Unlocking the Potential of Li‐Rich Mn‐Based Oxides for High‐Rate Rechargeable Lithium‐Ion Batteries

Abstract

Lithium‐rich Mn‐based oxides have gained significant attention worldwide as potential cathode materials for the next generation of high‐energy density lithium‐ion batteries due to their discharge capacities exceeding 250 mAh g–1. Nonetheless, the inferior rate capability and voltage decay issues present formidable challenges. Conventional approaches to improving rate performance, like nano‐ and porous structural design, increase surface area of cathode and consequently accelerate harmful Mn‐ion migration and oxygen loss. Here, we initially synthesize a Li‐rich material equipped with quasi‐three‐dimensional Li‐ion diffusion channels by introducing twin structures with high Li‐ion diffusion coefficients into the crystal and constructing a “bridge” between different Li‐ion diffusion tunnels. The as‐prepared material exhibits monodispersed micron‐sized primary particles, delivering a specific capacity of 303 mAh g−1 at 0.1C and an impressive capacity of 253 mAh g−1 at 1C. More importantly, the twin structure also serves as a “breakwater” to inhibit the migration of Mn ions and improve the overall structural stability, leading to long‐term cycling stability with 85% capacity retention at 1C after 200 cycles. Our proposed strategy of constructing quasi‐three‐dimensional channels in the layered Li‐rich cathodes will open up new avenues for the research and development of other layered oxide cathodes, with potential applications in industry.This article is protected by copyright. All rights reserved

Achieving the High Capacity and High Stability of Li‐Rich Oxide Cathode in Garnet‐Based Solid‐State Battery

“…OAR is one typical characteristic in Li-rich oxide cathodes which has been extensively explored in LE-based cells. [55][56][57] Knowing about the OAR behavior of LRMO in SSBs is also quite important. RIXS has a very good sensitivity to the oxidation state of O, [58] and for this reason, it is applied to detect the state of O 2À at different voltages on the LRMO cathode both in SSBs and LE-based cells.…”

Rejuvenating manganese-based rechargeable batteries: fundamentals, status and promise

“…Lithium-rich manganese oxide has poor magnification performance and voltage attenuation. By introducing a twin structure with a high lithium-ion diffusion coefficient into the crystal and building a “bridge” between different lithium-ion diffusion channels, Xia et al 120 initially synthesized a lithium-rich material with a quasi-three-dimensional lithium-ion diffusion channel. The prepared material has monodispersed micron-scale primary particles that provide a specific capacity of 303 mA h g −1 at 0.1C and 253 mA h g −1 at 1C.…”

Perspective on High-Stability Single-Crystal Li-Rich Cathode Materials for Li-Ion Batteries

“…These results suggested SC morphology and size have great effect on activation of oxygen-related capacity and its reversibility. Besides, Yang et al developed the SC Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 with micrometer-sized primary particles (MP) by the combination of coprecipitation, calcination, and ion-exchange methods, displaying a high reversible discharge capacity of 303 mAh g –1 with Coulombic efficiency of 94.4% during the third cycle in voltage range of 2.1–4.8 V, which demonstrated the high oxygen stability can be achieved in MP electrode during activation process . In contrast, a limited discharge capacity of 285 mAh g –1 with Coulombic efficiency of 87.7% was obtained in a PC cathode with the morphology of agglomerated particle (AP) (Figure f).…”

“…Recently, Yang et al obtained a dispersed SC Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 (MP) with uniform particle size of 1−2 μm via ion-exchange strategy,34 in which XRD pattern can be indexed by layered structure (belongs to R/3m space group) and ordered arrangement of Li/Mn in TM layer (belongs to C/2m space group) (Figure9g). −1 at same current densities (Figure9h), which can be ascribed to its 3D Li-ion diffusion network to achieve excellent Li + dynamics.…”