ORIGINAL RESEARCH

published: 08 February 2021

doi: 10.3389/fenrg.2020.606494

High-Performance All-Solid-State
Lithium–Sulfur Batteries Enabled by
Slurry-Coated Li6PS5Cl/S/C
Composite Electrodes
Chao Zheng, Kai Wang, Lujie Li, Hui Huang, Chu Liang, Yongping Gan, Xinping He,
Wenkui Zhang and Jun Zhang *
College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou, China

Among many lithium secondary batteries, lithium–sulfur batteries stand out because of
their high theoretical specific energy, low cost, non-toxicity and the fact that they cause no
environmental pollution. However, due to poor electronic and ionic conductivity, shuttle
effect, lithium dendrites and other defects, it remains a big challenge to achieve large-scale
application of lithium-sulfur batteries. Here we report an all-solid-state lithium–sulfur battery
based on Li-argyrodite Li6PS5Cl solid-state electrolytes through a slurry-coating method.
Li6PS5Cl with a high ionic conductivity of 1.3 × 10–3 S cm−1 at room temperature is used as
Edited by:
the solid electrolyte and the ion conductive additive in the electrode. The sulfur-based
Jiarui He,
University of Texas at Austin, composite cathode is fabricated through a slurry-coating process by dispersing sulfur,
United States Li6PS5Cl, ethyl cellulose, and carbon black in 1,3-dioxolane (DOL). This method can
Reviewed by: disperse the Li6PS5Cl around sulfur particles well, and the solvent does not react with any
Huan Pang,
Yangzhou University, China
component of composite cathodes during preparation. The battery delivers a high
Xiulin Fan, discharge capacity of 962 mA h g−1 at room temperature for the first cycle at
Zhejiang University, China
80 mA g−1. While the Coulombic efficiency is approximately 99.5% during 100 cycles.
*Correspondence:
This work provides a new insight into the combination method between the sulfide-type
Jun Zhang
[email protected] SSEs and sulfur cathodes, which is critical to the electrochemical performance of all-solid-
state lithium-sulfur batteries.
Specialty section:
This article was submitted to Keywords: lithium-sulfur batteries, all-solid-state batteries, Li6PS5Cl, slurry-coating, lithium metal anode
Electrochemical Energy Conversion
and Storage,
a section of the journal INTRODUCTION
Frontiers in Energy Research
Received: 15 September 2020 With the rapid increase in the energy requirements for energy storage devices, it has been difficult to
Accepted: 31 December 2020 meet these needs using traditional lithium-ion batteries (LIBs) due to low energy density, poor cycle
Published: 08 February 2021 stability, and high cost. In the future, energy devices will require higher and higher energy density
Citation: (Armand and Tarascon, 2008; Nitta et al., 2015; Liu et al., 2018; Wang et al., 2018b). When lithium
Zheng C, Wang K, Li L, Huang H, metal (low density and high electronegativity) is paired with elemental sulfur (theoretical capacity of
Liang C, Gan Y, He X, Zhang W and up to 1,672 mA h g−1) to form a lithium-sulfur battery, the theoretical capacity density of the battery
Zhang J (2021) High-Performance All-
can reach 2600 W h kg−1 or 2800 W h L−1 (Ji et al., 2009; Yin et al., 2013). Moreover, compared with
Solid-State Lithium–Sulfur Batteries
Enabled by Slurry-Coated Li6PS5Cl/S/
traditional LIBs, lithium-sulfur batteries have many unmatched advantages, such as being low cost,
C Composite Electrodes. non-toxic, causes no environmental pollution and has a safer working voltage (Lochala et al., 2017;
Front. Energy Res. 8:606494. Qu et al., 2018). Based on the above advantages, lithium-sulfur batteries are regarded as the most
doi: 10.3389/fenrg.2020.606494 promising next-generation energy storage product. However, there are still some bottlenecks in the

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Zheng et al. Solid Li-S Battery

application of lithium-sulfur batteries: 1) Liquid electrolytes are 2011). As an isostructural alternative to LGPS, Li10SnP2S12 has the
easy to flow, and flammable; 2) Sulfur is an insulator, and its poor advantages of being low cost and easily promoted, but it shows a
conductivity and low active material utilization seriously affect lower ionic conductivity of 4 × 10–3 S cm−1, because of a slightly
the battery rate performance; 3) Polysulfide is easily dissolved in different lithium ion disorder (Bron et al., 2013). The highest
the electrolyte and the polysulfide shuttle effects lead to poor reported ionic conductivity was found in the doping binary
Coulombic efficiency and cycle performance; 4) Lithium system, Li9.54Si1.74P1.44S11.7Cl0.3, 2.5 × 10–2 S cm−1 at RT (Kato
dendrites can pierce the separator, causing short circuits et al., 2016). Li-argyrodite Li6PS5Cl was reported as a promising
(Balakumar and Kalaiselvi, 2015; Pang et al., 2016; Chen et al., electrolyte with a high ionic conductivity of 1.3 × 10–3 S cm−1 at
2018b). RT (Boulineau et al., 2012; Zhang et al., 2018a; Zhang et al., 2019).
Aiming to solve the problems mentioned above, many studies The disadvantages of most sulfide electrolytes are their narrow
mainly focus on the optimization of the electrode. Currently, the electrochemical window and the electrochemical instability
most common solution is to combine carbon materials between the electrolytes and lithium metal (Han et al., 2016b).
(mesoporous carbon (Ji et al., 2009; Han et al., 2020), hollow The theoretical calculation results (Zhu et al., 2015; Han et al.,
porous carbon (Jayaprakash et al., 2011), carbon nanotube (Guo 2016b; Zhu et al., 2016) show that LGPS begins to be lithiated and
et al., 2011; Zheng et al., 2019), and graphene (Wang et al., 2011; reduced at 1.7 V. The phase equilibrium components of LGPS at
Liu et al., 2020), etc.) with sulfur to improve sulfur utilization and 0 V consist of Li3P, Li2S, and Li15G4, which have also been
to fix the polysulfide. But the surface of the carbon material is observed in experiments. The interphase has a higher growth
non-polar, it therefore cannot exert a strong anchoring effect on rate between LGPS and lithium, which means the presence of
the polar polysulfide. In addition to carbon materials, metal cations in SSEs such as Ge, Sn, Ti is detrimental to the formation
oxides (TiO2 (Wei Seh et al., 2013), MnO2 (Liang et al., 2015), of stable interface (Sakuma et al., 2016). But Li6PS5Cl can form a
Al2O3 (Han et al., 2013), Fe2O3 (Zheng et al., 2017), and V2O5 stable SEI, the thickness of SEI and interfacial resistance become
(Carter et al., 2017), etc.) can also fix polysulfide and conductive stable after a certain time and no longer increase over time
polymers (polyaniline (PANI) (Liu et al., 2015), and polypyrrole (Wenzel et al., 2016a; Wenzel et al., 2016b; Wenzel et al.,
(PPy) (Zhang et al., 2016; Geng et al., 2019), etc.) can improve 2018). Many cathode active materials such as LiCoO2,
electronic conductivity of composite sulfur electrodes. The low LiNi0.8Co0.1Mn0.1O2, S, and Li2S have been used in all-solid-
electronic conductivity of metal oxides and the high cost of state lithium batteries (ASSLBs) with Li6PS5Cl (Boulineau et al.,
conductive polymers are still not optimal solutions to the 2012; Boulineau et al., 2013; Huang et al., 2015; Yubuchi et al.,
serious capacity decay during cycling for a lithium-sulfur 2015; Han et al., 2016a; Yu et al., 2016; Zhang et al., 2018a; Zhao
battery. Replacing the liquid electrolyte with solid-state et al., 2019; Zhang et al., 2020). Han et al. used a novel bottom-up
electrolytes to achieve an all-solid-state lithium-sulfur battery method to synthesize nanocomposite cathode by dissolving Li2S
is one of the most promising strategies to solve these issues (Lin and Li6PS5Cl in ethanol, which showed a large reversible capacity
et al., 2013; Han et al., 2016a; Zhang et al., 2017; Fan et al., 2018; of 830 mAh g−1 at 50 mA g−1 for 60 cycles (Han et al., 2016a). Yu
Zhang et al., 2018b). The conversion of sulfur does not generate et al. fabricated the S/Li6PS5Cl/Li-In ASSLBs with a ball-milled
soluble polysulfide, so it can fundamentally solve the polysulfide S-Li6PS5Cl composite cathode (Yu et al., 2016). The batteries
shuttle effect (Yan et al., 2019). At the same time, the ultra-high displayed large capacity around 1,400 mAh g−1 during the first
mechanical modulus of SSEs can also effectively inhibit the cycle and decayed rapidly 400 mA h g−1 after 20 cycles. In 2018,
growth of lithium dendrites, thereby improving the Coulombic Nan et al. employed the nano-sulfur/multiwall carbon nanotube
efficiency and safety of the battery (Chen et al., 2018a; Cheng composites combined with Li6PS5Cl as the cathode, which
et al., 2019; Shen et al., 2019; Zhao et al., 2020). Unlike traditional delivered a high discharge capacity of 1850 mA h g−1 at 0.1 C
lithium-sulfur batteries that rely on the infiltration of liquid for the first cycle and 1,393 mAh g−1 after 50 cycles (Wang
electrolytes to achieve rapid ion migration, in the all-solid- et al., 2018a).
state lithium-sulfur batteries, the ion migration is mainly However, there are very few works on the synthesis of sulfur
achieved through solid electrolytes (Kato et al., 2016; Yan composite cathodes for ASSLBs by wet chemical methods. In this
et al., 2019; Zhao et al., 2019; Bai et al., 2020; Ding et al., 2020). work, we proposed a new preparation method about sulfur-
Among various SSEs, sulfide SSEs stand out because of their composite electrodes for ASSLBs using a liquid-phase process
high ionic conductivity, low grain boundary resistance, compatible with a DOL solution. The sulfur-composite electrodes consist of
interface with sulfur-based cathodes, and their easy processability sulfur as the active material, Li6PS5Cl as the solid electrolyte, ethyl
(Chen et al., 2018a; Ma et al., 2018). The most well-studied sulfide cellulose as the binder, and Super P (SP) as the conductive
SSEs are the binary xLi2S-(100-x)P2S5 system (x  0.4–0.8) (Zhang additive. The microstructure, ionic and electronic conductivity,
and Kennedy, 1990; Kanno and Murayama, 2001; Ohtomo et al., and electrochemical stability of Li6PS5Cl were systematically
2013). The ionic conductivity of β-Li3PS4 synthesized via wet- investigated. The electrochemical property of the sandwich-
chemistry is 1.6 × 10–4 S cm−1 with an activation energy of 0.36 eV type S/Li6PS5Cl/Li cell was tested at 80 mA g−1 and 30 °C.
(Liu et al., 2013). Crystalline Li7P3S11 is also an important member Finally, to further investigate how interface affects battery
of the binary system, because of its very high ionic conductivity performance, S/Li6PS5Cl interface properties before and after
(1.7 × 10–2 S cm−1 at room temperature (RT)) (Seino et al., 2014). cycling were examined by ex situ characterizations including
In 2011, Li10GeP2S12 (LGPS) was found to have a an extremely scanning electron microscopy (SEM), energy-dispersive spectra
high ionic conductivity of 1.2 × 10–2 S cm−1 at RT (Kamaya et al., (EDS), and electrochemical impedance spectra (EIS).

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Zheng et al. Solid Li-S Battery

(λ  0.15418 nm). Data was recorded in the 2-theta range of

10–80°. The Raman spectra in a range of 100–2,500 cm−1 were
collected using a DXR Raman microscope (Renishaw InVia
Raman spectrometer) with He-Ne 532 nm laser excitation and
a ×50 objective. The laser beam with a laser spot size of ca. 1 μm
was focused on each sample and the acquisition time for each
spectrum was 20 s. The morphology of samples was observed by
SEM (SEM, Hitachi S4700). An elemental analysis was conducted
on EDS attached to SEM. The cyclic voltammetry (CV)
measurement, the linear sweep voltammetry (LSV)
measurement, and the direct-current (DC) polarization test
FIGURE 1 | Schematic diagram of the slurry Li6PS5Cl-coated sulfur-
was conducted on a CHI660D electrochemical workstation
composite electrode and S/Li6PS5Cl/Li ASSLBs. (Chenhua, Shanghai). The CV curve of S/Li6PS5Cl/Li cell was
recorded between 0.4 V and 3 V with a sweep rate of 0.1 mV s−1.
The LSV curve of SS/Li6PS5Cl/Li cell was recorded in the
EXPERIMENTAL SECTION potential range from 0 to 6 V with a sweep rate of 0.1 mV s−1.
DC polarization test of a blocking SS/Li6PS5Cl/SS cell at 2 V to
Material Synthesis determine the electronic conductivity. The ionic conductivity of
Synthesis of Li6PS5Cl: The Li6PS5Cl was prepared using a method Li6PS5Cl was calculated by the equation:
described in our previous work (Zhang et al., 2018a; Zhang et al.,
d
2019; Zhang et al., 2020). In brief, a stoichiometric mixture of σ (1)
laboratory-grade Li2S, P2S5 (99%, Aladdin), and LiCl (99.99%, S×R
Aladdin) was milled at 500 rpm for 24 h. Subsequently, the where R is the total resistance of the electrolyte, d is the sample
mixture was sealed in a stainless-steel tube and annealed at thickness, and S is the area of the electrolyte. The total resistance
500 °C for 2 h to obtain argyrodite Li6PS5Cl. All the of Li6PS5Cl was measured on the SS/Li6PS5Cl/SS cell using the
experiments were carried out in an Ar-filled glove box (H2O Zennium electrochemical workstation (ZAHNER, Germany), in
and O2 < 0.5 ppm). which the frequency ranges from 100 mHz to 4 MHz with an
amplitude of 10 mV and the testing temperature ranges from
25 °C to 60 °C in stepwise increments of 5 °C. The EIS
Fabrication of All-Solid-State Lithium-Sulfur measurements of the S/Li6PS5Cl/Li cell before and after the
Batteries cycle were measured using the same instrument in the same
The sulfur-composite electrodes (sulfur powder (99%, Alfa frequency. A Galvanostatic discharge-charge test of S/Li6PS5Cl/Li
Aesar): Li6PS5Cl: SP (SCM industrial Chemical Co., Ltd.): cell was performed in a potential range from 0.4 to 3 V (vs. Li+/Li)
ethyl cellulose (Aladdin)) were dispersed with anhydrous DOL at 80 mA g−1 using a Neware battery test system (Neware,
(≥99.8%, Aladdin) in a mass ratio of 60 : 25: 10 : 5 under Shenzhen). The stability of lithium against Li6PS5Cl was tested
continuous stirring for 6 h. The slurry was then coated onto by the Neware using symmetric Li/Li6PS5Cl/Li cell at a current
carbon-coated aluminum foil with a glass rod and dried at 55°C density of 0.1 mA cm−2.
for 24 h. The average sulfur loading in each electrode is
0.95 mg cm−2. For the assembly of S/Li6PS5Cl/Li cell, the
sulfur-composite electrode was covered with 120 mg Li6PS5Cl RESULT AND DISCUSSION
powder and pressed together under 350 MPa in a stainless-steel
tank with a diameter of 12 mm. After that, lithium metal as the The crystal structure, composition, and morphology of the sulfur-
counter electrode was attached on the other side of the Li6PS5Cl composite electrode were characterized by XRD, Raman, and
layer. Finally, three-layered pellets (shown in Figure 1) were SEM, respectively. Figure 2A shows the typical XRD patterns of
assembled with a 2032 coin-type cell in an Ar-filled glove box. For the sulfur-composite electrode and all the materials used in the
the SS/Li6PS5Cl/Li, Li/Li6PS5Cl/Li cell and SS/Li6PS5Cl/SS, synthesis process. After sintering at 500 °C for 2 h, the peaks of
lithium foil or stainless steel (SS) as the working electrode, the Li6PS5Cl can be indexed to the crystalline Li7PS6 structure, where
assembling procedure remained exactly the same. All the the Cl atoms can replace S atoms in Li7PS6 (Deiseroth et al.,
procedures were carried out in an Ar-filled glove box (H2O 2008). Regarding the sulfur-composite electrode, there are no
and O2 < 0.5 ppm). obvious peaks of sulfur; the main diffraction peaks and the broad
diffraction peaks are indexed as Li6PS5Cl and amorphous carbon
materials with low crystallization degree, respectively. It indicates
Characterization and Electrochemical that Li6PS5Cl can distribute evenly on the surface of sulfur
Measurements particles. By comparing the Raman spectra (Figure 2B) of all
X-ray diffraction (XRD) patterns of samples were recorded by an materials, the sulfur-composite electrode can be further analyzed.
X-ray diffractometer (Rigaku Ultima IV) with Cu Kα radiation The weak peak at 425 cm−1 associated with PS43− (ortho-

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Zheng et al. Solid Li-S Battery

FIGURE 2 | (A) XRD patterns and (B) Raman spectra of the conductive additives (SP), sulfur, Li6PS5Cl, sulfur-composite electrode (C) The SEM image and
corresponding elemental mappings of sulfur-composite electrode.

FIGURE 3 | (A) Temperature dependence of the ionic conductivity of Li6PS5Cl (B) DC polarization of a blocking SS/Li6PS5Cl/SS cell (C) LSV curve of the SS/
Li6PS5Cl/Li cell (D) Voltage profile of the symmetric Li/Li6PS5Cl/Li cell at 0.1 mA cm−2.

thiophosphate) from the ionic formula (Li+)6(PS43−)S2−Cl− DOL solvent during the synthesis process. As shown in
(Deiseroth et al., 2008; Ohara et al., 2016) and peaks at Supplementary Figure S1, the irregular shape of the Li6PS5Cl
153 cm−1, 219 cm−1 and 474 cm−1 associated with S–S bond particle is beneficial to increasing the contact area between the
were observed, indicating no chemical reaction occurred in active material and electrolyte in the composite cathode. As seen

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Zheng et al. Solid Li-S Battery

FIGURE 4 | (A) Charge-discharge profiles during the first threes cycles and (B) cycling performance of S/Li6PS5Cl/Li cell at 80 mA g−1 and 30°C (C) Nyquist plots of
S/Li6PS5Cl/Li cell before cycling and after 100 cycles at 80 mA g−1.

from the morphology and elemental distribution in Figure 2C, Figure 4A shows the charge-discharge profiles of the
the sulfur particles are well embedded in the solid electrolyte and S/Li6PS5Cl/Li cell between 0.4 and 3.0 V during the first three
conductive additives, resulting in a dense composite and a low cycles. The current density is 80 mA g-1 and the test temperature
interfacial resistance. is 30 °C. The initial discharge capacity of ASSLBs is 962 mAh g-1
The temperature dependence of the ionic conductivity of and the corresponding Coulombic efficiency is as low as 56%,
Li6PS5Cl was systematically investigated. Supplementary which are ascribed to the activation process for the sulfur cathode,
Figure S2 shows the different impedance spectra of Li6PS5Cl interfacial decomposition, and the interfacial chemical reaction
at different temperatures. Through calculations based on between the electrolyte and electrode (Zhang et al., 2015; Han
resistance values, the ionic conductivity of Li6PS5Cl exhibits a et al., 2016a). As shown in Supplementary Figure S3, the CV was
gradual increase as the temperature increases, as shown in used to study the mechanism of the electrode reaction. During the
Figure 3A. It shows the ionic conductivities of 1.30 × first cycle, one reduction peak can be observed at 1.8 V due to the
10–3 S cm−1 and 1.05 × 10–2 S cm−1 at 25 °C and 60 °C, reduction of S to Li2S and the oxidation peak at 2.5 V can be
respectively. The activation energy Ea is calculated from the attributed to the oxidation of Li2S to S (Takeuchi et al., 2010;
slope of the linear Arrhenius plot according to the Arrhenius Wang et al., 2018a). During the subsequent cycles, both reduction
equation: and oxidation peaks slightly shift, which means a good
reversibility of the composite cathode. Figure 4B presents the
σ(T)  A × e(−k×T ) , cycling performance and Coulombic efficiency, the cell delivers a
Ea
(2)
high Coulombic efficiency of nearly 100% after three cycles,
where T is the absolute temperature, A is a pre-exponential factor, specific capacity decreases to 387 mAh g-1, and capacity
and k is the Boltzmann constant. According to Figure 3A, the Ea retention reaches 66% after 100 cycles. The impedance
value of Li6PS5Cl is 0.32 eV, which is low in comparison to most changes for the S/Li6PS5Cl/Li cell before and after cycling are
sulfide SSEs. In addition to ionic conductivity, the electronic shown in Figure 4C. Two Nyquist plots were fitted into one
conductivity of Li6PS5Cl has also been investigated by the DC equivalent circuit. The equivalent circuit is constructed to
polarization test (Figure 3B). It shows a low electronic distinguish common resistances: Rse, Rct1, Rct2, and Zw,
conductivity of 3.56 × 10–8 S cm−1, which is beneficial for representing the bulk resistance, two interfacial resistances,
suppressing lithium dendrite growth. LSV was used to and Warburg impedance, respectively (Deng et al., 2015;
determine the electrochemical window, which is important in Takada et al., 2015). Based on our previous work (Zhang
evaluating the stability of Li6PS5Cl against a lithium anode and et al., 2020), the Rct1 and Rct2 represent the interfacial
cathode. As shown in Figure 3C, the decomposition current resistance between lithium and the electrolyte, and the
corresponding to Li stripping (Li → Li+ + e−) is observed around interfacial resistance between the cathode and electrolyte,
0 V vs Li/Li+. There is no significant current change in the respectively. The bulk and interfacial resistance values increase
potential range from 0 to 6 V vs Li/Li+. Assembling the after cycling. But the variations of Rse and Rct1 are very small
symmetric Li/Li6PS5Cl/Li cell is also an important (≈40 Ω). There is a large difference in value (≈675 Ω) of Rct2,
experimental method to investigate the stability between which is attributed to interfacial reactions or a chemo-mechanical
Li6PS5Cl and lithium. The voltage profile of Li6PS5Cl remains failure (Ohno et al., 2019). These negative effects may be the main
at a lower voltage (≈10mV) during 400 h at 0.1 mA cm−2. The reason for the low initial Coulombic efficiency and the
results of LSV and symmetric battery prove that the Li6PS5Cl is subsequent capacity loss.
suitable to pair with the lithium anode. Considering the high ionic To investigate the interfacial reactions or chemo-mechanical
conductivity, low electronic conductivity, and wide failure in the S/Li6PS5Cl/Li cell after cycling, a cross-sectional
electrochemical window, Li6PS5Cl is an appropriate candidate SEM was conducted, and the elemental distributions of Al, S, P,
for an ionic conductor and battery separator. Cl, and C elements in the red selected area were assessed by EDS,

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Zheng et al. Solid Li-S Battery

FIGURE 5 | The cross-sectional SEM images and the corresponding elemental mappings of the interface between Li6PS5Cl and sulfur-composite electrode (A)
before cycling and after (B) 100 cycles at 80 mA g−1.

as depicted in Figure 5. Since both active material and electrolytes solution. The slurry coating achieved intimate contact between
are sulfur-based materials, it is difficult to determine where the the S/C particles and the Li6PS5Cl solid electrolyte, guaranteeing
chemical decomposition products at the interface come from. adequate lithium-ion pathways. The battery shows a high initial
Compared to the morphologies and elemental distribution of the discharge capacity of 962 mAh g−1 at 80 mA g−1 and a specific
C element at the S/Li6PS5Cl interface, it was found that the capacity of 387 mAh g−1. After 100 cycles, the capacity retention
thickness of the sulfur-composite electrode after cycling is more reaches 66%. Although the Li6PS5Cl solid electrolyte can
than twice what it was before. This significant change can be eliminate the shuttle effect and alleviate interfacial reaction,
explained by the volume change (chemo-mechanical failure) the volume change of sulfur still seriously affects the
because of the conversion reaction of S and a small number of performance of ASSLBs.
Li6PS5Cl. There is about 80% added volume in the cathode after
discharging, when 1 mole of S8 converted into 8 moles of Li2S.
The loose distribution of the C element after cycling, confirms DATA AVAILABILITY STATEMENT
that the volume increase stresses the surrounding matrix of solid
electrolytes and carbon materials, resulting in a lot of pores and The raw data supporting the conclusions of this article will be
voids in the cathode. Thus, at this scale, such a large volume made available by the authors, without undue reservation.
change has a much greater impact on interfacial resistance than
on chemical reactions. In other words, chemo-mechanical failure
is an urgent issue that needs to be resolved in all-solid-state AUHTOR CONTRIBUTIONS
lithium-sulfur batteries.
Conceptualization, JZ, HH, and WK; experimental, CZ, KW, and
LL; data analysis, CZ, YG, YX, and CL; writing—original draft
CONCLUSION preparation, ZC; writing—review and editing, JZ; supervision, JZ,
and WZ. All authors have read and agreed to the submitted
Argyrodite Li6PS5Cl is an ionic conductor with high ionic version of the manuscript.
conductivity and a wide electrochemical window. The Li6PS5Cl
possesses good potential for applications in lithium-sulfur
batteries. We successfully demonstrated a new strategy to FUNDING
fabricate a sulfur cathode for ASSLBs via the solution coating
method by mixing sulfur materials, Li6PS5Cl solid electrolyte, The authors acknowledge the support of the Zhejiang Provincial
ethyl cellulose binder, and SP conductive additive in a DOL Natural Science Foundation of China under grant No.

Frontiers in Energy Research | www.frontiersin.org 6 February 2021 | Volume 8 | Article 606494

Zheng et al. Solid Li-S Battery

LR20E020002, the National Natural Science Foundation of China SUPPLEMENTARY MATERIAL

(NSFC) under grant No. 21972127, 51677170, 51777194, and
51722210, the China Postdoctoral Science Foundation under The Supplementary Material for this article can be found online at:
grant No. 2020M671786 and the Zhejiang Xinmiao Talents https://www.frontiersin.org/articles/10.3389/fenrg.2020.606494/
Program No. 2020R403086. full#supplementary-material.

Han, X., Xu, Y., Chen, X., Chen, Y.-C., Weadock, N., Wan, J., et al. (2013).
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07.005 Conflict of Interest: The authors declare that the research was conducted in the
Yan, M., Wang, W.-P., Yin, Y.-X., Wan, L.-J., and Guo, Y.-G. (2019). Interfacial absence of any commercial or financial relationships that could be construed as a
design for lithium-sulfur batteries: from liquid to solid. Energy 1 (1), 100002. potential conflict of interest.
doi:10.1016/j.enchem.2019.100002
Yin, Y. X., Xin, S., Guo, Y. G., and Wan, L. J. (2013). Lithium-sulfur batteries: Copyright © 2021 Zheng, Wang, Li, Huang, Liang, Gan, He, Zhang and Zhang. This
electrochemistry, materials, and prospects. Angew Chem. Int. Ed. Engl. 52 (50), is an open-access article distributed under the terms of the Creative Commons
13186–13200. doi:10.1002/anie.201304762 Attribution License (CC BY). The use, distribution or reproduction in other forums is
Yu, C., van Eijck, L., Ganapathy, S., and Wagemaker, M. (2016). Synthesis, permitted, provided the original author(s) and the copyright owner(s) are credited
structure and electrochemical performance of the argyrodite Li 6 PS 5 Cl and that the original publication in this journal is cited, in accordance with accepted
solid electrolyte for Li-ion solid state batteries. Electrochim. Acta 215, 93–99. academic practice. No use, distribution or reproduction is permitted which does not
doi:10.1016/j.electacta.2016.08.081 comply with these terms.

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