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化学进展 2023, Vol. 35 Issue (11): 1625-1637 DOI: 10.7536/PC230324 前一篇   后一篇

• 综述 •

固态钠离子电池用PEO基聚合物固体电解质

赵兰清1, 侯敏杰1, 张达1,2,3,*(), 周英杰1, 解志鹏1, 梁风1,2,3,*()   

  1. 1 昆明理工大学 云南省有色金属真空冶金重点实验室 昆明 650093
    2 昆明理工大学 真空冶金国家工程研究中心 昆明 650093
    3 昆明理工大学 冶金与能源工程学院 昆明 650093
  • 收稿日期:2023-03-27 修回日期:2023-07-12 出版日期:2023-11-24 发布日期:2023-08-07
  • 通讯作者: 张达, 梁风
  • 作者简介:

    张达 昆明理工大学讲师,2021年博士毕业于昆明理工大学冶金与能源工程学院,主要从事纳米材料的等离子体制备和改性、新能源材料与器件等方面的研究。

    梁风 昆明理工大学教授,博士生导师,日本九州大学客座教授。博士毕业于日本东京工业大学,入选“国家高层次人才”青年学者、国家人力资源与社会保障部资助高层次留学回国人才计划、云南省高端科技人才、云南省兴滇英才计划-产业创新人才等多项人才计划。主要从事高能量密度储能器件(固态电池、金属空气电池等)开发等离子体制备和改性能源材料等方面的研究。

  • 基金资助:
    国家自然科学基金项目(12175089); 国家自然科学基金项目(12205127); 云南省重点研发计划项目(202103AF140006); 云南省基础研究计划项目(202001AW070004); 云南省基础研究计划项目(202301AS070051); 云南省基础研究计划项目(202301AU070064); 云南省重大科技计划项目(202202AG050003)
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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:2023-03-27 Revised:2023-07-12 Online:2023-11-24 Published:2023-08-07
  • 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)

固态钠离子电池采用固体电解质替代传统有机电解液,具有安全性能高、能量密度高和循环寿命长等优点,被认为是大规模储能应用中最有前景的候选电池之一。在众多固体电解质材料中,聚环氧乙烷(PEO)基聚合物固体电解质因安全性高、成本低、能量密度高、电化学稳定性好、对钠盐溶解度高等特点,被认为是极具前景的固体电解质材料。然而环氧乙烷(EO)链段的高结晶度导致其室温离子电导率低而无法满足实际应用。为此研究人员采用不同策略来降低PEO基聚合物固体电解质的结晶度以提高其离子电导率,常见方法包括聚合物嵌段共聚、共混、交联、添加增塑剂和添加无机填料。本文对PEO基聚合物固体电解质的物理化学性质、制备工艺及上述改性技术进行了评价,并综述了PEO基聚合物固体电解质最新研究进展。

关键词： 固态钠离子电池, 固体电解质, 聚环氧乙烷, 制备方法, 改性策略

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
()
表1 常用聚合物基体优缺点对比
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
图1 (a)PEO及PEO基CPE结构示意图[16];(b)Na+在结晶PEO中的缓慢迁移[16]
Fig.1 (a) Structure diagram of PEO and PEO based CPE[16]; (b) The slow migration of Na+ in crystalline PEO[16]
图2 (a)聚合物基固态钠离子电池示意图[13];(b)固态钠离子电池聚合物固体电解质内聚合物相[28]
Fig.2 (a) Schematic of polymer-based solid sodium ion battery[13] and (b) Polymer phase in polymer solid electrolyte[28]
图3 PEO聚合物固体电解质中Na+传输机制[28]
Fig.3 Mechanism of sodium ion transport in PEO[28]
图4 (a)21-β-CD-g-PTFEMA新型聚合物的合成路径[49];(b)密度泛函理论(DFT)分析最高占据分子轨道(HOMO)和不同聚合物单元的电子云密度分布概率[49];(c)非晶态PPC和NASICON颗粒掺入结晶PEO基体中的CPE优化示意图[51];(d)Na-CMC为骨架的三维交联结构SPE的高倍FESEM[55];(e)Na|SPE|Na3V2(PO4)3电池在1 C倍率下的比容量和库仑效率曲线[56]
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]
表2 基于聚合物共混、嵌段共聚、交联改性固体电解质离子电导率对比
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
表3 基于添加增塑剂改性聚合物固体电解质离子电导率对比
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
图5 (a)PEO/NaPO3和PEO/NaPO3 + 50%(质量分数)PEG SPE的DSC曲线[58];(b)PEO-PAM共混电解质体系中添加(EC + PC)混合增塑剂的离子电导率[64];(c)PEO/NaClO4/EC-PC SPE的合成示意图[65];(d)具有紧密界面接触的双层PEO-SN-NaClO4|NZSP-NSO电解质[66];(e)NZP-PEO和NZP-PEO@IL CPEs的Na+传导途径示意图[69];(f)PEO/NaClO4-Pyr13FSI SPE组成结构及FSI-阴离子与PEO链相互作用的示意图[70]
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]
图6 (a)溶液浇铸法制备PEO/PVP/NaPO3/Al2O3 CPE示意图[74];(b)Na3PS4-PEO CPE结构示意图及其在全固态电池中的电化学性能[86];(c)PEO-NZTO CPE的数码照片和背散射电子图像[87];(d)Na|PEO-NZTO|NVP全固态电池在80℃,0.2 C倍率下恒流充放电循环过程中的比容量[87];(e)PEO-NaClO4-NASICON CPE组成示意图及其在全固态电池中的电化学性能[88]
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]
表4 基于复合聚合物固体电解质离子电导率对比
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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