Journal
CHEMICAL ENGINEERING JOURNAL
Volume 450, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.138318
Keywords
Chemistry of electrolyte; Anchor-oxygen interface layer; Electrode/electrolyte interface; Li-rich Mn-based oxide cathode; Lithium ion batteries
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Funding
- National Key Research and Development Program of China [2019YFC1907805]
- National Natural Science Foundation of China [U21A20284]
- Fundamental Research Funds for the Central Universities of Central South University [2021zzts0072]
- MCD-B (Soochow Beamline for Energy Materials) at NSRL
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The study demonstrates a novel strategy to enhance the cycling stability of cathode materials in lithium-ion batteries by manipulating the electrolyte additive and solvent polarity, minimizing lattice oxygen escape and inhibiting irreversible phase transformation.
Sacrificial additive as an electrolyte engineering could regulate the electrode/electrolyte interface for advanced energy storage devices. In particular, the evolution of cathode electrolyte interface (CEI) is closely related with the epitaxial coordination environment of cathode materials. Herein, polarly modulated solvent strategy is successfully achieved, in which the electrochemical oxidation potential of perfluorinated electrolyte with tris (trimethylsilyl)borate additive is manipulated by the polarity of solvent structure. By taking Li-rich Mn-based oxide (LRM) as a model cathode, the interfacial quasicrystal bonding effects are ingeniously aroused between the interfacial lattice oxygen of LRM cathode and anchor oxygen CEI layer. More greatly, the formation energy of oxygen vacancy is effectively elevated by constructing the epitaxially strong covalent B/Si-O bonding, thereby considerably mitigating the lattice oxygen escaping and inhibiting the irreversible phase transformation. Consequently, LRM cathode with robust anchor oxygen CEI renders improved cycling stability after 200 loops with 87.5% capacity retention at 1C as compared to anchor oxygen-free LRM with only 61.9%. Given this, these findings inform new chemical and interface strategies to facilitate the application of high voltage cathodes.
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