Computational Insights into Electrolyte-Dependent Li-Ion Charge-Transfer Kinetics at the Li x CoO 2 Interface
Source abstract
Abstract
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 CoO 2 (0.5 ≤ x ≤ 1.0) electrode in varied organic electrolytes with LiPF 6 and LiClO 4 salts are reproduced, identifying Li + transfer energy and Li + adsorption energy as decisive factors influencing the enhanced kinetics in LiClO 4 -based electrolytes over LiPF 6, rationalized by a stronger surface interaction of ClO 4 –
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Advanced Battery Technologies Research
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
KBR, Inc., Intelligent Systems Division, NASA Ames Research Center, Moffett Field, California 94035, United States
Department of Materials Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States
Department of Mechanical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Ave., Cambridge, Massachusetts 02139, United States
Research Laboratory of Electronics, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States
Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02142, United States
Department of Mathematics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02142, United States
Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
Intelligent Systems Division, NASA Ames Research Center, Moffett Field, California 94035, United States
Funding
Aeronautics Research Mission Directorate · National Aeronautics and Space Administration · Shell International Exploration and Production Inc.
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