On the first coordination shell of lithium ion in linear carbonate solvents as electrolyte model for lithium-ion batteries: a computational study

Ashassi-Sorkhabi, Habib; Kazempour, Amir; Salehi-Abar, Parvin

doi:10.1007/s11581-019-02918-5

Cited by 2 publications

(2 citation statements)

References 11 publications

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“…The electrolytes containing 1 M salts had similar 𝑤 + (Fig. 3E), consistent with their similar Li + solvation numbers (~4) in carbonate solvents (51)(52)(53)(54). Interestingly, decreasing the LiPF6 concentration in EMC:EC 7:3 from 2 M to 0.02 M (Fig.…”

Section: Data and Materials Availabilitysupporting

confidence: 68%

Lithium-ion intercalation by coupled ion-electron transfer

Zhang,

Fraggedakis,

Gao

et al. 2024

Preprint

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Lithium-ion batteries are powering a revolution in electrification, but the underlying intercalation mechanism at the electrified interface remains poorly understood. Here, we provide experimental and theoretical evidence that lithium intercalation occurs by coupled ion-electron transfer (CIET), in which classical ion transfer from the electrolyte is coupled with quantum-mechanical electron transfer from the electrode to form an ion-electron pair in the reduced state. Current-voltage responses and reaction-limited capacities, corresponding to small and large overpotentials, respectively, were measured for common electrode materials and linked by the theory. The experiments showed universal dependence of the (de-)intercalation rate on Li-ion filling fraction, as well as temperature and electrolyte effects consistent with the theory. These results could be used to guide the design of high-rate battery interfaces that maximize the CIET reaction-limited current.

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Section: Data and Materials Availabilitysupporting

confidence: 68%

Lithium-ion intercalation by coupled ion-electron transfer

Zhang,

Fraggedakis,

Gao

et al. 2024

Preprint

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“…Based on this understanding, we speculate that an AI-ISC structure may be formed in the electrolytes even using high-coordination-number solvents (HCNSs) if adding a certain amount of low-coordination-number solvents (LCNSs) to Li + into the electrolytes, in which the anions could be induced into the first solvation sheath of Li + due to the incomplete coordination of solvent molecules . In principle, many linear carbonates or ethers have low polarities and low permittivity, possibly being used as a low CN (usually ≤3) solvent to induce the formation of an AI-ISC structure in electrolytes. − Thus, we can modulate the electrochemical stability window of an electrolyte by creating an AI-ISC structure in the electrolyte through adjusting the CNs of solvents and cosolvents. This new strategy could be considered as a CN rule, with which the electrochemical compatibility of electrolytes can be tuned by appropriate matching of HCNSs with LCNSs.…”

mentioning

confidence: 99%

Designing Advanced Electrolytes for Lithium Secondary Batteries Based on the Coordination Number Rule

Liu¹,

Shen²,

Luo³

et al. 2021

ACS Energy Lett.

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Advanced electrolytes play a key role in the development of next-generation lithium secondary batteries. However, many strong polar solvents, as a major component of the electrolyte, are incompatible with the commercialized graphite anode in Li-ion batteries. In this work, we propose a new concept of the coordination number (CN) rule to tune electrochemical compatibility of electrolytes by regulating the ion–solvent-coordinated (ISC) structure. Based on this rule, we introduced the low-coordination-number solvents (LCNSs) into the high-coordination-number solvent (HCNS) electrolytes to induce anions into the first solvation shell of Li+, forming the anion-induced ISC (AI-ISC) structure. The HCNS-LCNS electrolytes with the AI-ISC structure show enhanced reduction stability, enabling reversible lithiation/delithiation of the graphite anode. Infrared analysis and theoretical calculations confirm the working mechanism of the electrochemical compatibility in the HCNS-LCNS electrolytes based on the CN rule. Therefore, the CN rule provides guidance for the design of highly stable and multifunctional electrolytes to develop next-generation lithium secondary batteries.

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On the first coordination shell of lithium ion in linear carbonate solvents as electrolyte model for lithium-ion batteries: a computational study

Cited by 2 publications

References 11 publications

Lithium-ion intercalation by coupled ion-electron transfer

Lithium-ion intercalation by coupled ion-electron transfer

Designing Advanced Electrolytes for Lithium Secondary Batteries Based on the Coordination Number Rule

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