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Unveiling the potential-dependent interfacial solvation and reaction chemistry at charged lithium metal anodes
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DOI：10.1016/j.jechem.2026.04.064.png)
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Abstract
En 中文
Constructing a robust solid-electrolyte interphase (SEI) via electrolyte engineering is pivotal for enabling high-energy-density lithium metal batteries. However, rational electrolyte design is severely impeded by the lack of molecular-level understanding of electrochemical processes at the realistic polarized electrode interface, which significantly diverges from bulk electrolytes or simplified uncharged models. Here, by introducing a key applied potential into molecular dynamics (MD) simulations and density functional theory (DFT) calculations, we quantitatively elucidate the significant differences in solvation structures and dynamics between the charged interface and bulk electrolytes through representative ether-based electrolytes. Critically, we reveal that the introduction of a fluorinated diluent (TTE) fundamentally reshapes the electric double layer (EDL) chemistry, establishing a unique interfacial environment with a distinctive contact ion pair cluster. This unique regulation enhances interfacial Li+ diffusion and deposition kinetics. Furthermore, the interfacial electrochemistry and characteristic reactivity of these electrolytes toward Li metal demonstrate that even for the same electrolyte, the SEI formed by its reaction with Li metal exhibits markedly different decomposition pathways and compositional distributions depending on the presence or absence of an applied interfacial potential. This work extends solvation and reaction chemistry to charged interfaces that reflect realistic battery operating conditions, propelling future research at electrode-electrolyte interfaces to a deeper and more experimental realism level.
Keywords:
Electrolyte engineering
Solid-electrolyte interphase (SEI)
Lithium metal anode
Molecular dynamics
Density functional theory
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14.9
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6.0K
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4.5W
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