Kinetically corrected Monte Carlo-molecular dynamics simulations of solid electrolyte interphase growth

Abbott, Joseph W; Hanke, Felix

doi:10.26434/chemrxiv-2021-l8c7b

Cited by 1 publication

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“…In this work, the EDL is defined as the region within 10.0 Å from the surface of the negatively charged graphene electrode. 40 A species was considered to be located within the EDL if any of the atoms of the species was in the EDL (a distribution near the negatively charged surface is shown as an inset in Figure 1). Since the Li + coordination can increase the reduction voltage of a solvent species dramatically, 24 we analyzed the statistics of the electrolyte in the EDL in terms of (a) solvents/anions coordinated with Li + in the first solvation shell and (b) free solvent/anions species (not coordinated to any Li + ).…”

Section: Simulations Of the Edlmentioning

confidence: 99%

Effect of the Electric Double Layer (EDL) in Multicomponent Electrolyte Reduction and Solid Electrolyte Interphase (SEI) Formation in Lithium Batteries

McDowell

2023

J. Am. Chem. Soc.

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Electrolytes, consisting of salts, solvents, and additives, must form a stable solid electrolyte interphase (SEI) to ensure the performance and durability of lithium(Li)-ion batteries. However, the electric double layer (EDL) structure near charged surfaces is still unsolved, despite its importance in dictating the species being reduced for SEI formation near a negative electrode. In this work, a newly developed model was used to illustrate the effect of EDL on SEI formation in two essential electrolytes, the carbonate-based electrolyte for Li-ion batteries and the ether-based electrolyte for batteries with Li-metal anodes. Both electrolytes have fluoroethylene carbonate (FEC) as a common additive to form the beneficial F-containing SEI component (e.g., LiF). However, the role of FEC drastically differs in these electrolytes. FEC is an effective SEI modifier for the carbonate-based electrolyte by being the only F-containing species entering the EDL and being reduced, as the anion (PF6 –) will not enter the EDL. For the ether-based electrolyte, both the anion (TFSI–) and FEC can enter the EDL and be reduced. The competition of the two species within the EDL due to the surface charge and temperature leads to a unique temperature effect observed in prior experiments: the FEC additive is more effective in modulating SEI components at a low temperature (−40 °C) than at room temperature (20 °C) in the ether-based electrolyte. These collective quantitative agreements with experiments emphasize the importance of incorporating the effect of the EDL in multicomponent electrolyte reduction reactions in simulations/experiments to predict/control the formation of the SEI layer.

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Section: Simulations Of the Edlmentioning

confidence: 99%

Effect of the Electric Double Layer (EDL) in Multicomponent Electrolyte Reduction and Solid Electrolyte Interphase (SEI) Formation in Lithium Batteries

McDowell

2023

J. Am. Chem. Soc.

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Kinetically corrected Monte Carlo-molecular dynamics simulations of solid electrolyte interphase growth

Cited by 1 publication

References 0 publications

Effect of the Electric Double Layer (EDL) in Multicomponent Electrolyte Reduction and Solid Electrolyte Interphase (SEI) Formation in Lithium Batteries

Effect of the Electric Double Layer (EDL) in Multicomponent Electrolyte Reduction and Solid Electrolyte Interphase (SEI) Formation in Lithium Batteries

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