An<i>in situ</i>formed copolymer electrolyte with high ionic conductivity and high lithium-ion transference number for dendrite-free solid-state lithium metal batteries

Ren, Zhiheng; Li, Jixiao; Cai, Ming; Yin, Ruo-Nan; Liang, Jianneng; Zhang, Qianling; He, Chuanxin; Jiang, Xiantao; Ren, Xiangzhong

doi:10.1039/d2ta07516d

Cited by 33 publications

(28 citation statements)

References 72 publications

(109 reference statements)

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“…Figure 3h statistically compares the reported performance of PDOL-based solidstate batteries in terms of ionic conductivity and lithium transference number. [19,24,[32][33][34][35][36][37][38] From the comparison of these DOLbased electrolytes, it is clear that our work has high ionic conductivity and high lithium mobility, which is a significant improvement over previously published work, and that this hybrid crosslinked solid electrolyte provides new research ideas for high performance solid-state battery.…”

Section: + Transport Properties Of Hcpementioning

confidence: 90%

Hybrid Crosslinked Solid Polymer Electrolyte via In‐Situ Solidification Enables High‐Performance Solid‐State Lithium Metal Batteries

Wang

Dong

et al. 2023

Advanced Materials

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Solid‐state lithium‐metal batteries constructed by in‐situ solidification of cyclic ether, are considered to be a critical strategy for the next generation of solid‐state batteries with high energy density and safety. However, the poor thermal/electrochemical stability of linear polyethers and severe interfacial reactions limit its further development. Herein, in‐situ ring‐opening hybrid crosslinked polymerization is proposed for organic/inorganic hybrid polymer electrolyte (HCPE) with superior ionic conductivity of 2.22×10−3 S cm−1 at 30°C, ultrahigh Li+ transference number of 0.88, and wide electrochemical stability window of 5.2 V. These allow highly stable lithium stripping/plating cycling for over 1000 h at 1 mA cm−2, which also reveal a well‐defined interfacial stabilization mechanism. Thus HCPE endows assembled solid‐state lithium‐metal batteries with excellent long‐cycle performance over 600 cycles at 2 C (25°C) and superior capacity retention of 92.1%. More importantly, our proposed non‐combustible HCPE opens up a new frontier to promote the practical application of high safety and high energy density solid‐state batteries via in‐situ solidification.This article is protected by copyright. All rights reserved

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Section: + Transport Properties Of Hcpementioning

confidence: 90%

Hybrid Crosslinked Solid Polymer Electrolyte via In‐Situ Solidification Enables High‐Performance Solid‐State Lithium Metal Batteries

Wang

Dong

et al. 2023

Advanced Materials

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“…It is important to note that poly(DOL‐TTE) exhibited quite well electrochemical stability to lithium metal, the symmetrical cells maintained stable voltage profiles for 2000 h at a current density of 0.5 mA cm − 2 . In a report by Ren et al, [ 71 ] DOL and 1,3,5‐trioxane (trioxymethylene) (TXE) were randomly polymerized into linear copolymers. Copolymerization changed the structure of the PDOL chain and reduced the crystallinity of PDOL‐based SPEs, thus poly(DOL‐TXE) SPEs had a high room temperature ionic conductivity of 4.06 × 10 −4 S cm −1 after adding SN as a plasticizer.…”

Section: In Situ Polymerized Spesmentioning

confidence: 99%

“…Copolymerizing several monomers into linear polymers or cross-linked polymers has attracted extensive attention due to its designability. [67,[69][70][71] Wen et al [67] proposed a novel strategy to construct an ultrathin cross-linked SPE via copolymerization (Figure 6F). The cross-linked SPE was prepared by in situ copolymerization of DOL and trimethylolpropane triglycidyl ether (TTE) under the catalysis of Lewis acid LiBF 4 .…”

Section: 3-dioxanementioning

confidence: 99%

Progress and perspectives of in situ polymerization method for lithium‐based batteries

Xiao

Hao

Bai

et al. 2023

Interdisciplinary Materials

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The application of lithium-based batteries is challenged by the safety issues of leakage and flammability of liquid electrolytes. Polymer electrolytes (PEs) can address issues to promote the practical use of lithium metal batteries.However, the traditional preparation of PEs such as the solution-casting method requires a complicated preparation process, especially resulting in side solvents evaporation issues. The large thickness of traditional PEs reduces the energy density of the battery and increases the transport bottlenecks of lithium-ion. Meanwhile, it is difficult to fill the voids of electrodes to achieve good contact between electrolyte and electrode. In situ polymerization appears as a facile method to prepare PEs possessing excellent interfacial compatibility with electrodes. Thus, thin and uniform electrolytes can be obtained. The interfacial impedance can be reduced, and the lithium-ion transport throughput at the interface can be increased. The typical in situ polymerization process is to implant a precursor solution containing monomers into the cell and then in situ solidify the precursor under specific initiating conditions, and has been widely applied for the preparation of PEs and battery assembly. In this review, we focus on the preparation and application of in situ polymerization method in gel polymer electrolytes, solid polymer electrolytes, and composite polymer electrolytes, in which different kinds of monomers and reactions for in situ polymerization are discussed. In addition, the various compositions and structures of inorganic fillers, and their effects on the electrochemical properties are summarized. Finally, challenges and perspectives for the practical application of in situ polymerization methods in solidstate lithium-based batteries are reviewed.

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“…[82] For example, through the ROP of 1,3-dioxolane and 1,3,5-trioxane, the lithium-ion migration number of the corresponding SPE has been significantly improved. [83] A comprehensive analysis of Table 4 shows that a very rich variety of monomers has been developed, and a series of SPEs with tunable properties have been obtained by ring opening of monomers triggered by different types of initiators. Among them, the SPEs prepared based on 1,3-dioxolane show the best performance overall and have been extensively studied.…”

Section: History and Trends Of Rop In Preparing Spesmentioning

confidence: 99%

Designing Polymer Electrolytes via Ring‐Opening Polymerization for Advanced Lithium Batteries

Wang,

Zhang,

Zeng

et al. 2023

Advanced Energy Materials

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Replacing liquid electrolytes with solid‐state polymer electrolytes (SPEs) can solve the safety hazards of Li metal batteries (LMBs) while increasing their energy density. However, there has been limited success so far in preparing advanced SPEs with controllable molecular structure and chemical composition, posing great obstacles to further promoting its application in LMBs. Recently, ring‐opening polymerization (ROP), including cationic ROP, anionic ROP, and ring‐opening metathesis polymerization, has become a dazzling new star in achieving SPEs due to its mild polymerization conditions and controllable chemical composition (molecular structure, functional group), etc. Besides, there is no small molecule released during the polymerization process, which means reduced interfacial side reaction. Hence, in this review, the merits of ROP in preparing SPEs and its mechanism as well as interfering factors, etc are evaluated from the perspective of synthetic chemistry. Furthermore, the review focuses on outlining the existing cases related to ROP as much as possible and summarize them from different ring structures (from triple ring to multivariate ring) and polymerization methods, hoping to provide a comprehensive understanding and serve as strategic guidance for designing high‐performance SPEs. Challenges and opportunities regarding this burgeoning field are also discussed at the end.

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Anin situformed copolymer electrolyte with high ionic conductivity and high lithium-ion transference number for dendrite-free solid-state lithium metal batteries

Abstract: Polymer electrolytes (PEs) synthesized from in-situ polymerization strategy are considered as the promising candidates to improve the interfacial compatibility, however, most in-situ formed PEs still face problems such as low...

Cited by 33 publications

References 72 publications

Hybrid Crosslinked Solid Polymer Electrolyte via In‐Situ Solidification Enables High‐Performance Solid‐State Lithium Metal Batteries

Hybrid Crosslinked Solid Polymer Electrolyte via In‐Situ Solidification Enables High‐Performance Solid‐State Lithium Metal Batteries

Progress and perspectives of in situ polymerization method for lithium‐based batteries

Designing Polymer Electrolytes via Ring‐Opening Polymerization for Advanced Lithium Batteries

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