ELSEVIER

Temperature Effects Influencing the

Spectral and Total Emissivity of Refractories
J. J. P. Elich
J. A. Wieringa*
Del Universityof Technology,
Department of Applied Physics,
Del, Zhe Netherlands

wThe spectral reflectivity of some refractories has been measured. This has
been done to obtain specific (instead of general) data that will be used in
the modeling of radiative heat transfer in furnaces. The measurements
were performed using an integrating sphere method. Because of the lack of
a diffuse reference sample for longer wavelengths, a procedure was developed for the use of a specular reference sample. Although the individual
reflectivities follow the general trend, two characteristics features can be
reported. Refractory material that has not been heated yet has a higher
reflectivity than heated material in the spectral range 2.5-4 pm. This is
attributed to water absorption. Refractory material that came from the
inner side of a combustion
chamber of a glass melting furnace showed
different
reflectivity behavior for wavelengths
smaller than about 5 pm
than that of material of the furnace wall originating from a position about
20 cm away from the inner side. The hemispherical
emissivity as a function
of temperature
is lowered by the first effect and increased by the second.

The magnitude of the effects can be up to 20%.

Keywords: spectral reflectivity, integrating sphere method, refiactoly,
temperature dependence, total emissiuity.

INTRODUCTION
In modeling radiative heat transfer there is a choice
between a gray approximation
and a spectral treatment.
The latter makes the calculations more complicated but is
sometimes necessary to gain good insight, for instance, in
the analysis of radiation exchange in an enclosure with a
flame [l, 21. The specific case of a regenerative natural gas
fired glass melting furnace has been studied by us [3-51.
In such a high-temperature
furnace the radiative heat
transfer from the flame to the melt is the dominant means
of heat transfer. Post [61 concluded that the convective
flux is even less than 1% of the total flux.
We will elucidate the importance
of a spectral treatment of the walls using Fig. 1. The radiation from a
nonluminous
flame is mainly emitted in the infrared by
the combustion gases H,O and CO,. The emission and
absorption of nonluminous
flames is in certain bands that
can be described by band models [7-lo]. Owing to the
spectral properties of the gas, the refractory emissivity is
expected to influence radiative heat transfer. If the refractory emissivity is low, most of the banded flame radiation
is reflected. The wavelength distribution
is unchanged by

*Currently at Unilever Research Laboratorium, Vlaardingen, The

Netherlands.
Address correspondence
The Netherlands.

reflection, and the reflected flux is strongly absorbed again

in the emission/absorption
bands of the gas. If, on the
other hand, the refractory is dark, most of the flame
radiation is absorbed and reemitted in a more continuous
wavelength distribution.
The transparent
wavelength regions of the flame spectrum will transmit a great part of
this flux. The conclusion is that a dark refractory material
promotes heat transfer. A partly compensating effect will
be that the flame becomes less hot so that the direct flux
from the flame to the glass is decreased.
Thus, good knowledge of the spectral emissivity of a
refractory will enhance the accuracy of modeling results.
Of course, there have been many publications
on the
optical properties of a variety of materials ([ll-151 and
the references therein). Such publications give the trend
of the spectral behavior for refractories. However, one is
sometimes forced to measure the properties oneself, for
instance, in the case of specific material from a manufacturer, a surface treatment, or a material history [16].
For the modeling of a glass melting furnace we have
measured the reflectivity of a few specific refractories
using the integrating sphere method. This is a well-known
method (see, e.g., the survey article of Sacadura [17]) and
is also applied in commercial apparatus. However, a problem can arise in the choice of the reference sample. We
discuss this further on in a survey of the experimental
errors, after a description of the experimental
setup. In

to Dr. J. J. Ph. Elich, Department of Applied Physics, Delft University of Technology P.O. Box 5046, 2600 GA Delft,

fiperimental
Thermal and Fluid Science 1995; 10:318-326
0 Elsevier Science Inc., 1995

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Spectral and Total Emissivity of Refractories

319

refractory

Figure 1. Schematic

representation
of the initial radiative
fluxes in a glass furnace. The figure shows a cross section of
the combustion chamber. Qd, direct flux from the flame to
the glass; Q,, flux via the refractory.
the Measurement
Results section, some results are presented that give some insight into the temperature
dependence and thermal aging of the spectral reflectivity of
refractories. After a general discussion, attention is paid
to the calculation of the temperature
dependence
of the
total emissivity.
EXPERIMENTAL

SETUP

Figure 2 shows the experimental equipment schematically.

The light of the source (I) is focused by two mirrors (M,
and M,) into the entrance of a monochromator
(3). The
radiation transmitted
in a wavelength band is reflected
into the integrating sphere (4) by three mirrors CM,--M,).
In the sphere the incident radiation hits the sample (81,
which is either the reference or the sample of unknown
reflectivity.
Two light sources were used. A quartz tungsten-halogen
lamp was used for the wavelength region 0.67-3 pm. In
the further infrared, from 3 to about 10 pm, an electrically heated ceramic element was used.
The monochromator
was an Oriel7240, with a long-pass
filter placed behind the exit slit. To cover the whole
spectral range, four gratings and additional filters were
used.
The integrating sphere was constructed by our departments workshop. A sketch of the sphere is given in Fig. 3.
The cross section shows the position of the beam entrance
port, sample port, and detector port. The diameters of
these ports are 2.2, 2.0, and 0.7 cm, respectively, and the
inner diameter of the sphere is 20 cm. To obtain a diffuse,
high-reflectivity
sphere wall, the brass sphere had first
been roughened by blasting with glass balls and subsequently coated with a gold layer of about l-pm thickness.
The upper part of the sphere is a ceramic ring. If
measurements
are performed with the sample at elevated
temperature,
the sample is placed in a furnace on top of
the sphere (see Fig. 4). The ceramic ring has an insulating
function, but the sphere is also cooled with water. The
upper part of the sphere has a hollow wall, and the lower
part has cooling pipes on the outside. The furnace is
cylindrical and, in addition to having heat reflection shields
and insulation outside, has a ceramic holder for the heating wire. Inside this heating device is a massive tantalum
cylinder resting upon the sample for conductive heating.
The sample hangs in a tantalum sample holder with an
angle of 8 between sample normal and incident beam.
Two reference samples were used. A diffuse sample
(Spectralon manufactured
by Labsphere) with a reflectivity close to 1 was used for wavelengths up to 2.5 pm. For

Figure 2. Experimental setup for the measurement of the

near-normal hemispherical reflectivity. 1, Infrared source; 2,
chopper; 3, monochromator; 4, integrating sphere; 5, detector; 6, chopper control; 7, lock-in amplifier; 8, sample;
M,-M,, mirrors.
longer wavelengths a gold sample (a gold layer of 0.4 pm
deposited by evaporation on a glass substrate) was used.
This is discussed further on when a comparison of the use
of these samples at low wavelengths is given.
The influence of absorption by H,O and CO, in the
sphere was avoided by flushing it with nitrogen during the
measurements.
The detector is a Golay type (Cathodeon IR50) with a
KRS-5 window, usable in the wavelength range from 0.4
pm to the far infrared. The opening angle of the field of
view (FOV) is 60 (see Fig. 3).
The electronic system for the data acquisition is shown
schematically in Fig. 5. To eliminate to a great extent the
influence of unwanted radiation or stray light, a chopper is
placed close to the entrance slit of the monochromator;
the operating
frequency
is 9 Hz. A lock-in amplifier
(EG & G 5104) is used to attenuate higher frequencies at
12 dB/octave. The output signal of the amplifier is digitized by a data logger (Doric Digitrend 240) at a sampling
rate of 10 Hz. The data are stored in a Hewlett-Packard
computer and processed further later on. At each wavesample

inputbaam

Figure 3. Schematic cross section of the integrating

320

J. J. P. Elich and J. A. Wieringa

Figure 4. Cross section of furnace on

top of the sphere. 1, Ceramic holder for
heating wire; 2, massive titanium cylinder; 3, ceramic insulation plate; 4, sample; 5, tantalum sample holder; 6, thermocouple lead-through; 7, heating wires
lead-through; 8, insulation; 9, tantalum
radiation shields; 10, heating wire with
separate inner and outer spiral windings;
11, upper side integrating sphere, 12,
cooling channel and water supply to
upper part of sphere.
length the output of the lock-in amplifier is read a number
of times, typically 30 or 60. This permits the calculation of
an average and other statistical variables.
The wavelength can be selected automatically
by the
computer. The position of the grating in the monochromator is adjusted by a stepper motor operating on the same
principle as a servo recorder.
ESTIMATION

OF EXPERIMENTAL

ERRORS

With the wavelength selection as just described, a certain

required wavelength can be obtained with an uncertainty
smaller than 0.1% (including zero point error and deadband [ 183).
Drift may appear in both the source and the detector.
The drift has been examined but is negligible over a
period of several hours. The detector non-linearity
is
specified to be less than 1%. Below 2.5 pm the standard
deviation in the signal was low, less than 0.1% of the
signal, except at the smallest wavelengths. Above 2.5 Mm,

there is a larger spread in the signal. Up to 10 pm the

standard deviation is of the order of 0.5% except when the
sample reflectivity is extremely low. In those cases, and
above 10 pm, the standard deviation can increase to a few
percent.
Besides the errors in precision, errors in accuracy can
occur. In the following some possible sources of error are
discussed. This is done with room-temperature
measurement in mind. The error in the sample temperature is also
discussed.
Sample Substitution
In our measurement
procedure the sample is replaced by
a reference
in order to compare them (substitution
method). In the substitution
method a systematic error
exists because the mean sphere wall reflectivity is changed
when a sample is replaced by the reference. The mean
sphere reflectivity j?, is defined as

(1)
interface

t
stepper
motor

slide
resistor

monochromator
datalogger

detector
lock-in amplifier

I
HP9000

Figure 5. The electronic part of the experimental equipment.

The chopper is placed close to the entrance slit of the
monochromator. The stepper motor adjusts the wavelength.

where pw is the sphere wall reflectivity (which is assumed

to be uniform over the wall), pi is the reflectivity of port i,
and fi is the fraction of the sphere area occupied by
port i.
The effect of the change in the mean sphere reflectivity
has been
treated
by, for example,
Jacquez
and
Kuppenheim
[19] and Hanssen [20]. When a diffuse sample and diffuse reference are compared in the substitution
method, we can write [19]

-Qds,A =

Ps,n(l

Q:', A

Pr,*(l

Pw,J
i&A)

(2a)

Spectral and Total Emissivity of Refractories

Table 1. Dimensions

of the Integrating

Sphere

Diameter (cm)

Area (cm2)

2.0
0.7
2.2
20.0

3.1
0.4
3.8
1257*
1249+

Sample port
Detector port
Entrance port
Sphere

Equating the two expressions for Q, at a certain wavelength yields a value for +I~ that is given by

*Including ports.
Excluding ports.
instead

of

K,

PI, A

Here Qd is the flux incident on the detector, and the

subscripts r and s denote the use of the reference or
unknown sample, respectively. The dependence
on wavelength is indicated by a subscript. For our geometry (see
Table l), and assuming a wall reflectivity of 0.96, the
maximum relative error when using Eq. (2b) instead of
Eq. (2a) is found to be 4% for a sample reflectivity ps = 0.
In the absolute sense, the largest error will occur for
ps = 0.5, having a value of 0.01. Therefore, no correction
was applied for the sample substitution.
Because the
sphere wall reflectivity is close to 1, such a correction
would also have a high inaccuracy due to the uncertainty
of L,,, I and &,,, h.
Unequal

Directional

Behavior

of Sample

and Reference

If the sample and reference are not both perfectly diffuse

or specular, more errors can in principle arise, especially
when the detector field of view (FOV) is not hemispherical. Hanssen [20] gives expressions for the sphere throughput for various cases. For specular samples, extreme situations occur if the beam that is reflected by the sample falls
either inside or outside the FOV.
Because a calibrated, diffuse standard in the wavelength
region above 2.5 pm was not on hand, a specular reference sample was used in this region. This was a 0.4-pm
gold layer deposited by evaporation on a glass substrate.
To minimize the error of using a specular reference, we
directed the orientation
of the sample (and therefore the
reflected beam) in such a way that the detector response
was equal to that of our diffuse reflection standard in the
wavelength region below 2.5 pm.
With the diffuse reflection standard (reference l), the
spectral flux Q, incident on the dectector is given by [20]

Q::=fd

P,&fv,

_;

1 A
w,r ,

where fd is the fraction of the sphere surface occupied by

the detector, prl,* is the reflectivity of reference 1, QR is
the incident flux on the reference sample, and f, is the
fraction of the sphere area that is inside the FOV.
The specular gold reference (r2) gives a flux
Qr: =fdPrz,diPw,A

where 77~is the fraction

falling into the FOV.

%
+f,,

_p;A,,
W,I >

of the specularly

reflected

321

(4)

beam

If pr2, &,, p,, and f, are independent

of wavelength, the
specular gold sample can be used as if it were the diffuse
standard at the wavelength where the two fluxes with both
references are made equal by rotating the specular sample. Since the reflectivity of gold is nearly constant above
2.5 wrn and the FOV is determined
by the detector
geometry, it was assumed that this is indeed possible. In
practice it appeared to be possible to reproduce with
reasonable accuracy (within 3%) the same flux with the
gold sample and the diffuse sample for A between 0.8 and
2.5 Frn.
Dark Sample

Reading

Error

An error that appears to be significant in our equipment is

the dark sample reading error 1211. This error arises
because part of the incident radiation comes onto the
sphere wall as a halo of stray light around the sample.
This is especially important when the sample reflectivity is
low. The effect has been measured by removing the sample and is on the order of 2% of the detector response
with the reference sample. This error has been corrected
for.
Polarization

of Incident

Radiation

When the incident beam hits the sample at a direction far

from the normal, polarization
of the incident radiation
can play a role [17]. The reason for this is that reflectivities are, in principle, different for the two components
(parallel and perpendicular
to the plane of incident radiation). Equations derived from electromagnetic
theory are
given by Siegel and Howell [8], for instance. With the
values given in their Tables 4-2 and 4-3 we find differences between the two components of reflectivity of less
than 0.3%. At lower wavelengths where the reflectivity
decreases below 0.98 (which occurs below 0.8 pm), this
difference increases to much higher values.
Sample

Flatness

The samples that have been used are

follow the curve of the integrating sphere.
another error. This error is, however, an
tude smaller than the error due to sample
and has therefore been neglected.

flat and do not

This introduces
order of magnisubstitution [191

Temperature
The measurements
at elevated temperature
were performed at sample temperatures
of about 500 and 700C.
The uncertainty
in the sample surface temperature
is
estimated to be respectively about 50 and 100C. The
temperatures
and their uncertainty follow from an extrapolation of two temperatures
measured behind the sample.
In the following the sample temperature
can be regarded
more as a qualitative measure than as a quantitative one;
it does not affect the conclusions.

322

J. J. P. Elich and J. A. Wieringa

IMPLEMENTATION
ESTIMATION

OF CORRECTION
OF UNCERTAINTY

Table 2. Survey of the Refractory Samples

and Their Composition

AND

In accordance with the above considerations,

the comparison of the sample and the reference is implemented in the
following way. For each wavelength the spectral, 8 hemispherical reflectivity pi of the sample is found from

(6)
where U, and U, are output values from the lock-in
amplifier for the sample and the reference and U, is the
voltage with empty sample holder. In this way we corrected for the dark sample error.
To assess the accuracy of the measurements,
the reflectivity of a Spectralon diffuse sample with
=
was
compared
the
The
flectivity was
with
diffuse reference with
with
gold reference. The
are
P = 1 as well
shown in Fig.
The difference between expected and
measured values is less than
only
wavelengths
were larger deviations
due to
relative increase in
influence
the lower
output
the detector.
the grating and/or
the
had to be replaced. The
gave good agreement. The error
few
hundredths.
The total experimental
the reflectivity
and
Below 1 pm
uncertainty
due to
statistical spread.
2.5 pm
uncertainty
also
becomes
the
of a specular
and because
The
uncertainty
the case
low reflectivity, the
the dark sample reading
and
uncertainty
For very low
the relative uncertainties
can
few tens
the error is still no
more than

o.44
0.5

1. 0

1. 5

2. 0

0.6

2. 5

Sample

Material

Composition (mass%)

1. Furnace brick,

Silica

2. Furnace brick,
inner side
3. Belret silica
VMA
4. Zs 65AA

Silica

96SiO,, 2.6 CaO,

0.5 Al,o,,
0.2 Fe,O, (avr.1
See Sample 1.

Silica

See Sample 1.

Zirconium silicate

5. Stella GG
6. Belret Super

Silica
Silica
(purer)

32 SiO,, > 63 ZrO,

< 1.5 HfO
See Sample 1.
> 96 SiO,

flame side

The foregoing figures hold for room temperature

results. During measurements
at elevated temperatures
the
uncertainty
increases. We return to that during the presentation of these measurements.
MEASUREMENT

The above-described
experimental equipment was used to
measure the spectral, near normal hemispherical
reflectivity pf of refractory samples. In the following, results
are presented for four refractories
as delivered by the
manufacturer
and for two samples taken from a refractory
brick that came from the inner side of a glass melting
furnace after several years of operation. In Table 2 some
data about the composition are given, to the extent known
to us.
Samples 1 and 2 were taken from the same brick.
Sample 1 came from the part of the brick that was at the
inner side of the combustion chamber, facing the flames.
This part of the refractory is the hottest, and some chemical or physical changes have taken place here. An important part can be played through
contamination
by
volatilization products originating from the melt or batch
blanket [22]. Sample 1 looks light gray, nearly white to the
eye. Sample 2 came from the opposite side of the brick,
which was about 20 cm away from the combustion chamber side. This sample appears brown to the eye. All other
samples were taken from new brick, and these appear
brown, some speckled with gray. Although samples taken
from the same kind of bricks show somewhat different
colors, some duplicate measurements
on another sample
from the same material, or on the same sample after
rotation around the surface axis in the sample holder,
showed no significant difference.
Results from the measurements
were converted to the
spectral near-normal
emissivity l
i according to

Gm)

Figure 6. Comparison of measured spectral, near-normal

hemispherical reflectivity p,f of a gray diffuse reference
using a white diffuse reference (-1
and specular gold
reference (---) with manufacturers specifications ( 1.. ). The
right ordinate shows the reflectivity; the left ordinate shows
the allied emissivity Q to facilitate comparison with the
following figures. The vertical scales show only part of the
domain (0, 1).

RESULTS

e;=
Room-Temperature

1 -p;.

(7)

Results

The results of measurements

at room temperature
are
shown in Figs. 7-9 together with additional results from
measurements
with a Perkin-Elmer
spectrophotometer
of

323

Spectral and Total Emissivity of Refractories

sample 1
....,...
sample 1 (TNO)
-.-.-sample
2
-----samnk
2 ITNO
-

I1

OO

I
10

Figure 7. Spectral near-normal emissivity ET of samples 1

and 2, as obtained from the measured near-normal hemispherical reflectivity. Results obtained with our equipment
and with the TN0 equipment are indicated.

Figure 9. Spectral near-normal emissivity Q of samples 5

and 6, as obtained from the measured near-normal hemispherical reflectivity. Results obtained with our equipment
and with the TN0 equipment are indicated.

the TN0 Institute

of Applied Physics in Delft. The
Perkin-Elmer
instrument
is a double-beam
spectrophotometer with an integrating sphere of 60 mm coated with
BaSO,. Reflectivity is also measured at an angle of 8. The
uncertainty
of results obtained with this equipment
is
estimated to be about 5%. In the overlap region with our
measurements,
from 0.67 to 2.5 pm, emissivity values
follow the same pattern, but the mean level of the TN0
results is in general higher than our results. Taking into
account the uncertainties
of both results, there is no
significant difference, so they can be judged to agree [23].
Although the results are discussed further below, one
special aspect has to be mentioned now. This comes from
a comparison of samples 1 and 2 in Fig. 7. In the optical
region the emissivity of sample 1 stays more or less at the
same level, whereas the emissivity of sample 2 decreases
with increasing wavelengths. This explains the white and
brown appearance.
Most striking, however, is the difference in the region l-5 pm. The difference
between
samples 1 and 2 can be attributed to the fact that sample
1 stayed at a higher temperature
and had direct contact
with the combustion gases and vapors in the furnace; it
does not show the intrinsic temperature
dependence of a
refractory material. The emissivity in this region, and so a

possible temperature
dependence,
greatly influences the
radiation exchange between gas and walls in furnaces.
Therefore, additional measurements
were performed to
investigate this temperature
dependence.

i-.
.
1

o,6

High-Temperature

Measurements

Measurements
were performed at higher temperatures,
mostly at about 500 and 700C. A temperature
dependence of the spectral reflectivity was not found in the case
of previously heated samples, that is, those that had been
heated to a temperature
of 500 or 700C for some hours
before the measurements
were made. This can be seen in
Figs. 10-12, where results are given for three refractories.
Because the measurements
with our equipment
were
rather time-consuming,
the reflectivity was measured only
from about 1.4 to 6 pm. During these measurements
the
noise level of the detector was higher than during roomtemperature
measurements,
The estimated error in the

&+.J

\:?:
.y .,i J

El
0.4

01
0

.ii-

.
-.-.---

samle
sa&le

3
3 (TNO)
sample 4
sample4(TNO)

--

0.2 -

I
OO

1
10

Gm)

Figure 8. Spectral near-normal emissivity eI; of samples 3

and 4, as obtained from the measured near-normal hemispherical reflectivity. Results obtained with our equipment
and with the TN0 equipment are indicated.

I
1

I
2

T, -20 C. not heated before

Ts EJ20 C. heated before
Ts = 5OOC, heated before

-_

It

I
5

I
6

Wn)

Figure 10. Sample 3. Spectral near-normal emissivity Q as

obtained from the measured near-normal hemispherical reflectivity. Sample temperature T, during the measurement
and heat treatment: (-1
Room temperature, sample never
heated; (---I room temperature, sample heated before; (...I
about 5OOC,sample heated before.

324 J. J. P. Elich and J. A. Wieringa

0.2 -

I
0

I
2

T, x 20 C, not heated before

--_Ts ;e 20 C, heated before
. . . . . . . Ts = 5OOC, heated before
-.-._
Ts z 70 C, heated before
I
I
I
I
I
I
4
6
3
5
A&m)

Figure 11. Sample 4. Spectral near-normal emissivity Q as

obtained from the measured near-normal hemispherical reflectivity. Sample temperature T, and heat treatment: (---_)
Room temperature, sample never heated; (---I room temperature, sample heated before; ( ... 1 about 500C sample heated
before; (-.-I about 700C sample heated before.
reflectivity is 0.05 in the absolute sense for the regions
below 1 pm and above 2.5 pm.
For comparison, in Figs. lo-12 the room-temperature
results are also given for each material as obtained from
the manufacturer.
DISCUSSION

OF MEASUREMENTS

The room-temperature
results of all samples show similar
behavior. The trend of low emissivities up to about 2.5 pm
and higher values at higher wavelengths is found for many
refractory oxides such as MgO, Al,O,, and SiO,Zr [24,25].
Our results are very similar to the silica refractory results
of Bauer and Steinhardt [261 and the sand results given in
the survey of Touloukian
and Dewitt [12], including the
peak at 3 pm and the dip at 9 pm.
Comparison
of the room-temperature
results in Figs.

1.0

7-9 and the high-temperature

results in Figs. lo-12 shows
a significant difference in the region from 2.7 pm to about
3.5 or 4 pm. We checked refractory Sample 4 using X-ray
diffraction to see if there was a change in composition
after heat treatment. No difference was found.
Our hypothesis is that the change in spectral reflectivity
after heat treatment is due to dehydration of the samples.
Water will be bound to the refractory material in the
original refractory, and water molecules have a strong
absorption in the 2.5-3.5 pm region. Water also absorbs
in bands around 1.4 and 1.9 pm and in the region 4.5-8.5
pm. However, the absorptivity of the two bands at lower
wavelengths is low. Unfortunately,
the broad band from
4.5 to 8.5 pm is partly outside our measurement
domain.
Because no significant difference is found between 4.5 and
6 pm, the absorption
of the refractory is apparently
dominant in this region.
PRACTICAL

SIGNIFICANCE

Total emissivities can be calculated as a function of temperature using the spectral reflectivity or spectral emissivity. If it is assumed that the spectral emissivity is independent of temperature,
the total emissivity is calculated by

(8)

with E,,h the blackbody emissive power or Planck distribution. As we have measured the spectral near-normal
hemispherical
reflectivity pt,
we will obtain by Eqs. (7)
and (8) the total near-normal emissivity E. Because of the
weak angular dependence
in the neighborhood
of the
normal direction, this can be taken as the value for the
total normal emissivity. The practical significance of our
study is that the influence of the measurement
procedure,
the way of calculation,
and the influence of extended
exposure at the inner side of a furnace on the calculated
e(T) can be shown.

sample 6

0.6 -

n
Eh

0.2 -

I
0

I
1

I
2

Ts = 20 C, not heated before

__--Tsr
20 C, heated before
Ts t: 500C. heated before
-.-.
- Ts = 7OOC, heated before
I
I
I
I
I
II
4
5
6
3
Gm)

Figure 12. Sample 6. Spectral near-normal emissivity Q as

obtained from the measured near-normal hemispherical reflectivity. Sample temperature T, and heat treatment: (~1
Room temperature, sample never heated; (---) room temperature, sample heated before; ( ... > about 5OOC,sample heated
before; (-.-I about 700C sample heated before.

Figure 13. The calculated temperature dependence of the

total near-normal emissivity E of sample 4. The spectral
reflectivity result obtained with the sample before it was
heated is used with Eq. (8) in two ways: with integration
boundaries 0.6 and 10 (long dashes) and with integration
boundaries 0.6 and 30 and extrapolated spectrum (solid line).
The spectral reflectivities measured with th sample after heat
treatment are given in the extrapolated way by the other
curves. T, and heat treatment indicated as in Fig. 11.

Spectral and Total Emissivity of Refractories

Figure 13 shows results for sample 4 using the measurements given in Fig. 11. It clearly shows the difference in a
sample before and after heat treatment.
Equation (8) implies an integration from zero to infinity. In our case the measurements
are restricted to a
specific spectral region, and we do not know of a model
that describes the behavior outside this region (such as
the Hagen-Rubens
relation, which is sometimes used for
metals 17,271). If one integrates only over the measured
region, this will result in a shift of the total emissivity with
respect to the expected behavior. In Fig. 13 the dashed
curve is obtained by carrying out the integrations
of Eq.
(8) from 0.6 to 10 pm. The solid curve is obtained by
using the same spectral results but extrapolated to 30 pm
with a constant value of 0.95. The difference between the
two curves shows how important the effect is and therefore how important it is to extrapolate as well as possible.
One has to keep in mind that such an extrapolation will in
general be no more than an acceptable first-order correction. (For instance, the sand results in [12] suggest that a
dip can occur around 20 pm.) We extrapolated the measurements on sample 4 after heat treatment (region up to
6 pm) by taking the spectral dependence
before heat
treatment (region up to 10 Fm).and an extrapolation
to
30 Frn as just discussed. If the total emissivity is calculated for higher temperatures,
an extrapolation to smaller
wavelength is necessary. The uncertainty in the total emissivity in Fig. 13 is about 5% for high temperatures,
mainly
due to the uncertainty in the spectral emissivity at smaller
wavelengths. The relative importance of this contribution
is less at lower temperatures,
but the contribution
to the
uncertainty due to the extrapolation of the measurements
will increase with decreasing temperature.
In this case
also, 5% is used as a (rough) estimate for the total
uncertainty.
Finally the difference between sample 1 from the flame
side and sample 2 from the inner side can be seen in Fig.
14. The results for the other refractories are also given for
comparison. The calculated near-normal
emissivities are
based on the measured data presented in Figs. 7-9.
Although all the results presented up to now concern
near-normal
emissivities, these conclusions also hold for
the total hemispherical emissivity. This value can be calculated using a theoretical ratio of hemispherical
to normal
emissivity for pure dielectrics [7,8]. The hemispherical

value is about
refractories.

325

5% lower in the case of the discussed

CONCLUSIONS
Measurements
of the spectral near-normal
reflectivity of
six refractory samples were performed using the integrated sphere method. The optical properties of refractories are characterized by a general behavior. In that sense
the presented results agree with results that can be found
in the literature. Nevertheless
there are specific differences between the various refractories. The use of the
specific optical properties of materials is recommended
for spectral modeling studies based on a real situation.
This also holds for modeling studies in which the total
heat transfer properties are used. This sometimes allows
for a better estimate of the costs of a process to be
obtained. An example is a glass melting furnace [28] for
which the relative variation in the heat fluxes due to a
variation in total emissivity of the walls has been studied
131.
One has to be careful in obtaining the specific results.
In this study it was found that the total emissivity of a
sample taken from a new brick is affected significantly by
some hours of heat treatment at a temperature
of a few
hundred degrees Celsius. So, in practice, the total emissivity will be lower than expected from measurements
on a
sample that has never been heated. The order of magnitude is 20% for operating temperatures
of at least some
hundreds of degrees Celsius.
Further, in the corrosive surrounding
of the inner wall
of a glass melting furnace, it is possible that the surface
region of the brick changes in such a way that its total
emissivity will increase. In Fig. 14 the order of magnitude
found for one of the refractories is 20% for temperatures
above 1000C. This will increase an emissivity of almost
0.6 to 0.7. It is expected that if such an effect occurs, it
will be over the course of time.
This study was performed under contract with the Netherlands
Agency for Energy and Environment (NOVEM). We are grateful to
Mrs. B. D. Arhatari for carrying out the reflectivity measurements.
We also thank A. J. van den Berg and the Solid State Group for
measuring the X-ray diffraction patterns and P. A. van Nijnatten and
the TPD @NO-Institute of Applied Physics) for the use of their
spectrophotometer.

NOMENCLATURE
E

lps5i;,
300

600

900

1200

1500

1800

1
2100

T(K)

Figure 14. The calculated

temperature
dependence
of
the total near-normal emissivity E of all samples listed in
Table 1.

$
f"
Q
T

blackbody emissive power, W/(m pm)

fraction of sphere area of port i, m2
fraction of sphere area that is inside the FOV, m2
incident flux, W
temperature,
C (K in Figs. 13 and 14)
output of lock-in amplifier, V

Greek Symbols
emissivity, dimensionless
fraction of reflected beam from sample falling into the
FOV, dimensionless
wavelength, pm
reflectivity, dimensionless
average reflectivity, dimensionless

326

d
r
rl
r2
S
W
A

J. J. P. Elich and J. A. Wieringa

Subscripts
absence of sample, open port
detector
reference
reference 1 (Spectralon)
reference 2 (specular gold)
sample
wall
wavelength
Superscripts

dectector
S
sample
I
directional quantity
n near-normal
C-l hemispherical
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Received April 12, 1994; revised August 30, 1994.