of a liquid along an initially dry Fig.5 Bubble growth stages: (a) contact angle readjustment;
surface. As a liquid flows into a microcavity, it keeps (b) in-cavity growth; (c) growth on the cavity mouth and
a dynamic contact angle,/3 d (where/3, ~/3dl --~ /3d,A) contact angle readjustment; (d) growth on outer surface
with the cavity wall (Fig.4). During the process, it is 1. Contact angle readjustment (Fig.5a)
assumed that no mass transfer occurs. The trapping Following the filling of the cavity by liquid, a small
condition is that the dynamic contact angle is larger increase in bubble volume due to vapor inflow and
than the effective angle of the cavity (Bankoff, 1958; the resulting motion of the vapor/liquid interface will
Tong et al., 1990a), i.e., lead to a decrease in contact angle to its static re-
ceding value, /3,,R. During this process, the bubble
/3d > 2~ (3) three-phase line remains fixed at its initial position on
the cavity wall. With radii R2 corresponding to/3,,R,
and R1, corresponding to/3,, the following geometric
The trapped vapor constitutes a bubble embryo in relationship can be determined:
the cavity, awaiting the appropriate thermal condi-
tions to emerge from the cavity as a vapor bubble. R2 cos(/3. - ~)
The ratio of the embryonic bubble radius, R1, to the R1 = cos(/3,,R - ~) (9)
50 Journal of Therma] Science, Vol. I, No.l, 1992

For the cases that flo > ~ and/9,,g _> 0, since both the the contact angle, fl, changes immediately and spon-
inverse bubble radius and the bubble volume increase taneously from its static receding value, ]~s,R, to a
during this process, A(1/R)/AV is positive and the dynamic contact angle value, ]~d (where fld,R < ~d2 ~_
bubble growth is restrained (positive-sloped segment fls)- It remains at its dynamic value throughout the
in the coordinates of Fig.fib). Following Thormfihlen process. The bubble volume during this phase can be
(1986), this process will, henceforth, be referred to calculated as
as ~restrained growth ~. For the cases that fl~ < ~b,
A(1/R)/AV is negative (Fig.fia) and consequently, 3 [cos 3( d - ¢)
v= 3 +2
the process is unstable.

1.5e+6 (11)

The slope of the segment corresponding to this pro-


i .0¢+6 • cess is negative (Figs.6a and fib). Therefore, the bub-
I/R ble will continuously expand until it reaches the edge
(m'!) of the cavity.
5.0e+5 •
3. Growth at the cavity mouth IFig.Sc)
As the bubble moves toward the mouth of the cav-
O.Qc+O ity, the contact angle retains the dynamic value. How-
I0 -17 10 -16
ever, at the mouth, the contact angle readjusts to its
Bubble Volume (m 3)
static receding value and the bubble radius changes
correspondingly from R3 to R4. During the process,
Fig.fa Bubble growth process for FC-72 (/3. : 2 ° , the bubble volume is given as
~.,R = 0.5°,]~#I = 20°,]9a2 = 1°, Ro = 1.0pro)
V- ~rR°s 1 - sin3~ - - - 3
3 sin 3/~
1.10~6 - where fl varies from (~r/2 - ~b+/~d) to Po,R.
When the dynamic contact angle, fld, is greater than
1,00c+6" the half cavity angle, ~b, bubble growth can be divided
into two sub-periods. During the first sub-period the
fIR bubble interface moves from point 03 to A and the
9,00c+5
(mL) radius, R, decreases continuously from R3 to R0 (the
minimum value of radius for this stage) while the vol-
8,lX}c,+.5
ume of the bubble increases. Consequently, t h e slope
of this subsegment in the coordinates of Fig.fb is pos-
7.00¢+~
5.00¢-17 6.00e-17 7.00¢-i7 8.00e-17
itive and the growth is stable. The radius R3 is
Bubble V o l u m e ( m 3)
R3- cos{ d -- 0) (13)
Flg.fb Bubble growth process for FC-72 (8. = 5°,
~.,R = 1-5°,~dx = 20°,~d2 = 2, ~ = I °, During the second sub-period the center of curva-
Ro : 1.O~rn) ture of the bubble moves from point A to 04 (corre-
sponding to fl = fls,R,R ----R4). The slope of the
subsegment is negative and the bubble grows without
During contact angle readjustment, the bubble em- restraint until it leaves the heated surface.
bryo volume increases as
Ro
R4 = 04)
V -- lrR33 c°s3(fl+cos3(fl
---~)'[c°s3(flt-~n~-~b) + 2

-3 sin( - 0) + sin3( - 0)] (10) For situations in which fld --< 0, the bubble radius
increases directly from R3 to R4 without the appear-
where ~ varies from fl, to fl+,R- ance of the second peak on the bubble growth curve
For highly wetting liquids, since fl+,R is close to (fia).
fl+, R2 approximately equals Rz.
4. Growth on the outer surface and bubble depar-
2. In-cavity growth (Fig.Sb) ture (Fig.5d)
As additional vapor forms and the embryonic bub- After reaching the point R = R4, the bubble will
ble grows, the liquid/vapor interface moves toward the continuously expand until it leaves the heated surface
mouth of the cavity. At the beginning of this phase, under the influence of buoyancy and/or momentum
Avram Bar-Cohen Theoretical Aspects of Nucleate Pool Boiling with Dielectric Liquids 51

forces. During this stage, the base of the bubble is the Clansius-Clapeyron relation is applied. However,
pinched by inflowing liquid, trapping a new bubble this is appropriate only under the circumstances in
embryo in this active site. While the details of this which saturation curve is approximately linear over
process will determine the radius of the trapped vapor the superheat range of interest. Since the critical radii
embryo and, consequently, influence the generation of in highly-wetting liquids are often of order 1 0 - l # m for
subsequent bubbles from this site, it may be expected nucleate pool boiling (Danielson et al., 1987), high in-
that the trapped volume and radius will be relatively cipience superheats may be reached and, thus, a more
large. exact formulation is needed.
Following the classical analysis of nucleate boiling,
the force balance on a bubble can be used to determine
CRITICAL BUBBLE RADIUS the wall temperature at incipience, as

The critical bubble radius is defined as the mini-


mum bubble radius during bubble growth. This is a
P,(T.) - P , = 2 Ro
(Tw) (18)
very important parameter because it determines boil-
where Pt is the liquid pressure over the bubble inter-
ing incipience. For conventional liquids, the critical
bubble radius is taken to equal the cavity radius, but face and the ~ Pg term contains the partial pressures
of different gases within the bubble. The vapor pres-
this is not the case for highly-wetting liquids.
During trapping and subsequent growth, the bub- sure can be determined by using an empirical relation
ble radius of curvature varies in a complex manner for the saturation line (Reid et al.,1987)
with bubble volume, tracing the characteristic "two h
hump" trajectory shown in Fig.6b. Consequently, the Po = e x p ( a - --5--) 09)
superheat required to insure explosive bubble growth Tw
and, thereby, boiling incipience, is determined by the
where a and b are constants. Because the nuclei of
highest of the two inverse-radius peaks.
embryonic bubbles in highly-wetting liquids are very
Ignoring the difference between R1 and R2, the crit-
small and are inside the cavities, the bubble temper-
ical bubble radius, R~, for highly-wetting liquids is
ature can be taken to equal the wall temperature,
given as Tw. Thus, both the vapor pressure, P~, and the
R o ( ~ - 2¢)i/2~dI/2 surface tension, a,are evaluated at the wall temper-
R~ : {1 + ¢[2 - 3(ft, - ¢) + (~. - ¢ ) 3 ] } 1 / 3
(15) ature. Hence, the governing equation (18) can be re-
expressed as
Calculated results for highly-wetting liquids show that
R~ is always less than Ro, hence, the critical bubble exp(a (2o)
radius is always located inside the cavity.
As discussed in the previous sections, the radius of
a bubble embryo is dependent upon the trapped va-
25
por/gas volume and, thus, is also dependent on the
dynamic contact angle. Since the superheat required
for boiling incipience varies inversely with the bubble 20- /'\ '., \\'
~ "%
"....2,-- 20.
J
I
radius, it can be concluded that for increasing values ,.o \ - . \ .-. I
of fig, the incipience superheat decreases. IS-
(AT,) i
I0"
(K)
CONTACT ANGLE EFFECTS ON BOILING
INCIPIENCE S-

The frequently-used model in heat transfer litera- o " I " I • ! " I ' " I

ture to calculate incipience superheat, which employs o I0 20 30 40 50


the Clausius-Clapeyron relation, is given as (assuming 15~- 13, (de~re~s)
no dissolved gas in the liquid),
2Nuc Fig.7 Comparison of incipience superheat of highly-wetting
(ATs), -- Rc (16) liquids

where Nuc, the Nucleation number, is defined as: Since this equation is a transcendental equation in
the dependent variable, T~, it must be solved by a
trial and error method.
Nuc -= (17) A comparison of superheats calculated from the
htgpg
present model and equation {16) for FC-72 of ~ = 2 °
where the surface tension is based on the saturation and Ro = 0.5pm, is given in Fig.7 for a system free
temperature. It is to be noted that in equation (16) of non-condensable gas (the dissolved gas effect will
52 Journal of Thermal Science, Vol. 1, No.l, 1992

be discussed in the following sections). From this fig- liquid to an embryonic bubble, the partial pressure of
ure it may be seen that equation (16) deviates from gas inside the bubble, P~, can be expressed as:
the present model for all dynamic contact angles.
Thus,though equation (16) is simpler than (20), the
present model is recommended since: (a) the assump- P; = -ff
tion of linearity of the saturation curve, as must be
done to use the Clausius-Clapeyron relation, may be Boiling incipience will be reached when the bubble
improper for situation of large superheat with highly- radius reaches its criticalvalue. Substituting equa-
wetting liquids and (b), since the position of the crit- tions (22) and (23) into (20), yields
ical radius is always inside of the cavity for highly-
wetting liquids, the surface tension at the bubble in- b 2cr,r, (T~, N0) Me i l
terface should be evaluated at the wall temperature exp[a Yw Rc p ~ p m t ( T w , N o ) yw - Pl
rather than at the saturation temperature correspond-
ing to the system pressure. 2¢r,n (Tw, Ng)
R¢ W- (24)
The wall temperature can be numerically calculated
EFFECT OF DISSOLVED GAS ON BOILING
from the above equation and the incipience superheat
INCIPIENCE
can be obtained, as
Curvature Effect on Vapor Pressure inside a (AT.),,g = - T"
Bubble
By considering the equilibrium of a liquid contained
in a capillary tube in a sealed vessel, Lord Kelvin first RuT's (25)
= ( A T . ) , - [ M . n , (Ng)h,g(T.) ]Na
derived an equation which described how the vapor
pressure acting upon a curved surface in thermody-
T. in the above equation is the saturation tempera-
namic equilibrium differs from that for a plane sur-
ture of the pure liquid at the vapor pressure.
face. Since the critical bubble radii in highly-wetting
liquids are generally small (much smaller than those
in water), the curvature effect on the vapor pressure 37.3
inside an embryonic bubble may be more important
than in water; According to the Kelvin equation, the
vapor pressure over a curved interface, P~, takes the 37.0
form (ATsh,s
Pe
P;--- .2or Me 1 (21)
(K) 36.7
expt ~ R-~pt T]
where Pe is the saturated vapor pressure over a plane
surface at the particular temperature, T, and R is the 36.4 I |
radius of the curvature at the bubble interface. 0.000 0.(}02 0.004 0~006
For the cases with dissolved gas in a liquid, equation N,~ (moles/mole)
(21) is written as

N.) = Fig.8 Effect of dissolved air on boiling incipience superheat


for FC-72 when P~ is fixed at 1 arm
e x p ( a - __b) (assuming fl d : /3, )
Tw (22)
Ng) Me 1 N11merical E x a m p l e
exp[ 2~,,~--~Tw, Rup,m (Tw, Ng) Tw ]
To illustratethe dissolved gas effect on boiling in-
cipience with a highly-wetting liquid, FC-72 (/~.-- 2 °)
is chosen as the working liquid and a cavity geometry
Gas Pressure inside a Bubble (2~ ---- 1.95 ° and Ro : 0.5pro) is assumed. Thus, us-
To estimate the partial pressure of gas inside an ing equations (24) and (25), the relationship of boiling
embryonic bubble, the concentration of dissolved gas incipience superheat and content of dissolved gas can
in the liquid must be investigated. When the sys- be easily plotted for the particular conditions of inter-
tem is in equilibrium, the content of dissolved gas est. Two systems axe considered:
can be predicted by Henry's law. Since Henry's pa- a. Let the vapor pressure be a constant (Pc : latin)
rameter appears to be independent of temperature for and let the gas pressure vary from zero to I atm. The
highly-wetting liquids, the dissolved gas mole fraction saturation temperature, T,, at the vapor pressure in
remains constant as the system reaches thermal equi- this system is then a constant. The results show that
librium. Assuming that there is no curvature effect on the incipience superheat, (AT,)~, decreases linearly
the gas pressure, for dissolved gas released from the with an increase of dissolved air in the liquid (Fig.g)
Avram Bar-Cohen Theoretical Aspects of Nucleate Pool Boiling with Dielectric Liquids 53

due to the chemical potential effect. However, this Departure Diameter


change is less than 0.3K when the dissolved gas is less It has been found that the Cole-Rohsenow model
then 0.006 moles/mole. (1969) for predicting bubble departure diameter is the
b. Keeping the total pressure constant (P = 2 atm) best for highly-wetting liquids (Fig.10)
while varying the gas pressure from zero to 1 atm,
the vapor pressure changes correspondingly from 2 to
[ uE 11/2 (26)
1 atm. As seen in Fig.9, both Tw and To decrease Db= g(Pi -- Pg)
with an increase of dissolved air mole fraction. Since
To decreases more than Tw with a decrease in vapor where
pressure, the incipience superheat will increase with
increased dissolved gas content, Arc. In this exam- E 1/2 --- (1.5 X 10-4)(J~) 5/4 for water
ple, due to dissolved gas addition the decreases of the
wall superheat and saturation temperature are l l K
and 23K (from 79°CQ2 atm to 56°CQ1 atm), respec- E 1/2 ---- (4.65 x 10-4)(3~) 6/4 for other fluids
tively.
and the modified Jacob number, J~, is defined as
36.0
CtPIT~ (27)
J~ -- pohtg

32.0 Note that the thermophysical properties in the above


(AT, li.s equations are based on saturation temperature, To.

(K) 28.0 B u b b l e F r e q u e n c y a n d Rise Velocity


The bubble frequency, fb~ is coupled with the
bubble departure diameter, Db. Although in the
past a distinction was made between different bub-
24.0 I !
ble regimes, Malenkov's review (1968) of the available
0.000 0.002 0.004 0.006
experimental data, including five different fluids at at-
N.~ (molcs/mole) mospheric pressure, led to a single correlation, using
the bubble rise velocity and heat flux to account for
F i g . 9 Effect of dissolved air on boiling incipience s u p e r h e a t the observed variation in the fbDb product. This cor-
for FC-72 w h e n the total pressure is fixed at 2 a t m
relation takes the form
(assuming fla = ~*)
Ub
fbDb = 1 (28)
l.O • Tolubinsky & Oslrov~iy, 1966 Ir(l I

o Borishanskiyetai., 1981 1 + Ubpohlg/¢'j


Cole & ~ w , 1969
0.8-
.... Ka~l,l~!s~_ 7P& Gogonin (&T = 15 K) where Ub is the rise velocity of an individual bubble
--" Jensea el ai., 1986 (AT = 15 K)
Db 0.6- , -- Borishanskiyel al.. 1981
[ J ..... Jenscli el al., 1986 9Db(pl - pg) 2~ .]i/2 (29)
i\ I ..... Cole & Shutman, 1966 = I +
(mm) 0.4"
Db(:1+:o) ~

0.2"
/
o RI2 (Tolubinsky & Ostmvskiy, 1966)
0.0 • s • ! " I " • • I

0.00 0.05 0.10 0.15 0.20 0.25


P/Pc 200
fb R I 2 ~
F i g . 1 0 C o m p a r i s o n of e x p e r i m e n t a l d a t a and various bubble (l/s)
departure d i a m e t e r models for R12

BUBBLE CHARACTERISTICS 0 ! ! !

0 I0 20 30 40
The bubble characteristics are the basis for under- AT, (K)
standing heat transfer in pool boiling. In this section,
some of bubble characteristics for highly-wetting liq-
uids will be addressed. F|g.lla Bubble freqtmncy of highly-wetting liquids
54 Journal of Thermal Science, Vol. 1, No.I, lgg2

0.3 occupies only a small fraction of the nucleate boil-


Water ing curve, approximately 8%, of the total boiling heat
flux (Gaertner, 1965). The earliest model for predict-
ing the transition heat flux, at which nucleate boiling
0.2 R12
changes from the isolated bubble regime to the vapor
Vb
RiI3 column regime, was proposed by Zuber (1962). Using
this model, with an assumed static contact angle of
(m/s) approximately 50 °, Zuber found the transition heat
0.1 FC-72
flux for water to be

,O'g(Pl -- Pg),l/4
:
. . lr
, o % p,, ,gL
-
J (30)
0.0 l I l |

0 I0 20 30 40 50
AT, (K) From experimental observations, Moissis and
Berenson (1963) concluded that for small separation
distances between two consecutive bubbles, the trail-
Fig.lib Bubble rise velocity at 1 atm ing bubble is accelerated by the wake of the lead-
ing bubble and the two bubbles agglomerate. Using
The comparisons of the bubble frequency and the Fritz's relation (1935) for the bubble departure diam-
bubble rise velocity, between highly-wetting liquids eter, they obtained an expression for the transition
and water, are shown in F i g s . l l a and l l b , respec- heat flux, as
tively.

Pl -- Pg

BUBBLE/VAPOR FLOW REGIMES where fl,, the static contact angle, is in degrees.
A comparison of the transition heat fluxes of highly-
Visual and photographic studies of nucleate boil- wetting liquids (assuming 3, = 2 °) and water (assum-
ing in water have suggested that there are four dis- ing fl, = 50 °) is given in Fig.12. From this figure, it
tinct regimes of vapor flow from the surface (Gaertner, may be seen that the transition heat fluxes calculated
1965). The first regime is called the isolated bubble from equations (28) and (29) for water agree closely
regime. It begins at boiling incipience and continues with each other and, at about 16 W / c m 2, are in ap-
into fully-developed nucleate boiling. In this regime, proximate agreement with the experimental data (also
there is no interference between bubbles either gen- see Moissis and Berenson, 1963). It would, thus, ap-
erated from the same bubble site or different bubble pear possible to use equation (29) to predict q~'r for
sites. Increasing the heat flux will lead to bubble co- FC liquids using empirical values of ~,. However, the
alescence, either vertically to form vapor columns or calculated transition values for the highly-wetting liq-
laterally to form vapor mushrooms on a heated sur- uids with an assumed 3, of 2 ° are far lower, in the
face. When the heat flux approaches critical heat range of 1-2 W / c m 2, and thus fall approximately in
flux (CHF), several mushrooms may join to form a the range of boiling incipience for these liquids (Tong,
large vapor patch. Thus, the four bubble/vapor flow et al., 1991). This unlikely result suggests that equa-
regimes are: tion (31) may be improper for highly-wetting liquids
i. Isolated bubble regime; due to their vanishingly small static contact angles
ii. Bubble column regime;
iii. Vapor mushroom regime; 20
iv. Local vapor patc h regime.
The purpose of investigating bubble flow regimes is
to identify boiling heat transfer mechanisms. For ex- 15 D 0
ample, in the isolated bubble regime, the heat trans-
it
ported from a surface can be considered to be the sum
of the latent heat carried by bubbles and the sensible q" 10"
Wa~ (Eq.M)
heat carried in bubble wakes. In the bubble column (W/cm~) W ~ (Gammer,1965)
regime, the primary contribution to the total heat re- FC-72, Ri2, RI13 (Eq. 31)
5'
moval must be by latent heat in the vapor column.
Since most boiling models, such as Rohesnow's, are
based on the isolated bubble behavior, it is desired to | ! I !

find the region for which it is valid in nucleate boiling 10 20 30 40 50


of highly-wetting liquids. AT, (K)
The value of q" which defines the boundary be-
tween isolated-bubble and bubble-column regimes is
defined as the transition heat flux. Experimental re- Fig.12 The comparison of transition heat fluxes of
sults of water show that the isolated bubble regime highly-wetting liquids and water
Avram Bar-Cohen Theoretical Aspects of Nucleate Pool Boiling with Dielectric Liquids 55

and that an alternative correlation, which is nct di- Except very low heat flux, the last term can be ig-
rectly dependent on the contact angle, is needed. nored (Tong, et al.,1990b). The predictive equation
Based on the assumption t h a t the termination of for latent heat transport from an individual bubble
isolated bubble behavior is due to the merging of con- site is
secutive vapor bubbles above the heated surface, the
upper-bound for the transition heat flux can be found
qL = -'-~--pghtgA (35)
by equating the product of the bubble departure di-
ameter and frequency to the bubble rise velocity, i.e., To determine the contribution of the sensible heat
fbDb = fib (32) by bubble wakes, the bubble wake volume, Vw, must
be determined. Defining, the influence area, Ain/, to
Using equations (28) an d (29) in equation (32), the be the equivalent area over which the entire super-
transition heat flux is found as heated layer is removed by a departing bubble, one
can define an influence area ratio, Kinl, as
q"tr = ( ~ - l)pghlo[g~( (p:l-A_'--p~g)
A,.s (30)
Kinl- Ab
2t7 .11/2 (33)
-t Db(pt + pg)' where Ab is the maximum bubble projected area on
the heated surface. The thickness of the superheated
The calculated results from equation (33) for three layer, resulting from transient heating of liquid along
highly-wetting liquids are much higher than the CHF the surface, can be expressed as
values for these liquids (Fig.13), reported in the liter-
ature. For instance, the predicted transition heat flux ~ut = ~/~/ fb (37)
for FC-72 at atmospheric pressure (P/Pc = 0.055) is
about 3 0 W / c m 2 while the CHF of saturated pool boil- Thus, the bubble wake volume becomes
ing ranges from 10.4 to 13.3W/cm 2, depending upon v. = K~.:D~6~ (3s)
the heater sizes (Saylor et al., 1989). This result sug-
gests that the isolated-bubble behavior may dominate and the sensible heat transported bythe bubble wake
the nucleate boiling regime for highly-wetting liquids. is
This analytic result has been verified by a visual and
photographic study (Tong, et al., 1991). qw = C~pIVw A A T m (39)
where
40
,,/ A T . , = C{T,,, - To) {40)
I -_-:--- Fc.=
RII3
:
it:
:

l
and C is an empirical constant. Since the average
temperature in the "pumped" superheat layer always
// / lies between Tw and T,, C ranges from 0 to 1 and may
q':,
OV/cm')
20 °
~.
;/
// be assumed to equal 0.5.
The comparison of qL and qw over a Kin! range of
2.0 to 6.3 is given in Fig.14 for FC-72. The results in-
10- dicate that in the isolated bubble region, latent heat
transport plays a dominant role at low wall super-
heat(low heat fluxes) while sensible heat transport
0 . . . . . . . •t . . . . . . . "t . . . . . . . . i . . . . . . .

.0001 001 .01 .1 0.08


P/Pc
Flg.l$ Comparison of predicted transition heat fluxes and Vw/Vb= 0 . 5 / q w / /
CHF for highly-wetting liquids 0.06

q
0.04
WAKE - PUMPING THERMAL TRANS-
PORT (W/Site)
0.02
In saturated pool boiling, heat transfer is associated
with the rise of bubble from many distinct nucleation
sites on the heated surface. The heat transfer from an 0.00
active bubble site can be considered to be the sum of 5 I0 15 20
three principal components; latent heat in the bubble AT, (K)
vapor, qL, sensible heat in the liquid of the bubble
wake, q,,, and sensible heat in liquid associated with
natural convection from non-boiling area, q,,c. Or, Fig.14 Comparison of latent and sensible heat transfer
from single bubble site for FC-72
qb = qL + qw + qne (34)
56 Journal of Thermal Science, Vol. 1, No.l, 1992

carried by bubble wakes plays the dominant role for departing bubbles dominates heat removal from the
more typical superheats. Since the K~,~! value de- heated surface. These twin findings justify the use of
creases with increasing wall superheat, sensible heat conventional isolated-bubble relations for the correla-
reduces in importance at very high heat fluxes. tion of pool boiling data.

CONCLUSIONS REFERENCES

The preceding has examined the characteristics of Bankoff, S.G., 1958, "Entrapment of Gas in the Spreading of a
vapor bubbles and nucleate pool boiling of dielectric Liquid over a Rough Surface," A/C'7~ Jour~d, 4,pp.24-26.
Cole,R, and Rohesenow, W.M.1969, "Correlation of Bubble
liquids. While these liquids possess superior electri- Departure Diameter for Boiling of Saturated Liquids," C'~mi~
cal properties, they are relatively poor coolants, with En~neering Prog~ss Sympodum Series, 65, No.92,pp.211-213.
low thermal conductivities, specific heats, and latent Danielson, R.D., Tousignant, L., and Bar-Cohen, A., 1987,
heats of evaporation. In addition, these liquids are "Saturated Pool Boiling Characteristics of Commercially Avail-
able Perfluorinated Inert Liquids," 2nd ASME/JSME Thermal
characterized by low surface tension and a high affin- Engineering Joint Conference, 3,pp.419-430.
ity for c o m m o n atmospheric gases. These properties Fritz, W., 1935, "Maximum Volume of Vapor Bubbles,"
result in substantially different vapor bubble charac- Phy~ische Z~chrifl, 36,pp.379-384.
teristics than encountered in conventional liquids and Gaertner, R.F., 1965, "Photographic Study of Nucleate Pool
Boiling on a Horizontal Surfaces," ASME Journal o.f Heat Trans-
lead to the observed anomalies in nucleate pool boiling fer, 87,pp.17-29.
behavior. Malenkov, I.G., 1968, "Detachment Frequency as a Function of
The presence of dissolved gas is known to affect Vapor Bubble," ln~. Fi~ Zhur., 20,pp.998.
the surface tension and boiling point of the liquid. Moissis, R., and Berenson, P.J., 1963, "On the Hydrodynamic
Transitions in Nucleate Boiling," ASME Journal o]Heat Trans]er,
Despite the high gas solubility of the perfluorinated 85,pp.221-229.
liquids, the surface tension for a gas-saturated liquid Murrell, J.N., and Boucher, E.A., 1982, Properties of Liquids
was found to decrease by just 1.5%, while the boil- and Solutions, John Wiley & Sons, New York.
Reid, R.C., Prausnitz, J.M., and Poling, B.E., 1987, The Prop-
ing point increase by just 0.5°C for pressures close erties of Gases & Liquids, Fourth edition, McGraw-Hill, New
to 1 atmosphere. Due to the low wetting angles of York.
the perfluorinated liquids, the advancing liquid traps Rohsenow, W.M., 1952, "A Method of Correlating Heat Trans-
a vani.shingly-small volume of gas/vapor in the surviv- fer Data for Surface Boiling of Liquids," ASME Transactions,
74,pp.73-78.
ing nucleation sites. It is the effective radius of cur- Saylor, J., Simon, T.W., and Bar-Cohen, A., 1989, "The Effect
vature of this volume, rather than the mouth-radius of a Dimensionless Length Scale on the Critical Heat Flux in
of the cavity, which establishes the boiling incipience Saturated, Pool Boiling," National Heat Transfer Conference,
superheat. The variations in wetting angle with sur- HTD-108, pp.71-79.
Schwartz, A.M. and Tejada, S.B., 1972, "Studies of Dynamic
face chemistry, direction of flow, and velocity can then Contact Angle on Solids," Journal of Colloid Interlace Science, 38,
be expected to produce large variations in the boiling pp.359-375.
incipience superheat, as reported in the literature. Thorm/ihlen, I 1986, "Superheating of Liquids at the Onset of
The surface temperature at incipience is also sig- Boiling," Proceedings, 8th International Heat Transfer Confer-
ence, Hemisphere Publishing Corporation, Washington, DC, 4,
nificantly affected by the dissolved gas content of the pp.2001-2006.
liquid. As the gas mole fraction increases, the liquid Tong, W., Bar-Cohen, A., and Simon, T.W., 1991, "Investigate
saturation temperature and the wall temperature de- of Bubble Flow Regimes in Nucleate Boiling of Highly-Wetting
crease, though at different rates. Consequently, for Liquids," 3nd ASME/JSME Thermal Engineering Joint Con-
ference, 2, pp.433-439.
fixed total pressures, an increasing gas fraction can Tong, W., Bar-Cohen, A., Simon, T.W., and You, S.Y., 1990a,
be expected to lead to larger incipience superheat but "Contact Angle Effects on Boiling Incipience of Highly-Wetting
lower wall temperatures than encountered in the boil- Liquids," lntemationol Journal o/ Hint and M ~ s T~n~er, SS,
pp.91-103.
ing of a degassed liquid. Tong, W., Bar-Cohen, A., and Simon, T.W., 1990b, "Ther-
Due to the properties of the perfluorinated, dielec- mal Transport Mechanisms in Nucleate Pool Boiling of Highly-
tric liquids, use of the Malenkov correlation reveals Wetting Liquids," Proceedings, 9th International Heat Transfer
the vapor bubbles generated during nucleate boiling Conference, 2, pp.27-32, Jerusalem, Israel.
Tong, W., Simon, T.W., and Bar-Cohen, A., 1990c, "Effect of
to be significantly smaller, to rise more slowly, and Dissolved G as on Boiling Incipience in Highly-Wetting Liquids,"
to be released at a higher frequency than found for Multi-Phase Transport and Particulate Phenomena (Veziroglu
nucleation sites in boiling water. Despite these differ- ed.), i, pp.365-387, Taylor & Francis/Hemisphere Pub.
ences, the isolated bubble regime appears to dominate Zuber, N.1962, "Nucleate Boiling. The Region of Isolated Bub-
bles and the Similarity with Natural Convection," lntern~'onal
the nucleate pool boiling of these dielectric liquids. Journal of Heat and M~ss Transfer, 6, pp.53-78.
Furthermore, for all but the lowest values of surface 3M Company,1987, Product Manual, "FLUORINERT Elec-
superheat, sensible heat transport in the wakes of the tronic Liquids," St. Paul, Minnesota.
Avram Bar-Cohen T h e o r e t i c a l A s p e c t s of N u c l e a t e P o o l Boiling w i t h Dielectric Liquids 57

Table 1. Fluid Properties at Atmospheric Pressure Boiling Point [Danielson et al. (1987)]

PERFLOURINATED LIQUID DESIGNATION


FC-77 R-113 Water
FC-72 FC-75
Property FC-87 L-1402 FC-86 FC-84 FC-104 FC-43
Boiling point
degrees C 30 51 52 83 100 172 48 100
Liquid density
pl ,kg/m 8 1633 1635 1592 1575 1590 1545 1511 958
Vapor density
pu,kg/m s 11.58 11.25 12.68 13.28 14.31 18.35 7.40 0.59
Dynamic viscosity
p ,kg/m sec 4.20E-04 5.20E-04 4.50E-04 4.20E-04 4.50E-04 3.90E-04 5.03E-04 2.70E-04
Specific heat
c,J/kg K 1088 1059 1088 1130 1172 1255 979 4184
Heat vaporization
hfg,J/kg 87927 104675 87927 79553 83740 71179 146824 2257044
T h e r m conductivity
~,W/m K 5.51F_,-02 5.96E-02 5.45E-02 5.35E-02 5.70E-02 6.50E-02 7.02E-02 6.83F_~01
Surface tension
a, N / m 8.90E-03 1.09E-02 8.50E-03 7.70E-03 8.00E-03 4.50E-03 1.47E-02 5.89E-02
Therm coef expan
fl ,K - l 1.60E-03 1.60E-03 1.60E-03 1.50E-03 1.40E-03 1.20E-03 1.70E-03 2.00E-04
Dielectric const 1.71 1.77 1.72 1.71 1.75 1.68 2.40 78.00
Average molecular
weight, gin/mole 288 299 338 388 438 670 187 18

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