Response to Comment on “Self‐Suppression of Lithium Dendrite in All‐Solid‐State Lithium Metal Batteries with Poly(vinylidene difluoride)‐Based Solid Electrolytes”

Zhang, Xue; Wang, Shuo; Xue, Chuanjiao; Xin, Chengzhou; Lin, Yuanhua; Shen, Yang; Li, Liangliang; Nan, Ce‐Wen

doi:10.1002/adma.202000026

Cited by 45 publications

(37 citation statements)

References 17 publications

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“…The band for Li + •••OCN coordination (bound DMF) appears at ≈670 cm −1 , while that of uncoordinated OCN (free DMF) in pure DMF is at 656.9 cm −1 (Figure 1d). [20] With molar fraction of LiTFSI increasing, intensity of free DMF is gradually suppressed. Particularly, detectable free DMF is almost not presented at n = 2 and 3.…”

Section: Resultsmentioning

confidence: 99%

Quasi‐Ionic Liquid Enabling Single‐Phase Poly(vinylidene fluoride)‐Based Polymer Electrolytes for Solid‐State LiNi_0.6Co_0.2Mn_0.2O₂||Li Batteries with Rigid‐Flexible Coupling Interphase

et al. 2021

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Poly(vinylidene fluoride)‐based polymer electrolytes are being intensely investigated for solid‐state lithium metal batteries. However, phase separation and porous structures are still pronounced issues in traditional preparing procedure. Herein, a bottom‐to‐up strategy is employed to design single‐phase and densified polymer electrolytes via incorporating quasi‐ionic liquid with poly(vinylidene fluoride‐co‐hexafluoropropylene). Due to strong ion/dipole–dipole interaction, the optimized polymer electrolyte delivers high room‐temperature ionic conductivity of 1.55 × 10−3 S cm−1, superior thermal and oxidation stability of 4.97 V, excellent stretchability of over 1500% and toughness of 43 MJ cm−3 as well as desirable self‐extinguishing ability. Furthermore, the superb compatibility toward Li anode enables over 3000 h cycling of Li plating/stripping and ≈98% Coulombic efficiency in Li||Cu test at 0.1 mA cm−2. In particular, lithium metal battery Li||LiNi0.6Co0.2Mn0.2O2 exhibits a room‐temperature discharge retention rate of 96% after 500 cycles under a rate of 0.1 C, which is associated with the rigid‐flexible coupling electrodes/electrolytes interphase. This investigation demonstrates the potential application of quasi‐ionic liquid/polymer electrolytes in safe lithium metal batteries.

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Section: Resultsmentioning

confidence: 99%

Quasi‐Ionic Liquid Enabling Single‐Phase Poly(vinylidene fluoride)‐Based Polymer Electrolytes for Solid‐State LiNi_0.6Co_0.2Mn_0.2O₂||Li Batteries with Rigid‐Flexible Coupling Interphase

et al. 2021

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“…More importantly, no Raman and FITR signal from free DMF was observed in PVHLi-x electrolyte membranes (Figure S3c,d), suggesting that these electrolyte membranes do not contain free solvent and the residual DMF exists in the bound form. [49] This is exactly the reason why our PISSE is still solid-state. Moreover, the mechanical behavior of PVHLi-1.1 was tested and shown in Figure 3 c.…”

Section: Resultsmentioning

confidence: 86%

Designing Polymer‐in‐Salt Electrolyte and Fully Infiltrated 3D Electrode for Integrated Solid‐State Lithium Batteries

Liu

et al. 2021

Angewandte Chemie

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Solid-state lithium batteries (SSLBs) are promising owing to enhanced safety and high energy density but plagued by the relatively low ionic conductivity of solid-state electrolytes and large electrolyte-electrode interfacial resistance. Herein, we design a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based polymer-in-salt solid electrolyte (PISSE) with high room-temperature ionic conductivity (1.24 10 À4 S cm À1 ) and construct a model integrated TiO 2 /Li SSLB with 3D fully infiltration of solid electrolyte. With forming aggregated ion clusters, unique ionic channels are generated in the PISSE, providing much faster Li + transport than common polymer electrolytes. The integrated device achieves maximized interfacial contact and electrochemical and mechanical stability, with performance close to liquid electrolyte. A pouch cell made of 2 SSLB units in series shows high voltage plateau (3.7 V) and volumetric energy density comparable to many commercial thin-film batteries.

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“…S9). Although this phenomenon remains unclear [50,51], we postulate that this type of CPE is a solid electrolyte, not a gel (Fig. S10).…”

Section: Articles Science China Materialsmentioning

confidence: 91%

Modulating composite polymer electrolyte by lithium closo-borohydride achieves highly stable solid-state battery at 25°C

et al. 2021

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Rational composite design is highly important for the development of high-performance composite polymer electrolytes (CPEs) for solid-state lithium (Li) metal batteries. In this work, Li closo-borohydride, Li 2 B 12 H 12 , is introduced to poly(vinylidene fluoride)-Li-bis-(trifluoromethanesulfonyl) imide (PVDF-LiTFSI) with a bound N-methyl pyrrolidone plasticizer to form a novel CPE. This CPE shows superb Li + conduction properties, as evidenced by its conductivity of 1.43 × 10 −4 S cm −1 and Li + transference number of 0.34 at 25°C. Density functional theory calculations reveal that Li 2 B 12 H 12 , which features electron-deficient multicenter bonds, can facilitate the dissociation of LiTFSI and enhance the immobilization of TFSI to improve the Li + conduction properties of the CPE. Moreover, the fabricated CPE exhibits excellent electrochemical, thermal, and mechanical stability. The addition of Li 2 B 12 H 12 can help form a protective layer at the anode/ electrolyte interface, thereby preventing unwanted reactions. The above benefits of the fabricated CPE contribute to the high compatibility of the electrode. Symmetric Li cells can be stably cycled at 0.2 mA cm −2 for over 1200 h, and Li||LiFePO 4 cells can deliver a reversible specific capacity of 140 mA h g −1 after 200 cycles at 1 C at 25°C with a capacity retention of 98%.

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Response to Comment on “Self‐Suppression of Lithium Dendrite in All‐Solid‐State Lithium Metal Batteries with Poly(vinylidene difluoride)‐Based Solid Electrolytes”

Cited by 45 publications

References 17 publications

Quasi‐Ionic Liquid Enabling Single‐Phase Poly(vinylidene fluoride)‐Based Polymer Electrolytes for Solid‐State LiNi_0.6Co_0.2Mn_0.2O₂||Li Batteries with Rigid‐Flexible Coupling Interphase

Quasi‐Ionic Liquid Enabling Single‐Phase Poly(vinylidene fluoride)‐Based Polymer Electrolytes for Solid‐State LiNi_0.6Co_0.2Mn_0.2O₂||Li Batteries with Rigid‐Flexible Coupling Interphase

Designing Polymer‐in‐Salt Electrolyte and Fully Infiltrated 3D Electrode for Integrated Solid‐State Lithium Batteries

Modulating composite polymer electrolyte by lithium closo-borohydride achieves highly stable solid-state battery at 25°C

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Response to Comment on “Self‐Suppression of Lithium Dendrite in All‐Solid‐State Lithium Metal Batteries with Poly(vinylidene difluoride)‐Based Solid Electrolytes”

Cited by 45 publications

References 17 publications

Quasi‐Ionic Liquid Enabling Single‐Phase Poly(vinylidene fluoride)‐Based Polymer Electrolytes for Solid‐State LiNi0.6Co0.2Mn0.2O2||Li Batteries with Rigid‐Flexible Coupling Interphase

Quasi‐Ionic Liquid Enabling Single‐Phase Poly(vinylidene fluoride)‐Based Polymer Electrolytes for Solid‐State LiNi0.6Co0.2Mn0.2O2||Li Batteries with Rigid‐Flexible Coupling Interphase

Designing Polymer‐in‐Salt Electrolyte and Fully Infiltrated 3D Electrode for Integrated Solid‐State Lithium Batteries

Modulating composite polymer electrolyte by lithium closo-borohydride achieves highly stable solid-state battery at 25°C

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Quasi‐Ionic Liquid Enabling Single‐Phase Poly(vinylidene fluoride)‐Based Polymer Electrolytes for Solid‐State LiNi_0.6Co_0.2Mn_0.2O₂||Li Batteries with Rigid‐Flexible Coupling Interphase

Quasi‐Ionic Liquid Enabling Single‐Phase Poly(vinylidene fluoride)‐Based Polymer Electrolytes for Solid‐State LiNi_0.6Co_0.2Mn_0.2O₂||Li Batteries with Rigid‐Flexible Coupling Interphase