Dataset Information

High-Efficacy and Polymeric Solid-Electrolyte Interphase for Closely Packed Li Electrodeposition.

ABSTRACT: The industrial application of lithium metal anode requires less side reaction between active lithium and electrolyte, which demands the sustainability of the electrolyte-induced solid-electrolyte interface. Here, through a new diluted lithium difluoro(oxalato)borate-based (LiDFOB) high concentration electrolyte system, it is found that the oxidation behavior of aggregated LiDFOB salt has a great impact on solid-electrolyte interphase (SEI) formation and Li reversibility. Under the operation window of Cu/LiNi_0.8Co_0.1Mn_0.1O₂ full cells (rather than Li/Cu configuration), a polyether/coordinated borate containing solid-electrolyte interphase with inner Li₂O crystalline can be observed with the increasing concentration of salt, which can be ascribed to the reaction between aggregated electron-deficient borate species and electron-rich alkoxide SEI components. The high Li reversibility (99.34%) and near-theoretical lithium deposition enable the stable cycling of LiNi_0.8Co_0.1Mn_0.1O₂/Li cells (N/P < 2, 350 Wh kg^-1) under high cutoff voltage condition of 4.6 V and lean electrolyte condition (E/C ≈ 3.2 g Ah^-1).

SUBMITTER: Li S

PROVIDER: S-EPMC7967057 | biostudies-literature | 2021 Mar

REPOSITORIES: biostudies-literature

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High-Efficacy and Polymeric Solid-Electrolyte Interphase for Closely Packed Li Electrodeposition.

Li Siyuan S Liu Qilei Q Zhang Weidong W Fan Lei L Wang Xinyang X Wang Xiao X Shen Zeyu Z Zang Xiaoxian X Zhao Yu Y Ma Fuyuan F Lu Yingying Y

Advanced science (Weinheim, Baden-Wurttemberg, Germany) 20210129 6

The industrial application of lithium metal anode requires less side reaction between active lithium and electrolyte, which demands the sustainability of the electrolyte-induced solid-electrolyte interface. Here, through a new diluted lithium difluoro(oxalato)borate-based (LiDFOB) high concentration electrolyte system, it is found that the oxidation behavior of aggregated LiDFOB salt has a great impact on solid-electrolyte interphase (SEI) formation and Li reversibility. Under the operation wind ...[more]

PMID: 33747731

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Project description:Fluorinated electrolytes based on fluoroethylene carbonate (FEC) have been considered as promising alternative electrolytes for high-voltage and high-energy capacity lithium-ion batteries (LIBs). However, the compatibility of the fluorinated electrolytes with graphite negative electrodes is unclear. In this paper, we have systematically investigated, for the first time, the stability of fluorinated electrolytes with graphite negative electrodes, and the result shows that unlike the ethylene carbonate (EC)-based electrolyte, the FEC-based electrolyte (EC was totally replaced by FEC) is incapable of forming a protective and effective solid electrolyte interphase (SEI) that protects the electrolyte from runaway reduction on the graphite surface. The reason is that the lowest unoccupied molecular orbital energy levels are also lowered by the introduction of fluorine into the solvent, and the FEC solvent has poorer resistance against reduction, leading to instability on the graphite negative electrode. To tackle this problem, two lithium salts of lithium bis(oxalato)borate and lithium difluoro(oxalato)borate (LiDFOB) have been investigated as negative-electrode film-forming additives. Incorporation of only 0.5 wt % LiDFOB to a FEC-based electrolyte [1.0 M LiPF6 in 3:7 (FEC-ethyl methyl carbonate)] results in excellent cycling performance of the graphite negative electrode. This improved property originates from the generation of a thinner and better quality SEI film with little LiF by the sacrificial reduction of the LiDFOB additive on the graphite negative electrode surface. On the other hand, this additive can stabilize the electrolyte by scavenging HF. Meanwhile, the incorporated LiDFOB additive has positive influence on the interphase layer on the positive electrode surface and significantly decreases the amount of HF formation, finally leading to improved cycling stability and rate capability of LiNi0.5Mn1.5O4 electrodes at a high cutoff voltage of 5 V. The data demonstrate that the LiDFOB additive not only exhibits a superior compatibility with graphite but also improves the electrochemical properties of high-voltage spinel LiNi0.5Mn1.5O4 positive electrodes considerably, confirming its potential as a prospective, multifunctional additive for 5 V fluorinated electrolytes in high-energy capacity lithium-ion batteries (LIBs).

Dataset Information

High-Efficacy and Polymeric Solid-Electrolyte Interphase for Closely Packed Li Electrodeposition.

Publications

High-Efficacy and Polymeric Solid-Electrolyte Interphase for Closely Packed Li Electrodeposition.

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