2019 6th International Conference on Electric Vehicular Technology (ICEVT)
November 18-21, 2019, Bali, Indonesia
Review of Solid-State Battery Technology Progress
Samuel Rahardian
Faculty of Mechanical & Aerospace Engineering
Institut Teknologi Bandung
Bandung, Indonesia
samuelrahardian@students.itb.ac.id
Poetro Lebdo Sambegoro
Faculty of Mechanical & Aerospace Engineering
Institut Teknologi Bandung
Bandung, Indonesia
National Center for Sustainable Transportation Technology
poetro@ftmd.itb.ac.id
Abstract—Battery development is essential to satisfy the
green technology trend that requires electric-based technology.
Lithium-ion battery (LIB) is the most popular battery that has
been used in various electric technology. However, LIB has a
concern on the safety aspect by using liquid electrolyte which is
prone to thermal failure that leads to flame or explosion. Solid-
state battery (SSB) recent development could handle such
thermal problems due to the non-flammable characteristic of
the solid electrolyte. SSB also has potential for future main
battery candidates due to high energy & power density.
Although there are many advantages, SSB also has several
problems in recent development. Interfacial stability, low ionic
conductivity on room temperature, mechanical properties, etc.
need to be studied further to make an adjustment for further
development. This review would give information regarding
recent progress on SSB development from various types of
electrolyte and failure mechanisms.
Keywords—battery, solid-state, electrolyte, interfacial
stability, SSB development.
I. INTRODUCTION
The urgency for cleaner energy requires technology
renewal. One of the solutions is replacing Internal
Combustion Engine (ICE) cars into Electric Vehicle (EV)
[1]. The migration from ICE to EV could cause massive
power demand for battery charging [2, 3]. Battery
development is the core of future EV technology to make
energy usage more efficient. The trend of EV sales parallel to
lower production cost and performance of battery [4, 5].
Lithium-Ion Batteries (LIB) is the popular choice for
energy storage for EV because LIB has several advantages
such as lightweight, high energy density, high power density,
and long life. Currently, LIB could reach energy density up
to 260 Wh/kg [6-8]. Aside from several advantages that LIB
had, there are several disadvantages to LIB. The thermal
runaway is the main issue for LIB usage. Thermal runaway
leads to thermal fail such as burning, fire, or explosion that
occurred due to a relatively low operating temperature of
liquid electrolyte. One of the most used electrolytes for LIB
are based on LiPF6 and mixtures of cyclic and linear
carbonate solvents highly volatile and had a relatively low
flash point between 16-33°C. Dendrite formation across the
electrolyte also occurred when the battery was in
charge/discharge cycle. When the dendrite grew and reached
978-1-7281-2917-4/19/$31.00 ©2019 IEEE 310
Bentang Arief Budiman
Faculty of Mechanical & Aerospace Engineering
Institut Teknologi Bandung
Bandung, Indonesia
National Center for Sustainable Transportation Technology
bentang@ftmd.itb.ac.id
Ignatius Pulung Nurprasetio
Faculty of Mechanical & Aerospace
Engineering
Institut Teknologi Bandung
Bandung, Indonesia
ipn@ftmd.itb.ac.id
the other electrode, a short circuit will happen and the flame
might occur. Battery thermal management for LIB should be
considered for battery design [9-15].
Replacing liquid electrolytes with solid-state electrolytes
(SSE) could prevent thermal runway issues stated before.
SSE could handle higher operating temperatures better than
the liquid electrolyte. SSE also has the potential for higher
energy density and higher power density [16]. There are
several SSE that have been developed for SSB. First is solid
oxide electrolytes consist of NASICON-type, Perovskite-
type, Garnet-type, Amorphous/glass-type, etc. The second
one is solid sulfide electrolytes consist of Li2S-SiS2 based
electrolytes, Li2S-P2S5 based electrolytes, Thio-LISICON.
The third one is solid polymer electrolytes (SPEs) consist of
PEO and PEO like-based SPEs, Non-polyether-based SPEs,
and Single Lithium-ion conducting based SPEs [17].
Despite of the advantages SSB had, there are several
issues that affect the performance of the SSB such as ionic
conductivity, interfacial ion transport mechanism, interface
properties, capacity loss, and short life cycle [18].
II. SOLID ELECTROLYTE ION TRANSPORT MECHANISM
The main difference between LIB and SSB was the ion
transport mechanism. In LIB ion was transported by liquid
diffusion of Lithium-ion across the liquid electrolyte. In
SSB Lithium-ion diffuse across the solid electrolyte as been
shown in Figure 1. There were three possibilities for solid
diffusion in SSB. First is vacancy diffusion where the ion
migrates to a vacant spot on neighboring site, the second
possibility was the direct interstitial mechanism, and the
third is the correlated mechanism where the ion knocking
neighboring stable ion into metastable cation side.
Schematics for three diffusion mechanisms of SSB shown in
Figure 2. The ionic conductivity on SSB could be calculated
by (1) which follow Arrhenius relationship.
(1)
Where (u) is the mobility of the ion, (q) is the product of
charge, (n) is the concentration, (σ0) is the conductivity for
uncorrelated hopping, (T) is the temperature, (m) is a
constant with -1 value, (Ea) is the activation energy and, (kB)
is Boltzmann coefficient [19].
Fig. 1. Schematics of ion and electron transport of LIB and SSB.
Fig. 2. (a)Diffusion mechanism due to vacancy, (b) interstitial diffusion
mechanism, (c) correlated diffusion mechanism (knocking lattice ion into
the adjacent metastable site)
III. SOLID-STATE ELECTROLYTE
A. Solid Oxide Electrolyte
For solid oxide electrolytes type that has been developed
until now consist of NASICON type, perovskite-type, garnet
type, γ-Li3PO4 type, and amorphous/glass type. The solid
oxide electrolyte generally has good chemical stability which
not releasing toxic gases when decomposed [20,21]
1) NASICON
Hong and Goodenough had been developed the
first 3D NASICON structure which enables fast Na+ ion
transport with electrical resistivity ≤ 5Ω-cm at 300°C.
The electrolyte consists of Na1+xZr2SixP3-xO12 which
becomes the basic framework for NASICON type
electrolyte [22]. Currently, Aono et al. developed
electrolytes with the structure of Li1.3M0.3Ti1.7(PO4)3 (M
= Al or Sc). The electrolyte has conductivity 7×10-4
S/cm at 298K [23].
2) Perovskite
Perovskite type electrolyte has high conductivity
due to its structure. Dyer and White found a general
formula Ln1/3NbO3 (Ln=La, Ce, Pr, Nd) [24,25]. One of
the most promising perovskites was
Li3/8Sr7/16Hf1/4Ta3/4O3 with conductivity 3.8×10−4 S/cm
however this electrolyte has a high cost due to Ta
311
composition [26]. Development of perovskite-type
electrolyte depends on the substitution of Ta material
and maintain its chemical stability after replacement.
3) Garnet
The development of Li7La3Zr2O12 (LLZO) for
electrolyte was promising due to its high conductivity at
2×10-4S/cm [27]. The problem that occurred in
processing cubic phased LLZO which has higher ionic
conductivity was its high calcination temperature and
bad interfacial resistance which could be solved by
doping another species such as Ga. With Ga ion doping
the conductivity will be 5.4×10-4Scm-1 [28]. The
development of Garnet type electrolytes will be focused
on the calcination temperature.
4) Amorphous/glass
For Amorphous electrolyte the latest type
conductivity still low. Lithium Phosphorous Oxynitride
(LIPON) has an average conductivity of 2.3(±0.7) ×10−6
S/cm at 25°C [29]. Further development was needed for
this type of electrolyte.
5) γ-Li3PO4
One of the best conductivity results for this type of
electrolyte was Li3.6Ge0.6V0.4O4 with a conductivity of
4×10−5 S/cm at 18 °C and will rise to 10-2 S/cm at 190°C.
This electrolyte easy to synthesize, thermodynamically
stable, and insensitive to atmospheric attack [30]
B. Solid Sulfide Electrolyte
Solid sulfide electrolyte become one of the most
promising solid electrolytes. High polarizability of sulfide
ions weakens the interaction between the anions and the
lithium ions sulfides resulting in fast ionic conduction.
Another advantage is low grain boundary size resulting in
easier to build bulk type battery [31].
1) Li2S-SiS2 based
From Kennedy et al. SiS2-Li2S- Li glass is unstable
in contact with lithium metal [32]. With doping with
Li3PO4 with the composition 0.03Li3PO4-0.59LizS-
0.38SiS2 at ambient pressure by quenching in liquid
nitrogen, the conductivity at room temperature was
6.9×10-4 S/cm and the stability of the glass towards
electrochemical reduction was dramatically improved
[33].
2) Li2S-P2S5 based
Li2S−P2S5 glasses and glass-ceramics have the
advantage of high lithium-ion conductivities. The major
issue for this sulfide electrolytes is that they must be
handled in an inert gas atmosphere since they have low
chemical stability in air. Hydrolysis from sulfide and
water create harmful H2S gas [34]. A novel glass-
ceramic electrolyte of 99(70Li2S-30P2S5)-1Li2ZrO3
made by a vibratory ball-milling method and followed
by a heat-treatment process was created with high
conductivity of 2.85×10−3 S/cm at room temperature.
This electrolyte also has a stable crystal structure and a
high lithium-ion diffusion coefficient [35].
 3) Thio-LISICON
Electrolyte Li10GeP2S12 was made by Kamaya et al.
with a conductivity of 12×10−3 S/cm exceeding liquid
organic electrolyte. This value is the highest
conductivity achieved by the solid electrolyte. It also has
stability, safety, and excellent electrochemical properties
[36]. Although Li10GeP2S12 has many advantages, Ge
used in that electrolyte cost very high. Li10SnP2S12 was
made by replacing Ge with Sn and resulting relatively
high conductivity 7×10−3 S/cm [37].
C. Solid Polymer Electrolytes (SPEs)
Solid polymer electrolytes have good
processability, low flammability, good flexibility, safety
and close contact with the electrodes but this type of
electrolytes having bad mechanical properties [38].
1) PEO and PEO like-based
Polyethylene oxide (PEO)-salt system is one of the
most extensively studied polymeric electrolytes. This
electrolyte has relatively small conductivity, but with
synthesizing copolymer by the macromonomer method,
PAN-PEO was created and has conductivity of
6.79×10−4 S/cm at 25 °C [39].
2) Non-polyether-based
Zhang et al. synthesized a novel cross-linked
siloxane-based solid polymer network and found that the
ionic conductivity of this network doped with LiTFSI
was as high as 1.33×10−3 S/cm at ambient temperature
[40]. Finding a better polymer host structure was needed
to improve this kind of electrolyte.
3) Single lithium-ion conducting-based
Single Lithium-ion SLIC-SPEs electrolyte was
made to solve the dual ion conductor problem. These
polymers were synthesized by the simple radical
copolymerization of the SSPSILi and MA monomers
resulting in high Lithium-ion conductivity of 2.67×10-3
S/cm with good mechanical strength, thermal stability,
and wide electrochemical stability [41].
IV. FAILURE MECHANISM OF SOLID-STATE LITHIUM
BATTERIES
With many developed solid electrolytes described before,
the cycle life of SSB should be identified to be used in a real
application. The solid electrolyte/electrode interface is very
important for SSB performance. Failure mechanisms such as
electrochemical, mechanical, or chemical affecting the cycle
life of SSB crucially. Interface stability of solid
electrolyte/cathode and electrolyte/anode needs to be studied
to find a better understanding of the failure mechanism and
develop better SSB in the future [18]. The mechanical failure
for the SSB summed in Table I.
A. Solid Electrolyte/Cathode interface
1) Space Charge Layer
Space Charge Layer (SCL) is developed at the
interface in which Lithium-ion transfer from the sulfide
electrolytes to the oxide electrodes driven by the
312
chemical potential difference. lithium ions transfer from
the sulfide to maintain the equilibrium of chemical
potentials at the interface and lead to a very high
interfacial resistance. Because the resistance is rising
then the power density would be decreased. [42]. Further
experiments should be conducted to find the
electrolyte/cathode combination which produces lower
SCL.
2) Element interdiffusion
Element interdiffusion usually occurred between
inorganic solid electrolyte and oxide cathode during high
temperature or high pressure. This interdiffusion
increases interfacial resistance that could lower battery
performance. The charging process potentially produces
interdiffusion due to temperature rise during the process.
High operating conditions also could promote this
phenomenon to occur. Element interdiffusion is
observed at the LiCoO2/Li7La3Zr2O12 interface after high
temperature processing [43].
3) Cathode active material/electrolyte interface reaction
During high voltage operation, oxidation
decomposition of solid electrolyte also could occur. This
decomposition will reduce ionic conductivity and
increase interfacial resistance which could produce poor
cycle performance. Preventive action should be
performed to suppress the interface reaction such as
spray coating [44].
4) Electrochemomechanical failure
Mechanical failure could affect battery
performance. The lithium-ion transfer could be
decreased as loss of contact due to fracture or other
mechanical failures [45]. During the cycling process, the
volume of electrolyte and electrode will expand or
shrink based on the process due to Lithium-ion transfer
[46].
Mechanical properties affecting the materials to
prevent micro cracking. Micro cracking will be resulting
in contact loss, resistance increment, and affect the
battery performance. Fracture toughness could be
identified for predicting whether the cracking would
occur. Fracture toughness for brittle materials could be
determined by using a Vickers test. The parameter
affecting fracture toughness including E and H as the
values determined by instrumented indentation
hysteresis experiments, P was load applied with the
value 9.81N, c was the crack length, and k was Vickers
constant with the value 0.016. The relation between each
parameter could be derived into (2). [47]
(2)
Tippens et al. conducting an experiment for
symmetry LAGP and observe cracking mechanism
during electrochemical cycling. Interphase formation
expands the volume of the cell and causing stress in the
electrolyte which initiates a crack. Impedance rise was
 the result of the cracking due to interphase formation. strategies to tune the interfacial structures to improve ion
The deformation gradient ۴ will be affected by elastic transport.
(۴e), plastic (۴p), and chemical (۴c) distortions. The
relation of the deformation gradient could be stated in TABLE I. MECHANICAL FAILURE
(3) [48].
Failure
Authors Case
Criteria
F=FpFcFe (3) Fracture
McGrogan, et
Li2S−P2S5 toughness of
al.[39]
electrolyte
Monroe C. & Dendrite
PEO
5) Conductive additive material/ electrolyte reaction Newman J. [42] formation
Bending due to
Zhang, et al. In/Li10GeP2S12/
Conductive additive sometimes introduced in the [44] LiCoO2
volume
cathode to improve electron transfer of cathode and expansion
Crack due to
increasing performance of the SSB. The reaction Tippens, J. et
LAGP interphase
between conductive additive material and electrolyte al. [43]
formation
could result in unknown phase formation. This phase
formation could restrict the conduction of electron and V. INDUSTRIALIZATION PROGRESS
lithium-ion transfer. This restriction could increase SSB potential for replacing conventional LIB leads to
interfacial resistance and capacity loss [49] shifting trends for battery technology. Many big industries
conducting research and development for SSB. They believe
B. Solid Electrolyte/Anode Interface that SSB would solve popular LIB battery problem also
1) Lithium dendrite provide better performance.
In conventional LIB, dendrite formation becomes a Solid Power CEO Doug Campbell is building in
problem resulting in a short circuit [50]. SSB becomes Louisville the largest solid-state battery factory in the U.S.
the solution to prevent dendrite formation due to high after raising $20 million. Bloomberg New Energy Finance
mechanical strength with a solid electrolyte. However, in projects that by 2040, EVs will account for 55 percent of all
the real application, Lithium dendrite still formed and new-car sales. Investment in better power storage
grow. In polymer electrolyte, dendrite grows pushing technology becomes the main concern for this trend. Solid
polymer electrolyte, curling and expand towards outside Power is getting backing from automakers BMW, Samsung
delaminating the surface between polymer and substrate. and Hyundai. Ionic Materials, based in Woburn,
This phenomenon analyzed by employing linear elastic Massachusetts, has among its backers Renault, Nissan, and
theory by Monroe and Newman. The displacement due Mitsubishi. [54].
to dendrite formation is derived from (4) [51]. Japan manufacturers also developing their own SSB.
Honda and Nissan have teamed up for SSB research to
develop better battery technology for their EV that has
affordable production price [55]. Toyota also aims for
commercialization for SSB in 2022. Toyota cooperates with
the University of Southampton spinoff firm, Ilika to develop
SSB technology [56].
(4)
Qing Tao Energy Development Co, a startup that spun
off of Tsinghua University, claims to have a first solid-state
In inorganic electrolytes like garnet, dendrite battery production line in the country. Their production line
formation growing in confined space of the material located in the city of Kunshan, East China has a capacity of
such as void, defect, and grain boundaries. The main 100 MWh per year and planned to upgrade it to 700 MWh
difference between conventional LIB and SSB is the per year in 2020. They claim that they have achieved battery
dendrite formation could be predicted in SSB so material that has an energy density of over 400 Wh/kg which
engineering could be performed to prevent the dendrite compared to commercial LIB with an energy density of 250
formation [52]. – 300 Wh/kg [57].

2) Li metal/ electrolyte interface reaction
Interface of Li metal and electrolyte could be
determined by three types (a) Thermodynamically stable
interface which has no reaction between Li metal and
solid electrolyte. (b) Reactive and mixed conducting
interface (MRI), in which the interphase has ionic
conductivity that promotes self-discharge of the SSB. (c)
Reactive and metastable solid electrolyte interface (SEI)
which has interphase that is thermodynamically unstable
[53]. With interphase formation, interface resistance of
the solid electrolyte will be increased, therefore
For Europe manufacturers, there are Bolloré group and
KOLIBRI. France's Bolloré group launch Blue Car EV
which using battery produced by BatScap and composed of
LiFePO4/PEO/Li, exhibiting an energy density of 1000
Wh/kg and capacity retention of 80% after 1300 cycles.
German KOLIBRI batteries have been applied in Audi A2.
Lithium metal oxide/polymer solid electrolyte film/graphite
was the composition of the battery. The outcome of energy
density was claimed to be 300 Wh/kg [58].

313
 VI. CONCLUSION
With SSB technology development the main issues for
SSB commercialization were the production cost. Raw
material, production preparation, and low-cost material
usage were several factors to be considered in the
industrialization process. With better knowledge of various
SSB electrolytes and failure mechanism, SSB development
will go in the right direction for replacing conventional LIB.
ACKNOWLEDGMENT
This research is partially funded by LPDP through
RISPRO program.
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