Mechanistic understanding of the correlation between structure and dynamics of liquid carbonate electrolytes: impact of polarization

Maiti, Moumita; Krishnamoorthy, Anand Narayanan; Mabrouk, Youssef; Mozhzhukhina, Nataliia; Xiong, Shizhao; Diddens, Diddo; Heuer, Andreas

doi:10.1039/d3cp01236k

Phys. Chem. Chem. Phys.

2023

DOI: 10.1039/d3cp01236k

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Mechanistic understanding of the correlation between structure and dynamics of liquid carbonate electrolytes: impact of polarization

Moumita Maiti

Anand Narayanan Krishnamoorthy

Youssef Mabrouk

et al.

Abstract: Liquid electrolyte design and modelling is an essential part of the development of improved lithium ion batteries. For mixed organic carbonates (ethylene carbonate (EC) and ethyl-methyl carbonate (EMC) mixtures)-based electrolytes...

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2024

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Cited by 2 publications

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Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte

Shi,

Wang,

Tehrani

et al. 2024

Advanced Science

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Flame‐retardant phosphate‐based electrolytes effectively enhance lithium‐ion battery safety but suffer from poor compatibility with graphite anodes and high‐voltage cathodes, hindering scalability. Fluorinated phosphates, though widely used, increase interfacial resistance at the anode, degrading performance. In this work, carbonate solvents with strong polarity are introduced to prevent tris(2,2,2‐trifluoroethyl) phosphate (TFEP) from participating in the solvation structure of lithium ions. This strategy forms a quasi‐localized high‐concentration solvation structure, thereby restricting the reduction of TFEP and its impact on the graphite anode. The LiNi0.8Mn0.1Co0.1O2 (NCM811) | Graphite (Gr) pouch cell with optimized electrolyte exhibits a capacity retention rate of 80.1% after 370 cycles at 0.5C, which is much more stable than the electrolyte with TFEP‐involved solvation structure (capacity retention rate: 47.1% after 300 cycles). The corresponding pouch cell with cut‐off voltage to 4.5 V exhibits a capacity retention rate of 82.8% after 125 cycles, significantly outperforming cells employing commercial carbonate electrolytes (capacity retention rate: 56.9% after 125 cycles). Thus, the developed quasi‐localized high‐concentration solvation structure can effectively stabilize the electrode interface, greatly enhancing the cycling performance of phosphate‐based flame‐retardant electrolytes.

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Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte

Shi,

Wang,

Tehrani

et al. 2024

Advanced Science

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Exploring the capabilities and limitations of the Van Hove function to understand directional correlations in ion movements within Li-ion battery electrolytes

Mitra,

Biswas

2024

The Journal of Chemical Physics

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Understanding microscopic directional correlations in ion movements within lithium-ion battery (LIB) electrolytes is important because these correlations directly affect the ionic conductivity. Onsager transport coefficients are widely used to understand these correlations. On the other hand, the Van Hove function (VHF) is also capable of determining correlated motions. However, identifying various types of ion correlated motions in LIB electrolytes using VHF is not well explored. Here, we have conducted molecular dynamics simulations of a representative experimental LIB electrolyte system—lithium hexafluorophosphate (LiPF6)—at different concentrations in a (9:1 wt. %) mixture of ethyl methyl carbonate and fluoroethylene carbonate in order to explore the capabilities and limitations of using VHF to understand different types of ion correlations. We conclude that analysis of VHF can qualitatively describe both the positive correlation between cation–anion at different salt concentrations and the negative correlation between cation–cation and anion–anion present in high salt concentration, but it cannot foretell which correlation is dominating at any given electrolyte concentration. This type of quantitative information can be obtained only via Onsager’s approach. This could be seen as a limitation of relying solely on VHF to fully understand ion correlation in electrolyte media.

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Mechanistic understanding of the correlation between structure and dynamics of liquid carbonate electrolytes: impact of polarization

Abstract: Liquid electrolyte design and modelling is an essential part of the development of improved lithium ion batteries. For mixed organic carbonates (ethylene carbonate (EC) and ethyl-methyl carbonate (EMC) mixtures)-based electrolytes...

Cited by 2 publications

References 65 publications

Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte

Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte

Exploring the capabilities and limitations of the Van Hove function to understand directional correlations in ion movements within Li-ion battery electrolytes

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