Role of Lithium Salt on Solid Electrolyte Interface (SEI) Formation and Structure in Lithium Ion Batteries

Nie, Mengyun; Lucht, Brett L.

doi:10.1149/2.054406jes

Cited by 220 publications

(204 citation statements)

References 36 publications

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“…Therefore, the 'ionicities' of the electrolytes are all lower than that of the LP30 electrolyte and follows the same trend as the conductivity values. [36]. For the LiDFOB electrolyte, the peak is much larger and starts around 1.8 V vs. Li/Li + , which is also similar to what is seen in carbonate-based electrolytes [36].…”

Section: Vtf Fittingsupporting

confidence: 69%

“…[36]. For the LiDFOB electrolyte, the peak is much larger and starts around 1.8 V vs. Li/Li + , which is also similar to what is seen in carbonate-based electrolytes [36]. In this case, the peak has a symmetrical triangular shape that is characteristic of a reduction reaction controlled by the saturation of surface sites.…”

Section: Vtf Fittingsupporting

confidence: 63%

“…where no obvious differences were observed with LiPF6 and LiBF4 electrolytes [36]. All electrolytes but that with LiTDI allows lithium deposition at ca.…”

Section: This Contrasts To What Was Reported In Ec-based Electrolymentioning

confidence: 86%

“…electrolyte without any SEI forming additives [35]. As it is known that the Li salt can have a strong influence on the SEI formation on graphite [36][37][38], we examine here the effect of various lithium salts, (shown in Figure 1a), on the physico-chemical properties of SL:DMC-based electrolytes and assess their suitability for graphite electrode operation.…”

Section: Introductionmentioning

confidence: 99%

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Towards practical sulfolane based electrolytes: Choice of Li salt for graphite electrode operation

Zhang

Porcher

Paillard

2018

Journal of Power Sources

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Abstract:Sulfolane (tetramethylene sulfone, SL) is known for leading to Li-ion electrolytes with high anodic stability. However, the operation of graphite electrodes in alternative electrolytes is usually challenging, especially when ethylene carbonate (EC) is not used as co-solvent. Thus, we study here the influence of the lithium salt on the physico-chemical and electrochemical properties of EC-free SL-based electrolytes and on the performance of graphite electrodes based on carboxymethyl cellulose (CMC). SL mixed with dimethyl carbonate (DMC) leads to electrolytes as conductive as state-of-theart alkyl carbonate-based electrolytes with wide electrochemical stability windows. The compatibility with graphite electrodes depends on the Li salt used and, even though cycling is possible with most salts, lithium difluoro-oxalato borate (LiDFOB) is especially interesting for graphite operation.LiDFOB electrolytes are conductive at room temperature (ca. 6 mS cm -1 ) with an anodic stability slightly below 5 V vs. Li/Li + on particulate carbon black electrodes. In addition, it allows cycling graphite electrodes with steady capacity and high coulombic efficiency without any additive. The testing of graphite electrodes in half-cells is, however, problematic with SL:DMC mixtures and, by switching the Li metal counter electrode for LiFePO4, the graphite electrode achieves better practical performance in terms of rate capability.

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Section: Vtf Fittingsupporting

confidence: 69%

Section: Vtf Fittingsupporting

confidence: 63%

“…where no obvious differences were observed with LiPF6 and LiBF4 electrolytes [36]. All electrolytes but that with LiTDI allows lithium deposition at ca.…”

Section: This Contrasts To What Was Reported In Ec-based Electrolymentioning

confidence: 86%

Section: Introductionmentioning

confidence: 99%

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Towards practical sulfolane based electrolytes: Choice of Li salt for graphite electrode operation

Zhang

Porcher

Paillard

2018

Journal of Power Sources

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“…Considering the electrolyte volume 120 μl LP57 at a density of 1.2 g/cm 3 and the EC to EMC ratio of 3/7 wt/wt, the amount of EC in the cell amounts to 43.2 mg. With the molecular weight of EC (88 g/mol) that number translates into 419 μmol of EC. Assuming that two reduced EC molecules recombine to release one C 2 H 4 molecule, 12 we can conclude that 2 · 0.75 μmol = 1.50 μmol of EC were reduced during the first negative going scan. Consequently, the evolution of 2000 ppm C 2 H 4 corresponds to a breakdown of 1.50 μmol / 491 μmol = 0.3% of the total amount of EC in the cell.…”

Section: Discussionmentioning

confidence: 95%

Gas Evolution at Graphite Anodes Depending on Electrolyte Water Content and SEI Quality Studied by On-Line Electrochemical Mass Spectrometry

Bernhard

Metzger

Gasteiger

2015

J. Electrochem. Soc.

153

179

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The gas evolution during the formation of graphite electrodes is quantified by On-line Electrochemical Mass Spectrometry (OEMS) for dry electrolyte (< 20 ppm H 2 O) and 4000 ppm H 2 O containing electrolyte to mimic the effect of trace water during the formation process. While the formation in dry electrolyte mainly shows ethylene (C 2 H 4 ) from the reduction of ethylene carbonate (EC) and small amounts of hydrogen (H 2 ), the formation in water-containing electrolyte yields large amounts of H 2 and considerable amounts of CO 2 in addition to the expected C 2 H 4 evolution. We could show that a protective solid-electrolyte interphase (SEI) layer formed by pre-cycling the graphite electrode in 2% vinylene carbonate (VC) containing electrolyte can reduce the H 2 evolution in watercontaining electrolyte by a factor of 7.5 compared to a pristine graphite electrode. Consequently, the ability of graphite electrodes to form an SEI prevents excessive gassing from trace water, which, e.g., is observed for non-SEI forming lithium titanate ( Today's Li-ion batteries usually employ graphite or lithium titanate Li 4 Ti 5 O 12 (LTO) as anode material. Graphite electrodes are known to have an irreversible capacity loss upon the first charge, i.e., during the first Li + -ion intercalation into the layered graphite structure. 1 This effect is related to the formation of the so called solid-electrolyte interphase (SEI) and depends strongly on the electrolyte composition and the electrode potential.2 The capacity loss is explained by the reduction of electrolyte components on the graphite surface, which irreversibly consumes Li + -ions and forms the protective and passivating SEI layer on the negative electrode. On the one hand, the SEI inhibits further reduction reactions on the anode surface due to its electronically insulating nature, on the other hand it is still permeable for Li + -ions, allowing for Li + intercalation. [3][4][5][6][7][8][9][10][11] Recent work by the group of Brett Lucht showed that lithium ethylene dicarbonate (LEDC) and LiF are the main constituents of the SEI layer on graphite, when ethylene carbonate-based electrolytes are used, independent of the type of lithium salt. 12 The main gaseous components formed during electrolyte reduction on graphite anodes are ethylene (C 2 H 4 ), hydrogen (H 2 ) and other hydrocarbons like propylene (depending on the cyclic carbonate, which is used in the electrolyte mixture).13-15 When employing the common alkyl carbonate electrolytes containing ethylene carbonate (EC), dimethylcarbonate (DMC), diethylcarbonate (DEC) and/or ethyl methyl carbonate (EMC) with LiPF 6 , no carbon dioxide (CO 2 ) formation is observed during the SEI formation. 10In contrast to graphite, LTO is generally believed to possess no SEI protection, since its lithiation potential (1.55 V Li ) is too high to allow reduction of electrolyte components. Thus, LTO is more prone to gassing from trace water and other impurities in the alkyl carbonate electrolyte.16 Gassing studies with LTO as anode material...

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Advanced Liquid Electrolytes for Rechargeable Li Metal Batteries

Jie

Ren

Cao

et al. 2020

Adv Funct Materials

249

156

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Rechargeable lithium metal batteries (LMBs) have attracted wide attention for future electric vehicles and next‐generation energy storage because of their exceptionally high specific energy density. Recently, the development of electrode materials for LMBs has been extensively discussed and reviewed in the literature, but there have been very few reports that systematically review the status and progress of electrolytes for such applications. Actually, the viability of practical LMBs critically depends on the development of suitable liquid electrolytes due to the high reactivity of Li metals toward most solvents. This paper provides a systematic summary of the background and recent advances of the electrolytes for LMBs with an emphasis on the thermodynamic and kinetic stabilities at the interfaces. In addition, the emerging advanced characterization techniques for understanding the electrolyte–electrode interfaces are surveyed. Finally, a perspective for future directions is provided.

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Role of Lithium Salt on Solid Electrolyte Interface (SEI) Formation and Structure in Lithium Ion Batteries

Cited by 220 publications

References 36 publications

Towards practical sulfolane based electrolytes: Choice of Li salt for graphite electrode operation

Towards practical sulfolane based electrolytes: Choice of Li salt for graphite electrode operation

Gas Evolution at Graphite Anodes Depending on Electrolyte Water Content and SEI Quality Studied by On-Line Electrochemical Mass Spectrometry

Advanced Liquid Electrolytes for Rechargeable Li Metal Batteries

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