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SUPERCRITICAL HEAT TRANSFER

Jackson, J. D.
DOI:10.1615/AtoZ.s.supercritical_heat_transfer
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Physical Properties Near the Critical Point
The principal difference in the behavior of a fluid as its temperature is raised above the
critical temperature is evident from the pressure-volume diagram shown in Figure 1. Below
the critical temperature T
c
the variation of pressure p and volume v along an isotherm shows
discontinuities where the isotherm intersects the saturation line. Phase change occurs at the
saturation line, and the horizontal constant pressure segment of the isotherm represents the
presence of vapor and liquid in varying proportions. The critical temperature isotherm has
zero slope at one point, the pressure there being the critical pressure, p
c
. Above the critical
temperature, isotherms show no discontinuity and from a macroscopic standpoint there is a
continuous variation from a liquid-like fluid to a gas-like fluid.

Figure 1.
Since the pressure variation across most thermal boundary layers is negligible, it is the
variation of properties along an isobar that is important. The variation of specific volume v,
specific heat c
p
, absolute viscosity , thermal conductivity and specific enthalpy h for water
at pressure of 245 bar is shown in Figure 2 The temperature at which the specific heat reaches
a peak is known as the pseudocritical temperature, T
pc
. As the pressure is increased this
temperature increases, the maximum value of the specific heat falls, and the variation of the
other properties becomes less severe.

Figure 2.
Forced Convection Heat Transfer at Supercritical Pressure
Convective heat transfer near the critical point is characterized by properties having rapid
variation with temperature. As a consequence, the flow and heat transfer processes are linked.
Moreover, the equation describing the temperature distribution in the fluid is essentially
nonlinear, so that the proportionality between heat flux and temperature difference no longer
exists; in these circumstances heat transfer coefficient is a parameter of doubtful utility which
can take widely differing values depending on the conditions.
Forced convection heat transfer measurements in pipes to fluids at supercritical pressure have
been made using a wide range of fluids: water, carbon dioxide, nitrogen, hydrogen and helium
are examples. By far the most extensive collections of data are for water and carbon dioxide,
and fortunately the accuracy of physical property data for these fluids is good. The incentive
for work on water has been its use in supercritical pressure "boilers" for power stations,
particularly in the U.S.A. and the U.S.S.R. For the experimentalist carbon dioxide is an easier
fluid to handle because of its lower critical temperature and pressure (31C and 73.8 bar,
compared with 370C and 221 bar for water).
Several reviews of supercritical pressure forced convection have been written: for example,
Petukhov (1970), Hall (1971) and Hall, Jackson (1978). This account is largely based on the
last of these.
General Characteristics
Low heat fluxes
At very low heat fluxes, and therefore with small temperature variations in the fluid, one
approaches the case of constant properties. Their actual value in this small temperature range
will, of course, depend upon where the temperature lies in relation to the critical temperature.
Thus, while the physical properties may remain almost uniform throughout the fluid, they
may be made to traverse a wide range of values by adjusting the bulk mean temperature of the
fluid in the limiting case of a very small heat flux. There is no reason why constant property
equations should not work. Consider the well-known expression
(1)

where Nu is the Nusselt Number (= D/), Re is the Reynolds Number (= D/), and Pr is
the Prandtl Number (=c
p
/), in which is Heat Transfer Coefficient and is mass flow rate
per unit area.
From this it follows that
(2)

Noting that the variations with temperature, of the thermal conductivity , and the viscosity
are rather similar in form (Figure 2), one would not expect a major effect on the heat transfer
coefficient on this account. The specific heat, on the other hand, becomes very large in the
vicinity of the pseudocritical temperature, and one might expect the heat transfer coefficient
to behave in a similar manner. This, in fact, happens, as is well illustrated by the data of
Yamagata et al. for water (Figure 3). It will be noted that as the heat flux increases the
magnitude of the peak in the heat transfer coefficient decreases. This is because the region of
fluid at high Prandtl Number contracts as the heat flux, and hence the temperature gradient,
increases.

Figure 3.
I ntermediate and high heat fluxes
Heat flux is not the sole determinant of the effects, which are about to be described. However,
for a given size and orientation of pipe and a given flow rate, the effects are very largely
determined by heat flux. Under some conditions the orientation of the pipe becomes
important, and very different results are obtained depending upon whether the pipe is
horizontal or vertical, and whether in the latter case the flow is upwards or downwards.
In cases where orientation is not important the deterioration in heat transfer coefficient with
heat flux that was evident in Figure 3 becomes more marked both with decreasing mass
velocity and increase of heat flux. Figure 4 shows the water data of Vikhrev et al. for a
constant mass flow and three levels of heat flux, the highest of which results in virtually no
enhancement of a as the bulk temperature traverses the pseudocritical temperature.

Figure 4.
Turning to data in which the orientation of the pipe is important, we find that under some
conditions of pipe diameter, mass flow and heat flux, heat transfer to a fluid is much better in
a vertical pipe when the flow is in the downward rather than upward. When it was first
observed, this behavior was difficult to reconcile with the currently held view that forced and
free convection reinforced each other when they acted in the same direction. An example of
this behavior is shown in Figure 5 where the data of Jackson and Evans-Lutterudt for carbon
dioxide at two different heat fluxes are shown for both upward and downward flow. It will be
seen that there is a rapid deterioration in heat transfer following a relatively small increase in
heat flux with upward flow but not with downward flow.


Figure 5.
An interesting comparison between carbon dioxide data that is unaffected by the direction of
flow and with data that is so affected is shown in Figure 6. All three sets of data have been
selected so that, in the absence of any gravitational effect, they would be expected to yield
similar distributions of wall temperature against bulk enthalpy. In the case of one set of data
(due to Shiralkar and Griffith), no difference between upward and downward flow was found,
whereas the other two sets (due to Jackson and Evans-Lutterudt and Bourke et al.) showed
such a difference. The sharp temperature peaks appear to be characteristic of upward heated
flows in which gravitation is important. Note that, following these peaks, heat transfer is
better than it would have been in the absence of gravitational effects, and also that in
downward flow there is substantially improved heat transfer with no wall temperature peaks.

Figure 6.
A Criterion for buoyancy affected flow
The examples of the effect of orientation of the pipe that have been quoted above confirm the
importance of interactions between forced and free convection. The sharp peaks in the wall
temperature that occur with upward heated flows were first attributed to "pseudofilm boiling".
The true nature of the phenomenon was revealed when results for both upward and downward
flow became available, and it is now possible to say with some confidence whether it is likely
to occur in given circumstances. The exclusion of data affected by buoyancy is clearly
necessary preliminary before any attempt can be made to correlate data for pure forced
convection.
An explanation of the mechanism by which buoyancy affects heat transfer has been proposed
by Hall and Jackson (1969). The dominant factor is the modification of the shear stress
distribution across the pipe, with a consequential change in turbulence production.
It can be shown that a criterion for negligible buoyancy effects is
(3)

where is the Grashof Number (= g(
b
)D
3
/ ), in which is the integrated mean
density and the subscript b indicates physical properties evaluated at the local bulk
temperature.
The application of the above criterion is made difficult by the fact that evaluation of the
Grashof Number requires that the wall temperature T
w
is known, so that in applications where
the wall heat flux is specified a correlation describing forced convection heat transfer (with
negligible buoyancy effects) must be used in conjunction with the criterion.
Forced Convection in the Absence of Buoyancy
The enhancement of heat transfer coefficient at small temperature differences when the bulk
temperature is close to the pseudocritical temperature has already been noted and attributed to
the large value of c
p
in this region. As the temperature difference is increased, the proportion
of the flow experiencing this high specific heat shrinks, and the heat transfer coefficient is
reduced. If we take the temperature difference as the main factor affecting enhancement of the
heat transfer coefficient (for a given fluid and bulk temperature) then it follows that the effect
should be characterized by a quantity such as . Attempts have been made to express the
ratio of the heat transfer coefficient to that for constant properties in terms of the quantity
; typical of these are the generalized curves of Lokshin for water at 250 bar (Figure 7). It
is seen that above a value of 0.7 no enhancement occurs and there is a monotonic
decrease in a as the fluid bulk temperature traverses the pseudocritical temperature.

Figure 7.
Many attempts have been made to correlate forced convection data in terms of conventional
dimensionless groups with modifications to allow for the effect of physical property variation.
Jackson et al. (1975) have made a study of virtually all known correlations and have
compared their performance when tested against forced convection data for water and for
carbon dioxide. The fact that they were able to exclude data that may have been affected by
buoyancy constituted an important advance over earlier attempts to correlate forced
convection data. They found that by far the most effective correlation was that published in
1965 by Krasnoschekov and Protopopov (1966). This utilizes the Petukhov-Kirrillov equation
for constant properties forced convection and accounts for property variation by additional
terms involving wall to bulk density ratio and integrated to bulk specific heat ratio, each
raised to suitable powers. It correlated 80% of the data points to within 15% and 91% to
within 20%. Because the Petukhov-Kirrillov equation was rather cumbersome to use
Jackson and Fewster also tried the following simpler version in which a Dittus-Boelter form
of constant properties forced convection equation is used instead:
(4)

where suffix w refers to conditions at the wail,

and




In this form the equation correlated 77% of the data points to 15% and 90% to within
20%. Approximately 2000 data points were tested against the correlation.
Mixed Convection in Pipes
Vertical pipes
This topic has already received some discussion and a criterion for the onset of buoyancy
effects has been given. Also the tendency towards the sudden occurrence of localized peaking
of the wall temperature in upward flow with increase of heat flux has been noted. In view of
this instability it is not surprising that the magnitude of the subsequent increase in wall
temperature (for conditions of specified heat flux) has proved difficult to predict. For a
detailed picture of the influences of buoyancy on heat transfer to fluids in vertical pipes,
including fluids at supercritical pressure, see Jackson and Hall (1980).
For a downward heated flow there is a continuous enhancement in heat transfer as buoyancy
becomes relatively stronger. This behavior has been found with many fluids at supercritical
pressure and also with other fluids. Not only is the heat transfer improved, but wall
temperatures are less sensitive to heat flux.
Horizontal pipes
As might be expected, buoyancy in uniformly heated horizontal pipes causes a progressive
increase in the temperature of the upper surface relative to the lower surface of the pipe. This
is undoubtedly due in part to a stratification of the flow, the hotter and less dense fluid
occupying the upper part of the pipe; there may also be an effect due to the damping effect of
the stabilizing density gradient on turbulence near the upper surface of the pipe. At the lower
surface heat transfer is frequently better than for forced convection alone, suggesting that
there may be some amplification of turbulence by the destabilizing density gradient in this
region. For a detailed review of the effects of buoyancy on heat transfer to fluids flowing in
horizontal tubes, including fluids at supercritical pressure, see Jackson (1983).
A considerable number of measurements on horizontal pipes have been made using fluids at
supercritical pressure. A typical set of data presented by Belyakov et al. is reproduced in
Figure 8. The deterioration of the upper surface occurs progressively along the pipe and does
not show the sharp peaks that are obtained with upward flow.

Figure 8.
Free Convection
Free convection in supercritical pressure fluids has received a good deal less attention than
has forced convection, presumably because there have been fewer pressing industrial
applications. The situation was reviewed by Hall (1971), and little further data have been
reported since that time.
The general picture is one of enhancement of heat transfer at low heat fluxes with surface and
fluid temperature spanning the pseudocritical temperature. As with forced convection, the
enhancement is greatest when the bulk temperature is close to the critical temperature, but
there is no evidence of the impairment of heat transfer that is found at high heat fluxes with
forced convection.
Boiling
Nucleation at high subcritical pressures
Nucleation at a boiling site of a given size becomes easier as the pressure of a boiling liquid
increases. The decrease of surface tension means that a smaller difference between vapor and
liquid pressure is required in order to make a nucleus grow; moreover, a given pressure
difference can be achieved with a smaller superheat as the pressure level increases. For a
given superheat, therefore, it will be possible to activate smaller nuclei at higher pressures.
In addition to this effect, there is the possibility of spontaneous nucleation occurring as a
result of thermal fluctuations in a superheated liquid at a surface as p/pc approaches unity.
Indeed, it may be that the very "quiet" transition to film boiling that occurs at high pressure
may be a consequence of spontaneous nucleation.
Pool boiling
The effect of pressure on nucleate boiling is well established: as the pressure is raised towards
the critical pressure the heat transfer coefficient increases, and the limiting heat flux for
transition from nucleate to film boiling first increases, reaches a maximum at a value of p/pc
of about 0.35, and then decreases.
Pool boiling experiments at high pressures show very clearly how the range of conditions
under which nucleate boiling occurs is contracted by transition to film boiling.
Following transition to film boiling at pressures close to the critical value, a highly regular
flow of vapor from the heated surface is observed. At p/p
c
0.9 uniformly spaced columns of
bubbles are observed to rise from a heated wire. As the critical pressure is approached these
columns change into "tubes" of vapor, again with very regular spacing, and finally change
further into what appears to be a sheet of vapor rising from the wire.
Flow boiling
As indicated earlier, the general picture of supercritical pressure forced convection has
become comparatively clear. In contrast, very few detailed investigations have been made at
high subcritical pressures.
Figure 9 shows data for water flowing upwards in a 20-mm diameter pipe for pressures
extending from subcritical to slightly supercritical, taken from the work of Herkenrath et al. It
is of interest to compare the subcritical curves, each of which involves a local heat transfer
crisis, with the curve for supercritical pressure, which does not. Note that the conditions are
such that buoyancy induced temperature peaks would not be expected in the case of the
supercritical data.

Figure 9.
It will be seen from Figure 9 that as the pressure is increased the position of the heat transfer
crisis shifts towards the region of lower quality; the magnitude of the wall temperature step at
first decreases, then increases and finally decreases as the critical pressure is approached.
Furthermore, the shape changes from a sharp to a more gradual increase in wall temperature.
Some data obtained by the present author and co-workers using carbon dioxide at a reduced
pressure, p/p
c
= 0.99, for both upward and downward flow showed an increase in wall
temperature following transition which was rather gradual (the curve for p = 215 bar in
Figure 9) and that in upward flow peaks develop due to buoyancy influence as they do at
supercritical pressure. It was also apparent that at high subcritical pressures downward flow
was advantageous, just as at supercritical pressures: transition occurred later in downward
flow and the consequences were less severe. Experiments with carbon dioxide at lower
pressure show a sharp transition rather similar to those illustrated in Figure 9.
The beneficial consequences of buoyancy in downward flow do not appear to persist as the
pressure is dropped further, where the above mentioned trend appears to be reversed.
References:
Hall, W. B. (1971) Heat transfer near the critical points, Advances in Heat Transfer, Vol. 6,
Academic Press, New York.
Hall, W. B. and Jackson, J. D. (1969) Laminarisation of a turbulent pipe flow by buoyancy
forces, ASME Paper No. 69-HT-55.
Hall, W. B. and Jackson, J. D. (1978) Heat transfer near the critical point, Keynote Lecture,
Sixth International Heat Transfer Conference, Toronto, Canada.
Jackson, J. D. (1983) Effects of Buoyancy on Heat Transfer to Fluids Flowing in Horizontal
Heat Tubes, Proc. H.T.F.S. Research Symposium, University of Bath, Paper RS 471, 97-115.
Jackson, J. D., Hall, W. B., Fewster, J., Watson, A., and Watts, M. J. (1975) Heat Transfer to
Supercritical Pressure Fluids, H.T.F.S. Design Report No. 34, Part 1Summary of design
recommendations and equations, Part 2Critical reviews with design recommendations,
AERE-R8157 and R8158, U.K.A.E.A., AERE, Harwell.
Jackson, J. D. and Hall, W. B. (1980) Influences of buoyancy on heat transfer to fluids
flowing in vertical tubes under turbulent conditions, 563-611, Turbulent Forced Convection in
Channels and Rod Bundles, published by Hemisphere Publishing Corporation, USA (S.
Kakacs and D.B. Spalding, Eds.)
Krasnoschekov, E. A. and Protopopov, V. S. (1966) Experimental study of heat exchange in
carbon dioxide in the supercritical range at high temperature drops, Teplofizika Vysokikh
Temperatur, Vol. 4, No. 3.
Petukliov, B. S. (1970) Heat transfer and friction in turbulent pipe flow with variable physical
properties, Advances in Heat Transfer, Vol. 6, Academic Press, New York.

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