Interconnected Vertically Stacked 2D-MoS₂ for Ultrastable Cycling of Rechargeable Li-Ion Battery

A two-dimensional (2D) layer-structured material is often a high-capacity ionic storage material with fast ionic transport within the layers. This appears to be the case for nonconversion layer structure, such as graphite. However, this is not the case for conversion-type layered structure such as transition-metal sulfide, in which localized congestion of ionic species adjacent to the surface will induce localized conversion, leading to the blocking of the fast diffusion channels and fast capacity fading, which therefore constitutes one of the critical barriers for the application of transition-metal sulfide layered structure. In this work, we report the tackling of this critical barrier through nanoscale engineering. We discover that interconnected vertically stacked two-dimensional-molybdenum disulfide can dramatically enhance the cycling stability. Atomic-level in situ transmission electron microscopy observation reveals that the molybdenum disulfide (MoS2) nanocakes assembled with tangling {100}-terminated nanosheets offer abundant open channels for Li+ insertion through the {100} surface, featuring an exceptional cyclability performance for over 200 cycles with a capacity retention of 90%. In contrast, (002)-terminated MoS2 nanoflowers only retain 10% of original capacity after 50 cycles. The present work demonstrates a general principle and opens a new route of crystallographic design to enhance electrochemical performance for assembling 2D materials for energy storage.