Solid State Ionics 370 (2021) 115748

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Solid State Ionics

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Effect of Ce0.85Sm0.15O2-δ–CuO interlayer on the performance of

intermediate-temperature solid oxide electrolysis cell
Xiaoyan Wang , Ji Yu *, Ning Tian *, Hai Shen
College of Physics Science and Technology, Shenyang Normal University, Shenyang 110034, China

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

Keywords: To improve the performance of intermediate-temperature solid oxide electrolysis cells (IT-SOECs) based on the
Solid oxide electrolysis cell Ce0.85Sm0.15O2-δ (SDC) interlayer, a transition metal oxide (CuO) was added to the interlayer to enhance its
Interlayer oxygen ion conduction, and thereby, reduce the oxygen electrode polarization resistance of the SOEC. The
Oxygen electrode
performance of SOECs based on the SDC–CuO interlayers was studied. The experimental results showed that
SDC–CuO interlayers sintered for 10 h at 1050 ◦ C, 1075 ◦ C, and 1100 ◦ C (referred to as SDC–CuO-1050,
SDC–CuO-1075, and SDC–CuO-1100, respectively) are highly dense. This indicates that the preparation tem­
perature of a dense SDC interlayer can be reduced by compositing it with CuO. The performances of SOECs based
on the SDC–CuO-1050, SDC–CuO-1075, and SDC–CuO-1100 interlayers were higher than that of the SOEC based
on the SDC interlayer. This indicates that oxygen ions can move faster from the SDC–CuO-1050, SDC–CuO-1075,
and SDC–CuO-1100 interlayers to the oxygen electrode to participate in the electrochemical reaction. This re­
duces the polarization resistance of oxygen electrodes and improves the performance of the SOECs. The per­
formance of the SOEC based on the SDC–CuO-1050 interlayer is the highest, indicating that sintering at 1050 ◦ C
for 10 h is the best condition to prepare high-performance SDC–CuO interlayers. Thus, this study provides an
effective method for improving the performance of IT-SOEC based on SDC interlayer.

1. Introduction
At present, intermediate-temperature (600–800 ◦ C) solid oxide
electrolysis cells (IT-SOECs) are widely considered an advanced
hydrogen production technology because of their high efficiency and
environment-friendliness [1–5]. According to the different carriers
transported in these, SOECs can be categorized into oxide-ion-
conducting and proton-conducting SOECs [6–10]. The research on
SOECs focuses mainly on the oxide-ion conducting SOEC. Yttria-
stabilized zirconia (YSZ) with a significantly low electronic conductiv­
ity is commonly used as the electrolyte material in oxide-ion-conducting
SOECs. However, most of the high-performance IT-SOEC oxygen elec­
trodes are made of materials containing Sr (e.g., La1-xSrxCo1-yFeyO3-δ,
La1-xSrxCoO3-δ, La1-xSrxFeO3-δ, and Ba1-xSrxCoyFe1-yO3-δ). The Sr in these
oxygen electrode materials straightforwardly diffuse during the prepa­
ration and operation of an oxygen electrode and react with the Zr in the
YSZ electrolyte to form an SrZrO3 insulating phase [11–16]. This hinders
the transport of oxygen ions from the electrolyte to the oxygen electrode,
and thereby increases the polarization resistance of the oxygen electrode
and reduces the electrolysis capability of the SOEC. To solve this prob­
lem, a doped ceria (e.g., Sm-doped ceria (SDC) or Gd-doped ceria (GDC))
interlayer is added between the electrolyte and oxygen electrode to
prevent the diffusion of Sr and the formation of the SrZrO3 insulating
phase [11–18], which facilitates lowering of the polarization resistance
of the oxygen electrode. The interlayer hinders the diffusion of Sr and
functions as a bridge to transport oxygen ions from the electrolyte to the
oxygen electrode. Thereby, the oxygen ion conduction of the interlayer
would affect the polarization resistance of the oxygen electrode. If the
oxygen ion conductivity of the interlayer is improved, oxygen ions
would move faster to the oxygen electrode to participate in the elec­
trochemical reaction. This would reduce the polarization resistance of
the oxygen electrode. However, interdiffusion would occur between the
YSZ and the GDC or SDC interlayers during high-temperature sintering.
This is not conducive to the transport of oxygen ions. The reaction be­
tween these would be weakened if the sintering temperature of inter­
layer is reduced. The transition metal oxide CuO can reportedly reduce
the sintering temperature of SDC material and improve its oxygen ion
conductivity [19–22]. For example, the preliminary studies by our

* Corresponding author.
E-mail addresses: yuji4268@163.com (J. Yu), tiann08@163.com (N. Tian).

https://doi.org/10.1016/j.ssi.2021.115748
Received 14 April 2021; Received in revised form 4 August 2021; Accepted 26 August 2021
Available online 2 September 2021
0167-2738/© 2021 Elsevier B.V. All rights reserved.
 X. Wang et al.
research group demonstrated that the SDC–CuO electrolyte with 0.5 mol
% CuO sintered at 1000 ◦ C had similar relative theoretical density and
higher grain boundary conduction and total electrical conduction
compared to those of the SDC electrolytes sintered at higher tempera­
tures (1250–1400 ◦ C) [19,20]. Our research results demonstrated that
the addition of an appropriate amount of CuO can effectively enhance
the sintering and oxygen ion conductivity of SDC. Y. C. Dong et al. re­
ported that the densification temperature of SDC was lowered by doping
with 1 mol% CuO. The density of an SDC–CuO electrolyte with 1 mol%
CuO sintered at 950–1100 ◦ C was similar to that of an SDC electrolyte
sintered at 1400 ◦ C [21]. In addition, the CuO additive improved the
electrical conductivity of SDC by decreasing its activation energy. S. Y.
Toor et al. reported that the oxygen ion conductivity of an SDC–CuO
electrolyte with 10 mol% CuO sintered at 1100 ◦ C was higher than that
of an SDC electrolyte sintered at 1450 ◦ C [22]. Furthermore, the total
conductivity of an SDC–CuO electrolyte with 5 mol% CuO was similar
with that of an SDC electrolyte. However, the electronic conductivity of
the former was 1/3 times lower than that of the latter. Their experi­
mental results indicated that CuO sintering could improve the electrical
property of SDC.
Based on the above results, it can be inferred that the addition of the
transition metal oxide CuO to the SDC interlayer of an SOEC can yield a
dense SDC interlayer at a lower sintering temperature and enhance its
oxygen ion conductivity. In other words, an SDC–CuO interlayer can
reduce the polarization resistance of an oxygen electrode and improve
the performance of the SOEC. To verify the above inference, herein we
studied the effect of an SDC–CuO interlayer on the performance of an
SOEC. Specifically, we studied the performance of SOECs with SDC–CuO
interlayers sintered at five sintering temperatures (1000 ◦ C, 1025 ◦ C,
1050 ◦ C, 1075 ◦ C, and 1100 ◦ C) within the melting point range of CuO
(1000–1100 ◦ C), and determined the most suitable sintering tempera­
ture for an SDC–CuO interlayer.
2. Experimental
2.1. Sample preparation
In this study, SDC and SDC–CuO (CuO content 0.5 mol%), used as
interlayer materials, were prepared by the glycine–nitrate process. The
preparation process is described in detail elsewhere [19,20,23–26]. The
raw materials Ce(NO3)3, Sm(NO3)3, and Cu(NO3)3 were weighed ac­
cording to the molar ratio of metal cations in SDC–CuO, and then dis­
solved in deionized water. Glycine was added according to the molar
ratio of glycine to the total metal cations (1.7). The solution was turned
into a gel on heating, and then, into ashes by spontaneous combustion.
The SDC–CuO powder was obtained by calcining the above-mentioned
ashes in air at 600 ◦ C for 6 h. (Y2O3)0.08(ZrO2)0.92 (YSZ; purchased
from Ningbo SOFCMAN Energy Technology Co., Ltd.), (La0.6Sr0.4)0.95
Co0.2Fe0.8O3-δ (LSCF; purchased from Nexceris, LLC, Fuelcellmaterials,
Lewis Center, OH, USA), and NiO (prepared by the glycine–nitrate
process) were used as the electrolyte material, oxygen electrode mate­
rial, and hydrogen material of the SOECs. YSZ electrolyte ceramic sheets
of SOEC were prepared by pressing YSZ powder into green sheets (with a
diameter of 13 mm) at 300 MPa and by sintering at 1400 ◦ C for 4 h. The
thickness of the electrolyte sheets after sanding was approximately 400
μm. The SDC interlayer of SOEC was prepared at 1250 ◦ C for 10 h. The
SDC–CuO interlayers of the SOECs were prepared by sintering for 10 h at
different temperatures: 1000 ◦ C, 1025 ◦ C, 1050 ◦ C, 1075 ◦ C, and
1100 ◦ C, and were referred to as SDC–CuO-1000, SDC-CuO-1025,
SDC–CuO-1050, SDC–CuO-1075, and SDC–CuO-1100, respectively.
The preparation process of the symmetrical cells with an LSCF–SDC/
interlayer/YSZ/interlayer/LSCF–SDC structure was as follows: First, the
weight of each interlayer material was approximately 10 mg. A mixture
of terpineol and ethylcellulose was mixed with the interlayer material
powders to obtain well-distributed slurries. The interlayer was coated on
both sides of the YSZ electrolyte sheet by the screen printing method and
2
­
Solid State Ionics 370 (2021) 115748
then, sintered at a high temperature. There were six types of interlayer
used in the symmetrical cells: SDC, SDC–CuO-1000, SDC–CuO-1025,
SDC–CuO-1050, SDC–CuO-1075, and SDC–CuO-1100. Second,
LSCF–SDC composite oxygen electrode (mass ratio of LSCF to SDC = 7:3)
was coated on the surface of the interlayer by the screen printing method
and calcined at 950 ◦ C for 5 h. The preparation process of the SOEC with
an NiO–SDC/YSZ/interlayer/LSCF–SDC structure was as follows. First,
the interlayer was prepared on one side of the YSZ electrolyte sheet,
under conditions identical to those for preparing the interlayer in the
symmetrical cells. Second, NiO–SDC hydrogen electrode (mass ratio of
NiO to SDC = 6:4) was prepared on the other side of the electrolyte sheet
by the screen printing method, and then calcined at 1000 ◦ C for 5 h.
Then, LSCF–SDC oxygen electrode was prepared on the surface of the
interlayer under a condition similar to that of the LSCF–SDC of the
symmetrical cell. Notably, the effective oxygen electrode area of the
above symmetric cells and SOECs was 0.4 cm × 0.4 cm. Silver paste and
silver wire were used as the collector and conductor, respectively, of the
symmetrical cells and SOECs. Silver paste was also used as a sealant to
fix the SOECs on one end of the ceramic tubes, which were used as the
gas chambers for the hydrogen electrodes.
2.2. Measurement of samples
The surface morphologies of the SDC and SDC–CuO interlayers and
the cross-sectional morphologies of the LSCF–SDC/interlayer/YSZ
structures were characterized by an FEI Quanta FEG 250 scanning
electron microscope (SEM). An energy-dispersive X-ray spectrometer
(EDS) installed in this SEM was used to study the Sr distribution across
the LSCF–SDC/interlayer/YSZ structures. The impedance spectra of the
symmetrical cells and SOECs were characterized by the electrochemical
workstation CHI 760E (Shanghai Chenhua Instrument Corporation,
China) operated over a frequency range of 10− 1–106 Hz and at signal
amplitude of 50 mV. The stability of the symmetrical cells was tested by
the chronopotentiometry function of the electrochemical workstation
(current density = 0.2 A/cm2). The current density–voltage character­
istic curves of the SOECs were obtained using the linear sweep vol­
tammetry function of the electrochemical workstation (sweep rate = 9
mV/s). During the SOEC performance test, a mixture of water vapor,
hydrogen, and nitrogen was introduced into the hydrogen electrode,
wherein the hydrogen flow rate was 40 mL min− 1, the nitrogen flow rate
was 50 mL min− 1, and the relative humidity of the mixture was 40 vol%.
3. Results and discussion
Fig. 1(a)–(f) show the surface morphologies of the SDC–CuO-1000,
SDC–CuO-1025, SDC–CuO-1050, SDC–CuO-1075, SDC–CuO-1100, and
SDC interlayers, respectively. The six interlayers are relatively flat,
which is conductive to their integration with other parts of an SOEC. The
SDC–CuO-1050, SDC–CuO-1075, SDC–CuO-1100, and SDC interlayers
are relatively dense, whereas the SDC–CuO-1000 and SDC–CuO-1025
interlayers have low density and many pores. Fig. 1(g)–(l) show the
cross-sectional morphologies of the LSCF–SDC/SDC–CuO-1000/YSZ,
LSCF–SDC/SDC–CuO-1025/YSZ, LSCF–SDC/SDC–CuO-1050/YSZ,
LSCF–SDC/SDC–CuO-1075/YSZ, LSCF–SDC/SDC–CuO-1100/YSZ, and
LSCF–SDC/SDC/YSZ structures, respectively. The area between the
dotted lines in each figure represents an interlayer. Evidently, the six
interlayers are combined well with the oxygen electrodes and electro­
lytes, which ensures the stability of the SOECs. The densities of cross-
sectional morphology of the SDC–CuO-1050, SDC–CuO-1075,
SDC–CuO-1100, and SDC interlayers are high, whereas those of the
SDC–CuO-1000 and SDC–CuO-1025 interlayers are significantly low.
This indicates that sintering for 10 h at 1000 ◦ C and 1025 ◦ C are not
suitable for the preparation of dense SDC–CuO interlayers. The density
of the interlayer determines its oxygen ion conductivity. Oxygen ions
would move faster from the dense interlayer to the oxygen electrode of
an SOEC to participate in the electrochemical reaction of the oxygen
X. Wang et al. Solid State Ionics 370 (2021) 115748

Fig. 1. Interlayer surface morphologies of (a) SDC–CuO-1000, (b) SDC–CuO-1025, (c) SDC–CuO-1050, (d) SDC–CuO-1075, (e) SDC–CuO-1100, and (f) SDC, and cross-sectional morphologies of (g) LSCF–SDC/SDC–CuO-
1000/YSZ, (h) LSCF–SDC/SDC–CuO-1025/YSZ, (i) LSCF–SDC/SDC–CuO-1050/YSZ, (j) LSCF–SDC/SDC–CuO-1075/YSZ, (k) LSCF–SDC/SDC–CuO-1100/YSZ, and (l) LSCF–SDC/SDC/YSZ structures.
Fig. 2. AC impedance spectra of symmetrical cells with LSCF–SDC/interlayer/
YSZ/interlayer/LSCF–SDC structure under the open circuit voltage (OCV), in air
atmosphere, and at 800 ◦ C.

electrode. This is conducive to lowering the polarization resistance of

the oxygen electrode and improving the performance of the SOEC. The
density of the interlayer also determines the formation of an SrZrO3
insulating phase. In our case, the non-dense SDC–CuO-1000 interlayer
and relatively dense SDC–CuO-1050 interlayer were selected as exam­
ples to study the Sr diffusion. EDS line scans were performed on the
LSCF–SDC/SDC–CuO-1000/YSZ and LSCF–SDC/SDC–CuO-1050/YSZ
structures (Fig. S1). It was observed that Sr was distributed in the oxygen
electrode, interlayer, and electrolyte of the LSCF–SDC/SDC–CuO-1000/
YSZ structure, indicating that the non-dense SDC–CuO-1000 interlayer
could not effectively inhibit Sr diffusion. For the LSCF–SDC/SDC–CuO-
1050/YSZ structure, Sr was distributed mainly in the oxygen electrode
and less in the interlayer and electrolyte, indicating that the relatively
dense SDC–CuO-1050 interlayer could effectively inhibit Sr diffusion.
The SrZrO3 insulating phase increased the polarization resistance of the
oxygen electrode. Hence, a dense interlayer (e.g., SDC–CuO-1050,
SDC–CuO-1075, SDC–CuO-1100, and SDC) is effective for realizing a
low polarization resistance of an oxygen electrode. In other words, the
dense SDC–CuO-1050, SDC–CuO-1075, SDC–CuO-1100, and SDC in­
terlayers are suitable for high-performance SOEC.
The symmetric cells with the LSCF–SDC/interlayer/YSZ/interlayer/
LSCF–SDC structure were constructed to study the effect of interlayer on
the performance of the oxygen electrode in an SOEC. The AC impedance
spectra of the symmetrical cells under the open circuit voltage (OCV)
and at 800 ◦ C were measured (see Fig. 2). To directly compare the po­
larization resistance of oxygen electrodes in symmetrical cells, the
ohmic resistance of symmetrical cells are subtracted from the impedance
spectra. For symmetrical cells, the electrode polarization resistance in
Fig. 2 is for one electrode. It is obtained by dividing the symmetrical cell
electrode polarization resistance from two. For each AC impedance
spectrum, the difference between the high- and low-frequency intercepts
(with the real axis) is the polarization resistance (Rp) of the oxygen
electrode. The oxygen electrode polarization resistances of the sym­
metrical cells based on the SDC–CuO-1050, SDC–CuO-1075, and
SDC–CuO-1100 interlayers were lower than that of the symmetrical cell
based on the SDC interlayer. This is because the oxygen ion conduction
in the SDC–CuO-1050, SDC–CuO-1075, and SDC–CuO-1100 interlayers
was higher than that in the SDC interlayer, in which oxygen ions can
move faster to the oxygen electrode of symmetrical cell to participate in
the electrochemical reaction of oxygen electrode, and thereby reduce
the oxygen electrode polarization resistance. Hence, it indicates that the
performances of SDC–CuO-1050, SDC–CuO-1075, and SDC–CuO-1100

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X. Wang et al. Solid State Ionics 370 (2021) 115748

Table 1
RH, RL, and Rp values of the symmetrical cells based on the six types of interlayer
(SDC–CuO-1000, SDC–CuO-1025, SDC–CuO-1050, SDC–CuO-1075, SDC–CuO-
1100, and SDC) obtained by an equivalent circuit fitting of the impedance
spectra. Note that the unit of R is Ω cm2.
RH RL Rp

SDC-CuO-1000 0.031 0.047 0.078

SDC-CuO-1025 0.028 0.054 0.082
SDC-CuO-1050 0.017 0.009 0.026
SDC-CuO-1075 0.016 0.012 0.028
SDC-CuO-1100 0.026 0.017 0.043
SDC 0.027 0.020 0.047

Fig. 3. Polarization resistance stability curves of oxygen electrodes of sym­

metrical cells based on the six types of interlayer, obtained by short-term
electrolysis durability test under OCV in air atmosphere and at 800 ◦ C.

interlayers were superior to that of an SDC interlayer. The oxygen

electrode polarization resistance of the symmetrical cell based on the
SDC–CuO-1050 interlayer is also lower than those of the symmetrical
cell based on the SDC–CuO-1075 and SDC–CuO-1100 interlayers. This
indicates that sintering at 1050 ◦ C for 10 h is the best method for pre­
paring high-performance SDC–CuO interlayers. Furthermore, it is
evident that the oxygen electrode polarization resistance of the sym­
metrical cell based on the SDC–CuO-1000 and SDC–CuO-1025 in­
terlayers is higher than that of the other symmetrical cells. This may be
because SDC–CuO interlayers sintered for 10 h at 1000 ◦ C and 1025 ◦ C
are not dense, which results in its low oxygen ion transport capability
and the formation of the SrZrO3 insulating phase, and thereby increases
the oxygen electrode polarization resistance of the symmetrical cell.
Fig. 4. (a) Voltage–current density characteristic curves of SOECs based on the
Therefore, sintering at 1000 ◦ C for 10 h and 1025 ◦ C for 10 h are not six types of interlayer at 800 ◦ C with relative humidity of 40 vol%. (b) AC
suitable for the preparation of high-performance SDC–CuO interlayers. impedance spectra of electrodes of SOECs based on the six types of interlayer
There are two arcs for each AC impedance spectrum: high-frequency arc under OCV conditions and at 800 ◦ C with relative humidity of 40 vol%. (c) Ro,
and low-frequency arc. An equivalent circuit of Ro(RH/CPEH)(RL/CPEL) Rp, and Rt values of SOECs fitted from the above AC impedance spectra.
is developed to fit the spectra, where Ro is the ohmic resistance, CPE is
the constant phase element, the subscripts H and L correspond to the durability test, AC impedance measurements of the symmetrical cells
high- and low-frequency arcs respectively, and Rp = RH + RL. The fitting were conducted every 5 h under OCV conditions with interruptions of
values of the RH, RL, and Rp of the symmetrical cells are listed in Table 1. the electrolysis test. Fig. 3 shows the polarization resistance stability
The Rp value of the oxygen electrode in the symmetrical cell based on curves of the oxygen electrodes of the symmetrical cells in the short-
the SDC–CuO-1050 interlayer can be 0.026 Ω cm2, which is comparable term electrolysis durability test. All the oxygen electrodes of the sym­
to that of the reported LSCF oxygen electrode with remarkable perfor­ metrical cells showed good stability, indicating that the performances of
mance [14–16]. the six types of interlayer were stable.
To study the stabilities of the six types of interlayer, the short-term The electrical properties of the SOECs with the NiO–SDC/YSZ/
stabilities of their symmetrical cells was tested for 30 h at 800 ◦ C and interlayer/LSCF–SDC structure based on the six types of interlayer were
under a current of 0.2 A cm− 2. During the short-term electrolysis studied. The voltage–current density characteristic curves of SOECs

4
X. Wang et al.
based on the six types of interlayer at 800 ◦ C are shown in the Fig. 4(a).
At 1.5 V, the current densities of the SOECs based on the SDC–CuO-
1000, SDC–CuO-1025, SDC–CuO-1050, SDC–CuO-1075, SDC–CuO-
1100, and SDC interlayers are 0.16, 0.17, 0.40, 0.32, 0.25, and 0.19 A
cm− 2, respectively. Clearly, the SOEC based on the SDC–CuO-1050
interlayer showed the best electrolytic performance, indicating that the
oxygen ion transport capability of the SDC-CuO-1050 interlayer was the
highest among the six types of interlayer. Fig. 4(b) shows the AC
impedance spectra of the electrodes of the SOECs based on the six types
of interlayer under the OCV conditions and at 800 ◦ C. An equivalent
circuit of R0(Rp/CPE) was developed to fit the spectra. Here, the total
resistance (Rt) was given as the sum of Ro and Rp. The fitting values of
the Ro, Rp, and Rt of the SOECs are shown in the Fig. 4(c). In all the
SOECs, Ro accounts for a larger proportion of Rt than Rp does. This
phenomenon is related to the electrolyte-supported structure of the
SOECs. Evidently, the Rp value of the SOEC based on the SDC–CuO-1050
interlayer is the lowest. Because the preparation conditions of the
NiO–SDC hydrogen electrodes of the SOECs were identical, the differ­
ence in the Rp values of the SOECs was caused mainly by their oxygen
electrodes. The performances of the oxygen electrodes of the SOECs
were affected by their interlayers. This also demonstrates that the per­
formance of the SDC–CuO-1050 interlayer was the highest among the six
types of interlayer.
4. Conclusions
With the addition of CuO to the SDC interlayer of an SOEC, the ox­
ygen ion conduction of the interlayer is enhanced, which in turn, im­
proves the performance of the SOEC. The performance of SOECs based
on SDC–CuO interlayer was studied. The experimental results show that
the SDC–CuO-1050, SDC–CuO-1075, and SDC–CuO-1100 interlayers
were highly dense. This indicates that the preparation temperature of a
dense SDC interlayer can be reduced by compositing it with CuO. The
performances of the SOECs based on SDC–CuO-1050, SDC–CuO-1075,
and SDC–CuO-1100 interlayers were higher than that of the SOEC based
on the SDC interlayer. This indicates that the oxygen ion transport ca­
pabilities of SDC-CuO-1050, SDC-CuO-1075, and SDC-CuO-1100 in­
terlayers are higher than that of an SDC interlayer. Oxygen ions can
move faster from SDC-CuO-1050, SDC-CuO-1075, and SDC-CuO-1100
interlayers to participate in the electrochemical reaction of oxygen
electrodes. This reduces the polarization resistance of oxygen electrodes
and improves the performance of the SOECs. The performance of the
SOEC based on the SDC-CuO-1050 interlayer was the best. This indicates
that sintering at 1050 ◦ C for 10 h is the best method for preparing high-
performance SDC–CuO interlayers. The above results show that
compositing CuO with SDC interlayers is an effective method for
improving the SDC-interlayer performance of IT-SOEC.
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.ssi.2021.115748.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgments
This study was financed by Natural Science Foundation of Liaoning
Province (2019JH3/30100036, 2019-ZD-0480).
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