Towards safe lithium<strong>‒</strong>sulfur batteries from liquid-state electrolyte to solid-state electrolyte

doi:10.1007/s11706-023-0630-3

Front. Mater. Sci.

2023, Vol. 17

Issue (1) : 230630 https://doi.org/10.1007/s11706-023-0630-3

REVIEW ARTICLE

Towards safe lithium‒sulfur batteries from liquid-state electrolyte to solid-state electrolyte

Zhiyuan Pang¹, Hongzhou Zhang¹(

), Lu Wang²(

), Dawei Song¹, Xixi Shi¹, Yue Ma¹, Linglong Kong³(

), Lianqi Zhang¹

¹. Tianjin Key Laboratory for Photoelectric Materials and Devices, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
². College of Chemistry and Materials Science, Shandong Agricultural University, Taian 271018, China
³. State Forestry and Grassland Administration Key Laboratory of Silviculture in Downstream Areas of the Yellow River, School of Forestry, Shandong Agricultural University, Taian 271018, China

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Abstract

Lithium–sulfur (Li‒S) battery has been considered as one of the most promising future batteries owing to the high theoretical energy density (2600 W·h·kg⁻¹) and the usage of the inexpensive active materials (elemental sulfur). The recent progress in fundamental research and engineering of the Li‒S battery, involved in electrode, electrolyte, membrane, binder, and current collector, has greatly promoted the performance of Li‒S batteries from the laboratory level to the approaching practical level. However, the safety concerns still deserve attention in the following application stage. This review focuses on the development of the electrolyte for Li‒S batteries from liquid state to solid state. Some problems and the corresponding solutions are emphasized, such as the soluble lithium polysulfides migration, ionic conductivity of electrolyte, the interface contact between electrolyte and electrode, and the reaction kinetics. Moreover, future perspectives of the safe and high-performance Li‒S batteries are also introduced.

Keywords lithium–sulfur battery liquid electrolyte polymer electrolyte solid-state electrolyte battery safety

Corresponding Author(s): Hongzhou Zhang,Lu Wang,Linglong Kong

About author:

Changjian Wang and Zhiying Yang contributed equally to this work.

Issue Date: 01 March 2023

Cite this article:

Zhiyuan Pang,Hongzhou Zhang,Lu Wang, et al. Towards safe lithium‒sulfur batteries from liquid-state electrolyte to solid-state electrolyte[J]. Front. Mater. Sci., 2023, 17(1): 230630.

URL:

https://academic.hep.com.cn/foms/EN/10.1007/s11706-023-0630-3
https://academic.hep.com.cn/foms/EN/Y2023/V17/I1/230630

Fig.1 (a) The energy densities of several energy storage systems. (b) The ranking of properties of LIBs.

Fig.2 A brief roadmap containing the important development of the Li–S battery.

Fig.3 The reaction mechanism of the Li–S battery in different liquid electrolytes. (a) Schematic of the reactions in Li–S cell. Reproduced with permission from Ref. [45]. (b) The typical discharge and charge profile of the Li–S cell. Reproduced with permission from Ref. [46]. (c) Sulfur K-edge XANES upon charge and discharge. Reproduced with permission from Ref. [47]. (d) Schematic illustration of the reaction mechanism of the nanoporous carbon–sulfur composite in carbonate electrolyte. Reproduced with permission from Ref. [48]. (e) Schematic of the lithiation/delithiation processes of S chains in a Li–S battery. Reproduced with permission from Ref. [49]. (f) Overall reaction of Li/SPAN cell. Reproduced from Ref. [50]. (g)(h) A voltage profiles of cells at C/20 and the corresponding ex-situ XPS spectra of S 2p core-level at the final discharged state. Reproduced from Ref. [51]. (i) A schematic illustration of the charge/discharge mechanism of the sulfur cathode in the carbonate/ether co-solvent electrolyte with the corresponding (j) charge/discharge profiles and (k) TEM image of the cycled cathode. Reproduced with permission from Ref. [52].

Tab.1 The employed lithium salts in Li–S batteries [56–69]

Tab.2 Melting points and boiling points of ester and ether electrolytes [70–73]

Fig.4 (a) Schematic illustration of safe Li–S battery with intrinsic flame-retardant organic electrolyte. Reproduced with permission from Ref. [80]. (b) Flame tests with the effect of TTFP, and (c) SET and conductivity of the electrolytes with different TTFP contents. Reproduced with permission from Ref. [81]. (d) 6.5 mol·L^?1 LiTFSI/FEC and 1 mol·L^?1 LiTFSI/FEC added in liquid-state electrolyte. Reproduced with permission from Ref. [82]. (e) Schematic illustration of Li–S batteries using standard carbonate (STD) electrolyte and TEP/TTE (IFR) electrolyte. Reproduced with permission from Ref. [80].

Fig.5 (a) [Li(G₄)_x][TFSA]/HFE electrolyte used in Li–S battery. Reproduced with permission from Ref. [84]. (b) Preparation route of polymer/LiTFSI/ionic liquid electrolyte. Reproduced with permission from Ref. [85]. (c) Li–S battery without ionic liquid, (d) Li–S battery with ionic liquid, (e) Li–S battery approach the flame without ionic liquid, and (f) Li–S battery approach the flame with ionic liquid. Reproduced with permission from Ref. [86].

Fig.6 (a) Schematic illustration of safe Li?S battery with 1,4-BDT additives. Reproduced with permission from Ref. [93]. (b) The schematic of reaction between SOCl₂ and lithium anode, and the cycled Li (c) without and (d) with the protection by SOCl₂. Reproduced with permission from Ref. [95]. (e) SEM image of lithium anode surface, (f) SEM image of lithium anode surface without protection, and (g) SEM image of lithium anode protection by TBAI. Reproduced with permission from Ref. [96].

Tab.3 The Li–S battery with gel polymer-based electrolyte [101,108,110–127]

Fig.7 (a) The morphologies of semi-crystalline PEO and (b) the related mechanism of ion transport. Reproduced with permission from Ref. [104].

Fig.8 (a) Schematic illustration of polymer electrolyte-based quasi-solid-state Li–S battery. Reproduced with permission from Ref. [131]. (b) The immobilization mechanism for polymer electrolyte reduces the lithium polysulfide dissolve in electrolyte. Reproduced with permission from Ref. [132]. (c) Interlayer used in polymer electrolyte-based quasi-solid-state Li–S battery. Reproduced with permission from Ref. [112].

Fig.9 (a) Principle of gel electrolyte with high ionic conductive, (b) synthesis of novel gel electrolyte, and (c) discharge/charge profiles of Li–S battery with gel electrolyte at 0.2 C. Reproduced with permission from Ref. [125]. (d) Synthesis route of multifunction gel polymer, and (e) Li⁺-ion transportation in gel polymer electrolyte. Reproduced with permission from Ref. [108]. (f) Possible mechanism of Li⁺-ion transportation. Reproduced with permission from Ref. [127].

Fig.10 (a) MOF-PVDF gel polymer electrolyte for the Li–S battery, and (b) Li⁺-ion transport in MOF. Reproduced with permission from Ref. [118].

Fig.11 (a) Optic photograph of GPE membrane and Cellgard 2300 separator; SEM images of the surface morphology of lithium electrodes after stripping/deposition cycles for (b) Li/LE/Li cell and (c) Li/GPE/Li cell; (d) the evolution of polarization in lithium symmetric cells along with the lithium stripping/deposition cycles. Reproduced with permission from Ref. [148]. (e) Synthesis of cross-linked polymers, and (f) Li?S battery with polymer electrolyte. Reproduced with permission from Ref. [149]. (g) The mechanisms of bare Li and polymer modified-Li during cycling. Reproduced with permission from Ref. [150].

Fig.12 (a) Historical development of solid electrolytes. Reproduced with permission from Ref. [158]. (b) Reported total ionic conductivity of solid-state lithium-ion conductors at room temperature. Reproduced with permission from Ref. [165]. (c) Electrochemical stability ranges of various electrolyte materials grouped by anion, with corresponding binary for comparison. Reproduced with permission from Ref. [166]. (d) The schematic of the solid-state Li–S battery. Reproduced with permission from Ref. [167].

Tab.4 The reported solid-state electrolytes in Li–S batteries [173–175,178–194]

Fig.13 (a) The preparation schematic of S@BP2000 for all-solid-state Li–S battery; high-resolution TEM images of (b)(c) BP2000 and (d)(e) S@BP2000, and (f) cycle performance of S@BP2000 cathode in solid-state electrolyte-based all-solid-state Li–S battery at 3 C. Reproduced with permission from Ref. [207]. CNT and sulfur with (g) uniform and (h) nonuniform electronic pathway. Reproduced with permission from Ref. [208]. (i) Synthesis of Li₂S/C nanocomposite. Reproduced with permission from Ref. [185].

Fig.14 (a)(b) SEM images and (c) XRD pattern of VS₂; (d)(e) SEM images and (f) TGA curve of VS₂/S composite (sulfur content ≈ 33 wt.%); (g) the proposed microstructure and discharge mechanism for the Li–S/VS₂ battery; (h) electrochemical profiles of Li–S/VS₂ battery at a cathode loading of 7.7 mg·cm^?2 and (i) the capacity of cells with an active material loading of 15.5 mg·cm^?2. Reproduced with permission from Ref. [210]. (j) Synthesis of 10% rGO-VS₄@Li₇P₃S₁₁ used as sulfur carrying material in all-solid-state Li–S battery. Reproduced with permission from Ref. [193]. (k) Synthesis of FeS₂@S nanoparticles as cathode used in all-solid-state Li–S battery. Reproduced with permission from Ref. [211].

Fig.15 (a) The S–C|Li₁₀SnP₂S₁₂|Li–In all-solid-state Li–S battery assembled by conventional methods. Reproduced with permission from Ref. [186]. (b) High-temperature mechanical milling synthesis sulfur cathode. Reproduced with permission from Ref. [213]. (c) Synthesis of Li₂S@Li₃PS₄ nanoparticle; SEM images of (d) nano Li₂S and (e) Li₂S@Li₃PS₄ (LSS); (f)(g) Electrochemical characteristic of nano Li₂S and LSS as the cathode used in Li–S battery. Reproduced with permission from Ref. [178].

Tab.5 The properties of modified inorganic solid-state electrolytes [171,173,177,187,219–238]

Fig.16 (a) Preparation of all-solid-state Li–S battery with the Li₇P_2.9Sb_0.1S_10.75O_0.25 electrolyte, and (b) rate performance and (c) cycling stability of Li–S battery with the Li₇P_2.9Sb_0.1S_10.75O_0.25 solid-state electrolyte. Reproduced with permission from Ref. [187]. (d) Li–S battery with the Li₇P_2.9Ce_0.2S_10.9Cl_0.3 electrolyte, and (e) impedance spectra and (f) ionic conductivities of the solid-state electrolytes of Li₇P₃S₁₁, Li₇P_2.9Ce_0.2S_11.1, and Li₇P_2.9Ce_0.2S_10.9Cl_0.3. Reproduced with permission from Ref. [220].

Fig.17 (a) LLZO filled in PEO assemble of Li–S battery. Reproduced with permission from Ref. [247]. (b) Design of cathode/electrolyte (CNF/S-PEO/LLTO) bilayer structure for Li–S battery. Reproduced with permission from Ref. [248]. (c) Synthesis of LLZTO/PEGDA composite solid electrolyte, and (d) possible mechanism for LLZTO/PEGDA electrolyte suppression of shuttle effect. Reproduced with permission from Ref. [249]. (e) The difference between liquid-state solid-state and solid/polymer composite electrolyte used in Li–S battery. Reproduced with permission from Ref. [250].

Fig.18 (a) Schematic of Li?S battery with Li?Al alloy anode and its reaction mechanism; (b) practical stability window of the LGPS1 electrolyte and the chemical potential of different anode; images of (c) pristine LGPS1, and that (d) after contacting with Li_0.8Al for 8 h, (e) after the Li_0.8Al-LGPS-Li_0.8Al cell cycling for 100 h, and (f) after contacting with Li for 8 h; (g) galvanostatic Li plating/stripping profiles of the Li-LGPS1-Li cell at 0.5 mA·h·cm^?2 (blue) and 0.1 mA·h·cm^?2 (gray), and the Li_0.8Al-LGPS1-Li_0.8Al cell at 0.5 mA·h·cm^?2 (red). Reproduced from Ref. [268]. (h) Theoretical energy densities of Li?S battery with different anode materials. Reproduced from Ref. [269].

Fig.19 The Radar map of the basic properties of the electrolyte for Li–S batteries.

Fig.20 The main research directions of polymer electrolyte-based Li–S battery and all-solid-state Li–S battery.

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