In Situ Molecular Engineering Strategy to Construct Hierarchical MoS 2 Double-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 situ molecular engineering strategy for the simultaneous construction of hierarchical MoS ₂ double-layer nanotubes (MoS ₂ -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 Zn ²⁺ diffusion efficiency and interface reaction kinetics of MoS ₂ -DLTs are enhanced. When coupled with a homemade ZnMn ₂ O ₄ cathode, the assembled MoS ₂ -DLTs//ZnMn ₂ O ₄ full battery exhibited impressive cycling stability with a capacity retention of 86.6% over 10 000 cycles under 1 A g ^-1 _anode , outperforming most of the reported "rocking-chair" AZIBs. The Zn ²⁺ /H ⁺ cointercalation mechanism of MoS ₂ -DLTs is investigated by synchrotron in situ powder X-ray diffraction and multiple ex situ characterizations. This research demonstrates the feasibility of MoS ₂ for Zn-storage anodes that can be used to construct reliable aqueous full batteries.