A Review of Polymer‐based Solid‐State Electrolytes for Lithium‐Metal Batteries: Structure, Kinetic, Interface Stability, and Application

Zhao, Xiaoxue; Wang, Chao; Liu, Hong; Liang, Yuhao; Fan, Li‐Zhen

doi:10.1002/batt.202200502

Cited by 22 publications

(13 citation statements)

References 170 publications

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“…Li-ion transference number (t Li + ) is a crucial parameter for polymer electrolytes because the high t Li + can decrease the electrode polarization and promote the uniform deposition of Li + . [19] Figure 3a demonstrates the time-dependent response of the direct-current polarization and electrochemical impedance spectra before and after chronoamperometry. The calculated t Li + of PAN 1.2 -SPE is 0.55, indicating that the high ionic conductivity is mainly contributed by lithium-ion migration.…”

Section: Methodsmentioning

confidence: 99%

Eutectic‐Based Polymer Electrolyte with the Enhanced Lithium Salt Dissociation for High‐Performance Lithium Metal Batteries

Zhang,

Liu,

Sun

et al. 2023

Angew Chem Int Ed

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The deployment of lithium metal anode in solid‐state batteries with polymer electrolytes has been recognized as a promising approach to achieving high‐energy‐density technologies. However, the practical application of the polymer electrolytes is currently constrained by various challenges, including low ionic conductivity, inadequate electrochemical window, and poor interface stability. To address these issues, a novel eutectic‐based polymer electrolyte consisting of succinonitrile (SN) and poly (ethylene glycol) methyl ether acrylate (PEGMEA) is developed. The research results demonstrate that the interactions between SN and PEGMEA promote the dissociation of the lithium difluoro(oxalato) borate (LiDFOB) salt and increase the concentration of free Li+. The well‐designed eutectic‐based PAN1.2‐SPE (PEGMEA: SN=1: 1.2 mass ratio) exhibits high ionic conductivity of 1.30 mS cm−1 at 30 °C and superior interface stability with Li anode. The Li/Li symmetric cell based on PAN1.2‐SPE enables long‐term plating/stripping at 0.3 and 0.5 mA cm−2, and the Li/LiFePO4 cell achieves superior long‐term cycling stability (capacity retention of 80.3 % after 1500 cycles). Moreover, Li/LiFePO4 and Li/LiNi0.6Co0.2Mn0.2O2 pouch cells employing PAN1.2‐SPE demonstrate excellent cycling and safety characteristics. This study presents a new pathway for designing high‐performance polymer electrolytes and promotes the practical application of high‐stable lithium metal batteries.

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Section: Methodsmentioning

confidence: 99%

Eutectic‐Based Polymer Electrolyte with the Enhanced Lithium Salt Dissociation for High‐Performance Lithium Metal Batteries

Zhang,

Liu,

Sun

et al. 2023

Angew Chem Int Ed

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“…9 To be used in batteries, solid electrolytes must have conductivity values higher than 10 −4 S cm −1 at room temperature, wide chemical and electrochemical stability, good processability, and high elastic modulus to block dendrites growth. 10 At the same time, they must allow the formation of a stable solid electrolyte interface (SEI). 11,12 Indeed, among the possible solutions, an interesting class of ion conductors is that of solid polymer electrolytes (SPEs), 13 where a polymer is used both as a physical separator and as a medium to enable the transport of lithium ions.…”

Section: Introductionmentioning

confidence: 99%

“…To this aim, ceramic, polymers, composites, and organic–inorganic hybrids can be exploited . To be used in batteries, solid electrolytes must have conductivity values higher than 10 –4 S cm –1 at room temperature, wide chemical and electrochemical stability, good processability, and high elastic modulus to block dendrites growth . At the same time, they must allow the formation of a stable solid electrolyte interface (SEI). , …”

Section: Introductionmentioning

confidence: 99%

Host–Guest Interactions and Transport Mechanism in Poly(vinylidene fluoride)-Based Quasi-Solid Electrolytes for Lithium Metal Batteries

Vallana,

Carena,

Ceribelli

et al. 2024

ACS Appl. Energy Mater.

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All-solid-state lithium metal batteries (SS-LMBs) are expected to meet the strong requirements of the automotive sector in terms of performance and safety. Among the different solid electrolytes, poly(vinylidene fluoride) (PVDF)-based systems offer good performance in terms of ionic conductivity and stability at the anodic interface. However, despite the high polymer permittivity (ε′ ≈ 10−11) which should allow efficient salt dissociation, there is growing evidence that the ionic transport requires the presence of a non-negligible amount of residual, or permanent, solvent in the membrane. In this paper, we study the Li + transport mechanism in a model system consisting of poly(vinylidene fluoride-cohexafluoropropylene) (PFDF-HFP), lithium bis(fluorosulfonyl)imide (LiFSI) salt, and dimethylformamide (DMF) as permanent solvent, combining a large set of experimental techniques (thermal analysis, NMR, IR and Raman spectroscopy, impedance spectroscopy) and accurate density functional theory (DFT) modeling. We show that Li + −DMF interactions are predominant in these quasi-solid electrolytes (QSEs) and are the basis of the effective ion transport mechanism. Permanent solvent amounts on the order of [DMF]/[Li + ] ∼ 2−3 are required to make QSEs able to practically work in a real environment.

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“…Solid polymer electrolytes (SPEs) have been extensively studied in this field due to their low cost, mechanical flexibility, and excellent large-scale manufacturing processability [ 20 , 21 , 22 ]. However, their low ionic conductivity at room temperature is the main obstacle to their final application, especially for the most typically studied SPE, polyethylene oxide (PEO), as it is required to work above its melting temperature of 65 °C [ 23 , 24 ].…”

Section: Introductionmentioning

confidence: 99%

Dehydrofluorination Process of Poly(vinylidene difluoride) PVdF-Based Gel Polymer Electrolytes and Its Effect on Lithium-Sulfur Batteries

Castillo

Robles-Fernandez

Cid

et al. 2023

Gels

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Gel polymer electrolytes (GPEs) are emerging as suitable candidates for high-performing lithium-sulfur batteries (LSBs) due to their excellent performance and improved safety. Within them, poly(vinylidene difluoride) (PVdF) and its derivatives have been widely used as polymer hosts due to their ideal mechanical and electrochemical properties. However, their poor stability with lithium metal (Li0) anode has been identified as their main drawback. Here, the stability of two PVdF-based GPEs with Li0 and their application in LSBs is studied. PVdF-based GPEs undergo a dehydrofluorination process upon contact with the Li0. This process results in the formation of a LiF-rich solid electrolyte interphase that provides high stability during galvanostatic cycling. Nevertheless, despite their outstanding initial discharge, both GPEs show an unsuitable battery performance characterized by a capacity drop, ascribed to the loss of the lithium polysulfides and their interaction with the dehydrofluorinated polymer host. Through the introduction of an intriguing lithium salt (lithium nitrate) in the electrolyte, a significant improvement is achieved delivering higher capacity retention. Apart from providing a detailed study of the hitherto poorly characterized interaction process between PVdF-based GPEs and the Li0, this study demonstrates the need for an anode protection process to use this type of electrolytes in LSBs.

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A Review of Polymer‐based Solid‐State Electrolytes for Lithium‐Metal Batteries: Structure, Kinetic, Interface Stability, and Application

Cited by 22 publications

References 170 publications

Eutectic‐Based Polymer Electrolyte with the Enhanced Lithium Salt Dissociation for High‐Performance Lithium Metal Batteries

Eutectic‐Based Polymer Electrolyte with the Enhanced Lithium Salt Dissociation for High‐Performance Lithium Metal Batteries

Host–Guest Interactions and Transport Mechanism in Poly(vinylidene fluoride)-Based Quasi-Solid Electrolytes for Lithium Metal Batteries

Dehydrofluorination Process of Poly(vinylidene difluoride) PVdF-Based Gel Polymer Electrolytes and Its Effect on Lithium-Sulfur Batteries

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