Elastomeric Electrolytes via Thiourethane Dynamic Chemistry and Hierarchical Hydrogen-Bonding Interactions

Shi, Zhen; Zhou, Hongru; Guo, Kairui; Nie, Hui; Zhou, Xingping; Xue, Zhigang

doi:10.1021/acs.macromol.3c01695

Cited by 3 publications

References 71 publications

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Waterborne Polyurethane Micelles Reinforce PEO‐Based Electrolytes for Lithium Metal Batteries

Shi,

Zhou,

Fan

et al. 2024

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Although solid polymer electrolytes have been developed for several decades, poly(ethylene oxide) (PEO) or polymers with ethoxy (EO) segments are still one of the most promising candidates for advanced batteries. The low ionic conductivity and lithium‐ion transference number as well as the deterioration of mechanical properties after coupling with lithium salts restrict its further adoption. Herein, a serial of PEO‐based composite electrolytes optimized by waterborne polyurethane are prepared via blend method. With the assistance of H2O, ionic type waterborne polyurethane assembles into flexible micelles, in which hydrophobic segments as the core and hydrophilic groups as the shell. Utilizing this feature of waterborne polyurethane, PEO and Li salt (LiTFSI) aqueous solution is slowly added to the organic solution of waterborne polyurethane to compound in situ, and polymer composite electrolytes are fabricated. The multilevel (hydrogen bonds with different binding energy) and multiscale (deformation of flexible micelles) dynamic interaction endows the composite electrolyte with attractive mechanical properties. The assembled Li|Li symmetric battery with the molar ratio of EO to Li salts of 8:1 exhibits excellent cycling stability up to 800 h at 0.1 mA cm−2, and the assembled Li|LiFePO4 battery can be stably cycled at 1C for >400 cycles.

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Waterborne Polyurethane Micelles Reinforce PEO‐Based Electrolytes for Lithium Metal Batteries

Shi,

Zhou,

Fan

et al. 2024

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In Situ Fabrication of Solvent-Free Solid Polymer Electrolytes for Wide-Temperature All-Solid-State Lithium Metal Batteries

Gan,

Cui,

et al. 2024

Langmuir

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All-solid-state lithium metal batteries (ASSLMBs) have been regarded as promising candidates to settle the safety issues of liquid electrolytes for rechargeable lithium batteries. However, the currently reported gel polymer electrolytes still have flammable liquid solvents, thus leading to the potential safety hazard. Here, solvent-free deep eutectic solid polymer electrolytes (SPEs) are designed and fabricated via an in situ polymerization, which are composed of a poly(vinylidene fluoride−hexafluoropropylene) (PVDF−HFP) electrospun membrane, succinonitrile (SN), poly(ethylene glycol) diacrylate (PEGDA200, M n = 200 g mol −1 ), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and lithium difluoro(oxalato)borate (LiDFOB). The deep eutectic solvent (DES) with SN/LiTFSI provides a superior room-temperature ionic conductivity, while the PEGDA200 precursor acts as cross-linking network to form SPEs under thermal initiation for free radical polymerization, and LiDFOB can form a stable solid electrolyte interface (SEI) layer. The PVDF−HFP electrospun membrane with a three-dimensional nanofibrous network structure for SN/PEGDA200/LiTFSI/LiDFOB SPEs exhibits a wide electrochemical stability window, high lithium-ion transference number, and good compatibility with the lithium metal anode. Furthermore, the obtained SPEs assembled with Li//LiMn 0.6 Fe 0.4 PO 4 , Li//LiFePO 4 , and Li//LiNi 0.8 Co 0.1 Mn 0.1 O 2 asymmetric cells show excellent cycling performance and rate capability at a wide temperature. This strategy provides a promising path in designing high-energy-density ASSLMBs for practical application.

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Solvent-Free In-Situ Polymerization for Wide Temperature All-Solid-State Lithium Metal Batteries Enabled by Dilithium Salt of Litfsi and Lidfob

Gan,

Cui,

et al. 2024

Preprint

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Elastomeric Electrolytes via Thiourethane Dynamic Chemistry and Hierarchical Hydrogen-Bonding Interactions

Cited by 3 publications

References 71 publications

Waterborne Polyurethane Micelles Reinforce PEO‐Based Electrolytes for Lithium Metal Batteries

Waterborne Polyurethane Micelles Reinforce PEO‐Based Electrolytes for Lithium Metal Batteries

In Situ Fabrication of Solvent-Free Solid Polymer Electrolytes for Wide-Temperature All-Solid-State Lithium Metal Batteries

Solvent-Free In-Situ Polymerization for Wide Temperature All-Solid-State Lithium Metal Batteries Enabled by Dilithium Salt of Litfsi and Lidfob

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