Polymer Degradation and Stability 167 (2019) 1e9

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Polymer Degradation and Stability

journal homepage: www.elsevier.com/locate/polydegstab

Influence of residual chlorine and pressure on degradation of

polybutylene pipe
Takehiro Fujii a, b, Yuichi Matsui a, Hideo Hirabayashi b, Kazuhisa Igawa c, Saori Okada d,
Hidekazu Honma d, Hiroyuki Nishimura a, Kazushi Yamada a, *
a
Faculty of Fiber Science and Engineering, Kyoto Institute of Technology, Matsugasaki, Sakyo-ku, Kyoto, 606-8585, Japan
b
Shinwasangyo Co. Ltd, Suminoe-ku, Osaka, 559-0015, Japan
c
Maezawa Kyuso Industries Co. Ltd, Motomiya City, Fufukshima, 969-1204, Japan
d
KRI Inc, Konohana-ku, Osaka, 554-0051, Japan

a r t i c l e i n f o a b s t r a c t

Article history: In this paper, we report a novel technique that enabled us to easily and effectively conduct an accelerated
Received 6 November 2018 degradation test on a small pressure vessel for potable and hot water pipes. Accelerated degradation tests
Received in revised form were carried out on polybutene (PB) pipes with and without pressurization, under chlorinated and non-
15 June 2019
chlorinated water at 80  C; the higher-order structure changes, residual antioxidant agents, and degra-
Accepted 17 June 2019
dation characteristics of the PB pipes were evaluated. In the degradation test under chlorine water, the
Available online 19 June 2019
isothermal oxidation induction time (I-OIT) time and the mechanical properties decreased with
increasing aging time. Additionally, micro- Fourier transform infrared spectroscopy (FT-IR) imaging
Keywords:
Residual chlorine
revealed the distribution of antioxidants in the PB pipe before and after the test, while in the degradation
Accelerated degradation test test under pressure, the residual amount of antioxidants was smaller, and the chemiluminescence in-
Polybutylene tensity was higher compared with the test that was not pressurized. These results strongly suggest that
Water pressure not only dissolved chlorine but also water pressure contribute to promoting the degradation of plastic
pipes, and that the simple pressure vessels allow the safe and easy testing of accelerated degradation.
© 2019 Elsevier Ltd. All rights reserved.

1. Introduction
Copper pipes for water supply and hot water supply have been
replaced by plastic pipes such as polyethylene (PE), crosslinked
polyethylene (PEX), and polybutene (PB), which have many ad-
vantages, such as flexibility and corrosion resistance, and are
widely used in the construction of new houses. In addition, since
these pipes are installed in walls and floors for use as domestic
piping, it is extremely difficult to easily exchange these plastic
pipes. Therefore, creep tests [1e4] and accelerated degradation
tests [5e8] for PE, PEX, and PP pipes, are very important for eval-
uating the long-term durability of plastic pipes.
Generally, tap water is sterilized with methods such as ozona-
tion, ultraviolet (UV) radiation, or with chlorine compounds, such
as chlorine dioxide (ClO2), chlorine hydroxide (HOCl), and sodium
chlorite (NaClO2), in order to make tap water potable, and many
studies on sterilization processing have been conducted [9e12].
* Corresponding author.
E-mail address: kazushi@kit.ac.jp (K. Yamada).
However, these compounds remain in taps and pipes, and this re-
sidual chlorine degrades many substances in contact relatively
rapidly. Therefore, extensive research on plastic pipes [13e15] and
films [16,17] has been conducted, to understand the influence of
residual chlorine on pipes.
On the other hand, PB pipes were in use in the United States
since the late 1970s; however, they are not currently used in the
U.S. and Canada due to degradation problems, with PEX pipes being
mainly used currently. As PB pipes are inexpensive and relatively
flexible, with the same properties as PEX, they are currently used
and installed as piping for water and hot water supply in the EU,
China, South Korea, and Japan. PB is obtained by polymerizing
butene-1, which is a decomposition product of naphtha obtained
with a catalyst such as the Ziegler-Natta catalyst [18e20]. PB has a
high molecular weight, between 1,000,000 and 3,000,000 (g/mol),
exceptional heat creep resistance, stress crack resistance, impact
resistance, and abrasion resistance e properties which are not
found in thermoplastic resin due to the specificity of the molecular
structure; further, its elastic modulus is low and it is flexible
compared with HDPE and PP.. As with general polyolefins, PB pipes

https://doi.org/10.1016/j.polymdegradstab.2019.06.012
0141-3910/© 2019 Elsevier Ltd. All rights reserved.
2 T. Fujii et al. / Polymer Degradation and Stability 167 (2019) 1e9
are also excellent for water and chemical resistance, and electrical
insulation; owing to its excellent heat creep resistance and flexi-
bility, PB is used in various water supply and oil feed pipes.
To investigate the influence of tap water on plastic pipes in the
long-term, it is important to add not only chlorine water but also
examine the influence under a water hammer and high-pressure
environment. However, there is no research on accelerated degra-
dation tests under a high concentration of chlorine and high
pressure on the PB pipe. In addition, it is very important to evaluate
the degradation of PB pipes, which are still widely used with
chlorine and under pressure. Therefore, in this study, we aim to
evaluate the influence of residual chlorine on the long-term dura-
bility. An accelerated degradation test was conducted in a self-
produced pressure vessel under a water pressure of 0.5 MPa and
a chlorine concentration of 30 ppm. We discussed the effects of
residual chlorine and pressure with results from differential scan-
ning calorimetry (DSC), isothermal oxidation induction time (I-
OIT), Fourier transform infrared spectroscopy (FT-IR), and scanning
electron microscopy (SEM) analyses, as well as chemiluminescence
(CL) measurements and tensile tests.
2. Materials and methods
2.1. Materials
In this study, a PB pipe (JIS K 6792) manufactured by JFE Pipe
Fitting Mfg. Co. Ltd., Japan, was used. The pipe had an outer
diameter of 13 mm, inner diameter of 9.8 mm, and a thickness of
1.6 mm; further, all pipes were cut to a length of ca. 30 cm, so as to
fit in the pressurized container. A sodium hypochlorite solution
(NaClO, Grade: Extra pure grade; Purity > 5.0%; Kanto Chemical Co.
Ltd., Japan) was used as a concentration turning agent in the
accelerated degradation test.
2.2. Accelerated degradation test
An accelerated degradation test was conducted to evaluate the
long-term durability of the samples and the effect of water pressure
and residual chlorine. Table 1 shows the water pressure and re-
sidual chlorine conditions in the accelerated degradation test. Four
types of accelerated degradation tests were carried out at 80  C in a
high-temperature chamber (PH-402, Espec Corp., Japan). The con-
centration of hypochlorite was adjusted to 30 ppm every morning,
and the chlorine water in the container was replaced once a week.
In this research, the pH was controlled from 7.5 to 8, and it is
considered that the water included both HOCl and ClO . Addi-
tionally, in order to prevent the pipe from moving in the pressure
vessel, it was set to be the same as the pipe length and the height
inside the vessel. An illustration of the accelerated degradation test
is shown in Fig. 1. Firstly, PB pipe specimens in the self-produced
pressure vessel were placed in a constant-temperature chamber
set to each condition. Thereafter, samples were collected after 500,
1,000, 3,000, and 5000 h, and used for measurement. The pressure
vessel is made of stainless steel (SUS304), with an inner diameter of
170 mm and a depth of 200 mm. Note that the Teflon bag is put
inside the container and the chlorine water and sample pipes are
Table 1
Conditions of chlorine and water pressure in the accelerated degradation test.
Chlorine conc. (ppm) Water pressure (MPa)
Condition 1 0 0 degradation test were characterized by tensile testing. Specimens
Condition 2 0 0.5
Condition 3 30 0 2-1BA using a Super Dumbbell cutter (SDL-100: Dumbbell Co. Ltd.,
Condition 4 30 0.5
put in the bag in order to prevent the stainless-steel container from
being affected by chlorine.
2.3. Differential scanning calorimetry
Differential scanning calorimetry (DSC) was performed with a
Thermal Analysis DSC 2920 TA Instrument. To evaluate the thermal
history of each specimen after the accelerated degradation test, 1st
heating curves were recorded at 50  C/min from 40  C to 230  C
under the flow of nitrogen gas at 50 mL/min. The average values of
heat of fusion (DH) and melting point (Tm) in DSC were evaluated
using three independent samples. In this research, the melting
point was defined as the melting peak temperature (ºC).
2.4. Isothermal oxidation induction time (I-OIT) measurement
To evaluate the oxidative stability of the PB pipes, isothermal
oxidation induction time (I-OIT) measurement was performed us-
ing DSC equipment (DSC-60A, Shimadzu, Corp., Japan). The
experimental method for I-OIT is illustrated in Fig. 3(a). Firstly, a
sample was heated in nitrogen atmosphere, following which the
temperature was maintained at 200  C. After 7.5 min, the atmo-
sphere was changed to oxygen. After changing to oxygen, the time
from the gas change to the observed exothermic peak was
measured.
2.5. 2D imaging analysis with micro-FT-IR spectroscopy
To measure the oxidation state and distribution of antioxidants
in each sample, the 50 mm-thick sample was sliced with a micro-
tome and imaged at 600 mm  600 mm square, and analyzed using
FT-IR (Nicolet iN10 MX, Thermo Fisher Scientific, Japan). The
measurement range was 4000 cm 1 to 400 cm 1. The wavenumber
resolution was 8 cm 1 and the integration frequency was 16 times/
point. The semi-quantitative analysis mode by area ratio was used
for 2D color imaging. Generally, a carboxyl group is formed on the
surface when the polyolefin is oxidized [21]. For oxidative degra-
dation evaluation, the peak area of 1720 cm 1 1705 cm 1 derived
from the carboxyl group generated by oxidation (the peak around
1714 cm 1, [21]) was calculated and mapped with
1850 cm 1 1690 cm 1 as the baseline. To identify the antioxidants,
the peak area of 1765 cm 1 1720 cm 1 derived from the carboxyl
group of the antioxidant (the peak around 1745 cm 1, [22]) was
calculated and mapped from 1850 cm 1 to 1690 cm 1 as the
baseline. The chemical structures of antioxidants and FT-IR spectra
of PB are shown in Fig. 4(a) and (b).
2.6. Chemiluminescence measurement
To evaluate the surface oxidation degradation of the PB pipes, CL
measurements were conducted with a CL analyzer (CLA-FS3,
Tohoku Electronic Industrial Co. Ltd., Japan). A sample cut from the
PB pipe was used for each condition. The total intensity of the CL
spectra was recorded at 120  C for 10 min under a flow of 150 mL/
min of nitrogen gas. The pipe for measurement was immersed in
hot water at 80  C for 8 h before CL measurement to remove the
mold release agent from the surface of the molded pipe.
2.7. Tensile test
The mechanical properties of the PB pipes after the accelerated
from each PB pipe were shaped to a dumbbell according to ISO 527-
Japan). The tensile tests were performed using a universal testing
 T. Fujii et al. / Polymer Degradation and Stability 167 (2019) 1e9
Fig. 1. Illustration of accelerated degradation test and each specimen.
machine (TGI-50kN: Minebea-Mitsumi Inc., Japan) at 25  C at a
crosshead speed of 100 mm/min. The average values ± standard
deviations of tensile strengths and elongation at break were eval-
uated using three independent specimens. In this research, tensile
strength was defined as ultimate stress.
2.8. Scanning electron microscopy
The pipe surface and fractured surface of each sample before
and after the accelerated degradation test at 80  C were observed
by scanning electron microscopy (SEM, JSM-6010LA InTouchScope,
JEOL, Japan). The electron accelerating voltage was set at 10 kV. All
specimens were coated with gold using an ion sputtering machine
(JFC-1600 Auto Fine Coater: JEOL Co. Ltd., Japan) before the SEM
observation.
3. Results and discussion
3.1. Thermal properties of PB pipes before and after the accelerated
degradation test
Typical DSC curves of each sample up to 5000 h at 80  C before
and after the accelerated degradation test are shown in Fig. 2(a).
After the accelerated degradation test, for all conditions, the
melting point increased. The heat of fusion and the melting point of
each sample up to 5000 h at 80  C before and after the accelerated
degradation test for all conditions are shown in Fig. 2(b) and (c).
The heat of fusion after the accelerated degradation test and the
melting enthalpy (DH) increased with increasing the elapsed time.
Generally, when a polymer is maintained above its crystallization
temperature, crystallization is promoted [23]. A constant heat
treatment at 80  C may provide a good crystallization condition,
considering that Tc is approximately 75  C [24]. Therefore, it is
assumed that the increase of DH is due to the promotion of the
crystallization of PB.
DSC is among the methods to evaluate oxidative stability, in
terms of the oxidation induction time (OIT). Generally, a polymer is
oxidized in an oxygen-rich atmosphere, which degrades the me-
chanical and thermal properties. In this study, an I-OIT measure-
ment was performed using DSC, in order to evaluate the oxidative
stability of the PB pipes at 200  C, as shown in Fig. 3(a). Typical I-
OIT exotherm curves of the PB pipes are presented in the graph, and
the OIT was defined as the amount of time elapsed until the
exothermal oxidation of the sample begins. Fig. 3(b) shows the I-
OIT values for all conditions of the PB pipes before and after the
3
accelerated degradation test. The I-OIT of the PB pipe for 0 MPa and
0 ppm was almost constant at 100 min, without decreasing, until
5000 h, whereas the I-OIT of the PB pipes for other conditions
decreased with increasing accelerated degradation time. Addi-
tionally, in samples corresponding to conditions 0 MPa, 30 ppm and
0.5 MPa, 30 ppm, with the addition of chlorine, the I-OIT values
remarkably decreased, compared with the samples without the
addition of chlorine. In this case, the I-OIT after 5000 h was
approximately 10 min or less. Chlorine derivatives affect the
oxidation of antioxidants in the pipes, as the I-OIT of the PB pipe
decreases by immersing the pipe in chlorine water [25]. Moreover,
the I-OIT of the sample that was accelerated and degraded in the
pressurized container, clearly decreased, compared with the un-
pressurized sample. These results strongly suggest that not only the
presence of chlorine derivatives, but also the water pressure affects
the degradation of a PB pipe.
3.2. FT-IR and chemiluminescence analysis before and after
accelerated degradation test
To confirm the effect of chlorine derivatives or water pressure
on degradation, we measured the oxidation state and distribution
of antioxidants in each sample by FT-IR spectroscopy with semi-
quantitative analysis mode. It is possible to reduce noise and
measure on the sample surface with high sensitivity by using the
semi-quantitative analysis based on the area ratio. After degrada-
tion, the absorption band around 1714 cm 1, which can be assigned
to the C]O stretching vibration of a ketone group, grows in in-
tensity with extended aging [6,21]. Therefore, the peak area of
1720 cm 1 to 1705 cm 1 derived from the carboxyl group generated
by the oxidation was calculated and mapped with 1850 cm 1 to
1690 cm 1 as a baseline. Fig. 4 shows the 2D image of the carboxyl
groups, which are attributed to the oxidation of pipe samples from
the surface to the inside. In the figure, the bright (red) color in-
dicates that the degree of oxidation is higher, whereas the darker
(blue) color represents the raw pipe that is not oxidized. This shows
that the vicinity of the pipe surface became slightly brighter due to
oxidation degradation with increasing immersion time. On the
other hand, the color inside the PB pipe hardly changed as
compared with the color of surface, and this indicates that the
surface is more easily oxidized than the inside.
Antioxidants are generally reduced by physical migration and
leaching into the contact environment [22,26,27]. Therefore, it is
important to map the amount of migration or decrease of the
antioxidant with the increase of the degradation time in order to
4 T. Fujii et al. / Polymer Degradation and Stability 167 (2019) 1e9

Fig. 2. Typical DSC curves, heat of fusion, and melting point of each sample after accelerated degradation test.

Fig. 3. Typical I-OIT curves (a) and I-OIT plots (b) for each condition before and after accelerated degradation test.
 T. Fujii et al. / Polymer Degradation and Stability 167 (2019) 1e9 5

Fig. 4. Micro-FT-IR images of carboxyl groups by FT-IR from the surface to the inside for each condition, (a) chemical structures of antioxidants, (b) FT-IR spectra of PB pipe surface,
(c) 2D mapping.
6 T. Fujii et al. / Polymer Degradation and Stability 167 (2019) 1e9
evaluate the degradation of the pipe. As the absorption band
around 1745 cm 1, which can be assigned to the C]O stretching
vibration of a ketone group of antioxidants [6,22,26,28], the peak
area of 1765 cm 1 1720 cm 1 derived from the carboxyl group of
the antioxidant was calculated and mapped with 1850 cm cm 1 to
1690 cm 1 as a baseline. Fig. 5 shows 2D images indicating the
amount of antioxidants in the PB pipe from the surface to the in-
side. The image shifts from red to blue as the degradation time
increases in all conditions: that is, the amount of antioxidant in the
PB pipe decreases with elapsed time. Especially since red or orange
cannot be seen at 3000 h or more, it is found that the degradation is
suddenly promoted. Comparing the effects of water pressure with
and without chlorine at 0.5 MPa, the surface of the sample at
0.5 MPa and 0 ppm for 1000 h changed blue in color, and the color
of the inside for 0 and 30 ppm at 0.5 MPa changed to orange,
whereas the sample at 0 MPa retains the red color. In images after
5000 h, the sample with water pressure was generally nearly blue
in color, whereas the color of the sample without water pressure
remained light green. These results indicate that by applying water
Fig. 5. Micro-FT-IR images of antioxidants by FT-IR from the surface to the inside for each condition.
pressure, the amount of antioxidant inside the PB pipe decreases
faster than in the sample that does not apply water pressure.
Comparing the influence of chlorine with water pressure, the
sample with water pressure at 0.5 MPa was slightly darker in color
as compared with 0 MPa, and additionally the sample accelerated
with chlorine became blue faster than the sample without chlorine.
It is noted that the peak area of 1765 cm 1 1720 cm 1 derived
from the carboxyl group may contain a slight amount of degraded
products associated with the oxidative degradation of the PB
pipe and the antioxidants. If the amount of the degraded product
is larger than that of the antioxidant in the range of
1765 cm 1 1720 cm 1, the peak area may increase with the in-
crease of the accelerated degradation time. However, as the peak
area decreased with the increase of degradation time, ie the color of
the 2D image shown in Fig. 5 approaches blue, this trend is in good
agreement with the results of S. Damodaran et al. [6]. We consider
that the influence of degraded products on the peak area is
extremely low. Therefore, it was concluded that the rate of decrease
of the antioxidant is higher in the accelerated degradation test with
 T. Fujii et al. / Polymer Degradation and Stability 167 (2019) 1e9
Fig. 6. Typical chemiluminescence spectra (a) and plots of maximum intensity (b) of each spectrum after accelerated degradation test.
chlorine water and this method is very useful for visualizing the
degradation process with time inside the resin.
Owing to the easy oxidation of the PB pipe with decreasing
amount of antioxidant, the change in the CL intensity due to
oxidative degradation of the PB pipe was evaluated. Fig. 6 shows
the typical total intensity curves of CL for 0 MPa, 0 ppm and the plot
of the maximum CL intensity for each sample. From Fig. 6(a), the CL
intensity of PB for 0 MPa, 0 ppm gradually decrease with increasing
aging time. On the other hand, the CL intensity of the samples
accelerated and degraded under water pressure or chlorine water,
increases with increasing degradation time in Fig. 6(b). It should be
noted here that the CL intensity values obtained under water
pressure are higher than those without water pressure. Degrada-
tion of the polymer is accelerated by chlorine ions [29,30], and the
polymer that is oxidatively degraded exhibits higher CL intensity
than the sample before degradation [31]. The CL intensity change
indicates that the degradation of the PB pipe is promoted by
chlorine water, whereas the degradation of the PB pipes is accel-
erated due to decreasing amount of the antioxidant even under
water pressure. This trend supports the results of micro-FT-IR im-
aging in Fig. 5.
3.3. Mechanical properties and morphology before and after
accelerated degradation test
To evaluate the mechanical properties of the PB pipe after the
accelerated degradation test, a tensile test was conducted with a
dumbbell-shaped specimen cut out from the PB pipe. The
maximum load and elongation at break are shown in Fig. 7. The size
Fig. 7. Mechanical properties of each sample after accelerated degradation test, (a) maximum load and (b) elongation at break.
7
of the dumbbell-shaped specimen is the same for all samples;
however, because the minor axis direction of the specimen is
slightly curved along the arc of the pipe, the evaluation was per-
formed with the maximum load and elongation at break of the
load-displacement diagram in the tensile test. The maximum load
of the PB pipe after the accelerated degradation test decreased with
increasing elapsed time, whereas the maximum load of the PB pipe
degraded under 30 ppm chlorine water had lower values,
compared with the chlorine-free water. In addition, the elongation
at break of the PB pipe after the accelerated degradation test also
decreased with increasing elapsed time, while the elongation at
break of the PB pipe degraded under 30 ppm chlorine water yielded
lower values as compared with the chlorine-free water. It has been
reported that the mechanical properties of PE pipes are also
degraded by chlorine water [32,33], and the results of the present
study with PB pipes concur.
Fig. 8 shows the SEM images of the pipe surface and fracture
surface of each sample after an accelerated degradation test for
5000 h, conducted after the tensile test. SEM images show that the
surface of the PB pipe accelerated and degraded in the chlorine
water environment possesses larger irregularities on the surface,
compared with the pipe accelerated and degraded with chlorine-
free water. Furthermore, as shown in the inset, small cracks are
formed on the pipe surface by degradation with water pressure or
chlorine water. These cracks were attributed to advanced material
embrittlement, and were influenced by the effects of water
pressure and chlorine derivatives [13,32]. On the other hand,
SEM images of the fracture surface indicate dependence on the
presence or absence of chlorine derivatives; that is, many ductile
8 T. Fujii et al. / Polymer Degradation and Stability 167 (2019) 1e9

Fig. 8. SEM images of pipe surface and fracture surface after accelerated degradation test for 5000 h.

parts are observed on the fracture surface of the sample acceler-
ated and degraded with chlorine-free water, while the fracture
surface of the sample accelerated and degraded with chlorine
water is more brittle. These results strongly suggest that the
degradation of PB pipes is accelerated not only by chlorine water
but also by the removal of antioxidants under the influence of
water pressure.
4. Conclusion
This study aims to provide novel strategies for the accelerated
degradation test, such as aging tests by immersion into hot water,
based on the effect of water pressure. Here, a self-produced pres-
sure vessel was used to evaluate the influence of residual chlorine
and water pressure on the long-term durability, and accelerated
 T. Fujii et al. / Polymer Degradation and Stability 167 (2019) 1e9
degradation tests were performed at a high concentration of
chlorine (30 ppm) or water pressure (0.5 MPa). In the accelerated
degradation test with chlorine water, the I-OIT and mechanical
properties of the PB pipes showed degradation, whereas with water
pressure, the amount of antioxidants in the PB pipe, I-OIT, and the
mechanical properties decreased with increasing elapsed time. On
the other hand, the CL intensity change indicated that the degra-
dation of the PB pipe was promoted by chlorine water, and accel-
erated due to decreasing amount of the antioxidant even under
water pressure. Additionally, the antioxidants distributed in the PB
pipes could be mapped, and the decreasing change due to the
accelerated degradation test was visualized by micro-FT-IR imag-
ing. We strongly believe that our simple accelerated aging test
method with a pressure vessel can overcome the limitations of
conventional and complicated test methods. These results will
provide many possibilities to evaluate plastic pipes for drinking
water supply and hot water supply via the accelerated degradation
test. A continuous accelerated degradation test is also being
developed for industrial up-scaling.
Acknowledgement
The authors deeply appreciate the experimental assistance from
the laboratory staff and students at the Kyoto Institute of
Technology.
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.polymdegradstab.2019.06.012.
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