Thermal and Electrochemical Properties of Solid Polymer Electrolytes Prepared via Lithium Salt-Catalyzed Epoxide Ring Opening Polymerization

Foran, Gabrielle; Verdier, Nina; Lepage, David; Prébé, Arnaud; Aymé‐Perrot, David; Dollé, Mickaël

doi:10.3390/app11041561

Cited by 7 publications

(4 citation statements)

References 88 publications

(290 reference statements)

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“…Since tracking FWHM may not accurately represent changes in lithium mobility as a function of temperature in the SIL, T 1 relaxation times in the ceramic and SIL phases of the liquid–ceramic hybrid solid composite electrolytes were also analyzed (Table ). Decreasing T 1 relaxation is generally indicative of increased mobility as molecular motion provides a mechanism through which relaxation can occur Table ).…”

Section: Resultsmentioning

confidence: 99%

NMR Study of Lithium Transport in Liquid–Ceramic Hybrid Solid Composite Electrolytes

Foran

Méry

Bertrand

et al. 2022

ACS Appl. Mater. Interfaces

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Despite their high conductivity, factors such as being fragile enough to face processing issues and interfacial incompatibility with lithium electrodes are some of the main drawbacks hindering the commercialization of inorganic (mainly oxide-based) solid electrolytes for use in all-solid-state lithium batteries. To this end, strategies such as the addition of solid polymer electrolytes have been proposed to improve the electrode−electrolyte interface. Hybrid electrolytes, which are usually composed of ceramic particles dispersed in a polymer, generally have a better affinity with electrodes and higher ionic conductivity than pure inorganic electrolytes. However, a significant downside of this strategy is that differences in lithium transportability between electrolyte layers can result in the formation of a high interfacial energy barrier across the cell. One strategy to ensure sufficient "wetting" of ceramics is to incorporate a liquid electrolyte directly into the solid inorganic electrolyte resulting in the formation of a hybrid liquid−ceramic electrolyte. To this end, liquid−ceramic hybrid electrolytes were prepared by adding LiG 4 TFSI, a solvate ionic liquid (SIL), to garnet, NASICON, and perovskite-type ceramic electrolytes. Although SIL addition resulted in increased ionic conductivity, comparisons between the pure SIL and the hybrid systems revealed that improvements were due to the SIL alone. A thorough investigation of the hybrid systems by solid-state nuclear magnetic resonance (NMR) revealed little to no lithium exchange between the ceramic and the SIL. This confirms that lithium conductivity preferentially occurs through the SIL in these hybrid systems. The primary role of the ceramic is to provide mechanical strength.

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Section: Resultsmentioning

confidence: 99%

NMR Study of Lithium Transport in Liquid–Ceramic Hybrid Solid Composite Electrolytes

Foran

Méry

Bertrand

et al. 2022

ACS Appl. Mater. Interfaces

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“…Although SPEs can alleviate electrolyte/electrode interface problems to some extent, the poor thermal stability with a generally low ionic conductivity at room temperature limits their commercial application. Even more importantly, CPEs are a class of polymer electrolytes obtained by blending, plasticizing, and compounding with inorganic substances based on polymers. − It is noteworthy that ISEs and SPEs can be combined into CPEs to maximize performance, thus eliminating interface problems with relatively high room temperature conductivity, good processability, and nonflammability . Therefore, it is necessary to review CPEs as promising solid electrolyte materials to summarize the latest development.…”

Section: Introductionmentioning

confidence: 99%

Recent Advances and Future Perspectives of PVDF-Based Composite Polymer Electrolytes for Lithium Metal Batteries: A Review

et al. 2023

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Lithium metal batteries (LMBs) using solid-state electrolytes (SSEs) can achieve dual enhancement of energy density and safety performance and have attracted considerable attention. In spite of their excellent flexibility and processability, poly(vinylidene fluoride) (PVDF)-based electrolytes, regarded as a prominent member of SSEs in LMBs, suffer from low ionic conductivity and high internal resistance. The structure of PVDF-based composite polymer electrolytes (CPEs) allows them to combine the advantages of inorganic components and PVDF substrates. The use of modification and advanced technology can achieve higher mechanical strength and improved electrochemical properties of PVDF-based CPEs, but their practical application still needs to be explored. This paper reviews recent research progress of PVDF-based CPEs in LMBs, focuses on the methods to improve the electrochemical and safety performance of PVDF-based CPEs, and specifically discusses five aspects of properties upgrading as the main line, namely, the ionic conductivity, ion migration properties, mechanical properties, thermal stability, and electrochemical stability windows. Finally, the challenges and application prospects of high-performance PVDF-based CPEs in future development are presented.

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“…Lithium salts can initiate the ring-opening polymerization (ROP) of epoxides due to the lewis-acid characteristics of Li + -details of relevant studies can be found in the supporting information. [14][15][16] LiBF 4 and LiPF 6 are the most efficient lithium salt catalysts as traces of BF 3 and PF 3 form highly reactive species with trace water catalyzing the ROP. 15,17 However, the incompatibility of these lithium salts with aqueous media excludes them from use in WISEs.…”

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confidence: 99%

“…18 Furthermore LiTFSI, has previously been used to create solid polymer electrolytes from epoxide terminated polymers in the bulk state. 14,19 In the present paper, poly(ethylene glycol) diglycidyl ether (PDE) was added into 21 m LiTFSI WISE as a novel additive in order to further reduce free water content. It was found that novel networks based on crosslinked PDE, LiTFSI, and water were formed by taking advantage of the catalytic properties LiTFSI to initiate the epoxide ring-opening polymerization of the PDE end-groups.…”

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confidence: 99%

Self-Crosslinking Poly(Ethylene Glycol) Diglycidyl Ether in Water-in-Salt Electrolytes for Minimal Hydrogen Evolution Reactions and Extended LiTFSI Solubility

Burton¹,

Zhu²,

Droguet³

et al. 2022

J. Electrochem. Soc.

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Water-in-salt electrolytes - WISEs - are prevailing thanks to their compelling extended voltage window due to the reduced free water molecules at the electrode interface. However, as has been reported elsewhere, free-water content still can be reduced further. In our previous work, an unstable phenomenon of solid electrolyte interphase (SEI) and salt precipitation/dissolution issue were revealed. Herein, we propose a novel approach in order to alleviate those issues using poly(ethylene glycol) diglycidyl ether (PDE) as an additive. Indeed, upon mixing LiTFSI, water and PDE at high concentrations, we observed a ring-opening reaction of PDE that was confirmed via Raman spectroscopy, FTIR and ionic conductivity measurements. These crosslinked networks could also increase the solubility limits of LiTFSI in water, which was identified by adding more LiTFSI or LiOTf. Differential scanning calorimetry (DSC) measurement demonstrated that these crosslinked electrolytes effectively suppress the crystallization of water molecules with the WISE. Linear sweep voltammetry (LSV) measurements revealed that these novel crosslinked electrolytes considerably reduce free water content which effectively drives the HER to more negative potentials. More significantly, the SEI formed with these novel electrolytes remains present and stable on the electrode surface after a resting period of 1 h. Our work herein offers a new approach to tackling SEI instability and precipitation/dissolution issues.

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Thermal and Electrochemical Properties of Solid Polymer Electrolytes Prepared via Lithium Salt-Catalyzed Epoxide Ring Opening Polymerization

Cited by 7 publications

References 88 publications

NMR Study of Lithium Transport in Liquid–Ceramic Hybrid Solid Composite Electrolytes

NMR Study of Lithium Transport in Liquid–Ceramic Hybrid Solid Composite Electrolytes

Recent Advances and Future Perspectives of PVDF-Based Composite Polymer Electrolytes for Lithium Metal Batteries: A Review

Self-Crosslinking Poly(Ethylene Glycol) Diglycidyl Ether in Water-in-Salt Electrolytes for Minimal Hydrogen Evolution Reactions and Extended LiTFSI Solubility

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