In Situ Construction of Zn₂Mo₃O₈/ZnO Hierarchical Nanosheets on Graphene as Advanced Anode Materials for Lithium-Ion Batteries

Transition-metal oxides as anodes for lithium-ion batteries (LIBs) have attracted enormous interest because of their high theoretical capacity, low cost, and high reserve abundance. Unfortunately, they commonly suffer from poor electronic and ionic conductivity and relatively large volume expansion during discharge/charge processes, thereby triggering inferior cyclic performance and rate capability. Herein, a molybdenum-zinc bimetal oxide-based composite structure (Zn2Mo3O8/ZnO/rGO) with rectangular Zn2Mo3O8/ZnO nanosheets uniformly dispersed on reduced graphene oxide (rGO) has been prepared by using a simple and controllable cyanometallic framework template method. The Zn2Mo3O8/ZnO rectangular nanosheets with desirable porous features are composed of nanocrystalline subunits, facilitating the exposure of abundant active sites and providing sufficient contact with the electrolyte. Benefiting from the composition and structural merits as well as the induced synergistic effects, the Zn2Mo3O8/ZnO/rGO composite as LIB anodes delivers superior electrochemical properties, including high reversible capacity (960 mA h g-1 after 100 cycles at 200 mA g-1), outstanding rate performance (417 mA h g-1 at 10,000 mA g-1), and admirable long-term cyclic stability (862 mA h g-1 after 400 cycles at 1000 mA g-1). The mechanism of lithium storage and the formation of SEI film are systematically elucidated. This work provides an effective strategy for synthesizing promising Mo-cluster compound-based anodes for high-performance LIBs.