Electrochemical reduction of an anion for ionic-liquid molecules on a lithium electrode studied by first-principles calculations

Ando, Yasunobu; Kawamura, Yoshiumi; Ikeshoji, Tamio; Otani, Minoru

doi:10.1016/j.cplett.2014.08.028

Cited by 22 publications

(27 citation statements)

References 25 publications

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“…Such a peak was recently obtained also upon stepwise deposition of Li onto an adsorbed IL (sub)monolayer on HOPG under UHV conditions, where details about the decomposition mechanism were revealed by a combined computational analysis . The formation of LiF as decomposition product is also in excellent agreement with ab initio molecular dynamic simulations by Ando and co‐workers, which included electric field effects. These authors predicted that [TFSI] − is reduced on a lithium electrode independently of the applied potential.…”

Section: Resultssupporting

confidence: 68%

Surface Science and Electrochemical Model Studies on the Interaction of Graphite and Li‐Containing Ionic Liquids

et al. 2020

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Section: Resultssupporting

confidence: 68%

Surface Science and Electrochemical Model Studies on the Interaction of Graphite and Li‐Containing Ionic Liquids

et al. 2020

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“…results in products of 56 In a computational study, using ab initio molecular dynamic simulations with electric fields, Ando et al predicted that [TFSI]is reduced on lithium independent of the applied potential, resulting in the formation of LiF. 57 Despite of these results, however, the fundamental understanding of the interaction of ILs and Li adsorbed on single crystalline electrode surfaces is rare.…”

Section: Considering the Interaction Of LI With Ils Aurbach Et Al Smentioning

confidence: 99%

Structure formation and surface chemistry of ionic liquids on model electrode surfaces—Model studies for the electrode | electrolyte interface in Li-ion batteries

Büchner

Uhl

Forster-Tonigold

et al. 2018

The Journal of Chemical Physics

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Ionic liquids (ILs) are considered as attractive electrolyte solvents in modern battery concepts such as Li-ion batteries. Here we present a comprehensive review of the results of previous model studies on the interaction of the battery relevant IL 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide ([BMP]+[TFSI]−) with a series of structurally and chemically well-defined model electrode surfaces, which are increasingly complex and relevant for battery applications [Ag(111), Au(111), Cu(111), pristine and lithiated highly oriented pyrolytic graphite (HOPG), and rutile TiO2(110)]. Combining surface science techniques such as high resolution scanning tunneling microscopy and X-ray photoelectron spectroscopy for characterizing surface structure and chemical composition in deposited (sub-)monolayer adlayers with dispersion corrected density functional theory based calculations, this work aims at a molecular scale understanding of the fundamental processes at the electrode | electrolyte interface, which are crucial for the development of the so-called solid electrolyte interphase (SEI) layer in batteries. Performed under idealized conditions, in an ultrahigh vacuum environment, these model studies provide detailed insights on the structure formation in the adlayer, the substrate–adsorbate and adsorbate–adsorbate interactions responsible for this, and the tendency for chemically induced decomposition of the IL. To mimic the situation in an electrolyte, we also investigated the interaction of adsorbed IL (sub-)monolayers with coadsorbed lithium. Even at 80 K, postdeposited Li is found to react with the IL, leading to decomposition products such as LiF, Li3N, Li2S, LixSOy, and Li2O. In the absence of a [BMP]+[TFSI]− adlayer, it tends to adsorb, dissolve, or intercalate into the substrate (metals, HOPG) or to react with the substrate (TiO2) above a critical temperature, forming LiOx and Ti3+ species in the latter case. Finally, the formation of stable decomposition products was found to sensitively change the equilibrium between surface Li and Li+ intercalated in the bulk, leading to a deintercalation from lithiated HOPG in the presence of an adsorbed IL adlayer at >230 K. Overall, these results provide detailed insights into the surface chemistry at the solid | electrolyte interface and the initial stages of SEI formation at electrode surfaces in the absence of an applied potential, which is essential for the further improvement of future Li-ion batteries.

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“…The ab initio molecular dynamics (AIMD) simulation was combined with ESM model to the problem of oxygen reduction reaction or water splitting on Pt, 277,[364][365][366] hydrogen evolution on Ag, 367 and an ionic liquid on Li. 368 The constant chemical potential scheme was applied to the problem of redox level, 369 Pt electrode, 110 and oxygen evolution reaction pathways. 370 The ESM-RISM was applied to an oxidized Pt, 371 and a graphitic surface.…”

Section: Summary and Remarks For This Sectionmentioning

confidence: 99%

Advances and challenges for experiment and theory for multi-electron multi-proton transfer at electrified solid–liquid interfaces

Sakaushi

Kumeda

Hammes‐Schiffer

et al. 2020

Phys. Chem. Chem. Phys.

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Electrochemical reduction of an anion for ionic-liquid molecules on a lithium electrode studied by first-principles calculations

Cited by 22 publications

References 25 publications

Surface Science and Electrochemical Model Studies on the Interaction of Graphite and Li‐Containing Ionic Liquids

Surface Science and Electrochemical Model Studies on the Interaction of Graphite and Li‐Containing Ionic Liquids

Structure formation and surface chemistry of ionic liquids on model electrode surfaces—Model studies for the electrode | electrolyte interface in Li-ion batteries

Advances and challenges for experiment and theory for multi-electron multi-proton transfer at electrified solid–liquid interfaces

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