Investigating the solid electrolyte interphase using binder-free graphite electrodes

Kang, Suk Hoon; Abraham, Daniel P.; Xiao, Ang; Lucht, Brett L.

doi:10.1016/j.jpowsour.2007.08.112

Cited by 147 publications

(128 citation statements)

References 28 publications

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“…These carbonyl-rich oligomers may be responsible for the higher graphite impedance in the LiBOB and LiBOB additive cells because the SEI formed on graphite edge planes (the sites of lithium intercalation) is mainly responsible for impeding Li + motion. The graphite SEI in LiF 2 OB electrolyte is believed to contain lithium alkyl carbonates, lithium alkoxides and alkyl esters of oxalic acid (or lithium oxalate) [28]. The significantly lower graphite impedance in the LiF 2 OB and LiF 2 OB additive cells evidently reflects the effect of fluorine in modifying the SEI at the graphite edge planes.…”

Section: Discussionmentioning

confidence: 99%

Effect of electrolyte composition on initial cycling and impedance characteristics of lithium-ion cells

Abraham

Furczon

Kang

et al. 2008

Journal of Power Sources

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105

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Section: Discussionmentioning

confidence: 99%

Effect of electrolyte composition on initial cycling and impedance characteristics of lithium-ion cells

Abraham

Furczon

Kang

et al. 2008

Journal of Power Sources

Self Cite

105

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“…5 This advance is also due to the use of novel experimental techniques such as solid state NMR and TEM. 6,7 The focus of these studies are the standard LiPF 6 /organic carbonate mixtures on graphite and silicon anodes.…”

mentioning

confidence: 99%

Revealing SEI Morphology: In-Depth Analysis of a Modeling Approach

Single

Horstmann

Latz

2017

J. Electrochem. Soc.

101

132

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In this article, we present a novel theory for the long term evolution of the solid electrolyte interphase (SEI) in lithium-ion batteries and propose novel validation measurements. Both SEI thickness and morphology are predicted by our model as we take into account two transport mechanisms, i.e., solvent diffusion in the SEI pores and charge transport in the solid SEI phase. We show that a porous SEI is created due to the interplay of these transport mechanisms. Different dual layer SEIs emerge from different electrolyte decomposition reactions. We reveal the behavior of such dual layer structures and discuss its dependence on system parameters. Model analysis enables us to interpret SEI thickness fluctuations and link them to the rate-limiting transport mechanism. Our results are general and independent of specific modeling choices, e.g., for charge transport and reduction reactions. In the near future, automotive and mobile applications demand power storage with large energy and power density. Currently, lithiumion batteries (LIBs) are the technology of choice for devices with these demands. They operate at high cell potentials and offer high specific capacities while providing long lifetimes. The latter is a consequence of the stable chemistry of modern LIB systems. A significant part of this stability can be attributed to the passivation ability of the solid electrolyte interphase (SEI). This thin layer forms between the negative electrode and the electrolyte. Hence contact between these phases is prevented and the continuous reduction of electrolyte molecules is suppressed. These reduction processes occur because the operating potential of the negative electrode lies well below the stability window of the electrolyte.1 They are suppressed because reduction products quickly form the SEI during the first charge of a pristine electrode. The self passivating ability is one of the most important distinctions between a well and a badly performing lithium-ion battery chemistry. It is of such importance because the reduction reactions consume lithium-ions, directly reducing battery capacity. However, a real SEI is not perfectly passivating and electrolyte reduction is never completely suppressed. Consequently, the lifetime of a battery is directly related to the long-term passivating ability of the SEI.Numerous studies on SEI have been conducted since Peled reported on this correlation in 1979.2 Most of these studies are experimental, investigating cycling stability as well as SEI impedance and composition. Theoretical studies are scarce in comparison, despite established methods such as DFT and DFT/MD derivatives. This can be partially explained with the chemical diversity of SEI, which has been investigated by Aurbach et al. for decades. Results are summarized in Refs. 3, 4 and include the study of SEI formation on graphite electrodes in organic solvent mixtures. The most significant finding of this time is that ethylene carbonate (EC) forms a stable SEI on graphite as opposed to propylene carbonate (PC). Another...

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“…Figure 8 shows the XPS spectra of the graphite electrodes after cycling tests in different electrolytes. In the C1s spectra, the peak binding energy at 284.8 eV is the C-H bond, which is attributable to alcohol lithium, alkyl esters, or alkyl lithium carbonate [17]. The peak binding energy at 287.9 eV is attributable to the OCO 2 bond from R-CH 2 OCO 2 Li, which was present only in the samples with 0.06 and 0.09 wt% KPF 6 [14].…”

Section: Ftir Analysismentioning

confidence: 97%

“…The P2p spectra of the graphite electrodes contain two characteristic peaks at 136.9 and 133.5 eV, which correspond to the P-F bond of LiPF 6 and the P-O bond of Li x PO y F z , respectively [17,24,25]. The two peak positions clearly differ in the P2p spectrum with 0.09 wt% KPF 6 in the electrolyte.…”

Section: Xps Analysismentioning

confidence: 99%

“…Figure 9 shows the X-ray diffraction (XRD) spectra of the graphite electrodes after cycling tests in different electrolytes. The characteristic diffraction peaks of the graphite material are the (002) peak, (100) peak, (101) peak, and (004) peak [17,26]. The (002) peak reflects the structure of the carbon material, so we can use the change in the (002) peak to analyze the structure of the carbon material.…”

Section: Xps Analysismentioning

confidence: 99%

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Effects of KPF6 on the electrochemical performance of natural graphite/Li

Wei

Qin

Zhang

et al. 2015

Ionics

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Lithium hexafluorophosphate (LiPF 6 ) is the best electrolyte for lithium-ion batteries because of its excellent performance. The conversion of KPF 6 into LiPF 6 is a green chemical process. However, KPF 6 residues are introduced into the electrolyte during the preparation process. In this study, we evaluated the effects of KPF 6 on the electrochemical performance of natural graphite/Li. The results of a cycling test showed that as the KPF 6 content increased in the electrolyte, the specific capacity of the graphite electrode also increased gradually. The impedance of a solid electrolyte interphase (SEI) film was decreased by the addition of KPF 6 . Cyclic voltammograms showed that the addition of KPF 6 had no effects on the insertion and extraction reactions of lithium ions on the graphite electrode. Analyses of the graphite electrodes using scanning electron microscopy, X-ray diffraction analysis, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy suggested that the addition of 0.09 and 0.2 wt% KPF 6 did not change the main components of the SEI film, but the ROCO 2 Li content decreased and the Li 2 CO 3 content increased. Therefore, the electrochemical performance of the graphite electrode was improved by lithiumion migration on the SEI film, which protected the graphite layer.

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Investigating the solid electrolyte interphase using binder-free graphite electrodes

Cited by 147 publications

References 28 publications

Effect of electrolyte composition on initial cycling and impedance characteristics of lithium-ion cells

Effect of electrolyte composition on initial cycling and impedance characteristics of lithium-ion cells

Revealing SEI Morphology: In-Depth Analysis of a Modeling Approach

Effects of KPF6 on the electrochemical performance of natural graphite/Li

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