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1 W
p
W
1
W1
1
jgas
j
rad
_ _
..
1
1 W
p
u j
part
1 u j
core
..
2
. 1
W describes the porosity of the packed bed. u expresses
the heat transfer between the solidsolid contact points
depending on the size of the contact surface, the state
of the surface and the elasticity of the material. The
ratios j
gas
and j
rad
(gas and radiative conduction in
the intergranular voids, respectively), j
part
(conduction
of the particle) and j
core
(average conduction of a unit
cell) are the corresponding thermal conductivities re-
lated to the thermal conductivity of the free gas (see
Fig. 6).
The rst term of Eq. (1) describes the heat transport
in the intergranular voids where only gas and radia-
tive conduction take place. In the second term are the
thermal conduction of the pure solidsolid-transfer j
part
and the thermal conduction of the core j
core
, in which
the interacting heat transfer between solid and void is ta-
ken into consideration. The coupling of radiative con-
duction, gas conduction and solid conduction as well
as the packed bed properties make up the so-called core
conductivity
j
core
2
N
Bj
part
j
rad
1
N
2
j
gas
j
part
_
ln
j
part
j
rad
Bj
gas
1 j
gas
j
part
j
rad
B 1
2B
j
rad
j
gas
B 1
1 j
gas
j
gas
j
rad
_ _ _ _
B 1
Nj
gas
_
2
with
N
1
j
gas
1
j
rad
Bj
gas
j
part
_ _
B
1
j
gas
1
_ _
1
j
rad
j
part
_ _
.
3
The deformation factor B, which enters the quantity j
core
in Eq. (1) derived from Bauer and Schlu nder (1978),
Mollekopf and Martin (1982), Zehner and Schlu nder
(1970) and Zehner and Schlu nder (1972), expresses the
strength and type of the deformation of the particles.
B = 1 expresses spherical particles; B > 1 an elliptical
shape, and B < 1 pin-point contact. A Gaussian distribu-
tion was assumed for the particle sizes; the distribution is
taken into account in the deformation factor.
In the case of a packed bed of particles that are par-
tially transparent in the infrared range like silica aerogel,
the heat transferred directly by radiation (j
direct
) has to
be taken into account as well as an additional term (see
path 3 in Figs. 5 and 6) added to Eq. (1):
j
translucentbed
j
bed
j
direct
. 4
The inuence of the packed bed properties on the
thermal conductivity is much greater than the bulk-spe-
cic thermal conductivity of the silica-aerogel, which is
itself pressure-dependent due to the nanoporous struc-
Fig. 5. Heat transfer mechanisms in a packed bed of semitransparent spheres.
R
part
R
part
R
rad
R
gas
R
rad
R
gas
R
rad
R
gas
R
rad
heat resistance of the packed bed
(1)
(1)
(2)
(2)
(3)
(3)
Fig. 6. Heat resistance model for calculating the thermal
behaviour of a translucent packed bed.
134 M. Reim et al. / Solar Energy 79 (2005) 131139
ture of the aerogel. The modied ZB model (Eq. (4))
was only used at pressures where the gas conductivity
within the aerogel bulk was fully suppressed (usually
at pressures below about 10
4
Pa (100 mbar)).
The eective thermal conductivity of a porous med-
ium of a packed bed of silica aerogel can also be
described by an empirical model considering two dier-
ent pore sizes (voids and nanopores) with a mean pore
size
d and a Gaussian pore size distribution with the dis-
tribution width w. The volume fraction of the two dier-
ent types of pores, V
d1
and V
d2
, is considered by a
weight factor W
1
= V
d1
/V, W
2
= V
d2
/V with V = total
pore volume (V
solid
(V
total
).
k
eff
A k W
1
_
1
0
GD
d
1
; w
1
1 T
room
c=p
gas
d
dd
_
W
2
_
1
0
GD
d
2
; w
2
1 T
room
c=p
gas
d
dd
_
; 5
where the constant A equals the sum of the solid
and radiative thermal conductivity, p
gas
is the gas
pressure, T
room
= 300 K is the room temperature,
c = 0.35 lm Pa/K is the accommodation coecient and
d
1
, d
2
the pore size diameters.
2.1. Eective thermal conductivity
The eective thermal conductivity depending on the
gas pressure, temperature and gas lling was measured
with our evacuable guarded hot-plate apparatus LOLA
3 (Heinemann et al., 1995). Pressure and temperature-
dependent thermal conductivity measurements were car-
ried out on sample B, a silica-aerogel granulate from
BASF AG (Broecker et al., 1986) produced from water-
glass using supercritical drying with respect to CO
2
. The
size of the aerogel granules was between about 1 and
2 mm; therefore a Gaussian distribution at 1.5 mm with
a distribution width of 2 mm was used for the calcula-
tions. Thermal conductivity measurements with diering
gas llings were carried out on translucent aerogel frag-
ments from Cabot GmbH (sample F2). In this case the
size of the granules was between 2 and 4 mm.
2.1.1. Dependence on gas pressure and external load
In the case of the evacuated solar collector the aero-
gel granulate has to withstand the atmospheric pressure,
which means an external load of 1 bar (10
5
Pa). In order
to test the mechanical stability, the packed bed was
rstly measured without load, then with 3.2 bar
(3.2 10
5
Pa) external load and nally once again with-
out load (Figs. 7ac). It can be recognized from the
packed bed thickness alonewhich does not return to
its initial value after loadingthat the granulate remains
more densely packed after the external pressure load has
been released. Fig. 7 also contains t curves according to
both models mentioned; the t parameters are shown in
Tables 1 and 2.
2.1.2. Dependence on gas type
In practice, dierent gas llings (for example, argon
or krypton) are frequently used in glazing systems. The
10
-6
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
Translucent packed-bed model (Eq. 1 and 2)
8
10
12
14
16
18
20
22
p
ex
= 10
4
Pa (0.1 bar); d = 24.4 mm
T
m
= 45C
gas conduction
suppressed in
inter-granular voids
gas conduction
suppressed only in
mesopores
Fit according to Eq. 3
p
gas
[hPa]
[
1
0
-
3
W
/
m
K
]
10
-6
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
Translucent packed-bed model (Eq. 1 and 2)
8
10
12
14
16
18
20
22
T
m
= 45C
gas conduction
suppressed in
inter-granular voids gas conduction
suppressed only in
mesopores
Fit according to Eq. 3
p
ex
= 3.2 bar (3.2*10
5
Pa); d = 19.4 mm
p
gas
[hPa]
[
1
0
-
3
W
/
m
K
]
10
-6
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
Translucent packed-bed model (Eq. 1 and 2)
8
10
12
14
16
18
20
22 p
ex
= 0.1 bar (10
4
Pa); d = 22.3 mm
T
m
= 45C
gas conduction
suppressed in
inter-granular voids
gas conduction
suppressed only
in mesopores
Fit according to Eq. 3
p
gas
[hPa]
[
1
0
-
3
W
/
m
K
]
(c)
(b)
(a)
Fig. 7. (ac) Measured and calculated thermal conductivities of
sample B depending on gas pressure at a mean temperature of
45 C, without load (0.1 bar (10
4
Pa) (a), loaded (3.2 bar
(3.2 10
5
Pa) (b) and once again without load (0.1 bar
(10
4
Pa) (c). Clearly visible are the two pressure ranges, where
the gas conduction in the intergranular voids and the mesopores
is suppressed.
M. Reim et al. / Solar Energy 79 (2005) 131139 135
thermal conductivity of the evacuated collectors micro-
porous rear side insulation depends on the kind of resid-
ual gas. Thus it is of interest to measure and calculate
the thermal conductivity depending on the gas pressure
for a packed bed of silica aerogel granules for dierent
gas llings (Fig. 8). The curves were calculated using
the modied ZB model from the t results (Table 1,
step 1). Additional measurements were performed for
dierent gases at a xed gas pressure of 1000 Pa
(10 mbar) using a dierent type of granular aerogel.
The variances between the calculations and measure-
ments are mainly caused by the dierent aerogel granu-
lates used (manufactured by BASF and Cabot), but the
potential to reduce the thermal conductivity by changing
the gas type is clearly visible.
2.1.3. Dependence on temperature
The packed beds thermal conductivity was also mea-
sured depending on temperature, with a gas pressure of
p
gas
= 100 Pa (1 mbar) and an external load of p
ex
=
3.2 bar (3.2 10
5
Pa) (Fig. 9).
The temperature dependence of the thermal conduc-
tivity is mainly caused by radiative transfer, which can
considerably exceed the heat transport via solid and
gas, since the radiative thermal conductivity k
rad
in-
creases by the third power of the absolute temperature
T for radiative diusion:
k
rad
16
3
n
2
r
e
T q
T
3
. 6
Here, n is the eective refraction index of the material
with the density q and r is the Stefan Boltzmann con-
stant. The mass specic extinction e*(T) is a tempera-
ture-dependent material value characterizing the
radiative attenuation, which should be as large as possi-
ble for eective insulation. In this sense, eective
means that the anisotropy of the scattered radiation is
taken into account.
In the infrared spectral range below 7 lm wave-
length, SiO
2
aerogels have a small extinction (see Fig.
10). The wavelength of the maximum spectral radiative
power I
Planck,max
is proportional to 1/T and therefore
Table 1
Fit-parameters (ZB-model) for the gas-pressure-dependent thermal conductivity of sample B at dierent external loads
External load p
ex
Inter-granular voids [mm] k
part
[10
3
W/(m K)] k
direct
[10
3
W/(m K)]
0.1 bar (10
4
Pa, step 1) 1.0 0.1 10.6 0.9 4.5 0.5
3.2 bar ((3.2 10
5
Pa, step 2) 0.3 0.1 6.9 0.7 4.5 0.5
0.1 bar (10
4
Pa, step 3) 0.6 0.1 7.2 0.7 4.5 0.5
The measurements were performed in the following order: without load (step 1), loaded (step 2), without load (step 3).
Table 2
Fit-parameters (empirical model) for the gas-pressure-depen-
dent thermal conductivity of sample B at dierent external
loads
External load p
ex
Inter-granular
voids [mm]
Mesopore
size [lm]
0.1 bar (10
4
Pa, step 1) 1.0 0.1 0.05 0.04
3.2 bar ((3.2 10
5
Pa, step 2) 0.3 0.1 0.05 0.04
0.1 bar (10
4
Pa, step 3) 0.6 0.1 0.05 0.04
10
-4
10
-3
10
-2
10
-1
10
0
10
1
krypton
CO
2
argon
air
CO
2,
measured
11
12
13
14
15
16
17
kr, measured
air, measured
evacuated
p
gas
[hPa]
[
1
0
-
3
W
/
m
K
]
Fig. 8. Thermal conductivity of sample F2 depending on gas
pressure for a packed bed of silica aerogel granules for dierent
gas llings at room temperature.
50 100 150 200 250 300 350
0
10
20
30
40
50
60
70
80
90
measured values
p
ex
= 3.2 bar (3.210
5
Pa)
p
gas
= 100 Pa (1 mbar)
model
Temperature [C]
[
1
0
-
3
W
/
(
m
K
)
]
Fig. 9. Measured and calculated total thermal conductivity of
sample B depending on the temperature at 3.2 bar (3.2 10
5
Pa)
external load and a gas pressure of 100 Pa (1 mbar).
136 M. Reim et al. / Solar Energy 79 (2005) 131139
shifts into this spectral range with increasing tempera-
ture. At the same time, the total radiant exitance in-
creases considerably ($T
4
, not visible in Fig. 10 due to
normalization). In order to take this into account the
Rosseland-averaged specic extinction (Fig. 11) was
used to calculate the temperature-dependent radiation
conduction (j
direct
) in the ZB-model. For this calcula-
tion the t results (Table 1, step 3) were used, the
temperature dependence of k
direct
was determined
according to Eq. (6).
2.2. Optical properties and structure
The directional-hemispherical transmittance and
reectance of the aerogel granulates were measured with
an integrating sphere arrangement in a wavelength range
from 400 nm to 2000 nm (Reim et al., 2002). Packed
beds of silica aerogel with dierent thicknesses were
investigated between two highly transparent glass panes.
The transmittance of the aerogel alone was calculated
(taking multiple reexions into account)for a 10 mm
packed bed see Table 3. For calculating dierent day-
lighting and solar control systems, the transmittance
and reectance of the PMMA double skin sheet was
measured and the absorptance was calculated.
In the visible spectral range the absorptance is lower
than 5%, absorptance of the aerogel and the PMMA oc-
cur in the near infra-red.
The light scattering behaviour was examined on sin-
gle rotating granules with a HeNe-laser (wavelength
543 nm). Structural information resulted from these
measurements and from small angle X-ray scattering
(SAXS and USAXS) (Reim et al., 2004).
Both semi-translucent aerogels show nearly the same
nanostructure, the dierence in the scattering behaviour
is caused by their macroscopic shape. The surface of the
spheres contains cracks and scratches, so the spheres
have a lower transmittance. The nanostructure of the
translucent aerogel is dierent from the semi-translucent
material. The bulk material of the translucent aerogel is
relatively homogeneous without any large clusters, in the
semi-translucent material there are clusters in a size
range from 10 nm to 17 nm (Reim et al., 2002). Decisive
for the high translucence is the structure between 5 nm
and 100 nm (scattering vector between q = 0.01 nm
1
and q = 0.2 nm
1
), in this size range the scattering of
the semi-translucent aerogels is much stronger than for
the translucent ones.
3. Results and discussion
Using the measured thermal and optical properties of
the granular aerogel samples the performance of the sys-
tems investigated can be determined.
3.1. Aerogel glazing
The visual, solar and total energy transmittance and
the U-value of aerogel glazing can be calculated using
standard procedures (ISO 9050, 1990). Table 4 shows re-
sults for dierent types of low-e-coated glass, aerogel
and gas lling. The range given indicates the dierent
aerogel types investigated (visual transmittance and g-
value) or gas llings (U-value). The daylighting system
2 4 6 8 10 20
10
-4
10
-3
10
-2
10
-1
SiO
2
aerogel
200C
20C
0.0
0.2
0.4
0.6
0.8
1.0
Wavelength [m]
S
p
e
c
i
f
i
c
e
x
t
i
n
c
t
i
o
n
[
a
r
b
.
u
n
i
t
s
]
r
e
l
.
i
n
t
e
n
s
i
t
y
Fig. 10. Spectral radiative power density I
planck
for tempera-
tures of 20 C and 200 C, normalized to a maximum value of
one, and spectral extinction of a SiO
2
aerogel monolith.
100 1000
0.00
0.05
0.10
0.15
50C 350C
T [K]
e
[
m
2
/
g
]
Fig. 11. Rosseland-averaged mass specic extinction of a SiO
2
aerogel depending on temperature.
Table 3
Measured solar and visual transmittance of a 10 mm thick
packed bed of aerogel granules without cover panes
Sample Description s
nh,solar
s
nh,vis
F2 Translucent
fragments
0.88 0.04 0.85 0.04
F1 Semi-translucent
fragments
0.72 0.04 0.65 0.04
S Semi-translucent
spheres
0.53 0.04 0.43 0.03
M. Reim et al. / Solar Energy 79 (2005) 131139 137
combines a very low U-value with a high visual transmit-
tance. For the solar control glazing glass panes with a
dierent low-e-coating were used in order to get a low
g-value.
3.2. Solar collector
At an average temperature of 60 C the evacuated
solar collector lled with aerogel granules has a heat
transfer coecient of about 1.4 W/(m
2
K) at the front
and about 0.5 W/(m
2
K) for the 1 cm thick porous insu-
lation at the back (total heat loss is about 1.9 W/(m
2
K)).
Comparing this with a conventional at-plate collector
with a 4 mm white glass pane at the front (solar trans-
mittance 0.89) and a selective absorber (for example,
Interpane Sunselect with solar absorptance 0.96, emis-
sivity 0.05), the heat loss through the front is about
2.4 W/(m
2
K) and 0.8 W/(m
2
K) through the back
(5 cm mineral wool). The aerogel collector not only
has a 3 cm smaller system thickness than the conven-
tional at-plate collector but also 40% less heat loss.
When integrating the collector into a roof construc-
tion, the U-value of the whole system is important (for
example, for heat loss at night). Here, the aerogel collec-
tor has a heat transfer coecient of about 0.35 W/
(m
2
K) compared with the conventional at-plate collec-
tors with 0.56 W/(m
2
K). By increasing the thickness of
the back insulation to 4 cm, the U-value of the whole
system can be reduced to passive building level for roof
insulation (0.15 W/(m
2
K)) at a system thickness of only
about 6 cm. This corresponds to the U-value of a 25 cm
thick mineral wool insulation.
4. Conclusions
The optical properties of silica aerogel granulate
packed beds have been investigated, also with respect
to their structure. The inuence of the structure on the
directional-hemispherical transmittance s
dh
is due to
the fact that there are no clusters in the highly-translu-
cent granulate (s
dh,solar
= 88%, s
dh,vis
= 85%, at 10 mm
packed bed thickness) in the range between 5 nm and
100 nm. The semi-translucent granulates (s
dh,solar
6
72%, s
dh,vis
6 65%, at 10 mm packed bed thickness) con-
tain clusters in the range between 10 nm and 20 nm
(Reim et al., 2002). The semi-translucent, spherical gran-
ulate has a more scratched surface than the semi-trans-
lucent granulate fragments. These scratches reduce the
transmittance by another 10%. A daylighting system
using these aerogels achieves a heat transfer coecient
of less than 0.4 W/(m
2
K) and a total solar energy trans-
mittance between 17% and 45% with a thickness of less
than 50 mm. This aerogel glazing has already been inte-
grated into facades, and has turned out to be a visually
attractive, light-scattering daylighting element with ex-
tremely low energy loss during the heating period. To
use silica aerogel granulate in a at-plate collector, a
heat transport model for packed bed granulate was up-
graded for semi-transparent, non-grey media and veri-
ed using gas-pressure and temperature-dependent
thermal conductivity measurements. The focus was on
the packed bed properties of the aerogel. Good agree-
ment was achieved despite simplifying the coupling of
the individual heat transport mechanisms in the mono-
lithic part of the granulate. The heat transport proper-
ties of the packed bed dominate the resulting eective
thermal conductivity.
Acknowledgements
This work was supported by the Bayerische For-
schungsstiftung (Munich) within the project ISOTEG
and by Cabot GmbH (Kempten, Germany).
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Calculated visual directional-hemispherical transmittance and total energy transmittance (g-value) for systems with semi-translucent
and highly translucent aerogel granulate
s
nh,vis
g-value U-value (W/m
2
K)
Daylighting system
(two low-e-coatings 0.08)
0.240.54 0.330.45 0.440.56
Semi-translucenttranslucent Semi-translucenttranslucent Kryptonargon
Sun protection system
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0.190.38 0.170.23 0.370.47
Semi-translucenttranslucent Semi-translucenttranslucent Krypton-argon
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