Acta Phys. -Chim. Sin. ›› 2025, Vol. 41 ›› Issue (1): 100004.doi: 10.3866/PKU.WHXB202309019
Special Issue: Frontiers in Electrochemistry
• REVIEW • Previous Articles Next Articles
Mingyang Men1,2, Jinghua Wu1,2, Gaozhan Liu1,2, Jing Zhang1,2, Nini Zhang1,2, Xiayin Yao1,2,*(
)
Received:2023-09-12
Revised:2023-10-11
Accepted:2023-10-30
Published:2023-12-20
Contact:
Email: yaoxy@nimte.ac.cn; Tel.: +86-574-8632-4359 (Xiayin Yao)
Supported by:Mingyang Men, Jinghua Wu, Gaozhan Liu, Jing Zhang, Nini Zhang, Xiayin Yao. Sulfide Solid Electrolyte Synthesized by Liquid Phase Approach and Application in All-Solid-State Lithium Batteries[J]. Acta Phys. -Chim. Sin. 2025, 41(1), 100004. doi: 10.3866/PKU.WHXB202309019
Table 1
Classification of electrolytes synthesized by liquid-phase method."
| Sulfide solid electrolyte | Ionic conductivity (S∙cm−1) | Temperature (℃) | Solvent | Synthesis type | Reference |
| Li3PS4 | 1.6 × 10−4 | 25 | THF | Suspension type | |
| Li3PS4 | 3.3 × 10−4 | 25 | EA | Suspension type | |
| Li3PS4 | 1.2 × 10−4 | 30 | ACN | Suspension type | |
| Li3PS4 | 6.4 × 10−6 | 20 | DMC | Suspension type | |
| Li3PS4 | 2.3 × 10−6 | 25 | NMF | Suspension type | |
| Li3PS4 | 5.0 × 10−5 | 25 | EDA | Solution type | |
| Li3PS4 | 2.0 × 10−4 | 30 | THF-O-xylene | Solution type | |
| Li7PS6 | 1.1 × 10−4 | 30 | EtOH | Solution type | |
| Li7P3S11 | 1.0 × 10−3 | – | ACN | Suspension type | |
| Li7P3S11 | 1.05 × 10−3 | – | EA | Suspension type | |
| Li7P3S11 | 2.7 × 10−4 | 25 | DME | Solution type | |
| Li4PS4I | 1.0 × 10−3 | 25 | EP | Suspension type | |
| Li4PS4I | 1.2 × 10−4 | 25 | DME | Mixed type | |
| Li3.2P0.8Sn0.2S4 | 1.9 × 10−4 | 30 | EDA-EDT-THF | Suspension type | |
| Li3.25Ge0.25P0.75S4 | 1.82 × 10−4 | 30 | Hydrazine | Dissolution-precipitation type | |
| 80Li2S∙20P2S5 | 2.6 × 10−6 | – | NMF | Dissolution-precipitation type | |
| Li10GeP2S12 | 1.6 × 10−3 | – | DME-THF | Suspension type | |
| Li10GeP2S12 | 1.2 × 10−3 | 30 | EDA-ET | Solution type | |
| Li10GeP2S12 | 1.8 × 10−3 | 25 | EtOH-THF | Mixed type | |
| Li5.5PS4.5Cl1.5 | 2.87 × 10−3 | 25 | EDA | Mixed type | |
| Li6PS5Cl | 1.3 × 10−3 | 30 | EDA-EDT | Solution type | |
| Li6PS5Cl | 2.1 × 10−4 | 30 | EtOH | Solution type | |
| Li6PS5Cl | 1.1 × 10−3 | 30 | EA | Mixed type | |
| Li6PS5Cl | 2.79 × 10−3 | 25 | ACN | Mixed type | |
| Li6PS5Cl | 1.4 × 10−5 | – | EtOH | Dissolution-precipitation type | |
| Li6PS5Br | 3.1 × 10−3 | 25 | THF-EtOH | Solution type | |
| Li6PS5Br | 1.9 × 10−4 | 25 | EtOH | Dissolution-precipitation type |
Fig 6
Reaction mechanism in the synthesis of Li7P3S11 electrolyte in ACN 71–73. (a) A core-shell structure of Li3PS4 with Li2S∙P2S5 formed by Li2S-P2S5 binary system in ACN 71; (b) transformation mechanism of Li2S-P2S5 binary system in ACN 73; (c) the precipitate phase Li3PS4∙ACN and the soluble phase Li4P2S7∙ACN are formed by Li2S-P2S5 binary system in ACN, and they transform into Li7P3S11 after subsequent heat treatment 72. (a) Adapted with permission from Ref. 71, Copyright 2018, American Chemical Society; (b) Adapted with permission from Ref. 73, Copyright 2020, American Chemical Society; (c) Adapted with permission from Ref. 72, Copyright 2023, Elsevier Inc."
Fig 7
Dissolution results of sulfide solide-state electrolyte precursors in EDA-EDT cosolvents 62. (a) Raman spectra of EDA-EDT cosolvents with varying volume ratio; (b) photograph of sulfide solide-state electrolyte precursors, Li2S, P2S5, Na2S, LiCl, in EDA-EDT; (c) photograph of GeS2 in EDA and EDA-EDT; (d) photograph of SnS2 in EDA-EDT; (e) Raman spectra for the solution of GeS2 dissolved in EDA-EDT. (a, b, c, d, e) Adapted with permission from Ref. 62, Copyright 2022, Wiley-VCH."
Fig 8
Interaction between solvents and electrolytes. (a) Schematic illustration of Li6PS5Cl synthesized in THF/THF-EtOH 77, (b) the generation mechanism of Li3PO4 during the synthesis of Li6PS5Cl by liquid-phase method 92. (a) Adapted with permission from Ref. 77, Copyright 2023, Wiley-VCH; (b) Adapted with permission from Ref. 92, Copyright 2023, American Chemical Society."
Fig 9
Morphology of sulfide electrolytes prepared in different solvents. (a) Li3PS4 with nanoporous structure prepared in THF 42; (b) rod-like Li6PS5Cl synthesized in EA solvent 65; (c) SEM and HR-TEM images of plate-like Li3PS4 solid electrolyte prepared in EP via liquid-phase shaking. 46; (d) small-particle Li6PS5Cl electrolytes prepared in EtOH/ACN using Triton X-100 as dispersant agent 94. (a) Adapted with permission from Ref. 42, Copyright 2013, American Chemical Society; (b) Adapted with permission from Ref. 65, Copyright 2019, IOP Science; (c) Adapted with permission from Ref. 46, Copyright 2023, Springer Nature; (d) Adapted with permission from Ref. 94, Copyright 2023, Elsevier Inc."
Fig 11
The composite of electrode material and electrolyte synthesized by liquid-phase method. (a) Structural schematic and cycling performance of Co9S8-Li7P3S11 99; (b) schematic of 10% rGO-VS4@Li7P3S11 composite cathode and (c) cycling performance 113. (a) Adapted with permission from Ref. 99, Copyright 2016, American Chemical Society; (b) Adapted with permission from Ref. 113, Copyright 2013, Elsevier Inc."
Fig 12
Preparation of composites by injecting the electrolyte into the porous electrode by liquid-phase method. (a) Schematic of composite electrode preparation using Li6PS5Cls solution dissolved in ethanol and (b) SEM and EDS images corresponding to the composite electrodes 114; (c) schematic and cycling performance of sulfur-carbon replica-Li10.05Ge1.05P1.95S12 composite cathode 116. (a, b) Adapted with permission from Ref. 114, Copyright 2017, American Chemical Society; (c) Adapted with permission from Ref. 116, Copyright 2018, American Chemical Society."
Fig 13
Interfacial modification of electrolytes and electrodes by liquid phase method. (a) Flowchart of the preparation of Li2S-Li6PS5Cl-Carbon composite cathode and (b) HR-TEM image 117; (c) schematic of Li2S/OMC/Li6PS5Cl composites prepared by liquid-phase method; cycling performance of all-solid-state lithium-sulfur batteries using Li2S/OMC/Li6PS5Cl as cathode material at (d) 0.2C and (e) 2.0C 118. (a, b) Adapted with permission from Ref. 117, Copyright 2016, American Chemical Society; (c, d, e) Adapted with permission from Ref. 118, Copyright 2023, Elsevier Inc."
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