Interlayer-Spacing-Modification of MoS₂ via Inserted PANI with Fast Kinetics for Highly Reversible Aqueous Zinc-Ion...

Layered transition metal dichalcogenides (TMDs) have gained considerable attention as promising cathodes for aqueous zinc-ion batteries (AZIBs) because of their tunable interlayer architecture and rich active sites for Zn²⁺ storage. However, unmodified TMDs face significant challenges, including limited redox activity, sluggish kinetics, and insufficient structural stability during cycling. These limitations are primarily attributed to their narrow interlayer spacing, strong electrostatic interactions, the large ionic hydration radius, and their high binding energy of Zn²⁺ ions. To address these restrictions, an in situ organic polyaniline (PANI) intercalation strategy is proposed to construct molybdenum disulfide (MoS₂)-based cathodes with extended layer spacing, thereby improving the zinc storage capabilities. The intercalation of PANI effectively enhances interplanar spacing of MoS₂ from 0.63 nm to 0.98 nm, significantly facilitating rapid Zn²⁺ diffusion. Additionally, the π-conjugated electron structure introduced by PANI effectively shields the electrostatic interaction between Zn²⁺ ions and the MoS₂ host, thereby promoting Zn²⁺ diffusion kinetics. Furthermore, PANI also serves as a structural stabilizer, maintaining the integrity of the MoS₂ layers during Zn-ion insertion/extraction processes. Furthermore, the conductive conjugated PANI boosts the ionic and electronic conductivity of the electrodes. As expected, the PANI-MoS₂ electrodes exhibit exceptional electrochemical performance, delivering a high specific capacity of 150.1 mA h g^-1 at 0.1 A g^-1 and retaining 113.3 mA h g^-1 at 1 A g^-1, with high capacity retention of 81.2% after 500 cycles. Ex situ characterization techniques confirm the efficient and reversible intercalation/deintercalation of Zn²⁺ ions within the PANI-MoS₂ layers. This work supplies a rational interlayer engineering strategy to optimize the electrochemical performance of MoS₂-based electrodes. By addressing the structural and kinetic limitations of TMDs, this approach offers new insights into the development of high-performance AZIBs for energy storage applications.