energies
Article
Effects of Pre-Crosslinking on Space Charge and Breakdown
Characteristics of XLPE Cable Insulation
Zhenpeng Zhang 1,2 , You Wu 3, *, Chao Fu 2 , Shaoxin Meng 1,2 , Chao Peng 2 , Zhonglei Li 3, *






Citation: Zhang, Z.; Wu, Y.; Fu, C.;
Meng, S.; Peng, C.; Li, Z.; Du, B.
Effects of Pre-Crosslinking on Space
Charge and Breakdown
Characteristics of XLPE Cable
Insulation. Energies 2022, 15, 2360.
https://doi.org/10.3390/en15072360
Academic Editor: Pawel Rozga
Received: 13 February 2022
Accepted: 22 March 2022
Published: 24 March 2022
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with regard to jurisdictional claims in
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iations.
Copyright: © 2022 by the authors.
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This article is an open access article
distributed under the terms and
conditions of the Creative Commons
Attribution (CC BY) license (https://
creativecommons.org/licenses/by/
4.0/).
Energies 2022, 15, 2360. https://doi.org/10.3390/en15072360
and Boxue Du 3
1 State Key Laboratory of Power Grid Environmental Protection, Wuhan 430073, China;
13971276891@163.com (Z.Z.); shaoxinmeng@163.com (S.M.)
2 China Electric Power Research Institute, Wuhan 430073, China; chaofu@163.com (C.F.);
pengchao@163.com (C.P.)
3 Key Laboratory of Smart Grid of Education Ministry, School of Electrical and Information Engineering,
Tianjin University, Tianjin 300072, China; boxuedu@tju.edu.cn
* Correspondence: wuyou1021@tju.edu.cn (Y.W.); lizhonglei@tju.edu.cn (Z.L.)
Abstract: This study focused on the effect of pre-crosslinking on the electrical properties of XLPE
insulation for HVDC cables. The XLPE samples were pre-crosslinked at 140, 150 and 160 ◦ C. The space
charge and DC breakdown characteristics of the XLPE samples with and without pre-crosslinking
were investigated. The results show that the pre-crosslinked XLPE samples have an obvious space
charge injection and transportation, resulting in more severe electric field distortion. Under the
electric field of 100 kV/mm, the electric field distortion rates of the XLPE samples pre-crosslinked
at 150 and 160 ◦ C reached 51% and 72% respectively, which were much higher than that of the
XLPE sample without pre-crosslinking (14%.) Compared with the XLPE without pre-crosslinking,
the breakdown strengths of XLPE pre-crosslinked at 140, 150 and 160 ◦ C were reduced by 11%, 6%
and 7% respectively, at the temperature of 50 ◦ C. It is concluded that the pre-crosslinking leads to
imperfect crystallization and micro-defects in the amorphous region of XLPE, thereby leading to more
space charge accumulation and reduced DC breakdown. The pre-crosslinking of XLPE insulation
therefore should be prevented during HVDC cable manufacturing.
Keywords: HVDC cable; XLPE insulation; space charge; breakdown strength
1. Introduction
As a basic requirement of economic development, the electric power industry plays
an irreplaceable role in human life. However, there is a contradiction between supply and
demand in the power industry, and the generation of high-voltage direct current (HVDC)
transmission provides a new option to solve this problem. It is worth noting that the
insulation problem has always been a key problem that has restricted the development
of greater transmission capacity and grades. Due to their advantages of long distance,
large capacity and low loss, high-voltage submarine cables are an economical and effective
method to transmit power to islands or offshore platforms, and to achieve grid connection
of offshore wind power stations and interconnection of power grids [1–3]. The manufacture
of long-distance submarine cables can greatly improve the production efficiency, reduce
energy consumption, and reduce the number of factory connectors, thereby reducing the
impact of factory soft joints on cable insulation performance [4–6]. The main insulation
material of high-voltage cable is crosslinked polyethylene (XLPE), which is produced by
crosslinking polyethylene material. In the process of crosslinking, peroxide dissociates
at high temperature to form free radicals, the molecular chains of polyethylene can be
connected to each other in the form of crosslinking bonds, and their molecular structure
changes from a linear structure to a three-dimensional network structure. This process
also improves the overall heat resistance, dielectric properties and mechanical properties
of insulating materials [7–9]. However, in the 30-day continuous production process of
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Energies 2022, 15, 2360 2 of 13

high-voltage submarine cables, it is inevitable that the local extrusion temperature is too
high or the time is too long. Therefore, the crosslinking agent will be thermally decomposed
in advance under the action of high temperature in the extrusion process, resulting in the
pre-crosslinking of XLPE insulation [10,11]. The pre-crosslinked product of XLPE insulation
can generate gel, which blocks the filter screen of the extruder, thereby further affecting
the rheological properties during the insulation extrusion [12]. In addition, part of the
pre-crosslinked product may pass through the filter screen of the extruder into the cable
insulation, resulting in inherent defects in the insulation of the HV cable [13]. Therefore, it is
crucial to study the effect of pre-crosslinking on the electrical properties of cable insulation.
Space charge characteristics and DC breakdown characteristics are the key properties
for HVDC cable insulation that influence the reliability of cable insulation [14–16]. The
production process of XLPE cable successively includes the production steps of extrusion
molding, high-temperature crosslinking, cooling and degassing [17]. Among these, in
the research on the latter two steps, scholars in related fields have conducted a large
number of experimental studies. For the high-temperature crosslinking process, Liao et al.
investigated the effect of the concentration of DCP agents on the space charge accumulation,
and found the increased crosslinking degree can effectively increase the electric field
threshold for space charge injection, thereby suppressing the injection of space charges into
XLPE insulation [18]. Zhong et al. researched the influence of the crystal and crosslinked
morphology on the breakdown strength of XLPE insulation for submarine cable factory
joints. It was demonstrated that there is an increase in the content of crosslinked by-products
and a reduction in grain size and crystallinity in the XLPE insulation of factory joints,
thereby resulting in a lower breakdown strength than that of the cable bulk insulation [19].
Regarding the process of cooling and degassing, Zhou et al. studied the effect of the
non-isothermal crystallization process on the onset and motility of positive space charge
packets in low density polyethylene (LDPE). The results show that LDPE with a lower
cooling rate has higher crystallinity and trap depth, resulting in a lower charge motility
and the accumulation of a large number of space charges [20]. Yin et al. found that
prolonging the degassing time can effectively reduce the by-products of DCP and inhibit
the ionized heterocharges, thereby improving the space charge characteristics of XLPE
cable insulation [21]. However, the influence of extrusion temperature on the insulation
properties of materials in the extrusion molding stage is often ignored. In view of the fact
that insufficient experimental exploration of the process of material pre-crosslinking has
been undertaken, the influence of this process on XLPE insulation performance, and its
mechanism, are not clear.
This study investigated the effect of pre-crosslinking on the electrical properties of
XLPE insulation for HVDC cables. The XLPE samples were pre-crosslinked at 140, 150
and 160 ◦ C. The space charge and DC breakdown characteristics of the XLPE samples with
and without pre-crosslinking were investigated, and the effects of crystallinity and crystal
morphology on the space charge and breakdown strength were analyzed.

2. Materials and Methods

2.1. Materials
The raw material was supplied by Borealis Company (Vienna, Austria) and had a
density of ~0.92 g/cm3 , and mainly contained low-density polyethylene (LDPE), dicumyl
peroxide (DCP) and anti-oxide agents. In this study, the pre-crosslinking temperature of
XLPE insulating material was set at 140, 150 and 160 ◦ C, followed by high temperature
crosslinking at 180 ◦ C. The specific steps were as follows. The XLPE was melted at a
temperature of 120 ◦ C for 10 min. Then, the pre-crosslinking process was carried out
at 140, 150 and 160 ◦ C, while maintaining the pressure at 15 MPa for 15 min. After the
pre-crosslinking, the samples were fully cured for 15 min at a temperature of 180 ◦ C and
a pressure of 15 MPa. All the above tests were carried out in a flat vulcanizer. Using this
method, sheet XLPE insulation materials with thicknesses of 100 and 200 µm were prepared.
To eliminate the by-products of crosslinking, the prepared materials were put in a vacuum
Energies 2022, 15, 2360 3 of 13

chamber at a temperature of 80 ◦ C for 48 h before testing. In addition, the XLPE without

pre-crosslinking was prepared as a reference. These samples were melted at a temperature
of 120 ◦ C for 10 min, and then crosslinked at a temperature of 180 ◦ C and a pressure of
15 MPa for 15 min

2.2. Methods
In order to analyze the effect of pre-crosslinking temperature on the crystallization of
XLPE insulation, a scanning electron microscope (SEM, Merlin Compact, ZEISS Company
of Germany) was employed to observe the spherulite morphology of the XLPE samples
after surface etching. The surface-etching process was carried out in a mixed solution of
98% concentrated sulfuric acid solution and potassium permanganate powder (95 and
5 mass parts, respectively) for 4 h. The etched XLPE samples were cleaned with deionized
water to remove impurities on the surface of the samples, so as to avoid affecting the
SEM images.
The pulse electroacoustic (PEA) method was employed to investigate the space charge
behavior of the XLPEs. The HV electrode is a semiconducting layer, and the ground
electrode is aluminum. The specific settings of the PEA experimental equipment can
be found in our previous paper [22]. The 10 min polarization experiment at −75, −100
and −125 kV/mm, and the 10 min depolarization experiments, were carried out at room
temperature for each sample. Furthermore, in order to ensure the repeatability of the
experiment and the validity of the data, each group of samples was tested 3 times during
the experiment.
Breakdown strength experiments were carried out using a system comprising a pair of
ball-plate electrodes at 30, 50 and 70 ◦ C [23]. The high-voltage upper ball-plate electrode is
a copper sphere with a radius of 12.5 mm, the grounded lower electrode is a copper circular
plate with a radius of 17.5 mm, the edge chamfer is an arc with a radius of 12.5 mm, and
the upper and lower electrodes are coaxial. To prevent flashover during voltage boost, the
XLPEs and electrodes were dipped in insulating oil. A DC power source with a ramping
speed of 1 kV/s was used for this measurement. The tests were repeated 15 times for each
material, and the test results were analyzed using the Weibull distribution.
The two-parameter Weibull distribution can be expressed as:
"   #
E β
P( E) = 1 − exp − (1)
α

where α is the scale parameter, indicating the corresponding DC breakdown field strength
value when the breakdown probability is 63.2%, and β is the shape parameter, which is
inversely related to the data dispersion. E represents the breakdown strength.

3. Results
3.1. Effect of Pre-Crosslinking on Crystallization
Figure 1 shows the SEM images of surface-etched XLPE samples with and without pre-
crosslinking. It can be seen from the SEM images that the microscopic crystal morphology
of the XLPE samples with different components can be clearly observed. By comparing
the crystallization of XLPE samples with different pre-crosslinking temperatures, it can
be found that the spherulite size of the samples pre-crosslinked at 140 ◦ C (Figure 1a) is
significantly smaller than that of the other two groups of pre-crosslinked XLPE samples
and normal crosslinked samples. The spherulite size of the pre-crosslinked XLPE samples
at 150 and 160 ◦ C increased to a certain extent compared with the pre-crosslinked samples
at 140 ◦ C due to the increase in the pre-crosslinking temperature. At the same time, the
dispersion of the spherulite size was also increased accordingly. From the images, it can
also be seen that the amorphous region accounts for a large area in the microstructure of
the sample, which leads to a larger interval width between adjacent spherulites.
 The differential scanning calorimetry (DSC) test was employed to characterize the
crystallinity of the bulk XLPE samples. The crystallinity of the insulation with pre-cross-
linking temperatures of 140, 150, and 160 °C was 30.7%, 26.8% and 26.7%, respectively.
These value were significantly lower than that of the XLPE without pre-crosslinking
Energies 2022, 15, 2360 (34.3%). The crystallinity results obtained by the DSC test are consistent with the SEM 4 of 13
images.

(a) (b)

(c) (d)
Figure
Figure1. SEM images
1. SEM images of of
surface-etched
surface-etchedXLPE
XLPEsamples: (a) (a)
samples: pre-crosslinked XLPE
pre-crosslinked at 140
XLPE °C;◦ (b)
at 140 pre-
C; (b) pre-
crosslinked
crosslinked XLPE at at
XLPE 150150
°C; C;
◦ (c)(c)
pre-crosslinked XLPE
pre-crosslinked at at
XLPE 150150°C; C;
◦ (d)(d)
XLPE without
XLPE pre-crosslinking.
without pre-crosslinking.

3.2. Effect of Pre-Crosslinking

Compared on Space Charge Behaviors
with the pre-crosslinked XLPEs, the spherulite size of the XLPE sample
without pre-crosslinking is relatively uniform,
Figure 2 shows the space charge characteristics andandtheelectric
spherulites are closely arranged.
field distributions of the
Additionally, the distance between the spherulites is small,
XLPE samples under the DC electric field of −75 kV/mm at room temperature and the area ratioofof30
the amor-
°C. It
phous region is relatively small. Therefore, the crystal structure of the
can be seen from Figure 2 that, compared with the XLPE without pre-crosslinking, an ob- normally crosslinked
XLPE
vious insulating
injection sample
of space is relatively
charge more complete.
packets occurs in the pre-crosslinked XLPE samples during
The differential scanning calorimetry (DSC)
the polarization process. Under the action of an external test waselectric
employed to acharacterize
field, large number the crys-
of
tallinity of the bulk XLPE samples.
same-polarity charges are injected from The crystallinity
the anode of
side the
of insulation
the with
pre-crosslinked pre-crosslinking
XLPE sam-
temperatures of 140, 150, and 160 ◦ was 30.7%, 26.8% and 26.7%, respectively. These
ple. With the polarization process, the C
positive charge moves towards the cathode in the
value were significantly lower than that of the XLPE without pre-crosslinking (34.3%). The
form of charge packets until it migrates near the cathode and is extracted from the cath-
crystallinity results obtained by the DSC test are consistent with the SEM images.
ode. Among the pre-crosslinked XLPEs, the injection and migration of space charge pack-
ets3.2.
in the XLPE
Effect pre-crosslinked
of Pre-Crosslinking onat 140 Charge
Space °C were the most obvious, with the highest space
Behaviors
charge density. Additionally, the migration process of two space charge packets appeared
Figure 2 shows the space charge characteristics and electric field distributions of the
XLPE samples under the DC electric field of −75 kV/mm at room temperature of 30 ◦ C.
It can be seen from Figure 2 that, compared with the XLPE without pre-crosslinking, an
obvious injection of space charge packets occurs in the pre-crosslinked XLPE samples
during the polarization process. Under the action of an external electric field, a large
number of same-polarity charges are injected from the anode side of the pre-crosslinked
XLPE sample. With the polarization process, the positive charge moves towards the cathode
in the form of charge packets until it migrates near the cathode and is extracted from the
cathode. Among the pre-crosslinked XLPEs, the injection and migration of space charge
packets in the XLPE pre-crosslinked at 140 ◦ C were the most obvious, with the highest space
charge density. Additionally, the migration process of two space charge packets appeared
after 300 s, whereas only one space charge packet was injected in the pre-crosslinked XLPE
samples at 150 ◦ C and 160 ◦ C.
 Energies 2022, 15, 2360 5 of 13

阳极
Anode 阴极
Cathode 120 阳极
Anode 阴极
Cathode
80 0s
30s

Space charge density (C/m3 )

60s

Electric field (kV/mm)

40 100s 80
300s
600s
0 0s
40 30s
60s
-40 100s
0 300s
140℃预交联
Pre-crosslinked 140℃预交联
Pre-crosslinked 600s
-80 XLPE
at 140 °C XLPE
at 140 °C
-50 0 50 100 150 200 -50 0 50 100 150
Thickness (μm) Thickness (μm)
   
(a) 
  120
阳极
Anode 阴极
Cathode
80 Anode Cathode 0s
30s
60s

Electric field (kV/mm)

Space charge density(C/m3)

80
40 100s
300s
600s 0s
0 40 30s
60s
100s
-40
300s
0
150℃预交联
Pre-crosslinked 600s
Pre-crosslinked
at 150 °C
XLPE
-80 at 150℃
-50 0 50 100 150
-50 0 50 100 150 200 Thickness (μm)
Thickness (μm)  
 
(b) 
阳极 阴极 120
Anode Cathode 0s 阳极
Anode 阴极
Cathode
80
30s
Space charge density (C/m3 )

60s
Electric field (kV/mm)

40 100s 80
300s
600s
0
0s
40
30s
-40 60s
100s
0 300s
-80 Pre-crosslinked
160℃预交联 160℃预交联
Pre-crosslinked 600s
at 160 °C
XLPE XLPE
at 160 °C
-50 0 50 100 150 200 -50 0 50 100 150
Thickness (μm) 厚度 (μm)
Thickness
   
(c) 
阳极
Anode 阴极
Cathode 0s 阳极 阴极
80 Anode Cathode
30s
60s 80
Space charge density (C/m3 )

100s
40
Electric field (kV/mm)

300s
600s
0s
40 30s
0
60s
100s
300s
40 正常交联 正常交联 600s
Without XLPE
pre-crosslinking 0
Without
XLPEpre-crosslinking
-50 0 50 100 150 200 -50 0 50 100 150
厚度/ (μm)
Thickness Thickness (μm)
   
(d) 
Figure 
Figure2. 2.
Space  charge 
Space chargecharacteristics 
characteristicsand 
andelectric 
electricfield 
fielddistributions 
distributionsof ofthe 
the XLPE sample under
XLPE sample under the DC electric field of −75 kV/mm at a test temperature of 
the DC electric field of −75 kV/mm at a test temperature of 30 ◦ C: (a) XLPE pre-crosslinked at
30 °C: (a) XLPE pre‐crosslinked at 140 °C; (b) XLPE pre‐crosslinked at 150 °C; 
140 ◦ C; (b) XLPE pre-crosslinked at 150 ◦ C; (c) XLPE pre-crosslinked at 160 ◦ C; (d) XLPE without
(c) XLPE pre‐crosslinked at 160 °C; (d) XLPE without pre‐crosslinking. 
pre-crosslinking.

1 
 
Energies 2022, 15, 2360 6 of 13

The injection and migration of space charge packets also led to the occurrence of local
field intensity distortion inside the pre-crosslinked XLPE samples. Due to the injection of
the same polarity charge near the anode, an induced electric field opposite to the applied
electric field is generated, thereby weakening the electric field strength near the anode.
The migration process of the space charge packets leads to the enhancement of the local
electric field strength inside the insulating sample, and with the migration direction of the
charge packets, the enhancement of the local electric field gradually moves from the anode
to the cathode.
Figure 3 shows the space charge characteristics and electric field distributions of
the XLPE samples under the DC electric field of −100 kV/mm at room temperature of
30 ◦ C. It can be seen that the injection of space charge packets in the pre-crosslinked XLPE
samples under the −100 kV/mm DC electric field is more evident than that under the
−75 kV/mm DC electric field. The increase in the amount of charge injected from the
anode leads to a significant increase in the amplitude of the charge density of the injected
space charge packets inside the sample. When the polarization time is 100 s, the maximum
density of space charge packet of the XLPE pre-crosslinked at 140 ◦ C is only 40 C/m3 under
−75 kV/mm, whereas the space charge density amplitude under −100 kV/mm reaches
120 C/m3 . Additionally, an apparent negative space charge packet injection occurs at the
electric field of −100 kV/mm as the polarization time is 300 s.
By comparison, the injection depth and migration speed of space charge packets
inside the medium also increase significantly with the increase in the electric field. When
the polarization time was 300 s, the migration distance of the charge packets of the pre-
crosslinked XLPE samples at 140 ◦ C was 85 µm under −75 kV/mm, and did not migrate
to the cathode. However, under the DC electric field of −100 kV/mm, the first charge
packet appearing in the medium migrated to and was extracted from the cathode, and the
injection of the second space charge packet also occurred.
The increase in the amplitude of the charge density of the injected charge packet
in the insulating sample also caused more serious local electric field distortion in the
sample. Compared with the XLPE samples without pre-crosslinking, the 150 and 160 ◦ C
pre-crosslinked XLPE samples underwent obvious electric field distortion near the cathode
with the migration of charge packets, and the maximum electric field appeared in both
cases at the polarization time of 600 s. The electric field distortion rate is employed to
characterize the time-dependent electric field distribution inside the sample, which is
defined as follows [24]:
| Emax − E0 |
δ= × 100% (2)
E0
where Emax is the maximum electric field strength distorted by the space charge. E0 is the
average value of the applied field. The electric field distortion rates of the 150 and 160 ◦ C
pre-crosslinked XLPE samples reached 51% and 72%, respectively, which are much higher
than that of XLPE sample without pre-crosslinking (14%).
Figure 4 presents the space charge and electric field distributions of XLPE samples un-
der a DC electric field of −125 kV/mm at 30 ◦ C. Under the DC electric field of −125 kV/mm,
the space charge packets injected into the pre-crosslinked XLPE samples not only increased
the amplitude of the space charge packets, but also increased their width. From the migra-
tion process of the space charge packets in the pre-crosslinked XLPE medium at 140 ◦ C, it
can be observed that the migration speed of the injected positive charge packets gradually
slows during the process of migrating from the anode to the cathode under the action of
an external electric field. The reason for this phenomenon is that the electrons inside the
medium migrate from the cathode to the anode under the action of the external electric
field, whereas the positive space charge packets migrate from the anode to the cathode. The
electrons recombine with positive charges, resulting in a slowing of the migration of space
charge packets [25]. Compared with other XLPE insulation samples, multiple injections of
positive space charge packets appeared in the XLPE pre-crosslinked at 140 ◦ C.
 Energies
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150
阳极
Anode 阴极
Cathode 0s 160 Anode Cathode
30s

3)3 )
100

(C/m
60s

Electric field(kV/mm)
(C/m
120
100s

charge density
50 300s

空间电荷密度/
600s 80
0 0s
30s
40
60s
Space
-50
100s
140℃预交联
Pre-crosslinked 0 300s
-100 Pre-crosslinked
at 140
XLPE°C 600s
at 140℃
-50 0 50 100 150 200 -50 0 50 100 150
厚度/μm
Thickness (μm) Thickness（μm）
空间电荷分布
(a)
120 阳极
Anode 阴极
Cathode 阳极
Anode 阴极
Cathode
0s 150
30s
)
3)3

80
(C/m

60s

kV/mm)
field((kV/mm)
(C/m

100s
40 100
charge density

300s
空间电荷密度/

600s
0

电场强度/
0s
50
30s

Electric
-40 60s
Space

100s
-80 0 300s
150℃预交联
Pre-crosslinked 150℃预交联
Pre-crosslinked
600s
150 °C
at XLPE at 150 °C
XLPE
-120
-50 0 50 100 150 200 -50 0 50 100 150
厚度/μm(μm)
Thickness 厚度/μm
Thickness (μm)
空间电荷分布 电场强度分布
(b)
150 200
阳极
Anode 阴极
Cathode 0s 阳极
Anode 阴极
Cathode
30s
100
Space charge density (C/m 3 )

60s 150
(kV/mm)
空间电荷密度/(C/m3)

100s
(kV/mm

50 300s
600s 100
field

0
电场强度/

0s
50
Electric

-50 30s
60s
0 100s
-100
160℃预交联
Pre-crosslinked 160℃预交联
Pre-crosslinked 300s
160 °C
atXLPE at 160 °C
XLPE 600s
-150 -50
-50 0 50 100 150 200 -50 0 50 100 150
厚度/μm
Thickness (μm) 厚度/μm
Thickness (μm)
空间电荷分布 电场强度分布
(c)
150
阳极
Anode 阴极
Cathode 阳极
Anode 阴极
Cathode
100 0s
30s
3)
3)

60s
(C/m

(kV/mm)
)
(C/m

100
field(kV/mm

50 100s
charge density

300s
空间电荷密度/

600s
0s
电场强度/

0 50
30s
Electric

60s
100s
Space

-50
0 300s
正常交联
XLPE 正常交联 600s
Without pre-crosslinking Without
XLPE pre-crosslinking
-100
-50 0 50 100 150 200 -50 0 50 100 150
厚度/μm
Thickness (μm) 厚度/μm
Thickness (μm)
空间电荷分布 电场强度分布
(d)
Figure 3. Space charge characteristics and electric field distributions of the XLPE sample under the
Figure 3. Space charge characteristics and electric field distributions of the XLPE sample under
DC electric field of −100 kV/mm at a test temperature of 30 °C: (a) XLPE pre-crosslinked at 140 °C;
the DC electric field of −100 kV/mm at a test temperature of 30 ◦ C: (a) XLPE pre-crosslinked at
(b) XLPE pre-crosslinked at 150 °C; (c) XLPE pre-crosslinked at 160 °C; (d) XLPE without pre-
140 ◦ C; (b) XLPE pre-crosslinked at 150 ◦ C; (c) XLPE pre-crosslinked at 160 ◦ C; (d) XLPE without
crosslinking.
pre-crosslinking.
 Energies
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200
阳极
Anode 阴极
Cathode 0s 阳极 阴极
Anode Cathode

) 3)
200

Electric field (kV/mm)

(C/m3(C/m
150 30s
60s
100 150

Space charge density

100s

电场强度/(kV/mm)
50 300s
100

空间电荷密度/
600s
0
50
0s
-50 30s
0
60s
-100 100s
140℃预交联
Pre-crosslinked -50
-150 at 140 °C 140℃预交联
Pre-crosslinked 300s
XLPE
at 140 °C
XLPE 600s
-50 0 50 100 150 200 -100
厚度/μm(μm) -50 0 50 100 150
Thickness 厚度/μm
Thickness (μm)
空间电荷分布
电场强度分布
(a)
150 200
阳极
Anode 阴极
Cathode 0s 阳极
Anode 阴极
Cathode
100 30s
3)3 )

(kV/mm)
60s 150
(C/m

)
(C/m

(kV/mm
100s
50
300s
charge density

100
空间电荷密度/

600s

Electric field
0

电场强度/
0s
50 30s
-50 60s
100s
Space

0 300s
-100
150℃预交联
Pre-crosslinked 150℃预交联
Pre-crosslinked 600s
at 150 °C
XLPE at 150 °C
XLPE
-150 -50
-50 0 50 100 150 200 -50 0 50 100 150
厚度/μm
Thickness (μm) 厚度/μm(μm)
Thickness
空间电荷分布 电场强度分布
(b)
200
阳极
Anode 阴极
Cathode 阳极
Anode 阴极
Cathode
150 0s
30s
150
(kV/mm)

100 60s
3)3 )

(kV/mm )
(C/m

100s
(C/m

50 300s 100
charge density

600s
Electric field
空间电荷密度/

0s
电场强度/

0
50 30s
-50 60s
100s
0 300s
Space

-100 160℃预交联
Pre-crosslinked 160℃预交联
Pre-crosslinked 600s
atXLPE
160 °C at 160 °C
XLPE
-150 -50
-50 0 50 100 150 200 -50 0 50 100 150
厚度/μm(μm)
Thickness 厚度/μm
Thickness (μm)
空间电荷分布 电场强度分布
(c)
150
阳极
Anode 阴极
Cathode 0s 160 阳极
Anode 阴极
Cathode
30s
100
(C/m)3 )

60s
120
电场强度/(kV/mm)
3

Electric field (kV/mm)

100s
(C/m

50 300s
charge density

600s
空间电荷密度/

80
0s
0 30s
40 60s
-50 100s
Space

300s
正常交联 0
正常交联 600s
-100 Without pre-crosslinking
XLPE Without
XLPE pre-crosslinking
-50 0 50 100 150 200 -50 0 50 100 150
厚度/μm
Thickness (μm) 厚度/μm
Thickness (μm)
空间电荷分布 电场强度分布
(d)
Figure 4. Space
Figure charge
4. Space characteristics
charge and and
characteristics electric field field
electric distributions of theof
distributions XLPE samplesample
the XLPE under the
under
DC electric field of −125 kV/mm at a test temperature of 30 °C: (a) XLPE ◦ pre-crosslinked at 140 °C;
the DC electric field of −125 kV/mm at a test temperature of 30 C: (a) XLPE pre-crosslinked at
(b) XLPE pre-crosslinked at 150 °C; (c) XLPE pre-crosslinked at 160 °C; (d) XLPE without pre-
140 ◦ C; (b) XLPE pre-crosslinked at 150 ◦ C; (c) XLPE pre-crosslinked at 160 ◦ C; (d) XLPE without
crosslinking.
pre-crosslinking.
3.3. Effect of Pre-Crosslinking on Breakdown Strength
Energies 2022, 15, 2360 9 of 13

It is concluded that the pre-crosslinked XLPE samples significantly enhance the space
charge injection, which has a serious impact on the electric field distortion and insulation
aging during the operation of the DC cable.
Energies 2022, 15, x FOR PEER REVIEW 9 of 13

3.3. Effect of Pre-Crosslinking on Breakdown Strength

Figure 55 shows
Figure shows the
the Weibull
Weibull distributions
distributions of
of the
the DC
DC breakdown
breakdown strength
strength of
of XLPE
XLPE
samples atat 30,
30, 50
50 and
and 70 ◦
70 °C.
C. ItIt can
can be
be seen
seen that
that under
under any
any temperature
temperature condition,
condition, the
the
samples
breakdown field strength of the pre-crosslinked XLPE sample decreases significantly
breakdown field strength of the pre-crosslinked XLPE sample decreases significantly com-
pared with the normal XLPE sample. Among the samples, the breakdown field strength of
compared with the normal XLPE sample. Among the samples, the breakdown field
the pre-crosslinked XLPE sample at 140 ◦ C is the lowest, mainly resulting from its lower
strength of the pre-crosslinked XLPE sample at 140 °C is the lowest, mainly resulting from
degrees of crosslinking and crystallinity. The breakdown first occurred at the micro-defect
its lower degrees of crosslinking and crystallinity. The breakdown first occurred at the
inside the amorphous region, resulting in a lower breakdown field strength of the specimen
micro-defect inside the amorphous region, resulting in a lower breakdown field strength
compared to the other groups of XLPE specimens [26].
of the specimen compared to the other groups of XLPE specimens [26].

99 99

30 50

63.2 Weibull Probability (%) 63.2

Weibull Probability (%)

30 30

10 10

140 140
3 150
3
150
160 160
Without Without
1 1
290 310 330 350 370 250 275 300 325 350
Breakdown strength (kV/mm) Breakdown strength (kV/mm)
(a) (b)
99

70

63.2
Weibull Probability (%)

30

10

140
3 150
160
Without
1
180 205 230 255 280
Breakdown strength (kV/mm)
(c)
Figure 5. Weibull distributions of the breakdown strength of XLPE samples under the temperature
Figure
of: Weibull
(a) 305.°C; (b) 50distributions
°C; (c) 70 °C. of the breakdown strength of XLPE samples under the temperature
of: (a) 30 ◦ C; (b) 50 ◦ C; (c) 70 ◦ C.
Table 1 shows the Weibull parameters of the breakdown strength of XLPE samples
Table 1 shows the Weibull parameters of the breakdown strength of XLPE samples at
at different temperatures. It can be seen that under the test temperature condition of ◦50
different temperatures. It can be seen that under the test temperature condition of 50 C,
°C, the scale parameters of the breakdown strength of XLPE pre-crosslinked at 140, 150
the scale parameters of the breakdown strength of XLPE pre-crosslinked at 140, 150 and
and ◦160 °C were reduced by 11%, 6% and 7%, respectively, compared with the samples
160 C were reduced by 11%, 6% and 7%, respectively, compared with the samples without
without pre-crosslinking. The results of the breakdown strength test show that the exist-
pre-crosslinking. The results of the breakdown strength test show that the existence of
ence of the pre-crosslinking process results in defects in the crosslinking structure and
crystalline morphology of the sample, resulting in a decrease in the dielectric strength of
the XLPE sample. It also can be seen that, with the increase in temperature, the scale and
shape parameters of XLPEs both decreased. Compared with the XLPE without pre-cross-
linking, the increase in temperature has a more significant effect on the electrical strength
Energies 2022, 15, 2360 10 of 13

the pre-crosslinking process results in defects in the crosslinking structure and crystalline
morphology of the sample, resulting in a decrease in the dielectric strength of the XLPE
sample. It also can be seen that, with the increase in temperature, the scale and shape
parameters of XLPEs both decreased. Compared with the XLPE without pre-crosslinking,
the increase in temperature has a more significant effect on the electrical strength of the
pre-crosslinked XLPE.

Table 1. Weibull parameters of the breakdown strength of XLPE samples at different temperatures.

Temperature Pre-Crosslinking SCALE Parameter α

Shape Parameter β
(◦ C) Temperature (◦ C) (kV/mm)
140 333.4 34.20
150 335.4 82.56
30
160 339.8 57.00
Without
355.5 68.22
pre-crosslinking
140 301.7 30.50
150 318.9 24.10
50
160 316.1 34.64
Without
338.3 42.94
pre-crosslinking
140 213.5 27.58
150 223.9 25.91
70
160 226.1 29.26
Without
258.2 26.18
pre-crosslinking

Under the test temperature condition of 30 ◦ C, the dimension parameters of XLPE

pre-crosslinked at 140 ◦ C are 6% lower than those of normal XLPE. At the test temperature
of 70 ◦ C, the dimensional parameters of the XLPE pre-crosslinked at 140 ◦ C decreased by
17% compared with the normal XLPE. With the increase in the ambient temperature, the
electrical strength of the pre-crosslinked sample decreased by a higher percentage than that
of the XLPE without pre-crosslinking.
Additionally, the shape parameter value of pre-crosslinked XLPE decreased signifi-
cantly with the increase in temperature. The decrease in the shape parameters indicates
that the dispersion of the test data becomes larger, which proves that the pre-crosslinking
not only causes the decrease in the electrical strength of XLPE, but also leads to the decrease
in the insulation stability of the material. In other words, high temperature causes the
micro-defects in the amorphous region of the pre-crosslinked XLPE material to be more
prone to breakdown.

4. Discussion
To further analyze the effect of pre-crosslinking on the space charge transportation,
the amplitudes and motilities of the space charge packets under different DC electric fields
were quantitatively calculated. The solid lines in Figure 6 are the amplitudes of the space
charge packets in the bulk of XLPE samples under different electric fields. This shows that
the average amplitude of the space charge packets injected into the normal XLPE samples
is relatively small, whereas the amplitude of the space charge packets injected into the pre-
crosslinked XLPE samples is significantly increased. This is because the pre-crosslinking
process causes imperfect crystallization of the XLPE sample, and the micro-defect in the
amorphous region increases the probability of the homopolar charges being injected into
the XLPE samples. Among the pre-crosslinked XLPE samples, those at 140 ◦ C have the
highest amplitude of the injected space charge packets.
Energies2022,
Energies 2022,15,
15,2360
x FOR PEER REVIEW 11 of
11 of 13
13

200
140

Space charge packet density (C/m3 )

150 4

Space charge packet mobility

160
160 Without

（10 15 m 3/sec·V）
120

2
80

1
40

0 0

75 100 125
Electric field（ kV/mm)
Figure 6.6. Amplitude
Figure Amplitudeand
andmotilities
motilitiesofofthe
the space
space charge
charge package
package of XLPE
of XLPE samples
samples under
under different
different DC
DC electric
electric fields.
fields.

ItThe
canspace
also be charge
observed packet
thatresults in Section
the amplitude 3.2 positive
of the also indicate
spacethe positive
charge packagecharges mi-
injected
grate
into the from
samplethe increases
anode to continuously
the cathode inside with the theincrease
dielectrics,
in theand the motilities
applied of the
electric field space
strength.
charge
For the XLPEpackets are not
sample pre-crosslinked at 140 ◦ C, that
constant. Considering the space
the average charge packet
amplitude is a non-uni-
of the space charge
inside the dielectrics process,
is only 46the C/m 3 under −defined
form transportation motility of the DC electric
a space field of is
charge packet 75 kV/mm, but
as the as the
average
electric field intensity increases to −
value over a period of time, which can be expressed as:100 and − 125 kV/mm, the average amplitudes of the
charge packets increased to 116 and 154 C/m , respectively. 3
 L1also1indicate the positive charges migrate
L2 3.2
The space charge packet results inM Section
SCP =  (3)
from the anode to the cathode inside the dielectrics, t2  t1 Eand appl the motilities of the space charge

packets are not constant. Considering that the space charge packet is a non-uniform
where t1 and t2 correspond to the start and end times of the apparent displacement of the
transportation process, the motility of a space charge packet is defined as the average value
space charge packet, respectively. L1 and L2 correspond to the position of the space charge
over a period of time, which can be expressed as:
packet at t1 and t2, respectively. Eappl is the applied electric field.
The motilities of the space charge packets L −L under different
1 DC electric fields are shown
by the dashed lines in Figure 6. It SCP
M = 2 from
can be seen
1
× the figure that the average motility(3) of
t2 − t1 Eappl
the charge packets in the normal crosslinked XLPE sample is the lowest, and the average
where
motility t1 and
is 0.77t2 correspond
× 10−15 m2/sec· to the start and
V under theend timeselectric
applied of the apparent displacement
field strength of the
of 75 kV/mm.
space
However, charge thepacket,
pre-crosslinking L1 and Lleads
respectively.process 2 correspond to the position
to the relatively of the space
incomplete charge
crosslinked
packet
structure at tof
1 andthetsample, which Eresults
2 , respectively. appl is the
in aapplied electric field.
rapid increase in the average motility of the
charge Thepackage
motilities of the
inside thespace charge
medium. packets
Among theunder different
samples, DC electric
the average fieldsofare
motility theshown
XLPE
by the dashed lines in Figure 6. It can be seen from
pre-crosslinked at 140 °C was the highest, and was 3.44 × 10 m /sec·V. the figure that
−15 the
2 average motility of the
charge packets in the normal crosslinked XLPE sample is the lowest,
Combined with the experimental results in Section 3.1, it is considered that the pre- and the average motil-
ity is 0.77 × 10 −15 m2 /s·V under the applied electric field strength of 75 kV/mm. However,
crosslinking process leads to the reduction in the crystallinity of the XLPE sample and the
the pre-crosslinking
reduction processsize,
in the spherulite leadswhich
to themakes
relatively the incomplete
injection of crosslinked
charge packets structure
more of the
likely
sample, which results in a rapid increase in the average
to occur inside the sample. As the temperature of the pre-crosslinked XLPE decreases, themotility of the charge package
inside
larger the themedium. Among theof
average amplitude samples,
the space thecharge
averagepackets
motilityinjected
of the XLPEinsidepre-crosslinked
the insulating
at 140 ◦ C was the highest, and was 3.44 × 10−15 m2 /s·V.
material, the higher the average motility.
Combined
Additionally, with thethe experimental
higher the applied results
electricin Section 3.1, it isthe
field strength, considered
lower the that the pre-
average mo-
crosslinking process leads to the reduction in the crystallinity
tility of the charge packets within the sample. This is mainly due to the recombination of the XLPE sample and the of
reduction in the spherulite size, which makes the injection
heteropolar charges inside the XLPE samples. With the increase in the field strength fromof charge packets more likely to
occur
75 to 125 inside the sample.
kV/mm, As thespace
the negative temperature of the pre-crosslinked
charge injection phenomenon appears XLPE decreases, the
near the cath-
larger the average amplitude of the space charge packets injected inside the insulating
ode, and the negative space charges migrate from the cathode to the anode under the ac-
material, the higher the average motility.
tion of the electric field force. During the migration process, the recombination process of
Additionally, the higher the applied electric field strength, the lower the average
negative and positive space charge packets occurs in the sample, resulting in a decrease
motility of the charge packets within the sample. This is mainly due to the recombination
in charge motility. It has been proven that the recombination of charge carriers would
of heteropolar charges inside the XLPE samples. With the increase in the field strength
produce hot electrons due to non-radiative transition of energy via an Auger-type process
from 75 to 125 kV/mm, the negative space charge injection phenomenon appears near the
Energies 2022, 15, 2360 12 of 13

cathode, and the negative space charges migrate from the cathode to the anode under the
action of the electric field force. During the migration process, the recombination process of
negative and positive space charge packets occurs in the sample, resulting in a decrease in
charge motility. It has been proven that the recombination of charge carriers would produce
hot electrons due to non-radiative transition of energy via an Auger-type process [27]. The
hot electrons may have sufficient energy to collide with a molecule and dissociate into free
radicals. This process can be expressed as:

AB + e− (hot) → A∗ + B∗ + e− (cold)
(4)
or → A∗ + B∗ + e− (trapped) + energy release

The energy released from the charge combination process results in the formation of
a low-density region, in which electrons are more easily accelerated by the electric field
and gain kinetic energies to cause chain scission. As a result, the chain scissions and
micro-defects in amorphous regions may cause partial discharge and further develop into
the breakdown of polymer, which contributes to the decrease in breakdown strength [28].

5. Conclusions
This study investigated the effect of pre-crosslinking on space charge and break-
down characteristics of XLPE insulation for HVDC cables. The main conclusions can be
summarized as follows:
(1) The pre-crosslinking temperature affects the crystalline morphology of the XLPE
samples. With the decrease in the pre-crosslinking temperature, the grain size of the
sample gradually decreases, and the spherulite arrangement becomes looser, which leads
to decreases in the integrity of the crystalline structure and the crystallinity of the pre-
crosslinked XLPE sample.
(2) Compared with the XLPE sample without pre-crosslinking, the pre-crosslinked
XLPE is more prone to the injection of charge packets into the bulk due to its imperfect
crystalline structure. As the DC electric field increases from 75 to 125 kV/mm, the amplitude
of the injected space charge packet increases significantly, resulting in increased electric
field distortion.
(3) Pre-crosslinking leads to a significant decrease in the DC breakdown field strength,
which is closely related to the imperfect spherulite structure and micro-defects of the
XLPE insulation.
Considering the actual operating conditions of the cable, XLPE insulation is not only
affected by the electric field, but also by the operating temperature. Comprehensive analysis
of the effect of pre-crosslinking on the dielectric properties of materials, such as the space
charge under the condition of multi-physics coupling, and exploration of the structure–
activity relationship between the microstructure and macroscopic properties of materials,
will be the direction and focus of future work.

Author Contributions: Conceptualization, Z.Z., Z.L. and B.D.; methodology, Y.W.; software, Y.W.;
validation, Y.W. and Z.Z.; formal analysis, Y.W. and Z.Z.; investigation, Y.W. and Z.Z.; resources,
Y.W., Z.Z., C.F., S.M. and C.P.; data curation, Y.W. and Z.Z.; writing—original draft preparation,
Z.L. and B.D.; writing—review and editing, Z.L. and B.D.; visualization, Z.L. and B.D.; supervision,
Z.Z.; project administration, Z.Z.; funding acquisition, Z.Z. All authors have read and agreed to the
published version of the manuscript.
Funding: This research was supported by Open Fund of State Key Laboratory of Power Grid
Environmental Protection (China Electric Power Research Institute) (No. GYW51202101371).
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: Not applicable.
Conflicts of Interest: The authors declare no conflict of interest.
Energies 2022, 15, 2360 13 of 13

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