In SituMolecular Engineering Strategy to Construct Hierarchical MoS2Double-Layer Nanotubes for Ultralong Lifespan “Rocking-Chair” Aqueous Zinc-Ion Batteries

Rechargeable aqueous zinc ion batteries (AZIBs) have gained considerable attention owing to their low cost and high safety, but dendrite growth, low plating/stripping efficiency, surface passivation, and self-erosion of the Zn metal anode are hindering their application. Herein, a one-step in situmolecular engineering strategy for the simultaneous construction of hierarchical MoS2double-layer nanotubes (MoS2-DLTs) with expanded layer-spacing, oxygen doping, structural defects, and an abundant 1T-phase is proposed, which are designed as an intercalation-type anode for “rocking-chair” AZIBs, avoiding the Zn anode issues and therefore displaying a long cycling life. Benefiting from the structural optimization and molecular engineering, the Zn2+diffusion efficiency and interface reaction kinetics of MoS2-DLTs are enhanced. When coupled with a homemade ZnMn2O4cathode, the assembled MoS2-DLTs//ZnMn2O4full battery exhibited impressive cycling stability with a capacity retention of 86.6% over 10 000 cycles under 1 A g–1anode, outperforming most of the reported “rocking-chair” AZIBs. The Zn2+/H+cointercalation mechanism of MoS2-DLTs is investigated by synchrotron in situpowder X-ray diffraction and multiple ex situcharacterizations. This research demonstrates the feasibility of MoS2for Zn-storage anodes that can be used to construct reliable aqueous full batteries.