Functional Composite Dual-Phase In Situ Self-Reconstruction Design for High-Energy-Density Li-Rich Cathodes

The unique anionic redox mechanism provides, high-capacity, irreversible oxygen release and voltage/capacity degradation to Li-rich cathode materials (LRO, Li_1.2Mn_0.54Co_0.13Ni_0.13O₂). In this study, an integrated stabilized carbon–rock salt/spinel composite heterostructured layers (C@spinel/MO) is constructed by in situ self-reconstruction, and the generation mechanism of the in situ reconstructed surface is elucidated. The formation of atomic-level connections between the surface-protected phase and bulk-layered phase contributes to electrochemical performance. The best-performing sample shows a high increase (63%) of capacity retention compared to that of the pristine sample after 100 cycles at 1C, with an 86.7% reduction in surface oxygen release shown by differential electrochemical mass spectrometry. Soft X-ray results show that Co³⁺ and Mn⁴⁺ are mainly reduce in the carbothermal reduction reaction and participate in the formation of the spinel/MO rock-salt phase. The results of oxygen release characterized by Differential electrochemical mass spectrometry (DEMS) strongly prove the effectiveness of surface reconstruction.