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Journal of Building Engineering 31 (2020) 101348

Contents lists available at ScienceDirect

Journal of Building Engineering


journal homepage: http://www.elsevier.com/locate/jobe

Determination of the thermal insulation properties of cylindrical PUR foam


products throughout the entire life cycle using accelerated
aging procedures
Agnieszka Winkler-Skalna *, Beata Łoboda
Instytut Techniki Budowlanej, ul. Filtrowa 1, 00-611, Warsaw, Poland

A R T I C L E I N F O A B S T R A C T

Keywords: PUR foams are one of the more frequent used thermal insulation materials, especially as pipe insulation. The
Thermal conductivity main parameter characterizing materials in terms of thermal insulation is the thermal conductivity coefficient
Polyurethane foam signed as λ. In the case of PUR foams, aging occurs, consisting in the diffusion of gases contained in the foam
PUR
cells, as a result of which material insulating properties go worse. Prediction of changes in the λ coefficient is
Insulation materials
Accelerated aging
essential and its value after aging should be included in the calculation of the long-term insulation performance.
The use of methods that accelerate the aging process contributes to shortening the time and costs associated with
testing new products. In this work, for the purpose of testing cylindrical products, the methodology of aging of
flat products contained in the standard EN 14308 was adapted. Coatings made of closed cell PUR foam with
densities of 40 kg/m3, 60 kg/m3, 80 kg/m3 and 120 kg/m3, foamed with n-pentane were aged by conditioning at
70 � C for 175 days. Based on the λ coefficient measurements, its increment after 7, 21 and 90 days was also
determined. The effects of foam density, sample diameter, sample thickness and average test temperature on the
velocity and range of λ coefficient changes after successive conditioning periods were analyzed. The final λ
coefficient values obtained using two aging procedures were compared. The obtained results indicate an increase
in the importance of choosing the aging procedure along with an increase in foam density and an increase in
average measurement temperature. Quantitative estimation of changes in the λ coefficient value caused by
material aging is very important for both manufacturers and designers of heating networks and other industrial
installations.

1. Introduction coefficient”, which are in compliance with the mentioned standards.


Many researchers are persistently searching for new solutions, better
The primary objective of thermal insulation materials and products materials, optimal use of raw materials, and all these efforts are aimed to
used both as thermal insulation for buildings and industrial installations reduce the costs associated with delivery of heat to buildings [3–5].
is to effectively reduce heat loss (or maintain low temperature in the Polyurethane foam (PUR) and polyisocyanurate foam (PIR) are exam­
case of the transfer of refrigerating agents), and thus to reduce operating ples of most commonly applied thermal insulation materials in indus­
costs. In view of the above, one of the main parameters characterizing trial installations and in building construction, along with EPS, XPS,
the said materials is the thermal conductivity coefficient in W/(mK), MW, foam glass, granular materials and more and more frequently used
which is used to determine thermal resistance of an insulation layer. The aerogels [4,6–12]. PUR foams have also been used for many years in
value of this coefficient closely depends on the average temperature of pre-insulated pipes. Many publications describe thermal insulation
measurement [1]. The λ coefficient measured directly is referred to as properties test results after aging for that products [13–15]. The subject
effective thermal conductivity coefficient, because in addition to con­ which addresses the aging of polyurethane foam has been well examined
ductivity, the influence of other ways of heat transfer, i.e. radiation and and described in terms of its application in pre-insulated pipes. The
convection, is also taken into account [2]. For the needs of this study, we standard EN 253 [31], involving the identification of the properties of
will be using the term “thermal conductivity coefficient” or “λ pre-insulated pipes, provides also a methodology used to determine

* Corresponding author.
E-mail addresses: a.winkler-skalna@itb.pl (A. Winkler-Skalna), b.loboda@itb.pl (B. Łoboda).

https://doi.org/10.1016/j.jobe.2020.101348
Received 4 December 2019; Received in revised form 14 February 2020; Accepted 10 March 2020
Available online 15 March 2020
2352-7102/© 2020 Elsevier Ltd. All rights reserved.
A. Winkler-Skalna and B. Łoboda Journal of Building Engineering 31 (2020) 101348

thermal conductivity coefficient of PUR foam after the aging process. As In various articles researchers presents the thermal conductivity
specified in the standard, the determination of thermal conductivity coefficient test results after aging for PUR foams of different density,
coefficient of a pipe assembly consisting of a service pipe, PUR foam blowing with various agents. The researchers carry out aging under
insulation and an outer casing should be carried out after prior heating various temperature conditions and at different periods of conditioning
at 90 � C for 150 days. In that case, however, it is essential to allow for the time. For example, in article [26] the thermal conductivity coefficient
impact of protective casing and that of possible diffusion barrier which test results of PU foam samples after conditioning at 40 � C for a week are
delay the aging process, as well as the impact of the production method present. For sample 1, an increase in thermal conductivity after condi­
of pre-insulated pipes. It is generally known that the rate of diffusion of tioning compared to the initial value by 1.7% was noted, while for
intracellular gases depends on the density of foam, coating thickness and sample 2 by 3.6%. In those work are also present the results of mea­
the applied blowing agent. The gases remaining in the cells of the surements of thermal conductivity of PU foams subjected to high (70 � C)
finished product after the blowing process are characterized by varying and low ( 40 � C) temperature for one week. For sample 1, the thermal
properties [15,17]. In the case of the aforementioned pre-insulated conductivity coefficient increased by 11.8% and for sample 2 by 8.4%.
pipes, apart from thermal insulation properties, also dimensional sta­ In Ref. [21] proposed a method for predicting the thermal resistance of
bility and strength parameters (compressive strength, foam adhesion to PIR foam boards blowing with cyclopentane, isopentane and water.
the service pipe) play a very important role. The issues regarding me­ Different test conditions adopted by researchers make it difficult to
chanical properties were described in the works [13,14,18,19]. Also compare the obtained results. In addition, assuming the 30-year life
studies on the aging process in the air and in the atmosphere of nitrogen cycle of PUR foams, it is important to predict properties throughout the
have been carried out. The studies have demonstrated that the rate of entire life cycle. Due to the mentioned difficulties, the assumptions
PUR degradation reaction in the air is notably accelerated due to the adopted in the study and the results of the tests were referred to the
presence of oxygen [18,20,21]. Another factor having a very large standardised aging method described in the standards [29,30].
impact on thermal insulation is the pressure of gas contained in the cells The standards EN 13165 [29] and EN 14308 [30] provide two
and foam pores [22]. A significant improvement of thermal conductivity methods of PUR foam aging prior to the determination of thermal con­
coefficient was obtained in the so-called vacuum insulations [22]. The ductivity coefficient for flat products: the method of fixed increments
influence of aging on insulation properties is also tested for vacuum and the method of accelerated aging. In the case of the fixed increments
insulations [23,24]. However, since in real conditions the aging process procedure, 20 mm thick foam is heated at 70 � C for 21 days, and
takes place in the air, and the use of vacuum insulation is a costly so­ depending on the obtained results, further steps aimed at determining
lution, the work focuses on the “traditional” application of PUR. Very thermal conductivity coefficient after the aging process are carried out.
good thermal insulation properties of PUR foams can be attributed to the In the accelerated aging procedure, PUR foam is heated at 70 � C for 175
blowing agents of high molecular weight used in the production process, days. As a part of this work, tests using the accelerated aging procedure
such as hydrocarbons (e.g. pentanes) and hydrofluorocarbons (e.g. were carried out, and in addition, changes in the λ coefficient after
HFC365mfc, HFC134a, HFC245fa, 227ea), which are called permanent shorter conditioning periods were controlling. Aging was also carried
agents [2,22,25]. We can also use the mixtures of permanent agents and out according to fixed increment procedure (21 conditioning days at 70
carbon dioxide, which in turn is a non-permanent blowing gas [30]. The �
C). Due to the fact that PUR has different properties, depending on the
mentioned blowing agents remain inside the cells, after the foam has direction of foam growth, the direct application of this procedure for
been manufactured, and over time they are replaced with air. The aging cylindrical products may raise doubts. Standard EN 14308 [30] allows
of foam effected by gas diffusion leads to the deterioration of thermal the replacement of test for cylindrical products with test for flat prod­
insulation properties which is associated with the fact that the thermal ucts, provided that has been demonstrated that the results give safe
conductivity coefficient of gases remaining in the cells after the blowing (higher) values. This means that for PUR products the measurement of
process is lower than the λ coefficient of air components [15,26,30]. the thermal conductivity shall carried out in the rise direction of the
Exemplary values of the thermal conductivity coefficient of gases filling product [30]. Such an approach can be quite easily applied to products
up the cells are given in Table 1 [16,26]. The issues involving the process cut from the foam blocks. The bigger problem are the products manu­
of gas diffusion and the aging of PUR foams have been described in factured from the production process, in which the finished product is
detail in the works [27,28]. Since it is assumed that PUR foams have the cylindrical. In this case, it is technologically difficult to make flat sam­
service life of 30 years, it is very important to identify the value of λ ples with identical properties (foam density, foam rise direction) like
coefficient after the aging. At temperatures close to room temperature, cylindrical sample for the purpose of testing. This work attempts to
the aging process can last for tens of years, and its rate depends on the demonstrate that standardised aging procedures dedicated for flat
type of polymer and on the gas filling the cells, as well as on the con­ products can also be used for cylindrical products. In order to identify
ditions in which the foam is used - the most important ones are tem­ the extent of aging, the studies were conducted on the coatings without
perature and humidity. High temperature accelerates the diffusion any diffusion barriers. Since the applied foam can be considered ho­
process, while high humidity destroys the solid substance. The methods mogeneous, the studies were carried out using two different thicknesses
accelerating the aging process allow to reduce the time and costs asso­ of samples. It enabled us to test out the effect of thickness on the rate of
ciated with launching new products on the market. According to the occurring changes.
Ref. [8], the seasoning of samples exposed to the prevailing environ­
ment, and periodic checking of the properties may last even 2.5 years. 2. Materials and methods

2.1. Description of test samples and aging procedure


Table 1
Typical thermal conductivity of typical cell gases at 25 � C [16,26]. Six types of rigid closed-cell polyurethane foam (PUR) blown with n-
Gas Gas thermal conductivity at 25 � C pentane, marked in succession as A, B, C, D, E, F, were subjected to
W/(mK) testing. The types of foam varied in terms of apparent density of the
material, internal diameter of cylindrical samples and the thickness of
Air 0.0259
Carbon dioxide 0.0162 samples.
Cyclopentane 0.0130 The first stage of the studies was aimed to determine the initial value
Isopentane 0.0150 of the λ coefficient for individual types of samples, measured immedi­
HCFC-141b 0.0100 ately after the delivery of the samples to the laboratory, from 1 to 8 days
HFC-245fa 0.0122
after their fabrication. The sets of samples for the subsequent

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A. Winkler-Skalna and B. Łoboda Journal of Building Engineering 31 (2020) 101348

measurement stages were conditioned at 70 � C for 7 days, 21 days, 90 � �


days and 175 days. Each set contained from 1 to 5 samples. Fig. 1 shows Φln DD20
a diagram of activities carried out from the moment of delivery samples λ¼ ; (1)
to the laboratory until obtaining the measurement results. 2πLðT0 T2 Þ
Closed-cell polyurethane foam samples of the density of 40 kg/m3,
where: Φ - heat flux in W, D2 - external diameter of pipe insulation in m,
60 kg/m3, 80 kg/m3 and 120 kg/m3, blown with n-pentane were tested.
D0 - external diameter of the heating pipe in m, L - length of the
The aging temperature was adopted basing on the standard EN 14308
measured section in m, T0 - surface temperature of the heating pipe in
[30]. The measurements were made at the average temperature of 0 � C, �
C, T2 - temperature of the outer surface of the insulation in � C. The
10 � C, 50 � C, 100 � C and 130 � C.
expanded uncertainty of measurement with the 95% confidence level
Table 2 Presents individual types of foam along with the information
and with the coverage factor of k ¼ 2 is 3%.
on subsequent stages of aging and the average temperature at which the
The measurements were carried out in a TAURUS pipe apparatus
measurements were carried out. Since uncontrolled aging of PUR foam is
with protective cylinders at the ends of the test (heating) pipe and with a
taking place during the measurements at high temperature, a different
horizontal arrangement of the pipe. The pipe apparatus and test samples
set of samples from the same product batch was used for the measure­
are presented in Fig. 2 (a) and 2 (b). And Fig. 3 Presents a schematic of
ments after subsequent conditioning steps.
the heating pipe with a sample and marked temperature measurement
For measurements of the thermal conductivity coefficient, it is rec­
points on the heater and on the external surface of the sample. The
ommended (EN ISO 13787) that the minimum temperature difference
measuring points are arranged spirally, at an equal distance from each
over the sample thickness is at least 10 � C. In the case of measurement
other, along the length of the measured section. In addition, control
results in this article, the difference was from 13 � C to 20 � C.
measuring points were placed on the protective sections of the heater.
The diameter of the heating pipe was 0.035 m or 0.06 m. The length of
2.2. Description of method for the determination of steady-state thermal
the measured part was 0.6 m, the length of the guarded part on both
conductivity coefficient
sides of the heating section was 0.2 m. Air was applied as the cooling
agent outside the sample.
The values of thermal conductivity coefficient were determined in
All measurement results, both auxiliary, such as determination of
compliance with the method described in EN ISO 8497 [32], using the
sample dimensions and masses, temperature measurement during con­
following equation:
ditioning and final λ coefficient measurement, were obtained using
equipment with current calibration certificates. Fig. 4 shows an example

Fig. 1. Sample handling scheme.

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A. Winkler-Skalna and B. Łoboda Journal of Building Engineering 31 (2020) 101348

Table 2
Summary of the tested samples.
PUR type Density Inside diameter Thickness Conditioning time Number of samples for conditioning time respectively Average temperature of test
3
kg/m mm mm days items �
C

A 40 60 20 0; 7; 21; 90; 175 5; 5; 4; 5; 4 0; 10; 50; 100; 130


B 60 35 20 0; 21; 90; 175 3; 3; 1; 2 0; 10; 50; 100
C 60 35 50 0; 21; 90; 175 3; 3; 3; 2 0; 10; 50; 100
D 80 35 20 0; 21; 90; 175 3; 3; 3; 3 0; 10; 50; 100
E 80 35 50 0; 21; 90; 175 3; 3; 3; 2 0; 10; 50; 100
F 120 60 20 0; 7; 21; 90; 175 3; 3; 3; 3; 3 0; 10; 50; 100; 130

Fig. 2. Pipe apparatus with protective cylinders at the ends of the test tube (a); a part of test samples (b).

4. Discussion

4.1. Initial value of thermal conductivity coefficient depending on the


density of PUR foam

The relation presented in Fig. 6 demonstrates that for low densities


(below 60 kg/m3) the value of λ coefficient is decreasing with the rise of
density. For densities higher than 60 kg/m3, the trend is reversed - the
value of λ coefficient is increasing with the rise of the apparent density of
the foam. For low densities, this relation may result from the fact that the
share of radiation in heat transfer is significant, which is directly related
to a larger pore size. In that case, the reduction of density brings about
Fig. 3. Arrangement of the measuring points on the tested sample in the the deterioration of thermal insulation properties. In turn, for higher
pipe apparatus. densities, heat conductivity is becoming dominant both by the solid
component of PUR and by the gas filling up the pores. Since with the rise
of the results obtained from the λ coefficient measurements for a single of foam density the share of gases in the volume decreases, and the share
PUR type A sample after 7 days conditioning. of solid component increases, the ultimate value of thermal conductivity
coefficient increases. It should be noted that the purpose of the work was
3. Results not to estimate the share of different ways in the total heat transfer
through the tested material, and the presented relationship is to show
As part of the work, 81 samples were tested. Fig. 5 (a) shows graphs the differences between the tested types of PUR foams.
of the initial value of the thermal conductivity coefficient for different
types of PUR at different average temperatures. In Fig. 5 (b) and 5 (c), 5 4.2. Changes in the thermal conductivity coefficient dependent on
(d), and 5 (e), the graphs of values after 7 days, 21 days, 90 days and 175 temperature
days, respectively. Then, for the results of measurements in particular
period of conditioning, linear regression equations showing the change For the tested range, linear dependence of the λ coefficient on tem­
of λ coefficient value depending on the average measurement temper­ perature was determined. Table 3 Presents the averaged values of the λ
ature were determined. The regression equations and the correlation coefficient, calculated using linear regression equations. In the pre­
coefficients R for each PUR type are given in the graphs. Then, using the sented equations, the symbol t denotes the average measurement tem­
determined equations, thermal conductivity coefficients were calculated perature. The calculations of the λ coefficient at the preset average
for the assumed temperatures within the range of average measurement temperature of 0 � C, 10 � C, 50 � C, 100 � C and 130 � C were carried out in
temperatures (interpolation). compliance with the standard EN ISO 13787 [33]. The correlation co­
Based on the measurement results of the initial value of λ coefficient efficient R for all equations was within the range from 0.965 to 1.000.
at the average temperature of 10 � C, the dependence of that coefficient
on the density of PUR foam was determined. The relation is presented in 4.3. Percentage changes in the thermal conductivity coefficient after
Fig. 6. subsequent conditioning stages

Tables 4 and 5 demonstrate the percentage increment of λ with


respect to the initial value and for subsequent conditioning stages
respectively.

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A. Winkler-Skalna and B. Łoboda Journal of Building Engineering 31 (2020) 101348

Fig. 4. Example of λ measurement results for a single PUR type A sample after 7 days conditioning.

Calculation of the averaged thermal conductivity coefficient values intensive gas exchange, shortly after the foam was fabricated - similarly
determined for specific temperature allows to compare the increase in its as for the PUR type A. There was no increment of the λ coefficient be­
value after subsequent conditioning stages for different PUR foam types. tween day 7 and day 21, while between day 21 and 90 and between day
This approach was possible due to the large number of measurements. 90 and 175, the observed increment was similar.
For the PUR type A foam, the highest increment of the λ coefficient
was observed in the first 7 days of conditioning. It is also the shortest
storage time of samples at raised temperatures, which bespeaks of an 4.4. Influence of foam density, diameter and thickness of samples on
intensive gas exchange within a short time after the fabrication of the aging speed
foam. The tests after 7 days of heating were carried out only for the foam
having the lowest and the highest density. An inconsiderable increment Fig. 7 (a) and (c) present a graphical representation of the percentage
was observed between day 21 and 90, which increased again in the last changes of the λ coefficient in the subsequent stages of conditioning, and
stage of the test. Fig. 7 (d) the total percentage increase of the λ coefficient after 175 days
For the PUR type B, the highest increment of the λ coefficient was of conditioning. The changes were presented for the entire tested
observed in the first 21 days of conditioning. Similarly to the foam A, the average temperature range.
fastest change in the value of λ coefficient was observed in the initial For PUR foams of the density in the range from 40 kg/m3 do 80 kg/
conditioning stage. In the last stage, no increment in the coefficient m3 (PUR type A, B, C, D, E), after the first 21 days of conditioning, we
value was observed. observe a distinct drop in the rise of the λ coefficient with the increasing
For the PUR type C, the increment of the λ coefficient is similar in the density of the foam. This means that the diffusion of gas is taking place
first two conditioning stages. In the last stage, the increment of the co­ faster in the material of lower density, because the lower is the apparent
efficient value was not observed. density of the material, the higher is the proportion of gas filling up the
For the PUR type D, the highest increment in the value of λ coeffi­ cells, and thus the higher is the impact of aging associated with diffu­
cient was reported in the first 21 days of conditioning for the average sion. In addition, as expected, gas exchange is faster in the samples of
test temperature of 0 � C and 10 � C; for 50 � C it was similar in the first two lower thickness (PUR type A, B, D). It is clearly seen when comparing
periods, while for 100 � C a higher increment of the λ coefficient was foam samples of the density of 60 kg/m3 and 80 kg/m3, where two
reported in the second stage. In the last stage (between day 90 and 175), sample thicknesses were tested: 20 mm and 50 mm, and the internal
an inconsiderable increment of the λ coefficient was observed. diameter was 35 mm. It is related to the ratio of the surface of the
For the PUR type E, the increment of the λ coefficient was similar in samples, through which gas exchange takes place, to their volume. For
the first and third conditioning stages. In the second stage, for the the samples 20 mm thick, it is 52, and for the samples of the thickness of
average test temperature of 0 � C and 10 � C, the observed increment was 50 mm, it is 22. In the analysis we ignored the comparison of the results
higher than that in the other stages, while for 50 � C and 100 � C, the obtained for the samples of the same thickness, but with different in­
increment was lower. ternal diameters, since the ratio of their volume to the surface is similar,
For the PUR type F, the largest increment in the value of λ coefficient so it was assumed that this should not affect the diffusion rate of gases.
was reported in the first 7 days of conditioning. It was also the shortest And totally different was the behavior of the foam of the density of 120
storage period of the samples at raised temperature, which bespeaks of kg/m3. In that case, the change of the λ coefficient measured at 0 � C,
after 21 days of conditioning, exceeded 17%, and it was the highest

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A. Winkler-Skalna and B. Łoboda Journal of Building Engineering 31 (2020) 101348

Fig. 5. Results of measurement of thermal conductivity coefficient of six types of PUR foam, performed at the average measurement temperature of 0 � C, 10 � C, 50

C, 100 � C and 130 � C before conditioning (a); after 7 days of conditioning (b); after 21 days of conditioning (c); after 90 days of conditioning (d); after 175 days of
conditioning (e).

increase of the λ coefficient from among all tested types of foam.


In the next conditioning stage, between days 21 and 90, for the
lowest density, the increase of λ coefficient was minimal, and it was
increasing with the rise in density for most of the tested PUR foam types.
Gas exchange in this time period was definitely slower. A different
behavior was reported in the case of PUR type C, where for the tem­
peratures of 0 � C and 10 � C, the increase of thermal conductivity coef­
ficient was slightly higher than that in the first 21 days. For the foam of
the density of 120 kg/m3, after very intense exchange of gas in the first
21 days of conditioning, in the next stage (between day 21 and 90) those
changes were about 60% lower. Also the increment rate changed for
different thicknesses. At that stage, a higher increase was observed in the
samples of higher thickness as compared to thinner samples.
Negative increment values (PUR type E) reported in the second time
period may denote the end of gas exchange, but we must remember that
Fig. 6. Initial value of thermal conductivity λ coefficient depending on the a different set of samples was used for each stage of testing, and their
density of PUR foam measured at the average temperature along the sample homogeneity is dependent, among others, on the fabrication process. We
thickness of 10 � C.
should also allow for the expanded uncertainty of measurement of the
thermal conductivity λ coefficient, which was 3%. The divergence in the
density of samples used in the tests was contained in the ranges as in
Table 6.

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A. Winkler-Skalna and B. Łoboda Journal of Building Engineering 31 (2020) 101348

Table 3 Table 5
Coefficient λ determined on the basis of regression equations at the preset Percentage increment of the λ coefficient in subsequent conditioning stages.
average temperature. PUR Increment of Increment of Increment of Increment of
PUR Initial value λ after 7 λ after 21 λ after 90 λ after 175 type the λ coefficient the λ coefficient the λ coefficient the λ coefficient
type of λ, W/ days, W/ days, W/ days, W/ days, W/ over the first 7 between day 7 between day 21 between day 90
(mK) in 0 (mK) in 0 (mK) in 0 (mK) in 0 (mK) in 0 days, % in 0 � C; and 21, % in 0 and 90, % in 0 and 175, % in 0

C; 10 � C; �
C; 10 � C; �
C; 10 � C; �
C; 10 � C; �
C; 10 � C; 10 � C; 50 � C; �
C; 10 � C; 50 �
C; 10 � C; 50 �
C; 10 � C; 50
50 � C; 100 50 � C; 100 50 � C; 100 50 � C; 100 50 � C; 100 100 � C; 130 � C �
C; 100 � C; 130 �
C; 100 � C; 130 �
C; 100 � C; 130

C; 130 � C �
C; 130 � C �
C; 130 � C �
C; 130 � C �
C; 130 � C

C �
C �
C

A 0.0235; 0.0264; 0.0272; 0.0273; 0.0284; A 12.34; 11.37; 3.40; 3.14; 0.43; 0.39; 4.68; 4.31;
0.0255; 0.0284; 0.0292; 0.0293; 0.0304; 8.66; 6.67; 5.86 2.39; 1.84; 1.62 0.30; 0.23; 0.20 3.28; 2.53; 2.22
0.0335; 0.0364; 0.0372; 0.0373; 0.0384; B 15.26; 13.44; 4.34; 4.06; 0.04; 0.04;
0.0435; 0.0464; 0.0472; 0.0473; 0.0484; 8.05; 3.81; - 3.21; 2.55; - 0.03; 0.03; -
0.0495 0.0524 0.0532 0.0533 0.0544 C 10.19; 9.48; 12.10; 10.39; 2.62; 2.00;
B 0.0228; – 0.0263; 0.0273; 0.0273; 7.41; 5.83; - 5.41; 1.58; - 0.20; 1.18; -
0.0244; 0.0277; 0.0287; 0.0287; D 10.15; 8.75; 6.00; 5.63; 0.58; 0.54;
0.0308; 0.0333; 0.0343; 0.0343; 4.55; 1.17; - 4.52; 3.62; - 0.43; 0.35; -
0.0388; - 0.0403; - 0.0413; - 0.0413; - E 5.43; 5.08; 7.12; 5.85; 5.56; 5.20;
C 0.0214; – 0.0236; 0.0262; 0.0256; 4.03; 3.20; - 2.06; 0.92; - 4.13; 3.28; -
0.0230; 0.0252; 0.0276; 0.0271; F 18.19; 16.46; 0.73; 1.01; 5.08; 4.46; 4.08; 3.84;
0.0294; 0.0316; 0.0332; 0.0331; 11.23; 6.95; 1.87; 2.58; 2.56; 1.00; 0.32 3.11; 2.51; 2.26
0.0374; - 0.0396; - 0.0402; - 0.0406; - 5.08 2.89
D 0.0243; – 0.0268; 0.0283; 0.0284;
0.0259; 0.0282; 0.0297; 0.0298;
0.0323; 0.0338; 0.0353; 0.0354; � for the foams of the same density, but with different thicknesses, the
0.0403; - 0.0408; - 0.0423; - 0.0424; - increment for thicker samples is higher,
E 0.0230; 0.0243; 0.0259; 0.0272;
� for the density of 120 kg/m3, we observed the highest increment of

0.0246; 0.0259; 0.0273; 0.0286;
0.0310; 0.0323; 0.0329; 0.0342; the λ coefficient, which is in contrast with the results obtained for
0.0390; - 0.0403; - 0.0399; - 0.0412; - lower densities - a more precise analysis of the behavior of PUR
F 0.0289; 0.0342; 0.0340; 0.0354; 0.0366; foams of higher densities requires more laboratory tests to be carried
0.0307; 0.0358; 0.0355; 0.0368; 0.0380; out,
0.0379; 0.0422; 0.0415; 0.0424; 0.0436;
0.0469; 0.0502; 0.0490; 0.0494; 0.0506;
� for all types of foam, with the rise of average test temperature, the
0.0523 0.0550 0.0535 0.0536 0.0548 increment of the λ coefficient is decreasing - this may be due to aging
caused by heating the sample already during the testing.

Table 4 4.5. Comparison of λ coefficient values after aging obtained according to


Percentage increment of the λ coefficient relative to the initial value. fixed increments procedure and accelerated aging procedure
PUR Increment of Increment of Increment of Increment of
type the λ coefficient the λ coefficient the λ coefficient the λ coefficient For reference, the value of the λ coefficient after 21 days of condi­
after 7 days, % after 21 days, % after 90 days, % after 175 days, tioning was also presented to compare with the limit value of 0.006 W/
in 0 � C; 10 � C; in 0 � C; 10 � C; in 0 � C; 10 � C; % in 0 � C; 10
(mK) adopted in compliance with the standard EN 14308 [30].
50 � C; 100 � C; 50 � C; 100 � C; 50 � C; 100 � C; �
C; 50 � C; 100
130 � C 130 � C 130 � C �
C; 130 � C
The increments after 21 days shown in Table 7 did not exceed the
adopted limit value of 0.006 W/(mK) for any average temperature of the
A 12.34; 11.37; 15.74; 14.51; 16.17; 14.90; 20.85; 19.22;
tests. This means that for the tested foam types the fixed increments
8.66; 6.67; 5.86 11.04; 8.51; 11.34; 8.74; 14.63; 11.26;
7.47 7.68 9.90 procedure can be used.
B 15.26; 13.44; 19.60; 17.49; 19.55; 17.45; Table 8 shows the increments adopted on the basis of EN 14308 [30]
8.05; 3.81; - 11.26; 6.36; - 11.23; 6.34; - standard for both aging procedures. In the fixed increments procedure,
C 10.19; 9.48; 22.29; 19.87; 19.67; 17.87;
increments (which are varies according to temperature) are added to the
7.41; 5.83; - 12.82; 7.41; - 12.62; 8.58; -
D 10.15; 8.75; 16.15; 14.38; 16.73; 14.92;
initial value of the thermal conductivity coefficient. In the accelerated
4.55; 1.17; - 9.06; 4.79; - 9.50; 5.13; - aging procedure the same increment for each temperature is added to
E 5.43; 5.08; 12.55; 10.93; 18.11; 16.13; the λ coefficient values measured after 175 days of conditioning. Table 9
4.03; 3.20; - 6.09; 2.28; - 10.22; 5.56; - shows the initial value of λ coefficient, the value after 175 days of aging
F 18.19; 16.47; 17.46; 15.46; 22.54; 19.92; 26.63; 23.76;
and the final values calculated according to both procedures using the
11.23; 6.95; 9.36; 4.37; 2.20 11.92; 5.37; 15.03; 7.89;
5.08 2.52 4.78 increments given in Table 8.
Fig. 8 Present the comparison of calculation results obtained using
both aging procedures: fixed increments procedure and accelerated
And the increase in the last conditioning period, i.e. between day 90 aging procedure. The values given in the graph represent the difference
and 175, is not higher or close to the value of 3% of the measurement between the results (fixed increments procedure - accelerated aging
uncertainty. Thus, we can accept that the maximum conditioning time of procedure). The green lines limit the area of uncertainty of measurement
175 days is sufficient to assess the ultimate impact of aging at raised calculated as 3% (0,0011 W/mK) of the average value of obtained
temperature on the thermal conductivity of closed-cell PUR foams measurement results. For PUR type A (foams with the lowest apparent
blown with n-pentane. density tested of 40 kg/m3) the differences in the results obtained by
Having analyzed the total change of the λ coefficient after 175 days both methods are within the uncertainty of measurement. In this case,
of aging at 70 � C, we can conclude that: both aging procedures can be considered to give comparable results.
In the case of PUR types B, C, D, E, no significant difference was
� for the density in the range from 40 kg/m3 to 80 kg/m3, the incre­ recorded only for 0 � C and 10 � C. At higher temperatures (50 � C, 100 � C,
ment of the value of thermal conductivity coefficient is decreasing 130 � C), the results obtained using the fixed increments procedure are
with the rising density, significantly higher than using the accelerated aging procedure.
In case of PUR type F for 0 � C and 10 � C higher results were obtained

7
A. Winkler-Skalna and B. Łoboda Journal of Building Engineering 31 (2020) 101348

Fig. 7. Percentage change of the thermal conductivity coefficient value in subsequent conditioning stages, for the average measurement temperature of 0 � C, 10 � C,
50 � C, 100 � C and 130 � C after 21 days conditioning (a); between 21 and 90 day of conditioning (b); between 90 and 175 day of conditioning (c); total percentage
increase of the λ coefficient after 175 days of conditioning (d).

Table 6 Table 9
Ranges of the density of samples used in the tests. Coefficient λ values with increments according to the fixed increments proced­
PUR type A B C D E F
ure and the accelerated aging procedure in 0 � C; 10 � C; 50 � C; 100 � C; 130 � C.
PUR Initial value Value after Value with Value with
Range of density, 37–40 57–62 58–63 80–83 82–84 113–117
type for fixed aging for of increments for increments for
kg/m3
increments accelerated the fixed accelerated
procedure aging procedure increments aging procedure
W/(mK) W/(mK) procedure W/ W/(mK)
Table 7 (mK)
The difference between the value of λ coefficient after 21 days and the initial A 0.0235; 0.0284; 0.0304; 0.0290; 0.0313; 0.0294; 0.0314;
value of λ coefficient (increment). 0.0255; 0.0384; 0.0484; 0.0397; 0.0502; 0.0394; 0.0494;
0.0335; 0.0544 0.0563 0.0554
PUR type For 0 � C For 10 � C For 50 � C For 100 � C For 130 � C
0.0435;
W/(mK) W/(mK) W/(mK) W/(mK) W/(mK)
0.0495
A 0.0037 0.0037 0.0037 0.0037 0.0037 B 0.0228; 0.0273; 0.0287; 0.0283; 0.0302; 0.0283; 0.0297;
B 0.0035 0.0033 0.0025 0.0015 – 0.0244; 0.0343; 0.0413; 0.0370; 0.0455; 0.0353; 0.0423;
C 0.0022 0.0022 0.0022 0.0022 – 0.0308; - - -
D 0.0025 0.0023 0.0015 0.0005 – 0.0388; -
E 0.0013 0.0013 0.0013 0.0013 – C 0.0214; 0.0256; 0.0271; 0.0269; 0.0288; 0.0266; 0.0281;
F 0.0051 0.0048 0.0036 0.0021 0.0012 0.0230; 0.0331; 0.0406; 0.0356; 0.0441; 0.0341; 0.0416;
0.0294; - - -
0.0374; -
D 0.0243; 0.0284; 0.0298; 0.0298; 0.0317; 0.0294; 0.0308;
Table 8 0.0259; 0.0354; 0.0424; 0.0385; 0.0470; 0.0364; 0.0434;
Values of increments for the fixed increments procedure and accelerated aging 0.0323; - - -
procedure in 0 � C; 10 � C; 50 � C; 100 � C; 130 � C. 0.0403; -
E 0.0230; 0.0272; 0.0286; 0.0285; 0.0304; 0.0282; 0.0296;
Increments for the fixed increments Increments for the accelerated aging 0.0246; 0.0342; 0.0412; 0.0372; 0.0457; 0.0352; 0.0422;
procedure in 0 � C; 10 � C; 50 � C; 100 � C; procedure in 0 � C; 10 � C; 50 � C; 100 � C; 0.0310; - - -
130 � C 130 � C 0.0390; -
W/(mK) W/(mK) F 0.0289; 0.0366; 0.0380; 0.0344; 0.0365; 0.0376; 0.0390;
0.0055; 0.0058; 0.0062; 0.0067; 0.0068 0.0010 0.0307; 0.0436; 0.0506; 0.0441; 0.0536; 0.0446; 0.0516;
0.0379; 0.0548 0.0591 0.0558
0.0469;
0.0523

8
A. Winkler-Skalna and B. Łoboda Journal of Building Engineering 31 (2020) 101348

Fig. 8. The difference between the λ coefficient obtained using fixed increments procedure and the λ coefficient obtained using accelerated aging procedure.

using accelerated aging procedure, for 50 C the difference between the results obtained using the fixed increments procedure are signifi­
results obtained from the two procedures was not significant, while for cantly higher than using the accelerated aging procedure.
100 � C and 130 � C significantly higher results were obtained from fixed � For PUR of 120 kg/m3 density for 0 � C and 10 � C higher results were
increments procedure. obtained using accelerated aging procedure, for 50 C the difference
between the results obtained from the two procedures was not sig­
5. Conclusions nificant, while for 100 � C and 130 � C significantly higher results were
obtained from fixed increments procedure.
The results of research studies presented in the paper involving the
changes of thermal conductivity λ coefficient of thermal insulation cy­ The biggest difference (8,9%) between the λ coefficient values
lindrical products made of closed-cell polyurethane foam (PUR) blown received using two aging procedures was obtained for PUR type D for an
with n-pentane, constitute a significant database of information that can average measurement temperature of 100 � C. The differences in the λ
be useful both for manufacturers of these products and for designers of coefficient values calculated on the basis of different aging procedures
thermal insulation used mainly in industrial installations, but also in show that by choosing a fixed increments procedure we can determine
construction engineering. The presented analysis of results has demon­ the λ coefficient after aging in a shorter period of time (21 days), but its
strated that the applied aging procedure, based on the methodology for value will be higher (worse) than using a long accelerated procedure.
flat products in compliance with the standards EN 13165 and EN 14308, However, this is not the case with foam with a density of 120 kg/m3, for
can be accepted as appropriate for pipe insulation products. which, as mentioned in section 4.4 a more precise analysis of the
Significant influence on the range and velocity of the thermal con­ behavior of PUR foams of higher densities requires more laboratory tests
ductivity coefficient change of cylindrical products both foam density to be carried out.
and sample thickness was shown. For the density in the range from 40 Also PUR foams fabricated with the use of other blowing agents as
kg/m3 to 80 kg/m3, the total increment of the value λ coefficient after well as products of the densities and thicknesses outside the scope of this
175 days of conditioning is decreasing with the rising density. For work may be subjected to a similar testing. In further perspective, a
samples of the same thickness, the increment for foam of 80 kg/m3 simultaneous testing of the composition of cellular gas after subsequent
density at an average measurement temperature of 0 � C was 19,7% conditioning stages may be also carried out.
lower than for foam of 40 kg/m3 density. At 100 � C the difference was as Important in terms of processes involving the application/assembly
much as 55,4%. In this case there the difference increases with the of PUR coating is the information about very fast gas exchange occurring
temperature. The effect of sample thicknesses on the magnitude of λ in the initial period after the fabrication. For this reason, it is very vital
coefficient changes is smaller and ranges from about 2% to about 35%. for the manufacturers of insulation to safeguard the foam against air as
In this case there is no dependence on temperature. Within the range soon as possible, e.g. by applying an anti-diffusion layer on the coating.
tested, no significant influence of sample diameter was noted.
Based on the final calculations of the λ coefficient values after the Funding
application of fixed and accelerated aging procedures, the following
conclusions are made: This research was funded by Ministerstwo Nauki i Szkolnictwa
Wy_zszego (NZF-112/2019).
� For PUR of 40 kg/m3 density the differences in the results obtained
by both methods is not significant and are within the 3% uncertainty Declaration of competing interest
of measurement.
� For PUR of 60 kg/m3 to 80 kg/m3 density no significant difference The authors declare that they have no known competing financial
was recorded only for 0 � C and 10 � C. At higher temperatures, the interests or personal relationships that could have appeared to influence
the work reported in this paper.

9
A. Winkler-Skalna and B. Łoboda Journal of Building Engineering 31 (2020) 101348

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