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Progress in Chemistry 2021, Vol. 33 Issue (8): 1344-1361 DOI: 10.7536/PC200772 Previous Articles   Next Articles

• Review •

Inorganic Solid Electrolytes for the Lithium-Ion Batteries

Jiasheng Lu1, Jiamiao Chen1,2, Tianxian He2, Jingwei Zhao2,3(), Jun Liu4, Yanping Huo1,3   

  1. 1 College of light industry and chemical engineering, Guangdong University of Technology,Guangzhou 510006, China
    2 Guangzhou Tinci Materials Technology Co., Ltd,Guangzhou 510700, China
    3 Key Laboratory of Organofluorine Chemistry, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences,Shanghai 200032, China
    4 Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials, School of Materials Science and Engineering, South China University of Technology,Guangzhou 510641, China
  • Received: Revised: Online: Published:
  • Contact: Jingwei Zhao, Jun Liu, Yanping Huo
  • Supported by:
    National Natural Science Foundation of China(21975055); National Natural Science Foundation of China(61671162); National Natural Science Foundation of China(21975053); Guangdong Province Key Field R&D Program Project(2020B0101030005)
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Liquid lithium-ion batteries have fatal safety problems such as flammability, explosion, and short-circuit, as well as technical problems such as cruising range anxiety. The development of lithium-ion batteries with good safety performance and high energy density is an urgent need for industrial development. Compared with traditional liquid lithium-ion batteries, all-solid-state batteries have the advantages of safe use and high theoretical specific capacity, so they have been extensively studied and are known as the mainstream technology of next-generation batteries. Among them, the inorganic solid electrolyte plays an important role in the all-solid-state battery, and scientific researchers at home and abroad have conducted a lot of research work on this. This article introduces the latest developments in different types of inorganic solid electrolytes, including oxide solid electrolytes, sulfide solid electrolytes, and halide solid electrolytes. The researches on interface problems, crystal structure, preparation methods, and doping modification of inorganic solid electrolytes are also elaborated. Finally, the problems to be solved in inorganic solid electrolytes in recent years are discussed, and the future research directions are also given.

Contents

1 Introduction

2 Solid oxide electrolytes

2.1 Garnet type solid electrolytes

2.2 Perovskite solid electrolytes

2.3 NASICON type solid electrolytes

2.4 LiPON thin films electrolytes

3 Solid sulfide electrolytes

4 Solid halide electrolytes

5 Conclusion and outlook

Key words: lithium-ion batteries, inorganic solid electrolytes, interface compatibility, crystal structure, electrochemical performance
Table 1 A summary of different lithium-ion inorganic solid electrolytes
Type Conductivity(S/cm) Advantage Disadvantage
Solid oxide electrolytes 10-5~10-3 High electrochemical oxidation Voltage and electrochemical stability
High mechanical strength		 Non-flexible
Expensive large-scale Production
Thin film electrolytes 10-7~10-5 Stable with cathode materials or lithium metal Expensive large-scale Production
Low conductivity
Solid sulfide electrolytes 10-7~10-2 High conductivity and low grain-boundary resistance
Good mechanical strength and mechanical flexibility		 Poor compatibility with cathode materials
Low oxidation stability
Solid halide electrolytes 10-8~10-2 Wide electrochemical windows
Stable with cathode materials		 Sensitive to moisture
Table 2 Comparison of ionic conductivity and activation energy of different lithium-ion inorganic solid electrolytes
Type Material Conductivity(S/cm) Activation energy(eV) Refs
Solid oxide electrolytes Li3Nd3Te2O12 1.0×10-5, 600 ℃ 1.22 16
Li5La3Nb2O12 1.0×10-6, RT 0.43 19
Li5La3Ta2O12 1.0×10-6, RT 0.56 19
Li7La3Zr2O12 3.0×10-4, RT 0.32 20
Li6.25Ga0.25La3Zr2O12 1.46×10-3, RT 0.25 23
Li7La3ZrNb0.5Y0.5O12 8.29×10-4, 30 ℃ 0.30 25
Li6.5La3Zr1.5Ta0.5O12 4.8×10-4, RT 0.30 26
Li0.34La0.56TiO3 2.0×10-5, RT - 40
Li0.39La0.50Sr0.06TiO3 1.95×10-3, 30 ℃ 0.30 41
Li0.33La0.46Y0.1TiO3 9.51×10-4, RT - 42
Li0.38Sr0.44Ta0.7Hf0.3O2.95F0.05 4.8×10-4, RT - 45
Li1.3Al0.3Ti1.7(PO4)3 4.6×10-4, RT 0.28 54
Li1.5Al0.5Ge1.5(PO4)3 8.85×10-4, 60 ℃ - 55
Li1.3Al0.3Ti1.7(PO4)3 0.32×10-3, RT - 58
Li1.3Al0.3Ti1.7P(O4)3 1.75×10-3, 60 ℃ - 62
3.3×10-3, RT
Solid sulfide electrolytes Li10GeP2S12 1.2×10-2, 27 ℃ - 78
Li9.54Si1.74P1.44S11.7Cl0.3 2.5×10-2, RT - 79
Li9.54Si1.74P1.44S11.7I0.3 1.35×10-3, RT - 80
Li6PS5X(X = Cl, Br, I) 10-2~10-3, RT - 82
Li7P3S11 1.7×10-2, RT 0.18 87
Solid halide electrolytes LiGaBr4 7.0×10-6, 127 ℃ - 94
Li3YBr6 1.7×10-3, RT 0.37 96
Li3YCl6 1.7×10-3, RT 0.40 96
Li3ScCl6 3.02×10-3, RT 0.36 101
Li3.5ScCl6.5 2.42×10-4, RT 0.36 102
Li2.5ScCl5.5 3.02×10-3, RT 0.37 106
Li2.5Y0.5Zr0.5Cl6 1.4×10-3, RT 0.33 109
Li3InCl6 2.04×10-3, RT 0.34 114
Li1.52Mn1.24Cl4 1.5×10-5, RT -
LiOHBrF 2.9×10-4, 120 ℃ 0.62
Fig. 1 The crystal structure of a conventional garnet A3B3C2O12[15]. Copyright 2020, Royal Society of Chemistry
Fig. 2 (a) Crystal structure of Li7-3xGaxLa3Zr2O12;(b) Li+ and Ga3+ environment;(c) lithium-ion diffusion pathways in Li7-3xGaxLa3Zr2O12[23]. Copyright 2020, American Chemical Society
Fig. 3 Schematic of Li-metal batteries with garnet LLZT and LLZT-C(C: carbon)[26]. Copyright 2020, American Chemical Society
Fig. 4 First-principle calculations of different interfaces of(a) LLZO/Li,(b) LLZT/Li,(c) Li2CO3/Li,(d) Li2O/Li;(e) Schematic of different wetting behaviors of garnet surfaces with molten Li;(f) Galvanostatic cycling of symmetric Li/LLZT/Li cells[33]
Fig. 5 Crystal structure of tetragonal LLTO[38]. Copyright 2020, American Chemical Society
Fig. 6 (a) The Nyquist plots;(b) cycling performance at 0.1 C;(c) rate performance;(d) galvanostatic charge/discharge curves of Li/PEO/LLTO-41/LFP cell at 65 ℃;(e) Schematic for preparation of LLTO film using tape-casting method[40]. Copyright 2020, John Wiley and Sons
Fig. 7 (a) plot of |Z| vs Frequency for LLTO/LMO, LMO, LLTO, and the mathematical addition of LMO and LLTO;(b) Phase angle vs Frequency plot for LLTO/LMO, LLTO and LMO;(c) Nyquist plot of the interphase from 10 kHz to 5 Hz, and the fitted curve based on the equivalent circuit above;(d) HRTEM image of the interphase between LMO and LLTO[43]. Copyright 2020, John Wiley and Sons
Fig. 8 (a) A comparison of Li+ conductivities along with schematics of the domain microstructures of the LLTO electrolytes: low-T LLTO, high-T LLTO and Li-excess LLTO. (b) Arrhenius plots of the boundary conductivities for low-T LLTO, high-T LLTO and Li-excess LLTO measured over a temperature range of -20 to 70 ℃. (c) Schematics of the domain microstructures of the LLTO electrolytes[44]. Copyright 2020, Royal Society of Chemistry
Fig. 9 The chemical and electrochemical stability of LSTHF5 in water with different pH values[45]. Copyright 2020, John Wiley and Sons
Fig. 10 Rhombohedral R3c structure of NASICON[49]. Copyright 2020, Royal Society of Chemistry
Fig. 11 Illustration of the fabrication of the SSLMB with in-situ forming ionogel interlayers and the schematics of the LATP/Li metal anode interfaces with the ionogel interlayer.[58]. Copyright 2020, American Chemical Society
Fig. 12 Galvanic cycle of(a) Li/LAGP/Li with P(AA-co-MA)Li as the interface layer;(b) LiCl-added P(AA-co-MA)Li interface layer;(c) overpotential versus current density of the interface-modified Li/Interface/LAGP/Interface/Li symmetrical cell.[60]. Copyright 2020, American Chemical Society
Fig. 13 Crystal structure of argyrodite-type Li6PS5X(X = Cl, Br, I) that crystallizes with cubic symmetry in the space group F43m.[81]
Fig. 14 Battery performance of Li4Ti5O12 + LSPS-Cl + C/LSPS-Cl/glass fiber/Li cells incorporating different LSPS-Cl materials annealed at different temperatures[90]. Copyright 2020, Nature
Fig. 15 Photographs(top views) of the LGPS SE pellet surface(A) without and(B) with LiTFSI/PYR13TFSI;(C) Nyquist profiles for the Li/LGPS/Li symmetric cells with and without LiTFSI/PYR13TFSI;(D) time evolution of impedance response of the Li/LGPS/Li cell with LiTFSI/PYR13TFSI at various storage times[93]. Copyright 2020, American Chemical Society
Fig. 16 The crystal structures of LYC(left) and LYB(right) obtained after Rietveld refinement[96]. Copyright 2020, John Wiley and Sons
Fig. 17 The 1D migration pathway in the ab plane[102]. Copyright 2020, American Chemical Society
Fig. 18 Illustration of water-mediated synthesis route for Li3InCl6 SSE and the reversible interconversion between the hydrated Li3InCl6·xH2O and dehydrated Li3InCl6. Green Cl, purple In, blue Li.[106]Copyright 2020, John Wiley and Sons
Fig. 19 Diffusion coefficients from FPMD for Li4Ga4I16,Li7Ga8Br24, Li8Cs4I12, Li20Ge2P4S24, Li40Cl24O8, Li20Cl12O4 and Li56Ta8O48[115]. Copyright 2020, Royal Society of Chemistry
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