Cryogenics 31( 1997) 305-3 12

0 1997 Elsevier Science Ltd

Printed in Great Britain. All rights reserved
PII: SOOll-2275(97)00023-4 001 l-2275/97/$17.00

Thermal conductivity of polyurethane

foams from room temperature to 20 K
Chung-jen Tseng *, Masahito Yamaguchit and Takao Ohmorit

*The New Energy and Industrial Technology Development Organization, Sunshine

60, 29F, l-l, 3 chome Higashi-lkebukuro, Toshima-ku, Tokyo 170, Japan
tAdvanced Technology Department, Research Institute, Ishikawajima-Harima Heavy
Industries Co. Ltd, 1 Shin-nakahara-cho, Isogo-ku, Yokohama 235, Japan

Received 5 December 1996; revised 20 January 1997

The thermal conductivity of the polyurethane (PU) foam in the temperature range
between 300 and 20 K is investigated theoretically and experimentally for the develop-
ment of liquid hydrogen storage tanks. An experimental set-up based on the JIS stan-
dard A1412 is built to measure the thermal conductivity of the foams under various
temperature and pressure conditions. An analytical model, including the contributions
from radiative heat transfer, is used to predict the thermal conductivity of the PU
foams. The model is found to be able to accurately predict the thermal conductivity
of the PU foams under normal and reduced pressures. The thermal conductivity of
the PU foam can be reduced by as much as 70% by evacuating the gases in the foam
cells. Radiative heat transfer is found to account for about IO-20% at room tempera-
ture. The thermal conductivity data below 90 K are available for the first time. 0 1997
Elsevier Science Ltd.

Keywords: thermal conductivity; liquid hydrogen; polyurethane foam; insulation

Nomenclature Greek letters

Accommodation coefficient
A, Coefficient defined in Equation (4)
Extinction coefficient (m-')
d Mean pore diameter (m)
Constant defined in Equation (5)
H Insulation thickness (m)
; Porosity
k Thermal conductivity (W m-'K-')
f7 Stefan-Boltzmann constant (5.6696 x
k Boltzmann’s constant (1.38 x lo- 23J K-‘)
10H8W me2 Ke4)
k,, Monatomic value of thermal conductivity
5 Molecule diameter
Kn Knudsen number (Z/d)
1 Mean free path (m)
L Heater length (m) Superscripts and subscripts
M Molecular weight (kg kmol-‘)
Refractive index C Convection
F Pressure (N rnm2) eff Effective
9 Heat flux (W m-2) g Gas
Q Heater power (W) in Inner surface
R Radius (m) out Outer surface
T Temperature (K) r Radiative
X Mole fraction S Solid
Z Axial coordinate t Total

Introduction storage pose a new challenge to engineers due to its

Hydrogen will become one of the primary energy sources
in the 21st century. It offers a non-polluting, inexhaustible,
efficient, and potentially cost-effective energy system.
However, large-scale liquid hydrogen transportation and
extremely low temperature (20 K). High performance ther-
mal insulation systems are required. The polyurethane (PU)
foam is chosen as one of the candidates for the insulation
system because it offers a high strength-to-weight ratio, low
thermal conductivity, and low cost. Currently, the thermal

Cryogenics 1997 Volume 37, Number 6 305

Thermal conductivity of polyurethane foams: C. Tseng et al.
conductivity data of PU foams are available only for tem-
peratures above 95 K’. This work will provide the thermal
conductivity data for temperatures down to 20 K. Heat
transfer mechanisms in PU foams are studied to help better
understand the thermal performance of PU foams.
Heat transfer mechanisms
The PU foam used in this study has a closed-cell porous
structure and a density of 32 kg mp3. The average diameter
of the cells is approximately 400 pm (see Figure 1).
Heat is transferred through the PU foam via four mech-
anisms: (1) gas conduction qg, (2) solid conduction qS, (3)
radiation qr, and (4) convection qc. The total heat flow qt
is a result of the interactions between the four modes:
Natural convection within the pores is negligible since
the pore size is so small ( < 0.5 mm) that the Rayleigh
number is much less than the critical value ( - 1000) for
the onset of convection.
Radiative heat transfer
Radiative heat transfer refers to the transport of energy by
electromagnetic waves and attenuation of radiation takes
place in the forms of reflection, absorption, and scattering.
Resins used for making PU foams are partially transparent
in the 2 to 30 pm range of wavelength?. Sections associa-
ted with thermal insulations, however, are normally
optically thick (optical thickness>>photon mean free path).
The optical thickness is defined as PH, where p is the
extinction coefficient ( = scattering coefficient + absorption
coefficient) and H the insulation thickness. Tien and Cun-
nington3 stated that the extinction coefficient of a 35 kg me3
PU foam is about 3000 m-‘. More recently, Stem4 used an
infra-red spectrometer to measure the transmission, and
then deduced the extinction coefficient of PU foams. His
results ranged from 2040 m-’ for 28 kg mm3 samples to
4250 m-l for 43 kg m-3 samples. In this work, the extinc-
tion coefficient is taken as 3000 m-’ for the 32 kg me3 sam-
ple used.
Figure 1 Microscopic view of the pore structure of a 32 kg m3
polyurethane foam
306 Cryogenics 1997 Volume 37, Number 6
For optically thick media, radiation can be considered as
a diffuse process with an effective radiative conductivity
given by?
k = 16nQT3
r (2)
3P
where n is the refractive index of the insulation, g is the
Stefan-Boltzmann constant (5.6696 x lo- ’ W m-2 K- 4).
and T is the mean temperature of the insulation. For such
(optically thick) systems, radiation and conduction contri-
butions can be effectively separated6.
Solid conduction
Solid conduction is due primarily to two mechanisms: lat-
tice vibrations, and translation of free conduction electrons.
The free-electron contribution dominates in the energy
transport in metals and the lattice vibration contribution is
predominant in dielectric solids. The disordered dielectrics
with no free electrons and considerable lattice imperfection
are the poorest solid conductors of heat, and consequently
most porous insulations are made of materials such as glass
or polymeric plastics.
Solid conduction in PU foams takes place through the
cell walls and membranes of the foam. Since PU resins
are made up of disordered materials, there is little lattice
conduction at low temperatures. The only currently avail-
able thermal conductivity data of pure PU is cited by
Kikuike7 as 0.17-0.23 mW m-’ K-’ at room temperature.
Figure 2 shows the thermal conductivity of three polymers,
Teflon, nylon, and polyvinyl chloride (PVC), which are
available for cryogenic temperatures8*9.The curve for PVC
is obtained by a polynomial fitting of available data
(denoted by the ‘ + ’ symbols) and the zero point. Because
all three curves have similar temperature dependence trend,
and the thermal conductivity of PVC at 300 K is closest to
the value cited in reference 7, it will be used in this work
as the pure solid thermal conductivity.
Gas conduction
The remaining mode of heat transfer is gas conduction in
the foam cells. The PU foams used in the present study are
expanded by CO, and HCFC 141b (R141b)‘O. Figure 37
shows the partial pressures of the major gas components
for a PU foam expanded by Rll and CO,. Initially only
CO, and Rl 1 are present in the cells. While CO, soon dif-
fuses out of the cells due to its high diffusivity, Rll
remains almost unchanged because of its very low diffusiv-
ity. Air has a diffusivity approximately 20 times larger than
that of Rl 1. It diffuses into the cells continuously and
reaches about 50 kPa after 35 days. Eventually, the air par-
tial pressure will reach 1 atm. No similar data is available
for the CO, and R141b system of the sample used”, how-
ever. Because the sample used in this work had been stored
for more than a year at the time of measurement, the air
pressure is assumed to be 100 kPa at 300 K in the analytical
model. The partial pressure of R141b at 300 K is not known
for the experimental sample. Although it is thought to be
lower than the partial pressure of Rl 1 (50 kPa) due to the
lower vapour pressure and diffusivity of R141b, no data is
available. Several values were used in this study to best fit
the measurement results.
 Thermal conductivity of polyurethane foams: C. Tseng et al.

250

0 50 100 150 200 250 300 350

Temperature (K)

Figure 2 Thermal conductivity of Teflon9, nylong, and PVC?

80

60 - Total

0 5 10 15 20 25 30 35 40

days
Figure3 Cell gas pressure variation with time for a 25 mm thick PU foam sample blown by CO2 and RI1

The thermal conductivity of the major gases found in where the Xi are mole fractions of the species, and the ki
the insulating foams is shown in Figure 4. The thermal are the thermal conductivities of the corresponding species.
conductivity data of R141b is obtained from a recent work Equation (3) usually overestimates the mixture thermal
by Tanaka et al. ’ ‘. The conductivities of Rl 1, NZ, and O2 conductivity, especially for non-polar-polar and polar-
are obtained from Touloukian et cd.*. It can be seen from polar gas mixtures, such as the air-R14lb system in the
the figure that while the thermal conductivity of R141b is present case. For such cases Reid et al. I2 recommend the
slightly higher than that of R 11, both are much lower than use of the modification of Wassiljewa equation of Mason
that of N, and Oz. The values of the thermal conductivities and Saxena.
shown in Figure 4 are used in the numerical calculation in The Wassiljewa equation takes the form
this study.
When a mixture of gases is present, the gas conductivity kp = i X&i
kg can be estimated by ___, Aji= 1 (4)
‘=’ -&A,
j=1
k, = ~ Xiki (3)
i=l where A, is a function to be specified.

Cryogenics 1997 Volume 37, Number 6 307

 Thermal conductivity of polyurethane foams: C. Tseng et al.

G- 25

-t- R141b gas

0 50 100 150 200 250 300 350

Temperature (K)

Figure 4 Thermal conductivity of commonly used gases*

Mason and Saxena suggest the following form for Ati:

(7)
A,. = 4l + (kr,iiktij )"*(Mi/Mj )“4l2
I/ (5)
[8( 1 + MiIM,)]‘”

The effective gas thermal conductivity at reduced press-

where M is molecular weight, k, is the monatomic value ures is then
of the thermal conductivity, and E is an empirical constant.
The details can be found in Reid et al.‘*.
k,’ = ak,&
Due to the very low temperature involved in this work,
the partial pressures of individual gases may be low enough
that pressure dependence of the gas conduction needs to be where Q is the accommodation coefficient. The accommo-
considered. The voids could be cryopumped for tempera- dation coefficient is a measure of the efficiency of the ther-
tures near 20 K. The various regions of gas conduction can mal energy interchange that occurs when a gas molecule
be defined according to the Knudsen number, Kn = lfd collides with the surface. It may vary between 1 (complete
where I is the molecular mean free path, and d the charac- accommodation, diffuse re-emission) and 0 (specular re-
teristic length of the physical system (the pore size in the emission).
present case)3:

1. Kn> 10, free molecule, Effective thermal conductivity

2. 0.1 < Kn < 10, transition,
By considering the effects of void space and solid walls,
3. 0.01 < Kn < 0.1, temperature-jump (slip) region,
Russell13 proposed the following equation for calculating
4. Kn -=c0.01, continuum.
the effective (apparent) thermal conductivity keff of a
porous medium:
The mean free path can be calculated by

kT krr = k
l=---- (6)
Jp2?r P
where 4 is the porosity of the foam.
where k is Boltzmann’s constant (1.38 x 10 - 23 J K-l), & is No data of 4 of the PU foams used in the experiment is
the molecule diameter, and P is the pressure of the gas. available. The manufacturer (Nichiasu Co. Ltd) suggests
Due to its extremely complicated nature, gas conduction in using the density of the PU foam and that of pure PU resins
PU foam insulations defies any rigorous quantitative ( - 1100 kg mm3) to estimate the porosity’“. Therefore, for
description and semi-empirical representation becomes the 32 kg me3 foams, 4 is approximately 0.97.
necessary. A convenient semi-empirical technique is based The above equations do not take into account radiation.
on the use of an effective mean free patb3, which takes into As mentioned previously, conduction and radiation can be
account both the molecule-to-molecule and molecule-to- treated independently for this optically thick medium.
wall collisions: Therefore the radiation contribution can be accounted for

308 Cryogenics 1997 Volume 37, Number 6

 Thermal conductivity of polyurethane foams: C. Tseng et al.

by using the radiative thermal conductivity k, as defined in
Equation (3).
The final form of the equation for calculating k,, can be
expressed as:
k =k _ 4J’+Al-4’) 16n2aT3
eff
“+Q+Al-$J’+9)+ 3p
Thermal conductivity measurement
This section describes the experimental set-up and pro-
cedure used to measure the thermal conductivity of PU
foams from room temperature down to liquid hydrogen
temperature (20 K) under atmospheric pressure and evacu-
ated condition.
Experimental set-up
An experimental apparatus has been built to measure the
k,, of the PU foams. The steady cylindrical method is
employed. It is based on the JIS standard A1412. As shown
in Figure 5, the system consists of a test section which is
placed in a vacuum chamber, a vacuum pump, a two-stage
GM refrigerator, a digital recorder, a temperature control-
ler, and a computer. The test section is a sealed vessel
placed horizontally. The initial pressure in the test chamber
can be set at various values.
Details of the test section are shown in Figure 6. The
test samples are hollow cylinders, 400 mm long, with inner
and outer diameters of 30 and 70 mm, respectively. A film
heater is stuck to the inner surface of the test sample with
GE varnish. It is joule heated by a d.c. power supply. The
film heater is made of Nichrome foil, 0.1 mm thick and
300 mm long. High conductive alumina powder is used to
fill the space inside the heater, so that a uniform tempera-
ture can be realized on the heater surface. At both ends of
the test sample, fibre glass insulator and the same PUF are
(10) used to reduce heat loss. Copper-made cooling plates are
used to enclose the outer surface of the sample which is
connected to a constant power GM refrigerator. The tem-
perature of the cooling plates is controlled by adjusting the
temperature of the refrigerator with a heater embedded in
the cold head.
The inner and outer surface temperatures are measured
by using Celnox sensors (Lake Shore Cryotronics Inc.).
These sensors are of resistant thermometer type and have
a wide operating temperature range (about l-325 K) with
an accuracy of 0.02 K at 20 K and 0.14 K at 300 K. Four
sensors are placed on each surface. A radiation shield is
also placed in the vacuum chamber and is connected to the
first stage of the GM refrigerator, thus reducing radiative
heating from outside the test section.
Experimental procedure
In this work, a 32 kg rnM3sample was used in the measure-
ment. Two sets of measurements were performed. In the
first set, the test section (inner chamber) was cooled from
300 K at atmospheric pressure down to 20 K gradually, and
then back up to 300 K again. In the second set, the inner
chamber was connected to the outer chamber by drilling
several holes on the inner chamber, so that the inner
chamber could be evacuated. The same sample was evacu-
ated for three weeks at 300 K before being cooled down.
There were no observable difference (cracks, fallen pieces,
etc.) of the sample before and after the experiment.

Refrigerator
temperature
controller

Data Recorder

--.--.-.-
Temperature sensor leads

-I A’- Turbo
Molecular pump 56 C/s

GM Ref

Radiation shield Rotary pump

Vacuum chamber (volume 86 C )

Experimental setup
Figure 5 The experimental set-up for the thermal conductivity measurement

Cryogenics 1997 Volume 37, Number 6 309

 Thermal conductivity of polyurethane foams: C. Tseng et al.

10

-
8 6 1 2 3 4 5 7

1. Test chamber Copper cooling plates

2. Test sample End insulator (PU foam)
3. Film heater Fibrous insulation
4. Alumina powder Refrigerator head
Temperature sensors

Test section
Figure 6 Details of the test section

The procedure starts with setting the refrigerator tem-

perature. The heater power is then set to a value so that (12)
the temperature difference between the inner and outer sur-
faces of the sample is approximately 10 K. The tempera- where the conductivity is a function of position. The control
tures are obtained by measuring the resistance of the ther- volume approachi is employed to numerically solve the
mometers, and then converting the resistance data to above equation with Q and outer surface temperature values
temperatures using the resistance-temperature calibration from the experimental measurement. The inner surface tem-
data. The computer calculates the temperatures continu- perature is used as a way to verify the numerical model.
ously. If the change in the temperatures is less than 0.1 K The uncertainty of the measurement can be estimated
within a 30 min span, steady state is assumed and the tem- from the error propagation equation of Equation (11):
peratures and the heater power data are recorded. Eleven
readings are recorded for each steady-state temperature. It
usually takes an additional 30 min to log the data. The (!z)‘=(!g+(!?q+(!s)
refrigerator is then set to another temperature, and the pro-
cess is repeated.
The whole process is controlled by the computer so that
the measurement can be performed 24 h a day. It usually
+(Ri
lI120/Ri,)2
+(Rc ln’~JRi))*
(13)

takes 6- 12 h to obtain one data point.

The uncertainty of the thermal conductivity measure-

Data deduction ment, Sk/k, is found to be approximately 10%.

The steady cylindrical method is adopted in this measure-

ment. The thermal conductivity can be calculated by the
Results and discussion
following equation:
By using the numerical simulation, end heat loss is found
k _ Q ln (Rout/&n) to be approximately 7.5% of total power input. This end
eff 23rL (Tin - T,,,,)
(11)
heat loss has been accounted for in the results presented
hereafter.
where Q is the heater power, L is the length of the heater, Figure 7 shows the thermal conductivity measurement
Ri” and R,,, are the radii of the inner and outer surfaces, results along with the theoretical predictions for the case
respectively, and Ti” and To,, are the average temperatures that the sample was cooled from 300 K at atmospheric
of the inner and outer surfaces, respectively. pressure. The uncertainties of the measurement data are
The heat loss through both ends of the sample can be indicated by vertical bars. At around room temperature, the
estimated by solving the two-dimensional steady-state heat thermal conductivity decreases with temperature as
conduction equation: expected. However, it increases as temperature further

310 Cryogenics 1997 Volume 37, Number 6

 Thermal
Temperature
Figure 7 Comparison of theoretical predictions of thermal conductivity
decreases from about 270 K due to the condensation of the
lower conductivity gas, R141b (which, in turn, increases
the mole fraction of the higher conductivity gas, air). The
R141b completely condenses at about 230 K, and the ther-
mal conductivity decreases as temperature decreases
further. At around 50 K, air starts to condense, and solid
conduction becomes the only mode of heat transfer
below 40 K.
As for the theoretical model, results for three different
initial R141b partial pressures are shown in the figure for
comparison. The accommodation coefficients are assumed
to be constant with values of 1.0 and 0.6 for R141b and
air, respectively. As mentioned previously, air pressure at
300 K is assumed to be 100 kPa for all three cases. All
three cases converge below 230 K when R141b completely
condenses. Between 220 and 250 K, all three cases under-
estimate the thermal conductivity. Above 260 K, the
30 kPa-R14lb case fits the measurement data quite well
while the 10 kPa-R14lb case overestimates and the 50 kPa-
R141b case underestimates. This is because R141b has a
lower thermal conductivity than air. The fact that the
30 kPa-R14lb case fits the measurement results best is in
accordance with the estimation that the R141b initial partial
pressure is lower than 50 kPa, as discussed previously.
Figure 8 shows the thermal conductivity results for the
evacuated case. Clearly, most cell gases were evacuated as
the thermal conductivity was reduced sharply when com-
pared with the previous case. However, a small amount of
residual gas remains in the foam cells. This can be seen
from the higher measured values than the completely
evacuated values predicted by the model (shown by the
dashed line). The thermal conductivity decreases monoton-
ically from about 14 mW m-r K-’ at 300 K to about
6 mW m-’ K-’ at 150 K, and about 1 mW m-r K-’ at 20 K.
The reversal in the 230-280 K region of the previous case
shifts to the 150-180 K region in this case because of the
much lower pressure in the cells (and hence the conden-
sation temperatures).
For this low pressure case, the mean free paths at 250 K
conductivity of polyurethane foams: C. Tseng et al.
Pair =lOOkPa
r, measurement
I R141b 10 kPa
-+-R141b30kPa
----O- .- R141b 50 kPa
W)
with measurement results. Atmospheric pressure case
for N2 and O2 are 600 and 2600 pm, respectively. There-
fore, they are limited by the pore size of 400 pm. The ther-
mal conductivities of N2 and O2 are thus further reduced.
On the other hand, the mean free path at 250 K for R141 b
is about 6 pm, much smaller than the pore size. Hence the
thermal conductivity of R141b is almost unaffected by the
pore size limitation. So R141b is the dominant gas in the
foam cells in this temperature region. The R141b starts to
condense at about 200 K. However, it still dominates in this
region, so the thermal conductivity of the foam continues
to decrease. At about 170 K, the R141b condenses to such
an extent that it no longer dominates, and hence the reversal
occurs again. The R141b completely condenses at about
150 K, and the thermal conductivity decreases with tem-
perature again. The theoretical model slightly overpredicts
the thermal conductivity from 50 to 130 K.
The contribution of radiation is indicated in the figure
by the dashed line. It is negligibly small below 150 K, but
accounts for about 20% of the effective thermal conduc-
tivity at 300 K.
Due to the various processing conditions, methods, and
blowing agents used in expanding PU foams, the thermal
conductivity data in the high temperature region (above
200 K) may not be applicable to other samples. However,
the data in the low temperature region should be applicable
to most 32 kg m-3 closed-cell PU foams because conduc-
tion by air and solid dominates in this region. These data
are very useful for cryogenic applications.
Conclusions
The heat transfer mechanisms in a PU foam are reviewed
and discussed. An experiment has been set up to measure
the thermal conductivity of PU foams for temperatures
down to 20 K. An analytical model is proposed to estimate
the thermal conductivity of the PU foam. The results are
compared with the measured values. Heat loss in the experi-
ment is analysed numerically. Based on the results, the fol-
lowing conclusions can be drawn.
Cryogenics 1997 Volume 37, Number 6 311
Thermal conductivity of polyurethane foams: C. Tseng et al.

25 - 0 measurement

- R141b 0.8 kPa Air 0.02 kPa

20 - - - R141 b 0 kPa Air 0 kPa

Krad

15 -

10 -

5-

0 50 100 150 200 250 300 350

Temperature (K)
Figure 8 Comparison of theoretical predictions of thermal conductivity with measurement results. Evacuated case

1. The theoretical model proposed in the study predicts the help and support of the Engineering Advancement
the thermal conductivity quite well. The discrepancy Association of Japan (ENAA) and Ishikawajima-Harima
in the high temperature region can be ascribed to either Heavy Industries Co. Ltd (IHI).
the uncertainty of the gas composition inside the cells,
the pure solid conductivity, or the radiative properties References
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uating the gas can greatly improve the thermal per- Standards, Boulder, CO, 1984.
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Chem. Eng. Prog., 1961, 57, 55-59.
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Siegel, R. and Howell, J.R., Thermal Radiation Heat Transfer, 3rd
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with as much CO, as possible if it is to be evacuated, Wang, L.S. and Tien, CL., A study of various limits in radiation heat
such as when used in the thermal insulation system of transfer problems. ht. J. Heat Mass Transfer, 1967, 10, 1327-1338.
a liquid hydrogen storage tank because the diffusivity Kikuike, S., Rigid polyurethane foam insulations. Japan Industrial
Standards Explanation, Tokyo, Japan, 1991
of CO, is much higher than that of R141b.
Touloukian, Y.S., Liley, P.E. and Saxena, S.C., Thermal Conduc-
5. The thermal conductivity data of pure PU solid is tivity, Thennophysical Properties of Matter. IFI/Plenum, New
needed for more accurate theoretical predictions of the York, 1970.
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Plenum Press, New York, 1989, p. 75.
10. Inamoto, M., Private communication, Nichiasu Co. Ltd, Tokyo,
Japan, 1997.
Acknowledgements 11. Tanaka, Y., Nakada, M., Kuboda, H. and Tokita, K., The thermal
conductivity of HFC134a, HFC143a, HCFC14lb, and HCFC142b
This study was performed as part of the WE-NET gases. Proc. 1989 Symp. of the Japanese Refrigeration Association,
(International Clean Energy Network using Hydrogen 1989, pp. 9-12 (in Japanese).
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312 Cryogenics 1997 Volume 37, Number 6