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Progress in Chemistry 2023, Vol. 35 Issue (3): 390-406 DOI: 10.7536/PC220913 Previous Articles   Next Articles

• Review •

Application of Polyacrylonitrile in the Electrolytes of Lithium Metal Battery

Yu Xiaoyan, Li Meng, Wei Lei, Qiu Jingyi, Cao Gaoping, Wen Yuehua()   

  1. Research Institute of Chemical Defense, Beijing Key Laboratory of Advanced Chemical Energy Storage Technology and Materials,Beijing 100191, China
  • Received: Revised: Online: Published:
  • Contact: *e-mail: wen_yuehua@126.com
  • Supported by:
    National Natural Science Foundation of China(21975284)
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With the rapid development of portable electronic devices, electric vehicles, and smart grids, there is an increasing interest in high-energy-density lithium metal batteries. Uneven Li stripping or deposition on the surface of lithium metal will lead to the growth of lithium dendrites, which can easily pierce the separator and cause the short circuit in the battery. Moreover, the highly reactive lithium metal will continue to react with the electrolyte, resulting in an unstable solid electrolyte. interfacial (SEI) film and irreversible capacity loss. Taking high-energy-density and high safety into account is a key scientific problem that needs to be solved urgently in the development and application of lithium metal batteries. The interaction of strong electron withdrawing group (C≡N) in polyacrylonitrile (PAN) polymer and C=O in carbonate solvent can form a more stable SEI film. As a lithium anode coating, PAN can also inhibit the growth of lithium dendrites. In addition, due to the low lowest unoccupied molecular orbital, high electrochemical stability and wide electrochemical window, PAN can be regard as polymer electrolytes for lithium metal batteries, and matched with a high-voltage cathode to achieve both high energy density and safety. Thus, PAN polymer has significant potential application in electrolytes for lithium metal batteries. This review mainly starts from the different states of electrolytes (liquid, gel, and solid state). Recent research development of PAN polymer as separators and lithium anode protective layers in liquid electrolytes, as well as its application in gel electrolytes and solid-state electrolytes are presented. Finally, the review prospects the development trend of PAN polymer in lithium metal battery electrolytes.

Contents

1 Introduction

2 The application of PAN in liquid state electrolytes

2.1 As separator

2.2 As lithium anode protective layers

3 The application of PAN in gel electrolytes

4 The application of PAN in solid-state electrolyte

4.1 Monolayer electrolytes containing PAN

4.2 Heterogeneous multilayer electrolytes containing PAN

4.3 PAN electrospinning fiber membrane

5 Conclusion and outlook

Key words: polyacrylonitrile, separator, lithium anode, gel electrolyte, solid-state electrolyte
Table 1 The PAN-based separators and their physical performance
Component Thickness (μm) σ
(mS·
cm-1)		 Porosity (%) Electrolyte Uptake (%) Fracture strength
(MPa)/ Elongation
(%)		 Cathode ref
1 PAN 26 0.94 62.0 300 49.6/3.8 LiFePO4 36
2 PAN 24 1.06 54.7 336 - LiMn2O4 33
3 PDA@PAN 50 1.39 83.3 341 13.9/31.3 LiFePO4 37
4 PAN/cellulose/ nylon6/PVPK30 - - 55.7 225 71.24/33.7 - 38
5 PAN/CA/HAP 46 3.02 61 268 11.8/11.8 LiFePO4 39
6 PAN/ZSM-5 - 2.16 55.5 308 13/- LiFePO4 40
7 PAN/PEO/PAN 25 1.54 68 650 - LiFePO4 41
8 PAN/DOPO - 6.49 - 310 - LiFePO4 42
9 PAN/HPTCP - 0.95 46 162 40 NCM622 43
10 PAN-PEI 60 0.19 - - 19 S/NCM523 44
11 PAN-SiO2 115 1.98 85.3 - 9.6 NVP/LiFePO4 45
Fig. 1 Illustration of Li-S batteries with (a) conventional PP (Celgard) separator and (b) APANF separator; (c) Voltage profiles of symmetrical cells with different separators[44]. Copyright 2020, Elsevier
Fig. 2 (a) The merits of a PBA@PAN separator in Li metal batteries; The SEM images and crystalline structures of (b) FeFe-PB, (c) NiFe-PBA, and (d) NiCo-PBA[46]. Copyright 2022, American Chemical Society
Fig. 3 (a) Cathodic linear sweep at 1 mV·s-1 scan rate; (b) Galvanostatic Li deposition curves at 1 mA·cm-2 in 5 M LiFSI electrolytes without and with AN additive; (c) Calculated reduction potential of the representative Li+ solvation structures; (d) Calculated reduction potential of Li+-AN, Li+-EC, Li+-DEC, and Li+-FSI- pairs[51]. Copyright 2021, Elsevier
Fig. 4 (a) Electrostatic potential maps of PAN and EC; (b) Schematic illustration of the dipole-dipole interaction between the C≡N group of PAN and the C=O group of EC; (c) Cross-sectional and surface SEM morphologies of bare Li and Li sheets coated with polar polymer network after cycling under 5 mA·cm-2 [55]. Copyright 2019, Royal Society of Chemistry (d) Binding energy between the two polymers and solvent molecules; (e) Li/ELPAN and Li/ELPS after 5 cycles in a Li-Li symmetric battery[56]. Copyright 2022, Elsevier
Table 2 Solid electrolyte based on blending PAN polymer with different fillers
Component σ(S·cm-1) Electrochemical window (V) t L i + Cathode ref
1 PAN/LiClO4/LLZO nanowires 1.31×104 (20 ℃) - 0.3 - 81
2 PVA/PAN/LATP/SN/LiTFSI 1.13×104 (25 ℃) 5.1 0.507 LiFePO4 82
3 PAN/LiClO4/LLTO nanotubes 3.6×104 (RT) 5 0.38 LiFePO4 83
4 PAN/LiClO4/LLZTO 2.2×104 (40 ℃) 4.9 0.3 LiFePO4 84
5 PAN/LiClO4/ graphene oxide 4×104 (30 ℃) 4.3 0.42 LiFePO4 85
6 PAN/LiTFSI/SiO2 1.8×104 (60 ℃) 4.8 0.47 LiFePO4 86
7 PAN/SiO2/LiTFSI/EMIMTFSI 3.5×104 (20 ℃) 5.2 0.52 LiFePO4/NCM622 22
8 SNE@SAG/PAN 7.45×104 (30 ℃) 5 0.7 NCM811 87
Fig. 5 ( a ) Synthetic routes of the PAN in situ; ( b ) Schematic illustration of the composite SPE with SiO2 networks[22]. Copyright 2022, Elsevier
Fig. 6 ( a ) The function mechanism of PAN-modified SCN electrolyte interphase on the surface of LLZTO electrolyte[94]. Copyright 2021, Wiley ( b )1H NMR spectra of PAN and PAN with different amounts of LLZTO; ( c ) Schematic illustration showing the interparticle Li+ transport in the bulk of the composite electrolyte[95]. Copyright 2021, American Chemical Society
Fig. 7 (a) Schematic diagram of the heterogeneous multilayered solid electrolyte[96]. Copyright 2019, Wiley (b) Illustrations of the solid full battery with pristine LATP and DPCE[97]. Copyright 2019, American Chemical Society. (c) Schematic diagram of the NCM622‖heterogeneous dual-layered electrolyte membrane‖Li battery[98]. Copyright 2021, Elsevier. (d) Schematic illustration of the preparation process for SPE membrane[99]. Copyright 2021, Elsevier. (e) The preparation diagram of the double-layer UFF/ PEO/PAN/LiTFSI SPE[100]. Copyright 2021, Wiley
Fig. 8 Schematic illustrations of the micro-wetting design in a solid- state battery using thin and high-strength PAN network infused with PEO/LiTFSI electrolyte (PLN). (a) A schematic diagram of the battery assembly; (b) the position of the liquid electrolyte and the vapor generation process; (c) the mixed solvent forming fast-ion-transport channels at the internal PAN/PEO interface inside PLN; (d) the adsorption of TFSI- anions by the PAN network; (e) LiPO2F2, as the decomposition product of the electrolyte vapor, is generated at the external anode/electrolyte interface[103]. Copyright 2021, Royal Society of Chemistry
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