Received: 14 June 2023

DOI: 10.1049/hve2.12396

ORIGINAL RESEARCH
- -Revised: 28 August 2023 Accepted: 10 September 2023

- High Voltage

Effect of nucleating agents on the electrical properties of cross‐

linked polyethylene under tensile stress

Yunqi Xing1 | Jiahao Liu1 | Jingang Su2 | Junwei Zha3 | Guochang Li4 |
Ze Guo1 | Xiaozhen Zhao1 | Mengjia Feng1
1
State Key Laboratory of Reliability and Intelligence of Electrical Equipment, Hebei University of Technology, Tianjin, China
2
Electric Power Research Institute of State Grid Hebei Electric Power Supply Co., Ltd., Shijiazhuang, China
3
Beijing Advanced Innovation Center for Materials Genome Engineering, School of Chemistry and Biological Engineering, University of Science & Technology Beijing, Beijing, China
4
Institute of Advanced Electrical Materials, Qingdao University of Science and Technology, Qingdao, China

Correspondence Abstract
Mengjia Feng, State Key Laboratory of Reliability During the operation of high‐voltage cables, external stress and residual stress can affect
and Intelligence of Electrical Equipment, Hebei
University of Technology, Tianjin 300123, China.
the aggregated structure of insulating materials and lead to significant deterioration in
Email: [email protected] their electrical performance. To investigate the evolution characteristics of the electrical
properties of cross‐linked polyethylene (XLPE) under mechanical stress, this paper ex-
Associate Editor: Mona Ghassemi plains the relationship between the aggregated structure of XLPE and its electrical
properties and proposes a method for improving insulation performance under me-
Funding information chanical stress. The results show that metallocene polyethylene used as a nucleating agent
Key Laboratory of Special Machine and High
can promote crystallisation through heterogeneous nucleation and increase Young's
Voltage Apparatus, Ministry of Education, Grant/
Award Number: KFKT202207; the Natural Science modulus by non‐uniform nucleation, increasing crystallinity and reducing interplanar
Foundation of Hebei Province, Grant/Award spacing, resulting in more complete crystal forms and reduced damage to the aggregated
Number: E2021521003; Hebei Province Innovative
structure during the tensile process. After nucleating agent modification, the XLPE
Capacity Development Program for Research
Students, Grant/Award Number: CXZZSS2023018 crystallisation becomes more uniform, and interfacial adhesion forces increase. The
weakened interface damage process between the amorphous and crystalline regions under
tensile stress effectively inhibits the process of molecular chain polarisation turning and
reduces trap density. The modified XLPE crystal structure shows a tendency towards
densification and enhanced molecular chain interactions, which can reduce the damage to
the aggregated structure under tensile stress, while the reduced free volume inside the
material and the shortened average free path of carriers can weaken the damage of high‐
energy electrons to molecular chains, thereby inhibiting the process of electrical tree
degradation. The results show that nucleating agents have great potential for maintaining
the stable operation of XLPE cables under mechanical stress.

1 | INTRODUCTION limitations of the laying environment, the cable will inevitably

bend. Long‐term exposure to external mechanical stress can
Cross‐linked polyethylene (XLPE) meets the requirements of lead to problems such as sheath rupture and insulation
high‐temperature resistance and mechanical properties for deformation, causing cable failures [3, 4]. Moreover, external
insulation materials in high‐voltage power cable transmission mechanical stress can damage the aggregated structure of the
of large capacity. It is widely used in the power system, and insulation material, accelerate the growth of electrical trees in
its reliability is closely related to the stable operation of the the insulation material, and seriously threaten the reliability of
power system [1, 2]. During cable laying, due to the cable operation [5, 6].

-
This is an open access article under the terms of the Creative Commons Attribution‐NonCommercial‐NoDerivs License, which permits use and distribution in any medium, provided the
original work is properly cited, the use is non‐commercial and no modifications or adaptations are made.
© 2023 The Authors. High Voltage published by John Wiley & Sons Ltd on behalf of The Institution of Engineering and Technology and China Electric Power Research Institute.

High Voltage. 2024;9:429–439. wileyonlinelibrary.com/journal/hve2 429

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- XING ET AL.

In order to explore the changes in the electrical properties water trees [17]. Sabet improved the performance of LDPE by
of insulation materials under mechanical stress, Wang studied doping with graphene and found that graphene can reduce the
the effect of tensile stress on low density polyethylene (LDPE) activation energy and increase the crystallisation initiation
and found that the DC breakdown strength of LDPE temperature to form crystal nuclei [18]. Mai studied the effects
decreased and the dielectric constant and dielectric loss of two types of nucleating agents, organic phosphates (A) and
increased after tensile deformation, reducing the insulation sorbitol (D), on the crystallisation of polypropylene and found
performance of the material [7]. Billing studied the electric tree that the nucleating agents can shorten the half‐crystallisation
initiation voltage of polymeric insulation materials under time of polypropylene, and nucleating agent A has a better
bending strain and found that when the bending strain was effect [19]. Gao studied the effects of β‐nucleating agents on
between 5% and 8%, the initiation voltage of the electric tree PP/POE blends and found that polypropylene can form
decreased by about 40%, indicating that mechanical stress ac- hexagonal β‐phase after adding the β‐nucleating agent [20].
celerates the degradation of electric trees [8]. Jiang studied the Zhu studied the change of crystal morphology during the
changes in the aggregated structure of LDPE under different crosslinking process of XLPE. The results showed that the
stretching ratios and found that the crystal structure was acetophenone generated by the decomposition of peroxide
initially compact before stretching. Stretching first damages during the crosslinking process could be used as a nucleating
their original crystal structure and then causes molecular chain agent to promote the nucleation process of crystallisation [21].
fracture inside the material [9]. Du investigated the influence of Li used ethylene/ethyl acrylate copolymer (EEA) as a nucle-
different stretching ratios on space charge accumulation in PP/ ating agent to improve the water tree resistance of XLPE. The
POE blends and found that the samples after stretching results showed that EEA adjusted the crystal morphology of
accumulated more space charges in the same polarisation time XLPE, increased the strength and toughness of the material,
[10]. David studied the effect of residual internal stress on and increased the water tree resistance [22]. However, the
XLPE electric trees and found that the sample with the largest relationship between the nucleating agent‐regulated changes in
residual stress had the longest electric trees and the most the aggregated structure of XLPE under mechanical stress and
serious performance degradation after 1 h [11]. Amyot studied insulation failure is still to be explored.
the effect of residual mechanical stress on breakdown field In this study, metallocene polyethylene (MPE) was selected
strength and found that with the increase of mechanical stress, as the nucleating agent. 1 wt% of MPE was added to the XLPE
the breakdown field strength gradually decreased [12]. Cross‐ material through melt blending. The material before and after the
linked polyethylene has a complex aggregated structure, so addition of the nucleating agent was subjected to different de-
establishing the relationship between the changes in the grees of tensile processing (0%, 10%, 20%, and 30%). The
aggregated structure and insulation failure of XLPE under changes in the aggregated structure of XLPE before and after
mechanical stress is an urgent issue that needs to be addressed. the addition of the nucleating agent under different stretching
A common method to enhance the electrical properties of ratios were analysed using infrared spectroscopy and X‐ray
high‐voltage cable insulation materials is doping with inorganic diffractometer (XRD). The dielectric properties of the material
nanoparticles. However, high concentration nanoparticles are were characterised by measuring the dielectric constant, con-
easy to agglomerate, which affects the insulation performance. ductivity, and trap energy level of XLPE before and after adding
Wang studied the effect of different contents of TiO2 on the the nucleating agent under different tensile ratios. The length of
insulation properties of XLPE. The results show that when the electric trees and breakdown field strength of XLPE before and
content is 1 wt%, the nanoparticles are agglomerated and the after the addition of the nucleating agent under different
breakdown voltage is lower than that of pure XLPE [13]. At stretching ratios were measured to characterise the insulation
present, it has been proposed to use nanoparticles with con- failure of XLPE. The electrical properties of nucleating agent‐
centrations higher than normal and gradually adjust the elec- reinforced XLPE under mechanical stress were mechanistically
trical properties of the shell until an increased filler cluster size explained by calculating Young's modulus through tensile tests.
(high k) and inhibition of electron transfer between particles This article clarifies the intrinsic relationship between changes in
(low dielectric loss) are obtained. However, the production the aggregated state structure of XLPE under mechanical stress
process is complex and is still in the research stage [14, 15]. and its dielectric properties, as well as insulation degradation
Nucleating agents are simple to produce, and improving the failure. By regulating the XLPE aggregated state structure to
structure of aggregates with nucleating agents is an effective improve its electrical properties, this article proposes a method
means of improving electrical performance. This has led to for enhancing the insulation performance of XLPE under
extensive research by scholars. Seven studied the effects of external mechanical stress.
organic and inorganic nucleating agents on the breakdown
strength of polyethylene and found that both types of nucle-
ating agents can increase the number of spherulites, thereby 2 | EXPERIMENT
improving the breakdown field strength of the material [16].
Wang studied the relationship between crystal morphology and 2.1 | Sample preparation
water tree growth and found that after adding a nucleating
agent, the degree of crystallinity of the LDPE increased and We first put 1 wt% of MPE and XLPE pellets into a twin‐
the size of the spherulites decreased, inhibiting the growth of screw mixer for melt blending at a temperature of 120°C.
 23977264, 2024, 2, Downloaded from https://ietresearch.onlinelibrary.wiley.com/doi/10.1049/hve2.12396 by South Korea National Provision, Wiley Online Library on [23/07/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
XING ET AL.
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Then, we subjected the blend to a hot pressing process in a flat type specimens, tested by an electronic universal testing ma-
vulcanising machine at 15 MPa and 180°C for 15 min to obtain chine at 25°C, and the tensile rate was 100 mm/min.
XLPE samples with and without the addition of MPE nucle-
ating agent in the form of sheets of sizes 20 mm � 60 mm
� 4 mm and 40 mm � 50 mm � 0.4 mm. The former was 3 | EXPERIMENTAL RESULTS AND
used for electric tree growth experiments, while the latter was DISCUSSION
used for other experimental tests. We then used a universal
testing machine to prepare samples with stretching ratios of 3.1 | Microstructure characteristics of XLPE
λ = 0%, 10%, 20%, and 30% at a speed of 5 mm/min. A before and after addition of nucleating agents
standard dumbbell‐shaped specimen with a thickness of 1 mm at different stretching ratios
and a total length of 75 mm was produced and marked with a
working interval of 20 mm. In order to investigate the effect of tensile stress on the
microstructure of XLPE before and after the addition of a
nucleating agent, Fourier transform infrared spectroscopy was
2.2 | Experimental method used to analyse the changes in the internal functional groups of
the material. The experimental results are shown in Figure 1.
The Fourier‐transform infrared spectrometer (V80) was used The characteristic absorption peak at 719 cm−1 corresponds to
to analyse the changes in the molecular chains and functional the in‐plane bending and rocking vibration peak of C–H in
groups of the material before and after the addition of the CH2, the characteristic absorption peak at 1462 cm−1 corre-
nucleating agent under different stretching ratios. The wave- sponds to the in‐plane bending and shearing vibration peak of
number range was 400–4000 cm−1. The XRD was used to C–H in CH2, the characteristic absorption peak at 2850 cm−1
measure the changes in the crystallinity and interplanar corresponds to the symmetric stretching vibration peak of C–
spacing of the material before and after the addition of the H in CH2, and the characteristic absorption peak at 2918 cm−1
nucleating agent under different stretching ratios in the range corresponds to the asymmetric stretching vibration peak of C–
of 10°–30° of the scanning angle 2θ. The broadband H in CH2 [23–25].
dielectric spectroscopy analyser was used to measure the With the increase of tensile ratio, the peak intensity of each
dielectric constant of the material before and after the absorption peak of XLPE decreases and the content of
addition of the nucleating agent under different stretching functional groups decreases. At the beginning of applying
ratios in the frequency range of 100–106 Hz. The stress, the molecular chain will move in the direction of the
conductivity of XLPE before and after adding the nucleating force. With the continuous increase of tensile ratio, the mo-
agent under different tensile ratios was measured by the lecular chain will undergo disentanglement and orientation
three‐electrode method. The isothermal surface potential movement. Excessive tensile stress will cause the internal
decay (ISPD) method was used to calculate the trap level of the molecular chain of XLPE to break and then form small cav-
material before and after the addition of the nucleating agent ities; these small cavities will extend through the middle of the
under different stretching ratios. The charging voltage was system and eventually form large cracks or even cause the
−10 kV, the charging time was 20 min, and after the charging entire system to rupture [26–28]. After adding the nucleating
was completed, the power supply was immediately turned off, agent, the number of functional groups increased, which
and the change in the surface potential of the material was promoted the entanglement between molecular chains and
recorded by the electrostatic voltmeter by quickly moving the enhanced the performance of XLPE [29]. The structure con-
sample under the Kelvin probe. For the electric tree growth necting the molecular chains between the single crystals
experiment, a steel needle with a tip curvature radius of 3 μm increased, and the interaction force between the molecular
and a chamfer of 30° was inserted into the centre of the sample chains also increased. During the tensile process, it is not easy
to a depth of (18 � 0.1) mm by using a thermal shrinkage for the molecular chains to break. Compared with XLPE, the
method. The sample was immersed in transformer oil to content of functional groups in the nucleating agent‐added
prevent surface flashover and corona discharge. The voltage XLPE increases at the same tensile ratio.
was increased at a rate of 1 kV/s to 9 kV and maintained Figure 2 shows the X‐ray diffraction patterns of XLPE
constant during the experiment. Images of the electric tree before and after the addition of a nucleating agent under
growth pattern were collected and saved every 10 min, and different tensile ratios. The sharp diffraction peaks around
three samples were tested for each group. For the breakdown 21.6° and 24° correspond to the (110) and (200) planes of the
test, a sphere‐sphere electrode with a diameter of 25 mm was XLPE crystal, respectively [30]. With the increase of tensile
used, and the sample was immersed in transformer oil to ratio, the intensity of the diffraction peaks decreases. After
prevent surface flashover and corona discharge. The voltage adding the nucleating agent, the intensity of the diffraction
was increased at a rate of 1 kV/s until an electrical breakdown peaks increases significantly without any additional diffraction
occurred in the sample. The basic mechanical properties of the peaks, indicating that the crystal structure remains unchanged.
material were analysed by using the tensile test, and the According to formulas (1) and (2), the crystallinity and lattice
Young's modulus was obtained from the stress–strain curve in spacing were calculated [31–33], and the results are shown in
the tensile test. The test specimens were standard dumbbell‐ Table 1.
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432
- XING ET AL.

F I G U R E 1 The Fourier transform infrared spectroscopy

characterisation of the samples under strains. (a) Cross‐linked polyethylene
(XLPE), (b) XLPE/metallocene polyethylene (MPE).

F I G U R E 2 X‐ray diffraction pattern of the samples under strains.

(a) Cross‐linked polyethylene (XLPE), (b) XLPE/metallocene polyethylene
Ið110Þ þ 1:42Ið200Þ (MPE).
W ¼ � 100% ð1Þ
Ið110Þ þ 1:42Ið200Þ þ 0:68IðAÞ
TABLE 1 XRD parameters of the samples under strains.
nλ
d¼ ð2Þ Interplanar
2 sin θ
2θ (°) spacing (nm)

Where W is the quality crystallinity of the tested sample, Samples (elongation ratio) 110 200 W (%) 110 200
I(110), I(200), and I(A) are the diffraction peak integral area of the XLPE (0%) 21.78 24.12 52.98 0.40759 0.36855
(110) and (200) crystal planes and the diffraction peak area
XLPE/MPE (0%) 21.95 24.25 54.68 0.40445 0.36662
scattered by the amorphous region, θ is the angle between the
X‐ray and the corresponding crystal plane, λ is the wavelength XLPE (10%) 21.76 24.04 51.98 0.40794 0.36974
of X‐ray, and n is the diffraction order. XLPE/MPE (10%) 21.86 24.24 52.65 0.40610 0.36674
With the increase of stretching stress, the internal molec-
XLPE (20%) 21.73 24.04 50.35 0.40852 0.36976
ular chains of XLPE break, crystals are crushed, partially
crystalline regions transform into amorphous regions, the de- XLPE/MPE (20%) 21.76 23.96 52.90 0.40794 0.37096
gree of crystallinity decreases, the interplanar distance in- XLPE (30%) 21.66 23.90 49.01 0.40980 0.37188
creases, and the molecules become more disordered. A
XLPE/MPE (30%) 21.56 23.96 51.08 0.41166 0.37097
network structure is formed during the crosslinking process of
XLPE, which affects its own degree of crystallinity. After Abbreviations: MPE, metallocene polyethylene; XLPE, cross‐linked polyethylene; XRD,
X‐ray diffractometer.
adding a nucleating agent, MPE acts as a heterogeneous
nucleation centre, which helps to form crystal nuclei, increases
the rate of crystallisation, reduces the size of microcrystals, and crystalline regions are more tightly packed, improving the
further promotes the crystallisation of XLPE [34, 35]. The aggregated structure inside XLPE, and the tightly packed
nucleating agent leads to an increase in the degree of crystal- crystalline regions are not easily deformed during stretching.
linity of XLPE, a decrease in interplanar distance, indicating Under the same stretching ratio, XLPE with a nucleating agent
that the internal crystallisation of XLPE becomes more uni- has a higher degree of crystallinity than pure XLPE, and the
form and forms more complete crystallisation, the arranged crystalline surface spacing is smaller than that of XLPE.
 23977264, 2024, 2, Downloaded from https://ietresearch.onlinelibrary.wiley.com/doi/10.1049/hve2.12396 by South Korea National Provision, Wiley Online Library on [23/07/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
XING ET AL.
- 433

3.2 | Dielectric properties of samples before

and after the addition of nucleating agents at
different stretching ratios

The dielectric constant of XLPE before and after adding a

nucleating agent under different stretching ratios is shown in
Figure 3. With the increase of the stretching ratio, the internal
crystalline regions of XLPE decrease, the interplanar distance
increases, the distance between molecular chains increases, and
polarisation is more easily established, resulting in a gradual
increase in the dielectric constant. Adding a nucleating agent
increases the internal grains of XLPE, making their arrange-
ment more regular and restricting the movement of molecular
chains. As a result, polarisation is more difficult to establish,
and the dielectric constant of XLPE is reduced [36]. The
increased structural connection between molecular chains leads
to enhanced intermolecular forces, which can well suppress the
orientation polarisation of polarity groups during stretching.
Therefore, under the same stretching ratio, adding a nucleating
agent to XLPE leads to a decrease in dielectric performance
relative to pure XLPE but improves insulation performance.
The conductivity changes of XLPE before and after adding
nucleating agent under different tensile ratios are shown in
Figure 4. The conductivity of XLPE under different tensile
ratios is 3.54 � 10−13 S/m, 3.68 � 10−13 S/m, 3.81 � 10−13 S/
m and 3.93 � 10−13 S/m. The conductivity of XLPE with a
nucleating agent under different tensile ratios is 3.27 � 10−13
S/m, 3.55 � 10−13 S/m, 3.68 � 10−13 S/m, and 3.81 � 10−13 F I G U R E 3 The relative permittivity for the samples under strains.
S/m. With the increase of tensile ratio, the crystal region is (a) Cross‐linked polyethylene (XLPE), (b) XLPE/metallocene polyethylene
destroyed, the slip between grains occurs, and the proportion (MPE).
of amorphous region increases, resulting in the release of some
carriers by traps. At the same time, the loose amorphous region
is also conducive to the directional migration of carriers, so the
macroscopic conductivity increases [37]. The addition of a
nucleating agent increases the crystallisation rate of XLPE
insulation, reduces the interplanar spacing, improves the crystal
structure, and increases the inter‐spherulite force. It can well
resist the external mechanical stress during the stretching
process. Compared with the addition of a nucleating agent, it
maintains a higher crystallinity and a better spherulite structure
at the same stretching ratio, which inhibits the charge transfer
in XLPE insulation, showing a decrease in conductivity and an
increase in insulation performance.
The decay of the negative polar surface potential of XLPE
before and after the addition of the nucleating agent is shown in
Figure 5. With the increase of applied stress, the surface potential
decay curve of the specimens gradually shifted downward. The F I G U R E 4 The conductivity of the samples before and after adding
pure XLPE specimens show an increase of initial surface po- the nucleating agent under strains.
tential along with the increase of stretching ratio, and the
remaining surface potential after decaying is larger. The initial
surface potential before and after stretching of XLPE with the In this paper, the ISPD method is used to analyse the trap
nucleating agent is basically the same, but the dissipation rate of distribution characteristics of XLPE before and after adding a
unstretched samples is significantly faster than that of stretched nucleating agent under different stretching ratios. According to
samples, and the dissipated potential decreases compared with Simmons' model for ISPD, the relationship formula between
that of pure XLPE, indicating that the charges on the surface and surface trap energy levels and trap density can be obtained as
inside of the specimens are less likely to be delocalised. follows [38]:
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434
- XING ET AL.

F I G U R E 5 The surface potential decay curves of negatively charged

samples under strains. (a) Cross‐linked polyethylene (XLPE), (b) XLPE/
metallocene polyethylene (MPE).
F I G U R E 6 The distribution of trapped charges on the surface of
negatively charged samples under strains. (a) cross‐linked polyethylene
(XLPE), (b) XLPE/metallocene polyethylene (MPE).
� �
Nt ðEÞ 4ε0 εr � dV ðtÞ �
�t dt �
¼ 2 2 2 � � ð3Þ T A B L E 2 Deep trap density of cross‐linked polyethylene (XLPE)
Et eL k T ln ðvtÞ before and after the addition of nucleating agents at different stretching
ratios.
where Et is the energy of the sample trap, eV; Nt is the density Samples (elongation ratio) Deep trap density (1019 eV−1⋅m−3)
at the corresponding energy, eV−1 ⋅ m−3; ε0εr is the dielectric
XLPE (0%) 9.148
constant of the sample under test, F/m; e is the meta‐charge
charge, C; L is the thickness of the sample under test in the XLPE/MPE (0%) 7.484
charge/discharge direction, m; k is the Boltzmann constant, XLPE (10%) 10.243
J/K; T is temperature, K; v is the carrier escape frequency, Hz;
XLPE/MPE (10%) 8.649
t and V(t) are the time parameter and surface potential of the
sample ISPD. XLPE (20%) 10.421
The trap energy levels obtained according to Equation (3) XLPE/MPE (20%) 9.398
are shown in Figure 6 and Table 2. The deep trap energy level
XLPE (30%) 11.706
of XLPE is between 0.91 and 0.95 eV, while that of XLPE with
a nucleating agent is between 0.89 and 0.93 eV, indicating little XLPE/MPE (30%) 9.623
difference. The deep trap density of XLPE before and after
adding a nucleating agent increases with the increase of the
stretching ratio, but the deep trap density after adding a Adding a nucleating agent increases the proportion of
nucleating agent is slightly lower than that of pure XLPE. crystalline regions, makes their arrangement more compact,
Stretching pure XLPE leads to a decrease in crystallinity, reduces the amorphous defects of XLPE, decreases the deep
disintegration of grains, and the generation of more amor- trap density, and reduces the accumulation of charges. The
phous/crystalline interface areas, leading to the formation of nucleating agent provides strong interfacial adhesion force,
defects inside XLPE, which generate more deep traps, increase produces fewer amorphous/crystalline interface areas during
the accumulation of space charges, and reduce the insulation stretching, and increases the structural connection between
performance of XLPE [39]. molecular chains, enhancing the intermolecular forces, making
 23977264, 2024, 2, Downloaded from https://ietresearch.onlinelibrary.wiley.com/doi/10.1049/hve2.12396 by South Korea National Provision, Wiley Online Library on [23/07/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
XING ET AL.
- 435

the structure between molecules more compact, and effectively

suppressing the destruction of amorphous regions during
stretching [40]. Therefore, the defect density of XLPE after
adding a nucleating agent is lower than that of pure XLPE
under the same stretching ratio, and the deep trap density is
decreased, effectively improving the electrical performance of
XLPE under mechanical stress.

3.3 | Breakdown degradation of samples

before and after addition of nucleating agents
at different stretching ratios

The electric tree growth characteristics of XLPE before and

after adding a nucleating agent under different stretching ratios
are shown in Figures 7–9. With the increase of the stretching
ratio, the length of electric tree increases. After adding a
nucleating agent, there is no electric tree growth in un‐
stretched XLPE, and the length of the electric tree after
stretching is smaller than that of pure XLPE. Cross‐linked
polyethylene is composed of crystalline and amorphous re-
gions, and the crystallinity affects the insulation performance
of XLPE to a certain extent [41–43].
Mechanical stress will destroy the internal structure of
XLPE, leading to molecular chain breakage and decreased the
functional group content. Under stretching, the interplanar
distance increases, indicating that the lattice perfection of
XLPE decreases and the defects between lattices and amor-
phous regions increase, causing spherulite rupture and an in-
crease in amorphous regions. The tensile stress also causes the
molecular chains to move along the direction of force, F I G U R E 7 Growth morphology of electrical tree under strains.
increasing the distance between the molecular chains, (a) Cross‐linked polyethylene (XLPE), (b) XLPE/metallocene polyethylene
increasing the free volume, and the energy transferred by (MPE).
charge transport in the free volume increases. At the same
time, the energy barrier between molecular chains decreases,
which is conducive to the transport of charges, and the damage and the addition of a nucleating agent to XLPE improves the
of carrier on the molecular chain structure is strengthened [44– trap distribution inside the material under the same stretching
46]. This easily forms electric field distortion and triggers ratio compared to pure XLPE, limits the effect of collision
partial discharge, promoting the degradation of the insulation ionisation, and makes it more difficult for the electric tree to
medium molecular chain, showing an increase in the degra- grow.
dation area of the electric tree and rapid growth of the electric The AC breakdown field strength of XLPE before and
tree. after adding a nucleating agent under different stretching ratios
After adding a nucleating agent, the crystallinity of XLPE is shown in Figure 10 and Table 3. The breakdown voltage of
increases, the interplanar distance decreases, the grain XLPE decreases with the increase of the stretching ratio. When
arrangement becomes more regular and the increase in crys- the stretching ratio is 30%, the breakdown voltage decreases
tallinity improves the trap distribution of XLPE, enhances the from 88.85 kV/mm to 82.18 kV/mm. After adding a nucle-
regulation ability of charge transport, and reduces the average ating agent, the breakdown voltage is higher than XLPE at the
free path of carriers [47, 48], weakening the collision ionisation same tensile ratio.
effect. This leads to more energy needed for the growth of the The traps and charge jumping points of carriers in XLPE
electric tree, which suppresses the growth of the electric tree. are generally located in the amorphous region and the interface
The nucleating agent increases the structural connection between crystalline/amorphous regions, such as defects and
between molecular chains, enhances the interaction between voids. The electrical breakdown channel mainly occurs in the
them, and suppresses the destruction of aggregated structures amorphous region of polymer and develops along the interface
during stretching. The defects inside XLPE decrease, and the between crystalline/amorphous regions through crystalline
free volume decreases. The average free path of carriers is phases or lattice spaces [49–51]. Tensile stress leads to the
shortened, and the damage of high‐energy electrons to mo- transformation of the crystalline region into the amorphous
lecular chains is weakened. The partial discharge is reduced, region, and the disintegration of grains produces a large
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436
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F I G U R E 8 Variation of length of the electrical tree under strains with

time. (a) Cross‐linked polyethylene (XLPE), (b) XLPE/metallocene F I G U R E 1 0 Relation between the probability and the breakdown
polyethylene (MPE). strength at different stretching ratios. (a) Cross‐linked polyethylene
(XLPE), (b) XLPE/metallocene polyethylene (MPE).

T A B L E 3 Weibull breakdown strength of cross‐linked polyethylene

(XLPE) before and after the addition of nucleating agents at different
stretching ratios.

Samples (elongation ratio) AC breakdown field strength (kV/mm)

XLPE (0%) 88.85

XLPE/MPE (0%) 95.56

XLPE (10%) 85.18

XLPE/MPE (10%) 90.27

XLPE (20%) 84.96

XLPE/MPE (20%) 89.19

XLPE (30%) 82.18

F I G U R E 9 The length of cross‐linked polyethylene (XLPE) electrical XLPE/MPE (30%) 87.38

tree before and after adding the nucleating agent under strains for 30 min.

number of crystalline/amorphous region interfaces, intro- reduce the current, thus effectively improving the breakdown
ducing many deep traps and causing the accumulation of performance of the material [52, 53]. In addition, the nucle-
charges. At the same time, the distance between lattices in- ating agent provides a strong interfacial adhesion force, pro-
creases, leading to the rapid development of channels and a duces fewer crystalline/amorphous region interfaces during
decrease in the breakdown field strength. The addition of a stretching, and decreases the traps and charge jumping points
nucleating agent can increase the crystallinity of XLPE, make of carriers. As a result, the breakdown voltage increases
the internal arrangement more compact, reduce the generation compared to XLPE under the same stretching ratio, effectively
of defects, reduce the number of charge transition points, and improving the insulation failure performance of XLPE.
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XING ET AL.
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Figure 11 shows the stress–strain curve of XLPE before When the blended specimen is impacted, the molecular chains
and after the addition of a nucleating agent. The first peak in of the elastic material undergo displacement, converting the
the graph is the yield point of the sample under tension. The impact energy into elongation energy and storing it. When the
linear segment of the sample under tension at the beginning of external force is removed, the molecules of the elastic material
stretching is usually considered as the elastic deformation zone, shrink back, releasing energy and restoring their original state.
where the material undergoes elastic deformation that can be This acts as a buffer to external forces, thereby toughening the
completely recovered when the stress is removed. At this stage, blend, increasing the Young's modulus, tensile strength, and
the molecular chain slip in the crystal region mainly occurs, mechanical properties [56].
which increases the chain spacing, and the change of non‐bond When carriers are injected into the interior of XLPE
energy is the main factor. The nucleating agent enhances the through a needle tip, if the electrons on the conductor acquire
number of functional groups, promotes the entanglement be- the energy released during carrier implantation or recombina-
tween molecules, enhances the intermolecular force, and leads tion, they may cross the barrier to become hot electrons. When
to an increase in the elastic deformation stage [54]. The zone hot electrons collide with XLPE molecular chains, the
from elastic to plastic deformation up to the yield point is the instantaneous release of kinetic energy may cause molecular
elastic‐plastic deformation zone. At this stage, the original chain breakage, partial dielectric breakdown, and the produc-
crystalline structure of XLPE began to destroy, the lamellae tion of electrical tree branches. Tensile stress causes an increase
were divided into many small crystals and twisted along the in free volume inside the material, an increase in carrier
tensile direction. After adding the nucleating agent, the crys- mobility and average free path, and under the accelerating
tallinity increased, the crystal plane spacing decreased, the effect of the electric field, carriers gain higher energy, leading to
structure was closer, the degree of lamellar damage decreased, an increased degree of damage to the XLPE molecular chains
and the elastic‐plastic deformation zone stage increased [26]. and accelerated growth of electrical trees. The addition of
Before the yield point, the molecular orientation gradually materials increases the mechanical properties. The heat
aligns in the stretching direction. After the yield point, the generated by partial discharge during stretching reduces the
sample presents a fine necking region that continues to expand damage caused by the pressure increase inside the channel,
until the working area completely thins and hardens, and then reducing the destruction of the aggregated state structure of
the stress continues to increase until the sample fractures [55]. the material, reducing the rate of molecular chain breakage,
The Young's modulus increased from 215.43 to 271.26 MPa lowering the density of deep traps inside the material, short-
after the addition of the nucleating agent. ening the average free path length of carriers, and weakening
When no nucleating agent is added, the grains are relatively the collision ionisation effect, thus suppressing the growth of
loose, and the molecular friction between the chains is greater electrical trees [57].
when the material is stretched by an external force, resulting in
more severe damage. The nucleating agent plays a role in
heterogeneous nucleation, which refines the crystallisation of 4 | CONCLUSION
XLPE, makes the grains smaller, the structure more compact,
strengthens the entanglement of molecular chains, increases This article observes the microscopic structural changes in
the intermolecular forces, reduces the friction between crys- materials under tensile stress. It explains the changes in ma-
talline particles during stretching, and reduces the degree of terial dielectric and breakdown degradation properties through
damage. This can effectively improve the material's resistance changes in the structure of aggregated states. The article pro-
to deformation. At the same time, MPE is an elastic material. poses a method for improving material insulating properties by
regulating the structure of aggregated states using MPE as a
nucleating agent. The following conclusions are drawn in this
article:

1. MPE, as a nucleating agent, can serve as heterogeneous

nucleation sites, increase the crystallinity of XLPE, reduce
the distance between crystal faces, and make the crystalline
region more compact. Also, nucleating agents can increase
the Young's modulus of the material. The tightly packed
crystalline region is less likely to undergo deformation
during the stretching process, which reduces the degree of
damage to the aggregated state structure during stretching.
Compared to XLPE with the same stretching ratio, the
crystallinity is higher.
2. Nucleating agents make the crystalline region more compact
and regular, with fewer defects, reducing the material's deep
trap density. Meanwhile, they provide strong interfacial
FIGURE 11 Stress–strain curve of the samples. adhesion, enhancing the external forces' resistance of
 23977264, 2024, 2, Downloaded from https://ietresearch.onlinelibrary.wiley.com/doi/10.1049/hve2.12396 by South Korea National Provision, Wiley Online Library on [23/07/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
438
- XING ET AL.

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