Li−N Interaction Induced Deep Eutectic Gel Polymer Electrolyte for High Performance Lithium‐Metal Batteries

Pei, Xiaopeng; Li, Yiju; Ou, Ting; Liang, Xuechen; Yang, Yun; Jia, Erna; Tan, Ying; Guo, Shaojun

doi:10.1002/ange.202205075

Cited by 9 publications

(2 citation statements)

References 56 publications

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“…35). To the best of our knowledge, the electrochemical performances of our developed Li||PDTL||NCM811 and Li||PDTL||Li cells largely outperform the other recently reported solid-state batteries 6,25,[39][40][41][42][43][44][45][46] (Fig. 4h and Supplementary Table 1).…”

Section: Electrochemical Performances Of the Pdtl-based Batteriesmentioning

confidence: 53%

Trace weak solvation environment enabling ultra-stable high-voltage solid-state lithium metal battery

Yang

Jiao

et al. 2022

Preprint

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Poly(vinylidene fluoride) (PVDF)-based solid-state electrolytes with “Li salt-polymer-trace residual solvent” configuration are the most promising candidates for room-temperature solid-state batteries. However, we reveal that an unstable high concentration [Li(N, N-dimethylformamide (DMF))x]+ solution structure is locally aggregated in PVDF matrix acting as solid diluent, which presents strong intermolecular interactions with PVDF that greatly restricts the high throughput ion transport and interfacial stability. Here, we propose a universal strategy to construct stable weakened solvation environment by partially replacing the DMF using 2,2,2-trifluoroacetamide (TFA). The TFA presents much lower binding energy with both Li+ and PVDF than DMF, which synchronously achieve high ionic conductivity (7.0×10-4 S cm-1) and Li transference number (0.67) of PVDF-based electrolyte. The TFA can also tailor the solvation structures to form abundant contact ion pairs and aggregates that generate inorganic-rich interfaces to greatly enhance the stability with both Li metal anode and high voltage cathode. The developed composite electrolyte enables record cycling of 2890 and 600 hours in solid-state Li||Li symmetric cells at 0.5 mA cm-2 and 1 mA cm-2, respectively. The solid-state Li||LiNi0.8Co0.1Mn0.1O2 full cells show ultra-long lifespan of 4900 and 3000 times with cut-off voltage of 4.3 V and 4.5 V, respectively, and deliver superior stability under practical conditions from -20 to 45 °C and pouch cell level.

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Section: Electrochemical Performances Of the Pdtl-based Batteriesmentioning

confidence: 53%

Trace weak solvation environment enabling ultra-stable high-voltage solid-state lithium metal battery

Yang

Jiao

et al. 2022

Preprint

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“…Finally, DFT calculations were employed to further investigate the interaction between the polymer and lithium salt within the PEA-based PE. 67,68 The optimized geometric structure of PEA with Li + has two configurations (Figure 6a). One is that Li + complexes with two carbonyl groups in the chain, i.e., Li + -PEA-(C�O) 2 .…”

mentioning

confidence: 99%

In Situ Formed Poly(ester-alt-acetal) Electrolytes with High Oxidation Potential and Electrode–Electrolyte Interface Stability

Guo,

Liu,

Cao

et al. 2023

ACS Energy Lett.

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Eutectogel Electrolyte Constructs Robust Interfaces for High‐Voltage Safe Lithium Metal Battery

Wu,

Li,

Gao

et al. 2024

Advanced Science

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Dramatic growth of lithium dendrite, structural deterioration of LiCoO2 (LCO) cathode at high voltages, and unstable electrode/electrolyte interfaces pose significant obstacles to the practical application of high‐energy‐density LCO||Li batteries. In this work, a novel eutectogel electrolyte is developed by confining the nonflammable eutectic electrolyte in a polymer matrix. The eutectogel electrolyte can construct a robust solid electrolyte interphase (SEI) with inorganic‐rich LiF and Li3N, contributing to a uniform Li deposition. Besides, the severe interface side reactions between LCO cathode and electrolyte can be retarded with an in situ formed protective layer. Correspondingly, Li||Li symmetrical cells achieve highly reversible Li plating/stripping over 1000 h. The LCO||Li full cell can maintain 72.5% capacity after 1500 cycles with a decay rate of only 0.018% per cycle at a high charging voltage of 4.45 V. Moreover, the well‐designed eutectogel electrolyte can even enable the stable operation of LCO at an extremely high cutoff voltage of 4.6 V. This work introduces a promising avenue for the advancement of eutectogel electrolytes, the nonflammable nature and well‐regulated interphase significantly push forward the future application of lithium metal batteries and high‐voltage utilization of LCO cathode.

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Li−N Interaction Induced Deep Eutectic Gel Polymer Electrolyte for High Performance Lithium‐Metal Batteries

Cited by 9 publications

References 56 publications

Trace weak solvation environment enabling ultra-stable high-voltage solid-state lithium metal battery

Trace weak solvation environment enabling ultra-stable high-voltage solid-state lithium metal battery

In Situ Formed Poly(ester-alt-acetal) Electrolytes with High Oxidation Potential and Electrode–Electrolyte Interface Stability

Eutectogel Electrolyte Constructs Robust Interfaces for High‐Voltage Safe Lithium Metal Battery

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