Fluorinated Electrolytes for High-Energy Ni-rich NCA90 Lithium-Ion Batteries at a Cylindrical Cell Configuration: A Deep Dive into Decomposition Pathways.

IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY ChemSusChem Pub Date : 2025-03-12 DOI:10.1002/cssc.202500238
Kan Homlamai, Thitiphum Sangsanit, Ronnachai Songthan, Worapol Tejangkura, Montree Sawangphruk
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引用次数: 0

Abstract

This study investigates the electrochemical performance, stability, and decomposition mechanisms of fluorine-based electrolytes in large-scale cylindrical Ni-rich lithium-ion batteries (LIBs) under high-voltage conditions (up to 4.8 V). We examine fluoroethylene carbonate (FEC) and di-fluoroethylene carbonate (DFEC) in electrolyte formulations and their effects on battery longevity, gas evolution, and solvation dynamics. While FEC is known for improving the solid electrolyte interphase (SEI), DFEC remains underexplored. Using molecular dynamics (MD) simulations, density functional theory (DFT) calculations, and electrochemical analysis, we identify key solvation properties, ion transport characteristics (tLi+, CIP%), and electronic structures influencing electrolyte stability. The 1.2 M LiPF6 in DMC/FEC/DFEC (4:0.5:0.5% v/v) electrolyte achieves the highest capacity retention (85.11% after 1,000 cycles), with DFEC reducing solvation shell binding energy and stabilizing electrolyte performance. Differential electrochemical mass spectrometry (DEMS) and nuclear magnetic resonance (NMR) spectroscopy reveal that FEC leads to higher CO2 production via ring-opening and de-fluorination to vinylene carbonate (VC), while DFEC reduces gas evolution. These insights provide a holistic framework for optimizing high-energy electrolyte formulations, supporting the development of safer, more efficient LIBs for electric vehicles and energy storage applications.

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来源期刊
ChemSusChem
ChemSusChem 化学-化学综合
CiteScore
15.80
自引率
4.80%
发文量
555
审稿时长
1.8 months
期刊介绍: ChemSusChem Impact Factor (2016): 7.226 Scope: Interdisciplinary journal Focuses on research at the interface of chemistry and sustainability Features the best research on sustainability and energy Areas Covered: Chemistry Materials Science Chemical Engineering Biotechnology
期刊最新文献
Atomic intercalation - an approach to enhance photogenerated carrier dynamics for efficient photocatalysis carbon dioxide reduction. Fluorinated Electrolytes for High-Energy Ni-rich NCA90 Lithium-Ion Batteries at a Cylindrical Cell Configuration: A Deep Dive into Decomposition Pathways. Non-copper-based Catalysts for CO2 Electroreduction to Multi-carbon Compounds. Role of Ethylene Diamine Tetraacetate as an Additive in Electrolyte on Intermediate Stabilization in Electrochemical CO2 Reduction. Carbon-coated Urchin-like Silica Nanospheres for Enhanced Photothermal Catalysis.
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