A Bifunctional-Modulated Conformal Li/Mn-Rich Layered Cathode for Fast-Charging, High Volumetric Density and Durable...

Lithium- and manganese-rich (LMR) layered cathode materials hold the great promise in designing the next-generation high energy density lithium ion batteries. However, due to the severe surface phase transformation and structure collapse, stabilizing LMR to suppress capacity fade has been a critical challenge. Here, a bifunctional strategy that integrates the advantages of surface modification and structural design is proposed to address the above issues. A model compound Li_1.2Mn_0.54Ni_0.13Co_0.13O₂ (MNC) with semi-hollow microsphere structure is synthesized, of which the surface is modified by surface-treated layer and graphene/carbon nanotube dual layers. The unique structure design enabled high tap density (2.1 g cm^-3) and bidirectional ion diffusion pathways. The dual surface coatings covalent bonded with MNC via C-O-M linkage greatly improves charge transfer efficiency and mitigates electrode degradation. Owing to the synergistic effect, the obtained MNC cathode is highly conformal with durable structure integrity, exhibiting high volumetric energy density (2234 Wh L^-1) and predominant capacitive behavior. The assembled full cell, with nanographite as the anode, reveals an energy density of 526.5 Wh kg^-1, good rate performance (70.3% retention at 20 C) and long cycle life (1000 cycles). The strategy presented in this work may shed light on designing other high-performance energy devices.