Abstract
Lithium-ion batteries with transition metal sulfides (TMSs) anodes promise a high capacity, abundant resources, and environmental friendliness, yet they suffer from fast degradation and low Coulombic efficiency. Here, a heterostructured bimetallic TMS anode is fabricated by in situ encapsulating SnS(2)/MoS(2) nanoparticles within an amphiphilic hollow double-graphene sheet (DGS). The hierarchically porous DGS consists of inner hydrophilic graphene and outer hydrophobic graphene, which can accelerate electron/ion migration and strongly hold the integrity of alloy microparticles during expansion and/or shrinkage. Moreover, catalytic Mo converted from lithiated MoS(2) can promote the reaction kinetics and suppress heterointerface passivation by forming a building-in-electric field, thereby enhancing the reversible conversion of Sn to SnS(2). Consequently, the SnS(2)/MoS(2)/DGS anode with high gravimetric and high volumetric capacities achieves 200 cycles with a high initial Coulombic efficiency of >90%, as well as excellent low-temperature performance. When the commercial Li(Ni(0.8)Co(0.1)Mn(0.1))O(2) (NCM811) cathode is paired with the prelithiated SnS(2)/MoS(2)/DGS anode, the full cells deliver high gravimetric and volumetric energy densities of 577 Wh kg(-1) and 853 Wh L(-1), respectively. This work highlights the significance of integrating spatial confinement and atomic heterointerface engineering to solve the shortcomings of conversion-/alloying typed TMS-based anodes to construct outstanding high-energy LIBs.