Unraveling the “Gap‐Filling” Mechanism of Multiple Charge Carriers in Aqueous Zn‐MoS2 Batteries

The utilization rate of active sites in cathode materials for Zn‐based batteries is a key factor determining the reversible capacities. However, a long‐neglected issue of the strong electrostatic repulsions among divalent Zn2+ in hosts inevitably causes the squander of some active sites (i.e., gap sites). Herein, we address this conundrum by unraveling the “gap‐filling” mechanism of multiple charge carriers in aqueous Zn‐MoS2 batteries. The tailored MoS2/(reduced graphene quantum dots) hybrid features an ultra‐large interlayer spacing (2.34 nm), superior electrical conductivity/hydrophilicity, and robust layered structure, demonstrating highly reversible NH4+/Zn2+/H+ co‐insertion/extraction chemistry in the 1 M ZnSO4+0.5 M (NH4)2SO4 aqueous electrolyte. The NH4+ and H+ ions can act as gap fillers to fully utilize the active sites and screen electrostatic interactions to accelerate the Zn2+ diffusion. Thus, unprecedentedly high rate capability (439.5 and 104.3 mAh g−1 at 0.1 and 30 A g−1, respectively) and ultra‐long cycling life (8000 cycles) are achieved. A novel MoS2/(reduced graphene quantum dots) hybrid featuring ultra‐large interlayer spacing, superior electrical conductivity/hydrophilicity, and robust layered structure demonstrates highly reversible NH4+/Zn2+/H+ co‐insertion/extraction chemistry in aqueous Zn‐based batteries, where NH4+ and H+ can serve as “gap‐filling” ions to improve the utilization rate of active sites and screen electrostatic interactions to facilitate the Zn2+ diffusion.