Renewable and Sustainable Energy Reviews 131 (2020) 110048

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Renewable and Sustainable Energy Reviews

journal homepage: http://www.elsevier.com/locate/rser

Lithium-ion battery aging mechanisms and diagnosis method for

automotive applications: Recent advances and perspectives
Rui Xiong a, *, Yue Pan a, Weixiang Shen b, Hailong Li c, Fengchun Sun a
a
National Engineering Laboratory for Electric Vehicles, School of Mechanical Engineering, Beijing Institute of Technology, Beijing, 100081, China
b
Faculty of Science, Engineering and Technology, Swinburne University of Technology, Hawthorn, Victoria, 3122, Australia
c
School of Business, Society and Engineering, M€
alardalen University, SE, 72123, V€asterås, Sweden

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

Keywords: Lithium-ion batteries decay every time as it is used. Aging-induced degradation is unlikely to be eliminated. The
Lithium-ion battery aging mechanisms of lithium-ion batteries are manifold and complicated which are strongly linked to many
Intelligent battery management systems interactive factors, such as battery types, electrochemical reaction stages, and operating conditions. In this paper,
Aging mechanism
we systematically summarize mechanisms and diagnosis of lithium-ion battery aging. Regarding the aging
Diagnosis
Accelerated aging tests
mechanism, effects of different internal side reactions on lithium-ion battery degradation are discussed based on
the anode, cathode, and other battery structures. The influence of different external factors on the aging
mechanism is explained, in which temperature can exert the greatest impact compared to other external factors.
As for aging diagnosis, three widely-used methods are discussed: disassembly-based post-mortem analysis, curve-
based analysis, and model-based analysis. Generally, the post-mortem analysis is employed for cross-validation
while the curve-based analysis and the model-based analysis provide quantitative analysis. The challenges in the
use of quantitative diagnosis and on-board diagnosis on battery aging are also discussed, based on which insights
are provided for developing online battery aging diagnosis and battery health management in the next gener­
ation of intelligent battery management systems (BMSs).

1. Introduction
With the growing concerns about using clean and renewable re­
sources, batteries are attracting a huge amount of attention due to the
ability to store intermittent energy. Batteries, which convert chemical
energy into electrical energy through electrochemical reactions, are
widely utilized to store energy in various applications, like electronic
mobile equipment, aerospace aviation, road transportation, power grid,
and national defense industry [1–3]. As an energy supplier, batteries are
the heart of electric vehicles (EVs). Among all commercially-available
battery types, a lithium-ion battery has stood out with tremendous ad­
vantages, such as high working voltage, high specific energy, and long
cycle life [4–10]. Receiving extensive attention from manufacturers and
researchers, it has achieved market dominance in a wide range of EVs.
For better utilization of lithium-ion batteries, increasingly special
and high requirements have been placed on battery management system
(BMS), especially in terms of all-climate, all-electricity ranges, full-
lifetime and high accuracy battery state estimation like the state of
charge (SOC) ,state of health (SOH), fault and safety status . However,
the aging-induced degradation in battery capacity and power is inevi­
table over the use of lithium-ion batteries, which reduces EV driving
range and service life, and even gives rise to some safety hazards [11,
12]. The limited external characteristic parameters of batteries collected
by BMSs make it hard to obtain clear battery aging status. It is necessary
to study battery aging mechanisms for the establishment of a connection
between the degradation of battery external characteristics (i.e. terminal
voltage or discharging power) and internal side reactions, in order to
provide reliable solutions to predict remaining useful life (RUL), esti­
mate SOH and guarantees safe EV operations.
Over the years, researchers have made great efforts to study complex
physical and chemical reactions inside lithium-ion batteries. With the
advent of more accurate electrochemical analysis equipment, the aging
of different structures within batteries has been better understood.
Doron mainly focused on the side reactions at the electrode/electrolyte
interface [13]. The dissolution, migration, and deposition of transition
metal cathode were elaborated in Ref. [14]. Based on previous studies,

* Corresponding author. Dept. of Vehicle Engineering, School of Mechanical Engineering, Beijing Institute of Technology, No. 5 South Zhongguancun Street,
Haidian District, Beijing, 100081, China.
E-mail address: rxiong@bit.edu.cn (R. Xiong).

https://doi.org/10.1016/j.rser.2020.110048
Received 18 February 2020; Received in revised form 12 June 2020; Accepted 27 June 2020
Available online 15 July 2020
1364-0321/© 2020 Elsevier Ltd. All rights reserved.
R. Xiong et al.
this paper systematically expounds on the possible side reactions inside
different types of batteries during battery storage and cycling. Further­
more, the battery aging mechanism varies with different external fac­
tors. Thus the evolution of the dominant aging mechanism under
different external factors is specifically discussed in this paper to provide
a theoretical basis for a better design of accelerated aging tests, which is
a prominent work.
Given that battery performance degradation originates from several
various internal side reactions and their interactions that are susceptible
to external factors such as temperature and charge-discharge rate, it is
also necessary to study the diagnosis methods of aging. The diagnosis
methods can be divided into destructive in situ and non-destructive ex-
situ analysis. In the recent review work, the implementation and com­
parison of different diagnosis methods were reviewed, but the in situ
analysis was not included [15]. This paper discusses three diagnosis
methods including disassembly-based post-mortem analysis,
curve-based analysis, and model-based analysis. The operational pro­
cedure of each post-mortem method has been established which could
be selected with demands. The latest progress and challenges of diag­
nosis methods in quantitative analysis and on-board applications have
also been elaborated, providing important insights regarding the
improvement of diagnosis methods.
In addition to the diagnosis of battery aging, the aging prognosis is
also of great importance. It predicts the dominant aging mechanism in
the next aging stage based on the current diagnosis results, which is a
meaningful work in terms of battery echelon utilization and safety
management. At present, the main concern lies in the battery health
prognosis, focusing on battery SOH estimation and RUL prediction.
According to Hu et al. [16], current RUL prediction methods can be
divided into model-based, data-driven, and hybrid methods. These
methods vary in terms of computational complexity, model accuracy,
and requirements for electrochemical knowledge. The data-driven
model incorporating electrochemical mechanisms is considered to be a
promising RUL prognosis technology. Mejdoubi et al. [17] innovatively
use the battery aging conditions (temperature and voltage) as inputs to
the prognostic model. The battery RUL is predicted by obtaining the
Fig. 1. Framework for systematic review of battery aging mechanism and diagnosis.
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Renewable and Sustainable Energy Reviews 131 (2020) 110048
posterior values of aging indicators such as capacity and internal resis­
tance based on the Rao-Blackwellization particle filter.
This paper elaborates on battery aging mechanisms, aging diagnosis
methods and its further applications. The other sections are arranged as
follows: Section 2 explains aging mechanisms due to basic side reactions
at the cathode, anode, and other parts inside batteries. Section 3 dis­
cusses the impact of different external factors on the inside aging re­
actions based on accelerated aging tests. Section 4 introduces the
implementation of aging diagnosis methods and summarizes the prog­
ress and challenges in quantitative analysis and on-board applications of
aging diagnosis. A comparison of the above diagnosis methods is made
and the prospects for future development directions are proposed in
Section 5. Conclusions are given in Section 6. The framework of this
paper and the relationship between each section are demonstrated in
Fig. 1.
2. Aging mechanisms of lithium-ion batteries
A lithium-ion battery mainly consists of a carbonaceous anode, a
metal oxide cathode, a lithium salt electrolyte, and a separator that only
allows lithium ions to pass through. The entire life of a battery includes
cycle life and calendar life. In the cycle process, there are inevitable side
reactions (also called aging reactions) other than the main reactions
inside a battery, which lead to a decrease in battery power and capacity
and an increase in internal resistance as the number of cycles increases.
It is commonly accepted that 80% of the rated capacity marks the end of
battery life in EVs [18]. Fig. 2 outlines internal physical and chemical
reactions and external characteristics influenced by aging from the
perspectives of anode, cathode, and other parts of the battery (inactive
materials). For a more convenient understanding, we divide those
physical and chemical reactions into two main aging modes, the loss of
lithium inventory (LLI) and the loss of active material (LAM).
It can be seen that battery aging is mainly caused by the formation of
solid electrolyte interphase (SEI) film at the electrode/electrolyte sur­
face, lithium deposition, electrode structure destruction, a phase change
of electrode material, dissolution of active material and electrolyte
R. Xiong et al.
Fig. 2. Overview of basic physical and chemical reactions inside a battery.
decomposition. Most of the internal aging reactions happen at the anode
and cathode. However, there are large differences in reaction types and
their influence on capacity loss. For example, although the reactions on
inactive materials such as fluid collectors, binders, and separators are
indispensable, they have less influence on battery aging compared to
electrolyte and active materials of anode and cathode. In the battery
storage process, there are two types of capacity loss. One is the reversible
capacity decrease due to self-discharge, and the other is the irreversible
capacity loss caused by changes in battery storage conditions (e.g.
temperature, battery SOC before storage, and battery storage time).
Aging in the battery storage process is also important since 95% of
battery life is in the storage condition, like parking [19].
2.1. Reactions at the carbonaceous anode
Changes of the passive film, deposition of metal lithium, and atten­
uation of active materials are the common aging reactions at the
carbonaceous anode.
At the electrode/electrolyte interface, the change of the passive film,
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Renewable and Sustainable Energy Reviews 131 (2020) 110048
which is often called SEI film throughout the aging process, can be seen
as a cyclic process of formation, growth, decomposition, and regrowth of
SEI film. It causes not only the loss of active lithium ions but also the rise
of anode/electrolyte surface diffusion resistance. The first formation of
SEI film can be mainly attributed to the reduced electrolyte on the anode
surface when the battery was first charged [20]. This process probably
consumes 10% of active lithium ions and challenges the design of a
proper anode/cathode capacity ratio for a battery. The onset electrolyte
potential of SEI formation is not fixed, which is closely related to the
composition of the electrolyte and the content of additives inside the
battery. For different batteries, it is observed to be 0.8 V [21], 1 V [22],
1.7 V [23], and 2 V [24] vs. Li/Liþ. The formation of SEI film is a set of
reactions involving multiple components in the electrolyte, and these
reactions compete or promote each other [25]. This leads to the
complicated and controversial composition of the SEI film. The SEI film
is roughly composed of the salt degradation products (inorganic com­
ponents) and the partial or total reduction products of electrolyte sol­
vent (organic components) [26]. The composition, compactness, and
stability of the SEI film are greatly affected by the components of
R. Xiong et al.
electrolyte and electrode, and external factors like current and temper­
ature also play a role. Therefore, it is vital to improve the performance
and stability of SEI film [27] using suitable electrolyte additives and
anode surface modification. This would postpone battery aging process
and prolong battery life.
The deposition of metal lithium at the anode is generally prone to
extreme conditions such as charging at high rates and overcharging
[28]. The anodic reactions during different charging processes are
depicted in Fig. 3 [29]. It can be seen that lithium deposition rarely
occurs under normal charging conditions. When it comes to (c) and (d),
lithium-ion enrichment can be observed at the anode/electrolyte inter­
face since the solubility of lithium ions in the liquid phase (in the elec­
trolyte) outnumbers that in the solid phase (in the graphite anode).
When the solubility of lithium ions overflows, the deposition of metal
lithium is observed, causing the loss of active lithium ions. The depos­
ited lithium can bring a variety of negative effects. First of all, the anode
can be plated with lithium which increases the anode polarization and
hinders the performance of anode. Moreover, the lithium plated on the
electrode would react with the nearby electrolyte to generate various
side reaction products. Besides, partial lithium ions fail to work because
they have turned to metal sinking in the electrolyte. This may cause
short circuits inside a battery if lithium dendrites appear in the elec­
trolyte, triggering serious safety issues [30]. This also explains why
overcharging is strictly prohibited in practical applications.
The attenuation of active materials includes the mechanical failure of
graphite particles and the change of crystal structure. The mechanical
failure is attributed to the mechanical stress during lithium insertion and
delithiation and the gas (e.g. CO, H2, C2H4) escaping from anode
reduction reactions. It is generally believed that the failure of mechan­
ical structure exerts a great impact on battery degradation. The lithium
insertion and delithiation process is always accompanied by the volume
change of active materials. The expansion of graphite layers can cause
cracks in the SEI film, where part of the active material contacts the
electrolyte to generate a new SEI film. It consumes the active material,
leading to an irreversible capacity loss. Besides, the evolution of gas can
cause the stripping and cracking of graphite. In this case, the contact loss
between graphite particles increases, which increases resistance. The
structural changes in the graphite crystal are observed between the form
of hexagonal and rhombohedral structures [31–33]. It is believed that
the increase of the hexagonal structure would reduce the reversible
Fig. 3. Anodic reactions during different charging processes: (a) initial battery SOC (50%); (b) charged to 100% SOC at a normal rate; (c) charged at a high rate; (d)
overcharged.
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Renewable and Sustainable Energy Reviews 131 (2020) 110048
capacity owing to the reduced Faradaic efficiency of the lithium
insertion.
2.2. Reactions at the metal oxide cathode
For metal oxide cathodes, the main problems related to battery aging
are electrode material dissolution, electrode structure destruction, and
phase transition. The dissolution of cathode materials contributes the
most to the decline of battery cycle life since it is often accompanied by
the migration of the dissolved products and the deposition at the anode.
Thus, the dissolution can exacerbate the decomposition of electrolyte,
resulting in continuous growth of the passive film in the cathode/elec­
trolyte interface. The degree of electrode material dissolution varies
with different types of electrode materials [34]. Generally, the dissolu­
tion of Mn-based cathode is considered as the most intense [35–37]
compared with the relatively slight dissolution of Ni-based cathode [14,
38,39]. Vetter et al. [35] showed two aging mechanisms for the
Mn-based cathode which are the disproportionation of Mn at low po­
tential and the dissolution of Mn affected by Hþ with the coproduct of
LiF at medium and high potential.
Similar to the anode, the passive film, which is also called cathode
electrolyte interface (CEI) film, can appear with the oxidation of elec­
trolyte and the decomposition of LiPF6 during the first and subsequent
charging. The possible composition of CEI includes ROCO2Li (a product
of a nucleophilic reaction between LixMOy and an alkyl carbonate
molecule), polycarbonate (a product from an acidic component of a
polymerization solution or the positively charged cathode), and LiF (a
product of an acid-base reaction between LixMOy and HF) [40]. The CEI
film is usually thinner than SEI film and doesn’t fully cover the cathode
surface. As the number of battery cycles increases, the CEI film grows at
the cathode/electrolyte interface, which increases the interface resis­
tance and deepens the cathode polarization. As a consequence, it can
affect battery reversible capacity and its rate capacity [41,42].
The structural destruction of the cathode material includes cation
mixing and lithium vacancies. Since some transition metal ions (Ni2þ,
Mn3þ, Fe2þ) and lithium ions are close in radius, the cation mixing
usually occurs at the transition metal cathode. It can not only reduce
battery capacity due to the inability of some lithium ions to intercalate
but also expand the interlayer spacing of the transition metal layer,
thereby hindering the diffusion of lithium ions and increasing the
R. Xiong et al. Renewable and Sustainable Energy Reviews 131 (2020) 110048

battery polarization. For LiCoO2 cathodes, lithium vacancies would
occur due to the smaller radius of Co2þ, which brings about structural
instability [43].
There may be irreversible phase transitions of the cathode material
as the battery aging deepens. Some phase transitions could generate
great mechanical stress, leading to irreversible capacity degradation.
The Ni-based cathode would experience an enhanced degree of phase
transition between monoclinic and hexagonal and an increased disorder
of lithium-nickel compounds, reducing the structural stability [35]. As
for the Mn-based cathode, it is the formation of superstructures and
double hexagonal structures that make up of the major phase transitions
[44]. The excessive embedding of lithium ions at low potentials is
responsible for Jahn-Teller distortion, which increases the difficulty of
lithium insertion [45].
2.3. Reactions at other parts of a battery and battery storage aging
Reactions at other parts of a battery mainly occur on the inactive
materials such as current collectors, separators, conductive agents, and
binders. The binders and current collectors are likely to be corroded
when using batteries, resulting in a resistance increase and contact loss
between active materials [46]. The separator serves as a channel for
ions, and its porosity change affects the ion through-rate and thus bat­
tery capacity [33]. Vetter et al. [35] attributed the aging reactions on the
inactive materials to the volume change of active materials, leading to
four kinds of contact loss. These kinds of contact loss exist in the graphite
particles and the pairwise combination of the current collector, the
binder, and the graphite, which have a close relationship with the rise of
battery resistance.
Battery storage can also reduce battery capacity due to its self-
discharge [47,48], and some of the reduced capacity can be recovered
through battery charging. Battery self-discharge can be caused by many
factors, such as internal or external electron leakage, electrolyte leakage,
electrode/electrolyte reactions, partial dissolution of active material,
electrode passivation, and mechanical decomposition [49]. Among
those factors, the loss of active lithium ions, which is manifested by the
growth of passive film at the electrode/electrolyte interface, dominates
performance degradation during battery storage [19,50]. It is pointed
3.1. Temperature
As shown in many accelerated aging tests, environment temperature
accounts for the greatest impact on battery capacity degradation
[54–56]. And the dominant aging mechanisms are different at high and
low temperatures [54,57]. Table 1 elaborates on the aging mechanisms
at different temperatures. When it is above 25 � C, the aging rate in­
creases with rising temperature. When it is below 25 � C, the aging rate
increases as the temperature decreases [57].
For the temperatures less than 25 � C, the irreversible consumption of
active lithium ions caused by lithium plating at the anode is a major
concern. Low temperature can hinder the intercalation dynamics of
lithium ions, making lithium plating more competitive [59]. It is pro­
posed that lithium plating at low temperatures has a terrible influence
on battery safety [58].
For the temperatures above 25 � C, the thickening of SEI film and
degradation of the cathode are the dominant reactions of battery aging
[57]. The capacity degradation rate caused by cathode degradation at
45 � C is 10 times that of 25 � C [54]. High temperature causes the brit­
tleness of SEI film, exhibiting high-density defects due to the film
modification and by-product formation such as gas despite the positive
effect on the film growth [55]. This characteristic leads to the degra­
dation of anode performance. Moreover, the disappearance of carbonate
components in SEI film and the failure of some inactive materials (e.g.
binder) have been observed at extremely high temperatures [60]. This is
attributed to the large resistance increase and the deteriorated condition
for lithium-ion migration.
Table 1
Observation and mechanisms at various temperatures.
Temperature Experimental Observation Mechanisms Ref
conditions
Low T LixNi1/3Mn1/ Cycle life at 10 Severe [58]
3Co1/3O2/ C: 33 times mechanical
�

LiyMn2O4 More deformation of

out by Kassema et al. [51] that the reconfiguration of SEI film at the 18650 pronounced self- the anode
graphite anode stored at a potential of 3 V is mainly driven by partial battery@-10 heating Reaction
dissolution and secondary reaction with the electrolyte. In addition, the �
C between
internal aging reactions vary with battery storage conditions and elec­ deposited lithium
and electrolyte
trode materials [50–53]. Both temperature and storage SOC could
LFP 26650 An increase in Self- [59]
deteriorate the capacity degradation of lithium iron phosphate (LFP) battery@-22 the capacity suppressing
battery during storage, and the impact of temperature is greater [51]. �
C degradation rate lithium plating
The temperature mainly causes LLI at the anode, while the electrode followed by a
decrease
structure is hardly degraded. Also, the battery internal resistance in­
Mid T LiCoO2/ Cycle life at 45 25 � C/35 � C: [54]
creases with storage time. As for the Mn-based cathode, the dissolution MCMB �
C (84 times) is 1/ polarization
of LiMn2O4 would occur driven by Hþ when the temperature exceeds 65 battery@25 4 what it is at 25 effect, irreversible
�
C [52]. The migrated Mn2þ deposits at the anode in the form of Mn or �
C/35 � C/45 �
C (332 times) loss of active
MnO2, increasing the battery resistance.
�
C Different lithium ions (SEI)
capacity 45 � C: cathode
degradation rates degradation
3. External factors affecting aging at 45 � C
Nickel-cobalt- Consistent Increased [56]
To study battery aging mechanisms, a great deal of time (i.e. thou­ manganese change of ohmic lithium plating
sands of cycles) and experimental resources are required to conduct (NCM) pouch resistance Thickened SEI
cell@ room Increasing film
aging tests before battery failure. Thus, it is necessary to expedite aging temperature/ polarization Obvious
tests. It is observed that the aging rate and RUL of batteries vary 45 � C/C45 � C resistance under cathode
significantly under different external factors, which provides the possi­ &D65 � C C45 � C &D65 � C degradation
bility to accelerate battery aging tests. The external factors to be dis­ High T NCM Significant Degradation [60]
battery@60 resistance and failure of the
cussed in this section include temperature, charge-discharge rate, and �
C/85 � C/120 increase at 120 � C binder
depth of discharge. By revealing their effects on battery aging mecha­ �
C Disappearance Compositional
nisms, we hope to provide a litter inspiration for the design of acceler­ of carbonate change of SEI
ated aging tests and the postponement of battery aging. components in SEI
film

C45 � C &D65 � C: charged at 45 � C and discharged at 65 � C.

5
R. Xiong et al. Renewable and Sustainable Energy Reviews 131 (2020) 110048

3.2. Charge-discharge rate Table 3

Aging mechanisms of different batteries under different DOD.
The increasing charge-discharge rate is effective for accelerating Experiment Conclusions Mechanisms Ref
battery aging. Table 2 lists the effects of different current rates (C rates) factors
on battery aging. NCA battery: Narrow-band DOD suppresses Micro cracks on [67]
As the C rate increases, lithium plating and deposition occur on the DOD the adverse influence of high the cathode
anode surface, accompanied by structure attenuation. The charge- Temperature temperatures on battery capacity
discharge rates would affect the time when the battery capacity reten­ degradation
LFP battery: Aging effect at C/2: Loss of active [68]
tion curve reaches the inflection point. Smaller charge rate and larger DOD Temperature > DOD lithium ions
discharge rate can retards the emergence of the inflection point. Because Temperature Cycle time > DOD Cathode
a small charge rate tends to decrease the over-potential and inhibit Discharge degradation
lithium plating, and a large discharge rate helps to avoid severe deli­ rate
Cycle time
thiation of the anode [66].
NCM battery: Aging effect: power > cycle High power: [69]
It is found that the effective capacity of the anode is the limitation of DOD time > DOD > average SOC Formation of
battery performance at high C rates [61]. On the contrary, the cathode is Temperature High power: resistance lithium dendrite
less sensitive to high C rates, and even reaches an excellent status with Power decrease Micro short
the best reversible capacity and rate ability at 3C, which can guide fast Average SOC circuits
Removal of
charging. Researchers can concentrate on improving the anode capacity resistive layers
to reduce the adverse impacts of a large charge rate on battery useful
life. The aging rates at 2.4C and 3C are observed to be slightly slower
than that at 1.5C, mainly on account of the increased battery polariza­ VC- or Li-organo-borate complex (25 CE), can increase the stability of
tion at high C rates [62]. Owing to the short time for constant current SEI film, reduce the barrier for lithium ions to pass and accelerate the
charging, the actual charge cut-off voltage of the battery drops, and the kinetic velocity of the electrode [70], leading to a positive effect on the
capacity decay slowly. aging of a graphite anode, especially at high temperatures. Since the
reactions at the electrode/electrolyte interface can be inhibited, coating
3.3. Depth of discharge the cathode active particles is also a good choice. In addition, reducing
the electrode loadings or replacing natural graphite with artificial
The depth of discharge (DOD) is influential in the cycle performance graphite can retard the rate of capacity degradation [71].
of lithium-ion batteries, but the influences vary greatly with different Extreme temperature, large charge-discharge rate, and high DOD are
cathode materials as shown in Table 3 [67–69]. Compared with LFP and common accelerated aging factors in battery use. Besides, the cutoff
NCM batteries, the cycle performance of NCA batteries is closely related voltage of charge and discharge as well as the operating voltage window
to the range of DOD. Note that it is the width of the discharge interval (ΔV) could also affect the aging mechanisms inside the battery. The ef­
that accelerates degradation rather than the upper and lower boundary fects of charge-discharge rate, temperature, and ΔV on the aging of the
value of DOD [67]. When DOD is limited to 10%–70%, batteries degrade NCM/graphite battery are discussed in Ref. [66]. It is shown that a high
slower compared with DOD of 0–100%. Also, the capacity retention charge rate, low temperature, and high ΔV could shorten the linear
capability remains great even at 60 � C in the range of 10%–70% DOD. aging stage and accelerate the nonlinear aging process. The battery
However, the influence of DOD on LFP and NCM batteries seems to aging rate rises rapidly at the nonlinear stage, and the dominant aging
negligible compared with temperature and cycle time [68,69]. mechanism changes from SEI growth to lithium deposition. Since aging
at low temperatures is a severe threat to safety, the preheating method
for batteries makes a great contribution to improving battery perfor­
3.4. Measures to postpone battery aging
mance and reducing aging in alpine and cold regions. Developing a
reasonable fast-charge strategy and setting a suitable discharge rate
Based on the aforementioned discussion, the postponement of bat­
threshold by limiting the maximum power are battery life-friendly
tery aging can be fulfilled through the exploration in battery
measures as well.
manufacturing and use.
It is proved to be helpful to alleviate battery aging by adding suitable
4. Diagnosis methods of aging of lithium-ion batteries
additives to the electrolyte in the manufacture of batteries because ad­
ditives could suppress the occurrence of some aging reactions. For
The aforementioned reactions have different impacts on battery
example, experimental results demonstrate that the common additives,

Table 2
Observation and mechanisms under different C rates.
C rates Experimental conditions Observation Mechanisms Ref

Charge/ LiCoO2/graphite battery@0.6C/1.2C/ C > 1.8C: a new peak occurs in the voltage range Uneven lithium deposition [61]
discharge rate 1.8C/3.0C of 4.1V–4.2 V Reaction between deposited lithium and
electrolyte
LiCoO2/MCMB battery@0.6C/1.2C/ C > 1.5C: slower cathode degradation as C rate Irreversible loss of lithium ions [62]
1.5C/1.8C/2.4C/3C increases Battery polarization
Charge rate NiMnCo/graphite battery@ 0.7C/2C/ C > 6C: further increase in battery resistance Transformation of SEI composition [63]
4C/6C More obvious film growth along the middle of the Temperature rise of the middle strip due to the
electrode unevenly wetted electrode
Discharge rate LiCoO2/C battery@ 1C/2C/3C 3C: 27.7% increase of battery surface film Decay of anode carbon material [64]
resistance and ohmic resistance Cracks in the SEI
Disappearance of carbonate components in SEI Electrode rupture
NCA battery: 1C/25C/PWM(10 Increase of impulsive discharge rate is more Electrode damage [65]
kHz@50%@83C) significant for battery aging New surfaces for SEI growth
Less available position for lithium ion insertion

PWM (10 kHz@50%@83C): pulse width modulated discharge mode (frequency@ duty cycle@ peak current).

6
R. Xiong et al.
capacity loss in a specific aging process [72,73], which can be used to
diagnose the aging of batteries. At present, the diagnosis methods can be
classified into three categories: disassembly-based post-mortem anal­
ysis, curve-based analysis, and model-based analysis. The post-mortem
analysis is a kind of direct observation by disassembling aged batte­
ries, while the other two are non-destructive methods based on elec­
trochemical impedance spectrum (EIS), open-circuit voltage (OCV)
curve and battery model parameters.
4.1. Disassembly-based post-mortem analysis
Post-mortem analysis is to disassemble aged batteries in a special
environment and observe each component of the batteries to determine
aging mechanisms through material analysis [57,74–76]. As an essential
step, battery disassembly requires safety and no contamination. Special
attention should be paid to: (1) to prevent internal short-circuit and
other safety problems during battery opening, non-destructive testing
technologies such as computed tomography (CT) [77,78] and X-ray [79]
are used to determine the best cutting position before opening a battery.
(2) the sealed operating environment filled with inert gas and suitable
humidity is required to ensure that the disassembly is safe and free from
contamination. An argon-filled glovebox is a common choice. Some­
times the nitrogen-filled glovebox can also be adopted but nitrogen can
react with lithium inside a battery to form Li3N. (3) contacts between the
components inside a battery should be avoided so the
cross-contamination in the process of battery disassembly will not
happen. The samples of the separated components are demanded to be
rinsed with dimethyl carbonate (DMC) [57,76,80–82], diethyl carbon­
ate (DEC) [83], or ethyl methyl carbonate (EMC) [84] before conducting
the analysis. Based on the physicochemical analysis, the post-mortem
analysis can be divided into three types, namely the morphology anal­
ysis method, composition analysis method, and structure analysis
method.
4.1.1. Morphology analysis method
In order to analyze the morphology of the electrode surface, optical
microscopy [75], scanning electron microscopy (SEM) [77,85] and
transmission electron microscopy (TEM) [86] are widely used to meet
the requirements of different resolutions. The optical microscopy has the
lowest resolution which focuses on the surface profile of the sample at a
micron-scale [80]. It can be used to diagnose the aging reactions at the
electrode level, such as electrode deformation and cracks in the elec­
trode coating. Both TEM and SEM have relatively high resolutions,
which can diagnose the aging of active material particles. SEM is only
used in a vacuum environment [87]. It manages to identify the surface
structure by generating a high-resolution three-dimensional image of
the sample surface, indicating the growth of SEI film, particle cracks and
lithium deposition at the anode [88,89]. TEM has higher resolutions
than SEM and can display particle morphology, crystallinity, stress, and
other characteristics of samples. For instance, it can observe the for­
mation of CEI film during battery aging. However, TEM has stricter re­
quirements for sample size, cleanliness [86], etc., limiting its
application.
4.1.2. Composition analysis method
The composition analysis includes determining the composition of
elements, the concentration distribution of elements on the surface and
along with the depth, and the chemical valence of surface elements.
Methods that are frequently used in composition analysis are energy
dispersive X-Ray spectroscopy (EDX) [90], X-ray photoelectron spec­
troscopy (XPS) [80], and inductively coupled plasma (ICP) atomic (or
optical) emission spectrometry (ICP-AES or ICP-OES) [91].
EDX analysis can characterize the element composition of active
materials and detect the mass concentration of different elements. It is
usually combined with SEM in practical to handle the failure of
detecting lithium and fulfill a more complete surface composition
7
Renewable and Sustainable Energy Reviews 131 (2020) 110048
analysis of the sample [74].
It is known that the concentration of some particular chemical ele­
ments varies along with the depth of the sample. In addition to
measuring the relative percentage content of elements, XPS can observe
changes in elemental composition at different depths. Therefore, it is
used to observe the SEI film, such as detecting the products of SEI for­
mation and decomposition inside the battery [92]. As a complement to
XPS, the time-of-flight secondary ion mass spectrometry (TOF-SIMS)
[93] also helps study the chemical structure of SEI.
The ICP-AES consists of ICP and spectrometer. The method can
demonstrate the presence of a transition metal dissolution reaction [94]
and detect the growth of SEI film [95] by showing fluctuations in the
lithium content of cathode and anode.
4.1.3. Structure analysis method
The structure analysis is to figure out the crystal structure informa­
tion on the surface, such as atomic arrangement, crystal size, and crystal
orientation.
The X-ray diffraction (XRD) [86] is mostly used for structural anal­
ysis of active materials. In the spectrum, the intensity and quantity of
XRD peaks reflect the electrode degradation and also indicate the
changes in SEI film and lattice parameters of active materials [96].
It is worth noting that none of the methods manage to cover all the
aging reactions. Multiple methods are often required to diagnose aging
effects holistically, which helps to understand the aging mechanism.
4.2. Curve-based analysis
Incremental capacity analysis (ICA) and differential voltage analysis
(DVA) based on battery OCV curves are widely adopted curve-based
analysis methods. Since the OCV curve itself is not sensitive to
changes in battery operating conditions and the environment in prac­
tical applications, the influence of charge-discharge rate on battery
electrochemical characteristics at each aging stage can hardly be
recognized through the OCV curve [97,98]. Therefore, mathematical
transformations of the OCV curve are necessary to amplify the hidden
aging influences, leading to the emergency of ICA and DVA.
4.2.1. Incremental capacity analysis
The first step of ICA is to obtain the IC curve based on the battery
OCV curve. It shows the way of the capacity increment (dQ dV ) changing
with battery voltage (V). Generally, the voltage interval (dV) is taken as
a fixed value which is selected according to different sets of data. The
raw IC curve cannot be directly used due to the noise, which needs to be
removed by a filter, such as the third-order polynomial Savitzky-Golay
filter with a segmented sliding window [99]. The voltage plateau in
the OCV curve is successfully transformed into several peaks in IC curve.
As shown in Fig. 4(a), the area between the IC curve and the hori­
zontal axis indicates the capacity charged in the corresponding voltage
interval, and the peaks in the curve indicate different phase transition
stages of the nickel-cobalt-aluminum (NCA) battery. Therefore, the
second step is to clarify the phase transitions of both anode and cathode
corresponding to each IC peak. For example, the NCA cathode experi­
ences three phase transitions during battery charging, namely the phase
transition of initial hexagonal to monoclinic, monoclinic to new hex­
agonal, and new hexagonal to another new hexagonal (H1-M-H2-H3).
And there are four different phase transitions (C6–C72–C36–C18–C12)
at the anode. Then the phase transitions of both cathode and anode are
superimposed to form four IC peaks of different heights in Fig. 4(a),
numbered as P1, P2, P3, and P4. Note that the numbers and forms of IC
peaks vary with electrode materials. The IC curve of LFP battery is
relatively simple in which the phase transitions of anode and cathode
correspond to three peaks and one peak, respectively [100]. There is an
interesting finding in NCA battery with the composite anode of graphite
and SiOx [101]. Compared to graphite delithiation, SiOx delithiation has
R. Xiong et al. Renewable and Sustainable Energy Reviews 131 (2020) 110048

Fig. 4. (a) IC curves and (b) DV curves of NCA battery under different cycles.

one more peak. modes including LAM, chemistry change (CC), under-discharge (UD),
The next step is to give a qualitative diagnosis of battery aging and undercharge (UC) has been proposed in Ref. [97]. A capacity loss of
mechanism based on the changes of the magnitude, width, and position 14.5% occurs after 301 cycles at the discharge rate of C/25, in which UD
of IC peaks in different cycles [102]. To simplify the analysis, the in­ and UC account for 9% and LAM for 5.5%.
ternal aging reactions are categorized into three modes: LLI, LAM, and
ohmic resistance increase (ORI). The dominant mode can be diagnosed 4.2.2. Differential voltage analysis
by ICA in different aging stages. The IC peaks shifting to the right are Similarly, DV is acquired by differentiating battery voltage con­
generally related to the increase of polarization resistance. Some IC cerning capacity (dV/dQ), which can be used to identify the aging re­
peaks would even disappear when the increased resistance prevents actions inside a battery.
some phase transitions from occurring at the original voltage. Though it Illustrated in Fig. 5, the DV curve is inversely related to the IC curve.
indicates LLI during constant current charging, part of the lithium in­ Therefore, the valleys in the DV curve represent the phase transitions of
ventory would be recovered during constant voltage charging. The the electrode active material, while a peak indicates a single phase of the
decrease in IC peaks often indicates LAM. When the IC peaks decline active material. Aging effects reflected on the DV curve are overall
inconsistently, it can be speculated that there are both LAM and LLI consistent with those reflected on the IC curve. Since the capacity loss of
inside the battery. Dubarry et al. [103] proposed two aging stages for the each phase transition can be easily obtained by measuring the distance
whole battery life cycle. The contribution and correlation of the three between the two adjacent peaks, the DV curve has an advantage of
modes in the two stages are separated and quantified. The results show quantifying degradation effects and the corresponding contribution
that the LLI is dominated in the first stage which affects ORI and LAM in rates more directly compared with the IC curve. Besides, dQ dV
can be
the second stage. Furthermore, LLI is the cause of battery performance transformed into:
degradation at middle and low level of SOC, while LAM and ORI are
responsible for the battery performance degradation at high level of dV dðVcathode Vanode Þ
¼
dV
¼ ð Þcathode
dV
​ ð Þanode
SOC. Sometimes, different ways of classifying the aging modes are dQ dQ dQ dQ
employed. For example, the assumption of four capacity degradation Thus we can distinguish the anode and cathode capacity loss, and

Fig. 5. Relationship between IC curves and DV curves.

8
R. Xiong et al.
determine the electrode that has a greater effect on battery aging. The
above two methods are used together to verify each other in practice.
4.3. Model-based analysis
The model-based diagnosis methods include the EIS-based method
and the electrochemical parameter identification-based method.
4.3.1. EIS-based method
The EIS-based method was introduced to study the performance
degradation caused by the increase in battery internal resistance. EIS
applies a small amplitude alternating current (AC) sinusoidal potential
signal on an electrochemical system under the condition of an open
circuit state or a certain stable direct current (DC) polarization. As a
result of the input potential signal, there is a sinusoidal current response
with a phase shift. The current response and the potential input can be
used to calculate electrochemical AC impedance in the frequency
domain. The main procedure for applying EIS to diagnose the internal
mechanisms inside a battery is illustrated in Fig. 6 [104].
The EIS spectrum plotted by the test data is generally represented by
a Nyquist plot or a Bode plot, which is usually modeled by an equivalent
circuit model (ECM). The AR-ECM shown in Fig. 6 is a commonly used
model [105] which consists of three parts [35,104,106]. The first part is
the series of Rohm and L to indicate ORI during battery aging, where Rohm
is the sum of the ohmic resistance of binder, current collector, electrodes
and electrolyte, and L represents the induction phenomenon of collector
at high frequencies. Rohm can be obtained by solving the intersection
between the impedance spectrum and the real axis in the high-frequency
region of the Nyquist plot, while L is determined by the positive imag­
inary part of the impedance. The second part is the parallel of CPESEI and
RSEI. It is related to the formation, decomposition, and regrowth process
of SEI film. RSEI in the Nyquist plot can be calculated by the span of the
first semicircle at intermediate frequencies on the real axis. The last part
is also a parallel of CPEdl and the series of Rct and Zw. Similar to RSEI, Rct is
Fig. 6. Main procedure for applying EIS to diagnose battery internal reaction mechanisms [104].
9
Renewable and Sustainable Energy Reviews 131 (2020) 110048
used to simulate charge transfer resistance and can be obtained by the
span of the second semicircle at low frequencies on the real axis. CPEdl is
used to simulate the double-layer effect during battery discharge which
is positively correlated with the porosity and curvature of the electrode.
Related to solid-phase diffusion resistance, Zw donates the diffusion of
active particles between the electrolyte and the electrode at low fre­
quencies. In battery aging analysis, RSEI and Rct jointly reflect the LLI
while Zw reflects the LAM.
It can be seen from the above analysis that each component in the
ECM corresponds to different aging reactions and the combination of
these aging reactions demonstrates the aging behavior of a battery.
Therefore, it is feasible to observe the changes of different resistances
during battery aging and analyze the corresponding aging reactions by
identifying parameters of ECM.
4.3.2. Electrochemical model parameter identification-based method
The electrochemical model (EM) describes physical and chemical
processes such as electrochemical reactions, diffusion, and migration of
lithium and ohmic action inside a battery. It shows the relationship
between external characteristics and internal parameters. Therefore, it is
possible to identify, compare, and analyze the EM parameters to
differentiate the specific aging reactions inside the battery and under­
stand the corresponding aging modes. Those EM parameters can be the
volume fraction of active material, the lithium embedding rate of the
electrode, the diffusion coefficient of the solid or liquid phase, and the
SEI film resistance during battery aging [107–111].
The exchange current density of the solvent reduction reaction
counts for a great deal in battery aging. When it shows a rising trend,
capacity loss tends to be exacerbated if other conditions remain the same
[112]. Based on the decrease of the volume fraction of active material
and the increase of SEI resistance, it is inferred by Fu et al. that the
power degradation is related to the SEI growth [111]. Also, the decrease
in the electrolyte diffusion coefficient reflects the consumption of elec­
trolytes. Characterizing the change of battery internal resistance by
R. Xiong et al. Renewable and Sustainable Energy Reviews 131 (2020) 110048

liquid conductivity, Schmidt et al. [109] calculated the capacity loss degradation) as examples, Ansea �n et al. elaborated on the imple­
caused by ORI and LAM of the cathode during battery aging. mentation steps and verified the diagnosis results.
Many on-board applications of battery aging diagnosis methods have
4.4. Challenges in the application been developed [120]. Table 4 illustrates the objectives, approaches,
and features of on-board applications for the curve-based analysis.
There are two challenges in the application of aging diagnosis The EIS-based method relies on complex equipment that restricts its
methods. One is to perform quantitative aging diagnosis, and the other is application to the laboratory. It is proposed to rebuild an on-board
to implement the aging diagnosis methods into on-board applications. impedance excitation and measurement system to meet the re­
quirements of low cost, lightweight, and high precision for EVs. The
4.4.1. Quantitative aging diagnosis system consists of an excitation module, a measurement module, and a
There is a one-to-many relationship between battery external char­ signal processing module. Table 5 demonstrates the objectives, ap­
acteristics and internal aging reactions under a particular working proaches, and features of the on-board application for the EIS-based
condition. Qualitative aging diagnosis can only help identify the domi­ method.
nant aging mechanisms. To quantify the effects of those aging mecha­
nisms, quantitative aging diagnosis needs to be further developed. 5. Comparison and prospects
The existing quantitative diagnosis consists of two steps. The first
step is to classify the battery aging reactions. LLI and LAM are the most 5.1. Comparison of diagnosis methods
common aging modes. On this basis, Birkl et al. believe that LAM in­
cludes two modes: LAMNE and LAMPE [113]. It is the first time that the Both advantages and disadvantages of different diagnosis methods
three aging modes have been proved in experiments through coin cells are listed in Table 6. The post-mortem analysis has the advantage of
with known lithium inventory and active materials. Dubarry et al. [114] observing battery aging inintuitively. However, it can only conduct one-
further refined LAMNE and LAMPE into LAMdePE, LAMdeNE, LAMliPE, and time sampling and testing at a single life point of the battery during the
LAMliNE to explain the active material loss during the de-intercalation whole aging process owing to the need for battery disassembly. Besides,
and intercalation process of lithium ions, respectively. It usually ends this method requires a complicated operation, high experimental cost,
up to three aging modes including LLI, LAMPE, and LAMNE [115]. Since and high dependence on equipment precision. Consequently, the post-
both LAMliPE and LAMliNE could be regarded as the linear combination of mortem analysis method is restricted in a laboratory.
LLI, LAMdePE, and LAMdeNE, the above five aging modes can be simpli­ The curve-based analysis is often combined with post-mortem anal­
fied to LLI, LAMdePE, and LAMdeNE [116]. ysis for a more reliable result. This method is computationally simple,
The following step is to analyze the contribution rates of each mode but it needs to deal with the noise when obtaining the IC or DV curves.
which is generally expressed as the percentage of decaying capacity or Also, the acquisition of IC and DV curves usually requires a small current
rising resistance. Take the lithium titanium oxide (LTO) battery as an rate, which may encounter difficulties in practical applications. The
example, the entire DV curve is divided into four regions by three peaks model-based analysis has good versatility and high accuracy at the
[117]. The range of each region at the horizontal axis represents expense of a heavy calculation burden. Note that there are many pa­
charging capacity, which corresponds to the area under each IC peak. rameters involved in the EM, only a few of which are related to battery
The aging reactions at different regions can be quantified by observing aging mechanisms, it is essential to avoid the interference of irrelevant
the range variation of each region at the horizontal axis. Compared with parameters on the target parameters. Besides, EIS measurement requires
calculating the area under the IC peak, the region range at the horizontal special equipment, and the result is easy to be disturbed by contact
axis on the DV curve is easier to figure out, making DV curves more resistance.
popular than IC curves in the quantitative analysis. Since the aging re­
actions include cathode degradation, anode degradation, and SEI for­ 5.2. Prospects for future development
mation [118], their respective contribution rates to battery aging can be
calculated as the equivalent capacity loss which is considered as the We have identified battery internal reactions related to battery
amount of active lithium-ion loss. Besides, it can be helpful to estimate aging, which can be used to establish battery aging models for RUL
the aging state under multiple factors if the contribution rate of each prediction and SOH estimation. The mechanism-driven methods simu­
specific aging reaction under a single factor is solved. Thus, the quan­ late specific physical and chemical reactions. Since the model
titative aging diagnosis method could be further applied to accelerated
aging tests and battery RUL prediction.
Table 4
Objectives, approaches and features of the on-board curve-based analysis.
4.4.2. On-board aging diagnosis
Objectives Approaches Features Ref
Different from battery aging diagnosis in a laboratory, the on-board
diagnosis is more demanding in terms of robustness, calculation capa­ Low computational Equivalent point Reduce calculation [107]
load in BMSs counting method burden
bility, data storage capacity, real-time performance, cost, and accuracy
Free from filtering and
[119]. Therefore, the curve-based analysis and EIS-based method have data smoothing issues
received much attention in the on-board aging diagnosis. Low measurement Gaussian filter for Balance curve fidelity [121]
For curve-based analysis, the comment flow can be divided into three noises curve smoothing and BMS cost
steps: (1) obtain clear IC/DV curves from battery charging curves; (2) Less sensitive to SOC-based ICA and Estimate SOC [122]
battery DVA Expand to the battery
extract feature points (FOIs), including position or height of peaks, area polarization pack level
under IC peaks, etc.; (3) diagnose battery aging in current BMSs using Quick capture of Support vector High accuracy [123]
the look-up table method. A look-up table method based on ICA and FOIs points regression Medium computation
peak area (PA) technology was presented by Ansea �n et al. [115]. The PA Fuzzy logic Fast calculation [107]
Less error with Differential thermal Measure changes in cell [124]
technology quantifies the capacity loss of battery phase change at each
temperature voltammetry (DTV) surface temperature and
stage by calculating the change of area under the corresponding IC peak. changes cell voltage
The look-up table is constructed using the relationship between the FOIs Small experimental Computer-aided Match visible voltage [116]
and six aging modes (LLI, LAMdePE, LAMdeNE, LAMliPE, LAMliNE, and matrix voltage curve response with aging
ORI). Taking three typical capacity degradation trajectories (linear mechanisms
Reduce experiment cost
degradation, power factor degradation, and nonlinear second-order

10
R. Xiong et al. Renewable and Sustainable Energy Reviews 131 (2020) 110048

Table 5 amount and the accuracy of diagnosis needs to be carefully balanced.

Objectives, approaches and features of the on-board EIS-based method. Developing diagnosis methods based on cloud computing also becomes
Objectives Approaches Features Ref possible and attracts more and more attention. The data collected by
BMSs can be sent to the cloud, based on which model training and
Low-cost Current fluctuation Reduce the cost of the [125]
current caused by a battery load active signal generator parameter identification can be done. Results can be sent back to BMSs
excitation Motor controller Easy to acquire [126] in EVs for subsequent execution.
Broadband noise Another trend is to develop an integrated framework for aging
during EV operation diagnosis, prognosis, and health management. Under this framework,
Direct digital Generate an arbitrary [127]
synthesizer sinusoidal reference signal
once the aging stage of batteries is diagnosed online, its impacts on
Low system Cascaded integrator- Variable sampling rates [127] battery RUL and SOH can be evaluated and prognosis of possible aging
data storage comb decimation filter Map EIS data into the stages could be realized. This plays an important role in the development
battery impedance circuit of the next generation BMSs.
equivalent model
Ultra-low Diagnosis based on Simulate VR during the [128]
resistance voltage relaxation (VR) battery rest period 6. Concluding remarks
detection behavior Save time
This paper summarizes the aging mechanisms of lithium-ion batte­
ries and the diagnosis methods of battery aging. A coupling result arising
Table 6 from a variety of aging reactions reduces the battery capacity and in­
Comparison of aging diagnosis methods. creases internal resistance. Different temperatures, charge-discharge
Methods Advantages Disadvantages rates, and DOD can give rise to the evolution of the dominant aging
reactions. This can offer guidance to the selection of a reasonable factor
Disassembly-based Intuitive observation of Irreversible destruction to
post-mortem the inside aging reactions batteries range when designing accelerated aging tests.
analysis Complicated operation Three methods have been widely used to diagnose battery aging,
High experimental cost which are disassembly-based post-mortem analysis, curve-based anal­
Curve-based analysis Non-destructive Cross-validation required ysis, and model-based analysis. For the development of advanced
diagnosis Noise handling trouble
diagnosis method, accuracy and feasibility shall be balanced especially
Good versatility Restricted current rate to
Low computational obtain the curves for on-board applications. The fusion of ECM, EM, and fractional order
burden Sensitive to battery model may be able to achieve a better diagnosis. This provides a new
polarization angle to find the intrinsic relation between parameters in the EM and
Model-based analysis Non-destructive Heavy computational
peak information in IC/DV curves.
diagnosis burden
Good versatility Interference by irrelevant Online diagnosis enabled by the cloud computing, machine learning,
High accuracy parameters in the EM digital twin, and virtual scene modeling technology is becoming a new
Hard to measure EIS emerging promising direction and hot topic, which can further
Interference by contact contribute to the development of novel advanced intelligent BMSs.
resistance in EIS
However, some challenges still exist, such as data collection, merging,
measurement
self-correcting, sharing, and developing new frames that can compatible
with multi-source, fragment, and asynchronous sparse data, as well as
parameters have clear electrochemical meanings, the model is promi­ taking into account batteries with different application scenarios,
nent in accuracy. However, it also brings high complexity and limits in different sizes, and also different configuration parameters.
the application. Note that the data-driven methods, independent of
specific models, use fitting or learning algorithms to extract aging in­
formation from historical data. The flexibility and strong applicability of Declaration of competing interest
data-driven methods can help balance the complexity of mechanism-
driven methods. The fusion of the two models can be considered. Be­ The authors declare that they have no known competing financial
sides, the application of intelligent optimization algorithms such as deep interests or personal relationships that could have appeared to influence
learning and reinforcement learning in battery state estimation gradu­ the work reported in this paper.
ally stands out and becomes a popular research trend [129].
For battery aging diagnosis, the pros and cons of each method have Acknowledgments
been clarified. To develop a smarter BMS, we summarize some unre­
solved problems in diagnosis methods and give several possible di­ This work was supported by the National Natural Science Foundation
rections in the future. for Excellent Young Scholars of China (Grant No. 51922006).
Since the recent on-board aging diagnosis device is usually designed
for a specific battery system, further exploration and research are still
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