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Progress in Chemistry 2023, Vol. 35 Issue (11): 1625-1637 DOI: 10.7536/PC230324 Previous Articles   Next Articles

• Review •

Poly(Ethylene Oxide)-Based Solid Polymer Electrolytes for Solid-State Sodium Ion Batteries

Zhao Lanqing1, Hou Minjie1, Zhang Da1,2,3(), Zhou Yingjie1, Xie Zhipeng1, Liang Feng1,2,3()   

  1. 1 Key Laboratory for Nonferrous Vacuum Metallurgy of Yunnan Province, Kunming University of Science and Technology,Kunming 650093, China
    2 National Engineering Research Center of Vacuum Metallurgy, Kunming University of Science and Technology,Kunming 650093, China
    3 Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology,Kunming 650093, China
  • Received: Revised: Online: Published:
  • Contact: Zhang Da, Liang Feng
  • Supported by:
    National Natural Science Foundation of China(12175089); National Natural Science Foundation of China(12205127); Key Research and Development Program of Yunnan Province(202103AF140006); Applied Basic Research Programs of Yunnan Provincial Science and Technology Department(202001AW070004); Applied Basic Research Programs of Yunnan Provincial Science and Technology Department(202301AS070051); Applied Basic Research Programs of Yunnan Provincial Science and Technology Department(202301AU070064); Yunnan Major Scientific and Technological Projects(202202AG050003)
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One of the most promising candidates for large-scale energy storage applications is the solid-state sodium ion battery, which replaces conventional organic liquid electrolytes with solid electrolytes and has the advantages of high safety, high energy density, and extended cycle life. Among many solid electrolyte materials, Poly(ethylene oxide) (PEO)-based polymer solid electrolytes are considered promising solid electrolyte materials because of their high safety, easy manufacturing, low cost, high energy density, favorable electrochemical stability, and excellent solubility in sodium salts. However, the high crystallinity of the ethylene oxide (EO) chain segment results in low ionic conductivity at room temperature, which is unable to meet the requirements of practical application. To overcome the aforementioned limitations, researchers have used a variety of strategies to lessen the crystallinity of PEO-based polymer electrolyte and hence increase its ionic conductivity. Common techniques include polymer block copolymerization, blending, crosslinking, adding plasticizers, and adding inorganic fillers. In the review, the physical and chemical properties, preparation methods, and modification techniques of PEO-based polymer electrolytes are evaluated, and the most recent advancements on PEO-based polymer electrolytes are reviewed.

Contents

1 Introduction

2 PEO-based polymer solid electrolyte

2.1 Physicochemical properties of PEO

2.2 PEO polymer solid electrolyte

2.3 Ion transport mechanism

3 Preparation method of PEO-based polymer solid electrolyte

3.1 Solution casting

3.2 Hot pressing

3.3 Other methods

4 Modification strategy

4.1 Polymer block copolymerization, blending and crosslinking

4.2 Adding plasticizers

4.3 Adding inorganic fillers

5 Conclusion and outlook

Key words: solid-state sodium ion batteries, solid-state electrolytes, poly(ethylene oxide) (PEO), preparation methods, modification strategy
Table 1 Comparison of advantages and disadvantages of common polymer matrix
Polymer matrix Advantages Disadvantages
PEO High safety, good electrochemical stability, low price, good
film forming property		 High crystallinity and low room temperature ionic conductivity
PAN High thermal stability and ionic conductivity Poor mechanical properties, brittle after film formation
PVDF High safety, dielectric constant and oxidation resistance Poor mechanical properties, low ionic conductivity
PVP Good film forming and chemical stability Poor mechanical properties, brittle after film formation
PMMA Good interface stability and low price High crystallinity, Poor mechanical properties and low ionic conductivity
Fig.1 (a) Structure diagram of PEO and PEO based CPE[16]; (b) The slow migration of Na+ in crystalline PEO[16]
Fig.2 (a) Schematic of polymer-based solid sodium ion battery[13] and (b) Polymer phase in polymer solid electrolyte[28]
Fig.3 Mechanism of sodium ion transport in PEO[28]
Fig.4 (a) Synthetic route for 21-β-CD-g-PTFEMA[49]; (b) Density functional theory (DFT) analysis of the highest occupied molecular orbital (HOMO) and probability of electron cloud density distributions for different polymer units[49]; (c) Schematic of the optimizing steps for amorphous PPC and NASICON particles incorporated into the crystalline PEO host[51]; (d) FESEM analysis at high magnification of the three-dimensional cross-linked structure SPE with Na-CMC as the skeleton[55]; (e) Specific capacity and coulombic efficiency curves of Na|SPE|Na3V2(PO4)3 battery cycled at 1 C rate[56]
Table 2 Comparison of ionic conductivity of solid electrolyte modified by polymer blending, block copolymerization and cross-linking
Electrolyte Test temperature/℃ Conductivity/ S·cm-1 Electrode ref
PEO/PVP/NaPO3 RT 1.07×10-5 Na‖(C + I2 + Electrolyte) 48
PEO/ASPE 80 > 10-4 Na‖Na3V2(PO4)3 49
PEO/PVDF/NaClO4/TiO2 RT 8.75×10-5 — 50
PEO/PPC/NASICON 60 1.2×10-5 Na‖Na3V2(PO4)3 51
PEO/PFPE 80 > 10-4 Na‖Na3V2(PO4)3 53
PEO/Na-CMC/NaClO4 55 > 10-5 Na‖NaFePO4 55
PEG/PVDF-HFP 30 2.4×10-4 Na‖NaFePO4 56
Table 3 Comparison of ionic conductivity of solid electrolyte modified by adding plasticizer
Electrolyte Test temperature/℃ Conductivity/ S·cm-1 Electrode ref
PEO/PEG/NaPO3 RT 8.9×10-7 Na‖(C + I2 + PEO) 58
PEO/PEG-NaClO3 30 3.07×10-5 Na‖MnO2 59
PEO/PAM/NaCF3SO3/EC-PC 60 5.74×10-4 — 64
PEO/NaClO4/EC-PC RT 9.5×10-3 — 65
PEO/NaClO4/NZSP/SN 60 2.68×10-4 Na‖Na3V2(PO4)3 66
PEO/NaClO4/NZSP/[Py13]+[NTf2]- RT 1.48×10-4 Na‖Na3V2(PO4)3 69
PEO/NaClO4/Pyr13FSI RT 6.8×10-5 Na‖Na3V2(PO4)3 70
NaTFSI(PEO)n-Pyr13TFSI RT ~10-4 — 71
NaFSI(PEO)n-Pyr13TFSI RT ~10-4 — 71
Fig.5 (a) DSC traces of PEO/NaPO3 and PEO/NaPO3 + 50% PEG SPE[58] ; (b) Ionic conductivity of (EC + PC) mixed plasticizer in PEO-PAM blended electrolyte system[64]; (c) Schematic representation of synthesis route for PEO/NaClO4/EC-PC SPE[65]; (d) The asymmetric PEO-SN-NaClO4|NZSP-NSO SPE with close interface contact[66]; (e) Schematic illustration of the proposed Na+ conduction pathways for the NZP-PEO and NZP-PEO@IL CPEs[69]; (f) Composition of PEO/NaClO4-Pyr13FSI SPE and schematic diagram illustrating the interaction of FSI- anion and PEO chain[70]
Fig.6 (a) Schematic diagram of preparation of PEO/PVP/NaPO3/Al2O3 CPE by solution casting technique[74]; (b) Structure diagram of Na3PS4-PEO CPE and its electrochemical performance in all solid-state batteries[86]; (c) Photograph and back scattered electron image of the PEO/NZTO CPE[87]; (d) Specific capacities of Na|PEO-NZTO|NVP all-solid-state batteries during the galvanostatic charge/discharge cycling at a rate of 0.2 C at 80℃[87]; (e) Schematic diagram of composition of PEO-NaClO4-NASICON CPE and its electrochemical performance in all solid-state batteries[88]
Table 4 Comparison of ionic conductivity based on composite polymer solid electrolyte
Electrolyte Test temperature/℃ Conductivity/ S·cm-1 Electrode Ref
PEO/PVP/NaPO3/Al2O3 RT > 10-5 — 74
PEO/NaClO4/SiO2 RT 7.6×10-6 — 75
PEO/NaPF6/NaAl5O8 70 3.6×10-6 Na‖Na 84
PEO/NaPF6/TiO2 80 2×10-4 Na‖Na3Ti2(PO4)3 85
PEO/NaClO4/Na3PS4 RT 9.5×10-4 Na‖SnS2 86
PEO/NaTFSI/NZTO 80 1×10-3 Na‖Na3V2(PO4)3 87
PEO/NaClO4/NASICON 60 5.6×10-4 Na‖Na2MnFe(CN)6 88
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