The integration of LiNi0.8Co0.1Mn0.1O2 coatings on separators for elevated battery performance

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## Nitou et al. Energy Mater. 2025, 5, 500018 Energy Materials

DOI: 10.20517/energymater.2024.105

Article Open Access

# The integration of LiNi0.8Co0.1Mn0.1O2 coatings on separators for elevated battery performance

Modeste Venin Mendieev Nitou1,2, Xiaodong Fang1, Jiaqi Wang1,3, Rui Liu1,3, Yashuai Pang1, Yinghua

Niu1,2,3,*, Wu Qin4, Chao Zhao5,*, Yuanfu Chen2,*, Zhen Zhang5, Weiqiang Lv1,3,*

Modeste Venin Mendieev Nitou

1,2,3,*, Wu Qin4, Chao Zhao5,*, Yuanfu Chen2,*, Zhen Zhang5, Weiqiang Lv1,3,*

1School of Physics, University of Electronic Science and Technology of China, Chengdu 611731, Sichuan, China.
2School of Integrated Circuit Science and Engineering (Exemplary School of Microelectronics), Chengdu 611731, Sichuan, China.
3Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313001, Zhejiang,
China.
4National Engineering Laboratory for Biomass Power Generation Equipment, School of Renewable Energy Engineering, North
China Electric Power University, Beijing 102206, China.
5School of Chemical Engineering and Technology, Center for Biosafety Research and Strategy, Tianjin University, Tianjin 300072,
China.

*Correspondence to: Dr. Yinghua Niu, School of Physics, University of Electronic Science and Technology of China, No. 2006,
Xiyuan Ave, West Hi-Tech Zone, Chengdu 611731, Sichuan, China. E-mail: yh_niu@uestc.edu.cn; Dr. Yuanfu Chen, School of

Integrated Circuit Science and Engineering (Exemplary School of Microelectronics), Chengdu 611731, Sichuan, China. E-mail:

yfchen@uestc.edu.cn; Dr. Weiqiang Lv, School of Physics, University of Electronic Science and Technology of China, No. 2006,

Xiyuan Ave, West Hi-Tech Zone, Chengdu 611731, Sichuan, China. E-mail: eselwq@uestc.edu.cn; Dr. Chao Zhao, School of

Chemical Engineering and Technology, Center for Biosafety Research and Strategy, Tianjin University, No. 92, Weijin Road,

Tianjin 300072, China. E-mail: zhao_chao@tju.edu.cn

How to cite this article: Nitou, M. V. M.; Fang, X.; Wang, J.; Liu, R.; Pang, Y.; Niu, Y.; Qin, W.; Zhao, C.; Chen, Y.; Zhang, Z.; Lv, W.
The integration of LiNi0.8Co0.1Mn0.1O2 coatings on separators for elevated battery performance. _Energy Mater._ 2025, _5_, 500018.
[https://dx.doi.org/10.20517/energymater.2024.105](https://dx.doi.org/10.20517/energymater.2024.105)

Received: 3 Aug 2024 First Decision: 12 Oct 2024 Revised: 27 Oct 2024 Accepted: 31 Oct 2024 Published: 10 Jan 2025

Academic Editor: Jiazhao Wang Copy Editor: Fangling Lan Production Editor: Fangling Lan

Abstract

Improving the efficiency and safety of lithium-ion batteries (LIBs) with high-energy cathodes is crucial, yet

challenging due to the limitations of commercial separators. Herein, we find that “giving” a portion of the Ni-rich
LiNi0.8Co0.1Mn0.1O2 (NCM811) positive electrode to the Al2O3-coated polyethylene (PE) (PE/Al2O3) separator as an
active and thick ceramic coating (> 10 µm) can more efficiently enhance the separator's wettability and thermal
stability compared with the inert and thin (< 5 µm, typically 1~2 µm) Al2O3 coating. The NCM811 coating on the
separator can take part in the electrochemical reaction and contribute capacity without increasing the cell dead

weight. The NCM811-coated separator has a low thermal shrinkage of 0.8% at 160 °C and a high lithium-ion

transfer number of 0.66. Notably, the NCM811-coated separator enhances electrochemical performance, delivering
higher capacities compared to traditional PE and PE/Al2O3 separators. Furthermore, it effectively mitigates lithium

© The Author(s) 2025. Open Access This article is licensed under a Creative Commons Attribution 4.0
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Page 2 of 13 Nitou _et al. Energy Mater._ 2025, _5_, 500018 https://dx.doi.org/10.20517/energymater.2024.105

dendrite formation, thereby bolstering LIB safety. Our findings demonstrate the potential of using active cathode

materials as separator coatings to advance LIB technology with high-energy cathodes.

Keywords: Lithium-ion batteries, separator, NCM811 coating, thermal stability, lithium dendrites

## INTRODUCTION

Rechargeable batteries with lithium-ion (LIBs) are in high demand for large-scale applications, including
portable electronics [1,2], electric automobiles [3-5], and energy storage systems (ESSs) [6-8] . To meet the demand,
various cathodes have been explored to increase the energy density of LIBs [9-12] . However, higher energy
density also means more electrochemically active material [13,14], which can cause safety problems due to
unfavorable reactions during charging and discharging cycles [15,16] . Moreover, high-energy materials can
pose a risk to consumers by triggering fires, explosions, and pollution if the batteries are used in abnormal
conditions. Therefore, many studies have focused on improving the performance of battery components [17],
especially the separator, which acts as a key factor for battery thermal stability [18-20], as it separates the anode
and the cathode [21-23] . Currently, most industrial LIBs use polyolefin separators, such as polypropylene (PP),
polyethylene (PE), and their blends due to their suitable chemical stability, reasonable cost, and acceptable
mechanical strength [24-26] . However, these separators have low porosity, and poor wettability, which limit
their electrolyte uptake and ionic conductivity [27,28] . They also have poor thermal stability and low melting
points (around 130-170 °C), which compromise the safety of LIBs [29-32] . One of the effective solutions to the
above problems is to coat polyolefin separators with ceramic particles [33-37] . Ceramic particles, such as
SiO2[38,39], TiO2[40].and Al2O3[41], are often applied on one or both sides of polyolefin separators to enhance

SiO2[38,39], TiO2[40].and Al2O3[41], are often applied on one or both sides of polyolefin separators to enhance

their thermal stability and electrolyte absorption. Additionally, 3D imaging and analysis techniques are also
employed to demonstrate how pore size distribution, tortuosity, and phase connectivity influence ion
transport and reaction kinetics [42] . However, these electrochemically inert ceramic layers must be thin
enough (< 5 µm, typically 1~2 µm) to avoid increasing the dead weight of batteries [43], and thus show limited
improvement in thermal stability and wettability. Therefore, further improvement of ceramic-coated
separators is needed.

[38,39], TiO2

[40].and Al2O3

In this research, we suggest a novel separator design using Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM811) as a
coating component on PE/Al2O3 separators. NCM811 is a high-energy cathode material that has high
capacity and energy density but also poses safety risks due to poor thermal stability during repeated cycling,
gas evolution, phase transition, and microcracks [44] . By using NCM811 as a coating material on PE/Al2O3
separators, we aim to improve not only the separator properties but also the electrochemical proprieties and
safety of the NCM811 cathode. The NCM811 coating layer is directly coated on PE/Al2O3 separators by a
simple casting method. Compared with the inert and thin Al2O3 coating, the active NCM811 coating on
separators can participate in the electrochemical reactions to contribute capacities, which allow applying
thicker ceramic layers (> 10 µm) to more efficiently improve the wettability, thermal stability, ionic
diffusion, and Li-ion transfer number of separators.

## EXPERIMENTAL AND CALCULATION METHODS

The bare PE separator, the Al2O3 inert ceramic coated PE separator, and NCM811 were all purchased from
Canrd New Energy Technology Co., Ltd. The PE/Al2O3 separator has a model of MC112S1D and shows a
structure of polyvinylidene fluoride (PVDF)/PE/Al2O3/PVDF with a thickness of 1 + 7 + 2 + 1 μm. The bare
PE separator has a model MA-EN-SE-0C011E and a thickness of 12 μm. The NCM811 material was milled
[by a planetary ball mill for 225 min to reduce the particle size [Supplementary Figure 1A]. The NCM811](https://oaepublishstorage.blob.core.windows.net/articlepdfpreview202501/em40105-SupplementaryMaterials.pdf)
coated slurry was prepared using PVDF, NCM811, and Ketjen black (KB) dispersed in N-methyl

Nitou _et al. Energy Mater._ 2025, _5_, 500018 https://dx.doi.org/10.20517/energymater.2024.105 Page 3 of 13

pyrrolidone (NMP). The weight ratios of NCM811, KB, and PVDF were 90:3:7. The coating slurry was
stirred uniformly and coated on a 10 [µm thick PE/Al2O3 separator [Supplementary Figure 1B]. The](https://oaepublishstorage.blob.core.windows.net/articlepdfpreview202501/em40105-SupplementaryMaterials.pdf)
separator was dried in a vacuum oven at 80 °C for one day. The total thicknesses of NCM-unmilled and
NCM-crushed coated separators were about 32 and 28 µm, respectively.

The surface morphologies of the separators were examined by scanning electronic microscopy (SEM). The
mechanical strength of the separators was assessed using a mechanical testing system. The separator’s
thermal stability was evaluated via an infrared thermal imager (FLIR, model A655sc). The thermal shrinkage
was determined by measuring the separator’s areas before and after heating for 30 min at various
temperatures. The electrolyte uptake was determined by measuring the separator’s weights before and after
being immersed in the electrolyte for 30 min. The separator’s wettability was measured by a surface contact
angle test. The ionic conductivities at various temperatures were measured by AC impedance spectroscopy.

The electrochemical performance of the NCM811 cathode with different separators was evaluated by
assembling coin-type half-cells (CR2032) in an argon-filled glove box. The positive electrode was prepared
by mixing NCM811, PVDF, and KB with a weight ratio of 85:10:5. The negative electrode was a lithium
metal foil. The electrolyte was 1.0 M LiPF6 in ethylene carbonate (EC) and ethyl methyl carbonate (EMC)
with a weight ratio of 3:7. The cells were cycled between 2.4 and 4.8 V at various current rates using a
battery tester (LAND CT2001A). The total active material in both cathode and separator active coatings is
included for calculating mass specific capacity. The electrochemical impedance spectroscopy (EIS)
measurements were performed on a CHI660E electrochemical workstation in the frequency range from
100 kHz to 10 mHz with an amplitude of 5 mV. The lithium-ion transference number ( ) was calculated
through the EIS impedance before and after a direct-current (DC) polarization using the electrochemical
workstation (DH7001B, DongHua Analytical). The was calculated at room temperature using:

where ΔV represents the applied DC polarization voltage (0.01 V) in the chronoamperometric step, and I0
and Is denote the initial and steady-state currents, respectively. The initial and steady-state interfacial
resistances are denoted by Ro and Rs, respectively.

The interaction between separator layers was studied by determining the atomic configurations and
adsorption energies of PE with Al2O3 and NCM811 using density functional theory (DFT) calculation
implemented by the Dmol3 package within a generalized gradient approximation (GGA) of the PerdewBurke-Ernzerhof (PBE) functional. The Double Numeric with polarization (DNP) basis sets with effective
core potential were employed for self-consistent field (SCF) calculations with 1 × 10 -6 eV/atom SCF
tolerance, 1000 Max. SCF cycles, and Gamma K-point was used for molecule and surface model
optimization. Butane molecule was used to represent the fragment of the PE polymer chain. Al2O3(001)
surface and NCM(100) were created and optimized before absorption calculation. A small Al2O3 cluster was
used to calculate the interaction between NCM(100) surface and Al2O3.

## RESULTS AND DISCUSSION

As illustrated in Figure 1, the performances of the bare PE separator, Al2O3 inert ceramic coated PE
separator, and NCM811 active material coated PE/Al2O3 separators are compared under a high-temperature
environment. At higher temperatures, as shown in Figure 1A, PE shrinks and melts, causing short circuits

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Figure 1. Schematic illustrating diagram of the failure mechanism of high-temperature stability of (A) polyolefin-based separator, (B)
inert ceramic-coated separator, (C) active material-coated separator. (D) Schematic illustrating capacity increase by using active
material coated separator instead of using a thick cathode.

of cells with pure PE separators. Thin Al2O3 ceramic particles in PE/Al2O3 separators [Figure 1B] lost their
support and collapse. However, the active material particles remain intact and supported by the Al2O3
ceramic layer. The active material coating not only has excellent thermal resistance, but also creates a
current path and electrochemical reaction due to the physical contact with the cathode, providing additional
capacity [Figure 1D].

[Supplementary Figure 1 illustrates the ball milling process of NCM811 and the preparation process of](https://oaepublishstorage.blob.core.windows.net/articlepdfpreview202501/em40105-SupplementaryMaterials.pdf)
[NCM811 coated separators. Supplementary Figure 2 shows that the NCM-unmilled powders had a larger](https://oaepublishstorage.blob.core.windows.net/articlepdfpreview202501/em40105-SupplementaryMaterials.pdf)
average particle size of 5.21 µm with some aggregates of smaller particles. The average particle dimension
was reduced from 5.21 µm to 2.64 µm after ball milling. Figure 2 exhibits the SEM images of the surfaces
and cross-sections of different separators. The SEM image of the bare PE separator in Figure 2A shows
uniform submicron pores. A uniform structured layer was formed when Al2O3 was coated on a bare PE
separator surface regardless of its shape [Figure 2B]. Similarly, the crushed NCM particles were well
distributed when they were coated on a PE/Al2O3 composite separator, as shown in Figure 2C. However, the
unmilled NCM particles had some small aggregates due to their large size, which might hinder their
uniform distribution in the coating layer [Figure 2D]. The energy dispersive X-Ray spectroscopy (EDX)
[mapping in Supplementary Figure 3 confirms the presence and uniform distribution of NCM811 coating on](https://oaepublishstorage.blob.core.windows.net/articlepdfpreview202501/em40105-SupplementaryMaterials.pdf)
the PE/Al2O3 separator. The cross-sectional image in Figure 2E demonstrates that the bare PE separator had
a thickness of 12 μm. The smooth cross-section layer of a PE/Al2O3 separator in Figure 2F demonstrates that
the Al2O3 ceramic material coating layer adhered to the surface of the pure PE separator and the Al2O3 layer
had a thickness of about 3 µm thick on one side. The coating layers of crushed and unmilled NCM particles
in Figure 2G and H were attached securely to the PE/Al2O3 ceramic-coated separator and had a thickness of
about 18 µm on one side.

Nitou _et al. Energy Mater._ 2025, _5_, 500018 https://dx.doi.org/10.20517/energymater.2024.105 Page 5 of 13

Figure 2. SEM images surface of (A) bare PE, (B) PE/Al2O 3, (C) NCM-crushed coated, and (D) NCM-unmilled coated separators.
Cross-sectional SEM image of (E) bare PE separator, (F) PE/Al2O3 separator, (G) NCM-crushed coated separator, and (H) NCMunmilled separator. (I) Contact angle pictures of different separators.

The separator’s wettability was evaluated by measuring the contact angle with the electrolyte and the
electrolyte uptake. Figure 2I shows that the Al2O3-coated separator was more hydrophilic than the bare PE
separator, as its contact angle reduced from 40° to 15° due to the presence of Al2O3 ceramic particles on its
surface. The NCM-coated separator was even more hydrophilic, with a contact angle of 8.5°, because of the
[NCM powder’s affinity for polar solvents. The electrolyte uptake in Supplementary Table 1 also confirmed](https://oaepublishstorage.blob.core.windows.net/articlepdfpreview202501/em40105-SupplementaryMaterials.pdf)
this trend. The bare PE separators had low electrolyte uptake because of their hydrophobic nature. While
the Al2O3-coated separators exhibited higher electrolyte uptake, the NCM coating can further increase
electrolyte uptake because of their hydrophilic nature and compatibility with the electrolyte solution.
Figure 3A shows the ionic conductivities of bare PE, Al2O3-coated PE, and NCM-coated PE/Al2O3
separators increased with temperature from 30 to 80 °C. The NCM-coated separator had the highest ionic
conductivity at all temperatures. Indicating that Li + ions could move more easily between the electrodes
[through the electrolyte. Supplementary Table 1 shows the ionic conductivity of several separators at 30 °C.](https://oaepublishstorage.blob.core.windows.net/articlepdfpreview202501/em40105-SupplementaryMaterials.pdf)
NCM-coated separators had an ionic conductivity of 0.85 mS cm -1, much higher than the 0.49 mS cm -1 of
the pure PE separator and the 0.54 mS cm -1 of the Al2O3-coated separator. The reason for the enhanced
ionic conductivity was the increased electrolyte absorption and wettability of the NCM-coated separator.

The mechanical properties of a separator are important for its industrial applications. Figure 3B compares
the mechanical properties of separators. NCM-crushed coated separators had a larger tensile strength of
[160.3 MPa than the PE/Al2O3 separator (158.5 MPa), as shown in Supplementary Table 1. The NCM-](https://oaepublishstorage.blob.core.windows.net/articlepdfpreview202501/em40105-SupplementaryMaterials.pdf)
unmilled coated separator had a lower tensile strength and puncture resistance, but a higher elongation, due
to the unevenness of the NCM-unmilled particles. Figure 3C and Table 1 show that the NCM-crushed
coated separator had a slightly greater puncture property of 4.6 N than the Al2O3-coated separator (4.4 N).
The thermal stability of separators was evaluated by measuring their shrinkage after being heated for half an
hour, as shown in Figure 3D. The pure PE separator had a high thermal shrinkage ratio of 60% at 160 °C,
due to its low melting point and isotropic structure. The Al2O3-coated PE separator had a lower thermal
shrinkage ratio of 26.3% at the same temperature. The NCM-unmilled coated and NCM-crushed coated

Page 6 of 13 Nitou _et al. Energy Mater._ 2025, _5_, 500018 https://dx.doi.org/10.20517/energymater.2024.105

Table 1. Summary of cell performance with different separators

Separators PE PE/Al2O3 NCM-unmilled NCM-crushed

NCM mass loading on cathode (mg/cm2) 7.87 7.86 7.93 7.88

NCM mass loading on separator (mg/cm2) 0 0 2.79 2.77

Discharge capacity (mAh/g)

0.5 C 166.5 178 216.3 219

1 C 102.4 134.8 152.8 184.9

2 C 64.5 109.7 120.7 142.5

4 C 24.6 69.2 82.6 92.3

Figure 3. (A) The ionic conductivities of pure PE, PE/Al2O 3, NCM-crushed and NCM-unmilled separators at different temperatures. (B)
Stress-strain profiles of different separators. (C) Force-displacement profiles for punch strength of various separators. (D) Heat
shrinkage for different separators under different temperatures.

separators had even lower thermal shrinkage ratios of 1% and 0.8%, respectively, because of the improved
thermal stability of the NCM particles.

Figure 4A shows optical images of different separators before and after heating them at 160 °C for 30 min.
The pure PE separator shrank significantly. The NCM-unmilled and crushed coated separators, on the
other hand, did not change their shape much, because of the thermal stability of NCM. This layer prevented
the polyolefin separator’s heat shrinkage effectively. Figure 4B shows the infrared images of different
separators. The bare PE separator began to shrink at 80 °C and reached its maximum shrinkage at 140 °C,
while Al2O3-coated separators were stable at 80 °C but began to shrink at 120 °C. NCM-unmilled and
crushed separators, however, remained stable even above the melting point of the bare PE separator. The
NCM layer on the separators improved their thermal stability, because of the superior thermal
performances of NCM811. The separator’s physical properties are important for the safety of LIBs,
especially for large-scale applications such as electric vehicles [45] . A combustion experiment was performed

Nitou _et al. Energy Mater._ 2025, _5_, 500018 https://dx.doi.org/10.20517/energymater.2024.105 Page 7 of 13

Figure 4. (A) Photographs of bare PE, PE/Al2O 3, NCM-crushed and NCM-unmilled coated separators after being exposed to the
temperature from 120-160 °C for 30 min. (B) FLIR thermal photos of the different separators. (C) Combustion photos of several
separators.

to compare the flame retardancy of different separators. Figure 4C shows the images of different separators
before, during, and after ignition. The bare PE separator blazed fast and disappeared after ignition. The
Al2O3-coated separator had better flame retardancy than the PE separator, because of the thermal stability of
Al2O3 ceramic particles. The NCM-coated separator burned slightly in the flames but did not burn
completely, showing its superior flame retardancy and non-flammability. Therefore, the NCM-coated
separator enhanced the safety performance of rechargeable batteries by increasing their heat resistance and
flame retardancy.

The EIS spectra of the LIB with different separators are shown in Figure 5A. All spectra showed two
overlapping semicircles, which represented the resistance of Li + ions through the surface layer on the
electrodes and the charge transport resistance at the electrode/electrolyte interface [46-48] . The cell with the
NCM-coated separator had the lowest interface resistances. The cyclic voltammetry (CV) tests were carried
out in the voltage range of 2.4-4.7 V at a scan rate of 0.1 mV/ s [Figure 5B]. The CV profiles showed two
couple of redox peaks, which corresponded to the redox reaction of Ni 2+ /Ni 4+ in the insertion and extraction
of lithium-ions during charge-discharge processes [49,50] . The potential intervals (∆E) between the anodic and
cathodic peaks reflected the electrochemical process involving electron transfer across the electrodes and
lithium-ion diffusion in the electrode/electrolyte interface. The first anodic peak which represented the
extraction of lithium-ions and the oxidation of Ni ions and the first cathodic peak which represented the
insertion of Li-ions and the reduction of Ni ions of the cell with pure PE separators were at 3.80 and 3.70 V
(∆E = 0.10 V), respectively. The redox peaks of the cell with Al2O3-coated separators were at 3.81 and 3.70 V
(∆E = 0.11 V). The redox peaks of the cell with NCM-crushed coated separators were at 3.84 and 3.67 V
(∆E = 0.17 V) while the redox peaks for the cell with NCM-unmilled-coated separators were at 3.88 and
3.69 V (∆E = 0.19 V). The ∆E values of Li-ion half-cells with pure PE separators were smaller than those of
Al2O3-coated and NCM-coated separators, suggesting that the coating layers did not affect the

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Figure 5. (A) Nyquist plot of NCM811/Li cells with the pure PE separator, Al2O3-coated separator, NCM-crushed coated separator, and
NCM-unmilled coated separator. (B) Cyclic voltammetry (CV) profiles of NCM811/Li half-cells with various separators. (C-E)
Charge/discharge curves of cells between the 1st and 150th cycles at 0.5 C with (C) pure PE separator, (D) PE/Al2O3 separator, and (E)
NCM-crushed coated separator, respectively. (F) The rate capability of NCM811/Li cells with various separators. (G) Cycling
performances of NCM811/Li cells with several separators in the voltage of 2.4-4.7 V at 0.5 C.

electrochemical polarization process of cathode materials. However, the strong cathodic/anodic peaks in the
cell with Al2O3- and NCM-coated separators suggest that the Li-ion and electron diffusion was faster. The
[normalized CV curves are shown in Supplementary Figure 4. The NCM-coated separators show higher](https://oaepublishstorage.blob.core.windows.net/articlepdfpreview202501/em40105-SupplementaryMaterials.pdf)
specific peak currents than the uncoated separators, indicating improved utilization of the active material;
the integrated area of the CV curves, which correlates to capacity, is larger for the NCM-coated separators
on a per-gram basis.

The charge and discharge curves of cells with different separators after the 1st and 150th cycles at 0.5 C are
displayed in Figure 5C-E. The voltage hysteresis increased during the charge and discharge process as the
cycling increased for all cells. However, the cells with bare PE separators and PE/Al2O3 separators exhibited
low discharge capacities compared to the cells with NCM-coated separators. The initial discharge capacities
at 0.5 C within 2.4-4.7 V were 166.5, 178, 219.03 and 216.32 mAh g -1 for the bare PE separator, PE/Al2O3
separator, NCM-crushed coated separator, and NCM-unmilled coated separator, respectively. After 150
cycles, the cell discharge capacities were 119.3, 134, 166.7 and 157.56 mAh g -1 for the same separators,
respectively. The cell with the NCM-crushed coated separator showed the largest discharge capacity even
after 150 cycles compared to cells with the other separators. Figure 5F shows the discharge capacities at
different C rates from 0.5 to 4.0 C, changing every five cycles. The relative capacity in this figure is
calculated as the difference between the starting discharge capacity at 0.5 C and the discharge capacity at a

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Figure 6. (A) Chronoamperometric of the Li||NCM-crushed||Li cell with a potential step of 0.01 V. (B) rate performances at 0.1, 0.2 and
0.5 mA cm-2. (C) cycle stability Li plating/stripping property with different separators at 0.5 mA cm-2.

given C-rate. The cell using the NCM-coated separator exhibited the highest discharge capacities for all the
C-rates compared to the cells using bare PE or PE/Al2O3 separators, which agreed with the highest ionic
conductivity of the NCM-coated separator. Figure 5G shows the cycling capabilities of the cells with various
separators at 0.5 C. The capacity retentions of the cell with the bare PE separator, the Al2O3-coated
separator, the NCM-crushed coated separator, and the NCM-unmilled coated separator are 71.6%, 75.3%,
76.1%, and 72.8%, respectively. The cell with an NCM-crushed coated separator exhibits the highest capacity
retention compared with the cells with other separators. This was due to the strong interaction between the
NCM-crushed layer and the ceramic Al2O3 particle layer. The performances of the cells with various
separators are summarized in Table 1. The calculation of cell capacity has included the total mass of active
material from both the cathode and the active coating on a separator. The mass loading of NCM on the
cathode ranges from 7.87 to 7.93 mg cm -2, while on the separator, it ranges from 2.77 to 2.79 mg cm -2 . This
indicates that the NCM coating on the separator adds approximately 35% more active material compared to
[the cathode alone. Supplementary Figure 5 provides charge/discharge profiles of three cells with different](https://oaepublishstorage.blob.core.windows.net/articlepdfpreview202501/em40105-SupplementaryMaterials.pdf)
configurations and illustrates that NCM811 coating on the separator participates in the electrochemical
reaction and contributes additional cell capacity. A comparative analysis of the estimated cost of the various
[separators is presented in Supplementary Table 1.](https://oaepublishstorage.blob.core.windows.net/articlepdfpreview202501/em40105-SupplementaryMaterials.pdf)

The Li-ion transference, which indicates the electrolyte's ability to Li-ion transport, was analyzed. A higher
Li-ion transference can prevent the lithium dendrite growth and increase the battery capacity and cycle
life [51,52] . As shown in Figure 6A, the cell using NCM-coated separators showed a larger tLi+ of 0.66 compared
to those using the bare PE and PE/Al2O3 separators, which had of 0.31 and 0.43, respectively. Figure 6B
shows the overpotential of the Li/Li cells with various separators at different current densities of 0.1, 0.2, and
0.5 mA/cm 2 . The overpotential increased with the current density for all cells. The Li/Li cells with bare PE

Page 10 of 13 Nitou _et al. Energy Mater._ 2025, _5_, 500018 https://dx.doi.org/10.20517/energymater.2024.105

Figure 7. Absorption energy calculation of the PE, Al2O3 and NCM811 in the separator: (A) PE and NCM(100). (B) PE and Al2O3(001).
(C) Al2O3 and NCM(100). Slices of the electron density distribution: (D) PE and NCM(100). (E) PE and Al2O3(001). (F) Al2O3 and
NCM(100). In the Figure, the gray, white, green, red, steel blue, slate blue, medium purple and pink balls represent C, H, Li, O, Ni, Co,
Mn and Al, respectively.

and PE/Al2O3 separators had similar overpotential under 300 hours at distinct current densities, while the
cells with NCM-crushed separators displayed lower overpotential at the same current densities. The cycling
performance of Li/Li symmetric cells with different separators was evaluated to assess their ability to
suppress the Li dendrite growth [Figure 6C]. The Li/Li cells with the bare PE and PE/Al2O3 separators at
0.1 mA cm -2 showed more fluctuations in voltages than the Li/Li cells using NCM-crushed coated
separators, indicating the Li dendrite growth during cycling. However, the cell with the NCM-crushed
coated separator had a stable and a small overpotential during the cycling under 400 h and also shows
cycling uniformity from 0 to 400 h than the other cells. This was because of the high ionic conductivity,
good interfacial adhesion with the anode, strong mechanical strength, and unified Li + flux by NCM-crushed
coating. These findings agree with previous research by Yang _et al._ [52] . When using Li/Li cells to test the
dendrite performance, direct contact between the NCM811 coating on the separator contact Li metal can
induce phase change or reactions. However, the results still show that NCM811 layers effectively suppress Li
dendrite growth. In actual Li/NCM half-cell or graphite/NCM full-cell configurations, the NCM coating on
the separator will face the cathode side. The Al2O3 layer and the PE base separator will separate the NCM811
coating from the anode, avoiding any side reactions or phase changes between NCM811 and Li.

DFT computations were used to study the interface interaction of the PE/Al2O3/NCM811-coated separator
and the impact of the Al2O3 and NCM811 layers. Figure 7A-C displays the calculated adsorption energies of
PE-NCM811(100) surface, PE-Al2O3(100) surface, and Al2O3-NCM811(100) surface, respectively. The
results show that PE-Al2O3 has a higher adsorption energy of -0.58 eV than PE-NCM811(-0.30 eV).
However, the adsorption energy increases significantly to -6.11 eV between NCM811 and Al2O3, indicating
a strong interfacial interaction between them. Therefore, the strong interfacial interactions of PE-Al2O3 and

Nitou _et al. Energy Mater._ 2025, _5_, 500018 https://dx.doi.org/10.20517/energymater.2024.105 Page 11 of 13

Al2O3-NCM811 confirm the high mechanical proprieties and thermal stability of the PE/Al2O3/NCM811
separator, which ensures the electrochemical proprieties of NCM811/Li cells. Figure 7D-F also shows the
strong interfacial contacts of the layers by the bonding electron cloud between atoms for each layer such as
PE-NCM811 (C-O, 3.93 Å), PE- Al2O3 (C-O, 3.57 Å), and Al2O3-NCM811 (O-O, 2.54 Å). The stronger the
binding between the atoms of Al2O3 and NCM811, the more stable their layers become, enhancing the
interfacial interactions between layers and the integrity of the pore framework of the PE/Al2O3/NCM811
separator. The DFT results were consistent with our experimental measurements.

## CONCLUSIONS

In this work, we have developed a novel separator design using NCM811 as a coating material on PE/Al2O3
separators for improving the performance and safety of LIBs with high-energy cathodes. The NCM811
coating layer was directly cast on PE/Al2O3 separators. This layer enhances wettability, thermal stability,
ionic conductivity, and Li-ion transfer number of the PE/Al2O3 separator. The NCM811|Li half-cell with
NCM811-coated separators showed higher capacity retention and better rate performance than those with
PE or PE/Al2O3 separators. The NCM811 coating layer also prevented the growth of lithium dendrites on
the anode surface during cycling, which enhanced the safety of LIBs. This work demonstrated that using
active cathode material as a coating layer on a separator was an effective strategy to improve the
performance and safety of LIBs with high-energy cathodes. This work also provided a new perspective for
designing separators with active materials for various battery systems.

## DECLARATIONS

Authors’ contributions
Investigation, data curation, formal analysis, writing - original draft: Nitou, M. V. M.
Investigation, data curation, writing - review & editing: Fang, X.; Liu, R.; Pang, Y.
Software, simulation, data curation, writing - review & editing: Wang, J.; Qin, W.
Formal analysis, writing - review & editing: Zhang, Z.
Supervision, administration, funding, validation, writing - review & editing: Niu, Y.; Zhao, C.; Chen, Y.; Lv,
W.

Availability of data and materials
The raw/processed data required to reproduce these findings cannot be shared at this time due to technical
or time limitations.

Financial support and sponsorship
This work was supported by the Natural Science Foundation of China (Grant Nos. 51972043 and 52102212),
the fellowship of China Postdoctoral Science Foundation (No. 2022M720653), the Sichuan-Hong Kong
Collaborative Research Fund (No. 2021YFH0184) and the Natural Science Foundation of Sichuan Province
(Nos. 2023NSFSC0417 and 2023NSFSC0974).

Conflict of interest
All authors declared that there are no conflicts of interest.

Ethical approval and consent to participate
Not applicable.

Consent for publication
Not applicable.

Page 12 of 13 Nitou _et al. Energy Mater._ 2025, _5_, 500018 https://dx.doi.org/10.20517/energymater.2024.105

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