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Tao et al. Energy Mater 2022;2:200036 https://dx.doi.org/10.20517/energymater.2022.46 Page 3 of 35

Table 1. Comparison of liquid electrolyte-based LSBs and ASSLSBs
Batteries Advantages Disadvantages Ref.
Liquid electrolyte-based Higher conductivity Polysulfide dissolution and shuttle [1,3]
LSBs Lower interfacial impedance Electrolyte decomposition
Safety concerns (e.g., liquid leakage, inflammability and
explosiveness)
ASSLSBs Excellent thermal stability Poor interfacial stability [7-10]
Nonflammable SSEs Poor interfacial compatibility Large interfacial impedance
High operating voltages
Low self-discharge
Suppression of polysulfide
dissolution
Elimination of polysulfide shuttle

Figure 1. (A) Schematic illustration of interfacial compatibility and stability challenges in ASSLSBs. (B) Various interfaces in cathode
composites (reproduced with permission from [17] ).

ASSLSBs are briefly introduced here. The development of ASSLSBs has been accompanied by the study of
fast lithium-ion conductors, such as Li S-P S glasses, Li P S glass-ceramics, solid polymer materials, thio-
7 3 11
2 5
2
LISICON (Li superionic conductor, Li A B S (A = Si or Ge; B=Zn, Al or Pt)), Li GeP S , argyrodites
4-x
1-y y 4
2 12
10
Li PS X (X = Cl, Br or I) and composite polymer electrolytes, which have a history that can be traced back to
5
6
-3
the 1970s [24-26] . Following the discovery of SSEs with high ionic conductivities on the order of 10 -10 S cm ,
-2
-1
continuous efforts have been devoted to the fabrication of high-performance ASSLSBs. Currently, the Li-ion
conductivity of LGPS-type Li Si P S Cl is the highest (25 mS cm ) among all SSEs at room
-1
0.3
1.74 1.44 11.7
9.54
temperature [27,28] , illustrating its potential application in ASSLSBs.
The number of publications dedicated to SSEs has increased dramatically since 2010, as shown in Figure 2A,
indicating that they have become a research focus for energy storage with high power and density. The
article search was limited from 1977 to December 2020 using Google Scholar. Of the 610 publications found
[Figure 2B], 49.24% are focused on SSEs, suggesting that significant improvements have been achieved in
their high Li-ion conductivities. The articles related to cathodes and anodes account for 16.75% and 11.68%
of the total publications, respectively, aiming to resolve key issues in ASSLSBs, including volume change in
the electrodes, low content or loading of active materials, insulating properties of S and Li S,
2
chemical/electrochemical/physical instabilities, Li dendrite growth and side reactions between electrodes
and SSEs. Only 3.21% and 5.75% of the publications investigate the mechanism and interfacial properties of
ASSLSBs, respectively, showing that resolving the challenges at the electrode/electrolyte and
electrolyte/electrolyte interfaces and revealing their mechanisms with advanced characterization tools
remain significant challenges.