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Interfacial Engineering of Dry-Processed High-Loading LiNi0.5Mn1.5O4 Cathodes: Additive Dissolution and Bilayer
Zhicheng Liu1, Xing Ma1, Dingyi Zhang1
1State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China.
ACS Applied Materials & Interfaces
|June 6, 2026
Summary
This study enhances lithium metal batteries (LMBs) by engineering interfaces to prevent electrolyte breakdown. Novel electrode and electrolyte modifications enable stable high-voltage performance and long cycle life for advanced energy storage.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Lithium metal batteries (LMBs) with high-voltage cathodes like LiNi0.5Mn1.5O4 (LNMO) offer high energy density but face electrolyte instability.
- Carbonate-based electrolytes are incompatible with reactive high-voltage cathodes and anodes, limiting practical applications of LNMO/Li batteries.
Purpose of the Study:
- To develop a novel interfacial engineering strategy for LNMO/Li batteries to overcome electrolyte incompatibility issues.
- To improve the cycling stability, energy density, and overall performance of high-voltage LMBs using conventional electrolytes.
Main Methods:
- Implemented a dry electrode fabrication process using vapor-grown carbon fibers (VGCFs) coated with polytetrafluoroethylene (PTFE) to passivate active sites.
- Incorporated lithium nonafluorobutanesulfonate (LNBS) and succinonitrile (SN) as functional additives in the cathode for interfacial modification.
- Utilized lithium difluoro(oxalato)borate (LiODFB) for preferential decomposition at the cathode interface, forming a protective bilayer.
Main Results:
- The synergistic interfacial modifications enabled LNMO/Li batteries with high-loading cathodes (20 mg cm-2) to achieve 88.6% capacity retention after 400 cycles at 0.5 C.
- The cells demonstrated an average Coulombic efficiency of 99.44% and maintained an open-circuit voltage above 4.68 V for over 1400 hours when charged to 4.85 V.
- The strategy effectively suppressed electrolyte oxidation and transition metal ion dissolution, leading to exceptional cycling and storage stability.
Conclusions:
- The proposed electrode-electrolyte interfacial engineering strategy successfully enhances the stability and performance of high-voltage LNMO/Li batteries.
- This approach allows the use of conventional carbonate-based electrolytes, paving the way for practical next-generation energy storage solutions.
- The developed methods offer a viable pathway for realizing the full potential of high-energy-density lithium metal batteries.
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