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Research Progress and Challenges of Solid-State Electrolytes for Polymer Lithium Metal Batteries AITranslate

Lingjuan Wang1; Guorui Liu1; Jiamin Fan1; Fengzhang Tu2; Zhuangzhuang Zhang1;
1.College of Chemistry and Chemical Engineering，Henan Normal University，Xinxiang 453007，China
2.Fujian Provincial Key Laboratory of Clean Energy Materials，Longyan University，Longyan 364012，China
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Abstract AITranslate

In recent years, electrochemical energy storage has undergone significant advancements, with lithium-ion batteries gaining widespread application in various electronic devices and the automotive sector. As a critical component of battery architecture, conventional liquid electrolytes are predominantly organic solvents, which introduce safety concerns such as leakage and volatilization. In contrast, solid-state electrolytes have garnered considerable attention due to their enhanced safety, superior interfacial contact, ease of processing, and numerous other advantages. Solid-state polymer electrolytes have been shown to exhibit excellent flexibility and ease of processing. These advantages can enhance the poor interfacial contact between the electrolyte and the electrode. It has led to their emergence as a key focus area in research related to lithium metal batteries. However, the deficiencies of low ionic conductivity of polymer electrolytes, reduced mechanical properties after conductivity increase, and low lithium-ion mobility number limit its practical application. So many scholars have devoted themselves to the study of improving the ionic conductivity of polymer electrolytes. Solid-state batteries have a long history of development and many advantages. Lithium-ion batteries are highly efficient energy storage devices, but due to the limited capacity of the anode graphite, there is a need for high-energy-density batteries, which has led to a resurgence of interest in lithium metal batteries. Solid electrolytes can be divided into inorganic solid electrolytes, organic polymer electrolytes, and composite polymer-based electrolytes. While organic polymer electrolytes possess numerous advantageous characteristics, their low level of ionic conductivity has restricted their development and application. However, analyzing the studies on the ionic conduction mechanism of polymer electrolytes, it can be seen that the widely accepted mechanism is that ion transfer is achieved by the jump of lithium ions between coordination sites on the polymer chain segments and the movement of lithium ions along with the polymer chain segments. In addition, a series of research models for the mechanism have been proposed by many scholars. Currently, most researchers tend to believe that the ion transport process mainly takes place in the amorphous region. It has been established that increasing the ambient temperature results in the formation of an amorphous region within the electrolyte, thereby facilitating the movement of polymer chain segments and enhancing ionic conductivity. Consequently, the primary considerations for the design of polymer electrolytes with high ionic conductivity are the reduction of crystallinity, the decrease of glass transition temperature, and the promotion of ionic dissociation. Polymer solid electrolytes comprise a dual composition, incorporating lithium salts and polymer matrices. In this configuration, the lithium salt fulfils the role of a carrier. The electrolyte's conductivity, being of an ionically conductive nature, is primarily influenced by the lithium salt's dissociation and the flexibility of the polymer chain. Therefore, the judicious selection of a polymer matrix becomes imperative. The most common substances used as polymer matrix are poly （ethylene oxide） （PEO）, polyacrylonitrile （PAN）, polyvinylidene fluoride （PVDF）, and other polymers, each of which has its own advantages and disadvantages. The high crystallinity of PEO is not conducive to Li+ conduction at room temperature, so the main direction of thinking to improve the lithium ionic conductivity of PEO-based electrolytes is to reduce the crystallinity of PEO. While PAN has good mechanical strength and a wide electrochemical window, it is very incompatible with lithium electrodes, and a serious passivation reaction occurs after contacting with a lithium metal anode. The PVDF-based polymer electrolyte has a polar lithiophilic group C-F so it can dissolve lithium salts. But as a semi-crystalline polymer, it is difficult to achieve high ionic conductivity, hexafluoropropylene is introduced into the PVDF chain segment to reduce the crystallinity of PVDF itself.However, the presence of spherical particles in the PVDF-HFP-based polymer electrolyte results in a gap in the middle, thus hindering lithium-ion transport. PMMA is a lightweight and transparent polymer with low interfacial impedance between the gel electrolyte and the lithium electrode prepared on its substrate, but it suffers from low ionic conductivity at room temperature. In addition to these popular groups, there are also polycarbonate groups, silicone groups, and others. The paper focuses on the research progress of modification strategies such as interfacial optimization, construction of frameworks, and addition of fillers in different polymer matrices to compensate for the shortcomings of various polymer matrices. This review concluded with a summary of the various polymer electrolyte preparation methods, including solution casting, phase transition, in-situ polymerization, ultraviolet curing, and electrostatic spinning. Different preparation methods also had a certain effect on the ionic conductivity. There were some problems of poor interfacial contact and residual solvent side reactions brought by the non-in-situ polymerization method. The in-situ polymerization method could solve these problems by injecting the liquid precursor solution into Li-ion battery and then initiating the polymerization of the precursor solution in a specific environment. Finally, the future research directions were analyzed in the light of the future development of solid polymer electrolytes, and the application needed in lithium metal batteries：in-depth study of the ionic conduction mechanism in solid polymer electrolytes； improvement of ionic conductivity； interface engineering breakthroughs； and solid-state battery industrialization exploration.

KeyWords AITranslate

ionic conductivity solid polymer electrolyte lithium metal battery lithium-ion conduction high energy density

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Basic Information:

DOI：10.13373/j.cnki.cjrm.XY25030021

Chinese Library Classification Number:TK91

Citation Information:

In recent years, electrochemical energy storage has undergone significant advancements, with lithium-ion batteries gaining widespread application in various electronic devices and the automotive sector. As a critical component of battery architecture, conventional liquid electrolytes are predominantly organic solvents, which introduce safety concerns such as leakage and volatilization. In contrast, solid-state electrolytes have garnered considerable attention due to their enhanced safety, superior interfacial contact, ease of processing, and numerous other advantages. Solid-state polymer electrolytes have been shown to exhibit excellent flexibility and ease of processing. These advantages can enhance the poor interfacial contact between the electrolyte and the electrode. It has led to their emergence as a key focus area in research related to lithium metal batteries. However, the deficiencies of low ionic conductivity of polymer electrolytes, reduced mechanical properties after conductivity increase, and low lithium-ion mobility number limit its practical application. So many scholars have devoted themselves to the study of improving the ionic conductivity of polymer electrolytes. Solid-state batteries have a long history of development and many advantages. Lithium-ion batteries are highly efficient energy storage devices, but due to the limited capacity of the anode graphite, there is a need for high-energy-density batteries, which has led to a resurgence of interest in lithium metal batteries. Solid electrolytes can be divided into inorganic solid electrolytes, organic polymer electrolytes, and composite polymer-based electrolytes. While organic polymer electrolytes possess numerous advantageous characteristics, their low level of ionic conductivity has restricted their development and application. However, analyzing the studies on the ionic conduction mechanism of polymer electrolytes, it can be seen that the widely accepted mechanism is that ion transfer is achieved by the jump of lithium ions between coordination sites on the polymer chain segments and the movement of lithium ions along with the polymer chain segments. In addition, a series of research models for the mechanism have been proposed by many scholars. Currently, most researchers tend to believe that the ion transport process mainly takes place in the amorphous region. It has been established that increasing the ambient temperature results in the formation of an amorphous region within the electrolyte, thereby facilitating the movement of polymer chain segments and enhancing ionic conductivity. Consequently, the primary considerations for the design of polymer electrolytes with high ionic conductivity are the reduction of crystallinity, the decrease of glass transition temperature, and the promotion of ionic dissociation. Polymer solid electrolytes comprise a dual composition, incorporating lithium salts and polymer matrices. In this configuration, the lithium salt fulfils the role of a carrier. The electrolyte's conductivity, being of an ionically conductive nature, is primarily influenced by the lithium salt's dissociation and the flexibility of the polymer chain. Therefore, the judicious selection of a polymer matrix becomes imperative. The most common substances used as polymer matrix are poly （ethylene oxide） （PEO）, polyacrylonitrile （PAN）, polyvinylidene fluoride （PVDF）, and other polymers, each of which has its own advantages and disadvantages. The high crystallinity of PEO is not conducive to Li+ conduction at room temperature, so the main direction of thinking to improve the lithium ionic conductivity of PEO-based electrolytes is to reduce the crystallinity of PEO. While PAN has good mechanical strength and a wide electrochemical window, it is very incompatible with lithium electrodes, and a serious passivation reaction occurs after contacting with a lithium metal anode. The PVDF-based polymer electrolyte has a polar lithiophilic group C-F so it can dissolve lithium salts. But as a semi-crystalline polymer, it is difficult to achieve high ionic conductivity, hexafluoropropylene is introduced into the PVDF chain segment to reduce the crystallinity of PVDF itself.However, the presence of spherical particles in the PVDF-HFP-based polymer electrolyte results in a gap in the middle, thus hindering lithium-ion transport. PMMA is a lightweight and transparent polymer with low interfacial impedance between the gel electrolyte and the lithium electrode prepared on its substrate, but it suffers from low ionic conductivity at room temperature. In addition to these popular groups, there are also polycarbonate groups, silicone groups, and others. The paper focuses on the research progress of modification strategies such as interfacial optimization, construction of frameworks, and addition of fillers in different polymer matrices to compensate for the shortcomings of various polymer matrices. This review concluded with a summary of the various polymer electrolyte preparation methods, including solution casting, phase transition, in-situ polymerization, ultraviolet curing, and electrostatic spinning. Different preparation methods also had a certain effect on the ionic conductivity. There were some problems of poor interfacial contact and residual solvent side reactions brought by the non-in-situ polymerization method. The in-situ polymerization method could solve these problems by injecting the liquid precursor solution into Li-ion battery and then initiating the polymerization of the precursor solution in a specific environment. Finally, the future research directions were analyzed in the light of the future development of solid polymer electrolytes, and the application needed in lithium metal batteries：in-depth study of the ionic conduction mechanism in solid polymer electrolytes； improvement of ionic conductivity； interface engineering breakthroughs； and solid-state battery industrialization exploration.

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GB/T 7714-2015 [1] Lingjuan Wang, Guorui Liu, Jiamin Fan, et al. Research Progress and Challenges of Solid-State Electrolytes for Polymer Lithium Metal Batteries[J]. Chinese Journal of Rare Metals, 2026, 50(8): 1361-1375. DOI:10.13373/j.cnki.cjrm.XY25030021.
MLA [1] Lingjuan Wang, et al., "Research Progress and Challenges of Solid-State Electrolytes for Polymer Lithium Metal Batteries." Chinese Journal of Rare Metals, vol. 50, no. 8, 2026, pp. 1361-1375, https://doi.org/10.13373/j.cnki.cjrm.XY25030021.
APA [1] Lingjuan Wang, Guorui Liu, Jiamin Fan, Fengzhang Tu, & Zhuangzhuang Zhang. (2026). Research Progress and Challenges of Solid-State Electrolytes for Polymer Lithium Metal Batteries. Chinese Journal of Rare Metals, 50(8), 1361-1375. https://doi.org/10.13373/j.cnki.cjrm.XY25030021
IEEE [1] Lingjuan Wang, Guorui Liu, Jiamin Fan, Fengzhang Tu, and Zhuangzhuang Zhang, "Research Progress and Challenges of Solid-State Electrolytes for Polymer Lithium Metal Batteries," Chinese Journal of Rare Metals, vol. 50, no. 8, pp. 1361-1375, 2026, doi: 10.13373/j.cnki.cjrm.XY25030021. keywords: {ionic conductivity;solid polymer electrolyte;lithium metal battery;lithium-ion conduction;high energy density}