Dataset Information

Correlative Electrochemical Microscopy for the Elucidation of the Local Ionic and Electronic Properties of the Solid Electrolyte Interphase in Li-Ion Batteries.

ABSTRACT: The solid-electrolyte interphase (SEI) plays a key role in the stability of lithium-ion batteries as the SEI prevents the continuous degradation of the electrolyte at the anode. The SEI acts as an insulating layer for electron transfer, still allowing the ionic flux through the layer. We combine the feedback and multi-frequency alternating-current modes of scanning electrochemical microscopy (SECM) for the first time to assess quantitatively the local electronic and ionic properties of the SEI varying the SEI formation conditions and the used electrolytes in the field of Li-ion batteries (LIB). Correlations between the electronic and ionic properties of the resulting SEI on a model Cu electrode demonstrates the unique feasibility of the proposed strategy to provide the two essential properties of an SEI: ionic and electronic conductivity in dependence on the formation conditions, which is anticipated to exhibit a significant impact on the field of LIBs.

SUBMITTER: Santos CS

PROVIDER: S-EPMC9322322 | biostudies-literature | 2022 Jun

REPOSITORIES: biostudies-literature

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Correlative Electrochemical Microscopy for the Elucidation of the Local Ionic and Electronic Properties of the Solid Electrolyte Interphase in Li-Ion Batteries.

Santos Carla S CS Botz Alexander A Bandarenka Aliaksandr S AS Ventosa Edgar E Schuhmann Wolfgang W

Angewandte Chemie (International ed. in English) 20220505 26

The solid-electrolyte interphase (SEI) plays a key role in the stability of lithium-ion batteries as the SEI prevents the continuous degradation of the electrolyte at the anode. The SEI acts as an insulating layer for electron transfer, still allowing the ionic flux through the layer. We combine the feedback and multi-frequency alternating-current modes of scanning electrochemical microscopy (SECM) for the first time to assess quantitatively the local electronic and ionic properties of the SEI v ...[more]

PMID: 35312219

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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

Correlative Electrochemical Microscopy for the Elucidation of the Local Ionic and Electronic Properties of the Solid Electrolyte Interphase in Li-Ion Batteries.

Publications

Correlative Electrochemical Microscopy for the Elucidation of the Local Ionic and Electronic Properties of the Solid Electrolyte Interphase in Li-Ion Batteries.

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