Synergistic Optimization of Composition-Structure-Conductive Network for High-Performance Integrated Transition Metal Oxide Anodes for Lithium-Ion Batteries

Abstract

Transition metal oxides (TMOs) exhibit great potential as anodes for lithium-ion batteries due to their superior theoretical capacity. However, significant volumetric expansion and low electron/ion migration rate limit the practical applications of TMOs. In this work, we have developed a hierarchically porous MnO-rich CuMn bimetallic oxide electrode with an in-situ formed Cu conductive network(hpCM-CMO-Cu), which represents a promising solution to address these challenges. Benefiting from the synergistic optimization of composition -structure-conductive network, hpCM-CMO-Cu not only achieves high energy density but also demonstrates outstanding electrical conductivity and stability. Due to the exceptional capacity offered by manganese oxide, hpCM-CMO-Cu achieves a remarkable reversible capacity of 5.57 mAh cm-2 at 0.4 mA cm-2. The in-situ constructed conductive network and robust chemical bonding between oxide and substrate effectively prevent active material detachment and enhance electrode conductivity, enabling a high areal capacity of 4.38 mA h cm-2 at 1.0 mA cm-2 after 250 cycles. The abundant void spaces within the hierarchical porous structure effectively accommodate the volume expansion of oxides during cycling, exhibits negligible macroscopic swelling after 50 cycles. The cost-effective electrode design mitigates the intrinsic poor conductivity and substantial volume expansion of TMOs anodes, demonstrating significant potential for their commercialization in lithium-ion batteries.