Computational Insights into Electrolyte-Dependent Li-Ion Charge-Transfer Kinetics at the Li x CoO2 Interface

doi:10.1021/acsenergylett.4c01375

Computational Insights into Electrolyte-Dependent Li-Ion Charge-Transfer Kinetics at the Li x CoO2 Interface

2024-07-03

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Joakim Halldin Stenlid *

DOI：10.1021/acsenergylett.4c01375

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Interface engineering remains a largely underexplored area, and yet it holds the keys to high-performance Li-ion batteries. It is the charge transfer across electrode-electrolyte interfaces, its inefficient energetics, and sluggish kinetics that are oftentimes significant obstacles for achieving fast charging and high power regimes without compromising battery lifespan. This work propose a Boltzmann-averaged first-principles workflow based on constant potential and constrained density functional theory for estimation of atomic scale factors influencing coupled ion-electron charge transfer kinetics across battery electrode-electrolyte interfaces. The approach estimates diabatic Li+ interface energy landscapes as a function of the interface character and operational conditions, needed to simulate charging/discharging currents. Experimental trends for the Li x CoO2 (0.5 <= x <= 1.0) electrode in varied organic electrolytes with LiPF6 and LiClO4 salts are reproduced, identifying Li+ transfer energy and Li+ adsorption energy as decisive factors influencing the enhanced kinetics in LiClO4-based electrolytes over LiPF6, rationalized by a stronger surface interaction of ClO4 -

Keywords:

REORGANIZATION ENERGIES

TRANSITION

LICOO2

INTERCALATION

DENSITY

STABILITY

CONTINUUM

Computational Insights into Electrolyte-Dependent Li-Ion Charge-Transfer Kinetics at the Li x CoO2 Interface

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