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Lee, Myeong Hwan

Publications and source records attributed to Lee, Myeong Hwan.

A Fiber-Based 3D Lithium Host for Lean Electrolyte Lithium Metal Batteries

3D hosts are promising to extend the cycle life of lithium metal anodes but have rarely been implemented with lean electrolytes thus impacting the practical cell energy density. To overcome this challenge, a 3D host that is lightweight and easy to fabricate with optimum pore size that enables full utilization of its pore volume, essential for lean electrolyte operations, is reported. The host is fabricated by casting a VGCF (vapor-grown carbon fiber)-based slurry loaded with a sparingly soluble rubidium nitrate salt as an additive. The network of fibers generates uniform pores of ≈3 µm in diameter with a porosity of 80%, while the nitrate additive enhances lithiophilicity. This 3D host delivers an average coulombic efficiency of 99.36% at 1 mA cm -2 and 1 mAh cm -2 for over 860 cycles in half-cell tests. Full cells containing an anode with 1.35-fold excess lithium paired with LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathodes exhibit capacity retention of 80% over 176 cycles at C/2 under a lean electrolyte condition of 3 g Ah -1 . This work provides a facile and scalable method to advance 3D lithium hosts closer to practical lithium-metal batteries.

36 MATERIALS SCIENCE↗

High-Voltage Phosphate Cathodes for Rechargeable Ca-Ion Batteries

Calcium-ion batteries (CIBs) are under investigation as next-generation energy storage devices due to their theoretically high operating potentials and lower costs tied to the high natural abundance of calcium. However, the development of CIBs has been limited by the lack of available positive electrode materials. In this study, for the first time, we report two functional polyanionic phosphate materials as high-voltage cathodes for CIBs at room temperature. NaV 2 (PO 4 ) 3 electrodes were found to reversibly intercalate 0.6 mol of Ca 2+ (81 mA h g –1 ) near 3.2 V (vs Ca 2+ /Ca) with stable cycling performance at a current density of 3.5 mA g –1 . The olivine framework material FePO 4 reversibly intercalates 0.2 mol of Ca 2+ (72 mA h g –1 ) near 2.9 V (vs Ca 2+ /Ca) at a current density of 7.5 mA g –1 in the first cycle. Structural, electronic, and compositional changes are consistent with reversible Ca 2+ intercalation into these two materials.

25 ENERGY STORAGE↗

Voltage decay and redox asymmetry mitigation by reversible cation migration in lithium-rich layered oxide electrodes

Despite the high energy density of lithium-rich layered-oxide electrodes, their real-world implementation in batteries is hindered by the substantial voltage decay on cycling. This voltage decay is widely accepted to mainly originate from progressive structural rearrangements involving irreversible transition-metal migration. As prevention of this spontaneous cation migration has proven difficult, a paradigm shift toward management of its reversibility is needed. Herein, we demonstrate that the reversibility of the cation migration of lithium-rich nickel manganese oxides can be remarkably improved by altering the oxygen stacking sequences in the layered structure and thereby dramatically reducing the voltage decay. The preeminent intra-cycle reversibility of the cation migration is experimentally visualized, and first-principles calculations reveal that an O2-type structure restricts the movements of transition metals within the Li layer, which effectively streamlines the returning migration path of the transition metals. Furthermore, we propose that the enhanced reversibility mitigates the asymmetry of the anionic redox in conventional lithium-rich electrodes, promoting the high-potential anionic reduction, thereby reducing the subsequent voltage hysteresis. Our findings demonstrate that regulating the reversibility of the cation migration is a practical strategy to reduce voltage decay and hysteresis in lithium-rich layered materials.

25 ENERGY STORAGE↗