Research Progresses and Development Prospects on Cathode
Materials for Lithium-Ion Batteries
Yuchen Lu
1
, Yang Zhao
2,*
and Yiduo Zhao
3
1
School of Chemical and Pharmaceutical, Wuhan Institute of Technology, Wuhan 430205, China
2
School of Materials Science and Engineering, Nanjing Tech University, Nanjing 211816, China
3
School of Material Chemistry, Xi’an Jiaotong University, Xi’an 710049, China
*
Keywords: Lithium-Ion Batteries, Cathode Materials, Modification Method.
Abstract: Fossil fuels are in short supply, and people are trying to find new energy sources to replace them. Recently
we have an increasing demand for high energy density lithium-ion batteries, especially in the field of daily
life, such as electric cars and other. The existing cathode material technology has become a limiting factor in
the discovery of lithium-ion batteries. Accordingly, it is of extraordinary significance to conduct in-depth
research on high-performance and high-energy-density cathode materials. Cathode materials at this stage have
their own characteristics. However, they are still immature in many ways like security, steadiness and inner
framework. A lot of recent research revolves around the discovery of lithium-ion battery cathode materials
with greater cycle life, higher energy density, and greater stability. Herein, the structure and mechanism of
several main cathode materials, as well as their problems in charge and discharge are summarized, and the
recent studies one improving electrochemical properties of cathode materials by modification are reviewed.
1 INTRODUCTION
As our modern science and technology continues to
advance rapidly, the immense utilization of fossil
fuels is triggering increasingly nasty climate
variability and global warming (Zhao et al,
2021).Because the development of sustainable energy
storage technology is crucial to building a low-carbon
society, lithium-ion batteries (LIBs) have drawn
rising interest (Li et al, 2022). In general, LIBs have
notable benefits like high energy densities, efficient
cycling performance, and rapid response times. Their
suitability for energy storage ranging from kilowatts
to megawatts with swift response times is
acknowledged. Furthermore, LIBs automotive supply
chain is global and has a mature infrastructure in
place, making it highly desirable among consumers.
These existing capabilities could serve as a
cornerstone for the accelerated deployment of LIBs in
grid-scale energy storage applications (Yang et al,
2022). Recently, we've noticed an increasingly
obvious problem surge in the advancement of electric
vehicles (EVs). Simultaneously, considerable
research endeavors are focused on uncovering
cathode materials for LIBs that exhibit continued
cycle longevity, elevated energy density, and
structural stability (Cai et al, 2021).
The primary commercial cathode materials
utilized in LIBs include LiCoO
2
, LiMn
2
O
4,
LiFePO
4
,
and LiNiCoMnO
2
. Among these, LiCoO
2
stands out
as one of the earliest materials extensively employed
in portable electronics owing to its elevated
operational voltage, extended cycling durability,
minimal self-discharge, and eco-friendliness.
Nonetheless, whether it can be used commercially or
not we still need to consider its disadvantages.
LiCoO
2
does present certain disadvantages, outlined
as follows. Firstly, the limited availability of cobalt
resources results in the high cost of LiCoO
2
. Secondly,
the inherent structural instability of LiCoO
2
contributes to significant capacity deficiencies.
Thirdly, cobalt is a toxic element, posing
environmental concerns. Specifically, its discharge
capacity and cycling efficiency deteriorate rapidly
when operating above 4.2 volts (Chen et al, 2021).
After discovering that LiCoO
2
could be difficult to
use commercially because of its shortcomings,
through years of research, researchers discovered
LiMn
2
O
4
.However, the cycling performance of
LiMn
2
O
4
falls short due to the Jahn-Teller effect, Mn
dissolution, and electrolyte disintegration at high
charge voltage (Li et al, 2021). Goodenough
Lu, Y., Zhao, Y. and Zhao, Y.
Research Progresses and Development Prospects on Cathode Materials for Lithium-Ion Batteries.
DOI: 10.5220/0013936600004914
Paper published under CC license (CC BY-NC-ND 4.0)
In Proceedings of the 2nd International Conference on Renewable Energy and Ecosystem (ICREE 2024), pages 325-330
ISBN: 978-989-758-776-4
Proceedings Copyright © 2025 by SCITEPRESS – Science and Technology Publications, Lda.
325

discovered a commercially available cathode material
that possesses a smooth voltage plateau, as evidenced
by high energy density, substantial power and
structural stability, and that's the LiFePO
4
.
Nevertheless, LiFePO
4
has its drawbacks, including a
relatively platforms with low charging voltage and
poor conductivity. Consequently, to achieve optimal
electrochemical performance, LiFePO
4
requires a
conductive layer coating, a process that contributes to
its lower tap density.
With the discovery of anode material, many
researchers created a novel material which was called
layered lithium nickel cobalt manganese (NCM) that
might be economically employed in LIBs (Akhilash
et al, 2023). The NCM material is really classified
like NCM111, NCM523, NCM622, NCM811 and so
on. Each metallic element has an important purpose
in the multilayer NCM, the Ni ingredient provides a
high actual capacity, while the Co element adds to
desirable cycle life. There is high structural stability
observed in NCM, attributed to the presence of the
Mn element. The electrochemical capacity of NCM
shows a positive correlation with the content of Ni
ions, as Ni ions are the main active redox material,
and NCM has recently become one of the alternatives
for commercial cathode materials.
Despite the fact that NCM exhibits several
advantages like higher reversible capacity, reduced
cost, and enhanced environmental compatibility over
the widely utilized LiCoO
2
. It also has some notable
disadvantages. For example, the durability of NCM
during cycling is insufficient to satisfy the stringent
demands for the extended lifespan of LIBs.
Furthermore, NCM demonstrates substandard
electrochemical performance under high speed
charge and discharge conditions. Besides, it performs
poorly thermally at high temperatures and the issue
will get considerably worse as the Ni concentration
rises. To address these issues, we need to continue to
attack the future. In the last several years, a lot of in-
depth research has been done by scientists on it to
solve the problems like low energy density and short
cycling life is present in the LIBS cathode materials
and achieved significant advancements in
performance. In conclusion, these issues may be
resolved in a number of methods, including surface
treatment or surface coating, ion incorporation, core-
shell architecture and improved electrolyte, and more.
Hereunder, We conclude with a summary of the
latest research advances on high-energy LIBs cathode
materials and offer some suggestions and directions
for future research. We hope that this contributes to
the ongoing research efforts in the field of LIBs.
2 CATHODE MATERIALS
2.1 LiCoO
2
LiCoO
2
stands out as one of the earliest commercially
available cathode materials for LIBs (Li et al, 2018).
Its appeal in the market stems from its simple
preparation method, high specific capacity, stable
cycling performance, and good thermal stability.
LiCoO
2
demonstrates three primary crystal structures:
layered, spinel, and rock salt phases. Of these, the
ordered α-NaFeO
2
layered structure facilitates rapid
and reversible lithium ions insertion/extraction
during production expansion, making it the most
utilized configuration, accounting for over 31% of
lithium-ion battery usage (Qian et al, 2018).
The stratified arrangement of LiCoO
2
, resembling
the α-NaFeO
2
structure, belongs to the hexagonal
crystal system, with specific lattice constants. Within
this structure, CoO
2
forms a two-dimensional atomic
layer, with oxygen atoms adopting a cubic dense
packing. Cobalt and lithium ions alternate between
octahedral positions within oxygen atoms, allowing
lithium ions to move between the atomic layers.
However, due to varying interaction forces between
ions and oxygen atoms, the oxygen atoms deviate
from an ideal cubic close-packed structure, distorting
into a hexagonal close-packed structure and reducing
lattice symmetry.
Despite the theoretical specific capacity is 274
mAhg
−1
, the actual discharge capacity equals limited
to 135~140 mAhg
−1
. This discrepancy arises from the
charge and discharge process, involving specific
reactions. During lithium ions extraction, vacancies
form in the original lattice, impacting atomic
arrangement and inducing a phase transition. Varying
levels of lithium ions
extraction generate multiple
phases, with transition states marked by changes in
lattice parameters. As lithium extraction increases,
the crystal structure shifts from hexagonal to
monoclinic, leading to local asymmetrical expansion
and contraction, ultimately compromising battery
cycling stability.
In practical charge and discharge processes, only
approximately 53% of lithium ions can reversibly
intercalate and deintercalated (Liu et al, 2020).
Increasing charging voltage enhances lithium
extraction, but excessive extraction damages cycling
stability, necessitating a voltage limit of 4.2V (vs.
Li/Li
+
). This limitation results in an actual capacity of
135~140 mAhg
−1
(Li
1−x
CoO
2
, x ≈ 0.5, ~ 4.2 V vs.
Li/Li
+
), highlighting the need to enhance cathode
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material stability under high voltage conditions (Qian
et al, 2018).
2.2 NCM
In the realm of cathode materials for batteries,
ongoing research focuses on three main structures:
one-dimensional olivine, two-dimensional layered,
and three-dimensional spinel. Among these, the NCM
cementitious materials hold a prominent position due
to their high capacity and power ratings, ideal for
high-energy density battery production.
NCM shares a similar layered structure with the
α-NaFeO
2
type, residing within the hexagonal crystal
system under space group R-3m. Here, nickel ions,
trivalent cobalt ions, and tetravalent manganese ions
occupy octahedral center positions, forming a cubic
close-packed arrangement in a layred fashion (Ko et
al, 2023). Ternary materials offer distinct advantages
over unary and binary counterparts, thanks to the
unique roles of different cations: nickel ions enhance
specific capacity, trivalent cobalt ions
reduce cation
mixing and enhances structural stability and
electronic conductivity, while tetravalent manganese
ions introduce cost-effectiveness and improves
thermal stability (Qian et al, 2018).
However, simply increasing cation content doesn't
universally enhance material performance. For
instance, heightened Co
3+
content may diminish
NCM's reversible specific capacity and inflate battery
production costs. Similarly, excessive nickel ions
content risks gasification and deliquescence during
charge and discharge, compromising thermal cycling
stability (Yan et al, 2020). Moreover, an
overabundance of tetravalent manganese ions can
introduce a spinel phase, disrupting the material's
layered structure and impairing rate performance
(Ein‐Eli et al, 1998).
Furthermore, NCM's morphology significantly
influences battery volumetric energy density. While
traditional lithium cobalt oxide boasts a theoretical
density of 3.9 g/cm
3
, NCM materials hover around
3.6 g/cm
3
(Wang et al, 2020). To elevate volumetric
energy density and voltage platform, tailored
morphological modifications are essential to align
with user demands.
2.3 LiFePO
4
LiFePO
4
boasts a typical olivine structure
characterized by robust covalent bonds between
phosphorus and oxygen, imparting exceptional
strength, high-temperature resistance, and chemical
stability. Its three-dimensional olivine structure
fosters a one-dimensional channel for lithium ions
transport, effectively constraining ion diffusion. In
contrast to ternary lithium batteries, LiFePO
4
batteries exhibit superior structural stability and
enhanced safety.
The operational principle of LiFePO
4
batteries
hinges on the relocation of lithium ions across the
electrodes of a cell to facilitate charging and
discharging (Su, 2022). During charging, lithium ions
disintercalate from the anode material (LiFePO
4
) and
intercalate into the cathode material (typically
graphite) via the electrolyte, enabling reversible
multi-cycle charge-discharge capability. The charging
process involves the positive electrode compound
LiFePO
4
, where lithium ions disintercalate to form
FePO
4
, liberating electrons. The negative electrode,
graphite, demonstrates efficient lithium ions insertion
and extraction, with lithium ions migrating into the
graphite from the electrolyte while concurrently
releasing electrons. Organic solvents containing
lithium salts, like LiPF
6
, function as electrolytes,
facilitating lithium ion transport (Apachitei et al,
2023).
LiFePO
4
batteries offer higher energy density,
translating to extended range. Compared to other
lithium-ion variants, they exhibit prolonged lifespan
and increased charge-discharge cycle endurance.
Additionally, they demonstrate robust stability,
minimizing risks of overheating, combustion, and
related safety concerns. Environmentally, LiFePO
4
batteries are advantageous as they lack heavy metals
and harmful substances. However, they exhibit
relatively slower charging rates and necessitate
longer charging durations (Su, 2022). The relatively
intricate manufacturing processes contribute to
higher prices.
2.4 LiMn
2
O
4
The crystal structure of lithium manganese oxide
comprises monoclinic and orthorhombic phases. The
monoclinic phase, akin to LiCoO
2
but with lower
symmetry, contrasts with the more stable
orthorhombic phase. Despite its inherent stability,
lithium manganese oxide is susceptible to Jahn-Teller
distortion, rendering it thermodynamically unstable.
Cycling induces a transformation to the more stable
spinel structure LiMn
2
O
4
, causing a notable reduction
in reversible capacity.
In the charge-discharge cycle of lithium
manganese oxide batteries, manganese ions undergo
oxidation-reduction reactions. Charging oxidizes
Mn
+
to Mn
4+
, liberating lithium ions, while
discharging reduces Mn
+
to Mn
3+
, re-embedding
Research Progresses and Development Prospects on Cathode Materials for Lithium-Ion Batteries
327

lithium ions into the lattice. This redox reaction is
pivotal to the battery's operation. Lithium ions shuttle
between electrodes, embedding into and extracting
from the crystal structure. This process forms the core
of the battery's charge-discharge mechanism (Li et al,
2021).
The spinel structure of lithium manganese oxide
exhibits robust stability, enduring the embedding and
extraction of lithium ions, thus contributing to cycling
stability and longevity. Abundant resources, low
production costs, and mature manufacturing
processes make lithium manganese oxide suitable for
practical applications. It offers higher specific
capacity and energy density, alongside good safety
and environmental attributes. However, its cycling
stability is compromised by structural changes and
dissolution, curtailing battery lifespan (Li et al, 2021).
Jahn-Teller distortion, particle aggregation, and
surface reactions further impact its electrochemical
performance.
2.5 LiNiO
2
Lithium nickel oxide adopts a layered crystal
structure, featuring both rock salt and α-NaFeO
2
configurations. Within this structure, nickel ions and
lithium ions coexist. The integration of nickel ions
into the lithium layers introduces additional
complexity to the crystal lattice. Moreover, the
phenomenon of non-stoichiometry arises due to high-
temperature calcination, resulting in lithium loss from
the crystal structure and deviating from strict
stoichiometry.
Irreversible phase transitions occur in lithium
nickel oxide, leading to the formation of an inactive
NiO
2
phase upon charging to higher voltages, which
in turn contributes to capacity decay. The distinctive
characteristics of lithium nickel oxide, namely its
layered structure and non-stoichiometric nature,
significantly influence its electrochemical
performance and cycling lifespan (Kalyani &
Kalaiselvi, 2005).
During charge and discharge, trivalent nickel ions
undergo oxidation to tetravalent nickel ions. However,
migration of some nickel ions to lithium sites within
the structure compromises cycling lifespan. Lithium
nickel oxide exists in two structural forms: cubic and
layered hexagonal phases, with only the latter
exhibiting electrochemical activity (Kalyani &
Kalaiselvi, 2005). Cycling induces phase transitions,
such as the conversion from hexagonal to monoclinic
phases, altering the crystal structure and impacting
electrochemical performance.
The conductivity of lithium nickel oxide is closely
tied to the positioning of nickel ions within the crystal
lattice. Migration of nickel ions disrupts electron
conduction paths between nickel ions, reducing
conductivity. Additionally, changes in nickel ion
positions affect ion diffusion rates, further
influencing charge and discharge performance.
With a maximum specific energy density of 160
mA/g, LiNiO
2
surpasses other cathode materials
(Kalyani & Kalaiselvi, 2005). It demonstrates
minimal capacity decay during cycling, boasting an
excellent cycling lifespan. LiNiO
2
can withstand deep
discharge conditions below 2 V, maximizing energy
storage capacity. However, its phase transition
process is only partially reversible and slower
compared to LiCoO
2
, necessitating optimization of
synthesis conditions to mitigate these challenges.
3 MODIFICATION METHODS
FOR CATHODE ELECTRODE
Current research on cathode electrode materials
primarily focuses on doping modification and surface
coating of high-nickel ternary and lithium-rich
cathode electrode materials, as well as their structural
evolution during extended cycling.
3.1 Surface Modification
Many experts are looking for the ways of surface
coating to improve performance. For the modification
of surface coatings nowadays, in order to enhance
their corrosion resistance, electrical conductivity,
abrasion resistance and structural optimisation, the
main methods are the selection of coating materials
with excellent properties, such as polymers, ceramics
and metal oxides. Or to carry out coating design to
design coatings with optimised structure and
thickness. Or proper cleaning, roughening or
functionalisation of the cell surface before applying
the coating to enhance the adhesion of the coating. We
have also summarised some studies as follows.For
example, Tan et al. utilized ZrTiO (ZTO) as an
epitaxial layer to enhance the mechanical stability of
ultra-high nickel LiNi
0.8
Co
0.1
Mn
0.1
O
2
(NCM90).
Structural characterization and multi-field analysis
revealed that the congruent ZTO layer and Zr doping
effectively suppressed internal strain and lattice
oxygen release, inhibiting local stress accumulation
during cycling. The protective ZTO layer also
prevented electrolyte erosion, preserving the intact
surface structure of NCM90. NCM90 exhibited
improved cycling Voltage endurance (4.5 V),
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possessing a capacity retention rate of 71% after 100
cycles. Also, Wu et al. proposed a powder coating
method, exemplified by coating a nickel cathode with
Al(OH)
3
nanoparticles, to illustrate the chemical
changes on the cathode surface with varying coating
levels. This coated cathode exhibited improved
cycling stability and rate capability, attributed to
effective surface protection against side reactions and
enhanced lithium ions transport. Furthermore,
environmental and thermal stability were enhanced.
3.2 Doping Modification
There are also experts who work on improving
material properties through doping modification.
Zhang et al. addressed irreversible phase transitions
and cracking issues in LiNiO
2
-based cathode
electrodes by doping single crystal
LiNi
0.83
Co
0.07
Mn
0.1
O
2
(SNCM) with tungsten boride
(WB). Through microscopy and spectroscopic
evidence, they demonstrated that Trivalent boron ions
entering the SNCM matrix expanded the interlayer
spacing, facilitating lithium ions diffusion, while W
3+
formed a non-crystalline surface layer composed of
Li
x
W
y
O
z
(LWO) and Li
x
B
y
O
z
(LBO), contributing to
the creation of a robust cathode electrolyte interphase
(CEI) membrane structure. WB doping effectively
controlled c-axis contraction and oxygen gas release
at high voltages, with an optimal doping
concentration of 0.6 wt.% resulting in 93.2% capacity
endurance after 200 cycles at 2.7-4.3 V. Also, Fan et
al. introduced a method to substituteTransition-
element cations in LiNi
0.83
Co
0.11
Mn
0.06
O
2
with Mo-
NCM, investigating the preparation structure
evolution due to Mo substitute and the constancy of
the Mo-NCM positive electrode. Experimental and
computational results revealed that partial
substitution with hexavalent molybdenum ions
induced cation ordering and facilitated lithium ions
diffusion kinetics, with pentavalent molybdenum ions
cations acting as pillars to avoid local failure and
structural distortion. Strong Mo-O bonds stabilized
lattice oxygen, enhancing the chemical durability of
the nickel-rich positive electrode. Besides, Huang et
al. proposed a TSS together with the addition of
crystallization modifiers, including phase generation,
grain enlargement, and phase retention. MoO
3
addition inhibited grain enlargement and cluster
formation, leading to highly dispersed Mo surface-
doped single crystal NCM cubes (MSC-NCM) with
an mean particle count diameter of 1.3 μm. Lithium
ions migration preferred the (104) crystal plane in
MSC-NCM cubes due to surface molybdenum
doping and reduced surface energy, resulting in
significantly improved rate performance compared to
conventional single crystal NCM materials (SC-
NCM). Furthermore, Li et al. introduced a method
involving ammonium niobium oxalate treatment to
create oxygen vacancies and pentavalent niobium
ions doping on cobalt-free lithium-rich layered oxide
(LRO) materials. The modified sample, LRO-Nb-0.5,
exhibited exceptional electrochemical capability,
providing a discharge capacity per unit mass of
209.77 mAh/g at 1C, with a capacity retention rate of
93.22% after 300 cycles. Moreover, LRO-Nb-0.5
demonstrated enhanced rate performance, achieving
a discharge specific capacity of 178.70 mAh/g at 5 C.
Pentavalent niobium ions doping and oxygen vacancy
regulation emerged as crucial approaches to
enhancing performance metrics of cobalt-free
lithium-rich cathode materials in electrochemical
applications.
3.3 Structure Modification
There are many experts who have changed the
structure to achieve this in order to improve its
performance, and the results show that it is indeed a
feasible method. For example, Tan et al. integrated a
tenon-mortise structure into the layered phase of
LiNi
0.8
Co
0.1
Mn
0.1
O
2
(NCM811), mitigating volume
changes and facilitating lithium ions transport. The
discharge capacity reached 215 mAh/g at 0.1 C with
an initial Coulombic efficiency of 97.5%. After 1200
cycles at 1 C, the retention of capacity rate was 82.2%.
Also Shi et al. investigated the degradation process of
single-crystal high-nickel cathode material (SCNCM)
during room temperature storage. Exposure to air led
to a changing from a layered to a NiO rock salt phase,
resulting in decreased electrochemical performance
due to oxygen precipitation and the formation of
oxygen vacancies. Besides, Zhao et al. studied quasi-
single-crystal LiNi
0.65
Co
0.15
Mn
0.20
O
2
(SC-NCM65)
and found that maintaining a cutoff voltage of 4.6 V
preserved over 77% capacity retention after 400
cycles, while at 4.7 V, capacity dropped to 56%. SC-
NCM65 degradation was primarily due to rock salt
phase accumulation on particle surfaces, increasing
impedance and transition metal dissolution. The
thickness of the rock salt layer exhibited a linear
relationship with capacity loss, indicating charge
transfer kinetics as a crucial factor hindered by lower
lithium ions diffusion in the NiO phase. Additionally,
Li et al. introduced a method involving ammonium
niobium oxalate treatment to create oxygen vacancies
and pentavalent niobium ions doping on cobalt-free
lithium-rich layered oxide (LRO) materials. The
modified sample, LRO-Nb-0.5, exhibited exceptional
Research Progresses and Development Prospects on Cathode Materials for Lithium-Ion Batteries
329

electrochemical capability, delivering a discharge
specific capacity of 209.77 mAh/g at 1C, with a
capacity retention rate of 93.22% after 300 cycles.
Moreover, LRO-Nb-0.5 demonstrated enhanced rate
capacity, achieving a discharge specific performance
of 178.70 mAh/g at 5 C. Pentavalent niobium ions
doping and oxygen vacancy regulation emerged as
crucial approaches to enhancing the capacity of
cobalt-free lithium-rich cathode materials in terms of
electrical and chemical characteristics.
4 CONCLUSION AND OUTLOOK
Among these batteries, LIBs have relatively high
energy density and high charge/discharge efficiency,
but they cannot withstand high temperatures. The
lithium iron phosphate battery can make the cathode
structure more stable, which makes its cycle life
longer than other kinds of batteries, and has a lower
cost. However, the energy density and
charge/discharge efficiency of lithium iron phosphate
batteries are low, and their performance is poor at low
temperatures. In order to improve the shortcomings
of these batteries, we have also searched and
summarised some modification methods such as
surface modification treatment, ionic doping,
improved electrolyte and so on. However, the existing
methods can't solve all the battery problems well, and
we still need to carry out in-depth research on safety
issues and internal structure of batteries in the future.
And for the existing problems, we summarise
some directions for research to solve them.
Regardless of whether the energy density of NCM has
been developed to the upper limit or not, it is obvious
that it cannot meet the further development needs of
battery energy storage, so we need to find ways to
develop new cathode materials with high Ni content.
In this process, how to replace the Co element, how
to control the cost, and how to save the limited
resources of the earth are also huge challenges for us.
In addition, for some of the modification methods we
are now researching and developing, although there
is some improvement in electrochemical performance,
the cost is difficult to control, and the industrial
process is difficult to achieve commercially.
Therefore, we can put more effort into new types of
batteries, such as lithium-sulfur batteries and solid-
state batteries, compared with traditional lithium-ion
batteries. In conclusion, a simple and feasible
modification scheme is crucial in developing high
energy density batteries in the future. However, I
believe that with the development of technology and
further research on batteries, we will eventually solve
these problems well.
AUTHORS CONTRIBUTION
All the authors contributed equally and their names
were listed in alphabetical order.
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